Broadband measurements of aerosol extinction in the ultraviolet spectral region

NASA Astrophysics Data System (ADS)

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

2013-04-01

Aerosols influence the Earth's radiative budget by scattering and absorbing incoming solar radiation. The optical properties of aerosols vary as a function of wavelength, but few measurements have reported the wavelength dependence of aerosol extinction cross sections and complex refractive indices. We describe a new laboratory instrument to measure aerosol optical extinction as a function of wavelength, using cavity enhanced spectroscopy with a broadband light source. 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 determined aerosol extinction cross sections and directly observed Mie scattering resonances for aerosols that are purely scattering (polystyrene latex spheres and ammonium sulfate), slightly absorbing (Suwannee River fulvic acid), and strongly absorbing (nigrosin dye). We describe an approach for retrieving refractive indices as a function of wavelength from the measured extinction cross sections over the 360-420 nm wavelength region. The retrieved refractive indices for PSL and ammonium sulfate agree within uncertainty with the literature values for this spectral region. The refractive index determined for nigrosin is 1.78 (± 0.03) + 0.19 (± 0.08)i at 360 nm and 1.63 (± 0.03) + 0.21 (± 0.05)i at 420 nm. The refractive index determined for Suwannee River fulvic acid is 1.71 (± 0.02) + 0.07 (± 0.06)i at 360 nm and 1.66 (± 0.02) + 0.06 (± 0.04)i at 420 nm. These laboratory results support the potential for a field instrument capable of determining ambient aerosol optical extinction, average aerosol extinction cross section, and complex refractive index as a function of wavelength.

Broadband measurements of aerosol extinction in the ultraviolet spectral region

NASA Astrophysics Data System (ADS)

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

2013-01-01

Aerosols influence the Earth's radiative budget by scattering and absorbing incoming solar radiation. The optical properties of aerosols vary as a function of wavelength, but few measurements have reported the wavelength dependence of aerosol extinction cross-sections and complex refractive indices. We describe a new laboratory instrument to measure aerosol optical extinction as a function of wavelength, using cavity enhanced spectroscopy with a broadband light source. 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 determined aerosol extinction cross-sections and directly observed Mie scattering resonances for aerosols that are purely scattering (polystyrene latex spheres and ammonium sulfate), slightly absorbing (Suwannee River fulvic acid), and strongly absorbing (nigrosin dye). We describe an approach for retrieving refractive indices as a function of wavelength from the measured extinction cross-sections over the 360-420 nm wavelength region. The retrieved refractive indices for PSL and ammonium sulfate agree within uncertainty with literature values for this spectral region. The refractive index determined for nigrosin is 1.78 (±0.03) + 0.19 (±0.08) i at 360 nm and 1.53 (±0.03) + 0.21 (±0.05) i at 420 nm. The refractive index determined for Suwannee River fulvic acid is 1.71 (±0.02) + 0.07 (±0.06) i at 360 nm and 1.66 (±0.02) + 0.06 (±0.04) i at 420 nm. These laboratory results support the potential for a field instrument capable of determining ambient aerosol optical extinction, average aerosol extinction cross-section, and complex refractive index as a function of wavelength.

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.

Direct measurements of the optical cross sections and refractive indices of individual volatile and hygroscopic aerosol particles.

PubMed

Mason, B J; Cotterell, M I; Preston, T C; Orr-Ewing, A J; Reid, J P

2015-06-04

We present measurements of the evolving extinction cross sections of individual aerosol particles (spanning 700-2500 nm in radius) during the evaporation of volatile components or hygroscopic growth using a combination of a single particle trap formed from a Bessel light beam and cavity ring-down spectroscopy. For single component organic aerosol droplets of 1,2,6-hexanetriol, polyethylene glycol 400, and glycerol, the slow evaporation of the organic component (over time scales of 1000 to 10,000 s) leads to a time-varying size and extinction cross section that can be used to estimate the refractive index of the droplet. Measurements on binary aqueous-inorganic aerosol droplets containing one of the inorganic solutes ammonium bisulfate, ammonium sulfate, sodium nitrate, or sodium chloride (over time scales of 1000 to 15,000 s) under conditions of changing relative humidity show that extinction cross-section measurements are consistent with expectations from accepted models for the variation in droplet refractive index with hygroscopic growth. In addition, we use these systems to establish an experimental protocol for future single particle extinction measurements. The advantages of mapping out the evolving light extinction cross-section of an individual particle over extended time frames accompanied by hygroscopic cycling or component evaporation are discussed.

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.

Open-path, closed-path and reconstructed aerosol extinction at a rural site.

PubMed

Gordon, Timothy D; Prenni, Anthony J; Renfro, James R; McClure, Ethan; Hicks, Bill; Onasch, Timothy B; Freedman, Andrew; McMeeking, Gavin R; Chen, Ping

2018-04-09

The Handix Scientific Open-Path Cavity Ringdown Spectrometer (OPCRDS) was deployed during summer 2016 in Great Smoky Mountains National Park (GRSM). Extinction coefficients from the relatively new OPCRDS and from a more well-established extinction instrument agreed to within 7%. Aerosol hygroscopic growth (f(RH)) was calculated from the ratio of ambient extinction measured by the OPCRDS to dry extinction measured by a closed-path extinction monitor (Aerodyne's Cavity Attenuated Phase Shift Particulate Matter Extinction Monitor, CAPS PMex). Derived hygroscopicity (RH < 95%) from this campaign agreed with data from 1995 at the same site and time of year, which is noteworthy given the decreasing trend for organics and sulfate in the eastern U.S. However, maximum f(RH) values in 1995 were less than half as large as those recorded in 2016-possibly due to nephelometer truncation losses in 1995. Two hygroscopicity parameterizations were investigated using high time resolution OPCRDS+CAPS PMex data, and the K ext model was more accurate than the γ model. Data from the two ambient optical instruments, the OPCRDS and the open-path nephelometer, generally agreed; however, significant discrepancies between ambient scattering and extinction were observed, apparently driven by a combination of hygroscopic growth effects, which tend to increase nephelometer truncation losses and decrease sensitivity to the wavelength difference between the two instruments as a function of particle size. There was not a statistically significant difference in the mean reconstructed extinction values obtained from the original and the revised IMPROVE (Interagency Monitoring of Protected Visual Environments) equations. On average IMPROVE reconstructed extinction was ~25% lower than extinction measured by the OPCRDS, which suggests that the IMPROVE equations and 24-hr aerosol data are moderately successful in estimating current haze levels at GRSM. However, this conclusion is limited by the coarse

Spectral Aerosol Extinction (SpEx): A New Instrument for In situ Ambient Aerosol Extinction Measurements Across the UV/Visible Wavelength Range

NASA Technical Reports Server (NTRS)

Jordan, C. E.; Anderson, B. E.; Beyersdorf, A. J.; Corr, C. A.; Dibb, J. E.; Greenslade, M. E.; Martin, R. F.; Moore, R. H.; Scheuer, E.; Shook, M. A.;

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.

Impact of organic coating on growth of ammonium sulfate particles: light extinction measurements relevant for the direct effect

NASA Astrophysics Data System (ADS)

Robinson, C. B.; Zarzana, K. J.; Hasenkopf, C. A.; Tolbert, M. A.

2012-12-01

Light extinction by particles is strongly dependent on chemical composition, particle size, and water uptake. Relative humidity affects extinction by causing changes in refractive index and particle size due to hygroscopic growth. The ability of particles to take up water depends on their composition and structure. In both laboratory and field studies, inorganic salts completely covered by an organic coating have been observed. The impact of this coating on water uptake is uncertain, and a systematic study that examines water uptake as a function of relative humidity is highly desirable. These data are critical to evaluate the aerosol direct effect on climate, which is one of the most uncertain aspects of future climate change. In this study, we probe the connection between aerosol composition, size and light extinction directly by measuring fRHext, the ratio of the extinction coefficient for humidified particles to the extinction coefficient for dry particles. Particles were composed of 1,2,6-hexanetriol and ammonium sulfate, a system that forms organic coatings around the inorganic core. A cavity ring-down aerosol extinction spectrometer at 532 nm is used to measure the optical growth factor as a function of relative humidity. The fRHext values for a range of %RH for pure ammonium sulfate, pure 1,2,6-hexanetriol, and ammonium sulfate particles with 1,2,6-hexanetriol coatings were measured. The coated particles are created using a method of liquid-liquid separation, where the particles are exposed to water vapor creating a RH% above their deliquescence RH%. The particles are then dried with a Nafion dryer to a RH% that is below the point where liquid-liquid phase separation is observed, but above the efflorescence RH%. Pure 1,2,6-hexanetriol takes up little water over the observed RH range of 45-65%, and therefore fRHext ~ 1. With pure ammonium sulfate for the same RH% range, the fRHext varied from 1.5 - 2, depending on the RH% and the particle size. For the

Extinction cross section measurements for a single optically trapped particle

NASA Astrophysics Data System (ADS)

Cotterell, Michael I.; Preston, Thomas C.; Mason, Bernard J.; Orr-Ewing, Andrew J.; Reid, Jonathan P.

2015-08-01

Bessel beam (BB) optical traps have become widely used to confine single and multiple aerosol particles across a broad range of sizes, from a few microns to < 200 nm in radius. The radiation pressure force exerted by the core of a single, zeroth-order BB incident on a particle can be balanced by a counter-propagating gas flow, allowing a single particle to be trapped indefinitely. The pseudo non-diffracting nature of BBs enables particles to be confined over macroscopic distances along the BB core propagation length; the position of the particle along this length can be finely controlled by variation of the BB laser power. This latter property is exploited to optimize the particle position at the center of the TEM00 mode of a high finesse optical cavity, allowing cavity ring-down spectroscopy (CRDS) to be performed on single aerosol particles and their optical extinction cross section, σext, measured. Further, the variation in the light from the illuminating BB elastically scattered by the particle is recorded as a function of scattering angle. Such intensity distributions are fitted to Lorenz-Mie theory to determine the particle radius. The trends in σext with particle radius are modelled using cavity standing wave Mie simulations and a particle's varying refractive index with changing relative humidity is determined. We demonstrate σext measurements on individual sub-micrometer aerosol particles and determine the lowest limit in particle size that can be probed by this technique. The BB-CRDS method will play a key role in reducing the uncertainty associated with atmospheric aerosol radiative forcing, which remains among the largest uncertainties in climate modelling.

Evaluation of SAGE II and Balloon-Borne Stratospheric Aerosol Measurements: Evaluation of Aerosol Measurements from SAGE II, HALOE, and Balloonborne Optical Particle Counters

NASA Technical Reports Server (NTRS)

Hervig, Mark; Deshler, Terry; Moddrea, G. (Technical Monitor)

2002-01-01

Stratospheric aerosol measurements from the University of Wyoming balloonborne optical particle counters (OPCs), the Stratospheric Aerosol and Gas Experiment (SAGE) II, and the Halogen Occultation Experiment (HALOE) were compared in the period 1982-2000, when measurements were available. The OPCs measure aerosol size distributions, and HALOE multiwavelength (2.45-5.26 micrometers) extinction measurements can be used to retrieve aerosol size distributions. Aerosol extinctions at the SAGE II wavelengths (0.386-1.02 micrometers) were computed from these size distributions and compared to SAGE II measurements. In addition, surface areas derived from all three experiments were compared. While the overall impression from these results is encouraging, the agreement can change with latitude, altitude, time, and parameter. In the broadest sense, these comparisons fall into two categories: high aerosol loading (volcanic periods) and low aerosol loading (background periods and altitudes above 25 km). When the aerosol amount was low, SAGE II and HALOE extinctions were higher than the OPC estimates, while the SAGE II surface areas were lower than HALOE and the OPCS. Under high loading conditions all three instruments mutually agree to within 50%.

Aerosol Extinction Profile Mapping with Lognormal Distribution Based on MPL Data

NASA Astrophysics Data System (ADS)

Lin, T. H.; Lee, T. T.; Chang, K. E.; Lien, W. H.; Liu, G. R.; Liu, C. Y.

2017-12-01

This study intends to challenge the profile mapping of aerosol vertical distribution by mathematical function. With the similarity in distribution pattern, lognormal distribution is examined for mapping the aerosol extinction profile based on MPL (Micro Pulse LiDAR) in situ measurements. The variables of lognormal distribution are log mean (μ) and log standard deviation (σ), which will be correlated with the parameters of aerosol optical depht (AOD) and planetary boundary layer height (PBLH) associated with the altitude of extinction peak (Mode) defined in this study. On the base of 10 years MPL data with single peak, the mapping results showed that the mean error of Mode and σ retrievals are 16.1% and 25.3%, respectively. The mean error of σ retrieval can be reduced to 16.5% under the cases of larger distance between PBLH and Mode. The proposed method is further applied to MODIS AOD product in mapping extinction profile for the retrieval of PM2.5 in terms of satellite observations. The results indicated well agreement between retrievals and ground measurements when aerosols under 525 meters are well-mixed. The feasibility of proposed method to satellite remote sensing is also suggested by the case study. Keyword: Aerosol extinction profile, Lognormal distribution, MPL, Planetary boundary layer height (PBLH), Aerosol optical depth (AOD), Mode

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

Field Studies of Broadband Aerosol Optical Extinction in the Ultraviolet Spectral Region

NASA Astrophysics Data System (ADS)

Washenfelder, R. A.; Attwood, A.; Brock, C. A.; Brown, S. S.

2013-12-01

Aerosols influence the Earth's radiative budget by scattering and absorbing incoming solar radiation. The optical properties of aerosols vary as a function of wavelength, but few measurements have reported the wavelength dependence of aerosol extinction cross sections and complex refractive indices. In the case of brown carbon, its wavelength-dependent absorption in the ultraviolet spectral region has been suggested as an important component of aerosol radiative forcing. We describe a new field instrument to measure aerosol optical extinction as a function of wavelength, using cavity enhanced spectroscopy with a broadband light source. 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 deployed this instrument during the Fire Lab at Missoula Experiment during Fall 2012 to measure biomass burning aerosol, and again during the Southern Oxidant and Aerosol Study in summer 2013 to measure organic aerosol in the Southeastern U.S. In both field experiments, we determined aerosol optical extinction as a function of wavelength and can interpret this together with size distribution and composition measurements to characterize the aerosol optical properties and radiative forcing.

The impacts of aerosol loading, composition, and water uptake on aerosol extinction variability in the Baltimore-Washington, D.C. region

NASA Astrophysics Data System (ADS)

Beyersdorf, A. J.; Ziemba, L. D.; Chen, G.; Corr, C. A.; Crawford, J. H.; Diskin, G. S.; Moore, R. H.; Thornhill, K. L.; Winstead, E. L.; Anderson, B. E.

2016-01-01

In order to utilize satellite-based aerosol measurements for the determination of air quality, the relationship between aerosol optical properties (wavelength-dependent, column-integrated extinction measured by satellites) and mass measurements of aerosol loading (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, and hygroscopicity - and to the surrounding atmosphere, such as temperature, relative humidity (RH), and altitude, all of which can vary spatially and temporally. During the DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality) project, extensive in situ atmospheric profiling in the Baltimore, MD-Washington, D.C. region was performed during 14 flights in July 2011. Identical flight plans and profile locations throughout the project provide meaningful statistics for determining the variability in and correlations between aerosol loading, composition, optical properties, and meteorological conditions. Measured water-soluble aerosol mass was composed primarily of ammonium sulfate (campaign average of 32 %) and organics (57 %). A distinct difference in composition was observed, with high-loading days having a proportionally larger percentage of sulfate due to transport from the Ohio River Valley. This composition shift caused a change in the aerosol water-uptake potential (hygroscopicity) such that higher relative contributions of inorganics increased the bulk aerosol hygroscopicity. These days also tended to have higher relative humidity, causing an increase in the water content of the aerosol. Conversely, low-aerosol-loading days had lower sulfate and higher black carbon contributions, causing lower single-scattering albedos (SSAs). The average black carbon concentrations were 240 ng m-3 in the lowest 1 km, decreasing to 35 ng m-3 in the free troposphere (above

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.

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 Ozone Mapping and Profiler Suite (OMPS) Limb Profiler (LP) Version 1 aerosol extinction retrieval algorithm: theoretical basis

NASA Astrophysics Data System (ADS)

Loughman, Robert; Bhartia, Pawan K.; Chen, Zhong; Xu, Philippe; Nyaku, Ernest; Taha, Ghassan

2018-05-01

The theoretical basis of the Ozone Mapping and Profiler Suite (OMPS) Limb Profiler (LP) Version 1 aerosol extinction retrieval algorithm is presented. The algorithm uses an assumed bimodal lognormal aerosol size distribution to retrieve aerosol extinction profiles at 675 nm from OMPS LP radiance measurements. A first-guess aerosol extinction profile is updated by iteration using the Chahine nonlinear relaxation method, based on comparisons between the measured radiance profile at 675 nm and the radiance profile calculated by the Gauss-Seidel limb-scattering (GSLS) radiative transfer model for a spherical-shell atmosphere. This algorithm is discussed in the context of previous limb-scattering aerosol extinction retrieval algorithms, and the most significant error sources are enumerated. The retrieval algorithm is limited primarily by uncertainty about the aerosol phase function. Horizontal variations in aerosol extinction, which violate the spherical-shell atmosphere assumed in the version 1 algorithm, may also limit the quality of the retrieved aerosol extinction profiles significantly.

On the accuracy of stratospheric aerosol extinction derived from in situ size distribution measurements and surface area density derived from remote SAGE II and HALOE extinction measurements

DOE PAGES

Kovilakam, Mahesh; Deshler, Terry

2015-08-26

In situ stratospheric aerosol measurements, from University of Wyoming optical particle counters (OPCs), are compared with Stratospheric Aerosol Gas Experiment (SAGE) II (versions 6.2 and 7.0) and Halogen Occultation Experiment (HALOE) satellite measurements to investigate differences between SAGE II/HALOE-measured extinction and derived surface area and OPC-derived extinction and surface area. Coincident OPC and SAGE II measurements are compared for a volcanic (1991-1996) and nonvolcanic (1997-2005) period. OPC calculated extinctions agree with SAGE II measurements, within instrumental uncertainty, during the volcanic period, but have been a factor of 2 low during the nonvolcanic period. Three systematic errors associated with the OPCmore » measurements, anisokineticity, inlet particle evaporation, and counting efficiency, were investigated. An overestimation of the OPC counting efficiency is found to be the major source of systematic error. With this correction OPC calculated extinction increases by 15-30% (30-50%) for the volcanic (nonvolcanic) measurements. These changes significantly improve the comparison with SAGE II and HALOE extinctions in the nonvolcanic cases but slightly degrade the agreement in the volcanic period. These corrections have impacts on OPC-derived surface area density, exacerbating the poor agreement between OPC and SAGE II (version 6.2) surface areas. Furthermore, this disparity is reconciled with SAGE II version 7.0 surface areas. For both the volcanic and nonvolcanic cases these changes in OPC counting efficiency and in the operational SAGE II surface area algorithm leave the derived surface areas from both platforms in significantly better agreement and within the ± 40% precision of the OPC moment calculations.« less

On the accuracy of stratospheric aerosol extinction derived from in situ size distribution measurements and surface area density derived from remote SAGE II and HALOE extinction measurements

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

Kovilakam, Mahesh; Deshler, Terry

In situ stratospheric aerosol measurements, from University of Wyoming optical particle counters (OPCs), are compared with Stratospheric Aerosol Gas Experiment (SAGE) II (versions 6.2 and 7.0) and Halogen Occultation Experiment (HALOE) satellite measurements to investigate differences between SAGE II/HALOE-measured extinction and derived surface area and OPC-derived extinction and surface area. Coincident OPC and SAGE II measurements are compared for a volcanic (1991-1996) and nonvolcanic (1997-2005) period. OPC calculated extinctions agree with SAGE II measurements, within instrumental uncertainty, during the volcanic period, but have been a factor of 2 low during the nonvolcanic period. Three systematic errors associated with the OPCmore » measurements, anisokineticity, inlet particle evaporation, and counting efficiency, were investigated. An overestimation of the OPC counting efficiency is found to be the major source of systematic error. With this correction OPC calculated extinction increases by 15-30% (30-50%) for the volcanic (nonvolcanic) measurements. These changes significantly improve the comparison with SAGE II and HALOE extinctions in the nonvolcanic cases but slightly degrade the agreement in the volcanic period. These corrections have impacts on OPC-derived surface area density, exacerbating the poor agreement between OPC and SAGE II (version 6.2) surface areas. Furthermore, this disparity is reconciled with SAGE II version 7.0 surface areas. For both the volcanic and nonvolcanic cases these changes in OPC counting efficiency and in the operational SAGE II surface area algorithm leave the derived surface areas from both platforms in significantly better agreement and within the ± 40% precision of the OPC moment calculations.« less

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.

In Situ Aerosol Profile Measurements and Comparisons with SAGE 3 Aerosol Extinction and Surface Area Profiles at 68 deg North

NASA Technical Reports Server (NTRS)

2005-01-01

Under funding from this proposal three in situ profile measurements of stratospheric sulfate aerosol and ozone were completed from balloon-borne platforms. The measured quantities are aerosol size resolved number concentration and ozone. The one derived product is aerosol size distribution, from which aerosol moments, such as surface area, volume, and extinction can be calculated for comparison with SAGE III measurements and SAGE III derived products, such as surface area. The analysis of these profiles and comparison with SAGE III extinction measurements and SAGE III derived surface areas are provided in Yongxiao (2005), which comprised the research thesis component of Mr. Jian Yongxiao's M.S. degree in Atmospheric Science at the University of Wyoming. In addition analysis continues on using principal component analysis (PCA) to derive aerosol surface area from the 9 wavelength extinction measurements available from SAGE III. Ths paper will present PCA components to calculate surface area from SAGE III measurements and compare these derived surface areas with those available directly from in situ size distribution measurements, as well as surface areas which would be derived from PCA and Thomason's algorithm applied to the four wavelength SAGE II extinction measurements.

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.

The Influence of Aerosol Hygroscopicity on Retrieving the Aerosol Extincting Coefficient from MPL Data

NASA Astrophysics Data System (ADS)

Zhao, G.; Zhao, C.

2016-12-01

Micro-pulse Lidar (MPL) measurements have been widely used to profile the ambient aerosol extincting coefficient(). Lidar Ratio (LR) ,which highly depends on the particle number size distribution (PNSD) and aerosol hygroscopicity, is the most important factor to retrieve the profile. A constant AOD constrained LR is usually used in current algorithms, which would lead to large bias when the relative humidity (RH) in the mixed layer is high. In this research, the influences of PNSD, aerosol hygroscopicity and RH profiles on the vertical variation of LR were investigated based on the datasets from field measurements in the North China Plain (NCP). Results show that LR can have an enhancement factor of more than 120% when the RH reaches to 92%. A new algorithm of retrieving the profile is proposed based on the variation of LR due to aerosol hygroscopicity. The magnitude and vertical structures of retrieved using this method can be significantly different to that of the fiexed LR method. The relative difference can reach up to 40% when the RH in the mixed layer is higher than 90% . Sensitivity studies show that RH profile and PNSD affect most on the retrieved by fiexed LR method. In view of this, a scheme of LR enhancement factor by RH is proposed in the NCP. The relative differnce of the calculated between using this scheme and the new algorithm with the variable LR can be less than 10%.

Selection Algorithm for the CALIPSO Lidar Aerosol Extinction-to-Backscatter Ratio

NASA Technical Reports Server (NTRS)

Omar, Ali H.; Winker, David M.; Vaughan, Mark A.

2006-01-01

The extinction-to-backscatter ratio (S(sub a)) is an important parameter used in the determination of the aerosol extinction and subsequently the optical depth from lidar backscatter measurements. We outline the algorithm used to determine Sa for the Cloud and Aerosol Lidar and Infrared Pathfinder Spaceborne Observations (CALIPSO) lidar. S(sub a) for the CALIPSO lidar will either be selected from a look-up table or calculated using the lidar measurements depending on the characteristics of aerosol layer. Whenever suitable lofted layers are encountered, S(sub a) is computed directly from the integrated backscatter and transmittance. In all other cases, the CALIPSO observables: the depolarization ratio, delta, the layer integrated attenuated backscatter, beta, and the mean layer total attenuated color ratio, gamma, together with the surface type, are used to aid in aerosol typing. Once the type is identified, a look-up-table developed primarily from worldwide observations, is used to determine the S(sub a) value. The CALIPSO aerosol models include desert dust, biomass burning, background, polluted continental, polluted dust, and marine aerosols.

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.

