Brown carbon absorption in the red and near-infrared spectral region

NASA Astrophysics Data System (ADS)

Hoffer, András; Tóth, Ádám; Pósfai, Mihály; Eddy Chung, Chul; Gelencsér, András

2017-06-01

Black carbon (BC) aerosols have often been assumed to be the only light-absorbing carbonaceous particles in the red and near-infrared spectral regions of solar radiation in the atmosphere. Here we report that tar balls (a specific type of organic aerosol particles from biomass burning) do absorb red and near-infrared radiation significantly. Tar balls were produced in a laboratory experiment, and their chemical and optical properties were measured. The absorption of these particles in the range between 470 and 950 nm was measured with an aethalometer, which is widely used to measure atmospheric aerosol absorption. We find that the absorption coefficient of tar balls at 880 nm is more than 10 % of that at 470 nm. The considerable absorption of red and infrared light by tar balls also follows from their relatively low absorption Ångström coefficient (and significant mass absorption coefficient) in the spectral range between 470 and 950 nm. Our results support the previous finding that tar balls may play an important role in global warming. Due to the non-negligible absorption of tar balls in the near-infrared region, the absorption measured in the field at near-infrared wavelengths cannot solely be due to soot particles.

Aerosol optical properties over the Svalbard region of Arctic: ground-based measurements and satellite remote sensing

NASA Astrophysics Data System (ADS)

Gogoi, Mukunda M.; Babu, S. Suresh

2016-05-01

In view of the increasing anthropogenic presence and influence of aerosols in the northern polar regions, long-term continuous measurements of aerosol optical parameters have been investigated over the Svalbard region of Norwegian Arctic (Ny-Ålesund, 79°N, 12°E, 8 m ASL). This study has shown a consistent enhancement in the aerosol scattering and absorption coefficients during spring. The relative dominance of absorbing aerosols is more near the surface (lower single scattering albedo), compared to that at the higher altitude. This is indicative of the presence of local anthropogenic activities. In addition, long-range transported biomass burning aerosols (inferred from the spectral variation of absorption coefficient) also contribute significantly to the higher aerosol absorption in the Arctic spring. Aerosol optical depth (AOD) estimates from ground based Microtop sun-photometer measurements reveals that the columnar abundance of aerosols reaches the peak during spring season. Comparison of AODs between ground based and satellite remote sensing indicates that deep blue algorithm of Moderate Resolution Imaging Spectroradiometer (MODIS) retrievals over Arctic snow surfaces overestimate the columnar AOD.

Light Absorption of Stratospheric Aerosols: Long-Term Trend and Contribution by Aircraft

NASA Technical Reports Server (NTRS)

Pueschel , R. F.; Gore, Waren J. Y. (Technical Monitor)

1997-01-01

Measurements of aerosol light-absorption coefficients are useful for studies of radiative transfer and heating rates. Ogren appears to have published the first light- absorption coefficients in the stratosphere in 1981, followed by Clarke in 1983 and Pueschel in 1992. Because most stratospheric soot appears to be due to aircraft operations, application of an aircraft soot aerosol emission index to projected fuel consumption suggests a threefold increase of soot loading and light absorption by 2025. Together, those four data sets indicate an increase in mid-visible light extinction at a rate of 6 % per year. This trend is similar to the increase per year of sulfuric acid aerosol and of commercial fleet size. The proportionality between stepped-up aircraft operations above the tropopause and increases in stratospheric soot and sulfuric acid aerosol implicate aircraft as a source of stratospheric pollution. Because the strongly light-absorbing soot and the predominantly light-scattering sulfuric acid aerosol increase at similar rates, however, the mid-visible stratospheric aerosol single scatter albedo is expected to remain constant and not approach a critical value of 0.98 at which stratospheric cooling could change to warming.

[Determination of the error of aerosol extinction coefficient measured by DOAS].

PubMed

Si, Fu-qi; Liu, Jian-guo; Xie, Pin-hua; Zhang, Yu-jun; Wang, Mian; Liu, Wen-qing; Hiroaki, Kuze; Liu, Cheng; Nobuo, Takeuchi

2006-10-01

The method of defining the error of aerosol extinction coefficient measured by differential optical absorption spectroscopy (DOAS) is described. Some factors which could bring errors to result, such as variation of source, integral time, atmospheric turbulence, calibration of system parameter, displacement of system, and back scattering of particles, are analyzed. The error of aerosol extinction coefficient, 0.03 km(-1), is determined by theoretical analysis and practical measurement.

Aerosol optical properties at rural background area in Western Saudi Arabia

NASA Astrophysics Data System (ADS)

Lihavainen, H.; Alghamdi, M. A.; Hyvärinen, A.; Hussein, T.; Neitola, K.; Khoder, M.; Abdelmaksoud, A. S.; Al-Jeelani, H.; Shabbaj, I. I.; Almehmadi, F. M.

2017-11-01

To derive the comprehensive aerosol in situ characteristics at a rural background area in Saudi Arabia, an aerosol measurements station was established to Hada Al Sham, 60 km east from the Red Sea and the city of Jeddah. The present sturdy describes the observational data from February 2013 to February 2015 of scattering and absorption coefficients, Ångström exponents and single scattering albedo over the measurement period. The average scattering and absorption coefficients at wavelength 525 nm were 109 ± 71 Mm- 1 (mean ± SD, at STP conditions) and 15 ± 17 Mm- 1 (at STP conditions), respectively. As expected, the scattering coefficient was dominated by large desert dust particles with low Ångström scattering exponent, 0.49 ± 0.62. Especially from February to June the Ångström scattering exponent was clearly lower (0.23) and scattering coefficients higher (124 Mm- 1) than total averages because of the dust outbreak season. Aerosol optical properties had clear diurnal cycle. The lowest scattering and absorption coefficients and aerosol optical depths were observed around noon. The observed diurnal variation is caused by wind direction and speed, during night time very calm easterly winds are dominating whereas during daytime the stronger westerly winds are dominating (sea breeze). Positive Matrix Factorization mathematical tool was applied to the scattering and absorption coefficients and PM2.5 and coarse mode (PM10-PM2.5) mass concentrations to identify source characteristics. Three different factors with clearly different properties were found; anthropogenic, BC source and desert dust. Mass absorption efficiencies for BC source and desert dust factors were, 6.0 m2 g- 1 and 0.4 m2 g- 1, respectively, and mass scattering efficiencies for anthropogenic (sulphate) and desert dust, 2.5 m2 g- 1 and 0.8 m2 g- 1, respectively.

Vertical Profiles of Light-Absorbing Aerosol: A Combination of In-situ and AERONET Observations during NASA DISCOVER-AQ

NASA Astrophysics Data System (ADS)

Ziemba, L. D.; Beyersdorf, A. J.; Chen, G.; Corr, C.; Crumeyrolle, S.; Giles, D. M.; Holben, B. N.; Hudgins, C.; Martin, R.; Moore, R.; Shook, M.; Thornhill, K. L., II; Winstead, E.; Anderson, B. E.

2014-12-01

Understanding the vertical profile of atmospheric aerosols plays a vital role in utilizing spaceborne, column-integrated satellite observations. The properties and distribution of light-absorbing aerosol are particularly uncertain despite significant air quality and climate ramifications. Advanced retrieval algorithms are able to derive complex aerosol properties (e.g., wavelength-dependent absorption coefficient and single scattering albedo) from remote-sensing measurements, but quantitative relationships to surface conditions remain a challenge. Highly systematic atmospheric profiling during four unique deployments for the NASA DISCOVER-AQ project (Baltimore, MD, 2011; San Joaquin Valley, CA, 2013; Houston, TX, 2013; Denver, CO, 2014) allow statistical assessment of spatial, temporal, and source-related variability for light-absorbing aerosol properties in these distinct regions. In-situ sampling in conjunction with a dense network of AERONET sensors also allows evaluation of the sensitivity, limitations, and advantages of remote-sensing data products over a wide range of conditions. In-situ aerosol and gas-phase observations were made during DISCOVER-AQ aboard the NASA P-3B aircraft. Aerosol absorption coefficients were measured by a Particle Soot Absorption Photometer (PSAP). Approximately 200 profiles for each of the four deployments were obtained, from the surface (25-300m altitude) to 5 km, and are used to calculate absorption aerosol optical depths (AAODs). These are quantitatively compared to AAOD derived from AERONET Level 1.5 retrievals to 1) explore discrepancies between measurements, 2) quantify the fraction of AAOD that exists directly at the surface and is often missed by airborne sampling, and 3) evaluate the potential for deriving ground-level black carbon (BC) concentrations for air quality prediction. Aerosol size distributions are used to assess absorption contributions from mineral dust, both at the surface and aloft. SP2 (Single Particle Soot Photometer) mixing state and coating thickness analyses will be explored to explain in-situ/AERONET discrepancies, and ground-based absorption coefficient and BC-mass observations will be utilized whenever possible to fully obtain the true absorption vertical profile.

Aethalometer multiple scattering correction Cref for mineral dust aerosols

NASA Astrophysics Data System (ADS)

Di Biagio, Claudia; Formenti, Paola; Cazaunau, Mathieu; Pangui, Edouard; Marchand, Nicolas; Doussin, Jean-François

2017-08-01

In this study we provide a first estimate of the Aethalometer multiple scattering correction Cref for mineral dust aerosols. Cref is an empirical constant used to correct the aerosol absorption coefficient measurements for the multiple scattering artefact of the Aethalometer; i.e. the filter fibres on which aerosols are deposited scatter light and this is miscounted as absorption. The Cref at 450 and 660 nm was obtained from the direct comparison of Aethalometer data (Magee Sci. AE31) with (i) the absorption coefficient calculated as the difference between the extinction and scattering coefficients measured by a Cavity Attenuated Phase Shift Extinction analyser (CAPS PMex) and a nephelometer respectively at 450 nm and (ii) the absorption coefficient from a MAAP (Multi-Angle Absorption Photometer) at 660 nm. Measurements were performed on seven dust aerosol samples generated in the laboratory by the mechanical shaking of natural parent soils issued from different source regions worldwide. The single scattering albedo (SSA) at 450 and 660 nm and the size distribution of the aerosols were also measured. Cref for mineral dust varies between 1.81 and 2.56 for a SSA of 0.85-0.96 at 450 nm and between 1.75 and 2.28 for a SSA of 0.98-0.99 at 660 nm. The calculated mean for dust is 2.09 (±0.22) at 450 nm and 1.92 (±0.17) at 660 nm. With this new Cref the dust absorption coefficient by the Aethalometer is about 2 % (450 nm) and 11 % (660 nm) higher than that obtained by using Cref = 2.14 at both 450 and 660 nm, as usually assumed in the literature. This difference induces a change of up to 3 % in the dust SSA at 660 nm. The Cref seems to be independent of the fine and coarse particle size fractions, and so the obtained Cref can be applied to dust both close to sources and following transport. Additional experiments performed with pure kaolinite minerals and polluted ambient aerosols indicate Cref of 2.49 (±0.02) and 2.32 (±0.01) at 450 and 660 nm (SSA = 0.96-0.97) for kaolinite, and Cref of 2.32 (±0.36) at 450 nm and 2.32 (±0.35) at 660 nm for pollution aerosols (SSA = 0.62-0.87 at 450 nm and 0.42-0.76 at 660 nm).

Comparison of experimental and modeled absorption enhancement by black carbon (BC) cored polydisperse aerosols under hygroscopic conditions.

PubMed

Shamjad, P M; Tripathi, S N; Aggarwal, S G; Mishra, S K; Joshi, Manish; Khan, Arshad; Sapra, B K; Ram, Kirpa

2012-08-07

The quantification of the radiative impacts of light absorbing ambient black carbon (BC) particles strongly depends on accurate measurements of BC mass concentration and absorption coefficient (β(abs)). In this study, an experiment has been conducted to quantify the influence of hygroscopic growth of ambient particles on light absorption. Using the hygroscopic growth factor (i.e., Zdanovskii-Stokes-Robinson (ZSR) approach), a model has been developed to predict the chemical composition of particles based on measurements, and the absorption and scattering coefficients are derived using a core-shell assumption with light extinction estimates based on Mie theory. The estimated optical properties agree within 7% for absorption coefficient and 30% for scattering coefficient with that of measured values. The enhancement of absorption is found to vary according to the thickness of the shell and BC mass, with a maximum of 2.3 for a shell thickness of 18 nm for the particles. The findings of this study underline the importance of considering aerosol-mixing states while calculating their radiative forcing.

Comparison of different Aethalometer correction schemes and a reference multi-wavelength absorption technique for ambient aerosol data

NASA Astrophysics Data System (ADS)

Saturno, Jorge; Pöhlker, Christopher; Massabò, Dario; Brito, Joel; Carbone, Samara; Cheng, Yafang; Chi, Xuguang; Ditas, Florian; Hrabě de Angelis, Isabella; Morán-Zuloaga, Daniel; Pöhlker, Mira L.; Rizzo, Luciana V.; Walter, David; Wang, Qiaoqiao; Artaxo, Paulo; Prati, Paolo; Andreae, Meinrat O.

2017-08-01

Deriving absorption coefficients from Aethalometer attenuation data requires different corrections to compensate for artifacts related to filter-loading effects, scattering by filter fibers, and scattering by aerosol particles. In this study, two different correction schemes were applied to seven-wavelength Aethalometer data, using multi-angle absorption photometer (MAAP) data as a reference absorption measurement at 637 nm. The compensation algorithms were compared to five-wavelength offline absorption measurements obtained with a multi-wavelength absorbance analyzer (MWAA), which serves as a multiple-wavelength reference measurement. The online measurements took place in the Amazon rainforest, from the wet-to-dry transition season to the dry season (June-September 2014). The mean absorption coefficient (at 637 nm) during this period was 1.8 ± 2.1 Mm-1, with a maximum of 15.9 Mm-1. Under these conditions, the filter-loading compensation was negligible. One of the correction schemes was found to artificially increase the short-wavelength absorption coefficients. It was found that accounting for the aerosol optical properties in the scattering compensation significantly affects the absorption Ångström exponent (åABS) retrievals. Proper Aethalometer data compensation schemes are crucial to retrieve the correct åABS, which is commonly implemented in brown carbon contribution calculations. Additionally, we found that the wavelength dependence of uncompensated Aethalometer attenuation data significantly correlates with the åABS retrieved from offline MWAA measurements.

Light extinction by Secondary Organic Aerosol: an intercomparison of three broadband cavity spectrometers

NASA Astrophysics Data System (ADS)

Varma, R. M.; Ball, S. M.; Brauers, T.; Dorn, H.-P.; Heitmann, U.; Jones, R. L.; Platt, U.; Pöhler, D.; Ruth, A. A.; Shillings, A. J. L.; Thieser, J.; Wahner, A.; Venables, D. S.

2013-07-01

Broadband optical cavity spectrometers are maturing as a technology for trace gas detection, but only recently have they been used to retrieve the extinction coefficient of aerosols. Sensitive broadband extinction measurements allow explicit separation of gas and particle phase spectral contributions, as well as continuous spectral measurements of aerosol extinction in favourable cases. In this work, we report an intercomparison study of the aerosol extinction coefficients measured by three such instruments: a broadband cavity ring-down spectrometer (BBCRDS), a cavity-enhanced differential optical absorption spectrometer (CE-DOAS), and an incoherent broadband cavity-enhanced absorption spectrometer (IBBCEAS). Experiments were carried out in the SAPHIR atmospheric simulation chamber as part of the NO3Comp campaign to compare the measurement capabilities of NO3 and N2O5 instrumentation. Aerosol extinction coefficients between 655 and 690 nm are reported for secondary organic aerosols (SOA) formed by the NO3 oxidation of β-pinene under dry and humid conditions. Despite different measurement approaches and spectral analysis procedures, the three instruments retrieved aerosol extinction coefficients that were in close agreement. The refractive index of SOA formed from the β-pinene + NO3 reaction was 1.61, and was not measurably affected by the chamber humidity or by aging of the aerosol over several hours. This refractive index is significantly larger than SOA refractive indices observed in other studies of OH and ozone-initiated terpene oxidations, and may be caused by the large proportion of organic nitrates in the particle phase. In an experiment involving ammonium sulphate particles the aerosol extinction coefficients as measured by IBBCEAS were found to be in reasonable agreement with those calculated using Mie theory. The results of the study demonstrate the potential of broadband cavity spectrometers for determining the optical properties of aerosols.

Light extinction by secondary organic aerosol: an intercomparison of three broadband cavity spectrometers

NASA Astrophysics Data System (ADS)

Varma, R. M.; Ball, S. M.; Brauers, T.; Dorn, H.-P.; Heitmann, U.; Jones, R. L.; Platt, U.; Pöhler, D.; Ruth, A. A.; Shillings, A. J. L.; Thieser, J.; Wahner, A.; Venables, D. S.

2013-11-01

Broadband optical cavity spectrometers are maturing as a technology for trace-gas detection, but only recently have they been used to retrieve the extinction coefficient of aerosols. Sensitive broadband extinction measurements allow explicit separation of gas and particle phase spectral contributions, as well as continuous spectral measurements of aerosol extinction in favourable cases. In this work, we report an intercomparison study of the aerosol extinction coefficients measured by three such instruments: a broadband cavity ring-down spectrometer (BBCRDS), a cavity-enhanced differential optical absorption spectrometer (CE-DOAS), and an incoherent broadband cavity-enhanced absorption spectrometer (IBBCEAS). Experiments were carried out in the SAPHIR atmospheric simulation chamber as part of the NO3Comp campaign to compare the measurement capabilities of NO3 and N2O5 instrumentation. Aerosol extinction coefficients between 655 and 690 nm are reported for secondary organic aerosols (SOA) formed by the NO3 oxidation of β-pinene under dry and humid conditions. Despite different measurement approaches and spectral analysis procedures, the three instruments retrieved aerosol extinction coefficients that were in close agreement. The refractive index of SOA formed from the β-pinene + NO3 reaction was 1.61, and was not measurably affected by the chamber humidity or by aging of the aerosol over several hours. This refractive index is significantly larger than SOA refractive indices observed in other studies of OH and ozone-initiated terpene oxidations, and may be caused by the large proportion of organic nitrates in the particle phase. In an experiment involving ammonium sulfate particles, the aerosol extinction coefficients as measured by IBBCEAS were found to be in reasonable agreement with those calculated using the Mie theory. The results of the study demonstrate the potential of broadband cavity spectrometers for determining the optical properties of aerosols.

AIP1OGREN: Aerosol Observing Station Intensive Properties Value-Added Product

DOE Office of Scientific and Technical Information (OSTI.GOV)

Koontz, Annette; Flynn, Connor

The aip1ogren value-added product (VAP) computes several aerosol intensive properties. It requires as input calibrated, corrected, aerosol extensive properties (scattering and absorption coefficients, primarily) from the Aerosol Observing Station (AOS). Aerosol extensive properties depend on both the nature of the aerosol and the amount of the aerosol. We compute several properties as relationships between the various extensive properties. These intensive properties are independent of aerosol amount and instead relate to intrinsic properties of the aerosol itself. Along with the original extensive properties we report aerosol single-scattering albedo, hemispheric backscatter fraction, asymmetry parameter, and Ångström exponent for scattering and absorption withmore » one-minute averaging. An hourly averaged file is produced from the 1-minute files that includes all extensive and intensive properties as well as submicron scattering and submicron absorption fractions. Finally, in both the minutely and hourly files the aerosol radiative forcing efficiency is provided.« less

Aerosol absorption profiling from the synergy of lidar and sun-photometry: the ACTRIS-2 campaigns in Germany, Greece and Cyprus

NASA Astrophysics Data System (ADS)

Tsekeri, Alexandra; Amiridis, Vassilis; Lopatin, Anton; Marinou, Eleni; Giannakaki, Eleni; Pikridas, Michael; Sciare, Jean; Liakakou, Eleni; Gerasopoulos, Evangelos; Duesing, Sebastian; Corbin, Joel C.; Gysel, Martin; Bukowiecki, Nicolas; Baars, Holger; Engelmann, Ronny; Wehner, Birgit; Kottas, Michael; Mamali, Dimitra; Kokkalis, Panagiotis; Raptis, Panagiotis I.; Stavroulas, Iasonas; Keleshis, Christos; Müller, Detlef; Solomos, Stavros; Binietoglou, Ioannis; Mihalopoulos, Nikolaos; Papayannis, Alexandros; Stachlewska, Iwona S.; Igloffstein, Julia; Wandinger, Ulla; Ansmann, Albert; Dubovik, Oleg; Goloub, Philippe

2018-04-01

Aerosol absorption profiling is crucial for radiative transfer calculations and climate modelling. Here, we utilize the synergy of lidar with sun-photometer measurements to derive the absorption coefficient and single scattering albedo profiles during the ACTRIS-2 campaigns held in Germany, Greece and Cyprus. The remote sensing techniques are compared with in situ measurements in order to harmonize and validate the different methodologies and reduce the absorption profiling uncertainties.

Investigating cloud absorption effects: Global absorption properties of black carbon, tar balls, and soil dust in clouds and aerosols

NASA Astrophysics Data System (ADS)

Jacobson, Mark Z.

2012-03-01

This study examines modeled properties of black carbon (BC), tar ball (TB), and soil dust (SD) absorption within clouds and aerosols to understand better Cloud Absorption Effects I and II, which are defined as the effects on cloud heating of absorbing inclusions in hydrometeor particles and of absorbing aerosol particles interstitially between hydrometeor particles at their actual relative humidity (RH), respectively. The globally and annually averaged modeled 550 nm aerosol mass absorption coefficient (AMAC) of externally mixed BC was 6.72 (6.3-7.3) m2/g, within the laboratory range (6.3-8.7 m2/g). The global AMAC of internally mixed (IM) BC was 16.2 (13.9-18.2) m2/g, less than the measured maximum at 100% RH (23 m2/g). The resulting AMAC amplification factor due to internal mixing was 2.41 (2-2.9), with highest values in high RH regions. The global 650 nm hydrometeor mass absorption coefficient (HMAC) due to BC inclusions was 17.7 (10.6-19) m2/g, ˜9.3% higher than that of the IM-AMAC. The 650 nm HMACs of TBs and SD were half and 1/190th, respectively, that of BC. Modeled aerosol absorption optical depths were consistent with data. In column tests, BC inclusions in low and mid clouds (CAE I) gave column-integrated BC heating rates ˜200% and 235%, respectively, those of interstitial BC at the actual cloud RH (CAE II), which itself gave heating rates ˜120% and ˜130%, respectively, those of interstitial BC at the clear-sky RH. Globally, cloud optical depth increased then decreased with increasing aerosol optical depth, consistent with boomerang curves from satellite studies. Thus, CAEs, which are largely ignored, heat clouds significantly.

Vertical variability of aerosol single-scattering albedo and equivalent black carbon concentration based on in-situ and remote sensing techniques during the iAREA campaigns in Ny-Ålesund

NASA Astrophysics Data System (ADS)

Markowicz, K. M.; Ritter, C.; Lisok, J.; Makuch, P.; Stachlewska, I. S.; Cappelletti, D.; Mazzola, M.; Chilinski, M. T.

2017-09-01

This work presents a methodology for obtaining vertical profiles of aerosol single scattering properties based on a combination of different measurement techniques. The presented data were obtained under the iAREA (Impact of absorbing aerosols on radiative forcing in the European Arctic) campaigns conducted in Ny-Ålesund (Spitsbergen) during the spring seasons of 2015-2017. The retrieval uses in-situ observations of black carbon concentration and absorption coefficient measured by a micro-aethalometer AE-51 mounted onboard a tethered balloon, as well as remote sensing data obtained from sun photometer and lidar measurements. From a combination of the balloon-borne in-situ and the lidar data, we derived profiles of single scattering albedo (SSA) as well as absorption, extinction, and aerosol number concentration. Results have been obtained in an altitude range from about 400 m up to 1600 m a.s.l. and for cases with increased aerosol load during the Arctic haze seasons of 2015 and 2016. The main results consist of the observation of increasing values of equivalent black carbon (EBC) and absorption coefficient with altitude, and the opposite trend for aerosol concentration for particles larger than 0.3 μm. SSA was retrieved with the use of lidar Raman and Klett algorithms for both 532 and 880 nm wavelengths. In most profiles, SSA shows relatively high temporal and altitude variability. Vertical variability of SSA computed from both methods is consistent; however, some discrepancy is related to Raman retrieval uncertainty and absorption coefficient estimation from AE-51. Typically, very low EBC concentration in Ny-Ålesund leads to large error in the absorbing coefficient. However, SSA uncertainty for both Raman and Klett algorithms seems to be reasonable, e.g. SSA of 0.98 and 0.95 relate to an error of ±0.01 and ± 0.025, respectively.

Spatial and temporal variations of aerosols around Beijing in summer 2006: 2. Local and column aerosol optical properties

DOE Office of Scientific and Technical Information (OSTI.GOV)

Matsui, Hitoshi; Koike, Makoto; Kondo, Yutaka

Weather Research and Forecasting (WRF)-chem model calculations were conducted to study aerosol optical properties around Beijing, China, during the Campaign of Air Quality Research in Beijing and Surrounding Region 2006 (CAREBeijing-2006) period. In this paper, we interpret aerosol optical properties in terms of aerosol mass concentrations and their chemical compositions by linking model calculations with measurements. In general, model calculations reproduced observed features of spatial and temporal variations of various surface and column aerosol optical parameters in and around Beijing. Spatial and temporal variations of aerosol absorption, scattering, and extinction coefficient corresponded well to those of elemental carbon (primary aerosol),more » sulfate (secondary aerosol), and the total aerosol mass concentration, respectively. These results show that spatial and temporal variations of the absorption coefficient are controlled by local emissions (within 100 km around Beijing during the preceding 24 h), while those of the scattering coefficient are controlled by regional-scale emissions (within 500 km around Beijing during the preceding 3 days) under synoptic-scale meteorological conditions, as discussed in our previous study of aerosol mass concentration. Vertical profiles of aerosol extinction revealed that the contribution of secondary aerosols and their water uptake increased with altitude within the planetary boundary layer, leading to a considerable increase in column aerosol optical depth (AOD) around Beijing. These effects are the main factors causing differences in regional and temporal variations between particulate matter (PM) mass concentration at the surface and column AOD over a wide region in the northern part of the Great North China Plain.« less

Measurement of aerosol optical properties by integrating cavity ring-down spectroscopy and nephelometery

NASA Astrophysics Data System (ADS)

Tedela, Getachew; Singh, Sujeeta; Fiddler, Marc; Bililign, Solomon

2013-03-01

Accurate measurement of optical properties of aerosols is crucial for quantifying the influence of aerosols on climate. Aerosols that scatter and absorb radiation can have a cooling or warming effect depending on the magnitude of the respective scattering and absorption terms. One example is black carbon known for its strong absorption. The reported refractive indices for black carbon particles range from 1.2 +0i to 2.75 +1.44i. Our work attempts to measure extinction coefficient, and scattering coefficient of black carbon particles at different incident beam wavelengths using a cavity ring-down spectrometer and a Nephelometer and compare to Mie theory predictions. We report calibration results using polystyrene latex spheres and preliminary results on using commercial black carbon particles. The work is supported by the Department of Defense grant W911NF-11-1-0188.

Atmospheric effects on CO2 laser propagation

NASA Technical Reports Server (NTRS)

Murty, S. S. R.; Bilbro, J. W.

1978-01-01

An investigation was made of the losses encountered in the propagation of CO2 laser radiation through the atmosphere, particularly as it applies to the NASA/Marshall Space Flight Center Pulsed Laser Doppler System. As such it addresses three major areas associated with signal loss: molecular absorption, refractive index changes in a turbulent environment, and aerosol absorption and scattering. In particular, the molecular absorption coefficients of carbon dioxide, water vapor, and nitrous oxide are calculated for various laser lines in the region of 10.6 mu m as a function of various pressures and temperatures. The current status in the physics of low-energy laser propagation through a turbulent atmosphere is presented together with the analysis and evaluation of the associated heterodyne signal power loss. Finally, aerosol backscatter and extinction coefficients are calculated for various aerosol distributions and the results incorporated into the signal-to-noise ratio equation for the Marshall Space Flight Center system.

Assessing the measurement of aerosol single scattering albedo by Cavity Attenuated Phase-Shift Single Scattering Monitor (CAPS PMssa)

NASA Astrophysics Data System (ADS)

Perim de Faria, Julia; Bundke, Ulrich; Onasch, Timothy B.; Freedman, Andrew; Petzold, Andreas

2016-04-01

The necessity to quantify the direct impact of aerosol particles on climate forcing is already well known; assessing this impact requires continuous and systematic measurements of the aerosol optical properties. Two of the main parameters that need to be accurately measured are the aerosol optical depth and single scattering albedo (SSA, defined as the ratio of particulate scattering to extinction). The measurement of single scattering albedo commonly involves the measurement of two optical parameters, the scattering and the absorption coefficients. Although there are well established technologies to measure both of these parameters, the use of two separate instruments with different principles and uncertainties represents potential sources of significant errors and biases. Based on the recently developed cavity attenuated phase shift particle extinction monitor (CAPS PM_{ex) instrument, the CAPS PM_{ssa instrument combines the CAPS technology to measure particle extinction with an integrating sphere capable of simultaneously measuring the scattering coefficient of the same sample. The scattering channel is calibrated to the extinction channel, such that the accuracy of the single scattering albedo measurement is only a function of the accuracy of the extinction measurement and the nephelometer truncation losses. This gives the instrument an accurate and direct measurement of the single scattering albedo. In this study, we assess the measurements of both the extinction and scattering channels of the CAPS PM_{ssa through intercomparisons with Mie theory, as a fundamental comparison, and with proven technologies, such as integrating nephelometers and filter-based absorption monitors. For comparison, we use two nephelometers, a TSI 3563 and an Aurora 4000, and two measurements of the absorption coefficient, using a Particulate Soot Absorption Photometer (PSAP) and a Multi Angle Absorption Photometer (MAAP). We also assess the indirect absorption coefficient measurement from the CAPS PM_{ssa (calculated as the difference from the measured extinction and scattering). The study was carried out in the laboratory with controlled particle generation systems. We used both light absorbing aerosols (Regal 400R pigment black from Cabot Corp. and colloidal graphite - Aquadag - from Agar Scientific) and purely scattering aerosols (ammonium sulphate and polystyrene latex spheres), covering single scattering albedo values from approximately 0.4 to 1.0. A new truncation angle correction for the CAPS PM_{ssa integrated sphere is proposed.

Modeling visibility in the Paso del Norte (PDN) Region

NASA Astrophysics Data System (ADS)

Medina Calderon, Richard

Poor visibility is a subject of growing public concern throughout the U.S, and an active area of research. Its societal impacts on air quality, aviation transport and traffic are significant. Aerosols play a fundamental role in the attenuation of solar radiation, and also affect visibility. The scattering and extinction coefficients of aerosol particles in the Paso del Norte Region have been calculated using the T- matrix model in conjunction with a laser particle counter. Inter-comparison of the model's results of the scattering and absorption coefficients against the corresponding data from a Photoacustic extinctiometer instrument (which measures in-situ absorption and scattering coefficients of aerosol particles) shows excellent agreement. In addition, the volume-weighted method is used to determine the composite index of refraction which is representative of the aerosols for the Paso del Norte Region to obtain information of the type of aerosol particles present in the Region. The Single Scattering Albedo has also been retrieved using this methodology to obtain further insight into the type of aerosols present on a given day. Finally, the Koschmieder equation has been used to calculate the visual range or visibility, and was correlated with the PM2.5 and PM10 particle concentration present in the Region. Our methodology will allow a better understanding of the size and type of aerosol particles that are most detrimental to the visibility for the Paso Del Norte Region.

Variability in aerosol optical properties over an urban site, Kanpur, in the Indo-Gangetic Plain: A case study of haze and dust events

NASA Astrophysics Data System (ADS)

Ram, Kirpa; Singh, Sunita; Sarin, M. M.; Srivastava, A. K.; Tripathi, S. N.

2016-06-01

In this study, we report on three important optical parameters, viz. absorption and scattering coefficients (babs, bscat) and single scattering abledo (SSA) based on one-year chemical-composition data collected from an urban site (Kanpur) in the Indo-Gangetic-Plain (IGP) of northern India. In addition, absorption Ängstrom exponent (AAE) was also estimated in order to understand the wavelength dependence of absorption and to decipher emission sources of carbonaceous aerosols, in particular of black carbon. The absorption and scattering coefficients ranged between 8.3 to 95.2 Mm- 1 (1 Mm- 1 = 10- 6 m- 1) and 58 to 564 Mm- 1, respectively during the study period (for n = 66; from January 2007 to March 2008) and exhibit large seasonal variability with higher values occurring in winter and lower in the summer. Single scattering albedo varied from 0.65 to 0.92 whereas AAE ranged from 0.79 to 1.40 during pre-monsoon and winter seasons, respectively. The strong seasonal variability in aerosol optical properties is attributed to varying contribution from different emission sources of carbonaceous aerosols in the IGP. A case study of haze and dust events further provide information on extreme variability in aerosol optical parameters, particularly SSA, a crucial parameter in atmospheric radiative forcing estimates.

Evolution of wavelength-dependent mass absorption cross sections of carbonaceous aerosols during the 2010 DOE CARES campaign

NASA Astrophysics Data System (ADS)

Flowers, B. A.; Dubey, M. K.; Subramanian, R.; Sedlacek, A. J.; Kelley, P.; Luke, W. T.; Jobson, B. T.; Zaveri, R. A.

2011-12-01

Predictions of aerosol radiative forcing require process level optical property models that are built on precise and accurate field observations. Evolution of aerosol optical properties for urban influenced carbonaceous aerosol undergoing transport and mixing with rural air masses was a focal point of the DOE Carbonaceous Aerosol and Radiative Effects (CARES) campaign near Sacramento, CA in summer 2010. Urban aerosol was transported from Sacramento, CA (T0) to the foothills of the Sierra Nevada Mountains to a rural site located near Cool, CA (T1). Aerosol absorption and scattering coefficients were measured at the T0 and T1 sites using integrated photoacoustic acoustic/nephelometer instruments (PASS-3 and PASS-UV) at 781, 532, 405, and 375 nm. Single particle soot photometry (SP2) instrumentation was used to monitor black carbon (BC) mass at both sites. Combining data from these sensors allows estimate of the wavelength-dependent mass absorption coefficient (MAC(λ)) and partitioning of MAC(λ) into contributions from the BC core and from enhancements from coating of BC cores. MAC(λ) measured in this way is free of artifacts associated with filter-based aerosol absorption measurements and takes advantage of the single particle sensitivity of the SP2 instrument, allowing observation of MAC(λ) on 10 minute and faster time scales. Coating was observed to enhance MAC(λ) by 20 - 30 % and different wavelength dependence for MAC(λ) was observed for urban and biomass burning aerosol. Further, T0 - T1 evolution of MAC(λ) was correlated with separately measured NO/NOy ratios and CO/CO2 ratios to understand the effects of aging & transport on MAC(λ) and the implications of aerosol processing that links air quality to radiative forcing on a regional scale. Aircraft observations made from the Gulfstream-1 during CARES are also analyzed to enhance process level understanding of the optical properties of fresh and aged carbonaceous aerosol in the urban-rural interface.

Estimation of black carbon content for biomass burning aerosols from multi-channel Raman lidar data

NASA Astrophysics Data System (ADS)

Talianu, Camelia; Marmureanu, Luminita; Nicolae, Doina

2015-04-01

Biomass burning due to natural processes (forest fires) or anthropical activities (agriculture, thermal power stations, domestic heating) is an important source of aerosols with a high content of carbon components (black carbon and organic carbon). Multi-channel Raman lidars provide information on the spectral dependence of the backscatter and extinction coefficients, embedding information on the black carbon content. Aerosols with a high content of black carbon have large extinction coefficients and small backscatter coefficients (strong absorption), while aerosols with high content of organic carbon have large backscatter coefficients (weak absorption). This paper presents a method based on radiative calculations to estimate the black carbon content of biomass burning aerosols from 3b+2a+1d lidar signals. Data is collected at Magurele, Romania, at the cross-road of air masses coming from Ukraine, Russia and Greece, where burning events are frequent during both cold and hot seasons. Aerosols are transported in the free troposphere, generally in the 2-4 km altitude range, and reaches the lidar location after 2-3 days. Optical data are collected between 2011-2012 by a multi-channel Raman lidar and follows the quality assurance program of EARLINET. Radiative calculations are made with libRadTran, an open source radiative model developed by ESA. Validation of the retrievals is made by comparison to a co-located C-ToF Aerosol Mass Spectrometer. Keywords: Lidar, aerosols, biomass burning, radiative model, black carbon Acknowledgment: This work has been supported by grants of the Romanian National Authority for Scientific Research, Programme for Research- Space Technology and Advanced Research - STAR, project no. 39/2012 - SIAFIM, and by Romanian Partnerships in priority areas PNII implemented with MEN-UEFISCDI support, project no. 309/2014 - MOBBE

Chemical, optical and radiative characteristics of aerosols during haze episodes of winter in the North China Plain

NASA Astrophysics Data System (ADS)

Ding, Jing; Zhang, Yufen; Han, Suqin; Xiao, Zhimei; Wang, Jiao; Feng, Yinchang

2018-05-01

Aerosol and water vapor radiative forcings, shortwave atmospheric heating rates and longwave atmospheric cooling rates were determined based on in situ physical and chemical measurements of aerosol, associated with the Mie theory and a radiative transfer model, LOWTRAN7, during the two haze episodes in the winter of 2013 in Tianjin, China. The aerosol types considered in LOWTRAN7 included rural, urban, marine, desert and custom aerosols. The default ratio of the absorption coefficient to the extinction coefficient for urban aerosol in LOWTRAN7 was approximately double of those found in this work, implying the weaker absorption ability of aerosols in the North China Plain (NCP). Moreover, the aerosol is assumed to be evenly distributed below 1 km of planetary boundary layer (PBL) on hazy days in LOWTRAN7. If the default urban aerosol optical properties and extinction profile in LOWTRAN7 is employed directly, a larger energy imbalance between the atmosphere and surface is generated and the warming effect of the aerosol is magnified. Hence, modified urban aerosol optical properties were established to replace the corresponding parameters' database in LOWTRAN7. The aerosol extinction profiles were obtained based on a 255-m meteorological tower and observed results from the studies about Tianjin. In the NCP, the aerosol had little impact on atmospheric counter radiation. The water vapor is the crucial factor that affects atmospheric counter radiation. Both modified high shortwave heating rates and longwave cooling rates occur near the surface due to the abundance of aerosol and water vapor. The modified net atmospheric heating rate near the surface is 1.2 K d-1 on hazy days and 0.3 K d-1 on non-hazy days. Compared with the default urban aerosol optical properties and its vertical distribution in LOWTRAN7, the feedback effect of the modified urban aerosol on the boundary layer may not necessarily result in a stable lower atmosphere, but depends on the aerosol light absorption ability and its vertical distribution.

Scattering and Absorption of E&M radiation by small particles-applications to study impact of biomass aerosols on climate

NASA Astrophysics Data System (ADS)

Bililign, Solomon; Singh, Sujeeta; Fiddler, Marc; Smith, Damon

2015-03-01

The phenomena of scattering, absorption, and emission of light and other electromagnetic radiation by small particles are central to many science and engineering disciplines. Absorption of solar radiation by black carbon aerosols has a significant impact on the atmospheric energy distribution and hydrologic processes. By intercepting incoming solar radiation before it reaches the surface, aerosols heat the atmosphere and, in turn, cool the surface. The magnitude of the atmospheric forcing induced by anthropogenic absorbing aerosols, mainly black carbon (BC) emitted from biomass burning and combustion processes has been suggested to be comparable to the atmospheric forcing by all greenhouse gases (GHGs). Despite the global abundance of biomass burning for cooking, forests clearing for agriculture and wild fires, the optical properties of these aerosols have not been characterized at wide range of wavelengths. Our laboratory uses a combination of Cavity ring down spectroscopy and integrating nephelometry to measure optical properties of (extinction, absorption and scattering coefficients) of biomass aerosols. Preliminary results will be presented. Supported by the Department of Defense under Grant #W911NF-11-1-0188.

Measurement of wavelength-dependent extinction to distinguish between absorbing and nonabsorbing aerosol particulates

NASA Technical Reports Server (NTRS)

Portscht, R.

1977-01-01

Measurements of spectral transmission factors in smoky optical transmission paths reveal a difference between wavelength exponents of the extinction cross section of high absorption capacity and those of low absorption capacity. A theoretical explanation of this behavior is presented. In certain cases, it is possible to obtain data on the absorption index of aerosol particles in the optical path by measuring the spectral decadic extinction coefficient at, at least, two wavelengths. In this manner it is possible, for instance, to distinguish smoke containing soot from water vapor.

Steady increase of secondary organic aerosol mass concentration and light extinction during the CARES 2010 Field Campaign

NASA Astrophysics Data System (ADS)

Gyawali, M. S.; Arnott, W. P.; Flowers, B. A.; Dubey, M. K.; Atkinson, D. B.; Song, C.; Zaveri, R. A.; Setyan, A.; Zhang, Q.; Mazzoleni, C.; Gorkowski, K.

2011-12-01

We present multispectral (355, 375, 405, 532, 870, 781, and 1047 nm) aerosol light absorption and scattering measurements for the 2010 Carbonaceous Aerosols and Radiative Effects (CARES) campaign in Sacramento, CA and the Sierra Nevada foothills. The short wavelength scattering at both sites gradually increased during the last 10 days of the campaign as diagnosed by a systematic increase in the Ångström exponent of scattering. The UV and near UV enhanced scattering was likely a consequence of the ultra and sub-micron aerosol which began to grow vigorously in the size range where scattering at shorter wavelengths begins to increase. Multispectral aerosol light absorption coefficients suggest the absence of short wavelength light absorption by brown carbon. Aerosol mass spectrometer data also shows the steady increase of secondary organic aerosol during the last 10 days of CARES. The time series of the measurements made between the two sites (T0 and T1) separated by the slope of the foothills are strikingly similar, except for isolated night time episodes of enhanced absorption at T0. This is possibly due to paving events or other nocturnal emissions markers

Aerosol Angstrom Absorption Coefficient Comparisons during MILAGRO.

NASA Astrophysics Data System (ADS)

Marley, N. A.; Marchany-Rivera, A.; Kelley, K. L.; Mangu, A.; Gaffney, J. S.

2007-12-01

Measurements of aerosol absorption were obtained as part of the MAX-Mex component of the MILAGRO field campaign at site T0 (Instituto Mexicano de Petroleo in Mexico City) by using a 7-channel aethalometer (Thermo- Anderson) during the month of March, 2006. The absorption measurements obtained in the field at 370, 470, 520, 590, 660, 880, and 950 nm were used to determine the aerosol Angstrom absorption exponents by linear regression. Since, unlike other absorbing aerosol species (e.g. humic like substances, nitrated PAHs), black carbon absorption is relatively constant from the ultraviolet to the infrared with an Angstrom absorption exponent of -1 (1), a comparison of the Angstrom exponents can indicate the presence of aerosol components with an enhanced UV absorption over that expected from BC content alone. The Angstrom exponents determined from the aerosol absorption measurements obtained in the field varied from - 0.7 to - 1.3 during the study and was generally lower in the afternoon than the morning hours, indicating an increase in secondary aerosol formation and photochemically generated UV absorbing species in the afternoon. Twelve-hour integrated samples of fine atmospheric aerosols (<0.1micron) were also collected at site T0 and T1 (Universidad Technologica de Tecamac, State of Mexico) from 5 am to 5 pm (day) and from 5 pm to 5 am (night) during the month of March 2006. Samples were collected on quartz fiber filters with high volume impactor samplers. Continuous absorption spectra of these aerosol samples have been obtained in the laboratory from 280 to 900nm with the use of an integrating sphere coupled to a UV spectrometer (Beckman DU with a Labsphere accessory). The integrating sphere allows the detector to collect and spatially integrate the total radiant flux reflected from the sample and therefore allows for the measurement of absorption on highly reflective or diffusely scattering samples. These continuous spectra have also been used to obtain the aerosol Angstrom absorption exponents by linear regression over the entire UV-visible spectral range. These results are compared to results obtained from the absorbance measurements obtained in the field. The differences in calculated Angstrom absorption exponents between the field and laboratory measurements are attributed partly to the differences in time resolution of the sample collection resulting in heavier particle pileup on the filter surface of the 12-hour samples. Some differences in calculated results can also be attributed to the presence of narrow band absorbers below 400 nm that do not fall in the wavelengths covered by the 7 wavelengths of the aethalometer. 1. Marley, N.A., J.S. Gaffney, J.C. Baird, C.A. Blazer, P.J. Drayton, and J.E. Frederick, "The determination of scattering and absorption coefficients of size-fractionated aerosols for radiative transfer calculations." Aerosol Sci. Technol., 34, 535-549, (2001). This work was conducted as part of the Department of Energy's Atmospheric Science Program as part of the Megacity Aerosol Experiment - Mexico City during MILAGRO. This research was supported by the Office of Science (BER), U.S. Department of Energy Grant No. DE-FG02-07ER64329. We also wish to thank Mexican Scientists and students for their assistance from the Instituto Mexicano de Petroleo (IMP) and CENICA.

The Ascension Island Boundary Layer in the Remote Southeast Atlantic is Often Smoky

NASA Astrophysics Data System (ADS)

Zuidema, Paquita; Sedlacek, Arthur J.; Flynn, Connor; Springston, Stephen; Delgadillo, Rodrigo; Zhang, Jianhao; Aiken, Allison C.; Koontz, Annette; Muradyan, Paytsar

2018-05-01

Observations from June to October 2016, from a surface-based ARM Mobile Facility deployment on Ascension Island (8°S, 14.5°W) indicate that refractory black carbon (rBC) is almost always present within the boundary layer. The rBC mass concentrations, light absorption coefficients, and cloud condensation nuclei concentrations vary in concert and synoptically, peaking in August. Light absorption coefficients at three visible wavelengths as a function of rBC mass are approximately double that calculated from black carbon in lab studies. A spectrally-flat absorption angstrom exponent suggests most of the light absorption is from lens-coated black carbon. The single-scattering-albedo increases systematically from August to October in both 2016 and 2017, with monthly means of 0.78 ± 0.02 (August), 0.81 ± 0.03 (September), and 0.83 ± 0.03 (October) at the green wavelength. Boundary layer aerosol loadings are only loosely correlated with total aerosol optical depth, with smoke more likely to be present in the boundary layer earlier in the biomass burning season, evolving to smoke predominantly present above the cloud layers in September-October, typically resting upon the cloud top inversion. The time period with the campaign-maximum near-surface light absorption and column aerosol optical depth, on 13-16 August 2016, is investigated further. Backtrajectories that indicate more direct boundary layer transport westward from the African continent is central to explaining the elevated surface aerosol loadings.

The Measurement of Aerosol Optical Properties using Continuous Wave Cavity Ring-Down Techniques

NASA Technical Reports Server (NTRS)

Strawa, Anthony W.; Castaneda, Rene; Owano, Thomas; Baer, Douglas S.; Paldus, Barbara A.; Gore, Warren J. (Technical Monitor)

2002-01-01

Large uncertainties in the effects that aerosols have on climate require improved in situ measurements of extinction coefficient and single-scattering albedo. This paper describes the use of continuous wave cavity ring-down (CW-CRD) technology to address this problem. The innovations in this instrument are the use of CW-CRD to measure aerosol extinction coefficient, the simultaneous measurement of scattering coefficient, and small size suitable for a wide range of aircraft applications. Our prototype instrument measures extinction and scattering coefficient at 690 nm and extinction coefficient at 1550 nm. The instrument itself is small (60 x 48 x 15 cm) and relatively insensitive to vibrations. The prototype instrument has been tested in our lab and used in the field. While improvements in performance are needed, the prototype has been shown to make accurate and sensitive measurements of extinction and scattering coefficients. Combining these two parameters, one can obtain the single-scattering albedo and absorption coefficient, both important aerosol properties. The use of two wavelengths also allows us to obtain a quantitative idea of the size of the aerosol through the Angstrom exponent. Minimum sensitivity of the prototype instrument is 1.5 x 10(exp -6)/m (1.5 M/m). Validation of the measurement of extinction coefficient has been accomplished by comparing the measurement of calibration spheres with Mie calculations. This instrument and its successors have potential to help reduce uncertainty currently associated with aerosol optical properties and their spatial and temporal variation. Possible applications include studies of visibility, climate forcing by aerosol, and the validation of aerosol retrieval schemes from satellite data.

The Measurement of Aerosol Optical Properties Using Continuous Wave Cavity Ring-Down Techniques

NASA Technical Reports Server (NTRS)

Strawa, A. W.; Owano, T.; Castaneda, R.; Baer, D. S.; Paldus, B. A.; Gore, Warren J. (Technical Monitor)

2002-01-01

Large uncertainties in the effects that aerosols have on climate require improved in-situ measurements of extinction coefficient and single-scattering albedo. This abstract describes the use of continuous wave cavity ring-down (CW-CRD) technology to address this problem. The innovations in this instrument are the use of CW-CRD to measure aerosol extinction coefficient, the simultaneous measurement of scattering coefficient, and small size suitable for a wide range of aircraft applications. Our prototype instrument measures extinction and scattering coefficient at 690 nm and extinction coefficient at 1550 nm. The instrument itself is small (60 x 48 x 15 cm) and relatively insensitive to vibrations. The prototype instrument has been tested in our lab and used in the field. While improvements in performance are needed, the prototype has been shown to make accurate and sensitive measurements of extinction and scattering coefficients. Combining these two parameters, one can obtain the single-scattering albedo and absorption coefficient, both important aerosol properties. The use of two wavelengths also allows us to obtain a quantitative idea of the size of the aerosol through the Angstrom exponent. Minimum sensitivity of the prototype instrument is 1.5 x 10(exp -6)/m (1.5/Mm). Validation of the measurement of extinction coefficient has been accomplished by comparing the measurement of calibration spheres with Mie calculations. This instrument and its successors have potential to help reduce uncertainty currently associated with aerosol optical properties and their spatial and temporal variation. Possible applications include studies of visibility, climate forcing by aerosol, and the validation of aerosol retrieval schemes from satellite data.

A new approach to correct for absorbing aerosols in OMI UV

NASA Astrophysics Data System (ADS)

Arola, A.; Kazadzis, S.; Lindfors, A.; Krotkov, N.; Kujanpää, J.; Tamminen, J.; Bais, A.; di Sarra, A.; Villaplana, J. M.; Brogniez, C.; Siani, A. M.; Janouch, M.; Weihs, P.; Webb, A.; Koskela, T.; Kouremeti, N.; Meloni, D.; Buchard, V.; Auriol, F.; Ialongo, I.; Staneck, M.; Simic, S.; Smedley, A.; Kinne, S.

2009-11-01

Several validation studies of surface UV irradiance based on the Ozone Monitoring Instrument (OMI) satellite data have shown a high correlation with ground-based measurements but a positive bias in many locations. The main part of the bias can be attributed to the boundary layer aerosol absorption that is not accounted for in the current satellite UV algorithms. To correct for this shortfall, a post-correction procedure was applied, based on global climatological fields of aerosol absorption optical depth. These fields were obtained by using global aerosol optical depth and aerosol single scattering albedo data assembled by combining global aerosol model data and ground-based aerosol measurements from AERONET. The resulting improvements in the satellite-based surface UV irradiance were evaluated by comparing satellite and ground-based spectral irradiances at various European UV monitoring sites. The results generally showed a significantly reduced bias by 5-20%, a lower variability, and an unchanged, high correlation coefficient.

In situ aerosol optics in Reno, NV, USA during and after the summer 2008 California wildfires and the influence of absorbing and non-absorbing organic coatings on spectral light absorption

NASA Astrophysics Data System (ADS)

Gyawali, M.; Arnott, W. P.; Lewis, K.; Moosmüller, H.

2009-10-01

Hundreds of wildfires in Northern California were sparked by lightning during the summer of 2008, resulting in downwind smoke for the months of June and July. Comparisons are reported for aerosol optics measurements in Reno, Nevada made during the very smoky month of July and the relatively clean month of August. Photoacoustic instruments equipped with integrating nephelometers were used to measure aerosol light scattering and absorption coefficients at wavelengths of 405 nm and 870 nm, revealing a strong variation of aerosol light absorption with wavelength. Insight on fuels burned is gleaned from comparison of Ångström exponents of absorption (AEA) versus single scattering albedo (SSA) of the ambient measurements with laboratory biomass smoke measurements for many fuels. Measurements during the month of August, which were largely unaffected by fire smoke, exhibit surprisingly low AEA for aerosol light absorption when the SSA is highest, again likely as a consequence of the underappreciated wavelength dependence of aerosol light absorption by particles coated with non-absorbing organic and inorganic matter. Coated sphere calculations were used to show that AEA as large as 1.6 are possible for wood smoke even with non-absorbing organic coatings on black carbon cores, suggesting care be exercised when diagnosing AEA.

Optical, physical, and chemical properties of springtime aerosol over Barrow Alaska in 2008

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shantz, Nicole C.; Gultepe, Ismail; Andrews, Elisabeth

2014-03-06

Airborne observations from four flights during the 2008 Indirect and Semi-Direct Aerosol Campaign (ISDAC) are used to examine some cloud-free optical, physical, and chemical properties of aerosol particles in the springtime Arctic troposphere. The number concentrations of particles larger than 0.12 μm (Na>120), important for light extinction and cloud droplet formation, ranged from 15 to 2260 cm -3, with the higher Na>120 cases dominated by measurements from two flights of long-range transported biomass burning (BB) aerosols. The two other flights examined here document a relatively clean aerosol and an Arctic Haze aerosol impacted by larger particles largely composed of dust.more » For observations from the cleaner case and the BB cases, the particle light scattering coefficients at low relative humidity (RH<20%) increased nonlinearly with increasing Na>120, driven mostly by an increase in mean sizes of particles with increasing Na>120 (BB cases). For those three cases, particle light absorption coefficients also increased nonlinearly with increasing Na>120 and linearly with increasing submicron particle volume concentration. In addition to black carbon, brown carbon was estimated to have increased light absorption coefficients by 27% (450 nm wavelength) and 14% (550 nm) in the BB cases. For the case with strong dust influence, the absorption relative to submicron particle volume was small compared with the other cases. There was a slight gradient of Passive Cavity Aerosol Spectrometer Probe (PCASP) mean volume diameter (MVD) towards smaller sizes with increasing height, which suggests more scavenging of the more elevated particles, consistent with a typically longer lifetime of particles higher in the atmosphere. However, in approximately 10% of the cases, the MVD increased (>0.4 μm) with increasing altitude, suggesting transport of larger fine particle mass (possibly coarse particle mass) at high levels over the Arctic. This may be because of transport of larger particles at higher elevations and relatively slow deposition to the surface.« less

Evolution of Multispectral Aerosol Absorption Properties in a Biogenically-Influenced Urban Environment during the CARES Campaign

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gyawali, Madhu; Arnott, W.; Zaveri, Rahul

We present the evolution of multispectral optical properties as urban aerosols aged and interacted with biogenic emissions resulting in stronger short wavelength absorption and formation of moderately brown secondary organic aerosols. Ground-based aerosol measurements were made during June 2010 within the Sacramento urban area (site T0) and at a 40-km downwind location (site T1) in the forested Sierra Nevada foothills area. Data on black carbon and non-refractory aerosol mass and composition were collected at both sites. In addition, photoacoustic (PA) instruments with integrating nephelometers were used to measure spectral absorption and scattering coefficients for wavelengths ranging from 355 to 870more » nm. The daytime absorption Ångström exponent (AAE) indicated a modest wavelength-dependent enhancement of absorption at both sites throughout the study. From the 22nd to the 28th of June, secondary organic aerosol mass increased significantly at both sites due to increased biogenic emissions coupled with intense photochemical activity and air mass recirculation in the area. During this period, the median BC mass-normalized absorption cross-section (MAC) values for 405 nm and 532 nm at T1 increased by ~23% and ~35%, respectively, compared to the relatively less aged urban emissions at the T0 site. In contrast, the average MAC values for the 870 nm wavelength were similar for both sites. These results suggest formation of moderately brown secondary organic aerosols in biogenically-influenced urban air.« less

Evolution of Multispectral Aerosol Absorption Properties in a Biogenically-Influenced Urban Environment during the CARES Campaign

DOE PAGES

Gyawali, Madhu; Arnott, W.; Zaveri, Rahul; ...

2017-11-13

We present the evolution of multispectral optical properties through urban aerosols that have aged and interacted with biogenic emissions, resulting in stronger short wavelength absorption and the formation of moderately brown secondary organic aerosols. Ground-based aerosol measurements were made in June 2010 within the Sacramento urban area (site T0) and at a 40-km downwind location (site T1) in the forested Sierra Nevada foothills area. Data on black carbon (BC) and non-refractory aerosol mass and composition were collected at both sites. In addition, photoacoustic (PA) instruments with integrating nephelometers were used to measure spectral absorption and scattering coefficients for wavelengths rangingmore » from 355 to 870 nm. The daytime absorption Ångström exponent (AAE) indicated a modest wavelength-dependent enhancement of absorption at both sites throughout the study. From 22 to 28 June 2010, secondary organic aerosol mass increased significantly at both sites, which was due to increased biogenic emissions coupled with intense photochemical activity and air mass recirculation in the area. During this period, the median BC mass-normalized absorption cross-section (MAC) values for 405 nm and 532 nm at T1 increased by ~23% and ~35%, respectively, compared with the relatively less aged urban emissions at the T0 site. In contrast, the average MAC values for the 870 nm wavelength were similar for both sites. These results suggest the formation of moderately brown secondary organic aerosols in biogenically-influenced urban air.« less

Evolution of Multispectral Aerosol Absorption Properties in a Biogenically-Influenced Urban Environment during the CARES Campaign

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gyawali, Madhu; Arnott, W.; Zaveri, Rahul

We present the evolution of multispectral optical properties through urban aerosols that have aged and interacted with biogenic emissions, resulting in stronger short wavelength absorption and the formation of moderately brown secondary organic aerosols. Ground-based aerosol measurements were made in June 2010 within the Sacramento urban area (site T0) and at a 40-km downwind location (site T1) in the forested Sierra Nevada foothills area. Data on black carbon (BC) and non-refractory aerosol mass and composition were collected at both sites. In addition, photoacoustic (PA) instruments with integrating nephelometers were used to measure spectral absorption and scattering coefficients for wavelengths rangingmore » from 355 to 870 nm. The daytime absorption Ångström exponent (AAE) indicated a modest wavelength-dependent enhancement of absorption at both sites throughout the study. From 22 to 28 June 2010, secondary organic aerosol mass increased significantly at both sites, which was due to increased biogenic emissions coupled with intense photochemical activity and air mass recirculation in the area. During this period, the median BC mass-normalized absorption cross-section (MAC) values for 405 nm and 532 nm at T1 increased by ~23% and ~35%, respectively, compared with the relatively less aged urban emissions at the T0 site. In contrast, the average MAC values for the 870 nm wavelength were similar for both sites. These results suggest the formation of moderately brown secondary organic aerosols in biogenically-influenced urban air.« less

The Ascension Island boundary layer in the remote southeast Atlantic is often smoky

DOE PAGES

Zuidema, Paquita; Sedlacek III, Arthur J.; Flynn, Connor; ...

2018-03-31

Observations from June through October, 2016, from a surface-based ARM Mobile Facility deployment on Ascension Island (8°S, 14.5°W) indicate that refractory black carbon (rBC) is almost always present within the boundary layer. rBC mass concentrations, light absorption coefficients, and cloud condensation nuclei concentrations vary in concert and synoptically, peaking in August. Light absorption coefficients at three visible wavelengths as a function of rBC mass indirectly indicate the presence of other light-absorbing aerosols (e.g., brown carbon), most pronounced in June. The single-scattering-albedo increases systematically from August to October in both 2016 and 2017, with monthly-means of 0.78±0.02 (August), 0.81±0.03 (September) andmore » 0.83±0.03 (October) at the green wavelength. Boundary-layer aerosol loadings are only loosely correlated with total aerosol optical depth, with smoke more likely to be present in the boundary layer earlier in the biomass-burning season, evolving to smoke predominantly present above the cloud layers in September-October, typically resting upon the cloud-top inversion. The time period with the campaign-maximum near-surface light absorption and column aerosol optical depth, on 13-16 August of 2016, is investigated further. Also, backtrajectories indicate more direct boundary layer transport westward from the African continent is central to explaining the elevated surface aerosol loadings.« less

The Ascension Island boundary layer in the remote southeast Atlantic is often smoky

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zuidema, Paquita; Sedlacek III, Arthur J.; Flynn, Connor

Observations from June through October, 2016, from a surface-based ARM Mobile Facility deployment on Ascension Island (8°S, 14.5°W) indicate that refractory black carbon (rBC) is almost always present within the boundary layer. rBC mass concentrations, light absorption coefficients, and cloud condensation nuclei concentrations vary in concert and synoptically, peaking in August. Light absorption coefficients at three visible wavelengths as a function of rBC mass indirectly indicate the presence of other light-absorbing aerosols (e.g., brown carbon), most pronounced in June. The single-scattering-albedo increases systematically from August to October in both 2016 and 2017, with monthly-means of 0.78±0.02 (August), 0.81±0.03 (September) andmore » 0.83±0.03 (October) at the green wavelength. Boundary-layer aerosol loadings are only loosely correlated with total aerosol optical depth, with smoke more likely to be present in the boundary layer earlier in the biomass-burning season, evolving to smoke predominantly present above the cloud layers in September-October, typically resting upon the cloud-top inversion. The time period with the campaign-maximum near-surface light absorption and column aerosol optical depth, on 13-16 August of 2016, is investigated further. Also, backtrajectories indicate more direct boundary layer transport westward from the African continent is central to explaining the elevated surface aerosol loadings.« less

On Aethalometer measurement uncertainties and an instrument correction factor for the Arctic

NASA Astrophysics Data System (ADS)

Backman, John; Schmeisser, Lauren; Virkkula, Aki; Ogren, John A.; Asmi, Eija; Starkweather, Sandra; Sharma, Sangeeta; Eleftheriadis, Konstantinos; Uttal, Taneil; Jefferson, Anne; Bergin, Michael; Makshtas, Alexander; Tunved, Peter; Fiebig, Markus

2017-12-01

Several types of filter-based instruments are used to estimate aerosol light absorption coefficients. Two significant results are presented based on Aethalometer measurements at six Arctic stations from 2012 to 2014. First, an alternative method of post-processing the Aethalometer data is presented, which reduces measurement noise and lowers the detection limit of the instrument more effectively than boxcar averaging. The biggest benefit of this approach can be achieved if instrument drift is minimised. Moreover, by using an attenuation threshold criterion for data post-processing, the relative uncertainty from the electronic noise of the instrument is kept constant. This approach results in a time series with a variable collection time (Δt) but with a constant relative uncertainty with regard to electronic noise in the instrument. An additional advantage of this method is that the detection limit of the instrument will be lowered at small aerosol concentrations at the expense of temporal resolution, whereas there is little to no loss in temporal resolution at high aerosol concentrations ( > 2.1-6.7 Mm-1 as measured by the Aethalometers). At high aerosol concentrations, minimising the detection limit of the instrument is less critical. Additionally, utilising co-located filter-based absorption photometers, a correction factor is presented for the Arctic that can be used in Aethalometer corrections available in literature. The correction factor of 3.45 was calculated for low-elevation Arctic stations. This correction factor harmonises Aethalometer attenuation coefficients with light absorption coefficients as measured by the co-located light absorption photometers. Using one correction factor for Arctic Aethalometers has the advantage that measurements between stations become more inter-comparable.

Radiative and Thermal Impacts of Smoke Aerosol Longwave Absorption during Fires in the Moscow Region in Summer 2010

NASA Astrophysics Data System (ADS)

Gorchakova, I. A.; Mokhov, I. I.; Anikin, P. P.; Emilenko, A. S.

2018-03-01

The aerosol longwave radiative forcing of the atmosphere and heating rate of the near-surface aerosol layer are estimated for the extreme smoke conditions in the Moscow region in summer 2010. Thermal radiation fluxes in the atmosphere are determined using the integral transmission function and semiempirical aerosol model developed on the basis of standard aerosol models and measurements at the Zvenigorod Scientific Station, Obukhov Institute of Atmospheric Physics, Russian Academy of Sciences. The aerosol radiative forcing reached 33 W/m2 at the lower atmospheric boundary and ranged between-1.0 and 1.0 W/m2 at the upper atmospheric boundary. The heating rate of the 10-m atmospheric layer near surface was up to 0.2 K/h during the maximum smoke conditions on August 7-9. The sensitivity of the aerosol longwave radiative forcing to the changes in the aerosol absorption coefficient and aerosol optical thickness are estimated.

Gas-particle partitioning of semi-volatile organics on organic aerosols using a predictive activity coefficient model: analysis of the effects of parameter choices on model performance

NASA Astrophysics Data System (ADS)

Chandramouli, Bharadwaj; Jang, Myoseon; Kamens, Richard M.

The partitioning of a diverse set of semivolatile organic compounds (SOCs) on a variety of organic aerosols was studied using smog chamber experimental data. Existing data on the partitioning of SOCs on aerosols from wood combustion, diesel combustion, and the α-pinene-O 3 reaction was augmented by carrying out smog chamber partitioning experiments on aerosols from meat cooking, and catalyzed and uncatalyzed gasoline engine exhaust. Model compositions for aerosols from meat cooking and gasoline combustion emissions were used to calculate activity coefficients for the SOCs in the organic aerosols and the Pankow absorptive gas/particle partitioning model was used to calculate the partitioning coefficient Kp and quantitate the predictive improvements of using the activity coefficient. The slope of the log K p vs. log p L0 correlation for partitioning on aerosols from meat cooking improved from -0.81 to -0.94 after incorporation of activity coefficients iγ om. A stepwise regression analysis of the partitioning model revealed that for the data set used in this study, partitioning predictions on α-pinene-O 3 secondary aerosol and wood combustion aerosol showed statistically significant improvement after incorporation of iγ om, which can be attributed to their overall polarity. The partitioning model was sensitive to changes in aerosol composition when updated compositions for α-pinene-O 3 aerosol and wood combustion aerosol were used. The octanol-air partitioning coefficient's ( KOA) effectiveness as a partitioning correlator over a variety of aerosol types was evaluated. The slope of the log K p- log K OA correlation was not constant over the aerosol types and SOCs used in the study and the use of KOA for partitioning correlations can potentially lead to significant deviations, especially for polar aerosols.

Source apportionment of PM2.5 light extinction in an urban atmosphere in China.

PubMed

Lan, Zijuan; Zhang, Bin; Huang, Xiaofeng; Zhu, Qiao; Yuan, Jinfeng; Zeng, Liwu; Hu, Min; He, Lingyan

2018-01-01

Haze in China is primarily caused by high pollution of atmospheric fine particulates (PM 2.5 ). However, the detailed source structures of PM 2.5 light extinction have not been well established, especially for the roles of various organic aerosols, which makes haze management lack specified targets. This study obtained the mass concentrations of the chemical compositions and the light extinction coefficients of fine particles in the winter in Dongguan, Guangdong Province, using high time resolution aerosol observation instruments. We combined the positive matrix factor (PMF) analysis model of organic aerosols and the multiple linear regression method to establish a quantitative relationship model between the main chemical components, in particular the different sources of organic aerosols and the extinction coefficients of fine particles with a high goodness of fit (R 2 =0.953). The results show that the contribution rates of ammonium sulphate, ammonium nitrate, biomass burning organic aerosol (BBOA), secondary organic aerosol (SOA) and black carbon (BC) were 48.1%, 20.7%, 15.0%, 10.6%, and 5.6%, respectively. It can be seen that the contribution of the secondary aerosols is much higher than that of the primary aerosols (79.4% versus 20.6%) and are a major factor in the visibility decline. BBOA is found to have a high visibility destroying potential, with a high mass extinction coefficient, and was the largest contributor during some high pollution periods. A more detailed analysis indicates that the contribution of the enhanced absorption caused by BC mixing state was approximately 37.7% of the total particle absorption and should not be neglected. Copyright © 2017. Published by Elsevier B.V.

The Ascension Island Boundary Layer in the Remote Southeast Atlantic is Often Smoky

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zuidema, Paquita; Sedlacek, Arthur J.; Flynn, Connor

Observations from June through October, 2016, from a surface-based ARM Mobile Facility deployment on Ascension Island (8°S, 14.5°W) indicate that refractory black carbon (rBC) is almost always present within the boundary layer. rBC mass concentrations, light absorption coefficients, and cloud condensation nuclei concentrations vary in concert and synoptically, peaking in August. Derived mass absorption cross-sections using light absorptioin coefficients at three wavelengths as a function of rBC mass indirectly indicate the presence of other light-absorbing organic aerosols (e.g., brown carbon), most pronounced in June. A filter-based estimate of single-scattering-albedo increases systematically from August to October, also apparent in 2017. Boundary-layermore » aerosol loadings are only loosely correlated with total aerosol optical depth, with smoke more likely to be present in the boundary layer earlier in the biomass-burning season, evolving to smoke predominantly present in the free-troposphere in September-October, typically resting upon the cloud-top inversion. The time period with the campaign-maximum near-surface light absorption and column aerosol optical depth, on 13-16 August of 2016, is investigated further. Back trajectories indicate the boundary layer transport was directly westward from the African continent, which is unusual in August.« less

Evolution of multispectral aerosol optical properties in a biogenically-influenced urban environment during the CARES campaign

NASA Astrophysics Data System (ADS)

Gyawali, M.; Arnott, W. P.; Zaveri, R. A.; Song, C.; Pekour, M.; Flowers, B.; Dubey, M. K.; Setyan, A.; Zhang, Q.; Harworth, J. W.; Radney, J. G.; Atkinson, D. B.; China, S.; Mazzoleni, C.; Gorkowski, K.; Subramanian, R.; Jobson, B. T.; Moosmüller, H.

2013-03-01

Ground-based aerosol measurements made in June 2010 within Sacramento urban area (site T0) and at a 40-km downwind location (site T1) in the forested Sierra Nevada foothills area are used to investigate the evolution of multispectral optical properties as the urban aerosols aged and interacted with biogenic emissions. Along with black carbon and non-refractory aerosol mass and composition observations, spectral absorptio (βabs), scattering (βsca), and extinction (βext) coefficients for wavelengths ranging from 355 to 1064 nm were measured at both sites using photoacoustic (PA) instruments with integrating nephelometers and using cavity ring-down (CRD) instruments. The daytime average Ångström exponent of absorption (AEA) was ~1.6 for the wavelength pair 405 and 870 nm at T0, while it was ~1.8 for the wavelength pair 355 and 870 nm at T1, indicating a modest wavelength-dependent enhancement of absorption at both sites throughout the study. The measured and Mie theory calculations of multispectral βsca showed good correlation (R2=0.85-0.94). The average contribution of supermicron aerosol (mainly composed of sea salt particles advected in from the Pacific Ocean) to the total scattering coefficient ranged from less than 20% at 405 nm to greater than 80% at 1064 nm. From 22 to 28 June, secondary organic aerosol mass increased significantly at both sites due to increased biogenic emissions coupled with intense photochemical activity and air mass recirculation in the area. During this period, the short wavelength scattering coefficients at both sites gradually increased due to increase in the size of submicron aerosols. At the same time, BC mass-normalized absorption cross-section (MAC) values for ultraviolet wavelengths at T1 increased by ~60% compared to the relatively less aged urban emissions at the T0 site. In contrast, the average MAC values for 870 nm wavelength were identical at both sites. These results suggest formation of moderately brown secondary organic aerosols formed in biogenically-influenced urban air.

Contribution of Brown Carbon to Direct Radiative Forcing over the Indo-Gangetic Plain.

PubMed

Shamjad, P M; Tripathi, S N; Pathak, Ravi; Hallquist, M; Arola, Antti; Bergin, M H

2015-09-01

The Indo-Gangetic Plain is a region of known high aerosol loading with substantial amounts of carbonaceous aerosols from a variety of sources, often dominated by biomass burning. Although black carbon has been shown to play an important role in the absorption of solar energy and hence direct radiative forcing (DRF), little is known regarding the influence of light absorbing brown carbon (BrC) on the radiative balance in the region. With this in mind, a study was conducted for a one month period during the winter-spring season of 2013 in Kanpur, India that measured aerosol chemical and physical properties that were used to estimate the sources of carbonaceous aerosols, as well as parameters necessary to estimate direct forcing by aerosols and the contribution of BrC absorption to the atmospheric energy balance. Positive matrix factorization analyses, based on aerosol mass spectrometer measurements, resolved organic carbon into four factors including low-volatile oxygenated organic aerosols, semivolatile oxygenated organic aerosols, biomass burning, and hydrocarbon like organic aerosols. Three-wavelength absorption and scattering coefficient measurements from a Photo Acoustic Soot Spectrometer were used to estimate aerosol optical properties and estimate the relative contribution of BrC to atmospheric absorption. Mean ± standard deviation values of short-wave cloud free clear sky DRF exerted by total aerosols at the top of atmosphere, surface and within the atmospheric column are -6.1 ± 3.2, -31.6 ± 11, and 25.5 ± 10.2 W/m(2), respectively. During days dominated by biomass burning the absorption of solar energy by aerosols within the atmosphere increased by ∼35%, accompanied by a 25% increase in negative surface DRF. DRF at the top of atmosphere during biomass burning days decreased in negative magnitude by several W/m(2) due to enhanced atmospheric absorption by biomass aerosols, including BrC. The contribution of BrC to atmospheric absorption is estimated to range from on average 2.6 W/m(2) for typical ambient conditions to 3.6 W/m(2) during biomass burning days. This suggests that BrC accounts for 10-15% of the total aerosol absorption in the atmosphere, indicating that BrC likely plays an important role in surface and boundary temperature as well as climate.

Aerosol absorption coefficient and Equivalent Black Carbon by parallel operation of AE31 and AE33 aethalometers at the Zeppelin station, Ny Ålesund, Svalbard

NASA Astrophysics Data System (ADS)

Eleftheriadis, Konstantinos; Kalogridis, Athina-Cerise; Vratolis, Sterios; Fiebig, Markus

2016-04-01

Light absorbing carbon in atmospheric aerosol plays a critical role in radiative forcing and climate change. Despite the long term measurements across the Arctic, comparing data obtained by a variety of methods across stations requires caution. A method for extracting the aerosol absorption coefficient from data obtained over the decades by filter based instrument is still under development. An IASOA Aerosol working group has been initiated to address this and other cross-site aerosol comparison opportunities. Continuous ambient measurements of EBC/light attenuation by means of a Magee Sci. AE-31 aethalometer operating at the Zeppelinfjellet station (474 m asl; 78°54'N, 11°53'E), Ny Ålesund, Svalbard, have been available since 2001 (Eleftheriadis et al, 2009), while a new aethalometer model (AE33, Drinovec et al, 2014) has been installed to operate in parallel from the same inlet since June 2015. Measurements are recorded by a Labview routine collecting all available parameters reported by the two instrument via RS232 protocol. Data are reported at 1 and 10 minute intervals as averages for EBC (μg m-3) and aerosol absorption coefficients (Mm-1) by means of routine designed to report Near Real Time NRT data at the EBAS WDCA database (ebas.nilu.no) Results for the first 6 month period are reported here in an attempt to evaluate comparative performance of the two instruments in terms of their response with respect to the variable aerosol load of light absorbing carbon during the warm and cold seasons found in the high arctic. The application of available conversion schemes for obtaining the absorption coefficient by the two instruments is found to demonstrate a marked difference in their output. During clean periods of low aerosol load (EBC < 30 ng m-3), the two instruments display a better agreement with regression slope for the 880 nm signal between the two at ~ 0.9 compared to a slope at ~ 0.6 during the period of higher absorbing carbon loads (400< EBC<30 ng m-3) A detailed analysis of the variability observed in the wavelength dependence and possible association with air mass origin was also conducted. Drinovec, L., Močnik, G., Zotter, P., Prévôt, A. S. H., Ruckstuhl, C., Coz, E., Rupakheti, M., Sciare, J., Müller, T., Wiedensohler, A., and Hansen, A. D. A. The "dual-spot" Aethalometer: an improved measurement of aerosol black carbon with real-time loading compensation, Atmos. Meas. Tech., 8, 1965-1979, doi:10.5194/amt-8-1965-2015, 2015. Eleftheriadis, K., Vratolis, S., and Nyeki, S.: Aerosol black carbon in the European Arctic: Measurements at Zeppelin station, Ny-Ålesund, Svalbard from 1998-2007, Geophys. Res. Lett., 36, L02809, doi:10.1029/2008GL035741, 2009

A Tale of two Cities: Photoacoustic and Aethalometer Measurements Comparisons of Light Absorption in Mexico City and Las Vegas, NV, USA

NASA Astrophysics Data System (ADS)

Paredes-Miranda, G.; Arnott, W. P.; Marley, N. A.; Gaffney, J. S.

2007-05-01

As part of the Megacity Impacts on Regional and Global Environments, MIRAGE-Mex deployment to Mexico City in the period of 30 days, March 2006, a suite of photoacoustic spectrometers (PAS; W. Arnott & G. Paredes), nephelometer scattering, and aetholemeter absorption instruments (N. Marley & J.Gaffney) were installed to measure at ground level the light absorption and scattering by aerosols at the urban site at Instituto Mexicano del Petroleo (Mexican Oil Institute, denoted by IMP). This IMP site gave in-situ characterization of the Mexico City plume under favorable wind conditions. The PAS used at IMP operates at 532 nm, and conveniently allowed for characterization of gaseous absorption at this wavelength as well. Light scattering measurements are accomplished within the PAS by the reciprocal nephelometery method. In the urban site the aerosol absorption coefficient typically varies between 20 and 180 Mm-1 during the course of the day and significant diurnal variation of the aerosol single scattering albedo was observed. The Las Vegas, NV site was located at East Charleston Street on January-February, 2003. In east Las Vegas typical westerly winds carry the city plume across the site. Comparisons of PAS aerosol light absorption and aetholemeter absorption measurements at 521 nm at both Las Vegas NV and Mexico City sites will be presented. We will also present a broad overview of the diurnal variation of the scattering and absorption as well as the single scattering albedo and fraction of absorption due to gases at the sites in relation to secondary aerosol formation.

Long term measurements of optical properties and their hygroscopic enhancement

NASA Astrophysics Data System (ADS)

Hervo, M.; Sellegri, K.; Pichon, J. M.; Roger, J. C.; Laj, P.

2014-11-01

Optical properties of aerosols were measured from the GAW Puy de Dôme station (1465 m) over a seven year period (2006-2012). The impact of hygroscopicity on aerosol optical properties was calculated over a two year period (2010-2011). The analysis of the spatial and temporal variability of the optical properties showed that while no long term trend was found, a clear seasonal and diurnal variation was observed on the extensive parameters (scattering, absorption). Scattering and absorption coefficients were highest during the warm season and daytime, in concordance with the seasonality and diurnal variation of the PBL height reaching the site. Intensive parameters (single scattering albedo, asymmetry factor, refractive index) did not show such a strong diurnal variability, but still indicated different values depending on the season. Both extensive and intensive optical parameters were sensitive to the air mass origin. A strong impact of hygroscopicity on aerosol optical properties was calculated, mainly on aerosol scattering, with a dependence on the aerosol type. At 90% humidity, the scattering factor enhancement (fσsca) was more than 4.4 for oceanic aerosol that have mixed with a pollution plume. Consequently, the aerosol radiative forcing was estimated to be 2.8 times higher at RH = 90% and 1.75 times higher at ambient RH when hygroscopic growth of the aerosol was considered. The hygroscopicity enhancement factor of the scattering coefficient was parameterized as a function of humidity and air mass type.

Determination of the refractive index of insoluble organic extracts from atmospheric aerosol over the visible wavelength range using optical tweezers

NASA Astrophysics Data System (ADS)

Shepherd, Rosalie H.; King, Martin D.; Marks, Amelia A.; Brough, Neil; Ward, Andrew D.

2018-04-01

Optical trapping combined with Mie spectroscopy is a new technique used to record the refractive index of insoluble organic material extracted from atmospheric aerosol samples over a wide wavelength range. The refractive index of the insoluble organic extracts was shown to follow a Cauchy equation between 460 and 700 nm for organic aerosol extracts collected from urban (London) and remote (Antarctica) locations. Cauchy coefficients for the remote sample were for the Austral summer and gave the Cauchy coefficients of A = 1.467 and B = 1000 nm2 with a real refractive index of 1.489 at a wavelength of 589 nm. Cauchy coefficients for the urban samples varied with season, with extracts collected during summer having Cauchy coefficients of A = 1.465 ± 0.005 and B = 4625 ± 1200 nm2 with a representative real refractive index of 1.478 at a wavelength of 589 nm, whilst samples extracted during autumn had larger Cauchy coefficients of A = 1.505 and B = 600 nm2 with a representative real refractive index of 1.522 at a wavelength of 589 nm. The refractive index of absorbing aerosol was also recorded. The absorption Ångström exponent was determined for woodsmoke and humic acid aerosol extract. Typical values of the Cauchy coefficient for the woodsmoke aerosol extract were A = 1.541 ± 0.03 and B = 14 800 ± 2900 nm2, resulting in a real refractive index of 1.584 ± 0.007 at a wavelength of 589 nm and an absorption Ångström exponent of 8.0. The measured values of refractive index compare well with previous monochromatic or very small wavelength range measurements of refractive index. In general, the real component of the refractive index increases from remote to urban to woodsmoke. A one-dimensional radiative-transfer calculation of the top-of-the-atmosphere albedo was applied to model an atmosphere containing a 3 km thick layer of aerosol comprising pure water, pure insoluble organic aerosol, or an aerosol consisting of an aqueous core with an insoluble organic shell. The calculation demonstrated that the top-of-the-atmosphere albedo increases by 0.01 to 0.04 for pure organic particles relative to water particles of the same size and that the top-of-the-atmosphere albedo increases by 0.03 for aqueous core-shell particles as volume fraction of the shell material increases to 25 %.

A Solar Radiation Parameterization for Atmospheric Studies. Volume 15

NASA Technical Reports Server (NTRS)

Chou, Ming-Dah; Suarez, Max J. (Editor)

1999-01-01

The solar radiation parameterization (CLIRAD-SW) developed at the Goddard Climate and Radiation Branch for application to atmospheric models are described. It includes the absorption by water vapor, O3, O2, CO2, clouds, and aerosols and the scattering by clouds, aerosols, and gases. Depending upon the nature of absorption, different approaches are applied to different absorbers. In the ultraviolet and visible regions, the spectrum is divided into 8 bands, and single O3 absorption coefficient and Rayleigh scattering coefficient are used for each band. In the infrared, the spectrum is divided into 3 bands, and the k-distribution method is applied for water vapor absorption. The flux reduction due to O2 is derived from a simple function, while the flux reduction due to CO2 is derived from precomputed tables. Cloud single-scattering properties are parameterized, separately for liquid drops and ice, as functions of water amount and effective particle size. A maximum-random approximation is adopted for the overlapping of clouds at different heights. Fluxes are computed using the Delta-Eddington approximation.

The characteristics of brown carbon aerosol during winter in Beijing

NASA Astrophysics Data System (ADS)

Cheng, Yuan; He, Ke-bin; Du, Zhen-yu; Engling, Guenter; Liu, Jiu-meng; Ma, Yong-liang; Zheng, Mei; Weber, Rodney J.

2016-02-01

Brown carbon (i.e., light-absorbing organic carbon, or BrC) exerts important effects on the environment and on climate in particular. Based on spectrophotometric absorption measurements on extracts of bulk aerosol samples, this study investigated the characteristics of BrC during winter in Beijing, China. Organic compounds extractable by methanol contributed approximately 85% to the organic carbon (OC) mass. Light absorption by the methanol extracts exhibited a strong wavelength dependence, with an average absorption Ångström exponent of 7.10 (fitted between 310 and 450 nm). Normalizing the absorption coefficient (babs) measured at 365 nm to the extractable OC mass yielded an average mass absorption efficiency (MAE) of 1.45 m2/g for the methanol extracts. This study suggests that light absorption by BrC could be comparable with black carbon in the spectral range of near-ultraviolet light. Our results also indicate that BrC absorption and thus BrC radiative forcing could be largely underestimated when using water-soluble organic carbon (WSOC) as a surrogate for BrC. Compared to previous work relying only on WSOC, this study provides a more comprehensive understanding of BrC aerosol based on methanol extraction.

Absorption Ångström exponents of aerosols and light absorbing carbon (LAC) obtained from in situ data in Covilhã, central Portugal.

PubMed

Mogo, S; Cachorro, V E; de Frutos, A; Rodrigues, A

2012-12-01

A field campaign was conducted from October 2009 to July 2010 at Covilhã, a small town located in the region of Beira Interior (Portugal) in the interior of the Iberian Peninsula. The ambient light-absorption coefficient, σ(a) (522 nm), obtained from a Particle Soot Absorption Photometer (PSAP), presented a daily mean value of 12.1 Mm⁻¹ (StD = 7.3 Mm⁻¹). The wavelength dependence of aerosol light absorption is investigated through the Ångström parameter, α(a). The α(a) values for the pair of wavelengths 470-660 nm ranged from 0.86 to 1.47 during the period of measurements. The PSAP data were used to infer the mass of light absorbing carbon (LAC) and the daily mean varied from 0.1 to 6.8 μg m⁻³. A detailed study of special events with different aerosol characteristics is carried out and, to support data interpretation, air masses trajectory analysis is performed.

Aerosol Light Absorption and Scattering in Mexico City: Comparison With Las Vegas, NV, and Los Angeles, CA.

NASA Astrophysics Data System (ADS)

Paredes-Miranda, G.; Arnott, W. P.; Gaffney, J. S.; Marley, N. A.; Campbell, D.; Fujita, E.

2007-12-01

Aerosol light scattering and absorption measurements were deployed in and near Mexico City in March 2006 as part of the Megacity Impacts on Regional and Global Environments (MIRAGE). The primary site in Mexico City was an urban site at Instituto Mexicano del Petroleo (Mexican Oil Institute, denoted by IMP). Similar campaigns were held in Las Vegas, NV in January-February, 2003; and Los Angeles, CA at numerous sites during all seasons from 2003 through 2007. The IMP site gave in-situ characterization of the Mexico City plume under favorable wind conditions. The photoacoustic instrument (PAS) used at IMP operates at 532 nm, and conveniently allowed for characterization of gaseous absorption at this wavelength as well. Light scattering measurements are accomplished within the PAS by the reciprocal nephelometery method. In Mexico City the aerosol absorption coefficient typically varies between 20 and 180 Mm-1 during the course of the day and significant diurnal variation of the aerosol single scattering albedo was observed probably as a consequence of secondary aerosol formation. We will present the diurnal variation of the scattering and absorption as well as the single scattering albedo and fraction of absorption due to gases at the IMP site and compare with Las Vegas diurnal variation. Mexico City 'breaths' more during the course of the day than Las Vegas, Nevada in part because the latitude of Mexico City resulted in more direct solar radiation. Further insight on the meteorological connections and population dynamics will be discussed.

Seven years of aerosol scattering hygroscopic growth measurements from SGP: Factors influencing water uptake: Aerosol Scattering Hygroscopic Growth

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jefferson, A.; Hageman, D.; Morrow, H.

Long-term measurements of changes in the aerosol scattering coefficient hygroscopic growth at the U.S. Department of Energy Southern Great Plains site provide information on the seasonal as well as size and chemical dependence of aerosol hygroscopic growth. Annual average sub 10 um fRH values (the ratio of aerosol scattering at 85%/40% RH) were 1.75 and 1.87 for the gamma and kappa fit algorithms, respectively. The study found higher growth rates in the winter and spring seasons that correlated with high aerosol nitrate mass fraction. FRH, exhibited strong, but differing correlations with the scattering Ångström exponent and backscatter fraction, two opticalmore » size-dependent parameters. The aerosol organic fraction had a strong influence, with fRH decreasing with increases in the organic mass fraction and absorption Ångström exponent and increasing with the aerosol single scatter albedo. Uncertainty analysis if the fit algorithms revealed high uncertainty at low scattering coefficients and slight increases in uncertainty at high RH and fit parameters values.« less

Light-Absorbing Aerosol during NASA GRIP: Overview of Observations in the Free Troposphere and Associated with Tropical Storm Systems

NASA Astrophysics Data System (ADS)

Ziemba, L. D.; Beyersdorf, A. J.; Chen, G.; Corr, C. A.; Craig, L.; Dhaniyala, S.; Dibb, J. E.; Hudgins, C. H.; Ismail, S.; Latham, T.; Nenes, A.; Thornhill, K. L.; Winstead, E.; Anderson, B. E.

2010-12-01

Aerosols play a significant role in regulating Earth’s climate. Absorbing aerosols typically constitute a small fraction of ambient particle mass but can contribute significantly to direct and indirect climate forcing depending on size, mixing state, concentration, chemical composition, and vertical and spatial distribution. Aerosols may also significantly affect tropical storm/hurricane dynamics through direct light absorption and activation as cloud nuclei. An extensive suite of instrumentation measuring aerosol chemical, physical, and optical properties was deployed aboard the NASA DC-8 to characterize aerosol during the NASA GRIP (Genesis and Rapid Intensification Processes; August-September 2010) mission. The majority of flight time was spent at high altitude (greater than 9 km) and thus much of the sampling was done in the free troposphere, including extensive sampling in the vicinity of tropical storm systems and more diffuse cirrus clouds. With operations based in Fort Lauderdale, FL and St. Croix, U.S. Virgin Islands, a large geographic region was sampled including much of the Gulf of Mexico and tropical Atlantic Ocean. Observations are reported for light-absorbing carbon aerosol (mainly black carbon, BC) primarily using a single particle soot photometer (SP2). The SP2 employs single-particle laser-induced incandescence to provide a mass-specific measurement not subject to scattering interference that is optimal for the low concentration environments like those encountered during GRIP. BC mass concentrations, 100-500 nm size distributions, and mixing state (i.e. coating thickness of scattering material) are presented. Total and sub-micron aerosol absorption coefficients (principally from BC and dust aerosol) are reported using a particle soot absorption photometer (PSAP) along with comparisons with calculated absorption coefficients derived from SP2 observations in various conditions. In addition, dust aerosol is specifically identified using optical and aerodynamic size distributions obtained from an optical particle counter (OPC) and aerodynamic particle sizer (APS), respectively, as well as by filter-based analyses of chemical composition. BC and dust concentrations, size distribution, and optical properties are reported for clear-sky conditions and in the regions surrounding tropical storms to better understand the radial and vertical distribution of light-absorbing aerosol associated with hurricanes. Observations during GRIP are compared to an extensive characterization of the Saharan Air Layer (SAL) made during the 2006 NAMMA (NASA African Monsoon Multidisciplinary Analyses) mission to assess changes in concentration and aerosol size distribution during transport and cloud interaction.

Absorption and Scattering of Aerosol measured onboard R/V Gisang1 over the Yellow Sea

NASA Astrophysics Data System (ADS)

Inae, K.; Lee, M.; Shin, B.; Ryoo, S.; Jung, J.; Kim, S. W.

2017-12-01

Absorption and scattering coefficient were measured onboard RV Gisang 1 over the Yellow Sea (covering 124° 127°E, 31° 38°N) during May June, 2016. BC concentration was analyzed at seven wavelengths (370, 470, 520, 590, 660, 880, and 950nm) every 1 minute by Aethalometer. Scattering coefficient was measured at three wavelengths (450, 550, and 750nm) every 5 minutes with Nephelometer. The mean absorption coefficient was 1.2 Mm-1 at 880nm and the mean scattering coefficient was 116Mm-1 at 550nm. Single scattering albedo(SSA) reached the maximum value of 3.0 at 700nm. The calculated mean scattering angstrom exponent(SAE) was 1.6 and absorbing angstrom exponent(AAE) was 1.1. The AAE and SAE were higher in aged Chinese plume.

Using the OMI Aerosol Index and Absorption Aerosol Optical Depth to evaluate the NASA MERRA Aerosol Reanalysis

NASA Astrophysics Data System (ADS)

Buchard, V.; da Silva, A. M.; Colarco, P. R.; Darmenov, A.; Randles, C. A.; Govindaraju, R.; Torres, O.; Campbell, J.; Spurr, R.

2014-12-01

A radiative transfer interface has been developed to simulate the UV Aerosol Index (AI) from the NASA Goddard Earth Observing System version 5 (GEOS-5) aerosol assimilated fields. The purpose of this work is to use the AI and Aerosol Absorption Optical Depth (AAOD) derived from the Ozone Monitoring Instrument (OMI) measurements as independent validation for the Modern Era Retrospective analysis for Research and Applications Aerosol Reanalysis (MERRAero). MERRAero is based on a version of the GEOS-5 model that is radiatively coupled to the Goddard Chemistry, Aerosol, Radiation, and Transport (GOCART) aerosol module and includes assimilation of Aerosol Optical Depth (AOD) from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensor. Since AI is dependent on aerosol concentration, optical properties and altitude of the aerosol layer, we make use of complementary observations to fully diagnose the model, including AOD from the Multi-angle Imaging SpectroRadiometer (MISR), aerosol retrievals from the Aerosol Robotic Network (AERONET) and attenuated backscatter coefficients from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) mission to ascertain potential misplacement of plume height by the model. By sampling dust, biomass burning and pollution events in 2007 we have compared model produced AI and AAOD with the corresponding OMI products, identifying regions where the model representation of absorbing aerosols was deficient. As a result of this study over the Saharan dust region, we have obtained a new set of dust aerosol optical properties that retains consistency with the MODIS AOD data that were assimilated, while resulting in better agreement with aerosol absorption measurements from OMI. The analysis conducted over the South African and South American biomass burning regions indicates that revising the spectrally-dependent aerosol absorption properties in the near-UV region improves the modeled-observed AI comparisons. Finally, during a period where the Asian region was mainly dominated by anthropogenic aerosols, we have performed a qualitative analysis in which the specification of anthropogenic emissions in GEOS-5 is adjusted to provide insight into discrepancies observed in AI comparisons.

Using the OMI aerosol index and absorption aerosol optical depth to evaluate the NASA MERRA Aerosol Reanalysis

NASA Astrophysics Data System (ADS)

Buchard, V.; da Silva, A. M.; Colarco, P. R.; Darmenov, A.; Randles, C. A.; Govindaraju, R.; Torres, O.; Campbell, J.; Spurr, R.

2015-05-01

A radiative transfer interface has been developed to simulate the UV aerosol index (AI) from the NASA Goddard Earth Observing System version 5 (GEOS-5) aerosol assimilated fields. The purpose of this work is to use the AI and aerosol absorption optical depth (AAOD) derived from the Ozone Monitoring Instrument (OMI) measurements as independent validation for the Modern Era Retrospective analysis for Research and Applications Aerosol Reanalysis (MERRAero). MERRAero is based on a version of the GEOS-5 model that is radiatively coupled to the Goddard Chemistry, Aerosol, Radiation, and Transport (GOCART) aerosol module and includes assimilation of aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensor. Since AI is dependent on aerosol concentration, optical properties and altitude of the aerosol layer, we make use of complementary observations to fully diagnose the model, including AOD from the Multi-angle Imaging SpectroRadiometer (MISR), aerosol retrievals from the AErosol RObotic NETwork (AERONET) and attenuated backscatter coefficients from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) mission to ascertain potential misplacement of plume height by the model. By sampling dust, biomass burning and pollution events in 2007 we have compared model-produced AI and AAOD with the corresponding OMI products, identifying regions where the model representation of absorbing aerosols was deficient. As a result of this study over the Saharan dust region, we have obtained a new set of dust aerosol optical properties that retains consistency with the MODIS AOD data that were assimilated, while resulting in better agreement with aerosol absorption measurements from OMI. The analysis conducted over the southern African and South American biomass burning regions indicates that revising the spectrally dependent aerosol absorption properties in the near-UV region improves the modeled-observed AI comparisons. Finally, during a period where the Asian region was mainly dominated by anthropogenic aerosols, we have performed a qualitative analysis in which the specification of anthropogenic emissions in GEOS-5 is adjusted to provide insight into discrepancies observed in AI comparisons.

Airborne Cavity Ring-Down Measurement of Aerosol Extinction and Scattering During the Aerosol IOP

NASA Technical Reports Server (NTRS)

Strawa, A. W.; Ricci, K.; Provencal, R.; Schmid, B.; Covert, D.; Elleman, R.; Arnott, P.

2003-01-01

Large uncertainties in the effects of aerosols on climate require improved in-situ measurements of extinction coefficient and single-scattering albedo. This paper describes preliminary results from Cadenza, a new continuous wave cavity ring-down (CW-CRD) instrument designed to address these uncertainties. Cadenza measures the aerosol extinction coefficient for 675 nm and 1550 nm light, and simultaneously measures the scattering coefficient at 675 nm. In the past year Cadenza was deployed in the Asian Dust Above Monterey (ADAM) and DOE Aerosol Intensive Operating Period (IOP) field projects. During these flights Cadenza produced measurements of aerosol extinction in the range from 0.2 to 300 Mm-1 with an estimated precision of 0.1 Min-1 for 1550 nm light and 0.2 Mm-1 for 675 nm light. Cadenza data from the ADAM and Aerosol IOP missions compared favorably with data from the other instruments aboard the CIRPAS Twin Otter aircraft and participating in those projects.= We present comparisons between the Cadenza measurements and those friom a TSI nephelometer, Particle Soot Absorption Photometer (PSAP), and the AATS 14 sun-photometer. Measurements of the optical properties of smoke and dust plumes sampled during these campaigns are presented and estimates of heating rates due to these plumes are made.

Cavity Ring-Down Measurement of Aerosol Optical Properties During the Asian Dust Above Monterey Experiment and DOE Aerosol Intensive Operating Period

NASA Technical Reports Server (NTRS)

Ricci, K.; Strawa, A. W.; Provencal, R.; Castaneda, R.; Bucholtz, A.; Schmid, B.

2004-01-01

Large uncertainties in the effects of aerosols on climate require improved in-situ measurements of extinction coefficient and single-scattering albedo. This paper describes preliminary results from Cadenza, a new continuous wave cavity ring-down (CW-CRD) instrument designed to address these uncertainties. Cadenza measures the aerosol extinction coefficient for 675 nm and 1550 nm light, and simultaneously measures the scattering coefficient at 675 nm. In the past year Cadenza was deployed in the Asian Dust Above Monterey (ADAM) and DOE Aerosol Intensive Operating Period (IOP) field projects. During these flights Cadenza produced measurements of aerosol extinction in the range from 0.2 to 300/Mm with an estimated precision of 0.1/Mm for 1550 nm light and 0.2/Mm for 675 nm light. Cadenza data from the ADAM and Aerosol IOP missions compared favorably with data from the other instruments aboard the CIRPAS Twin Otter aircraft and participating in those projects. We present comparisons between the Cadenza measurements and those from a TSI nephelometer, Particle Soot Absorption Photometer (PSAP), and the AATS 14 sun-photometer. Measurements of the optical properties of smoke and dust plumes sampled during these campaigns are presented and estimates of heating rates due to these plumes are made.

Cavity Ring-Down Measurement of Aerosol Optical Properties During the Asian Dust Above Monterey Experiment and DOE Aerosol Intensive Operating Period

NASA Astrophysics Data System (ADS)

Ricci, K.; Strawa, A. W.; Provencal, R.; Castaneda, R.; Bucholtz, A.; Schmid, B.