Aerosol optical extinction during the Front Range Air Pollution and Photochemistry Éxperiment (FRAPPÉ) 2014 summertime field campaign, Colorado, USA

NASA Astrophysics Data System (ADS)

Dingle, Justin H.; Vu, Kennedy; Bahreini, Roya; Apel, Eric C.; Campos, Teresa L.; Flocke, Frank; Fried, Alan; Herndon, Scott; Hills, Alan J.; Hornbrook, Rebecca S.; Huey, Greg; Kaser, Lisa; Montzka, Denise D.; Nowak, John B.; Reeves, Mike; Richter, Dirk; Roscioli, Joseph R.; Shertz, Stephen; Stell, Meghan; Tanner, David; Tyndall, Geoff; Walega, James; Weibring, Petter; Weinheimer, Andrew

2016-09-01

Summertime aerosol optical extinction (βext) was measured in the Colorado Front Range and Denver metropolitan area as part of the Front Range Air Pollution and Photochemistry Éxperiment (FRAPPÉ) campaign during July-August 2014. An Aerodyne cavity attenuated phase shift particle light extinction monitor (CAPS-PMex) was deployed to measure βext (at average relative humidity of 20 ± 7 %) of submicron aerosols at λ = 632 nm at 1 Hz. Data from a suite of gas-phase instrumentation were used to interpret βext behavior in various categories of air masses and sources. Extinction enhancement ratios relative to CO (Δβext / ΔCO) were higher in aged urban air masses compared to fresh air masses by ˜ 50 %. The resulting increase in Δβext / ΔCO for highly aged air masses was accompanied by formation of secondary organic aerosols (SOAs). In addition, the impacts of aerosol composition on βext in air masses under the influence of urban, natural oil and gas operations (O&G), and agriculture and livestock operations were evaluated. Estimated non-refractory mass extinction efficiency (MEE) values for different air mass types ranged from 1.51 to 2.27 m2 g-1, with the minimum and maximum values observed in urban and agriculture-influenced air masses, respectively. The mass distribution for organic, nitrate, and sulfate aerosols presented distinct profiles in different air mass types. During 11-12 August, regional influence of a biomass burning event was observed, increasing the background βext and estimated MEE values in the Front Range.

Airborne Aerosol Closure Studies During PRIDE

NASA Technical Reports Server (NTRS)

Redemann, Jens; Livingston, John M.; Russell, Philip B.; Schmid, Beat; Reid, Jeff

2000-01-01

The Puerto Rico Dust Experiment (PRIDE) was conducted during June/July of 2000 to study the properties of Saharan dust aerosols transported across the Atlantic Ocean to the Caribbean Islands. During PRIDE, the NASA Ames Research Center six-channel (380 - 1020 nm) airborne autotracking sunphotometer (AATS-6) was operated aboard a Piper Navajo airplane alongside a suite of in situ aerosol instruments. The in situ aerosol instrumentation relevant to this paper included a Forward Scattering Spectrometer Probe (FSSP-100) and a Passive Cavity Aerosol Spectrometer Probe (PCASP), covering the radius range of approx. 0.05 to 10 microns. The simultaneous and collocated measurement of multi-spectral aerosol optical depth and in situ particle size distribution data permits a variety of closure studies. For example, vertical profiles of aerosol optical depth obtained during local aircraft ascents and descents can be differentiated with respect to altitude and compared to extinction profiles calculated using the in situ particle size distribution data (and reasonable estimates of the aerosol index of refraction). Additionally, aerosol extinction (optical depth) spectra can be inverted to retrieve estimates of the particle size distributions, which can be compared directly to the in situ size distributions. In this paper we will report on such closure studies using data from a select number of vertical profiles at Cabras Island, Puerto Rico, including measurements in distinct Saharan Dust Layers. Preliminary results show good agreement to within 30% between mid-visible aerosol extinction derived from the AATS-6 optical depth profiles and extinction profiles forward calculated using 60s-average in situ particle size distributions and standard Saharan dust aerosol refractive indices published in the literature. In agreement with tendencies observed in previous studies, our initial results show an underestimate of aerosol extinction calculated based on the in situ size distributions

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.

Series cell light extinction monitor

DOEpatents

Novick, Vincent J.

1990-01-01

A method and apparatus for using the light extinction measurements from two or more light cells positioned along a gasflow chamber in which the gas volumetric rate is known to determine particle number concentration and mass concentration of an aerosol independent of extinction coefficient and to determine estimates for particle size and mass concentrations. The invention is independent of particle size. This invention has application to measurements made during a severe nuclear reactor fuel damage test.

Forwardscattering corrections for optical extinction measurements in aerosol media. II - Polydispersions

NASA Technical Reports Server (NTRS)

Deepak, A.; Box, M. A.

1978-01-01

The paper presents a parametric study of the forwardscattering corrections for experimentally measured optical extinction coefficients in polydisperse particulate media, since some forward scattered light invariably enters, along with the direct beam, into the finite aperture of the detector. Forwardscattering corrections are computed by two methods: (1) using the exact Mie theory, and (2) the approximate Rayleigh diffraction formula for spherical particles. A parametric study of the dependence of the corrections on mode radii, real and imaginary parts of the complex refractive index, and half-angle of the detector's view cone has been carried out for three different size distribution functions of the modified gamma type. In addition, a study has been carried out to investigate the range of these parameters in which the approximate formulation is valid. The agreement is especially good for small-view cone angles and large particles, which improves significantly for slightly absorbing aerosol particles. Also discussed is the dependence of these corrections on the experimental design of the transmissometer systems.

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.

Optical extinction dependence on wavelength and size distribution of airborne dust

NASA Astrophysics Data System (ADS)

Pangle, Garrett E.; Hook, D. A.; Long, Brandon J. N.; Philbrick, C. R.; Hallen, Hans D.

2013-05-01

The optical scattering from laser beams propagating through atmospheric aerosols has been shown to be very useful in describing air pollution aerosol properties. This research explores and extends that capability to particulate matter. The optical properties of Arizona Road Dust (ARD) samples are measured in a chamber that simulates the particle dispersal of dust aerosols in the atmospheric environment. Visible, near infrared, and long wave infrared lasers are used. Optical scattering measurements show the expected dependence of laser wavelength and particle size on the extinction of laser beams. The extinction at long wavelengths demonstrates reduced scattering, but chemical absorption of dust species must be considered. The extinction and depolarization of laser wavelengths interacting with several size cuts of ARD are examined. The measurements include studies of different size distributions, and their evolution over time is recorded by an Aerodynamic Particle Sizer. We analyze the size-dependent extinction and depolarization of ARD. We present a method of predicting extinction for an arbitrary ARD size distribution. These studies provide new insights for understanding the optical propagation of laser beams through airborne particulate matter.

Spectral signatures of polar stratospheric clouds and sulfate aerosol

NASA Technical Reports Server (NTRS)

Massie, S. T.; Bailey, P. L.; Gille, J. C.; Lee, E. C.; Mergenthaler, J. L.; Roche, A. E.; Kumer, J. B.; Fishbein, E. F.; Waters, J. W.; Lahoz, W. A.

1994-01-01

Multiwavelength observations of Antarctic and midlatitude aerosol by the Cryogenic Limb Array Etalon Spectrometer (CLAES) experiment on the Upper Atmosphere Research Satellite (UARS) are used to demonstrate a technique that identifies the location of polar stratospheric clouds. The technique discussed uses the normalized area of the triangle formed by the aerosol extinctions at 925, 1257, and 1605/cm (10.8, 8.0, and 6.2 micrometers) to derive a spectral aerosol measure M of the aerosol spectrum. Mie calculations for spherical particles and T-matrix calculations for spheriodal particles are used to generate theoretical spectral extinction curves for sulfate and polar stratospheric cloud particles. The values of the spectral aerosol measure M for the sulfate and polar stratospheric cloud particles are shown to be different. Aerosol extinction data, corresponding to temperatures between 180 and 220 K at a pressure of 46 hPa (near 21-km altitude) for 18 August 1992, are used to demonstrate the technique. Thermodynamic calculations, based upon frost-point calculations and laboratory phase-equilibrium studies of nitric acid trihydrate, are used to predict the location of nitric acid trihydrate cloud particles.

Influence of particle aspect ratio on the midinfrared extinction spectra of wavelength-sized ice crystals.

PubMed

Wagner, Robert; Benz, Stefan; Möhler, Ottmar; Saathoff, Harald; Schnaiter, Martin; Leisner, Thomas

2007-12-20

We have used the T-matrix method and the discrete dipole approximation to compute the midinfrared extinction cross-sections (4500-800 cm(-1)) of randomly oriented circular ice cylinders for aspect ratios extending up to 10 for oblate and down to 1/6 for prolate particle shapes. Equal-volume sphere diameters ranged from 0.1 to 10 microm for both particle classes. A high degree of particle asphericity provokes a strong distortion of the spectral habitus compared to the extinction spectrum of compactly shaped ice crystals with an aspect ratio around 1. The magnitude and the sign (increase or diminution) of the shape-related changes in both the absorption and the scattering cross-sections crucially depend on the particle size and the values for the real and imaginary part of the complex refractive index. When increasing the particle asphericity for a given equal-volume sphere diameter, the values for the overall extinction cross-sections may change in opposite directions for different parts of the spectrum. We have applied our calculations to the analysis of recent expansion cooling experiments on the formation of cirrus clouds, performed in the large coolable aerosol and cloud chamber AIDA of Forschungszentrum Karlsruhe at a temperature of 210 K. Depending on the nature of the seed particles and the temperature and relative humidity characteristics during the expansion, ice crystals of various shapes and aspect ratios could be produced. For a particular expansion experiment, using Illite mineral dust particles coated with a layer of secondary organic matter as seed aerosol, we have clearly detected the spectral signatures characteristic of strongly aspherical ice crystal habits in the recorded infrared extinction spectra. We demonstrate that the number size distributions and total number concentrations of the ice particles that were generated in this expansion run can only be accurately derived from the recorded infrared spectra when employing aspect ratios as high as

Using Airborne High Spectral Resolution Lidar Data to Evaluate Combined Active Plus Passive Retrievals of Aerosol Extinction Profiles

NASA Technical Reports Server (NTRS)

Burton, S. P.; Ferrare, R. A.; Kittaka, C.; Hostetler, C. A.; Hair, J. W.; Obland, M. D.; Rogers, R. R.; Cook, A. L.; Haper, D. B.

2008-01-01

Aerosol extinction profiles are derived from backscatter data by constraining the retrieval with column aerosol optical thickness (AOT), for example from coincident MODIS observations and without reliance on a priori assumptions about aerosol type or optical properties. The backscatter data were acquired with the NASA Langley High Spectral Resolution Lidar (HSRL). The HSRL also simultaneously measures extinction independently, thereby providing an ideal data set for evaluating the constrained retrieval of extinction from backscatter. We will show constrained extinction retrievals using various sources of column AOT, and examine comparisons with the HSRL extinction measurements and with a similar retrieval using data from the CALIOP lidar on the CALIPSO satellite.

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

SAGE 1 and SAM 2 measurements of 1 micron aerosol extinction in the free troposphere

NASA Technical Reports Server (NTRS)

Kent, G. S.; Farrukh, U. O.; Wang, P. H.; Deepak, A.

1988-01-01

The SAGE 1 and SAM 2 satellite sensors were designed to measure, with global coverage, the 1 micron extinction produced by the stratospheric aerosol. In the absence of high altitude cloud, similar measurements may be made for the free tropospheric aerosol. Median extinction values in the Northern Hemisphere, for altitudes between 5 and 10 km, are found to be one-half to one order of magnitude greater than values at corresponding latitudes in the Southern Hemisphere. In addition, a seasonal increase by a factor of 1.5 yields 2 is observed in both hemispheres in local spring and summer. Following major volcanic eruptions, a long-lived enhancement of the aerosol extinction is observed for altitudes above 5 km.

Vertical distribution of aerosol extinction cross section and inference of aerosol imaginary index in the troposphere by lidar technique

NASA Technical Reports Server (NTRS)

Spinhirne, J. D.; Reagan, J. A.; Herman, B. M.

1980-01-01

The paper reports on vertical profiles of aerosol extinction and backscatter in the troposphere which were obtained from multi zenith angle lidar measurements. It is reported that a direct slant path solution was found to be not possible due to horizontal inhomogeneity of the atmosphere. Attention is given to the use of a regression analysis with respect to zenith angle for a layer integration of the angle dependent lidar equation in order to determine the optical thickness and aerosol extinction-to-backscatter ratio for defined atmospheric layers and the subsequent evaluation of cross-section profiles.

Raman Lidar Measurements of Aerosol Extinction and Backscattering. Report 2; Derivation of Aerosol Real Refractive Index, Single-Scattering Albedo, and Humidification Factor using Raman Lidar and Aircraft Size Distribution

NASA Technical Reports Server (NTRS)

Ferrare, R. A.; Melfi, S. H.; Whiteman, D. N.; Evans, K. D.; Poellot, M.; Kaufman, Y. J.

1998-01-01

Aerosol backscattering and extinction profiles measured by the NASA Goddard Space Flight Center Scanning Raman Lidar (SRL) during the remote cloud sensing (RCS) intensive operations period (IOP) at the Department of Energy Atmospheric Radiation Measurement (ARM) southern Great Plains (SGP) site during two nights in April 1994 are discussed. These profiles are shown to be consistent with the simultaneous aerosol size distribution measurements made by a PCASP (Passive Cavity Aerosol Spectrometer Probe) optical particle counter flown on the University of North Dakota Citation aircraft. We describe a technique which uses both lidar and PCASP measurements to derive the dependence of particle size on relative humidity, the aerosol real refractive index n, and estimate the effective single-scattering albedo Omega(sub 0). Values of n ranged between 1.4-1.5 (dry) and 1.37-1.47 (wet); Omega(sub 0) varied between 0.7 and 1.0. The single-scattering albedo derived from this technique is sensitive to the manner in which absorbing particles are represented in the aerosol mixture; representing the absorbing particles as an internal mixture rather than the external mixture assumed here results in generally higher values of Omega(sub 0). The lidar measurements indicate that the change in particle size with relative humidity as measured by the PCASP can be represented in the form discussed by Hattel with the exponent gamma = 0.3 + or - 0.05. The variations in aerosol optical and physical characteristics captured in the lidar and aircraft size distribution measurements are discussed in the context of the meteorological conditions observed during the experiment.

Raman lidar measurements of aerosol extinction and backscattering: 2. Derivation of aerosol real refractive index, single-scattering albedo, and humidification factor using Raman lidar and aircraft size distribution measurements

NASA Astrophysics Data System (ADS)

Ferrare, R. A.; Melfi, S. H.; Whiteman, D. N.; Evans, K. D.; Poellot, M.; Kaufman, Y. J.

1998-08-01

Aerosol backscattering and extinction profiles measured by the NASA Goddard Space Flight Center Scanning Raman Lidar (SRL) during the remote cloud sensing (RCS) intensive operations period (IOP) at the Department of Energy Atmospheric Radiation Measurement (ARM) southern Great Plains (SGP) site during two nights in April 1994 are discussed. These profiles are shown to be consistent with the simultaneous aerosol size distribution measurements made by a PCASP (Passive Cavity Aerosol Spectrometer Probe) optical particle counter flown on the University of North Dakota Citation aircraft. We describe a technique which uses both lidar and PCASP measurements to derive the dependence of particle size on relative humidity, the aerosol real refractive index n, and estimate the effective single-scattering albedo ω0. Values of n ranged between 1.4-1.5 (dry) and 1.37-1.47 (wet); ω0 varied between 0.7 and 1.0. The single-scattering albedo derived from this technique is sensitive to the manner in which absorbing particles are represented in the aerosol mixture; representing the absorbing particles as an internal mixture rather than the external mixture assumed here results in generally higher values of ω0. The lidar measurements indicate that the change in particle size with relative humidity as measured by the PCASP can be represented in the form discussed by Hanel [1976] with the exponent γ = 0.3 ± 0.05. The variations in aerosol optical and physical characteristics captured in the lidar and aircraft size distribution measurements are discussed in the context of the meteorological conditions observed during the experiment.

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.

Vertical profiles of fine and coarse aerosol particles over Cyprus: Comparison between in-situ drone measurements and remote sensing observations

NASA Astrophysics Data System (ADS)

Mamali, Dimitra; Marinou, Eleni; Pikridas, Michael; Kottas, Michael; Binietoglou, Ioannis; Kokkalis, Panagiotis; Tsekeri, Aleksandra; Amiridis, Vasilis; Sciare, Jean; Keleshis, Christos; Engelmann, Ronny; Ansmann, Albert; Russchenberg, Herman W. J.; Biskos, George

2017-04-01

Vertical profiles of the aerosol mass concentration derived from light detection and ranging (lidar) measurements were compared to airborne dried optical particle counter (OPC MetOne; Model 212) measurements during the INUIT-BACCHUS-ACTRIS campaign. The campaign took place in April 2016 and its main focus was the study of aerosol dust particles. During the campaign the NOA Polly-XT Raman lidar located at Nicosia (35.08° N, 33.22° E) was providing round-the-clock vertical profiles of aerosol optical properties. In addition, an unmanned aerial vehicle (UAV) carrying an OPC flew on 7 days during the first morning hours. The flights were performed at Orounda (35.1018° N, 33.0944° E) reaching altitudes of 2.5 km a.s.l, which allows comparison with a good fraction of the recorded lidar data. The polarization lidar photometer networking method (POLIPHON) was used for the estimation of the fine (non-dust) and coarse (dust) mode aerosol mass concentration profiles. This method uses as input the particle backscatter coefficient and the particle depolarization profiles of the lidar at 532 nm wavelength and derives the aerosol mass concentration. The first step in this approach makes use of the lidar observations to separate the backscatter and extinction contributions of the weakly depolarizing non-dust aerosol components from the contributions of the strongly depolarizing dust particles, under the assumption of an externally mixed two-component aerosol. In the second step, sun photometer retrievals of the fine and the coarse modes aerosol optical thickness (AOT) and volume concentration are used to calculate the associated concentrations from the extinction coefficients retrieved from the lidar. The estimated aerosol volume concentrations were converted into mass concentration with an assumption for the bulk aerosol density, and compared with the OPC measurements. The first results show agreement within the experimental uncertainty. This project received funding from the

Using Airborne High Spectral Resolution Lidar Data to Evaluate Combined Active Plus Passive Retrievals of Aerosol Extinction Profiles

NASA Technical Reports Server (NTRS)

Burton, S. P.; Ferrare, R. A.; Hostetler, C. A.; Hair, J. W.; Kittaka, C.; Vaughn, M. A.; Remer, L. A.

2010-01-01

We derive aerosol extinction profiles from airborne and space-based lidar backscatter signals by constraining the retrieval with column aerosol optical thickness (AOT), with no need to rely on assumptions about aerosol type or lidar ratio. The backscatter data were acquired by the NASA Langley Research Center airborne High Spectral Resolution Lidar (HSRL) and by the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument on the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite. The HSRL also simultaneously measures aerosol extinction coefficients independently using the high spectral resolution lidar technique, thereby providing an ideal data set for evaluating the retrieval. We retrieve aerosol extinction profiles from both HSRL and CALIOP attenuated backscatter data constrained with HSRL, Moderate-Resolution Imaging Spectroradiometer (MODIS), and Multiangle Imaging Spectroradiometer column AOT. The resulting profiles are compared with the aerosol extinction measured by HSRL. Retrievals are limited to cases where the column aerosol thickness is greater than 0.2 over land and 0.15 over water. In the case of large AOT, the results using the Aqua MODIS constraint over water are poorer than Aqua MODIS over land or Terra MODIS. The poorer results relate to an apparent bias in Aqua MODIS AOT over water observed in August 2007. This apparent bias is still under investigation. Finally, aerosol extinction coefficients are derived from CALIPSO backscatter data using AOT from Aqua MODIS for 28 profiles over land and 9 over water. They agree with coincident measurements by the airborne HSRL to within +/-0.016/km +/- 20% for at least two-thirds of land points and within +/-0.028/km +/- 20% for at least two-thirds of ocean points.

Reallocation in modal aerosol models: impacts on predicting aerosol radiative effects

NASA Astrophysics Data System (ADS)

Korhola, T.; Kokkola, H.; Korhonen, H.; Partanen, A.-I.; Laaksonen, A.; Lehtinen, K. E. J.; Romakkaniemi, S.

2013-08-01

In atmospheric modelling applications the aerosol particle size distribution is commonly represented by modal approach, in which particles in different size ranges are described with log-normal modes within predetermined size ranges. Such method includes numerical reallocation of particles from a mode to another for example during particle growth, leading to potentially artificial changes in the aerosol size distribution. In this study we analysed how this reallocation affects climatologically relevant parameters: cloud droplet number concentration, aerosol-cloud interaction coefficient and light extinction coefficient. We compared these parameters between a modal model with and without reallocation routines, and a high resolution sectional model that was considered as a reference model. We analysed the relative differences of the parameters in different experiments that were designed to cover a wide range of dynamic aerosol processes occurring in the atmosphere. According to our results, limiting the allowed size ranges of the modes and the following numerical remapping of the distribution by reallocation, leads on average to underestimation of cloud droplet number concentration (up to 100%) and overestimation of light extinction (up to 20%). The analysis of aerosol first indirect effect is more complicated as the ACI parameter can be either over- or underestimated by the reallocating model, depending on the conditions. However, for example in the case of atmospheric new particle formation events followed by rapid particle growth, the reallocation can cause around average 10% overestimation of the ACI parameter. Thus it is shown that the reallocation affects the ability of a model to estimate aerosol climate effects accurately, and this should be taken into account when using and developing aerosol models.

A Chronology of Annual-Mean Effective Radii of Stratospheric Aerosols from Volcanic Eruptions During the Twentieth Century as Derived From Ground-based Spectral Extinction Measurements

NASA Technical Reports Server (NTRS)

Strothers, Richard B.; Hansen, James E. (Technical Monitor)

2001-01-01

Stratospheric extinction can be derived from ground-based spectral photometric observations of the Sun and other stars (as well as from satellite and aircraft measurements, available since 1979), and is found to increase after large volcanic eruptions. This increased extinction shows a characteristic wavelength dependence that gives information about the chemical composition and the effective (or area weighted mean) radius of the particles responsible for it. Known to be tiny aerosols constituted of sulfuric acid in a water solution, the stratospheric particles at midlatitudes exhibit a remarkable uniformity of their column-averaged effective radii r(sub eff) in the first few months after the eruption. Considering the seven largest eruptions of the twentieth century, r(sub eff) at this phase of peak aerosol abundance is approx. 0.3 micrometers in all cases. A year later, r(sub eff) either has remained about the same size (almost certainly in the case of the Katmai eruption of 1912) or has increased to approx. 0.5 micrometers (definitely so for the Pinatubo eruption of 1991). The reasons for this divergence in aerosol growth are unknown.

Use of In Situ Cloud Condensation Nuclei, Extinction, and Aerosol Size Distribution Measurements to Test a Method for Retrieving Cloud Condensation Nuclei Profiles From Surface Measurements

NASA Technical Reports Server (NTRS)

Ghan, Stephen J.; Rissman, Tracey A.; Ellman, Robert; Ferrare, Richard A.; Turner, David; Flynn, Connor; Wang, Jian; Ogren, John; Hudson, James; Jonsson, Haflidi H.;

Mixed-phase aerosol particles

NASA Astrophysics Data System (ADS)

Corti, T.; Krieger, U. K.; Koop, T.; Peter, T.

2003-04-01

Within a liquid aerosol particle a solid phase may coexist with the liquid over a wide range of ambient conditions. The optical properties of such particles are of interest for a number of reasons. They will affect the scattering albedo of atmospheric aerosols, may cause depolarisation in lidar measurements, and potentially open a window for studying the internal morphology and physical properties (e.g. wetting properties, diffusion constants) of composite particles in laboratory experiments. In this contribution, we will present results of experimental and theoretical work on mixed-phase aerosol particles. The optical properties of mixed-phase particles depend on the location of the inclusion in the liquid phase, which is determined by the surface tensions of the involved interfaces. In the case of complete wetting, the energetically favoured position of the inclusion is in the volume of the liquid phase. For partial wetting, a position at the surface of the liquid phase is favoured, with the contact angle between the solid, liquid and air being described by Young's equation. For systems with small contact angles, the difference in energy between an inclusion situated at the droplets surface and in its volume may be so small that the thermal energy kT is sufficient to displace the inclusion from the droplet surface into its volume. The critical contact angle depends on the size of the inclusion and the droplet and ranges from 0.1 to 10 degrees. Examples of mixed-phase aerosol particles are aged soot particles and sea salt particles at low relative humidity. For aged soot, contact angles on sulphuric acid clearly above 10 degrees have been reported, so that soot inclusions are expected to be located at the surface of aerosol particles. For mixed-phase sea salt particles, consisting of a solid NaCl inclusion and an aqueous solution of mainly NaCl and MgCl2, our measurements on macroscopic NaCl crystals show a contact angle clearly below 10 degrees and possibly as

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

Aerosol particle size distribution in the stratosphere retrieved from SCIAMACHY limb measurements

NASA Astrophysics Data System (ADS)

Malinina, Elizaveta; Rozanov, Alexei; Rozanov, Vladimir; Liebing, Patricia; Bovensmann, Heinrich; Burrows, John P.

2018-04-01

aerosols in the Earth's atmosphere is of a great importance in the scientific community. While tropospheric aerosol influences the radiative balance of the troposphere and affects human health, stratospheric aerosol plays an important role in atmospheric chemistry and climate change. In particular, information about the amount and distribution of stratospheric aerosols is required to initialize climate models, as well as validate aerosol microphysics models and investigate geoengineering. In addition, good knowledge of stratospheric aerosol loading is needed to increase the retrieval accuracy of key trace gases (e.g. ozone or water vapour) when interpreting remote sensing measurements of the scattered solar light. The most commonly used characteristics to describe stratospheric aerosols are the aerosol extinction coefficient and Ångström coefficient. However, the use of particle size distribution parameters along with the aerosol number density is a more optimal approach. In this paper we present a new retrieval algorithm to obtain the particle size distribution of stratospheric aerosol from space-borne observations of the scattered solar light in the limb-viewing geometry. While the mode radius and width of the aerosol particle size distribution are retrieved, the aerosol particle number density profile remains unchanged. The latter is justified by a lower sensitivity of the limb-scattering measurements to changes in this parameter. To our knowledge this is the first data set providing two parameters of the particle size distribution of stratospheric aerosol from space-borne measurements of scattered solar light. Typically, the mode radius and w can be retrieved with an uncertainty of less than 20 %. The algorithm was successfully applied to the tropical region (20° N-20° S) for 10 years (2002-2012) of SCIAMACHY observations in limb-viewing geometry, establishing a unique data set. Analysis of this new climatology for the particle size

SAGE II aerosol extinction and scattering data from balloon-borne photography

NASA Technical Reports Server (NTRS)

Ackerman, M.; Lippens, G.; Chu, W.; De Muer, D.

1987-01-01

Earth limb radiance and extinction near sunset have been observed from a balloon-borne gondola nearly simultaneously and on air masses close to those probed by the SAGE II instrumentation on April 22, 1985. The results show the importance of accuracy of the altitude determination on the aerosol measurements. They indicate an important altitude dependence of the stratospheric aerosol granulometry in agreement with SAGE II results.

The Complex Refractive Index of Volcanic Ash Aerosol Retrieved From Spectral Mass Extinction

NASA Astrophysics Data System (ADS)

Reed, Benjamin E.; Peters, Daniel M.; McPheat, Robert; Grainger, R. G.

2018-01-01

The complex refractive indices of eight volcanic ash samples, chosen to have a representative range of SiO2 contents, were retrieved from simultaneous measurements of their spectral mass extinction coefficient and size distribution. The mass extinction coefficients, at 0.33-19 μm, were measured using two optical systems: a Fourier transform spectrometer in the infrared and two diffraction grating spectrometers covering visible and ultraviolet wavelengths. The particle size distribution was measured using a scanning mobility particle sizer and an optical particle counter; values for the effective radius of ash particles measured in this study varied from 0.574 to 1.16 μm. Verification retrievals on high-purity silica aerosol demonstrated that the Rayleigh continuous distribution of ellipsoids (CDEs) scattering model significantly outperformed Mie theory in retrieving the complex refractive index, when compared to literature values. Assuming the silica particles provided a good analogue of volcanic ash, the CDE scattering model was applied to retrieve the complex refractive index of the eight ash samples. The Lorentz formulation of the complex refractive index was used within the retrievals as a convenient way to ensure consistency with the Kramers-Kronig relation. The short-wavelength limit of the electric susceptibility was constrained by using independently measured reference values of the complex refractive index of the ash samples at a visible wavelength. The retrieved values of the complex refractive indices of the ash samples showed considerable variation, highlighting the importance of using accurate refractive index data in ash cloud radiative transfer models.

Microphysical processes affecting stratospheric aerosol particles

NASA Technical Reports Server (NTRS)

Hamill, P.; Toon, O. B.; Kiang, C. S.

1977-01-01

Physical processes which affect stratospheric aerosol particles include nucleation, condensation, evaporation, coagulation and sedimentation. Quantitative studies of these mechanisms to determine if they can account for some of the observed properties of the aerosol are carried out. It is shown that the altitude range in which nucleation of sulfuric acid-water solution droplets can take place corresponds to that region of the stratosphere where the aerosol is generally found. Since heterogeneous nucleation is the dominant nucleation mechanism, the stratospheric solution droplets are mainly formed on particles which have been mixed up from the troposphere or injected into the stratosphere by volcanoes or meteorites. Particle growth by heteromolecular condensation can account for the observed increase in mixing ratio of large particles in the stratosphere. Coagulation is important in reducing the number of particles smaller than 0.05 micron radius. Growth by condensation, applied to the mixed nature of the particles, shows that available information is consistent with ammonium sulfate being formed by liquid phase chemical reactions in the aerosol particles. The upper altitude limit of the aerosol layer is probably due to the evaporation of sulfuric acid aerosol particles, while the lower limit is due to mixing across the tropopause.

Reconciling aerosol light extinction measurements from spaceborne lidar observations and in-situ measurements in the Arctic

NASA Astrophysics Data System (ADS)

Tesche, M.; Rastak, N.; Charlson, R. J.; Glantz, P.; Zieger, P.; Hansson, H.-C.

2014-03-01

In this study we investigate to what degree it is possible to reconcile continuously recorded particle light extinction coefficients derived from dry in-situ measurements at Zeppelin station (78.92° N, 11.85° E, 475 m a.s.l.) at Ny-Ålesund, Svalbard, that are recalculated to ambient relative humidity, and simultaneous ambient observations with the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) aboard the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) satellite. To our knowledge, this represents the first study that compares spaceborne lidar measurements to optical aerosol properties from short-term in-situ observations (averaged over 5 h) on a case-by-case basis. Finding suitable comparison cases requires an elaborate screening and matching of the CALIOP data with respect to the location of the Zeppelin station as well as in the selection of temporal and spatial averaging intervals for both the ground-based and spaceborne observations. Trustworthy reconciliation of these data cannot be achieved with the closest approach method that is often used in matching CALIOP observations to those taken at ground sites due to the transport pathways of the air parcels that were sampled. The use of trajectories allowed us to establish a connection between spaceborne and ground-based observations for 57 individual overpasses out of a total of 2018 that occurred in our region of interest around Svalbard (0 to 25° E; 75 to 82° N) in the considered year of 2008. Matches could only be established during winter and spring, since the low aerosol load during summer in connection with the strong solar background and the high occurrence rate of clouds strongly influences the performance and reliability of CALIOP observations. Extinction coefficients in the range from 1 to 100 Mm-1 were found for successful matches with an agreement of a factor of 1.85 (median value for a range from 0.38 to 17.9) between the findings of in-situ and spaceborne

1984-1995 Evolution of Stratospheric Aerosol Size, Surface Area, and Volume Derived by Combining SAGE II and CLAES Extinction Measurements

NASA Technical Reports Server (NTRS)

Russell, Philip B.; Bauman, Jill J.

2000-01-01

This SAGE II Science Team task focuses on the development of a multi-wavelength, multi- sensor Look-Up-Table (LUT) algorithm for retrieving information about stratospheric aerosols from global satellite-based observations of particulate extinction. The LUT algorithm combines the 4-wavelength SAGE II extinction measurements (0.385 <= lambda <= 1.02 microns) with the 7.96 micron and 12.82 micron extinction measurements from the Cryogenic Limb Array Etalon Spectrometer (CLAES) instrument, thus increasing the information content available from either sensor alone. The algorithm uses the SAGE II/CLAES composite spectra in month-latitude-altitude bins to retrieve values and uncertainties of particle effective radius R(sub eff), surface area S, volume V and size distribution width sigma(sub g).

Relations Between Cloud Condensation Nuclei And Aerosol Optical Properties Relevant to Remote Sensing: Airborne Measurements in Biomass Burning, Pollution and Dust Aerosol Over North America

NASA Astrophysics Data System (ADS)

Shinozuka, Y.; Clarke, A.; Howell, S.; Kapustin, V.; McNaughton, C.; Zhou, J.; Decarlo, P.; Jimenez, J.; Roberts, G.; Tomlinson, J.; Collins, D.

2008-12-01

Remote sensing of the concentration of cloud condensation nuclei (CCN) would help investigate the indirect effect of tropospheric aerosols on clouds and climate. In order to assess its feasibility, this paper evaluates the spectral-based retrieval technique for aerosol number and seeks one for aerosol solubility, using in-situ aircraft measurements of aerosol size distribution, chemical composition, hygroscopicity, CCN activity and optical properties. Our statistical analysis reveals that the CCN concentration over Mexico can be optically determined to a relative error of <20%, smaller than that for the mainland US and the surrounding oceans (~a factor of 2). Mexico's advantage is four-fold. Firstly, many particles originating from the lightly regulated industrial combustion and biomass burning are large enough to significantly affect light extinction, elevating the correlation between extinction and CCN number in absence of substantial dust. Secondly, the generally low ambient humidity near the major aerosol sources limits the error in the estimated response of particle extinction to humidity changes. Thirdly, because many CCN contain black carbon, light absorption also provides a measure of the CCN concentration. Fourthly, the organic fraction of volatile mass of submicron particles (OMF) is anti-correlated with the wavelength dependence of extinction due to preferential anion uptake by coarse dust, which provides a potential tool for remote-sensing OMF and the particle solubility.

Applications of Sunphotometry to Aerosol Extinction and Surface Anisotropy

NASA Technical Reports Server (NTRS)

Tsay, S. C.; Holben, B. N.; Privette, J. L.

2005-01-01

Support cost-sharing of a newly developed sunphotometer in field deployment for aerosol studies. This is a cost-sharing research to deploy a newly developed sun-sky-surface photometer for studying aerosol extinction and surface anisotropy at the ARM SGP, TWP, and NSA-AAO CART sites and in many field campaigns. Atmospheric aerosols affect the radiative energy balance of the Earth, both directly by perturbing the incoming/outgoing radiation fields and indirectly by influencing the properties/processes of clouds and reactive greenhouse gases. The surface bidirectional reflectance distribution function (BRDF) also plays a crucial role in the radiative energy balance, since the BRDF is required to determine (1) the spectral and spectrally-averaged surface albedo, and (2) the top-of-the-atmosphere (TOA) angular distribution of radiance field. Therefore, the CART sites provide an excellent, albeit unique, opportunity to collect long-term climatic data in characterizing aerosol properties and various types of surface anisotropy.

The Aerosol Models in MODTRAN: Incorporating Selected Measurements From Northern Australia

DTIC Science & Technology

2005-12-01

biomass burning smoke aerosol is modelled assuming the particles are spherical and Mie scattering theory is used to calculate the extinction and...and therefore internally mixed aerosol particles are hygroscopic . Shettle and Fenn model the growth in the size of aerosol particles and changes in...by Sutherland and Khanna [21] was to obtain measurements of the optical properties of organic -based aerosols produced by burning vegetation.

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

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

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

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

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 Impact of Aerosol Particle Mixing State on the Hygroscopicity of Sea Spray Aerosol.

PubMed

Schill, Steven R; Collins, Douglas B; Lee, Christopher; Morris, Holly S; Novak, Gordon A; Prather, Kimberly A; Quinn, Patricia K; Sultana, Camille M; Tivanski, Alexei V; Zimmermann, Kathryn; Cappa, Christopher D; Bertram, Timothy H

2015-06-24

Aerosol particles influence global climate by determining cloud droplet number concentrations, brightness, and lifetime. Primary aerosol particles, such as those produced from breaking waves in the ocean, display large particle-particle variability in chemical composition, morphology, and physical phase state, all of which affect the ability of individual particles to accommodate water and grow into cloud droplets. Despite such diversity in molecular composition, there is a paucity of methods available to assess how particle-particle variability in chemistry translates to corresponding differences in aerosol hygroscopicity. Here, an approach has been developed that allows for characterization of the distribution of aerosol hygroscopicity within a chemically complex population of atmospheric particles. This methodology, when applied to the interpretation of nascent sea spray aerosol, provides a quantitative framework for connecting results obtained using molecular mimics generated in the laboratory with chemically complex ambient aerosol. We show that nascent sea spray aerosol, generated in situ in the Atlantic Ocean, displays a broad distribution of particle hygroscopicities, indicative of a correspondingly broad distribution of particle chemical compositions. Molecular mimics of sea spray aerosol organic material were used in the laboratory to assess the volume fractions and molecular functionality required to suppress sea spray aerosol hygroscopicity to the extent indicated by field observations. We show that proper accounting for the distribution and diversity in particle hygroscopicity and composition are important to the assessment of particle impacts on clouds and global climate.

An Aerosol Extinction-to-Backscatter Ratio Database Derived from the NASA Micro-Pulse Lidar Network: Applications for Space-based Lidar Observations

NASA Technical Reports Server (NTRS)

Welton, Ellsworth J.; Campbell, James R.; Spinhime, James D.; Berkoff, Timothy A.; Holben, Brent; Tsay, Si-Chee; Bucholtz, Anthony

2004-01-01

Backscatter lidar signals are a function of both backscatter and extinction. Hence, these lidar observations alone cannot separate the two quantities. The aerosol extinction-to-backscatter ratio, S, is the key parameter required to accurately retrieve extinction and optical depth from backscatter lidar observations of aerosol layers. S is commonly defined as 4*pi divided by the product of the single scatter albedo and the phase function at 180-degree scattering angle. Values of S for different aerosol types are not well known, and are even more difficult to determine when aerosols become mixed. Here we present a new lidar-sunphotometer S database derived from Observations of the NASA Micro-Pulse Lidar Network (MPLNET). MPLNET is a growing worldwide network of eye-safe backscatter lidars co-located with sunphotometers in the NASA Aerosol Robotic Network (AERONET). Values of S for different aerosol species and geographic regions will be presented. A framework for constructing an S look-up table will be shown. Look-up tables of S are needed to calculate aerosol extinction and optical depth from space-based lidar observations in the absence of co-located AOD data. Applications for using the new S look-up table to reprocess aerosol products from NASA's Geoscience Laser Altimeter System (GLAS) will be discussed.

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

Unique DNA-barcoded aerosol test particles for studying aerosol transport

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

Harding, Ruth N.; Hara, Christine A.; Hall, Sara B.

Data are presented for the first use of novel DNA-barcoded aerosol test particles that have been developed to track the fate of airborne contaminants in populated environments. Until DNATrax (DNA Tagged Reagents for Aerosol eXperiments) particles were developed, there was no way to rapidly validate air transport models with realistic particles in the respirable range of 1–10 μm in diameter. The DNATrax particles, developed at Lawrence Livermore National Laboratory (LLNL) and tested with the assistance of the Pentagon Force Protection Agency, are the first safe and effective materials for aerosol transport studies that are identified by DNA molecules. The usemore » of unique synthetic DNA barcodes overcomes the challenges of discerning the test material from pre-existing environmental or background contaminants (either naturally occurring or previously released). The DNATrax particle properties are demonstrated to have appropriate size range (approximately 1–4.5 μm in diameter) to accurately simulate bacterial spore transport. As a result, we describe details of the first field test of the DNATrax aerosol test particles in a large indoor facility.« less

Unique DNA-barcoded aerosol test particles for studying aerosol transport

DOE PAGES

Harding, Ruth N.; Hara, Christine A.; Hall, Sara B.; ...

2016-03-22

Data are presented for the first use of novel DNA-barcoded aerosol test particles that have been developed to track the fate of airborne contaminants in populated environments. Until DNATrax (DNA Tagged Reagents for Aerosol eXperiments) particles were developed, there was no way to rapidly validate air transport models with realistic particles in the respirable range of 1–10 μm in diameter. The DNATrax particles, developed at Lawrence Livermore National Laboratory (LLNL) and tested with the assistance of the Pentagon Force Protection Agency, are the first safe and effective materials for aerosol transport studies that are identified by DNA molecules. The usemore » of unique synthetic DNA barcodes overcomes the challenges of discerning the test material from pre-existing environmental or background contaminants (either naturally occurring or previously released). The DNATrax particle properties are demonstrated to have appropriate size range (approximately 1–4.5 μm in diameter) to accurately simulate bacterial spore transport. As a result, we describe details of the first field test of the DNATrax aerosol test particles in a large indoor facility.« less

Extinction-to-Backscatter Ratios of Lofted Aerosol Layers Observed During the First Three Months of CALIPSO Measurements

NASA Technical Reports Server (NTRS)

Omar, Ali H.; Vaughan, Mark A.; Liu, Zhaoyan; Hu, Yongxiang; Reagan, John A.; Winker, David M.

2007-01-01

Case studies from the first three months of the Cloud and Aerosol Lidar and Infrared Pathfinder Spaceborne Observations (CALIPSO) measurements of lofted aerosol layers are analyzed using transmittance [Young, 1995] and two-wavelength algorithms [Vaughan et al., 2004] to determine the aerosol extinction-to-backscatter ratios at 532 and 1064 nm. The transmittance method requires clear air below the layer so that the transmittance through the layer can be determined. Suitable scenes are selected from the browse images and clear air below features is identified by low 532 nm backscatter signal and confirmed by low depolarization and color ratios. The transmittance and two-wavelength techniques are applied to a number of lofted layers and the extinction-to-backscatter ratios are compared with values obtained from the CALIPSO aerosol models [Omar et al., 2004]. The results obtained from these studies are used to adjust the aerosol models and develop observations based extinction-to-backscatter ratio look-up tables and phase functions. Values obtained by these techniques are compared to Sa determinations using other independent methods with a goal of developing probability distribution functions of aerosol type-specific extinction to backscatter ratios. In particular, the results are compared to values determined directly by the High Spectral Resolution Lidar (HSRL) during the CALIPSO CloudSat Validation Experiments (CCVEX) and Sa determined by the application of the two-wavelength lidar Constrained Ratio Aerosol Model-fit (CRAM) retrieval approach [Cattrall et al., 2005; Reagan et al., 2004] to the HSRL data. The results are also compared to values derived using the empirical relationship between the multiple-scattering fraction and the linear depolarization ratio by using Monte Carlo simulations of water clouds [Hu et al., 2006].

Enhanced THz extinction in arrays of resonant semiconductor particles.

PubMed

Schaafsma, Martijn C; Georgiou, Giorgos; Rivas, Jaime Gómez

2015-09-21

We demonstrate experimentally the enhanced THz extinction by periodic arrays of resonant semiconductor particles. This phenomenon is explained in terms of the radiative coupling of localized resonances with diffractive orders in the plane of the array (Rayleigh anomalies). The experimental results are described by numerical calculations using a coupled dipole model and by Finite-Difference in Time-Domain simulations. An optimum particle size for enhancing the extinction efficiency of the array is found. This optimum is determined by the frequency detuning between the localized resonances in the individual particles and the Rayleigh anomaly. The extinction calculations and measurements are also compared to near-field simulations illustrating the optimum particle size for the enhancement of the near-field.

How well can we Measure the Vertical Profile of Tropospheric Aerosol Extinction?

NASA Technical Reports Server (NTRS)

Schmid, Beat; Ferrare, R.; Flynn, C.; Elleman, R.; Covert, D.; Strawa, A.; Welton, E.; Turner, D.; Jonsson, H.; Redemann, J.

2005-01-01

The recent Department of Energy Atmospheric Radiation Measurement (ARM) Aerosol Intensive Operations Period (MOP, May 2003) yielded one of the best measurement sets obtained to-date to assess our ability to measure the vertical profile of ambient aerosol extinction sigma(sub ep)(lambda) in the lower troposphere. During one month, a heavily instrumented aircraft with well characterized aerosol sampling ability carrying well proven and new aerosol instrumentation, devoted most of the 60 available flight hours to flying vertical profiles over the heavily instrumented ARM Southern Great Plains (SGP) Climate Research Facility (CRF). This allowed us to compare vertical extinction profiles obtained from 6 different instuments: airborne Sun photometer (AATS-14), airborne nephelometer/absorption photometer, airborne cavity ring-down system, ground-based Raman lidar and 2 ground-based elastic backscatter lidars. We find the in-situ measured sigma(sub ep)(lambda) to be lower than the AATS-14 derived values. Bias differences are 0.002 - 0.004 K/m equivalent to 12-17% in the visible, or 45% in the near-infrared. On the other hand, we find that with respect to AATS-14, the lidar sigma(sub ep)(lambda) are higher. An unnoticed loss of sensitivity of the Raman lidar had occurred leading up to AIOP and we expect better agreement from the recently restored system looking at the collective results from 6 field campaigns conducted since 1996, airborne in situ measurements of sigma(sub ep)(lambda) tend to be biased slightly low (17% at visible wavelengths) when compared to airborne Sun photometer sigma(sub ep)(lambda). On the other hand, sigma(sub ep)(lambda) values derived from lidars tend to have no or positive biases. From the bias differences we conclude that the typical systematic error associated with measuring the tropospheric vertical profile of the ambient aerosol extinction with current state of-the art instrumentation is 15-20% at visible wavelengths and potentially larger in

Study of MPLNET-Derived Aerosol Climatology over Kanpur, India, and Validation of CALIPSO Level 2 Version 3 Backscatter and Extinction Products

NASA Technical Reports Server (NTRS)

Misra, Amit; Tripathi, S. N.; Kaul, D. S.; Welton, Ellsworth J.

2012-01-01

The level 2 aerosol backscatter and extinction profiles from the NASA Micropulse Lidar Network (MPLNET) at Kanpur, India, have been studied from May 2009 to September 2010. Monthly averaged extinction profiles from MPLNET shows high extinction values near the surface during October March. Higher extinction values at altitudes of 24 km are observed from April to June, a period marked by frequent dust episodes. Version 3 level 2 Cloud Aerosol Lidar with Orthogonal Polarization (CALIOP) aerosol profile products have been compared with corresponding data from MPLNET over Kanpur for the above-mentioned period. Out of the available backscatter profiles, the16 profiles used in this study have time differences less than 3 h and distances less than 130 km. Among these profiles, four cases show good comparison above 400 m with R2 greater than 0.7. Comparison with AERONET data shows that the aerosol type is properly identified by the CALIOP algorithm. Cloud contamination is a possible source of error in the remaining cases of poor comparison. Another source of error is the improper backscatter-to-extinction ratio, which further affects the accuracy of extinction coefficient retrieval.

Extinction by a Homogeneous Spherical Particle in an Absorbing Medium

NASA Technical Reports Server (NTRS)

Mishchenko, Michael I.; Videen, Gorden; Yang, Ping

2017-01-01

We use a recent computer implementation of the first principles theory of electromagnetic scattering to compute far-field extinction by a spherical particle embedded in an absorbing unbounded host. Our results show that the suppressing effect of increasing absorption inside the host medium on the ripple structure of the extinction efficiency factor as a function of the size parameter is similar to the well-known effect of increasing absorption inside a particle embedded in a nonabsorbing host. However, the accompanying effects on the interference structure of the extinction efficiency curves are diametrically opposite. As a result, sufficiently large absorption inside the host medium can cause negative particulate extinction. We offer a simple physical explanation of the phenomenon of negative extinction consistent with the interpretation of the interference structure as being the result of interference of the field transmitted by the particle and the diffracted field due to an incomplete wave front resulting from the blockage of the incident plane wave by the particle's geometrical projection.

Evaluation, Feasibility, and Design of a Three-Wavelength Infrared Atmospheric Aerosol Extinctiometer.

DTIC Science & Technology

1980-09-02

laser or searchlight measurements . The study program consisted of three basic tasks: (1) a review of existing techniques for measuring aerosol extinction ...to aerosol extinction along a path can be deduced. Solutions to this problcaii fall into several classes. One class of solutions invoLves measuring ...employed such a windowless system to measure the absorption of an artificial aerosol consisting of quartz particles, using a CO 2 laser in the

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

Light extinction in the atmosphere

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

Laulainen, N.

1992-06-01

Atmospheric aerosol particles originating from natural sources, such as volcanos and sulfur-bearing gas emissions from the oceans, and from human sources, such as sulfur emissions from fossil fuel combustion and biomass burning, strongly affect visual air quality and are suspected to significantly affect radiative climate forcing of the planet. During the daytime, aerosols obscure scenic vistas, while at night they diminish our ability to observe stellar objects. Scattering of light is the main means by which aerosols attenuate and redistribute light in the atmosphere and by which aerosols can alter and reduce visibility and potentially modify the energy balance ofmore » the planet. Trends and seasonal variability of atmospheric aerosol loading, such as column-integrated light extinction or optical depth, and how they may affect potential climate change have been difficult to quantify because there have been few observations made of important aerosol optical parameters, such as optical depth, over the globe and over time and often these are of uneven quality. To address questions related to possible climate change, there is a pressing need to acquire more high-quality aerosol optical depth data. Extensive deployment of improved solar radiometers over the next few years will provide higher-quality extinction data over a wider variety of locations worldwide. An often overlooked source of turbidity data, however, is available from astronomical observations, particularly stellar photoelectric photometry observations. With the exception of the Project ASTRA articles published almost 20 years ago, few of these data ever appear in the published literature. This paper will review the current status of atmospheric extinction observations, as highlighted by the ASTRA work and augmented by more recent solar radiometry measurements.« less

Stratospheric Aerosol and Gas Experiment (SAGE) II and III Aerosol Extinction Measurements in the Arctic Middle and Upper Troposphere

NASA Technical Reports Server (NTRS)

Treffeisen, R. E.; Thomason, L. W.; Strom, J.; Herber, A. B.; Burton, S. P.; Yamanouchi, T.

2006-01-01

In recent years, substantial effort has been expended toward understanding the impact of tropospheric aerosols on Arctic climate and chemistry. A significant part of this effort has been the collection and documentation of extensive aerosol physical and optical property data sets. However, the data sets present significant interpretive challenges because of the diverse nature of these measurements. Among the longest continuous records is that by the spaceborne Stratospheric Aerosol and Gas Experiment (SAGE) II. Although SAGE tropospheric measurements are restricted to the middle and upper troposphere, they may be able to provide significant insight into the nature and variability of tropospheric aerosol, particularly when combined with ground and airborne observations. This paper demonstrates the capacity of aerosol products from SAGE II and its follow-on experiment SAGE III to describe the temporal and vertical variations of Arctic aerosol characteristics. We find that the measurements from both instruments are consistent enough to be combined. Using this combined data set, we detect a clear annual cycle in the aerosol extinction for the middle and upper Arctic troposphere.