2003-12-01

Large uncertainties in the effects of aerosols on climate require improved in-situ measurements of extinction coefficient and single-scattering albedo. This paper describes preliminary results from Cadenza, a new continuous wave cavity ring-down (CW-CRD) instrument designed to address these uncertainties. Cadenza measures the aerosol extinction coefficient for 675 nm and 1550 nm light, and simultaneously measures the scattering coefficient at 675 nm. In the past year Cadenza was deployed in the Asian Dust Above Monterey (ADAM) and DOE Aerosol Intensive Operating Period (IOP) field projects. During these flights Cadenza produced measurements of aerosol extinction in the range from 0.2 to 300 Mm-1 with an estimated precision of 0.1 Mm-1 for 1550 nm light and 0.2 Mm-1 for 675 nm light. Cadenza data from the ADAM and Aerosol IOP missions compared favorably with data from the other instruments aboard the CIRPAS Twin Otter aircraft and participating in those projects. We present comparisons between the Cadenza measurements and those from a TSI nephelometer, Particle Soot Absorption Photometer (PSAP), and the AATS14 sun-photometer. Measurements of the optical properties of smoke and dust plumes sampled during these campaigns are presented and estimates of heating rates due to these plumes are made.

Reduction in biomass burning aerosol light absorption upon humidification: roles of inorganically-induced hygroscopicity, particle collapse, and photoacoustic heat and mass transfer

NASA Astrophysics Data System (ADS)

Lewis, K. A.; Arnott, W. P.; Moosmüller, H.; Chakrabarty, R. K.; Carrico, C. M.; Kreidenweis, S. M.; Day, D. E.; Malm, W. C.; Laskin, A.; Jimenez, J. L.; Ulbrich, I. M.; Huffman, J. A.; Onasch, T. B.; Trimborn, A.; Liu, L.; Mishchenko, M. I.

2009-07-01

Smoke particle emissions from the combustion of biomass fuels typical for the western and southeastern United States were studied and compared under high humidity and ambient conditions in the laboratory. The fuels used are Montana ponderosa pine (Pinus ponderosa), southern California chamise (Adenostoma fasciculatum), and Florida saw palmetto (Serenoa repens). Information on the non-refractory chemical composition of biomass burning aerosol from each fuel was obtained with an aerosol mass spectrometer and through estimation of the black carbon concentration from light absorption measurements at 870 nm. Changes in the optical and physical particle properties under high humidity conditions were observed for hygroscopic smoke particles containing substantial inorganic mass fractions that were emitted from combustion of chamise and palmetto fuels. Light scattering cross sections increased under high humidity for these particles, consistent with the hygroscopic growth measured for 100 nm particles in HTDMA measurements. Photoacoustic measurements of aerosol light absorption coefficients reveal a 20% reduction with increasing relative humidity, contrary to the expectation of light absorption enhancement by the liquid coating taken up by hygroscopic particles. This reduction is hypothesized to arise from two mechanisms: 1. Shielding of inner monomers after particle consolidation or collapse with water uptake; 2. The contribution of mass transfer through evaporation and condensation at high relative humidity to the usual heat transfer pathway for energy release by laser-heated particles in the photoacoustic measurement of aerosol light absorption. The mass transfer contribution is used to evaluate the fraction of aerosol surface covered with liquid water solution as a function of RH.

Direct radiative effect due to brownness in organic carbon aerosols generated from biomass combustion

NASA Astrophysics Data System (ADS)

Rathod, T. D.; Sahu, S. K.; Tiwari, M.; Pandit, G. G.

2016-12-01

We report the enhancement in the direct radiative effect due the presence of Brown carbon (BrC) as a part of organic carbon aerosols. The optical properties of organic carbon aerosols generated from pyrolytic combustion of mango tree wood (Magnifera Indica) and dung cake at different temperatures were considered. Mie codes were used to calculate absorption and scattering coefficients coupled with experimentally derived imaginary complex refractive index. The direct radiative effect (DRE) for sampled organic carbon aerosols was estimated using a wavelength dependent radiative transfer equation. The BrC DRE was estimated taking virtually non absorbing organic aerosols as reference. The BrC DRE from wood and dung cake was compared at different combustion temperatures and conditions. The BrC contributed positively to the direct top of the atmosphere radiative effect. Dung cake generated BrC aerosols were found to be strongly light absorbing as compared to BrC from wood combustion. It was noted that radiative effects of BrC from wood depended on its generation temperature and conditions. For BrC aerosols from dung cake such strong dependence was not observed. The average BrC aerosol DRE values were 1.53±0.76 W g-1 and 17.84±6.45 W g-1 for wood and dung cake respectively. The DRE contribution of BrC aerosols came mainly (67-90%) from visible light absorption though they exhibited strong absorption in shorter wavelengths of the UV-visible spectrum.

In situ airborne measurements of aerosol optical properties during photochemical pollution events

NASA Astrophysics Data System (ADS)

Mallet, M.; van Dingenen, R.; Roger, J. C.; Despiau, S.; Cachier, H.

2005-02-01

Dry aerosol optical properties (scattering, absorbing coefficients, and single scattering albedo) were derived from in situ airborne measurements during two photochemical pollution events (25 and 26 June) observed during the Experience sur Site pour Contraindre les Modeles de Pollution atmospherique et de Transport d'Emissions (ESCOMPTE) experiment. Two flights were carried out during daytime (one during the morning and one at noon) over a domain, allowing the investigation of how an air pollution event affects the particle optical properties. Both horizontal distribution and vertical profiles are presented. Results from the horizontal mapping show that plumes of enhanced scattering and absorption are formed in the planetary boundary layer (PBL) during the day in the sea breeze-driven outflow of the coastal urban-industrial area of Marseille-Fos de Berre. The domain-averaged scattering coefficient (at 550 nm) over land σs changes from 35 (28) Mm-1 during land breeze to 63 (43) Mm-1 during sea breeze on 25 June (26 June), with local maxima reaching > 100 Mm-1. The increase in the scattering coefficient is associated with new particle formation, indicative of secondary aerosol formation. Simultaneously, the domain-averaged absorption coefficient increases from 5.6 (3.4) Mm-1 to 9.3 (8.0) Mm-1. The pollution plume leads to strong gradients in the single scattering albedo ωo over the domain studied, with local values as low as 0.73 observed inside the pollution plume. The role of photochemistry and secondary aerosol formation during the 25 June case is shown to increase ωo and to make the aerosol more `reflecting' while the plume moves away from the sources. The lower photochemical activity, observed in the 26 June case, induces a relatively higher contribution of black carbon, making the aerosol more absorbing. Results from vertical profiles at a single near-urban location in the domain indicate that the changes in optical properties happen almost entirely within the PBL. No significant variation of σs, σa, and ωo is observed in the upper layer (1-3 km), where the aerosol optical properties are considered to be well mixed.

Optical properties and CCN activity of aerosols in a high-altitude Himalayan environment: Results from RAWEX-GVAX: CCN activity of aerosols over Himalayas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gogoi, Mukunda M.; Babu, S. Suresh; Jayachandran, V.

2015-03-27

The seasonality and mutual dependence of aerosol optical properties and cloud condensation nuclei (CCN) activity under varying meteorological conditions at the high-altitude Nainital site (~2 km) in the Indo-Gangetic Plains were examined using nearly year-round measurements (June 2011 to March 2012) at the Atmospheric Radiation Measurement (ARM) mobile facility as part of the RAWEX-GVAX experiment of the Indian Space Research Organization and the U.S. Department of Energy. The results from collocated measurements provided enhanced aerosol scattering and absorption coefficients, CCN concentrations and total condensation nuclei (CN) concentrations during the dry autumn and winter months. The CCN concentration (at a supersaturationmore » of 0.46) was higher during periods of high aerosol absorption (single-scattering albedo (SSA) < 0.80) than during periods of high aerosol scattering (SSA > 0.85), indicating that the aerosol composition seasonally changes and influences the CCN activity. The monthly mean CCN activation ratio (at a supersaturation of 0.46) was highest (> 0.7) in late autumn (November); this finding is attributed to the contribution of biomass-burning aerosols to CCN formation at high supersaturation conditions.« less

Determination of UV-visible-NIR absorption coefficient of graphite bulk using direct and indirect methods

NASA Astrophysics Data System (ADS)

Smausz, T.; Kondász, B.; Gera, T.; Ajtai, T.; Utry, N.; Pintér, M.; Kiss-Albert, G.; Budai, J.; Bozóki, Z.; Szabó, G.; Hopp, B.

2017-10-01

Absorption coefficient of graphite bulk pressed from 1 to 5 μm-sized crystalline grains was measured in UV-Vis-NIR range with three different methods: (i) determination of pulsed laser ablation rate as the function of laser fluence for different wavelengths (248, 337, 532, and 1064 nm, respectively); (ii) production of aerosol particles by UV laser ablation of the bulk graphite in inert atmosphere and determination of the mass-specific absorption coefficient with a four-wavelength (266, 355, 532, and 1064 nm, respectively) photoacoustic spectrometer, and (iii) spectroscopic ellipsometry in 250-1000 nm range. Taking into account the wide range of the absorption coefficients of different carbon structures, an overall relatively good agreement was observed for the three methods. The ellipsometric results fit well with the ablation rate measurement, and the data obtained with photoacoustic method are also similar in the UV and NIR region; however, the values were somewhat higher in visible and near-UV range. Taking into account the limitations of the methods, they can be promising candidates for the determination of absorption coefficient when the samples are strongly scattering and there is no possibility to perform transmissivity measurements.

MAX-DOAS retrieval of aerosol extinction properties in Madrid, Spain

NASA Astrophysics Data System (ADS)

Wang, Shanshan; Cuevas, Carlos A.; Frieß, Udo; Saiz-Lopez, Alfonso

2017-04-01

We present Multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements performed in the urban environment of Madrid, Spain, from March to September 2015. The O4 absorption in the ultraviolet (UV) spectral region was used to retrieve the aerosol extinction profile using an inversion algorithm. The results show a good agreement between the hourly retrieved aerosol optical depth (AOD) and the correlative Aerosol Robotic Network (AERONET) product. Higher AODs are found in the summer season due to the more frequent occurrence of Saharan dust intrusions. The surface aerosol extinction coefficient as retrieved by the MAX-DOAS measurements was also compared to in situ PM2:5 concentrations. The level of agreement between both measurements indicates that the MAX-DOAS retrieval has the ability to characterize the extinction of aerosol particles near the surface. The retrieval algorithm was also used to study a case of severe dust intrusion on 12 May 2015. The capability of the MAX-DOAS retrieval to recognize the dust event including an elevated particle layer is investigated along with air mass back-trajectory analysis.

Aerosol Optical Properties of Smoke from the Las Conchas Wildfire, Los Alamos, NM

NASA Astrophysics Data System (ADS)

Gorkowski, K.; Dubey, M. K.; Flowers, B. A.; Aiken, A. C.; Klein, B. Z.; Mazzoleni, C.; Sharma, N.; China`, S.

2011-12-01

The Las Conchas wildfire in Northern New Mexico started on June, 26 2011 and spread rapidly, eventually burning an area of 634 km2 (245 mi2). Due to the close proximity to the fire, the Los Alamos National Laboratory (LANL) was shut down and the town evacuated for several days. Immediately after LANL reopened (7/6/2011) the Earth and Environmental Sciences Division (EES-14) attained unique measurements of the smoke by sampling the ambient air. Three Integrated Photoacoustic/Nephelometer Spectrometers (DMT Inc.) were set up to measure aerosol light absorption and scattering coefficients. A University of Northwest Switzerland thermodenuder was used to remove compounds that are volatile at temperatures up to 200C. The aerosol's optical properties were measured before and after denuding the sample at 405nm (blue), 532nm (green), 781nm (red), and for non-denuded particles also at 375nm (ultraviolet). The aerosol size distributions were measured after the denuder with a Laser Aerosol Spectrometer (LAS, TSI Inc.) and black carbon was measured with a Single Particle Soot Photometer (SP2, DMT Inc.). Additionally, ambient measurements of Total Particulate Matter (PM2.5 and PM10) were collected continuously at the LANL air monitoring stations. These measurements are used in conjunction with numerical simulations to determine the bulk optical properties of the aerosol. Aerosols in wildfire smoke are composed of organic and black carbon (soot) particles that are formed during wood combustion and pyrolysis. The optical properties of the smoke particles are complex and lead to large uncertainties in assessing the global climate. During the measurement period, the Las Conchas fire provided very high particle concentrations (up to 200 μg/m3) that were exploited to investigate their optical properties. By heating the particles to temperatures ranging from 75 to 200C in the denuder, volatile organics were removed and the optical properties of the remaining particles were measured. Denuding of the aerosols, removed the outer organic coatings leaving behind the inner core of black carbon (soot) and any compounds that did not volatize completely. By simultaneously measuring the optical properties of the non-denuded as well as the denuded aerosol, we can study how the coatings affect the optical properties. The absorption coefficient measurements showed that coatings can cause an increase or decrease in absorption. The photoacoustic measurements were also combined with SP2 measurements to gain a mechanistic understanding of the effect of composition on the mass light absorption cross-sections of carbonaceous aerosols emitted by fires.

Aerosol Absorption Measurements in MILAGRO.

NASA Astrophysics Data System (ADS)

Gaffney, J. S.; Marley, N. A.; Arnott, W. P.; Paredes-Miranda, L.; Barnard, J. C.

2007-12-01

During the month of March 2006, a number of instruments were used to determine the absorption characteristics of aerosols found in the Mexico City Megacity and nearby Valley of Mexico. These measurements were taken as part of the Department of Energy's Megacity Aerosol Experiment - Mexico City (MAX-Mex) that was carried out in collaboration with the Megacity Interactions: Local and Global Research Observations (MILAGRO) campaign. MILAGRO was a joint effort between the DOE, NSF, NASA, and Mexican agencies aimed at understanding the impacts of a megacity on the urban and regional scale. A super-site was operated at the Instituto Mexicano de Petroleo in Mexico City (designated T-0) and at the Universidad Technologica de Tecamac (designated T-1) that was located about 35 km to the north east of the T-0 site in the State of Mexico. A third site was located at a private rancho in the State of Hidalgo approximately another 35 km to the northeast (designated T-2). Aerosol absorption measurements were taken in real time using a number of instruments at the T-0 and T-1 sites. These included a seven wavelength aethalometer, a multi-angle absorption photometer (MAAP), and a photo-acoustic spectrometer. Aerosol absorption was also derived from spectral radiometers including a multi-filter rotating band spectral radiometer (MFRSR). The results clearly indicate that there is significant aerosol absorption by the aerosols in the Mexico City megacity region. The absorption can lead to single scattering albedo reduction leading to values below 0.5 under some circumstances. The absorption is also found to deviate from that expected for a "well-behaved" soot anticipated from diesel engine emissions, i.e. from a simple 1/lambda wavelength dependence for absorption. Indeed, enhanced absorption is seen in the region of 300-450 nm in many cases, particularly in the afternoon periods indicating that secondary organic aerosols are contributing to the aerosol absorption. This is likely due to carbonyl- and nitro- functional groups on conjugated and aromatic organic structures (e.g. PAH, and terpene derived products). Using 12-hour fine (0.1-1.0 micron) aerosol samples collected in the field on quartz filters, uv/vis and infrared spectra were obtained in the laboratory using integrating spheres and diffuse reflectance spectroscopy, respectively. An inter-comparison of the "real-time" measurements made by the photo-acoustic, aethalometer and MAAP techniques have been described. In addition, the in situ aethalometer (seven-channel) results are compared with continuous integrating sphere uv-visible spectra to examine the angstrom absorption coefficient variance. These results will be briefly overviewed and the specific posters detailing these results will be highlighted highlighted. This work was performed as part of the Department of Energy's Megacity Aerosol Experiment - Mexico City under the support of the Atmospheric Science Program. "This researchwas supported by the Office of Science (BER), U. S. Department of Energy, Grant No. DE-FG02-07ER64329.

Seven years of aerosol scattering hygroscopic growth measurements from SGP: Factors influencing water uptake: Aerosol Scattering Hygroscopic Growth

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jefferson, A.; Hageman, D.; Morrow, H.

Long-term measurements of changes in the aerosol scattering coefficient hygroscopic growth at the U.S. Department of Energy Southern Great Plains site provide information on the seasonal as well as size and chemical dependence of aerosol water uptake. Annual average sub-10 μm fRH values (the ratio of aerosol scattering at 85%/40% relative humidity (RH)) were 1.78 and 1.99 for the gamma and kappa fit algorithms, respectively. Our study found higher growth rates in the winter and spring seasons that correlated with a high aerosol nitrate mass fraction. fRH exhibited strong, but differing, correlations with the scattering Ångström exponent and backscatter fraction,more » two optical size-dependent parameters. The aerosol organic mass fraction had a strong influence on fRH. Increases in the organic mass fraction and absorption Ångström exponent coincided with a decrease in fRH. Similarly, fRH declined with decreases in the aerosol single scatter albedo. The uncertainty analysis of the fit algorithms revealed high uncertainty at low scattering coefficients and increased uncertainty at high RH and fit parameters values.« less

Seven years of aerosol scattering hygroscopic growth measurements from SGP: Factors influencing water uptake: Aerosol Scattering Hygroscopic Growth

DOE PAGES

Jefferson, A.; Hageman, D.; Morrow, H.; ...

2017-09-11

Long-term measurements of changes in the aerosol scattering coefficient hygroscopic growth at the U.S. Department of Energy Southern Great Plains site provide information on the seasonal as well as size and chemical dependence of aerosol water uptake. Annual average sub-10 μm fRH values (the ratio of aerosol scattering at 85%/40% relative humidity (RH)) were 1.78 and 1.99 for the gamma and kappa fit algorithms, respectively. Our study found higher growth rates in the winter and spring seasons that correlated with a high aerosol nitrate mass fraction. fRH exhibited strong, but differing, correlations with the scattering Ångström exponent and backscatter fraction,more » two optical size-dependent parameters. The aerosol organic mass fraction had a strong influence on fRH. Increases in the organic mass fraction and absorption Ångström exponent coincided with a decrease in fRH. Similarly, fRH declined with decreases in the aerosol single scatter albedo. The uncertainty analysis of the fit algorithms revealed high uncertainty at low scattering coefficients and increased uncertainty at high RH and fit parameters values.« less

Performance of a newly designed continuous soot monitoring system (COSMOS).

PubMed

Miyazaki, Yuzo; Kondo, Yutaka; Sahu, Lokesh K; Imaru, Junichi; Fukushima, Nobuhiko; Kano, Minoru

2008-10-01

We designed a continuous soot monitoring system (COSMOS) for fully automated, high-sensitivity, continuous measurement of light absorption by black carbon (BC) aerosols. The instrument monitors changes in transmittance across an automatically advancing quartz fiber filter tape using an LED at a 565 nm wavelength. To achieve measurements with high sensitivity and a lower detectable light absorption coefficient, COSMOS uses a double-convex lens and optical bundle pipes to maintain high light intensity and signal data are obtained at 1000 Hz. In addition, sampling flow rate and optical unit temperature are actively controlled. The inlet line for COSMOS is heated to 400 degrees C to effectively volatilize non-refractory aerosol components that are internally mixed with BC. In its current form, COSMOS provides BC light absorption measurements with a detection limit of 0.45 Mm(-1) (0.045 microg m(-3) for soot) for 10 min. The unit-to-unit variability is estimated to be within +/- 1%, demonstrating its high reproducibility. The absorption coefficients determined by COSMOS agreed with those by a particle soot absorption photometer (PSAP) to within 1% (r2 = 0.97). The precision (+/- 0.60 Mm(-1)) for 10 min integrated data was better than that of PSAP and an aethalometer under our operating conditions. These results showed that COSMOS achieved both an improved detection limit and higher precision for the filter-based light absorption measurements of BC compared to the existing methods.

Aerosol and CCN properties at Princess Elisabeth station, East Antarctica: seasonality, new particle formation events and properties around precipitation events

NASA Astrophysics Data System (ADS)

Mangold, Alexander; Laffineur, Quentin; De Backer, Hugo; Herenz, Paul; Wex, Heike; Gossart, Alexandra; Souverijns, Niels; Gorodetskaya, Irina; Van Lipzig, Nicole

2016-04-01

Since 2010, several complementary ground-based instruments for measuring the aerosol composition of the Antarctic atmosphere have been operated at the Belgian Antarctic research station Princess Elisabeth, in Dronning Maud Land, East Antarctica (71.95° S, 23.35° E, 1390 m asl.). In addition, three ground-based remote sensing instruments for cloud and precipitation observations have been installed for continuous operation, including a ceilometer (cloud base height, type, vertical extent), a 24 Ghz micro-rain radar (vertical profiles of radar effective reflectivity and Doppler velocity), and a pyrometer (cloud base temperature). The station is inhabited from November to end of February and operates under remote control during the other months. In this contribution, the general aerosol and cloud condensation nuclei (CCN) properties will be described with a special focus on new particle formation events and around precipitation events. New particle formation events are important for the atmospheric aerosol budget and they also show that aerosols are not only transported to Antarctica but are also produced there, also inland. Aerosols are essential for cloud formation and therefore also for precipitation, which is the only source for mass gain of the Antarctic ice sheet. Measured aerosol properties comprise size distribution, total number, total mass concentration, mass concentration of light-absorbing aerosol and absorption coefficient and total scattering coefficient. In addition, a CCN counter has been operated during austral summers 2013/14, 2014/15 and 2015/16. The baseline total number concentration N-total was around some hundreds of particles/cm3. During new particle formation events N-total increased to some thousands of particles/cm3. Simultaneous measurements of N-total, size distribution and CCN number revealed that mostly the number of particles smaller than 100 nm increased and that the concentration of cloud condensation nuclei increased only very weakly, respectively. Further analysis of the CCN data indicate that the aerosol measured at Princess Elisabeth station consisted mainly of material with a hygroscopicity close to that of sulfate. The measured wavelength-dependent aerosol absorption and scattering coefficients give further insight on the aerosol type, showing that mainly strongly scattering aerosol dominates. However, the fraction of light-absorbing aerosol increased during the passage of some extra-tropical cyclones or frontal systems, indicating the presence of aged, long-range transported aerosol. The characterisation of the atmospheric aerosol at Princess Elisabeth station will be used in this contribution to compare it with simultaneously measured precipitation observations.

Reduction in biomass burning aerosol light absorption upon humidification: roles of inorganically-induced hygroscopicity, particle collapse, and photoacoustic heat and mass transfer

NASA Astrophysics Data System (ADS)

Lewis, K. A.; Arnott, W. P.; Moosmüller, H.; Chakrabarty, R. K.; Carrico, C. M.; Kreidenweis, S. M.; Day, D. E.; Malm, W. C.; Laskin, A.; Jimenez, J. L.; Ulbrich, I. M.; Huffman, J. A.; Onasch, T. B.; Trimborn, A.; Liu, L.; Mishchenko, M. I.

2009-11-01

Smoke particle emissions from the combustion of biomass fuels typical for the western and southeastern United States were studied and compared under high humidity and ambient conditions in the laboratory. The fuels used were Montana ponderosa pine (Pinus ponderosa), southern California chamise (Adenostoma fasciculatum), and Florida saw palmetto (Serenoa repens). Information on the non-refractory chemical composition of biomass burning aerosol from each fuel was obtained with an aerosol mass spectrometer and through estimation of the black carbon concentration from light absorption measurements at 870 nm. Changes in the optical and physical particle properties under high humidity conditions were observed for hygroscopic smoke particles containing substantial inorganic mass fractions that were emitted from combustion of chamise and palmetto fuels. Light scattering cross sections increased under high humidity for these particles, consistent with the hygroscopic growth measured for 100 nm particles in HTDMA measurements. Photoacoustic measurements of aerosol light absorption coefficients revealed a 20% reduction with increasing relative humidity, contrary to the expectation of light absorption enhancement by the liquid coating taken up by hygroscopic particles. This reduction is hypothesized to arise from two mechanisms: (1) shielding of inner monomers after particle consolidation or collapse with water uptake; (2) the lower case contribution of mass transfer through evaporation and condensation at high relative humidity (RH) to the usual heat transfer pathway for energy release by laser-heated particles in the photoacoustic measurement of aerosol light absorption. The mass transfer contribution is used to evaluate the fraction of aerosol surface covered with liquid water solution as a function of RH.

Relative importance of black carbon, brown carbon, and absorption enhancement from clear coatings in biomass burning emissions

NASA Astrophysics Data System (ADS)

Pokhrel, Rudra P.; Beamesderfer, Eric R.; Wagner, Nick L.; Langridge, Justin M.; Lack, Daniel A.; Jayarathne, Thilina; Stone, Elizabeth A.; Stockwell, Chelsea E.; Yokelson, Robert J.; Murphy, Shane M.

2017-04-01

A wide range of globally significant biomass fuels were burned during the fourth Fire Lab at Missoula Experiment (FLAME-4). A multi-channel photoacoustic absorption spectrometer (PAS) measured dry absorption at 405, 532, and 660 nm and thermally denuded (250 °C) absorption at 405 and 660 nm. Absorption coefficients were broken into contributions from black carbon (BC), brown carbon (BrC), and lensing following three different methodologies, with one extreme being a method that assumes the thermal denuder effectively removes organics and the other extreme being a method based on the assumption that black carbon (BC) has an Ångström exponent of unity. The methodologies employed provide ranges of potential importance of BrC to absorption but, on average, there was a difference of a factor of 2 in the ratio of the fraction of absorption attributable to BrC estimated by the two methods. BrC absorption at shorter visible wavelengths is of equal or greater importance to that of BC, with maximum contributions of up to 92 % of total aerosol absorption at 405 nm and up to 58 % of total absorption at 532 nm. Lensing is estimated to contribute a maximum of 30 % of total absorption, but typically contributes much less than this. Absorption enhancements and the estimated fraction of absorption from BrC show good correlation with the elemental-carbon-to-organic-carbon ratio (EC / OC) of emitted aerosols and weaker correlation with the modified combustion efficiency (MCE). Previous studies have shown that BrC grows darker (larger imaginary refractive index) as the ratio of black to organic aerosol (OA) mass increases. This study is consistent with those findings but also demonstrates that the fraction of total absorption attributable to BrC shows the opposite trend: increasing as the organic fraction of aerosol emissions increases and the EC / OC ratio decreases.

Scattering and absorption characteristics of aerosols at an urban megacity over IGB: Implications to radiative forcing

NASA Astrophysics Data System (ADS)

Srivastava, A. K.; Bisht, D. S.; Singh, Sachchidanand; Kishore, N.; Soni, V. K.; Singh, Siddhartha; Tiwari, S.

2018-06-01

Aerosol scattering and absorption characteristics were investigated at an urban megacity Delhi in the western Indo-Gangetic Basin (IGB) during the period from October 2011 to September 2012 using different in-situ measurements. The scattering coefficient (σsp at 550 nm) varied between 71 and 3014 Mm-1 (mean 710 ± 615 Mm-1) during the entire study period, which was about ten times higher than the absorption coefficient (σabs at 550 nm 67 ± 40 Mm-1). Seasonally, σsp and σabs were substantially higher during the winter/post-monsoon periods, which also gave rise to single scattering albedo (SSA) by 5%. The magnitude of SSA (at 550 nm) varied between 0.81 and 0.94 (mean: 0.89 ± 0.05). Further, the magnitude of scattering Ångström exponent (SAE) and back-scattering Ångström exponent (BAE) showed a wide range from -1.20 to 1.57 and -1.13 to 0.87, respectively which suggests large variability in aerosol sizes and emission sources. Relatively higher aerosol backscatter fraction (b at 550 nm) during the monsoon (0.25 ± 0.10) suggests more inhomogeneous scattering, associated with the coarser dust particles. However, lower value of b during winter (0.13 ± 0.02) is associated with more isotropic scattering due to dominance of smaller size particles. This is further confirmed with the estimated asymmetry parameter (AP at 550 nm), which exhibits opposite trend with b. The aerosol optical parameters were used in a radiative transfer model to estimate aerosol radiative forcing. A mean radiative forcing of -61 ± 22 W m-2 (ranging from -111 to -40 W m-2) was observed at the surface and 42 ± 24 W m-2 (ranging from 18 to 87 W m-2) into the atmosphere, which can give rise to the mean atmospheric heating rate of 1.18 K day-1.

Optical absorption characteristics of brown carbon aerosols during the KORUS-AQ campaign at an urban site

NASA Astrophysics Data System (ADS)

Park, Seungshik; Yu, Geun-Hye; Lee, Sangil

2018-05-01

This study investigates the absorption characteristics of brown carbon (BrC) obtained from water and methanol extracts of fine particulate matter measured at an urban site in Gwangju, Korea during the KOREA U.S. - Air Quality campaign (May 2-June 11, 2016). The measurement period was classified into two intervals: biomass burning (BB) and non-BB periods. During the non-BB period, water-soluble organic carbon (WSOC) and humic-like substances (HULIS) primarily resulted from secondary organic aerosol (SOA) formation and primary vehicle emissions. Water-soluble organic aerosols during the BB period, meanwhile, were closely related to SOA formation and regionally transported BB emissions. The light absorption coefficient measured at 365 nm (babs,365) by methanol extracts was 2.6 and 6.1 times higher than the coefficients from the water and HULIS extracts, respectively, indicating the importance of BrC absorption by water-insoluble organic carbon. This was demonstrated by a good correlation between the water-insoluble BrC absorption and the elemental carbon concentration. A comparison of babs,365 between the methanol- and water-extracted BrC indicated that water-insoluble BrC accounted for approximately 61% (33-86%) of the total BrC absorption. The contributions of SOA, primary BB emissions, and traffic emissions to the water extract babs,365 were estimated using a stepwise multiple linear regression (MLR) analysis and found to be 1.17 ± 0.55, 0.65 ± 0.62, and 0.25 ± 0.09 Mm- 1, respectively, accounting for 59.6, 26.1, and 14.3% of the absorption coefficient by the water-soluble BrC. Further, it was determined that the contribution of the BB emissions to the water-soluble BrC absorption was approximately two times higher in the BB period than in the non-BB period. The average absorption Ångstrӧm exponent was 4.8 ± 0.3, 5.3 ± 0.7, and 6.8 ± 0.8 for the methanol, water, and HULIS extracts, respectively. The average mass absorption efficiency (MAE365) of methanol extracted BrC was 1.3 ± 0.4 m2/g·C. Water- and HULIS-extracted BrC had a MAE365 of 1.0 ± 0.3 and 0.8 ± 0.3 m2/g·C, respectively. These results suggest that methanol-extracted BrC could provide a better estimation of BrC absorption compared to WSOC and HULIS.

Aircraft observations of the physical and radiative properties of biomass aerosol particles during SAFARI-2000.

NASA Astrophysics Data System (ADS)

Osborne, S. R.; Haywood, J. M.

2001-12-01

An initial analysis will be shown from the ~80 h of data collected between 2--18 September 2000 by the UK Met Office C-130 aircraft during the dry season campaign of the Southern African Regional Science Initiative (SAFARI-2000). The talk will concentrate on the physical and optical properties of the biomass aerosol. The evolution of the particle size spectrum and its optical properties at emission and after ageing will be shown. The vertical distribution of the biomass plume over the land and sea will be compared in view of the local meteorology. A generalised three log-normal model is shown to represent aged biomass aerosol over the sea areas, both in terms of the number and mass particle size spectra, but also derived optical properties (e.g. asymmetry factor, single scatter albedo (ω 0) and extinction coefficient) as calculated using Mie theory and appropriate refractive indices. ω 0 was determined independently using a particle soot absorption photometer (giving the absorption coefficient at a wavelength of 0.567 μ m) and a nephelometer (giving the scattering coefficients at 0.45, 0.55 and 0.65 μ m). Good agreement was found between the measurements and those obtained from the Mie calculations and observed size distributions. A typical value of ω 0 at 0.55 μ m for aged biomass aerosol was 0.90. The radiative properties of the biomass aerosol over both land and sea will be summarised. Stratocumulus cloud was present on some of the days over the sea and the surprising lack of interaction between the elevated biomass plume (containing significant levels of cloud condensation nuclei) and the cloud capping the marine boundary layer will be illustrated. Using the cloud-free and cloudy case studies we can begin to elucidate the levels of direct and indirect forcing of the biomass aerosol on a regional scale. >http://www.mrfnet.demon.co.uk/africa/SAFARI2000.htm

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the United Kingdom

NASA Astrophysics Data System (ADS)

McMeeking, G. R.; Morgan, W. T.; Flynn, M.; Highwood, E. J.; Turnbull, K.; Haywood, J.; Coe, H.

2011-09-01

Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the United Kingdom. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA observed in urban plumes compared to regional aerosol (0.85 versus 0.9-0.95). We attribute these differences to the presence of relatively rapidly formed secondary aerosol, primarily OOA and ammonium nitrate, which must be taken into account in radiative forcing calculations.

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the UK

NASA Astrophysics Data System (ADS)

McMeeking, G. R.; Morgan, W. T.; Flynn, M.; Highwood, E. J.; Turnbull, K.; Haywood, J.; Coe, H.

2011-05-01

Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the UK. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA observed in urban plumes compared to regional aerosol (0.85 versus 0.9-0.95). We attribute these differences to the presence of relatively rapidly formed secondary aerosol, primarily OOA and ammonium nitrate, which must be taken into account in radiative forcing calculations.

Field Measurements of Trace Gases and Aerosols Emitted by Undersampled Combustion Sources Including Wood and Dung Cooking Fires, Garbage and Crop Residue Burning, and Indonesian Peat Fires

NASA Astrophysics Data System (ADS)

Stockwell, C.; Jayarathne, T. S.; Goetz, D.; Simpson, I. J.; Selimovic, V.; Bhave, P.; Blake, D. R.; Cochrane, M. A.; Ryan, K. C.; Putra, E. I.; Saharjo, B.; Stone, E. A.; DeCarlo, P. F.; Yokelson, R. J.

2017-12-01

Field measurements were conducted in Nepal and in the Indonesian province of Central Kalimantan to improve characterization of trace gases and aerosols emitted by undersampled combustion sources. The sources targeted included cooking with a variety of stoves, garbage burning, crop residue burning, and authentic peat fires. Trace gas and aerosol emissions were studied using a land-based Fourier transform infrared spectrometer, whole air sampling, photoacoustic extinctiometers (405 and 870nm), and filter samples that were analyzed off-line. These measurements were used to calculate fuel-based emission factors (EFs) for up to 90 gases, PM2.5, and PM2.5 constituents. The aerosol optical data measured included EFs for the scattering and absorption coefficients, the single scattering albedo (at 870 and 405 nm), as well as the absorption Ångström exponent. The emissions varied significantly by source, although light absorption by both brown and black carbon (BrC and BC, respectively) was important for all non-peat sources. For authentic peat combustion, the emissions of BC were negligible and absorption was dominated by organic aerosol. The field results from peat burning were in reasonable agreement with recent lab measurements of smoldering Kalimantan peat and compare well to the limited data available from other field studies. The EFs can be used with estimates of fuel consumption to improve regional emissions inventories and assessments of the climate and health impacts of these undersampled sources.

Atmospheric aerosols in Amazonia and land use change: from natural biogenic to biomass burning conditions.

PubMed

Artaxo, Paulo; Rizzo, Luciana V; Brito, Joel F; Barbosa, Henrique M J; Arana, Andrea; Sena, Elisa T; Cirino, Glauber G; Bastos, Wanderlei; Martin, Scot T; Andreae, Meinrat O

2013-01-01

In the wet season, a large portion of the Amazon region constitutes one of the most pristine continental areas, with very low concentrations of atmospheric trace gases and aerosol particles. However, land use change modifies the biosphere-atmosphere interactions in such a way that key processes that maintain the functioning of Amazonia are substantially altered. This study presents a comparison between aerosol properties observed at a preserved forest site in Central Amazonia (TT34 North of Manaus) and at a heavily biomass burning impacted site in south-western Amazonia (PVH, close to Porto Velho). Amazonian aerosols were characterized in detail, including aerosol size distributions, aerosol light absorption and scattering, optical depth and aerosol inorganic and organic composition, among other properties. The central Amazonia site (TT34) showed low aerosol concentrations (PM2.5 of 1.3 +/- 0.7 microg m(-3) and 3.4 +/- 2.0 microg m(-3) in the wet and dry seasons, respectively), with a median particle number concentration of 220 cm(-3) in the wet season and 2200 cm(-3) in the dry season. At the impacted site (PVH), aerosol loadings were one order of magnitude higher (PM2.5 of 10.2 +/- 9.0 microg m(-3) and 33.0 +/- 36.0 microg m(-3) in the wet and dry seasons, respectively). The aerosol number concentration at the impacted site ranged from 680 cm(-3) in the wet season up to 20 000 cm(-3) in the dry season. An aerosol chemical speciation monitor (ACSM) was deployed in 2013 at both sites, and it shows that organic aerosol account to 81% to the non-refractory PM1 aerosol loading at TT34, while biomass burning aerosols at PVH shows a 93% content of organic particles. Three years of filter-based elemental composition measurements shows that sulphate at the impacted site decreases, on average, from 12% of PM2.5 mass during the wet season to 5% in the dry season. This result corroborates the ACSM finding that the biomass burning contributed overwhelmingly to the organic fine mode aerosol during the dry season in this region. Aerosol light scattering and absorption coefficients at the TT34 site were low during the wet season, increasing by a factor of 5, approximately, in the dry season due to long range transport of biomass burning aerosols reaching the forest site in the dry season. Aerosol single scattering albedo (SSA) ranged from 0.84 in the wet season up to 0.91 in the dry. At the PVH site, aerosol scattering coefficients were 3-5 times higher in comparison to the TT34 site, an indication of strong regional background pollution, even in the wet season. Aerosol absorption coefficients at PVH were about 1.4 times higher than at the forest site. Ground-based SSA at PVH was around 0.92 year round, showing the dominance of scattering aerosol particles over absorption, even for biomass burning aerosols. Remote sensing observations from six AERONET sites and from MODIS since 1999, provide a regional and temporal overview. Aerosol Optical Depth (AOD) at 550 nm of less than 0.1 is characteristic of natural conditions over Amazonia. At the perturbed PVH site, AOD550 values greater than 4 were frequently observed in the dry season. Combined analysis of MODIS and CERES showed that the mean direct radiative forcing of aerosols at the top of the atmosphere (TOA) during the biomass burning season was -5.6 +/- 1.7 W m(-2), averaged over whole Amazon Basin. For high AOD (larger than 1) the maximum daily direct aerosol radiative forcing at the TOA was as high as -20 W m(-2) locally. This change in the radiation balance caused increases in the diffuse radiation flux, with an increase of Net Ecosystem Exchange (NEE) of 18-29% for high AOD. From this analysis, it is clear that land use change in Amazonia shows alterations of many atmospheric properties, and these changes are affecting the functioning of the Amazonian ecosystem in significant ways.

Light absorption and morphological properties of soot-containing aerosols observed at an East Asian outflow site, Noto Peninsula, Japan

NASA Astrophysics Data System (ADS)

Ueda, S.; Nakayama, T.; Taketani, F.; Adachi, K.; Matsuki, A.; Iwamoto, Y.; Sadanaga, Y.; Matsumi, Y.

2015-09-01

The coating of black carbon (BC) with inorganic salts and organic compounds can enhance the magnitude of light absorption by BC. To elucidate the enhancement of light absorption of aged BC particles and its relation to the mixing state and morphology of individual particles, we conducted observations of particles at an Asian outflow site in Noto Peninsula, Japan, in the spring of 2013. Absorption and scattering coefficients at 405, 532, and 781 nm and mass concentrations/mixing states of refractory-BC in PM2.5 were measured using a three-wavelength photoacoustic soot spectrometer and a single-particle soot photometer (SP2), respectively, after passage through a heater maintained at 300 or 400 °C or a bypass line maintained at room temperature (25 °C). The average enhancement of BC light absorption due to coating was estimated by comparing absorption coefficients at 781 nm for particles that with and without passing through the heater and was found to be 22-23 %. The largest enhancements (> 30 %) were observed under high absorption coefficient conditions when the air mass was long-range transported from urban areas in China. Aerosol samples were also analyzed using a transmission electron microscope (TEM) equipped with an energy dispersive X-ray analyzer. The morphological features and mixing states of soot-containing particles of four samples collected during the high absorption coefficient events were analyzed by comparing microphotographs before and after the evaporation of beam-sensitive materials by irradiation with a high density electron beam. The majority of the soot in all samples was found as mixed particles with spherical sulfate or as clusters of sulfate spherules. For samples showing high enhancement (> 30 %) of BC light absorption, TEM showed that the internally mixed soot-containing particles tended to have a more spherical shape and to be embedded into the sulfate. The SP2 measurements also suggested that the proportion of thickly-coated soot was greater. Thus, the observed enhancement of BC light absorption was found to differ according to the mixing states and morphology of soot-containing particles. The enhancement of BC light absorption in our in situ measurements and its relation with individual features of soot-containing particles will be useful to evaluate direct radiative forcing in the leeward areas of large emission sources of BC.

Radiative effects of absorbing aerosols over northeastern India: Observations and model simulations

NASA Astrophysics Data System (ADS)

Gogoi, Mukunda M.; Babu, S. Suresh; Moorthy, K. Krishna; Bhuyan, Pradip Kumar; Pathak, Binita; Subba, Tamanna; Chutia, Lakhima; Kundu, Shyam Sundar; Bharali, Chandrakala; Borgohain, Arup; Guha, Anirban; De, Barin Kumar; Singh, Brajamani; Chin, Mian

2017-01-01

Multiyear measurements of spectral properties of aerosol absorption are examined over four geographically distinct locations of northeastern India. Results indicated significant spatiotemporal variation in aerosol absorption coefficients (σabs) with highest values in winter and lowest in monsoon. The western parts of the region, close to the outflow of Indo-Gangetic Plains, showed higher values of σabs and black carbon (BC) concentration—mostly associated with fossil fuel combustion. But, the eastern parts showed higher contributions from biomass-burning aerosols, as much as 20-25% to the total aerosol absorption, conspicuously during premonsoon season. This is attributed to a large number of burning activities over the Southeast Asian region, as depicted from Moderate Resolution Imaging Spectroradiometer fire count maps, whose spatial extent and magnitude peaks during March/April. The nearly consistent high values of aerosol index (AI) and layer height from Ozone Monitoring Instrument indicate the presence of absorbing aerosols in the upper atmosphere. The observed seasonality has been captured fairly well by Goddard Chemistry Aerosol Radiation and Transport (GOCART) as well as Weather Research and Forecasting-Chemistry (WRF-Chem) model simulations. The ratio of column-integrated optical depths due to particulate organic matter and BC from GOCART showed good coincidence with satellite-based observations, indicating the increased vertical dispersion of absorbing aerosols, probably by the additional local convection due to higher fire radiative power caused by the intense biomass-burning activities. In the WRF-Chem though underperformed by different magnitude in winter, the values are closer or overestimated near the burnt areas. Atmospheric forcing due to BC was highest ( 30 Wm-2) over the western part associated with the fossil fuel combustion.

Urban impacts on regional carbonaceous aerosols: case study in central Texas.

PubMed

Barrett, Tate E; Sheesley, Rebecca J

2014-08-01

Rural and background sites provide valuable information on the concentration and optical properties of organic, elemental, and water-soluble organic carbon (OC, EC, and WSOC), which are relevant for understanding the climate forcing potential of regional atmospheric aerosols. To quantify climate- and air quality-relevant characteristics of carbonaceous aerosol in the central United States, a regional background site in central Texas was chosen for long-term measurement. Back trajectory (BT) analysis, ambient OC, EC, and WSOC concentrations and absorption parameters are reported for the first 15 months of a long-term campaign (May 2011-August 2012). BT analysis indicates consistent north-south airflow connecting central Texas to the Central Plains. Central Texas aerosols exhibited seasonal trends with increased fine particulate matter (< 2.5 microm aerodynamic diameter, PM2.5) and OC during the summer (PM2.5 = 10.9 microg m(-3) and OC = 3.0 microg m(-3)) and elevated EC during the winter (0.22 microg m(-3)). When compared to measurements in Dallas and Houston, TX, central Texas OC appears to have mixed urban and rural sources. However central Texas EC appears to be dominated by transport of urban emissions. WSOC averaged 63% of the annual OC, with little seasonal variability in this ratio. To monitor brown carbon (BrC), absorption was measured for the aqueous WSOC extracts. Light absorption coefficients for EC and BrC were highest during summer (EC MAC = 11 m2 g(-1) and BRC MAE365 = 0.15 m2 g(-1)). Results from optical analysis indicate that regional aerosol absorption is mostly due to EC with summertime peaks in BrC attenuation. This study represents the first reported values of WSOC absorption, MAE365, for the central United States. Implications: Background concentration and absorption measurements are essential in determining regional potential radiative forcing due to atmospheric aerosols. Back trajectory, chemical, and optical analysis of PM2.5 was used to determine climatic and air quality implications of urban outflow to a regional receptor site, representative of the central United States. Results indicate that central Texas organic carbon has mixed urban and rural sources, while elemental carbon is controlled by the transport of urban emissions. Analysis of aerosol absorption showed black carbon as the dominant absorber, with less brown carbon absorption than regional studies in California and the southeastern United States.

Characterizing the Vertical Profile of Aerosol Particle Extinction and Linear Depolarization over Southeast Asia and the Maritime Continent: The 2007-2009 View from CALIOP

NASA Technical Reports Server (NTRS)

Campbell, James R.; Reid, Jeffrey S.; Westphal, Douglas L.; Zhang, Jianglong; Tackett, Jason L.; Chew, Boon Ning; Welton, Ellsworth J.; Shimizu, Atsushi; Sugimoto, Nobuo; Aoki, Kazuma;

Evaluation of Air Pollution Applications of AERONET and MODIS Aerosol Column Optical Depth by Comparison with In Situ Measurements of Aerosol Light Scattering and Absorption for Reno, NV, USA

NASA Astrophysics Data System (ADS)

Loria Salazar, S.; Arnott, W. P.; Moosmuller, H.; Colucci, D.

2012-12-01

Reno, Nevada, USA is subject to typical urban aerosol, wind-blown dust, and occasional biomass burning smoke from anthropogenic and natural fires. Reno has complex air flow at levels relevant for aerosol transport. At times recirculating mountain and urban flow arrives from the Sierra Nevada, San Francisco, CA and Sacramento, CA. The urban plumes are further modified by biogenic forest emissions and secondary aerosol formation during transport over the Sierra Nevada Mountains to Reno. This complicates the use of MODIS aerosol optical depth (AOD) for air quality measurements in Reno. Our laboratory at the University of Nevada Reno has collocated multispectral photoacoustic instruments and reciprocal nephelometers to measure light absorption and light scattering coefficients as well as an AERONET operated CIMEL CE-318 ground-based sunphotometer. Preliminary measurements from August 2011 indicate substantially larger Cimel AOD than could be accounted for by use of the in situ aerosol extinction measurements combined with mixing height estimate. This poster presents new results comparing AERONET AOD and single scattering albedo and MODIS AOD with in situ measurements for summer and fall 2012, along with extensive back trajectory analysis, to evaluate conditions when satellite measurement may be useful for air pollution applications in Reno.

Assessing the aerosol direct and first indirect effects using ACM/GCM simulation results

NASA Astrophysics Data System (ADS)

Huang, H.; Gu, Y.; Xue, Y.; Lu, C. H.

2016-12-01

Atmospheric aerosols have been found to play an important role in global climate change but there are still large uncertainty in evaluating its role in the climate system. The aerosols generally affect global and regional climate through the scattering and the absorption of solar radiation (direct effect) and through their influences on cloud particle, number and sizes (first indirect effect). The indirect effect will further affects cloud water content, cloud top albedo and surface precipitations. In this study, we investigate the global climatic effect of aerosols using a coupled NCEP Global Forecast System (GFS) and a land surface model (SSiB2) The OPAC (Optical Properties of Aerosols and Clouds) database is used for aerosol effect. The OPAC data provides the optical properties (i.e., the extinction, scattering and absorption coefficient, single-scattering albedo, asymmetry factor and phase function) of ten types of aerosols under various relative humidity conditions for investigating the global direct and first indirect effects of dust aerosols. For indirect forcings due to liquid water, we follow the approach presented by Jiang et al (2011), in which a parameterization of cloud effective radius was calculated to describe its variance with convective strength and aerosol concentration. Since the oceans also play an important role on aerosol climatic effect, we also design a set of simulations using a coupled atmosphere/ocean model (CFS) to evaluate the sensitivity of aerosol effect with two-way atmosphere-ocean interactions.

Campaign datasets for Biomass Burning Observation Project (BBOP)

DOE Data Explorer

Kleinman,Larry; Mei,Fan; Arnott,William; Buseck,Peter; Chand,Duli; Comstock,Jennifer; Dubey,Manvendra; Lawson,Paul; Long,Chuck; Onasch,Timothy; Sedlacek,Arthur; Senum,Gunnar; Shilling,John; Springston,Stephen; Tomlinson,Jason; Wang,Jian

2014-04-24

This field campaign will address multiple uncertainties in aerosol intensive properties, which are poorly represented in climate models, by means of aircraft measurements in biomass burning plumes. Key topics to be investigated are: 1. Aerosol mixing state and morphology 2. Mass absorption coefficients (MACs) 3. Chemical composition of non-refractory material associated with light-absorbing carbon (LAC) 4. Production rate of secondary organic aerosol (SOA) 5. Microphysical processes relevant to determining aerosol size distributions and single scattering albedo (SSA) 6. CCN activity. These topics will be investigated through measurements near active fires (0-5 hours downwind), where limited observations indicate rapid changes in aerosol properties, and in biomass burning plumes aged >5 hours. Aerosol properties and their time evolution will be determined as a function of fire type, defined according to fuel and the mix of flaming and smoldering combustion at the source.

The Global Ozone and Aerosol Profiles and Aerosol Hygroscopic Effect and Absorption Optical Depth (GOA2HEAD) Network Initiative

NASA Astrophysics Data System (ADS)

Gao, R. S.; Elkins, J. W.; Frost, G. J.; McComiskey, A. C.; Murphy, D. M.; Ogren, J. A.; Petropavlovskikh, I. V.; Rosenlof, K. H.

2014-12-01

Inverse modeling using measurements of ozone (O3) and aerosol is a powerful tool for deriving pollutant emissions. Because they have relatively long lifetimes, O3 and aerosol are transported over large distances. Frequent and globally spaced vertical profiles rather than ground-based measurements alone are therefore highly desired. Three requirements necessary for a successful global monitoring program are: Low equipment cost, low operation cost, and reliable measurements of known uncertainty. Conventional profiling using aircraft provides excellent data, but is cost prohibitive on a large scale. Here we describe a new platform and instruments meeting all three global monitoring requirements. The platform consists of a small balloon and an auto-homing glider. The glider is released from the balloon at about 5 km altitude, returning the light instrument package to the launch location, and allowing for consistent recovery of the payload. Atmospheric profiling can be performed either during ascent or descent (or both) depending on measurement requirements. We will present the specifications for two instrument packages currently under development. The first measures O3, RH, p, T, dry aerosol particle number and size distribution, and aerosol optical depth. The second measures dry aerosol particle number and size distribution, and aerosol absorption coefficient. Other potential instrument packages and the desired spatial/temporal resolution for the GOA2HEAD monitoring initiative will also be discussed.

Aerosol Light Absorption and Scattering Assessments and the Impact of City Size on Air Pollution

NASA Astrophysics Data System (ADS)

Paredes-Miranda, Guadalupe

The general problem of urban pollution and its relation to the city population is examined in this dissertation. A simple model suggests that pollutant concentrations should scale approximately with the square root of city population. This model and its experimental evaluation presented here serve as important guidelines for urban planning and attainment of air quality standards including the limits that air pollution places on city population. The model was evaluated using measurements of air pollution. Optical properties of aerosol pollutants such as light absorption and scattering plus chemical species mass concentrations were measured with a photoacoustic spectrometer, a reciprocal nephelometer, and an aerosol mass spectrometer in Mexico City in the context of the multinational project "Megacity Initiative: Local And Global Research Observations (MILAGRO)" in March 2006. Aerosol light absorption and scattering measurements were also obtained for Reno and Las Vegas, NV USA in December 2008-March 2009 and January-February 2003, respectively. In all three cities, the morning scattering peak occurs a few hours later than the absorption peak due to the formation of secondary photochemically produced aerosols. In particular, for Mexico City we determined the fraction of photochemically generated secondary aerosols to be about 75% of total aerosol mass concentration at its peak near midday. The simple 2-d box model suggests that commonly emitted primary air pollutant (e.g., black carbon) mass concentrations scale approximately as the square root of the urban population. This argument extends to the absorption coefficient, as it is approximately proportional to the black carbon mass concentration. Since urban secondary pollutants form through photochemical reactions involving primary precursors, in linear approximation their mass concentration also should scale with the square root of population. Therefore, the scattering coefficient, a proxy for particulate matter mass concentration, is also expected to scale the same way. Experimental data for five cities: Mexico City, Mexico; Las Vegas and Reno, NV, USA; Beijing, China; and Delhi, India (the data for the last two cities were obtained from the literature); are in reasonable accord with the model. The scaling relation provided by the model may be considered a useful metric depending on the assumption that specific city conditions (such as latitude, altitude, local meteorological conditions, degree of industrialization, population density, number of cars per capita, city shape, etc.) vary randomly, independent of city size. While more detailed studies (including data from more cities) are needed, we believe that this relatively weak dependence of the pollution concentration on the city population might help to explain why the worsening of urban air quality does not directly lead to a decrease in the rate of growth in city population.

Deriving brown carbon from multiwavelength absorption measurements: Method and application to AERONET and Aethalometer observations

DOE PAGES

Wang, X.; Heald, C. L.; Sedlacek, A.; ...

2016-10-13

The radiative impact of organic aerosols (OA) is a large source of uncertainty in estimating the global direct radiative effect (DRE) of aerosols. This radiative impact includes not only light scattering but also light absorption from a subclass of OA referred to as brown carbon (BrC). However the absorption properties of BrC are poorly understood leading to large uncertainties in modelling studies. To obtain observational constraints from measurements, a simple Absorption Ångström Exponent (AAE) method is often used to separate the contribution of BrC absorption from that of black carbon (BC). However, this attribution method is based on assumptions regardingmore » the spectral dependence of BC that are often violated in the ambient atmosphere. Here we develop a new method that decreases the uncertainties associated with estimating BrC absorption. By applying this method to multi-wavelength absorption aerosol optical depth (AAOD) measurements at AERONET sites worldwide and surface aerosol absorption measurements at multiple ambient sites, we estimate that BrC globally contributes 6-40% of the absorption at 440nm. We find that the mass absorption coefficient of OA (OA-MAC) is positively correlated with BC/OA mass ratio. Based on the variability of BC properties and BC/OA emission ratio, we estimate a range of 0.05-1.2 m 2/g for OA-MAC at 440nm. Using the combination of AERONET and OMI UV absorption observations we estimate that the AAE 388/440nm for BrC is generally ~4 world-wide, with a smaller value in Europe (< 2). Our analyses of two surface sites (Cape Cod, to the southeast of Boston, and the GoAmazon2014/5 T3 site, to the west of Manaus, Brazil) reveal no significant relationship between BrC absorptivity and photochemical aging in typical urban influenced conditions. However, the absorption of BrC measured during the biomass burning season near Manaus is found to decrease with photochemical aging with a lifetime of ~1 day. This lifetime is comparable to previous observations within a biomass burning plume but much slower than estimated from laboratory studies.« less

Aerosol optical properties measurements by a CAPS single scattering albedo monitor: Comparisons between summer and winter in Beijing, China

NASA Astrophysics Data System (ADS)

Han, Tingting; Xu, Weiqi; Li, Jie; Freedman, Andrew; Zhao, Jian; Wang, Qingqing; Chen, Chen; Zhang, Yingjie; Wang, Zifa; Fu, Pingqing; Liu, Xingang; Sun, Yele

2017-02-01

Aerosol optical properties were measured in Beijing in summer and winter using a state-of-the-art cavity attenuated phase shift single scattering albedo monitor (CAPS PMssa) along with aerosol composition measurements by aerosol mass spectrometers and aethalometers. The SSA directly measured by the CAPS PMssa showed overall agreements with those derived from colocated measurements. However, substantial differences were observed during periods with low SSA values in both summer and winter, suggesting that interpretation of low SSA values needs to be cautious. The average (±σ) extinction coefficient (bext) and absorption coefficient (bap) were 336 (±343) Mm-1 and 44 (±41) Mm-1, respectively, during wintertime, which were approximately twice those observed in summer, while the average SSA was relatively similar, 0.86 (±0.06) and 0.85 (±0.04) in summer and winter, respectively. Further analysis showed that the variations in SSA can be approximately parameterized as a function of mass fraction of secondary particulate matter (fSPM), which is SSA = 0.74 + 0.19 × fSPM (fSPM > 0.3, r2 = 0.85). The contributions of aerosol species to extinction coefficients during the two seasons were also estimated. Our results showed that the light extinction was dominantly contributed by ammonium sulfate (30%) and secondary organic aerosol (22%) in summer, while organic aerosol was the largest contributor (51%) in winter. Consistently, SPM played the major role in visibility degradation in both seasons by contributing 70% of the total extinction.

The Global Atmosphere Watch Aerosol Programme

NASA Astrophysics Data System (ADS)

Baltensperger, U.

2003-04-01

The Global Atmosphere Watch (GAW) programme is a WMO sponsored activity and currently supported by about 80 WMO member countries. It is the goal of GAW to develop and maintain long-term measurements of atmospheric constituents in order to detect trends, develop aerosol predictive capabilities and understand proc- esses. With respect to aerosols, the objective of GAW is to support a global network determining the spatio-temporal distribution of aerosol properties related to climate forcing and air quality up to multi-decadal time scales. The GAW network consists of 22 Global stations and some 300 Regional stations. The Scientific Advisory Group (SAG) for Aerosols will soon publish their recommendations for aerosol measurements. Each site should have an acceptable aerosol sampling inlet. Regional stations measure aerosol optical depth, as well as the aerosol light scattering and absorption coefficient. If possible these should be complemented by routine mass concentration and composition measurements in two aerosol size fractions. At Global stations, a larger number of measurements are desirable. These include the Regional parameters list above as well as the light scattering, hemispheric backscat- tering, and absorption coefficients at various wavelengths, aerosol number concen- tration, cloud condensation nuclei (CCN) concentration at 0.5% supersaturation, and diffuse, global and direct solar radiation. Additional parameters such as the aerosol size distribution, detailed size fractionated chemical composition, dependence of aerosol properties on relative humidity, CCN concentration at various supersatura- tions, and the vertical distribution of aerosol properties should be measured intermit- tently at Global stations. Examples from the Jungfraujoch (Swiss Alps, 3580 m asl) will be given, where many of the parameters listed above are measured. Data are delivered to and made available by the World Data Centre for Aerosols (WDCA, located in Ispra, Italy http://ies.jrc.cec.eu.int/wdca/) using the NARSTO data exchange standard. The Institute for Tropospheric Research in Leipzig hosts a GAW World Calibration Centre (WCC) for physical aerosol parameters. A host for the chemical parameters still must be located. None of the Global sites perform a full set of measurements, and many Regional sites have not yet started with aerosol ac- tivities at all. Capacity building and fund raising are therefore important priorities in order to achieve the goals of the GAW global aerosol programme. It should be em- phasized that GAW works with many partners in the World Meteorological Organi- zation as well as other agencies in an attempt to develop an integrated system of satellite and non-satellite observations of the global aerosol.

Physical and optical properties of aged biomass burning aerosol from wildfires in Siberia and the Western USA at the Mt. Bachelor Observatory

NASA Astrophysics Data System (ADS)

Laing, James R.; Jaffe, Daniel A.; Hee, Jonathan R.

2016-12-01

The summer of 2015 was an extreme forest fire year in the Pacific Northwest. Our sample site at the Mt. Bachelor Observatory (MBO, 2.7 km a.s.l.) in central Oregon observed biomass burning (BB) events more than 50 % of the time during August. In this paper we characterize the aerosol physical and optical properties of 19 aged BB events during August 2015. Six of the 19 events were influenced by Siberian fires originating near Lake Baikal that were transported to MBO over 4-10 days. The remainder of the events resulted from wildfires in Northern California and Southwestern Oregon with transport times to MBO ranging from 3 to 35 h. Fine particulate matter (PM1), carbon monoxide (CO), aerosol light scattering coefficients (σscat), aerosol light absorption coefficients (σabs), and aerosol number size distributions were measured throughout the campaign. We found that the Siberian events had a significantly higher Δσabs/ΔCO enhancement ratio, higher mass absorption efficiency (MAE; Δσabs/ΔPM1), lower single scattering albedo (ω), and lower absorption Ångström exponent (AAE) when compared with the regional events. We suggest that the observed Siberian events represent that portion of the plume that has hotter flaming fire conditions and thus enabled strong pyroconvective lofting and long-range transport to MBO. The Siberian events observed at MBO therefore represent a selected portion of the original plume that would then have preferentially higher black carbon emissions and thus an enhancement in absorption. The lower AAE values in the Siberian events compared to regional events indicate a lack of brown carbon (BrC) production by the Siberian fires or a loss of BrC during transport. We found that mass scattering efficiencies (MSE) for the BB events ranged from 2.50 to 4.76 m2 g-1. We measured aerosol size distributions with a scanning mobility particle sizer (SMPS). Number size distributions ranged from unimodal to bimodal and had geometric mean diameters (Dpm) ranging from 138 to 229 nm and geometric standard deviations (σg) ranging from 1.53 to 1.89. We found MSEs for BB events to be positively correlated with the geometric mean of the aerosol size distributions (R2 = 0.73), which agrees with Mie theory. We did not find any dependence on event size distribution to transport time or fire source location.

Vertical profiles of aerosol absorption coefficient from micro-Aethalometer data and Mie calculation over Milan.

PubMed

Ferrero, L; Mocnik, G; Ferrini, B S; Perrone, M G; Sangiorgi, G; Bolzacchini, E

2011-06-15

Vertical profiles of aerosol number-size distribution and black carbon (BC) concentration were measured between ground-level and 500m AGL over Milan. A tethered balloon was fitted with an instrumentation package consisting of the newly-developed micro-Aethalometer (microAeth® Model AE51, Magee Scientific, USA), an optical particle counter, and a portable meteorological station. At the same time, PM(2.5) samples were collected both at ground-level and at a high altitude sampling site, enabling particle chemical composition to be determined. Vertical profiles and PM(2.5) data were collected both within and above the mixing layer. Absorption coefficient (b(abs)) profiles were calculated from the Aethalometer data: in order to do so, an optical enhancement factor (C), accounting for multiple light-scattering within the filter of the new microAeth® Model AE51, was determined for the first time. The value of this parameter C (2.05±0.03 at λ=880nm) was calculated by comparing the Aethalometer attenuation coefficient and aerosol optical properties determined from OPC data along vertical profiles. Mie calculations were applied to the OPC number-size distribution data, and the aerosol refractive index was calculated using the effective medium approximation applied to aerosol chemical composition. The results compare well with AERONET data. The BC and b(abs) profiles showed a sharp decrease at the mixing height (MH), and fairly constant values of b(abs) and BC were found above the MH, representing 17±2% of those values measured within the mixing layer. The BC fraction of aerosol volume was found to be lower above the MH: 48±8% of the corresponding ground-level values. A statistical mean profile was calculated, both for BC and b(abs), to better describe their behaviour; the model enabled us to compute their average behaviour as a function of height, thus laying the foundations for valid parametrizations of vertical profile data which can be useful in both remote sensing and climatic studies. Copyright © 2011 Elsevier B.V. All rights reserved.

OM/OC Ratio and Specific Attenuation Coefficient in Ambient Particulate Matter at a Rural Site in Southern Ontario: Implications for Aerosol Aging and Emission Sources

NASA Astrophysics Data System (ADS)

Chan, T. W.; Huang, L.; Leaitch, R.; Sharma, S.; Brook, J.; Slowik, J.; Abbatt, J.

2008-05-01

Carbonaceous species (organic carbon (OC) and elemental carbon (EC)) contribute a large portion of atmospheric fine particle mass and influence air quality, human health, and climate forcing. However, their emission sources and atmospheric aging processes are not well understood. The OM/OC ratio, defined as the organic mass per unit OC mass, is useful to understand the degree of oxidation of aerosol particles in atmospheric processes. We define the modified BC/EC (mod BC/EC) ratio as the ratio of the non-scattering corrected absorption coefficient per unit mass of EC. The mod BC/EC ratio has a similar meaning as the site specific attenuation coefficient, which is an important parameter used to convert light absorption measurements to black carbon mass. The mod BC/EC ratio can vary due to light scattering effect on absorption measurements, in which the oxygenated organics may play a role. The pyrolysis organic carbon (POC) is defined as the carbon mass fraction obtained at T= 870°C under a pure helium environment using the thermal separation method [Huang et al., 2006]. Since POC mass is generally proportional to the amount of oxygenated OC, studying the relationships among OC, EC, POC, as well as OM/OC and mod BC/EC ratios may help us understand the mechanisms of aerosol aging from different emission sources. Two 1-month field studies were conducted at a rural site in southern Ontario (NW of Toronto) during fall 2005 and spring 2007. Quartz filter samples were collected and analyzed for OC, POC, and EC concentrations using a thermal/optical method [Huang et al., 2006]. Together with the total organic matter measured by an Aerodyne Aerosol Mass Spectrometer (AMS) and the absorption coefficient obtained from a Particle Soot Absorption Photometer (PSAP), the OM/OC and mod BC/EC ratios for ambient aerosols were obtained. Our results show that when air mass was mainly from south, OC, POC, and EC were relatively high, with average ratios of OC/EC, OM/OC, and POC/EC as 1.94, 1.41, and 0.52, respectively; this indicates significant anthropogenic impacts and relatively large portion of oxygenated OC, which might be due to either primary emissions or photo-chemical reactions occurred in a short period of time. When air mass was mainly from north, OC, POC, and EC were much lower, with average ratios of OC/EC, OM/OC, and POC/EC as 3.10, 1.20, and 0.79, respectively; this suggests less influence from anthropogenic emissions and relatively aged air mass from biogenic-source dominated clean air. Using POC, we estimate the specific attenuation at the site to be 5.8 m2 g-1 independent of the air mass origin. The relationships among OM/OC, mod BC/EC, and POC will be further discussed. References: Huang, L., Brook, J.R., Zhang, W., Li, S.M., Graham, L., Ernst, D., Chivulescu, A., and Lu, G. (2006) Stable isotope measurements of carbon fractions (OC/EC) in airborne particulate: a new dimension for source characterization and apportionment, Atmospheric Environment, 40, 2690-2705.

Absorption and scattering properties of organic carbon vs. sulfate dominant aerosols at Gosan climate observatory in Northeast Asia

NASA Astrophysics Data System (ADS)

Lim, S.; Lee, M.; Kim, S.-W.; Yoon, S.-C.; Lee, G.; Lee, Y.

2013-12-01

Carbonaceous and soluble ionic species of PM1.0 and PM10 were measured along with the absorption and scattering properties and aerosol number size distributions at Gosan climate observatory (GCO) from January to September 2008. The daily averaged equivalent black carbon (EBC) measured as aerosol absorption exhibited two types of spectral dependence with a distinct maximum (peak) at either 370 nm or 880 nm, by which two subsets were extracted and classified into the respective groups (370 nm and 880 nm). The 370 nm group was distinguished by high organic carbon (OC) concentrations relative to elemental carbon (EC) and sulfate, but sulfate was predominant for the 880 nm group. The PM1.0 OC of the 370 nm group was mainly composed of refractory and pyrolized components that correlated well with PM1.0 EC1, referred to as char EC, which suggests biofuel and biomass combustion as the source of these OC fractions, particularly during winter. The scanning electron microscope (SEM) images and the number size distributions implied that aerosols of the 370 nm group were externally mixed upon transport in fast-moving air masses that passed through the Beijing area in about one day. In contrast, the aerosols of the 880 nm group were characterized by high sulfate concentrations, and seemed to be internally mixed during slow transport over the Yellow Sea region over approximately two to four days. The absorption and scattering coefficients of the 880 nm group were noticeably higher compared to those of the 370 nm group. The average absorption ångström exponent (AAE) was estimated to be 1.29 and 1.0 for the 370 nm and 880 nm groups, respectively, in the range 370-950 nm. These results demonstrated that the optical properties of aerosols were intimately linked to chemical composition and mixing state, characteristics determined both by source and atmospheric aging processes. In OC dominant aerosols, absorption was enhanced in the UV region, which was possibly due to refractory and pyrolized OC compounds. Under sulfate dominant conditions, the sulfate coating on BC particles contributed to the absorption of the longer visible light. Consequently, single scattering albedo (SSA) was higher for the 880 nm group than for the 370 nm group, emphasizing that the relative abundances of absorbing and scattering constituents are also important in estimating the climate effect of aerosols.

Absorption and scattering properties of organic carbon versus sulfate dominant aerosols at Gosan climate observatory in Northeast Asia

NASA Astrophysics Data System (ADS)

Lim, S.; Lee, M.; Kim, S.-W.; Yoon, S.-C.; Lee, G.; Lee, Y. J.

2014-08-01

Carbonaceous and soluble ionic species of PM1.0 and PM10 were measured along with the absorption and scattering properties and aerosol number size distributions at Gosan Climate Observatory (GCO) from January to September 2008. The daily averaged equivalent black carbon (EBC) measured as aerosol absorption exhibited two types of spectral dependence with a distinct maximum (peak) at either 370 nm or 880 nm, by which two subsets were extracted and classified into the respective groups (370 and 880 nm). The 370 nm group was distinguished by high organic carbon (OC) concentrations relative to elemental carbon (EC) and sulfate, but sulfate was predominant for the 880 nm group. The PM1.0 OC of the 370 nm group was mainly composed of refractory and pyrolized components that correlated well with PM1.0 EC1, referred to as char EC, which suggests biofuel and biomass combustion as the source of these OC fractions, particularly during winter. The scanning electron microscope (SEM) images and the number size distributions implied that aerosols of the 370 nm group were externally mixed upon transport in fast-moving air masses that passed through the Beijing area in about one day. In contrast, the aerosols of the 880 nm group were characterized by high sulfate concentrations, and seemed to be internally mixed during slow transport over the Yellow Sea region over approximately 2 to 4 days. The absorption and scattering coefficients of the 880 nm group were noticeably higher compared to those of the 370 nm group. The average absorption ångström exponent (AAE) was estimated to be 1.29 and 1.0 for the 370 and 880 nm groups, respectively, in the range 370-950 nm. These results demonstrated that the optical properties of aerosols were intimately linked to chemical composition and mixing state, characteristics determined both by source and atmospheric aging processes. In OC dominant aerosols, absorption was enhanced in the UV region, which was possibly due to refractory and pyrolized OC compounds. Under sulfate dominant conditions, the sulfate coating on BC particles likely contributed to the absorption of the longer visible light. Consequently, single scattering albedo (SSA) was higher for the 880 nm group than for the 370 nm group, emphasizing that the relative abundances of absorbing and scattering constituents are also important in estimating the climate effect of aerosols.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, X.; Heald, C. L.; Sedlacek, A.

The radiative impact of organic aerosols (OA) is a large source of uncertainty in estimating the global direct radiative effect (DRE) of aerosols. This radiative impact includes not only light scattering but also light absorption from a subclass of OA referred to as brown carbon (BrC). However the absorption properties of BrC are poorly understood leading to large uncertainties in modelling studies. To obtain observational constraints from measurements, a simple Absorption Ångström Exponent (AAE) method is often used to separate the contribution of BrC absorption from that of black carbon (BC). However, this attribution method is based on assumptions regardingmore » the spectral dependence of BC that are often violated in the ambient atmosphere. Here we develop a new method that decreases the uncertainties associated with estimating BrC absorption. By applying this method to multi-wavelength absorption aerosol optical depth (AAOD) measurements at AERONET sites worldwide and surface aerosol absorption measurements at multiple ambient sites, we estimate that BrC globally contributes 6-40% of the absorption at 440nm. We find that the mass absorption coefficient of OA (OA-MAC) is positively correlated with BC/OA mass ratio. Based on the variability of BC properties and BC/OA emission ratio, we estimate a range of 0.05-1.2 m 2/g for OA-MAC at 440nm. Using the combination of AERONET and OMI UV absorption observations we estimate that the AAE 388/440nm for BrC is generally ~4 world-wide, with a smaller value in Europe (< 2). Our analyses of two surface sites (Cape Cod, to the southeast of Boston, and the GoAmazon2014/5 T3 site, to the west of Manaus, Brazil) reveal no significant relationship between BrC absorptivity and photochemical aging in typical urban influenced conditions. However, the absorption of BrC measured during the biomass burning season near Manaus is found to decrease with photochemical aging with a lifetime of ~1 day. This lifetime is comparable to previous observations within a biomass burning plume but much slower than estimated from laboratory studies.« less

Radiocarbon-based Source Apportionment of Organic, Elemental and Water-soluble Organic Carbon Aerosols and the Light Absorption of Water-soluble Organic Carbon Aerosols in the East Asia High-intensity Winter Campaigns in 2014

NASA Astrophysics Data System (ADS)

Fang, W.; Andersson, A.; Zheng, M.; Lee, M.; Kim, S. W.; Du, K.; Gustafsson, O.

2016-12-01

Improved understanding of anthropogenic aerosol effects on atmospheric chemistry and climate as well as efficient mitigation actions are hampered by the limited comprehension of the relative contributions of different sources of carbonaceous aerosols and of their subsequent atmospheric processing. Here, we present dual carbon isotope constrained source apportionment and optical properties of carbonaceous aerosols simultaneously both at urban and rural receptor sites, includes North China Plain (NCP, Beijing and Tianjin), Yangtze River Delta (YRD, Shanghai, Zhejiang), and Jeju Island (Korea Climate Observatory at Gosan) during January 2014 field campaigns. The radiocarbon (Δ14C) data show that fossil combustions contribute equally ˜80 ± 5% to elemental carbon (EC) aerosol in Beijing, Tianjin, and Shanghai, and 66 ± 9% to Gosan-EC aerosol, while the specific sources of the dominant fossil fuel component were dramatically different among these sites. The mean fraction coal combustion of Beijing-EC, Tianjin-EC, and Gosan-EC is double that of Shanghai-EC. The other large fraction (72―92%) of carbonaceous aerosol is organic carbon (OC) aerosol which contains water soluble and water insoluble organic carbon (WSOC and WISOC). OC, WISOC, and WSOC in Beijing and Gosan sites were still observed largely from fossil sources (53―75%). The more 13C-enriched signature of Gosan-WSOC (-22.8 ± 0.2‰) compared to Gosan-EC (-23.9 ± 0.4‰) and Beijing-WSOC (-23.5 ± 0.7‰) reflects that WSOC is likely more affected by atmospheric aging during long-rang transport than is EC. The high light absorption coefficients of PM2.5, PM1, and TSP were observed at Gosan during this study and was frequently reaching 20―60 Mm-1 by aethalometer and continuous light absorption photometer. The mass absorption cross section of WSOC (MAC365) for above sites is high (1.5 ± 0.8 m2/g), accounted for ˜14 ± 5% of the total direct absorbance relative to EC, which is significantly higher than the previous findings in S. Asia, N. America, and Europe.

Measurements of aerosol absorption and scattering in the Mexico City Metropolitan Area during the MILAGRO field campaign: a comparison of results from the T0 and T1 sites

NASA Astrophysics Data System (ADS)

Marley, N. A.; Gaffney, J. S.; Castro, T.; Salcido, A.; Frederick, J.

2008-07-01

Measurements of aerosol absorption and scattering were obtained in Mexico City during the MILAGRO (Megacity Initiative: Local and Global Research Observations) field campaign in March 2006. A comparison of aerosol absorption and scattering was obtained in Mexico City at site T0 located in the northern part of Mexico City at the Instituto Mexicano del Petróleo Laboratories and at site T1 located at the Universidad Tecnológica de Tecamac, 18 miles northwest of T0. Hourly averages of aerosol absorption were similar at both sites, ranging from 6 93 Mm-1 with an average of 31 Mm-1 at T0; and from 2 104 Mm-1 with an average of 19 Mm-1 at T1. Aerosol scattering at T0 ranged from 16 344 Mm-1 with an average of 105 Mm-1; while the scattering values at T1 were lower than T0 ranging from 2 136 with an average of 53 Mm-1. Aerosol single scattering albedos (SSAs) were determined at both sites using these data. SSAs at T1 ranged from 0.44 0.90 with an average 0.75 as compared to hose at T0, range 0.51 0.93 with an average of 0.77. Broadband UV-B intensity was found to be higher at site T0, with an average of 64 μW/cm2 at solar noon, than at site T1, which had an average of 54 μW/cm2 at solar noon. Comparisons of clear-sky modeled UV-B intensities with the simultaneous UV-B measurements obtained at site T0 and at site T1 for cloudless days indicate a larger diffuse radiation field at site T0 than at site T1. The determination of aerosol scattering Ångstrom coefficient at T0 suggests the larger diffuse radiation is due to the predominance of submicron aerosols at T0 with aerosol scattering of UV-B radiation peaked in the forward direction, leading to the enhancement observed at ground level.

Light-absorbing oligomer formation in secondary organic aerosol from reactive uptake of isoprene epoxydiols.

PubMed

Lin, Ying-Hsuan; Budisulistiorini, Sri Hapsari; Chu, Kevin; Siejack, Richard A; Zhang, Haofei; Riva, Matthieu; Zhang, Zhenfa; Gold, Avram; Kautzman, Kathryn E; Surratt, Jason D

2014-10-21

Secondary organic aerosol (SOA) produced from reactive uptake and multiphase chemistry of isoprene epoxydiols (IEPOX) has been found to contribute substantially (upward of 33%) to the fine organic aerosol mass over the Southeastern U.S. Brown carbon (BrC) in rural areas of this region has been linked to secondary sources in the summer when the influence of biomass burning is low. We demonstrate the formation of light-absorbing (290 < λ < 700 nm) SOA constituents from reactive uptake of trans-β-IEPOX onto preexisting sulfate aerosols as a potential source of secondary BrC. IEPOX-derived BrC generated in controlled chamber experiments under dry, acidic conditions has an average mass absorption coefficient of ∼ 300 cm(2) g(-1). Chemical analyses of SOA constituents using UV-visible spectroscopy and high-resolution mass spectrometry indicate the presence of highly unsaturated oligomeric species with molecular weights separated by mass units of 100 (C5H8O2) and 82 (C5H6O) coincident with the observations of enhanced light absorption, suggesting such oligomers as chromophores, and potentially explaining one source of humic-like substances (HULIS) ubiquitously present in atmospheric aerosol. Similar light-absorbing oligomers were identified in fine aerosol collected in the rural Southeastern U.S., supporting their atmospheric relevance and revealing a previously unrecognized source of oligomers derived from isoprene that contributes to ambient fine aerosol mass.

Real-time black carbon emission factors of light-duty vehicles tested on a chassis dynamometer

NASA Astrophysics Data System (ADS)

Forestieri, S. D.; Cappa, C. D.; Kuwayama, T.; Collier, S.; Zhang, Q.; Kleeman, M. J.

2012-12-01

Eight light-duty gasoline vehicles were tested on a Chassis dynamometer using the California Unified Driving Cycle (UDC) at the Haagen-Smit vehicle test facility at the California Air Resources Board (CARB) in El Monte, CA during September 2011. In addition, one light-duty gasoline vehicle, one ultra low-emission vehicle, one diesel passenger vehicle, and one gasoline direct injection vehicle were tested on a constant velocity driving cycle. Vehicle exhaust was diluted through CARB's CVS tunnel and a secondary dilution system in order to examine particulate matter (PM) emissions at atmospherically relevant concentrations (5-30 μg-m3). A variety of real-time instrumentation was used to characterize how the major PM components vary during a typical driving cycle, which includes a cold start phase followed by a hot stabilized running phase. Aerosol absorption coefficients were obtained at 532 nm and 405 nm with a time resolution of 2 seconds from a photo-acoustic spectrometer. These absorption coefficients were then converted to black carbon (BC) concentrations via a mass absorption coefficient. Non-refractory organic and inorganic PM and CO2 concentrations were quantified with a time resolution of 10 seconds using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS). Real-time BC and CO2 concentrations allowed for the determination of BC emission factors (EFs), providing insights into the variability of BC EFs during different phases of a typical driving cycle and aiding in the modeling BC emissions.

Spatial Interpolation of Aerosol Optical Depth Pollution: Comparison of Methods for the Development of Aerosol Distribution

NASA Astrophysics Data System (ADS)

Safarpour, S.; Abdullah, K.; Lim, H. S.; Dadras, M.

2017-09-01

Air pollution is a growing problem arising from domestic heating, high density of vehicle traffic, electricity production, and expanding commercial and industrial activities, all increasing in parallel with urban population. Monitoring and forecasting of air quality parameters are important due to health impact. One widely available metric of aerosol abundance is the aerosol optical depth (AOD). The AOD is the integrated light extinction coefficient over a vertical atmospheric column of unit cross section, which represents the extent to which the aerosols in that vertical profile prevent the transmission of light by absorption or scattering. Seasonal aerosol optical depth (AOD) values at 550 nm derived from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensor onboard NASA's Terra satellites, for the 10 years period of 2000 - 2010 were used to test 7 different spatial interpolation methods in the present study. The accuracy of estimations was assessed through visual analysis as well as independent validation based on basic statistics, such as root mean square error (RMSE) and correlation coefficient. Based on the RMSE and R values of predictions made using measured values from 2000 to 2010, Radial Basis Functions (RBFs) yielded the best results for spring, summer and winter and ordinary kriging yielded the best results for fall.

Long term measurements of the estimated hygroscopic enhancement of aerosol optical properties

NASA Astrophysics Data System (ADS)

Hervo, Maxime; Sellegri, Karine; Pichon, Jean Marc; Roger, Jean Claude; Laj, Paolo

2015-04-01

Water vapour has a major impact on aerosol optical properties, thus on the Radiative Forcing for aerosol-radiation interaction (RFari). However there is few studies measuring this impact over a large period. Optical properties of aerosols were measured at the GAW Puy de Dôme station (1465m) over a seven year period (2006-2012). The impact of hygroscopicity on aerosol optical properties was calculated over a two year period (2010-2011). The analysis of the spatial and temporal variability of the dry optical properties showed that while no long term trend was found, a clear seasonal and diurnal variation was observed on the extensive parameters (scattering, absorption). Scattering and absorption coefficients were highest during the warm season and daytime, in concordance with the seasonality and diurnal variation of the planetary boundary layer height reaching the site. Intensive parameters (single scattering albedo, asymmetry factor, refractive index) did not show such a strong diurnal variability, but still indicated different values depending on the season. Both extensive and intensive optical parameters were sensitive to the air mass origin. A strong impact of hygroscopicity on aerosol optical properties was calculated, mainly on aerosol scattering, with a dependence on the aerosol type and the season. At 90% humidity, the scattering factor enhancement (fsca) was more than 4.4 for oceanic aerosol that have mixed with a pollution plume. Consequently, the aerosol radiative forcing was estimated to be 2.8 times higher at RH= 90% and 1.75 times higher at ambient RH when hygroscopic growth of the aerosol was considered. The hygroscopicity enhancement factor of the scattering coefficient was parameterized as a function of humidity and air mass type. To our knowledge, these results are one of the first presenting the impact of water vapour on the aerosol optical properties for a long period, and the first for a site at the border between the planetary boundary layer and the free troposphere. Acknowledgements. The authors would like to acknowledge the OPGC and its staff and INSU/CNRS for their contribution to establishing and maintaining the PdD measurement site. This work was performed in the frame of the european EUSAAR (R113-CT-2006-026140) and EUCAARI (0136833-2) and the french ORAURE SOERE.

Nitrogen dioxide and kerosene-flame soot calibration of photoacoustic instruments for measurement of light absorption by aerosols

DOE Office of Scientific and Technical Information (OSTI.GOV)

Arnott, W. Patrick; Moosmu''ller, Hans; Walker, John W.

2000-12-01

A nitrogen dioxide calibration method is developed to evaluate the theoretical calibration for a photoacoustic instrument used to measure light absorption by atmospheric aerosols at a laser wavelength of 532.0 nm. This method uses high concentrations of nitrogen dioxide so that both a simple extinction and the photoacoustically obtained absorption measurement may be performed simultaneously. Since Rayleigh scattering is much less than absorption for the gas, the agreement between the extinction and absorption coefficients can be used to evaluate the theoretical calibration, so that the laser gas spectra are not needed. Photoacoustic theory is developed to account for strong absorptionmore » of the laser beam power in passage through the resonator. Findings are that the photoacoustic absorption based on heat-balance theory for the instrument compares well with absorption inferred from the extinction measurement, and that both are well within values represented by published spectra of nitrogen dioxide. Photodissociation of nitrogen dioxide limits the calibration method to wavelengths longer than 398 nm. Extinction and absorption at 532 and 1047 nm were measured for kerosene-flame soot to evaluate the calibration method, and the single scattering albedo was found to be 0.31 and 0.20 at these wavelengths, respectively.« less

Aerosol source apportionment based on multi-wavelength photoacoustic light absorption measurements: a simulation method for system's optimisation

NASA Astrophysics Data System (ADS)

Simon, Károly; Ajtai, Tibor; Kiss-Albert, Gergely; Utry, Noémi; Pintér, Máté; Szabó, Gábor; Bozóki, Zoltán

2017-04-01

Aerosol source apportionment is currently one of the outstanding challenges for environmental monitoring. In most cases atmospheric aerosol is a heterogeneous mixture as it typically originates from various sources. Consequently, each aerosol type has distinct chemical and physical properties. Contrary to chemical properties, optical absorption and size distribution of airborne particles can be measured in real time with high time resolution i.e. their measurement facilitates real time source apportionment (Favez et al (2009), Ajtai et al (2011), Favez et al (2010)). The wavelength dependency of the optical absorption coefficient (OAC) is usually characterised by the Absorption Angström Exponent (AAE). So far, the selection of light sources (lasers) into a photoacoustic aerosol measuring system was based on rule of thumb type estimations only. Recently, we proposed a simulation method that can be used to estimate the accuracy of aerosol source apportionment in case of a dual wavelength photoacoustic system (Simon et al., (2017)). This simulation is based on the assumption that the atmospheric aerosol load is dominated by two distinct sources and each of them is strongly light absorbing with specific AAE values. This is a typical scenario e.g. for urban measurements under wintry conditions when dominating aerosol sources are fossil fuel and wood burning with characteristic AAE 1 and 2, respectively. The wavelength pair of 405 and 1064 nm was found to be optimal for source apportionment in this case. In the presented study we investigated the situation when there are aerosol components with only slightly different AAE values and searched for a photoacoustic system which is optimal for distinguishing these components. Ajtai, T.; Filep, Á.; Utry, N.; Schnaiter, M.; Linke, C.; Bozóki, Z.; Szabó, G. and Leisner T. (2011) Journal of Aerosol Science 42, 859-866. Favez, O.; Cachier, H.; Sciare, J.; Sarda-Estève, R. and Martinon, L. (2009) Atmospheric Environment 43, 3640-3644. Favez, O.; El Haddad, I.; Piot, C.; Boréave, A.; Abidi, E.; Marchand, N.; Jaffrezo, J. L.; Besombes, J. L.; Personnaz, M. B.; Sciare, J.; Wortham, H.; George, C. and D'Anna, B. (2010), Atmos. Chem. Phys. 10, 5295-5314. Simon, K.A.; Ajtai, T; Gulyas, G; Utry, N; Pinter, M; Szabo, G. and Bozoki, Bozoki, Z. (2017), Journal of Aerosol Science 104, 10-15.

Light absorption and morphological properties of soot-containing aerosols observed at an East Asian outflow site, Noto Peninsula, Japan

NASA Astrophysics Data System (ADS)

Ueda, Sayako; Nakayama, Tomoki; Taketani, Fumikazu; Adachi, Kouji; Matsuki, Atsushi; Iwamoto, Yoko; Sadanaga, Yasuhiro; Matsumi, Yutaka

2016-03-01

The coating of black carbon (BC) with inorganic salts and organic compounds can enhance the magnitude of light absorption by BC. To elucidate the enhancement of light absorption of aged BC particles and its relation to the mixing state and morphology of individual particles, we conducted observations of particles at an Asian outflow site in Noto Peninsula, Japan, in the spring of 2013. Absorption and scattering coefficients at 405, 532, and 781 nm and mass concentrations/mixing states of refractory BC in PM2.5 were measured using a three-wavelength photoacoustic soot spectrometer and a single-particle soot photometer (SP2), respectively, after passage through a thermodenuder (TD) maintained at 300 or 400 °C or a bypass line maintained at room temperature (25 °C). The average enhancement factor of BC light absorption due to coating was estimated by comparing absorption coefficients at 781 nm for particles that with and without passing through the TD at 300 °C and was found to be 1.22. The largest enhancements (> 1.30) were observed under high absorption coefficient periods when the air mass was long-range transported from urban areas in China. Aerosol samples were also analyzed using a transmission electron microscope (TEM) equipped with an energy dispersive X-ray analyzer. The morphological features and mixing states of soot-containing particles of four samples collected during the high absorption events were analyzed by comparing microphotographs before and after the evaporation of beam-sensitive materials by irradiation with a high-density electron beam. The majority of the soot in all samples was found as mixed particles with sulfate-containing spherules or as clusters of such spherules. For samples showing high enhancement (> 1.30) of BC light absorption, the TEM showed that the internally mixed soot-containing particles tended to have a more spherical shape and to be thickly coated. The SP2 measurements also suggested that the proportion of thickly coated soot was greater. Thus, the observed enhancement of BC light absorption was found to differ according to the mixing states and morphology of soot-containing particles. The enhancement of BC light absorption in our in situ measurements and its relation with individual features of soot-containing particles will be useful to evaluate direct radiative forcing in the downwind areas of large emission sources of BC.

Vertical distribution of aerosol optical properties based on aircraft measurements over the Loess Plateau in China.

PubMed

Li, Junxia; Liu, Xingang; Yuan, Liang; Yin, Yan; Li, Zhanqing; Li, Peiren; Ren, Gang; Jin, Lijun; Li, Runjun; Dong, Zipeng; Li, Yiyu; Yang, Junmei

2015-08-01

Vertical distributions of aerosol optical properties based on aircraft measurements over the Loess Plateau were measured for the first time during a summertime aircraft campaign, 2013 in Shanxi, China. Data from four flights were analyzed. The vertical distributions of aerosol optical properties including aerosol scattering coefficients (σsc), absorption coefficients (σab), Angström exponent (α), single scattering albedo (ω), backscattering ratio (βsc), aerosol mass scattering proficiency (Qsc) and aerosol surface scattering proficiency (Qsc(')) were obtained. The mean statistical values of σsc were 77.45 Mm(-1) (at 450 nm), 50.72 Mm(-1) (at 550n m), and 32.02 Mm(-1) (at 700 nm). The mean value of σab was 7.62 Mm(-1) (at 550 nm). The mean values of α, βsc and ω were 1.93, 0.15, and 0.91, respectively. Aerosol concentration decreased with altitude. Most effective diameters (ED) of aerosols were less than 0.8 μm. The vertical profiles of σsc,, α, βsc, Qsc and Qsc(') showed that the aerosol scattering properties at lower levels contributed the most to the total aerosol radiative forcing. Both α and βsc had relatively large values, suggesting that most aerosols in the observational region were small particles. The mean values of σsc, α, βsc, Qsc, Qsc('), σab and ω at different height ranges showed that most of the parameters decreased with altitude. The forty-eight hour backward trajectories of air masses during the observation days indicated that the majority of aerosols in the lower level contributed the most to the total aerosol loading, and most of these particles originated from local or regional pollution emissions. Copyright © 2015. Published by Elsevier B.V.

Phase function, backscatter, extinction, and absorption for standard radiation atmosphere and El Chichon aerosol models at visible and near-infrared wavelengths

NASA Technical Reports Server (NTRS)

Whitlock, C. H.; Suttles, J. T.; Lecroy, S. R.

1985-01-01

Tabular values of phase function, Legendre polynominal coefficients, 180 deg backscatter, and extinction cross section are given for eight wavelengths in the atmospheric windows between 0.4 and 2.2 microns. Also included are single scattering albedo, asymmetry factor, and refractive indices. These values are based on Mie theory calculations for the standard rediation atmospheres (continental, maritime, urban, unperturbed stratospheric, volcanic, upper atmospheric, soot, oceanic, dust, and water-soluble) assest measured volcanic aerosols at several time intervals following the El Chichon eruption. Comparisons of extinction to 180 deg backscatter for different aerosol models are presented and related to lidar data.

Atmospheric Optical Properties and Spectral Analysis of Desert Aerosols

NASA Astrophysics Data System (ADS)

Yvgeni, D.; Karnieli, A.; Kaufman, Y. J.; Andreae, M. O.; Holben, B. N.; Maenhaut, W.

2002-05-01

Scientific background Aerosols can interact directly with solar and terrestrial radiation by scattering as well as absorption. In addition, they can indirectly alter the planetary albedo by modifying the properties of clouds. Objectives Investigations have been devoted to two main areas: (1) Aerosol climatology situation in the Negev desert, investigations of physical and chemical characteristics of aerosols, and study of the local and long-range transport trajectory of polluted air masses over the Negev desert; and (2) An estimation of the optical properties throughout the atmospheric column by surface measurements via performance of spectral and statistical analysis of the data received from two measurement systems. Results and conclusions Analyzed data from the Sede Boker site, in the Negev Desert of Israel, shows an increase in aerosol optical depth during the summer seasons and a decrease during winter. One of the possible reasons for this characteristic is an increase of the precipitable water (reaches 3.0-3.5 cm) due to a constant wind stream from the Mediterranean Sea in same time. The highest probability distribution of the aerosol optical depth is in the range of 0.15-0.20; and of the Angstrom parameter is in range of 0.83 - 1.07. During dust storm events, the scattering coefficient range at 670 nm and 440 nm wavelengths were inverted. It was discovered that the dust particles in this case had non-spherical character. Comparison between optical depth, measured through all atmospheric column, and scattering coefficient from surface measurements provides correlation coefficient (r) equal to 0.64. The Angstrom parameter, calculated via optical depth and via scattering coefficient, provides a correlation coefficient of 0.66. Thus we can obtain an estimate of the influence of the surface aerosol situation on column optical properties. The combined analysis of dust cloud altitude and optical depth as a function of the time indicates long-term transport and settling of the aerosol, thus this analysis allowed to get a qualitative relation with trajectories and transport models. An additional finding is that except for the dust storms, the aerosol optical properties defined by fine particles, i.e. product of urban pollution. Possible explanations for this situation are the pollution sources in the Israeli Mediterranean coast, where population and industrial centers are concentrated, and long-range transport of polluted air masses from the European region.

View From a Megacity: Aerosol Light Absorption and Scattering at Four Sites in and Near Mexico City.

NASA Astrophysics Data System (ADS)

Paredes-Miranda, G.; Arnott, W. P.; Gaffney, J. S.; Marley, N. A.

2006-12-01

As part of the Megacity Impacts on Regional and Global Environments, MIRAGE-Mex deployment to Mexico City in the period of 30 days, March 2006, a suite of photoacoustic spectrometers (PAS) were installed to measure at ground level the light absorption and scattering by aerosols at four sites: an urban site at Instituto Mexicano del Petroleo (Mexican Oil Institute, denoted by IMP), a suburban site at the Technological University of Tecamac, a rural site at "La Biznaga" ranch, and a site at the Paseo de Cortes (altitude 3,810 meters ASL) in the rural area above Amecameca in the State of Mexico, on the saddle between the volcanoes Popocatepetl and Iztaccihuatl. The IMP site gave in-situ characterization of the Mexico City plume under favorable wind conditions while the other sites provided characterization of the plume, mixed in with any local sources. The second and third sites are north of Mexico City, and the fourth site is south. The PAS used at IMP operates at 532 nm, and conveniently allowed for characterization of gaseous absorption at this wavelength as well. Instruments at the second and third sites operate at 870 nm, and the one at the fourth site at 780 nm. Light scattering measurements are accomplished within the PAS by the reciprocal nephelometery method. In the urban site the aerosol absorption coefficient typically varies between 40 and 250 Mm-1 during the course of the day and significant diurnal variation of the aerosol single scattering albedo was observed. Comparisons with TSI nephelometer scattering and Aetholemeter absorption measurements at the T0 site will be presented. We will present a broad overview of the diurnal variation of the scattering and absorption as well as the single scattering albedo and fraction of absorption due to gases at the IMP site. Insight on the dynamical connections will be discussed.

Exploring the observational constraints on the simulation of brown carbon

NASA Astrophysics Data System (ADS)

Wang, X.; Heald, C. L.; Liu, J.; Weber, R. J.; Campuzano-Jost, P.; Jimenez, J. L.; Schwarz, J. P.; Perring, A. E.

2017-12-01

Brown carbon (BrC) is the component of organic aerosols (OA) which strongly absorbs solar radiation in the near-UV range of the spectrum. However the sources, evolution, and optical properties of BrC remain highly uncertain, and therefore constitute a large source of uncertainty in estimating the global direct radiative effect (DRE) of aerosols. Previous modeling studies of BrC optical properties and DRE have been unable to fully evaluate the skill of their simulations, given the lack of direct measurements of organic aerosol absorption. In this study, we develop a global model simulation (GEOS-Chem) of BrC and test it against BrC absorption measurements from two aircraft campaigns in the U.S. (SEAC4RS and DC3). To our knowledge, this is the first study to compare simulated BrC absorption with direct, continuous ambient measurements. We show that the laboratory-based BrC absorption properties from biomass burning overestimate the aircraft measurements of ambient BrC. In addition, applying a photochemical whitening scheme to simulated BrC is better able to represent the observed BrC absorption. These observations are consistent with a mass absorption coefficient (MAC) of freshly emitted biomass burning OA of 0.57m2g-1. Using the RRTMG model integrated with GEOS-Chem, we estimate that the all-sky top-of-atmosphere direct radiative effect (DRE) of OA is -0.350 Wm-2, 10% higher than that without consideration of BrC absorption. Therefore, our best estimate of the absorption DRE of BrC is +0.042 Wm-2. We suggest that the DRE of BrC has been overestimated previously due to the lack of observational constraints from direct measurements as well as neglect of the effects of photochemical whitening.

Synergic use of TOMS and Aeronet Observations for Characterization of Aerosol Absorption

NASA Technical Reports Server (NTRS)

Torres, O.; Bhartia, P. K.; Dubovik, O.; Holben, B.; Siniuk, A.

2003-01-01

The role of aerosol absorption on the radiative transfer balance of the earth-atmosphere system is one of the largest sources of uncertainty in the analysis of global climate change. Global measurements of aerosol single scattering albedo are, therefore, necessary to properly assess the radiative forcing effect of aerosols. Remote sensing of aerosol absorption is currently carried out using both ground (Aerosol Robotic Network) and space (Total Ozone Mapping Spectrometer) based observations. The satellite technique uses measurements of backscattered near ultraviolet radiation. Carbonaceous aerosols, resulting from the combustion of biomass, are one of the most predominant absorbing aerosol types in the atmosphere. In this presentation, TOMS and AERONET retrievals of single scattering albedo of carbonaceous aerosols, are compared for different environmental conditions: agriculture related biomass burning in South America and Africa and peat fires in Eastern Europe. The AERONET and TOMS derived aerosol absorption information are in good quantitative agreement. The most absorbing smoke is detected over the African Savanna. Aerosol absorption over the Brazilian rain forest is less absorbing. Absorption by aerosol particles resulting from peat fires in Eastern Europe is weaker than the absorption measured in Africa and South America. This analysis shows that the near UV satellite method of aerosol absorption characterization has the sensitivity to distinguish different levels of aerosol absorption. The analysis of the combined AERONET-TOMS observations shows a high degree of synergy between satellite and ground based observations.