Single Aerosol Particle Studies Using Optical Trapping Raman And Cavity Ringdown Spectroscopy

NASA Astrophysics Data System (ADS)

Gong, Z.; Wang, C.; Pan, Y. L.; Videen, G.

2017-12-01

Due to the physical and chemical complexity of aerosol particles and the interdisciplinary nature of aerosol science that involves physics, chemistry, and biology, our knowledge of aerosol particles is rather incomplete; our current understanding of aerosol particles is limited by averaged (over size, composition, shape, and orientation) and/or ensemble (over time, size, and multi-particles) measurements. Physically, single aerosol particles are the fundamental units of any large aerosol ensembles. Chemically, single aerosol particles carry individual chemical components (properties and constituents) in particle ensemble processes. Therefore, the study of single aerosol particles can bridge the gap between aerosol ensembles and bulk/surface properties and provide a hierarchical progression from a simple benchmark single-component system to a mixed-phase multicomponent system. A single aerosol particle can be an effective reactor to study heterogeneous surface chemistry in multiple phases. Latest technological advances provide exciting new opportunities to study single aerosol particles and to further develop single aerosol particle instrumentation. We present updates on our recent studies of single aerosol particles optically trapped in air using the optical-trapping Raman and cavity ringdown spectroscopy.

A Miniature Aerosol Sensor for Detecting Polydisperse Airborne Ultrafine Particles.

PubMed

Zhang, Chao; Wang, Dingqu; Zhu, Rong; Yang, Wenming; Jiang, Peng

2017-04-22

Counting and sizing of polydisperse airborne nanoparticles have attracted most attentions owing to increasing widespread presence of airborne engineered nanoparticles or ultrafine particles. Here we report a miniature aerosol sensor to detect particle size distribution of polydisperse ultrafine particles based on ion diffusion charging and electrical detection. The aerosol sensor comprises a couple of planar electrodes printed on two circuit boards assembled in parallel, where charging, precipitation and measurement sections are integrated into one chip, which can detect aerosol particle size in of 30-500 nm, number concentration in range of 5 × 10²-10⁷ /cm³. The average relative errors of the measured aerosol number concentration and the particle size are estimated to be 12.2% and 13.5% respectively. A novel measurement scheme is proposed to actualize a real-time detection of polydisperse particles by successively modulating the measurement voltage and deducing the particle size distribution through a smart data fusion algorithm. The effectiveness of the aerosol sensor is experimentally demonstrated via measurements of polystyrene latex (PSL) aerosol and nucleic acid aerosol, as well as sodium chloride aerosol particles.

[Analysis of visible extinction spectrum of particle system and selection of optimal wavelength].

PubMed

Sun, Xiao-gang; Tang, Hong; Yuan, Gui-bin

2008-09-01

In the total light scattering particle sizing technique, the extinction spectrum of particle system contains some information about the particle size and refractive index. The visible extinction spectra of the common monomodal and biomodal R-R particle size distribution were computed, and the variation in the visible extinction spectrum with the particle size and refractive index was analyzed. The corresponding wavelengths were selected as the measurement wavelengths at which the second order differential extinction spectrum was discontinuous. Furthermore, the minimum and the maximum wavelengths in the visible region were also selected as the measurement wavelengths. The genetic algorithm was used as the inversion method under the dependent model The computer simulation and experiments illustrate that it is feasible to make an analysis of the extinction spectrum and use this selection method of the optimal wavelength in the total light scattering particle sizing. The rough contour of the particle size distribution can be determined after the analysis of visible extinction spectrum, so the search range of the particle size parameter is reduced in the optimal algorithm, and then a more accurate inversion result can be obtained using the selection method. The inversion results of monomodal and biomodal distribution are all still satisfactory when 1% stochastic noise is put in the transmission extinction measurement values.

Wind reduction by aerosol particles

NASA Astrophysics Data System (ADS)

Jacobson, Mark Z.; Kaufman, Yoram J.

2006-12-01

Aerosol particles are known to affect radiation, temperatures, stability, clouds, and precipitation, but their effects on spatially-distributed wind speed have not been examined to date. Here, it is found that aerosol particles, directly and through their enhancement of clouds, may reduce near-surface wind speeds below them by up to 8% locally. This reduction may explain a portion of observed ``disappearing winds'' in China, and it decreases the energy available for wind-turbine electricity. In California, slower winds reduce emissions of wind-driven soil dust and sea spray. Slower winds and cooler surface temperatures also reduce moisture advection and evaporation. These factors, along with the second indirect aerosol effect, may reduce California precipitation by 2-5%, contributing to a strain on water supply.

A Miniature Aerosol Sensor for Detecting Polydisperse Airborne Ultrafine Particles

PubMed Central

Zhang, Chao; Wang, Dingqu; Zhu, Rong; Yang, Wenming; Jiang, Peng

2017-01-01

Counting and sizing of polydisperse airborne nanoparticles have attracted most attentions owing to increasing widespread presence of airborne engineered nanoparticles or ultrafine particles. Here we report a miniature aerosol sensor to detect particle size distribution of polydisperse ultrafine particles based on ion diffusion charging and electrical detection. The aerosol sensor comprises a couple of planar electrodes printed on two circuit boards assembled in parallel, where charging, precipitation and measurement sections are integrated into one chip, which can detect aerosol particle size in of 30–500 nm, number concentration in range of 5 × 102–5 × 107 /cm3. The average relative errors of the measured aerosol number concentration and the particle size are estimated to be 12.2% and 13.5% respectively. A novel measurement scheme is proposed to actualize a real-time detection of polydisperse particles by successively modulating the measurement voltage and deducing the particle size distribution through a smart data fusion algorithm. The effectiveness of the aerosol sensor is experimentally demonstrated via measurements of polystyrene latex (PSL) aerosol and nucleic acid aerosol, as well as sodium chloride aerosol particles. PMID:28441740

Selection of quasi-monodisperse super-micron aerosol particles

NASA Astrophysics Data System (ADS)

Rösch, Michael; Pfeifer, Sascha; Wiedensohler, Alfred; Stratmann, Frank

2014-05-01

Size-segregated quasi monodisperse particles are essential for e.g. fundamental research concerning cloud microphysical processes. Commonly a DMA (Differential Mobility Analyzer) is used to produce quasi-monodisperse submicron particles. Thereto first, polydisperse aerosol particles are bipolarly charged by a neutralizer, and then selected according to their electrical mobility with the DMA [Knutson et al. 1975]. Selecting a certain electrical mobility with a DMA results in a particle size distribution, which contains singly charged particles as well as undesired multiply charged larger particles. Often these larger particles need to either be removed from the generated aerosol or their signals have to be corrected for in the data inversion and interpretation process. This problem becomes even more serious when considering super-micron particles. Here we will present two different techniques for generating quasi-monodisperse super-micron aerosol particles with no or only an insignificant number of larger sized particles being present. First, we use a combination of a cyclone with adjustable aerodynamic cut-off diameter and our custom-built Maxi-DMA [Raddatz et al. 2013]. The cyclone removes particles larger than the desired ones prior to mobility selection with the DMA. This results in a reduction of the number of multiply charged particles of up to 99.8%. Second, we utilize a new combination of cyclone and PCVI (Pumped Counterflow Virtual Impactor), which is based on purely inertial separation and avoids particle charging. The PCVI instrument was previously described by Boulter et al. (2006) and Kulkarni et al. (2011). With our two setups we are able to produce quasi-monodisperse aerosol particles in the diameter range from 0.5 to 4.4 µm without a significant number of larger undesired particles being present. Acknowledgements: This work was done within the framework of the DFG funded Ice Nucleation research UnIT (INUIT, FOR 1525) under WE 4722/1-1. References

The PM2.5 threshold for aerosol extinction in the Beijing megacity

NASA Astrophysics Data System (ADS)

Kong, Lingbin; Xin, Jinyuan; Liu, Zirui; Zhang, Kequan; Tang, Guiqian; Zhang, Wenyu; Wang, Yuesi

2017-10-01

Particulate pollution has remained at a high level in the megacity of Beijing in the past decade. The PM2.5, PM10, aerosol optical depth (AOD), Angstrom exponent(α), and PM2.5/PM10 ratio (the proportion of PM2.5 in PM10) in Beijing were 70±6 μg m-3, 128±6 μg m-3, 0.57 ± 0.05, 1.10 ± 0.08, 45 ± 4%, respectively, from 2005 to 2014. The annual means of PM concentration, AOD, α, and PM2.5/PM10 ratio decreased slightly during this decade, meanwhile PM concentration increased in the winter. Furthermore, we found there were thresholds of PM2.5 concentration for aerosol extinction. When the PM concentration was lower than a certain threshold, AOD decreased quickly with the decline of PM concentration. To make the improvement of the particle pollution more noticeable, the PM concentration should be controlled under the threshold. The annual averaged threshold is 63 μg m-3, and the threshold values reached the maximum of 74 μg m-3 in spring, ranged from 54 to 56 μg m-3 in the three other seasons. The threshold values ranged from 55 to 77 μg m-3 under other relevant factors, including air masses directions and relative humidity.

Accelerated simulation of stochastic particle removal processes in particle-resolved aerosol models

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

Curtis, J.H.; Michelotti, M.D.; Riemer, N.

2016-10-01

Stochastic particle-resolved methods have proven useful for simulating multi-dimensional systems such as composition-resolved aerosol size distributions. While particle-resolved methods have substantial benefits for highly detailed simulations, these techniques suffer from high computational cost, motivating efforts to improve their algorithmic efficiency. Here we formulate an algorithm for accelerating particle removal processes by aggregating particles of similar size into bins. We present the Binned Algorithm for particle removal processes and analyze its performance with application to the atmospherically relevant process of aerosol dry deposition. We show that the Binned Algorithm can dramatically improve the efficiency of particle removals, particularly for low removalmore » rates, and that computational cost is reduced without introducing additional error. In simulations of aerosol particle removal by dry deposition in atmospherically relevant conditions, we demonstrate about 50-times increase in algorithm efficiency.« less

The Influence of Chemical Composition and Relative Humidity on the Optical Properties of Aerosols During the Southern Oxidant and Aerosol Study (SOAS)

NASA Astrophysics Data System (ADS)

Attwood, A. R.; Washenfelder, R. A.; Brock, C. A.; Brown, S. S.; Hu, W.; Campuzano Jost, P.; Day, D. A.; Palm, B. B.; Simoes de Sa, S.; Jimenez, J. L.

2013-12-01

Atmospheric particles are produced from a wide variety of both anthropogenic and natural sources and play an important role in the Earth's radiative budget by direct scattering and absorption of radiation. To address this impact, in situ measurements of aerosol optical, chemical and hygroscopic properties were performed during the Southern Oxidant and Aerosol Study (SOAS), which took place in the summer of 2013. Ground based measurements of sub-micron aerosol in the southeastern United States were made to investigate the influence of chemical composition and hygroscopicity on aerosol optical properties. We report the wavelength dependence of aerosol extinction cross sections measured with a novel broadband cavity enhanced spectrometer covering a wavelength range of 360-420 nm using two light emitting diodes (LED) and a separate cavity ring down (CRDS) channel. The sensitivity of the relative humidity dependence of extinction based on the type of aerosol present is examined and we show that the optical properties and hygroscopicity of aerosols are greatly influenced by the fraction of sulfate and organics within the particles. Additional data analysis from the SOAS campaign will be presented. The results, thus far, illustrate that the variability in aerosol chemical composition can impact visibility and climate forcing in this region.

A miniature particle counter LOAC under meteorological balloon for the survey of stratospheric aerosols - comparison with other datasets

NASA Astrophysics Data System (ADS)

Vignelles, Damien; Berthet, Bwenael; Renard, Jean-Baptiste; Rieger, Landon; Bourassa, Adam; Vernier, Jean-Paul; Taha, Ghassan; Khaykin, Sergey; Lurton, Thibaut; Jegou, Fabrice; Couté, Benoît; Duverger, Vincent

2017-04-01

some of the difference between remote sensing methods and in-situ measurements but suggest also that local variations in the stratospheric aerosol contents may exist during volcanic quiescent periods. Flights made through the Calbucoplume in stratosphere during the summer 2015 show that LOAC can describe distribution in size and particle concentrations in a perturbed lower stratosphere. In the stratosphere free of volcanic influence, an integration time of 10 minutes shows better results. Kremser et al. (2016) Stratospheric aerosol—Observations, processes, and impact on climate. Rev. Geophys. 54, 2015RG000511. doi:10.1002/2015RG000511 Neely, R.R., English, J.M., Toon, O.B., Solomon, S., Mills, M., Thayer, J.P., 2011. Implications of extinction due to meteoritic smoke in the upper stratosphere: EXTINCTION DUE TO METEORITIC SMOKE. Geophys. Res. Lett. 38, doi:10.1029/2011GL049865 Renard et al. (2016) LOAC: a small aerosol optical sounter/sizer for ground-based and balloon measurements AMT. 9, 1721-1742. doi:10.5194/amt-9-1724-2016

Dispersion of aerosol particles undergoing Brownian motion

NASA Astrophysics Data System (ADS)

Alonso, Manuel; Endo, Yoshiyuki

2001-12-01

The variance of the position distribution for a Brownian particle is derived in the general case where the particle is suspended in a flowing medium and, at the same time, is acted upon by an external field of force. It is shown that, for uniform force and flow fields, the variance is equal to that for a free particle. When the force field is not uniform but depends on spatial location, the variance can be larger or smaller than that for a free particle depending on whether the average motion of the particles takes place toward, respectively, increasing or decreasing absolute values of the field strength. A few examples concerning aerosol particles are discussed, with especial attention paid to the mobility classification of charged aerosols by a non-uniform electric field. As a practical application of these ideas, a new design of particle-size electrostatic classifier differential mobility analyser (DMA) is proposed in which the aerosol particles migrate between the electrodes in a direction opposite to that for a conventional DMA, thereby improving the resolution power of the instrument.

Fluorescence lifetime imaging of optically levitated aerosol: a technique to quantitatively map the viscosity of suspended aerosol particles.

PubMed

Fitzgerald, C; Hosny, N A; Tong, H; Seville, P C; Gallimore, P J; Davidson, N M; Athanasiadis, A; Botchway, S W; Ward, A D; Kalberer, M; Kuimova, M K; Pope, F D

2016-08-21

We describe a technique to measure the viscosity of stably levitated single micron-sized aerosol particles. Particle levitation allows the aerosol phase to be probed in the absence of potentially artefact-causing surfaces. To achieve this feat, we combined two laser based techniques: optical trapping for aerosol particle levitation, using a counter-propagating laser beam configuration, and fluorescent lifetime imaging microscopy (FLIM) of molecular rotors for the measurement of viscosity within the particle. Unlike other techniques used to measure aerosol particle viscosity, this allows for the non-destructive probing of viscosity of aerosol particles without interference from surfaces. The well-described viscosity of sucrose aerosol, under a range of relative humidity conditions, is used to validate the technique. Furthermore we investigate a pharmaceutically-relevant mixture of sodium chloride and salbutamol sulphate under humidities representative of in vivo drug inhalation. Finally, we provide a methodology for incorporating molecular rotors into already levitated particles, thereby making the FLIM/optical trapping technique applicable to real world aerosol systems, such as atmospheric aerosols and those generated by pharmaceutical inhalers.

Research on the peculiarity of optical parameters of atmospheric aerosol in Guangzhou coastal areas

NASA Astrophysics Data System (ADS)

Li, Shasha; Li, Xuebin; Zhang, Wenzhong; Bai, Shiwei; Liu, Qing; Zhu, Wenyue; Weng, Ningquan

2018-02-01

The long-term measurement of atmospheric aerosol is constructed via such equipment as visibility meter, optical particle counter, solar radiometer, automatic weather station, aerosol laser radar and aerosol scattering absorption coefficient measurer and so on during the year of 2010 and 2017 in the coastal areas of Guangzhou, China to study the optical parameter characteristics of atmospheric aerosol and establish the aerosol optical parameter mode in such areas. The effects of temperature and humidity on aerosol concentration, extinction and absorption coefficient are analyzed and the statistical characteristics of atmospheric temperature and humidity, visibility, extinction profiles and other parameters in different months are tallied, preliminarily establishing the atmospheric aerosol optical parameter pattern in Guangzhou coastal areas.

The necessity of microscopy to characterize the optical properties of size-selected, nonspherical aerosol particles.

PubMed

Veghte, Daniel P; Freedman, Miriam A

2012-11-06

It is currently unknown whether mineral dust causes a net warming or cooling effect on the climate system. This uncertainty stems from the varied and evolving shape and composition of mineral dust, which leads to diverse interactions of dust with solar and terrestrial radiation. To investigate these interactions, we have used a cavity ring-down spectrometer to study the optical properties of size-selected calcium carbonate particles, a reactive component of mineral dust. The size selection of nonspherical particles like mineral dust can differ from spherical particles in the polydispersity of the population selected. To calculate the expected extinction cross sections, we use Mie scattering theory for monodisperse spherical particles and for spherical particles with the polydispersity observed in transmission electron microscopy images. Our results for calcium carbonate are compared to the well-studied system of ammonium sulfate. While ammonium sulfate extinction cross sections agree with Mie scattering theory for monodisperse spherical particles, the results for calcium carbonate deviate at large and small particle sizes. We find good agreement for both systems, however, between the calculations performed using the particle images and the cavity ring-down data, indicating that both ammonium sulfate and calcium carbonate can be treated as polydisperse spherical particles. Our results indicate that having an independent measure of polydispersity is essential for understanding the optical properties of nonspherical particles measured with cavity ring-down spectroscopy. Our combined spectroscopy and microscopy techniques demonstrate a novel method by which cavity ring-down spectroscopy can be extended for the study of more complex aerosol particles.

The Life Cycle of Stratospheric Aerosol Particles

NASA Technical Reports Server (NTRS)

Hamill, Patrick; Jensen, Eric J.; Russell, P. B.; Bauman, Jill J.

1997-01-01

This paper describes the life cycle of the background (nonvolcanic) stratospheric sulfate aerosol. The authors assume the particles are formed by homogeneous nucleation near the tropical tropopause and are carried aloft into the stratosphere. The particles remain in the Tropics for most of their life, and during this period of time a size distribution is developed by a combination of coagulation, growth by heteromolecular condensation, and mixing with air parcels containing preexisting sulfate particles. The aerosol eventually migrates to higher latitudes and descends across isentropic surfaces to the lower stratosphere. The aerosol is removed from the stratosphere primarily at mid- and high latitudes through various processes, mainly by isentropic transport across the tropopause from the stratosphere into the troposphere.

The Angstrom Exponent and Bimodal Aerosol Size Distributions

NASA Technical Reports Server (NTRS)

Schuster, Gregory L.; Dubovik, Oleg; Holben, Brent H.

2005-01-01

Powerlaws have long been used to describe the spectral dependence of aerosol extinction, and the wavelength exponent of the aerosol extinction powerlaw is commonly referred to as the Angstrom exponent. The Angstrom exponent is often used as a qualitative indicator of aerosol particle size, with values greater than two indicating small particles associated with combustion byproducts, and values less than one indicating large particles like sea salt and dust. In this study, we investigate the relationship between the Angstrom exponent and the mode parameters of bimodal aerosol size distributions using Mie theory calculations and Aerosol Robotic Network (AERONET) retrievals. We find that Angstrom exponents based upon seven wavelengths (0.34, 0.38, 0.44, 0.5, 0.67, 0.87, and 1.02 micrometers) are sensitive to the volume fraction of aerosols with radii less then 0.6 micrometers, but not to the fine mode effective radius. The Angstrom exponent is also known to vary with wavelength, which is commonly referred to as curvature; we show how the spectral curvature can provide additional information about aerosol size distributions for intermediate values of the Angstrom exponent. Curvature also has a significant effect on the conclusions that can be drawn about two-wavelength Angstrom exponents; long wavelengths (0.67, 0.87 micrometers) are sensitive to fine mode volume fraction of aerosols but not fine mode effective radius, while short wavelengths (0.38, 0.44 micrometers) are sensitive to the fine mode effective radius but not the fine mode volume fraction.

Comparison of the DiSCmini aerosol monitor to a handheld condensation particle counter and a scanning mobility particle sizer for submicrometer sodium chloride and metal aerosols

PubMed Central

Mills, Jessica B.; Park, Jae Hong; Peters, Thomas M.

2016-01-01

We evaluated the robust, lightweight DiSCmini (DM) aerosol monitor for its ability to measure the concentration and mean diameter of submicrometer aerosols. Tests were conducted with monodispersed and polydispersed aerosols composed of two particle types (sodium chloride, NaCl, and spark generated metal particles, which simulate particles found in welding fume) at three different steady-state concentration ranges (Low, <103; Medium, 103–104; and High, >104 particles/cm3). Particle number concentration, lung deposited surface area (LDSA) concentration, and mean size measured with the DM were compared to those measured with reference instruments, a scanning mobility particle sizer (SMPS) and a handheld condensation particle counter (CPC). Particle number concentrations measured with the DM were within 21% of those measured by reference instruments for polydisperse aerosols. Poorer agreement was observed for monodispersed aerosols (±35% for most tests and +130% for 300-nm NaCl). LDSA concentrations measured by the DM were 96% to 155% of those estimated with the SMPS. The geometric mean diameters measured with the DM were within 30% of those measured with the SMPS for monodispersed aerosols and within 25% for polydispersed aerosols (except for the case when the aerosol contained a substantial number of particles larger than 300 nm). The accuracy of the DM is reasonable for particles smaller than 300 nm but caution should be exercised when particles larger than 300 nm are present. PMID:23473056

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.;

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

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

Polarization resolved angular optical scattering of aerosol particles

NASA Astrophysics Data System (ADS)

Redding, B.; Pan, Y.; Wang, C.; Videen, G.; Cao, Hui

2014-05-01

Real-time detection and identification of bio-aerosol particles are crucial for the protection against chemical and biological agents. The strong elastic light scattering properties of airborne particles provides a natural means for rapid, non-invasive aerosol characterization. Recent theoretical predictions suggested that variations in the polarization dependent angular scattering cross section could provide an efficient means of classifying different airborne particles. In particular, the polarization dependent scattering cross section of aggregate particles is expected to depend on the shape of the primary particles. In order to experimentally validate this prediction, we built a high throughput, sampling system, capable of measuring the polarization resolved angular scattering cross section of individual aerosol particles flowing through an interrogating volume with a single shot of laser pulse. We calibrated the system by comparing the polarization dependent scattering cross section of individual polystyrene spheres with that predicted by Mie theory. We then used the system to study different particles types: Polystyrene aggregates composed 500 nm spheres and Bacillus subtilis (BG, Anthrax simulant) spores composed of elongated 500 nm × 1000 nm cylinder-line particles. We found that the polarization resolved scattering cross section depends on the shape of the constituent elements of the aggregates. This work indicates that the polarization resolved scattering cross section could be used for rapid discrimination between different bio-aerosol particles.

Microphysical processing of aerosol particles in orographic clouds

NASA Astrophysics Data System (ADS)

Pousse-Nottelmann, S.; Zubler, E. M.; Lohmann, U.

2015-01-01

An explicit and detailed treatment of cloud-borne particles allowing for the consideration of aerosol cycling in clouds has been implemented in the regional weather forecast and climate model COSMO. The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener-Bergeron-Findeisen process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snow flakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snow flakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. However, the processes not only impact the total aerosol number and mass, but also the shape of the aerosol size distributions by enhancing the internally mixed/soluble accumulation mode and generating coarse mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases the cloud droplet number concentration with possible implications for the ice

Microphysical processing of aerosol particles in orographic clouds

NASA Astrophysics Data System (ADS)

Pousse-Nottelmann, S.; Zubler, E. M.; Lohmann, U.

2015-08-01

An explicit and detailed treatment of cloud-borne particles allowing for the consideration of aerosol cycling in clouds has been implemented into COSMO-Model, the regional weather forecast and climate model of the Consortium for Small-scale Modeling (COSMO). The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed us to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener-Bergeron-Findeisen (WBF) process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snowflakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snowflakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. Thereby, the processes impact the total aerosol number and mass and additionally alter the shape of the aerosol size distributions by enhancing the internally mixed/soluble Aitken and accumulation mode and generating coarse-mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases

Airborne Sunphotometer Measurements of Aerosol Optical Depth and Water Vapor in ACE-Asia and Their Comparisons to Correlative Measurements

NASA Technical Reports Server (NTRS)

Schmid, B.; Redemann, J.; Livingston, J.; Russell, P.; Hegg, D.; Wang, J.; Kahn, R.; Hsu, C.; Masonis, S.; Murayama, T.;

Determination of the aerosol size distribution by analytic inversion of the extinction spectrum in the complex anomalous diffraction approximation.

PubMed

Franssens, G; De Maziére, M; Fonteyn, D

2000-08-20

A new derivation is presented for the analytical inversion of aerosol spectral extinction data to size distributions. It is based on the complex analytic extension of the anomalous diffraction approximation (ADA). We derive inverse formulas that are applicable to homogeneous nonabsorbing and absorbing spherical particles. Our method simplifies, generalizes, and unifies a number of results obtained previously in the literature. In particular, we clarify the connection between the ADA transform and the Fourier and Laplace transforms. Also, the effect of the particle refractive-index dispersion on the inversion is examined. It is shown that, when Lorentz's model is used for this dispersion, the continuous ADA inverse transform is mathematically well posed, whereas with a constant refractive index it is ill posed. Further, a condition is given, in terms of Lorentz parameters, for which the continuous inverse operator does not amplify the error.

Electrospray ionizer for mass spectrometry of aerosol particles

DOEpatents

He, Siqin; Hogan, Chris; Li, Lin; Liu, Benjamin Y. H.; Naqwi, Amir; Romay, Francisco

2017-09-19

A device and method are disclosed to apply ESI-based mass spectroscopy to submicrometer and nanometer scale aerosol particles. Unipolar ionization is utilized to charge the particles in order to collect them electrostatically on the tip of a tungsten rod. Subsequently, the species composing the collected particles are dissolved by making a liquid flow over the tungsten rod. This liquid with dissolved aerosol contents is formed into highly charged droplets, which release unfragmented ions for mass spectroscopy, such as time-of-flight mass spectroscopy. The device is configured to operate in a switching mode, wherein aerosol deposition occurs while solvent delivery is turned off and vice versa.

SAGE II Measurements of Stratospheric Aerosol Properties at Non-Volcanic Levels

NASA Technical Reports Server (NTRS)

Thomason, Larry W.; Burton, Sharon P.; Luo, Bei-Ping; Peter, Thomas

2008-01-01

Since 2000, stratospheric aerosol levels have been relatively stable and at the lowest levels observed in the historical record. Given the challenges of making satellite measurements of aerosol properties at these levels, we have performed a study of the sensitivity of the product to the major components of the processing algorithm used in the production of SAGE II aerosol extinction measurements and the retrieval process that produces the operational surface area density (SAD) product. We find that the aerosol extinction measurements, particularly at 1020 nm, remain robust and reliable at the observed aerosol levels. On the other hand, during background periods, the SAD operational product has an uncertainty of at least a factor of 2 during due to the lack of sensitivity to particles with radii less than 100 nm.

Condensation Kinetics of Water on Amorphous Aerosol Particles.

PubMed

Rothfuss, Nicholas E; Marsh, Aleksandra; Rovelli, Grazia; Petters, Markus D; Reid, Jonathan P

2018-06-25

Responding to changes in the surrounding environment, aerosol particles can grow by water condensation changing rapidly in composition and changing dramatically in viscosity. The timescale for growth is important to establish for particles undergoing hydration processes in the atmosphere or during inhalation. Using an electrodynamic balance, we report direct measurements at -7.5, 0, and 20 °C of timescales for hygroscopic condensational growth on a range of model hygroscopic aerosol systems. These extend from viscous aerosol particles containing a single saccharide solute (sucrose, glucose, raffinose, or trehalose) and a starting viscosity equivalent to a glass of ∼10 12 Pa·s, to nonviscous (∼10 -2 Pa·s) tetraethylene glycol particles. The condensation timescales observed in this work indicate that water condensation occurs rapidly at all temperatures examined (<10 s) and for particles of all initial viscosities spanning 10 -2 to 10 12 Pa·s. Only a marginal delay (<1 order of magnitude) is observed for particles starting as a glass.

Supercritical Fluid Extraction and Analysis of Tropospheric Aerosol Particles

NASA Astrophysics Data System (ADS)

Hansen, Kristen J.

An integrated sampling and supercritical fluid extraction (SFE) cell has been designed for whole-sample analysis of organic compounds on tropospheric aerosol particles. The low-volume extraction cell has been interfaced with a sampling manifold for aerosol particle collection in the field. After sample collection, the entire SFE cell was coupled to a gas chromatograph; after on-line extraction, the cryogenically -focused sample was separated and the volatile compounds detected with either a mass spectrometer or a flame ionization detector. A 20-minute extraction at 450 atm and 90 ^circC with pure supercritical CO _2 is sufficient for quantitative extraction of most volatile compounds in aerosol particle samples. A comparison between SFE and thermal desorption, the traditional whole-sample technique for analyses of this type, was performed using ambient aerosol particle samples, as well as samples containing known amounts of standard analytes. The results of these studies indicate that SFE of atmospheric aerosol particles provides quantitative measurement of several classes of organic compounds. SFE provides information that is complementary to that gained by the thermal desorption analysis. The results also indicate that SFE with CO _2 can be validated as an alternative to thermal desorption for quantitative recovery of several organic compounds. In 1989, the organic constituents of atmospheric aerosol particles collected at Niwot Ridge, Colorado, along with various physical and meteorological data, were measured during a collaborative field study. Temporal changes in the composition of samples collected during summertime at the rural site were studied. Thermal desorption-GC/FID was used to quantify selected compounds in samples collected during the field study. The statistical analysis of the 1989 Niwot Ridge data set is presented in this work. Principal component analysis was performed on thirty-one variables selected from the data set in order to ascertain

Can Condensing Organic Aerosols Lead to Less Cloud Particles?

NASA Astrophysics Data System (ADS)

Gao, C. Y.; Tsigaridis, K.; Bauer, S.

2017-12-01

We examined the impact of condensing organic aerosols on activated cloud number concentration in a new aerosol microphysics box model, MATRIX-VBS. The model includes the volatility-basis set (VBS) framework in an aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state) that resolves aerosol mass and number concentrations and aerosol mixing state. Preliminary results show that by including the condensation of organic aerosols, the new model (MATRIX-VBS) has less activated particles compared to the original model (MATRIX), which treats organic aerosols as non-volatile. Parameters such as aerosol chemical composition, mass and number concentrations, and particle sizes which affect activated cloud number concentration are thoroughly evaluated via a suite of Monte-Carlo simulations. The Monte-Carlo simulations also provide information on which climate-relevant parameters play a critical role in the aerosol evolution in the atmosphere. This study also helps simplifying the newly developed box model which will soon be implemented in the global model GISS ModelE as a module.

Real-Time Detection Method And System For Identifying Individual Aerosol Particles

DOEpatents

Gard, Eric Evan; Fergenson, David Philip

2005-10-25

A method and system of identifying individual aerosol particles in real time. Sample aerosol particles are compared against and identified with substantially matching known particle types by producing positive and negative test spectra of an individual aerosol particle using a bipolar single particle mass spectrometer. Each test spectrum is compared to spectra of the same respective polarity in a database of predetermined positive and negative spectra for known particle types and a set of substantially matching spectra is obtained. Finally the identity of the individual aerosol particle is determined from the set of substantially matching spectra by determining a best matching one of the known particle types having both a substantially matching positive spectrum and a substantially matching negative spectrum associated with the best matching known particle type.

Single-particle characterization of the High Arctic summertime aerosol

NASA Astrophysics Data System (ADS)

Sierau, B.; Chang, R. Y.-W.; Leck, C.; Paatero, J.; Lohmann, U.

2014-01-01

Single-particle mass spectrometric measurements were carried out in the High Arctic north of 80° during summer 2008. The campaign took place onboard the icebreaker Oden and was part of the Arctic Summer Cloud Ocean Study (ASCOS). The instrument deployed was an Aerosol Time-of-Flight Mass Spectrometer (ATOFMS) that provides information on the chemical composition of individual particles and their mixing state in real-time. Aerosols were sampled in the marine boundary layer at stations in the open ocean, in the marginal ice zone, and in the pack ice region. The largest fraction of particles detected for subsequent analysis in the size range of the ATOFMS between approximately 200 nm to 3000 nm in diameter showed mass spectrometric patterns indicating an internal mixing state and a biomass burning and/or biofuel source. The majority of these particles were connected to an air mass layer of elevated particle concentration mixed into the surface mixed layer from the upper part of the marine boundary layer. The second largest fraction was represented by sea salt particles. The chemical analysis of the over-ice sea salt aerosol revealed tracer compounds that reflect chemical aging of the particles during their long-range advection from the marginal ice zone, or open waters south thereof prior to detection at the ship. From our findings we conclude that long-range transport of particles is one source of aerosols in the High Arctic. To assess the importance of long-range particle sources for aerosol-cloud interactions over the inner Arctic in comparison to local and regional biogenic primary aerosol sources, the chemical composition of the detected particles was analyzed for indicators of marine biological origin. Only a~minor fraction showed chemical signatures of potentially ocean-derived primary particles of that kind. However, a chemical bias in the ATOFMS's detection capabilities observed during ASCOS might suggest a presence of a particle type of unknown composition

Single-particle characterization of the high-Arctic summertime aerosol

NASA Astrophysics Data System (ADS)

Sierau, B.; Chang, R. Y.-W.; Leck, C.; Paatero, J.; Lohmann, U.

2014-07-01

Single-particle mass-spectrometric measurements were carried out in the high Arctic north of 80° during summer 2008. The campaign took place onboard the icebreaker Oden and was part of the Arctic Summer Cloud Ocean Study (ASCOS). The instrument deployed was an aerosol time-of-flight mass spectrometer (ATOFMS) that provides information on the chemical composition of individual particles and their mixing state in real time. Aerosols were sampled in the marine boundary layer at stations in the open ocean, in the marginal ice zone, and in the pack ice region. The largest fraction of particles detected for subsequent analysis in the size range of the ATOFMS between approximately 200 and 3000 nm in diameter showed mass-spectrometric patterns, indicating an internal mixing state and a biomass burning and/or biofuel source. The majority of these particles were connected to an air mass layer of elevated particle concentration mixed into the surface mixed layer from the upper part of the marine boundary layer. The second largest fraction was represented by sea salt particles. The chemical analysis of the over-ice sea salt aerosol revealed tracer compounds that reflect chemical aging of the particles during their long-range advection from the marginal ice zone, or open waters south thereof prior to detection at the ship. From our findings we conclude that long-range transport of particles is one source of aerosols in the high Arctic. To assess the importance of long-range particle sources for aerosol-cloud interactions over the inner Arctic in comparison to local and regional biogenic primary aerosol sources, the chemical composition of the detected particles was analyzed for indicators of marine biological origin. Only a minor fraction showed chemical signatures of potentially ocean-derived primary particles of that kind. However, a chemical bias in the ATOFMS's detection capabilities observed during ASCOS might suggest the presence of a particle type of unknown composition

Single-particle Analyses of Compositions, Morphology, and Viscosity of Aerosol Particles Collected During GoAmazon2014

NASA Astrophysics Data System (ADS)

Adachi, K.; Gong, Z.; Bateman, A. P.; Martin, S. T.; Cirino, G. G.; Artaxo, P.; Sedlacek, A. J., III; Buseck, P. R.

2014-12-01

Single-particle analysis using transmission electron microscopy (TEM) shows composition and morphology of individual aerosol particles collected during the GoAmazon2014 campaign. These TEM results indicate aerosol types and mixing states, both of which are important for evaluating particle optical properties and cloud condensation nuclei activity. The samples were collected at the T3 site, which is located in the Amazon forest with influences from the urban pollution plume from Manaus. Samples were also collected from the T0 site, which is in the middle of the jungle with minimal to no influences of anthropogenic sources. The aerosol particles mainly originated from 1) anthropogenic pollution (e.g., nanosphere soot, sulfate), 2) biogenic emissions (e.g., primary biogenic particles, organic aerosols), and 3) long-range transport (e.g., sea salts). We found that the biogenic organic aerosol particles contain homogeneously distributed potassium. Particle viscosity is important for evaluating gas-particle interactions and atmospheric chemistry for the particles. Viscosity can be estimated from the rebounding behavior at controlled relative humidities, i.e., highly viscous particles display less rebound on a plate than low-viscosity particles. We collected 1) aerosol particles from a plate (non-rebounded), 2) those that had rebounded from the plate and were then captured onto an adjacent sampling plate, and 3) particles from ambient air using a separate impactor sampler. Preliminary results show that more than 90% of non-rebounded particles consisted of nanosphere soot with or without coatings. The coatings mostly consisted of organic matter. Although rebounded particles also contain nanosphere soot (number fraction 64-69%), they were mostly internally mixed with sulfate, organic matter, or their mixtures. TEM tilted images suggested that the rebounded particles were less deformed on the substrate, whereas the non-rebounded particles were more deformed, which could

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.

A Comparison of Aerosol Optical Property Measurements Made During the DOE Aerosol Intensive Operating Period and Their Effects on Regional Climate

NASA Technical Reports Server (NTRS)

Strawa, Anthony W.; Hallar, A. G.; Arnott, W. P.; Covert, D.; Elleman, R.; Ogren, J.; Schmid, B.; Luu, A.

2004-01-01

The amount of radiant energy an aerosol absorbs has profound effects on climate and air quality. It is ironic that aerosol absorption coefficient is one of the most difficult to measure aerosol properties. One of the main purposes of the DOE Aerosol Intensive Operating Period (IOP) flown in May, 2003 was to assess our ability to measure absorption coefficient in situ. This paper compares measurements of aerosol optical properties made during the IOP. Measurements of aerosol absorption coefficient were made by Particle Soot Absorption Photometer (PSAP) aboard the CIRPAS Twin-Otter (U. Washington) and on the DOE Cessna 172 (NOAA-C,MDL). Aerosol absorption coefficient was also measured by a photoacoustic instrument (DRI) that was operated on an aircraft for the first time during the IOP. A new cavity ring-down (CRD) instrument, called Cadenza (NASA-AkC), measures the aerosol extinction coefficient for 675 nm and 1550 nm light, and simultaneously measures the scattering coefficient at 675 nm. Absorption coefficient is obtained from the difference of measured extinction and scattering within the instrument. Measurements of absorption coefficient from all of these instruments during appropriate periods are compared. During the IOP, several significant aerosol layers were sampled aloft. These layers are identified in the remote (AATS-14) as well as in situ measurements. Extinction profiles measured by Cadenza are compared to those derived from the Ames Airborne Tracking Sunphotometer (AATS-14, NASA-ARC). The regional radiative impact of these layers is assessed by using the measured aerosol optical properties in a radiative transfer model.

Remote sensing and in-situ measurements of tropospheric aerosol, a PAMARCMiP case study

NASA Astrophysics Data System (ADS)

Hoffmann, Anne; Osterloh, Lukas; Stone, Robert; Lampert, Astrid; Ritter, Christoph; Stock, Maria; Tunved, Peter; Hennig, Tabea; Böckmann, Christine; Li, Shao-Meng; Eleftheriadis, Kostas; Maturilli, Marion; Orgis, Thomas; Herber, Andreas; Neuber, Roland; Dethloff, Klaus

2012-06-01

In this work, a closure experiment for tropospheric aerosol is presented. Aerosol size distributions and single scattering albedo from remote sensing data are compared to those measured in-situ. An aerosol pollution event on 4 April 2009 was observed by ground based and airborne lidar and photometer in and around Ny-Ålesund, Spitsbergen, as well as by DMPS, nephelometer and particle soot absorption photometer at the nearby Zeppelin Mountain Research Station. The presented measurements were conducted in an area of 40 × 20 km around Ny-Ålesund as part of the 2009 Polar Airborne Measurements and Arctic Regional Climate Model Simulation Project (PAMARCMiP). Aerosol mainly in the accumulation mode was found in the lower troposphere, however, enhanced backscattering was observed up to the tropopause altitude. A comparison of meteorological data available at different locations reveals a stable multi-layer-structure of the lower troposphere. It is followed by the retrieval of optical and microphysical aerosol parameters. Extinction values have been derived using two different methods, and it was found that extinction (especially in the UV) derived from Raman lidar data significantly surpasses the extinction derived from photometer AOD profiles. Airborne lidar data shows volume depolarization values to be less than 2.5% between 500 m and 2.5 km altitude, hence, particles in this range can be assumed to be of spherical shape. In-situ particle number concentrations measured at the Zeppelin Mountain Research Station at 474 m altitude peak at about 0.18 μm diameter, which was also found for the microphysical inversion calculations performed at 850 m and 1500 m altitude. Number concentrations depend on the assumed extinction values, and slightly decrease with altitude as well as the effective particle diameter. A low imaginary part in the derived refractive index suggests weakly absorbing aerosols, which is confirmed by low black carbon concentrations, measured at the

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.

On-site ocean horizontal aerosol extinction coefficient inversion under different weather conditions on the Bo-hai and Huang-hai Seas

NASA Astrophysics Data System (ADS)

Zeng, Xianjiang; Xia, Min; Ge, Yinghui; Guo, Wenping; Yang, Kecheng

2018-03-01

In this paper, we explore the horizontal extinction characteristics under different weather conditions on the ocean surface with on-site experiments on the Bo-hai and Huang-hai Seas in the summer of 2016. An experimental lidar system is designed to collect the on-site experimental data. By aiming at the inhomogeneity and uncertainty of the horizontal aerosol in practice, a joint retrieval method is proposed to retrieve the aerosol extinction coefficients (AEC) from the raw data along the optical path. The retrieval results of both the simulated and the real signals demonstrate that the joint retrieval method is practical. Finally, the sequence observation results of the on-site experiments under different weather conditions are reported and analyzed. These results can provide the attenuation information to analyze the atmospheric aerosol characteristics on the ocean surface.

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

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.

On remote sensing of small aerosol particles with polarized light

NASA Astrophysics Data System (ADS)

Sun, W.

2012-12-01

The CALIPSO satellite mission consistently measures volume (including molecule and particulate) light depolarization ratio of ~2% for smoke, compared to ~1% for marine aerosols and ~15% for dust. The observed ~2% smoke depolarization ratio comes primarily from the nonspherical habits of particles in the smoke at certain particle sizes. The depolarization of linearly polarized light by small sphere aggregates and irregular Gaussian-shaped particles is studied, to reveal the physics between the depolarization of linearly polarized light and aerosol shape and size. It is found that randomly oriented nonspherical particles have some common depolarization properties as functions of scattering angle and size parameter. This may be very useful information for active remote sensing of small nonspherical aerosols using polarized light. We also show that the depolarization ratio from the CALIPSO measurements could be used to derive smoke aerosol particle size. The mean particle size of South-African smoke is estimated to be about half of the 532 nm wavelength of the CALIPSO lidar.

SAGE III Aerosol Extinction Validation in the Arctic Winter: Comparisons with SAGE II and POAM III

NASA Technical Reports Server (NTRS)

Thomason, L. W.; Poole, L. R.; Randall, C. E.

2007-01-01

The use of SAGE III multiwavelength aerosol extinction coefficient measurements to infer PSC type is contingent on the robustness of both the extinction magnitude and its spectral variation. Past validation with SAGE II and other similar measurements has shown that the SAGE III extinction coefficient measurements are reliable though the comparisons have been greatly weighted toward measurements made at mid-latitudes. Some aerosol comparisons made in the Arctic winter as a part of SOLVE II suggested that SAGE III values, particularly at longer wavelengths, are too small with the implication that both the magnitude and the wavelength dependence are not reliable. Comparisons with POAM III have also suggested a similar discrepancy. Herein, we use SAGE II data as a common standard for comparison of SAGE III and POAM III measurements in the Arctic winters of 2002/2003 through 2004/2005. During the winter, SAGE II measurements are made infrequently at the same latitudes as these instruments. We have mitigated this problem through the use potential vorticity as a spatial coordinate and thus greatly increased the number of coincident events. We find that SAGE II and III extinction coefficient measurements show a high degree of compatibility at both 1020 nm and 450 nm except a 10-20% bias at both wavelengths. In addition, the 452 to 1020-nm extinction ratio shows a consistent bias of approx. 30% throughout the lower stratosphere. We also find that SAGE II and POAM III are on average consistent though the comparisons show a much higher variability and larger bias than SAGE II/III comparisons. In addition, we find that the two data sets are not well correlated below 18 km. Overall, we find both the extinction values and the spectral dependence from SAGE III are robust and we find no evidence of a significant defect within the Arctic vortex.

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

Properties of Arctic Aerosol Particles and Residuals of Warm Clouds: Cloud Activation Efficiency and the Aerosol Indirect Effect

NASA Astrophysics Data System (ADS)

Zelenyuk, A.; Imre, D. G.; Leaitch, R.; Ovchinnikov, M.; Liu, P.; Macdonald, A.; Strapp, W.; Ghan, S. J.; Earle, M. E.

2012-12-01

Single particle mass spectrometer, SPLAT II, was used to characterize the size, composition, number concentration, density, and shape of individual Arctic spring aerosol. Background particles, particles above and below the cloud, cloud droplet residuals, and interstitial particles were characterized with goal to identify the properties that separate cloud condensation nuclei (CCN) from background aerosol particles. The analysis offers a comparison between warm clouds formed on clean and polluted days, with clean days having maximum particle concentrations (Na) lower than ~250 cm-3, as compared with polluted days, in which maximum concentration was tenfold higher. On clean days, particles were composed of organics, organics mixed with sulfates, biomass burning (BB), sea salt (SS), and few soot and dust particles. On polluted days, BB, organics associated with BB, and their mixtures with sulfate dominated particle compositions. Based on the measured compositions and size distributions of cloud droplet residuals, background aerosols, and interstitial particles, we conclude that these three particle types had virtually the same compositions, which means that cloud activation probabilities were surprisingly nearly composition independent. Moreover, these conclusions hold in cases in which less than 20% or more than 90% of background particles got activated. We concluded that for the warm clouds interrogated in this study particle size played a more important factor on aerosol CCN activity. Comparative analysis of all studied clouds reveals that aerosol activation efficiency strongly depends on the aerosol concentrations, such that at Na <200 cm-3, nearly all particles activate, and at higher concentrations the activation efficiency is lower. For example, when Na was greater than 1500 cm-3, less than ~30% of particles activated. The data suggest that as the number of nucleated droplets increases, condensation on existing droplets effectively competes with particle

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

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

A recirculation aerosol wind tunnel for evaluating aerosol samplers and measuring particle penetration through protective clothing materials.

PubMed

Jaques, Peter A; Hsiao, Ta-Chih; Gao, Pengfei

2011-08-01

A recirculation aerosol wind tunnel was designed to maintain a uniform airflow and stable aerosol size distribution for evaluating aerosol sampler performance and determining particle penetration through protective clothing materials. The oval-shaped wind tunnel was designed to be small enough to fit onto a lab bench, have optimized dimensions for uniformity in wind speed and particle size distributions, sufficient mixing for even distribution of particles, and minimum particle losses. Performance evaluation demonstrates a relatively high level of spatial uniformity, with a coefficient of variation of 1.5-6.2% for wind velocities between 0.4 and 2.8 m s(-1) and, in this range, 0.8-8.5% for particles between 50 and 450 nm. Aerosol concentration stabilized within the first 5-20 min with, approximately, a count median diameter of 135 nm and geometric standard deviation of 2.20. Negligible agglomerate growth and particle loss are suggested. The recirculation design appears to result in unique features as needed for our research.

Real-time detection method and system for identifying individual aerosol particles

DOEpatents

Gard, Eric E [San Francisco, CA; Coffee, Keith R [Patterson, CA; Frank, Matthias [Oakland, CA; Tobias, Herbert J [Kensington, CA; Fergenson, David P [Alamo, CA; Madden, Norm [Livermore, CA; Riot, Vincent J [Berkeley, CA; Steele, Paul T [Livermore, CA; Woods, Bruce W [Livermore, CA

2007-08-21

An improved method and system of identifying individual aerosol particles in real time. Sample aerosol particles are collimated, tracked, and screened to determine which ones qualify for mass spectrometric analysis based on predetermined qualification or selection criteria. Screening techniques include one or more of determining particle size, shape, symmetry, and fluorescence. Only qualifying particles passing all screening criteria are subject to desorption/ionization and single particle mass spectrometry to produce corresponding test spectra, which is used to determine the identities of each of the qualifying aerosol particles by comparing the test spectra against predetermined spectra for known particle types. In this manner, activation cycling of a particle ablation laser of a single particle mass spectrometer is reduced.

Optimal estimation retrieval of aerosol microphysical properties from SAGE~II satellite observations in the volcanically unperturbed lower stratosphere

NASA Astrophysics Data System (ADS)

Wurl, D.; Grainger, R. G.; McDonald, A. J.; Deshler, T.

2010-05-01

Stratospheric aerosol particles under non-volcanic conditions are typically smaller than 0.1 μm. Due to fundamental limitations of the scattering theory in the Rayleigh limit, these tiny particles are hard to measure by satellite instruments. As a consequence, current estimates of global aerosol properties retrieved from spectral aerosol extinction measurements tend to be strongly biased. Aerosol surface area densities, for instance, are observed to be about 40% smaller than those derived from correlative in situ measurements (Deshler et al., 2003). An accurate knowledge of the global distribution of aerosol properties is, however, essential to better understand and quantify the role they play in atmospheric chemistry, dynamics, radiation and climate. To address this need a new retrieval algorithm was developed, which employs a nonlinear Optimal Estimation (OE) method to iteratively solve for the monomodal size distribution parameters which are statistically most consistent with both the satellite-measured multi-wavelength aerosol extinction data and a priori information. By thus combining spectral extinction measurements (at visible to near infrared wavelengths) with prior knowledge of aerosol properties at background level, even the smallest particles are taken into account which are practically invisible to optical remote sensing instruments. The performance of the OE retrieval algorithm was assessed based on synthetic spectral extinction data generated from both monomodal and small-mode-dominant bimodal sulphuric acid aerosol size distributions. For monomodal background aerosol, the new algorithm was shown to fairly accurately retrieve the particle sizes and associated integrated properties (surface area and volume densities), even in the presence of large extinction uncertainty. The associated retrieved uncertainties are a good estimate of the true errors. In the case of bimodal background aerosol, where the retrieved (monomodal) size distributions naturally

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

Contributions of Organic Sources to Atmospheric Aerosol Particle Concentrations and Growth

NASA Astrophysics Data System (ADS)

Russell, L. M.