Light scattering and extinction measurements combined with laser-induced incandescence for the real-time determination of soot mass absorption cross section.

PubMed

Wei, Yiyi; Ma, Lulu; Cao, Tingting; Zhang, Qing; Wu, Jun; Buseck, Peter R; Thompson, J E

2013-10-01

An aerosol albedometer was combined with laser-induced incandescence (LII) to achieve simultaneous measurements of aerosol scattering, extinction coefficient, and soot mass concentration. Frequency doubling of a Nd:YAG laser line resulted in a colinear beam of both λ = 532 and 1064 nm. The green beam was used to perform cavity ring-down spectroscopy (CRDS), with simultaneous measurements of scattering coefficient made through use of a reciprocal sphere nephelometer. The 1064 nm beam was selected and directed into a second integrating sphere and used for LII of light-absorbing kerosene lamp soot. Thermal denuder experiments showed the LII signals were not affected by the particle mixing state when laser peak power was 1.5-2.5 MW. The combined measurements of optical properties and soot mass concentration allowed determination of mass absorption cross section (M.A.C., m(2)/g) with 1 min time resolution when soot concentrations were in the low microgram per cubic meter range. Fresh kerosene nanosphere soot (ns-soot) exhibited a mean M.A.C and standard deviation of 9.3 ± 2.7 m(2)/g while limited measurements on dry ambient aerosol yielded an average of 8.2 ± 5.9 m(2)/g when soot was >0.25 μg/m(3). The method also detected increases in M.A.C. values associated with enhanced light absorption when polydisperse, laboratory-generated ns-soot particles were embedded within or coated with ammonium nitrate, ammonium sulfate, and glycerol. Glycerol coatings produced the largest fractional increase in M.A.C. (1.41-fold increase), while solid coatings of ammonium sulfate and ammonium nitrate produced increases of 1.10 and 1.06, respectively. Fresh, ns-soot did not exhibit increased M.A.C. at high relative humidity (RH); however, lab-generated soot coated with ammonium nitrate and held at 85% RH exhibited M.A.C. values nearly double the low-humidity case. The hybrid instrument for simultaneously tracking soot mass concentration and aerosol optical properties in real time is a valuable tool for probing enhanced absorption by soot at atmospherically relevant concentrations.

Effective absorption cross sections and photolysis rates of anthropogenic and biogenic secondary organic aerosols

NASA Astrophysics Data System (ADS)

Romonosky, Dian E.; Ali, Nujhat N.; Saiduddin, Mariyah N.; Wu, Michael; Lee, Hyun Ji (Julie); Aiona, Paige K.; Nizkorodov, Sergey A.

2016-04-01

Mass absorption coefficient (MAC) values were measured for secondary organic aerosol (SOA) samples produced by flow tube ozonolysis and smog chamber photooxidation of a wide range of volatile organic compounds (VOC), specifically: α-pinene, β-pinene, β-myrcene, d-limonene, farnesene, guaiacol, imidazole, isoprene, linalool, ocimene, p-xylene, 1-methylpyrrole, and 2-methylpyrrole. Both low-NOx and high-NOx conditions were employed during the chamber photooxidation experiments. MAC values were converted into effective molecular absorption cross sections assuming an average molecular weight of 300 g/mol for SOA compounds. The upper limits for the effective photolysis rates of SOA compounds were calculated by assuming unity photolysis quantum yields and convoluting the absorption cross sections with a time-dependent solar spectral flux. A more realistic estimate for the photolysis rates relying on the quantum yield of acetone was also obtained. The results show that condensed-phase photolysis of SOA compounds can potentially occur with effective lifetimes ranging from minutes to days, suggesting that photolysis is an efficient and largely overlooked mechanism of SOA aging.

403 nm cavity ring-down measurements of brown carbon aerosol

NASA Astrophysics Data System (ADS)

Kwon, D.; Grassian, V. H.; Kleiber, P.; Young, M. A.

2017-12-01

Atmospheric aerosol influences Earth's climate by absorbing and scattering incoming solar radiation and outgoing terrestrial radiation. One class of secondary organic aerosol (SOA), called brown carbon (BrC), has attracted attention for its wavelength dependent light absorbing properties with absorption coefficients that generally increase from the visible (Vis) to ultraviolet (UV) regions. Here we report results from our investigation of the optical properties of BrC aerosol products from the aqueous phase reaction of ammonium sulfate (AS) with methylglyoxal (MG) using cavity ring-down spectroscopy (CRDS) at 403 nm wavelength. We have measured the optical constants of BrC SOA from the AS/MG reaction as a function of reaction time. Under dry flow conditions, we observed no apparent variation in the BrC refractive index with aging over the course of 22 days. The retrieved BrC optical constants are similar to those of AS with n = 1.52 for the real component. Despite significant UV absorption observed from the bulk BrC solution, the imaginary index value at 403 nm is below our minimum detection limit which puts an upper bound of k as 0.03. These observations are in agreement with results from our recent studies of the light scattering properties of this BrC aerosol.

Optical Properties of Aerosols and Implications for Radiative Effects in Beijing During the Asia-Pacific Economic Cooperation Summit 2014

NASA Astrophysics Data System (ADS)

Zhou, Yaqing; Wang, Qiyuan; Huang, Rujin; Liu, Suixin; Tie, Xuexi; Su, Xiaoli; Niu, Xinyi; Zhao, Zhuzi; Ni, Haiyan; Wang, Meng; Zhang, Yonggang; Cao, Junji

2017-09-01

An intensive measurement campaign was conducted in Beijing during the Asia-Pacific Economic Cooperation (APEC) Summit 2014 to investigate the effectiveness of stringent emission controls on aerosol optical properties and direct radiative forcing (DRF). Average values of PM2.5, light scattering (bscat), and light absorption (babs) coefficients decreased by 40, 64, and 56%, respectively, during the APEC control period compared with noncontrol periods. For the APEC control period, the PM2.5 mass scattering and absorption efficiencies were both smaller than the noncontrol period by a factor of 2. Calculations based on a revised IMPROVE method and linear regression showed that sulfate, nitrate, organic matter, elemental carbon, and fine soil contributed comparably to the light extinction coefficient (bext) in both periods, but the bext values were 27-64% lower during the APEC period. A positive matrix factorization receptor model showed that bext from two secondary aerosol sources, biomass burning, traffic-related emissions, and coal burning decreased by 26-87% during the APEC control period. The average DRF calculated from the Tropospheric Ultraviolet and Visible radiation model was -11.9 and -4.6 W m-2 at the surface during the noncontrol and APEC control periods, respectively, suggesting an overall cooling effect. The reduction of DRF from each emission source ranged from 30-80% during the APEC control period. The results suggest that the pollution control measures implemented for APEC substantially reduced air pollution and could help mitigate the cooling effects of aerosols at the surface in Beijing.

Measurement of aerosol chemical, physical and radiative properties in the Yangtze delta region of China

NASA Astrophysics Data System (ADS)

Xu, Jin; Bergin, M. H.; Yu, X.; Liu, G.; Zhao, J.; Carrico, C. M.; Baumann, K.

In order to understand the possible influence of aerosols on the environment in the agricultural Yangtze delta region of China, a one-month field sampling campaign was carried out during November 1999 in Linan, China. Measurements included the aerosol light scattering coefficient at 530 nm, σsp, measured at both dry relative humidity (RH<40%) and under ambient conditions (sample RH=63±19%), and the absorption coefficient at 565 nm, σap, for aerosol particles having diameters <2.5 μm (PM 2.5). At the same time, daily filter samples of PM 2.5 as well as aerosol particles having diameters <10 μm (PM 10) were collected and analyzed for mass, major ion, organic compound (OC), and elemental carbon (EC) concentrations in order to determine which anthropogenic chemical species were primarily responsible for aerosol light extinction. The aerosol loading in the rural Yangtze delta region was comparable to highly polluted urban areas, with mean and standard deviation (S.D.) values for σsp, σap and PM 2.5 of 353 Mm -1 (202 Mm -1), 23 Mm -1 (14 Mm -1) and 90 μg m -3 (47 μg m -3), respectively. A clear diurnal pattern was observed in σsp and σap with minimum values occurring in the middle of the day, most likely associated with the maximum midday mixing height. The ratio of the change in light scattering coefficient at ambient RH to that at controlled RH (RH<40%), Fσsp (RH), indicates that condensed water typically contributed ˜40% to the light scattering budget in this region. The mass scattering efficiency of the dry aerosol, E scat_2.5, and mass absorption efficiency of EC, E abs_2.5, have mean and S.D. values of 4.0 m 2 g -1 (0.4 m 2 g -1) and 8.6 m 2 g -1 (7.0 m 2 g -1), respectively. PM 2.5 concentrations in Linan and two other locations in the Yangtze delta, Sheshan and Changshu (which have monthly mean values ranging from ˜80 to 110 μg m -3), are all significantly higher than the proposed 24-h average US PM 2.5 NAAQS of 65 μg m -3. Organic compounds are the dominant chemical species accounting for ˜50% of the PM 2.5 mass at all three sites. The results indicate that aerosol loadings in the agricultural Yangtze delta region of China are relatively high, and suggest that aerosols have a significant impact on visibility, climate, crop production, and human health in this region.

Light Absorption Enhancement of Black Carbon Aerosol Constrained by Particle Morphology.

PubMed

Wu, Yu; Cheng, Tianhai; Liu, Dantong; Allan, James D; Zheng, Lijuan; Chen, Hao

2018-06-19

The radiative forcing of black carbon aerosol (BC) is one of the largest sources of uncertainty in climate change assessments. Contrasting results of BC absorption enhancement ( E abs ) after aging are estimated by field measurements and modeling studies, causing ambiguous parametrizations of BC solar absorption in climate models. Here we quantify E abs using a theoretical model parametrized by the complex particle morphology of BC in different aging scales. We show that E abs continuously increases with aging and stabilizes with a maximum of ∼3.5, suggesting that previous seemingly contrast results of E abs can be explicitly described by BC aging with corresponding particle morphology. We also report that current climate models using Mie Core-Shell model may overestimate E abs at a certain aging stage with a rapid rise of E abs , which is commonly observed in the ambient. A correction coefficient for this overestimation is suggested to improve model predictions of BC climate impact.

Optical and physical properties of stratospheric aerosols from balloon measurements in the visible and near-infrared domains. I. Analysis of aerosol extinction spectra from the AMON and SALOMON balloonborne spectrometers

NASA Astrophysics Data System (ADS)

Berthet, Gwenaël; Renard, Jean-Baptiste; Brogniez, Colette; Robert, Claude; Chartier, Michel; Pirre, Michel

2002-12-01

Aerosol extinction coefficients have been derived in the 375-700-nm spectral domain from measurements in the stratosphere since 1992, at night, at mid- and high latitudes from 15 to 40 km, by two balloonborne spectrometers, Absorption par les Minoritaires Ozone et NOx (AMON) and Spectroscopie d'Absorption Lunaire pour l'Observation des Minoritaires Ozone et NOx (SALOMON). Log-normal size distributions associated with the Mie-computed extinction spectra that best fit the measurements permit calculation of integrated properties of the distributions. Although measured extinction spectra that correspond to background aerosols can be reproduced by the Mie scattering model by use of monomodal log-normal size distributions, each flight reveals some large discrepancies between measurement and theory at several altitudes. The agreement between measured and Mie-calculated extinction spectra is significantly improved by use of bimodal log-normal distributions. Nevertheless, neither monomodal nor bimodal distributions permit correct reproduction of some of the measured extinction shapes, especially for the 26 February 1997 AMON flight, which exhibited spectral behavior attributed to particles from a polar stratospheric cloud event.

Variations of aerosol size distribution, chemical composition and optical properties from roadside to ambient environment: A case study in Hong Kong, China

NASA Astrophysics Data System (ADS)

Zhang, Qian; Ning, Zhi; Shen, Zhenxing; Li, Guoliang; Zhang, Junke; Lei, Yali; Xu, Hongmei; Sun, Jian; Zhang, Leiming; Westerdahl, Dane; Gali, Nirmal Kumar; Gong, Xuesong

2017-10-01

This study investigated the ;roadside-to-ambient; evolution of particle physicochemical and optical properties in typical urban atmospheres of Hong Kong through collection of chemically-resolved PM2.5 data and PM2.5 size distribution at a roadside and an ambient site. Roadside particle size distribution showed typical peaks in the nuclei mode (30-40 nm) while ambient measurements peaked in the Aitken mode (50-70 nm), revealing possible condensation and coagulation growth of freshly emitted particles during aging processes. Much higher levels of anthropogenic chemical components, i.e. nitrate, sulfate, ammonium, organic carbon (OC) and elemental carbon (EC), but lower levels of OC/EC and secondary inorganic aerosols (SIA)/EC ratios appeared in roadside than ambient particles. The high OC/EC and SIA/EC ratios in ambient particles implied high contributions from secondary aerosols. Black carbon (BC), a strong light absorbing material, showed large variations in optical properties when mixed with other inorganic and organic components. Particle-bound polycyclic aromatic hydrocarbons (p-PAHs), an indicator of brown carbon (BrC), showed significant UV-absorbing ability. The average BC and p-PAHs concentrations were 3.8 and 87.6 ng m-3, respectively, at the roadside, but were only 1.5 and 18.1 ng m-3 at the ambient site, suggesting BC and p-PAHs concentrations heavily driven by traffic emissions. In contrast, PM2.5 UV light absorption coefficients (babs-BrC,370nm) at the ambient site (4.2 Mm-1) and at the roadside site (4.1 Mm-1) were similar, emphasizing that particle aging processes enhanced UV light-absorbing properties, a conclusion that was also supported by the finding that the Absorption Ångström coefficient (AAC) value at UV wavelengths (AAC_UV band) at the ambient site were ∼1.7 times higher than that at the roadside. Both aqueous reaction and photochemically produced secondary organic aerosol (SOA) for ambient aerosols contributed to the peak values of babs-BrC,370nm in ambient particles at midnight and around noon, highlighting that secondary BrC had different sources and particle aging in the atmosphere affected BrC and BC properties and related aerosol light absorption.

Aerosol Light Absorption and Scattering at Four Sites in and Near Mexico City: Comparison with Las Vegas, Nevada, USA

NASA Astrophysics Data System (ADS)

Arnott, W. P.; Miranda, G. P.; Gaffney, J. S.; Marley, N. A.

2007-05-01

Four photoacoustic spectrometers (PAS) for aerosol light scattering and absorption measurements were deployed in and near Mexico City in March 2006 as part of the Megacity Impacts on Regional and Global Environments (MIRAGE). The four sites included: an urban site at Instituto Mexicano del Petroleo (Mexican Oil Institute, denoted by IMP); a suburban site at the Technological University of Tecamac; a rural site at "La Biznaga" ranch; and a site at the Paseo de Cortes (altitude 3,810 meters ASL) in the rural area above Amecameca in the State of Mexico, on the saddle between the volcanoes Popocatepetl and Iztaccihuatl. A similar campaign was held in Las Vegas, Nevada, USA in January-February, 2003. The IMP site gave in-situ characterization of the Mexico City plume under favorable wind conditions while the other sites provided characterization of the plume, mixed in with any local sources. The second and third sites are north of Mexico City, and the fourth site is south. The PAS used at IMP operates at 532 nm, and conveniently allowed for characterization of gaseous absorption at this wavelength as well. Instruments at the second and third sites operate at 870 nm, and the one at the fourth site at 780 nm. Light scattering measurements are accomplished within the PAS by the reciprocal nephelometery method. In the urban site the aerosol absorption coefficient typically varies between 20 and 180 Mm-1 during the course of the day and significant diurnal variation of the aerosol single scattering albedo was observed probably as a consequence of secondary aerosol formation. Comparisons with TSI nephelometer scattering at the T0 site will be presented. We will present the diurnal variation of the scattering and absorption as well as the single scattering albedo and fraction of absorption due to gases at the IMP site and compare with Las Vegas diurnal variation. Mexico City 'breaths' more during the course of the day than Las Vegas, Nevada in part because the latitude of Mexico City resulted in more direct solar radiation. Further insight on the meteorological connections will be discussed.

Characterization of black carbon in an urban-rural fringe area of Beijing.

PubMed

Ji, Dongsheng; Li, Liang; Pang, Bo; Xue, Peng; Wang, Lili; Wu, Yunfei; Zhang, Hongliang; Wang, Yuesi

2017-04-01

Measuring black carbon (BC) is critical to understand the impact of combustion aerosols on air quality and climate change. In this study, BC was measured in 2014 at a unique community formed with rapid economic development and urbanization in an urban-rural fringe area of Beijing. Hourly BC concentrations were 0.1-33.5 μg/m 3 with the annual average of 4.4 ± 3.7 μg/m 3 . BC concentrations had clear diurnal, weekly, and seasonal variations, and were closely related with atmospheric visibility. The absorption coefficient of aerosols increased while its contribution to extinction coefficient decreased with the enhancement of PM 2.5 concentration. The high mass absorption efficiency (MAE) of EC was attributed to a combination of coal combustion, vehicular emission and rapidly coating by water-soluble ions and organic carbon (OC). BC concentrations followed a typical lognormal pattern, with over 88% samples in 0.1-10.0 μg/m 3 . Low BC levels were mostly bounded up with winds from north and northwest. Coal combustion and biomass burning were closely associated with severe haze pollution events. Firework discharge had significant UV absorption contribution. During the Asia-Pacific Economic Cooperation (APEC) forum in November 2014, air quality obviously improved due to various control strategies. Copyright © 2017 Elsevier Ltd. All rights reserved.

A review of current knowledge concerning PM2. 5 chemical composition, aerosol optical properties and their relationships across China

NASA Astrophysics Data System (ADS)

Tao, Jun; Zhang, Leiming; Cao, Junji; Zhang, Renjian

2017-08-01

To obtain a thorough knowledge of PM2. 5 chemical composition and its impact on aerosol optical properties across China, existing field studies conducted after the year 2000 are reviewed and summarized in terms of geographical, interannual and seasonal distributions. Annual PM2. 5 was up to 6 times the National Ambient Air Quality Standards (NAAQS) in some megacities in northern China. Annual PM2. 5 was higher in northern than southern cities, and higher in inland than coastal cities. In a few cities with data longer than a decade, PM2. 5 showed a slight decrease only in the second half of the past decade, while carbonaceous aerosols decreased, sulfate (SO42-) and ammonium (NH4+) remained at high levels, and nitrate (NO3-) increased. The highest seasonal averages of PM2. 5 and its major chemical components were typically observed in the cold seasons. Annual average contributions of secondary inorganic aerosols to PM2. 5 ranged from 25 to 48 %, and those of carbonaceous aerosols ranged from 23 to 47 %, both with higher contributions in southern regions due to the frequent dust events in northern China. Source apportionment analysis identified secondary inorganic aerosols, coal combustion and traffic emission as the top three source factors contributing to PM2. 5 mass in most Chinese cities, and the sum of these three source factors explained 44 to 82 % of PM2. 5 mass on annual average across China. Biomass emission in most cities, industrial emission in industrial cities, dust emission in northern cities and ship emission in coastal cities are other major source factors, each of which contributed 7-27 % to PM2. 5 mass in applicable cities. The geographical pattern of scattering coefficient (bsp) was similar to that of PM2. 5, and that of aerosol absorption coefficient (bap) was determined by elemental carbon (EC) mass concentration and its coating. bsp in ambient condition of relative humidity (RH) = 80 % can be amplified by about 1.8 times that under dry conditions. Secondary inorganic aerosols accounted for about 60 % of aerosol extinction coefficient (bext) at RH greater than 70 %. The mass scattering efficiency (MSE) of PM2. 5 ranged from 3.0 to 5.0 m2 g-1 for aerosols produced from anthropogenic emissions and from 0.7 to 1.0 m2 g-1 for natural dust aerosols. The mass absorption efficiency (MAE) of EC ranged from 6.5 to 12.4 m2 g-1 in urban environments, but the MAE of water-soluble organic carbon was only 0.05 to 0.11 m2 g-1. Historical emission control policies in China and their effectiveness were discussed based on available chemically resolved PM2. 5 data, which provides the much needed knowledge for guiding future studies and emissions policies.

Radiative and thermodynamic responses to aerosol extinction profiles during the pre-monsoon month over South Asia

DOE Office of Scientific and Technical Information (OSTI.GOV)

Feng, Y.; Kotamarthi, V. R.; Coulter, R.

Aerosol radiative effects and thermodynamic responses over South Asia are examined with the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) for March 2012. Model results of aerosol optical depths (AODs) and extinction profiles are analyzed and compared to satellite retrievals and two ground-based lidars located in northern India. The WRF-Chem model is found to heavily underestimate the AOD during the simulated pre-monsoon month and about 83 % of the model's low bias is due to aerosol extinctions below ~2 km. Doubling the calculated aerosol extinctions below 850 hPa generates much better agreement with the observed AOD and extinction profilesmore » averaged over South Asia. To separate the effect of absorption and scattering properties, two runs were conducted: in one run (Case I), the calculated scattering and absorption coefficients were increased proportionally, while in the second run (Case II) only the calculated aerosol scattering coefficient was increased. With the same AOD and extinction profiles, the two runs produce significantly different radiative effects over land and oceans. On the regional mean basis, Case I generates 48% more heating in the atmosphere and 21% more dimming at the surface than Case II. Case I also produces stronger cooling responses over the land from the longwave radiation adjustment and boundary layer mixing. These rapid adjustments offset the stronger radiative heating in Case I and lead to an overall lower-troposphere cooling up to -0.7K day −1, which is smaller than that in Case II. Over the ocean, direct radiative effects dominate the heating rate changes in the lower atmosphere lacking such surface and lower atmosphere adjustments due to fixed sea surface temperature, and the strongest atmospheric warming is obtained in Case I. Consequently, atmospheric dynamics (boundary layer heights and meridional circulation) and thermodynamic processes (water vapor and cloudiness) are shown to respond differently between Case I and Case II, underlining the importance of determining the exact portion of scattering or absorbing aerosols that lead to the underestimation of aerosol optical depth in the model. Additionally, the model results suggest that both the direct radiative effect and rapid thermodynamic responses need to be quantified for understanding aerosol radiative impacts.« less

Radiative and thermodynamic responses to aerosol extinction profiles during the pre-monsoon month over South Asia

DOE Office of Scientific and Technical Information (OSTI.GOV)

Feng, Y.; Kotamarthi, V. R.; Coulter, R.

Aerosol radiative effects and thermodynamic responses over South Asia are examined with a version of the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) for March 2012. Model results of Aerosol Optical Depth (AOD) and extinction profiles are analyzed and compared to satellite retrievals and two ground-based lidars located in the northern India. The WRF-Chem model is found to underestimate the AOD during the simulated pre-monsoon month and about 83 % of the model low-bias is due to aerosol extinctions below ~2 km. Doubling the calculated aerosol extinctions below 850 hPa generates much better agreement with the observed AODmore » and extinction profiles averaged over South Asia. To separate the effect of absorption and scattering properties, two runs were conducted: in one run (Case I), the calculated scattering and absorption coefficients were increased proportionally, while in the second run (Case II) only the calculated aerosol scattering coefficient was increased. With the same AOD and extinction profiles, the two runs produce significantly different radiative effects over land and oceans. On the regional mean basis, Case I generates 48 % more heating in the atmosphere and 21 % more dimming at the surface than Case II. Case I also produces stronger cooling responses over the land from the longwave radiation adjustment and boundary layer mixing. These rapid adjustments offset the stronger radiative heating in Case I and lead to an overall lower-troposphere cooling up to -0.7 K day −1, which is smaller than that in Case II. Over the ocean, direct radiative effects dominate the heating rate changes in the lower atmosphere lacking such surface and lower atmosphere adjustments due to fixed sea surface temperature, and the strongest atmospheric warming is obtained in Case I. Consequently, atmospheric dynamics (boundary layer heights and meridional circulation) and thermodynamic processes (water vapor and cloudiness) are shown to respond differently between Case I and Case II underlying the importance of determining the exact portion of scattering or absorbing aerosols that lead to the underestimation of aerosol optical depth in the model. In addition, the model results suggest that both direct radiative effect and rapid thermodynamic responses need to be quantified for understanding aerosol radiative impacts.« less

Radiative and thermodynamic responses to aerosol extinction profiles during the pre-monsoon month over South Asia

DOE PAGES

Feng, Y.; Kotamarthi, V. R.; Coulter, R.; ...

2016-01-18

Aerosol radiative effects and thermodynamic responses over South Asia are examined with the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) for March 2012. Model results of aerosol optical depths (AODs) and extinction profiles are analyzed and compared to satellite retrievals and two ground-based lidars located in northern India. The WRF-Chem model is found to heavily underestimate the AOD during the simulated pre-monsoon month and about 83 % of the model's low bias is due to aerosol extinctions below ~2 km. Doubling the calculated aerosol extinctions below 850 hPa generates much better agreement with the observed AOD and extinction profilesmore » averaged over South Asia. To separate the effect of absorption and scattering properties, two runs were conducted: in one run (Case I), the calculated scattering and absorption coefficients were increased proportionally, while in the second run (Case II) only the calculated aerosol scattering coefficient was increased. With the same AOD and extinction profiles, the two runs produce significantly different radiative effects over land and oceans. On the regional mean basis, Case I generates 48% more heating in the atmosphere and 21% more dimming at the surface than Case II. Case I also produces stronger cooling responses over the land from the longwave radiation adjustment and boundary layer mixing. These rapid adjustments offset the stronger radiative heating in Case I and lead to an overall lower-troposphere cooling up to -0.7K day −1, which is smaller than that in Case II. Over the ocean, direct radiative effects dominate the heating rate changes in the lower atmosphere lacking such surface and lower atmosphere adjustments due to fixed sea surface temperature, and the strongest atmospheric warming is obtained in Case I. Consequently, atmospheric dynamics (boundary layer heights and meridional circulation) and thermodynamic processes (water vapor and cloudiness) are shown to respond differently between Case I and Case II, underlining the importance of determining the exact portion of scattering or absorbing aerosols that lead to the underestimation of aerosol optical depth in the model. Additionally, the model results suggest that both the direct radiative effect and rapid thermodynamic responses need to be quantified for understanding aerosol radiative impacts.« less

Radiative and thermodynamic responses to aerosol extinction profiles during the pre-monsoon month over South Asia

DOE Office of Scientific and Technical Information (OSTI.GOV)

Feng, Y.; Kotamarthi, V. R.; Coulter, R.

Aerosol radiative effects and thermodynamic responses over South Asia are examined with the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) for March 2012. Model results of aerosol optical depths (AODs) and extinction profiles are analyzed and compared to satellite retrievals and two ground-based lidars located in northern India. The WRF-Chem model is found to heavily underestimate the AOD during the simulated pre-monsoon month and about 83 % of the model's low bias is due to aerosol extinctions below ~2 km. Doubling the calculated aerosol extinctions below 850 hPa generates much better agreement with the observed AOD and extinction profilesmore » averaged over South Asia. To separate the effect of absorption and scattering properties, two runs were conducted: in one run (Case I), the calculated scattering and absorption coefficients were increased proportionally, while in the second run (Case II) only the calculated aerosol scattering coefficient was increased. With the same AOD and extinction profiles, the two runs produce significantly different radiative effects over land and oceans. On the regional mean basis, Case I generates 48 % more heating in the atmosphere and 21 % more dimming at the surface than Case II. Case I also produces stronger cooling responses over the land from the longwave radiation adjustment and boundary layer mixing. These rapid adjustments offset the stronger radiative heating in Case I and lead to an overall lower-troposphere cooling up to -0.7 K day −1, which is smaller than that in Case II. Over the ocean, direct radiative effects dominate the heating rate changes in the lower atmosphere lacking such surface and lower atmosphere adjustments due to fixed sea surface temperature, and the strongest atmospheric warming is obtained in Case I. Consequently, atmospheric dynamics (boundary layer heights and meridional circulation) and thermodynamic processes (water vapor and cloudiness) are shown to respond differently between Case I and Case II, underlining the importance of determining the exact portion of scattering or absorbing aerosols that lead to the underestimation of aerosol optical depth in the model. In addition, the model results suggest that both the direct radiative effect and rapid thermodynamic responses need to be quantified for understanding aerosol radiative impacts.« less

Radiative and thermodynamic responses to aerosol extinction profiles during the pre-monsoon month over South Asia

DOE PAGES

Feng, Y.; Kotamarthi, V. R.; Coulter, R.; ...

2015-06-19

Aerosol radiative effects and thermodynamic responses over South Asia are examined with a version of the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) for March 2012. Model results of Aerosol Optical Depth (AOD) and extinction profiles are analyzed and compared to satellite retrievals and two ground-based lidars located in the northern India. The WRF-Chem model is found to underestimate the AOD during the simulated pre-monsoon month and about 83 % of the model low-bias is due to aerosol extinctions below ~2 km. Doubling the calculated aerosol extinctions below 850 hPa generates much better agreement with the observed AODmore » and extinction profiles averaged over South Asia. To separate the effect of absorption and scattering properties, two runs were conducted: in one run (Case I), the calculated scattering and absorption coefficients were increased proportionally, while in the second run (Case II) only the calculated aerosol scattering coefficient was increased. With the same AOD and extinction profiles, the two runs produce significantly different radiative effects over land and oceans. On the regional mean basis, Case I generates 48 % more heating in the atmosphere and 21 % more dimming at the surface than Case II. Case I also produces stronger cooling responses over the land from the longwave radiation adjustment and boundary layer mixing. These rapid adjustments offset the stronger radiative heating in Case I and lead to an overall lower-troposphere cooling up to -0.7 K day −1, which is smaller than that in Case II. Over the ocean, direct radiative effects dominate the heating rate changes in the lower atmosphere lacking such surface and lower atmosphere adjustments due to fixed sea surface temperature, and the strongest atmospheric warming is obtained in Case I. Consequently, atmospheric dynamics (boundary layer heights and meridional circulation) and thermodynamic processes (water vapor and cloudiness) are shown to respond differently between Case I and Case II underlying the importance of determining the exact portion of scattering or absorbing aerosols that lead to the underestimation of aerosol optical depth in the model. In addition, the model results suggest that both direct radiative effect and rapid thermodynamic responses need to be quantified for understanding aerosol radiative impacts.« less

Remote Sensing of Aerosol and Non-Aerosol Absorption

NASA Technical Reports Server (NTRS)

Kaufman, Y. J.; Dubovik, O.; Holben, B. N.; Remer, L. A.; Tanre, D.; Lau, William K. M. (Technical Monitor)

2001-01-01

Remote sensing of aerosol from the new satellite instruments (e.g. MODIS from Terra) and ground based radiometers (e.g. the AERONET) provides the opportunity to measure the absorption characteristics of the ambient undisturbed aerosol in the entire atmospheric column. For example Landsat and AERONET data are used to measure spectral absorption of sunlight by dust from West Africa. Both Application of the Landsat and AERONET data demonstrate that Saharan dust absorption of solar radiation is several times smaller than the current international standards. This is due to difficulties of measuring dust absorption in situ, and due to the often contamination of dust properties by the presence of air pollution or smoke. We use the remotely sensed aerosol absorption properties described by the spectral sin le scattering albedo, together with statistics of the monthly optical thickness for the fine and coarse aerosol derived from the MODIS data. The result is an estimate of the flux of solar radiation absorbed by the aerosol layer in different regions around the globe where aerosol is prevalent. If this aerosol forcing through absorption is not included in global circulation models, it may be interpreted as anomalous absorption in these regions. In a preliminary exercise we also use the absorption measurements by AERONET, to derive the non-aerosol absorption of the atmosphere in cloud free conditions. The results are obtained for the atmospheric windows: 0.44 microns, 0.66 microns, 0.86 microns and 1.05 microns. In all the locations over the land and ocean that were tested no anomalous absorption in these wavelengths, was found within absorption optical thickness of +/- 0.005.

A chamber investigation of the IR and visible wavelength obscuration properties of pyrotechnically generated smokes

NASA Astrophysics Data System (ADS)

Hanley, J. T.; Mack, E. J.

1985-05-01

The overall objective of the program is the development of an effective screening agent to both visible and IR wavelengths utilizing pyrotechnically-generated hygroscopic aerosol. In pursuit of an effective IR wavelength screen and an increased understanding of the particle formation mechanisms and resultant size distribution, the primary objective of this year's effort was to evaluate the influence of an energetic binder (GAP) on the performance of two pyrotechnics, one which produced a KCL aerosol, the other a mixed aerosol, the other a mixed aerosol of MgCl2 and carbon. Comparison tests were run, in Calspan's 600 cu m test chamber, in which the performance of the energetic vs. non-energetic pyrotechnics was compared in terms of mass yield, payload mass extinction coefficient, aerosol decay rate and size distribution. A secondary objective of limited scope was to investigate the potential of using IR absorbing surface active agents to coat the smoke aerosol so as to enhance the smoke's IR wavelength absorption as well as inhibit subsequent aerosol evaporation upon exposure to decreasing humidity.

Imaginary refractive index and other microphysical properties of volcanic ash, Sarahan dust, and other mineral aerosols

NASA Astrophysics Data System (ADS)

Rocha Lima, A.; Martins, J.; Krotkov, N. A.; Artaxo, P.; Todd, M.; Ben Ami, Y.; Dolgos, G.; Espinosa, R.

2013-12-01

Aerosol properties are essential to support remote sensing measurements, atmospheric circulation and climate models. This research aims to improve the understanding of the optical and microphysical properties of different types of aerosols particles. Samples of volcanic ash, Saharan dust and other mineral aerosols particles were analyzed by different techniques. Ground samples were sieved down to 45um, de-agglomerated and resuspended in the laboratory using a Fluidized Bed Aerosol Generator (FBAG). Particles were collected on Nuclepore filters into PM10, PM2.5, or PM1.0. and analyzed by different techniques, such as Scanning Electron Microscopy (SEM) for determination of size distribution and shape, spectral reflectance for determination of the optical absorption properties as a function of the wavelength, material density, and X-Ray fluorescence for the elemental composition. The spectral imaginary part of refractive index from the UV to the short wave infrared (SWIR) wavelength was derived empirically from the measurements of the spectral mass absorption coefficient, size distribution and density of the material. Some selected samples were also analyzed with the Polarized Imaging Nephelometer (PI-Neph) instrument for the characterization of the aerosol polarized phase function. This work compares results of the spectral refractive index of different materials obtained by our methodology with those available in the literature. In some cases there are significant differences both in magnitude and spectral dependence of the imaginary refractive index. These differences are evaluated and discussed in this work.

Atmospheric aerosol brown carbon in the high Himalayas

NASA Astrophysics Data System (ADS)

Kirillova, Elena; Decesari, Stefano; Marinoni, Angela; Bonasoni, Paolo; Vuillermoz, Elisa; Facchini, M. Cristina; Fuzzi, Sandro

2016-04-01

Anthropogenic light-absorbing atmospheric aerosol can reach very high concentrations in the planetary boundary layer in South-East Asia ("brown clouds"), affecting atmospheric transparency and generating spatial gradients of temperature over land with a possible impact on atmospheric dynamics and monsoon circulation. Besides black carbon (BC), an important light-absorbing component of anthropogenic aerosols is the organic carbon component known as 'brown carbon' (BrC). In this research, we provided first measurements of atmospheric aerosol BrC in the high Himalayas during different seasons. Aerosol sampling was conducted at the GAW-WMO Global station "Nepal Climate Observatory-Pyramid" (NCO-P) located in the high Khumbu valley at 5079 m a.s.l. in the foothills of Mt. Everest. PM10 aerosol samples were collected from July 2013 to November 2014. The sampling strategy was set up in order to discriminate the daytime valley breeze bringing polluted air masses up to the observatory and free tropospheric air during nighttime. Water-soluble BrC (WS-BrC) and methanol-soluble BrC (MeS-BrC) were extracted and analyzed using a UV/VIS spectrophotometer equipped with a 50 cm liquid waveguide capillary cell. In the polluted air masses, the highest levels of the BrC light absorption coefficient at 365 nm (babs365) were observed during the pre-monsoon season (1.83±1.46 Mm-1 for WS-BrC and 2.86±2.49 Mm-1 for MeS-BrC) and the lowest during the monsoon season (0.21±0.22 Mm-1 for WS-BrC and 0.32±0.29 Mm-1 for MeS-BrC). The pre-monsoon season is the most frequently influenced by a strong atmospheric brown cloud (ABC) transport to NCO-P due to increased convection and mixing layer height over South Asia combined with the highest up-valley wind speed and the increase of the emissions from open fires due to the agricultural practice along the Himalayas foothills and the Indo-Gangetic Plain. In contrast, the monsoon season is characterized by a weakened valley wind regime and an efficient removal of aerosols by wet scavenging. The wavelength dependence of the light absorption by BrC expressed as Ångström Exponent (AAE) within 330-500 nm was on average lower for MeS-BrC (3.9±1.1) compared to WS-BrC (4.8±0.8) and exhibited no diurnal or seasonal trend. The light absorption coefficient of BrC at 365 nm was about 13-17% (WS-BrC) and about 21-29% (MeS-BrC) of that of BC (AAEBC=1). Relative light absorption of BrC and BC considering the whole solar spectrum showed that at NCO-P WS-BrC absorbs 5±2% and MeS-BrC absorbs 12±7% compared to equivalent BC, as measured by Absorption Photometer (MAAP). These results are in line with previous in situ measurements at low altitude stations in South-East Asia, and do not support the strong enhancements of brown carbon absorption contribution in the upper part of the boundary layer and in the free troposphere suggested by remote sensing observations.

Optical Properties and Aging of Light Absorbing Secondary Organic Aerosol

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Jiumeng; Lin, Peng; Laskin, Alexander

2016-10-14

The light-absorbing organic aerosol (OA), commonly referred to as “brown carbon (BrC)”, has attracted considerable attention in recent years because of its potential to affect atmospheric radiation balance, especially in the ultraviolet region and thus impact photochemical processes. A growing amount of data has indicated that BrC is prevalent in the atmosphere, which has motivated numerous laboratory and field studies; however, our understanding of the relationship between the chemical composition and optical properties of BrC remains limited. We conducted chamber experiments to investigate the effect of various VOC precursors, NOx concentrations, photolysis time and relative humidity (RH) on the lightmore » absorption of selected secondary organic aerosols (SOA). Light absorption of chamber generated SOA samples, especially aromatic SOA, was found to increase with NOx concentration, at moderate RH, and for the shortest photolysis aging times. The highest mass absorption coefficients (MAC) value is observed from toluene SOA products formed under high NOx conditions at moderate RH, in which nitro-aromatics were previously identified as the major light absorbing compounds. BrC light absorption is observed to decrease with photolysis time, correlated with a decline of the organonitrate fraction of SOA. SOA formed from mixtures of aromatics and isoprene absorb less visible and UV light than SOA formed from aromatic precursors alone on a mass basis. However, the mixed-SOA absorption was underestimated when optical properties were predicted using a two-product SOA formation model, as done in many current climate models. Further investigation, including analysis on detailed mechanisms, are required to explain the discrepancy.« less

Long-term measurements of aerosols and carbon monoxide at the ZOTTO tall tower to characterize polluted and pristine air in the Siberian Taiga

NASA Astrophysics Data System (ADS)

Chi, X.; Winderlich, J.; Mayer, J.-C.; Panov, A. V.; Heimann, M.; Birmili, W.; Heintzenberg, J.; Cheng, Y.; Andreae, M. O.

2013-07-01

Siberia is one of few background regions in the Northern Hemisphere where the atmosphere may sometimes approach pristine conditions. We present the time series of aerosol and carbon monoxide (CO) measurements between September~2006 and December 2010 at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 90° E). We investigate the seasonal, weekly and diurnal variations of aerosol properties (including absorption and scattering coefficients and derived parameters, like equivalent black carbon (BCe), Ångström exponent, single scattering albedo, and backscattering ratio) and the CO mixing ratios. Criteria were established to distinguish polluted and near-pristine air masses and characterize them separately. Depending on the season, 15-47% of the sampling time at ZOTTO was representative of a clean atmosphere. The summer pristine data indicates that primary biogenic and/or secondary organic aerosol formation are quite strong particle sources in the Siberian Taiga. The summer seasons 2007-2008 are dominated by an Aitken mode of 80 nm size, whereas the summer 2009 with prevailing easterly winds produced aerosols in the accumulation mode around 200 nm size. We found these differences mainly related to air temperature, in parallel with production rates of biogenic volatile organic compounds (VOC). In winter, the footprint and aerosol size distribution (with a peak at 160 nm) of the clean background air are characteristic for aged aerosols from anthropogenic sources at great distances from ZOTTO and diluted biofuel burning emissions from heating. The wintertime polluted air originates from the large cities to the south and southwest of the site; these aerosols have a dominant mode around 100 nm, and the Δ BCe/Δ CO ratio of 7-11 ng m-3 ppb-1 suggests dominant contributions from coal and biofuel burning for heating. During summer, anthropogenic emissions are the dominant contributor to the pollution aerosols at ZOTTO, while only 12% of the polluted events are classified as biomass burning dominated, but then often associated with extremely high CO concentrations and aerosol absorption coefficients. Two biomass-burning case studies revealed different Δ BCe/Δ CO ratios from different fire types, with the agricultural fires in April 2008 yielding a very high ratio of 21 ng m-3 ppb-1. Overall, we find that anthropogenic sources dominate the aerosol population at our site most of the time, even during nominally clean episodes in winter, and that near-pristine conditions are encountered only episodically in the growing season.

Laboratory estimate of the regional shortwave refractive index and single scattering albedo of mineral dust from major sources worldwide

NASA Astrophysics Data System (ADS)

Di Biagio, C.; Formenti, P.; Caponi, L.; Cazaunau, M.; Pangui, E.; Journet, E.; Nowak, S.; Caquineau, S.; Andreae, M. O.; Kandler, K.; Saeed, T.; Piketh, S.; Seibert, D.; Williams, E.; Balkanski, Y.; Doussin, J. F.

2017-12-01

Mineral dust is one of the most abundant aerosol species in the atmosphere and strongly contributes to the global and regional direct radiative effect. Still large uncertainties persist on the magnitude and overall sign of the dust direct effect, where indeed one of the main unknowns is how much mineral dust absorbs light in the shortwave (SW) spectral range. Aerosol absorption is represented both by the imaginary part (k) of the complex refractive index or the single scattering albedo (SSA, i.e. the ratio of the scattering to extinction coefficient). In this study we present a new dataset of SW complex refractive indices and SSA for mineral dust aerosols obtained from in situ measurements in the 4.2 m3 CESAM simulation chamber at LISA (Laboratoire Interuniversitaire des Systemes Atmospheriques) in Créteil, France. Investigated dust aerosol samples were issued from major desert sources worldwide, including the African Sahara and Sahel, Eastern Asia, the Middle East, Southern Africa, Australia, and the Americas, with differing iron oxides content. Results from the present study provide a regional mapping of the SW absorption by dust and show that the imaginary part of the refractive index largely varies (by up to a factor 6, 0.003-0.02 at 370 nm and 0.001-0.003 at 950 nm) for the different source areas due to the change in the particle iron oxide content. The SSA for dust varies between 0.75-0.90 at 370 nm and 0.95-0.99 at 950 nm, with the largest absorption observed for Sahelian and Australian dust aerosols. Our range of variability for k and SSA is well bracketed by already published literature estimates, but suggests that regional‒dependent values should be used in models. The possible relationship between k and the dust iron oxides content is investigated with the aim of providing a parameterization of the regional‒dependent dust absorption to include in climate models.

Light extinction by fine atmospheric particles in the White Mountains region of New Hampshire and its relationship to air mass transport.

PubMed

Slater, John F; Dibb, Jack E; Keim, Barry D; Talbot, Robert W

2002-03-27

Chemical, optical, and physical measurements of fine aerosols (aerodynamic diameter < or = 2.5 microm) have been performed at a mountaintop location adjacent to the White Mountain National Forest in northern NH, USA. A 1-month long sampling campaign was conducted at Cranmore Mountain during spring 2000. We report on the apportionment of light extinction by fine aerosols into its major chemical components, and relationships between variations in aerosol parameters and changes in air mass origin. Filter-based, 24-h integrated samples were collected and analyzed for major inorganic ions, as well as organic (OC), elemental (EC), and total carbon. Light scattering and light absorption coefficients were measured at 5-min intervals using an integrating nephelometer and a light absorption photometer. Fine particle number density was measured with a condensation particle counter. Air mass origins and transport patterns were investigated through the use of 3-day backward trajectories and a synoptic climate classification system. Two distinct transport regimes were observed: (1) flow from the north/northeast (N/NE) occurred during 9 out of 18 sample-days; and (2) flow from the west/southwest (W/SW) occurred 8 out of 18 sample-days. All measured and derived aerosol and meteorological parameters were separated into two categories based on these different flow scenarios. During W/SW flow, higher values of aerosol chemical concentration, absorption and scattering coefficients, number density, and haziness were observed compared to N/NE flow. The highest level of haziness was associated with the climate classification Frontal Atlantic Return, which brought polluted air into the region from the mid-Atlantic corridor. Fine particle mass scattering efficiencies of (NH4)2SO4 and OC were 5.35 +/- 0.42 m2 g(-1) and 1.56 +/- 0.40 m2 g(-1), respectively, when transport was out of the N/NE. When transport was from the W/SW the values were 4.94 +/- 0.68 m2 g(-1) for (NH4)2SO4 and 2.18 +/- 0.91 m2 g(-1) for OC. EC mass absorption efficiency when transport was from the N/NE was 9.66 +/- 1.06 m2 g(-1) and 10.80 +/- 1.76 m2 g(-1) when transport was from the W/SW. Results from this work can be used to predict visual air quality in the White Mountain National Forest based on a forecasted synoptic climate classification and its associated visibility.

Biomass burning dominates brown carbon absorption in the rural southeastern United States

NASA Astrophysics Data System (ADS)

Washenfelder, R. A.; Attwood, A. R.; Brock, C. A.; Guo, H.; Xu, L.; Weber, R. J.; Ng, N. L.; Allen, H. M.; Ayres, B. R.; Baumann, K.; Cohen, R. C.; Draper, D. C.; Duffey, K. C.; Edgerton, E.; Fry, J. L.; Hu, W. W.; Jimenez, J. L.; Palm, B. B.; Romer, P.; Stone, E. A.; Wooldridge, P. J.; Brown, S. S.

2015-01-01

carbon aerosol consists of light-absorbing organic particulate matter with wavelength-dependent absorption. Aerosol optical extinction, absorption, size distributions, and chemical composition were measured in rural Alabama during summer 2013. The field site was well located to examine sources of brown carbon aerosol, with influence by high biogenic organic aerosol concentrations, pollution from two nearby cities, and biomass burning aerosol. We report the optical closure between measured dry aerosol extinction at 365 nm and calculated extinction from composition and size distribution, showing agreement within experiment uncertainties. We find that aerosol optical extinction is dominated by scattering, with single-scattering albedo values of 0.94 ± 0.02. Black carbon aerosol accounts for 91 ± 9% of the total carbonaceous aerosol absorption at 365 nm, while organic aerosol accounts for 9 ± 9%. The majority of brown carbon aerosol mass is associated with biomass burning, with smaller contributions from biogenically derived secondary organic aerosol.

Equivalent Black Carbon measurements and spectral analysis of absorption coefficient during a biomass burning episode in the city of Bogotá, Colombia.

NASA Astrophysics Data System (ADS)

Quirama, M.; Morales, R.

2016-12-01

Light-absorbing carbonaceous aerosol is recognized as a significant short lived climate pollutant that can contribute to direct and indirect radiative forcing. In urban environments, black carbon is an important contributor to the deterioration of local air quality. In this study, we report measurements of equivalent Black Carbon performed during the months of January, February, and March 2016 in the city of Bogotá, Colombia. During this period, a persistent condition of atmospheric stability lead to high concentrations of particulate matter throughout the city. During the month of February, the city was further impacted by a series of small-scale forest fires that took place on hills neighboring the city center. Equivalent Black Carbon (eBC) concentrations were monitored before, during, and after a mayor forest fire episode with a 7-wavelength Aethalometer. The monitoring instruments were located at a traffic impacted site, 18.3 km from the forest fire. To evaluate the contribution of biomass burning to the light-absorbing aerosol particle concentration, spectral analysis of the absorption coefficient of the sampled aerosol particles was performed. When the biomass burning plume directly impacted the monitoring station during the night of February 4, eBC concentrations of up to 40 µg/m3 were observed at nighttime. This concentration was significantly higher than average nighttime concentrations of eBC, observed to be 4 µg/m3 at the site. However, during the period most intensely affected by the biomass burning plume, the angstrom exponent computed between the 450nm and the 970 nm channel, was found to be close to 1. Angstrom exponent close to 1 is an indication that the contribution from traffic generated black carbon is dominant compared to the contribution of biomass burning. The data set collected during this period suggests that despite the significant contribution of the fresh biomass burning plume to the particulate matter concentration in the city, the spectral analysis of the light-absorption coefficient proved insufficient to detect the presence of UV absorbing carbonaceous material during this episode.

Identifying Aerosol Type/Mixture from Aerosol Absorption Properties Using AERONET

NASA Technical Reports Server (NTRS)

Giles, D. M.; Holben, B. N.; Eck, T. F.; Sinyuk, A.; Dickerson, R. R.; Thompson, A. M.; Slutsker, I.; Li, Z.; Tripathi, S. N.; Singh, R. P.;

Molecular Chemistry of Atmospheric Brown Carbon Inferred from a Nationwide Biomass Burning Event

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lin, Peng; Bluvshtein, Nir; Rudich, Yinon

Lag Ba'Omer, a nationwide bonfire festival in Israel, was chosen as a case study to investigate the influence of a major biomass burning event on the light absorption properties of atmospheric brown carbon (BrC). The chemical composition and optical properties of BrC chromophores were investigated using a high performance liquid chromatography (HPLC) platform coupled to photo diode array (PDA) and high resolution mass spectrometry (HRMS) detectors. Substantial increase of BrC light absorption coefficient was observed during the night-long biomass burning event. Most chromophores observed during the event were attributed to nitroaromatic compounds, comprising 28 elemental formulas of at least 63more » structural isomers. The NAC, in combination, accounted for 50-80% of the total visible light absorption (> 400 nm) by solvent extractable BrC. The results highlight that NAC, particular nitrophenols, are important light absorption contributors of biomass burning organic aerosol (BBOA), suggesting that night time chemistry of ·NO 3 and N 2O 5 with particles may play a significant role in atmospheric transformations of BrC. Nitrophenols and related compounds were especially important chromophores of BBOA. The absorption spectra of the BrC chromophores are influenced by the extraction solvent and solution pH, implying that the aerosol acidity is an important factor controlling the light absorption properties of BrC.« less

Molecular Chemistry of Atmospheric Brown Carbon Inferred from a Nationwide Biomass Burning Event

DOE PAGES

Lin, Peng; Bluvshtein, Nir; Rudich, Yinon; ...

2017-08-26

Lag Ba'Omer, a nationwide bonfire festival in Israel, was chosen as a case study to investigate the influence of a major biomass burning event on the light absorption properties of atmospheric brown carbon (BrC). The chemical composition and optical properties of BrC chromophores were investigated using a high performance liquid chromatography (HPLC) platform coupled to photo diode array (PDA) and high resolution mass spectrometry (HRMS) detectors. Substantial increase of BrC light absorption coefficient was observed during the night-long biomass burning event. Most chromophores observed during the event were attributed to nitroaromatic compounds, comprising 28 elemental formulas of at least 63more » structural isomers. The NAC, in combination, accounted for 50-80% of the total visible light absorption (> 400 nm) by solvent extractable BrC. The results highlight that NAC, particular nitrophenols, are important light absorption contributors of biomass burning organic aerosol (BBOA), suggesting that night time chemistry of ·NO 3 and N 2O 5 with particles may play a significant role in atmospheric transformations of BrC. Nitrophenols and related compounds were especially important chromophores of BBOA. The absorption spectra of the BrC chromophores are influenced by the extraction solvent and solution pH, implying that the aerosol acidity is an important factor controlling the light absorption properties of BrC.« less

Aerosol Absorption in the Atmosphere: Perspectives from Global Model, Ground-Based Measurements, and Field Observations

NASA Technical Reports Server (NTRS)

Chin, Mian; Dubovik, Oleg; Holben, Brent; Torres, Omar; Anderson, Tad; Quinn, Patricia; Ginoux, Paul

2004-01-01

Aerosol absorption in the atmosphere poses a major uncertainty in assessing the aerosol climate effects. This uncertainty arises from the poorly quantified aerosol sources, especially black carbon emissions, and our limited knowledge of aerosol mixing state and optical properties. Here we use a global model GOCART to simulate atmospheric aerosols, including sulfate, black carbon, organic carbon, dust, and sea salt. We compare the model calculated total aerosol optical thickness, extinction, and absorption with those quantities from the ground-based sun photometer measurements from AERONET, satellite retrievals from the TOMS instrument, and field observations from ACE-Asia. We will examine the most sensitive factors in determining the aerosol absorption. and the consequences of assessing the aerosol radiative forcing and atmospheric heating associated with those factors.

Aerosol Absorption in the Atmosphere: Perspectives from Global Model, Ground-Based Measurements, and Field Observations

NASA Technical Reports Server (NTRS)

Chin, Mian; Dubovik, Oleg; Holben, Brent; Anderson, Tad; Quinn, Patricia; Duncan, Bryan; Ginoux, Paul

2003-01-01

Aerosol absorption in the atmosphere poses a major uncertainty in assessing the aerosol climate effects. This uncertainty arises from the poorly quantified aerosol sources, especially black carbon emissions, and our limited knowledge of aerosol mixing state and optical properties. Here we use a global model GOCART to simulate atmospheric aerosols, including sulfate, black carbon, organic carbon, dust, and sea salt. We compare the model calculated total aerosol optical thickness, extinction, and absorption with those quantities from the ground-based sun photometer measurements from AERONET at several different wavelengths and the field observations from ACE-Asia. We will examine what are the most sensitive factors in determining the aerosol absorption, and the consequences of assessing the aerosol radiative forcing and atmospheric heating associated with those factors.

Aerosol Absorption in the Atmosphere: Perspectives from Global Model, Ground-Based Measurements, and Field Observations

NASA Technical Reports Server (NTRS)

Chin, Main; Dubovik, Oleg; Holben, Brent; Anderson, Tad; Quinn, Patricia; Duncan, Bryan; Ginoux, Paul

2004-01-01

Aerosol absorption in the atmosphere poses a major uncertainty in assessing the aerosol climate effects. This uncertainty arises from the poorly quantified aerosol sources, especially black carbon emissions, and our limited knowledge of aerosol mixing state and optical properties. Here we use a global model GOCART to simulate atmospheric aerosols, including sulfate, black carbon, organic carbon, dust, and sea salt. We compare the model calculated total aerosol optical thickness, extinction, and absorption with those quantities from the ground-based sun photometer measurements from AERONET at several different wavelengths and the field observations from ACE-Asia. We will examine the most sensitive factors in determining the aerosol absorption, and the consequences of assessing the aerosol radiative forcing and atmospheric heating associated with those factors.

Influence of Humidity on the Aerosol Scattering Coefficient and Its Effect on the Upwelling Radiance During ACE-2

NASA Technical Reports Server (NTRS)

Gasso, B. S.; Hegg, D. A.; Covert, D. S.; Collins, D.; Noone, K.; Oestroem, E.; Schmid, B.; Russell, P. B.; Livingston, J. M.; Durkee, P. A.;

Computation of Phase Equilibria, State Diagrams and Gas/Particle Partitioning of Mixed Organic-Inorganic Aerosols

NASA Astrophysics Data System (ADS)

Zuend, A.; Marcolli, C.; Peter, T.

2009-04-01

The chemical composition of organic-inorganic aerosols is linked to several processes and specific topics in the field of atmospheric aerosol science. Photochemical oxidation of organics in the gas phase lowers the volatility of semi-volatile compounds and contributes to the particulate matter by gas/particle partitioning. Heterogeneous chemistry and changes in the ambient relative humidity influence the aerosol composition as well. Molecular interactions between condensed phase species show typically non-ideal thermodynamic behavior. Liquid-liquid phase separations into a mainly polar, aqueous and a less polar, organic phase may considerably influence the gas/particle partitioning of semi-volatile organics and inorganics (Erdakos and Pankow, 2004; Chang and Pankow, 2006). Moreover, the phases present in the aerosol particles feed back on the heterogeneous, multi-phase chemistry, influence the scattering and absorption of radiation and affect the CCN ability of the particles. Non-ideal thermodynamic behavior in mixtures is usually described by an expression for the excess Gibbs energy, enabling the calculation of activity coefficients. We use the group-contribution model AIOMFAC (Zuend et al., 2008) to calculate activity coefficients, chemical potentials and the total Gibbs energy of mixed organic-inorganic systems. This thermodynamic model was combined with a robust global optimization module to compute potential liquid-liquid (LLE) and vapor-liquid-liquid equilibria (VLLE) as a function of particle composition at room temperature. And related to that, the gas/particle partitioning of semi-volatile components. Furthermore, we compute the thermodynamic stability (spinodal limits) of single-phase solutions, which provides information on the process type and kinetics of a phase separation. References Chang, E. I. and Pankow, J. F.: Prediction of activity coefficients in liquid aerosol particles containing organic compounds, dissolved inorganic salts, and water - Part 2: Consideration of phase separation effects by an XUNIFAC model, Atmos. Environ., 40, 6422-6436, 2006. Erdakos, G. B. and Pankow, J. F.: Gas/particle partitioning of neutral and ionizing compounds to single- and multi-phase aerosol particles. 2. Phase separation in liquid particulate matter containing both polar and low-polarity organic compounds, Atmos. Environ., 38, 1005-1013, 2004. Zuend, A., Marcolli, C., Luo, B. P., and Peter, T.: A thermodynamic model of mixed organic-inorganic aerosols to predict activity coefficients, Atmos. Chem. Phys., 8, 4559-4593, 2008.

Columnar characteristics of aerosols by spectroradiometer measurements in the maritime area of the Cadiz Gulf (Spain)

NASA Astrophysics Data System (ADS)

Vergaz, Ricardo; Cachorro, Victoria E.; de Frutos, Ángel M.; Vilaplana, José M.; de La Morena, Benito A.

2005-11-01

Atmospheric aerosol characteristics represented by the spectral aerosol optical depth AOD) and the Ångström turbidity parameter were determined in the coastal area of the Gulf of Cádiz, (southwest of Spain). The columnar aerosol properties presented here correspond to the 1996-1999 period, and were obtained by solar direct irradiance measurements carried out by a Licor1800 spectroradiometer. The performance of this type of medium-spectral resolution radiometric system is analysed over the measured period. The detailed spectral information of these irradiance measurements enabled the use of selected non-absorption gases spectral windows to determine the columnar spectral AOD that was modelled by Ångström formula to obtain the coefficient. Temporal evolutions of instantaneous values together with a general statistical analysis represented by seasonal values, frequency distributions and some representative correlations for the AOD and the derived Ångström coefficient gave us the first insight of aerosol characteristics in this coastal area. Special attention was paid to the analysis of these aerosol properties at the nominal wavelengths of 440 nm, 670 nm, 870 nm and 1020 nm for the near-future comparisons with the Cimel sun-photometer data. However, taking the most representative aerosol wavelength of 500 nm, the variability of the AOD ranges from 0.005 to 0.53, with a mean of 0.12 (s.d = 0.07) and that of the parameter is given by a mean value of 0.93 (s.d. = 0.58) falling inside the range of marine aerosols. A quantitative discrimination of aerosol types was conducted on the basis of the spectral aerosol properties and air mass back trajectory analysis, which resulted in a mixed type because of the specificity of this area, given by very frequent desert dust episodes, continental and polluted local influences. This study represents the first extended data characterization about columnar properties of aerosols in Spain which has been continued by Cimel-AERONET data. Copyright

Utilizing NASA Airborne Data to Investigate the Influence of Fuel Type on Biomass Burning Aerosol Properties

NASA Astrophysics Data System (ADS)

Odwuor, A.; Corr, C.; Griffin, R. J.; Pusede, S.; Anderson, B.; Beyersdorf, A. J.; Campuzano Jost, P.; Chen, G.; Day, D. A.; Diskin, G. S.; Jimenez, J. L.; Moore, R.; Nault, B.; Schwarz, J. P.; Shook, M.; Thornhill, K. L., II; Winstead, E.; Armin, W.; Ziemba, L. D.

2017-12-01

Climate models and satellite aerosol classification retrievals rely on well-characterized aerosol optical properties (e.g., scattering and absorption coefficients) that vary with aerosol type. However, generalized parameterizations of aerosol optical properties are weakened by actual variability in aerosol chemical and physical properties that arises from factors independent of aerosol source (e.g., meteorology). This is particularly true for biomass burning (BB) aerosol, which can vary in composition and size depending on burn conditions (e.g., smoldering versus flaming) and fuel. This work investigates the relationships between BB aerosol chemical, physical, and optical properties and fuel. We compare BB aerosol measured in fire plumes associated with distinct fuel types sampled during three NASA airborne research campaigns: boreal forest fires during the Arctic Research of the Troposphere from Aircraft and Satellites (ARCTAS) mission in Saskatchewan, Canada in July 2008; agricultural fires during the Studies of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS) over the continental U.S. in August/September 2013; and scrubland fires during the Student Airborne Research Program (SARP) mission in Southern California, U.S. in June 2016. Mean modified combustion efficiency values between 0.9 and 0.92 for the agricultural plumes and between 0.92 and 0.99 for the boreal and scrubland plumes indicate a significant flaming component to these fires. Despite similarities in burn conditions, SSA at 550nm was consistently lower for the agricultural and scrubland fires ( 0.92) compared to the boreal forest ( 0.96). While the ratio of black carbon to organic aerosol (OA) was similar among fires, differences in the OA were noted; f44/f60 ratios derived from Aerosol Mass Spectrometer OA measurements were consistently higher (>5) in scrubland and agricultural fires compared to boreal forest fires (<5). This suggests the amount of oxidized OA relative to fresh BB aerosol in fire plumes under flaming conditions may vary with fuel type and influence plume optical properties. The relationship between size distributions and optical properties is also explored in this work, with particular attention on the role of the coarse mode in aerosol absorption.

Analysis of derived optical parameters of atmospheric particles during a biomass burning event. Comparison with fossil fuel burning

NASA Astrophysics Data System (ADS)

Costa, A.; Mogo, S.; Cachorro, V.; de Frutos, A.; Medeiros, M.; Martins, R.; López, J. F.; Marcos, A.; Marcos, N.; Bizarro, S.; Mano, F.

2015-12-01

During the day November 26, 2014, a scheduled cleanup of the woods took place around the GOA-UVa aerosol measurement station located at the campus of the University of Beira Interior (40° 16’30”N, 7°30’35”W, 704m a.s.l.), Covilhã, Portugal. This cleanup included excessive vegetation removal during the morning, using fossil fuel-burning machinery, and burning of the vegetation during the afternoon. In situ measurements of aerosol optical properties were made and this study aims the characterization of the evolution of aerosol properties during the day. The optical parameters were monitored using a 3-wavelength nephelometer and a 3-wavelength particle soot absorption photometer. Selective sampling/exclusion of the coarse particles was done each 5 minutes. The scattering and absorption Ångström exponents as well as the single scattering albedo were derived and fully analyzed. The scattering and absorption coefficients increased dramatically during the event, reaching values as high as 720.3 Mm-1 and 181.9 Mm-1, respectively, for the green wavelength and PM10 size fraction. The spectral behavior of these parameters also changed wildly along the day and an inversion of the slope from positive to negative in the case of the single scattering albedo was observed.

Vertical profiles of BC direct radiative effect over Italy: high vertical resolution data and atmospheric feedbacks

NASA Astrophysics Data System (ADS)

Močnik, Griša; Ferrero, Luca; Castelli, Mariapina; Ferrini, Barbara S.; Moscatelli, Marco; Grazia Perrone, Maria; Sangiorgi, Giorgia; Rovelli, Grazia; D'Angelo, Luca; Moroni, Beatrice; Scardazza, Francesco; Bolzacchini, Ezio; Petitta, Marcello; Cappelletti, David

2016-04-01

Black carbon (BC), and its vertical distribution, affects the climate. Global measurements of BC vertical profiles are lacking to support climate change research. To fill this gap, a campaign was conducted over three Italian basin valleys, Terni Valley (Appennines), Po Valley and Passiria Valley (Alps), to characterize the impact of BC on the radiative budget under similar orographic conditions. 120 vertical profiles were measured in winter 2010. The BC vertical profiles, together with aerosol size distribution, aerosol chemistry and meteorological parameters, have been determined using a tethered balloon-based platform equipped with: a micro-Aethalometer AE51 (Magee Scientific), a 1.107 Grimm OPC (0.25-32 μm, 31 size classes), a cascade impactor (Siuotas SKC), and a meteorological station (LSI-Lastem). The aerosol chemical composition was determined from collected PM2.5 samples. The aerosol absorption along the vertical profiles was measured and optical properties calculated using the Mie theory applied to the aerosol size distribution. The aerosol optical properties were validated with AERONET data and then used as inputs to the radiative transfer model libRadtran. Vertical profiles of the aerosol direct radiative effect, the related atmospheric absorption and the heating rate were calculated. Vertical profile measurements revealed some common behaviors over the studied basin valleys. From below the mixing height to above it, a marked concentration drop was found for both BC (from -48.4±5.3% up to -69.1±5.5%) and aerosol number concentration (from -23.9±4.3% up to -46.5±7.3%). These features reflected on the optical properties of the aerosol. Absorption and scattering coefficients decreased from below the MH to above it (babs from -47.6±2.5% up to -71.3±3.0% and bsca from -23.5±0.8% up to -61.2±3.1%, respectively). Consequently, the Single Scattering Albedo increased above the MH (from +4.9±2.2% to +7.4±1.0%). The highest aerosol absorption was observed below the MH. The radiative power density absorbed into each atmospheric layer was normalized by the layer height to compare measurements taken at different sites with different vertical resolutions. The atmospheric absorption of radiative power below the MH ranged from +45.2±5.1 mW/m3 up to +103.3±16.2 mW/m3 and was ~2-3 times higher than above MH. The resulting heating rate was characterized by a vertical negative gradient with increasing height, from -2.6±0.2 K/(day km) up to -8.3±1.2 K/(day km), exerting a negative feedback on the atmospheric stability over basin valleys, weakening the ground-based thermal inversions and increasing the dispersal conditions.

Lidar investigations of ozone in the upper troposphere - lower stratosphere: technique and results of measurements

NASA Astrophysics Data System (ADS)

Romanovskii, O. A.; Burlakov, V. D.; Dolgii, S. I.; Nevzorov, A. A.; Nevzorov, A. V.; Kharchenko, O. V.

2016-12-01

Prediction of atmospheric ozone layer, which is the valuable and irreplaceable geo asset, is currently the important scientific and engineering problem. The relevance of the research is caused by the necessity to develop laser remote methods for sensing ozone to solve the problems of controlling the environment and climatology. The main aim of the research is to develop the technique for laser remote ozone sensing in the upper troposphere - lower stratosphere by differential absorption method for temperature and aerosol correction and analysis of measurement results. The report introduces the technique of recovering profiles of ozone vertical distribution considering temperature and aerosol correction in atmosphere lidar sounding by differential absorption method. The temperature correction of ozone absorption coefficients is introduced in the software to reduce the retrieval errors. The authors have determined wavelengths, promising to measure ozone profiles in the upper troposphere - lower stratosphere. We present the results of DIAL measurements of the vertical ozone distribution at the Siberian lidar station in Tomsk. Sensing is performed according to the method of differential absorption at wavelength pair of 299/341 nm, which are, respectively, the first and second Stokes components of SRS conversion of 4th harmonic of Nd:YAG laser (266 nm) in hydrogen. Lidar with receiving mirror 0.5 m in diameter is used to implement sensing of vertical ozone distribution in altitude range of 6-18 km. The recovered ozone profiles were compared with IASI satellite data and Kruger model. The results of applying the developed technique to recover the profiles of ozone vertical distribution considering temperature and aerosol correction in the altitude range of 6-18 km in lidar atmosphere sounding by differential absorption method confirm the prospects of using the selected wavelengths of ozone sensing 341 and 299 nm in the ozone lidar.

Optical properties and aging of light-absorbing secondary organic aerosol

DOE PAGES

Liu, Jiumeng; Lin, Peng; Laskin, Alexander; ...

2016-10-14

The light-absorbing organic aerosol (OA) commonly referred to as “brown carbon” (BrC) has attracted considerable attention in recent years because of its potential to affect atmospheric radiation balance, especially in the ultraviolet region and thus impact photochemical processes. A growing amount of data has indicated that BrC is prevalent in the atmosphere, which has motivated numerous laboratory and field studies; however, our understanding of the relationship between the chemical composition and optical properties of BrC remains limited. We conducted chamber experiments to investigate the effect of various volatile organic carbon (VOC) precursors, NO x concentrations, photolysis time, and relative humidity (RH) on the lightmore » absorption of selected secondary organic aerosols (SOA). Light absorption of chamber-generated SOA samples, especially aromatic SOA, was found to increase with NO x concentration, at moderate RH, and for the shortest photolysis aging times. The highest mass absorption coefficient (MAC) value is observed from toluene SOA products formed under high-NO x conditions at moderate RH, in which nitro-aromatics were previously identified as the major light-absorbing compounds. BrC light absorption is observed to decrease with photolysis time, correlated with a decline of the organic nitrate fraction of SOA. SOA formed from mixtures of aromatics and isoprene absorb less visible (Vis) and ultraviolet (UV) light than SOA formed from aromatic precursors alone on a mass basis. However, the mixed SOA absorption was underestimated when optical properties were predicted using a two-product SOA formation model, as done in many current climate models. Further investigation, including analysis on detailed mechanisms, are required to explain the discrepancy.« less

Radiative absorption enhancement from coatings on black carbon aerosols.

PubMed

Cui, Xinjuan; Wang, Xinfeng; Yang, Lingxiao; Chen, Bing; Chen, Jianmin; Andersson, August; Gustafsson, Örjan

2016-05-01

The radiative absorption enhancement of ambient black carbon (BC), by light-refractive coatings of atmospheric aerosols, constitutes a large uncertainty in estimates of climate forcing. The direct measurements of radiative absorption enhancement require the experimentally-removing the coating materials in ambient BC-containing aerosols, which remains a challenge. Here, the absorption enhancement of the BC core by non-absorbing aerosol coatings was quantified using a two-step removal of both inorganic and organic matter coatings of ambient aerosols. The mass absorption cross-section (MAC) of decoated/pure atmospheric BC aerosols of 4.4±0.8m(2)g(-1) was enhanced to 9.6±1.8m(2)g(-1) at 678-nm wavelength for ambiently-coated BC aerosols at a rural Northern China site. The enhancement of MAC (EMAC) rises from 1.4±0.3 in fresh combustion emissions to ~3 for aged ambient China aerosols. The three-week high-intensity campaign observed an average EMAC of 2.25±0.55, and sulfates were primary drivers of the enhanced BC absorption. Copyright © 2016 Elsevier B.V. All rights reserved.

Evaluating Model Parameterizations of Submicron Aerosol Scattering and Absorption with in situ Data from ARCTAS 2008

NASA Technical Reports Server (NTRS)

Alvarado, Matthew J.; Lonsdale, Chantelle R.; Macintyre, Helen L.; Bian, Huisheng; Chin, Mian; Ridley, David A.; Heald, Colette L.; Thornhill, Kenneth L.; Anderson, Bruce E.; Cubison, Michael J.;

Evaluating model parameterizations of submicron aerosol scattering and absorption with in situ data from ARCTAS 2008

NASA Astrophysics Data System (ADS)

Alvarado, Matthew J.; Lonsdale, Chantelle R.; Macintyre, Helen L.; Bian, Huisheng; Chin, Mian; Ridley, David A.; Heald, Colette L.; Thornhill, Kenneth L.; Anderson, Bruce E.; Cubison, Michael J.; Jimenez, Jose L.; Kondo, Yutaka; Sahu, Lokesh K.; Dibb, Jack E.; Wang, Chien

2016-07-01

Accurate modeling of the scattering and absorption of ultraviolet and visible radiation by aerosols is essential for accurate simulations of atmospheric chemistry and climate. Closure studies using in situ measurements of aerosol scattering and absorption can be used to evaluate and improve models of aerosol optical properties without interference from model errors in aerosol emissions, transport, chemistry, or deposition rates. Here we evaluate the ability of four externally mixed, fixed size distribution parameterizations used in global models to simulate submicron aerosol scattering and absorption at three wavelengths using in situ data gathered during the 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. The four models are the NASA Global Modeling Initiative (GMI) Combo model, GEOS-Chem v9-02, the baseline configuration of a version of GEOS-Chem with online radiative transfer calculations (called GC-RT), and the Optical Properties of Aerosol and Clouds (OPAC v3.1) package. We also use the ARCTAS data to perform the first evaluation of the ability of the Aerosol Simulation Program (ASP v2.1) to simulate submicron aerosol scattering and absorption when in situ data on the aerosol size distribution are used, and examine the impact of different mixing rules for black carbon (BC) on the results. We find that the GMI model tends to overestimate submicron scattering and absorption at shorter wavelengths by 10-23 %, and that GMI has smaller absolute mean biases for submicron absorption than OPAC v3.1, GEOS-Chem v9-02, or GC-RT. However, the changes to the density and refractive index of BC in GC-RT improve the simulation of submicron aerosol absorption at all wavelengths relative to GEOS-Chem v9-02. Adding a variable size distribution, as in ASP v2.1, improves model performance for scattering but not for absorption, likely due to the assumption in ASP v2.1 that BC is present at a constant mass fraction throughout the aerosol size distribution. Using a core-shell mixing rule in ASP overestimates aerosol absorption, especially for the fresh biomass burning aerosol measured in ARCTAS-B, suggesting the need for modeling the time-varying mixing states of aerosols in future versions of ASP.

Measurements of Nascent Soot Using a Cavity Attenauted Phase Shift (CAPS)-based Single Scattering Albedo Monitor

NASA Astrophysics Data System (ADS)

Freedman, A.; Onasch, T. B.; Renbaum-Wollf, L.; Lambe, A. T.; Davidovits, P.; Kebabian, P. L.

2015-12-01

Accurate, as compared to precise, measurement of aerosol absorption has always posed a significant problem for the particle radiative properties community. Filter-based instruments do not actually measure absorption but rather light transmission through the filter; absorption must be derived from this data using multiple corrections. The potential for matrix-induced effects is also great for organic-laden aerosols. The introduction of true in situ measurement instruments using photoacoustic or photothermal interferometric techniques represents a significant advance in the state-of-the-art. However, measurement artifacts caused by changes in humidity still represent a significant hurdle as does the lack of a good calibration standard at most measurement wavelengths. And, in the absence of any particle-based absorption standard, there is no way to demonstrate any real level of accuracy. We, along with others, have proposed that under the circumstance of low single scattering albedo (SSA), absorption is best determined by difference using measurement of total extinction and scattering. We discuss a robust, compact, field deployable instrument (the CAPS PMssa) that simultaneously measures airborne particle light extinction and scattering coefficients and thus the single scattering albedo (SSA) on the same sample volume. The extinction measurement is based on cavity attenuated phase shift (CAPS) techniques as employed in the CAPS PMex particle extinction monitor; scattering is measured using integrating nephelometry by incorporating a Lambertian integrating sphere within the sample cell. The scattering measurement is calibrated using the extinction measurement of non-absorbing particles. For small particles and low SSA, absorption can be measured with an accuracy of 6-8% at absorption levels as low as a few Mm-1. We present new results of the measurement of the mass absorption coefficient (MAC) of soot generated by an inverted methane diffusion flame at 630 nm. A value of 6.60 ±0.2 m2 g-1 was determined where the uncertainty refers to the precision of the measurement. The overall accuracy of the measurement, traceable to the properties of polystyrene latex particles, is estimated to be better than ±10%.

Formation of brown carbon via reactions of ammonia with secondary organic aerosols from biogenic and anthropogenic precursors

NASA Astrophysics Data System (ADS)

Updyke, Katelyn M.; Nguyen, Tran B.; Nizkorodov, Sergey A.

2012-12-01

Filter samples of secondary organic aerosols (SOA) generated from the ozone (O3)- and hydroxyl radical (OH)-initiated oxidation of various biogenic (isoprene, α-pinene, limonene, α-cedrene, α-humulene, farnesene, pine leaf essential oils, cedar leaf essential oils) and anthropogenic (tetradecane, 1,3,5-trimethylbenzene, naphthalene) precursors were exposed to humid air containing approximately 100 ppb of gaseous ammonia (NH3). Reactions of SOA compounds with NH3 resulted in production of light-absorbing "brown carbon" compounds, with the extent of browning ranging from no observable change (isoprene SOA) to visible change in color (limonene SOA). The aqueous phase reactions with dissolved ammonium (NH4+) salts, such as ammonium sulfate, were equally efficient in producing brown carbon. Wavelength-dependent mass absorption coefficients (MAC) of the aged SOA were quantified by extracting known amounts of SOA material in methanol and recording its UV/Vis absorption spectra. For a given precursor, the OH-generated SOA had systematically lower MAC compared to the O3-generated SOA. The highest MAC values, for brown carbon from SOA resulting from O3 oxidation of limonene and sesquiterpenes, were comparable to MAC values for biomass burning particles but considerably smaller than MAC values for black carbon aerosols. The NH3/NH4+ + SOA brown carbon aerosol may contribute to aerosol optical density in regions with elevated concentrations of NH3 or ammonium sulfate and high photochemical activity.

Photoacoustic and filter measurements related to aerosol light absorption during the Northern Front Range Air Quality Study (Colorado 1996/1997)

NASA Astrophysics Data System (ADS)

Moosmüller, H.; Arnott, W. P.; Rogers, C. F.; Chow, J. C.; Frazier, C. A.; Sherman, L. E.; Dietrich, D. L.

1998-11-01

A new photoacoustic instrument for the measurement of aerosol light absorption was collocated with conventional aerosol instrumentation during the 1996-1997 winter intensive monitoring period of the Northern Front Range Air Quality Study. Measurements of the light absorption efficiency for black carbon were 5 m2/g at 685 nm and 10 m2/g at 532 nm, and for elemental carbon, they were 3.6 m2/g at 685 nm. We show that these values together with previous photoacoustic measurements of aerosol light absorption shed some light on the wavelength dependence of absorption efficiency for carbonaceous aerosol in the visible and near-visible region. Integrating plate type filter measurements of aerosol light absorption result in far larger values than those measured with the photoacoustic instrument. We demonstrate that a recently published correction technique [Horvath, 1997] can yield improved agreement.

Spectral Absorption Properties of Atmospheric Aerosols

NASA Technical Reports Server (NTRS)

Bergstrom, R. W.; Pilewskie, P.; Russell, P. B.; Redemann, J.; Bond, T. C.; Quinn, P. K.; Sierau, B.

2007-01-01

We have determined the solar spectral absorption optical depth of atmospheric aerosols for specific case studies during several field programs (three cases have been reported previously; two are new results). We combined airborne measurements of the solar net radiant flux density and the aerosol optical depth with a detailed radiative transfer model for all but one of the cases. The field programs (SAFARI 2000, ACE Asia, PRIDE, TARFOX, INTEX-A) contained aerosols representing the major absorbing aerosol types: pollution, biomass burning, desert dust and mixtures. In all cases the spectral absorption optical depth decreases with wavelength and can be approximated with a power-law wavelength dependence (Absorption Angstrom Exponent or AAE). We compare our results with other recent spectral absorption measurements and attempt to briefly summarize the state of knowledge of aerosol absorption spectra in the atmosphere. We discuss the limitations in using the AAE for calculating the solar absorption. We also discuss the resulting spectral single scattering albedo for these cases.

Measurements and Modeling of Aerosol Absorption and Single Scattering Albedo at Ambient Relative Hum

NASA Technical Reports Server (NTRS)

Redemann, J.; Russell, P. B.; Hamill, P.

2000-01-01

Uncertainties in the aerosol single scattering albedo have been identified to be an important source of errors in current large-scale model estimates of the direct aerosol radiative forcing of climate. A number of investigators have obtained estimates of the single scattering albedo from a variety of remote sensing and in situ measurements during aerosol field experiments. During the Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX, 1996) for example, estimates of the aerosol single scattering albedo were obtained (1) as a best-fit parameter in comparing radiative flux changes measured by airborne pyranometer to those computed from independently measured aerosol properties; (2) from estimates of the aerosol complex index of refraction derived using a combination of airborne sunphotometer, lidar backscatter and in situ size distribution measurements; and (3) from airborne measurements of aerosol scattering and absorption using nephelometers and absorption photometers. In this paper, we briefly compare the results of the latter two methods for two TARFOX case studies, since those techniques provide height-resolved information about the aerosol single scattering albedo. Estimates of the aerosol single scattering albedo from nephelometer and absorption photometer measurements require knowledge of the scattering and absorption humidification (i.e., the increase in these properties in response to an increase in ambient relative humidity), since both measurements are usually carried out at a relative humidity different from the ambient atmosphere. In principle, the scattering humidification factor can be measured, but there is currently no technique widely available to measure the absorption of an aerosol sample as a function of relative humidity. Frequently, for lack of better knowledge, the absorption humidification is assumed to be unity (meaning that there is no change in aerosol absorption due to an increase in ambient relative humidity). This assumption then enters the estimate of the single scattering albedo at ambient relative humidity. To investigate the validity of this assumption we have carried out modeling studies of the absorption humidification factor, assuming that the aerosols contain an insoluble soot core and a coating which determines its hygroscopic growth behavior. The aerosol optical properties are then computed on the basis of the shell/core particle morphology using a Mie-code for concentric shells. From basic physical principles, it is conceivable that aerosol absorption increases when an atmospheric aerosol particle collects a non-absorbing shell, since the soot core is then exposed to an increased (focused) electric field strength. Indeed, our preliminary modeling studies show that the absorption of an atmospheric aerosol particle composed of a soot core and an aqueous sulfuric acid shell may increase by a factor of 50% due to a change in ambient relative humidity from 30 to 95%. We will show how this increased absorption is a function of the initial particle size and soot mass fraction.

Spectral Absorption Properties of Aerosol Particles from 350-2500nm

NASA Technical Reports Server (NTRS)

Martins, J. Vanderlei; Artaxo, Paulo; Kaufman, Yoram J.; Castanho, Andrea D.; Remer, Lorraine A.

2009-01-01

The aerosol spectral absorption efficiency (alpha (sub a) in square meters per gram) is measured over an extended wavelength range (350 2500 nm) using an improved calibrated and validated reflectance technique and applied to urban aerosol samples from Sao Paulo, Brazil and from a site in Virginia, Eastern US, that experiences transported urban/industrial aerosol. The average alpha (sub a) values (approximately 3 square meters per gram at 550 nm) for Sao Paulo samples are 10 times larger than alpha (sub a) values obtained for aerosols in Virginia. Sao Paulo aerosols also show evidence of enhanced UV absorption in selected samples, probably associated with organic aerosol components. This extra UV absorption can double the absorption efficiency observed from black carbon alone, therefore reducing by up to 50% the surface UV fluxes, with important implications for climate, UV photolysis rates, and remote sensing from space.

Aerosol Absorption and Radiative Forcing

NASA Technical Reports Server (NTRS)

Stier, Philip; Seinfeld, J. H.; Kinne, Stefan; Boucher, Olivier

2007-01-01

We present a comprehensive examination of aerosol absorption with a focus on evaluating the sensitivity of the global distribution of aerosol absorption to key uncertainties in the process representation. For this purpose we extended the comprehensive aerosol-climate model ECHAM5-HAM by effective medium approximations for the calculation of aerosol effective refractive indices, updated black carbon refractive indices, new cloud radiative properties considering the effect of aerosol inclusions, as well as by modules for the calculation of long-wave aerosol radiative properties and instantaneous aerosol forcing. The evaluation of the simulated aerosol absorption optical depth with the AERONET sun-photometer network shows a good agreement in the large scale global patterns. On a regional basis it becomes evident that the update of the BC refractive indices to Bond and Bergstrom (2006) significantly improves the previous underestimation of the aerosol absorption optical depth. In the global annual-mean, absorption acts to reduce the shortwave anthropogenic aerosol top-of-atmosphere (TOA) radiative forcing clear-sky from -0.79 to -0.53 W m(sup -2) (33%) and all-sky from -0.47 to -0.13W m(sup -2 (72%). Our results confirm that basic assumptions about the BC refractive index play a key role for aerosol absorption and radiative forcing. The effect of the usage of more accurate effective medium approximations is comparably small. We demonstrate that the diversity in the AeroCom land-surface albedo fields contributes to the uncertainty in the simulated anthropogenic aerosol radiative forcings: the usage of an upper versus lower bound of the AeroCom land albedos introduces a global annual-mean TOA forcing range of 0.19W m(sup -2) (36%) clear-sky and of 0.12W m(sup -2) (92%) all-sky. The consideration of black carbon inclusions on cloud radiative properties results in a small global annual-mean all-sky absorption of 0.05W m(sup -2) and a positive TOA forcing perturbation of 0.02W m(sup -2). The long-wave aerosol radiative effects are small for anthropogenic aerosols but become of relevance for the larger natural dust and sea-salt aerosols.

Quantitative retrieval of aerosol optical properties by means of ceilometers

NASA Astrophysics Data System (ADS)

Wiegner, Matthias; Gasteiger, Josef; Geiß, Alexander

2016-04-01

In the last few years extended networks of ceilometers have been established by several national weather services. Based on improvements of the hardware performance of these single-wavelength backscatter lidars and their 24/7 availability they are increasingly used to monitor mixing layer heights and to derive profiles of the particle backscatter profile. As a consequence they are used for a wide range of applications including the dispersion of volcanic ash plumes, validation of chemistry transport models and air quality studies. In this context the development of automated schemes to detect aerosol layers and to identify the mixing layer are essential, in particular as the latter is often used as a proxy for air quality. Of equal importance is the calibration of ceilometer signals as a pre-requisite to derive quantitative optical properties. Recently, it has been emphasized that the majority of ceilometers are influenced by water vapor absorption as they operate in the spectral range of 905 - 910 nm. If this effect is ignored, errors of the aerosol backscatter coefficient can be as large as 50%, depending on the atmospheric water vapor content and the emitted wavelength spectrum. As a consequence, any other derived quantity, e.g. the extinction coefficient or mass concentration, would suffer from a significant uncertainty in addition to the inherent errors of the inversion of the lidar equation itself. This can be crucial when ceilometer derived profiles shall be used to validate transport models. In this presentation, the methodology proposed by Wiegner and Gasteiger (2015) to correct for water vapor absorption is introduced and discussed.

Organic Aerosols from SÃO Paulo and its Relationship with Aerosol Absorption and Scattering Properties

NASA Astrophysics Data System (ADS)

Artaxo, P.; Brito, J. F.; Rizzo, L. V.

2012-12-01

The megacity of São Paulo with its 19 million people and 7 million cars is a challenge from the point of view of air pollution. High levels of organic aerosols, PM10, black carbon and ozone and the peculiar situation of the large scale use of ethanol fuel makes it a special case. Little is known about the impact of ethanol on air quality and human health and the increase of ethanol as vehicle fuel is rising worldwide An experiment was designed to physico-chemical properties of aerosols in São Paulo, as well as their optical properties. Aerosol size distribution in the size range of 1nm to 10 micrometers is being measured with a Helsinki University SMPS (Scanning Mobility Particle Sizer), an NAIS (Neutral ion Spectrometer) and a GRIMM OPC (Optical Particle Counter). Optical properties are being measured with a TSI Nephelometer and a Thermo MAAP (Multi Angle Absorption Photometer). A CIMEL sunphotometer from the AERONET network measure the aerosol optical depth. Furthermore, a Proton-Transfer-Reaction Mass Spectrometer (PTR-MS) and an Aerosol Chemical Speciation Monitor (ACSM) are used to real-time VOC analysis and aerosol composition, respectively. The ACSM was operated for 3 months continuosly during teh wintertime of 2012. The measured total particle concentration typically varies between 10,000 and 30,000 cm-3 being the lowest late in the night and highest around noon and frequently exceeding 50,000 cm-3. Clear diurnal patterns in aerosol optical properties were observed. Scattering and absorption coefficients typically range between 20 and 100 Mm-1 at 450 nm, and between 10 to 40 Mm-1 at 637 nm, respectively, both of them peaking at 7:00 local time, the morning rush hour. The corresponding single scattering albedo varies between 0.50 and 0.85, indicating a significant contribution of primary absorbing particles to the aerosol population. During the first month a total of seven new particle formation events were observed with growth rates ranging from 9 to 25 nm h-1. Interestingly enough there were also events were condensed vapors were evaporating from the condensed phase thus shrinking the size of the particles in all sizes. Aerosol optical thickness was relatively small at 0.1-0.3 at 500 nm, with high daily variability, showing how meteorological conditions are critical for the observed aerosol concentrations. The study allows the characterization of a unique fueled fleet emissions and its impact on atmospheric chemistry, particle formation and other atmospheric dynamic processes.

Estimation of the mass absorption cross-section of the black and brown carbon aerosols during GoPoEx 2014

NASA Astrophysics Data System (ADS)

Cho, C.; Kim, S. W.; Lee, M.; Gustafsson, O.; Fang, W.

2017-12-01

Black carbon (BC) is a major contributor to the atmospheric heating by absorbing the solar radiation. According to recent studies, the solar absorption of brown carbon (BrC) is not negligible and even comparable to that of BC at visible to UV wavelengths, but most optical instruments that quantify light absorption are unable to distinguish each other. Thus, light absorption properties of BC or BrC usually have been studied through modeling researches by using mass absorption cross-section (MAC). Although MAC has a large spatial and temporal variability, most modeling studies have used a specific value of BC MAC and even the absorption by BrC is seldom considered in most chemical and climate models. The generalization of modeling research can lead to serious errors of radiative forcing by BC and BrC. In this study, MAC of BC and BrC are separately determined and the contribution of BC and BrC on aerosol light absorption are estimated from co-located simultaneous in-situ measurements, COSMOS, CLAP and Sunset EC/OC analyzer, at Gosan climate observatory, Korea during Gosan Pollution Experiment in January 2014 (GoPoEx 2014). At 565 nm, MAC of BC is found to be about 6.4±1.5 m2 g-1 from COSMOS and Sunset EC/OC analyzer measurements. This value is similar to those from previous studies in China (Cui et al., STE, 2016), but lower than those observed to be ranged 10-18 m2 g-1 in America or Europe (Lack et al., PNAS, 2012). Aerosol absorption coefficient (AAC) and BC mass concentration from COSMOS, meanwhile, are approximately 15-20% lower than those of CLAP. This difference can be attributable to the contribution of BrC. The MAC of BrC was calculated using the absorption coefficient of BrC and by the following three methods: (1) the difference of mass concentration from Aethalometer and COSMOS applied new BC MAC of this study, (2) The mass concentration of water-soluble organic carbon, (3) a method using the mass concentration of organic carbon suggested by Chung et al. (ACP, 2012). The MAC of BrC values obtained from the three methods ranged from 1.0 m2 g-1 to 1.5 m2 g-1 at 565 nm which is slightly higher than those from previous studies (Srinivas et al., AE, 2016). The contribution of BC to AAC is estimated to be about 85-90%, while BrC accounts for about 10-15% of total AAC, having increases about 1% of BrC contribution when the BrC MAC value increases 10%.

Biomass Burning Dominates Brown Carbon Absorption in the Rural Southeastern U.S.

NASA Astrophysics Data System (ADS)

Washenfelder, R. A.; Attwood, A. R.; Brock, C. A.; Brown, S. S.; Guo, H.; Weber, R. J. J.; Xu, L.; Ng, N. L.; Stone, E. A.; Edgerton, E. S.; Baumann, K.; Hu, W.; Palm, B. B.; Jimenez, J. L.; Fry, J.; Ayres, B. R.; Draper, D.; Allen, H.

2014-12-01

Aerosol scattering and absorption are still among the largest uncertainties in quantifying radiative forcing. Brown carbon has a wavelength-dependent absorption that increases in the UV spectral region, and its major atmospheric sources include biomass burning, anthropogenic combustion of fossil fuels, and secondary organic aerosol. The rural Southeastern U.S. is influenced by high isoprene concentrations and varying concentrations of biomass burning aerosol, making it an ideal place to compare the relative contributions of these two sources to the brown carbon absorption budget. During the Southern Oxidant and Aerosol Study in summer 2013, we deployed a new field instrument that uses cavity enhanced spectroscopy with a broadband light source to measure aerosol optical extinction as a function of wavelength. The instrument consists of two broadband channels which span the 360-390 and 385-420 nm spectral regions using two light emitting diodes (LED) and a grating spectrometer with charge-coupled device (CCD) detector. We combine these data with direct absorption measurements of water-soluble organic carbon obtained from a novel UV/VIS-WSOC instrument, and with aerosol composition measurements. We examine these data sets to determine: 1) the optical closure between measured dry aerosol extinction and values calculated from aerosol composition and size distribution; 2) the magnitude of brown and black carbon absorption; 3) the relative contributions of biomass burning, anthropogenic, and secondary organic aerosol contributions to brown carbon absorption in the Southeast U.S. during the summer. We conclude that biomass burning is a major contributor to optical absorption by organic aerosol in the rural southeastern U.S.

Laboratory Measurements of Mass Specific Absorption Spectra for Suites of Black Carbon-like, Biomass Burning and Mineral Dust Aerosols

NASA Astrophysics Data System (ADS)

Radney, J.; Zangmeister, C.

2017-12-01

Light-absorbing atmospheric aerosols can be grouped into three categories: black carbon (BC), brown carbon (BrC) or mineral dust (MD). In many cases, the absorption of these species is best quantified using a mass-specific absorption cross section (MAC) since the particles are in the Rayleigh regime (BC) or optically thin (BrC and MD); notably, MAC values are both traceable to the SI and transferrable between photoacoustic spectroscopy and filter-based absorption measurements. Here, we present laboratory measurements of MAC for all three light-absorbing aerosol classes. Particles were size- and mass-selected using a differential mobility analyzer and aerosol particle mass analyzer, respectively, with absorption coefficients (αabs) and number concentrations (N) being measured by a broadband photoacoustic spectrometer and condensation particle counter, respectively. This suite of instrumentation allows for direct quantification of MAC from the measured parameters (MAC = αabs/Nmp). Further, the measurements contained > 8 data points spanning λ = 405 nm to 840 nm allowing for spectral curvatures (i.e. the Absorption Angstrom Exponent or AAE) to be fit from many data points versus the more common 2-point interpolations. For the carbonaceous, BC-like aerosols - five samples generated from flames, spark discharge soot (i.e. fullerene soot), graphene, reduced graphene oxide (rGO), and fullerene (C60) - we found: 1) measured MAC ranged between 2.4 m2 g-1 and 8.6 m2 g-1 at λ = 550 nm, 2) most AAEs ranged between 0.5 and 1.3; C60 AAE was 7.5 ± 0.9 and 3) MAC spectra were dependent on fuel type and formation conditions. For BrC particles generated from smoldering combustion of 3 hardwood (Oak, Hickory and Mesquite) and 3 softwood species (Western redcedar, Blue spruce and Baldcypress), we found: 1) median MAC values ranged from 1.4 x 10-2 m2 g-1 to 7.9 x 10-2 m2 g-1 at λ = 550 nm, 2) AAE values ranged between 3.5 and 6.2, and 3) Oak, Western redcedar and Blue spruce possessed statistically similar (p > 0.05) spectra while Hickory, Mesquite and Baldcypress were distinct (p < 0.01). Last, we measured seven dust and soil samples collected from across the continental U.S. and found: 1) absorption spectra can be classified as either brown/grey (AAE ≈ 3.5) or red (AAE > 4) and 2) the highest MAC at λ = 405 nm for all samples was ≈ 0.5 m2 g-1.

Investigating the Spectral Dependence of Biomass Burning Aerosol Optical Properties

NASA Astrophysics Data System (ADS)

Odwuor, A.; Corr, C.; Pusede, S.

2016-12-01

Aerosol optical properties, such as light absorption and scattering, are important for understanding how aerosols affect the global radiation budget and for comparison with data gathered from remote sensing. It has been established that the optical properties of aerosols are wavelength dependent, although some remote sensing measurements do not consider this. Airborne measurements of these optical properties were used to calculate the absorption Angstrom exponent, a parameter that characterizes the wavelength dependence of light absorption by aerosols, and single scattering albedo, which measures the relative magnitude of light scattering to total extinction (scattering and absorption combined). Aerosols produced by biomass burning in Saskatchewan, Canada in July 2008 and a forest fire in Southern California, U.S. in June 2016 were included in this analysis. These wildfires were sampled by the NASA DC-8 aircraft during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) and NASA Student Airborne Research Program (SARP) missions, respectively. Aerosol absorption was measured using a particle soot photometer (PSAP) at 470, 532 and 660 nm. Scattering was measured using a 3-wavelength (450, 550 and 700 nm) nephelometer. Absorption Angstrom exponents were calculated at 470 and 660 nm and single scattering albedos were calculated at 450 and 550 nm. Results of this study indicate that disregarding the wavelength dependence of organic aerosol can understate the positive radiative forcing (warming) associated with aerosol absorption.

Aerosol impacts on visible light extinction in the atmosphere of Mexico City.

PubMed

Eidels-Dubovoi, Silvia

2002-03-27

Eleven diurnal aerosol visible light absorption and scattering patterns were obtained from measurements done with an aethalometer and an integrating nephelometer during 28 February-10 March 1997 at two different sites in the Mexico City basin. Both measurement sites, the Merced site affected by regional and urban-scale aerosol and the Pedregal site dominated by regional-scale aerosol, showed a variety of diurnal light absorption and scattering patterns. For the majority of the 11 studied days, the highest absorption peaks appeared in the early morning, 07.00-09.30 h while those of scattering appeared later, 09.30-11.00 h. The earlier absorption peaks could be attributed to the elevated elemental carbon vehicular emissions during the heavy traffic hours whereas the later scattering peaks could be attributed to secondary aerosols formed photochemically in the atmosphere. During the period examined, the Pedregal site exhibited on the average a lower aerosol scattering and a higher aerosol absorption contribution to the total aerosol visible light extinction and a better visibility than that of the Merced site. Hence, the impact of aerosol absorption on the visibility degradation due to aerosols was greater at the less hazy Pedregal site. The overall 11-day aerosol visibility average of 20.9 km found at La Merced site, was only 9.4 km lower than that of 30.3 km found at the Pedregal site. This small aerosol visibility difference, of the order of the standard deviation, led to the conclusion that besides the regional-scale aerosol impact, the urban-scale aerosol impact on aerosol visible light extinction is very similar at La Merced and Pedregal sites.

Light absorption by secondary organic aerosol from α-pinene: Effects of oxidants, seed aerosol acidity, and relative humidity

DOE Office of Scientific and Technical Information (OSTI.GOV)

Song, Chen; Gyawali, Madhu; Zaveri, Rahul A.

2013-10-25

It is well known that light absorption from dust and black carbon aerosols has a warming effect on climate while light scattering from sulfate, nitrate, and sea salt aerosols has a cooling effect. However, there are large uncertainties associated with light absorption and scattering by different types of organic aerosols, especially in the near-UV and UV spectral regions. In this paper, we present the results from a systematic laboratory study focused on measuring light absorption by secondary organic aerosols (SOAs) generated from dark α-pinene + O 3 and α-pinene + NO x + O 3 systems in the presence ofmore » neutral and acidic sulfate seed aerosols. Light absorption was monitored using photoacoustic spectrometers at four different wavelengths: 355, 405, 532, and 870 nm. Significant light absorption at 355 and 405 nm was observed for the SOA formed from α-pinene + O 3 + NO 3 system only in the presence of highly acidic sulfate seed aerosols under dry conditions. In contrast, no absorption was observed when the relative humidity was elevated to greater than 27% or in the presence of neutral sulfate seed aerosols. Organic nitrates in the SOA formed in the presence of neutral sulfate seed aerosols were found to be nonabsorbing, while the light-absorbing compounds are speculated to be aldol condensation oligomers with nitroxy organosulfate groups that are formed in highly acidic sulfate aerosols. Finally and overall, these results suggest that dark α-pinene + O 3 and α-pinene + NO x + O 3 systems do not form light-absorbing SOA under typical atmospheric conditions.« less

Numerical simulation of infrared radiation absorption for diagnostics of gas-aerosol medium by remote sensing data

NASA Astrophysics Data System (ADS)

Voitsekhovskaya, O. K.; Egorov, O. V.; Kashirskii, D. E.; Shefer, O. V.

2015-11-01

Calculated absorption spectra of the mixture of gases (H2O, CO, CO2, NO, NO2, and SO2) and aerosol (soot and Al2O3), contained in the exhausts of aircraft and rocket engines are demonstrated. Based on the model of gas-aerosol medium, a numerical study of the spectral dependence of the absorptance for different ratios of gas and aerosol components was carried out. The influence of microphysical and optical properties of the components of the mixture on the spectral features of absorption of gas-aerosol medium was established.

LASE validation experiment: preliminary processing of relative humidity from LASE derived water vapor in the middle to upper troposphere

NASA Technical Reports Server (NTRS)

Brackett, Vincent G.; Ismail, Syed; Browell, Edward V.; Kooi, Susan A.; Clayton, Marian B.; Ferrare, Richard A.; Minnis, Patrick; Getzewich, Brian J.; Staszel, Jennifer

1998-01-01

Lidar Atmospheric Sensing Experiment (LASE) is the first fully engineered, autonomous airborne DIAL (Differentials Absorption Lidar) system to measure water vapor, aerosols, and clouds throughout the troposphere. This system uses a double-pulsed Ti:sapphire laser, which is pumped by a frequency-doubled flashlamp-pumped Nd: YAG laser, to transmit light in the 815 mn absorption band of water vapor. LASE operates by locking to a strong water vapor line and electronically tuning to any spectral position on the absorption line to choose the suitable absorption cross-section for optimum measurements over a range of concentrations in the atmosphere. During the LASE Validation Experiment, which was conducted over Wallops Island during September, 1995, LASE operated on either the strong water line for measurements in middle to upper troposphere, or on the weak water line for measurements made in the middle to lower troposphere including the boundary layer. Comparisons with water vapor measurements made by airborne dew point and frost point hygrometers, NASA/GSFC (Goddard Space Flight Center) Raman Lidar, and radiosondes showed the LASE water vapor mixing ratio measurements to have an accuracy of better than 6% or 0.01 g/kg, whichever is larger, throughout the troposphere. In addition to measuring water vapor mixing ratio profiles, LASE simultaneously measures aerosol backscattering profiles at the off-line wavelength near 815 nm from which atmospheric scattering ratio (ASR) profiles are calculated. ASR is defined as the ratio of total (aerosol + molecular) atmospheric scattering to molecular scattering. Assuming a region with very low aerosol loading can be identified, such as that typically found just below the tropopause, then the ASR can be determined. The ASR profiles are calculated by normalizing the scattering in the region containing enhanced aerosols to the expected scattering by the "clean" atmosphere at that altitude. Images of the total ASR clearly depict cloud regions, including multiple cloud layers, thin upper level cirrus, etc., throughout the troposphere. New data products that are being derived from the LASE aerosol and water measurements include: 1) aerosol extinction coefficient, 2) aerosol optical thickness, 3) precipitable water vapor, and 4) relative humidity (RH). These products can be compared with airborne in-situ, and ground and satellite remote sensing measurements,. This paper presents a preliminary examination of RH profiles in the middle to upper troposphere that are generated from LASE measured water vapor mixing ratio profiles coupled with rawinsonde profiles of temperature and pressure.

Molecular Characterization of Brown Carbon in Biomass Burning Aerosol Particles.

PubMed

Lin, Peng; Aiona, Paige K; Li, Ying; Shiraiwa, Manabu; Laskin, Julia; Nizkorodov, Sergey A; Laskin, Alexander

2016-11-01

Emissions from biomass burning are a significant source of brown carbon (BrC) in the atmosphere. In this study, we investigate the molecular composition of freshly emitted biomass burning organic aerosol (BBOA) samples collected during test burns of sawgrass, peat, ponderosa pine, and black spruce. We demonstrate that both the BrC absorption and the chemical composition of light-absorbing compounds depend significantly on the type of biomass fuels. Common BrC chromophores in the selected BBOA samples include nitro-aromatics, polycyclic aromatic hydrocarbon derivatives, and polyphenols spanning a wide range of molecular weights, structures, and light absorption properties. A number of biofuel-specific BrC chromophores are observed, indicating that some of them may be used as source-specific markers of BrC. On average, ∼50% of the light absorption in the solvent-extractable fraction of BBOA can be attributed to a limited number of strong BrC chromophores. The absorption coefficients of BBOA are affected by solar photolysis. Specifically, under typical atmospheric conditions, the 300 nm absorbance decays with a half-life of ∼16 h. A "molecular corridor" analysis of the BBOA volatility distribution suggests that many BrC compounds in the fresh BBOA have low saturation mass concentration (<1 μg m -3 ) and will be retained in the particle phase under atmospherically relevant conditions.

Remote Sensing of Non-Aerosol (anomalous) Absorption in Cloud Free Atmosphere

NASA Technical Reports Server (NTRS)

Kaufman, Yoram J.; Dubovik, Oleg; Smirnov, Alexander; Holben, Brent N.; Lau, William K. M. (Technical Monitor)

2001-01-01

The interaction of sunlight with atmospheric gases, aerosols and clouds is fundamental to the understanding of climate and its variation. Several studies questioned our understanding of atmospheric absorption of sunlight in cloudy or in cloud free atmospheres. Uncertainty in instruments' accuracy and in the analysis methods makes this problem difficult to resolve. Here we use several years of measurements of sky and sun spectral brightness by selected instruments of the Aerosol Robotic Network (AERONET), that have known and high measurement accuracy. The measurements taken in several locations around the world show that in the atmospheric windows 0.44, 0.06, 0.86 and 1.02 microns the only significant absorbers in cloud free atmosphere is aerosol and ozone. This conclusions is reached using a method developed to distinguish between absorption associated with the presence of aerosol and absorption that is not related to the presence of aerosol. Non-aerosol absorption, defined as spectrally independent or smoothly variable, was found to have an optical thickness smaller than 0.002 corresponding to absorption of sunlight less than 1W/sq m, or essentially zero.

The relative importance of aerosol scattering and absorption in remote sensing

NASA Technical Reports Server (NTRS)

Fraser, R. S.; Kaufman, Y. J.

1985-01-01

Previous attempts to explain the effect of aerosols on satellite measurements of surface properties for the visible and near-infrared spectrum have emphasized the amount of aerosols without consideration of their absorption properties. In order to estimate the importance of absorption, the radiances of the sunlight scattered from models of the earth-atmosphere system are computed as functions of the aerosol optical thickness and absorption. The absorption effect is small where the surface reflectance is weak, but is important for strong reflectance. These effects on classification of surface features, measuring vegetation index, and measuring surface reflectance are presented.

Aerosol Optical Properties and Chemical Composition Measured on the Ronald H. Brown During ACE-Asia

NASA Astrophysics Data System (ADS)

Quinn, P. K.; Bates, T. S.; Miller, T. L.; Coffman, D.

2001-12-01

Measurements of aerosol chemical, physical, and optical properties were made onboard the NOAA R/V Ronald H. Brown during the ACE-Asia Intensive Field Program to characterize Asian aerosol as it was transported across the Pacific Ocean. The ship traveled across the Pacific from Hawaii to Japan and into the East China Sea and the Sea of Japan. Trajectories indicate that remote marine air masses were sampled on the transit to Japan. In the ACE-Asia study region air masses from Japan, China, Mongolia, and the Korea Peninsula were sampled. A variety of aerosol types were encountered including those of marine, volcanic, crustal, and industrial origin. Presented here, for the different air masses encountered, are aerosol optical properties (scattering and absorption coefficients, single scattering albedo, Angstrom Exponent, and aerosol optical depth) and chemical composition (major ions, total organic and black carbon, and trace elements). Scattering by submicron aerosol (55 % RH and 550 nm) was less than 20 1/Mm during the transit from Hawaii to Japan. In continental air masses, values ranged from 60 to 320 1/Mm with the highest submicron scattering coefficients occurring during prefrontal conditions with a low marine boundary layer height and trajectories from Japan. For the continental air masses, the ratio of scattering by submicron to sub-10 micron aerosol during polluted conditions averaged 0.8 and during a dust event 0.41. Aerosol optical depth (500 nm) ranged from 0.08 during the Pacific transit to 1.3 in the prefrontal conditions described above. Optical depths during dust events ranged from 0.2 to 0.6. Submicron non-sea salt (nss) sulfate concentrations ranged from 0.5 ug/m-3 during the Pacific transit to near 30 ug/m-3 during the prefrontal conditions described above. Black carbon to total carbon mass ratios in air masses from Asia averaged 0.18 with highest values (0.32) corresponding to trajectories crossing the Yangtze River valley.

Inter-Comparison of ILAS-II Version 1.4 Aerosol Extinction Coefficient at 780 nm with SAGE II, SAGE III, and POAM III Aerosol Data

NASA Technical Reports Server (NTRS)

Saitoh, Naoko; Hayashida, S.; Sugita, T.; Nakajima, H.; Yokota, T.; Hayashi, M.; Shiraishi, K.; Kanzawa, H.; Ejiri, M. K.; Irie, H.;

The complex refractive index of atmospheric and model humic-like substances (HULIS) retrieved by a cavity ring down aerosol spectrometer (CRD-AS).

PubMed

Dinar, E; Riziq, A Abo; Spindler, C; Erlick, C; Kiss, G; Rudich, Y

2008-01-01

Atmospheric aerosols absorb and reflect solar radiation causing surface cooling and heating of the atmosphere. The interaction between aerosols and radiation depends on their complex index of refraction, which is related to the particles' chemical composition. The contribution of light absorbing organic compounds, such as HUmic-LIke Substances (HULIS) to aerosol scattering and absorption is among the largest uncertainties in assessing the direct effect of aerosols on climate. Using a Cavity Ring Down Aerosol Spectrometer (CRD-AS), the complex index of refraction of aerosols containing HULIS extracted from pollution, smoke, and rural continental aerosols, and molecular weight-fractionated fulvic acid was measured at 390 nm and 532 nm. The imaginary part of the refractive index (absorption) substantially increases towards the UV range with increasing molecular weight and aromaticity. At both wavelengths, HULIS extracted from pollution and smoke particles absorb more than HULIS from the rural aerosol. Sensitivity calculations for a pollution-type aerosol containing ammonium sulfate, organic carbon (HULIS), and soot suggests that accounting for absorption by HULIS leads in most cases to a significant decrease in the single scattering albedo and to a significant increase in aerosol radiative forcing efficiency, towards more atmospheric absorption and heating. This indicates that HULIS in biomass smoke and pollution aerosols, in addition to black carbon, can contribute significantly to light absorption in the ultraviolet and visible spectral regions.

Influence of Humidity On the Aerosol Scattering Coefficient and Its Effect on the Upwelling Radiance During ACE-2

NASA Technical Reports Server (NTRS)

Gasso, S.; Hegg, D. A.; Covert, D. S.; Collins, D.; Noone, K. J.; Oestroem, E.; Schmid, B.; Russell, P. B.; Livingston, J. M.; Durkee, P. A.

2000-01-01

Aerosol scattering coefficients (sigma(sub sp)) have been measured over the ocean at different relative humidities (RH) as a function of altitude in the region surrounding the Canary Islands during the Second Aerosol Characterization Experiment (ACE-2) in June and July 1997. The data were collected by the University of Washington passive humidigraph (UWPH) mounted on the Pelican research aircraft. Concurrently, particle size distributions, absorption coefficients and aerosol optical depth were measured throughout 17 flights. A parameterization of sigma(sub sp) as a function of RH was utilized to assess the impact of aerosol hydration on the upwelling radiance (normalized to the solar constant and cosine of zenith angle). The top of the atmosphere radiance signal was simulated at wavelengths corresponding to visible and near-infrared bands of the EOS (Earth Observing System) AM-1 (Terra) detectors, MODIS (Moderate Resolution Imaging Spectroradiometer) and MISR (Multi-angle Imaging Spectroradiometer). The UWPH measured sigma(sub sp) at two RHs, one below and the other above ambient conditions. Ambient sigma(sub sp) was obtained by interpolation of these two measurements. The data were stratified in terms of three types of aerosols: Saharan dust, clean marine (marine boundary layer background) and polluted marine aerosols (i.e., two- or one-day old polluted aerosols advected from Europe). An empirical relation for the dependence of sigma(sub sp) on RH, defined by sigma(sub sp)(RH) = k.(1 - RH/100)(sup gamma), was used with the hygroscopic exponent gamma derived from the data. The following gamma values were obtained for the 3 aerosol types: gamma(dust) = 0.23 +/- 0.05, gamma(clean marine) = 0.69 +/- 0.06 and gamma(polluted marine) = 0.57 +/- 0.06. Based on the measured gammas, the above equation was utilized to derive aerosol models with different hygroscopicities. The satellite simulation signal code 6S was used to compute the upwelling radiance corresponding to each of those aerosol models at several ambient humidities. For the prelaunch estimated precision of the sensors and the assumed viewing geometry of the instrument, the simulations suggest that the spectral and angular dependence of the reflectance measured by MISR is not sufficient to distinguish aerosol models with various different combinations of values for dry composition, gamma and ambient RH. A similar behavior is observed for MODIS at visible wavelengths. However, the 2100 nm band of MODIS appears to be able to differentiate between at least same aerosol models with different aerosol hygroscopicity given the MODIS calibration error requirements. This result suggests the possibility of retrieval of aerosol hygroscopicity by MODIS.

Influences of external vs. core-shell mixing on aerosol optical properties at various relative humidities.

PubMed

Ramachandran, S; Srivastava, Rohit

2013-05-01

Aerosol optical properties of external and core-shell mixtures of aerosol species present in the atmosphere are calculated in this study for different relative humidities. Core-shell Mie calculations are performed using the values of radii, refractive indices and densities of aerosol species that act as core and shell, and the core-shell radius ratio. The single scattering albedo (SSA) is higher when the absorbing species (black carbon, BC) is the core, while for a sulfate core SSA does not vary significantly as the BC in the shell dominates the absorption. Absorption gets enhanced in core-shell mixing of absorbing and scattering aerosols when compared to their external mixture. Thus, SSA is significantly lower for a core-shell mixture than their external mixture. SSA is more sensitive to core-shell ratio than mode radius when BC is the core. The extinction coefficient, SSA and asymmetry parameter are higher for external mixing when compared to BC (core)-water soluble aerosol (shell), and water soluble aerosol (core)-BC (shell) mixtures in the relative humidity range of 0 to 90%. Spectral SSA exhibits the behaviour of the species which acts as a shell in core-shell mixing. The asymmetry parameter for an external mixture of water soluble aerosol and BC is higher than BC (core)-water soluble aerosol (shell) mixing and increases as function of relative humidity. The asymmetry parameter for the water soluble aerosol (core)-BC (shell) is independent of relative humidity as BC is hydrophobic. The asymmetry parameter of the core-shell mixture decreases when BC aerosols are involved in mixing, as the asymmetry parameter of BC is lower. Aerosol optical depth (AOD) of core-shell mixtures increases at a higher rate when the relative humidity exceeds 70% in continental clean and urban aerosol models, whereas AOD remains the same when the relative humidity exceeds 50% in maritime aerosol models. The SSA for continental aerosols varies for core-shell mixing of water soluble aerosol (core)-shell (BC) when compared to their external mixture, while the SSA for maritime aerosols does not vary significantly for different mixing scenarios because of the dominance of sea salt aerosols. Thus, these results confirm that aerosol mixing can modify the physical and optical characteristics of aerosols, which vary as a function of relative humidity. These calculations will be useful in parameterising the effect of core-shell vs. external mixing of aerosols in global climate models, and in the evaluation of aerosol radiative effects.

Molecular Characterization of Brown Carbon (BrC) Chromophores in Secondary Organic Aerosol Generated From Photo-Oxidation of Toluene

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lin, Peng; Liu, Jiumeng; Shilling, John E.

Atmospheric Brown carbon (BrC) is a significant contributor to light absorption and climate forcing. However, little is known about a fundamental relationship between the chemical composition of BrC and its optical properties. In this work, light-absorbing secondary organic aerosol (SOA) was generated in the PNNL chamber from toluene photo-oxidation in the presence of NOx (Tol-SOA). Molecular structures of BrC components were examined using nanospray desorption electrospray ionization (nano-DESI) and liquid chromatography (LC) combined with UV/Vis spectroscopy and electrospray ionization (ESI) high-resolution mass spectrometry (HRMS). The chemical composition of BrC chromophores and the light absorption properties of toluene SOA (Tol-SOA) dependmore » strongly on the initial NOx concentration. Specifically, Tol-SOA generated under high-NOx conditions (defined here as initial NOx/toluene of 5/1) appears yellow and mass absorption coefficient of the bulk sample (MACbulk@365nm = 0.78 m2 g-1) is nearly 80 fold higher than that measured for the Tol-SOA sample generated under low-NOx conditions (NOx/toluene < 1/300). Fifteen compounds, most of which are nitrophenols, are identified as major BrC chromophores responsible for the enhanced light absorption of Tol-SOA material produced in the presence of NOx. The integrated absorbance of these fifteen chromophores accounts for 40-60% of the total light absorbance by Tol-SOA at wavelengths between 300 nm and 500 nm. The combination of tandem LC-UV/Vis-ESI/HRMS measurements provides an analytical platform for predictive understanding of light absorption properties by BrC and their relationship to the structure of individual chromophores. General trends in the UV/vis absorption by plausible isomers of the BrC chromophores were evaluated using theoretical chemistry calculations. The molecular-level understanding of BrC chemistry is helpful for better understanding the evolution and behavior of light absorbing aerosols in the atmosphere.« less

Formation of nitrogen- and sulfur-containing light-absorbing compounds accelerated by evaporation of water from secondary organic aerosols

NASA Astrophysics Data System (ADS)

Nguyen, Tran B.; Lee, Paula B.; Updyke, Katelyn M.; Bones, David L.; Laskin, Julia; Laskin, Alexander; Nizkorodov, Sergey A.

2012-01-01

Aqueous extracts of secondary organic aerosols (SOA) generated from the ozonolysis of d-limonene were subjected to dissolution, evaporation, and re-dissolution in the presence and absence of ammonium sulfate (AS). Evaporation with AS at pH 4-9 produced chromophores that were stable with respect to hydrolysis and had a distinctive absorption band at 500 nm. Evaporation accelerated the rate of chromophore formation by at least three orders of magnitude compared to the reaction in aqueous solution, which produced similar compounds. Absorption spectroscopy and high-resolution nanospray desorption electrospray ionization (nano-DESI) mass spectrometry experiments suggested that the molar fraction of the chromophores was small (<2%), and that they contained nitrogen atoms. Although the colored products represented only a small fraction of SOA, their large extinction coefficients (>105 L mol-1 cm-1 at 500 nm) increased the effective mass absorption coefficient of the residual organics in excess of 103 cm2 g-1 - a dramatic effect on the optical properties from minor constituents. Evaporation of SOA extracts in the absence of AS resulted in the production of colored compounds only when the SOA extract was acidified to pH ˜ 2 with sulfuric acid. These chromophores were produced by acid-catalyzed aldol condensation, followed by a conversion into organosulfates. The presence of organosulfates was confirmed by high resolution mass spectrometry experiments. Results of this study suggest that evaporation of cloud or fog droplets containing dissolved organics leads to significant modification of the molecular composition and serves as a potentially important source of light-absorbing compounds.

The analysis of in situ and retrieved aerosol properties measured during three airborne field campaigns

NASA Astrophysics Data System (ADS)

Corr, Chelsea A.

Aerosols can directly influence climate, visibility, and photochemistry by scattering and absorbing solar radiation. Aerosol chemical and physical properties determine how efficiently a particle scatters and/or absorbs incoming short-wave solar radiation. Because many types of aerosol can act as nuclei for cloud droplets (CCN) and a smaller population of airborne particles facilitate ice crystal formation (IN), aerosols can also alter cloud-radiation interactions which have subsequent impacts on climate. Thus aerosol properties determine the magnitude and sign of both the direct and indirect impacts of aerosols on radiation-dependent Earth System processes. This dissertation will fill some gaps in our understanding of the role of aerosol properties on aerosol absorption and cloud formation. Specifically, the impact of aerosol oxidation on aerosol spectral (350nm < lambda< 500nm) absorption was examined for two biomass burning plumes intercepted by the NASA DC-S aircraft during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission in Spring and Summer 2008. Spectral aerosol single scattering albedo (SSA) retrieved using actinic flux measured aboard the NASA DC-8 was used to calculate the aerosol absorption Angstrom exponents (AAE) for a 6-day-old plume on April 17 th and a 3-hour old plume on June 29th. Higher AAE values for the April 17th plume (6.78+/-0.38) indicate absorption by aerosol was enhanced in the ultraviolet relative to the visible portion of the short-wave spectrum in the older plume compared to the fresher plume (AAE= 3.34 0.11). These differences were largely attributed to the greater oxidation of the organic aerosol in the April 17th plume which can arise either from the aging of primary organic aerosol or the formation of spectrally-absorbing secondary organic aerosol. The validity of the actinic flux retrievals used above were also evaluated in this work by the comparison of SSA retrieved using actinic flux (AF SSA) to those retrieved using ratios of direct and diffuse irradiance (DDR SSA) at four wavelengths: 332, 368, 415, and 500 mn. Both actinic flux and irradiance were measured atop the University of Houston's Moody Tower in Houston, TX as part of the Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) mission in September 2013. AF SSA values were consistently lower than DDR SSAs with largest offsets observed when aerosol optical depths was < ~0.2. AF SSA were also lower than those reported by the AErosol RObotic NETwork (AERONET) and column-averaged values calculated from aerosol scattering and absorption coefficients measured aboard the NASA P3-B aircraft at 450 and 550 nm. However, AAE values calculated from AF SSAs compared well to AERONET and column-averaged AAEs suggesting actinic flux retrievals can correctly resolve the spectral dependence of aerosol absorption. Recent work has suggested that mineral dust is the most important IN found in both anvil and synoptically formed cirrus clouds over North America. The vertical transport processes sustaining significant mineral dust in the upper troposphere (> 9 km) where these clouds form are not well understood, but deep convective systems (thunder storms) likely play a role. Bulk aerosol Ca2+ concentrations and volume size distributions were measured aboard the NASA DC-8 during the NCAR Deep Convective Clouds and Chemistry Experiment (DC-3) conducted in May/June 2012 in both the inflow and outflow regions of twelve isolated, high cloud base storms over CO and OK. Outflow/inflow ratios of both Ca2+ and total coarse (limn < diameter < 5 microm) aerosol volume (Vc)were high (> ~0.9) suggesting a significant fraction of ingested coarse mode dust was transported through these systems. Elevated Ca2+ and Vc in the outflow were most likely not artifacts of ice shattering given the general absence of a relationship between these parameters and two ice concentration measurements (e.g., ice water content, 2D-S particle concentrations). Because mineral dust is an efficient IN, unactivated mineral dust particles are not expected in cold clouds. However, for these storms, inflow total coarse (0.5 microm < diameter < 5 microm) aerosol number (Nc)generally exceeded anvil cirrus ice particle concentrations, supporting the presence of interstitial dust in storm outflow. Thus efficient IN were likely made available in the upper troposphere by these twelve convective systems.

The influence of different black carbon and sulfate mixing methods on their optical and radiative properties

NASA Astrophysics Data System (ADS)

Zhang, Hua; Zhou, Chen; Wang, Zhili; Zhao, Shuyun; Li, Jiangnan

2015-08-01

Three different internal mixing methods (Core-Shell, Maxwell-Garnett, and Bruggeman) and one external mixing method are used to study the impact of mixing methods of black carbon (BC) with sulfate aerosol on their optical properties, radiative flux, and heating rate. The optical properties of a mixture of BC and sulfate aerosol particles are considered for three typical bands. The results show that mixing methods, the volume ratio of BC to sulfate, and relative humidity have a strong influence on the optical properties of mixed aerosols. Compared to internal mixing, external mixing underestimates the particle mass absorption coefficient by 20-70% and the particle mass scattering coefficient by up to 50%, whereas it overestimates the particle single scattering albedo by 20-50% in most cases. However, the asymmetry parameter is strongly sensitive to the equivalent particle radius, but is only weakly sensitive to the different mixing methods. Of the internal methods, there is less than 2% difference in all optical properties between the Maxwell-Garnett and Bruggeman methods in all bands; however, the differences between the Core-Shell and Maxwell-Garnett/Bruggeman methods are usually larger than 15% in the ultraviolet and visible bands. A sensitivity test is conducted with the Beijing Climate Center Radiation transfer model (BCC-RAD) using a simulated BC concentration that is typical of east-central China and a sulfate volume ratio of 75%. The results show that the internal mixing methods could reduce the radiative flux more effectively because they produce a higher absorption. The annual mean instantaneous radiative force due to BC-sulfate aerosol is about -3.18 W/m2 for the external method and -6.91 W/m2 for the internal methods at the surface, and -3.03/-1.56/-1.85 W/m2 for the external/Core-Shell/(Maxwell-Garnett/Bruggeman) methods, respectively, at the tropopause.

Chemical and physical characteristics of long-range transport submicron particles at the central Tibet Plateau

NASA Astrophysics Data System (ADS)

Xu, J.; Zhang, Q.; Shi, J.; Ge, X.; Xie, C.; Wang, J.

2016-12-01

Tibetan Plateau, the biggest and highest plateau on the Earth, is an ideal location for studying long range transport of air pollution due to the minimum of local emission. Recent studies in this region have revealed a significant influx of air pollution from south Asia during pre-monsoon period because of the favorable atmospheric circulation and less precipitation. In order to characterize the chemical composition of aerosol particles in this pristine area and elucidate the sources and optical properties of transported aerosol pollutants, we conducted an intensive field study during June 2015 at a high elevation station (4730 m a.s.l) on the central Tibetan Plateau by deploying a suite of advanced instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a nephelometer, and a multi-angle absorption photometer (MAAP). The average mass concentration of submicron particular matter (PM1) for the whole campaign period was 1.85 µg m-3, with organics accounting for 64% of the mass, followed by sulfate (16%), black carbon (9%), ammonium (8%), and nitrate (3%). The mass concentrations and chemical properties of PM1 were significantly different between pre-monsoon and monsoon periods. Elevated aerosol pollution episodes were observed during pre-monsoon period, while aerosol concentrations were persistently low during monsoon period. Aerosol composition was generally similar during the whole campaign period. However, organic aerosol was more oxidized during premonsoon period with an average atomic oxygen-to-carbon (O/C) ratio of = 0.7 compared to O/C = 0.52 during monsoon period. HYSPLIT trajectory calculations revealed that most of the arriving air masses traveled long distances (>1,000 km) and went through the northwest of India during premonsoon period. Positive matrix factorization of the HR-ToF-AMS spectra of organic aerosol identified two oxygenated organic aerosol (OOA) factors - a less oxidized OOA (LO-OOA) and a more oxidized OOA (MO-OOA). Further, the temporal variation of aerosol optical properties including aerosol extinction, scattering, absorption coefficients and single scattering, and chemical impacts on these optical properties are statistically evaluated.

Aerosol Absorption Effects in the TOMS UV Algorithm

NASA Technical Reports Server (NTRS)

Torres, O.; Krotkov, N.; Bhartia, P. K.

2004-01-01

The availability of global long-term estimates of surface UV radiation is very important, not only for preventive medicine considerations, but also as an important tool to monitor the effects of the stratospheric ozone recovery expected to occur in the next few decades as a result of the decline of the stratospheric chlorine levels. In addition to the modulating effects of ozone and clouds, aerosols also affect the levels of UV-A and W-B radiation reaching the surface. Oscillations in surface W associated with the effects of aerosol absorption may be comparable in magnitude to variations associated with the stratospheric ozone recovery. Thus, the accurate calculation of surface W radiation requires that both the scattering and absorption effects of tropospheric aerosols be taken into account. Although absorption effects of dust and elevated carbonaceous aerosols are already accounted for using Aerosol Index technique, this approach does not work for urban/industrial aerosols in the planetary boundary layer. The use of the new TOMS long-term global data record on UV aerosol absorption optical depth, can improve the accuracy of TOMS spectral UV products, by properly including the spectral attenuation effects of carbonaceous, urban/industrial and mineral aerosols. The TOMS data set on aerosol properties will be discussed, and results of its use in the TOMS surface W algorithm will be presented.

Black carbon and wavelength-dependent aerosol absorption in the North China Plain based on two-year aethalometer measurements

NASA Astrophysics Data System (ADS)

Ran, L.; Deng, Z. Z.; Wang, P. C.; Xia, X. A.

2016-10-01

Light-absorbing components of atmospheric aerosols have gained particular attention in recent years due to their climatic and environmental effects. Based on two-year measurements of aerosol absorption at seven wavelengths, aerosol absorption properties and black carbon (BC) were investigated in the North China Plain (NCP), one of the most densely populated and polluted regions in the world. Aerosol absorption was stronger in fall and the heating season (from November to March) than in spring and summer at all seven wavelengths. Similar spectral dependence of aerosol absorption was observed in non-heating seasons despite substantially strong absorption in fall. With an average absorption Angström exponent (α) of 1.36 in non-heating seasons, freshly emitted BC from local fossil fuel burning was thought to be the major component of light-absorbing aerosols. In the heating season, strong ultraviolet absorption led to an average α of 1.81, clearly indicating the importance of non-BC light-absorbing components, which were possibly from coal burning for domestic heating and aging processes on a regional scale. Diurnally, the variation of BC mass concentrations experienced a double-peak pattern with a higher level at night throughout the year. However, the diurnal cycle of α in the heating season was distinctly different from that in non-heating seasons. α peaked in the late afternoon in non-heating seasons with concomitantly observed low valley in BC mass concentrations. In contrast, α peaked around the midnight in the heating season and lowered down during the daytime. The relationship of aerosol absorption and winds in non-heating seasons also differed from that in the heating season. BC mass concentrations declined while α increased with increasing wind speed in non-heating seasons, which suggested elevated non-BC light absorbers in transported aged aerosols. No apparent dependence of α on wind speed was found in the heating season, probably due to well mixed regional pollution. Pollution episodes were mostly encountered under low winds and had a low level of α, implying aerosol absorption should be largely attributed to freshly emitted BC from local sources under such conditions. Extensive field campaigns and long-term chemical and optical measurements of light-absorbing aerosols are needed in the future to further advance our understanding on optical properties of light-absorbing aerosols and their radiative forcing in this region.

Spectral model for clear sky atmospheric longwave radiation

NASA Astrophysics Data System (ADS)

Li, Mengying; Liao, Zhouyi; Coimbra, Carlos F. M.

2018-04-01

An efficient spectrally resolved radiative model is used to calculate surface downwelling longwave (DLW) radiation (0 ∼ 2500 cm-1) under clear sky (cloud free) conditions at the ground level. The wavenumber spectral resolution of the model is 0.01 cm-1 and the atmosphere is represented by 18 non-uniform plane-parallel layers with pressure in each layer determined on a pressure-based coordinate system. The model utilizes the most up-to-date (2016) HITRAN molecular spectral data for 7 atmospheric gases: H2O, CO2, O3, CH4, N2O, O2 and N2. The MT_CKD model is used to calculate water vapor and CO2 continuum absorption coefficients. Longwave absorption and scattering coefficients for aerosols are modeled using Mie theory. For the non-scattering atmosphere (aerosol free), the surface DLW agrees within 2.91% with mean values from the InterComparison of Radiation Codes in Climate Models (ICRCCM) program, with spectral deviations below 0.035 W cm m-2. For a scattering atmosphere with typical aerosol loading, the DLW calculated by the proposed model agrees within 3.08% relative error when compared to measured values at 7 climatologically diverse SURFRAD stations. This relative error is smaller than a calibrated parametric model regressed from data for those same 7 stations, and within the uncertainty (+/- 5 W m-2) of pyrgeometers commonly used for meteorological and climatological applications. The DLW increases by 1.86 ∼ 6.57 W m-2 when compared with aerosol-free conditions, and this increment decreases with increased water vapor content due to overlap with water vapor bands. As expected, the water vapor content at the layers closest to the surface contributes the most to the surface DLW, especially in the spectral region 0 ∼ 700 cm-1. Additional water vapor content (mostly from the lowest 1 km of the atmosphere) contributes to the spectral range of 400 ∼ 650 cm-1. Low altitude aerosols ( ∼ 3.46 km or less) contribute to the surface value of DLW mostly in the spectral range 750 ∼ 1400 cm-1.

Aerosol optical properties at the Lulin Atmospheric Background Station in Taiwan and the influences of long-range transport of air pollutants

NASA Astrophysics Data System (ADS)

Hsiao, Ta-Chih; Chen, Wei-Nai; Ye, Wei-Cheng; Lin, Neng-Huei; Tsay, Si-Chee; Lin, Tang-Huang; Lee, Chung-Te; Chuang, Ming-Tung; Pantina, Peter; Wang, Sheng-Hsiang

2017-02-01

The Lulin Atmospheric Background Station (LABS, 23.47°N 120.87°E, 2862 m ASL) in Central Taiwan was constructed in 2006 and is the only high-altitude background station in the western Pacific region for studying the influence of continental outflow. In this study, extensive optical properties of aerosols, including the aerosol light scattering coefficient (σs) and light absorption coefficient (σa), were collected from 2013 to 2014. The intensive optical properties, including mass scattering efficiency (αs), mass absorption efficiency (αa), single scattering albedo (ω), scattering Ångstrӧm exponent (Å), and backscattering fraction (b), were determined and investigated, and the distinct seasonal cycle was observed. The value of αs began to increase in January and reached a maximum in April; the mean in spring was 5.89 m2 g-1 with a standard deviation (SD) of 4.54 m2 g-1 and a 4.48 m2 g-1 interquartile range (IQR: 2.95-7.43 m2 g-1). The trend was similar in αa, with a maximum in March and a monthly mean of 0.84 m2 g-1. The peak values of ω (Mean = 0.92, SD = 0.03, IQR: 0.90-0.93) and Å (Mean = 2.22, SD = 0.61, IQR: 2.12-2.47) occurred in autumn. These annual patterns of optical properties were associated with different long-range transport patterns of air pollutants such as biomass burning (BB) aerosol in spring and potential anthropogenic emissions in autumn. The optical measurements performed at LABS during spring in 2013 were compared with those simultaneously performed at the Doi Ang Kang Meteorology Station, Chiang Mai Province, Thailand (DAK, 19.93°N, 99.05°E, 1536 m a.s.l.), which is located in the Southeast Asia BB source region. Furthermore, the relationships among αs, αa, and b were used to characterize the potential aerosol types transported to LABS during different seasons, and the data were inspected according to the HYSPLIT 5-day backward trajectories, which differentiate between different regions of air mass origin.

Radiative forcing of the desert aerosol at Ouarzazate (Morocco)

NASA Astrophysics Data System (ADS)

Tahiri, Abdelouahid; Diouri, Mohamed

2018-05-01

The atmospheric aerosol contributes to the definition of the climate with direct effect, the diffusion and absorption of solar and terrestrial radiations, and indirect, the cloud formation process where aerosols behave as condensation nuclei and alter the optical properties. Satellites and ground-based networks (solar photometers) allow the terrestrial aerosol observation and the determination of impact. Desert aerosol considered among the main types of tropospheric aerosols whose optical property uncertainties are still quite important. The analysis concerns the optical parameters recorded in 2015 at Ouarzazate solar photometric station (AERONET/PHOTONS network, http://aeronet.gsfc.nasa.gov/) close to Saharan zone. The daily average aerosol optical depthτaer at 0.5μm, are relatively high in summer and less degree in spring (from 0.01 to 1.82). Daily average of the Angstrom coefficients α vary between 0.01 and 1.55. The daily average of aerosol radiative forcing at the surface range between -150W/m2 and -10 W/m2 with peaks recorded in summer, characterized locally by large loads of desert aerosol in agreement with the advections of the Southeast of Morocco. Those recorded at the Top of the atmosphere show a variation from -74 W/m2 to +24 W/m2

Satellite-Based Evidence of Wavelength-Dependent Aerosol Absorption in Biomass Burning Smoke Inferred from Ozone Monitoring Instrument

NASA Technical Reports Server (NTRS)

Jethva, H.; Torres, O.

2012-01-01

We provide satellite-based evidence of the spectral dependence of absorption in biomass burning aerosols over South America using near-UV measurements made by the Ozone Monitoring Instrument (OMI) during 2005-2007. In the current near-UV OMI aerosol algorithm (OMAERUV), it is implicitly assumed that the only absorbing component in carbonaceous aerosols is black carbon whose imaginary component of the refractive index is wavelength independent. With this assumption, OMI-derived aerosol optical depth (AOD) is found to be significantly over-estimated compared to that of AERONET at several sites during intense biomass burning events (August-September). Other well-known sources of error affecting the near-UV method of aerosol retrieval do not explain the large observed AOD discrepancies between the satellite and the ground-based observations. A number of studies have revealed strong spectral dependence in carbonaceous aerosol absorption in the near-UV region suggesting the presence of organic carbon in biomass burning generated aerosols. A sensitivity analysis examining the importance of accounting for the presence of wavelength-dependent aerosol absorption in carbonaceous particles in satellite-based remote sensing was carried out in this work. The results convincingly show that the inclusion of spectrally-dependent aerosol absorption in the radiative transfer calculations leads to a more accurate characterization of the atmospheric load of carbonaceous aerosols.

Long term change in atmospheric dust absorption, dust scattering and black carbon aerosols scattering coefficient parameters over western Indian locations

NASA Astrophysics Data System (ADS)

Satoliya, Anil Kumar; Vyas, B. M.; Shekhawat, M. S.

2018-05-01

The first time satellite space based measurement of atmospheric black carbon (BC) aerosols scattering coefficient at 550nm (BC SC at 550nm), dust aerosols scattering and dust aerosols extinction coefficient (DSC at 550nm and DEC at 550nm) parameters have been used to understand their long term trend of natural and anthropogenic aerosols behavior with its close association with ground based measured precipitation parameters such as Total Rain Fall (TRF), and Total Number of Rainy Days (TNRD) for the same period over western Indian regions concerned to the primary aerosols sources of natural activities. The basic objective of this study is an attempt to investigate the inter-correlation between dust and black carbon aerosols loading characteristics with a variation of rainfall pattern parameters as indirect aerosols induced effect i.e., aerosols-cloud interaction. The black carbon aerosols generated by diverse anthropogenic or human made activities are studied by choosing of measured atmospheric BC SC at 550nm parameter, whereas desert dust mineral aerosols primarily produced by varieties of natural activities pre-dominated of dust mineral desert aerosols mainly over Thar desert influenced area of hot climate and rural tropical site are investigated by selecting DSC at 550nm and DEC at 550nm of first semi-urban site i.e., Udaipur (UDP, 24.6°N, 73.35°E, 580m above surface level (asl)) situated in southern Rajasthan part as well as over other two Great Indian Thar desert locations i.e., Jaisalmer (JSM, 26.90°N, 69.90°E, 220m asl)) and Bikaner (BKN, 28.03°N, 73.30°E, 224m asl) located in the vicinity of the Thar desert region situated in Rajasthan state of the western Indian region. The source of the present study would be collection of longer period of monthly values of the above parameters of spanning 35 years i.e., 1980 to 2015. Such types of atmospheric aerosols-cloud monsoon interaction investigation is helpful in view of understanding their direct and indirect aerosols active role of optical absorption and scattering of solar light radiation at useful wavelength 550nm as well as heating of clouds over least explored region, i.e., the Thar desert region and also away from less dust dominated influenced provinces for longer period. The analysis of the above the result would also give a clear scientific evidence of alteration in enhancement in DSC at 550nm and DEC at 550nm and BC SC at 550nm variables with simultaneous corresponding reduction in the five yearly mean precipitation activity parameters such as TRF and TNRD. It is quite evident that anthropogenic BC aerosols activity are showing the significant increasing trend at all three locations, but it is more prominent over central Thar Desert influenced regime, i.e., JSM and BKN relative to semi-urban region i.e., UDP. The systematic increasing pattern of average monthly mean value of DSC at 550nm and DEC at 550nm or increasing aerosol loading have been revealed from acquiring their lowest value in January month and the highest values in July and retained with the broad peak values in pre-monsoon months. Subsequently, their respective values reduce sharply downward from August to December onwards. The mountain value of dust aerosols parameters, i.e., DSC at 550nm and DEC at 550nm are systematically enhanced toward from UDP to BKN and then maximized at JSM. It is clearly obvious fact that the following ascending order of desert aerosols loading influenced activity in different areas has been recorded, i.e., JSM> BKN>UDP. Several other interesting features of the earth-climate change implication in reference to the altering nature of reduction of precipitation parameter pattern with simultaneous observed elevated dust aerosol and BC aerosol loading have been also noticed in the course of present investigation. Overall reduction in rainfall pattern effect with increasing of dust aerosols loading or vice versa are seen more pronounced over JSM and lees prevalence over UDP. The more detailed investigations about other interesting results of Aerosols-Indian monsoon over western Indian locations are also discussed thoroughly in this paper.

Photoacoustics of single laser-trapped nanodroplets for the direct observation of nanofocusing in aerosol photokinetics

NASA Astrophysics Data System (ADS)

Cremer, Johannes W.; Thaler, Klemens M.; Haisch, Christoph; Signorell, Ruth

2016-03-01

Photochemistry taking place in atmospheric aerosol droplets has a significant impact on the Earth's climate. Nanofocusing of electromagnetic radiation inside aerosols plays a crucial role in their absorption behaviour, since the radiation flux inside the droplet strongly affects the activation rate of photochemically active species. However, size-dependent nanofocusing effects in the photokinetics of small aerosols have escaped direct observation due to the inability to measure absorption signatures from single droplets. Here we show that photoacoustic measurements on optically trapped single nanodroplets provide a direct, broadly applicable method to measure absorption with attolitre sensitivity. We demonstrate for a model aerosol that the photolysis is accelerated by an order of magnitude in the sub-micron to micron size range, compared with larger droplets. The versatility of our technique promises broad applicability to absorption studies of aerosol particles, such as atmospheric aerosols where quantitative photokinetic data are critical for climate predictions.

Photoacoustics of single laser-trapped nanodroplets for the direct observation of nanofocusing in aerosol photokinetics

PubMed Central

Cremer, Johannes W.; Thaler, Klemens M.; Haisch, Christoph; Signorell, Ruth

2016-01-01

Photochemistry taking place in atmospheric aerosol droplets has a significant impact on the Earth's climate. Nanofocusing of electromagnetic radiation inside aerosols plays a crucial role in their absorption behaviour, since the radiation flux inside the droplet strongly affects the activation rate of photochemically active species. However, size-dependent nanofocusing effects in the photokinetics of small aerosols have escaped direct observation due to the inability to measure absorption signatures from single droplets. Here we show that photoacoustic measurements on optically trapped single nanodroplets provide a direct, broadly applicable method to measure absorption with attolitre sensitivity. We demonstrate for a model aerosol that the photolysis is accelerated by an order of magnitude in the sub-micron to micron size range, compared with larger droplets. The versatility of our technique promises broad applicability to absorption studies of aerosol particles, such as atmospheric aerosols where quantitative photokinetic data are critical for climate predictions. PMID:26979973

Dependence of Aerosol Light Absorption and Single-Scattering Albedo On Ambient Relative Humidity for Sulfate Aerosols with Black Carbon Cores

NASA Technical Reports Server (NTRS)

Redemann, Jens; Russell, Philip B.; Hamill, Patrick

2001-01-01

Atmospheric aerosols frequently contain hygroscopic sulfate species and black carbon (soot) inclusions. In this paper we report results of a modeling study to determine the change in aerosol absorption due to increases in ambient relative humidity (RH), for three common sulfate species, assuming that the soot mass fraction is present as a single concentric core within each particle. Because of the lack of detailed knowledge about various input parameters to models describing internally mixed aerosol particle optics, we focus on results that were aimed at determining the maximum effect that particle humidification may have on aerosol light absorption. In the wavelength range from 450 to 750 nm, maximum absorption humidification factors (ratio of wet to 'dry=30% RH' absorption) for single aerosol particles are found to be as large as 1.75 when the RH changes from 30 to 99.5%. Upon lesser humidification from 30 to 80% RH, absorption humidification for single particles is only as much as 1.2, even for the most favorable combination of initial ('dry') soot mass fraction and particle size. Integrated over monomodal lognormal particle size distributions, maximum absorption humidification factors range between 1.07 and 1.15 for humidification from 30 to 80% and between 1.1 and 1.35 for humidification from 30 to 95% RH for all species considered. The largest humidification factors at a wavelength of 450 nm are obtained for 'dry' particle size distributions that peak at a radius of 0.05 microns, while the absorption humidification factors at 700 nm are largest for 'dry' size distributions that are dominated by particles in the radius range of 0.06 to 0.08 microns. Single-scattering albedo estimates at ambient conditions are often based on absorption measurements at low RH (approx. 30%) and the assumption that aerosol absorption does not change upon humidification (i.e., absorption humidification equal to unity). Our modeling study suggests that this assumption alone can introduce absolute errors in estimates of the midvisible single-scattering albedo of up to 0.05 for realistic dry particle size distributions. Our study also indicates that this error increases with increasing wavelength. The potential errors in aerosol single-scattering albedo derived here are comparable in magnitude and in addition to uncertainties in single-scattering albedo estimates that are based on measurements of aerosol light absorption and scattering.

New in situ Aerosol Spectral Optical Measurements over 300-700 nm, Extinction and Total Absorption, Paired with Absorption from Water- and Methanol-soluble Aerosol Extracts

NASA Astrophysics Data System (ADS)

Jordan, C. E.; Stauffer, R. M.; Lamb, B.; Novak, M. G.; Mannino, A.; Hudgins, C.; Thornhill, K. L., II; Crosbie, E.; Winstead, E.; Anderson, B.; Martin, R.; Shook, M.; Ziemba, L. D.; Beyersdorf, A. J.; Corr, C.

2017-12-01

A new in situ spectral aerosol extinction instrument (custom built, SpEx) built to cover the 300-700 nm range at 1 nm spectral resolution and temporal resolution of 4 minutes was deployed on the top deck ( 10 m above the water surface) of the R/V Onnuri during the KORUS-OC research cruise around South Korea in spring 2016. This new instrument was one component of a suite of in situ aerosol optical measurements that included 3-visible-wavelength scattering (Airphoton IN101 Nephelometer, at 450, 532, & 632 nm) and absorption (Brechtel Tricolor Absorption Photometer Model 2901, at 467, 528, & 652 nm) with sub-minute temporal resolution; two sets of filters (Teflon and glass fiber, both collected over 3 hour daytime and 12 hour overnight intervals) to provide aerosol absorption spectra over the same wavelength range as SpEx. The glass fiber filters were placed in the center of an integrating sphere (Labsphere DRA-CA-30) attached to a dual beam spectrophotometer (Cary 100 Bio UV-Visible Spectrophotometer) to measure total aerosol absorption spectra via an established method used by the ocean color community to obtain absorption spectra from particles suspended in sea water. Adapting this methodology for atmospheric aerosol measurements provides a new avenue to obtain spectral total aerosol absorption, particularly useful for expanding in situ measurement capabilities into the UV range. The Teflon filters were cut in half with one half extracted in deionized water and the other half extracted in methanol. The solutions were filtered and injected into a liquid waveguide capillary cell (World Precision Instruments LWCC-3100, 100 cm pathlength) to measure the absorption spectra for each solution. In addition, the water extracts were measured via ion chromatography (Dionex ICS-3000 Ion Chromatography System) to obtain water-soluble inorganic ion concentrations, as well as via aerosol mass spectrometry (Aerodyne Research, Inc. HR-ToF High Resolution Aerosol Mass Spectrometer) to obtain organic aerosol concentrations. Results from the KORUS-OC data set will be discussed. In particular, the relationships between the optical information and chemical information will be examined.

Observations of the vertical distributions of summertime atmospheric pollutants and the corresponding ozone production in Shanghai, China

NASA Astrophysics Data System (ADS)

Xing, Chengzhi; Liu, Cheng; Wang, Shanshan; Chan, Ka Lok; Gao, Yang; Huang, Xin; Su, Wenjing; Zhang, Chengxin; Dong, Yunsheng; Fan, Guangqiang; Zhang, Tianshu; Chen, Zhenyi; Hu, Qihou; Su, Hang; Xie, Zhouqing; Liu, Jianguo

2017-12-01

Ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) and lidar measurements were performed in Shanghai, China, during May 2016 to investigate the vertical distribution of summertime atmospheric pollutants. In this study, vertical profiles of aerosol extinction coefficient, nitrogen dioxide (NO2) and formaldehyde (HCHO) concentrations were retrieved from MAX-DOAS measurements using the Heidelberg Profile (HEIPRO) algorithm, while vertical distribution of ozone (O3) was obtained from an ozone lidar. Sensitivity study of the MAX-DOAS aerosol profile retrieval shows that the a priori aerosol profile shape has significant influences on the aerosol profile retrieval. Aerosol profiles retrieved from MAX-DOAS measurements with Gaussian a priori profile demonstrate the best agreements with simultaneous lidar measurements and vehicle-based tethered-balloon observations among all a priori aerosol profiles. Tropospheric NO2 vertical column densities (VCDs) measured with MAX-DOAS show a good agreement with OMI satellite observations with a Pearson correlation coefficient (R) of 0.95. In addition, measurements of the O3 vertical distribution indicate that the ozone productions do not only occur at surface level but also at higher altitudes (about 1.1 km). Planetary boundary layer (PBL) height and horizontal and vertical wind field information were integrated to discuss the ozone formation at upper altitudes. The results reveal that enhanced ozone concentrations at ground level and upper altitudes are not directly related to horizontal and vertical transportation. Similar patterns of O3 and HCHO vertical distributions were observed during this campaign, which implies that the ozone productions near the surface and at higher altitudes are mainly influenced by the abundance of volatile organic compounds (VOCs) in the lower troposphere.

Molecular Characterization of Brown Carbon in Biomass Burning Aerosol Particles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lin, Peng; Aiona, Paige K.; Li, Ying

Emissions from biomass burning are a significant source of brown carbon (BrC) in the atmosphere. In this study, we investigate the molecular composition of freshly-emitted biomass burning organic aerosol (BBOA) samples collected during test burns of selected biomass fuels: sawgrass, peat, ponderosa pine, and black spruce. We characterize individual BrC chromophores present in these samples using high performance liquid chromatography coupled to a photodiode array detector and a high-resolution mass spectrometer. We demonstrate that both the overall BrC absorption and the chemical composition of light-absorbing compounds depend significantly on the type of biomass fuels and burning conditions. Common BrC chromophoresmore » in the selected BBOA samples include nitro-aromatics, polycyclic aromatic hydrocarbon derivatives, and polyphenols spanning a wide range of molecular weights, structures, and light absorption properties. A number of biofuel-specific BrC chromophores are observed, indicating that some of them may be used as potential markers of BrC originating from different biomass burning sources. On average, ~50% of the light absorption above 300 nm can be attributed to a limited number of strong BrC chromophores, which may serve as representative light-absorbing species for studying atmospheric processing of BrC aerosol. The absorption coefficients of BBOA are affected by solar photolysis. Specifically, under typical atmospheric conditions, the 300 nm absorbance decays with a half-life of 16 hours. A “molecular corridors” analysis of the BBOA volatility distribution suggests that many BrC compounds in the fresh BBOA have low volatility (<1 g m-1) and will be retained in the particle phase under atmospherically relevant conditions.« less

Sensitivity of high-spectral resolution and broadband thermal infrared nadir instruments to the chemical and microphysical properties of secondary sulfate aerosols in the upper-troposphere/lower-stratosphere

NASA Astrophysics Data System (ADS)

Sellitto, Pasquale; Legras, Bernard

2016-04-01

The observation of upper-tropospheric/lower-stratospheric (UTLS) secondary sulfate aerosols (SSA) and their chemical and microphysical properties from satellite nadir observations (with better spatial resolution than limb observations) is a fundamental tool to better understand their formation and evolution processes and then to estimate their impact on UTLS chemistry, and on regional and global radiative balance. Thermal infrared (TIR) observations are sensitive to the chemical composition of the aerosols due to the strong spectral variations of the imaginary part of the refractive index in this band and, correspondingly, of the absorption, as a function of the composition Then, these observations are, in principle, well adapted to detect and characterize UTLS SSA. Unfortunately, the exploitation of nadir TIR observations for sulfate aerosol layer monitoring is today very limited. Here we present a study aimed at the evaluation of the sensitivity of TIR satellite nadir observations to the chemical composition and the size distribution of idealised UTLS SSA layers. The sulfate aerosol particles are assumed as binary systems of sulfuric acid/water solution droplets, with varying sulphuric acid mixing ratios. The extinction properties of the SSA, for different sulfuric acid mixing ratios and temperatures, are systematically analysed. The extinction coefficients are derived by means of a Mie code, using refractive indices taken from the GEISA (Gestion et Étude des Informations Spectroscopiques Atmosphériques: Management and Study of Spectroscopic Information) spectroscopic database and log-normal size distributions with different effective radii and number concentrations. High-spectral resolution pseudo-observations are generated using forward radiative transfer calculations performed with the 4A (Automatized Atmospheric Absorption Atlas) radiative transfer model, to estimate the impact of the extinction of idealised aerosol layers, at typical UTLS conditions, on the brightness temperature (BT) spectra observed by satellite instruments. We isolated a marked and typical spectral signature of these aerosol layers between 700 and 1200 cm-1, due to the absorption bands of the sulfate and bisulfate ions and the undissociated sulfuric acid, with the main absorption peaks at 1170 and 905 cm-1 (sulfuric acid vibrational bands). The dependence of the residual aerosol spectral BT signature to the sulfuric acid mixing ratio, and effective number concentration and radius, as well as the role of interfering parameters like the ozone, sulfur dioxide, carbon dioxide and ash absorption, and temperature and water vapour profile uncertainties, are analysed and critically discussed. The information content (degrees of freedom and retrieval uncertainties) of synthetic satellite observations is estimated for different instrumental configurations. High spectral resolution (Infrared Atmospheric Sounding Interferometer (IASI)-like pseudo-observations) and broadband spectral features (Moderate Resolution Imaging Spectroradiometer (MODIS) and Spinning Enhanced Visible and InfraRed Imager (SEVIRI)-like pseudo-observations) approaches are proposed and discussed.

Increased absorption by coarse aerosol particles over the Gangetic–Himalayan region

DOE PAGES

Manoharan, Vani Starry; Kotamarthi, R.; Feng, Yan; ...

2014-02-03

Each atmospheric aerosol type has distinctive light-absorption characteristics related to its physical/chemical properties. Climate models treat black carbon as the main light-absorbing component of carbonaceous atmospheric aerosols, while absorption by some organic aerosols is also considered, particularly at ultraviolet wavelengths. Most absorbing aerosols are assumed to be < 1 μm in diameter (sub-micron). Here we present results from a recent field study in India, primarily during the post-monsoon season (October–November), suggesting the presence of absorbing aerosols sized 1–10 μm. Absorption due to super-micron-sized particles was nearly 30% greater than that due to smaller particles. Periods of increased absorption by largermore » particles ranged from a week to a month. Radiative forcing calculations under clear-sky conditions show that super-micron particles account for nearly 44% of the total aerosol forcing. The origin of the large aerosols is unknown, but meteorological conditions indicate that they are of local origin. Such economic and habitation conditions exist throughout much of the developing world. Furthermore, large absorbing particles could be an important component of the regional-scale atmospheric energy balance.« less

’In situ’ Measurement of the Ratio of Aerosol Absorption to Extinction Coefficient.

DTIC Science & Technology

1980-08-01

procedure for settling measurements was to obtain a reference (presmoke) level of stabilized power on both of the calorimeters indicated in figure 1...sizing measurements which might be appropriate and accurate for this application as also being investigated. 16 REFERENCES 1. Selby, J. E. A., and L...Projectiles," ECOM-5570, August 1975. 7. Duncan, Louis D., "An Improved Algorithm for the Iterated Minimal Information Solution for Remote Sounding of

Some Optical Properties of Blowing Snow.

DTIC Science & Technology

1981-06-01

TR-0058, May 1980. 130. Heaps, Melvin G., Robert 0. Olsen, Warren Berning, John Cross, and Arthur Gilcrease, 񓟛 Solar Eclipse, Part I - Atmospheric...Near-Millimeter Wave (NMMW) 9ronacation Measurements," ASL-T.-OC63, August 1980. 135. Bruce, Charles W., Young Paul Yee, and S. G. Jennings, "In Situ...Measurement of the Ratio of Aerosol Absorption to Extinction Coefficient," ASL-TR-0064, August 1980. 136. Yee, Young Paul , Charles W. Bruce, and Ralph J

The absorption budget of fresh biomass burning aerosol from realistic laboratory fires

NASA Astrophysics Data System (ADS)

Wagner, N. L.; Adler, G. A.; Franchin, A.; Lamb, K.; Manfred, K.; Middlebrook, A. M.; Selimovic, V.; Schwarz, J. P.; Washenfelder, R. A.; Womack, C.; Yokelson, R. J.

2017-12-01

Wildfires are expected to increase globally due to climate change. The smoke from these wildfires has a highly uncertain radiative effect, largely due to the lack of detailed understanding of its optical properties. As part of the NOAA FIREX project, we have measured the optical properties of smoke primarily from laboratory burning of North American fuels at the Missoula Fire Sciences Laboratory. Here, we present a budget of the aerosol absorption from a portion of the laboratory fires. The total aerosol absorption was measured with photoacoustic spectrometers (PAS) at four wavelengths (405 nm, 532 nm, 660 nm, 870 nm) spanning the visible spectral region. The aerosol absorption is attributed to black carbon which absorbs broadly across the visible and ultraviolet (UV) spectral region and brown carbon (BrC) which absorbs in the blue and UV spectral regions. Then aerosol absorption measurements are compared with measurements of refractory black carbon (rBC) concentration by laser induced incandescence (SP2) and measurements of BrC concentration from a particle-into-liquid sampler coupled to a liquid absorption cell (BrC-PILS). Periodically, a thermodenuder was inserted upstream of all of the instruments to constrain the relationship between aerosol volatility and absorption. We synthesize these measurements to constrain the various contributors to total absorption including effects of lensing on rBC absorption, and of BrC that is not volatilized in the thermodenuder.

UManSysProp: An online and open-source facility for molecular property prediction and atmospheric aerosol calculations

NASA Astrophysics Data System (ADS)

Topping, David; Barley, Mark; McFiggans, Gordon; Aumont, Bernard

2016-04-01

The many thousands of individual aerosol components ensure that explicit manual calculation of properties that influence their environmental impacts is laborious and time-consuming. The emergence of explicit automatic mechanism generation techniques, including up to many millions of individual gas phase products as aerosol precursors, renders manual calculations impossible and automation is necessary. It can be difficult to establish what factors are responsible for the outcome of a model prediction. This is particularly true when the number of components might be high in, for example, SOA mass partitioning simulations. It then becomes difficult for others in the community to assess the results presented. This might be complicated by the need to include pure component vapour pressures or activity coefficient predictions for a wide range of highly multifunctional compounds. It isn't clear to what extent replication of results is ever achieved for a range of aerosol simulations. Whilst this might also be an issue with results from instrumentation, the development of community driven software at least enables modellers to tackle this problem directly. Here we describe the development and application of a new web based facility, UManSysProp, to tackle such issues. Current facilities include: pure component vapour pressures, critical properties and sub-cooled densities of organic molecules; activity coefficient predictions for mixed inorganic-organic liquid systems; hygroscopic growth factors and CCN activation potential of mixed inorganic/organic aerosol particles with associated Kappa-Kohler values; absorptive partitioning calculations with/without a treatment of non-ideality. The website can be found here: http://umansysprop.seaes.manchester.ac.uk/

High Altitude Emissions of Black Carbon Aerosols: Potential Climate Implications

NASA Astrophysics Data System (ADS)

Satheesh, S. K.

2017-12-01

Synthesizing a series of ground-based and airborne measurements of aerosols over the Indian region during summer and pre-monsoon seasons have revealed the persistence of elevated absorbing aerosol layers over most of the Indian region; more than 50% of which located above clouds. Subsequent, in situ measurements of black carbon (BC) using high-altitude balloons, showed surprising layers with high concentrations in the middle and upper troposphere even at an altitude of 8 to 10 kms. Simultaneous measurements of the vertical thermal structure have shown localized warming due to BC absorption leading to large reduction in lapse rate and sharp temperature inversion, which in turn increases the atmospheric stability. This aerosol-induced stable layer is conducive for maintaining the black carbon layer longer at that level, leading thereby to further solar absorption and subsequently triggering dry convection. These observations support the `solar escalator' concept through which absorption-warming-convection cycles lead to self-lifting of BC to upper troposphere or even to lower stratosphere under favorable conditions in a matter of a few days. Employing an on-line regional chemistry transport model (WRF-Chem), incorporating aircraft emissions, it is shown that emissions from high-flying aircrafts as the most likely source of these elevated black carbon layers. These in-situ injected particles, produce significant warming of the thin air in those heights and lift these layers to even upper tropospheric/lower stratospheric heights, aided by the strong monsoonal convection occurring over the region, which are known to overshoot the tropical tropopause leading to injection of tropospheric air mass (along with its constituent aerosols) into the stratosphere, especially during monsoon season when the tropical tropopause layer is known to be thinnest. These simulations are further supported by the CALIPSO space-borne LIDAR derived extinction coefficient profiles. Based on these, it is hypothesized that such intrusions of black carbon to lower stratosphere and its consequent longer residence time in the stratosphere, would have significant implications for stratospheric chemistry, considering the known ozone depleting potential of black carbon aerosols.

African dust particles and their impact on the solar energy budget in a Caribbean tropical montane cloud forest

NASA Astrophysics Data System (ADS)

Rivera, F. A.; Mayol-Bracero, O. L.; Torres-Delgado, E.

2017-12-01

To understand the impact of aerosols over the atmospheric energy budget it is essential to identify their size and chemical properties. Atmospheric aerosols emitted, for example, from African dust storms, directly affect climate by altering the dynamics of cloud formation and by reducing the amount of radiation reaching vegetation and the soil surface. In this project, we seek to improve our understanding of the variations in the concentrations of African dust and the role it might play in the energy budget at a Tropical Montane Cloud Forest (TMCF). Concentrations of particulate matter with diameters equal or less than 10µm (PM10) and aerosol optical properties (scattering and absorption) for years 2013 and 2014 were studied in northeastern Puerto Rico at the nature reserve of Cabezas de San Juan (CSJ). At CSJ we used an Integrating Nephelometer to measure light scattering at three wavelengths (450, 550 and 700 nm) and calculated the Scattering Angstrom Exponent (SAE), a measure inversely related to the size of the aerosol particle. We also used the Continuous Light Absorption Photometer (CLAP) to measure the light absorption at three wavelengths (450, 550 and 700). Visibility (meters) and radiation (total solar, UV and IR irradiation) were studied at the TMCF of Pico del Este (PE). PM10 data from stations at Cataño, Guaynabo, and Fajardo were also obtained. The PM10 data were used to study the variation in aerosol concentrations during the year and to study whether there was an effect on the incoming solar radiation. The periods under the influence of African dust were identified using the spectral coefficients measured at CSJ and the air mass back trajectories using the HYSPLIT model. During the summer period, an increase in PM10 concentrations, related to African Dust incursions, was observed. Preliminary results suggest that, for 2013 and 2014, in the presence of high concentrations of PM10 and with low SAE, the total radiation at PE decreased. This could be related to the interactions between solar radiation and aerosol particles and will be discussed in the presentation.

A study of remotely sensed aerosol properties from ground-based sun and sky scanning radiometers

NASA Astrophysics Data System (ADS)

Giles, David M.

Aerosol particles impact human health by degrading air quality and affect climate by heating or cooling the atmosphere. The Indo-Gangetic Plain (IGP) of Northern India, one of the most populous regions in the world, produces and is impacted by a variety of aerosols including pollution, smoke, dust, and mixtures of them. The NASA Aerosol Robotic Network (AERONET) mesoscale distribution of Sun and sky-pointing instruments in India was established to measure aerosol characteristics at sites across the IGP and around Kanpur, India, a large urban and industrial center in the IGP, during the 2008 pre-monsoon (April-June). This study focused on detecting spatial and temporal variability of aerosols, validating satellite retrievals, and classifying the dominant aerosol mixing states and origins. The Kanpur region typically experiences high aerosol loading due to pollution and smoke during the winter and high aerosol loading due to the addition of dust to the pollution and smoke mixture during the pre-monsoon. Aerosol emissions in Kanpur likely contribute up to 20% of the aerosol loading during the pre-monsoon over the IGP. Aerosol absorption also increases significantly downwind of Kanpur indicating the possibility of the black carbon emissions from aerosol sources such as coal-fired power plants and brick kilns. Aerosol retrievals from satellite show a high bias when compared to the mesoscale distributed instruments around Kanpur during the pre-monsoon with few high quality retrievals due to imperfect aerosol type and land surface characteristic assumptions. Aerosol type classification using the aerosol absorption, size, and shape properties can identify dominant aerosol mixing states of absorbing dust and black carbon particles. Using 19 long-term AERONET sites near various aerosol source regions (Dust, Mixed, Urban/Industrial, and Biomass Burning), aerosol absorption property statistics are expanded upon and show significant differences when compared to previous work. The sensitivity of absorption properties is evaluated and quantified with respect to aerosol retrieval uncertainty. Using clustering analysis, aerosol absorption and size relationships provide a simple method to classify aerosol mixing states and origins and potentially improve aerosol retrievals from ground-based and satellite-based instrumentation.

Brown carbon formation by aqueous-phase carbonyl compound reactions with amines and ammonium sulfate.

PubMed

Powelson, Michelle H; Espelien, Brenna M; Hawkins, Lelia N; Galloway, Melissa M; De Haan, David O

2014-01-21

Reactions between small water-soluble carbonyl compounds, ammonium sulfate (AS), and/or amines were evaluated for their ability to form light-absorbing species in aqueous aerosol. Aerosol chemistry was simulated with bulk phase reactions at pH 4, 275 K, initial concentrations of 0.05 to 0.25 M, and UV-vis and fluorescence spectroscopy monitoring. Glycolaldehyde-glycine mixtures produced the most intense absorbance. In carbonyl compound reactions with AS, methylamine, or AS/glycine mixtures, product absorbance followed the order methylglyoxal > glyoxal > glycolaldehyde > hydroxyacetone. Absorbance extended into the visible, with a wavelength dependence fit by absorption Ångstrom coefficients (Å(abs)) of 2 to 11, overlapping the Å(abs) range of atmospheric, water-soluble brown carbon. Many reaction products absorbing between 300 and 400 nm were strongly fluorescent. On a per mole basis, amines are much more effective than AS at producing brown carbon. In addition, methylglyoxal and glyoxal produced more light-absorbing products in reactions with a 5:1 AS-glycine mixture than with AS or glycine alone, illustrating the importance of both organic and inorganic nitrogen in brown carbon formation. Through comparison to biomass burning aerosol, we place an upper limit on the contribution of these aqueous carbonyl-AS-amine reactions of ≤ 10% of global light absorption by brown carbon.

Quantifying organic aerosol single scattering albedo over tropical biomass burning regions using ground-based observation

NASA Astrophysics Data System (ADS)

Chu, J. E.

2016-12-01

Despite growing evidence of light-absorbing organic aerosols (OAs), OA light absorption has been poorly understood due to difficulties in aerosol light absorption measurements. In this study, we developed an empirical method to quantify OA single scattering albedo (SSA), the ratio of light scattering to extinction, using ground-based Aerosol Robotic Network (AERONET) observation. Our method includes partitioning fine-mode aerosol optical depth (fAOD) to individual aerosol's optical depth (AOD), separating black carbon and OA absorption aerosol optical depths, and finally binding OA SSA and sulfate+nitrate AOD. Our best estimate of OA SSA over tropical biomass burning region is 0.91 at 550nm with a range of 0.82-0.93. It implies the common OA SSA values of 0.96-1.0 in aerosol CTMs and GCMs significantly underrepresent OA light absorption. Model experiments with prescribed OA SSA showed that the enhanced absorption of solar radiation due to light absorbing OA yields global mean radiative forcing is +0.09 Wm-2 at the TOA, +0.21 Wm-2 at the atmosphere, and -0.12 Wm-2 at the surface. Compared to the previous assessment of OA radiative forcing reported in AeroCom II project, our result indicate that OA light absorption causes TOA radiative forcing by OA to change from negative (i.e., cooling effect) to positive (warming effect).

Aqueous aerosol SOA formation: impact on aerosol physical properties.

PubMed

Woo, Joseph L; Kim, Derek D; Schwier, Allison N; Li, Ruizhi; McNeill, V Faye

2013-01-01

Organic chemistry in aerosol water has recently been recognized as a potentially important source of secondary organic aerosol (SOA) material. This SOA material may be surface-active, therefore potentially affecting aerosol heterogeneous activity, ice nucleation, and CCN activity. Aqueous aerosol chemistry has also been shown to be a potential source of light-absorbing products ("brown carbon"). We present results on the formation of secondary organic aerosol material in aerosol water and the associated changes in aerosol physical properties from GAMMA (Gas-Aerosol Model for Mechanism Analysis), a photochemical box model with coupled gas and detailed aqueous aerosol chemistry. The detailed aerosol composition output from GAMMA was coupled with two recently developed modules for predicting a) aerosol surface tension and b) the UV-Vis absorption spectrum of the aerosol, based on our previous laboratory observations. The simulation results suggest that the formation of oligomers and organic acids in bulk aerosol water is unlikely to perturb aerosol surface tension significantly. Isoprene-derived organosulfates are formed in high concentrations in acidic aerosols under low-NO(x) conditions, but more experimental data are needed before the potential impact of these species on aerosol surface tension may be evaluated. Adsorption of surfactants from the gas phase may further suppress aerosol surface tension. Light absorption by aqueous aerosol SOA material is driven by dark glyoxal chemistry and is highest under high-NO(x) conditions, at high relative humidity, in the early morning hours. The wavelength dependence of the predicted absorption spectra is comparable to field observations and the predicted mass absorption efficiencies suggest that aqueous aerosol chemistry can be a significant source of aerosol brown carbon under urban conditions.

The Secondary Organic Aerosol Processor (SOAP v1.0) model: a unified model with different ranges of complexity based on the molecular surrogate approach

NASA Astrophysics Data System (ADS)

Couvidat, F.; Sartelet, K.

2015-04-01

In this paper the Secondary Organic Aerosol Processor (SOAP v1.0) model is presented. This model determines the partitioning of organic compounds between the gas and particle phases. It is designed to be modular with different user options depending on the computation time and the complexity required by the user. This model is based on the molecular surrogate approach, in which each surrogate compound is associated with a molecular structure to estimate some properties and parameters (hygroscopicity, absorption into the aqueous phase of particles, activity coefficients and phase separation). Each surrogate can be hydrophilic (condenses only into the aqueous phase of particles), hydrophobic (condenses only into the organic phases of particles) or both (condenses into both the aqueous and the organic phases of particles). Activity coefficients are computed with the UNIFAC (UNIversal Functional group Activity Coefficient; Fredenslund et al., 1975) thermodynamic model for short-range interactions and with the Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) parameterization for medium- and long-range interactions between electrolytes and organic compounds. Phase separation is determined by Gibbs energy minimization. The user can choose between an equilibrium representation and a dynamic representation of organic aerosols (OAs). In the equilibrium representation, compounds in the particle phase are assumed to be at equilibrium with the gas phase. However, recent studies show that the organic aerosol is not at equilibrium with the gas phase because the organic phases could be semi-solid (very viscous liquid phase). The condensation-evaporation of organic compounds could then be limited by the diffusion in the organic phases due to the high viscosity. An implicit dynamic representation of secondary organic aerosols (SOAs) is available in SOAP with OAs divided into layers, the first layer being at the center of the particle (slowly reaches equilibrium) and the final layer being near the interface with the gas phase (quickly reaches equilibrium). Although this dynamic implicit representation is a simplified approach to model condensation-evaporation with a low number of layers and short CPU (central processing unit) time, it shows good agreements with an explicit representation of condensation-evaporation (no significant differences after a few hours of condensation).

The New MODIS-Terra, and the Proposed COBRA Mission: First Global Aerosol Distribution and Properties Over Land and Ocean, and Plans to Measure Global Black Carbon Absorption Over the Ocean Glint

NASA Technical Reports Server (NTRS)

Kaufman, Yoram J.; Tanre, Didier; Remer, Lorraine; Martins, Vanderlei; Schoeberl, Mark; Lau, William K. M. (Technical Monitor)

2001-01-01

The MODIS instrument was launched on the NASA Terra satellite in Dec. 1999. Since last Oct, the sensor and the aerosol algorithm reached maturity and provide global daily retrievals of aerosol optical thickness and properties. MODIS has 36 spectral channels in the visible to IR with resolution down to 250 m. This allows accurate cloud screening and multi-spectral aerosol retrievals. We derive the aerosol optical thickness over the ocean and most of the land areas, distinguishing between fine (mainly man-made aerosol) and coarse (mainly natural) aerosol particles. New methods to derive the aerosol absorption of sunlight are also being developed. These measurements are use to track different aerosol sources, transport and the radiative forcing at the top and bottom of the atmosphere. However MODIS or any present satellite sensor cannot measure absorption by Black Carbon over the oceans, a critical component in studying climate change and human health. For this purpose we propose the COBRA mission that observes the ocean at glint and off glint simultaneously measuring the spectral polarized light and deriving precisely the aerosol absorption.

Hygroscopic Characteristics of Organic Laden Ambient Aerosols in Yosemite National Park

NASA Astrophysics Data System (ADS)

Malm, W. C.; Day, D. E.; Kreidenweis, S. M.; Collett, J. L.; Carrico, C. M.; Lee, T.; Bench, G.; Carrillo, J.

2003-12-01

Water absorption by inorganic compounds can be modeled with some degree of certainty; however, water uptake by ambient organic aerosols remains speculative. To improve the understanding of organic hygroscopicity, an aerosol characterization study was conducted at Yosemite National Park, California, starting in July and ending in the first week of September 2002. High time resolution measurement (15-minute time increments) of PM2.5 ionic species (Cl-, SO42-, NO3-, Na+, NH4+, K+, Mg2+, and Ca2+) were measured using PILS (Particle-Into-Liquid-System)/IC (Ion Chromatography). Commercially available annular denuders and a PM2.5 cyclone (URG) were used upstream of the PILS/IC to remove particles greater than 2.5 μm and acidic and basic gases. A dual wavelength aethalometer and an R&P particulate carbon monitor were used to measure carbon on a semi-continuous basis while a DRUM sampler allowed for semi-continuous estimates of concentrations of elements associated with crustal material. Standard IMPROVE type samplers were used to measure 24-hr integrated samples of these same aerosols. Two nephelometers operated in tandem, one dry and the other with a controlled humidity environment, were used to measure f(RH) = bscat(RH)/bscat,dry, where bscat(RH) is the scattering coefficient measured at some relative humidity and bscat,dry is the scattering coefficient measured at RH <10%. The aerosol composition was highly variable in time, with a strong diurnal cycle. Organic carbon mass was observed to be, on the average, 70% of the fine mass with days where its contribution was well over 95% of the mass. Measurements of carbon isotopes revealed the fraction of carbon from biogenic sources to range from approximately 73 to 95%. Water soluble potassium was highly correlated with carbon mass, suggesting the influence of wood smoke. The ionic fraction of the aerosol consisted primarily of ammonium sulfate and in most cases nitrate was in the form of sodium nitrate. Fine soil mass was less than 1% of PM2.5 mass. The ambient aerosol was observed to deliquesce on days when the inorganic and organic aerosol were approximately equal in concentration; however, on days when the organic component was dominant, only smooth f(RH) curves were observed. Equilibrium models, exercised in combination with Mie scattering theory, were used to predict atmospheric aerosol water content and associated increases in aerosol scattering coefficient. The analyses suggest that in most cases the hygroscopic growth of inorganic salts alone could account for the observed increase in scattering as a function of relative humidity.

Light Absorption of Biogenic Aerosol Particles in Amazonia

NASA Astrophysics Data System (ADS)

Holanda, B. A.; Artaxo, P.; Ferreira De Brito, J.; Barbosa, H. M.; Andreae, M. O.; Saturno, J.; Pöhlker, C.; Holben, B. N.; Schafer, J.

2014-12-01

Aerosol absorption is a key issue in proper calculation of aerosol radiative forcing. Especially in the tropics with the dominance of natural biogenic aerosol and brown carbon, the so called anomalous absorption is of particular interest. A special experiment was designed to study the wavelength dependence of aerosol absorption for PM2.5 as well as for PM10 particles in the wet season in Central Amazonia. Aerosol analysis occurred from May to August 2014, in the ZF2 ecological reservation, situated at about 55 km North of Manaus in very pristine conditions Two 7 wavelengths AE33 Aethalometers were deployed measuring in parallel, but with a PM2.5 and PM10 inlets. Two MAAP (Multiangle Aerosol Absorption Photometer) were operated in parallel with the AE33 exactly at the same PM2.5 and PM10 inlets. Organic and elemental carbon was analyzed using collection with quartz filters and analysis using a Sunset OC/EC analyzer. Aerosol light scattering for 3 wavelengths was measured using Air Photon and TSI Nephelometers. Aerosol size distribution was measured with one TSI SMPS and a GRIMM OPC to have the size range from 10 nm to 10 micrometers. Particles were measured under dry conditions using diffusion dryers. Aerosol optical depth and absorption was also measured with an AERONET sunphotometer operated close to the site. As the experiment was run in the wet season, very low equivalent black carbon (EBC) were measured, with average concentrations around 50 ng/m³ during May, increasing to 130 ng/m³ in June and July. The measurements adjusted for similar wavelengths shows excellent agreement between the MAAP and AE33 for both inlets (PM2.5 and PM10). It was not possible statistically infer absorption from the coarse mode biogenic particles, since the absorption was completely dominated by fine mode particles. AERONET measurements shows very low values of AOD, at 0.17 at 500 nm and 0.13 at 870 nm, with very low absorption AOD values at 0.00086 at 676 nm and 0.0068 at 872 nm. Single scattering albedo values will be calculated.

Insight into global trends in aerosol composition from 2005 to 2015 inferred from the OMI Ultraviolet Aerosol Index

NASA Astrophysics Data System (ADS)

Hammer, Melanie S.; Martin, Randall V.; Li, Chi; Torres, Omar; Manning, Max; Boys, Brian L.

2018-06-01

Observations of aerosol scattering and absorption offer valuable information about aerosol composition. We apply a simulation of the Ultraviolet Aerosol Index (UVAI), a method of detecting aerosol absorption from satellite observations, to interpret UVAI values observed by the Ozone Monitoring Instrument (OMI) from 2005 to 2015 to understand global trends in aerosol composition. We conduct our simulation using the vector radiative transfer model VLIDORT with aerosol fields from the global chemical transport model GEOS-Chem. We examine the 2005-2015 trends in individual aerosol species from GEOS-Chem and apply these trends to the UVAI simulation to calculate the change in simulated UVAI due to the trends in individual aerosol species. We find that global trends in the UVAI are largely explained by trends in absorption by mineral dust, absorption by brown carbon, and scattering by secondary inorganic aerosol. Trends in absorption by mineral dust dominate the simulated UVAI trends over North Africa, the Middle East, East Asia, and Australia. The UVAI simulation resolves observed negative UVAI trends well over Australia, but underestimates positive UVAI trends over North Africa and Central Asia near the Aral Sea and underestimates negative UVAI trends over East Asia. We find evidence of an increasing dust source from the desiccating Aral Sea that may not be well represented by the current generation of models. Trends in absorption by brown carbon dominate the simulated UVAI trends over biomass burning regions. The UVAI simulation reproduces observed negative trends over central South America and West Africa, but underestimates observed UVAI trends over boreal forests. Trends in scattering by secondary inorganic aerosol dominate the simulated UVAI trends over the eastern United States and eastern India. The UVAI simulation slightly overestimates the observed positive UVAI trends over the eastern United States and underestimates the observed negative UVAI trends over India. Quantitative simulation of the OMI UVAI offers new insight into global trends in aerosol composition.

Refractive Index and Absorption Attribution of Highly Absorbing Brown Carbon Aerosols from an Urban Indian City-Kanpur.

PubMed

Shamjad, P M; Tripathi, S N; Thamban, Navaneeth M; Vreeland, Heidi

2016-11-24

Atmospheric aerosols influence Earth's radiative balance, having both warming and cooling effects. Though many aerosols reflect radiation, carbonaceous aerosols such as black carbon and certain organic carbon species known as brown carbon have the potential to warm the atmosphere by absorbing light. Black carbon absorbs light over the entire solar spectrum whereas brown carbon absorbs near-UV wavelengths and, to a lesser extent, visible light. In developing countries, such as India, where combustion sources are prolific, the influence of brown carbon on absorption may be significant. In order to better characterize brown carbon, we present experimental and modeled absorption properties of submicron aerosols measured in an urban Indian city (Kanpur). Brown carbon here is found to be fivefold more absorbing at 365 nm wavelength compared to previous studies. Results suggest ~30% of total absorption in Kanpur is attributed to brown carbon, with primary organic aerosols contributing more than secondary organics. We report the spectral brown carbon refractive indices along with an experimentally constrained estimate of the influence of aerosol mixing state on absorption. We conclude that brown carbon in Kanpur is highly absorbing in nature and that the mixing state plays an important role in light absorption from volatile species.

Refractive Index and Absorption Attribution of Highly Absorbing Brown Carbon Aerosols from an Urban Indian City-Kanpur

PubMed Central

Shamjad, P. M.; Tripathi, S. N.; Thamban, Navaneeth M.; Vreeland, Heidi

2016-01-01

Atmospheric aerosols influence Earth’s radiative balance, having both warming and cooling effects. Though many aerosols reflect radiation, carbonaceous aerosols such as black carbon and certain organic carbon species known as brown carbon have the potential to warm the atmosphere by absorbing light. Black carbon absorbs light over the entire solar spectrum whereas brown carbon absorbs near-UV wavelengths and, to a lesser extent, visible light. In developing countries, such as India, where combustion sources are prolific, the influence of brown carbon on absorption may be significant. In order to better characterize brown carbon, we present experimental and modeled absorption properties of submicron aerosols measured in an urban Indian city (Kanpur). Brown carbon here is found to be fivefold more absorbing at 365 nm wavelength compared to previous studies. Results suggest ~30% of total absorption in Kanpur is attributed to brown carbon, with primary organic aerosols contributing more than secondary organics. We report the spectral brown carbon refractive indices along with an experimentally constrained estimate of the influence of aerosol mixing state on absorption. We conclude that brown carbon in Kanpur is highly absorbing in nature and that the mixing state plays an important role in light absorption from volatile species. PMID:27883083

The impact of biogenic carbon emissions on aerosol absorption inMexico City

DOE Office of Scientific and Technical Information (OSTI.GOV)

Marley, N; Gaffney, J; Tackett, M J

2009-02-24

In order to determine the wavelength dependence of atmospheric aerosol absorption in the Mexico City area, the absorption angstrom exponents (AAEs) were calculated from aerosol absorption measurements at seven wavelengths obtained with a seven-channel aethalometer during two field campaigns, the Mexico City Metropolitan Area study in April 2003 (MCMA 2003) and the Megacity Initiative: Local and Global Research Observations in March 2006 (MILAGRO). The AAEs varied from 0.76 to 1.56 in 2003 and from 0.54 to 1.52 in 2006. The AAE values determined in the afternoon were consistently higher than the corresponding morning values, suggesting the photochemical formation of absorbingmore » secondary organic aerosols (SOA) in the afternoon. The AAE values were compared to stable and radiocarbon isotopic measurements of aerosol samples collected at the same time to determine the sources of the aerosol carbon. The fraction of modern carbon (fM) in the aerosol samples, as determined from {sup 14}C analysis, showed that 70% of the carbonaceous aerosols in Mexico City were from modern sources, indicating a significant impact from biomass burning during both field campaigns. The {sup 13}C/{sup 12}C ratios of the aerosol samples illustrate the significant impact of Yucatan forest fires (C-3 plants) in 2003 and local grass fires (C-4 plants) at site T1 in 2006. A direct comparison of the fM values, stable carbon isotope ratios, and calculated aerosol AAEs suggested that the wavelength dependence of the aerosol absorption was controlled by the biogenically derived aerosol components.« less

Host Model Uncertainty in Aerosol Radiative Forcing Estimates - The AeroCom Prescribed Experiment

NASA Astrophysics Data System (ADS)

Stier, P.; Kinne, S.; Bellouin, N.; Myhre, G.; Takemura, T.; Yu, H.; Randles, C.; Chung, C. E.

2012-04-01

Anthropogenic and natural aerosol radiative effects are recognized to affect global and regional climate. However, even for the case of identical aerosol emissions, the simulated direct aerosol radiative forcings show significant diversity among the AeroCom models (Schulz et al., 2006). Our analysis of aerosol absorption in the AeroCom models indicates a larger diversity in the translation from given aerosol radiative properties (absorption optical depth) to actual atmospheric absorption than in the translation of a given atmospheric burden of black carbon to the radiative properties (absorption optical depth). The large diversity is caused by differences in the simulated cloud fields, radiative transfer, the relative vertical distribution of aerosols and clouds, and the effective surface albedo. This indicates that differences in host model (GCM or CTM hosting the aerosol module) parameterizations contribute significantly to the simulated diversity of aerosol radiative forcing. The magnitude of these host model effects in global aerosol model and satellites retrieved aerosol radiative forcing estimates cannot be estimated from the diagnostics of the "standard" AeroCom forcing experiments. To quantify the contribution of differences in the host models to the simulated aerosol radiative forcing and absorption we conduct the AeroCom Prescribed experiment, a simple aerosol model and satellite retrieval intercomparison with prescribed highly idealised aerosol fields. Quality checks, such as diagnostic output of the 3D aerosol fields as implemented in each model, ensure the comparability of the aerosol implementation in the participating models. The simulated forcing variability among the models and retrievals is a direct measure of the contribution of host model assumptions to the uncertainty in the assessment of the aerosol radiative effects. We will present the results from the AeroCom prescribed experiment with focus on the attribution to the simulated variability to parametric and structural model uncertainties. This work will help to prioritise areas for future model improvements and ultimately lead to uncertainty reduction.

Aerosol optical properties at a coastal site in Hong Kong, South China: temporal features, size dependencies and source analysis

NASA Astrophysics Data System (ADS)

Wang, Jiaping; Ding, Aijun; Virkkula, Aki; Lee, Shuncheng; Shen, Yicheng; Chi, Xuguang; Xu, Zheng

2016-04-01

Hong Kong is a typical coastal city adjacent to the Pearl River Delta (PRD) region in southern China, which is one of the regions suffering from severe air pollution. Atmospheric aerosols can affect the earth's radiative balance by scattering and absorbing incoming solar radiation. Black Carbon (BC) aerosol is a particularly emphasized component due to its strong light absorption. Aerosol transported from different source areas consists of distinct size distributions, leading to different optical properties. As the byproducts of the incomplete oxidation, BC and CO both have relatively long life time, their relationship is a good indicator for distinguishing different pollutant sources. In this study, temporal variations of aerosol optical properties and concentrations of BC and CO at a coastal background station in Hong Kong were investigated. Transport characteristics and origins of aerosol were elucidated by analyzing backward Lagrangian particle dispersion modeling (LPDM) results, together with related parameters including the relationships between optical properties and particle size, BC-CO correlations, ship location data and meteorological variables. From February 2012 to September 2013 and March 2014 to February 2015, continuous in-situ measurements of light scattering and absorption coefficients, particle size distribution and concentrations of BC and CO were conducted at Hok Tsui (HT), a coastal background station on the southeast tip of Hong Kong Island (22.22°N, 114.25°E, 60 m above the sea level) with few local anthropogenic activities. Affected by the Asian monsoon, this region is dominated by continental outflow in winter and by marine inflow from the South China Sea in summer, which is an ideal station for identifying the transport characteristics of aerosol and their effects on optical properties from different anthropogenic emission sources. 7-day backward Lagrangian particle dispersion modeling was performed for source identification. Three types of cases dominantly influenced by the PRD regional emission, long-range transport and marine exhaust were compared and discussed in detail.

Improving Calculation Accuracies of Accumulation-Mode Fractions Based on Spectral of Aerosol Optical Depths

NASA Astrophysics Data System (ADS)

Ying, Zhang; Zhengqiang, Li; Yan, Wang

2014-03-01

Anthropogenic aerosols are released into the atmosphere, which cause scattering and absorption of incoming solar radiation, thus exerting a direct radiative forcing on the climate system. Anthropogenic Aerosol Optical Depth (AOD) calculations are important in the research of climate changes. Accumulation-Mode Fractions (AMFs) as an anthropogenic aerosol parameter, which are the fractions of AODs between the particulates with diameters smaller than 1μm and total particulates, could be calculated by AOD spectral deconvolution algorithm, and then the anthropogenic AODs are obtained using AMFs. In this study, we present a parameterization method coupled with an AOD spectral deconvolution algorithm to calculate AMFs in Beijing over 2011. All of data are derived from AErosol RObotic NETwork (AERONET) website. The parameterization method is used to improve the accuracies of AMFs compared with constant truncation radius method. We find a good correlation using parameterization method with the square relation coefficient of 0.96, and mean deviation of AMFs is 0.028. The parameterization method could also effectively solve AMF underestimate in winter. It is suggested that the variations of Angstrom indexes in coarse mode have significant impacts on AMF inversions.

Using Single-Scattering Albedo Spectral Curvature to Characterize East Asian Aerosol Mixtures

NASA Technical Reports Server (NTRS)

Li, Jing; Carlson, Barbara E.; Lacis, Andrew A.

2015-01-01

Spectral dependence of aerosol single-scattering albedo (SSA) has been used to infer aerosol composition. In particular, aerosol mixtures dominated by dust absorption will have monotonically increasing SSA with wavelength while that dominated by black carbon absorption has monotonically decreasing SSA spectra. However, by analyzing SSA measured at four wavelengths, 440, 675, 870, and 1020 nm from the Aerosol Robotic Network data set, we find that the SSA spectra over East Asia are frequently peaked at 675 nm. In these cases, we suggest that SSA spectral curvature, defined as the negative of the second derivative of SSA as a function of wavelength, can provide additional information on the composition of these aerosol mixtures. Aerosol SSA spectral curvatures for East Asia during fall and winter are considerably larger than those found in places primarily dominated by biomass burning or dust aerosols. SSA curvature is found to increase as the SSA magnitude decreases. The curvature increases with coarse mode fraction (CMF) to a CMF value of about 0.4, then slightly decreases or remains constant at larger CMF. Mie calculations further verify that the strongest SSA curvature occurs at approx. 40% dust fraction, with 10% scattering aerosol fraction. The nonmonotonic SSA spectral dependence is likely associated with enhanced absorption in the shortwave by dust, absorption by black carbon at longer wavelengths, and also the flattened absorption optical depth spectral dependence due to the increased particle size.

Aerosol and gamma background measurements at Basic Environmental Observatory Moussala

NASA Astrophysics Data System (ADS)

Angelov, Christo; Arsov, Todor; Penev, Ilia; Nikolova, Nina; Kalapov, Ivo; Georgiev, Stefan

2016-03-01

Trans boundary and local pollution, global climate changes and cosmic rays are the main areas of research performed at the regional Global Atmospheric Watch (GAW) station Moussala BEO (2925 m a.s.l., 42°10'45'' N, 23°35'07'' E). Real time measurements and observations are performed in the field of atmospheric chemistry and physics. Complex information about the aerosol is obtained by using a threewavelength integrating Nephelometer for measuring the scattering and backscattering coefficients, a continuous light absorption photometer and a scanning mobile particle sizer. The system for measuring radioactivity and heavy metals in aerosols allows us to monitor a large scale radioactive aerosol transport. The measurements of the gamma background and the gamma-rays spectrum in the air near Moussala peak are carried out in real time. The HYSPLIT back trajectory model is used to determine the origin of the data registered. DREAM code calculations [2] are used to forecast the air mass trajectory. The information obtained combined with a full set of corresponding meteorological parameters is transmitted via a high frequency radio telecommunication system to the Internet.

Measurements of Intensive Aerosol Optical Properties During TexAQS II

NASA Astrophysics Data System (ADS)

Atkinson, D. B.; Radney, J. G.; Wright, M. E.

2007-12-01

Time-resolved measurements of the bulk extensive aerosol optical properties - particle extinction coefficient (bext) and particle scattering coefficient (bscat) - and particle number concentrations were made as part of the six-week TRAMP experiment during the TexAQS II (2006) study. These measurements were done at a nominal surface site (the roof of an 18 story building) on the University of Houston campus near downtown Houston, Texas. Our ground-based tandem cavity ring-down transmissometer/nephelometer instrument (CRDT/N) provided the aerosol optical property measurements. A commercial Condensation Particle Counter (TSI 3007) was used to measure the number concentrations during part of the study period. The optical data was used to construct the intensive aerosol optical properties single scattering albedo ω0 at 532 nm and the Angstrom exponent for extinction between 532 nm and 1064 nm. Recent validation studies of size- selected laboratory generated aerosols are presented to illustrate the soundness of this approach using our instrument. The Angstrom exponent is compared to values from other instruments operating in the area and is found to be a characteristic of the regional air mass under some conditions. Size distributions measured during the study were used to create a new empirical adjustment to scattering measured by the Radiance Research nephelometer, resulting in improved results for particle absorption coefficient and single scattering albedo. The study average value of ω0(532 nm) = 0.78 is lower than expected from comparable field studies and even lower values are experienced during the study. Possible causes of this discrepancy are examined and the utility of using the current version of the CRDT/N instrument to measure the key radiative property ω0 is assessed. Observed episodes of rapid increases in particle number concentration with little corresponding growth in the optical properties can presumably be used to signal the occurrence of particle nucleation or growth via gas-phase condensation. These results may be confirmed by other data taken during the TRAMP experiment. These results will be discussed in the context of aerosol effects on regional and larger scale climate.

He-Ne and CW CO2 laser long-path systems for gas detection

NASA Technical Reports Server (NTRS)

Grant, W. B.

1986-01-01

This paper describes the design and testing of a laboratory prototype dual He-Ne laser system for the detection of methane leaks from underground pipelines and solid-waste landfill sites using differential absorption of radiation backscattered from topographic targets. A laboratory-prototype dual CW carbon dioxide laser system also using topographic backscatter is discussed, and measurement results for methanol are given. With both systems, it was observed that the time-varying differential absorption signal was useful in indicating the presence of a gas coming from a nearby source. Limitations to measurement sensitivity, especially the role of speckle and atmospheric turbulence, are described. The speckle results for hard targets are contrasted with those from atmospheric aerosols. The appendix gives appropriate laser lines and values of absorption coefficients for the hydrazine fuel gases.

Viscothermal Coupling Effects on Sound Attenuation in Concentrated Colloidal Dispersions.

NASA Astrophysics Data System (ADS)

Han, Wei

1995-11-01

This thesis describes a Unified Coupled Phase Continuum (UCPC) model to analyze sound propagation through aerosols, emulsions and suspensions in terms of frequency dependent attenuation coefficient and sound speed. Expressions for the viscous and thermal coupling coefficients explicitly account for the effects of particle size, shape factor, orientation as well as concentration and the sound frequency. The UCPC model also takes into account the intrinsic acoustic absorption within the fluid medium due to its viscosity and heat conductivity. The effective complex wave number as a function of frequency is derived. A frequency- and concentration-dependent complex Nusselt number for the interfacial thermal coupling coefficient is derived using an approximate similarity between the 'viscous skin drag' and 'heat conduction flux' associated with the discontinuous suspended phase, on the basis of a cell model. The theoretical predictions of attenuation spectra provide satisfactory agreement with reported experimental data on two concentrated suspensions (polystyrene latex and kaolin pigment), two concentrated emulsions (toluene -in-water, n-hexadecane-in-water), and two aerosols (oleic acid droplets-in-nitrogen, alumina-in-air), covering a wide range of relative magnitudes (from 10^ {-3} to 10^{3}) of thermal versus viscous contributions, for dispersed phase volume fractions as high as 50%. The relative differences between the additive result of separate viscous and thermal loss estimates and combined viscothermal absorption results are also presented. Effects of particle shape on viscous attenuation of sound in concentrated suspensions of non-spherical clay particles are studied. Attenuation spectra for 18 frequencies from 3 to 100 MHz are measured and analyzed for eleven kaolin clay slurries with solid concentrations ranging from 0.6% to 35% (w/w). A modified viscous drag coefficient that considers frequency, concentration, particle size, shape and orientation of spheroids, is developed and applied to estimate the viscous attenuation coefficients. With incorporation of particle size and shape distributions (PSSD), predictions agree quantitatively with observed attenuation coefficients. The effects of particle aspect ratio and orientation become more evident as particle concentrations and frequencies are increased. The UCPC model combined with the ultrasonic spectroscopy techniques can provide for theoretical and experimental frameworks in characterization of concentrated colloidal dispersions.

Spatial and temporal variations of aerosols around Beijing in summer 2006: 2. Local and column aerosol optical properties

NASA Astrophysics Data System (ADS)

Matsui, H.; Koike, M.; Kondo, Y.; Takegawa, N.; Fast, J. D.; PöSchl, U.; Garland, R. M.; Andreae, M. O.; Wiedensohler, A.; Sugimoto, N.; Zhu, T.

2010-11-01

Model calculations were conducted using the Weather Research and Forecasting model coupled with chemistry (WRF-chem) for the region around Beijing, China, in the summer of 2006, when the CAREBeijing-2006 intensive campaign was conducted. In this paper, we interpret aerosol optical properties in terms of aerosol mass concentrations and their chemical compositions by linking model calculations with measurements. The model calculations generally captured the observed variability of various surface and column aerosol optical parameters in and around Beijing. At the surface, the spatial and temporal variations of aerosol absorption and scattering coefficients corresponded well to those of elemental carbon and sulfate mass concentrations, respectively, and were controlled by local-scale (<100 km and <24 hours) and regional-scale (<500 km and <3 days) emissions, respectively. The contribution of secondary aerosols and their water uptake increased with altitude within the planetary boundary layer. This variation led to a considerable increase in column aerosol optical depth and was responsible for the differences in regional and temporal variations between surface and column aerosol optical properties around Beijing. These processes are expected to be common in other megacity regions as well. Model calculations, however, underestimated or overestimated the absolute levels of aerosol optical properties in and around Beijing by up to 60%. Sensitivity studies showed that these discrepancies were mostly due to the uncertainties in aerosol mixing state and aerosol density (affecting mass extinction efficiency) in the model calculations. Good agreement with measurements is achieved when these aerosol properties are accurately predicted or assumed; however, significant bias can result when these properties are inadequately treated, even if total aerosol mass concentrations are reproduced well in the model calculations.