2017-12-01

Organic molecules are important contributors to aerosol particle mass and number concentrations through primary emissions as well as secondary growth in the atmosphere. New techniques for measuring organic aerosol components in atmospheric particles have improved measurements of this contribution in the last 20 years, including Scanning Transmission X-ray Microscopy Near Edge X-ray Absorption Fine Structure (STXM-NEXAFS), Fourier Transform Infrared spectroscopy (FTIR), and High-Resolution Aerosol Mass Spectrometry (AMS). STXM-NEXAFS individual aerosol particle composition illustrated the variety of morphology of organic components in marine aerosols, the inherent relationships between organic composition and shape, and the links between atmospheric aerosol composition and particles produced in smog chambers. This type of single particle microscopy has also added to size distribution measurements by providing evidence of how surface-controlled and bulk-controlled processes contribute to the growth of particles in the atmosphere. FTIR analysis of organic functional groups are sufficient to distinguish combustion, marine, and terrestrial organic particle sources and to show that each of those types of sources has a surprisingly similar organic functional group composition over four different oceans and four different continents. Augmenting the limited sampling of these off-line techniques with side-by-side inter-comparisons to online AMS provides complementary composition information and consistent quantitative attribution to sources (despite some clear method differences). Single-particle AMS techniques using light scattering and event trigger modes have now also characterized the types of particles found in urban, marine, and ship emission aerosols. Most recently, by combining with off-line techniques, single particle composition measurements have separated and quantified the contributions of organic, sulfate and salt components from ocean biogenic and sea spray

SIZE DISTRIBUTIONS OF ELEMENTAL CARBON IN ATMOSPHERIC AEROSOLS

EPA Science Inventory

Environmental problems caused by atmospheric aerosols are well documented in the specialized literature. Studies reporting on the role of dense clouds of soil particles in past mass extinctions of life on Earth and, more recently (Turco et al., 1983), on calculations of potential...

Retrieval of spheroid particle size distribution from spectral extinction data in the independent mode using PCA approach

NASA Astrophysics Data System (ADS)

Tang, Hong; Lin, Jian-Zhong

2013-01-01

An improved anomalous diffraction approximation (ADA) method is presented for calculating the extinction efficiency of spheroids firstly. In this approach, the extinction efficiency of spheroid particles can be calculated with good accuracy and high efficiency in a wider size range by combining the Latimer method and the ADA theory, and this method can present a more general expression for calculating the extinction efficiency of spheroid particles with various complex refractive indices and aspect ratios. Meanwhile, the visible spectral extinction with varied spheroid particle size distributions and complex refractive indices is surveyed. Furthermore, a selection principle about the spectral extinction data is developed based on PCA (principle component analysis) of first derivative spectral extinction. By calculating the contribution rate of first derivative spectral extinction, the spectral extinction with more significant features can be selected as the input data, and those with less features is removed from the inversion data. In addition, we propose an improved Tikhonov iteration method to retrieve the spheroid particle size distributions in the independent mode. Simulation experiments indicate that the spheroid particle size distributions obtained with the proposed method coincide fairly well with the given distributions, and this inversion method provides a simple, reliable and efficient method to retrieve the spheroid particle size distributions from the spectral extinction data.

A new stochastic algorithm for inversion of dust aerosol size distribution

NASA Astrophysics Data System (ADS)

Wang, Li; Li, Feng; Yang, Ma-ying

2015-08-01

Dust aerosol size distribution is an important source of information about atmospheric aerosols, and it can be determined from multiwavelength extinction measurements. This paper describes a stochastic inverse technique based on artificial bee colony (ABC) algorithm to invert the dust aerosol size distribution by light extinction method. The direct problems for the size distribution of water drop and dust particle, which are the main elements of atmospheric aerosols, are solved by the Mie theory and the Lambert-Beer Law in multispectral region. And then, the parameters of three widely used functions, i.e. the log normal distribution (L-N), the Junge distribution (J-J), and the normal distribution (N-N), which can provide the most useful representation of aerosol size distributions, are inversed by the ABC algorithm in the dependent model. Numerical results show that the ABC algorithm can be successfully applied to recover the aerosol size distribution with high feasibility and reliability even in the presence of random noise.

Optical properties of mineral dust aerosol including analysis of particle size, composition, and shape effects, and the impact of physical and chemical processing

NASA Astrophysics Data System (ADS)

Alexander, Jennifer Mary

Atmospheric mineral dust has a large impact on the earth's radiation balance and climate. The radiative effects of mineral dust depend on factors including, particle size, shape, and composition which can all be extremely complex. Mineral dust particles are typically irregular in shape and can include sharp edges, voids, and fine scale surface roughness. Particle shape can also depend on the type of mineral and can vary as a function of particle size. In addition, atmospheric mineral dust is a complex mixture of different minerals as well as other, possibly organic, components that have been mixed in while these particles are suspended in the atmosphere. Aerosol optical properties are investigated in this work, including studies of the effect of particle size, shape, and composition on the infrared (IR) extinction and visible scattering properties in order to achieve more accurate modeling methods. Studies of particle shape effects on dust optical properties for single component mineral samples of silicate clay and diatomaceous earth are carried out here first. Experimental measurements are modeled using T-matrix theory in a uniform spheroid approximation. Previous efforts to simulate the measured optical properties of silicate clay, using models that assumed particle shape was independent of particle size, have achieved only limited success. However, a model which accounts for a correlation between particle size and shape for the silicate clays offers a large improvement over earlier modeling approaches. Diatomaceous earth is also studied as an example of a single component mineral dust aerosol with extreme particle shapes. A particle shape distribution, determined by fitting the experimental IR extinction data, used as a basis for modeling the visible light scattering properties. While the visible simulations show only modestly good agreement with the scattering data, the fits are generally better than those obtained using more commonly invoked particle shape

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

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.

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

Ambient measurement of fluorescent aerosol particles with a WIBS in the Yangtze River Delta of China: potential impacts of combustion-related aerosol particles

NASA Astrophysics Data System (ADS)

Yu, Xiawei; Wang, Zhibin; Zhang, Minghui; Kuhn, Uwe; Xie, Zhouqing; Cheng, Yafang; Pöschl, Ulrich; Su, Hang

2016-09-01

Fluorescence characteristics of aerosol particles in a polluted atmosphere were studied using a wideband integrated bioaerosol spectrometer (WIBS-4A) in Nanjing, Yangtze River Delta area of China. We observed strong diurnal and day-to-day variations of fluorescent aerosol particles (FAPs). The average number concentrations of FAPs (1-15 µm) detected in the three WIBS measurement channels (FL1: 0.6 cm-3, FL2: 3.4 cm-3, FL3: 2.1 cm-3) were much higher than those observed in forests and rural areas, suggesting that FAPs other than bioaerosols were detected. We found that the number fractions of FAPs were positively correlated with the black carbon mass fraction, especially for the FL1 channel, indicating a large contribution of combustion-related aerosols. To distinguish bioaerosols from combustion-related FAPs, we investigated two classification schemes for use with WIBS data. Our analysis suggests a strong size dependence for the fractional contributions of different types of FAPs. In the FL3 channel, combustion-related particles seem to dominate the 1-2 µm size range while bioaerosols dominate the 2-5 µm range. The number fractions of combustion-related particles and non-combustion-related particles to total aerosol particles were ˜ 11 and ˜ 5 %, respectively.

Aerosolization, Chemical Characterization, Hygroscopicity and Ice Formation of Marine Biogenic Particles

NASA Astrophysics Data System (ADS)

Alpert, P. A.; Radway, J.; Kilthau, W.; Bothe, D.; Knopf, D. A.; Aller, J. Y.

2013-12-01

The oceans cover the majority of the earth's surface, host nearly half the total global primary productivity and are a major source of atmospheric aerosol particles. However, effects of biological activity on sea spray generation and composition, and subsequent cloud formation are not well understood. Our goal is to elucidate these effects which will be particularly important over nutrient rich seas, where microorganisms can reach concentrations of 10^9 per mL and along with transparent exopolymer particles (TEP) can become aerosolized. Here we report the results of mesocosm experiments in which bubbles were generated by two methods, either recirculating impinging water jets or glass frits, in natural or artificial seawater containing bacteria and unialgal cultures of three representative phytoplankton species, Thalassiosira pseudonana, Emiliania huxleyi, and Nannochloris atomus. Over time we followed the size distribution of aerosolized particles as well as their hygroscopicity, heterogeneous ice nucleation potential, and individual physical-chemical characteristics. Numbers of cells and the mass of dissolved and particulate organic carbon (DOC, POC), TEP (which includes polysaccharide-containing microgels and nanogels >0.4 μm in diameter) were determined in the bulk water, the surface microlayer, and aerosolized material. Aerosolized particles were also impacted onto substrates for ice nucleation and water uptake experiments, elemental analysis using computer controlled scanning electron microscopy and energy dispersive analysis of X-rays (CCSEM/EDX), and determination of carbon bonding with scanning transmission X-ray microscopy and near-edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). Regardless of bubble generation method, the overall concentration of aerosol particles, TEP, POC and DOC increased as concentrations of bacterial and phytoplankton cells increased, stabilized, and subsequently declined. Particles <100 nm generated by means of jets

Dispersion of aerosol particles in the atmosphere: Fukushima

NASA Astrophysics Data System (ADS)

Haszpra, Tímea; Lagzi, István; Tél, Tamás

2013-04-01

Investigation of dispersion and deposition of aerosol particles in the atmosphere is an essential issue, because they have an effect on the biosphere and atmosphere. Moreover, aerosol particles have different transport properties and chemical and physical transformations in the atmosphere compared to gas phase air pollutants. The motion of a particle is described by a set of ordinary differential equations. The large-scale dynamics in the horizontal direction can be described by the equations of passive scalar advection, but in the vertical direction a well-defined terminal velocity should be taken into account as a term added to the vertical wind component. In the planetary boundary layer turbulent diffusion has an important role in the particle dispersion, which is taken into account by adding stochastic terms to the deterministic equations above. Wet deposition is also an essential process in the lower levels of the atmosphere, however, its precise parameterization is a challenge. For the simulations the wind field and other necessary data were taken from the ECMWF ERA-Interim database. In the case of the Fukushima Daiichi nuclear disaster (March-April 2011) radioactive aerosol particles were also released in the planetary boundary layer. Simulations (included the continuous and varying emission from the nuclear power plant) will be presented for the period of 14-23 March. Results show that wet deposition also has to be taken into consideration in the lower levels of the atmosphere. Furthermore, dynamical system characteristics are evaluated for the aerosol particle dynamics. The escape rate of particles was estimated both with and without turbulent diffusion, and in both cases when there was no wet deposition and also when wet deposition was taken into consideration.

Field test of a new instrument to measure UV/Vis (300-700 nm) ambient aerosol extinction spectra in Colorado during DISCOVER-AQ

NASA Astrophysics Data System (ADS)

Jordan, C. E.; Anderson, B. E.; Beyersdorf, A. J.; Dibb, J. E.; Greenslade, M. E.; Martin, R.; Scheuer, E. M.; Shook, M.; Thornhill, K. L., II; Troop, D.; Winstead, E.; Ziemba, L. D.

2014-12-01

An optical instrument has been developed to investigate aerosol extinction spectra in the ambient atmosphere. Based on a White-type cell design and using a differential optical approach, aerosol extinction spectra over the 300-700 nm ultraviolet and visible (UV/Vis) wavelength range are obtained. Laboratory tests conducted at NASA Langley Research Center (NASA LaRC) in March 2014 showed good agreement with Cavity Attenuated Phase Shift (CAPS PMex, Aerodyne Research) extinction measurements (at 450, 530, and 630 nm) for a variety of aerosols, e.g., scatterers such as polystyrene latex spheres and ammonium sulfate; absorbers such as dust (including pigmented minerals), smoke (generated in a miniCAST burning propane) and laboratory smoke analogs (e.g., fullerene soot and aquadag). The instrument was field tested in Colorado in July and August 2014 aboard the NASA mobile laboratory at various ground sites during the DISCOVER-AQ (Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality) field campaign. A description of the instrument, results from the laboratory tests, and summer field data will be presented. The instrument provides a new tool for probing in situ aerosol optical properties that may help inform remote sensing approaches well into the UV range.

Single-particle characterization of indoor aerosol particles collected at an underground shopping area in Seoul, Korea.

PubMed

Maskey, Shila; Kang, TaeHee; Jung, Hae-Jin; Ro, Chul-Un

2011-02-01

In this study, single-particle characterization of aerosol particles collected at an underground shopping area was performed for the first time. A quantitative single-particle analytical technique, low-Z particle electron probe X-ray microanalysis, was used to characterize a total of 7900 individual particles for eight sets of aerosol samples collected at an underground shopping area in Seoul, Korea. Based on secondary electron images and X-ray spectral data of individual particles, fourteen particle types were identified, in which primary soil-derived particles were the most abundant, followed by carbonaceous, Fe-containing, secondary soil-derived, and secondary sea-salt particles. Carbonaceous particles exist in three types: organic carbon, carbon-rich, and CNO-rich. A significant number of textile particles with chemical composition C, N, and O were encountered in some of the aerosol samples, which were from the textile shops and/or from clothes of passersby. Primary soil-derived particles showed seasonal variation, with peak values in spring samples, reflecting higher air exchange between indoor and outdoor environments in the spring. Secondary soil-derived, secondary sea-salt, and ammonium sulfate particles were frequently encountered in winter samples. Fe-containing particles, contributed from a nearby subway station, were in the range of about 19% relative abundances for all samples. In underground shopping areas, particulate matters can be a considerable health hazard to the workers, shoppers, passersby, and shop-keepers as they spend their considerable time in this closed microenvironment. However, no study on the characteristics of indoor aerosols in an underground shopping area has been reported to our knowledge. This work provides detailed information on characteristics of underground shopping area aerosols on a single particle level. © 2010 John Wiley & Sons A/S.

On the Nature of Aerosol Particles in the Atmosphere of Irkutsk

NASA Astrophysics Data System (ADS)

Yermakov, A. N.; Golobokova, L. P.; Netsvetaeva, O. G.; Aloyan, A. E.; Arutyunyan, V. O.; Khodzher, T. V.

2018-03-01

Monitoring data on the ion composition of precipitation and the water-soluble fraction of aerosol have been used to identify two types of aerosol particles in the surface atmosphere of Irkutsk ("metal" and "ammonia" groups). The aerosol acidity is basically governed by the acidity of ammonia particles, and the ion composition depends on air relative humidity (RH). Preliminary estimates are given for the distribution of major cations and anions by aerosol groups.

Aerosol Classification from High Spectral Resolution Lidar Measurements

NASA Astrophysics Data System (ADS)

Burton, S. P.; Hair, J. W.; Ferrare, R. A.; Hostetler, C. A.; Kahnert, M.; Vaughan, M. A.; Cook, A. L.; Harper, D. B.; Berkoff, T.; Seaman, S. T.; Collins, J. E., Jr.; Fenn, M. A.; Rogers, R. R.

2015-12-01

The NASA Langley airborne High Spectral Resolution Lidars, HSRL-1 and HSRL-2, have acquired large datasets of vertically resolved aerosol extinction, backscatter, and depolarization during >30 airborne field missions since 2006. The lidar measurements of aerosol intensive parameters like lidar ratio and color ratio embed information about intrinsic aerosol properties, and are combined to qualitatively classify HSRL aerosol measurements into aerosol types. Knowledge of aerosol type is important for assessing aerosol radiative forcing, and can provide useful information for source attribution studies. However, atmospheric aerosol is frequently not a single pure type, but instead is a mixture, which affects the optical and radiative properties of the aerosol. We show that aerosol intensive parameters measured by lidar can be understood using mixing rules for cases of external mixing. Beyond coarse classification and mixing between classes, variations in the lidar aerosol intensive parameters provide additional insight into aerosol processes and composition. This is illustrated by depolarization measurements at three wavelengths, 355 nm, 532 nm, and 1064 nm, made by HSRL-2. Particle depolarization ratio is an indicator of non-spherical particles. Three cases each have a significantly different spectral dependence of the depolarization ratio, related to the size of the depolarizing particles. For two dust cases, large non-spherical particles account for the depolarization of the lidar light. The spectral dependence reflects the size distribution of these particles and reveals differences in the transport histories of the two plumes. For a smoke case, the depolarization is inferred to be due to the presence of small coated soot aggregates. Interestingly, the depolarization at 355 nm is similar for this smoke case compared to the dust cases, having potential implications for the upcoming EarthCARE satellite, which will measure particle depolarization ratio only at 355 nm.

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.

Helicopter-borne observations of the continental background aerosol in combination with remote sensing and ground-based measurements

NASA Astrophysics Data System (ADS)

Düsing, Sebastian; Wehner, Birgit; Seifert, Patric; Ansmann, Albert; Baars, Holger; Ditas, Florian; Henning, Silvia; Ma, Nan; Poulain, Laurent; Siebert, Holger; Wiedensohler, Alfred; Macke, Andreas

2018-01-01

This paper examines the representativeness of ground-based in situ measurements for the planetary boundary layer (PBL) and conducts a closure study between airborne in situ and ground-based lidar measurements up to an altitude of 2300 m. The related measurements were carried out in a field campaign within the framework of the High-Definition Clouds and Precipitation for Advancing Climate Prediction (HD(CP)2) Observational Prototype Experiment (HOPE) in September 2013 in a rural background area of central Europe.The helicopter-borne probe ACTOS (Airborne Cloud and Turbulence Observation System) provided measurements of the aerosol particle number size distribution (PNSD), the aerosol particle number concentration (PNC), the number concentration of cloud condensation nuclei (CCN-NC), and meteorological atmospheric parameters (e.g., temperature and relative humidity). These measurements were supported by the ground-based 3+2 wavelength polarization lidar system PollyXT, which provided profiles of the particle backscatter coefficient (σbsc) for three wavelengths (355, 532, and 1064 nm). Particle extinction coefficient (σext) profiles were obtained by using a fixed backscatter-to-extinction ratio (also lidar ratio, LR). A new approach was used to determine profiles of CCN-NC for continental aerosol. The results of this new approach were consistent with the airborne in situ measurements within the uncertainties.In terms of representativeness, the PNSD measurements on the ground showed a good agreement with the measurements provided with ACTOS for lower altitudes. The ground-based measurements of PNC and CCN-NC are representative of the PBL when the PBL is well mixed. Locally isolated new particle formation events on the ground or at the top of the PBL led to vertical variability in the cases presented here and ground-based measurements are not entirely representative of the PBL. Based on Mie theory (Mie, 1908), optical aerosol properties under ambient conditions for

Altitude Differentiated Aerosol Extinction Over Tenerife (North Atlantic Coast) During ACE-2 by Means of Ground and Airborne Photometry and Lidar Measurements

NASA Technical Reports Server (NTRS)

Formenti, P.; Elias, T.; Welton, J.; Diaz, J. P.; Exposito, F.; Schmid, B.; Powell, D.; Holben, B. N.; Smirnov, A.; Andreae, M. O.;

Measurements of Primary Biogenic Aerosol Particles with an Ultraviolet Aerodynamic Particle Sizer (UVAPS) During AMAZE-08

NASA Astrophysics Data System (ADS)

Wollny, A. G.; Garland, R.; Pöschl, U.

2008-12-01

Biogenic aerosols are ubiquitous in the Earth's atmosphere and they influence atmospheric chemistry and physics, the biosphere, climate, and public health. They play an important role in the spread of biological organisms and reproductive materials, and they can cause or enhance human, animal, and plant diseases. Moreover, they influence the Earth's energy budget by scattering and absorbing radiation, and they can initiate the formation of clouds and precipitation as cloud condensation and ice nuclei. The composition, abundance, and origin of biogenic aerosol particles and components are, however, still not well understood and poorly quantified. Prominent examples of primary biogenic aerosol particles, which are directly emitted from the biosphere to the atmosphere, are pollen, bacteria, fungal spores, viruses, and fragments of animals and plants. During the AMazonian Aerosol CharacteriZation Experiment (AMAZE-08) a large number of aerosol and gas-phase measurements were taken on a remote site close to Manaus, Brazil, during a period of five weeks in February and March 2008. The presented study is focused on data from an ultraviolet aerodynamic particle sizer (UVAPS, TSI inc.) that has been deployed for the first time in Amazonia. In this instrument, particle counting and aerodynamic sizing over the range of 0.5-20 μm are complemented by the measurement of UV fluorescence at 355 nm (excitation) and 420-575 nm (emission), respectively. Fluorescence at these wavelengths is characteristic for reduced pyridine nucleotides (e.g., NAD(P)H) and for riboflavin, which are specific for living cells. Thus particles exhibiting fluorescence signals can be regarded as 'viable aerosols' or 'fluorescent bioparticles' (FBAP), and their concentration can be considered as lower limit for the actual abundance of primary biogenic aerosol particles. First data analyses show a pronounced peak of FBAP at diameters around 2-3 μm. In this size range the biogenic particle fraction was

Astronomical Extinction Over The ELT Moroccan Sites From Aerosol Satellite Data

NASA Astrophysics Data System (ADS)

Siher, E. A.; Benkhaldoun, Z.; Bounhir, A.

2006-08-01

Two Moroccan sites are selected to be characterized for the ELT telescopes. These sites are in the Atlas, between Oukaimeden (where is the national observatory) and The Canaries Islands. For a preliminary study, we will use the TOMS/Nimbus7 aerosol index (AI), threshold 0.7, to extract the astronomical extinction (AE), threshold 0.2 mag/airmass. In fact, on the one hand, one previously work showed the link between these parameters over the Canaries Islands (ORM Observatory). On the other hand, many studies proposed the dust characterization for the future extremely large telescope for a mandatory qualification.

Regional haze case studies in the southwestern U.S—I. Aerosol chemical composition

NASA Astrophysics Data System (ADS)

Macias, Edward S.; Zwicker, Judith O.; Ouimette, James R.; Hering, Susanne V.; Friedlander, Sheldon K.; Cahill, Thomas A.; Kuhlmey, Gregory A.; Richards, L. Willard

Aerosol chemical composition as a function of particle size was determined in the southwestern U.S.A. during four weeks of sampling in June, July and December, 1979 as a part of project VISITA. Samples were collected at two ground stations about 80 km apart near Page (AZ) and in two aircraft flying throughout the region. Several different size separating aerosol samplers and chemical analysis procedures were intercompared and were used in determining the size distribution and elemental composition of the aerosol. Sulfur was shown to be in the form of water soluable sulfate, highly correlated with ammonium ion, and with an average [NH +4]/[SO 2-4] molar ratio of 1.65. During the summer sampling period, three distinct regimes were observed, each with a different aerosol composition. The first, 24 h sampling ending 30 June, was characterized by a higher than average value of light scattering due to particles (b sp) of 24 × 10 -6m-1 and a fine particulate mass ( Mf) of 8.5 μg m -1. The fine particle aerosol was dominated by sulfate and carbon. Aircraft measurements showed the aerosol was homogeneous throughout the region at that time. The second regime, 5 July, had the highest average bsp of 51 × 10 -6m -1 during the sampling period with Mf of 3.2 μgm -3. The fine particle aerosol had nearly equal concentrations of carbon and ammonium sulfate. For all three regimes, enrichment factor analysis indicated fine and coarse particle Cu, Zn, Cl, Br, and Pb and fine particle K were enriched above crustal concentrations relative to Fe, indicating that these elements were present in the aerosol from sources other than wind blown dust. Particle extinction budgets calculated for the three regimes indicated that fine particles contributed most significantly, with carbon and (NH 4) 2SO 4 making the largest contributions. Fine particle crustal elements including Si did not contribute significantly to the extinction budget during this study. The December sampling was characterized

Assessment of aerosol's mass concentrations from measured linear particle depolarization ratio (vertically resolved) and simulations

NASA Astrophysics Data System (ADS)

Nemuc, A.; Vasilescu, J.; Talianu, C.; Belegante, L.; Nicolae, D.