Source Attribution of Observed Absorption Profiles During the Two Column Aerosol Project (TCAP) Using a Regional Model

NASA Astrophysics Data System (ADS)

Fast, J. D.; Berg, L. K.; Chand, D.; Ferrare, R. A.; Flynn, C. J.; Hostetler, C. A.; Redemann, J.; Sedlacek, A. J., III; Shilling, J.; Shinozuka, Y.; Tomlinson, J. M.; Zelenyuk, A.

2015-12-01

Relatively large uncertainties remain in climate model predictions of absorption resulting from black carbon (BC) and brown carbon (BrC). In this study, we focus on comparing simulated profiles of BC, biomass burning aerosols, absorption, and other aerosol optical properties obtained from the regional WRF-Chem model with in situ and remote sensing measurements made during the Department of Energy's Two-Column Aerosol Project (TCAP). TCAP was designed to investigate changes in aerosol mixing state, aerosol radiative forcing, CCN concentration, and cloud-aerosol interactions in two atmospheric columns: one over Cape Cod, Massachusetts and another located approximately 200 km to the east over the ocean. Measurements from the NASA second-generation airborne High Resolution Spectral Lidar reveal the presence distinct aerosol layers associated with the marine boundary layer, residual layer transported over the ocean and in the free troposphere. Analyses of SP2 and aerosol optical measurements indicate that particles in the free troposphere were more 'aged' and had a lower single scattering albebo than for aerosol layers at lower altitudes; however, BC concentrations aloft were lower in the free troposphere. Instead, particle classes derived from the miniSPLAT single particle measurements suggest that the increased absorption aloft may be due biomass burning aerosols. The model suggests that ambient winds likely transported smoke from large wildfires in central Canada as well as smoke from other fires into the sampling domain. The simulated percentage of biomass burning aerosols was consistent with the miniSPLAT data, but the model currently treats all organic matter as non-absorbing. Therefore, we perform sensitivity simulations to examine how the model's absorption and AOD responds to assumptions used for BrC associated with biomass burning and whether the predicted profiles agree with absorption data and wavelength dependent AOD data from 4STAR.

An Analysis of AERONET Aerosol Absorption Properties and Classifications Representative of Aerosol Source Regions

NASA Technical Reports Server (NTRS)

Giles, David M.; Holben, Brent N.; Eck, Thomas F.; Sinyuk, Aliaksandr; Smirnov, Alexander; Slutsker, Ilya; Dickerson, R. R.; Thompson, A. M.; Schafer, J. S.

2012-01-01

Partitioning of mineral dust, pollution, smoke, and mixtures using remote sensing techniques can help improve accuracy of satellite retrievals and assessments of the aerosol radiative impact on climate. Spectral aerosol optical depth (tau) and single scattering albedo (omega (sub 0) ) from Aerosol Robotic Network (AERONET) measurements are used to form absorption [i.e., omega (sub 0) and absorption Angstrom exponent (alpha(sub abs))] and size [i.e., extinction Angstrom exponent (alpha(sub ext)) and fine mode fraction of tau] relationships to infer dominant aerosol types. Using the long-term AERONET data set (1999-2010), 19 sites are grouped by aerosol type based on known source regions to: (1) determine the average omega (sub 0) and alpha(sub abs) at each site (expanding upon previous work); (2) perform a sensitivity study on alpha(sub abs) by varying the spectral omega (sub 0); and (3) test the ability of each absorption and size relationship to distinguish aerosol types. The spectral omega (sub 0) averages indicate slightly more aerosol absorption (i.e., a 0.0 < delta omega (sub 0) <= 0.02 decrease) than in previous work and optical mixtures of pollution and smoke with dust show stronger absorption than dust alone. Frequency distributions of alpha(sub abs) show significant overlap among aerosol type categories and at least 10% of the alpha(sub abs) retrievals in each category are below 1.0. Perturbing the spectral omega (sub 0) by +/- 0.03 induces significant alpha(sub abs) changes from the unperturbed value by at least approx. +/- 0.6 for Dust, approx. +/-0.2 for Mixed, and approx. +/-0.1 for Urban/Industrial and Biomass Burning. The omega (sub 0)440nm and alpha(sub ext) 440-870nm relationship shows the best separation among aerosol type clusters, providing a simple technique for determining aerosol type from surface- and future space-based instrumentation.

Cloud Cover Increase with Increasing Aerosol Absorptivity: A Counterexample to the Conventional Semidirect Aerosol Effect

NASA Technical Reports Server (NTRS)

Perlwitz, Jan; Miller, Ron L.

2010-01-01

We reexamine the aerosol semidirect effect using a general circulation model and four cases of the single-scattering albedo of dust aerosols. Contrary to the expected decrease in low cloud cover due to heating by tropospheric aerosols, we find a significant increase with increasing absorptivity of soil dust particles in regions with high dust load, except during Northern Hemisphere winter. The strongest sensitivity of cloud cover to dust absorption is found over land during Northern Hemisphere summer. Here even medium and high cloud cover increase where the dust load is highest. The cloud cover change is directly linked to the change in relative humidity in the troposphere as a result of contrasting changes in specific humidity and temperature. More absorption by aerosols leads to larger diabatic heating and increased warming of the column, decreasing relative humidity. However, a corresponding increase in the specific humidity exceeds the temperature effect on relative humidity. The net effect is more low cloud cover with increasing aerosol absorption. The higher specific humidity where cloud cover strongly increases is attributed to an enhanced convergence of moisture driven by dust radiative heating. Although in some areas our model exhibits a reduction of low cloud cover due to aerosol heating consistent with the conventional description of the semidirect effect, we conclude that the link between aerosols and clouds is more varied, depending also on changes in the atmospheric circulation and the specific humidity induced by the aerosols. Other absorbing aerosols such as black carbon are expected to have a similar effect.

Carbonaceous Aerosol Removal During Precipitation Events: Climate Implications

NASA Astrophysics Data System (ADS)

Gaffney, J. S.; Marley, N. A.; Bridges, G. L.; Marchany-Rivera, A.; Begum, M.

2009-12-01

Atmospheric aerosols and their links to clouds are one of the main focus areas of the Department of Energy’s Atmospheric Systems Research, due to the fact that aerosols and clouds constitute the major uncertainties in radiative forcing that need to be reduced for more accurate modeling of climate, particularly regional climate. The impact of absorbing aerosols on radiative balance of the atmosphere will depend on their atmospheric lifetimes as well as their UV-visible absorption profiles. Aerosol lifetimes depend on the aerosols ability to take up water and grow to sufficient size to be either removed by gravitational settling or to act as cloud condensation nuclei and be removed by precipitation scavenging. The investigation of uv-visible absorbing aerosols is underway using a seven-channel aethalometer to evaluate the change in aerosol optical absorption during precipitation events. Angstrom absorption exponents (AAEs) are determined before, during, and after rain events to examine the impact on the aerosol absorption profiles anticipated by removal of the water soluble short-wave absorbing species (i.e. HULIS) that can be produced by photochemical oxidation of biogenic emissions (isoprene, monoterpenes, sesquiterpenes). Aerosol absorption data are presented from observations made at the University of Arkansas at Little Rock and other sites, which clearly show that a significant amount of absorbing carbon is not removed during rain events, and that the organic matter removed is likely secondary organics produced from biogenic precursors. The dissolved organic carbon measured in precipitation samples along with determinations of natural radionuclide tracers are also used to help examine the extent of carbonaceous aerosol removal by precipitation. The data are discussed in terms of the potential impacts of anthropogenic enhancement of aerosol absorption by secondary organic aerosols adding to atmospheric heating and changes in atmospheric dynamics. The potential impacts of these organic aerosol species as sources of organic carbon in surface waters is also addressed. This work was supported by the Office of Science (BER), U.S. Department of Energy, Grant No. DE-FG02-07ER64328 and Grant No. DE-FG02-07-ER64329 as part of the Atmospheric Science Program.

Shortwave Radiative Fluxes, Solar-Beam Transmissions, and Aerosol Properties: TARFOX and ACE-2 Find More Absorption from Flux Radiometry than from Other Measurements

NASA Technical Reports Server (NTRS)

Russell, Philip B.; Redemann, J.; Schmid, B.; Livingston, J. M.; Bergstrom, R. W.; Ramirez, S. A.; Hipskind, R. Stephen (Technical Monitor)

2001-01-01

The Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX) and the Second Aerosol Characterization Experiment (ACE-2) made simultaneous measurements of shortwave radiative fluxes, solar-beam transmissions, and the aerosols affecting those fluxes and transmissions. Besides the measured fluxes and transmissions, other obtained properties include aerosol scattering and absorption measured in situ at the surface and aloft; aerosol single scattering albedo retrieved from skylight radiances; and aerosol complex refractive index derived by combining profiles of backscatter, extinction, and size distribution. These measurements of North Atlantic boundary layer aerosols impacted by anthropogenic pollution revealed the following characteristic results: (1) Better agreement among different types of remote measurements of aerosols (e.g., optical depth, extinction, and backscattering from sunphotometers, satellites, and lidars) than between remote and in situ measurements; 2) More extinction derived from transmission measurements than from in situ measurements; (3) Larger aerosol absorption inferred from flux radiometry than from other measurements. When the measured relationships between downwelling flux and optical depth (or beam transmission) are used to derive best-fit single scattering albedos for the polluted boundary layer aerosol, both TARFOX and ACE-2 yield midvisible values of 0.90 +/- 0.04. The other techniques give larger single scattering albedos (i.e. less absorption) for the polluted boundary layer, with a typical result of 0.95 +/- 0.04. Although the flux-based results have the virtue of describing the column aerosol unperturbed by sampling, they are subject to questions about representativeness and other uncertainties (e.g., unknown gas absorption). Current uncertainties in aerosol single scattering albedo are large in terms of climate effects. They also have an important influence on aerosol optical depths retrieved from satellite radiances. More tests are needed of the consistency among different methods and of the effects of changing humidity on aerosol.

Modeling investigation of light-absorbing aerosols in the Amazon Basin during the wet season

NASA Astrophysics Data System (ADS)

Wang, Qiaoqiao; Saturno, Jorge; Chi, Xuguang; Walter, David; Lavric, Jost; Moran-Zuloaga, Daniel; Ditas, Florian; Pöhlker, Christopher; Brito, Joel; Carbone, Samara; Artaxo, Paulo; Andreae, Meinrat

2017-04-01

We use a global chemical transport model (GEOS-Chem) to interpret observed light-absorbing aerosols in Amazonia during the wet season. Observed aerosol properties, including black carbon (BC) concentration and light absorption, at the Amazon Tall Tower Observatory (ATTO) site in the central Amazon have relatively low background levels but frequently show high peaks during the study period of January-April 2014. With daily temporal resolution for open fire emissions and modified aerosol optical properties, our model successfully captures the observed variation in fine/coarse aerosol and BC concentrations as well as aerosol light absorption and its wavelength dependence over the Amazon Basin. The source attribution in the model indicates the important influence of open fire on the observed variances of aerosol concentrations and absorption, mainly from regional sources (northern South America) and from northern Africa. The contribution of open fires from these two regions is comparable, with the latter becoming more important in the late wet season. The analysis of correlation and enhancement ratios of BC versus CO suggests transport times of < 3 days for regional fires and 11 days for African plumes arriving at ATTO during the wet season. The model performance of long-range transport of African plumes is also evaluated with observations from AERONET, MODIS, and CALIOP. Simulated absorption aerosol optical depth (AAOD) averaged over the wet season is lower than 0.0015 over the central Amazon, including the ATTO site. We find that more than 50% of total absorption at 550 nm is from BC, except for the northeastern Amazon and the Guianas, where the influence of dust becomes significant (up to 35 %). The brown carbon contribution is generally between 20 and 30 %. The distribution of absorption Ångström exponents (AAE) suggests more influence from fossil fuel combustion in the southern part of the basin (AAE 1) but more open fire and dust influence in the northern part (AAE > 1.8). Uncertainty analysis shows that accounting for absorption due to secondary organic aerosol (SOA) and primary biogenic aerosol (PBA) particles could result in differences of < 8 and 5-40% in total absorption, respectively.

AERONET derived (BC) aerosol absorption

NASA Astrophysics Data System (ADS)

Kinne, S.

2015-12-01

AERONET is a ground-based sun-/sky-photometer network with good annual statistics at more than 400 sites worldwide. Inversion methods applied to these data define all relevant column aerosol optical properties and reveal even microphysical detail. The extracted data include estimates for aerosol size-distributions and for aerosol refractive indices at four different solar wavelengths. Hereby, the imaginary parts of the refractive indices define the aerosol column absorption. For regional and global averages and radiative impact assessment with off-line radiative transfer, these local data have been extended with distribution patterns offered by AeroCom modeling experiments. Annual and seasonal absorption distributions for total aerosol and estimates for component contributions (such as BC) are presented and associated direct forcing impacts are quantified.

The Effect of Aerosol Hygroscopicity and Volatility on Aerosol Optical Properties During Southern Oxidant and Aerosol Study

NASA Astrophysics Data System (ADS)

Khlystov, A.; Grieshop, A. P.; Saha, P.; Subramanian, R.

2014-12-01

Secondary organic aerosol (SOA) from biogenic sources can influence optical properties of ambient aerosol by altering its hygroscopicity and contributing to light absorption directly via formation of brown carbon and indirectly by enhancing light absorption by black carbon ("lensing effect"). The magnitude of these effects remains highly uncertain. A set of state-of-the-art instruments was deployed at the SEARCH site near Centerville, AL during the Southern Oxidant and Aerosol Study (SOAS) campaign in summer 2013 to measure the effect of relative humidity and temperature on aerosol size distribution, composition and optical properties. Light scattering and absorption by temperature- and humidity-conditioned aerosols was measured using three photo-acoustic extinctiometers (PAX) at three wavelengths (405 nm, 532 nm, and 870 nm). The sample-conditioning system provided measurements at ambient RH, 10%RH ("dry"), 85%RH ("wet"), and 200 C ("TD"). In parallel to these measurements, a long residence time temperature-stepping thermodenuder (TD) and a variable residence time constant temperature TD in combination with three SMPS systems and an Aerosol Chemical Speciation Monitor (ACSM) were used to assess aerosol volatility and kinetics of aerosol evaporation. We will present results of the on-going analysis of the collected data set. We will show that both temperature and relative humidity have a strong effect on aerosol optical properties. SOA appears to increase aerosol light absorption by about 10%. TD measurements suggest that aerosol equilibrated fairly quickly, within 2 s. Evaporation varied substantially with ambient aerosol loading and composition and meteorology.

Closure on the single scattering albedo in the WRF-Chem framework using data from the MILAGRO campaign

NASA Astrophysics Data System (ADS)

Barnard, J. C.; Fast, J. D.; Paredes-Miranda, G.; Arnott, W. P.

2009-02-01

Data from the MILAGRO field campaign, which took place in the Mexico City Metropolitan Area (MCMA) during March 2006, is used to perform a closure experiment between aerosol chemical properties and aerosol optical properties. Measured aerosol chemical properties, obtained from the MILAGRO T1 site, are fed to two different "chemical to optical properties" modules. One module uses a sectional approach and is identical to that used in the WRF-Chem model, while the other is based on a modal approach. This modal code is employed as an independent check on the WRF-Chem module. Both modules compute aerosol optical properties and, in particular, the single-scattering albedo, ϖ0, as a function of time. The single-scattering albedos are compared to independent measurements obtained from a photoacoustic spectrometer (PAS). Because chemical measurements of the aerosol coarse mode were not available, and the inlet of the PAS could not ingest aerosols larger than about 2 to 3 μm, we focus here on the fine-mode ϖ0. At 870 nm, the wavelength of the PAS measurements, the agreement between the computed (modal and WRF-Chem) and observed fine-mode ϖ0, averaged over the course of the campaign, is reasonably good. The observed ϖ0 value is 0.77, while for both modules, the calculated value was 0.75 resulting in a difference of 0.02 between observations and both computational approaches. This difference is less than the uncertainty of the observed ϖ0 values (6%, or 0.05), and therefore "closure" is achieved, at least for mean values. After adjusting some properties of black carbon absorption and mass concentration within plausible uncertainty limits, the two modules simulate well the diurnal variation of ϖ0, and the absorption coefficient, Babs, but are less successful in calculating the variation of the scattering coefficient, Bscat. This difficulty is probably caused by the presence of larger particles during the day when windblown dust is ubiquitous; this dust likely increases the proportion of large particles introduced into the PAS. The dust also contributes to a very large aerosol mass loading in the coarse mode, and neglect of the coarse mode may cause significant errors, estimated to be as large as 0.07, in the calculation and measurement of ambient ϖ0. Finally, the observed ϖ0 is compared to the ϖ0 computed by the full WRF-Chem model, which includes prognostic aerosol chemistry. Unlike the results discussed above, a comparison between observed and simulated ϖ0 values reveals major differences. This large discrepancy is probably due, in part, to poor characterization of emissions near the T1 site, particularly black carbon emissions.

Analysis of reflectance spectra of UV-absorbing aerosol scenes measured by SCIAMACHY

NASA Astrophysics Data System (ADS)

de Graaf, M.; Stammes, P.; Aben, E. A. A.

2007-01-01

Reflectance spectra from 280-1750 nm of typical desert dust aerosol (DDA) and biomass burning aerosol (BBA) scenes over oceans are presented, measured by the space-borne spectrometer Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY). DDA and BBA are both UV-absorbing aerosols, but their effect on the top-of-atmosphere (TOA) reflectance is different due to differences in the way mineral aerosols and smoke reflect and absorb radiation. Mineral aerosols are typically large, inert particles, found in warm, dry continental air. Smoke particles, on the other hand, are usually small particles, although often clustered, chemically very active and highly variable in composition. Moreover, BBA are hygroscopic and over oceans BBA were invariably found in cloudy scenes. TOA reflectance spectra of typical DDA and BBA scenes were analyzed, using radiative transfer simulations, and compared. The DDA spectrum was successfully simulated using a layer with a bimodal size distribution of mineral aerosols in a clear sky. The spectrum of the BBA scene, however, was determined by the interaction between cloud droplets and smoke particles, as is shown by simulations with a model of separate aerosol and cloud layers and models with internally and externally mixed aerosol/cloud layers. The occurrence of clouds in smoke scenes when sufficient water vapor is present usually prevents the detection of optical properties of these aerosol plumes using space-borne sensors. However, the Absorbing Aerosol Index (AAI), a UV color index, is not sensitive to scattering aerosols and clouds and can be used to detect these otherwise obscured aerosol plumes over clouds. The amount of absorption of radiation can be expressed using the absorption optical thickness. The absorption optical thickness in the DDA case was 0.42 (340 nm) and 0.14 (550 nm) for an aerosol layer of optical thickness 1.74 (550 nm). In the BBA case the absorption optical thickness was 0.18 (340 nm) and 0.10 (550 nm) for an aerosol/cloud layer of optical thickness 20.0 (550 nm). However, this reduced the cloud albedo by about 0.2 (340 nm) and 0.15 (550 nm). This method can be an important tool to estimate the global impact of absorption of shortwave radiation by smoke and industrial aerosols inside clouds.

Direct radiative effect of carbonaceous aerosols from crop residue burning during the summer harvest season in East China

NASA Astrophysics Data System (ADS)

Yao, Huan; Song, Yu; Liu, Mingxu; Archer-Nicholls, Scott; Lowe, Douglas; McFiggans, Gordon; Xu, Tingting; Du, Pin; Li, Jianfeng; Wu, Yusheng; Hu, Min; Zhao, Chun; Zhu, Tong

2017-04-01

East China experiences extensive crop residue burnings in fields during harvest season. The direct radiative effect (DRE) of carbonaceous aerosols from crop residue burning in June 2013 in East China was investigated using the Weather Research and Forecasting Model coupled with Chemistry (WRF-Chem). Absorption of organic aerosol (OA) in the presence of brown carbon was considered using the parameterization of Saleh et al. (2014), in which the imaginary part of the OA refractive index is a function of wavelength and the ratio of black carbon (BC) and OA. The carbonaceous emissions from crop fires were estimated using the Moderate Resolution Imaging Spectroradiometer (MODIS) fire radiative power (FRP) product with a localized crop-burning-sourced BC-to-organic carbon (OC) ratio emission ratio of 0.27. Evaluation of the model results with in situ measurements of particulate matter with aerodynamic diameter less than 2.5 µm (PM2. 5) chemical composition, MODIS aerosol optical depth (AOD) detections and meteorological observations showed that this model was able to reproduce the magnitude, spatial variation and optical characteristics of carbonaceous aerosol pollution. The observed BC and OC peak concentrations at the site in Suixi, Anhui province, during the 2013 wheat burning season reached 55.3 µg m-3 and 157.9 µg m-3. WRF-Chem simulations reproduced these trends with a correlation coefficient of 0.74, estimating that crop residue burning contributed 86 and 90 % of peak BC and OC, respectively. The simulated hourly DRE from crop residue burning at the top of atmosphere (TOA) reached a maximum of +22.66 W m-2 at the Suixi site. On average, the simulations showed that the crop residue burning introduced a net positive DRE of +0.14 W m-2 at TOA throughout East China, with BC from this source as the main heating contributor (+0.79 W m-2). The OA DRE from crop burning (-0.22 W m-2) was a combined effect of the positive DRE of absorption (+0.21 W m-2) and a stronger negative DRE of scattering (-0.43 W m-2). Sensitivity tests showed that the DRE of OA absorption strongly depended on the imaginary part of the OA refractive index, the BC-to-OA emission ratio from crop residue burning and the assumed mixing state of the aerosol, whereby the volume mixing treatment resulted in a higher positive DRE compared to the core-shell treatment. The BC mixing state and associated absorption enhancement during BC aging processes will be investigated in detail in future research.

The Secondary Organic Aerosol Processor (SOAP v1.0) model: a unified model with different ranges of complexity based on the molecular surrogate approach

NASA Astrophysics Data System (ADS)

Couvidat, F.; Sartelet, K.

2014-01-01

The Secondary Organic Aerosol Processor (SOAP v1.0) model is presented. This model is designed to be modular with different user options depending on the computing time and the complexity required by the user. This model is based on the molecular surrogate approach, in which each surrogate compound is associated with a molecular structure to estimate some properties and parameters (hygroscopicity, absorption on the aqueous phase of particles, activity coefficients, phase separation). Each surrogate can be hydrophilic (condenses only on the aqueous phase of particles), hydrophobic (condenses only on the organic phase of particles) or both (condenses on both the aqueous and the organic phases of particles). Activity coefficients are computed with the UNIFAC thermodynamic model for short-range interactions and with the AIOMFAC parameterization for medium and long-range interactions between electrolytes and organic compounds. Phase separation is determined by Gibbs energy minimization. The user can choose between an equilibrium and a dynamic representation of the organic aerosol. In the equilibrium representation, compounds in the particle phase are assumed to be at equilibrium with the gas phase. However, recent studies show that the organic aerosol (OA) is not at equilibrium with the gas phase because the organic phase could be semi-solid (very viscous liquid phase). The condensation or evaporation of organic compounds could then be limited by the diffusion in the organic phase due to the high viscosity. A dynamic representation of secondary organic aerosols (SOA) is used with OA divided into layers, the first layer at the center of the particle (slowly reaches equilibrium) and the final layer near the interface with the gas phase (quickly reaches equilibrium).

Light Absorption of Brown Carbon Aerosol in the Pearl River Delta Region of China

NASA Astrophysics Data System (ADS)

Huang, X.

2015-12-01

X.F. Huang, J.F. Yuan, L.M. Cao, J. Cui, C.N. Huang, Z.J. Lan and L.Y. He Key Laboratory for Urban Habitat Environmental Science and Technology, School of Environment and Energy, Peking University Shenzhen Graduate School, Shenzhen 518055, ChinaCorresponding author. Tel.: +86 755 26032532; fax: +86 755 26035332. E-mail address: huangxf@pku.edu.cn (X. F. Huang). Abstract: The strong spectral dependence of light absorption of brown carbon (BrC) aerosol has been recognized in recent decades. The Absorption Angstrom Exponent (AAE) of ambient aerosol was widely used in previous studies to attribute light absorption of brown carbon at shorter wavelengths, with a theoretical assumption that the AAE of black carbon (BC) aerosol equals to unit. In this study, the AAE method was improved by statistical extrapolation based on ambient measurements in the polluted seasons in typical urban and rural areas in the Pearl River Delta (PRD) region of China. A three-wavelength photoacoustic soot spectrometer (PASS-3) and an aerosol mass spectrometer (AMS) were used to explore the relationship between the ambient measured AAE and the ratio of organic aerosol to BC aerosol, in order to extract the more realistic AAE by pure BC aerosol, which were found to be 0.86, 0.82 and 1.02 at 405nm and 0.70, 0.71, and 0.86 at 532nm in the campaigns of urban-winter, urban-fall, and rural-fall, respectively. Roadway tunnel experiment results further supported the effectiveness of the obtained AAE for pure BC aerosol. In addition, biomass burning experiments proved higher spectral dependence of more-BrC environment and further verified the reliability of the instruments' response. Then, the average light absorption contribution of BrC aerosol was calculated to be 11.7, 6.3 and 12.1% (with total relative uncertainty of 7.5, 6.9 and 10.0%) at 405nm and 10.0, 4.1 and 5.5% (with total relative uncertainty of 6.5, 8.6 and 15.4%) at 532nm of the three campaigns, respectively. These results indicate that the brown carbon contribution to the aerosol light absorption at shorter wavelengths is not negligible in the PRD region, with a rough magnitude of 10%. Key words: Light absorption, Absorption Angstrom Exponent (AAE), Brown carbon (BrC), Black carbon (BC)

Characterization of aerosol scattering and spectral absorption by unique methods: a polar/imaging nephelometer and spectral reflectance measurements of aerosol samples collected on filters

NASA Astrophysics Data System (ADS)

Dolgos, Gergely; Martins, J. Vanderlei; Remer, Lorraine A.; Correia, Alexandre L.; Tabacniks, Manfredo; Lima, Adriana R.

2010-02-01

Characterization of aerosol scattering and absorption properties is essential to accurate radiative transfer calculations in the atmosphere. Applications of this work include remote sensing of aerosols, corrections for aerosol distortions in satellite imagery of the surface, global climate models, and atmospheric beam propagation. Here we demonstrate successful instrument development at the Laboratory for Aerosols, Clouds and Optics at UMBC that better characterizes aerosol scattering phase matrix using an imaging polar nephelometer (LACO-I-Neph) and enables measurement of spectral aerosol absorption from 200 nm to 2500 nm. The LACO-I-Neph measures the scattering phase function from 1.5° to 178.5° scattering angle with sufficient sensitivity to match theoretical expectations of Rayleigh scattering of various gases. Previous measurements either lack a sufficiently wide range of measured scattering angles or their sensitivity is too low and therefore the required sample amount is prohibitively high for in situ measurements. The LACO-I-Neph also returns expected characterization of the linear polarization signal of Rayleigh scattering. Previous work demonstrated the ability of measuring spectral absorption of aerosol particles using a reflectance technique characterization of aerosol samples collected on Nuclepore filters. This first generation methodology yielded absorption measurements from 350 nm to 2500 nm. Here we demonstrate the possibility of extending this wavelength range into the deep UV, to 200 nm. This extended UV region holds much promise in identifying and characterizing aerosol types and species. The second generation, deep UV, procedure requires careful choice of filter substrates. Here the choice of substrates is explored and preliminary results are provided.

Competing Atmospheric and Surface-Driven Impacts of Absorbing Aerosols on the East Asian Summer Monsoon

NASA Astrophysics Data System (ADS)

Persad, G.; Paynter, D.; Ming, Y.; Ramaswamy, V.

2015-12-01

Absorbing aerosols, by attenuating shortwave radiation within the atmosphere and reemitting it as longwave radiation, redistribute energy both vertically within the surface-atmosphere column and horizontally between polluted and unpolluted regions. East Asia has the largest concentrations of anthropogenic absorbing aerosols globally, and these, along with the region's scattering aerosols, have both reduced the amount of solar radiation reaching the Earth's surface regionally ("solar dimming") and increased shortwave absorption within the atmosphere, particularly during the peak months of the East Asian Summer Monsoon (EASM). We here analyze how atmospheric absorption and surface solar dimming compete in driving the response of EASM circulation to anthropogenic absorbing aerosols, which dominates, and why—issues of particular importance for predicting how the EASM will respond to projected changes in absorbing and scattering aerosol emissions in the future. We probe these questions in a state-of-the-art general circulation model (GCM) using a combination of realistic and idealized aerosol perturbations that allow us to analyze the relative influence of absorbing aerosols' atmospheric and surface-driven impacts on EASM circulation. In combination, our results make clear that, although absorption-driven dimming has a less detrimental effect on EASM circulation than purely scattering-driven dimming, aerosol absorption is still a net impairment to EASM strength when both its atmospheric and surface effects are considered. Because atmospheric heating is not efficiently conveyed to the surface, the surface dimming and associated cooling from even a pure absorber is sufficient to counteract its atmospheric heating, resulting in a net reduction in EASM strength. These findings elevate the current understanding of the impacts of aerosol absorption on the EASM, improving our ability to diagnose EASM responses to current and future regional changes in aerosol emissions.

In situ aerosol optics in Reno, NV, USA during and after the summer 2008 California wildfires and the influence of aerosol coatings

NASA Astrophysics Data System (ADS)

Gyawali, M.; Arnott, W. P.; Lewis, K.; Moosmüller, H.

2009-06-01

Hundreds of wildfires in Northern California were sparked by lightning during the summer of 2008, resulting in downwind smoke for the months of June and July. Comparisons are reported for aerosol optics measurements in Reno Nevada made during the very smoky summer month of July and the relatively clean month of August. Photoacoustic instruments equipped with integrating nephelometers were used to measure aerosol light scattering and absorption at wavelengths of 405 nm and 870 nm, revealing a strong variation of the aerosol light absorption with wavelength. Coated sphere calculations were used to show that Ångström exponents of absorption (AEA) as large as 1.6 are possible even with non-absorbing organic coatings on black carbon cores, suggesting care be exercised when diagnosing AEA. Insight on fuels burned is gleaned from comparison of AEA versus single scattering albedo (SSA) of the ambient measurements with laboratory biomass smoke measurements for many fuels. Measurements during the month of August, which were largely unaffected by fire smoke, exhibit surprisingly low AEA for aerosol light absorption when the SSA is highest, again likely as a consequence of the underappreciated wavelength dependence of aerosol light absorption by particles coated with non absorbing organic and inorganic matter.

Particle size distribution of the stratospheric aerosol from SCIAMACHY limb measurements

NASA Astrophysics Data System (ADS)

Rozanov, Alexei; Malinina, Elizaveta; Bovensmann, Heinrich; Burrows, John

2017-04-01

A crucial role of the stratospheric aerosols for the radiative budget of the Earth's atmosphere and the consequences for the climate change are widely recognized. A reliable knowledge on physical and optical properties of the stratospheric aerosols as well as on their vertical and spatial distributing is a key issue to assure a proper initialization and running conditions for climate models. On a global scale this information can only be gained from space borne measurements. While a series of past, present and future instruments provide extensive date sets of such aerosol characteristics as extinction coefficient or backscattering ratio, information on a size distribution of the stratospheric aerosols is sparse. One of the important sources on vertically and spatially resolved information on the particle size distribution of stratospheric aerosols is provided by space borne measurements of the scattered solar light in limb viewing geometry performed in visible, near-infrared and short-wave infrared spectral ranges. SCIAMACHY (SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY) instrument operated on the European satellite Envisat from 2002 to 2102 was capable of providing spectral information needed to retrieve parameters of aerosol particle size distributions. In this presentation we discuss the retrieval method, present first validation results with SAGE II data and analyze first data sets of stratospheric aerosol particle size distribution parameters obtained from SCIAMACHY limb measurements. The research work was performed in the framework of ROMIC (Role of the middle atmosphere in climate) project.

Vertical Profiles of Aerosol Volume from High Spectral Resolution Infrared Transmission Measurements: Results

NASA Technical Reports Server (NTRS)

Eldering, Annmarie; Kahn, Brian H.; Mills, Franklin P.; Irion, Fredrick W.; Steele, Helen M.; Gunson, Michael R.

2004-01-01

The high-resolution infrared absorption spectra of the Atmospheric Trace Molecule Spectroscopy (ATMOS) experiment are utilized to derive vertical profiles of sulfate aerosol volume density and extinction coefficient. Following the eruption of Mt. Pinatubo in June 1991, the ATMOS spectra obtained on three Space Shuttle missions (1992, 1993, and 1994) provide a unique opportunity to study the global stratospheric sulfate aerosol layer shortly after a major volcanic eruption and periodically during the decay phase. Synthetic sulfate aerosol spectra are fit to the observed spectra, and a global fitting inversion routine is used to derive vertical profiles of sulfate aerosol volume density. Vertical profiles of sulfate aerosol volume density for the three missions over portions of the globe are presented, with the peak in aerosol volume density occurring from as low as 10 km (polar latitudes) to as high as 20 km (subtropical latitudes). Derived aerosol volume density is as high as 2-3.5 (mu)m(exp 3) per cubic centimeter +/-10% in 1992, decreasing to 0.2-0.5 (mu)m(exp 3) per cubic centimeter +/-20% in 1994, in agreement with other experiments. Vertical extinction profiles derived from ATMOS are compared with profiles from Improved Stratospheric And Mesospheric Sounder (ISAMS) and Cryogenic Limb Array Etalon Spectrometer (CLAES) that coincide in space and time and show good general agreement. The uncertainty of the ATMOS vertical profiles is similar to CLAES and consistently smaller than ISAMS at similar altitudes.

Exploring the observational constraints on the simulation of brown carbon

NASA Astrophysics Data System (ADS)

Wang, Xuan; Heald, Colette L.; Liu, Jiumeng; Weber, Rodney J.; Campuzano-Jost, Pedro; Jimenez, Jose L.; Schwarz, Joshua P.; Perring, Anne E.

2018-01-01

Organic aerosols (OA) that strongly absorb solar radiation in the near-UV are referred to as brown carbon (BrC). The sources, evolution, and optical properties of BrC remain highly uncertain and contribute significantly to uncertainty in the estimate of the global direct radiative effect (DRE) of aerosols. Previous modeling studies of BrC optical properties and DRE have been unable to fully evaluate model performance due to the lack of direct measurements of BrC absorption. In this study, we develop a global model simulation (GEOS-Chem) of BrC and test it against BrC absorption measurements from two aircraft campaigns in the continental US (SEAC4RS and DC3). To the best of our knowledge, this is the first study to compare simulated BrC absorption with direct aircraft measurements. We show that BrC absorption properties estimated based on previous laboratory measurements agree with the aircraft measurements of freshly emitted BrC absorption but overestimate aged BrC absorption. In addition, applying a photochemical scheme to simulate bleaching/degradation of BrC improves model skill. The airborne observations are therefore consistent with a mass absorption coefficient (MAC) of freshly emitted biomass burning OA of 1.33 m2 g-1 at 365 nm coupled with a 1-day whitening e-folding time. Using the GEOS-Chem chemical transport model integrated with the RRTMG radiative transfer model, we estimate that the top-of-the-atmosphere all-sky direct radiative effect (DRE) of OA is -0.344 Wm-2, 10 % higher than that without consideration of BrC absorption. Therefore, our best estimate of the absorption DRE of BrC is +0.048 Wm-2. We suggest that the DRE of BrC has been overestimated previously due to the lack of observational constraints from direct measurements and omission of the effects of photochemical whitening.

Chemical apportionment of aerosol optical properties during the Asia-Pacific Economic Cooperation summit in Beijing, China

NASA Astrophysics Data System (ADS)

Han, Tingting; Xu, Weiqi; Chen, Chen; Liu, Xingang; Wang, Qingqing; Li, Jie; Zhao, Xiujuan; Du, Wei; Wang, Zifa; Sun, Yele

2015-12-01

We have investigated the chemical and optical properties of aerosol particles during the 2014 Asia-Pacific Economic Cooperation (APEC) summit in Beijing, China, using the highly time-resolved measurements by a high-resolution aerosol mass spectrometer and a cavity attenuated phase shift extinction monitor. The average (±σ) extinction coefficient (bext) and absorption coefficient (bap) were 186.5 (±184.5) M m-1 and 23.3 (±21.9) M m-1 during APEC, which were decreased by 63% and 56%, respectively, compared to those before APEC primarily due to strict emission controls. The aerosol composition and size distributions showed substantial changes during APEC; as a response, the mass scattering efficiency (MSE) of PM1 was decreased from 4.7 m2 g-1 to 3.5 m2 g-1. Comparatively, the average single-scattering albedo (SSA) remained relatively unchanged, illustrating the synchronous reductions of bext and bap during APEC. MSE and SSA were found to increase as function of the oxidation degree of organic aerosol (OA), indicating a change of aerosol optical properties during the aging processes. The empirical relationships between chemical composition and particle extinction were established using a multiple linear regression model. Our results showed the largest contribution of ammonium nitrate to particle extinction, accounting for 35.1% and 29.3% before and during APEC, respectively. This result highlights the important role of ammonium nitrate in the formation of severe haze pollution during this study period. We also observed very different optical properties of primary and secondary aerosol. Owing to emission controls in Beijing and surrounding regions and also partly the influences of meteorological changes, the average bext of secondary aerosol during APEC was decreased by 71% from 372.3 M m-1 to 108.5 M m-1, whereas that of primary aerosol mainly from cooking, traffic, and biomass burning emissions showed a smaller reduction from 136.7 M m-1 to 71.3 M m-1. As a result, the contribution of primary aerosol to particle extinction increased from 26.8% to 39.6%, elucidating an enhanced role of local primary sources in visibility deterioration during APEC. Further analysis of chemically resolved particle extinction showed that the extinction contributions of aerosol species varied greatly between different air masses but generally with ammonium nitrate, ammonium sulfate, and secondary OA being the three major contributors.

Optical Properties of Black and Brown Carbon Aerosols from Laboratory Combustion of Wildland Fuels

NASA Astrophysics Data System (ADS)

Beres, N. D.; Molzan, J.

2015-12-01

Aerosol light absorption in the solar spectral region (300 nm - 2300 nm) of the atmosphere is key for the direct aerosol radiative forcing, which is determined by aerosol single scattering albedo (SSA), asymmetry parameter, and by the albedo of the underlying surface. SSA is of key importance for the sign and quantity of aerosol direct radiative forcing; that is, does the aerosol make the earth look darker (heating) or whiter (cooling)? In addition, these optical properties are needed for satellite retrievals of aerosol optical depth and properties. During wildland fires, aerosol optical absorption is largely determined by black carbon (BC) and brown carbon (BrC) emissions. BC is strongly absorbing throughout the solar spectrum, while BrC absorption strongly increases toward shorter wavelength and can be neglected in the red and infrared. Optical properties of BrC emitted from wildland fires are poorly understood and need to be studied as function of fuel type and moisture content and combustion conditions. While much more is known about BC optical properties, knowledge for the ultraviolet (UV) spectral region is still lacking and critically needed for satellite remote sensing (e.g., TOMS, OMI) and for modeling of tropospheric photochemistry. Here, a project to better characterize biomass burning aerosol optical properties is described. It utilizes a laboratory biomass combustion chamber to generate aerosols through combustion of different wildland fuels of global and regional importance. Combustion aerosol optics is characterized with an integrating nephelometer to measure aerosol light scattering and a photoacoustic instrument to measure aerosol light absorption. These measurements will yield optical properties that are needed to improve qualitative and quantitative understanding of aerosol radiative forcing and satellite retrievals for absorbing carbonaceous aerosols from combustion of wildland fuels.

Field measurements of trace gases and aerosols emitted by peat fires in Central Kalimantan, Indonesia, during the 2015 El Niño

NASA Astrophysics Data System (ADS)

Stockwell, Chelsea E.; Jayarathne, Thilina; Cochrane, Mark A.; Ryan, Kevin C.; Putra, Erianto I.; Saharjo, Bambang H.; Nurhayati, Ati D.; Albar, Israr; Blake, Donald R.; Simpson, Isobel J.; Stone, Elizabeth A.; Yokelson, Robert J.

2016-09-01

Peat fires in Southeast Asia have become a major annual source of trace gases and particles to the regional-global atmosphere. The assessment of their influence on atmospheric chemistry, climate, air quality, and health has been uncertain partly due to a lack of field measurements of the smoke characteristics. During the strong 2015 El Niño event we deployed a mobile smoke sampling team in the Indonesian province of Central Kalimantan on the island of Borneo and made the first, or rare, field measurements of trace gases, aerosol optical properties, and aerosol mass emissions for authentic peat fires burning at various depths in different peat types. This paper reports the trace gas and aerosol measurements obtained by Fourier transform infrared spectroscopy, whole air sampling, photoacoustic extinctiometers (405 and 870 nm), and a small subset of the data from analyses of particulate filters. The trace gas measurements provide emission factors (EFs; grams of a compound per kilogram biomass burned) for up to ˜ 90 gases, including CO2, CO, CH4, non-methane hydrocarbons up to C10, 15 oxygenated organic compounds, NH3, HCN, NOx, OCS, HCl, etc. The modified combustion efficiency (MCE) of the smoke sources ranged from 0.693 to 0.835 with an average of 0.772 ± 0.053 (n = 35), indicating essentially pure smoldering combustion, and the emissions were not initially strongly lofted. The major trace gas emissions by mass (EF as g kg-1) were carbon dioxide (1564 ± 77), carbon monoxide (291 ± 49), methane (9.51 ± 4.74), hydrogen cyanide (5.75 ± 1.60), acetic acid (3.89 ± 1.65), ammonia (2.86 ± 1.00), methanol (2.14 ± 1.22), ethane (1.52 ± 0.66), dihydrogen (1.22 ± 1.01), propylene (1.07 ± 0.53), propane (0.989 ± 0.644), ethylene (0.961 ± 0.528), benzene (0.954 ± 0.394), formaldehyde (0.867 ± 0.479), hydroxyacetone (0.860 ± 0.433), furan (0.772 ± 0.035), acetaldehyde (0.697 ± 0.460), and acetone (0.691 ± 0.356). These field data support significant revision of the EFs for CO2 (-8 %), CH4 (-55 %), NH3 (-86 %), CO (+39 %), and other gases compared with widely used recommendations for tropical peat fires based on a lab study of a single sample published in 2003. BTEX compounds (benzene, toluene, ethylbenzene, xylenes) are important air toxics and aerosol precursors and were emitted in total at 1.5 ± 0.6 g kg-1. Formaldehyde is probably the air toxic gas most likely to cause local exposures that exceed recommended levels. The field results from Kalimantan were in reasonable agreement with recent lab measurements of smoldering Kalimantan peat for "overlap species," lending importance to the lab finding that burning peat produces large emissions of acetamide, acrolein, methylglyoxal, etc., which were not measurable in the field with the deployed equipment and implying value in continued similar efforts. The aerosol optical data measured include EFs for the scattering and absorption coefficients (EF Bscat and EF Babs, m2 kg-1 fuel burned) and the single scattering albedo (SSA) at 870 and 405 nm, as well as the absorption Ångström exponents (AAE). By coupling the absorption and co-located trace gas and filter data we estimated black carbon (BC) EFs (g kg-1) and the mass absorption coefficient (MAC, m2 g-1) for the bulk organic carbon (OC) due to brown carbon (BrC). Consistent with the minimal flaming, the emissions of BC were negligible (0.0055 ± 0.0016 g kg-1). Aerosol absorption at 405 nm was ˜ 52 times larger than at 870 nm and BrC contributed ˜ 96 % of the absorption at 405 nm. Average AAE was 4.97 ± 0.65 (range, 4.29-6.23). The average SSA at 405 nm (0.974 ± 0.016) was marginally lower than the average SSA at 870 nm (0.998 ± 0.001). These data facilitate modeling climate-relevant aerosol optical properties across much of the UV/visible spectrum and the high AAE and lower SSA at 405 nm demonstrate the dominance of absorption by the organic aerosol. Comparing the Babs at 405 nm to the simultaneously measured OC mass on filters suggests a low MAC ( ˜ 0.1) for the bulk OC, as expected for the low BC/OC ratio in the aerosol. The importance of pyrolysis (at lower MCE), as opposed to glowing (at higher MCE), in producing BrC is seen in the increase of AAE with lower MCE (r2 = 0.65).

Retrieval of Aerosol Absorption Properties from Satellite Observations

NASA Technical Reports Server (NTRS)

Torres, Omar; Bhartia, Pawan K.; Jethva, H.; Ahn, Chang-Woo

2012-01-01

The Angstrom Absorption Exponent (AAE) is a parameter commonly used to characterize the wavelength-dependence of aerosol absorption optical depth (AAOD). It is closely related to aerosol composition. Black carbon (BC) containing aerosols yield AAE values near unity whereas Organic carbon (OC) aerosol particles are associated with values larger than 2. Even larger AAE values have been reported for desert dust aerosol particles. Knowledge of spectral AAOD is necessary for the calculation of direct radiative forcing effect of aerosols and for inferring aerosol composition. We have developed a satellitebased method of determining the spectral AAOD of absorbing aerosols. The technique uses multi-spectral measurements of upwelling radiation from scenes where absorbing aerosols lie above clouds as indicated by the UV Aerosol Index. For those conditions, the satellite measurement can be explained, using an approximations of Beer's Law (BL), as the upwelling reflectance at the cloud top attenuated by the absorption effects of the overlying aerosol layer. The upwelling reflectance at the cloud-top in an aerosol-free atmospheric column is mainly a function of cloud optical depth (COD). In the proposed method of AAE derivation, the first step is determining COD which is retrieved using a previously developed color-ratio based approach. In the second step, corrections for molecular scattering effects are applied to both the observed ad the calculated cloud reflectance terms, and the spectral AAOD is then derived by an inversion of the BL approximation. The proposed technique will be discussed in detail and application results making use of OMI multi-spectral measurements in the UV-Vis. will be presented.

Aerosol Optical Properties at the Lulin Atmospheric Background Station in Taiwan and the Influences of Long-Range Transport of Air Pollutants

NASA Technical Reports Server (NTRS)

Hsiao, Ta-Chih; Chen, Wei-Nai; Ye, Wei-Cheng; Lin, Neng-Huei; Tsay, Si-Chee; Lin, Tang-Huang; Lee, Chung-Te; Chuang, Ming-Tung; Pantina, Peter; Wang, Sheng-Hsiang

2016-01-01

The Lulin Atmospheric Background Station (LABS, 23.47 deg. N 120.87 deg. E, 2862 m ASL) in Central Taiwan was constructed in 2006 and is the only high-altitude background station in the western Pacific region for studying the influence of continental outflow. In this study, extensive optical properties of aerosols, including the aerosol light scattering coefficient [Sigma(sub s)] and light absorption coefficient [Sigma(sub a)], were collected from 2013 to 2014. The intensive optical properties, including mass scattering efficiency [Sigma(sub s)], mass absorption efficiency [Sigma(sub a)] single scattering albedo (Omega), scattering Angstrom exponent (A), and backscattering fraction (b), were determined and investigated, and the distinct seasonal cycle was observed. The value of [Alpha(sub a)] began to increase in January and reached a maximum in April; the mean in spring was 5.89 m(exp. 2) g(exp. -1) with a standard deviation (SD) of 4.54 m(exp. 2) g(exp. -1) and a 4.48 m(exp. 2) g(exp. -1) interquartile range (IQR: 2.95-7.43 m(exp. 2) g(exp. -1). The trend was similar in [Sigma(sub a)], with a maximum in March and a monthly mean of 0.84 m(exp. 2) g(exp. -1). The peak values of Omega (Mean = 0.92, SD = 0.03, IQR: 0.90 - 0.93) and A (Mean = 2.22, SD = 0.61, IQR: 2.12 = 2.47) occurred in autumn. These annual patterns of optical properties were associated with different long-range transport patterns of air pollutants such as biomass burning (BB) aerosol in spring and potential anthropogenic emissions in autumn. The optical measurements performed at LABS during spring in 2013 were compared with those simultaneously performed at the Doi Ang Kang Meteorology Station, Chiang Mai Province, Thailand (DAK, 19.93 deg. N, 99.05 deg. E, 1536 m a.s.l.), which is located in the Southeast Asia BB source region. Furthermore, the relationships among [Sigma(sub s)], [Sigma(sub a)], and (b) were used to characterize the potential aerosol types transported to LABS during different seasons, and the data were inspected according to the HYSPLIT 5-day backward trajectories, which differentiate between different regions of air mass origin.

Radiative Absorption by Light Absorbing Carbon: Uncertainty, Temporal and Spatial Variation in a Typical Polluted City in Yangtze River Delta

NASA Astrophysics Data System (ADS)

Chen, D.; Zhao, Y.; Lyu, R.

2017-12-01

The optical properties of light absorbing carbon (LAC) in atmospheric aerosols, including their uncertainties, temporal change and spatial pattern were studied at suburban, urban and industrial sites in Nanjing, a typical polluted city in Yangtze River Delta (YRD). The optical properties of black carbon (BC) and the uncertainty in radiative absorption of BC were quantified combining cavity attenuated phase shift (CAPS) and thermal-optical techniques. It was found that applying a constant value from previous studies for multiple scattering factor could not well represent the actual absorption characteristics of aerosols in Nanjing. The relative deviation between calculated and measured absorption coefficient of BC was up to 56 ± 34%. A significant positive correlation (R2=0.95) was found between multiple scattering factor (C*) and the mixing state of EC (ECopt/EC) within the ECopt/EC ranged 0.43 0.92 (C*=1.64(ECopt/EC)+1.47, 0.43opt/EC<0.57; C*=6.42(ECopt/EC)-1.39, 0.57opt/EC<0.92). However, C* were not linearly correlated with ECopt/EC when the ratios were below 0.43 or above 0.92. The content of isoprene from biogenic volatile organic compounds (BVOCs) was higher in summer (5.8%) than that in autumn (0.5%). Brown carbon (BrC) associated with anthropogenic precursors was stronger in light absorption than that from biogenic sources, thus precursors of secondary organic aerosol (SOA) was probably the main reason for seasonal variation in MAE of BrC. At industrial site, linear positive correlation (R=0.87) was found between measured MSOC and secondary organic carbon (SOC), suggesting SOA formation was the major source of MSOC in this area. The lower MAE values of MSOC indicated that BrC generated from secondary sources might demonstrate weaker light absorbing ability than that from primary emissions. Furthermore, quantitative analysis showed that MAE BrC, 365 reduced by 0.26 m2/g when SOC increased by 1μgC/m3. This study provided insights into a more comprehensive understanding of LAC aerosol in cities with heavy particle pollution, since MSOC served as a surrogate for BrC and EC was measured with reliable and effective methods.

Excitation-emission spectra and fluorescence quantum yields for fresh and aged biogenic secondary organic aerosols

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lee, Hyun Ji; Laskin, Alexander; Laskin, Julia

2013-05-10

Certain biogenic secondary organic aerosols (SOA) become absorbent and fluorescent when exposed to reduced nitrogen compounds such as ammonia, amines and their salts. Fluorescent SOA may potentially be mistaken for biological particles by detection methods relying on fluorescence. This work quantifies the spectral distribution and effective quantum yields of fluorescence of SOA generated from two monoterpenes, limonene and a-pinene, and two different oxidants, ozone (O3) and hydroxyl radical (OH). The SOA was generated in a smog chamber, collected on substrates, and aged by exposure to ~100 ppb ammonia vapor in air saturated with water vapor. Absorption and excitation-emission matrix (EEM)more » spectra of aqueous extracts of aged and control SOA samples were measured, and the effective absorption coefficients and fluorescence quantum yields (~0.005 for 349 nm excitation) were determined from the data. The strongest fluorescence for the limonene-derived SOA was observed for excitation = 420+- 50 nm and emission = 475 +- 38 nm. The window of the strongest fluorescence shifted to excitation = 320 +- 25 nm and emission = 425 +- 38 nm for the a-pinene-derived SOA. Both regions overlap with the excitation-emission matrix (EEM) spectra of some of the fluorophores found in primary biological aerosols. Our study suggests that, despite the low quantum yield, the aged SOA particles should have sufficient fluorescence intensities to interfere with the fluorescence detection of common bioaerosols.« less

Excitation-emission spectra and fluorescence quantum yields for fresh and aged biogenic secondary organic aerosols.

PubMed

Lee, Hyun Ji Julie; Laskin, Alexander; Laskin, Julia; Nizkorodov, Sergey A

2013-06-04

Certain biogenic secondary organic aerosols (SOA) become absorbent and fluorescent when exposed to reduced nitrogen compounds such as ammonia, amines, and their salts. Fluorescent SOA may potentially be mistaken for biological particles by detection methods relying on fluorescence. This work quantifies the spectral distribution and effective quantum yields of fluorescence of water-soluble SOA generated from two monoterpenes, limonene and α-pinene, and two different oxidants, ozone (O3) and hydroxyl radical (OH). The SOA was generated in a smog chamber, collected on substrates, and aged by exposure to ∼100 ppb ammonia in air saturated with water vapor. Absorption and excitation-emission matrix (EEM) spectra of aqueous extracts of aged and control SOA samples were measured, and the effective absorption coefficients and fluorescence quantum yields (∼0.005 for 349 nm excitation) were determined from the data. The strongest fluorescence for the limonene-derived SOA was observed for λexcitation = 420 ± 50 nm and λemission = 475 ± 38 nm. The window of the strongest fluorescence shifted to λexcitation = 320 ± 25 nm and λemission = 425 ± 38 nm for the α-pinene-derived SOA. Both regions overlap with the EEM spectra of some of the fluorophores found in primary biological aerosols. Despite the low quantum yield, the aged SOA particles may have sufficient fluorescence intensities to interfere with the fluorescence detection of common bioaerosols.

Estimation of UV index in the clear-sky using OMI PROFOZ and AERONET data

NASA Astrophysics Data System (ADS)

Lee, H.; Kim, J.; Jeong, U.

2016-12-01

Due to a strong influence to the human health and ecosystem environment, continuous monitoring of the surface-level ultraviolet (UV) radiation is important nowadays. UV index (UVI) is a simple parameter to show the strength of surface UV radiation, therefore UVI has been widely utilized for the purpose of UV monitoring. In this work, we also try to develop our own retrieval algorithm for better estimation of UVI. The amount of UVA (320-400 nm) and UVB (290-320 nm) radiation at the Earth surface depends on the extent of Rayleigh scattering by atmospheric gas molecules, the radiative absorption by ozone, radiative scattering by clouds, and both absorption and scattering by airborne aerosols. Thus advanced consideration of these factors is the essential part to establish the process of UVI estimation. In this study, we estimate UV Index (UVI) at Seoul first in a clear-sky atmosphere, and then validate this estimated UVI comparing to UVI from Brewer spectrophotometer measurements located at Yonsei University in Seoul. We use the Vector Linearized Discrete Ordinate Radiative Transfer (VLIDORT) model version 2.6 for our UVI calculation. To consider the ozone and aerosol influence in a real situation, we input ozone and temperature profiles from the Ozone Monitoring Instrument (OMI) Aura vertical profile ozone (PROFOZ) data, and aerosol properties from the AErosol RObotic NETwork (AERONET) measurements at Seoul into the model. Inter-comparison of UVI is performed for the year 2011, 2012 and 2014, and resulted in a high correlation coefficient (R=0.95) under clear-sky condition. But a slight overestimation of Brewer UVI occurred under high AOD conditions in clear-sky. Because our UVI algorithm does not account for surface absorbing aerosols, it is lead to systematic overestimation of surface UV irradiances. Therefore, we also investigate the effect of absorbing aerosol on the amount of UV irradiance in the clear-sky over East Asia.

1 Mixing state and absorbing properties of black carbon during Arctic haze

NASA Astrophysics Data System (ADS)

Zanatta, Marco; Gysel, Martin; Eleftheriadis, Kosas; Laj, Paolo; Hans-Werner, Jacobi

2016-04-01

The Arctic atmosphere is periodically affected by the Arctic haze occurring in spring. One of its particulate components is the black carbon (BC), which is considered to be an important contributor to climate change in the Arctic region. Beside BC-cloud interaction and albedo reduction of snow, BC may influence Arctic climate interacting directly with the solar radiation, warming the corresponding aerosol layer (Flanner, 2013). Such warming depends on BC atmospheric burden and also on the efficiency of BC to absorb light, in fact the light absorption is enhanced by mixing of BC with other atmospheric non-absorbing materials (lensing effect) (Bond et al., 2013). The BC reaching the Arctic is evilly processed, due to long range transport. Aging promote internal mixing and thus absorption enhancement. Such modification of mixing and is quantification after long range transport have been observed in the Atlantic ocean (China et al., 2015) but never investigated in the Arctic. During field experiments conducted at the Zeppelin research site in Svalbard during the 2012 Arctic spring, we investigated the relative precision of different BC measuring techniques; a single particle soot photometer was then used to assess the coating of Arctic black carbon. This allowed quantifying the absorption enhancement induced by internal mixing via optical modelling; the optical assessment of aged black carbon in the arctic will be of major interest for future radiative forcing assessment.Optical characterization of the total aerosol indicated that in 2012 no extreme smoke events took place and that the aerosol population was dominated by fine and non-absorbing particles. Low mean concentration of rBC was found (30 ng m-3), with a mean mass equivalent diameter above 200 nm. rBC concentration detected with the continuous soot monitoring system and the single particle soot photometer was agreeing within 15%. Combining absorption coefficient observed with an aethalometer and rBC mass concentration from SP2, a mass absorption cross section of 6.0 m2 g-1 was found at a wavelength of 880 nm. Concerning mixing, rBC cores with a dimeter between 170 nm and 280 nm were found to be covered by a layer of non-absorbing material having a median thickness of 50 nm. From Mie calculation, such mixing would lead to an enhancement of absorption of 46% compared to a bare BC core. The aforementioned absorption enhancement would lead to a net decrease of single scattering albedo of the total aerosol of less than 1%. The reliability of Mie approach was confirmed by agreement with observations, while MAC values commonly used in radiative forcing models might lead to discrepancies up to 80%. Our work provides all the major optical properties of total aerosol and BC to minimize the uncertainty of radiative estimations based on a priori assumptions.

Aerosol Correction for Remotely Sensed Sea Surface Temperatures From the NOAA AVHRR: Phase II

NASA Astrophysics Data System (ADS)

Nalli, N. R.; Ignatov, A.

2002-05-01

For over two decades, the National Oceanic and Atmospheric Administration (NOAA) has produced global retrievals of sea surface temperature (SST) using infrared (IR) data from the Advanced Very High Resolution Radiometer (AVHRR). The standard multichannel retrieval algorithms are derived from regression analyses of AVHRR window channel brightness temperatures against in situ buoy measurements under non-cloudy conditions thus providing a correction for IR attenuation due to molecular water vapor absorption. However, for atmospheric conditions with elevated aerosol levels (e.g., arising from dust, biomass burning and volcanic eruptions), such algorithms lead to significant negative biases in SST because of IR attenuation arising from aerosol absorption and scattering. This research presents the development of a 2nd-phase aerosol correction algorithm for daytime AVHRR SST. To accomplish this, a long-term (1990-1998), global AVHRR-buoy matchup database was created by merging the Pathfinder Atmospheres (PATMOS) and Oceans (PFMDB) data sets. The merged data are unique in that they include multi-year, global daytime estimates of aerosol optical depth (AOD) derived from AVHRR channels 1 and 2 (0.63 and 0.83 μ m, respectively), along with an effective Angstrom exponent derived from the AOD retrievals (Ignatov and Nalli, 2002). Recent enhancements in the aerosol data constitute an improvement over the Phase I algorithm (Nalli and Stowe, 2002) which relied only on channel 1 AOD and the ratio of normalized reflectance from channels 1 and 2. The Angstrom exponent and channel 2 AOD provide important statistical information about the particle size distribution of the aerosol. The SST bias can be parametrically expressed as a function of observed AVHRR channels 1 and 2 slant-path AOD, normalized reflectance ratio and the Angstrom exponent. Based upon these empirical relationships, aerosol correction equations are then derived for the daytime multichannel and nonlinear SST (MCSST and NLSST) algorithms. Separate sets of coefficients are utilized for two aerosol modes, these being stratospheric/tropospheric (e.g., volcanic aerosol) and tropospheric (e.g., dust, smoke). The algorithms are subsequently applied to retrospective PATMOS data to demonstrate the potential for climate applications. The minimization of cold biases in the AVHRR SST, as demonstrated in this work, should improve its overall utility for the general user community.

Impact of Tropospheric Aerosol Absorption on Ozone Retrieval from buv Measurements

NASA Technical Reports Server (NTRS)

Torres, O.; Bhartia, P. K.

1998-01-01

The impact of tropospheric aerosols on the retrieval of column ozone amounts using spaceborne measurements of backscattered ultraviolet radiation is examined. Using radiative transfer calculations, we show that uv-absorbing desert dust may introduce errors as large as 10% in ozone column amount, depending on the aerosol layer height and optical depth. Smaller errors are produced by carbonaceous aerosols that result from biomass burning. Though the error is produced by complex interactions between ozone absorption (both stratospheric and tropospheric), aerosol scattering, and aerosol absorption, a surprisingly simple correction procedure reduces the error to about 1%, for a variety of aerosols and for a wide range of aerosol loading. Comparison of the corrected TOMS data with operational data indicates that though the zonal mean total ozone derived from TOMS are not significantly affected by these errors, localized affects in the tropics can be large enough to seriously affect the studies of tropospheric ozone that are currently undergoing using the TOMS data.

Long-term measurements of aerosol and carbon monoxide at the ZOTTO tall tower to characterize polluted and pristine air in the Siberian taiga

NASA Astrophysics Data System (ADS)

Chi, X.; Winderlich, J.; Mayer, J.-C.; Panov, A. V.; Heimann, M.; Birmili, W.; Heintzenberg, J.; Cheng, Y.; Andreae, M. O.

2013-12-01

Siberia is one of few continental regions in the Northern Hemisphere where the atmosphere may sometimes approach pristine background conditions. We present the time series of aerosol and carbon monoxide (CO) measurements between September 2006 and December 2011 at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 89° E). We investigate the seasonal, weekly and diurnal variations of aerosol properties (including absorption and scattering coefficients and derived parameters, such as equivalent black carbon (BCe), Ångström exponent, single scattering albedo, and backscattering ratio) and the CO mixing ratios. Criteria were established to distinguish polluted from near-pristine air masses, providing quantitative characteristics for each type. Depending on the season, 23-36% of the sampling time at ZOTTO was found to be representative of a clean atmosphere. The summer pristine data indicate that primary biogenic and secondary organic aerosol formation are quite strong particle sources in the Siberian taiga. The summer seasons 2007-2008 were dominated by an Aitken mode around 80 nm size, whereas the summer 2009 with prevailing easterly winds produced particles in the accumulation mode around 200 nm size. We found these differences to be mainly related to air temperature, through its effect on the production rates of biogenic volatile organic compounds (VOC) precursor gases. In winter, the particle size distribution peaked at 160 nm, and the footprint of clean background air was characteristic for aged particles from anthropogenic sources at great distances from ZOTTO and diluted biofuel burning emissions from domestic heating. The wintertime polluted air originates mainly from large cities south and southwest of the site; these particles have a dominant mode around 100 nm, and the ΔBCe / ΔCO ratio of 7-11 ng m-3 ppb-1 suggests dominant contributions from coal and biofuel burning for heating. During summer, anthropogenic emissions are the dominant contributor to the pollution particles at ZOTTO, while only 12% of the polluted events are classified as biomass-burning-dominated, but then often associated with extremely high CO concentrations and aerosol absorption coefficients. Two biomass-burning case studies revealed different ΔBCe / ΔCO ratios from different fire types, with the agricultural fires in April~2008 yielding a very high ratio of 21 ng m-3 ppb-1. Overall, we find that anthropogenic sources dominate the aerosol population at ZOTTO most of the time, even during nominally clean episodes in winter, and that near-pristine conditions are encountered only in the growing season and then only episodically.

Asian dust aerosol: Optical effect on satellite ocean color signal and a scheme of its correction

NASA Astrophysics Data System (ADS)

Fukushima, H.; Toratani, M.

1997-07-01

The paper first exhibits the influence of the Asian dust aerosol (KOSA) on a coastal zone color scanner (CZCS) image which records erroneously low or negative satellite-derived water-leaving radiance especially in a shorter wavelength region. This suggests the presence of spectrally dependent absorption which was disregarded in the past atmospheric correction algorithms. On the basis of the analysis of the scene, a semiempirical optical model of the Asian dust aerosol that relates aerosol single scattering albedo (ωA) to the spectral ratio of aerosol optical thickness between 550 nm and 670 nm is developed. Then, as a modification to a standard CZCS atmospheric correction algorithm (NASA standard algorithm), a scheme which estimates pixel-wise aerosol optical thickness, and in turn ωA, is proposed. The assumption of constant normalized water-leaving radiance at 550 nm is adopted together with a model of aerosol scattering phase function. The scheme is combined to the standard algorithm, performing atmospheric correction just the same as the standard version with a fixed Angstrom coefficient except in the case where the presence of Asian dust aerosol is detected by the lowered satellite-derived Angstrom exponent. Some of the model parameter values are determined so that the scheme does not produce any spatial discontinuity with the standard scheme. The algorithm was tested against the Japanese Asian dust CZCS scene with parameter values of the spectral dependency of ωA, first statistically determined and second optimized for selected pixels. Analysis suggests that the parameter values depend on the assumed Angstrom coefficient for standard algorithm, at the same time defining the spatial extent of the area to apply the Asian dust scheme. The algorithm was also tested for a Saharan dust scene, showing the relevance of the scheme but with different parameter setting. Finally, the algorithm was applied to a data set of 25 CZCS scenes to produce a monthly composite of pigment concentration for April 1981. Through these analyses, the modified algorithm is considered robust in the sense that it operates most compatibly with the standard algorithm yet performs adaptively in response to the magnitude of the dust effect.

Wavelength dependence of aerosol backscatter coefficients obtained by multiple wavelength Lidar measurements

NASA Technical Reports Server (NTRS)

Sasano, Y.; Browell, E. V.

1986-01-01

Aerosols are often classified into several general types according to their origins and composition, such as maritime, continental, and stratospheric aerosols, and these aerosol types generally have different characteristics in chemical and physical properties. The present study aims at demonstrating the potential for distinguishing these aerosol types by the wavelength dependence of their backscatter coefficients obtained from quantitative analyses of multiple wavelength lidar signals. Data from the NASA Airborne Differential Abosrption lidar (DIAL) S ystems, which can measure aerosol backscatter profiles at wavelenghts of 300, 600, and 1064 nm and ozone profiles of backscatter coefficients for these three wavelength were derived from the observations of aerosols of different types. Observations were performed over the Atlantic Ocean, the Southwestern United States, and French Guyana.

Light absorption of organic aerosol from pyrolysis of corn stalk

NASA Astrophysics Data System (ADS)

Li, Xinghua; Chen, Yanju; Bond, Tami C.

2016-11-01

Organic aerosol (OA) can absorb solar radiation in the low-visible and ultra-violet wavelengths thereby modifying radiative forcing. Agricultural waste burning emits a large quantity of organic carbon in many developing countries. In this work, we improved the extraction and analysis method developed by Chen and Bond, and extended the spectral range of OC absorption. We examined light absorbing properties of primary OA from pyrolysis of corn stalk, which is a major type of agricultural wastes. Light absorption of bulk liquid extracts of OA was measured using a UV-vis recording spectrophotometer. OA can be extracted by methanol at 95%, close to full extent, and shows polar character. Light absorption of organic aerosol has strong spectral dependence (Absorption Ångström exponent = 7.7) and is not negligible at ultra-violet and low-visible regions. Higher pyrolysis temperature produced OA with higher absorption. Imaginary refractive index of organic aerosol (kOA) is 0.041 at 400 nm wavelength and 0.005 at 550 nm wavelength, respectively.

The OMI Aerosol Absorption Product: An A-train application

NASA Astrophysics Data System (ADS)

Torres, O.; Jethva, H. T.; Ahn, C.

2017-12-01

Because of the uniquely large sensitivity of satellite-measured near-UV radiances to absorption by desert dust, carbonaceous and volcanic ash aerosols, observations by a variety of UV-capable sensors have been routinely used over the last forty years in both qualitative and quantitative applications for estimating the absorption properties of these aerosol types. In this presentation we will discuss a multi-sensor application involving observations from A-train sensors OMI, AIRS and CALIOP for the creation of a 13-year record of aerosol optical depth (AOD) and single scattering albedo (SSA). Determination of aerosol type, in terms of particle size distribution and refractive index, is an important algorithmic step that requires using external information. AIRS CO measurements are used as carbonaceous aerosols tracer to differentiate this aerosol type from desert dust. On the other hand, the height of the absorbing aerosol layer, an important parameter in UV aerosol retrievals, is prescribed using a CALIOP-based climatology. The combined use of these observations in the developments of the OMI long-term AOD/SSA record will be discussed along with an evaluation of retrieval results using independent observations.

Toward a Combined SAGE II-HALOE Aerosol Climatology: An Evaluation of HALOE Version 19 Stratospheric Aerosol Extinction Coefficient Observations

NASA Technical Reports Server (NTRS)

Thomason, L. W.

2012-01-01

Herein, the Halogen Occultation Experiment (HALOE) aerosol extinction coefficient data is evaluated in the low aerosol loading period after 1996 as the first necessary step in a process that will eventually allow the production of a combined HALOE/SAGE II (Stratospheric Aerosol and Gas Experiment) aerosol climatology of derived aerosol products including surface area density. Based on these analyses, it is demonstrated that HALOE's 3.46 microns is of good quality above 19 km and suitable for scientific applications above that altitude. However, it is increasingly suspect at lower altitudes and should not be used below 17 km under any circumstances after 1996. The 3.40 microns is biased by about 10% throughout the lower stratosphere due to the failure to clear NO2 but otherwise appears to be a high quality product down to 15 km. The 2.45 and 5.26 micron aerosol extinction coefficient measurements are clearly biased and should not be used for scientific applications after the most intense parts of the Pinatubo period. Many of the issues in the aerosol data appear to be related to either the failure to clear some interfering gas species or doing so poorly. For instance, it is clear that the 3.40micronaerosol extinction coefficient measurements can be improved through the inclusion of an NO2 correction and could, in fact, end up as the highest quality overall HALOE aerosol extinction coefficient measurement. It also appears that the 2.45 and 5.26 micron channels may be improved by updating the Upper Atmosphere Pilot Database which is used as a resource for the removal of gas species otherwise not available from direct HALOE measurements. Finally, a simple model to demonstrate the promise of mixed visible/infrared aerosol extinction coefficient ensembles for the retrieval of bulk aerosol properties demonstrates that a combined HALOE/SAGE II aerosol climatology is feasible and may represent a substantial improvement over independently derived data sets.

Comparison between the optical properties of aerosols in the fine and coarse fractions over Valladolid, Spain.

PubMed

Mogo, S; López, J F; Cachorro, V E; de Frutos, A; Zocca, R; Barroso, A; Mateos, D; Conceição, E

2017-02-22

Continuous measurements of the optical properties of aerosol particles have been made at Valladolid, Spain, covering the period from June 2011 to July 2012. The measurements were made at two size cuts: sub-10 μm and sub-1 μm (PM10 and PM1). The data measured were the scattering and backscattering coefficients, σ s and σ bs , obtained from an integrating nephelometer, and the absorption coefficient, σ a , obtained from a particle soot absorption photometer. Spectrally resolved data were obtained from both instruments at 3 wavelengths (blue/green/red) at low relative humidity (RH < 40%). The statistical data for the instruments were calculated based on the hourly averages. For the PM10 fraction, the hourly mean values of σ s and σ a at 550 nm were 33 Mm -1 (StD = 30 Mm -1 ) and 4 Mm -1 (StD = 3 Mm -1 ), respectively. For the PM1 fraction, σ s and σ a mean values were 16 Mm -1 (StD = 14 Mm -1 ) and 4 Mm -1 (StD = 3 Mm -1 ), also at 550 nm. The derived parameters analyzed were the single scattering albedo, ω 0 , the backscatter fraction, σ bs /σ s , and the Ångström exponents of scattering, absorption and single scattering albedo, α s , α a and α ω 0 . The contribution of the PM10 and the PM1 fractions for all these parameters plays a central role throughout the paper, allowing an improved classification of aerosol types. Our data are dominated by elemental carbon (EC) and elemental carbon/organic carbon mixed (EC/OC). For the PM10 data, dust dominated aerosol is also observed. Although we found that fine particles contribute more than coarse particles for decreasing the ω 0 values, results suggest that it is also necessary to quantify the effect of coarse particles. Fine particles were found to produce ω 0 spectra that decrease with the wavelength, α ω 0 > 0, while PM10 fractions were found to produce spectra that can decrease or increase with the wavelength, 0 < α ω 0 < 0. Both daily cycle and monthly variations are analyzed and related to local features as well as the transport of particles from elsewhere. A diurnal pattern characteristic of urban areas is observed, but it is less evident on weekends. The main long range transport influences are Atlantic advection, anthropogenic events from Central Europe and dust events.

Spectral Absorption of Solar Radiation by Aerosols during ACE-Asia

NASA Technical Reports Server (NTRS)

Bergstrom, R. W.; Pilewskie, P.; Pommier, J.; Rabbette, M.; Russell, P. B.; Schmid, B.; Redermann, J.; Higurashi, A.; Nakajima, T.; Quinn, P. K.

2004-01-01

As part of the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia), the upward and downward spectral solar radiant fluxes were measured with the Spectral Solar Flux Radiometer (SSFR), and the aerosol optical depth was measured with the Ames Airborne Tracking Sunphotometer (AATS-14) aboard the Center for INterdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter aircraft. IN this paper, we examine the data obtained for two cases: a moderately thick aerosol layer, 12 April, and a relatively thin aerosol case, 16 April 2001. ON both days, the Twin Otter flew vertical profiles in the Korean Strait southeast of Gosan Island. For both days we determine the aerosol spectral absorption of the layer and estimate the spectral aerosol absorption optical depth and single-scattering albedo. The results for 12 April show that the single-scattering albedo increases with wavelength from 0.8 at 400 nm to 0.95 at 900 nm and remains essentially constant from 950 to 1700 nm. On 16 April the amount of aerosol absorption was very low; however, the aerosol single-scattering albedo appears to decrease slightly with wavelength in the visible region. We interpret these results in light of the two absorbing aerosol species observed during the ACE-asia study: mineral dust and black carbon. The results for 12 April are indicative of a mineral dust-black carbon mixture. The 16 April results are possibly caused by black carbon mixed with nonabsorbing pollution aerosols. For the 12 April case we attempt to estimate the relative contributions of the black carbon particles and the mineral dust particles. We compare our results with other estimates of the aerosol properties from a Sea-Viewing Wide Field-of-View Sensor (SeaWiFS) satellite analysis and aerosol measurements made aboard the Twin Otter, aboard the National Oceanic and Atmospheric Administration Ronald H Brown ship, and at ground sites in Gosan and Japan. The results indicate a relatively complicated aerosol mixture of both industrial pollution (including black carbon) and mineral dust. This underscores the need for careful measurements and analysis to separate out the absorption effects of mineral dust and black carbon in the east Asia region.

Improved aethalometer

DOEpatents

Hansen, A.D.

1988-01-25

An improved aethalometer having a single light source and a single light detector and two light paths from the light source to the light detector. A quartz fiber filter is inserted in the device, the filter having a collection area in one light path and a reference area in the other light path. A gas flow path through the aethalometer housing allows ambient air to flow through the collection area of the filter so that aerosol particles can be collected on the filter. A rotating disk with an opening therethrough allows light for the light source to pass alternately through the two light paths. The voltage output of the detector is applied to a VCO and the VCO pulses for light transmission separately through the two light paths, are counted and compared to determine the absorption coefficient of the collected aerosol particles. 5 figs.

Properties of transported African mineral dust aerosols in the Mediterranean region

NASA Astrophysics Data System (ADS)

Denjean, Cyrielle; Chevaillier, Servanne; Gaimoz, Cécile; Grand, Noel; Triquet, Sylvain; Zapf, Pascal; Loisil, Rodrigue; Bourrianne, Thierry; Freney, Evelyn; Dupuy, Regis; Sellegri, Karine; Schwarzenbock, Alfons; Torres, Benjamin; Mallet, Marc; Cassola, Federico; Prati, Paolo; Formenti, Paola

2015-04-01

The transport of mineral dust aerosols is a global phenomenon with strong climate implications. Depending on the travel distance over source regions, the atmospheric conditions and the residence time in the atmosphere, various transformation processes (size-selective sedimentation, mixing, condensation of gaseous species, and weathering) can modify the physical and chemical properties of mineral dust, which, in turn, can change the dust's optical properties. The model predictions of the radiative effect by mineral dust still suffer of the lack of certainty of these properties, and their temporal evolution with transport time. Within the frame of the ChArMex project (Chemistry-Aerosol Mediterranean experiment, http://charmex.lsce.ipsl.fr/), one intensive airborne campaign (ADRIMED, Aerosol Direct Radiative Impact in the regional climate in the MEDiterranean region, 06 June - 08 July 2013) has been performed over the Central and Western Mediterranean, one of the two major transport pathways of African mineral dust. In this study we have set up a systematic strategy to determine the optical, physical and optical properties of mineral dust to be compared to an equivalent dataset for dust close to source regions in Africa. This study is based on airborne observations onboard the SAFIRE ATR-42 aircraft, equipped with state of the art in situ instrumentation to measure the particle scattering and backscattering coefficients (nephelometer at 450, 550, and 700 nm), the absorption coefficient (PSAP at 467, 530, and 660 nm), the extinction coefficient (CAPS at 530 nm), the aerosol optical depth (PLASMA at 340 to 1640 nm), the size distribution in the extended range 40 nm - 30 µm by the combination of different particle counters (SMPS, USHAS, FSSP, GRIMM) and the chemical composition obtained by filter sampling. The chemistry and transport model CHIMERE-Dust have been used to classify the air masses according to the dust origin and transport. Case studies of dust transport from known but differing origins (source regions in Tunisia, Algeria, and Mauritania) and at different times after transport, will be presented. Results will be compared to equivalent measurements over source regions interpreted in terms of the evolution of the particle size distribution, chemical composition and optical properties.

Optical and microphysical properties of natural mineral dust and anthropogenic soil dust near dust source regions over northwestern China

NASA Astrophysics Data System (ADS)

Wang, Xin; Wen, Hui; Shi, Jinsen; Bi, Jianrong; Huang, Zhongwei; Zhang, Beidou; Zhou, Tian; Fu, Kaiqi; Chen, Quanliang; Xin, Jinyuan

2018-02-01

Mineral dust aerosols (MDs) not only influence the climate by scattering and absorbing solar radiation but also modify cloud properties and change the ecosystem. From 3 April to 16 May 2014, a ground-based mobile laboratory was deployed to measure the optical and microphysical properties of MDs near dust source regions in Wuwei, Zhangye, and Dunhuang (in chronological order) along the Hexi Corridor over northwestern China. Throughout this dust campaign, the hourly averaged (±standard deviation) aerosol scattering coefficients (σsp, 550 nm) of the particulates with aerodynamic diameters less than 2.5 µm (PM2.5) at these three sites were sequentially 101.5 ± 36.8, 182.2 ± 433.1, and 54.0 ± 32.0 Mm-1. Correspondingly, the absorption coefficients (σap, 637 nm) were 9.7 ± 6.1, 6.0 ± 4.6, and 2.3 ± 0.9 Mm-1; single-scattering albedos (ω, 637 nm) were 0.902 ± 0.025, 0.931 ± 0.037, and 0.949 ± 0.020; and scattering Ångström exponents (Åsp, 450-700 nm) of PM2.5 were 1.28 ± 0.27, 0.77 ± 0.51, and 0.52 ± 0.31. During a severe dust storm in Zhangye (i.e., from 23 to 25 April), the highest values of σsp2.5 ( ˜ 5074 Mm-1), backscattering coefficient (σbsp2.5, ˜ 522 Mm-1), and ω637 ( ˜ 0.993) and the lowest values of backscattering fraction (b2.5, ˜ 0.101) at 550 nm and Åsp2.5 ( ˜ -0.046) at 450-700 nm, with peak values of aerosol number size distribution (appearing at the particle diameter range of 1-3 µm), exhibited that the atmospheric aerosols were dominated by coarse-mode dust aerosols. It is hypothesized that the relatively higher values of mass scattering efficiency during floating dust episodes in Wuwei and Zhangye are attributed to the anthropogenic soil dust produced by agricultural cultivations.

Aerosol Optical Properties at the Ground Sites during the 2010 CARES Field Campaign

NASA Astrophysics Data System (ADS)

Atkinson, D. B.; Radney, J. G.; Harworth, J. W.

2010-12-01

Preliminary results from the ground sites at the 2010 CARES field campaign (T0 near Sacramento, CA and T1 near Cool, CA) will be presented. A number of aerosol optical properties were measured at high time resolution for the four week study period using custom instruments. The aerosol extinction coefficient was measured at T0 using a cavity ring-down transmissometer (CRDT) at two wavelengths (532 and 1064 nm) and the aerosol scattering coefficient was measured at 532 nm using a Radiance Research M903 nephelometer. At T1, a new CRDT instrument was deployed that measured the extinction coefficient at three wavelengths (355, 532, and 1064 nm) for sub-10 μm (nominal) and sub-2.5 μm aerosols at ambient, elevated, and reduced relative humidity. A new type of custom nephelometer that measures the aerosol scattering coefficient at 532 nm using an array detector was also deployed at T1.

Application of AERONET Single Scattering Albedo and Absorption Angstrom Exponent to Classify Dominant Aerosol Types during DRAGON Campaigns

NASA Astrophysics Data System (ADS)

Giles, D. M.; Holben, B. N.; Eck, T. F.; Schafer, J.; Crawford, J. H.; Kim, J.; Sano, I.; Liew, S.; Salinas Cortijo, S. V.; Chew, B. N.; Lim, H.; Smirnov, A.; Sorokin, M.; Kenny, P.; Slutsker, I.

2013-12-01

Aerosols can have major implications on human health by inducing respiratory diseases due to inhalation of fine particles from biomass burning smoke or industrial pollution and on radiative forcing whereby the presence of absorbing aerosol particles (e.g., black carbon) increases atmospheric heating. Aerosol classification techniques have utilized aerosol loading and aerosol properties derived from multi-spectral and multi-angle observations by ground-based (e.g., AERONET) and satellite instrumentation (e.g., MISR). Aerosol Robotic Network (AERONET) data have been utilized to determine aerosol types by implementing various combinations of measured aerosol optical depth or retrieved size and absorption aerosol properties (e.g., Gobbi et al., 2007; Russell et al., 2010). Giles et al. [2012] showed single scattering albedo (SSA) relationship with extinction Angstrom exponent (EAE) can provide an estimate of the general classification of dominant aerosol types (i.e., desert dust, urban/industrial pollution, biomass burning smoke, and mixtures) based on data from ~20 AERONET sites located in known aerosol source regions. In addition, the absorption Angstrom exponent relationship with EAE can provide an indication of the dominant absorbing aerosol type such as dust, black carbon, brown carbon, or mixtures of them. These classification techniques are applied to the AERONET Level 2.0 quality assured data sets collected during Distributed Regional Aerosol Gridded Observational Network (DRAGON) campaigns in Maryland (USA), Japan, South Korea, Singapore, Penang (Malaysia), and California (USA). An analysis of aerosol type classification for DRAGON sites is performed as well as an assessment of the spatial variability of the aerosol types for selected DRAGON campaigns. Giles, D. M., B. N. Holben, T. F. Eck, A. Sinyuk, A. Smirnov, I. Slutsker, R. R. Dickerson, A. M. Thompson, and J. S. Schafer (2012), An analysis of AERONET aerosol absorption properties and classifications representative of aerosol source regions, J. Geophys. Res., 117, D17203, doi:10.1029/2012JD018127. Gobbi, G. P., Y. J. Kaufman, I. Koren, and T. F. Eck (2007), Classification of aerosol properties derived from AERONET direct sun data, Atmos. Chem. Phys., 7, 453-458, doi:10.5194/acp-7-453-2007. Russell, P. B., R. W. Bergstrom, Y. Shinozuka, A. D. Clarke, P. F. DeCarlo, J. L. Jimenez, J. M. Livingston, J. Redemann, O. Dubovik, and A. Strawa (2010), Absorption Ångstrom Exponent in AERONET and related data as an indicator of aerosol composition, Atmos. Chem. Phys., 10, 1155-1169, doi:10.5194/acp-10-1155-2010.

Light Absorption and Excitation-Emission Fluorescence of Urban Organic Aerosol Components and Their Relationship to Chemical Structure.

PubMed

Chen, Qingcai; Ikemori, Fumikazu; Mochida, Michihiro

2016-10-18

The present study used a combination of solvent and solid-phase extractions to fractionate organic compounds with different polarities from total suspended particulates in Nagoya, Japan, and their optical characteristics were obtained on the basis of their UV-visible absorption spectra and excitation-emission matrices (EEMs). The relationship between their optical characteristics and chemical structures was investigated based on high-resolution aerosol mass spectra (HR-AMS spectra), soft ionization mass spectra and Fourier transform infrared (FT-IR) spectra. The major light-absorption organics were less polar organic fractions, which tended to have higher mass absorption efficiencies (MAEs) and lower wavelength dependent Ångström exponents (Å) than the more polar organic fractions. Correlation analyses indicate that organic compounds with O and N atoms may contribute largely to the total light absorption and fluorescence of the organic aerosol components. The extracts from the aerosol samples were further characterized by a classification of the EEM profiles using a PARAFAC model. Different fluorescence components in the aerosol organic EEMs were associated with specific AMS ions and with different functional groups from the FT-IR analysis. These results may be useful to determine and further classify the chromophores in atmospheric organic aerosols using EEM spectroscopy.

Finely dispersed brown carbon in a smoggy atmosphere

NASA Astrophysics Data System (ADS)

Gorchakov, G. I.; Vasiliev, A. V.; Verichev, K. S.; Semoutnikova, E. G.; Karpov, A. V.

2016-11-01

It is shown that the absorption capacity of smoke aerosol during mass forest and forest-peat fires is determined to a considerable degree by light absorbing organic compounds or brown carbon. According to the data from the AERONET global network of stations [1], the absorption spectra of smoke aerosol vary significantly if airborne particulate matter is contained in brown carbon. It is established that in several cases, the absorption spectra of smoke aerosol are approximated with satisfactory accuracy by exponents. It is shown that the finely dispersed (submicron) fraction of the smoke aerosol makes a major contribution to its optical characteristics in the 0.44-1.02 μm spectral region. Strong variation in the single scattering albedo is discovered in the presence of brown carbon in the smoke aerosol. It is shown that the optical characteristics of coarsely dispersed and finely dispersed fractions of smoke aerosol differ considerably.

Aerosol Radiative Forcing in Asian Continental Outflow

NASA Technical Reports Server (NTRS)

Pueschel, R.; Kinne, S.; Redemann, J.; Gore, Warren J. (Technical Monitor)

2000-01-01

Aerosols in elevated layers were sampled with FSSP-probes and wire impactors over the Pacific ocean aboard the NASA DC-8 aircraft. Analyses of particle size and morphology identifies two distinctly different aerosol types for cases when the mid-visible extinctions exceed 0.2/km. Smaller sizes (effective radii of 0.2 um) and moderate absorption (mid-visible single scattering albedo of.935) are typical for urban-industrial pollution. Larger sizes (effective radii of 0.7 um) and weak absorption (mid-visible single scattering albedo of 0.985) identify dust. This aerosol classification is in agreement with its origin as determined by airmass back trajectory analysis. Based on lidar vertical profiling, aerosol dominated by dust and urban-industrial pollution above 3km were assigned mid-visible optical depths of 0.50 and 0.27, respectively. Radiative transfer simulations, considering a 50% cloud-cover below the aerosol layers, suggest (on a daily tP C)C> basis) small reductions (-4W/m2) to the energy budget at the top of the atmosphere for both aerosol types. For c' 0 dust, more backscattering of sunlight (weaker solar absorption) is compensated by a stronger greenhouse effect due to larger sizes. Forced reductions to the energy budget at the surface are 12W/m2 for both aerosol types. In contrast, impacts on heating rates within the aerosol layers are quite different: While urban-industrial aerosol warms the layer (at +0.6K/day as solar heating dominates), dust cools (at -0.5K/day as infrared cooling dominates). Sensitivity tests show the dependence of the aerosol climatic impact on the optical depth, particle size, absorptivity, and altitude of the layers, as well as clouds and surface properties. Climatic cooling can be eliminated (1) for the urban-industrial aerosol if absorption is increased to yield a mid-visible single scattering albedo of 0.89, or if the ocean is replaced by a land surface; (2) for the dust aerosol if the effective radius is increased from 0.7 to 1.2 um. The removal of low-level clouds doubles the cooling at the top of the atmosphere to about -8W/m2.

Atmospheric Temperature Profile Measurements Using Mobile High Spectral Resolution Lidar

NASA Astrophysics Data System (ADS)

Razenkov, Ilya I.; Eloranta, Edwin W.

2016-06-01

The High Spectral Resolution Lidar (HSRL) designed at the University of Wisconsin-Madison discriminates between Mie and Rayleigh backscattering [1]. It exploits the Doppler effect caused by thermal motion of molecules, which broadens the spectrum of the transmitted laser light. That allows for absolute calibration of the lidar and measurements of the aerosol volume backscatter coefficient. Two iodine absorption filters with different absorption line widths (a regular iodine vapor filter and Argon buffered iodine filter) allow for atmospheric temperature profile measurements. The sensitivity of the measured signal-to-air temperature ratio is around 0.14%/K. The instrument uses a shared telescope transmitter-receiver design and operates in eyesafe mode (the product of laser average power and telescope aperture equals 0.1 Wm2 at 532 nm).

LASER APPLICATIONS AND OTHER TOPICS IN QUANTUM ELECTRONICS: On the aerosol backscattering coefficient in atmosphere in the spectral range 9-13.5μm

NASA Astrophysics Data System (ADS)

Vasil'ev, B. I.; Mannoun, Oussama

2007-05-01

The aerosol backscattering coefficient βπ in a surface atmospheric layer is calculated at the emission lines of NH3 and CO2 lasers (9-13.5 μm). It is shown that the coefficients βπ at the emission lines of an NH3 laser (11-13.5 μm) are comparable with the coefficients βπ at the emission lines of a CO2 laser near 10.6 μm. The dependence of βπ on the humidity and type of aerosols is studied. It is also shown that the coefficient βπ in a surface atmospheric layer at the lasing of an NH3 laser varies from 10-10 to 7×10-9 cm-1 sr-1. The lidar aerosol ratio is calculated as a function of the mean aerosol radius. It is found that this ratio is independent of the particle size for aerosol particles of radius exceeding 40 μm for the 11.7-μm aP(4,0) line of the ammonia laser.

Effect of Aerosols on Surface Radiation and Air Quality in the Central American Region Estimated Using Satellite UV Instruments

NASA Astrophysics Data System (ADS)

Bhartia, P. K.; Torres, O.; Krotkov, N. A.

2007-05-01

Solar radiation reaching the Earth's surface is reduced by both aerosol scattering and aerosol absorption. Over many parts of the world the latter effect can be as large or larger than the former effect, and small changes in the aerosol single scattering albedo can either cancel the former effect or enhance it. In addition, absorbing aerosols embedded in clouds can greatly reduce the amount of radiation reaching the surface by multiple scattering. Though the potential climatic effects of absorbing aerosols have received considerable attention lately, their effect on surface UV, photosynthesis, and photochemistry can be equally important for our environment and may affect human health and agricultural productivity. Absorption of all aerosols commonly found in the Earth's atmosphere becomes larger in the UV and blue wavelengths and has a relatively strong wavelength dependence. This is particularly true of mineral dust and organic aerosols. However, these effects have been very difficult to estimate on a global basis since the satellite instruments that operate in the visible are primarily sensitive to aerosol scattering. A notable exception is the UV Aerosol Index (AI), first produced using NASA's Nimbus-7 TOMS data. AI provides a direct measure of the effect of aerosol absorption on the backscattered UV radiation in both clear and cloudy conditions, as well as over snow/ice. Although many types of aerosols produce a distinct color cast in the visible images, and aerosols absorption over clouds and snow/ice could, in principle be detected from their color, so far this technique has worked well only in the UV. In this talk we will discuss what we have learned from the long-term record of AI produced from TOMS and Aura/OMI about the possible role of aerosols on surface radiation and air quality in the Central American region.

Effects of Aerosol on Atmospheric Dynamics and Hydrologic Processes During Boreal Spring and Summer

NASA Technical Reports Server (NTRS)

Lau, William K. M.; Kim, M. K.; Kim, K. M.; Chin, Mian

2005-01-01

Global and regional climate impacts of present-day aerosol loading during boreal spring are investigated using the NASA finite volume General Circulation Model (fvGCM). Three-dimensional distributions of loadings of five species of tropospheric aerosols, i.e., sulfate, black carbon, organic carbon, soil dust, and sea salt are prescribed from outputs of the Goddard Ozone Chemistry Aerosol Radiation and Transport model (GOCART). The aerosol loadings are used to calculate the extinction coefficient, single scattering albedo, and asymmetric factor at eleven spectral wavelengths in the radiative transfer code. We find that aerosol-radiative forcing during boreal spring excites a wavetrain-like pattern in tropospheric temperature and geopotential height that emanates from Northern Africa, through Eurasia, to northeastern Pacific. Associated with the teleconnection is strong surface cooling over regions with large aerosol loading, i.e., China, India, and Africa. Low-to-mid tropospheric heating due to shortwave absorption is found in regions with large loading of dust (Northern Africa, and central East Asia), and black carbon (South and East Asia). In addition pronounced surface cooling is found over the Caspian Sea and warming over Eurasian and northeastern Asia, where aerosol loadings are relatively low. These warming and cooling are components of teleconnection pattern produced primarily by atmospheric heating from absorbing aerosols, i.e., dust from North Africa and black carbon from South and East Asia. Effects of aerosols on atmospheric hydrologic cycle in the Asian monsoon region are also investigated. Results show that absorbing aerosols, i.e., black carbon and dust, induce large-scale upper-level heating anomaly over the Tibetan Plateau in April and May, ushering in an early onset of the Indian summer monsoon. Absorbing aerosols also enhance lower-level heating and anomalous ascent over northern India, intensifying the Indian monsoon. Overall, the aerosol-induced large-scale surface tempera- cooling leads to a reduction of monsoon rainfall over the East Asia continent, and adjacent oceanic regions.

Effects of Aerosol on Atmospheric Dynamics and Hydrologic Processes during Boreal Spring and Summer

NASA Technical Reports Server (NTRS)

Lau, William K. M.; Kim, M. K.; Chin, Mian; Kim, K. M.

2005-01-01

Global and regional climate impacts of present-day aerosol loading during boreal spring are investigated using the NASA finite volume General Circulation Model (fvGCM). Three-dimensional distributions of loadings of five species of tropospheric aerosols, i.e., sulfate, black carbon, organic carbon, soil dust, and sea salt are prescribed from outputs of the Goddard Ozone Chemistry Aerosol Radiation and Transport model (GOCART). The aerosol loadings are used to calculate the extinction coefficient, single scattering albedo, and asymmetric factor at eleven spectral wavelengths in the radiative transfer code. We find that aerosol-radiative forcing during boreal spring excites a wavetrain-like pattern in tropospheric temperature and geopotential height that emanates from Northern Africa, through Eurasia, to northeastern Pacific. Associated with the teleconnection is strong surface cooling over regions with large aerosol loading, i.e., China, India, and Africa. Low-to-mid tropospheric heating due to shortwave absorption is found in regions with large loading of dust (Northern Africa, and central East Asia), and black carbon (South and East Asia). In addition pronounced surface cooling is found over the Caspian Sea and warming over Eurasian and northeastern Asia, where aerosol loadings are relatively low. These warming and cooling are components of teleconnection pattern produced primarily by atmospheric heating from absorbing aerosols, i.e., dust from North Africa and.black carbon from South and East Asia. Effects of aerosols on atmospheric hydrologic cycle in the Asian monsoon region are also investigated. Results show that absorbing aerosols, i.e., black carbon and dust, induce large-scale upper-level heating anomaly over the Tibetan Plateau in April and May, ushering in an early onset of the Indian summer monsoon. Absorbing aerosols also enhance lower-level heating and anomalous ascent over northern India, intensifying the Indian monsoon. Overall, the aerosol-induced large-scale surface temperature cooling leads to a reduction of monsoon rainfall over the East Asia continent, and adjacent oceanic regions.

Aerosol optical properties along the northeast coast of North America during the New England Air Quality Study-Intercontinental Transport and Chemical Transformation 2004 campaign and the influence of aerosol composition

NASA Astrophysics Data System (ADS)

Wang, Wei; Rood, Mark J.; Carrico, Christian M.; Covert, David S.; Quinn, Patricia K.; Bates, Timothy S.

2007-05-01

Optical and hygroscopic properties of submicrometer diameter aerosol particles were measured on board the NOAA R/V Ronald H. Brown as part of the NEAQS-ITCT field campaign. The campaign occurred along the northeast coast of North America during the summer of 2004. A scanning relative humidity (RH) nephelometry system (humidograph) measured total light scattering and backscattering coefficients (σsp and σbsp, respectively) at three wavelengths (λs) and RH = 26% and while RH was scanned between 40% and 85%. These measurements were combined with aerosol light absorption and composition measurements to describe σsp, σbsp, single scattering albedo (ω), Ångström exponent (å), and hemispheric backscatter fraction (b) at a low reference RH of 26 ± 4% and the aerosol's hygroscopic properties based on its optical response up to 85% RH. Humidogram curve structure was dominated by hygroscopic growth without hysteresis (76% frequency). Dependence of the aerosol's σsp values with changes in RH, fσsp(RH, 26), was observed to decrease with increasing mass fraction of particulate organic matter (POM, FO). Statistical analyses indicated that increasing FO resulted in a less hygroscopic aerosol, while increasing molar equivalence ratio (ER) resulted in lower hysteresis factors based on the aerosols' optical responses at a 0.95 confidence level. ω showed little RH dependence while å and b decreased with increasing RH values. Values for å(λ1, λ2), b, and fσsp(82, 26) increased with increasing λ values. Sensitivities of top of the atmosphere aerosol radiative forcing to changes in ω, b, and σsp with RH were also estimated.

Spectrally-resolved measurements of aerosol extinction at ultraviolet and visible wavelengths

NASA Astrophysics Data System (ADS)

Flores, M.; Washenfelder, R. A.; Brock, C. A.; Brown, S. S.; Rudich, Y.

2012-12-01

Aerosols play an important role in the Earth's radiative budget. Aerosol extinction includes both the scattering and absorption of light, and these vary with wavelength, aerosol diameter, and aerosol composition. Historically, aerosol absorption has been measured using filter-based or extraction methods that are prone to artifacts. There have been few investigations of ambient aerosol optical properties at the blue end of the visible spectrum and into the ultraviolet. Brown carbon is particularly important in this spectral region, because it both absorbs and scatters light, and encompasses a large and variable group of organic compounds from biomass burning and secondary organic aerosol. We have developed a laboratory instrument that combines new, high-power LED light sources with high-finesse optical cavities to achieve sensitive measurements of aerosol optical extinction. This instrument contains two broadband channels, with spectral coverage from 360 - 390 nm and 385 - 420 nm. Using this instrument, we report aerosol extinction in the ultraviolet and near-visible spectral region as a function of chemical composition and structure. We have measured the extinction cross-sections between 360 - 420 nm with 0.5 nm resolution using different sizes and concentrations of polystyrene latex spheres, ammonium sulfate, and Suwannee River fulvic acid. Fitting the real and imaginary part of the refractive index allows the absorption and scattering to be determined.

Chemical and Optical Properties of Water-Soluble Organic Aerosols from Biomass Burning Emissions

NASA Astrophysics Data System (ADS)

Yu, J. M.; Park, S.; Cho, S. Y.

2016-12-01

Light absorption property by organic aerosols is an important parameter to determine their radiative forcing on global and regional scales. However, the optical measurements by light absorbing aerosols from biomass burning emissions are rather lacking. This study explored the chemical and light-absorption properties of humic-like substances (HULIS) from biomass burning aerosols of three types; rice straw (RS), pine needles (PN), and sesame stem (SS). Water-soluble organic carbon (WSOC) contributed 42.5, 42.0, and 57.0% to the OC concentrations of the RS, PN, and SS emissions, respectively. Respective HULIS (=1.94´HULIS-C) concentrations accounted for 29.5±2.0, 15.3±3.1, and 25.8±4.0% of PM2.5, and contributed 63±5, 36±10, and 51±8% to WSOC concentration. Absorption Ångström exponents (AAEs) of the WSOC fitted between 300 and 400 nm wavelengths were 7.4-8.3, indicating no significant differences among the biomass types. These AAEs are similar to those reported for aqueous extracts of biomass burning HULIS and fresh secondary organic aerosols from ozonolysis of terpenes. HULIS, which is a hydrophobic part of WSOC and a significant fraction of brown carbon, showed absorption spectra similar to brown carbon. WSOC mass absorption efficiency (MAE365) at 365 nm were 1.37, 0.86, and 1.38 m2/g×C for RS, PN, and SS burning aerosols, respectively. The MAE values by WSOC were less than 10% of MAE caused by light-absorbing black carbon. The light absorption of the water extracts at 365 nm indicated that light absorption was more strongly associated with HULIS from biomass burning emissions than with the hydrophilic WSOC fraction.

Utilization of O4 slant column density to derive aerosol layer height from a spaceborne UV-visible hyperspectral sensor: sensitivity and case study

NASA Astrophysics Data System (ADS)

Park, S. S.; Kim, J.; Lee, H.; Torres, O.; Lee, K.-M.; Lee, S. D.

2015-03-01

The sensitivities of oxygen-dimer (O4) slant column densities (SCDs) to changes in aerosol layer height are investigated using simulated radiances by a radiative transfer model, Linearized Discrete Ordinate Radiative Transfer (LIDORT), and Differential Optical Absorption Spectroscopy (DOAS) technique. The sensitivities of the O4 SCDs to aerosol types and optical properties are also evaluated and compared. Among the O4 absorption bands at 340, 360, 380, and 477 nm, the O4 absorption band at 477 nm is found to be the most suitable to retrieve the aerosol effective height. However, the O4 SCD at 477 nm is significantly influenced not only by the aerosol layer effective height but also by aerosol vertical profiles, optical properties including single scattering albedo (SSA), aerosol optical depth (AOD), and surface albedo. Overall, the error of the retrieved aerosol effective height is estimated to be 414 m (16.5%), 564 m (22.4%), and 1343 m (52.5%) for absorbing, dust, and non-absorbing aerosol, respectively, assuming knowledge on the aerosol vertical distribution type. Using radiance data from the Ozone Monitoring Instrument (OMI), a new algorithm is developed to derive the aerosol effective height over East Asia after the determination of the aerosol type and AOD from the MODerate resolution Imaging Spectroradiometer (MODIS). The retrieved aerosol effective heights are lower by approximately 300 m (27 %) compared to those obtained from the ground-based LIDAR measurements.

Correlations Between Optical, Chemical and Physical Properties of Biomass Burn Aerosols

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hopkins, Rebecca J.; Lewis, Keith M.; Dessiaterik, Yury

2007-09-20

Single scattering albedo (ω) and Angstrom absorption coefficient (αap) values are measured at 405, 532 and 870 nm for aerosols generated during controlled laboratory combustion of twelve wildland fuels. Considerable fuel dependent variation in these optical properties is observed at these wavelengths. Complementary microspectroscopy techniques are used to elucidate spatially resolved local chemical bonding, carbon-to-oxygen atomic ratios, percent of sp2 hybridization (graphitic nature), elemental composition, particle size and morphology. These parameters are compared directly with the corresponding optical properties for each combustion product, facilitating an understanding of the fuel dependent variability observed. Results indicate that combustion products can be dividedmore » into three categories based on chemical, physical and optical properties. Only materials displaying a high degree of sp2 hybridization, with chemical and physical properties characteristic of ‘soot’ or black carbon, exhibit ω and αap values that indicate a high light absorbing capacity.« less

Fine particulate matter characteristics and its impact on visibility impairment at two urban sites in Korea: Seoul and Incheon

NASA Astrophysics Data System (ADS)

Kim, Young J.; Kim, Kyung W.; Kim, Shin D.; Lee, Bo K.; Han, Jin S.

In order to investigate the causes of visibility degradation in the metropolitan area of Seoul, extensive chemical and optical monitoring of aerosol was conducted at two urban sites; Junnong, Seoul and Yonghyun, Incheon during several seasonal intensive monitoring periods between August 2002 and August 2004. Light extinction, scattering, and absorption coefficients were measured simultaneously with a transmissometer, a nephelometer, and an aethalometer, respectively. Continuous aerosol chemical measurement was also made with Sunset elemental carbon/organic carbon (EC/OC) analyzers and on-line ion monitors. The mean light extinction budget for five major aerosol components; ammonium sulfate, ammonium nitrate, fine carbonaceous particles (EC and OC), fine soil, and coarse particle was estimated based on the measurement results. Investigation of the haze level revealed that PM 2.5 mass concentrations at Junnong and Yonghyun measured under the Worst20% condition were approximately twice those of the Best20% condition. The worst visibility condition was well correlated with increases in mass concentrations of sulfate and nitrate, and EC particles. The mass concentration of aerosol components for the Worst20% was measured to be approximately two- to four-fold higher than those for the Best20%. Degree of visibility degradation was also analyzed based on the air mass pathway information obtained using the HYSPLIT model. Average light extinction coefficients under continental air flow condition at the Junnong and Yonghyun sites were the highest values of 704±414 and 773±546 Mm -1, respectively due to increased loading of fine particles. Visibility was greatly improved at both sites when atmosphere was impacted by air mass originated from Pacific Ocean.

A Long-term Record of Saharan Dust Aerosol Properties from TOMS Observations: Optical Depth and Single Scattering Albedo

NASA Technical Reports Server (NTRS)

Torres, Omar; Bhartia, P. K.; Herman, J. R.; Einaudi, Franco (Technical Monitor)

2000-01-01

The interaction between the strong Rayleigh scattering in the near UV spectral region (330-380 nm) and the processes of aerosol absorption and scattering, produce a clear spectral signal in the upwelling radiance at the top of the atmosphere. This interaction is the basis of the TOMS (Total Ozone Mapping Spectrometer) aerosol retrieval technique that can be used for their characterization and to differentiate non-absorbing sulfates from strongly UV-absorbing aerosols such as mineral dust. For absorbing aerosols, the characterization is in terms of the optical depth and single scattering albedo with assumptions about the aerosol plume height. The results for non-absorbing aerosols are not dependent on plume height. Although iron compounds represent only between 5% to 8% of desert dust aerosol mass, hematite (Fe2O3) accounts for most of the near UV absorption. Because of the large ultraviolet absorption characteristic of hematite, the near UV method of aerosol sensing is especially suited for the detection and characterization of desert dust aerosols. Using the combined record of near UV measurements by the Nimbus7 (1978-1992) and Earth Probe (1996-present) TOMS instruments, a global longterm climatology of near UV optical depth and single scattering albedo has been produced. The multi-year long record of mineral aerosol properties over the area of influence of the Saharan desert, will be discussed.

Estimation and Bias Correction of Aerosol Abundance using Data-driven Machine Learning and Remote Sensing

NASA Technical Reports Server (NTRS)

Malakar, Nabin K.; Lary, D. L.; Moore, A.; Gencaga, D.; Roscoe, B.; Albayrak, Arif; Petrenko, Maksym; Wei, Jennifer

2012-01-01

Air quality information is increasingly becoming a public health concern, since some of the aerosol particles pose harmful effects to peoples health. One widely available metric of aerosol abundance is the aerosol optical depth (AOD). The AOD is the integrated light extinction coefficient over a vertical atmospheric column of unit cross section, which represents the extent to which the aerosols in that vertical profile prevent the transmission of light by absorption or scattering. The comparison between the AOD measured from the ground-based Aerosol Robotic Network (AERONET) system and the satellite MODIS instruments at 550 nm shows that there is a bias between the two data products. We performed a comprehensive analysis exploring possible factors which may be contributing to the inter-instrumental bias between MODIS and AERONET. The analysis used several measured variables, including the MODIS AOD, as input in order to train a neural network in regression mode to predict the AERONET AOD values. This not only allowed us to obtain an estimate, but also allowed us to infer the optimal sets of variables that played an important role in the prediction. In addition, we applied machine learning to infer the global abundance of ground level PM2.5 from the AOD data and other ancillary satellite and meteorology products. This research is part of our goal to provide air quality information, which can also be useful for global epidemiology studies.

Absorption Properties of Mediterranean Aerosols Obtained from Multi-year Ground-based and Satellite Remote Sensing Observations

NASA Technical Reports Server (NTRS)

Mallet, M.; Dubovik, O.; Nabat, P.; Dulac, F.; Kahn, R.; Sciare, J.; Paronis, D.; Leon, J. F.

2013-01-01

Aerosol absorption properties are of high importance to assess aerosol impact on regional climate. This study presents an analysis of aerosol absorption products obtained over the Mediterranean Basin or land stations in the region from multi-year ground-based AERONET and satellite observations with a focus on the Absorbing Aerosol Optical Depth (AAOD), Single Scattering Albedo (SSA) and their spectral dependence. The AAOD and Absorption Angstrom Exponent (AAE) data set is composed of daily averaged AERONET level 2 data from a total of 22 Mediterranean stations having long time series, mainly under the influence of urban-industrial aerosols and/or soil dust. This data set covers the 17 yr period 1996-2012 with most data being from 2003-2011 (approximately 89 percent of level-2 AAOD data). Since AERONET level-2 absorption products require a high aerosol load (AOD at 440 nm greater than 0.4), which is most often related to the presence of desert dust, we also consider level-1.5 SSA data, despite their higher uncertainty, and filter out data with an Angstrom exponent less than 1.0 in order to study absorption by carbonaceous aerosols. The SSA data set includes both AERONET level-2 and satellite level-3 products. Satellite-derived SSA data considered are monthly level 3 products mapped at the regional scale for the spring and summer seasons that exhibit the largest aerosol loads. The satellite SSA dataset includes the following products: (i) Multi-angle Imaging SpectroRadiometer (MISR) over 2000-2011, (ii) Ozone Monitoring Instrument (OMI) near-UV algorithm over 2004-2010, and (iii) MODerate resolution Imaging Spectroradiometer (MODIS) Deep-Blue algorithm over 2005-2011, derived only over land in dusty conditions. Sun-photometer observations show that values of AAOD at 440 nm vary between 0.024 +/- 0.01 (resp. 0.040 +/- 0.01) and 0.050 +/- 0.01 (0.055 +/- 0.01) for urban (dusty) sites. Analysis shows that the Mediterranean urban-industrial aerosols appear "moderately" absorbing with values of SSA close to approximately 0.94-0.95 +/- 0.04 (at 440 nm) in most cases except over the large cities of Rome and Athens, where aerosol appears more absorbing (SSA approximately 0.89-0.90 +/- 0.04). The aerosol Absorption Angstrom Exponent (AAE, estimated using 440 and 870 nm) is found to be larger than 1 for most sites over the Mediterranean, a manifestation of mineral dust (iron) and/or brown carbon producing the observed absorption. AERONET level-2 sun-photometer data indicate the existence of a moderate East-West gradient, with higher values over the eastern basin (AAEEast. = 1.39/AAEWest. = 1.33) due to the influence of desert dust. The North-South AAE gradient is more pronounced, especially over the western basin. Our additional analysis of AERONET level-1.5 data also shows that organic absorbing aerosols significantly affect some Mediterranean sites. These results indicate that current climate models treating organics as nonabsorbing over the Mediterranean certainly underestimate the warming effect due to carbonaceous aerosols. Acomparative analysis of the regional SSA variability has been attempted using satellite data. OMI and MODIS data show an absorbing zone (SSA approximately 0.90 at 470-500 nm) over Northeastern Africa that does not appear in the MISR retrievals. In contrast, MISR seems able to observe the East-West SSA gradient during summer, as also detected by AERONET. Also, the analysis of SSA provided by satellites indicates that the aerosol over the Mediterranean Sea appears less absorbing during spring (MAM) than summer (JJA).

Brown Carbon Production in Ammonium- or Amine-Containing Aerosol Particles by Reactive Uptake of Methylglyoxal and Photolytic Cloud Cycling.

PubMed

De Haan, David O; Hawkins, Lelia N; Welsh, Hannah G; Pednekar, Raunak; Casar, Jason R; Pennington, Elyse A; de Loera, Alexia; Jimenez, Natalie G; Symons, Michael A; Zauscher, Melanie; Pajunoja, Aki; Caponi, Lorenzo; Cazaunau, Mathieu; Formenti, Paola; Gratien, Aline; Pangui, Edouard; Doussin, Jean-François

2017-07-05

The effects of methylglyoxal uptake on the physical and optical properties of aerosol containing amines or ammonium sulfate were determined before and after cloud processing in a temperature- and RH-controlled chamber. The formation of brown carbon was observed upon methylglyoxal addition, detected as an increase in water-soluble organic carbon mass absorption coefficients below 370 nm and as a drop in single-scattering albedo at 450 nm. The imaginary refractive index component k 450 reached a maximum value of 0.03 ± 0.009 with aqueous glycine aerosol particles. Browning of solid particles occurred at rates limited by chamber mixing (<1 min), and in liquid particles occurred more gradually, but in all cases occurred much more rapidly than in bulk aqueous studies. Further browning in AS and methylammonium sulfate seeds was triggered by cloud events with chamber lights on, suggesting photosensitized brown carbon formation. Despite these changes in optical aerosol characteristics, increases in dried aerosol mass were rarely observed (<1 μg/m 3 in all cases), consistent with previous experiments on methylglyoxal. Under dry, particle-free conditions, methylglyoxal reacted (presumably on chamber walls) with methylamine with a rate constant k = (9 ± 2) × 10 -17 cm 3 molecule -1 s -1 at 294 K and activation energy E a = 64 ± 37 kJ/mol.

Near-infrared light absorption by brown carbon in the ambient atmosphere

NASA Astrophysics Data System (ADS)

Chung, C.; Hoffer, A.; Beres, N. D.; Moosmüller, H.; Liu, C.; Green, M.; Kim, S. W.; Engelbrecht, J. P.; Gelencser, A.

2017-12-01

Organic aerosols have been assumed to have little-to-no absorption in the red and near-infrared spectral regions of solar radiation, even though a class of organic aerosols were shown to absorb significantly in these spectral regions. Here, we show that ambient atmospheric data from commonly-used 7-wavelength aethalometers contain evidence of abundant near-infrared light absorption by organic aerosol. This evidence comes from the absorption Ångström exponent over 880 950 nm, which often exceeds values explainable by fresh or coated black carbon, or mineral dust. This evidence is not due to an artifact from the instrument random errors or biases, either. The best explanation for these large 880/950 nm absorption Ångström exponent values in the aethalometer data is near-infrared light absorption by tar balls. Tar balls are among common particles from forest fire.

Calculations of Aerosol Radiative Forcing in the SAFARI Region from MODIS Data

NASA Technical Reports Server (NTRS)

Remer, L. A.; Ichoku, C.; Kaufman, Y. J.; Chu, D. A.

2003-01-01

SAFARI 2000 provided the opportunity to validate MODIS aerosol retrievals and to correct any assumptions in the retrieval process. By comparing MODIS retrievals with ground-based sunphotometer data, we quantified the degree to which the MODIS algorithm underestimated the aerosol optical thickness. This discrepancy was attributed to underestimating the degree of light absorption by the southern African smoke aerosol. Correcting for this underestimation of absorption, produces more realistic aerosol retrievals that allow various applications of the MODIS aerosol products. One such application is the calculation of the aerosol radiative forcing at the top and bottom of the atmosphere. The combination of MODIS accuracy, coverage, resolution and the ability to separate fine and coarse mode make this calculation substantially advanced over previous attempts with other satellites. We focus on the oceans adjacent to southern Africa and use a solar radiative transfer model to perform the flux calculations. The forcing at the top of atmosphere is calculated to be 10 W/sq m, while the forcing at the surface is -26 W/sq m. These results resemble those calculated from INDOEX data, and are most sensitive to assumptions of aerosol absorption, the same parameter that initially interfered with our retrievals.

The colors of biomass burning aerosols in the atmosphere.

PubMed

Liu, Chao; Chung, Chul Eddy; Zhang, Feng; Yin, Yan

2016-06-16

Biomass burning aerosols mainly consist of black carbon (BC) and organic aerosols (OAs), and some of OAs are brown carbon (BrC). This study simulates the colors of BrC, BC and their mixture with scattering OAs in the ambient atmosphere by using a combination of light scattering simulations, a two-stream radiative transfer model and a RGB (Red, Green, Blue) color model. We find that both BCs and tar balls (a class of BrC) appear brownish at small particle sizes and blackish at large sizes. This is because the aerosol absorption Ångström exponent (AAE) largely controls the color and larger particles give smaller AAE values. At realistic size distributions, BCs look more blackish than tar balls, but still exhibit some brown color. However, when the absorptance of aerosol layer at green wavelength becomes larger than approximately 0.8, all biomass burning aerosols look blackish. The colors for mixture of purely scattering and absorptive carbonaceous aerosol layers in the atmosphere are also investigated. We suggest that the brownishness of biomass burning aerosols indicates the amount of BC/BrC as well as the ratio of BC to BrC.

Are non-linearity effects of absorption important for MAX-DOAS observations?

NASA Astrophysics Data System (ADS)

Pukite, Janis; Wang, Yang; Wagner, Thomas

2017-04-01

For scattered light observations the absorption optical depth depends non-linearly on the trace gas concentrations if their absorption is strong. This is the case because the Beer-Lambert law is generally not applicable for scattered light measurements due to many (i.e. more than one) light paths contributing to the measurement. While in many cases a linear approximation can be made, for scenarios with strong absorption non-linear effects cannot always be neglected. This is especially the case for observation geometries with spatially extended and diffuse light paths, especially in satellite limb geometry but also for nadir measurements as well. Fortunately the effects of non-linear effects can be quantified by means of expanding the radiative transfer equation in a Taylor series with respect to the trace gas absorption coefficients. Herewith if necessary (1) the higher order absorption structures can be described as separate fit parameters in the DOAS fit and (2) the algorithm constraints of retrievals of VCDs and profiles can be improved by considering higher order sensitivity parameters. In this study we investigate the contribution of the higher order absorption structures for MAX-DOAS observation geometry for different atmospheric and ground properties (cloud and aerosol effects, trace gas amount, albedo) and geometry (different Sun and viewing angles).

The effect of airborne lead particle size on worker blood-lead levels: an empirical study of battery workers.

PubMed

Hodgkins, D G; Robins, T G; Hinkamp, D L; Schork, M A; Levine, S P; Krebs, W H

1991-12-01

Theoretical models and experimental data suggest that the particle size distribution of lead aerosols should affect the lead dose absorbed by exposed workers. In the present study, 44 workers in five major operations in a high-volume, lead-acid battery plant were studied for the influence of lead aerosol size on lead-in-blood (PbB) levels. A multiple linear regression analysis based on particle size assumptions made in the model used by the Occupational Safety and Health Administration to help select the permissible exposure level (PEL) for lead showed no improvement in prediction of PbB over that already present without any consideration of particle size. The use of the American Conference of Governmental Industrial Hygienists (ACGIH) regional size-selective criteria also failed to improve the prediction of PbB. However, when deposition models developed by Heyder et al were used in which the lead aerosol was separated into alveolar and extra-alveolar fractions, corresponding to what is considered respirable and ingestible lead, the coefficient of determination (R2) associated with the fractionated lead particulate increased approximately 25% over that attributable to only the total lead concentration. In addition, the deposition model, which closely matched the ACGIH reference worker criteria, resulted in ratios of the coefficients for the respirable to ingestible lead contributions to PbB that appeared to agree with experimental data, suggesting approximately a 10 to 1 ratio in absorption efficiency of the lung versus the gastrointestinal tract.

New Aerosol Models for the Retrieval of Aerosol Optical Thickness and Normalized Water-Leaving Radiances from the SeaWiFS and MODIS Sensors Over Coastal Regions and Open Oceans

NASA Technical Reports Server (NTRS)

Ahmad, Ziauddin; Franz, Bryan A.; McClain, Charles R.; Kwiatkowska, Ewa J.; Werdell, Jeremy; Shettle, Eric P.; Holben, Brent N.

2010-01-01

We describe the development of a new suite of aerosol models for the retrieval of atmospheric and oceanic optical properties from the SeaWiFs and MODIS sensors, including aerosol optical thickness (tau), angstrom coefficient (alpha), and water-leaving radiance (L(sub w)). The new aerosol models are derived from Aerosol Robotic Network (AERONET) observations and have bimodal lognormal distributions that are narrower than previous models used by the Ocean Biology Processing Group. We analyzed AERONET data over open ocean and coastal regions and found that the seasonal variability in the modal radii, particularly in the coastal region, was related to the relative humidity, These findings were incorporated into the models by making the modal radii, as well as the refractive indices, explicitly dependent on relative humidity, From those findings, we constructed a new suite of aerosol models. We considered eight relative humidity values (30%, 50%, 70%, 75%, 80%, 85%, 90%. and 95%) and, for each relative humidity value, we constructed ten distributions by varying the fine-mode fraction from zero to 1. In all. 80 distributions (8Rh x 10 fine-mode fractions) were created to process the satellite data. We. also assumed that the coarse-mode particles were nonabsorbing (sea salt) and that all observed absorptions were entirely due to fine-mode particles. The composition of fine mode was varied to ensure that the new models exhibited the same spectral dependence of single scattering albedo as observed in the AERONET data,

Investigation of shortcomings in simulated aerosol vertical profiles

NASA Astrophysics Data System (ADS)

Park, S.; Allen, R.

2017-12-01

The vertical distribution of aerosols is one important factor for aerosol radiative forcing. Previous studies show that climate models poorly reproduce the aerosol vertical profile, with too much aerosol aloft in the upper troposphere. This bias may be related to several factors, including excessive convective mass flux and wet removal. In this study, we evaluate the aerosol vertical profile from several Coupled Model Intercomparison Project 5 (CMIP5) models, as well as the Community Atmosphere Model 5 (CAM5), relative to the Cloud-Aerosol Lidar Infrared Pathfinder Satellite Observation (CALIPSO). The results show that all models significantly underestimate extinction coefficient in the lower troposphere, while overestimating extinction coefficient in the upper troposphere. In addition, the majority of models indicate a land-ocean dependence in the relationship between aerosol extinction coefficient in the upper troposphere and convective mass flux. Over the continents, more convective mass flux is related to more aerosol aloft; over the ocean, more convective mass flux is associated with less aerosol in upper troposphere. Sensitivity experiments are conducted to investigate the role that convection and wet deposition have in contributing to the deficient simulation of the vertical aerosol profile, including the land-ocean dependence.

Acid-catalyzed condensed-phase reactions of limonene and terpineol and their impacts on gas-to-particle partitioning in the formation of organic aerosols.

PubMed

Li, Yong Jie; Cheong, Gema Y L; Lau, Arthur P S; Chan, Chak K

2010-07-15

We investigated the condensed-phase reactions of biogenic VOCs with C double bond C bonds (limonene, C(10)H(16), and terpineol, C(10)H(18)O) catalyzed by sulfuric acid by both bulk solution (BS) experiments and gas-particle (GP) experiments using a flow cell reactor. Product analysis by gas chromatography-mass spectrometry (GC-MS) showed that cationic polymerization led to dimeric and trimeric product formation under conditions of relative humidity (RH) <20% (in the GP experiments) and a sulfuric acid concentration of 57.8 wt % (in the BS experiments), while hydration occurred under conditions of RH > 20% (in the GP experiments) and sulfuric acid concentrations of 46.3 wt % or lower (in the BS experiments). Apparent partitioning coefficients (K(p,rxn)) were estimated from the GP experiments by including the reaction products. Only under extremely low RH conditions (RH < 5%) did the values of K(p,rxn) ( approximately 5 x 10(-6) m(3)/microg for limonene and approximately 2 x 10(-5) m(3)/microg for terpineol) substantially exceed the physical partitioning coefficients (K(p) = 6.5 x 10(-8) m(3)/microg for limonene and =2.3 x 10(-6) m(3)/microg for terpineol) derived from the absorptive partitioning theory. At RH higher than 5%, the apparent partitioning coefficients (K(p,rxn)) of both limonene and terpineol were in the same order of magnitude as the K(p) values derived from the absorptive partitioning theory. Compared with other conditions including VOC concentration and degree of neutralization (by ammonium) of acidic particles, RH is a critical parameter that influences both the reaction mechanisms and the uptake ability (K(p,rxn) values) of these processes. The finding suggests that RH needs to be considered when taking the effects of acid-catalyzed reactions into account in estimating organic aerosol formation from C double bond C containing VOCs.

Aerosol Sources, Absorption, and Intercontinental Transport: Synergies among Models, Remote Sensing, and Atmospheric Measurements

NASA Technical Reports Server (NTRS)

Chin, Mian; Ginoux, Paul; Dubovik, Oleg; Holben, Brent; Kaufman, Yoram; chu, Allen; Anderson, Tad; Quinn, Patricia

2003-01-01

Aerosol climate forcing is one of the largest uncertainties in assessing the anthropogenic impact on the global climate system. This uncertainty arises from the poorly quantified aerosol sources, especially black carbon emissions, our limited knowledge of aerosol mixing state and optical properties, and the consequences of intercontinental transport of aerosols and their precursors. Here we use a global model GOCART to simulate atmospheric aerosols, including sulfate, black carbon, organic carbon, dust, and sea salt, from anthropogenic, biomass burning, and natural sources. We compare the model calculated aerosol extinction and absorption with those quantities from the ground-based sun photometer measurements from AERONET at several different wavelengths and the field observations from ACE-Asia, and model calculated total aerosol optical depth and fine mode fractions with the MODIS satellite retrieval. We will also estimate the intercontinental transport of pollution and dust aerosols from their source regions to other areas in different seasons.

Aerosol Sources, Absorption, and Intercontinental Transport: Synergies Among Models, Remote Sensing, and Atmospheric Measurements

NASA Technical Reports Server (NTRS)

Chin, Mian; Chu, Allen; Levy, Robert; Remer, Lorraine; Kaufman, Yoram; Dubovik, Oleg; Holben, Brent; Eck, Tom; Anderson, Tad; Quinn, Patricia

2004-01-01

Aerosol climate forcing is one of the largest uncertainties in assessing the anthropogenic impact on the global climate system. This uncertainty arises from the poorly quantified aerosol sources, especially black carbon emissions, our limited knowledge of aerosol mixing state and optical properties, and the consequences of intercontinental transport of aerosols and their precursors. Here we use a global model GOCART to simulate atmospheric aerosols, including sulfate, black carbon, organic carbon, dust, and sea salt, from anthropogenic, .biomass burning, and natural sources. We compare the model calculated aerosol extinction and absorption with those quantities from the ground-based sun photometer measurements from AERON" at several different wavelengths and the field observations from ACE-Asia, and model calculated total aerosol optical depth and fine mode fractions with the MODIS satellite retrieval. We will also estimate the intercontinental transport of pollution and dust aerosols from their source regions to other areas in different seasons.

On the evaluation of air mass factors for atmospheric near-ultraviolet and visible absorption spectroscopy

NASA Technical Reports Server (NTRS)

Perliski, Lori M.; Solomon, Susan

1993-01-01

The interpretation of UV-visible twilight absorption measurements of atmospheric chemical constituents is dependent on how well the optical path, or air mass factor, of light collected by the spectrometer is understood. A simple single scattering model and a Monte Carlo radiative transfer scheme have been developed to study the effects of multiple scattering, aerosol scattering, surface albedo and refraction on air mass factors for scattered light observations. At fairly short visible wavelengths (less than about 450 nm), stratospheric air mass factors are found to be relatively insensitive to multiple scattering, surface albedo and refraction, as well as aerosol scattering by background aerosols. Longer wavelengths display greater sensitivity to refraction and aerosol scattering. Tropospheric air mass factors are found to be highly dependent on aerosol scattering, surface albedo and, at long visible wavelengths (about 650 nm), refraction. Absorption measurements of NO2 and O4 are shown to support these conclusions.

The relative importance of aerosol scattering and absorption in remote sensing

NASA Technical Reports Server (NTRS)

Fraser, R. S.; Kaufman, Y. J.

1983-01-01

The relative importance of aerosol optical thickness and absorption is illustrated through computing radiances for radiative transfer models. The radiance of sunlight reflected from models of the earth-atmosphere system is computed as a function of the aerosol optical thickness and its albedo of single scattering; it is noted that the albedo varies from 0.6 in urban environment to nearly 1 in areas with low graphitic carbon content. The calculations are applied to the example of satellite measurements of biomass. It is found that when surface classifications are made by means of clustering techniques the presence of gradients in the aerosol optical properties results in the dispersion of points in the plot correlating radiances viewed in two different directions. Finally, though such a remote sensing parameter as contrast is weakly affected by aerosol absorption, it is highly dependent on its optical thickness.

Advances in atmospheric temperature profile measurements using high spectral resolution lidar

NASA Astrophysics Data System (ADS)

Razenkov, Ilya I.; Eloranta, Edwin W.

2018-04-01

This paper reports the atmospheric temperature profile measurements using a University of Wisconsin-Madison High Spectral Resolution Lidar (HSRL) and describes improvements in the instrument performance. HSRL discriminates between Mie and Rayleigh backscattering [1]. Thermal motion of molecules broadens the spectrum of the transmitted laser light due to Doppler effect. The HSRL exploits this property to allow the absolute calibration of the lidar and measurements of the aerosol volume backscatter coefficient. Two iodine absorption filters with different line widths are used to resolve temperature sensitive changes in Rayleigh backscattering for atmospheric temperature profile measurements.

Remote sensing of PM2.5 from ground-based optical measurements

NASA Astrophysics Data System (ADS)

Li, S.; Joseph, E.; Min, Q.

2014-12-01

Remote sensing of particulate matter concentration with aerodynamic diameter smaller than 2.5 um(PM2.5) by using ground-based optical measurements of aerosols is investigated based on 6 years of hourly average measurements of aerosol optical properties, PM2.5, ceilometer backscatter coefficients and meteorological factors from Howard University Beltsville Campus facility (HUBC). The accuracy of quantitative retrieval of PM2.5 using aerosol optical depth (AOD) is limited due to changes in aerosol size distribution and vertical distribution. In this study, ceilometer backscatter coefficients are used to provide vertical information of aerosol. It is found that the PM2.5-AOD ratio can vary largely for different aerosol vertical distributions. The ratio is also sensitive to mode parameters of bimodal lognormal aerosol size distribution when the geometric mean radius for the fine mode is small. Using two Angstrom exponents calculated at three wavelengths of 415, 500, 860nm are found better representing aerosol size distributions than only using one Angstrom exponent. A regression model is proposed to assess the impacts of different factors on the retrieval of PM2.5. Compared to a simple linear regression model, the new model combining AOD and ceilometer backscatter can prominently improve the fitting of PM2.5. The contribution of further introducing Angstrom coefficients is apparent. Using combined measurements of AOD, ceilometer backscatter, Angstrom coefficients and meteorological parameters in the regression model can get a correlation coefficient of 0.79 between fitted and expected PM2.5.

In-Situ and Remotely-Sensed Observations of Biomass Burning Aerosols at Doi Ang Khang, Thailand During 7-SEAS BASELInE 2015

NASA Technical Reports Server (NTRS)

Sayer, Andrew M.; Hsu, N. Christina; Hsiao, Ta-Chih; Pantina, Peter; Kuo, Ferret; Ou-Yang, Chang-Feng; Holben, Brent N.; Janjai, Serm; Chantara, Somporn; Wang, Sheng-Hsiang;

A photophonic instrument concept to measure atmospheric aerosol absorption. M.S. Thesis

NASA Technical Reports Server (NTRS)

Engle, C. D.

1982-01-01

A laboratory model of an instrument to measure the absorption of atmospheric aerosols was designed, built, and tested. The design was based on the photophonic phenomenon discovered by Bell and an acoustic resonator developed by Helmholtz. Experiments were done to show ways the signal amplitude could be improved and the noise reduced and to confirm the instrument was sensitive enough to be practical. The research was undertaken to develop concepts which show promise of being improvements on the instruments that are presently used to measure the absorption of the Sun's radiation by the Earth's atmospheric aerosols.

Light Source Effects on Aerosol Photoacoustic Spectroscopy Measurements

PubMed Central

Radney, James G.; Zangmeister, Christopher D.

2016-01-01

Photoacoustic spectroscopy measurements of flame-generated soot aerosol coated with small amounts of water yielded absorption enhancements that were dependent on the laser used: quasi-continuous wave (Q-CW, ≈ 650 ps pulse duration and 78 MHz repetition rate) versus continuous wave (CW). Water coating thickness was controlled by exposing the aerosol to a set relative humidity (RH). At ≈ 85 % RH, the mass of the soot particles increased by an amount comparable to a monolayer of water being deposited and enhanced the measured absorption by 36 % and 15 % for the Q-CW and CW lasers, respectively. Extinction measurements were also performed using a cavity ring-down spectrometer (extinction equals the sum of absorption and scattering) with a CW laser and negligible enhancement was observed at all RH. These findings demonstrate that source choice can impact measurements of aerosols with volatile coatings and that the absorption enhancements at high RH previously measured by Radney and Zangmeister (2015) [1] are the result of laser source used (Q-CW) and not from an increase in the particle absorption cross section. PMID:28066027

Absorption of Solar Radiation by Clouds: Observations Versus Models

NASA Technical Reports Server (NTRS)

Cess, R. D.; Zhang, M. H.; Minnis, P.; Corsetti, L.; Dutton, E. G.; Forgan, B. W.; Garber, D. P.; Gates, W. L.; Hack, J. J.; Harrison, E. F.;

Aerosol Absorption by Black Carbon and Dust: Implications of Climate Change and Air Quality in Asia

NASA Technical Reports Server (NTRS)

Chin, Mian

2010-01-01

Atmospheric aerosol distributions from 2000 to 2007 are simulated with the global model GOCART to attribute light absorption by aerosol to its composition and sources. We show the seasonal and interannual variations of absorbing aerosols in the atmosphere over Asia, mainly black carbon and dust. and their linkage to the changes of anthropogenic and dust emissions in the region. We compare our results with observations from satellite and ground-based networks, and estimate the importance of black carbon and dust on regional climate forcing and air quality.

UManSysProp: an online facility for molecular property prediction and atmospheric aerosol calculations

NASA Astrophysics Data System (ADS)

Topping, D.; Barley, M. H.; Bane, M.; Higham, N.; Aumont, B.; McFiggans, G.

2015-11-01

In this paper we describe the development and application of a new web based facility, UManSysProp (http://umansysprop.seaes.manchester.ac.uk), for automating predictions of molecular and atmospheric aerosol properties. Current facilities include: pure component vapour pressures, critical properties and sub-cooled densities of organic molecules; activity coefficient predictions for mixed inorganic-organic liquid systems; hygroscopic growth factors and CCN activation potential of mixed inorganic/organic aerosol particles; absorptive partitioning calculations with/without a treatment of non-ideality. The aim of this new facility is to provide a single point of reference for all properties relevant to atmospheric aerosol that have been checked for applicability to atmospheric compounds where possible. The group contribution approach allows users to upload molecular information in the form of SMILES strings and UManSysProp will automatically extract the relevant information for calculations. Built using open source chemical informatics, and hosted at the University of Manchester, the facilities are provided via a browser and device-friendly web-interface, or can be accessed using the user's own code via a JSON API. In this paper we demonstrate its use with specific examples that can be simulated using the web-browser interface.

Utilization of O4 slant column density to derive aerosol layer height from a space-borne UV-visible hyperspectral sensor: sensitivity and case study

NASA Astrophysics Data System (ADS)

Park, Sang Seo; Kim, Jhoon; Lee, Hanlim; Torres, Omar; Lee, Kwang-Mog; Lee, Sang Deok

2016-02-01

The sensitivities of oxygen-dimer (O4) slant column densities (SCDs) to changes in aerosol layer height are investigated using the simulated radiances by a radiative transfer model, the linearized pseudo-spherical vector discrete ordinate radiative transfer (VLIDORT), and the differential optical absorption spectroscopy (DOAS) technique. The sensitivities of the O4 index (O4I), which is defined as dividing O4 SCD by 1040 molecules2 cm-5, to aerosol types and optical properties are also evaluated and compared. Among the O4 absorption bands at 340, 360, 380, and 477 nm, the O4 absorption band at 477 nm is found to be the most suitable to retrieve the aerosol effective height. However, the O4I at 477 nm is significantly influenced not only by the aerosol layer effective height but also by aerosol vertical profiles, optical properties including single scattering albedo (SSA), aerosol optical depth (AOD), particle size, and surface albedo. Overall, the error of the retrieved aerosol effective height is estimated to be 1276, 846, and 739 m for dust, non-absorbing, and absorbing aerosol, respectively, assuming knowledge on the aerosol vertical distribution shape. Using radiance data from the Ozone Monitoring Instrument (OMI), a new algorithm is developed to derive the aerosol effective height over East Asia after the determination of the aerosol type and AOD from the MODerate resolution Imaging Spectroradiometer (MODIS). About 80 % of retrieved aerosol effective heights are within the error range of 1 km compared to those obtained from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) measurements on thick aerosol layer cases.

Utilization of O4 Slant Column Density to Derive Aerosol Layer Height from a Space-Borne UV-Visible Hyperspectral Sensor: Sensitivity and Case Study

NASA Technical Reports Server (NTRS)

Park, Sang Seo; Kim, Jhoon; Lee, Hanlim; Torres, Omar; Lee, Kwang-Mog; Lee, Sang Deok

2016-01-01

The sensitivities of oxygen-dimer (O4) slant column densities (SCDs) to changes in aerosol layer height are investigated using the simulated radiances by a radiative transfer model, the linearized pseudo-spherical vector discrete ordinate radiative transfer (VLIDORT), and the differential optical absorption spectroscopy (DOAS) technique. The sensitivities of the O4 index (O4I), which is defined as dividing O4 SCD by 10(sup 40) molecules (sup 2) per centimeters(sup -5), to aerosol types and optical properties are also evaluated and compared. Among the O4 absorption bands at 340, 360, 380, and 477 nanometers, the O4 absorption band at 477 nanometers is found to be the most suitable to retrieve the aerosol effective height. However, the O4I at 477 nanometers is significantly influenced not only by the aerosol layer effective height but also by aerosol vertical profiles, optical properties including single scattering albedo (SSA), aerosol optical depth (AOD), particle size, and surface albedo. Overall, the error of the retrieved aerosol effective height is estimated to be 1276, 846, and 739 meters for dust, non-absorbing, and absorbing aerosol, respectively, assuming knowledge on the aerosol vertical distribution shape. Using radiance data from the Ozone Monitoring Instrument (OMI), a new algorithm is developed to derive the aerosol effective height over East Asia after the determination of the aerosol type and AOD from the MODerate resolution Imaging Spectroradiometer (MODIS). About 80 percent of retrieved aerosol effective heights are within the error range of 1 kilometer compared to those obtained from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) measurements on thick aerosol layer cases.

Utilization of O4 Slant Column Density to Derive Aerosol Layer Height from a Spaceborne UV-Visible Hyperspectral Sensor: Sensitivity and Case Study

NASA Technical Reports Server (NTRS)

Park, Sang Seo; Kim, Jhoon; Lee, Hanlim; Torres, Omar; Lee, Kwang-Mog; Lee, Sang Deok

2016-01-01

The sensitivities of oxygen-dimer (O4) slant column densities (SCDs) to changes in aerosol layer height are investigated using the simulated radiances by a radiative transfer model, the linearized pseudo-spherical vector discrete ordinate radiative transfer (VLIDORT), and the Differential Optical Absorption Spectroscopy (DOAS) technique. The sensitivities of the O4 index (O4I), which is defined as dividing O4 SCD by 10(exp 40) sq molecules cm(exp -5), to aerosol types and optical properties are also evaluated and compared. Among the O4 absorption bands at 340, 360, 380, and 477 nm, the O4 absorption band at 477 nm is found to be the most suitable to retrieve the aerosol effective height. However, the O4I at 477 nm is significantly influenced not only by the aerosol layer effective height but also by aerosol vertical profiles, optical properties including single scattering albedo (SSA), aerosol optical depth (AOD), particle size, and surface albedo. Overall, the error of the retrieved aerosol effective height is estimated to be 1276, 846, and 739 m for dust, non-absorbing, and absorbing aerosol, respectively, assuming knowledge on the aerosol vertical distribution shape. Using radiance data from the Ozone Monitoring Instrument (OMI), a new algorithm is developed to derive the aerosol effective height over East Asia after the determination of the aerosol type and AOD from the MODerate resolution Imaging Spectroradiometer (MODIS). About 80% of retrieved aerosol effective heights are within the error range of 1 km compared to those obtained from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) measurements on thick aerosol layer cases.

Radiative transfer model for aerosols in infrared wavelengths for passive remote sensing applications.

PubMed

Ben-David, Avishai; Embury, Janon F; Davidson, Charles E

2006-09-10

A comprehensive analytical radiative transfer model for isothermal aerosols and vapors for passive infrared remote sensing applications (ground-based and airborne sensors) has been developed. The theoretical model illustrates the qualitative difference between an aerosol cloud and a chemical vapor cloud. The model is based on two and two/four stream approximations and includes thermal emission-absorption by the aerosols; scattering of diffused sky radiances incident from all sides on the aerosols (downwelling, upwelling, left, and right); and scattering of aerosol thermal emission. The model uses moderate resolution transmittance ambient atmospheric radiances as boundary conditions and provides analytical expressions for the information on the aerosol cloud that is contained in remote sensing measurements by using thermal contrasts between the aerosols and diffused sky radiances. Simulated measurements of a ground-based sensor viewing Bacillus subtilis var. niger bioaerosols and kaolin aerosols are given and discussed to illustrate the differences between a vapor-only model (i.e., only emission-absorption effects) and a complete model that adds aerosol scattering effects.

Quantification of Absorption Due to Black and Brown Carbon from Biomass Burning and Parameterizations for Comparison to Climate Models Result

NASA Astrophysics Data System (ADS)

Pokhrel, Rudra Prasad

This dissertation examines the optical properties of fresh and aged biomass burning aerosols, parameterization of these properties, and development of new instrumentation and calibration techniques to measure aerosol optical properties. Data sets were collected from the fourth Fire Lab at Missoula Experiment (FLAME-4) that took place from October 15 to November 16, 2012. Biomass collected from the various parts of the world were burned under controlled laboratory conditions and fresh emissions from different stages of burning were measured and analyzed. Optical properties of aged aerosol under different conditions was also explored. A photoacoustic absorption spectrometer (PAS) was built and integrated with a newly designed thermal denuder to improve upon observations made during Flame-4. A novel calibration technique for the PAS was developed. Single scattering albedo (SSA) and absorption Angstrom exponent (AAE) from 12 different fuels with 41 individual burns were estimated and parameterized with modified combustion efficiency (MCE) and the ratio of elemental carbon (EC) to organic carbon (OC) mass. The EC / OC ratio has better capability to parameterize SSA and AAE than MCE. The simple linear regression model proposed in this study accurately predicts SSA during the first few hours of plume aging with the ambient data from a biomass burning event. In addition, absorption due to brown carbon (BrC) can significantly lower the SSA at 405 nm resulting in a wavelength dependence of SSA. Furthermore, smoldering dominated burns have larger AAE values while flaming dominated burns have smaller AAE values indicating a large fraction of BrC is emitted during the smoldering stage of the burn. Enhancement in BC absorption (EAbs) due to coating by absorbing and non-absorbing substances is estimated at 405 nm and 660 nm. Relatively smaller values of EAbs at 660 nm compared to 405 nm suggests lensing is a less important contributor to biomass burning aerosol absorption at lower wavelengths. Multiple burns of the same fuel produced significantly different EAbs values at 405 nm, but show good correlation with the EC/OC ratio indicating less dependency on fuel type and more dependency on burn conditions. In addition, absorption due to BrC can contribute up to 92 % of the total biomass burning aerosol absorption at 405 nm and up to 58 % of the total absorption at 532 nm. Indicating BrC absorption in biomass burning emissions is equally or more important than the absorption due to BC at short wavelengths. Furthermore, fractional absorption due to BrC shows reasonably good correlation with EC/OC ratio and AAE. Primary organic aerosol is found to be more volatile than secondary organic aerosol and it is found that the thermal denuder deployed in this study removes less organic aerosol if secondary organic aerosol is present. SSA at 532 nm remains constant during different conditions of aging while SSA at 405 nm increases under certain conditions suggesting the degradation of BrC. Decreases in AAE under the same experiment further support the proposed BrC degradation. The novel thermal denuder designed completely removes non-refractory material and can be used under higher flow rates (maximum of 5 LPM) than the most commercially available thermal denuders. The new calibration techniques proposed for the photoacousitc absorption spectrometer will reduce uncertainty during calibration compared to the conventional calibration methods.

Using OMI Observations to Measure Aerosol Absorption of Biomass Burning Aerosols Above Clouds

NASA Technical Reports Server (NTRS)

Torres, Omar; Bhartia, P. K.; Jethva, Hiren

2011-01-01

The presence of absorbing aerosol layers above clouds is unambiguously detected by the TOMS/OMI UV Aerosol Index (AI) that uses satellite observations at two near-UV channels. A sensitivity study using radiative transfer calculations shows that the AI signal of resulting from the presence of aerosols above clouds is mainly driven by the aerosol absorption optical depth and the optical depth of the underlying cloud. Based on these results, an inversion algorithm has been developed to retrieve the aerosol optical depth (AOD) of aerosol layers above clouds. In this presentation we will discuss the sensitivity analysis, describe the retrieval approach, and present results of applications of the retrieval method to OMI observations over the South Atlantic Ocean. Preliminary error analyses, to be discussed, indicate that the AOD can be underestimated (up to -30%) or overestimated (up to 60%) depending on algorithmic assumptions.

Results of a comprehensive atmospheric aerosol-radiation experiment in the southwestern United States. I - Size distribution, extinction optical depth and vertical profiles of aerosols suspended in the atmosphere. II - Radiation flux measurements and

NASA Technical Reports Server (NTRS)

Deluisi, J. J.; Furukawa, F. M.; Gillette, D. A.; Schuster, B. G.; Charlson, R. J.; Porch, W. M.; Fegley, R. W.; Herman, B. M.; Rabinoff, R. A.; Twitty, J. T.

1976-01-01

Results are reported for a field test that was aimed at acquiring a sufficient set of measurements of aerosol properties required as input for radiative-transfer calculations relevant to the earth's radiation balance. These measurements include aerosol extinction and size distributions, vertical profiles of aerosols, and radiation fluxes. Physically consistent, vertically inhomogeneous models of the aerosol characteristics of a turbid atmosphere over a desert and an agricultural region are constructed by using direct and indirect sampling techniques. These results are applied for a theoretical interpretation of airborne radiation-flux measurements. The absorption term of the complex refractive index of aerosols is estimated, a regional variation in the refractive index is noted, and the magnitude of solar-radiation absorption by aerosols and atmospheric molecules is determined.

CALIOP near-real-time backscatter products compared to EARLINET data

NASA Astrophysics Data System (ADS)

Grigas, T.; Hervo, M.; Gimmestad, G.; Forrister, H.; Schneider, P.; Preißler, J.; Tarrason, L.; O'Dowd, C.

2015-03-01

The expedited near-real-time Level 1.5 Cloud-Aerosol Lidar (Light Detection and Ranging) with Orthogonal Polarization (CALIOP) products were evaluated against data from the ground-based European Aerosol Research Lidar Network (EARLINET). Over a period of three years, lidar data from 48 CALIOP overpasses with ground tracks within a 100 km distance from an operating EARLINET station were deemed suitable for analysis and they included a valid aerosol classification type (e.g. dust, polluted dust, clean marine, clean continental, polluted continental, mixed and/or smoke/biomass burning). For the complete dataset comprising both PBL and FT data, the correlation coefficient was 0.86, and when separated into separate layers, the PBL and FT correlation coefficients were 0.6 and 0.85 respectively. The presence of FT layers with high attenuated backscatter led to poor agreement in PBL backscatter profiles between the CALIOP and EARLINET measurements and prompted a further analysis filtering out such cases. However, the correlation coefficient value for the complete dataset decreased marginally from 0.86 to 0.84 while the PBL coefficient increased from 0.6 up to 0.65 and the FT coefficient also decreased from 0.85 to 0.79. For specific aerosol types, the correlation coefficient between CALIOP backscatter profiles and ground-based lidar data ranged from 0.37 for polluted continental aerosol in the planetary boundary layer (PBL) to 0.57 for dust in the free troposphere (FT). The results suggest different levels of agreement based on the location of the dominant aerosol layer and the aerosol type.

Aerosol remote sensing in polar regions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tomasi, Claudio; Kokhanovsky, Alexander A.; Lupi, Angelo

Multi-year sets of ground-based sun-photometer measurements conducted at 12 Arctic sites and 9 Antarctic sites were examined to determine daily mean values of aerosol optical thickness τ(λ) at visible and near-infrared wavelengths, from which best-fit values of Ångström's exponent α were calculated. Analysing these data, the monthly mean values of τ(0.50 μm) and α and the relative frequency histograms of the daily mean values of both parameters were determined for winter–spring and summer–autumn in the Arctic and for austral summer in Antarctica. The Arctic and Antarctic covariance plots of the seasonal median values of α versus τ(0.50 μm) showed: (i)more » a considerable increase in τ(0.50 μm) for the Arctic aerosol from summer to winter–spring, without marked changes in α; and (ii) a marked increase in τ(0.50 μm) passing from the Antarctic Plateau to coastal sites, whereas α decreased considerably due to the larger fraction of sea-salt aerosol. Good agreement was found when comparing ground-based sun-photometer measurements of τ(λ) and α at Arctic and Antarctic coastal sites with Microtops measurements conducted during numerous AERONET/MAN cruises from 2006 to 2013 in three Arctic Ocean sectors and in coastal and off-shore regions of the Southern Atlantic, Pacific, and Indian Oceans, and the Antarctic Peninsula. Lidar measurements were also examined to characterise vertical profiles of the aerosol backscattering coefficient measured throughout the year at Ny-Ålesund. Satellite-based MODIS, MISR, and AATSR retrievals of τ(λ) over large parts of the oceanic polar regions during spring and summer were in close agreement with ship-borne and coastal ground-based sun-photometer measurements. An overview of the chemical composition of mode particles is also presented, based on in-situ measurements at Arctic and Antarctic sites. Fourteen log-normal aerosol number size-distributions were defined to represent the average features of nuclei, accumulation and coarse mode particles for Arctic haze, summer background aerosol, Asian dust and boreal forest fire smoke, and for various background austral summer aerosol types at coastal and high-altitude Antarctic sites. The main columnar aerosol optical characteristics were determined for all 14 particle modes, based on in-situ measurements of the scattering and absorption coefficients. Diurnally averaged direct aerosol-induced radiative forcing and efficiency were calculated for a set of multimodal aerosol extinction models, using various Bidirectional Reflectance Distribution Function models over vegetation-covered, oceanic and snow-covered surfaces. These gave a reliable measure of the pronounced effects of aerosols on the radiation balance of the surface–atmosphere system over polar regions.« less

Aerosol Remote Sensing in Polar Regions

NASA Technical Reports Server (NTRS)

Tomasi, Claudio; Kokhanovsky, Alexander A.; Lupi, Angelo; Ritter, Christoph; Smirnov, Alexander; O'Neill, Norman T.; Stone, Robert S.; Holben, Brent N.; Nyeki, Stephan; Wehrli, Christoph

2014-01-01

Multi-year sets of ground-based sun-photometer measurements conducted at 12 Arctic sites and 9 Antarctic sites were examined to determine daily mean values of aerosol optical thickness tau(lambda) at visible and near-infrared wavelengths, from which best-fit values of Ångström's exponent alpha were calculated. Analyzing these data, the monthly mean values of tau(0.50 micrometers) and alpha and the relative frequency histograms of the daily mean values of both parameters were determined for winter-spring and summer-autumn in the Arctic and for austral summer in Antarctica. The Arctic and Antarctic covariance plots of the seasonal median values of alpha versus tau(0.50 micrometers) showed: (i) a considerable increase in tau(0.50 micrometers) for the Arctic aerosol from summer to winter-spring, without marked changes in alpha; and (ii) a marked increase in tau(0.50 micrometer) passing from the Antarctic Plateau to coastal sites, whereas alpha decreased considerably due to the larger fraction of sea-salt aerosol. Good agreement was found when comparing ground-based sun-photometer measurements of tau(lambda) and alpha at Arctic and Antarctic coastal sites with Microtops measurements conducted during numerous AERONET/MAN cruises from 2006 to 2013 in three Arctic Ocean sectors and in coastal and off-shore regions of the Southern Atlantic, Pacific, and Indian Oceans, and the Antarctic Peninsula. Lidar measurements were also examined to characterize vertical profiles of the aerosol backscattering coefficient measured throughout the year at Ny-Ålesund. Satellite-based MODIS, MISR, and AATSR retrievals of tau(lambda) over large parts of the oceanic polar regions during spring and summer were in close agreement with ship-borne and coastal ground-based sun-photometer measurements. An overview of the chemical composition of mode particles is also presented, based on in-situ measurements at Arctic and Antarctic sites. Fourteen log-normal aerosol number size-distributions were defined to represent the average features of nuclei, accumulation and coarse mode particles for Arctic haze, summer background aerosol, Asian dust and boreal forest fire smoke, and for various background austral summer aerosol types at coastal and high-altitude Antarctic sites. The main columnar aerosol optical characteristics were determined for all 14 particle modes, based on in-situ measurements of the scattering and absorption coefficients. Diurnally averaged direct aerosol-induced radiative forcing and efficiency were calculated for a set of multimodal aerosol extinction models, using various Bidirectional Reflectance Distribution Function models over vegetation-covered, oceanic and snow-covered surfaces. These gave a reliable measure of the pronounced effects of aerosols on the radiation balance of the surface-atmosphere system over polar regions.

Aerosol remote sensing in polar regions

DOE PAGES

Tomasi, Claudio; Kokhanovsky, Alexander A.; Lupi, Angelo; ...

2015-01-01

Multi-year sets of ground-based sun-photometer measurements conducted at 12 Arctic sites and 9 Antarctic sites were examined to determine daily mean values of aerosol optical thickness τ(λ) at visible and near-infrared wavelengths, from which best-fit values of Ångström's exponent α were calculated. Analysing these data, the monthly mean values of τ(0.50 μm) and α and the relative frequency histograms of the daily mean values of both parameters were determined for winter–spring and summer–autumn in the Arctic and for austral summer in Antarctica. The Arctic and Antarctic covariance plots of the seasonal median values of α versus τ(0.50 μm) showed: (i)more » a considerable increase in τ(0.50 μm) for the Arctic aerosol from summer to winter–spring, without marked changes in α; and (ii) a marked increase in τ(0.50 μm) passing from the Antarctic Plateau to coastal sites, whereas α decreased considerably due to the larger fraction of sea-salt aerosol. Good agreement was found when comparing ground-based sun-photometer measurements of τ(λ) and α at Arctic and Antarctic coastal sites with Microtops measurements conducted during numerous AERONET/MAN cruises from 2006 to 2013 in three Arctic Ocean sectors and in coastal and off-shore regions of the Southern Atlantic, Pacific, and Indian Oceans, and the Antarctic Peninsula. Lidar measurements were also examined to characterise vertical profiles of the aerosol backscattering coefficient measured throughout the year at Ny-Ålesund. Satellite-based MODIS, MISR, and AATSR retrievals of τ(λ) over large parts of the oceanic polar regions during spring and summer were in close agreement with ship-borne and coastal ground-based sun-photometer measurements. An overview of the chemical composition of mode particles is also presented, based on in-situ measurements at Arctic and Antarctic sites. Fourteen log-normal aerosol number size-distributions were defined to represent the average features of nuclei, accumulation and coarse mode particles for Arctic haze, summer background aerosol, Asian dust and boreal forest fire smoke, and for various background austral summer aerosol types at coastal and high-altitude Antarctic sites. The main columnar aerosol optical characteristics were determined for all 14 particle modes, based on in-situ measurements of the scattering and absorption coefficients. Diurnally averaged direct aerosol-induced radiative forcing and efficiency were calculated for a set of multimodal aerosol extinction models, using various Bidirectional Reflectance Distribution Function models over vegetation-covered, oceanic and snow-covered surfaces. These gave a reliable measure of the pronounced effects of aerosols on the radiation balance of the surface–atmosphere system over polar regions.« less

Identification of aerosol composition from multi-wavelength lidar measurements

NASA Technical Reports Server (NTRS)

Wood, S. A.

1984-01-01

This paper seeks to develop the potential of lidar for the identification of the chemical composition of atmospheric aerosols. Available numerical computations suggest that aerosols can be identified by the wavelength dependence of aerosol optical properties. Since lidar can derive the volume backscatter coefficient as a function of wavelength, a multi-wavelength lidar system may be able to provide valuable information on the composition of aerosols. This research theoretically investigates the volume backscatter coefficients for the aerosol classes, sea-salts, and sulfates, as a function of wavelength. The results show that these aerosol compositions can be characterized and identified by their backscatter wavelength dependence. A method to utilize multi-wavelength lidar measurements to discriminate between compositionally different thin aerosol layers is discussed.

International Laser Radar Conference (16th) held at the Massachusetts Institute of Technology, Cambridge, Massachusetts on 20-24 July 1992. Part 1

DTIC Science & Technology

1993-07-24

orders smaller than the Rayleigh cross section. We estimated the extinction coefficients of the Pinatubo volcanic aerosol in the stratosphere using a Raman...to a common aerosol parameter (e.g., backscatter coefficients at selected CO2 wavelengths), have all led to similar estimated values of that...increase only as -r 2 . During this phase, therefore, the backscatter coefficient of a coagulating aerosol population decreases as -r- The maximum

On-road measurement of black carbon mass, absorption, and single-scattering albedo

EPA Science Inventory

Absorption and scattering of solar radiation by aerosols emitted from combustion sources can affect the earth’s radiative balance and may potentially affect local and regional climate. Optical properties of aerosols emitted from mobile sources have not been thoroughly characteri...

Chemical Properties of Brown Carbon Aerosol Generated at the Missoula Fire Sciences Laboratory

NASA Astrophysics Data System (ADS)

Washenfelder, R. A.; Womack, C.; Franchin, A.; Middlebrook, A. M.; Wagner, N.; Manfred, K.

2017-12-01

Aerosol scattering and absorption are still among the largest uncertainties in quantifying radiative forcing. Biomass burning is a major source of light-absorbing carbonaceous aerosol in the United States. These aerosol are generally classified into two categories: black carbon (graphitic-like aerosol that absorbs broadly across the ultraviolet and visible spectral regions) and brown carbon (organic aerosol that absorbs strongly in the ultraviolet and near-visible spectral regions). The composition, volatility, and chemical aging of brown carbon are poorly known, but are important to understanding its radiative effects. We deployed three novel instruments to the Missoula Fire Sciences Laboratory in 2016 to measure brown carbon absorption: a photoacoustic spectrometer, broadband cavity enhanced spectrometer, and particle-into-liquid sampler coupled to a liquid waveguide capillary cell. The instruments sampled from a shared inlet with well-characterized dilution and thermal denuding. We sampled smoke from 32 controlled burns of fuels relevant to western U.S. wildfires. We use these measurements to determine the volatility of water-soluble brown carbon, and compare this to the volatility of water-soluble organic aerosol and total organic aerosol. We further examine the wavelength-dependence of the water-soluble brown carbon absorption as a function of denuder temperature. Together this gives new information about the solubility, volatility, and chemical composition of brown carbon.

Aerosol Composition and Variability in Baltimore Measured during DISCOVER-AQ

NASA Astrophysics Data System (ADS)

Beyersdorf, A. J.; Ziemba, L. D.; Chen, G.; Thornhill, K. L.; Winstead, E. L.; Diskin, G. S.; Chatfield, R. B.; Natraj, V.; Anderson, B. E.

2012-12-01

In order to relate satellite-based measurements of aerosols to ground-level air quality, the correlation between aerosol optical properties (wavelength-dependent scattering and absorption measured by satellites) and mass measurements of aerosol loading (i.e. PM2.5 used for air quality monitoring) must be understood. This connection varies with many factors including those specific to the aerosol type (such as composition, size, hygroscopicity, and mass scattering and absorption efficiencies) and to the surrounding atmosphere (such as temperature, relative humidity and altitude). The DISCOVER-AQ (Deriving Information on Surface conditions from COlumn and VERtically resolved observations relevant to Air Quality) project was designed to provide a unique dataset for determining variability in and correlations between aerosol loading, composition, optical properties and meteorological conditions. Extensive in-situ profiling of the lower atmosphere in the Baltimore-Washington D.C. region was performed during fourteen flights during July 2011. Identical flight plans and profile locations throughout the campaign provide meaningful statistics for analysis. Measured aerosol mass was composed primarily of ammonium sulfate (campaign average of 36%) and water-soluble organics (58%). A distinct difference in composition was related to aerosol loading with high-loading days having a proportionally larger percentage of ammonium sulfate (up to 60%). This composition shift causes a change in the water-uptake potential (hygroscopicity) of the aerosols with higher relative organic composition decreasing water-uptake. On average, sulfate mass increased during the day due to increased photochemistry, while organics decreased. Analysis of the linkage between aerosol loading and optical properties was also performed. The absorption by black carbon was dependent on the amount of organic coating with an increase in mass absorption efficiency from 7.5 m2/g for bare soot to 16 m2/g at an organic mass fraction of 70%. The organic fraction was also found to correlate with the absorption Angstrom exponent which is a solely optical measurement. This relationship allows for a possible understanding of aerosol composition based on solely-optical methods (such as satellite-based sensors). Comparison of aerosol composition to scattering indicated significant scattering from non-hydrophilic particles. The origin seemed to be hydrophobic organic material, and the scattering effects were roughly the same magnitude as the water-soluble organics. Such aerosols are not simulated in many air pollution models, and require more field study. 246 profiles were performed at six locations throughout the region. Variability in aerosol scattering (as a proxy for aerosol optical depth) amongst the six sites is dependent on variability in aerosol loading, composition, and relative humidity (the amount of water available for water uptake onto the aerosols). Aerosol loading was found to be the predominant source accounting for 68% on average of the measured variability in scattering with minor contributions from relative humidity (24%) and aerosol composition (8%).

Retrieval method of aerosol extinction coefficient profile by an integral lidar system and case study

NASA Astrophysics Data System (ADS)

Shan, Huihui; Zhang, Hui; Liu, Junjian; Wang, Shenhao; Ma, Xiaomin; Zhang, Lianqing; Liu, Dong; Xie, Chenbo; Tao, Zongming

2018-02-01

Aerosol extinction coefficient profile is an essential parameter for atmospheric radiation model. But it is difficult to get the full aerosol extinction profile from the ground to the tropopause especially in near ground precisely using backscattering lidar. A combined measurement of side-scattering, backscattering and Raman-scattering lidar is proposed to retrieve the aerosol extinction coefficient profile from the surface to the tropopause which covered a dynamic range of 5 orders. The side-scattering technique solves the dead zone and the overlap problem caused by the traditional lidar in the near range. Using the Raman-scattering the aerosol lidar ratio (extinction to backscatter ratio) can be obtained. The cases studies in this paper show the proposed method is reasonable and feasible.

Longwave radiative effects of Saharan dust during the ICE-D campaign

NASA Astrophysics Data System (ADS)

Brooke, Jennifer; Havemann, Stephan; Ryder, Claire; O'Sullivan, Debbie

2017-04-01

The Havemann-Taylor Fast Radiative Transfer Code (HT-FRTC) is a fast radiative transfer model based on Principal Components. Scattering has been incorporated into HT-FRTC which allows simulations of aerosol as well as clear-sky atmospheres. This work evaluates the scattering scheme in HT-FRTC and investigates dust-affected brightness temperatures using in-situ observations from Ice in Clouds Experiment - Dust (ICE-D) campaign. The ICE-D campaign occurred during August 2015 and was based from Cape Verde. The ICE-D campaign is a multidisciplinary project which achieved measurements of in-situ mineral dust properties of the dust advected from the Sahara, and on the aerosol-cloud interactions using the FAAM BAe-146 research aircraft. ICE-D encountered a range of low (0.3), intermediate (0.8) and high (1.3) aerosol optical depths, AODs, and therefore provides a range of atmospheric dust loadings in the assessment of dust scattering in HT-FRTC. Spectral radiances in the thermal infrared window region (800 - 1200 cm-1) are sensitive to the presence of mineral dust; mineral dust acts to reduce the upwelling infrared radiation caused by the absorption and re-emission of radiation by the dust layer. ARIES (Airborne Research Interferometer Evaluation System) is a nadir-facing interferometer, measuring infrared radiances between 550 and 3000 cm-1. The ARIES spectral radiances are converted to brightness temperatures by inversion of the Planck function. The mineral dust size distribution is important for radiative transfer applications as it provides a measure of aerosol scattering. The longwave spectral mineral dust optical properties including the mass extinction coefficients, single scattering albedos and the asymmetry parameter have been derived from the mean ICE-D size distribution. HT-FRTC scattering simulations are initialised with vertical mass fractions which can be derived from extinction profiles from the lidar along with the specific extinction coefficient, kext (m2/g) at 355 nm. In general the comparison between the lidar retrieval of aerosol extinction coefficients and in-situ measurements show a good agreement. The root mean square of the brightness temperature residuals in the window region for observations (ARIES) minus model simulations for i) clear-sky, ii) HT-FRTC 'line-by-line' scattering and, iii) HT-FRTC fast scattering are calculated. For the ICE-D case studies mineral dust impacts on the brightness temperature of the background on the order of 1 - 1.5 K.

Optical, physical and chemical properties of transported African mineral dust aerosols in the Mediterranean region

NASA Astrophysics Data System (ADS)

Denjean, Cyrielle; Di Biagio, Claudia; Chevaillier, Servanne; Gaimoz, Cécile; Grand, Noel; Loisil, Rodrigue; Triquet, Sylvain; Zapf, Pascal; Roberts, Greg; Bourrianne, Thierry; Torres, Benjamin; Blarel, Luc; Sellegri, Karine; Freney, Evelyn; Schwarzenbock, Alfons; Ravetta, François; Laurent, Benoit; Mallet, Marc; Formenti, Paola

2014-05-01

The transport of mineral dust aerosols is a global phenomenon with strong climate implications. Depending on the travel distance over source regions, the atmospheric conditions and the residence time in the atmosphere, various transformation processes (size-selective sedimentation, mixing, condensation of gaseous species, and weathering) can modify the physical and chemical properties of mineral dust, which, in turn, can change the dust's optical properties. The model predictions of the radiative effect by mineral dust still suffer of the lack of certainty of these properties, and their temporal evolution with transport time. Within the frame of the ChArMex project (Chemistry-Aerosol Mediterranean experiment, http://charmex.lsce.ipsl.fr/), two intensive airborne campaigns (TRAQA, TRansport and Air QuAlity, 18 June - 11 July 2012, and ADRIMED, Aerosol Direct Radiative Impact in the regional climate in the MEDiterranean region, 06 June - 08 July 2013) have been performed over the Central and Western Mediterranean, one of the two major transport pathways of African mineral dust. In this study we have set up a systematic strategy to determine the optical, physical and optical properties of mineral dust to be compared to an equivalent dataset for dust close to source regions in Africa. This study is based on airborne observations onboard the SAFIRE ATR-42 aircraft, equipped with state of the art in situ instrumentation to measure the particle scattering and backscattering coefficients (nephelometer at 450, 550, and 700 nm), the absorption coefficient (PSAP at 467, 530, and 660 nm), the extinction coefficient (CAPS at 530 nm), the aerosol optical depth (PLASMA at 340 to 1640 nm), the size distribution in the extended range 40 nm - 30 µm by the combination of different particle counters (SMPS, USHAS, FSSP, GRIMM) and the chemical composition obtained by filter sampling. The chemistry and transport model CHIMERE-Dust have been used to classify the air masses according to the dust origin and transport. Case studies of dust transport from known but differing origins (source regions in Tunisia, Algeria, and Mauritania) and at different times after transport, will be presented. Results will be compared to equivalent measurements over source regions interpreted in terms of the evolution of the particle size distribution, chemical composition and optical properties.

Constraining Carbonaceous Aerosol Climate Forcing by Bridging Laboratory, Field and Modeling Studies

NASA Astrophysics Data System (ADS)

Dubey, M. K.; Aiken, A. C.; Liu, S.; Saleh, R.; Cappa, C. D.; Williams, L. R.; Donahue, N. M.; Gorkowski, K.; Ng, N. L.; Mazzoleni, C.; China, S.; Sharma, N.; Yokelson, R. J.; Allan, J. D.; Liu, D.

2014-12-01

Biomass and fossil fuel combustion emits black (BC) and brown carbon (BrC) aerosols that absorb sunlight to warm climate and organic carbon (OC) aerosols that scatter sunlight to cool climate. The net forcing depends strongly on the composition, mixing state and transformations of these carbonaceous aerosols. Complexities from large variability of fuel types, combustion conditions and aging processes have confounded their treatment in models. We analyse recent laboratory and field measurements to uncover fundamental mechanism that control the chemical, optical and microphysical properties of carbonaceous aerosols that are elaborated below: Wavelength dependence of absorption and the single scattering albedo (ω) of fresh biomass burning aerosols produced from many fuels during FLAME-4 was analysed to determine the factors that control the variability in ω. Results show that ω varies strongly with fire-integrated modified combustion efficiency (MCEFI)—higher MCEFI results in lower ω values and greater spectral dependence of ω (Liu et al GRL 2014). A parameterization of ω as a function of MCEFI for fresh BB aerosols is derived from the laboratory data and is evaluated by field data, including BBOP. Our laboratory studies also demonstrate that BrC production correlates with BC indicating that that they are produced by a common mechanism that is driven by MCEFI (Saleh et al NGeo 2014). We show that BrC absorption is concentrated in the extremely low volatility component that favours long-range transport. We observe substantial absorption enhancement for internally mixed BC from diesel and wood combustion near London during ClearFlo. While the absorption enhancement is due to BC particles coated by co-emitted OC in urban regions, it increases with photochemical age in rural areas and is simulated by core-shell models. We measure BrC absorption that is concentrated in the extremely low volatility components and attribute it to wood burning. Our results support enhanced light absorption by internally mixed BC parameterizations in models and identify mixed biomass and fossil combustion regions where this effect is large. We unify the treatment of carbonaceous aerosol components and their interactions to simplify and verify their representation in climate models, and re-evaluate their direct radiative forcing.

Vertical Distribution of Black and Brown Carbon over Shanghai during Winter

NASA Astrophysics Data System (ADS)

Zheng, M.; Yan, C.; Wang, D.; Fu, Q.

2016-12-01

Carbonaceous aerosols (i.e., black carbon, BC, and organic aerosol, OA) have significant impact on Earth's energy budget by scattering and absorbing solar radiation. Extensive carbonaceous aerosols have been emitted in mainland China. It is essential to study the column burden of carbonaceous aerosol and associated light absorption to better understand its radiative forcing. In this study, a tethered balloon-based field campaign was conducted over a Chinese megacity, Shanghai, in December of 2015, with the primary goal to investigate the vertical profile of air pollutants within the lower troposphere, especially during the polluted days. A 7-wavelength Aethalometer (AE-31) were adopted in the observation to obtain vertical profiles of atmospheric carbonaceous aerosols within the lower troposphere. Light absorption by black and brown carbon, the light absorbing organic components, were distinguished and separated based on difference between light absorption at 450 nm versus 880 nm. Light absorption of brown carbon relative to black carbon were also estimated to pose the importance of brown carbon. Besides, diurnal variation of black and brown carbon vertical profiles would also be discussed, with consideration of variation of height of planetary boundary layer.

Microphysical and optical properties of aerosol particles in urban zone during ESCOMPTE

NASA Astrophysics Data System (ADS)

Mallet, M.; Roger, J. C.; Despiau, S.; Dubovik, O.; Putaud, J. P.

2003-10-01

Microphysical and optical properties of the main aerosol species on a peri-urban site have been investigated during the ESCOMPTE experiment. Ammonium sulfate (AS), nitrate (N), black carbon (BC), particulate organic matter (POM), sea salt (SS) and mineral aerosol (D) size distributions have been used, associated with their refractive index, to compute, from the Mie theory, the key radiative aerosol properties as the extinction coefficient Kext, the mass extinction efficiencies σext, the single scattering albedo ω0 and the asymmetry parameter g at the wavelength of 550 nm. Optical computations show that 90% of the light extinction is due to anthropogenic aerosol and only 10% is due to natural aerosol (SS and D). 44±6% of the extinction is due to (AS) and 40±6% to carbonaceous particles (20±4% to BC and 21±4% to POM). Nitrate aerosol has a weak contribution of 5±2%. Computations of the mass extinction efficiencies σext, single scattering albedo ω0 and asymmetry parameter g indicate that the optical properties of the anthropogenic aerosol are often quite different from those yet published and generally used in global models. For example, the (AS) mean specific mass extinction presents a large difference with the value classically adopted at low relative humidity ( h<60%) (2.6±0.5 instead of 6 m 2 g -1 at 550 nm). The optical properties of the total aerosol layer, including all the aerosol species, indicate a mean observed single-scattering albedo ω0=0.85±0.05, leading to an important absorption of the solar radiation and an asymmetry parameter g=0.59±0.05 which are in a reasonably good agreements with the AERONET retrieval of ω0 (=0.86±0.05) and g (=0.64±0.05) at this wavelength.

Aerosol Forcing of Climate Change and Anomalous Atmospheric Absorption

NASA Technical Reports Server (NTRS)

Hansen, James E.

2000-01-01

The forcings that drive long-term climate change are not known with an accuracy sufficient to define future climate change, Anthropogenic greenhouse gases (GHGs), which are well-measured, cause a strong positive (warming) forcing. But other, poorly measured, anthropogenic forcings, especially changes of atmospheric aerosols, clouds, and land-use patterns, cause a negative forcing that tends to offset greenhouse warming. We will focus on the role of aerosols as a climate forcing mechanism and the contribution that aerosols might make to the so-called "anomalous" atmospheric absorption that has been inferred from some atmospheric measurements.

Aerosol Forcing of Climate Change and "Anomalous" Atmospheric Absorption

NASA Technical Reports Server (NTRS)

Hansen, James E.

1999-01-01

The forcings that drive long-term climate change are not known with an accuracy sufficient to define future climate change. Anthropogenic greenhouse gases (GHGs), which are well-measured, cause a strong positive (warming) forcing. But other, poorly measured, anthropogenic forcings, especially changes of atmospheric aerosols, clouds, and land-use patterns, cause a negative forcing that tends to offset greenhouse warming. We will focus on the role of aerosols as a climate forcing mechanism and the contribution that aerosols might make to the so- called "anomalous" atmospheric absorption that has been inferred from some atmospheric measurements.

Chemical, microphysical and optical properties of the aerosols during foggy and nonfoggy day over a typical location in Indo-Gangetic Plain

NASA Astrophysics Data System (ADS)

Kaul, D. S.; Tripathi, S. N.; Gupta, T.

2012-04-01

An extensive experimental measurement was carried out from January 16, 2010 to February 20, 2010 at Kanpur to study the chemical, microphysical and optical properties of the aerosols. A Micro-Pulse Lidar Network (MPLNET), a part of National Aeronautic Space Administration (NASA), was used for identification of fog duration. PM1 samples and fogwater were collected to examine the organic and inorganic species of aerosol and fogwater. Organic Carbon (OC), Elemental Carbon (EC) and water soluble organic carbon analysis were carried out by an EC-OC analyzer and a TOC analyzer, respectively. Trace gases and solar flux measurement were carried out by gas analyzers and a pyranometer (a part of NASA Aeronet), respectively, to identify the photo-chemical activity. Meteorological data were measured by atmospheric weather station. The microphysical properties such as aerosol size distribution were measured using a scanning mobility particle sizer (SMPS). Optical properties were measured by a photo-acoustic soot spectrometer (PASS). Organic and inorganic species are processed by fog droplets such as production of secondary organic aerosol through aqueous mechanism (Kaul et al., 2011) and scavenging of various water soluble species. The concentrations of almost all the ionic species and organic carbon were higher in aerosols during foggy day. Presence of numerous ionic species and organic carbon in the fogwater indicates their wet scavenging and removal from the atmosphere by the fog droplets. Most of the aerosol is composed of inorganic component, ~80% during foggy day and ~85.5 % during clear day. Biomass burning contribution to PM1 mass concentration was considerably higher during clear days and lower during foggy days; lower concentration during foggy day could be due to wet scavenging of biomass generated aerosols. The study average higher number concentration of aerosol during foggy day during late evening and overnight was due to lower boundary layer height and subsequent accumulation of freshly emitted, previously aged particles in the atmosphere. The increase in both the number concentration and size of the aerosols as fog evaporated was caused by secondary aerosol formation. The fogwater organic and inorganic species and correlation among them indicate that organic and inorganic carbon is highly correlated with almost all the inorganic species. The higher correlation of sulfate and nitrate with organic carbon of fogwater droplets indicates presence of organo-sulfate and organo-nitrate compounds. The study average absorption and scattering coefficient of foggy day aerosols were higher. The formation of secondary organic aerosol during fog evaporation caused increase in scattering coefficient. Details of the finding on chemical, microphysical and optical properties will be presented. Reference: Kaul, D. S., Gupta, T., Tripathi, S. N., Tare, V., and Collett Jr., J. L.: Secondary Organic Aerosol: A comparison between foggy and non-foggy days, Environmental Science & Technology, 45, 7307-7313, 2011

A mobile differential absorption lidar to measure sub-hourly fluctuation of tropospheric ozone profiles in the Baltimore-Washington, D.C. region

NASA Astrophysics Data System (ADS)

Sullivan, J. T.; McGee, T. J.; Sumnicht, G. K.; Twigg, L. W.; Hoff, R. M.

2014-10-01

Tropospheric ozone profiles have been retrieved from the new ground-based National Aeronautics and Space Administration (NASA) Goddard Space Flight Center TROPospheric OZone DIfferential Absorption Lidar (GSFC TROPOZ DIAL) in Greenbelt, MD (38.99° N, 76.84° W, 57 m a.s.l.), from 400 m to 12 km a.g.l. Current atmospheric satellite instruments cannot peer through the optically thick stratospheric ozone layer to remotely sense boundary layer tropospheric ozone. In order to monitor this lower ozone more effectively, the Tropospheric Ozone Lidar Network (TOLNet) has been developed, which currently consists of five stations across the US. The GSFC TROPOZ DIAL is based on the DIAL technique, which currently detects two wavelengths, 289 and 299 nm, with multiple receivers. The transmitted wavelengths are generated by focusing the output of a quadrupled Nd:YAG laser beam (266 nm) into a pair of Raman cells, filled with high-pressure hydrogen and deuterium, using helium as buffer gas. With the knowledge of the ozone absorption coefficient at these two wavelengths, the range-resolved number density can be derived. An interesting atmospheric case study involving the stratospheric-tropospheric exchange (STE) of ozone is shown, to emphasize the regional importance of this instrument as well as to assess the validation and calibration of data. There was a low amount of aerosol aloft, and an iterative aerosol correction has been performed on the retrieved data, which resulted in less than a 3 ppb correction to the final ozone concentration. The retrieval yields an uncertainty of 16-19% from 0 to 1.5 km, 10-18% from 1.5 to 3 km, and 11-25% from 3 to 12 km according to the relevant aerosol concentration aloft. There are currently surface ozone measurements hourly and ozonesonde launches occasionally, but this system will be the first to make routine tropospheric ozone profile measurements in the Baltimore-Washington, D.C. area.

Light Absorption Properties and Radiative Effects of Primary Organic Aerosol Emissions

EPA Science Inventory

Organic aerosols (OA) in the atmosphere affect Earth’s energy budget by not only scattering but also absorbing solar radiation due to the presence of the so-called “brown carbon” (BrC) component. However, the absorptivities of OA are not or poorly represented in current climate m...

Aerosol optical properties retrieved from the future space lidar mission ADM-aeolus

NASA Astrophysics Data System (ADS)

Martinet, Pauline; Flament, Thomas; Dabas, Alain

2018-04-01

The ADM-Aeolus mission, to be launched by end of 2017, will enable the retrieval of aerosol optical properties (extinction and backscatter coefficients essentially) for different atmospheric conditions. A newly developed feature finder (FF) algorithm enabling the detection of aerosol and cloud targets in the atmospheric scene has been implemented. Retrievals of aerosol properties at a better horizontal resolution based on the feature finder groups have shown an improvement mainly on the backscatter coefficient compared to the common 90 km product.

Fast tracking of wind speed with a differential absorption LiDAR system: first results of an experimental campaign at Stromboli volcano

NASA Astrophysics Data System (ADS)

Parracino, Stefano; Santoro, Simone; Maio, Giovanni; Nuvoli, Marcello; Aiuppa, Alessandro; Fiorani, Luca

2017-04-01

Carbon dioxide (CO2) is considered a precursor gas of volcanic eruptions by volcanologists. Monitoring the anomalous release of this parameter, we can retrieve useful information for the mitigation of volcanic hazards, such as for air traffic security. From a dataset collected during the Stromboli volcano field campaign, an assessment of the wind speed, in both horizontal and vertical paths, performing a fast tracking of this parameter was retrieved. This was determined with a newly designed shot-per-shot differential absorption LiDAR system operated in the near-infrared spectral region due to the simultaneous reconstruction of CO2 concentrations and wind speeds, using the same sample of LiDAR returns. A correlation method was used for the wind speed retrieval in which the transport of the spatial inhomogeneities of the aerosol backscattering coefficient, along the optical path of the system, was analyzed.

Dynamic light absorption of biomass-burning organic carbon photochemically aged under natural sunlight

NASA Astrophysics Data System (ADS)

Zhong, M.; Jang, M.

2014-02-01

Wood-burning aerosol produced under smoldering conditions was photochemically aged with different relative humidity (RH) and NOx conditions using a 104 m3 dual outdoor chamber under natural sunlight. Light absorption of organic carbon (OC) was measured over the course of photooxidation using a UV-visible spectrometer connected to an integrating sphere. At high RH, the color decayed rapidly. NOx slightly prolonged the color of wood smoke, suggesting that NOx promotes the formation of chromophores via secondary processes. Overall, the mass absorption cross section (integrated between 280 and 600 nm) of OC increased by 11-54% (except high RH) in the morning and then gradually decreased by 19-68% in the afternoon. This dynamic change in light absorption of wood-burning OC can be explained by two mechanisms: chromophore formation and sunlight bleaching. To investigate the effect of chemical transformation on light absorption, wood smoke particles were characterized using various spectrometers. The intensity of fluorescence, which is mainly related to polycyclic aromatic hydrocarbons (PAHs), rapidly decreased with time, indicating the potential bleaching of PAHs. A decline of levoglucosan concentrations evinced the change of primary organic aerosol with time. The aerosol water content measured by Fourier transform infrared spectroscopy showed that wood-burning aerosol became less hygroscopic as photooxidation proceeded. A similar trend in light absorption changes has been observed in ambient smoke aerosol originating from the 2012 County Line wildfire in Florida. We conclude that the biomass-burning OC becomes less light absorbing after 8-9 h sunlight exposure compared to fresh wood-burning OC.

Simulating Aerosol Optical Properties With the Aerosol Simulation Program (ASP): Closure Studies Using ARCTAS Data

NASA Astrophysics Data System (ADS)

Alvarado, M. J.; Macintyre, H. L.; Bian, H.; Chin, M.; Wang, C.

2012-12-01

The scattering and absorption of ultraviolet and visible radiation by aerosols can significantly alter actinic fluxes and photolysis rates. Accurate modeling of aerosol optical properties is thus essential to simulating atmospheric chemistry, air quality, and climate. Here we evaluate the aerosol optical property predictions of the Aerosol Simulation Program (ASP) with in situ data on aerosol scattering and absorption gathered during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. The model simulations are initialized with in situ data on the aerosol size distribution and composition. We perform a set of sensitivity studies (e.g., internal vs. external mixture, core-in-shell versus Maxwell-Garnett, fraction of the organic carbon mass that is light-absorbing "brown carbon," etc.) to determine the model framework and parameters most consistent with the observations. We compare the ASP results to the aerosol optical property lookup tables in FAST-JX and suggest improvements that will better enable FAST-JX to simulate the impact of aerosols on photolysis rates and atmospheric chemistry.

Small-scale Scheimpflug lidar for aerosol extinction coefficient and vertical atmospheric transmittance detection.

PubMed

Sun, Guodong; Qin, Laian; Hou, Zaihong; Jing, Xu; He, Feng; Tan, Fengfu; Zhang, Silong

2018-03-19

In this paper, a new prototypical Scheimpflug lidar capable of detecting the aerosol extinction coefficient and vertical atmospheric transmittance at 1 km above the ground is described. The lidar system operates at 532 nm and can be used to detect aerosol extinction coefficients throughout an entire day. Then, the vertical atmospheric transmittance can be determined from the extinction coefficients with the equation of numerical integration in this area. CCD flat fielding of the image data is used to mitigate the effects of pixel sensitivity variation. An efficient method of two-dimensional wavelet transform according to a local threshold value has been proposed to reduce the Gaussian white noise in the lidar signal. Furthermore, a new iteration method of backscattering ratio based on genetic algorithm is presented to calculate the aerosol extinction coefficient and vertical atmospheric transmittance. Some simulations are performed to reduce the different levels of noise in the simulated signal in order to test the precision of the de-noising method and inversion algorithm. The simulation result shows that the root-mean-square errors of extinction coefficients are all less than 0.02 km -1 , and that the relative errors of the atmospheric transmittance between the model and inversion data are below 0.56% for all cases. The feasibility of the instrument and the inversion algorithm have also been verified by an optical experiment. The average relative errors of aerosol extinction coefficients between the Scheimpflug lidar and the conventional backscattering elastic lidar are 3.54% and 2.79% in the full overlap heights of two time points, respectively. This work opens up new possibilities of using a small-scale Scheimpflug lidar system for the remote sensing of atmospheric aerosols.

Comparisons of spectral aerosol single scattering albedo in Seoul, South Korea

NASA Astrophysics Data System (ADS)

Mok, Jungbin; Krotkov, Nickolay A.; Torres, Omar; Jethva, Hiren; Li, Zhanqing; Kim, Jhoon; Koo, Ja-Ho; Go, Sujung; Irie, Hitoshi; Labow, Gordon; Eck, Thomas F.; Holben, Brent N.; Herman, Jay; Loughman, Robert P.; Spinei, Elena; Lee, Seoung Soo; Khatri, Pradeep; Campanelli, Monica

2018-04-01

Quantifying aerosol absorption at ultraviolet (UV) wavelengths is important for monitoring air pollution and aerosol amounts using current (e.g., Aura/OMI) and future (e.g., TROPOMI, TEMPO, GEMS, and Sentinel-4) satellite measurements. Measurements of column average atmospheric aerosol single scattering albedo (SSA) are performed on the ground by the NASA AERONET in the visible (VIS) and near-infrared (NIR) wavelengths and in the UV-VIS-NIR by the SKYNET networks. Previous comparison studies have focused on VIS and NIR wavelengths due to the lack of co-incident measurements of aerosol and gaseous absorption properties in the UV. This study compares the SKYNET-retrieved SSA in the UV with the SSA derived from a combination of AERONET, MFRSR, and Pandora (AMP) retrievals in Seoul, South Korea, in spring and summer 2016. The results show that the spectrally invariant surface albedo assumed in the SKYNET SSA retrievals leads to underestimated SSA compared to AMP values at near UV wavelengths. Re-processed SKYNET inversions using spectrally varying surface albedo, consistent with the AERONET retrieval improve agreement with AMP SSA. The combined AMP inversions allow for separating aerosol and gaseous (NO2 and O3) absorption and provide aerosol retrievals from the shortest UVB (305 nm) through VIS to NIR wavelengths (870 nm).

Aerosol scattering and absorption modulation transfer function

NASA Astrophysics Data System (ADS)

Sadot, Dan; Kopeika, Norman S.

1993-08-01

Recent experimental measurements of overall atmospheric modulation transfer function (MTF) indicate significant difference between the turbulence and overall atmospheric MTFs, except often at midday when turbulence is strong. We suggest here a physical explanation for those results which essentially relates to what we call a practical instrumentation-based atmospheric aerosol MTF which is a modification of the classical aerosol MTF theory. It is shown that system field-of-view and dynamic range affect strongly aerosol and overall atmospheric MTFs. It is often necessary to choose between MTF and SNR depending upon dynamic range requirements. Also, a new approach regarding aerosol absorption is presented. It is shown that aerosol-absorbed irradiance is spatial frequency dependent and enhances the degradation in image quality arising from received scattered light. This is most relevant for thermal imaging. An analytically corrected model for the aerosol MTF is presented which is relevant for imaging. An important conclusion is that the aerosol MTF is often the dominant part in the actual overall atmospheric MTF all across the optical spectral region.

Broadband optical properties of biomass-burning aerosol and identification of brown carbon chromophores: OPTICAL AND CHEMICAL PROPERTIES OF BROWN CARBON AEROSOLS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bluvshtein, Nir; Lin, Peng; Flores, J. Michel

The radiative effects of biomass burning aerosols on regional and global scale is substantial. Accurate modeling of the radiative effects of smoke aerosols require wavelength-dependent measurements and parameterizations of their optical properties in the UV and visible spectral ranges along with improved description of their chemical composition. To address this issue, we used a recently developed approach to retrieve the time- and spectral-dependent optical properties of ambient biomass burning aerosols between 300 and 650 nm wavelength during a regional bonfire festival in Israel. During the biomass burning event, the overall absorption at 400 nm increased by about two orders ofmore » magnitude, changing the size-weighted single scattering albedo from a background level of 0.95 to 0.7. Based on the new retrieval method, we provide parameterizations of the wavelength-dependent effective complex refractive index from 350 to 650 nm for freshly emitted and aged biomass burning aerosols. In addition, PM2.5 filter samples were collected for detailed off-line chemical analysis of the water soluble organics that contribute to light absorption. Nitrophenols were identified as the main organic species responsible for the increased absorption at 400-500 nm. These include species such as 4- nitrocatechol, 4-nitrophenol, nitro-syringol and nitro-guaiacol; oxidation-nitration products of methoxyphenols, known products of lignin pyrolysis. Our findings emphasize the importance of both primary and secondary organic aerosol from biomass burning in absorption of solar radiation and in effective radiative forcing.« less

Spectral and Vertical Distribution Properties of Titan's Particulates from Thermal-IR CIRS Data: Physical Implications

NASA Technical Reports Server (NTRS)

Anderson, Carrie M.; Samuelson, Robert; Vinatier, Sandrine

2011-01-01

Analyses of far-IR spectra between 20 and 560/cm (500 and 18 micron) recorded by the Cassini Composite Infrared Spectrometer (CIRS) yield the spectral dependence and the vertical distribution of Titan's photochemical aerosol and stratospheric ice clouds. Below the stratopause (approx. 300 km) the aerosol appears to be incompletely mixed for the following reasons: 1) the altitude dependence of the aerosol mass absorption coefficient is larger at higher altitudes than at lower altitudes, 2} the aerosol scale height varies with altitude, which implies some kind of layering effect, and 3) the aerosol abundance varies with latitude. The spectral shape of the aerosol opacity appears to be independent in altitude and latitude below the stratopause, even though inhomogeneities in the abundance appear to be prevalent throughout this altitude region. This implies that aerosol chemistry is restricted to altitude regions above the stratopause, where pressures are less than approx 0.1 mbar. The aerosol exhibits an extremely broad emisSion feature with a spectral peak at 140/cm (71 micron), which is not evident in laboratory simulated Titan aerosols (tholin) that are created at pressures greater than 0.1 mbar. A strong broad emission feature centered roughly around 160 cm-1 corresponds very closely to those found in nitrile ice spectra. This feature is pervasive throughout the region from high northern to high southern latitudes. The inference of nitrile ices is consistent with the highly restricted altitude ranges over which these features are observed, and appear to be dominated by HCN and HC3N. At low and moderate latitudes these clouds are observed to be located between 60 and 100 km, whereas at high northern latitudes during northern winter these clouds are observed at altitudes between 150 and 165 km. The ubiquitous nature of these nitrile ice clouds is inconsistent with a simple meridional circulation concept, suggesting that the true dynamical situation is more complex.

Sunphotometry of the 2006-2007 aerosol optical/radiative properties at the Himalayan Nepal Climate Observatory-Pyramid (5079 m a.s.l.)

NASA Astrophysics Data System (ADS)

Gobbi, G. P.; Angelini, F.; Bonasoni, P.; Verza, G. P.; Marinoni, A.; Barnaba, F.

2010-11-01

In spite of being located at the heart of the highest mountain range in the world, the Himalayan Nepal Climate Observatory (5079 m a.s.l.) at the Ev-K2-CNR Pyramid is shown to be affected by the advection of pollution aerosols from the populated regions of southern Nepal and the Indo-Gangetic plains. Such an impact is observed along most of the period April 2006-March 2007 addressed here, with a minimum in the monsoon season. Backtrajectory-analysis indicates long-range transport episodes occurring in this year to originate mainly in the west Asian deserts. At this high altitude site, the measured aerosol optical depth is observed to be about one order of magnitude lower than the one measured at Ghandi College (60 m a.s.l.), in the Indo-Gangetic basin. As for Ghandi College, and in agreement with the in situ ground observations at the Pyramid, the fine mode aerosol optical depth maximizes during winter and minimizes in the monsoon season. Conversely, total optical depth maximizes during the monsoon due to the occurrence of elevated, coarse particle layers. Possible origins of these particles are wind erosion from the surrounding peaks and hydrated/cloud-processed aerosols. Assessment of the aerosol radiative forcing is then expected to be hampered by the presence of these high altitude particle layers, which impede an effective, continuous measurement of anthropogenic aerosol radiative properties from sky radiance inversions and/or ground measurements alone. Even though the retrieved absorption coefficients of pollution aerosols were rather large (single scattering albedo of the order of 0.6-0.9 were observed in the month of April 2006), the corresponding low optical depths (~0.03 at 500 nm) are expected to limit the relevant radiative forcing. Still, the high specific forcing of this aerosol and its capability of altering snow surface albedo provide good reasons for continuous monitoring.

Primary and secondary contributions to aerosol light scattering and absorption in Mexico City during the MILAGRO 2006 campaign

NASA Astrophysics Data System (ADS)

Paredes-Miranda, G.; Arnott, W. P.; Jimenez, J. L.; Aiken, A. C.; Gaffney, J. S.; Marley, N. A.

2009-06-01

A photoacoustic spectrometer, a nephelometer, an aethalometer, and an aerosol mass spectrometer were used to measure at ground level real-time aerosol light absorption, scattering, and chemistry at an urban site located in North East Mexico City (Instituto Mexicano del Petroleo, Mexican Petroleum Institute, denoted by IMP), as part of the Megacity Impact on Regional and Global Environments field experiment, MILAGRO, in March 2006. Photoacoustic and reciprocal nephelometer measurements at 532 nm accomplished with a single instrument compare favorably with conventional measurements made with an aethalometer and a TSI nephelometer. The diurnally averaged single scattering albedo at 532 nm was found to vary from 0.60 to 0.85 with the peak value at midday and the minimum value at 07:00 a.m. local time, indicating that the Mexico City plume is likely to have a net warming effect on local climate. The peak value is associated with strong photochemical generation of secondary aerosol. It is estimated that the photochemical production of secondary aerosol (inorganic and organic) is approximately 75% of the aerosol mass concentration and light scattering in association with the peak single scattering albedo. A strong correlation of aerosol scattering at 532 nm and total aerosol mass concentration was found, and an average mass scattering efficiency factor of 3.8 m2/g was determined. Comparisons of photoacoustic and aethalometer light absorption with oxygenated organic aerosol concentration (OOA) indicate a very small systematic bias of the filter based measurement associated with OOA and the peak aerosol single scattering albedo.

Primary and secondary contributions to aerosol light scattering and absorption in Mexico City during the MILAGRO 2006 campaign

NASA Astrophysics Data System (ADS)

Paredes-Miranda, G.; Arnott, W. P.; Jimenez, J. L.; Aiken, A. C.; Gaffney, J. S.; Marley, N. A.

2008-09-01

A photoacoustic spectrometer, a nephelometer, an aetholemeter, and an aerosol mass spectrometer were used to measure at ground level real-time aerosol light absorption, scattering, and chemistry at an urban site located in north east Mexico City (Instituto Mexicano del Petroleo, Mexican Petroleum Institute, denoted by IMP), as part of the Megacity Impact on Regional and Global Environments field experiment, MILAGRO, in March 2006. Photoacoustic and reciprocal nephelometer measurements at 532 nm accomplished with a single instrument compare favorably with conventional measurements made with an aethelometer and a TSI nephelometer. The diurnally averaged single scattering albedo at 532 nm was found to vary from 0.60 to 0.85 with the peak value at midday and the minimum value at 7 a.m. local time, indicating that the Mexico City plume is likely to have a net warming effect on local climate. The peak value is associated with strong photochemical generation of secondary aerosol. It is estimated that the same-day photochemical production of secondary aerosol (inorganic and organic) is approximately 40 percent of the aerosol mass concentration and light scattering in association with the peak single scattering albedo. A strong correlation of aerosol scattering at 532 nm and total aerosol mass concentration was found, and an average mass scattering efficiency factor of 3.8 m2/g was determined. Comparisons of photoacoustic and aethalometer light absorption with oxygenated organic aerosol concentration (OOA) indicate a very small systematic bias of the filter based measurement associated with OOA and the peak aerosol single scattering albedo.

Spatial Representativeness Error in the Ground-Level Observation Networks for Black Carbon Radiation Absorption

NASA Astrophysics Data System (ADS)

Wang, Rong; Andrews, Elisabeth; Balkanski, Yves; Boucher, Olivier; Myhre, Gunnar; Samset, Bjørn Hallvard; Schulz, Michael; Schuster, Gregory L.; Valari, Myrto; Tao, Shu

2018-02-01

There is high uncertainty in the direct radiative forcing of black carbon (BC), an aerosol that strongly absorbs solar radiation. The observation-constrained estimate, which is several times larger than the bottom-up estimate, is influenced by the spatial representativeness error due to the mesoscale inhomogeneity of the aerosol fields and the relatively low resolution of global chemistry-transport models. Here we evaluated the spatial representativeness error for two widely used observational networks (AErosol RObotic NETwork and Global Atmosphere Watch) by downscaling the geospatial grid in a global model of BC aerosol absorption optical depth to 0.1° × 0.1°. Comparing the models at a spatial resolution of 2° × 2° with BC aerosol absorption at AErosol RObotic NETwork sites (which are commonly located near emission hot spots) tends to cause a global spatial representativeness error of 30%, as a positive bias for the current top-down estimate of global BC direct radiative forcing. By contrast, the global spatial representativeness error will be 7% for the Global Atmosphere Watch network, because the sites are located in such a way that there are almost an equal number of sites with positive or negative representativeness error.