2013-11-01

Multi-wavelength depolarization Raman lidar measurements from Magurele, Romania are used in this study along with simulated mass-extinction efficiencies to calculate the mass concentration profiles of different atmospheric components, due to their different depolarization contribution to the 532 nm backscatter coefficient. Linear particle depolarization ratio (δpart) was computed using the relative amplification factor and the system-dependent molecular depolarization. The low depolarizing component was considered as urban/smoke, with a mean δpart of 3%, while for the high depolarizing component (mineral dust) a mean δpart of 35% was assumed. For this study 11 months of lidar measurements were analysed. Two study cases are presented in details: one for a typical Saharan dust aerosol intrusion, 10 June 2012 and one for 12 July 2012 when a lofted layer consisting of biomass burning smoke extended from 3 to 4.5 km height. Optical Properties of Aerosols and Clouds software package (OPAC) classification and conversion factors were used to calculate mass concentrations. We found that calibrated depolarization measurements are critical in distinguishing between smoke-reach aerosol during the winter and dust-reach aerosol during the summer, as well as between elevated aerosol layers having different origins. Good agreement was found between lidar retrievals and DREAM- Dust REgional Atmospheric Model forecasts in cases of Saharan dust. Our method was also compared against LIRIC (The Lidar/Radiometer Inversion Code) and very small differences were observed.

Assessment of aerosol's mass concentrations from measured linear particle depolarization ratio (vertically resolved) and simulations

NASA Astrophysics Data System (ADS)

Nemuc, A.; Vasilescu, J.; Talianu, C.; Belegante, L.; Nicolae, D.

2013-06-01

Multiwavelength depolarization Raman lidar measurements from Magurele, Romania are used in this study along with simulated mass-extinction efficiencies to calculate the mass concentrations profiles of different atmospheric components, due to their different depolarization contribution to the 532 nm backscatter coefficient. Linear particle depolarization ratio (δpart) was computed using the relative amplification factor and the system-dependent molecular depolarization. The low depolarizing component was considered as urban/smoke, with a mean δpart of 3%, while for the high depolarizing component (mineral dust) a mean δpart of 35% was assumed. For this study 11 months of lidar measurements were analyzed. Two study cases are presented in details: one for a typical Saharan dust aerosol intrusion, 10 June 2012 and one for 12 July 2012 when a lofted layer consisting of biomass burning smoke extended from 3 to 4.5 km height. Optical Properties of Aerosols and Clouds software package (OPAC) classification and conversion factors were used to calculate mass concentrations. We found that calibrated depolarization measurements are critical to distinguish between smoke-reach aerosol during the winter and dust-reach aerosol during the summer, as well as between elevated aerosol layers having different origins. Good agreement was found between lidar retrievals and DREAM- Dust REgional Atmospheric Model forecasts in cases of Saharan dust. Our method was also compared against LIRIC (The Lidar/Radiometer Inversion Code) and very small differences were observed.

Substantial convection and precipitation enhancements by ultrafine aerosol particles

NASA Astrophysics Data System (ADS)

Fan, Jiwen; Rosenfeld, Daniel; Zhang, Yuwei; Giangrande, Scott E.; Li, Zhanqing; Machado, Luiz A. T.; Martin, Scot T.; Yang, Yan; Wang, Jian; Artaxo, Paulo; Barbosa, Henrique M. J.; Braga, Ramon C.; Comstock, Jennifer M.; Feng, Zhe; Gao, Wenhua; Gomes, Helber B.; Mei, Fan; Pöhlker, Christopher; Pöhlker, Mira L.; Pöschl, Ulrich; de Souza, Rodrigo A. F.

2018-01-01

Ultrafine aerosol particles (smaller than 50 nanometers in diameter) have been thought to be too small to affect cloud formation. Fan et al. show that this is not the case. They studied the effect of urban pollution transported into the otherwise nearly pristine atmosphere of the Amazon. Condensational growth of water droplets around the tiny particles releases latent heat, thereby intensifying atmospheric convection. Thus, anthropogenic ultrafine aerosol particles may exert a more important influence on cloud formation processes than previously believed.

Retrieval of atmospheric backscatter and extinction profiles with the aladin airborne demonstrator (A2D)

NASA Astrophysics Data System (ADS)

Geiss, Alexander; Marksteiner, Uwe; Lux, Oliver; Lemmerz, Christian; Reitebuch, Oliver; Kanitz, Thomas; Straume-Lindner, Anne Grete

2018-04-01

By the end of 2017, the European Space Agency (ESA) will launch the Atmospheric laser Doppler instrument (ALADIN), a direct detection Doppler wind lidar operating at 355 nm. An important tool for the validation and optimization of ALADIN's hardware and data processors for wind retrievals with real atmospheric signals is the ALADIN airborne demonstrator A2D. In order to be able to validate and test aerosol retrieval algorithms from ALADIN, an algorithm for the retrieval of atmospheric backscatter and extinction profiles from A2D is necessary. The A2D is utilizing a direct detection scheme by using a dual Fabry-Pérot interferometer to measure molecular Rayleigh signals and a Fizeau interferometer to measure aerosol Mie returns. Signals are captured by accumulation charge coupled devices (ACCD). These specifications make different steps in the signal preprocessing necessary. In this paper, the required steps to retrieve aerosol optical products, i. e. particle backscatter coefficient βp, particle extinction coefficient αp and lidar ratio Sp from A2D raw signals are described.

MASS SPECTROMETRY OF INDIVIDUAL AEROSOL PARTICLES. (R823980)

EPA Science Inventory

Typically, in real-time aerosol mass spectrometry (RTAMS), individual airborne particles
are ablated and ionized with a single focused laser pulse. This technique yields information that
permits bulk characterization of the particle, but information about the particle's sur...

Time Resolved Measurements of Primary Biogenic Aerosol Particles in Amazonia

NASA Astrophysics Data System (ADS)

Wollny, A. G.; Garland, R.; Pöschl, U.

2009-04-01

Biogenic aerosols are ubiquitous in the Earth's atmosphere and they influence atmospheric chemistry and physics, the biosphere, climate, and public health. They play an important role in the spread of biological organisms and reproductive materials, and they can cause or enhance human, animal, and plant diseases. Moreover, they influence the Earth's energy budget by scattering and absorbing radiation, and they can initiate the formation of clouds and precipitation as cloud condensation and ice nuclei. The composition, abundance, and origin of biogenic aerosol particles and components are, however, still not well understood and poorly quantified. Prominent examples of primary biogenic aerosol particles, which are directly emitted from the biosphere to the atmosphere, are pollen, bacteria, fungal spores, viruses, and fragments of animals and plants. During the Amazonian Aerosol Characterization Experiment (AMAZE-08) a large number of aerosol and gas-phase measurements were taken on a remote site close to Manaus, Brazil, during a period of five weeks in February and March 2008. This presented study is focused on data from an ultraviolet aerodynamic particle sizer (UVAPS, TSI inc.) that has been deployed for the first time in Amazonia. In this instrument, particle counting and aerodynamic sizing over the range of 0.5-20 µm are complemented by the measurement of UV fluorescence at 355 nm (excitation) and 420-575 nm (emission), respectively. Fluorescence at these wavelengths is characteristic for reduced pyridine nucleotides (e.g., NAD(P)H) and for riboflavin, which are specific for living cells. Thus particles exhibiting fluorescence signals can be regarded as "viable aerosols" or "fluorescent bioparticles" (FBAP), and their concentration can be considered as lower limit for the actual abundance of primary biogenic aerosol particles. Data from the UVAPS were averaged over 5 minute time intervals. The presence of bioparticles in the observed size range has been

Reactions and mass spectra of complex particles using Aerosol CIMS

NASA Astrophysics Data System (ADS)

Hearn, John D.; Smith, Geoffrey D.

2006-12-01

Aerosol chemical ionization mass spectrometry (CIMS) is used both on- and off-line for the analysis of complex laboratory-generated and ambient particles. One of the primary advantages of Aerosol CIMS is the low degree of ion fragmentation, making this technique well suited for investigating the reactivity of complex particles. To demonstrate the usefulness of this "soft" ionization, particles generated from meat cooking were reacted with ozone and the composition was monitored as a function of reaction time. Two distinct kinetic regimes were observed with most of the oleic acid in these particles reacting quickly but with 30% appearing to be trapped in the complex mixture. Additionally, detection limits are measured to be sufficiently low (100-200 ng/m3) to detect some of the more abundant constituents in ambient particles, including sulfate, which is measured in real-time at 1.2 [mu]g/m3. To better characterize complex aerosols from a variety of sources, a novel off-line collection method was also developed in which non-volatile and semi-volatile organics are desorbed from particles and concentrated in a cold U-tube. Desorption from the U-tube followed by analysis with Aerosol CIMS revealed significant amounts of nicotine in cigarette smoke and levoglucosan in oak and pine smoke, suggesting that this may be a useful technique for monitoring particle tracer species. Additionally, secondary organic aerosol formed from the reaction of ozone with R-limonene and volatile organics from orange peel were analyzed off-line showing large molecular weight products (m/z > 300 amu) that may indicate the formation of oligomers. Finally, mass spectra of ambient aerosol collected offline reveal a complex mixture of what appears to be highly processed organics, some of which may contain nitrogen.

Lidar characterizations of atmospheric aerosols and clouds

NASA Astrophysics Data System (ADS)

Ferrare, R. A.; Hostetler, C. A.; Hair, J. W.; Burton, S. P.

2017-12-01

Knowledge of the vertical profile, composition, concentration, and size distribution of aerosols is required to quantify the impacts of aerosols on human health, global and regional climate, clouds and precipitation. In particular, radiative forcing due to anthropogenic aerosols is the most uncertain part of anthropogenic radiative forcing, with aerosol-cloud interactions (ACI) as the largest source of uncertainty in current estimates of global radiative forcing. Improving aerosol transport model predictions of the vertical profile of aerosol optical and microphysical characteristics is crucial for improving assessments of aerosol radiative forcing. Understanding how aerosols and clouds interact is essential for investigating the aerosol indirect effect and ACI. Through its ability to provide vertical profiles of aerosol and cloud distributions as well as important information regarding the optical and physical properties of aerosols and clouds, lidar is a crucial tool for addressing these science questions. This presentation describes how surface, airborne, and satellite lidar measurements have been used to address these questions, and in particular how High Spectral Resolution Lidar (HSRL) measurements provide profiles of aerosol properties (backscatter, extinction, depolarization, concentration, size) important for characterizing radiative forcing. By providing a direct measurement of aerosol extinction, HSRL provides more accurate aerosol measurement profiles and more accurate constraints for models than standard retrievals from elastic backscatter lidar, which loses accuracy and precision at lower altitudes due to attenuation from overlying layers. Information regarding particle size and abundance from advanced lidar retrievals provides better proxies for cloud-condensation-nuclei (CCN), which are required for assessing aerosol-cloud interactions. When combined with data from other sensors, advanced lidar measurements can provide information on aerosol and

New apparatus of single particle trap system for aerosol visualization

NASA Astrophysics Data System (ADS)

Higashi, Hidenori; Fujioka, Tomomi; Endo, Tetsuo; Kitayama, Chiho; Seto, Takafumi; Otani, Yoshio

2014-08-01

Control of transport and deposition of charged aerosol particles is important in various manufacturing processes. Aerosol visualization is an effective method to directly observe light scattering signal from laser-irradiated single aerosol particle trapped in a visualization cell. New single particle trap system triggered by light scattering pulse signal was developed in this study. The performance of the device was evaluated experimentally. Experimental setup consisted of an aerosol generator, a differential mobility analyzer (DMA), an optical particle counter (OPC) and the single particle trap system. Polystylene latex standard (PSL) particles (0.5, 1.0 and 2.0 μm) were generated and classified according to the charge by the DMA. Singly charged 0.5 and 1.0 μm particles and doubly charged 2.0 μm particles were used as test particles. The single particle trap system was composed of a light scattering signal detector and a visualization cell. When the particle passed through the detector, trigger signal with a given delay time sent to the solenoid valves upstream and downstream of the visualization cell for trapping the particle in the visualization cell. The motion of particle in the visualization cell was monitored by CCD camera and the gravitational settling velocity and the electrostatic migration velocity were measured from the video image. The aerodynamic diameter obtained from the settling velocity was in good agreement with Stokes diameter calculated from the electrostatic migration velocity for individual particles. It was also found that the aerodynamic diameter obtained from the settling velocity was a one-to-one function of the scattered light intensity of individual particles. The applicability of this system will be discussed.

Interactions between meteoric smoke particles and the stratospheric aerosol layer

NASA Astrophysics Data System (ADS)

Mann, G. W.; Marshall, L.; Brooke, J. S. A.; Dhomse, S.; Plane, J. M. C.; Feng, W.; Neely, R.; Bardeen, C.; Bellouin, N.; Dalvi, M.; Johnson, C.; Abraham, N. L.; Schmidt, A.; Carslaw, K. S.; Chipperfield, M.; Deshler, T.; Thomason, L. W.

2017-12-01

In-situ measurements in the Arctic, Antarctic and at mid-latitudes suggest a widespread presence of meteoric smoke particles (MSPs), as an inclusion within a distinct class of stratospheric aerosol particles. We apply the UM-UKCA stratosphere-troposphere composition-climate model, with interactive aerosol microphysics, to map the global distribution of these "meteoric-sulphuric particles" and explore the implications of their presence. Comparing to balloon-borne stratospheric aerosol measurements, we indirectly constrain the uncertain MSP flux into the upper mesosphere, and assess whether meteoric inclusion can explain observed refractory/non-volatile particle concentrations. Our experiments suggest meteoric-sulphuric particles are present at all latitudes, the Junge layer transitioning from mostly homogeneously nucleated particles at the bottom, to mostly meteoric-sulphuric particles at the top. We find MSPs exert a major influence on the quiescent Junge layer, with meteoric-sulphuric particles generally bigger than homogeneously nucleated particles, and therefore more rapidly removed into the upper troposphere. Resolving the smoke interactions weakens homogeneous nucleation in polar spring, reduces the quiescent sulphur burden, and improves comparisons to a range of different stratospheric aerosol measurements. The refractory nature of meteoric-sulphuric particles also means they "survive" ascent through the uppermost Junge layer, whereas homogeneously nucleated particles evaporate completely. Simulations through the Pinatubo-perturbed period are more realistic, with greater volcanic enhancement of effective radius, causing faster decay towards quiescent conditions, both effects matching better with observations. Overall, our experiments suggest meteoric-sulphuric particles are an important component of the Junge layer, strongly influential in both quiescent and volcanically perturbed conditions.

Inhomogeneities in particle composition of single, levitated aerosol particles observed by Mie resonance spectroscopy

NASA Astrophysics Data System (ADS)

Krieger, Ulrich; Lienhard, Daniel; Bastelberger, Sandra; Steimer, Sarah

2014-05-01

Recent observations have indicated that organic aerosol particles in the atmosphere may exist in an amorphous semi-solid or even solid (i.e. glassy) state, e.g. [1]. The influence of highly viscous and glassy states on the timescale of aerosol particle equilibration with respect to water vapor have been investigated for some model systems of atmospheric aerosol, e.g. [2,3]. In particular, it has been shown that the kinetics of the water absorption/desorption process is controlled entirely by liquid-phase diffusion of water molecules for a highly viscous aerosol particle. A liquid phase diffusion model based on numerically solving the non-linear diffusion equation predicts strong internal gradients in water concentration when condensed phase diffusion impedes the water uptake from the gas phase [2]. Here we observe and quantify the internal concentration gradients in single, levitated, micron size aerosol particles of aqueous shikimic acid using elastic Mie resonance spectroscopy. A single, aqueous particle is levitated in an electro-dynamic balance (for details see [2]), dried for several days at room temperature, cooled to the target temperature and exposed to a rapid change in relative humidity. In addition to measuring the elastically backscattered light of a "white light" LED source and recording the full spectrum with a spectrograph as in [2], we use a tunable diode laser (TDL) to scan high resolution TE- and TM spectra. This combination allows observing various Mie resonance mode orders simultaneously. Since we perform the experiment at low temperatures and low humidities the changes in the Mie-spectra due to water uptake are sufficiently slow to resolve the kinetics. Experimental Mie resonance spectra are inverted to concentration profiles of water within the particle by applying the numerical diffusion model [2] in conjunction with Mie calculations of multilayered spheres [4]. [1] A. Virtanen et al. (2010): An amorphous solid state of biogenic secondary

How Well do State-of-the-Art Techniques Measuring the Vertical Profile of Tropospheric Aerosol Extinction Compare?

NASA Technical Reports Server (NTRS)

Schmid, B.; Ferrare, R.; Flynn, C.; Elleman, R.; Covert, D.; Strawa, A.; Welton, E.; Turner, D.; Jonsson, H.; Redemann, J.;

Design of Aerosol Particle Coating: Thickness, Texture and Efficiency

PubMed Central

Buesser, B.; Pratsinis, S.E.

2013-01-01

Core-shell particles preserve the performance (e.g. magnetic, plasmonic or opacifying) of a core material while modifying its surface with a shell that facilitates (e.g. by blocking its reactivity) their incorporation into a host liquid or polymer matrix. Here coating of titania (core) aerosol particles with thin silica shells (films or layers) is investigated at non-isothermal conditions by a trimodal aerosol dynamics model, accounting for SiO2 generation by gas phase and surface oxidation of hexamethyldisiloxane (HMDSO) vapor, coagulation and sintering. After TiO2 particles have reached their final primary particle size (e.g. upon completion of sintering during their flame synthesis), coating starts by uniformly mixing them with HMDSO vapor that is oxidized either in the gas phase or on the particles’ surface resulting in SiO2 aerosols or deposits, respectively. Sintering of SiO2 deposited onto the core TiO2 particles takes place transforming rough into smooth coating shells depending on process conditions. The core-shell characteristics (thickness, texture and efficiency) are calculated for two limiting cases of coating shells: perfectly smooth (e.g. hermetic) and fractal-like. At constant TiO2 core particle production rate, the influence of coating weight fraction, surface oxidation and core particle size on coating shell characteristics is investigated and compared to pertinent experimental data through coating diagrams. With an optimal temperature profile for complete precursor conversion, the TiO2 aerosol and SiO2-precursor (HMDSO) vapor concentrations have the strongest influence on product coating shell characteristics. PMID:23729833

Growth rates of fine aerosol particles at a site near Beijing in June 2013

NASA Astrophysics Data System (ADS)

Zhao, Chuanfeng; Li, Yanan; Zhang, Fang; Sun, Yele; Wang, Pucai

2018-02-01

Growth of fine aerosol particles is investigated during the Aerosol-CCN-Cloud Closure Experiment campaign in June 2013 at an urban site near Beijing. Analyses show a high frequency (˜ 50%) of fine aerosol particle growth events, and show that the growth rates range from 2.1 to 6.5 nm h-1 with a mean value of ˜ 5.1 nm h-1. A review of previous studies indicates that at least four mechanisms can affect the growth of fine aerosol particles: vapor condensation, intramodal coagulation, extramodal coagulation, and multi-phase chemical reaction. At the initial stage of fine aerosol particle growth, condensational growth usually plays a major role and coagulation efficiency generally increases with particle sizes. An overview of previous studies shows higher growth rates over megacity, urban and boreal forest regions than over rural and oceanic regions. This is most likely due to the higher condensational vapor, which can cause strong condensational growth of fine aerosol particles. Associated with these multiple factors of influence, there are large uncertainties for the aerosol particle growth rates, even at the same location.

Aerosol Particle Shape and Radiative Coupling in a Three Dimensional Titan GCM

NASA Astrophysics Data System (ADS)

Larson, Erik J.; Toon, O. B.; Friedson, A. J.; West, R. A.

2010-10-01

Understanding the aerosols on Titan is imperative for understanding the atmosphere as a whole. The aerosols affect the albedo, optical depth, as well as heating and cooling rates which in turn affect the circulation on Titan leading to feedback with the aerosol distribution. Correctly representing the aerosols in atmospheric models is crucial to understanding this atmosphere. Friedson et al. (2009, A global climate model of Titan's atmosphere and surface. Planet. SpaceSci. 57, 1931-1949.) produced a three-dimensional model for Titan using the NCAR CAM3 model, to which we coupled the aerosol microphysics model CARMA. We have also made the aerosols produced by CARMA interactive with the radiation code in CAM. We compare simulations with radiatively interactive aerosols with those using a prescribed aerosol radiative effect. Preliminary results show that this model is capable of reproducing the seasonal changes in aerosols on Titan and many of the associated phenomena. For instance, the radiatively interactive aerosols are lofted by winds more in the summer hemisphere than the non-radiatively interactive aerosols, which is necessary to reproduce the observed seasonal cycle of the albedo. We compare simulations using spherical particles to simulations using fractal aggregate particles, which are expected from laboratory and observational data. Fractal particles have higher absorption in the UV, slower fall velocities and faster coagulation rates than equivalent mass spherical particles. We compare model simulations with observational data from the Cassini and Huygens missions.

Thermophoretic separation of aerosol particles from a sampled gas stream

DOEpatents

Postma, Arlin K.

1986-01-01

A method for separating gaseous samples from a contained atmosphere that includes aerosol particles uses the step of repelling particles from a gas permeable surface or membrane by heating the surface to a temperature greater than that of the surrounding atmosphere. The resulting thermophoretic forces maintain the gas permeable surface clear of aerosol particles. The disclosed apparatus utilizes a downwardly facing heated plate of gas permeable material to combine thermophoretic repulsion and gravity forces to prevent particles of any size from contacting the separating plate surfaces.

Direct comparison of extinction coefficients derived from Mie-scattering lidar and number concentrations of particles, subjective weather report in Japan

NASA Astrophysics Data System (ADS)

Shimizu, Atsushi; Sugimoto, Nobuo; Matsui, Ichiro; Nishizawa, Tomoaki

2015-03-01

Two components of the lidar extinction coefficient, the dust extinction and the spherical particles extinction, were obtained from observations made by the National Institute for Environmental Studies lidar network in Japan. These two extinctions were compared with the number concentration of particles measured by an optical particle counter, and with subjective weather reports recorded at the nearest meteorological observatories. The dust extinction corresponded well with the number concentration of large particles with diameters as great as 5 μm and during dry conditions with the number concentration of particles larger than 2 μm. The relationship between the spherical particle extinction and the number of small particles was nearly constant under all conditions. Asian dust was sometimes reported by meteorological observatories in the period of lower dust extinction. This indicates contradicting relationship between human-eye based reports and optical characteristics observed by lidars in some cases. The most consistent results between lidar observation and meteorological reports were obtained in dry mist conditions, in which lidars exhibited higher spherical extinction as expected by the definition of the atmospheric phenomenon of dry mist or haze.

A thermal desorption mass spectrometer for freshly nucleated secondary aerosol particles

NASA Astrophysics Data System (ADS)

Held, A.; Gonser, S. G.

2012-04-01

Secondary aerosol formation in the atmosphere is observed in a large variety of locations worldwide, introducing new particles to the atmosphere which can grow to sizes relevant for health and climate effects of aerosols. The chemical reactions leading to atmospheric secondary aerosol formation are not yet fully understood. At the same time, analyzing the chemical composition of freshly nucleated particles is still a challenging task. We are currently finishing the development of a field portable aerosol mass spectrometer for nucleation particles with diameters smaller than 30 nm. This instrument consists of a custom-built aerosol sizing and collection unit coupled to a time-of-flight mass spectrometer (TOF-MS). The aerosol sizing and collection unit is composed of three major parts: (1) a unipolar corona aerosol charger, (2) a radial differential mobility analyzer (rDMA) for aerosol size separation, and (3) an electrostatic precipitator for aerosol collection. After collection, the aerosol sample is thermally desorbed, and the resulting gas sample is transferred to the TOF-MS for chemical analysis. The unipolar charger is based on corona discharge from carbon fibres (e.g. Han et al., 2008). This design allows efficient charging at voltages below 2 kV, thus eliminating the potential for ozone production which would interfere with the collected aerosol. With the current configuration the extrinsic charging efficiency for 20 nm particles is 32 %. The compact radial DMA similar to the design of Zhang et al. (1995) is optimized for a diameter range from 1 nm to 100 nm. Preliminary tests show that monodisperse aerosol samples (geometric standard deviation of 1.09) at 10 nm, 20 nm, and 30 nm can easily be separated from the ambient polydisperse aerosol population. Finally, the size-segregated aerosol sample is collected on a high-voltage biased metal filament. The collected sample is protected from contamination using a He sheath counterflow. Resistive heating of the

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

Characterization of aerosol particles at the forested site in Lithuania

NASA Astrophysics Data System (ADS)

Rimselyte, I.; Garbaras, A.; Kvietkus, K.; Remeikis, V.

2009-04-01

Atmospheric particulate matter (PM), especially fine particles (particles with aerodynamic diameter less than 1 m, PM1), has been found to play an important role in global climate change, air quality, and human health. The continuous study of aerosol parameters is therefore imperative for better understanding the environmental effects of the atmospheric particles, as well as their sources, formation and transformation processes. The particle size distribution is particularly important, since this physical parameter determines the mass and number density, lifetime and atmospheric transport, or optical scattering behavior of the particles in the atmosphere (Jaenicke, 1998). Over the years several efforts have been made to improve the knowledge about the chemical composition of atmospheric particles as a function of size (Samara and Voutsa, 2005) and to characterize the relative contribution of different components to the fine particulate matter. It is well established that organic materials constitute a highly variable fraction of the atmospheric aerosol. This fraction is predominantly found in the fine size mode in concentrations ranging from 10 to 70% of the total dry fine particle mass (Middlebrook et al., 1998). Although organic compounds are major components of the fine particles, the composition, formation mechanism of organic aerosols are not well understood. This is because particulate organic matter is part of a complex atmospheric system with hundreds of different compounds, both natural and anthropogenic, covering a wide range of chemical properties. The aim of this study was to characterize the forest PM1, and investigate effects of air mass transport on the aerosol size distribution and chemical composition, estimate and provide insights into the sources and characteristics of carbonaceous aerosols through analysis ^13C/12C isotopic ratio as a function of the aerosol particles size. The measurements were performed at the Rugšteliškis integrated

Apparatus having reduced background for measuring radiation activity in aerosol particles

DOEpatents

Rodgers, John C.; McFarland, Andrew R.; Oritz, Carlos A.; Marlow, William H.