Polarization lidar for atmospheric monitoring

NASA Astrophysics Data System (ADS)

Liu, Qiaojun; Wu, Chengxuan; Yuk Sun Cheng, Andrew; Wang, Zhangjun; Meng, Xiangqian; Chen, Chao; Li, Xianxin; Liu, Xingtao; Zhang, Hao; Zong, Fangyi

2018-04-01

Aerosol plays an important role in global climate and weather changes. Polarization lidar captures parallel and perpendicular signals from atmosphere to research aerosols. The lidar system we used has three emission wavelengths and could obtain the atmospheric aerosol extinction coefficient, backscattering coefficient and depolarization ratio. In this paper, the design of the lidar is described. The methods of data acquisition and inversion are given. Some recent results are presented.

GOCI Yonsei Aerosol Retrieval (YAER) algorithm and validation during the DRAGON-NE Asia 2012 campaign

NASA Astrophysics Data System (ADS)

Choi, Myungje; Kim, Jhoon; Lee, Jaehwa; Kim, Mijin; Park, Young-Je; Jeong, Ukkyo; Kim, Woogyung; Hong, Hyunkee; Holben, Brent; Eck, Thomas F.; Song, Chul H.; Lim, Jae-Hyun; Song, Chang-Keun

2016-04-01

The Geostationary Ocean Color Imager (GOCI) onboard the Communication, Ocean, and Meteorological Satellite (COMS) is the first multi-channel ocean color imager in geostationary orbit. Hourly GOCI top-of-atmosphere radiance has been available for the retrieval of aerosol optical properties over East Asia since March 2011. This study presents improvements made to the GOCI Yonsei Aerosol Retrieval (YAER) algorithm together with validation results during the Distributed Regional Aerosol Gridded Observation Networks - Northeast Asia 2012 campaign (DRAGON-NE Asia 2012 campaign). The evaluation during the spring season over East Asia is important because of high aerosol concentrations and diverse types of Asian dust and haze. Optical properties of aerosol are retrieved from the GOCI YAER algorithm including aerosol optical depth (AOD) at 550 nm, fine-mode fraction (FMF) at 550 nm, single-scattering albedo (SSA) at 440 nm, Ångström exponent (AE) between 440 and 860 nm, and aerosol type. The aerosol models are created based on a global analysis of the Aerosol Robotic Networks (AERONET) inversion data, and covers a broad range of size distribution and absorptivity, including nonspherical dust properties. The Cox-Munk ocean bidirectional reflectance distribution function (BRDF) model is used over ocean, and an improved minimum reflectance technique is used over land. Because turbid water is persistent over the Yellow Sea, the land algorithm is used for such cases. The aerosol products are evaluated against AERONET observations and MODIS Collection 6 aerosol products retrieved from Dark Target (DT) and Deep Blue (DB) algorithms during the DRAGON-NE Asia 2012 campaign conducted from March to May 2012. Comparison of AOD from GOCI and AERONET resulted in a Pearson correlation coefficient of 0.881 and a linear regression equation with GOCI AOD = 1.083 × AERONET AOD - 0.042. The correlation between GOCI and MODIS AODs is higher over ocean than land. GOCI AOD shows better agreement with MODIS DB than MODIS DT. The other GOCI YAER products (AE, FMF, and SSA) show lower correlation with AERONET than AOD, but still show some skills for qualitative use.

GOCI Yonsei Aerosol Retrieval (YAER) Algorithm and Validation During the DRAGON-NE Asia 2012 Campaign

NASA Technical Reports Server (NTRS)

Choi, Myungje; Kim, Jhoon; Lee, Jaehwa; Kim, Mijin; Park, Young-Je; Jeong, Ukkyo; Kim, Woogyung; Hong, Hyunkee; Holben, Brent; Eck, Thomas F.;

Characterization and Scaling of Black Carbon Aerosol Concentration with City Population Based on In-Situ Measurements and Analysis

NASA Astrophysics Data System (ADS)

Paredes-Miranda, G.; Arnott, W. P.; Moosmuller, H.

2010-12-01

The global trend toward urbanization and the resulting increase in city population has directed attention toward air pollution in megacities. A closely related question of importance for urban planning and attainment of air quality standards is how pollutant concentrations scale with city population. In this study, we use measurements of light absorption and light scattering coefficients as proxies for primary (i.e., black carbon; BC) and total (i.e., particulate matter; PM) pollutant concentration, to start addressing the following questions: What patterns and generalizations are emerging from our expanding data sets on urban air pollution? How does the per-capita air pollution vary with economic, geographic, and meteorological conditions of an urban area? Does air pollution provide an upper limit on city size? Diurnal analysis of black carbon concentration measurements in suburban Mexico City, Mexico, Las Vegas, NV, USA, and Reno, NV, USA for similar seasons suggests that commonly emitted primary air pollutant concentrations scale approximately as the square root of the urban population N, consistent with a simple 2-d box model. The measured absorption coefficient Babs is approximately proportional to the BC concentration (primary pollution) and thus scales with the square root of population (N). Since secondary pollutants form through photochemical reactions involving primary pollutants, they scale also with square root of N. Therefore the scattering coefficient Bsca, a proxy for PM concentration is also expected to scale with square root of N. Here we present light absorption and scattering measurements and data on meteorological conditions and compare the population scaling of these pollutant measurements with predictions from the simple 2-d box model. We find that these basin cities are connected by the square root of N dependence. Data from other cities will be discussed as time permits.

Diurnal Cycles of Aerosol Optical Properties at Pico Tres Padres, Mexico City: Evidences for Changes in Particle Morphology and Secondary Aerosol Formation

NASA Astrophysics Data System (ADS)

Mazzoleni, C.; Dubey, M.; Chakrabarty, R.; Moosmuller, H.; Onasch, T.; Zavala, M.; Herndon, S.; Kolb, C.

2007-12-01

Aerosol optical properties affect planetary radiative balance and depend on chemical composition, size distribution, and morphology. During the MILAGRO field campaign, we measured aerosol absorption and scattering in Mexico City using the Los Alamos aerosol photoacoustic (LAPA) instrument operating at 781 nm. The LAPA was mounted on-board the Aerodyne Research Inc. mobile laboratory, which hosted a variety of gaseous and aerosol instruments. During the campaign, the laboratory was moved to different sites, capturing spatial and temporal variability. Additionally, we collected ambient aerosols on Nuclepore filters for scanning electron microscopy (SEM) analysis. SEM images of selected filters were taken to study particle morphology. Between March 7th and 19th air was sampled at the top of Pico Tres Padres, a mountain on the north side of Mexico City. Aerosol absorption and scattering followed diurnal patterns related to boundary layer height and solar insulation. We report an analysis of aerosol absorption, scattering, and morphology for three days (9th, 11th and 12th of March 2006). The single scattering albedo (SSA, ratio of scattering to total extinction) showed a drop in the tens-of-minutes-to-hour time frame after the boundary layer grew above the sampling site. Later in the day the SSA rose steadily reaching a maximum in the afternoon. The SEM images showed a variety of aerosol shapes including fractal-like aggregates, spherical particles, and other shapes. The absorption correlated with the CO2 signal and qualitatively with the fraction of fractal-like particles to the total particle count. In the afternoon the SSA qualitatively correlated with a relative increase in spherical particles and total particle count. These observed changes in optical properties and morphology can be explained by the dominant contribution of freshly emitted particles in the morning and by secondary particle formation in the afternoon. SSA hourly averaged values ranged from ~0.63 in the morning to ~0.83 in the afternoon/night, indicating light absorbing aerosols, which have a large impact on radiative forcing.

Remote sensing of soot carbon - Part 2: Understanding the absorption Ångström exponent

NASA Astrophysics Data System (ADS)

Schuster, G. L.; Dubovik, O.; Arola, A.; Eck, T. F.; Holben, B. N.

2016-02-01

Recently, some authors have suggested that the absorption Ångström exponent (AAE) can be used to deduce the component aerosol absorption optical depths (AAODs) of carbonaceous aerosols in the AERONET database. This AAE approach presumes that AAE ≪ 1 for soot carbon, which contrasts the traditional small particle limit of AAE = 1 for soot carbon. Thus, we provide an overview of the AERONET retrieval, and we investigate how the microphysics of carbonaceous aerosols can be interpreted in the AERONET AAE product. We find that AAE ≪ 1 in the AERONET database requires large coarse mode fractions and/or imaginary refractive indices that increase with wavelength. Neither of these characteristics are consistent with the current definition of soot carbon, so we explore other possibilities for the cause of AAE ≪ 1. AAE is related to particle size, and coarse mode particles have a smaller AAE than fine mode particles for a given aerosol mixture of species. We also note that the mineral goethite has an imaginary refractive index that increases with wavelength, is very common in dust regions, and can easily contribute to AAE ≪ 1. We find that AAE ≪ 1 can not be caused by soot carbon, unless soot carbon has an imaginary refractive index that increases with wavelength throughout the visible and near-infrared spectrums. Finally, AAE is not a robust parameter for separating carbonaceous absorption from dust aerosol absorption in the AERONET database.

Absorption and Clearance of Pharmaceutical Aerosols in the Human Nose: Effects of Nasal Spray Suspension Particle Size and Properties.

PubMed

Rygg, Alex; Hindle, Michael; Longest, P Worth

2016-04-01

The objective of this study was to use a recently developed nasal dissolution, absorption, and clearance (DAC) model to evaluate the extent to which suspended drug particle size influences nasal epithelial drug absorption for a spray product. Computational fluid dynamics (CFD) simulations of mucociliary clearance and drug dissolution were used to calculate total and microscale epithelial absorption of drug delivered with a nasal spray pump. Ranges of suspended particle sizes, drug solubilities, and partition coefficients were evaluated. Considering mometasone furoate as an example, suspended drug particle sizes in the range of 1-5 μm did not affect the total nasal epithelial uptake. However, the microscale absorption of suspended drug particles with low solubilities was affected by particle size and this controlled the extent to which the drug penetrated into the distal nasal regions. The nasal-DAC model was demonstrated to be a useful tool in determining the nasal exposure of spray formulations with different drug particle sizes and solubilities. Furthermore, the model illustrated a new strategy for topical nasal drug delivery in which drug particle size is selected to increase the region of epithelial surface exposure using mucociliary clearance while minimizing the drug dose exiting the nasopharynx.

Aethalometer

DOEpatents

Hansen, Anthony D.

1990-01-01

An improved aethalometer (10) having a single light source (18) and a single light detector (20) and two light paths (21, 22) from the light source (18) to the light detector (20). A quartz fiber filter (13) is inserted in the device, the filter (13) having a collection area (23) in one light path (21) and a reference area (24) in the other light path (22). A gas flow path (46) through the aethalometer housing (11) allows ambient air to flow through the collection area (23) of the filter (13) so that aerosol particles can be collected on the filter. A rotating disk (31) with an opening (33) therethrough allows light for the light source (18) to pass alternately through the two light paths (21, 22). The voltage output of the detector (20) is applied to a VCO (52) and the VCO pulses for light transmission separately through the two light paths (21, 22 ) are counted and compared to determine the absorption coefficient of the collected aerosol particles.

Enhanced UV Absorption in Carbonaceous Aerosols during MILAGRO and Identification of Potential Organic Contributors.

NASA Astrophysics Data System (ADS)

Mangu, A.; Kelley, K. L.; Marchany-Rivera, A.; Kilaparty, S.; Gunawan, G.; Gaffney, J. S.; Marley, N. A.

2007-12-01

Measurements of aerosol absorption were obtained as part of the MAX-Mex component of the MILAGRO field campaign at site T0 (Instituto Mexicano de Petroleo in Mexico City) during the month of March, 2006 by using a 7- channel aethalometer (Thermo-Anderson). These measurements, obtained at 370, 470, 520, 590, 660, 880, and 950 nm at a 5 minute time resolution, showed an enhanced absorption in the UV over that expected from carbon soot alone. Samples of fine atmospheric aerosols (less than 0.1micron) were also collected at site T0 and T1 (Universidad Technologica de Tecamac, State of Mexico) from 5 am to 5 pm (day) and from 5 pm to 5 am (night) during the month of March 2006. The samples were collected on quartz fiber filters with high volume impactor samplers. The samples have been characterized for total carbon content (stable isotope ratio mass spectroscopy) and natural radionuclide tracers (210Pb, 210Po, 210Bi, 7Be, 13C, 14C, 40K, 15N). Continuous absorption spectra of these aerosol samples have been obtained in the laboratory from 280 to 900nm with the use of an integrating sphere coupled to a UV-visible spectrometer (Beckman DU with a Labsphere accessory). The integrating sphere allows the detector to collect and spatially integrate the total radiant flux reflected from the sample and therefore allows for the measurement of absorption on highly reflective or diffusely scattering samples (1). The continuous spectra also show an enhanced UV absorption over that expected from carbon soot and the general profiles are quite similar to those observed for humic and fulvic acids found as colloidal materials in surface and groundwaters (2), indicating the presence of humic-like substances (HULIS) in the fine aerosols. The spectra also show evidence of narrow band absorbers below 400 nm typical of polycyclic aromatics (PAH) and nitrated aromatic compounds. Spectra were also obtained on NIST standard diesel soot (SRM 2975), NIST standard air particulate matter (SRM 8785), and nitrated PAH compounds for comparison. Potential organic aerosol components are identified which contribute to the enhanced absorption observed in the field. The wavelength dependence of the mass specific absorption is obtained from these spectra and total carbon measurements. The wavelength dependence of the aerosol complex refractive index (m = n +ik) in the UV-visible spectral region is determined by application of the Kramers Kronig function. The importance of the aerosol absorption in the infrared spectral region to radiative forcing will be discussed. 1. Marley, N.A., J.S. Gaffney, J.C. Baird, C.A. Blazer, P.J. Drayton, and J.E. Frederick, Aerosol Sci. Technol., 34, 535-549, (2001). 2. N.A. Marley, J.S. Gaffney, and K.A. Orlandini, Chapter 7 in Humic/Fulvic Acids and Organic Colloidal Materials in the Environment, ACS Symposium Series 651, American Chemical Society, Washington, D.C., pp. 96-107, 1996. This work was conducted as part of the Department of Energy's Atmospheric Science Program as part of the Megacity Aerosol Experiment - Mexico City during MILAGRO. This research was supported by the Office of Science (BER), U.S. Department of Energy Grant No. DE-FG02-07ER64329. We also wish to thank Mexican Scientists and students for their assistance from the Instituto Mexicano de Petroleo (IMP) and CENICA.

Broadband optical properties of biomass-burning aerosol and identification of brown carbon chromophores

NASA Astrophysics Data System (ADS)

Bluvshtein, Nir; Lin, Peng; Flores, J. Michel; Segev, Lior; Mazar, Yinon; Tas, Eran; Snider, Graydon; Weagle, Crystal; Brown, Steven S.; Laskin, Alexander; Rudich, Yinon

2017-05-01

The radiative effects of biomass-burning aerosols on regional and global scales can be substantial. Accurate modeling of the radiative effects of smoke aerosols requires wavelength-dependent measurements and parameterizations of their optical properties in the UV and visible spectral ranges along with improved description of their chemical composition. To address this issue, we used a recently developed approach to retrieve the time- and spectral-dependent optical properties of ambient biomass-burning aerosols from 300 to 650 nm wavelengths during a regional nighttime bonfire festival in Israel. During the biomass burning event, the overall absorption at 400 nm increased by about 2 orders of magnitude, changing the single scattering albedo from a background level of 0.95 to 0.7. Based on the new retrieval method, we provide parameterizations of the wavelength-dependent effective complex refractive index from 350 to 650 nm for freshly emitted and slightly aged biomass-burning aerosols. In addition, PM2.5 filter samples were collected for detailed offline chemical analysis of the water-soluble organics that contribute to light absorption. Nitroaromatics were identified as major organic species responsible for the increased absorption at 400 to 500 nm. Typical chromophores include 4-nitrocatechol, 4-nitrophenol, nitrosyringol, and nitroguaiacol; oxidation-nitration products of methoxyphenols; and known products of lignin pyrolysis. Our findings emphasize the importance of both primary and secondary organic aerosols from biomass burning in absorption of solar radiation and in effective radiative forcing.

Aerosol characteristics inversion based on the improved lidar ratio profile with the ground-based rotational Raman-Mie lidar

NASA Astrophysics Data System (ADS)

Ji, Hongzhu; Zhang, Yinchao; Chen, Siying; Chen, He; Guo, Pan

2018-06-01

An iterative method, based on a derived inverse relationship between atmospheric backscatter coefficient and aerosol lidar ratio, is proposed to invert the lidar ratio profile and aerosol extinction coefficient. The feasibility of this method is investigated theoretically and experimentally. Simulation results show the inversion accuracy of aerosol optical properties for iterative method can be improved in the near-surface aerosol layer and the optical thick layer. Experimentally, as a result of the reduced insufficiency error and incoherence error, the aerosol optical properties with higher accuracy can be obtained in the near-surface region and the region of numerical derivative distortion. In addition, the particle component can be distinguished roughly based on this improved lidar ratio profile.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hopkins, Rebecca J.; Lewis, K.; Desyaterik, Yury

Aerosols generated from burning different plant fuels were characterized to determine relationships between chemical, optical and physical properties. Single scattering albedo ({omega}) and Angstrom absorption coefficients ({alpha}{sub ap}) were measured using a photoacoustic technique combined with a reciprocal nephelometer. Carbon-to-oxygen atomic ratios, sp{sup 2} hybridization, elemental composition and morphology of individual particles were measured using scanning transmission X-ray microscopy coupled with near-edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS) and scanning electron microscopy with energy dispersion of X-rays (SEM/EDX). Particles were grouped into three categories based on sp2 hybridization and chemical composition. Measured {omega} (0.4-1.0 at 405 nm) and {alpha}{sub ap}more » (1.0-3.5) values displayed a fuel dependence. The category with sp{sup 2} hybridization >80% had values of {omega} (<0.5) and {alpha}{sub ap} ({approx}1.25) characteristic of light absorbing soot. Other categories with lower sp2 hybridization (20 to 60%) exhibited higher {omega} (>0.8) and {alpha}{sub ap} (1.0 to 3.5) values, indicating increased absorption spectral selectivity.« less

Measurement of phase function of aerosol at different altitudes by CCD Lidar

NASA Astrophysics Data System (ADS)

Sun, Peiyu; Yuan, Ke'e.; Yang, Jie; Hu, Shunxing

2018-02-01

The aerosols near the ground are closely related to human health and climate change, the study on which has important significance. As we all know, the aerosol is inhomogeneous at different altitudes, of which the phase function is also different. In order to simplify the retrieval algorithm, it is usually assumed that the aerosol is uniform at different altitudes, which will bring measurement error. In this work, an experimental approach is demonstrated to measure the scattering phase function of atmospheric aerosol particles at different heights by CCD lidar system, which could solve the problem of the traditional CCD lidar system in assumption of phase function. The phase functions obtained by the new experimental approach are used to retrieve the aerosol extinction coefficient profiles. By comparison of the aerosol extinction coefficient retrieved by Mie-scattering aerosol lidar and CCD lidar at night, the reliability of new experimental approach is verified.

Molecular-Size-Separated Brown Carbon Absorption for Biomass-Burning Aerosol at Multiple Field Sites.

PubMed

Di Lorenzo, Robert A; Washenfelder, Rebecca A; Attwood, Alexis R; Guo, Hongyu; Xu, Lu; Ng, Nga L; Weber, Rodney J; Baumann, Karsten; Edgerton, Eric; Young, Cora J

2017-03-21

Biomass burning is a known source of brown carbon aerosol in the atmosphere. We collected filter samples of biomass-burning emissions at three locations in Canada and the United States with transport times of 10 h to >3 days. We analyzed the samples with size-exclusion chromatography coupled to molecular absorbance spectroscopy to determine absorbance as a function of molecular size. The majority of absorption was due to molecules >500 Da, and these contributed an increasing fraction of absorption as the biomass-burning aerosol aged. This suggests that the smallest molecular weight fraction is more susceptible to processes that lead to reduced light absorption, while larger-molecular-weight species may represent recalcitrant brown carbon. We calculate that these large-molecular-weight species are composed of more than 20 carbons with as few as two oxygens and would be classified as extremely low volatility organic compounds (ELVOCs).

Comparison of AOD, AAOD and column single scattering albedo from AERONET retrievals and in situ profiling measurements

NASA Astrophysics Data System (ADS)

Andrews, Elisabeth; Ogren, John A.; Kinne, Stefan; Samset, Bjorn

2017-05-01

Here we present new results comparing aerosol optical depth (AOD), aerosol absorption optical depth (AAOD) and column single scattering albedo (SSA) obtained from in situ vertical profile measurements with AERONET ground-based remote sensing from two rural, continental sites in the US. The profiles are closely matched in time (within ±3 h) and space (within 15 km) with the AERONET retrievals. We have used Level 1.5 inversion retrievals when there was a valid Level 2 almucantar retrieval in order to be able to compare AAOD and column SSA below AERONET's recommended loading constraint (AOD > 0.4 at 440 nm). While there is reasonable agreement for the AOD comparisons, the direct comparisons of in situ-derived to AERONET-retrieved AAOD (or SSA) reveal that AERONET retrievals yield higher aerosol absorption than obtained from the in situ profiles for the low aerosol optical depth conditions prevalent at the two study sites. However, it should be noted that the majority of SSA comparisons for AOD440 > 0.2 are, nonetheless, within the reported SSA uncertainty bounds. The observation that, relative to in situ measurements, AERONET inversions exhibit increased absorption potential at low AOD values is generally consistent with other published AERONET-in situ comparisons across a range of locations, atmospheric conditions and AOD values. This systematic difference in the comparisons suggests a bias in one or both of the methods, but we cannot assess whether the AERONET retrievals are biased towards high absorption or the in situ measurements are biased low. Based on the discrepancy between the AERONET and in situ values, we conclude that scaling modeled black carbon concentrations upwards to match AERONET retrievals of AAOD should be approached with caution as it may lead to aerosol absorption overestimates in regions of low AOD. Both AERONET retrievals and in situ measurements suggest there is a systematic relationship between SSA and aerosol amount (AOD or aerosol light scattering) - specifically that SSA decreases at lower aerosol loading. This implies that the fairly common assumption that AERONET SSA values retrieved at high-AOD conditions can be used to obtain AAOD at low-AOD conditions may not be valid.

Light absorption properties of brown carbon over the southeastern Tibetan Plateau.

PubMed

Zhu, Chong-Shu; Cao, Jun-Ji; Huang, Ru-Jin; Shen, Zhen-Xing; Wang, Qi-Yuan; Zhang, Ning-Ning

2018-06-01

We present a study of the light-absorbing properties of water-soluble brown carbon (WS-BrC) and methanol-soluble brown carbon (MeS-BrC) at a remote site (Lulang, 3326m above sea level) in the southeastern Tibetan Plateau during the period 2015-2016. The light absorption coefficients at 365nm (b abs365 ) of WS-BrC and MeS-BrC were the highest during winter and the lowest during monsoon season. MeS-BrC absorbs about 1.5 times higher at 365nm compared to WS-BrC. The absorption at 550nm appears lower compared to that of 365nm for WS-BrC and MeS-BrC, respectively. Higher average value of the absorption Ångström exponent (AAE, 365-550nm) was obtained for MeS-BrC (8.2) than that for WS-BrC (6.9). The values of the mass absorption cross section at 365nm (MAC 365 ) indicated that BrC in winter absorbs UV-visible light more efficiently than in monsoon. The results confirm the importance of BrC in contributing to light-absorbing aerosols in this region. The understanding of the light absorption properties of BrC is of great importance, especially in modeling studies for the climate effects and transport of BrC in the Tibetan Plateau. Copyright © 2017 Elsevier B.V. All rights reserved.

Effects of morphology on the radiative properties of internally mixed light absorbing carbon aerosols with different aging status.

PubMed

Cheng, Tianhai; Wu, Yu; Chen, Hao

2014-06-30

Light absorbing carbon aerosols play a substantial role in climate change through radiative forcing, which is the dominant absorber of solar radiation. Radiative properties of light absorbing carbon aerosols are strongly dependent on the morphological factors and the mixing mechanism of black carbon with other aerosol components. This study focuses on the morphological effects on the optical properties of internally mixed light absorbing carbon aerosols using the numerically exact superposition T-matrix method. Three types aerosols with different aging status such as freshly emitted BC particles, thinly coated light absorbing carbon aerosols, heavily coated light absorbing carbon aerosols are studied. Our study showed that morphological factors change with the aging of internally mixed light absorbing carbon aerosols to result in a dramatic change in their optical properties. The absorption properties of light absorbing carbon aerosols can be enhanced approximately a factor of 2 at 0.67 um, and these enhancements depend on the morphological factors. A larger shell/core diameter ratio of volume-equivalent shell-core spheres (S/C), which indicates the degree of coating, leads to stronger absorption. The enhancement of absorption properties accompanies a greater enhancement of scattering properties, which is reflected in an increase in single scattering albedo (SSA). The enhancement of single scattering albedo due to the morphological effects can reach a factor of 3.75 at 0.67 μm. The asymmetry parameter has a similar yet smaller enhancement. Moreover, the corresponding optical properties of shell-and-core model determined by using Lorenz -Mie solutions are presented for comparison. We found that the optical properties of internally mixed light absorbing carbon aerosol can differ fundamentally from those calculated for the Mie theory shell-and-core model, particularly for thinly coated light absorbing carbon aerosols. Our studies indicate that the complex morphology of internally mixed light absorbing carbon aerosols must be explicitly considered in climate radiation balance.

Control of PM2.5 in Guangzhou during the 16th Asian Games period: implication for hazy weather prevention.

PubMed

Tao, Jun; Zhang, Leiming; Zhang, Zhisheng; Huang, Ruijin; Wu, Yunfei; Zhang, Renjian; Cao, Junji; Zhang, Yuanhang

2015-03-01

To evaluate the effectiveness of the integrated control measures for reducing PM2.5 (aerosol particles with an aerodynamic diameter of less than 2.5 μm) and hazy weather, day- and night-time PM2.5 samples were collected at an urban site in Guangzhou during the 16th Asian Games period in November 2010. PM2.5 samples were subject to chemical analysis for major water-soluble ions, organic carbon (OC), element carbon (EC), and biomass burning tracers-anhydrosugar levoglucosan (LG). In addition, aerosol scattering coefficient (bsp) at dry condition and aerosol absorption coefficient (bap) and visibility at ambient condition were measured. The seven major control measures were effective for reducing PM2.5 mass concentration and improving visibility during the Asian Games period. All monitored air pollutants except PM2.5 satisfied the National Ambient Air Quality Standards (NAAQS). However, daily PM2.5 concentrations still exceeded the NAAQS on 47% of the days and hazy weather also occurred on 80% of the days during this period. One factor causing the high frequency of hazy weather occurrence was the increased relative humidity during the Asian Games period. To avoid hazy weather occurrence, new PM2.5 standard was recommended based on visibility calculations using three available aerosol hygroscopic curves previously obtained for this city. The recommended PM2.5 standard was 63 μgm(-3) under dry condition and lower than 42 μg m(-3) under humid condition (RH ≥ 70%). These recommended value s were much stricter than the NAAQS value of 75 μg m(-3). To reach the new standard, more rigorous control measures for coal industries should be established in the Pearl River Delta (PRD) region. Copyright © 2014 Elsevier B.V. All rights reserved.

Comparisons of Spectral Aerosol Single Scattering Albedo in Seoul, South Korea

NASA Technical Reports Server (NTRS)

Mok, Jungbin; Krotkov, Nickolay A.; Torres, Omar; Jethva, Hiren; Loughman, Robert P.; Spinei, Elena; Campanelli, Monica; Li, Zhanqing; Go, Sujung; Labow, Gordon;

The Impact of Atmospheric Aerosols on the Fraction of absorbed Photosynthetically Active Radiation

NASA Astrophysics Data System (ADS)

Veroustraete, Frank

2010-05-01

Aerosol pollution attracts a growing interest from atmospheric scientists with regard to their impact on health, the global climate and vegetation stress. A hypothesis, less investigated, is whether atmospheric aerosol interactions in the solar radiation field affect the amount of radiation absorbed by vegetation canopies and hence terrestrial vegetation productivity. Typically, aerosols affect vegetation canopy radiation absorption efficiency by altering the physical characteristics of solar radiation incoming on for example a forest canopy. It has been illustrated, that increasing mixing ratio's of atmospheric particulate matter lead to a higher fraction of diffuse sunlight as opposed to direct sunlight. It can be demonstrated, based on the application of atmospheric (MODTRAN) and leaf/canopy radiative transfer (LIBERTY/SPRINT) models, that radiation absorption efficiency in the PAR band of Picea like forests increases with increasing levels of diffuse radiation. It can be documented - on a theoretical basis - as well, that increasing aerosol loads in the atmosphere, induce and increased canopy PAR absorption efficiency. In this paper it is suggested, that atmospheric aerosols have to be taken into account when estimating vegetation gross primary productivity (GPP). The results suggest that Northern hemisphere vegetation CO2 uptake magnitude may increase with increasing atmospheric aerosol loads. Many climate impact scenario's related to vegetation productivity estimates, do not take this phenomenon into account. Boldly speaking, the results suggest a larger sink function for terrestrial vegetation than generally accepted. Keywords: Aerosols, vegetation, fAPAR, CO2 uptake, diffuse radiation.

Assessment of biomass burning smoke influence on environmental conditions for multi-year tornado outbreaks by combining aerosol-aware microphysics and fire emission constraints.

PubMed

Saide, Pablo E; Thompson, Gregory; Eidhammer, Trude; da Silva, Arlindo M; Pierce, R Bradley; Carmichael, Gregory R

2016-09-16

We use the WRF system to study the impacts of biomass burning smoke from Central America on several tornado outbreaks occurring in the US during spring. The model is configured with an aerosol-aware microphysics parameterization capable of resolving aerosol-cloud-radiation interactions in a cost-efficient way for numerical weather prediction (NWP) applications. Primary aerosol emissions are included and smoke emissions are constrained using an inverse modeling technique and satellite-based AOD observations. Simulations turning on and off fire emissions reveal smoke presence in all tornado outbreaks being studied and show an increase in aerosol number concentrations due to smoke. However, the likelihood of occurrence and intensification of tornadoes is higher due to smoke only in cases where cloud droplet number concentration in low level clouds increases considerably in a way that modifies the environmental conditions where the tornadoes are formed (shallower cloud bases and higher low-level wind shear). Smoke absorption and vertical extent also play a role, with smoke absorption at cloud-level tending to burn-off clouds and smoke absorption above clouds resulting in an increased capping inversion. Comparing these and WRF-Chem simulations configured with a more complex representation of aerosol size and composition and different optical properties, microphysics and activation schemes, we find similarities in terms of the simulated aerosol optical depths and aerosol impacts on near-storm environments. This provides reliability on the aerosol-aware microphysics scheme as a less computationally expensive alternative to WRF-Chem for its use in applications such as NWP and cloud-resolving simulations.

Assessment of Biomass Burning Smoke Influence on Environmental Conditions for Multi-Year Tornado Outbreaks by Combining Aerosol-Aware Microphysics and Fire Emission Constraints

NASA Technical Reports Server (NTRS)

Saide, Pablo E.; Thompson, Gregory; Eidhammer, Trude; Da Silva, Arlindo M.; Pierce, R. Bradley; Carmichael, Gregory R.

2016-01-01

We use the WRF system to study the impacts of biomass burning smoke from Central America on several tornado outbreaks occurring in the US during spring. The model is configured with an aerosol-aware microphysics parameterization capable of resolving aerosol-cloud-radiation interactions in a cost-efficient way for numerical weather prediction (NWP) applications. Primary aerosol emissions are included and smoke emissions are constrained using an inverse modeling technique and satellite-based AOD observations. Simulations turning on and off fire emissions reveal smoke presence in all tornado outbreaks being studied and show an increase in aerosol number concentrations due to smoke. However, the likelihood of occurrence and intensification of tornadoes is higher due to smoke only in cases where cloud droplet number concentration in low level clouds increases considerably in a way that modifies the environmental conditions where the tornadoes are formed (shallower cloud bases and higher low-level wind shear). Smoke absorption and vertical extent also play a role, with smoke absorption at cloud-level tending to burn-off clouds and smoke absorption above clouds resulting in an increased capping inversion. Comparing these and WRF-Chem simulations configured with a more complex representation of aerosol size and composition and different optical properties, microphysics and activation schemes, we find similarities in terms of the simulated aerosol optical depths and aerosol impacts on near-storm environments. This provides reliability on the aerosol-aware microphysics scheme as a less computationally expensive alternative to WRFChem for its use in applications such as NWP and cloud-resolving simulations.

Quantifying the risks of solid aerosol geoengineering: the role of fundamental material properties

NASA Astrophysics Data System (ADS)

Dykema, J. A.; Keutsch, F. N.; Keith, D.

2017-12-01

Solid aerosols have been considered as an alternative to sulfate aerosols for solar geoengineering due to their optical and chemical properties, which lead to different and possibly more attractive risk profiles. Solid aerosols can achieve higher solar scattering efficiency due to their higher refractive index, and in some cases may also be less effective absorbers of thermal infrared radiation. The optical properties of solid aerosols are however sensitive functions of the detailed physical properties of solid materials in question. The relevant details include the exact crystalline structure of the aerosols, the physical size of the particles, and interactions with background stratospheric molecular and particulate constituents. In this work, we examine the impact of these detailed physical properties on the radiative properties of calcite (CaCO3) solid aerosols. We examine how crystal morphology, size, chemical reactions, and interaction with background stratospheric aerosol may alter the scattering and absorption properties of calcite aerosols for solar and thermal infrared radiation. For example, in small particles, crystal lattice vibrations associated with the particle surface may lead to substantially different infrared absorption properties than bulk materials. We examine the wavelength dependence of absorption by the particles, which may lead to altered patterns of stratospheric radiative heating and equilibrium temperatures. Such temperature changes can lead to dynamical changes, with consequences for both stratospheric composition and tropospheric climate. We identify important uncertainties in the current state of understanding, investigate risks associated with these uncertainties, and survey potential approaches to quantitatively improving our knowledge of the relevant material properties.

Low hygroscopicity of ambient fresh carbonaceous aerosols from pyrotechnics smoke

DOE PAGES

Carrico, Christian M.; Gomez, Samantha Laray; Dubey, Manvendra Krishna; ...

2018-01-31

Pyrotechnics (fireworks) displays are common for many cultures worldwide, with Independence Day celebrations occurring annually on July 4th as the most notable in the U.S. Given an episodic nature, fireworks aerosol properties are poorly characterized. Here we report observations of optical properties of fresh smoke emissions from Independence Day fireworks smoke sampled at Los Alamos National Laboratory, New Mexico U.S.A. on 4–5 July 2016. Aerosol optical properties were measured with a photoacoustic extinctiometer (PAX, DMT, Inc., Model 870 nm) at low RH < 30% and a humidity controlled nephelometry system (Ecotech, Inc., 450 nm Aurora). ‘Dry’ light scattering coefficient (σsp)more » increased from background < 15 Mm –1 reaching 120 Mm –1 (450 nm) as a 2-min event peak, while the absorption coefficient increased from background of 0.5–4.4 Mm –1 (870 nm). The event peak occurred at 00:35 on 5 July 2016, ~3 h after local fireworks events, and decreased to background by 04:00 on 5 July 2016, showing well mixed aerosol properties. A notable result is that the aerosol hygroscopic response, as characterized by the ratio of wet to dry light scattering or f(RH = 85%), declined to 1.02 at the peak fireworks influence from a background ~1.7. Strong wavelength dependence of light scattering with Ångström exponent ~2.2 throughout the event showed a size distribution dominated by sub-micrometer particles. Likewise, single scattering albedo at 870 nm remained constant throughout the event with ω = 0.86 ± 0.03, indicating light absorbing carbon, though not dominant, was mixed with organic carbon. Subsequent laboratory testing with ground-level sparklers showed that pyrotechnics smoke can generate a strong hygroscopic response, however. As confirmed with chemical analysis, the chemistry of the fireworks was key to defining the hygroscopic response. As a result, sparkler smoke was dominated by salt species such as hygroscopic potassium chloride while it lacked the black powder explosives in aerial fireworks that contribute organic and elemental carbon to its non-hygroscopic smoke.« less

Low hygroscopicity of ambient fresh carbonaceous aerosols from pyrotechnics smoke

DOE Office of Scientific and Technical Information (OSTI.GOV)

Carrico, Christian M.; Gomez, Samantha Laray; Dubey, Manvendra Krishna

Pyrotechnics (fireworks) displays are common for many cultures worldwide, with Independence Day celebrations occurring annually on July 4th as the most notable in the U.S. Given an episodic nature, fireworks aerosol properties are poorly characterized. Here we report observations of optical properties of fresh smoke emissions from Independence Day fireworks smoke sampled at Los Alamos National Laboratory, New Mexico U.S.A. on 4–5 July 2016. Aerosol optical properties were measured with a photoacoustic extinctiometer (PAX, DMT, Inc., Model 870 nm) at low RH < 30% and a humidity controlled nephelometry system (Ecotech, Inc., 450 nm Aurora). ‘Dry’ light scattering coefficient (σsp)more » increased from background < 15 Mm –1 reaching 120 Mm –1 (450 nm) as a 2-min event peak, while the absorption coefficient increased from background of 0.5–4.4 Mm –1 (870 nm). The event peak occurred at 00:35 on 5 July 2016, ~3 h after local fireworks events, and decreased to background by 04:00 on 5 July 2016, showing well mixed aerosol properties. A notable result is that the aerosol hygroscopic response, as characterized by the ratio of wet to dry light scattering or f(RH = 85%), declined to 1.02 at the peak fireworks influence from a background ~1.7. Strong wavelength dependence of light scattering with Ångström exponent ~2.2 throughout the event showed a size distribution dominated by sub-micrometer particles. Likewise, single scattering albedo at 870 nm remained constant throughout the event with ω = 0.86 ± 0.03, indicating light absorbing carbon, though not dominant, was mixed with organic carbon. Subsequent laboratory testing with ground-level sparklers showed that pyrotechnics smoke can generate a strong hygroscopic response, however. As confirmed with chemical analysis, the chemistry of the fireworks was key to defining the hygroscopic response. As a result, sparkler smoke was dominated by salt species such as hygroscopic potassium chloride while it lacked the black powder explosives in aerial fireworks that contribute organic and elemental carbon to its non-hygroscopic smoke.« less

Low hygroscopicity of ambient fresh carbonaceous aerosols from pyrotechnics smoke

NASA Astrophysics Data System (ADS)

Carrico, Christian M.; Gomez, Samantha L.; Dubey, Manvendra K.; Aiken, Allison C.

2018-04-01

Pyrotechnics (fireworks) displays are common for many cultures worldwide, with Independence Day celebrations occurring annually on July 4th as the most notable in the U.S. Given an episodic nature, fireworks aerosol properties are poorly characterized. Here we report observations of optical properties of fresh smoke emissions from Independence Day fireworks smoke sampled at Los Alamos National Laboratory, New Mexico U.S.A. on 4-5 July 2016. Aerosol optical properties were measured with a photoacoustic extinctiometer (PAX, DMT, Inc., Model 870 nm) at low RH < 30% and a humidity controlled nephelometry system (Ecotech, Inc., 450 nm Aurora). 'Dry' light scattering coefficient (σsp) increased from background < 15 Mm-1 reaching 120 Mm-1 (450 nm) as a 2-min event peak, while the absorption coefficient increased from background of 0.5-4.4 Mm-1 (870 nm). The event peak occurred at 00:35 on 5 July 2016, ∼3 h after local fireworks events, and decreased to background by 04:00 on 5 July 2016, showing well mixed aerosol properties. A notable result is that the aerosol hygroscopic response, as characterized by the ratio of wet to dry light scattering or f(RH = 85%), declined to 1.02 at the peak fireworks influence from a background ∼1.7. Strong wavelength dependence of light scattering with Ångström exponent ∼2.2 throughout the event showed a size distribution dominated by sub-micrometer particles. Likewise, single scattering albedo at 870 nm remained constant throughout the event with ω = 0.86 ± 0.03, indicating light absorbing carbon, though not dominant, was mixed with organic carbon. Subsequent laboratory testing with ground-level sparklers showed that pyrotechnics smoke can generate a strong hygroscopic response, however. As confirmed with chemical analysis, the chemistry of the fireworks was key to defining the hygroscopic response. Sparkler smoke was dominated by salt species such as hygroscopic potassium chloride while it lacked the black powder explosives in aerial fireworks that contribute organic and elemental carbon to its non-hygroscopic smoke.

Photochemical aging of light-absorbing secondary organic aerosol material.

PubMed

Sareen, Neha; Moussa, Samar G; McNeill, V Faye

2013-04-11

Dark reactions of methylglyoxal with NH4(+) in aqueous aerosols yield light-absorbing and surface-active products that can influence the physical properties of the particles. Little is known about how the product mixture and its optical properties will change due to photolysis as well as oxidative aging by O3 and OH in the atmosphere. Here, we report the results of kinetics and product studies of the photochemical aging of aerosols formed by atomizing aqueous solutions of methylglyoxal and ammonium sulfate. Experiments were performed using aerosol flow tube reactors coupled with an aerosol chemical ionization mass spectrometer (Aerosol-CIMS) for monitoring gas- and particle-phase compositions. Particles were also impacted onto quartz windows in order to assess changes in their UV-visible absorption upon oxidation. Photooxidation of the aerosols leads to the formation of small, volatile organic acids including formic acid, acetic acid, and glyoxylic acid. The atmospheric lifetime of these species during the daytime is predicted to be on the order of minutes, with photolysis being an important mechanism of degradation. The lifetime with respect to O3 oxidation was observed to be on the order of hours. O3 oxidation also leads to a net increase in light absorption by the particles due to the formation of additional carbonyl compounds. Our results are consistent with field observations of high brown carbon absorption in the early morning.

Assessment of biomass burning smoke influence on environmental conditions for multiyear tornado outbreaks by combining aerosol-aware microphysics and fire emission constraints

NASA Astrophysics Data System (ADS)

Saide, Pablo E.; Thompson, Gregory; Eidhammer, Trude; da Silva, Arlindo M.; Pierce, R. Bradley; Carmichael, Gregory R.

2016-09-01

We use the Weather Research and Forecasting (WRF) system to study the impacts of biomass burning smoke from Central America on several tornado outbreaks occurring in the U.S. during spring. The model is configured with an aerosol-aware microphysics parameterization capable of resolving aerosol-cloud-radiation interactions in a cost-efficient way for numerical weather prediction (NWP) applications. Primary aerosol emissions are included, and smoke emissions are constrained using an inverse modeling technique and satellite-based aerosol optical depth observations. Simulations turning on and off fire emissions reveal smoke presence in all tornado outbreaks being studied and show an increase in aerosol number concentrations due to smoke. However, the likelihood of occurrence and intensification of tornadoes is higher due to smoke only in cases where cloud droplet number concentration in low-level clouds increases considerably in a way that modifies the environmental conditions where the tornadoes are formed (shallower cloud bases and higher low-level wind shear). Smoke absorption and vertical extent also play a role, with smoke absorption at cloud-level tending to burn-off clouds and smoke absorption above clouds resulting in an increased capping inversion. Comparing these and WRF-Chem simulations configured with a more complex representation of aerosol size and composition and different optical properties, microphysics, and activation schemes, we find similarities in terms of the simulated aerosol optical depths and aerosol impacts on near-storm environments. This provides reliability on the aerosol-aware microphysics scheme as a less computationally expensive alternative to WRF-Chem for its use in applications such as NWP and cloud-resolving simulations.

Black carbon's contribution to aerosol absorption optical depth over S. Korea

NASA Astrophysics Data System (ADS)

Lamb, K.; Perring, A. E.; Beyersdorf, A. J.; Anderson, B. E.; Segal-Rosenhaimer, M.; Redemann, J.; Holben, B. N.; Schwarz, J. P.

2017-12-01

Aerosol absorption optical depth (AAOD) monitored by ground-based sites (AERONET, SKYNET, etc.) is used to constrain climate radiative forcing from black carbon (BC) and other absorbing aerosols in global models, but few validation studies between in situ aerosol measurements and ground-based AAOD exist. AAOD is affected by aerosol size distributions, composition, mixing state, and morphology. Megacities provide appealing test cases for this type of study due to their association with very high concentrations of anthropogenic aerosols. During the KORUS-AQ campaign in S. Korea, which took place in late spring and early summer of 2016, in situ aircraft measurements over the Seoul Metropolitan Area and Taehwa Research Forest (downwind of Seoul) were repeated three times per flight over a 6 week period, providing significant temporal coverage of vertically resolved aerosol properties influenced by different meteorological conditions and sources. Measurements aboard the NASA DC-8 by the NOAA Humidified Dual Single Particle Soot Photometers (HD-SP2) quantified BC mass, size distributions, mixing state, and the hygroscopicity of BC containing aerosols. The in situ BC mass vertical profiles are combined with estimated absorption enhancement calculated from observed optical size and hygroscopicity using Mie theory, and then integrated over the depth of the profile to calculate BC's contribution to AAOD. Along with bulk aerosol size distributions and hygroscopicity, bulk absorbing aerosol optical properties, and on-board sky radiance measurements, these measurements are compared with ground-based AERONET site measurements of AAOD to evaluate closure between in situ vertical profiles of BC and AAOD measurements. This study will provide constraints on the relative importance of BC (including lensing and hygroscopicity effects) and non-BC components to AAOD over S. Korea.

Characterization of Artifacts Introduced by the Empirical Volcano-Scan Atmospheric Correction Commonly Applied to CRISM and OMEGA Near-Infrared Spectra

NASA Technical Reports Server (NTRS)

Wiseman, S.M.; Arvidson, R.E.; Wolff, M. J.; Smith, M. D.; Seelos, F. P.; Morgan, F.; Murchie, S. L.; Mustard, J. F.; Morris, R. V.; Humm, D.;

Soot Particle Studies - Instrument Inter-Comparison – Project Overview

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cross, E.; Sedlacek, A.; Onasch, T. B.

2010-03-06

An inter-comparison study of instruments designed to measure the microphysical and optical properties of soot particles was completed. The following mass-based instruments were tested: Couette Centrifugal Particle Mass Analyzer (CPMA), Time-of-Flight Aerosol Mass Spectrometer - Scanning Mobility Particle Sizer (AMS-SMPS), Single Particle Soot Photometer (SP2), Soot Particle-Aerosol Mass Spectrometer (SP-AMS) and Photoelectric Aerosol Sensor (PAS2000CE). Optical instruments measured absorption (photoacoustic, interferometric, and filter-based), scattering (in situ), and extinction (light attenuation within an optical cavity). The study covered an experimental matrix consisting of 318 runs that systematically tested the performance of instruments across a range of parameters including: fuel equivalence ratiomore » (1.8 {le} {phi} {le} 5), particle shape (mass-mobility exponent (D{sub f m}), 2.0 {le} D{sub f m} {le} 3.0), particle mobility size (30 {le} d{sub m} {le} 300 nm), black carbon mass (0.07 {le} m{sub BC} {le} 4.2 fg) and particle chemical composition. In selected runs, particles were coated with sulfuric acid or dioctyl sebacate (DOS) (0.5 {le} {Delta}r{sub ve} {le} 201 nm) where {Delta}r{sub ve} is the change in the volume equivalent radius due to the coating material. The effect of non-absorbing coatings on instrument response was determined. Changes in the morphology of fractal soot particles were monitored during coating and denuding processes and the effect of particle shape on instrument response was determined. The combination of optical and mass based measurements was used to determine the mass specific absorption coefficient for denuded soot particles. The single scattering albedo of the particles was also measured. An overview of the experiments and sample results are presented.« less

Characterization of artifacts introduced by the empirical volcano-scan atmospheric correction commonly applied to CRISM and OMEGA near-infrared spectra

NASA Astrophysics Data System (ADS)

Wiseman, S. M.; Arvidson, R. E.; Wolff, M. J.; Smith, M. D.; Seelos, F. P.; Morgan, F.; Murchie, S. L.; Mustard, J. F.; Morris, R. V.; Humm, D.; McGuire, P. C.

2016-05-01

The empirical 'volcano-scan' atmospheric correction is widely applied to martian near infrared CRISM and OMEGA spectra between ∼1000 and ∼2600 nm to remove prominent atmospheric gas absorptions with minimal computational investment. This correction method employs division by a scaled empirically-derived atmospheric transmission spectrum that is generated from observations of the martian surface in which different path lengths through the atmosphere were measured and transmission calculated using the Beer-Lambert Law. Identifying and characterizing both artifacts and residual atmospheric features left by the volcano-scan correction is important for robust interpretation of CRISM and OMEGA volcano-scan corrected spectra. In order to identify and determine the cause of spectral artifacts introduced by the volcano-scan correction, we simulated this correction using a multiple scattering radiative transfer algorithm (DISORT). Simulated transmission spectra that are similar to actual CRISM- and OMEGA-derived transmission spectra were generated from modeled Olympus Mons base and summit spectra. Results from the simulations were used to investigate the validity of assumptions inherent in the volcano-scan correction and to identify artifacts introduced by this method of atmospheric correction. We found that the most prominent artifact, a bowl-shaped feature centered near 2000 nm, is caused by the inaccurate assumption that absorption coefficients of CO2 in the martian atmosphere are independent of column density. In addition, spectral albedo and slope are modified by atmospheric aerosols. Residual atmospheric contributions that are caused by variable amounts of dust aerosols, ice aerosols, and water vapor are characterized by the analysis of CRISM volcano-scan corrected spectra from the same location acquired at different times under variable atmospheric conditions.

Perturbations of the optical properties of mineral dust particles by mixing with black carbon: a numerical simulation study

DOE PAGES

Scarnato, B. V.; China, S.; Nielsen, K.; ...

2015-06-25

Field observations show that individual aerosol particles are a complex mixture of a wide variety of species, reflecting different sources and physico-chemical transformations. The impacts of individual aerosol morphology and mixing characteristics on the Earth system are not yet fully understood. Here we present a sensitivity study on climate-relevant aerosols optical properties to various approximations. Based on aerosol samples collected in various geographical locations, we have observationally constrained size, morphology and mixing, and accordingly simulated, using the discrete dipole approximation model (DDSCAT), optical properties of three aerosols types: (1) bare black carbon (BC) aggregates, (2) bare mineral dust, and (3)more » an internal mixture of a BC aggregate laying on top of a mineral dust particle, also referred to as polluted dust. DDSCAT predicts optical properties and their spectral dependence consistently with observations for all the studied cases. Predicted values of mass absorption, scattering and extinction coefficients (MAC, MSC, MEC) for bare BC show a weak dependence on the BC aggregate size, while the asymmetry parameter ( g) shows the opposite behavior. The simulated optical properties of bare mineral dust present a large variability depending on the modeled dust shape, confirming the limited range of applicability of spheroids over different types and size of mineral dust aerosols, in agreement with previous modeling studies. The polluted dust cases show a strong decrease in MAC values with the increase in dust particle size (for the same BC size) and an increase of the single scattering albedo (SSA). Furthermore, particles with a radius between 180 and 300 nm are characterized by a decrease in SSA values compared to bare dust, in agreement with field observations.This paper demonstrates that observationally constrained DDSCAT simulations allow one to better understand the variability of the measured aerosol optical properties in ambient air and to define benchmark biases due to different approximations in aerosol parametrization.« less

Black carbon measurements during winter 2013-2014 in Athens and intercomparison between different techniques

NASA Astrophysics Data System (ADS)

Liakakou, Eleni; Stravroulas, Jason; Roukounakis, Nikolaos; Paraskevopoulou, Despina; Fourtziou, Luciana; Psiloglou, Vassilis; Gerasopoulos, Evangelos; Sciare, Jean; Mihalopoulos, Nikolaos

2014-05-01

Black carbon (BC) is a particulate pollutant species emitted from the combustion of fuels, biomass burning for agricultural purposes and forest fires, with the first two anthropogenic sources being the major contributors to the atmospheric burden of BC. The presence of BC is important due to its direct and indirect physicochemical effects and its use as a tracer of burning and subsequent transport processes. Black carbon measurements took place during winter 2013 -2014 in the frame of a pollution monitoring experiment conducted at the urban site of Thissio, Athens (city center) at the premises of the National Observatory of Athens. The economic crisis in Greece and the resulting turn of Athens inhabitants to wood burning for domestic heating, has led to increased daily concentrations of BC in the range of 2-6 μg m-3, peaking at night time (15-20 μg m-3). Three different optical methods were used for the determination of BC. A Particle Soot Absorption Photometer (PSAP; Radiance Research) commercial instrument was used to monitor the light absorption coefficient (σap) at 565 nm of ambient aerosols, with 1 minute resolution. During parts of the campaign, a portable Aethalometer (AE-42; Magee Scientific) was also used to provide measurement of the aerosol BC content at 7 wavelengths over 5 minutes intervals. Exploiting the measurements at different wavelengths is was feasible to separate wood burning BC from BC related to fossil fuel. Two Multi Angle Absorption Photometers (MAAP; Thermo) were also operated as reference. Finally, aerosol samples were collected on 12-hour basis using a sequential dichotomous sampler for the sampling of PM2.5, PM2.5-10and PM10 fractions of aerosols on quartz filters, and the filters were analyzed for elemental carbon (EC) by a thermal - optical transmission technique. The main objective of the study is the intercomparison of the different BC monitoring techniques under a large range of ambient concentrations achieved due to the special circumstance occurring in Athens with the rapid increase of BC emission due to wood burning. In parallel, the BC measurements are used for the estimation of the contribution of wood burning in fireplaces and wood-stoves in ambient PM levels, compared to other known sources of local pollution (e.g. traffic, central heating).

DSCOVR EPIC AERUV Parameters

Atmospheric Science Data Center

2018-06-27

... AerosolType      The aerosol type associated with the ground pixel.        1 - Smoke ... algorithm flag associated with the ground pixel:     Aerosol extinction Optical Depth (AOD), Single Scattering Albedo (SSA), and     Aerosol Absorption Optical Depth (AAOD) Retrievals:        0 - Most ...

Aerosol Retrievals over the Ocean using Channel 1 and 2 AVHRR Data: A Sensitivity Analysis and Preliminary Results

NASA Technical Reports Server (NTRS)

Mishchenko, Michael I.; Geogdzhayev, Igor V.; Cairns, Brian; Rossow, William B.; Lacis, Andrew A.

1999-01-01

This paper outlines the methodology of interpreting channel 1 and 2 AVHRR radiance data over the oceans and describes a detailed analysis of the sensitivity of monthly averages of retrieved aerosol parameters to the assumptions made in different retrieval algorithms. The analysis is based on using real AVHRR data and exploiting accurate numerical techniques for computing single and multiple scattering and spectral absorption of light in the vertically inhomogeneous atmosphere-ocean system. We show that two-channel algorithms can be expected to provide significantly more accurate and less biased retrievals of the aerosol optical thickness than one-channel algorithms and that imperfect cloud screening and calibration uncertainties are by far the largest sources of errors in the retrieved aerosol parameters. Both underestimating and overestimating aerosol absorption as well as the potentially strong variability of the real part of the aerosol refractive index may lead to regional and/or seasonal biases in optical thickness retrievals. The Angstrom exponent appears to be the most invariant aerosol size characteristic and should be retrieved along with optical thickness as the second aerosol parameter.

Aerosols and lightning activity: The effect of vertical profile and aerosol type

NASA Astrophysics Data System (ADS)

Proestakis, E.; Kazadzis, S.; Lagouvardos, K.; Kotroni, V.; Amiridis, V.; Marinou, E.; Price, C.; Kazantzidis, A.

2016-12-01

The Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument on board the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) satellite has been utilized for the first time in a study regarding lightning activity modulation due to aerosols. Lightning activity observations, obtained by the ZEUS long range Lightning Detection Network, European Centre for Medium range Weather Forecasts (ECMWF) Convective Available Potential Energy (CAPE) data and Cloud Fraction (CF) retrieved by MODIS on board Aqua satellite have been combined with CALIPSO CALIOP data over the Mediterranean basin and for the period March to November, from 2007 to 2014. The results indicate that lightning activity is enhanced during days characterized by higher Aerosol Optical Depth (AOD) values, compared to days with no lightning. This study contributes to existing studies on the link between lightning activity and aerosols, which have been based just on columnar AOD satellite retrievals, by performing a deeper analysis into the effect of aerosol profiles and aerosol types. Correlation coefficients of R = 0.73 between the CALIPSO AOD and the number of lightning strikes detected by ZEUS and of R = 0.93 between ECMWF CAPE and lightning activity are obtained. The analysis of extinction coefficient values at 532 nm indicates that at an altitudinal range exists, between 1.1 km and 2.9 km, where the values for extinction coefficient of lightning-active and non-lightning-active cases are statistically significantly different. Finally, based on the CALIPSO aerosol subtype classification, we have investigated the aerosol conditions of lightning-active and non-lightning-active cases. According to the results polluted dust aerosols are more frequently observed during non-lightning-active days, while dust and smoke aerosols are more abundant in the atmosphere during the lightning-active days.

Solar absorption by elemental and brown carbon determined from spectral observations.

PubMed

Bahadur, Ranjit; Praveen, Puppala S; Xu, Yangyang; Ramanathan, V

2012-10-23

Black carbon (BC) is functionally defined as the absorbing component of atmospheric total carbonaceous aerosols (TC) and is typically dominated by soot-like elemental carbon (EC). However, organic carbon (OC) has also been shown to absorb strongly at visible to UV wavelengths and the absorbing organics are referred to as brown carbon (BrC), which is typically not represented in climate models. We propose an observationally based analytical method for rigorously partitioning measured absorption aerosol optical depths (AAOD) and single scattering albedo (SSA) among EC and BrC, using multiwavelength measurements of total (EC, OC, and dust) absorption. EC is found to be strongly absorbing (SSA of 0.38) whereas the BrC SSA varies globally between 0.77 and 0.85. The method is applied to the California region. We find TC (EC + BrC) contributes 81% of the total absorption at 675 nm and 84% at 440 nm. The BrC absorption at 440 nm is about 40% of the EC, whereas at 675 nm it is less than 10% of EC. We find an enhanced absorption due to OC in the summer months and in southern California (related to forest fires and secondary OC). The fractions and trends are broadly consistent with aerosol chemical-transport models as well as with regional emission inventories, implying that we have obtained a representative estimate for BrC absorption. The results demonstrate that current climate models that treat OC as nonabsorbing are underestimating the total warming effect of carbonaceous aerosols by neglecting part of the atmospheric heating, particularly over biomass-burning regions that emit BrC.

The impact of aerosol composition on the particle to gas partitioning of reactive mercury.

PubMed

Rutter, Andrew P; Schauer, James J

2007-06-01

A laboratory system was developed to study the gas-particle partitioning of reactive mercury (RM) as a function of aerosol composition in synthetic atmospheric particulate matter. The collection of RM was achieved by filter- and sorbent-based methods. Analyses of the RM collected on the filters and sorbents were performed using thermal extraction combined with cold vapor atomic fluorescence spectroscopy (CVAFS), allowing direct measurement of the RM load on the substrates. Laboratory measurements of the gas-particle partitioning coefficients of RM to atmospheric aerosol particles revealed a strong dependence on aerosol composition, with partitioning coefficients that varied by orders of magnitude depending on the composition of the particles. Particles of sodium nitrate and the chlorides of potassium and sodium had high partitioning coefficients, shifting the RM partitioning toward the particle phase, while ammonium sulfate, levoglucosan, and adipic acid caused the RM to partition toward the gas phase and, therefore, had partitioning coefficients that were lower by orders of magnitude.

Spatial Representativeness Error in the Ground‐Level Observation Networks for Black Carbon Radiation Absorption

PubMed Central

Andrews, Elisabeth; Balkanski, Yves; Boucher, Olivier; Myhre, Gunnar; Samset, Bjørn Hallvard; Schulz, Michael; Schuster, Gregory L.; Valari, Myrto; Tao, Shu

2018-01-01

Abstract There is high uncertainty in the direct radiative forcing of black carbon (BC), an aerosol that strongly absorbs solar radiation. The observation‐constrained estimate, which is several times larger than the bottom‐up estimate, is influenced by the spatial representativeness error due to the mesoscale inhomogeneity of the aerosol fields and the relatively low resolution of global chemistry‐transport models. Here we evaluated the spatial representativeness error for two widely used observational networks (AErosol RObotic NETwork and Global Atmosphere Watch) by downscaling the geospatial grid in a global model of BC aerosol absorption optical depth to 0.1° × 0.1°. Comparing the models at a spatial resolution of 2° × 2° with BC aerosol absorption at AErosol RObotic NETwork sites (which are commonly located near emission hot spots) tends to cause a global spatial representativeness error of 30%, as a positive bias for the current top‐down estimate of global BC direct radiative forcing. By contrast, the global spatial representativeness error will be 7% for the Global Atmosphere Watch network, because the sites are located in such a way that there are almost an equal number of sites with positive or negative representativeness error. PMID:29937603

Aerosols in coastal and inland areas in the equatorial African belt.

PubMed

Ssenyonga, Taddeo; Muyimbwa, Dennis; Okullo, Willy; Chen, Yi-Chun; Frette, Øvyind; Hamre, Børge; Steigen, Andreas; Dahlback, Arne; Stamnes, Jakob J

2014-05-10

Aerosols affect the climate directly through absorption and reflection of sunlight back to space and indirectly by acting as cloud condensation nuclei. This paper is based on more than three decades of satellite data (1979-1994 and 1996-2012) from total ozone mapping spectrometer (TOMS) and ozone monitoring instrument (OMI), which have provided measurements of backscattered radiances in the wavelength range from 331 to 380 nm. These data have been used to determine the aerosol climatology and to investigate the influence of the aerosol index (AI) on the ultraviolet index (UVI) in coastal land areas in Serrekunda (13.28°N, 16.34°W), The Gambia, and Dar-es-Salaam (6.8°S, 39.26°E), Tanzania, as well as in inland areas in Kampala (0.19°N, 32.34°E), Uganda. Heavy aerosol loadings were found to occur in the dry seasons at all three locations. To reduce the influence of clouds, we disregarded TOMS and OMI data for days during which the UV reflectivity was larger than 9% and investigated the correlation of the AI with the UVI for the remaining days at the three locations. We found a high correlation coefficient of 0.82 for Serrekunda, but poor correlation for Kampala and Dar-es-Salaam. The average AI for Serrekunda was found to be about three times higher than that for Kampala or Dar-es-Salaam, and a positive trend was found for the AI in Kampala and Dar-es-Salaam, whereas a negative trend was found for the AI in Serrekunda.

Evaluation of MERRAero (MERRA Aerosol Reanalysis)

NASA Technical Reports Server (NTRS)

Buchard, Virginie; da Silva, Arlindo; Randles, Cynthia; Colarco, Peter; Darmenov, Anton; Govindaraju, Ravi

2016-01-01

This presentation focuses on MERRA Aerosol Reanalysis (MERRAero) which is the first aerosol reanalysis produced at GMAO. This presentation involve an overview of MERRAero. The evaluation of MERRAero absorption and the evaluation of MERRAero Surface PM 2.5 will also be discussed.

An Accuracy Assessment of the CALIOP/CALIPSO Version 2/Version 3 Daytime Aerosol Extinction Product Based on a Detailed Multi-Sensor, Multi-Platform Case Study

NASA Technical Reports Server (NTRS)

Kacenelenbogen, M.; Vaughan, M. A.; Redemann, J.; Hoff, R. M.; Rogers, R. R.; Ferrare, R. A.; Russell, P. B.; Hostetler, C. A.; Hair, J. W.; Holben, B. N.

2011-01-01

The Cloud Aerosol LIdar with Orthogonal Polarization (CALIOP), on board the CALIPSO platform, has measured profiles of total attenuated backscatter coefficient (level 1 products) since June 2006. CALIOP s level 2 products, such as the aerosol backscatter and extinction coefficient profiles, are retrieved using a complex succession of automated algorithms. The goal of this study is to help identify potential shortcomings in the CALIOP version 2 level 2 aerosol extinction product and to illustrate some of the motivation for the changes that have been introduced in the next version of CALIOP data (version 3, released in June 2010). To help illustrate the potential factors contributing to the uncertainty of the CALIOP aerosol extinction retrieval, we focus on a one-day, multi-instrument, multiplatform comparison study during the CALIPSO and Twilight Zone (CATZ) validation campaign on 4 August 2007. On that day, we observe a consistency in the Aerosol Optical Depth (AOD) values recorded by four different instruments (i.e. spaceborne MODerate Imaging Spectroradiometer, MODIS: 0.67 and POLarization and Directionality of Earth s Reflectances, POLDER: 0.58, airborne High Spectral Resolution Lidar, HSRL: 0.52 and ground-based AErosol RObotic NETwork, AERONET: 0.48 to 0.73) while CALIOP AOD is a factor of two lower (0.32 at 532 nm). This case study illustrates the following potential sources of uncertainty in the CALIOP AOD: (i) CALIOP s low signal-to-noise ratio (SNR) leading to the misclassification and/or lack of aerosol layer identification, especially close to the Earth s surface; (ii) the cloud contamination of CALIOP version 2 aerosol backscatter and extinction profiles; (iii) potentially erroneous assumptions of the aerosol extinction-to-backscatter ratio (Sa) used in CALIOP s extinction retrievals; and (iv) calibration coefficient biases in the CALIOP daytime attenuated backscatter coefficient profiles. The use of version 3 CALIOP extinction retrieval for our case study seems to partially fix factor (i) although the aerosol retrieved by CALIOP is still somewhat lower than the profile measured by HSRL; the cloud contamination (ii) appears to be corrected; no particular change is apparent in the observation-based CALIOP Sa value (iii). Our case study also showed very little difference in version 2 and version 3 CALIOP attenuated backscatter coefficient profiles, illustrating a minor change in the calibration scheme (iv).

Chemical characteristics of N2O5 observed at a rural site in Beijing winter 2016: from clean to polluted air mass

NASA Astrophysics Data System (ADS)

Wang, H.; Lu, K.; Tan, Z.; Chen, X.; Wu, Z.; Zhu, Q.; Li, X.; Liu, Y.; Shang, D.; Wu, Y.; Min, H.; Zeng, L.; Schmitt, S. H.; Rohrer, F.; Kiendler-Scharr, A.; Wahner, A.; Zhang, Y.

2017-12-01

Dinitrogen pentoxide (N2O5) plays a vital role in the atmospheric oxidation, the NOX removal and the nitrate formation. A comprehensive campaign was conducted in the wintertime of 2016 in Beijing to focus on the atmospheric oxidation, new particle formation and aerosol light extinctions during the wintertime in Beijing. The site is located at a rural area in the northeast of Beijing and about 60 km away from the city center. A newly developed instrument based on the cavity enhanced absorption spectroscopy (CEAS) was deployed to measure ambient N2O5. Simultaneous measurements of the properties of particles and the relevant trace gases are available. The daily peaks of N2O5 in the clean episodes was lower than that of polluted episodes, the campaign maximum of 1.4 ppbv were captured in the most serious pollution episode. The averaged N2O5 maximum was about 120 pptv near 20:00, which is higher than that observed in summer. The uptake coefficient of N2O5 was derived from an iterative box model approach based on the Regional Atmospheric Chemical Mechanism version 2 (RACM2), constrained to observed trace gas compounds as well as the aerosol surface concentrations. The mechanisms of the chemical compounds of aerosols (measured by AMS) affects the N2O5 uptake coefficient are explored in several chemical coordinate systems. The chemical behaviors of the ambient N2O5 concentrations for this campaign is further discussed in the context of other campaigns performed in the urban and suburban areas in Beijing.

Water vapor variation and the effect of aerosols in China

NASA Astrophysics Data System (ADS)

Gui, Ke; Che, Huizheng; Chen, Quanliang; Zeng, Zhaoliang; Zheng, Yu; Long, Qichao; Sun, Tianze; Liu, Xinyu; Wang, Yaqiang; Liao, Tingting; Yu, Jie; Wang, Hong; Zhang, Xiaoye

2017-09-01

This study analyzes the annual and seasonal trends in precipitable water vapor (PWV) and surface temperature (Ts) over China from 1979 to 2015, and the relationships between PWV and Ts and between PWV and aerosol absorption optical depth (AAOD), using data from radiosonde stations, weather stations and multiple satellite observations. The results revealed a positive PWV trend between 1979 and 1999, and a negative PWV trend between 2000 and 2015. Analysis of the differences in the PWV trend among different stations types showed that the magnitude of the trends were in the order main urban stations > provincial capital stations > suburb stations, suggesting that anthropogenic activities have a strong influence on the PWV trend. The AAOD exhibited a significant positive trend in most regions of China from 2005 to 2015 (confidence level 95%). Using spatial correlation analysis, we showed that PWV trend derived from Moderate Resolution Imaging Spectroradiometer (MODIS) satellite observations is correlated with Ts, with an annual correlation coefficient of 0.596. In addition, the spatial correlation between PWV and AAOD showed a negative relationship, with the highest correlation coefficients of -0.76 and -0.71 observed in mid-eastern China and central northwest China, respectively, suggesting that the increase in AAOD in recent years may be one of the reasons for the decrease in PWV since the 2000s in China.

Retrieval of Black Carbon Absorption from Proposed Satellite Measurements Over the Ocean Glint

NASA Technical Reports Server (NTRS)

Kaufman, Y. J.; Matins, J. V.; Remer, L. A.; Schoeberl, M. R.; Yamasoe, M. A.; Lau, William K. M. (Technical Monitor)

2001-01-01

Haze and air pollution includes many chemicals that together form small particles suspended in the air called aerosols. One of the main ingredients found to affect climate and human health is Black Carbon. Black particles emitted from engines that do not burn the fuel completely, e.g. old trucks. Black carbon absorption of sunlight emerges as one of the key components of man-made forcing of climate. However, global characterization of black carbon emissions, distribution and pathways in which it can affect the amount of solar radiation absorbed by the atmosphere is very uncertain. A new method is proposed to measure sunlight absorption by fine aerosol particles containing black carbon over the ocean glint from a satellite mission designed for this purpose. The satellite will scan the same spot over the ocean in the glint plane and a plane 40 degrees off-glint a minute apart, collecting measurements of the reflected light across the solar spectrum. First the dark ocean off the glint is used to derive aerosol properties. Then the black carbon absorption is derived prop the attenuation of the bright glint by the aerosol layer. Such measurements if realized in a proposed future mission - COBRA are expected to produce global monthly climatology of black carbon absorption with high accuracy (110 to 15%) that can show their effect on climate.

Assessment of biomass burning smoke influence on environmental conditions for multi-year tornado outbreaks by combining aerosol-aware microphysics and fire emission constraints

PubMed Central

Saide, Pablo E.; Thompson, Gregory; Eidhammer, Trude; da Silva, Arlindo M.; Pierce, R. Bradley; Carmichael, Gregory R.

2018-01-01

We use the WRF system to study the impacts of biomass burning smoke from Central America on several tornado outbreaks occurring in the US during spring. The model is configured with an aerosol-aware microphysics parameterization capable of resolving aerosol-cloud-radiation interactions in a cost-efficient way for numerical weather prediction (NWP) applications. Primary aerosol emissions are included and smoke emissions are constrained using an inverse modeling technique and satellite-based AOD observations. Simulations turning on and off fire emissions reveal smoke presence in all tornado outbreaks being studied and show an increase in aerosol number concentrations due to smoke. However, the likelihood of occurrence and intensification of tornadoes is higher due to smoke only in cases where cloud droplet number concentration in low level clouds increases considerably in a way that modifies the environmental conditions where the tornadoes are formed (shallower cloud bases and higher low-level wind shear). Smoke absorption and vertical extent also play a role, with smoke absorption at cloud-level tending to burn-off clouds and smoke absorption above clouds resulting in an increased capping inversion. Comparing these and WRF-Chem simulations configured with a more complex representation of aerosol size and composition and different optical properties, microphysics and activation schemes, we find similarities in terms of the simulated aerosol optical depths and aerosol impacts on near-storm environments. This provides reliability on the aerosol-aware microphysics scheme as a less computationally expensive alternative to WRF-Chem for its use in applications such as NWP and cloud-resolving simulations. PMID:29619287

In Situ Measurement of Aerosol Extinction

NASA Technical Reports Server (NTRS)

Strawa, Anthony W.; Castaneda, R.; Owano, T. G.; Bear, D.; Gore, Warren J. (Technical Monitor)

2001-01-01

Aerosols are important contributors to the radiative forcing in the atmosphere. Much of the uncertainty in our knowledge of climate forcing is due to uncertainties in the radiative forcing due to aerosols as illustrated in the IPCC reports of the last ten years. Improved measurement of aerosol optical properties, therefore, is critical to an improved understanding of atmospheric radiative forcing. Additionally, attempts to reconcile in situ and remote measurements of aerosol radiative properties have generally not been successful. This is due in part to the fact that it has been impossible to measure aerosol extinction in situ in the past. In this presentation we introduce a new instrument that employs the techniques used in cavity ringdown spectroscopy to measure the aerosol extinction and scattering coefficients in situ. A prototype instrument has been designed and tested in the lab and the field. It is capable of measuring aerosol extinction coefficient to 2x10(exp -6) per meter. This prototype instrument is described and results are presented.

Infrared Absorption by Atmospheric Aerosols in Mexico City during MILAGRO.

NASA Astrophysics Data System (ADS)

Kelley, K. L.; Mangu, A.; Gaffney, J. S.; Marley, N. A.

2007-12-01

Past research in our group using cylindrical internal reflectance spectroscopy has indicated that aqueous aerosols could contribute to the radiative warming as greenhouse species (1,2). Although aerosol radiative effects have been known for sometime and are considered one of the major uncertainties in climate change modeling, most of the studies have focused on the forcing due to scattering and absorption of radiation in the uv- visible region (3). Infrared spectral information also allows the confirmation of key functional groups that are responsible for enhanced absorption observations from secondary organics in the uv-visible region. This work extends our efforts to evaluate the infrared absorption by aerosols, particularly organics, that are now found to be a major fraction of urban and regional aerosols in the 0.1 to 1.0 micron size range and to help identify key types of organics that can contribute to aerosol absorption. During the MILAGRO campaign, quartz filter samples were taken at 12-hour intervals from 5 am to 5 pm (day) and from 5 pm to 5 am (night) during the month of March 2006. These samples were taken at the two super-sites, T-0 (Instituto Mexicano de Petroleo in Mexico City) and T-1 (Universidad Technologica de Tecamac, State of Mexico). The samples have been characterized for total carbon content (stable isotope mass spectroscopy) and natural radionuclide tracers, as well as for their UV-visible spectroscopic properties by using integrating sphere diffuse reflectance spectroscopy (Beckman DU with a Labsphere accessory). These same samples have been characterized in the mid and near infrared spectral ranges using diffuse reflection spectroscopy (Nicolet 6700 FTIR with a Smart Collector accessory). Aerosol samples were removed from the surfaces of the aerosol filters by using Si-Carb sampler. The samples clearly indicate the presence of carbonyl organic constituents and the spectra are quite similar to those observed for humic and fulvic acids found as colloidal materials in surface and groundwaters (4). Examples of the IR spectra obtained and variance as a function of time at the two sites will be presented. The spectra are taken in Kubelka - Munk format, which also allows the infrared absorption strengths to be evaluated as function of wavelength. The wavelength dependence of the aerosol complex refractive index (m = n + ik) in the infrared spectral region is determined by application of the Kramers Kronig function. The importance of the aerosol absorption in the infrared spectral region to radiative forcing will be discussed. 1. N.A. Marley, J.S. Gaffney, and M.M. Cunningham,Environ. Sci. Technol. 27 2864-2869 (1993). 2. N.A. Marley, J.S. Gaffney, and M.M. Cunningham, Spectroscopy 7 44-53 (1992). 3. J.S. Gaffney and N.A. Marley, Atmospheric Environment, New Directions contribution, 32, 2873-2874 (1998). 4. N.A. Marley, J.S. Gaffney, and K.A. Orlandini, Chapter 7 in Humic/Fulvic Acids and Organic Colloidal Materials in the Environment, ACS Symposium Series 651, American Chemical Society, Washington, D.C., pp. 96-107, 1996. This work was performed as part of the Department of Energy's Megacity Aerosol Experiment - Mexico City (MAX- Mex) under the support of the Atmospheric Science Program. This research was supported by the Office of Science (BER), U.S. Department of Energy, Grant No. DE-FG02-07ER64328.

Critical Reflectance Derived from MODIS: Application for the Retrieval of Aerosol Absorption over Desert Regions

NASA Technical Reports Server (NTRS)

Wells, Kelley C.; Martins, J. Vanderlei; Remer, Lorraine A.; Kreidenweis, Sonia M.; Stephens, Graeme L.

2012-01-01

Aerosols are tiny suspended particles in the atmosphere that scatter and absorb sunlight. Smoke particles are aerosols, as are sea salt, particulate pollution and airborne dust. When you look down at the earth from space sometimes you can see vast palls of whitish smoke or brownish dust being transported by winds. The reason that you can see these aerosols is because they are reflecting incoming sunlight back to the view in space. The reason for the difference in color between the different types of aerosol is that the particles arc also absorbing sunlight at different wavelengths. Dust appears brownish or reddish because it absorbs light in the blue wavelengths and scatters more reddish light to space, Knowing how much light is scattered versus how much is absorbed, and knowin that as a function of wavelength is essential to being able to quantify the role aerosols play in the energy balance of the earth and in climate change. It is not easy measuring the absorption properties of aerosols when they are suspended in the atmosphere. People have been doing this one substance at a time in the laboratory, but substances mix when they are in the atmosphere and the net absorption effect of all the particles in a column of air is a goal of remote sensing that has not yet been completely successful. In this paper we use a technique based on observing the point at which aerosols change from brightening the surface beneath to darkening it. If aerosols brighten a surface. they must scatter more light to space. If they darken the surface. they must be absorbing more. That cross over point is called the critical reflectance and in this paper we show that critical reflectance is a monotonic function of the intrinsic absorption properties of the particles. This parameter we call the single scattering albedo. We apply the technique to MODIS imagery over the Sahara and Sahel regions to retrieve the single scattering albedo in seven wavelengths, compare these retrievals to ground-based retrievals from AERONET instruments and compute error bars on each retrieval. The results show that we can retrieve single scattering albedo for pure dust to within +/-0.02 and mixtures of dust and smoke to within +/-0.03. No other space based instrument has achieved a retrieval of single scattering albedo that spans the spectrum from 0.47 microns to 2.13 microns and produces regional maps of aerosol absorption showing gradients and changes. Applied in a more operational fashion, such information will narrow uncertainties in estimating aerosol forcing on climate.

Retrieval of Aerosol Parameters from Continuous H24 Lidar-Ceilometer Measurements

NASA Astrophysics Data System (ADS)

Dionisi, D.; Barnaba, F.; Costabile, F.; Di Liberto, L.; Gobbi, G. P.; Wille, H.

2016-06-01

Ceilometer technology is increasingly applied to the monitoring and the characterization of tropospheric aerosols. In this work, a method to estimate some key aerosol parameters (extinction coefficient, surface area concentration and volume concentration) from ceilometer measurements is presented. A numerical model has been set up to derive a mean functional relationships between backscatter and the above mentioned parameters based on a large set of simulated aerosol optical properties. A good agreement was found between the modeled backscatter and extinction coefficients and the ones measured by the EARLINET Raman lidars. The developed methodology has then been applied to the measurements acquired by a prototype Polarization Lidar-Ceilometer (PLC). This PLC instrument was developed within the EC- LIFE+ project "DIAPASON" as an upgrade of the commercial, single-channel Jenoptik CHM15k system. The PLC run continuously (h24) close to Rome (Italy) for a whole year (2013-2014). Retrievals of the aerosol backscatter coefficient at 1064 nm and of the relevant aerosol properties were performed using the proposed methodology. This information, coupled to some key aerosol type identification made possible by the depolarization channel, allowed a year-round characterization of the aerosol field at this site. Examples are given to show how this technology coupled to appropriate data inversion methods is potentially useful in the operational monitoring of parameters of air quality and meteorological interest.

Retrieve Aerosol Concentration Based On Surface Model and Distribution of Concentration of PM2.5 ——A Case Study of Beijing

NASA Astrophysics Data System (ADS)

Cui, H.

2017-12-01

As China's economy continues to grow, urbanization continues to advance, along with growth in all areas to pollutant emissions in the air industry, air quality also continued to deteriorate. Aerosol concentrations as a measure of air quality of the most important part of are more and more people's attention. Traditional monitoring stations measuring aerosol concentration method is accurate, but time-consuming and can't be done simultaneously measure a large area, can only rely on data from several monitoring sites to predict the concentration of the panorama. Remote Sensing Technology retrieves aerosol concentrations being by virtue of their efficient, fast advantages gradually into sight. In this paper, by the method of surface model to start with the physical processes of atmospheric transport, innovative aerosol concentration coefficient proposed to replace the traditional aerosol concentrations, pushed to a set of retrieval of aerosol concentration coefficient method, enabling fast and efficient Get accurate air pollution target area. At the same paper also monitoring data for PM2.5 in Beijing were analyzed from different angles, from the perspective of the data summarized in Beijing PM2.5 concentration of time, space, geographical distribution and concentration of PM2.5 and explored the relationship between aerosol concentration coefficient and concentration of PM2.5.

Final Project Report - ARM CLASIC CIRPAS Twin Otter Aerosol

DOE Office of Scientific and Technical Information (OSTI.GOV)

John A. Ogren

2010-04-05

The NOAA/ESRL/GMD aerosol group made three types of contributions related to airborne measurements of aerosol light scattering and absorption for the Cloud and Land Surface Interaction Campaign (CLASIC) in June 2007 on the Twin Otter research airplane operated by the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS). GMD scientists served as the instrument mentor for the integrating nephelometer and particle soot absorption photometer (PSAP) on the Twin Otter during CLASIC, and were responsible for (1) instrument checks/comparisons; (2) instrument trouble shooting/repair; and (3) data quality control (QC) and submittal to the archive.

Temporal Characteristics of Brown Carbon over the Central Indo-Gangetic Plain.

PubMed

Satish, Rangu; Shamjad, Puthukkadan; Thamban, Navaneeth; Tripathi, Sachchida; Rastogi, Neeraj

2017-06-20

Recent global models estimate that light absorption by brown carbon (BrC) in several regions of the world is ∼30-70% of that due to black carbon (BC). It is, therefore, important to understand its sources and characteristics on temporal and spatial scales. In this study, we conducted semicontinuous measurements of water-soluble organic carbon (WSOC) and BrC using particle-into-liquid sampler coupled with a liquid waveguide capillary cell and total organic carbon analyzer (PILS-LWCC-TOC) over Kanpur (26.5°N, 80.3°E, 142 m amsl) during a winter season (December 2015 to February 2016). In addition, mass concentrations of organic and inorganic aerosol and BC were also measured. Diurnal variability in the absorption coefficient of BrC at 365 nm (b abs_365 ) showed higher values (35 ± 21 Mm -1 ) during late evening to early morning hours and was attributed to primary emissions from biomass burning (BB) and fossil fuel burning (FFB). The b abs_365 reduced by more than 80% as the day progressed, which was ascribed to photo bleaching/volatilization of BrC and/or due to rising boundary layer height. Further, diurnal variability in the ratios of b abs_405 /b abs_365 and b abs_420 /b abs_365 suggests that the BrC composition was not uniform throughout a day. WSOC exhibited a strong correlation with b abs_365 (slope = 1.22 ± 0.007, r 2 = 0.70, n = 13 265, intercept = -0.69 ± 0.17), suggesting the presence of a significant but variable fraction of chromophores. Mass absorption efficiency (MAE) values of WSOC ranged from 0.003 to 5.26 m 2 g -1 (1.16 ± 0.60) during the study period. Moderate correlation (r 2 = 0.50, slope = 1.58 ± 0.019, n = 6471) of b abs_365 was observed with the semivolatile oxygenated organic aerosols (SV-OOA) fraction of BB resolved from positive matrix factorization (PMF) analysis of organic mass spectral data obtained from a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The low-volatility OOA (LV-OOA) fraction of BB had a similar correlation to b abs_365 (r 2 = 0.54, slope = 0.38 ± 0.004, n = 6471) but appears to have a smaller contribution to the absorption.

Black and Brown Carbon in Biogenic Settings with Different Levels of Anthropogenic Influence, and The Effect of Semivolatile Compounds on Aerosol Optical Properties

NASA Astrophysics Data System (ADS)

Tasoglou, A.; Ramachandran, S.; Khlystov, A.; Saha, P.; Grieshop, A. P.; Pandis, S. N.

2015-12-01

Secondary organic aerosol (SOA) is a major contributor to the global aerosol burden. Black carbon (BC) is a significant climate warming agent, while light-absorbing organic carbon (brown carbon, BrC), also impacts the atmospheric radiative balance. The optical properties of ambient aerosols can be affected by biogenic SOA through the lensing effect (coating of BC cores by semivolatile SOA), and by the potential formation of BrC from biogenic sources influenced by anthropogenic sources. To evaluate these effects, measurements of ambient aerosol optical properties and BC concentrations were made in rural Centreville, AL (a remote site with little anthropogenic influence) in summer 2013 and at Duke Forest in Chapel Hill, NC (a site close to high density vehicular traffic and industrial sources), during summer 2015. Photoacoustic extinctiometers (PAX, 405 nm and 532 nm) measured particulate light absorption and a single particle soot photometer (SP2) measured BC mass at both locations. A seven-wavelength Aethalometer and a three-wavelength nephelometer were also deployed at Duke Forest. A third PAX (870 nm) was deployed at Centreville. For absorption and BC measurements, the sample was cycled between a dry line and a dry/thermally-denuded line. Hourly samples were collected with a steam jet aerosol collector (SJAC) for online (2013) and offline (2015) chemical composition analysis. BC concentrations were generally higher at Duke Forest compared to the rural Centreville site. The Aethalometer readings at Duke Forest show greater absorption at the shorter wavelengths (370 nm and 470 nm) than expected from the absorption at 880 nm coupled with an inverse wavelength dependence, suggesting the presence of brown carbon. This presentation will examine the evidence for brown carbon at the two sites, as well as the effect of non-BC coatings on BC light absorption (the lensing effect.)

Infrared spectroscopy and Mie scattering of acetylene aerosols formed in a low temperature diffusion cell

NASA Technical Reports Server (NTRS)

Dunder, T.; Miller, R. E.

1990-01-01

A method is described for forming and spectroscopically characterizing cryogenic aerosols formed in a low temperature gas cell. By adjusting the cell pressure, gas composition and flow rate, the size distribution of aerosol particles can be varied over a wide range. The combination of pressure and flow rate determine the residence time of the aerosols in the cell and hence the time available for the particles to grow. FTIR spectroscopy, over the range from 600/cm to 6000/cm, is used to characterize the aerosols. The particle size distribution can be varied so that, at one extreme, the spectra show only absorption features associated with the infrared active vibrational bands and, at the other, they display both absorption and Mie scattering. In the latter case, Mie scattering theory is used to obtain semiquantitative aerosol size distributions, which can be understood in terms of the interplay between nucleation and condensation. In the case of acetylene aerosols, the infrared spectra suggest that the particles exist in the high temperature cubic phase of the solid.

Heterogeneous Uptake of HO2 Radicals onto Submicron Atmospheric Aerosols

NASA Astrophysics Data System (ADS)

Matthews, P. S.; George, I. J.; Brooks, B.; Whalley, L. K.; Baeza-Romero, M. T.; Heard, D. E.

2012-12-01

OH and HO2 (HOx) radicals are closely coupled and OH is responsible for the majority of the oxidation in the troposphere and controls the concentrations of many trace species. Therefore, it is important to be able to accurately predict HOx concentrations. However, some field measurement studies have reported significantly lower HO2 radical concentrations than calculated by constrained box models using detailed chemical mechanisms. Although the inclusion of halogen chemistry into the mechanisms can explain much of the differences in the marine boundary layer (MBL) (1,2), HO2 uptake by aerosols has been suggested as a possible sink in the MBL (2), the Arctic troposphere (3) and the upper troposphere (4). There have been very few laboratory studies (5,6) on HO2 uptake by aerosols and the rates and mechanism is still uncertain. The HO2 uptake coefficients were measured for a variety of atmospherically relevant inorganic and organic aerosols. The measurements were performed using an aerosol flow tube combined with a Fluorescence Assay by Gas Expansion (FAGE) detector. The sensitive FAGE cell allowed low HO2 concentrations (108-109 molecule cm-3) to be injected into the flow tube using a moveable injector. By moving the injector along the flow tube, position dependent HO2 decays were able to be recorded which when plotted against the total aerosol surface area allowed an uptake coefficient to be obtained. The aerosols were generated using an atomiser or by homogeneous nucleation and the total aerosol surface area was measured using a Scanning Mobility Particle Sizer. The HO2 uptake coefficient (γ) was measured at room temperature for dry inorganic salts and dry organics (γ< 0.004), wet inorganic salts and wet organics (γ= 0.002-0.005), wet copper doped ammonium sulfate aerosols (γ= 0.28± 0.05) and ammonium sulfate aerosols doped with different molar amounts of iron (γ= 0.003-0.06). The pH dependence of the HO2 uptake coefficient was investigated, however no dependence was observed. A time dependence has been observed, with higher HO2 uptake coefficients measured at short reaction times with the uptake coefficient decreasing at longer times. A HO2 concentration dependence has also been observed whereby a higher uptake coefficient is measured at lower HO2 concentrations. The time dependence and HO2 concentration dependence may suggest an aerosol saturation mechanism. The HO2 uptake temperature dependence is currently being investigated, as well as uptake on to a wider range of inorganic and organic aerosols. This work was supported by the National Environment Research Council under grant number NE/F020651/1. PSJM is grateful to NERC for a research studentship. References (1) Sommariva, R. et al. Atmos. Chem. Phys.2006, 6, 1135-1153. (2) Whalley, L.K. et al. Atmos. Chem. Phys. 2010, 10, 1555-1576. (3) Mao, J. et al. Atmos. Chem. Phys. 2010, 10, 5823-5838. (4) Jaegle, L. et al. J. Geophys. Atm. 2000, 105, 3877-3892. (5) Taketani, F. et al. J. Phys. Chem. 2008, 112, 2370-2377. (6) Thornton, J. et al. J. Geophys. Atm. 2005, 110, D08309.

Bounding the heterogeneous gas uptake on aerosols and ground using resistance model

NASA Astrophysics Data System (ADS)

Su, H.; Li, M.; Cheng, Y.

2017-12-01

Heterogeneous uptake on aerosols and ground are potential important atmospheric sinks for gases. Different schemes have been used to characterize the dry deposition and heterogeneous aerosol gas uptake, although they share similar characteristics. In this work, we propose a unified resistance model to compare the uptake flux on both ground and aerosols, to identify the dominate heterogeneous process within the planetary boundary layer (PBL). The Gamma(eq) is introduced to represent the reactive uptake coefficient on aerosols when these two processes are equally important. It's shown that Gamma(eq) is proportional to the dry deposition velocity, inversely proportional to aerosol surface area concentration. Under typical regional background condition, Gamma(eq) vary from 1x10-5 to 4x10-4 with gas species, land-use type and season, which indicates that aerosol gas uptake should be included in atmospheric models when uptake coefficient higher than 10-5. We address the importance of heterogeneous gas uptake on aerosols over ground especially for ozone uptake on liquid organic aerosols and for marine PBL atmosphere.

Aerosol Complexity and Implications for Predictability and Short-Term Forecasting

NASA Technical Reports Server (NTRS)

Colarco, Peter

2016-01-01

There are clear NWP and climate impacts from including aerosol radiative and cloud interactions. Changes in dynamics and cloud fields affect aerosol lifecycle, plume height, long-range transport, overall forcing of the climate system, etc. Inclusion of aerosols in NWP systems has benefit to surface field biases (e.g., T2m, U10m). Including aerosol affects has impact on analysis increments and can have statistically significant impacts on, e.g., tropical cyclogenesis. Above points are made especially with respect to aerosol radiative interactions, but aerosol-cloud interaction is a bigger signal on the global system. Many of these impacts are realized even in models with relatively simple (bulk) aerosol schemes (approx.10 -20 tracers). Simple schemes though imply simple representation of aerosol absorption and importantly for aerosol-cloud interaction particle-size distribution. Even so, more complex schemes exhibit a lot of diversity between different models, with issues such as size selection both for emitted particles and for modes. Prospects for complex sectional schemes to tune modal (and even bulk) schemes toward better selection of size representation. I think this is a ripe topic for more research -Systematic documentation of benefits of no vs. climatological vs. interactive (direct and then direct+indirect) aerosols. Document aerosol impact on analysis increments, inclusion in NWP data assimilation operator -Further refinement of baseline assumptions in model design (e.g., absorption, particle size distribution). Did not get into model resolution and interplay of other physical processes with aerosols (e.g., moist physics, obviously important), chemistry

Sources, Transport, and Climate Impacts of Biomass Burning Aerosols

NASA Technical Reports Server (NTRS)

Chin, Mian

2010-01-01

In this presentation, I will first talk about fundamentals of modeling of biomass burning emissions of aerosols, then show the results of GOCART model simulated biomass burning aerosols. I will compare the model results with observations of satellite and ground-based network in terms of total aerosol optical depth, aerosol absorption optical depth, and vertical distributions. Finally the long-range transport of biomass burning aerosols and the climate effects will be addressed. I will also discuss the uncertainties associated with modeling and observations of biomass burning aerosols

Environmental Temperature Effect on the Far-Infrared Absorption Features of Aromatic-Based Titan's Aerosol Analogs

NASA Technical Reports Server (NTRS)

Gautier, Thomas; Trainer, Melissa G.; Loeffler, Mark J.; Sebree, Joshua A.; Anderson, Carrie M.

2016-01-01

Benzene detection has been reported in Titans atmosphere both in the stratosphere at ppb levels by remote sensing and in the thermosphere at ppm levels by the Cassini's Ion and Neutral Mass Spectrometer. This detection supports the idea that aromatic and heteroaromatic reaction pathways may play an important role in Titans atmospheric chemistry, especially in the formation of aerosols. Indeed, aromatic molecules are easily dissociated by ultraviolet radiation and can therefore contribute significantly to aerosol formation. It has been shown recently that aerosol analogs produced from a gas mixture containing a low concentration of aromatic and/or heteroaromatic molecules (benzene, naphthalene, pyridine, quinoline and isoquinoline) have spectral signatures below 500/cm, a first step towards reproducing the aerosol spectral features observed by Cassini's Composite InfraRed Spectrometer (CIRS) in the far infrared. In this work we investigate the influence of environmental temperature on the absorption spectra of such aerosol samples, simulating the temperature range to which aerosols, once formed, are exposed during their transport through Titans stratosphere. Our results show that environmental temperature does not have any major effect on the spectral shape of these aerosol analogs in the far-infrared, which is consistent with the CIRS observations.

Dynamic light absorption of biomass burning organic carbon photochemically aged under natural sunlight

NASA Astrophysics Data System (ADS)

Zhong, M.; Jang, M.

2013-08-01

Wood burning aerosol produced under smoldering conditions was photochemically aged with different relative humidity (RH) and NOx conditions using a 104 m3 dual outdoor chamber under natural sunlight. Light absorption of organic carbon (OC) was measured over the course of photooxidation using a UV-visible spectrometer connected to an integrating sphere. At high RH, the color decayed rapidly. NOx slightly prolonged the color of wood smoke, suggesting that NOx promotes the formation of chromophores via secondary processes. Overall, the mass absorption cross-section (integrated between 280 nm and 600 nm) of OC increased by 11-54% (except high RH) in the morning and then gradually decreased by 19-68% in the afternoon. This dynamic change in light absorption of wood burning OC can be explained by two mechanisms: chromophore formation and sunlight bleaching. To investigate the effect of chemical transformation on light absorption, wood smoke particles were characterized using various spectrometers. The intensity of fluorescence, which is mainly related to polycyclic aromatic hydrocarbons (PAHs), rapidly decreased with time indicating the potential bleaching of PAHs. A decline of levoglucosan concentrations evinced the change of POA with time. The aerosol water content measured by Fourier transform infrared spectroscopy showed that wood burning aerosol became less hygroscopic as photooxidation proceeded. A similar trend in light absorption changes has been observed in ambient smoke aerosol originating from the 2012 County Line Wildfire in Florida. We conclude that the biomass burning OC becomes less light absorbing after 8-9 h sunlight exposure compared to fresh wood burning OC.

Exploitation of the UV Aerosol Index scattering angle dependence: Properties of Siberian smoke plumes

NASA Astrophysics Data System (ADS)

Penning de Vries, Marloes; Beirle, Steffen; Sihler, Holger; Wagner, Thomas

2017-04-01

The UV Aerosol Index (UVAI) is a simple measure of aerosols from satellite that is particularly sensitive to elevated layers of absorbing particles. It has been determined from a range of instruments including TOMS, GOME-2, and OMI, for almost four decades and will be continued in the upcoming Sentinel missions S5-precursor, S4, and S5. Despite its apparent simplicity, the interpretation of UVAI is not straightforward, as it depends on aerosol abundance, absorption, and altitude in a non-linear way. In addition, UVAI depends on the geometry of the measurement (viewing angle, solar zenith and relative azimuth angles), particularly if viewing angles exceed 45 degrees, as is the case for OMI and TROPOMI (on S5-precursor). The dependence on scattering angle complicates the interpretation and further processing (e.g., averaging) of UVAI. In certain favorable cases, however, independent information on aerosol altitude and absorption may become available. We present a detailed study of the scatter angle dependence using SCIATRAN radiative transfer calculations. The model results were compared to observations of an extensive Siberian smoke plume, of which parts reached 10-12 km altitude. Due to its large extent and the high latitude, OMI observed the complete plume in five consecutive orbits under a wide range of scattering angles. This allowed us to deduce aerosol characteristics (absorption and layer height) that were compared with collocated CALIOP lidar measurements.

Photochemical Cycling of Humic-Like Substances in Atmospheric Aerosols

NASA Astrophysics Data System (ADS)

Rincon, A. G.; Guzman, M. I.; Hoffmann, M. R.; Colussi, A. J.

2007-12-01

Colored, humic-like substances (HULIS) arising from the biodegradation of organic detritus are widespread in natural surface waters, where they ultimately undergo solar photolysis into small alpha-dicarbonylic species, such as glyoxal, glyoxylic and pyruvic acids. Diversely generated and chemically dissimilar HULIS are also found in the atmospheric aerosol. How are significant levels of colored HULIS produced and sustained in the concentrated aerosol phase under intense solar irradiation? Here, this issue is tackled by investigating the solar photolysis of aqueous pyruvic acid (PA) solutions at concentrations representative of the atmospheric aerosol using UV-absorption, high resolution electrospray mass, and nuclear magnetic resonance spectrometries. Under such conditions, PA is not photodegraded but yields polyfunctional polymers, whose mass and UV-absorption spectra remain unaffected after 3, 8 and 22 h photolysis. Unless diluted, these polymers undergo condensation/polymerization in the post-photolysis period into mass < 700 Da species that absorb in the visible, and are bleached upon resuming irradiation. The re- photolyzed solutions recover the mass and UV-absorption spectra of first photolyzed solutions. Whereas initial pH has no effect on the mechanism of reaction, ammonium bisulfate, a major component of the aerosol, markedly influences these processes. These findings suggest that the chemical identity and concentration levels of complex organic substances in the aerosol are the result of dynamic photochemical processing in the condensed phase.

Automatic remote sensing detection of the convective boundary layer structure over flat and complex terrain using the novel PathfinderTURB algorithm

NASA Astrophysics Data System (ADS)

Poltera, Yann; Martucci, Giovanni; Hervo, Maxime; Haefele, Alexander; Emmenegger, Lukas; Brunner, Dominik; Henne, stephan

2016-04-01

We have developed, applied and validated a novel algorithm called PathfinderTURB for the automatic and real-time detection of the vertical structure of the planetary boundary layer. The algorithm has been applied to a year of data measured by the automatic LIDAR CHM15K at two sites in Switzerland: the rural site of Payerne (MeteoSwiss station, 491 m, asl), and the alpine site of Kleine Scheidegg (KSE, 2061 m, asl). PathfinderTURB is a gradient-based layer detection algorithm, which in addition makes use of the atmospheric variability to detect the turbulent transition zone that separates two low-turbulence regions, one characterized by homogeneous mixing (convective layer) and one above characterized by free tropospheric conditions. The PathfinderTURB retrieval of the vertical structure of the Local (5-10 km, horizontal scale) Convective Boundary Layer (LCBL) has been validated at Payerne using two established reference methods. The first reference consists of four independent human-expert manual detections of the LCBL height over the year 2014. The second reference consists of the values of LCBL height calculated using the bulk Richardson number method based on co-located radio sounding data for the same year 2014. Based on the excellent agreement with the two reference methods at Payerne, we decided to apply PathfinderTURB to the complex-terrain conditions at KSE during 2014. The LCBL height retrievals are obtained by tilting the CHM15K at an angle of 19 degrees with respect to the horizontal and aiming directly at the Sphinx Observatory (3580 m, asl) on the Jungfraujoch. This setup of the CHM15K and the processing of the data done by the PathfinderTURB allows to disentangle the long-transport from the local origin of gases and particles measured by the in-situ instrumentation at the Sphinx Observatory. The KSE measurements showed that the relation amongst the LCBL height, the aerosol layers above the LCBL top and the gas + particle concentration is all but trivial. Retrieving the structure of the LCBL along the line of sight connecting KSE to the Sphinx Observatory allows to monitor when the LCBL top reaches the altitude of the in-situ instrumentation at the Sphinx and to relate the measured gas + particle concentration with the locally-produced aerosols. On the other hand, when the LCBL top is lower than the Sphinx altitude, the measured concentration of gas + particle at the Sphinx is either due to long transport of aerosols (>100 km) or to the residual aerosol layer reaching the Sphinx's height or to non-local (> 5 km and <100 km) CBL aerosols advected at the Sphinx's height. Except when the aerosol layer is decoupled from the LCBL underneath, for all the other cases the CHM15K sees the probed layer as a continuous (not necessarily well-mixed) aerosol layer starting at the KSE surface. The depth of this continuous layer has been retrieved by the PathfinderTURB and related with the black carbon absorption coefficient measured at Sphinx. The result of the comparison shows clearly that the depth of the layer is well correlated with the absorption coefficient measured at the Sphinx. This is an important result that allows not only to retrieve real-time CBL heights in an automatic and trustworthy way, but also to adapt the retrievals to complex-terrain and complex-atmospheric conditions with customized tilted instrument settings.

Smoke and Pollution Aerosol Effect on Cloud Cover

NASA Technical Reports Server (NTRS)

Kaufman, Yoram J.; Koren, Ilan

2006-01-01

Pollution and smoke aerosols can increase or decrease the cloud cover. This duality in the effects of aerosols forms one of the largest uncertainties in climate research. Using solar measurements from Aerosol Robotic Network sites around the globe, we show an increase in cloud cover with an increase in the aerosol column concentration and an inverse dependence on the aerosol absorption of sunlight. The emerging rule appears to be independent of geographical location or aerosol type, thus increasing our confidence in the understanding of these aerosol effects on the clouds and climate. Preliminary estimates suggest an increase of 5% in cloud cover.

Estimation of the absorption coefficients of two-layered media by a simple method using spatially and time-resolved reflectances

NASA Astrophysics Data System (ADS)

Shimada, M.; Sato, C.; Hoshi, Y.; Yamada, Y.

2009-08-01

Our newly developed method using spatially and time-resolved reflectances can easily estimate the absorption coefficients of each layer in a two-layered medium if the thickness of the upper layer and the reduced scattering coefficients of the two layers are known a priori. We experimentally validated this method using phantoms and examined its possibility of estimating the absorption coefficients of the tissues in human heads. In the case of a homogeneous plastic phantom (polyacetal block), the absorption coefficient estimated by our method agreed well with that obtained by a conventional method. Also, in the case of two-layered phantoms, our method successfully estimated the absorption coefficients of the two layers. Furthermore, the absorption coefficients of the extracerebral and cerebral tissue inside human foreheads were estimated under the assumption that the human heads were two-layered media. It was found that the absorption coefficients of the cerebral tissues were larger than those of the extracerebral tissues.

Aerosol absorption measurements and retrievals in shadow2 campaign

NASA Astrophysics Data System (ADS)

Hu, Qiaoyun; Goloub, Philippe; Podvin, Thierry; Veselovskiy, Igor; Lopatin, Anton; Dubovik, Oleg; Torres, Benjamìn; Revilini, Laura; Crumeyrolle, Suzanne; Lapionak, Tatsiana; Deroo, Christine

2018-04-01

Dust, maritime and dust-smoke mixture events observed during SHADOW2 (SaHAran Dust Over West Africa) field campaign are selected and analyzed by using Raman and GARRLiC retrievals. The derived aerosol optical and microphysical properties will be shown. Dust absorption profile and on ground level are derived from GARRLiC retrievals and Aethalometer measurements, respectively. Our results provide a closer insight about dust absorbing properties.

A study of aerosol absorption and height retrievals with a hyperspectral (UV to NIR) passive sensor

NASA Astrophysics Data System (ADS)

Gasso, S.

2017-12-01

With the deployment of the first sensor (TOMS, in 1978) with capabilities to detect aerosol absorption (AA) from space, there has been a continuous evolution in hardware and algorithms used to measured this property. Although with TOMS and its more advanced successors (such as OMI) made significant progress in globally characterizing AA , there is room for improvement especially by taking advantage of sensors with extended spectral coverage (UV to NIR) and high spatial resolution (<1 km). While such unique sensor does not exist yet, the collocation of observations from different platforms that jointly fulfill those characteristics (e.g. A-Train, S-NPP) confirm that it is possible to fully retrieve all AA parameters that modulate absorption in the upwelling radiance (AOD, SSA and aerosol layer height). However, such combined approaches still have some drawbacks such as the difficulty to account for cloud contamination. The upcoming deployment of satellite detectors with the desired features all in one sensor (PACE, TropOMI, GEMS) prompt a revision of the AA retrieval technique used in past approaches. In particular,the TropOMI mission, a hyperspectral UV-to-NIR sensor with moderate ( 5km nadir pixel) spatial resolution to be launched in Fall 2017. In addition , the sensor will include sensing capabilities for the wavelength range of the Oxygen bands A and B at very high wavelength resolution. This study will be centered on the aerosol detection capabilities of TropOMI. Because the spectral range covered, it is theoretically possible to simultaneously retrieve the aerosol optical depth, the single scattering albedo and aerosol mean height without assuming any of them as it was the case with previous retrieval approaches. Specifically, we intend to present a theoretical study based on simulated radiances at selected UV, VIS and near-IR bands (including the Oxygen bands) and evaluate the sensitivity of this sensor to different levels of aerosol concentration, height and absorption properties (imaginary index) along with particle size distribution.

Lidar Remote Sensing for Industry and Environment Monitoring

NASA Technical Reports Server (NTRS)

Singh, Upendra N. (Editor); Itabe, Toshikazu (Editor); Sugimoto, Nobuo (Editor)

2000-01-01

Contents include the following: 1. Keynote paper: Overview of lidar technology for industrial and environmental monitoring in Japan. 2. lidar technology I: NASA's future active remote sensing mission for earth science. Geometrical detector consideration s in laser sensing application (invited paper). 3. Lidar technology II: High-power femtosecond light strings as novel atmospheric probes (invited paper). Design of a compact high-sensitivity aerosol profiling lidar. 4. Lasers for lidars: High-energy 2 microns laser for multiple lidar applications. New submount requirement of conductively cooled laser diodes for lidar applications. 5. Tropospheric aerosols and clouds I: Lidar monitoring of clouds and aerosols at the facility for atmospheric remote sensing (invited paper). Measurement of asian dust by using multiwavelength lidar. Global monitoring of clouds and aerosols using a network of micropulse lidar systems. 6. Troposphere aerosols and clouds II: Scanning lidar measurements of marine aerosol fields at a coastal site in Hawaii. 7. Tropospheric aerosols and clouds III: Formation of ice cloud from asian dust particles in the upper troposphere. Atmospheric boundary layer observation by ground-based lidar at KMITL, Thailand (13 deg N, 100 deg. E). 8. Boundary layer, urban pollution: Studies of the spatial correlation between urban aerosols and local traffic congestion using a slant angle scanning on the research vessel Mirai. 9. Middle atmosphere: Lidar-observed arctic PSC's over Svalbard (invited paper). Sodium temperature lidar measurements of the mesopause region over Syowa Station. 10. Differential absorption lidar (dIAL) and DOAS: Airborne UV DIAL measurements of ozone and aerosols (invited paper). Measurement of water vapor, surface ozone, and ethylene using differential absorption lidar. 12. Space lidar I: Lightweight lidar telescopes for space applications (invited paper). Coherent lidar development for Doppler wind measurement from the International Space Station. 13. Space lidar II: Using coherent Doppler lidar to estimate river discharge. 14. Poster session: Lidar technology, optics for lidar. Laser for lidar. Middle atmosphere observations. Tropospheric observations (aerosols, clouds). Boundary layer, urban pollution. Differential absorption lidar. Doppler lidar. and Space lidar.

Modelling the light absorption coefficients of oceanic waters: Implications for underwater optical applications

NASA Astrophysics Data System (ADS)

Prabhakaran, Sai Shri; Sahu, Sanjay Kumar; Dev, Pravin Jeba; Shanmugam, Palanisamy

2018-05-01

Spectral absorption coefficients of particulate (algal and non-algal components) and dissolved substances are modelled and combined with the pure seawater component to determine the total light absorption coefficients of seawater in the Bay of Bengal. Two parameters namely chlorophyll-a (Chl) concentration and turbidity were measured using commercially available instruments with high sampling rates. For modelling the light absorption coefficients of oceanic waters, the measured data are classified into two broad groups - algal dominant and non-algal particle (NAP) dominant. With these criteria the individual absorption coefficients of phytoplankton and NAP were established based on their concentrations using an iterative method. To account for the spectral dependence of absorption by phytoplankton, the wavelength-dependent coefficients were introduced into the model. The CDOM absorption was determined by subtracting the individual absorption coefficients of phytoplankton and NAP from the measured total absorption data and then related to the Chl concentration. Validity of the model is assessed based on independent in-situ data from certain discrete locations in the Bay of Bengal. The total absorption coefficients estimated using the new model by considering the contributions of algal, non-algal and CDOM have good agreement with the measured total absorption data with the error range of 6.9 to 28.3%. Results obtained by the present model are important for predicting the propagation of the radiant energy within the ocean and interpreting remote sensing observation data.

Simulating return signals of a spaceborne high-spectral resolution lidar channel at 532 nm

NASA Astrophysics Data System (ADS)

Xiao, Yu; Binglong, Chen; Min, Min; Xingying, Zhang; Lilin, Yao; Yiming, Zhao; Lidong, Wang; Fu, Wang; Xiaobo, Deng

2018-06-01

High spectral resolution lidar (HSRL) system employs a narrow spectral filter to separate the particulate (cloud/aerosol) and molecular scattering components in lidar return signals, which improves the quality of the retrieved cloud/aerosol optical properties. To better develop a future spaceborne HSRL system, a novel simulation technique was developed to simulate spaceborne HSRL return signals at 532 nm using the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) cloud/aerosol extinction coefficients product and numerical weather prediction data. For validating simulated data, a mathematical particulate extinction coefficient retrieval method for spaceborne HSRL return signals is described here. We compare particulate extinction coefficient profiles from the CALIPSO operational product with simulated spaceborne HSRL data. Further uncertainty analysis shows that relative uncertainties are acceptable for retrieving the optical properties of cloud and aerosol. The final results demonstrate that they agree well with each other. It indicates that the return signals of the spaceborne HSRL molecular channel at 532 nm will be suitable for developing operational algorithms supporting a future spaceborne HSRL system.

Intercomparison of shortwave radiative transfer schemes in global aerosol modeling: results from the AeroCom Radiative Transfer Experiment

NASA Astrophysics Data System (ADS)

Randles, C. A.; Kinne, S.; Myhre, G.; Schulz, M.; Stier, P.; Fischer, J.; Doppler, L.; Highwood, E.; Ryder, C.; Harris, B.; Huttunen, J.; Ma, Y.; Pinker, R. T.; Mayer, B.; Neubauer, D.; Hitzenberger, R.; Oreopoulos, L.; Lee, D.; Pitari, G.; Di Genova, G.; Quaas, J.; Rose, Fred G.; Kato, S.; Rumbold, S. T.; Vardavas, I.; Hatzianastassiou, N.; Matsoukas, C.; Yu, H.; Zhang, F.; Zhang, H.; Lu, P.

2012-12-01

In this study we examine the performance of 31 global model radiative transfer schemes in cloud-free conditions with prescribed gaseous absorbers and no aerosols (Rayleigh atmosphere), with prescribed scattering-only aerosols, and with more absorbing aerosols. Results are compared to benchmark results from high-resolution, multi-angular line-by-line radiation models. For purely scattering aerosols, model bias relative to the line-by-line models in the top-of-the atmosphere aerosol radiative forcing ranges from roughly -10 to 20%, with over- and underestimates of radiative cooling at higher and lower sun elevation, respectively. Inter-model diversity (relative standard deviation) increases from ~10 to 15% as sun elevation increases. Inter-model diversity in atmospheric and surface forcing decreases with increased aerosol absorption, indicating that the treatment of multiple-scattering is more variable than aerosol absorption in the models considered. Aerosol radiative forcing results from multi-stream models are generally in better agreement with the line-by-line results than the simpler two-stream schemes. Considering radiative fluxes, model performance is generally the same or slightly better than results from previous radiation scheme intercomparisons. However, the inter-model diversity in aerosol radiative forcing remains large, primarily as a result of the treatment of multiple-scattering. Results indicate that global models that estimate aerosol radiative forcing with two-stream radiation schemes may be subject to persistent biases introduced by these schemes, particularly for regional aerosol forcing.

Intercomparison of shortwave radiative transfer schemes in global aerosol modeling: results from the AeroCom Radiative Transfer Experiment

NASA Astrophysics Data System (ADS)

Randles, C. A.; Kinne, S.; Myhre, G.; Schulz, M.; Stier, P.; Fischer, J.; Doppler, L.; Highwood, E.; Ryder, C.; Harris, B.; Huttunen, J.; Ma, Y.; Pinker, R. T.; Mayer, B.; Neubauer, D.; Hitzenberger, R.; Oreopoulos, L.; Lee, D.; Pitari, G.; Di Genova, G.; Quaas, J.; Rose, F. G.; Kato, S.; Rumbold, S. T.; Vardavas, I.; Hatzianastassiou, N.; Matsoukas, C.; Yu, H.; Zhang, F.; Zhang, H.; Lu, P.

2013-03-01

In this study we examine the performance of 31 global model radiative transfer schemes in cloud-free conditions with prescribed gaseous absorbers and no aerosols (Rayleigh atmosphere), with prescribed scattering-only aerosols, and with more absorbing aerosols. Results are compared to benchmark results from high-resolution, multi-angular line-by-line radiation models. For purely scattering aerosols, model bias relative to the line-by-line models in the top-of-the atmosphere aerosol radiative forcing ranges from roughly -10 to 20%, with over- and underestimates of radiative cooling at lower and higher solar zenith angle, respectively. Inter-model diversity (relative standard deviation) increases from ~10 to 15% as solar zenith angle decreases. Inter-model diversity in atmospheric and surface forcing decreases with increased aerosol absorption, indicating that the treatment of multiple-scattering is more variable than aerosol absorption in the models considered. Aerosol radiative forcing results from multi-stream models are generally in better agreement with the line-by-line results than the simpler two-stream schemes. Considering radiative fluxes, model performance is generally the same or slightly better than results from previous radiation scheme intercomparisons. However, the inter-model diversity in aerosol radiative forcing remains large, primarily as a result of the treatment of multiple-scattering. Results indicate that global models that estimate aerosol radiative forcing with two-stream radiation schemes may be subject to persistent biases introduced by these schemes, particularly for regional aerosol forcing.

Studies on absorption coefficient near edge of multi elements

NASA Astrophysics Data System (ADS)

Eisa, M. H.; Shen, H.; Yao, H. Y.; Mi, Y.; Zhou, Z. Y.; Hu, T. D.; Xie, Y. N.

2005-12-01

X-ray absorption near edge structure (XANES) was used to study the near edge mass-absorption coefficients of seven elements, such as, Ti, V, Fe, Co, Ni, Cu and Zn. It is well known that, on the near edge absorption of element, when incident X-ray a few eV change can make the absorption coefficient an order magnitude alteration. So that, there are only a few points mass-absorption coefficient at the near edge absorption and that always average value in published table. Our results showed a wide range of data, the total measured data of mass-absorption coefficient of the seven elements was about 505. The investigation confirmed that XANES is useful technique for multi-element absorption coefficient measurement. Details of experimental methods and results are given and discussed. The experimental work has been performed at Beijing Synchrotron Radiation Facility. The measured values were compared with the published data. Good agreement between experimental results and published data is obtained.

Impacts of Aerosol Direct Effects on the South Asian climate: Assessment of Radiative Feedback Processes Using Model Simulations and Satellite/surface Measurements

NASA Astrophysics Data System (ADS)

Wang, S.; Gautam, R.; Lau, W. K.; Tsay, S.; Sun, W.; Kim, K.; Chern, J.; Colarco, P. R.; Hsu, N. C.; Lin, N.

2011-12-01

Current assessment of aerosol radiative effect is hindered by our incomplete knowledge of aerosol optical properties, especially absorption, and our current inability to quantify physical and microphysical processes. In this research, we investigate direct aerosol radiative effect over heavy aerosol loading areas (e.g., Indo-Gangetic Plains, South/East Asia) and its feedbacks on the South Asian climate during the pre-monsoon season (March-June) using the Purdue Regional Climate Model (PRCM) with prescribed aerosol data derived by the NASA Goddard Earth Observing System Model (GEOS-5). Our modeling domain covers South and East Asia (60-140E and 0-50N) with spatial resolutions of 45 km in horizontal and 28 layers in vertical. The model is integrated from 15 February to 30 June 2008 continuously without nudging (i.e., only forced by initial/boundary conditions). Two numerical experiments are conducted with and without the aerosol-radiation effects. Both simulations are successful in reproducing the synoptic patterns on seasonal-to-interannual time scales and capturing a pre-monsoon feature of the northward rainfall propagation over Indian region in early June which shown in Tropical Rainfall Measuring Mission (TRMM) observation. Preliminary result suggests aerosol-radiation interactions mainly alter surface-atmosphere energetics and further result in an adjustment of the vertical temperature distribution in lower atmosphere (below 700 hPa). The modifications of temperature and associated rainfall and circulation feedbacks on the regional climate will be discussed in the presentation. In addition to modeling study, we will also present the most recent results on aerosol properties, regional aerosol absorption, and radiative forcing estimation based on NASA's operational satellite and ground-based remote sensing. Observational results show spatial gradients in aerosol loading and solar absorption accounting over Indo-Gangetic Plains during the pre-monsoon season. The direct radiative forcing of aerosols at surface to be -19-23 Wm-2 (12-15 % of the surface solar insolation) over NW India is estimated using an observational approach. A comparison of aerosol radiative forcing between numerical simulation and observational estimate will be presented. Overall, this work will demonstrate the aerosol direct effects from both modeling and observation perspectives, and further to assess the physical processes underlying the aerosol radiative feedbacks and possible impacts on the large-scale South Asian monsoon system.

Noninvasive photoacoustic measurement of absorption coefficient using internal light irradiation of cylindrical diffusing fiber

NASA Astrophysics Data System (ADS)

Peng, Dong-qing; Zhu, Li-li; Li, Zhi-fang; Li, Hui

2017-09-01

Absorption coefficient of biological tissue is an important parameter in biomedicine, but its determination remains a challenge. In this paper, we propose a method using focusing photoacoustic imaging technique and internal light irradiation of cylindrical diffusing fiber (CDF) to quantify the target optical absorption coefficient. Absorption coefficients for ink absorbers are firstly determined through photoacoustic and spectrophotometric measurements at the same excitation, which demonstrates the feasibility of this method. Also, the optical absorption coefficients of ink absorbers with several concentrations are measured. Finally, the two-dimensional scanning photoacoustic image is obtained. Optical absorption coefficient measurement and simultaneous photoacoustic imaging of absorber non-invasively are the typical characteristics of the method. This method can play a significant role for non-invasive determination of blood oxygen saturation, the absorption-based imaging and therapy.

Optical constants of ammonium sulfate in the infrared. [stratospheric aerosol refractive and absorption indices

NASA Technical Reports Server (NTRS)

Downing, H. D.; Pinkley, L. W.; Sethna, P. P.; Williams, D.

1977-01-01

The infrared spectral reflectance at near normal incidence has been measured for 3.2 M, 2.4 M, and 1.6 M solutions of ammonium sulfate, an aerosol abundant in the stratosphere and also present in the troposphere. Kramers-Kronig analysis was used to determine values of the refractive and absorption indices from the measured spectral reflectance. A synthetic spectrum of crystalline ammonium sulfate was obtained by extrapolation of the absorption index obtained for the solution to the absorber number densities of the NH4 and SO4 ions characteristic of the crystal.

Glyoxal in aqueous ammonium sulfate solutions: products, kinetics and hydration effects.

PubMed

Yu, Ge; Bayer, Amanda R; Galloway, Melissa M; Korshavn, Kyle J; Fry, Charles G; Keutsch, Frank N

2011-08-01

Reactions and interactions between glyoxal and salts in aqueous solution were studied. Glyoxal was found to react with ammonium to form imidazole, imidazole-2-carboxaldehyde, formic acid, N-glyoxal substituted imidazole, and minor products at very low concentrations. Overall reaction orders and rates for each major product were measured. Sulfate ions have a strong and specific interaction with glyoxal in aqueous solution, which shifts the hydration equilibria of glyoxal from the unhydrated carbonyl form to the hydrated form. This ion-specific effect contributes to the observed enhancement of the effective Henry's law coefficient for glyoxal in sulfate-containing solutions. The results of UV-vis absorption and NMR spectroscopy studies of solutions of glyoxal with ammonium, methylamine, and dimethylamine salts reveal that light absorbing compounds require the formation of nitrogen containing molecules. These findings have implications on the role of glyoxal in the atmosphere, both in models of the contribution of glyoxal to form secondary organic aerosol (SOA), the role of nitrogen containing species for aerosol optical properties and in predictions of the behavior of other carbonyls or dicarbonyls in the atmosphere.

A method for estimating the incident PAR on inclined surfaces

NASA Astrophysics Data System (ADS)

Xie, Xiaoping; Gao, Wei; Gao, Zhiqiang

2008-08-01

A new simple model has been developed that incorporates Digital Elevation Model (DEM) and Moderate Resolution Imaging Spectroradiometer (MODIS) products to produce incident photosynthetically active radiation (PAR) for tilted surface. The method is based on a simplification of the general radiative transfer equation, which considers five major processes of attenuation of solar radiation: 1) Rayleigh scattering, 2) absorption by ozone and water vapor, 3) aerosol scattering, 4) multiple reflectance between surface and atmosphere, and 5) three terrain factors: slope and aspect, isotropic sky view factor, and additional radiation by neighbor reflectance. A comparison of the model results with observational data from the Yucheng and Changbai Mountain sites of the Chinese Ecosystem Research Network (CERN) shows the correlation coefficient as 0.929 and 0.904, respectively. A comparison of the model results with the 2006 filed measured PAR in the Yucheng and Changbai sites shows the correlation coefficient as 0.929 and 0.904, respectively, and the average percent error as 10% and 15%, respectively.

Application of FIGAERO (Filter Inlet for Gases and AEROsol) coupled to a high resolution time of flight chemical ionization mass spectrometer to field and chamber organic aerosol: Implications for carboxylic acid formation and gas-particle partitioning from monoterpene oxidation

NASA Astrophysics Data System (ADS)

Lopez-Hilfiker, F.; Mohr, C.; Ehn, M.; Rubach, F.; Mentel, T. F.; Kleist, E.; Wildt, J.; Thornton, J. A.

2013-12-01

We present measurements of a large suite of gas and particle phase carboxylic acid containing compounds made with a Filter Inlet for Gas and AEROsol (FIGAERO) coupled to a high resolution time of flight chemical ionization mass spectrometer (HR-ToF-CIMS) developed at the University of Washington. A prototype operated with acetate negative ion proton transfer chemistry was deployed on the Julich Plant Atmosphere Chamber to study a-pinene oxidation, and a modified version was deployed at the SMEAR II forest station in Hyytiälä, Finland and SOAS, in Brent Alabama. We focus here on results from JPAC and Hyytiälä, where we utilized the same ionization method most selective towards carboxylic acids. In all locations, 100's of organic acid compounds were observed in the gas and particles and many of the same composition acids detected in the gas-phase were detected in the particles upon temperature programmed thermal desorption. Particulate organics detected by FIGAERO are highly correlated with organic aerosol mass measured by an AMS, providing additional volatility and molecular level information about collected aerosol. The fraction of a given compound measured in the particle phase follows expected trends with elemental composition, but many compounds would not be well described by an absorptive partitioning model assuming unity activity coefficients. Moreover the detailed structure in the thermal desorption signals reveals a contribution from thermal decomposition of large molecular weight organics and or oligomers with implications for partitioning measurements and model validation

Optical properties of size-resolved particles at a Hong Kong urban site during winter

NASA Astrophysics Data System (ADS)

Gao, Yuan; Lai, Senchao; Lee, Shun-Cheng; Yau, Pui Shan; Huang, Yu; Cheng, Yan; Wang, Tao; Xu, Zheng; Yuan, Chao; Zhang, Yingyi

2015-03-01

Visibility degradation in Hong Kong is related to the city's serious air pollution problems. To investigate the aerosols' optical properties and their relationship with the chemical composition and size distribution of the particles, a monitoring campaign was conducted at an urban site in the early winter period (from October to December, 2010). The particle light scattering coefficient (Bsp) and absorption coefficient (Bap) were measured. Two collocated Micro-Orifice Uniform Deposit Impactor samplers (MOUDI110, MSP, USA) with nominal 50% cut-off aerodynamic diameters of 18, 10, 5.6, 3.2, 1.8, 1, 0.56, 0.32, 0.18, 0.1, and 0.056 μm were used to collect size-resolved particle samples. The average Bsp and Bap were 201.96 ± 105.82 Mm- 1 and 39.91 ± 19.16 Mm- 1, with an average single scattering albedo (ωo) of 0.82 ± 0.07. The theoretical method of light extinction calculation was used to determine the extinction of the size-resolved particulate matters (PM). The reconstructed light scattering coefficient correlated well with the measured scattering value in the Hong Kong urban area. Droplet mode (0.56-1.8 μm) particles contributed most to the particle light extinction (~ 69%). Organic matter, ammonium sulphate and elemental carbon were the key components causing visibility degradation in the droplet (0.56-1.8 μm) and condensation (0.1-0.56 μm) size ranges. Five sources contributing to particle light extinction have been identified using positive matrix factorisation (PMF). Traffic/engine exhausts and secondary aerosols accounted for ~ 36% and ~ 32% of particle light extinction, respectively, followed by sea salt (15%). The remaining sources, soil/fugitive dust and tire dust, contributed by ~ 10% and 7%, respectively, to particle light extinction.

Spectral changes induced by pH variation of aqueous extracts derived from biomass burning aerosols: Under dark and in presence of simulated sunlight irradiation

NASA Astrophysics Data System (ADS)

Cai, Jing; Zhi, Guorui; Yu, Zhiqiang; Nie, Peng; Gligorovski, Sasho; Zhang, Yuzhe; Zhu, Like; Guo, Xixiang; Li, Pei; He, Tan; He, Youjiang; Sun, Jianzhong; Zhang, Yang

2018-07-01

Water soluble organic carbon (WSOC) can significantly influence the aerosol optical properties and the aqueous phase chemistry in cloudwater, fogwater and aerosol liquid water. Here, we examine how the changing pH (in acidic range) affects the absorption spectra of aqueous extracts from field biomass burning aerosols, under dark conditions and in presence of simulated sunlight illumination. The observation under dark conditions indicates that pH variation from 2 to 5 induces significantly enhanced light absorbance in the wavelength ranges of 235-270 nm and 300-550 nm, whereas the light absorbance decreased in the range of 270-300 nm, which might be partially ascribed to the deprotonation of carboxylic acids and phenols. During the extract photolysis, light absorption exhibits photo-bleaching below 380 nm and photo-enhancement above 380 nm, indicating that at acidic levels (pH = 2-5), the particle extracts could undergo a significant composition evolution leading to a modification of absorptive properties. Meanwhile, after 12 h-photolysis, the acidity ([H+]) normalized by WSOC concentration in aqueous extracts ([WSOCae]) increased with a variation of Δ[H+]/[WSOCae]=(3.7 ± 0.7) × 10-7 mol mgC-1 (mean ± standard deviation), suggesting the formation of new acidic substances. Although these findings were acquired in aqueous solutions more relevant to cloud and fog water, the similar evolution likely occurs in wetted aerosols. This calls more attention to the effect of acidity on the wetted aerosols in order to better estimate the aerosol radiative forcing.

Aerosol profiling using the ceilometer network of the German Meteorological Service

NASA Astrophysics Data System (ADS)

Flentje, H.; Heese, B.; Reichardt, J.; Thomas, W.

2010-08-01

The German Meteorological Service (DWD) operates about 52 lidar ceilometers within its synoptic observations network, covering Germany. These affordable low-power lidar systems provide spatially and temporally high resolved aerosol backscatter profiles which can operationally provide quasi 3-D distributions of particle backscatter intensity. Intentionally designed for cloud height detection, recent significant improvements allow following the development of the boundary layer and to detect denser particle plumes in the free tropospere like volcanic ash, Saharan dust or fire smoke. Thus the network builds a powerful aerosol plume alerting and tracking system. If auxiliary aerosol information is available, the particle backscatter coefficient, the extinction coefficient and even particle mass concentrations may be estimated, with however large uncertainties. Therefore, large synergistic benefit is achieved if the ceilometers are linked to existing lidar networks like EARLINET or integrated into WMO's envisioined Global Aerosol Lidar Observation Network GALION. To this end, we demonstrate the potential and limitations of ceilometer networks by means of three representative aerosol episodes over Europe, namely Sahara dust, Mediterranean fire smoke and, more detailed, the Icelandic Eyjafjoll volcano eruption from mid April 2010 onwards. The DWD (Jenoptik CHM15k) lidar ceilometer network tracked the Eyjafjoll ash layers over Germany and roughly estimated peak extinction coefficients and mass concentrations on 17 April of 4-6(± 2) 10-4 m-1 and 500-750(± 300) μg/m-3, respectively, based on co-located aerosol optical depth, nephelometer (scattering coefficient) and particle mass concentration measurements. Though large, the uncertainties are small enough to let the network suit for example as aviation advisory tool, indicating whether the legal flight ban threshold of presently 2 mg/m3 is imminent to be exceeded.

A New Satellite Aerosol Retrieval Using High Spectral Resolution Oxygen A-Band Measurements

NASA Astrophysics Data System (ADS)

Winker, D. M.; Zhai, P.

2014-12-01

Efforts to advance current satellite aerosol retrieval capabilities have mostly focused on polarimetric techniques. While there has been much interest in recent decades in the use of the oxygen A-band for retrievals of cloud height or surface pressure, these techniques are mostly based on A-band measurements with relatively low spectral resolution. We report here on a new aerosol retrieval technique based on high-resolution A-band spectra. Our goal is the development of a technique to retrieve aerosol absorption, one of the critical parameters affecting the global radiation budget and one which is currently poorly constrained by satellite measurements. Our approach relies on two key factors: 1) the use of high spectral resolution measurements which resolve the A-band line structure, and 2) the use of co-located lidar profile measurements to constrain the vertical distribution of scatterers. The OCO-2 satellite, launched in July this year and now flying in formation with the CALIPSO satellite, carries an oxygen A-band spectrometer with a spectral resolution of 21,000:1. This is sufficient to resolve the A-band line structure, which contains information on atmospheric photon path lengths. Combining channels with oxygen absorption ranging from weak to strong allows the separation of atmospheric and surface scattering. An optimal estimation algorithm for simultaneous retrieval of aerosol optical depth, aerosol absorption, and surface albedo has been developed. Lidar profile data is used for scene identification and to provide constraints on the vertical distribution of scatterers. As calibrated OCO-2 data is not expected until the end of this year, the algorithm has been developed and tested using simulated OCO-2 spectra. The simulations show that AOD and surface albedo can be retrieved with high accuracy. Retrievals of aerosol single scatter albedo are encouraging, showing good performance when AOD is larger than about 0.15. Retrieval performance improves as the albedo of the underlying surface increases. Thus, the technique shows great promise for retrieving the absorption optical depth of aerosols located above clouds. This presentation will discuss the basis of the approach and results of the A-band/lidar retrievals based on simulated data.

Laboratory Studies of Water Uptake by Biomass Burning Smoke: Role of Fuel Inorganic Content, Combustion Phase and Aging

NASA Astrophysics Data System (ADS)

Dubey, M. K.; Bixler, S. L.; Romonosky, D.; Lam, J.; Carrico, C.; Aiken, A. C.

2017-12-01

Biomass burning aerosol emissions have substantially increased with observed warming and drying in the southwestern US. While wildfires are projected to intensify missing knowledge on the aerosols hampers assessments. Observations demonstrate that enhanced light absorption by coated black carbon and brown carbon can offset the cooling effects of organic aerosols in wildfires. However, if mixing processes that enhance this absorption reduce the aerosol lifetime it would lower their atmospheric burden. In order to elucidate mechanisms regulating this tradeoff we performed laboratory studies of smoke from biomass burning. We focus on aerosol optical properties and their hygroscopic response. Fresh emissions from burning 30 fuels under flaming and smoldering conditions were investigated. We measured aerosol absorption, scattering and extinction at multiple wavelengths, water uptake at 85% relative humidity (fRH85%) with a humidity controlled dual nephelometer, and black carbon mass with a SP2. Trace gases and the ionic content of the fuel and smoke were also measured We find that whereas the optical properties of smoke were strongly dictated by the flaming versus smoldering nature of the burn, the observed hygroscopicity was intimately linked to the chemical composition of the fuel. The mean hygroscopicity ranged from nearly hydrophobic (fRH85% = 1) to very hydrophilic (fRH85% = 2.1) values typical of pure deliquescent salts. The k values varied from 0.004 to 0.18 and correlated well with inorganic content. Inorganic fuel content was the key driver of hygroscopicity with combustion phase playing a secondary but important role ( 20%). Flaming combustion promoted hygroscopicity by generating refractory black carbon and ions. Smoldering combustion suppressed hygroscopicity by producing hydrogenated organic species. Wildfire smoke was hydrophobic since the evergreen species with low inorganic content dominated in these fires. We also quantify the mass absorption cross-sections at 780nm and 430nm to evaluate the absorbing species. We plan to extend our studies to aged biomass burning smoke with a potential aerosol mass reactor and monitor the ionic content of black carbon with a SP-AMS. Our analysis will develop a mechanistic framework of water uptake and optical properties of biomass burning aerosols.

Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Davidovits, Paul

Aerosols containing black carbon (and some specific types of organic particulate matter) directly absorb incoming light, heating the atmosphere. In addition, all aerosol particles backscatter solar light, leading to a net-cooling effect. Indirect effects involve hydrophilic aerosols, which serve as cloud condensation nuclei (CCN) that affect cloud cover and cloud stability, impacting both atmospheric radiation balance and precipitation patterns. At night, all clouds produce local warming, but overall clouds exert a net-cooling effect on the Earth. The effect of aerosol radiative forcing on climate may be as large as that of the greenhouse gases, but predominantly opposite in sign andmore » much more uncertain. The uncertainties in the representation of aerosol interactions in climate models makes it problematic to use model projections to guide energy policy. The objective of our program is to reduce the uncertainties in the aerosol radiative forcing in the two areas highlighted in the ASR Science and Program Plan. That is, (1) addressing the direct effect by correlating particle chemistry and morphology with particle optical properties (i.e. absorption, scattering, extinction), and (2) addressing the indirect effect by correlating particle hygroscopicity and CCN activity with particle size, chemistry, and morphology. In this connection we are systematically studying particle formation, oxidation, and the effects of particle coating. The work is specifically focused on carbonaceous particles where the uncertainties in the climate relevant properties are the highest. The ongoing work consists of laboratory experiments and related instrument inter-comparison studies both coordinated with field and modeling studies, with the aim of providing reliable data to represent aerosol processes in climate models. The work is performed in the aerosol laboratory at Boston College. At the center of our laboratory setup are two main sources for the production of aerosol particles: (a) two well-characterized source of soot particles and (b) a flow reactor for controlled OH and/or O3 oxidation of relevant gas phase species to produce well-characterized SOA particles. After formation, the aerosol particles are subjected to physical and chemical processes that simulate aerosol growth and aging. A suite of instruments in our laboratory is used to characterize the physical and chemical properties of aerosol particles before and after processing. The Time of Flight Aerosol Mass Spectrometer (ToF-AMS) together with a Scanning Mobility Particle Sizer (SMPS) measures particle mass, volume, density, composition (including black carbon content), dynamic shape factor, and fractal dimension. The–ToF-AMS was developed at ARI with Boston College participation. About 120 AMS instruments are now in service (including 5 built for DOE laboratories) performing field and laboratory studies world-wide. Other major instruments include a thermal denuder, two Differential Mobility Analyzers (DMA), a Cloud Condensation Nuclei Counter (CCN), a Thermal desorption Aerosol GC/MS (TAG) and the new Soot Particle Aerosol Mass Spectrometer (SP-AMS). Optical instrumentation required for the studies have been brought to our laboratory as part of ongoing and planned collaborative projects with colleagues from DOE, NOAA and university laboratories. Optical instruments that will be utilized include a Photoacoustic Spectrometer (PAS), a Cavity Ring Down Aerosol Extinction Spectrometer (CRD-AES), a Photo Thermal Interferometer (PTI), a new 7-wavelength Aethalometer and a Cavity Attenuated Phase Shift Extinction Monitor (CAPS). These instruments are providing aerosol absorption, extinction and scattering coefficients at a range of atmospherically relevant wavelengths. During the past two years our work has continued along the lines of our original proposal. We report on 12 completed and/or continuing projects conducted during the period 08/14 to 0814/2015. These projects are described in 17 manuscripts published in refereed journals.« less

North Atlantic Aerosol Single Scattering Albedos: TARFOX and ACE-2 Results and Their Relation to Radiative Effects Derived from Satellite Optical Depths

NASA Technical Reports Server (NTRS)

Russell, P. B.; Bergstrom, R. W.; Schmid, B.; Livingston, J. M.; Redemann, J.; Quinn, P. K.; Carrico, C. M.; Rood, M. J.

2000-01-01

Bergstrom and Russell estimated direct solar radiative flux changes caused by atmospheric aerosols over the mid-latitude North Atlantic Ocean under cloud-free and cloudy conditions. They excluded African dust aerosols, primarily by restricting calculations to latitudes 25-60 N. As inputs they used midvisible aerosol optical depth (AOD) maps derived from AVHRR satellite measurements and aerosol intensive properties determined primarily in the 1996 IGAC Troposheric Aerosol Radiative Forcing Observational Experiment (TARFOX). Those aerosol intensive properties, which included optical depth wavelength dependence and spectra of single scattering albedo (SSA) and scattering asymmetry parameter, were also checked against initial properties from the 1997 North Atlantic Aerosol Characterization Experiment (ACE 2). Bergstrom and Russell investigated the sensitivity of their derived flux changes to assumed input parameters, including midvisible AOD, SSA, and scattering asymmetry parameter. Although the sensitivity of net flux change at the tropopause to SSA was moderate over the ocean (e.g., a SSA uncertainty of 0.07 produced a flux-change uncertainty of 21%), the sensitivity over common land surfaces can be much larger. Also, flux changes within and below the aerosol layer, which affect atmospheric stability, heating rates, and cloud formation and persistence, are quite sensitive to aerosol SSA. Therefore, this paper focuses on the question: "What have we learned from TARFOX and ACE 2 regarding aerosol single scattering albedo?" Three techniques were used in TARFOX to determine midvisible SSA. One of these derived SSA as a best-fit parameter in comparing radiative flux changes measured by airborne pyranometer to those computed from aerosol properties. Another technique combined airborne measurements of aerosol scattering and absorption by nephelometer and absorption photometer. A third technique obtained SSA from best-fit complex refractive indices derived by comparing vertical profiles of lidar backscatter, sunphotometer extinction, and relative size distribution. In ACE 2 midvisible SSA was determined both as a best-fit parameter in comparing measured and calculated flux changes at the surface and by combining nephelometer and absorption photometer measurements. The nephelometer/absorption-photometer results were obtained on the ACE 2 ship (10 m asl), at the Sagres, Portugal site at 50 m asl, and also on the Pelican aircraft. This paper presents and compares the TARFOX and ACE 2 SSA results from the above techniques for different situations (e.g., marine vs continental flows, "clean" vs polluted conditions). It also discusses the strengths and limitations of the techniques, including whether they describe the aerosol in its ambient state or as perturbed by sampling processes; whether they describe the aerosol at the surface, as a function of altitude, or integrated over a column; the ease of acquiring representative data sets; results obtained in tests of consistency with radiative flux changes, and the likelihood of various artifacts and errors.

Determination of nocturnal aerosol properties from a combination of lunar photometer and lidar observations

NASA Astrophysics Data System (ADS)

Li, Donghui; Li, Zhengqiang; Lv, Yang; Zhang, Ying; Li, Kaitao; Xu, Hua

2015-10-01

Aerosol plays a key role in the assessment of global climate change and environmental health, while observation is one of important way to deepen the understanding of aerosol properties. In this study, the newly instrument - lunar photometer is used to measure moonlight and nocturnal column aerosol optical depth (AOD, τ) is retrieved. The AOD algorithm is test and verified with sun photometer both in high and low aerosol loading. Ångström exponent (α) and fine/coarse mode AOD (τf, τc) 1 is derived from spectral AOD. The column aerosol properties (τ, α, τf, τc) inferred from the lunar photometer is analyzed based on two month measurement in Beijing. Micro-pulse lidar has advantages in retrieval of aerosol vertical distribution, especially in night. However, the typical solution of lidar equation needs lidar ratio(ratio of aerosol backscatter and extinction coefficient) assumed in advance(Fernald method), or constrained by AOD2. Yet lidar ratio is varied with aerosol type and not easy to fixed, and AOD is used of daylight measurement, which is not authentic when aerosol loading is different from day and night. In this paper, the nocturnal AOD measurement from lunar photometer combined with mie scattering lidar observations to inverse aerosol extinction coefficient(σ) profile in Beijing is discussed.

On the accuracy of aerosol photoacoustic spectrometer calibrations using absorption by ozone

NASA Astrophysics Data System (ADS)

Davies, Nicholas W.; Cotterell, Michael I.; Fox, Cathryn; Szpek, Kate; Haywood, Jim M.; Langridge, Justin M.

2018-04-01

In recent years, photoacoustic spectroscopy has emerged as an invaluable tool for the accurate measurement of light absorption by atmospheric aerosol. Photoacoustic instruments require calibration, which can be achieved by measuring the photoacoustic signal generated by known quantities of gaseous ozone. Recent work has questioned the validity of this approach at short visible wavelengths (404 nm), indicating systematic calibration errors of the order of a factor of 2. We revisit this result and test the validity of the ozone calibration method using a suite of multipass photoacoustic cells operating at wavelengths 405, 514 and 658 nm. Using aerosolised nigrosin with mobility-selected diameters in the range 250-425 nm, we demonstrate excellent agreement between measured and modelled ensemble absorption cross sections at all wavelengths, thus demonstrating the validity of the ozone-based calibration method for aerosol photoacoustic spectroscopy at visible wavelengths.

Black carbon aerosol size in snow.

PubMed

Schwarz, J P; Gao, R S; Perring, A E; Spackman, J R; Fahey, D W

2013-01-01

The effect of anthropogenic black carbon (BC) aerosol on snow is of enduring interest due to its consequences for climate forcing. Until now, too little attention has been focused on BC's size in snow, an important parameter affecting BC light absorption in snow. Here we present first observations of this parameter, revealing that BC can be shifted to larger sizes in snow than are typically seen in the atmosphere, in part due to the processes associated with BC removal from the atmosphere. Mie theory analysis indicates a corresponding reduction in BC absorption in snow of 40%, making BC size in snow the dominant source of uncertainty in BC's absorption properties for calculations of BC's snow albedo climate forcing. The shift reduces estimated BC global mean snow forcing by 30%, and has scientific implications for our understanding of snow albedo and the processing of atmospheric BC aerosol in snowfall.

Analysis of DIAL/HSRL aerosol backscatter and extinction profiles during the SEAC4RS campaign with an aerosol assimilation system

NASA Astrophysics Data System (ADS)

Weaver, C. J.; da Silva, A. M., Jr.; Colarco, P. R.; Randles, C. A.

2015-12-01

We retrieve aerosol concentrations and optical information from vertical profiles of airborne 532 nm extinction and 532 and 1064 nm backscatter measurements made during the SEAC4RS summer 2013 campaign. The observations are from the High Spectral Resolution Lidar (HSRL) Airborne Differential Absorption Lidar (DIAL) on board the NASA DC-8. Instead of retrieving information about aerosol microphysical properties such as indexes of refraction, we seek information more directly applicable to an aerosol transport model - in our case the Goddard Chemistry Aerosol Radiation and Transport (GOCART) module used in the GEOS-5 Earth modeling system. A joint atmosphere/aerosol mini-reanalysis was performed for the SEAC4RS period using GEOS-5. The meteorological reanalysis followed the MERRA-2 atmospheric reanalysis protocol, and aerosol information from MODIS, MISR, and AERONET provided a constraint on the simulated aerosol optical depth (i.e., total column loading of aerosols). We focus on the simulated concentrations of 10 relevant aerosol species simulated by the GOCART module: dust, sulfate, and organic and black carbon. Our first retrieval algorithm starts with the SEAC4RS mini-reanalysis and adjusts the concentration of each GOCART aerosol species so that differences between the observed and simulated backscatter and extinction measurements are minimized. In this case, too often we are unable to simulate the observations by simple adjustment of the aerosol concentrations. A second retrieval approach adjusts both the aerosol concentrations and the optical parameters (i.e., assigned mass extinction efficiency) associated with each GOCART species. We present results from DC-8 flights over smoke from forest fires over the western US using both retrieval approaches. Finally, we compare our retrieved quantities with in-situ observations of aerosol absorption, scattering, and mass concentrations at flight altitude.

A Global Modeling Study on Carbonaceous Aerosol Microphysical Characteristics and Radiative Effects

NASA Technical Reports Server (NTRS)

Bauer, S. E.; Menon, S.; Koch, D.; Bond, T. C.; Tsigaridis, K.

2010-01-01

Recently, attention has been drawn towards black carbon aerosols as a short-term climate warming mitigation candidate. However the global and regional impacts of the direct, indirect and semi-direct aerosol effects are highly uncertain, due to the complex nature of aerosol evolution and the way that mixed, aged aerosols interact with clouds and radiation. A detailed aerosol microphysical scheme, MATRIX, embedded within the GISS climate model is used in this study to present a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative effects. Our best estimate for net direct and indirect aerosol radiative flux change between 1750 and 2000 is -0.56 W/m2. However, the direct and indirect aerosol effects are quite sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative flux change can vary between -0.32 to -0.75 W/m2 depending on these carbonaceous particle properties at emission. Taking into account internally mixed black carbon particles let us simulate correct aerosol absorption. Absorption of black carbon aerosols is amplified by sulfate and nitrate coatings and, even more strongly, by organic coatings. Black carbon mitigation scenarios generally showed reduced radiative fluxeswhen sources with a large proportion of black carbon, such as diesel, are reduced; however reducing sources with a larger organic carbon component as well, such as bio-fuels, does not necessarily lead to a reduction in positive radiative flux.

A global modeling study on carbonaceous aerosol microphysical characteristics and radiative effects

NASA Astrophysics Data System (ADS)

Bauer, S. E.; Menon, S.; Koch, D.; Bond, T. C.; Tsigaridis, K.

2010-08-01

Recently, attention has been drawn towards black carbon aerosols as a short-term climate warming mitigation candidate. However the global and regional impacts of the direct, indirect and semi-direct aerosol effects are highly uncertain, due to the complex nature of aerosol evolution and the way that mixed, aged aerosols interact with clouds and radiation. A detailed aerosol microphysical scheme, MATRIX, embedded within the GISS climate model is used in this study to present a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative effects. Our best estimate for net direct and indirect aerosol radiative flux change between 1750 and 2000 is -0.56 W/m2. However, the direct and indirect aerosol effects are quite sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative flux change can vary between -0.32 to -0.75 W/m2 depending on these carbonaceous particle properties at emission. Taking into account internally mixed black carbon particles let us simulate correct aerosol absorption. Absorption of black carbon aerosols is amplified by sulfate and nitrate coatings and, even more strongly, by organic coatings. Black carbon mitigation scenarios generally showed reduced radiative fluxeswhen sources with a large proportion of black carbon, such as diesel, are reduced; however reducing sources with a larger organic carbon component as well, such as bio-fuels, does not necessarily lead to a reduction in positive radiative flux.

Current Status of Aerosol Retrievals from TOMS

NASA Technical Reports Server (NTRS)

Torres, O.; Herman, J. R.; Bhartia, P. K.; Ginoux, P.

1999-01-01

Properties of atmospheric aerosols over all land and water surfaces are retrieved from TOMS measurements of backscattered radiances. The TOMS technique, uses observations at two wavelengths. In the near ultraviolet (330-380 nm) range, where the effects of gaseous absorption are negligible. The retrieved properties are optical depth and a measure of aerosol absorptivity, generally expressed as single scattering albedo. The main sources of error of the TOMS aerosol products are sub-pixel cloud contamination and uncertainty on the height above the surface of UV-absorbing aerosol layers. The first error source is related to the large footprint (50 x 50 km at nadir) of the sensor, and the lack of detection capability of sub-pixel size clouds. The uncertainty associated with the height of the absorbing aerosol layers, on the other hand, is related to the pressure dependence of the molecular scattering process, which is the basis of the near-UV method of absorbing aerosol detection. The detection of non-absorbing aerosols is not sensitive to aerosol layer height. We will report on the ongoing work to overcome both of these difficulties. Coincident measurements of high spatial resolution thermal infrared radiances are used to address the cloud contamination issue. Mostly clear scenes for aerosol retrieval are selected by examining the spatial homogeneity of the IR radiance measurements within a TOMS pixel. The approach to reduce the uncertainty associated with the height of the aerosol layer by making use of a chemical transport model will also be discussed.

Relationship of extinction coefficient, air pollution, and meteorological parameters in an urban area during 2007 to 2009.

PubMed

Sabetghadam, Samaneh; Ahmadi-Givi, Farhang

2014-01-01

Light extinction, which is the extent of attenuation of light signal for every distance traveled by light in the absence of special weather conditions (e.g., fog and rain), can be expressed as the sum of scattering and absorption effects of aerosols. In this paper, diurnal and seasonal variations of the extinction coefficient are investigated for the urban areas of Tehran from 2007 to 2009. Cases of visibility impairment that were concurrent with reports of fog, mist, precipitation, or relative humidity above 90% are filtered. The mean value and standard deviation of daily extinction are 0.49 and 0.39 km(-1), respectively. The average is much higher than that in many other large cities in the world, indicating the rather poor air quality over Tehran. The extinction coefficient shows obvious diurnal variations in each season, with a peak in the morning that is more pronounced in the wintertime. Also, there is a very slight increasing trend in the annual variations of atmospheric extinction coefficient, which suggests that air quality has regressed since 2007. The horizontal extinction coefficient decreased from January to July in each year and then increased between July and December, with the maximum value in the winter. Diurnal variation of extinction is often associated with small values for low relative humidity (RH), but increases significantly at higher RH. Annual correlation analysis shows that there is a positive correlation between the extinction coefficient and RH, CO, PM10, SO2, and NO2 concentration, while negative correlation exists between the extinction and T, WS, and O3, implying their unfavorable impact on extinction variation. The extinction budget was derived from multiple regression equations using the regression coefficients. On average, 44% of the extinction is from suspended particles, 3% is from air molecules, about 5% is from NO2 absorption, 0.35% is from RH, and approximately 48% is unaccounted for, which may represent errors in the data as well as contribution of other atmospheric constituents omitted from the analysis. Stronger regression equation is achieved in the summer, meaning that the extinction is more predictable in this season using pollutant concentrations.

MIE Theory Sensitivity Studies. The Effects of Aerosol Complex Refractive Index and Size Distribution Variations on Extinction and Absorption Coefficients. Part 1. Tabulated Computational Results

DTIC Science & Technology

1977-11-01

0- - - 5 43- 65 -08-0- o3630S-01 .20,428-03 .69q .200 -. 010 .36506-01 .36129-01 .37754-03 󈨉q .200 -. 025 .36608-01 .35687-01 o81707-03 6494 .200...3177Tý𔃺 t- - .-- 5 -0 1.060 1.600 -6.000 .46412-rl .41401-01 .50114=02 -- •T.73i -. 01 1• 65 !9--- .3 l-Ot-- 7 377-02 1-060 1.700 -. 003 .46537-C1 .44156-01...IAD Reports Control Symbol S OSD- 1366 1. RESEARCH AND DEVELOPMENT TECHNICAL REPORT S•ECOM-DR-77- 5 MIE THEORY SENSITIVITY STUDIES - Si THE EFFECTS OF

Assessing the influence of NOx concentrations and relative humidity on secondary organic aerosol yields from α-pinene photo-oxidation through smog chamber experiments and modelling calculations

NASA Astrophysics Data System (ADS)

Stirnweis, Lisa; Marcolli, Claudia; Dommen, Josef; Barmet, Peter; Frege, Carla; Platt, Stephen M.; Bruns, Emily A.; Krapf, Manuel; Slowik, Jay G.; Wolf, Robert; Prévôt, Andre S. H.; Baltensperger, Urs; El-Haddad, Imad

2017-04-01

Secondary organic aerosol (SOA) yields from the photo-oxidation of α-pinene were investigated in smog chamber (SC) experiments at low (23-29 %) and high (60-69 %) relative humidity (RH), various NOx / VOC ratios (0.04-3.8) and with different aerosol seed chemical compositions (acidic to neutralized sulfate-containing or hydrophobic organic). A combination of a scanning mobility particle sizer and an Aerodyne high-resolution time-of-flight aerosol mass spectrometer was used to determine SOA mass concentration and chemical composition. We used a Monte Carlo approach to parameterize smog chamber SOA yields as a function of the condensed phase absorptive mass, which includes the sum of OA and the corresponding bound liquid water content. High RH increased SOA yields by up to 6 times (1.5-6.4) compared to low RH. The yields at low NOx / VOC ratios were in general higher compared to yields at high NOx / VOC ratios. This NOx dependence follows the same trend as seen in previous studies for α-pinene SOA. A novel approach of data evaluation using volatility distributions derived from experimental data served as the basis for thermodynamic phase partitioning calculations of model mixtures in this study. These calculations predict liquid-liquid phase separation into organic-rich and electrolyte phases. At low NOx conditions, equilibrium partitioning between the gas and liquid phases can explain most of the increase in SOA yields observed at high RH, when in addition to the α-pinene photo-oxidation products described in the literature, fragmentation products are added to the model mixtures. This increase is driven by both the increase in the absorptive mass and the solution non-ideality described by the compounds' activity coefficients. In contrast, at high NOx, equilibrium partitioning alone could not explain the strong increase in the yields with RH. This suggests that other processes, e.g. reactive uptake of semi-volatile species into the liquid phase, may occur and be enhanced at higher RH, especially for compounds formed under high NOx conditions, e.g. carbonyls.

Discrimination of Biomass Burning Smoke and Clouds in MAIAC Algorithm

NASA Technical Reports Server (NTRS)

Lyapustin, A.; Korkin, S.; Wang, Y.; Quayle, B.; Laszlo, I.

2012-01-01

The multi-angle implementation of atmospheric correction (MAIAC) algorithm makes aerosol retrievals from MODIS data at 1 km resolution providing information about the fine scale aerosol variability. This information is required in different applications such as urban air quality analysis, aerosol source identification etc. The quality of high resolution aerosol data is directly linked to the quality of cloud mask, in particular detection of small (sub-pixel) and low clouds. This work continues research in this direction, describing a technique to detect small clouds and introducing the smoke test to discriminate the biomass burning smoke from the clouds. The smoke test relies on a relative increase of aerosol absorption at MODIS wavelength 0.412 micrometers as compared to 0.47-0.67 micrometers due to multiple scattering and enhanced absorption by organic carbon released during combustion. This general principle has been successfully used in the OMI detection of absorbing aerosols based on UV measurements. This paper provides the algorithm detail and illustrates its performance on two examples of wildfires in US Pacific North-West and in Georgia/Florida of 2007.

Laser Ablation of Poly(methylmethacrylate) Doped with Aromatic Compounds: Laser Intensity Dependence of Absorption Coefficient

NASA Astrophysics Data System (ADS)

Wang, Jun; Niino, Hiroyuki; Yabe, Akira

1999-02-01

We developed a novel method of obtaining an absorption coefficient which depends on the laser intensity, since a single-photon absorption coefficient of a polymer could not be applied to laser ablation. The relationship between the nonlinear absorption coefficient and the laser intensity was derived from experimental data of transmission and incident laser intensities. Using the nonlinear absorption coefficient of poly(methylmethacrylate) doped with benzil and pyrene, we succeeded in fitting the relationship of etch depth and laser intensity, obtained experimentally, and discussed the energy absorbed by the polymer at the threshold fluence.

Characterizing and Understanding Aerosol Optical Properties: CARES - Final Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cappa, Christopher D; Atkinson, Dean B

The scientific focus of this study was to use ambient measurements to develop new insights into the understanding of the direct radiative forcing by atmospheric aerosol particles. The study used data collected by the PI’s and others as part of both the 2010 U.S. Department of Energy (DOE) sponsored Carbonaceous Aerosols and Radiative Effects Study (CARES), which took place in and around Sacramento, CA, and the 2012 Clean Air for London (ClearfLo) study. We focus on measurements that were made of aerosol particle optical properties, namely the wavelength-dependent light absorption, scattering and extinction. Interpretation of these optical property measurements ismore » facilitated through consideration of complementary measurements of the aerosol particle chemical composition and size distributions. With these measurements, we addressed the following general scientific questions: 1. How does light scattering and extinction by atmospheric aerosol particles depend on particle composition, water uptake, and size? 2. To what extent is light absorption by aerosol particles enhanced through the mixing of black carbon with other particulate components? 3. What relationships exist between intensive aerosol particle optical properties, and how do these depend on particle source and photochemical aging? 4. How well do spectral deconvolution methods, which are commonly used in remote sensing, retrieve information about particle size distributions?« less

Photoacoustic measurements of photokinetics in single optically trapped aerosol droplets

NASA Astrophysics Data System (ADS)

Covert, Paul; Cremer, Johannes; Signorell, Ruth; Thaler, Klemens; Haisch, Christoph

2017-04-01

It is well established that interaction of light with atmospheric aerosols has a large impact on the Earth's climate. However, uncertainties in the magnitude of this impact remain large, due in part to broad distributions of aerosol size, composition, and chemical reactivity. In this context, photoacoustic spectroscopy is commonly used to measure light absorption by aerosols. Here, we present photoacoustic measurements of single, optically-trapped nanodroplets to reveal droplet size-depencies of photochemical and physical processes. Theoretical considerations have pointed to a size-dependence in the magnitude and phase of the photoacoustic response from aerosol droplets. This dependence is thought to originate from heat transfer processes that are slow compared to the acoustic excitation frequency. In the case of a model aerosol, our measurements of single particle absorption cross-section versus droplet size confirm these theoretical predictions. In a related study, using the same model aerosol, we also demonstrate a droplet size-dependence of photochemical reaction rates [1]. Within sub-micron sized particles, photolysis rates were observed to be an order of magnitude greater than those observed in larger droplets. [1] J. W. Cremer, K. M. Thaler, C. Haisch, and R. Signorell. Photoacoustics of single laser-trapped nanodroplets for the direct observation of nanofocusing in aerosol photokinetics. Nat. Commun., 7:10941, 2016.

[Observation study on aerosol optical properties and radiative forcing using the ground-based and satellite remote sensing at background station during the regional pollution episodes].

PubMed

Zhang, Xiao-Ling; Xia, Xiang-Ao; Che, Hui-Zheng; Tang, Jie; Tang, Yi-Xi; Meng, Wei; Dong, Fan

2014-07-01

The significant effect of anthropogenic pollutants transportation on the physical and optical properties of regional background atmospheric aerosol was studied by using ground-based and satellite remote sensing data obtained at the atmospheric background station (Shangdianzi, Beijing) of North China during October 1 to 15 in 2011. The aerosol mass concentration and reactive gases concentration increased obviously during periods of October 4-5, October 7-9, and October 11-12. Comparing with the background period of October 1-3, volume concentration increased by a factor of 3-6 for reactive gases such as NO(x), and CO, and a factor of 10-20 for SO2. Mass concentration of PM2.5 was about 200 microg x m(-3) on October 9. During haze period, the AOD at 500 nm varied between 0.60 to 1.00. The single scattering albedo (SSA) was lower than 0.88. And the black carbon concentration increased 4-8 times, which suggested the aerosol absorption was very strong during this pollution episode. The absorption of aerosol particles could cause 100-400 W x m(-2) increase of atmospheric radiation. The surface radiation decreased by about 100-300 W x m(-2) due to the aerosol scattering and absorption. This could cause higher stability of atmosphere, which will significantly affect the cloud and precipitation, and thus the regional weather and climate.

Constraining Aerosol Optical Models Using Ground-Based, Collocated Particle Size and Mass Measurements in Variable Air Mass Regimes During the 7-SEAS/Dongsha Experiment

NASA Technical Reports Server (NTRS)

Bell, Shaun W.; Hansell, Richard A.; Chow, Judith C.; Tsay, Si-Chee; Wang, Sheng-Hsiang; Ji, Qiang; Li, Can; Watson, John G.; Khlystov, Andrey

2012-01-01

During the spring of 2010, NASA Goddard's COMMIT ground-based mobile laboratory was stationed on Dongsha Island off the southwest coast of Taiwan, in preparation for the upcoming 2012 7-SEAS field campaign. The measurement period offered a unique opportunity for conducting detailed investigations of the optical properties of aerosols associated with different air mass regimes including background maritime and those contaminated by anthropogenic air pollution and mineral dust. What appears to be the first time for this region, a shortwave optical closure experiment for both scattering and absorption was attempted over a 12-day period during which aerosols exhibited the most change. Constraints to the optical model included combined SMPS and APS number concentration data for a continuum of fine and coarse-mode particle sizes up to PM2.5. We also take advantage of an IMPROVE chemical sampler to help constrain aerosol composition and mass partitioning of key elemental species including sea-salt, particulate organic matter, soil, non sea-salt sulphate, nitrate, and elemental carbon. Our results demonstrate that the observed aerosol scattering and absorption for these diverse air masses are reasonably captured by the model, where peak aerosol events and transitions between key aerosols types are evident. Signatures of heavy polluted aerosol composed mostly of ammonium and non sea-salt sulphate mixed with some dust with transitions to background sea-salt conditions are apparent in the absorption data, which is particularly reassuring owing to the large variability in the imaginary component of the refractive indices. Extinctive features at significantly smaller time scales than the one-day sample period of IMPROVE are more difficult to reproduce, as this requires further knowledge concerning the source apportionment of major chemical components in the model. Consistency between the measured and modeled optical parameters serves as an important link for advancing remote sensing and climate research studies in dynamic aerosol-rich environments like Dongsha.

Evaluation Of The MODIS-VIIRS Land Surface Reflectance Fundamental Climate Data Record.

NASA Astrophysics Data System (ADS)

Roger, J. C.; Vermote, E.; Skakun, S.; Murphy, E.; Holben, B. N.; Justice, C. O.

2016-12-01

The land surface reflectance is a fundamental climate data record at the basis of the derivation of other climate data records (Albedo, LAI/Fpar, Vegetation indices) and has been recognized as a key parameter in the understanding of the land-surface-climate processes. Here, we present the validation of the Land surface reflectance used for MODIS and VIIRS data. This methodology uses the 6SV Code and data from the AERONET network. The first part was to define a protocol to use the AERONET data. To correctly take into account the aerosol model, we used the aerosol microphysical properties provided by the AERONET network including size-distribution (%Cf, %Cc, rf, rc, σr, σc), complex refractive indices and sphericity. Over the 670 available AERONET sites, we selected 230 sites with sufficient data. To be useful for validation, the aerosol model should be readily available anytime, which is rarely the case. We then used regressions for each microphysical parameter using the aerosol optical thickness at 440nm and the Angström coefficient as parameters. Comparisons with the AERONET dataset give good APU (Accuracy-Precision-Uncertainties) for each parameter. The second part of the study relies on the theoretical land surface retrieval. We generated TOA synthetic data using aerosol models from AERONET and determined APU on the surface reflectance retrieval while applying the MODIS and VIRRS Atmospheric correction software. Over 250 AERONET sites, the global uncertainties are for MODIS band 1 (red) is always lower than 0.0015 (when surface reflectance is > 0.04). This very good result shows the validity of our reference. Then, we used this reference for validating the MODIS and VIIRS surface reflectance products. The overall accuracy clearly reaches specifications. Finally, we will present an error budget of the surface reflectance retrieval. Indeed, to better understand how to improve the methodology, we defined an exhaustive error budget. We included all inputs i.e. sensor, calibration, aerosol properties, atmospheric conditions… This latter work provides a lot of information, such as the aerosol optical thickness obviously drives the uncertainties of the retrieval, the absorption and the volume concentration of the fine aerosol mode have an important impact as well…

40 CFR 796.1050 - Absorption in aqueous solution: Ultraviolet/visible spectra.

Code of Federal Regulations, 2013 CFR

2013-07-01

... by both molar absorption coefficient (molar extinction coefficient) and band width. However, the..., expressed in cm; and the molar absorption (extinction) coefficient,εi, of each species. The absorbance...

40 CFR 796.1050 - Absorption in aqueous solution: Ultraviolet/visible spectra.

Code of Federal Regulations, 2012 CFR

2012-07-01

... by both molar absorption coefficient (molar extinction coefficient) and band width. However, the..., expressed in cm; and the molar absorption (extinction) coefficient,εi, of each species. The absorbance...

40 CFR 796.1050 - Absorption in aqueous solution: Ultraviolet/visible spectra.

Code of Federal Regulations, 2014 CFR

2014-07-01

... by both molar absorption coefficient (molar extinction coefficient) and band width. However, the..., expressed in cm; and the molar absorption (extinction) coefficient,εi, of each species. The absorbance...

Validation of multi-angle imaging spectroradiometer aerosol products in China

Treesearch

J. Liu; X. Xia; Z. Li; P. Wang; M. Min; WeiMin Hao; Y. Wang; J. Xin; X. Li; Y. Zheng; Z. Chen

2010-01-01

Based on AErosol RObotic NETwork and Chinese Sun Hazemeter Network data, the Multi-angle Imaging SpectroRadiometer (MISR) level 2 aerosol optical depth (AOD) products are evaluated in China. The MISR retrievals depict well the temporal aerosol trend in China with correlation coefficients exceeding 0.8 except for stations located in northeast China and at the...

A Global, Decadal, Quantitative Record of Absorbing Aerosols above Cloud Using OMI's Near-UV Observations

NASA Astrophysics Data System (ADS)

Torres, O.; Jethva, H. T.; Ahn, C.

2016-12-01

Aerosol-cloud interaction continues to be one of the leading uncertain components of climate models, primarily due to the lack of an adequate knowledge of the complex microphysical and radiative processes of the aerosol-cloud system. The situations when aerosols and clouds are found in the same atmospheric column, for instance, when light-absorbing aerosols such as biomass burning generated carbonaceous particles or wind-blown dust overlay low-level cloud decks, are commonly found over several regions of the world. Contrary to the known cooling effects of these aerosols in cloud-free scenario over dark surface, the overlapping situation of absorbing aerosols over cloud can potentially exert a significant level of atmospheric absorption and produces a positive radiative forcing (warming) at top-of-atmosphere. The magnitude of direct radiative effects of aerosols above cloud directly depends on the aerosol loading, microphysical and optical properties of the aerosol layer and the underlying cloud deck, and geometric cloud fraction. We help in addressing this problem by introducing a novel product of above-cloud aerosol optical depth (ACAOD) of absorbing aerosols retrieved from near-UV observations made by the Ozone Monitoring Instrument (OMI) on board NASA's Aura platform. Physically based on the strong `color ratio' effect in the near-UV caused by the spectral absorption of aerosols above cloud, the algorithm, formally named as OMACA, retrieves the optical depths of aerosols and clouds simultaneously under a prescribed state of atmosphere. Here, we present the algorithm architecture and results from an 11-year global record (2005-2015) including global climatology of frequency of occurrence and ACAOD. The theoretical uncertainty analysis and planned validation activities using measurements from upcoming field campaigns are also discussed.

Detection of a gas flaring signature in the AERONET optical properties of aerosols at a tropical station in West Africa

NASA Astrophysics Data System (ADS)

Fawole, Olusegun G.; Cai, Xiaoming; Levine, James G.; Pinker, Rachel T.; MacKenzie, A. R.

2016-12-01

The West African region, with its peculiar climate and atmospheric dynamics, is a prominent source of aerosols. Reliable and long-term in situ measurements of aerosol properties are not readily available across the region. In this study, Version 2 Level 1.5 Aerosol Robotic Network (AERONET) data were used to study the absorption and size distribution properties of aerosols from dominant sources identified by trajectory analysis. The trajectory analysis was used to define four sources of aerosols over a 10 year period. Sorting the AERONET aerosol retrievals by these putative sources, the hypothesis that there exists an optically distinct gas flaring signal was tested. Dominance of each source cluster varies with season: desert-dust (DD) and biomass burning (BB) aerosols are dominant in months prior to the West African Monsoon (WAM); urban (UB) and gas flaring (GF) aerosol are dominant during the WAM months. BB aerosol, with single scattering albedo (SSA) at 675 nm value of 0.86 ± 0.03 and GF aerosol with SSA (675 nm) value of 0.9 ± 0.07, is the most absorbing of the aerosol categories. The range of Absorption Angstr&öm Exponent (AAE) for DD, BB, UB and GF classes are 1.99 ± 0.35, 1.45 ± 0.26, 1.21 ± 0.38 and 0.98 ± 0.25, respectively, indicating different aerosol composition for each source. The AAE (440-870 nm) and Angstr&öm Exponent (AE) (440-870 nm) relationships further show the spread and overlap of the variation of these optical and microphysical properties, presumably due in part to similarity in the sources of aerosols and in part, due to mixing of air parcels from different sources en route to the measurement site.

Radiative absorption enhancement of dust mixed with anthropogenic pollution over East Asia

NASA Astrophysics Data System (ADS)

Tian, Pengfei; Zhang, Lei; Ma, Jianmin; Tang, Kai; Xu, Lili; Wang, Yuan; Cao, Xianjie; Liang, Jiening; Ji, Yuemeng; Jiang, Jonathan H.; Yung, Yuk L.; Zhang, Renyi

2018-06-01

The particle mixing state plays a significant yet poorly quantified role in aerosol radiative forcing, especially for the mixing of dust (mineral absorbing) and anthropogenic pollution (black carbon absorbing) over East Asia. We have investigated the absorption enhancement of mixed-type aerosols over East Asia by using the Aerosol Robotic Network observations and radiative transfer model calculations. The mixed-type aerosols exhibit significantly enhanced absorbing ability than the corresponding unmixed dust and anthropogenic aerosols, as revealed in the spectral behavior of absorbing aerosol optical depth, single scattering albedo, and imaginary refractive index. The aerosol radiative efficiencies for the dust, mixed-type, and anthropogenic aerosols are -101.0, -112.9, and -98.3 Wm-2 τ-1 at the bottom of the atmosphere (BOA); -42.3, -22.5, and -39.8 Wm-2 τ-1 at the top of the atmosphere (TOA); and 58.7, 90.3, and 58.5 Wm-2 τ-1 in the atmosphere (ATM), respectively. The BOA cooling and ATM heating efficiencies of the mixed-type aerosols are significantly higher than those of the unmixed aerosol types over the East Asia region, resulting in atmospheric stabilization. In addition, the mixed-type aerosols correspond to a lower TOA cooling efficiency, indicating that the cooling effect by the corresponding individual aerosol components is partially counteracted. We conclude that the interaction between dust and anthropogenic pollution not only represents a viable aerosol formation pathway but also results in unfavorable dispersion conditions, both exacerbating the regional air pollution in East Asia. Our results highlight the necessity to accurately account for the mixing state of aerosols in atmospheric models over East Asia in order to better understand the formation mechanism for regional air pollution and to assess its impacts on human health, weather, and climate.

Measurements of Extensive Aerosol Optical Properties During TexAQS II: Implications for PM Compliance and Planning

NASA Astrophysics Data System (ADS)

Wright, M. E.; Atkinson, D. B.; Luke, W. T.

2007-12-01

In 2000, the Houston-Galveston Area (HGA) was designated as a non-attainment area for several criteria air pollutants by the US EPA. In order to meet the requirements of the federal Clean Air Act, the Second Texas Air Quality Study (TexAQS II) was designed to update the State Implementation Plan (SIP) by providing scientific air quality data over 18 months from June 2005 to October 2006. The data presented here was collected as part of the Texas Radical and Aerosol Measurement Program (TRAMP), a substudy of TexAQS II. Bulk aerosol optical properties were measured for six weeks atop the 60 m high Southwest Moody Tower on the University of Houston campus. The measurements were collected using a cavity ring-down transmissometer/nephelometer (CRDT/N) and consisted of the extensive aerosol coefficients: extinction (bext) at 532 and 1064 nm and scattering (bscat) at 530nm. In addition to daily and whole study averages and calculated mass values, positive correlations between the 1064 nm extinction and 532 nm absorption (babs = bext - bscat) values are displayed for this study period for the first time. Correlation between the particle scattering coefficient and the sum of AMS measured (UNH - PI: R. Griffin) sulfate and organic particle mass concentrations as well as covariance between optical properties and O3, CO and NOx values (ARL/NOAA - PI: W. Luke) are also examined. No correlation is expected between coarse particles (PM10), which are typically primary biogenic suspended soil minerals or windblown dust, and high ozone concentrations. Ozone levels are highest during periods of low wind when coarse particulate is likely to be at a minimum. On the other hand, secondary particles and O3 should be correlated on short time scales because both species tend to have the same precursors, NOx and VOC's, and formation of particles is favored during stagnant conditions. Fine particles (PM2.5) should also correlate with CO since both species have a common emission source. Wind roses are compared with pollution roses for each week of the study period, allowing for cluster analysis. Overall, the optical properties appear to be an effective measure of air quality when compared to other measurement techniques. Implications for aerosol effects on regional climate from long-range transport and synoptic scale recirculation are discussed.

Aerosol retrieval for APEX airborne imaging spectrometer: a preliminary analysis

NASA Astrophysics Data System (ADS)

Seidel, Felix; Nieke, Jens; Schläpfer, Daniel; Höller, Robert; von Hoyningen-Huene, Wolfgang; Itten, Klaus

2005-10-01

In order to achieve quantitative measurements of the Earth's surface radiance and reflectance, it is important to determine the aerosol optical thickness (AOT) to correct for the optical influence of atmospheric particles. An advanced method for aerosol detection and quantification is required, which is not strongly dependant on disturbing effects due to surface reflectance, gas absorption and Rayleigh scattering features. A short review of existing applicable methods to the APEX airborne imaging spectrometer (380nm to 2500nm), leads to the suggested aerosol retrieval method here in this paper. It will measure the distinct radiance change between two near-UV spectral bands (385nm & 412nm) due to aerosol induced scattering and absorption features. Atmospheric radiation transfer model calculations have been used to analyze the AOT retrieval capability and accuracy of APEX. The noise-equivalent differential AOT is presented along with the retrieval sensitivity to various input variables. It is shown, that the suggested method will be able to identify different aerosol model types and measure AOT and columnar size distribution. The proposed accurate AOT determination will lead to a unique opportunity of two-dimensional pixel-wise mapping of aerosol properties at a high spatial resolution. This will be helpful especially for regional climate studies, atmospheric pollution monitoring and for the improvement of aerosol dispersion models and the validation of aerosol algorithms on spaceborne sensors.

Development of absorbing aerosol index simulator based on TM5-M7

NASA Astrophysics Data System (ADS)

Sun, Jiyunting; van Velthoven, Peter; Veefkind, Pepijn

2017-04-01

Aerosols alter the Earth's radiation budget directly by scattering and absorbing solar and thermal radiation, or indirectly by perturbing clouds formation and lifetime. These mechanisms offset the positive radiative forcing ascribed to greenhouse gases. In particular, absorbing aerosols such as black carbon and dust strongly enhance global warming. To quantify the impact of absorbing aerosol on global radiative forcing is challenging. In spite of wide spatial and temporal coverage space-borne instruments (we will use the Ozone Monitoring Instrument, OMI) are unable to derive complete information on aerosol distribution, composition, etc. The retrieval of aerosol optical properties also partly depends on additional information derived from other measurements or global atmospheric chemistry models. Common quantities of great interest presenting the amount of absorbing aerosol are AAOD (absorbing aerosol optical depth), the extinction due to absorption of aerosols under cloud free conditions; and AAI (absorbing aerosol index), a measure of aerosol absorption more directly derivable from UV band observations than AAOD. When comparing model simulations and satellite observations, resemblance is good in terms of the spatial distribution of both parameters. However, the quantitative discrepancy is considerable, indicating possible underestimates of simulated AAI by a factor of 2 to 3. Our research, hence, has started by evaluating to what extent aerosol models, such as our TM5-M7 model, represent the satellite measurements and by identifying the reasons for discrepancies. As a next step a transparent methodology for the comparison between model simulations and satellite observations is under development in the form of an AAI simulator based on TM5-M7.

Earlinet validation of CATS L2 product

NASA Astrophysics Data System (ADS)

Proestakis, Emmanouil; Amiridis, Vassilis; Kottas, Michael; Marinou, Eleni; Binietoglou, Ioannis; Ansmann, Albert; Wandinger, Ulla; Yorks, John; Nowottnick, Edward; Makhmudov, Abduvosit; Papayannis, Alexandros; Pietruczuk, Aleksander; Gialitaki, Anna; Apituley, Arnoud; Muñoz-Porcar, Constantino; Bortoli, Daniele; Dionisi, Davide; Althausen, Dietrich; Mamali, Dimitra; Balis, Dimitris; Nicolae, Doina; Tetoni, Eleni; Luigi Liberti, Gian; Baars, Holger; Stachlewska, Iwona S.; Voudouri, Kalliopi-Artemis; Mona, Lucia; Mylonaki, Maria; Rita Perrone, Maria; João Costa, Maria; Sicard, Michael; Papagiannopoulos, Nikolaos; Siomos, Nikolaos; Burlizzi, Pasquale; Engelmann, Ronny; Abdullaev, Sabur F.; Hofer, Julian; Pappalardo, Gelsomina

2018-04-01

The Cloud-Aerosol Transport System (CATS) onboard the International Space Station (ISS), is a lidar system providing vertically resolved aerosol and cloud profiles since February 2015. In this study, the CATS aerosol product is validated against the aerosol profiles provided by the European Aerosol Research Lidar Network (EARLINET). This validation activity is based on collocated CATS-EARLINET measurements and the comparison of the particle backscatter coefficient at 1064nm.

LIDAR detection of forest fire smoke above Sofia

NASA Astrophysics Data System (ADS)

Grigorov, Ivan; Deleva, Atanaska; Stoyanov, Dimitar; Kolev, Nikolay; Kolarov, Georgi

2015-01-01

The distribution of aerosol load in the atmosphere due to two forest fires near Sofia (the capital city of Bulgaria) was studied using two aerosol lidars which operated at 510.6 nm and 1064 nm. Experimental data is presented as 2D-heatmaps of the evolution of attenuated backscatter coefficient profiles and mean profile of the aerosol backscatter coefficient, calculated for each lidar observation. Backscatter related Angstrom exponent was used as a criterion in particle size estimation of detected smoke layers. Calculated minimal values at altitudes where the aerosol layer was observed corresponded to predominant fraction of coarse aerosol. Dust-transport forecast maps and calculations of backward trajectories were employed to make conclusions about aerosol's origin. They confirmed the local transport of smoke aerosol over the city and lidar station. DREAM forecast maps predicted neither cloud cover, nor Saharan load in the air above Sofia on the days of measurements. The results of lidar observations are discussed in conjunction with meteorological situation, aiming to better explain the reason for the observed aerosol stratification. The data of regular radio sounding of the atmosphere showed a characteristic behavior with small differences of the values between the air temperature and dew-point temperature profiles at aerosol smoke layer altitude. So the resulting stratification revealed the existence of atmospheric layers with aerosol trapping properties.

The spectral irradiance of the moon

USGS Publications Warehouse

Kieffer, H.H.; Stone, T.C.

2005-01-01

Images of the Moon at 32 wavelengths from 350 to 2450 nm have been obtained from a dedicated observatory during the bright half of each month over a period of several years. The ultimate goal is to develop a spectral radiance model of the Moon with an angular resolution and radiometric accuracy appropriate for calibration of Earth-orbiting spacecraft. An empirical model of irradiance has been developed that treats phase and libration explicitly, with absolute scale founded on the spectra of the star Vega and returned Apollo samples. A selected set of 190 standard stars are observed regularly to provide nightly extinction correction and long-term calibration of the observations. The extinction model is wavelength-coupled and based on the absorption coefficients of a number of gases and aerosols. The empirical irradiance model has the same form at each wavelength, with 18 coefficients, eight of which are constant across wavelength, for a total of 328 coefficients. Over 1000 lunar observations are fitted at each wavelength; the average residual is less than 1%. The irradiance model is actively being used in lunar calibration of several spacecraft instruments and can track sensor response changes at the 0.1% level. ?? 2005. The American Astronomical Society. All rights reserved.

Cavity Attenuated Phase Shift (CAPS) Method for Airborne Aerosol Light Extinction Measurement: Instrument Validation and First Results from Field Deployment

NASA Astrophysics Data System (ADS)

Petzold, A.; Perim de Faria, J.; Berg, M.; Bundke, U.; Freedman, A.

2015-12-01

Monitoring the direct impact of aerosol particles on climate requires the continuous measurement of aerosol optical parameters like the aerosol extinction coefficient on a regular basis. Remote sensing and ground-based networks are well in place (e.g., AERONET, ACTRIS), whereas the regular in situ measurement of vertical profiles of atmospheric aerosol optical properties remains still an important challenge in quantifying climate change. The European Research Infrastructure IAGOS (In-service Aircraft for a Global Observing System; www.iagos.org) responds to the increasing requests for long-term, routine in situ observational data by using commercial passenger aircraft as measurement platform. However, scientific instrumentation for the measurement of atmospheric constituents requires major modifications before being deployable aboard in-service passenger aircraft. Recently, a compact and robust family of optical instruments based on the cavity attenuated phase shift (CAPS) technique has become available for measuring aerosol light extinction. While this technique was successfully deployed for ground-based atmospheric measurements under various conditions, its suitability for operation aboard aircraft in the free and upper free troposphere still has to be demonstrated. In this work, the modifications of a CAPS PMex instrument for measuring aerosol light extinction on aircraft, the results from subsequent laboratory tests for evaluating the modified instrument prototype, and first results from a field deployment aboard a research aircraft will be covered. In laboratory studies, the instrument showed excellent agreement (deviation < 5%) with theoretical values calculated from Rayleigh scattering cross-sections, when operated on pressurized air and CO2 at ambient and low pressure (~200 hPa). For monodisperse and polydisperse aerosols, reference aerosol extinction coefficients were calculated from measured size distributions and agreed with the CAPS PMex instrument response within 10% deviation. During the field deployment, aerosol extinction coefficients and associated aerosol size distributions have been measured and will be presented as comparison studies between measured and calculated data.

Aerosol size and chemical composition measurements at the Polar Environment Atmospheric Research Lab (PEARL) in Eureka, Nunavut

NASA Astrophysics Data System (ADS)

Hayes, P. L.; Tremblay, S.; Chang, R. Y. W.; Leaitch, R.; Kolonjari, F.; O'Neill, N. T.; Chaubey, J. P.; AboEl Fetouh, Y.; Fogal, P.; Drummond, J. R.

2016-12-01

This study presents observations of aerosol chemical composition and particle number size distribution at the Polar Environment Atmospheric Research Laboratory (PEARL) in the Canadian High Arctic (80N, 86W). The current aerosol measurement program at PEARL has been ongoing for more than a year providing long-term observations of Arctic aerosol size distributions for both coarse and fine modes. Particle nucleation events were frequently observed during the summers of 2015 and 2016. The size distribution data are also compared against similar measurements taken at the Alert Global Atmospheric Watch Observatory (82N, 62W) for July and August 2015. The nucleation events are correlated at the two sites, despite a distance of approximately 500 km, suggesting regional conditions favorable for particle nucleation and growth during this period. Size resolved chemical composition measurements were also carried out using an aerosol mass spectrometer. The smallest measured particles between 40 and 60 nm are almost entirely organic aerosol (OA) indicating that the condensation of organic vapors is responsible for particle growth events and possibly particle nucleation. This conclusion is further supported by the relatively high oxygen content of the OA, which is consistent with secondary formation of OA via atmospheric oxidation.Lastly, surface measurements of the aerosol scattering coefficient are compared against the coefficient values calculated using Mie theory and the measured aerosol size distribution. Both the actual and the calculated scattering coefficients are then compared to sun photometer measurements to understand the relationship between surface and columnar aerosol optical properties. The measurements at PEARL provide a unique combination of surface and columnar data sets on aerosols in the High Arctic, a region where such measurements are scarce despite the important impact of aerosols on Arctic climate.PEARL research is supported by the Natural Sciences and Engineering Research Council (NSERC) of Canada, the Canadian Space Agency (CSA), and Environment and Climate Change Canada (ECCC). In addition, the Alert GAW Observatory is supported by ECCC.

Emission Rates and Optical Properties of Pollutants Emitted from a Traditional and an Improved Wood-Burning Cookstove

NASA Astrophysics Data System (ADS)

Kirchstetter, T.; Hadley, O. L.; Preble, C.; Gadgil, A.

2010-12-01

Traditional cooking methods in developing regions of the world generate gas and particle phase pollutants that endanger the lives of more than a billion people and contribute appreciably to the burden of climate-changing particles in the atmosphere. This presentation compares pollutant emissions from the traditional “three-stone fire” and an improved cookstove developed for refugees in Darfur: the Berkeley-Darfur Stove (BDS). The BDS was designed for increased fuel efficiency to decrease the risk of assault that women often face when gathering fuel wood. Reduced pollutant exposure and climate impact are potential co-benefits. Testing of these stoves at the Lawrence Berkeley National Laboratory facility includes 1-Hz measurements of concentrations of particulate matter, black carbon, carbon monoxide, and carbon dioxide; coefficients of particle light absorption and scattering; and absorption Angstrom exponent. Absorption and scattering coefficients were measured at 532 nm using a photoacoustic absorption instrument equipped with a reciprocal nephelometer. The BDS heated food faster and consumed less wood in cooking tests compared to the three-stone fire. The BDS emitted less carbon monoxide and particulate matter but comparable mass of black carbon compared to the three-stone fire for the same cooking task. Values of the absorption Angstrom exponent ranged from about 1 - 3, indicating the emission of both black carbon and light-absorbing organic carbon (i.e., brown carbon). Values of (dry) aerosol single scattering albedo were mostly in the range of 0.25 - 0.55, indicating that the emitted particles tend to absorb more light than they scatter. Our analysis considered the variability of pollutant emissions during different phases of the fire. Particulate matter emissions were highest during the first several minutes of cooking, which included igniting the wood, whereas carbon monoxide emissions were highest during the last several minutes of cooking when smoldering became more dominant. Comparison of photoacoustic absorption and aethalometer black carbon provided an easy means of correcting black carbon concentrations, which were low by a factor of 2 at the end of the aethalometer sampling cycle if uncorrected.

Measurement of Absorption Coefficient of Paraformaldehyde and Metaldehyde with Terahertz Spectroscopy

NASA Astrophysics Data System (ADS)

Zhang, J.; Xia, T.; Chen, Q.; Sun, Q.; Deng, Y.; Wang, C.

2018-03-01

The characteristic absorption spectra of paraformaldehyde and metaldehyde in the terahertz frequency region are obtained by terahertz time-domain spectroscopy (THz-TDS). In order to reduce the absorption of terahertz (THz) wave by water vapor in the air and the background noise, the measurement system was filled with dry air and the measurements were conducted at the temperature of 24°C. Meanwhile, the humidity was controlled within 10% RH. The THz frequency domain spectra of samples and their references from 0 to 2.5 THz were analyzed via Fourier transform. The refractive index and absorption coefficients of the two aldehydes were calculated by the model formulas. From 0.1 to 2.5 THz, there appear two weak absorption peaks at 1.20 and 1.66 THz in the absorption spectra of paraformaldehyde. Only one distinct absorption peak emerges at 1.83 THz for metaldehyde. There are significant differences between the terahertz absorption coefficients of paraformaldehyde and metaldehyde, which can be used as "fingerprints" to identify these substances. Furthermore, the relationship between the average absorption coefficients and mass concentrations was investigated and the average absorption coefficient-mass concentration diagrams of paraformaldehyde and metaldehyde were shown. For paraformaldehyde, there is a linear relationship between the average absorption coefficient and the natural logarithm of mass concentration. For metaldehyde, there exists a simpler linear relationship between the average absorption coefficient and the mass concentration. Because of the characteristics of THz absorption of paraformaldehyde and metaldehyde, the THz-TDS can be applied to the qualitative and quantitative detection of the two aldehydes to reduce the unpredictable hazards due to these substances.

Modeling Gas-Particle Partitioning of SOA: Effects of Aerosol Physical State and RH

NASA Astrophysics Data System (ADS)

Zuend, A.; Seinfeld, J.

2011-12-01

Aged tropospheric aerosol particles contain mixtures of inorganic salts, acids, water, and a large variety of organic compounds. In liquid aerosol particles non-ideal mixing of all species determines whether the condensed phase undergoes liquid-liquid phase separation or whether it is stable in a single mixed phase, and whether it contains solid salts in equilibrium with their saturated solution. The extended thermodynamic model AIOMFAC is able to predict such phase states by representing the variety of organic components using functional groups within a group-contribution concept. The number and composition of different condensed phases impacts the diversity of reaction media for multiphase chemistry and the gas-particle partitioning of semivolatile species. Recent studies show that under certain conditions biogenic and other organic-rich particles can be present in a highly viscous, semisolid or amorphous solid physical state, with consequences regarding reaction kinetics and mass transfer limitations. We present results of new gas-particle partitioning computations for aerosol chamber data using a model based on AIOMFAC activity coefficients and state-of-the-art vapor pressure estimation methods. Different environmental conditions in terms of temperature, relative humidity (RH), salt content, amount of precursor VOCs, and physical state of the particles are considered. We show how modifications of absorptive and adsorptive gas-particle mass transfer affects the total aerosol mass in the calculations and how the results of these modeling approaches compare to data of aerosol chamber experiments, such as alpha-pinene oxidation SOA. For a condensed phase in a mixed liquid state containing ammonium sulfate, the model predicts liquid-liquid phase separation up to high RH in case of, on average, moderately hydrophilic organic compounds, such as first generation oxidation products of alpha-pinene. The computations also reveal that treating liquid phases as ideal mixtures substantially overestimates the SOA mass, especially at high relative humidity.

Light absorption properties and radiative effects of primary organic aerosol emissions

DOE PAGES

Lu, Zifeng; Streets, David G.; Winijkul, Ekbordin; ...

2015-03-26

Organic aerosols (OAs) in the atmosphere affect Earth’s energy budget by not only scattering but also absorbing solar radiation due to the presence of the so-called “brown carbon” (BrC) component. However, the absorptivities of OAs are not represented or are poorly represented in current climate and chemical transport models. In this study, we provide a method to constrain the BrC absorptivity at the emission inventory level using recent laboratory and field observations. We review available measurements of the light-absorbing primary OA (POA), and quantify the wavelength-dependent imaginary refractive indices (k OA, the fundamental optical parameter determining the particle’s absorptivity) andmore » their uncertainties for the bulk POA emitted from biomass/biofuel, lignite, propane, and oil combustion sources. In particular, we parametrize the k OA of biomass/biofuel combustion sources as a function of the black carbon (BC)-to-OA ratio, indicating that the absorptive properties of POA depend strongly on burning conditions. The derived fuel-type-based k OA profiles are incorporated into a global carbonaceous aerosol emission inventory, and the integrated k OA values of sectoral and total POA emissions are presented. The results of a simple radiative transfer model show that the POA absorptivity warms the atmosphere significantly and leads to ~27% reduction in the amount of the net global average POA cooling compared to results from the nonabsorbing assumption.« less

The SOA formation model combined with semiempirical quantum chemistry for predicting UV-Vis absorption of secondary organic aerosols.

PubMed

Zhong, Min; Jang, Myoseon; Oliferenko, Alexander; Pillai, Girinath G; Katritzky, Alan R

2012-07-07

A new model for predicting the UV-visible absorption spectra of secondary organic aerosols (SOA) has been developed. The model consists of two primary parts: a SOA formation model and a semiempirical quantum chemistry method. The mass of SOA is predicted using the PHRCSOA (Partitioning Heterogeneous Reaction Consortium Secondary Organic Aerosol) model developed by Cao and Jang [Environ. Sci. Technol., 2010, 44, 727]. The chemical composition is estimated using a combination of the kinetic model (MCM) and the PHRCSOA model. The absorption spectrum is obtained by taking the sum of the spectrum of each SOA product calculated using a semiempirical NDDO (Neglect of Diatomic Differential Overlap)-based method. SOA was generated from the photochemical reaction of toluene or α-pinene at different NO(x) levels (low NO(x): 24-26 ppm, middle NO(x): 49 ppb, high NO(x): 104-105 ppb) using a 2 m(3) indoor Teflon film chamber. The model simulation reasonably agrees with the measured absorption spectra of α-pinene SOA but underestimates toluene SOA under high and middle NO(x) conditions. The absorption spectrum of toluene SOA is moderately enhanced with increasing NO(x) concentrations, while that of α-pinene SOA is not affected. Both measured and calculated UV-visible spectra show that the light absorption of toluene SOA is much stronger than that of α-pinene SOA.

UManSysProp v1.0: an online and open-source facility for molecular property prediction and atmospheric aerosol calculations

NASA Astrophysics Data System (ADS)

Topping, David; Barley, Mark; Bane, Michael K.; Higham, Nicholas; Aumont, Bernard; Dingle, Nicholas; McFiggans, Gordon

2016-03-01

In this paper we describe the development and application of a new web-based facility, UManSysProp (http://umansysprop.seaes.manchester.ac.uk), for automating predictions of molecular and atmospheric aerosol properties. Current facilities include pure component vapour pressures, critical properties, and sub-cooled densities of organic molecules; activity coefficient predictions for mixed inorganic-organic liquid systems; hygroscopic growth factors and CCN (cloud condensation nuclei) activation potential of mixed inorganic-organic aerosol particles; and absorptive partitioning calculations with/without a treatment of non-ideality. The aim of this new facility is to provide a single point of reference for all properties relevant to atmospheric aerosol that have been checked for applicability to atmospheric compounds where possible. The group contribution approach allows users to upload molecular information in the form of SMILES (Simplified Molecular Input Line Entry System) strings and UManSysProp will automatically extract the relevant information for calculations. Built using open-source chemical informatics, and hosted at the University of Manchester, the facilities are provided via a browser and device-friendly web interface, or can be accessed using the user's own code via a JSON API (application program interface). We also provide the source code for all predictive techniques provided on the site, covered by the GNU GPL (General Public License) license to encourage development of a user community. We have released this via a Github repository (doi:10.5281/zenodo.45143). In this paper we demonstrate its use with specific examples that can be simulated using the web-browser interface.

Aerosol optical properties and direct radiative forcing based on measurements from the China Aerosol Remote Sensing Network (CARSNET) in eastern China

NASA Astrophysics Data System (ADS)

Che, Huizheng; Qi, Bing; Zhao, Hujia; Xia, Xiangao; Eck, Thomas F.; Goloub, Philippe; Dubovik, Oleg; Estelles, Victor; Cuevas-Agulló, Emilio; Blarel, Luc; Wu, Yunfei; Zhu, Jun; Du, Rongguang; Wang, Yaqiang; Wang, Hong; Gui, Ke; Yu, Jie; Zheng, Yu; Sun, Tianze; Chen, Quanliang; Shi, Guangyu; Zhang, Xiaoye

2018-01-01

Aerosol pollution in eastern China is an unfortunate consequence of the region's rapid economic and industrial growth. Here, sun photometer measurements from seven sites in the Yangtze River Delta (YRD) from 2011 to 2015 were used to characterize the climatology of aerosol microphysical and optical properties, calculate direct aerosol radiative forcing (DARF) and classify the aerosols based on size and absorption. Bimodal size distributions were found throughout the year, but larger volumes and effective radii of fine-mode particles occurred in June and September due to hygroscopic growth and/or cloud processing. Increases in the fine-mode particles in June and September caused AOD440 nm > 1.00 at most sites, and annual mean AOD440 nm values of 0.71-0.76 were found at the urban sites and 0.68 at the rural site. Unlike northern China, the AOD440 nm was lower in July and August (˜ 0.40-0.60) than in January and February (0.71-0.89) due to particle dispersion associated with subtropical anticyclones in summer. Low volumes and large bandwidths of both fine-mode and coarse-mode aerosol size distributions occurred in July and August because of biomass burning. Single-scattering albedos at 440 nm (SSA440 nm) from 0.91 to 0.94 indicated particles with relatively strong to moderate absorption. Strongly absorbing particles from biomass burning with a significant SSA wavelength dependence were found in July and August at most sites, while coarse particles in March to May were mineral dust. Absorbing aerosols were distributed more or less homogeneously throughout the region with absorption aerosol optical depths at 440 nm ˜ 0.04-0.06, but inter-site differences in the absorption Angström exponent indicate a degree of spatial heterogeneity in particle composition. The annual mean DARF was -93 ± 44 to -79 ± 39 W m-2 at the Earth's surface and ˜ -40 W m-2 at the top of the atmosphere (for the solar zenith angle range of 50 to 80°) under cloud-free conditions. The fine mode composed a major contribution of the absorbing particles in the classification scheme based on SSA, fine-mode fraction and extinction Angström exponent. This study contributes to our understanding of aerosols and regional climate/air quality, and the results will be useful for validating satellite retrievals and for improving climate models and remote sensing algorithms.