1992-01-01

Apparatus having reduced background for measuring radiation activity in aerosol particles. A continuous air monitoring sampler is described for use in detecting the presence of alpha-emitting aerosol particles. An inlet fractionating screen has been demonstrated to remove about 95% of freshly formed radon progeny from the aerosol sample, and approximately 33% of partially aged progeny. Addition of an electrical condenser and a modified dichotomous virtual impactor are expected to produce considerable improvement in these numbers, the goal being to enrich the transuranic (TRU) fraction of the aerosols. This offers the possibility of improving the signal-to-noise ratio for the detected alpha-particle energy spectrum in the region of interest for detecting TRU materials associated with aerosols, thereby enhancing the performance of background-compensation algorithms for improving the quality of alarm signals intended to warn personnel of potentially harmful quantities of TRU materials in the ambient air.

Ice Nucleation Activity of Various Agricultural Soil Dust Aerosol Particles

NASA Astrophysics Data System (ADS)

Schiebel, Thea; Höhler, Kristina; Funk, Roger; Hill, Thomas C. J.; Levin, Ezra J. T.; Nadolny, Jens; Steinke, Isabelle; Suski, Kaitlyn J.; Ullrich, Romy; Wagner, Robert; Weber, Ines; DeMott, Paul J.; Möhler, Ottmar

2016-04-01

Recent investigations at the cloud simulation chamber AIDA (Aerosol Interactions and Dynamics in the Atmosphere) suggest that agricultural soil dust has an ice nucleation ability that is enhanced up to a factor of 10 compared to desert dust, especially at temperatures above -26 °C (Steinke et al., in preparation for submission). This enhancement might be caused by the contribution of very ice-active biological particles. In addition, soil dust aerosol particles often contain a considerably higher amount of organic matter compared to desert dust particles. To test agricultural soil dust as a source of ice nucleating particles, especially for ice formation in warm clouds, we conducted a series of laboratory measurements with different soil dust samples to extend the existing AIDA dataset. The AIDA has a volume of 84 m3 and operates under atmospherically relevant conditions over wide ranges of temperature, pressure and humidity. By controlled adiabatic expansions, the ascent of an air parcel in the troposphere can be simulated. As a supplement to the AIDA facility, we use the INKA (Ice Nucleation Instrument of the KArlsruhe Institute of Technology) continuous flow diffusion chamber based on the design by Rogers (1988) to expose the sampled aerosol particles to a continuously increasing saturation ratio by keeping the aerosol temperature constant. For our experiments, soil dust was dry dispersed into the AIDA vessel. First, fast saturation ratio scans at different temperatures were performed with INKA, sampling soil dust aerosol particles directly from the AIDA vessel. Then, we conducted the AIDA expansion experiment starting at a preset temperature. The combination of these two different methods provides a robust data set on the temperature-dependent ice activity of various agriculture soil dust aerosol particles with a special focus on relatively high temperatures. In addition, to extend the data set, we investigated the role of biological and organic matter in more

Physicochemical Characterization of Capstone Depleted Uranium Aerosols I: Uranium Concentration in Aerosols as a Function of Time and Particle Size

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

Parkhurst, MaryAnn; Cheng, Yung-Sung; Kenoyer, Judson L.

2009-03-01

During the Capstone Depleted Uranium (DU) Aerosol Study, aerosols containing depleted uranium were produced inside unventilated armored vehicles (i.e., Abrams tanks and Bradley Fighting Vehicles) by perforation with large-caliber DU penetrators. These aerosols were collected and characterized, and the data were subsequently used to assess human health risks to personnel exposed to DU aerosols. The DU content of each aerosol sample was first quantified by radioanalytical methods, and selected samples, primarily those from the cyclone separator grit chambers, were analyzed radiochemically. Deposition occurred inside the vehicles as particles settled on interior surfaces. Settling rates of uranium from the aerosols weremore » evaluated using filter cassette samples that collected aerosol as total mass over eight sequential time intervals. A moving filter was used to collect aerosol samples over time particularly within the first minute after the shot. The results demonstrate that the peak uranium concentration in the aerosol occurred in the first 10 s, and the concentration decreased in the Abrams tank shots to about 50% within 1 min and to less than 2% 30 min after perforation. In the Bradley vehicle, the initial (and maximum) uranium concentration was lower than those observed in the Abrams tank and decreased more slowly. Uranium mass concentrations in the aerosols as a function of particle size were evaluated using samples collected in the cyclone samplers, which collected aerosol continuously for 2 h post perforation. The percentages of uranium mass in the cyclone separator stages from the Abrams tank tests ranged from 38% to 72% and, in most cases, varied with particle size, typically with less uranium associated with the smaller particle sizes. Results with the Bradley vehicle ranged from 18% to 29% and were not specifically correlated with particle size.« less

Physicochemical characterization of Capstone depleted uranium aerosols I: uranium concentration in aerosols as a function of time and particle size.

PubMed

Parkhurst, Mary Ann; Cheng, Yung Sung; Kenoyer, Judson L; Traub, Richard J

2009-03-01

During the Capstone Depleted Uranium (DU) Aerosol Study, aerosols containing DU were produced inside unventilated armored vehicles (i.e., Abrams tanks and Bradley Fighting Vehicles) by perforation with large-caliber DU penetrators. These aerosols were collected and characterized, and the data were subsequently used to assess human health risks to personnel exposed to DU aerosols. The DU content of each aerosol sample was first quantified by radioanalytical methods, and selected samples, primarily those from the cyclone separator grit chambers, were analyzed radiochemically. Deposition occurred inside the vehicles as particles settled on interior surfaces. Settling rates of uranium from the aerosols were evaluated using filter cassette samples that collected aerosol as total mass over eight sequential time intervals. A moving filter was used to collect aerosol samples over time, particularly within the first minute after a shot. The results demonstrate that the peak uranium concentration in the aerosol occurred in the first 10 s after perforation, and the concentration decreased in the Abrams tank shots to about 50% within 1 min and to less than 2% after 30 min. The initial and maximum uranium concentrations were lower in the Bradley vehicle than those observed in the Abrams tank, and the concentration levels decreased more slowly. Uranium mass concentrations in the aerosols as a function of particle size were evaluated using samples collected in a cyclone sampler, which collected aerosol continuously for 2 h after perforation. The percentages of uranium mass in the cyclone separator stages ranged from 38 to 72% for the Abrams tank with conventional armor. In most cases, it varied with particle size, typically with less uranium associated with the smaller particle sizes. Neither the Abrams tank with DU armor nor the Bradley vehicle results were specifically correlated with particle size and can best be represented by their average uranium mass concentrations of 65

Composition of individual aerosol particles above the Israelian Mediterranean coast during the summer time

NASA Astrophysics Data System (ADS)

Ganor, E.; Levin, Z.; Van Grieken, R.

Aerosol particles were collected aboard a ship in Haifa Bay and Tel Aviv, Israel, during the summer time. The aerosol particles (6170) were analyzed as individual particles and classified according to their chemical composition, size, number concentration per cubic centimeter and morphology. Most of the aerosol particles could be classified into four groups. The first contains gypsum from the sea and from industrial sources brought in by land breezes. A second group is characterized by continental aluminosilicate and quartz. A third group consists of sea salt mixed with sulfate particles. The fourth group is characterized by an abundance of sulfate particles, some of which are ammonium sulfate brought by the land breezes. The particles were identified as marine and mineral aerosols which originated in Eastern Europe and the Mediterranean sea, while local aerosols brought by land breeze characterized by phosphate, fly ash and soil particles originated in the Haifa industrial zone. In addition, the aerosols were analyzed for sulfates and nitrates. Aerosols of sea and land breezes differed as follows: (1) Sulfate and nitrate concentrations in the aerosols were 5-10 times higher during land breeze than during sea breeze, and the total content of suspended particles was, respectively, 6-12 times higher. (2) Particle size spectra during land breeze were broader than during sea breeze and their concentrations were about 20 times greater. Analyses of individual particles by electron microscopy revealed that during the sea breeze the aerosols contained calcium sulfate, sodium sulfate and sulfuric acid. The sulfuric acid, of pH 2.5, is due to the long-range transport as previously reported ( Ganor et al., 1993) while the other sulfates are from the sea. This explains the high concentration of sulfates in the atmospheric sea breeze above the Israelian Mediterranean coast during the summertime.

Aerosol characteristics and particle production in the upper troposphere over the Amazon Basin

NASA Astrophysics Data System (ADS)

Andreae, Meinrat O.; Afchine, Armin; Albrecht, Rachel; Amorim Holanda, Bruna; Artaxo, Paulo; Barbosa, Henrique M. J.; Borrmann, Stephan; Cecchini, Micael A.; Costa, Anja; Dollner, Maximilian; Fütterer, Daniel; Järvinen, Emma; Jurkat, Tina; Klimach, Thomas; Konemann, Tobias; Knote, Christoph; Krämer, Martina; Krisna, Trismono; Machado, Luiz A. T.; Mertes, Stephan; Minikin, Andreas; Pöhlker, Christopher; Pöhlker, Mira L.; Pöschl, Ulrich; Rosenfeld, Daniel; Sauer, Daniel; Schlager, Hans; Schnaiter, Martin; Schneider, Johannes; Schulz, Christiane; Spanu, Antonio; Sperling, Vinicius B.; Voigt, Christiane; Walser, Adrian; Wang, Jian; Weinzierl, Bernadett; Wendisch, Manfred; Ziereis, Helmut

2018-01-01

Airborne observations over the Amazon Basin showed high aerosol particle concentrations in the upper troposphere (UT) between 8 and 15 km altitude, with number densities (normalized to standard temperature and pressure) often exceeding those in the planetary boundary layer (PBL) by 1 or 2 orders of magnitude. The measurements were made during the German-Brazilian cooperative aircraft campaign ACRIDICON-CHUVA, where ACRIDICON stands for Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems and CHUVA is the acronym for Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (global precipitation measurement), on the German High Altitude and Long Range Research Aircraft (HALO). The campaign took place in September-October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with atmospheric trace gases, aerosol particles, and atmospheric radiation. Aerosol enhancements were observed consistently on all flights during which the UT was probed, using several aerosol metrics, including condensation nuclei (CN) and cloud condensation nuclei (CCN) number concentrations and chemical species mass concentrations. The UT particles differed sharply in their chemical composition and size distribution from those in the PBL, ruling out convective transport of combustion-derived particles from the boundary layer (BL) as a source. The air in the immediate outflow of deep convective clouds was depleted of aerosol particles, whereas strongly enhanced number concentrations of small particles (< 90 nm diameter) were found in UT regions that had experienced outflow from deep convection in the preceding 5-72 h. We also found elevated concentrations of larger (> 90 nm) particles in the UT, which consisted mostly of organic matter and nitrate and were very effective CCN. Our findings suggest a

Aerosol characteristics and particle production in the upper troposphere over the Amazon Basin

DOE PAGES

Andreae, Meinrat O.; Afchine, Armin; Albrecht, Rachel; ...

2018-01-25

Airborne observations over the Amazon Basin showed high aerosol particle concentrations in the upper troposphere (UT) between 8 and 15 km altitude, with number densities (normalized to standard temperature and pressure) often exceeding those in the planetary boundary layer (PBL) by 1 or 2 orders of magnitude. The measurements were made during the German–Brazilian cooperative aircraft campaign ACRIDICON–CHUVA, where ACRIDICON stands for Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems and CHUVA is the acronym for Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (globalmore » precipitation measurement), on the German High Altitude and Long Range Research Aircraft (HALO). The campaign took place in September–October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with atmospheric trace gases, aerosol particles, and atmospheric radiation. Aerosol enhancements were observed consistently on all flights during which the UT was probed, using several aerosol metrics, including condensation nuclei (CN) and cloud condensation nuclei (CCN) number concentrations and chemical species mass concentrations. The UT particles differed sharply in their chemical composition and size distribution from those in the PBL, ruling out convective transport of combustion-derived particles from the boundary layer (BL) as a source. The air in the immediate outflow of deep convective clouds was depleted of aerosol particles, whereas strongly enhanced number concentrations of small particles (< 90 nm diameter) were found in UT regions that had experienced outflow from deep convection in the preceding 5–72 h. We also found elevated concentrations of larger (> 90 nm) particles in the UT, which consisted mostly of organic matter and nitrate and were very effective CCN. Our findings suggest a conceptual

Aerosol characteristics and particle production in the upper troposphere over the Amazon Basin

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

Andreae, Meinrat O.; Afchine, Armin; Albrecht, Rachel

Airborne observations over the Amazon Basin showed high aerosol particle concentrations in the upper troposphere (UT) between 8 and 15 km altitude, with number densities (normalized to standard temperature and pressure) often exceeding those in the planetary boundary layer (PBL) by 1 or 2 orders of magnitude. The measurements were made during the German–Brazilian cooperative aircraft campaign ACRIDICON–CHUVA, where ACRIDICON stands for Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems and CHUVA is the acronym for Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (globalmore » precipitation measurement), on the German High Altitude and Long Range Research Aircraft (HALO). The campaign took place in September–October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with atmospheric trace gases, aerosol particles, and atmospheric radiation. Aerosol enhancements were observed consistently on all flights during which the UT was probed, using several aerosol metrics, including condensation nuclei (CN) and cloud condensation nuclei (CCN) number concentrations and chemical species mass concentrations. The UT particles differed sharply in their chemical composition and size distribution from those in the PBL, ruling out convective transport of combustion-derived particles from the boundary layer (BL) as a source. The air in the immediate outflow of deep convective clouds was depleted of aerosol particles, whereas strongly enhanced number concentrations of small particles (< 90 nm diameter) were found in UT regions that had experienced outflow from deep convection in the preceding 5–72 h. We also found elevated concentrations of larger (> 90 nm) particles in the UT, which consisted mostly of organic matter and nitrate and were very effective CCN. Our findings suggest a conceptual

Virtual Impactor for Sub-micron Aerosol Particles

NASA Astrophysics Data System (ADS)

Bolshakov, A. A.; Strawa, A. W.; Hallar, A. G.

2005-12-01

The objective of a virtual impactor is to separate out the larger particles in a flow from the smaller particles in such a way that both sizes of particles are available for sampling. A jet of particle-laden air is accelerated toward a collection probe so that a small gap exists between the acceleration nozzle and the probe. A vacuum is applied to deflect a major portion of the airstream away form the collection probe. Particles larger than a certain size have sufficient momentum so that they cross the deflected streamlines and enter the collection probe, whereas smaller particles follow the deflected streamlines. The result is that the collection probe will contain a higher concentration of larger particles than is in the initial airstream. Typically, virtual impactors are high-flow devices used to separate out particles greater than several microns in diameter. We have developed a special virtual impactor to concentrate aerosol particles of diameters between 0.5 to 1 micron for the purpose of calibrating the optical cavity ring-down instrument [1]. No similar virtual impactors are commercially available. In our design, we have exploited considerations described earlier [2-4]. Performance of our virtual impactor was evaluated in an experimental set-up using TSI 3076 nebulizer and TSI 3936 scanning mobility particle size spectrometer. Under experimental conditions optimized for the best performance of the virtual impactor, we were able to concentrate the 700-nm polystyrene particles no less than 15-fold. However, under experimental conditions optimized for calibrating our cavity ring-down instrument, a concentration factor attainable was from 4 to 5. During calibration experiments, maximum realized particle number densities were 190, 300 and 1600 cm-3 for the 900-nm, 700-nm and 500-nm spheres, respectively. This paper discusses the design of the impactor and laboratory studies verifying its performance. References: 1. A.W. Strawa, R. Castaneda, T. Owano, D.S. Baer

Sub 2 nm Particle Characterization in Systems with Aerosol Formation and Growth

NASA Astrophysics Data System (ADS)

Wang, Yang

Aerosol science and technology enable continual advances in material synthesis and atmospheric pollutant control. Among these advances, one important frontier is characterizing the initial stages of particle formation by real time measurement of particles below 2 nm in size. Sub 2 nm particles play important roles by acting as seeds for particle growth, ultimately determining the final properties of the generated particles. Tailoring nanoparticle properties requires a thorough understanding and precise control of the particle formation processes, which in turn requires characterizing nanoparticle formation from the initial stages. The knowledge on particle formation in early stages can also be applied in quantum dot synthesis and material doping. This dissertation pursued two approaches in investigating incipient particle characterization in systems with aerosol formation and growth: (1) using a high-resolution differential mobility analyzer (DMA) to measure the size distributions of sub 2 nm particles generated from high-temperature aerosol reactors, and (2) analyzing the physical and chemical pathways of aerosol formation during combustion. Part. 1. Particle size distributions reveal important information about particle formation dynamics. DMAs are widely utilized to measure particle size distributions. However, our knowledge of the initial stages of particle formation is incomplete, due to the Brownian broadening effects in conventional DMAs. The first part of this dissertation studied the applicability of high-resolution DMAs in characterizing sub 2 nm particles generated from high-temperature aerosol reactors, including a flame aerosol reactor (FLAR) and a furnace aerosol reactor (FUAR). Comparison against a conventional DMA (Nano DMA, Model 3085, TSI Inc.) demonstrated that the increased sheath flow rates and shortened residence time indeed greatly suppressed the diffusion broadening effect in a high-resolution DMA (half mini type). The incipient particle

FTIR Analysis of Functional Groups in Aerosol Particles

NASA Astrophysics Data System (ADS)

Shokri, S. M.; McKenzie, G.; Dransfield, T. J.

2012-12-01

Secondary organic aerosols (SOA) are suspensions of particulate matter composed of compounds formed from chemical reactions of organic species in the atmosphere. Atmospheric particulate matter can have impacts on climate, the environment and human health. Standardized techniques to analyze the characteristics and composition of complex secondary organic aerosols are necessary to further investigate the formation of SOA and provide a better understanding of the reaction pathways of organic species in the atmosphere. While Aerosol Mass Spectrometry (AMS) can provide detailed information about the elemental composition of a sample, it reveals little about the chemical moieties which make up the particles. This work probes aerosol particles deposited on Teflon filters using FTIR, based on the protocols of Russell, et al. (Journal of Geophysical Research - Atmospheres, 114, 2009) and the spectral fitting algorithm of Takahama, et al (submitted, 2012). To validate the necessary calibration curves for the analysis of complex samples, primary aerosols of key compounds (e.g., citric acid, ammonium sulfate, sodium benzoate) were generated, and the accumulated masses of the aerosol samples were related to their IR absorption intensity. These validated calibration curves were then used to classify and quantify functional groups in SOA samples generated in chamber studies by MIT's Kroll group. The fitting algorithm currently quantifies the following functionalities: alcohols, alkanes, alkenes, amines, aromatics, carbonyls and carboxylic acids.

Deposition flux of aerosol particles and 15 polycyclic aromatic hydrocarbons in the North China Plain.

PubMed

Wang, Xilong; Liu, Shuzhen; Zhao, Jingyu; Zuo, Qian; Liu, Wenxin; Li, Bengang; Tao, Shu

2014-04-01

The present study examined deposition fluxes of aerosol particles and 15 polycyclic aromatic hydrocarbons (PAHs) associated with the particles in the North China Plain. The annual mean deposition fluxes of aerosol particles and 15 PAHs were 0.69 ± 0.46 g/(m(2) ×d) and 8.5 ± 6.2 μg/(m(2) ×d), respectively. Phenanthrene, fluoranthene, pyrene, chrysene, benzo[b]fluoranthene, and benzo[k]fluoranthene were the dominant PAHs bound to deposited aerosol particles throughout the year. The total concentration of 15 PAHs in the deposited aerosol particles was the highest in winter but lowest in spring. The highest PAH concentration in the deposited aerosol particles in winter was because the heating processes highly increased the concentration in atmospheric aerosol particles. Low temperature and weak sunshine in winter reduced the degradation rate of deposited aerosol particle-bound PAHs, especially for those with low molecular weight. The lowest PAH concentration in deposited aerosol particles in spring resulted from the frequently occurring dust storms, which diluted PAH concentrations. The mean deposition flux of PAHs with aerosol particles in winter (16 μg/[m(2) ×d]) reached 3 times to 5 times that in other seasons (3.5-5.0 μg/[m(2) ×d]). The spatial variation of the deposition flux of PAHs with high molecular weight (e.g., benzo[a]pyrene) was consistent with their concentrations in the atmospheric aerosol particles, whereas such a phenomenon was not observed for those with low molecular weight (e.g., phenanthrene) because of their distinct hydrophobicity, Henry's law constant, and the spatially heterogeneous meteorological conditions. © 2013 SETAC.

Formation of highly porous aerosol particles by atmospheric freeze-drying in ice clouds

PubMed Central

Adler, Gabriela; Koop, Thomas; Haspel, Carynelisa; Taraniuk, Ilya; Moise, Tamar; Koren, Ilan; Heiblum, Reuven H.; Rudich, Yinon

2013-01-01

The cycling of atmospheric aerosols through clouds can change their chemical and physical properties and thus modify how aerosols affect cloud microphysics and, subsequently, precipitation and climate. Current knowledge about aerosol processing by clouds is rather limited to chemical reactions within water droplets in warm low-altitude clouds. However, in cold high-altitude cirrus clouds and anvils of high convective clouds in the tropics and midlatitudes, humidified aerosols freeze to form ice, which upon exposure to subsaturation conditions with respect to ice can sublimate, leaving behind residual modified aerosols. This freeze-drying process can occur in various types of clouds. Here we simulate an atmospheric freeze-drying cycle of aerosols in laboratory experiments using proxies for atmospheric aerosols. We find that aerosols that contain organic material that undergo such a process can form highly porous aerosol particles with a larger diameter and a lower density than the initial homogeneous aerosol. We attribute this morphology change to phase separation upon freezing followed by a glass transition of the organic material that can preserve a porous structure after ice sublimation. A porous structure may explain the previously observed enhancement in ice nucleation efficiency of glassy organic particles. We find that highly porous aerosol particles scatter solar light less efficiently than nonporous aerosol particles. Using a combination of satellite and radiosonde data, we show that highly porous aerosol formation can readily occur in highly convective clouds, which are widespread in the tropics and midlatitudes. These observations may have implications for subsequent cloud formation cycles and aerosol albedo near cloud edges. PMID:24297908

Formation of highly porous aerosol particles by atmospheric freeze-drying in ice clouds.

PubMed

Adler, Gabriela; Koop, Thomas; Haspel, Carynelisa; Taraniuk, Ilya; Moise, Tamar; Koren, Ilan; Heiblum, Reuven H; Rudich, Yinon

2013-12-17

The cycling of atmospheric aerosols through clouds can change their chemical and physical properties and thus modify how aerosols affect cloud microphysics and, subsequently, precipitation and climate. Current knowledge about aerosol processing by clouds is rather limited to chemical reactions within water droplets in warm low-altitude clouds. However, in cold high-altitude cirrus clouds and anvils of high convective clouds in the tropics and midlatitudes, humidified aerosols freeze to form ice, which upon exposure to subsaturation conditions with respect to ice can sublimate, leaving behind residual modified aerosols. This freeze-drying process can occur in various types of clouds. Here we simulate an atmospheric freeze-drying cycle of aerosols in laboratory experiments using proxies for atmospheric aerosols. We find that aerosols that contain organic material that undergo such a process can form highly porous aerosol particles with a larger diameter and a lower density than the initial homogeneous aerosol. We attribute this morphology change to phase separation upon freezing followed by a glass transition of the organic material that can preserve a porous structure after ice sublimation. A porous structure may explain the previously observed enhancement in ice nucleation efficiency of glassy organic particles. We find that highly porous aerosol particles scatter solar light less efficiently than nonporous aerosol particles. Using a combination of satellite and radiosonde data, we show that highly porous aerosol formation can readily occur in highly convective clouds, which are widespread in the tropics and midlatitudes. These observations may have implications for subsequent cloud formation cycles and aerosol albedo near cloud edges.

Scattering of aerosol particles by a Hermite-Gaussian beam in marine atmosphere.

PubMed

Huang, Qingqing; Cheng, Mingjian; Guo, Lixin; Li, Jiangting; Yan, Xu; Liu, Songhua

2017-07-01

Based on the complex-source-point method and the generalized Lorenz-Mie theory, the scattering properties and polarization of aerosol particles by a Hermite-Gaussian (HG) beam in marine atmosphere is investigated. The influences of beam mode, beam width, and humidity on the scattered field are analyzed numerically. Results indicate that when the number of HG beam modes u (v) increase, the radar cross section of aerosol particles alternating appears at maximum and minimum values in the forward and backward scattering, respectively, because of the special petal-shaped distribution of the HG beam. The forward and backward scattering of aerosol particles decreases with the increase in beam waist. When beam waist is less than the radius of the aerosol particle, a minimum value is observed in the forward direction. The scattering properties of aerosol particles by the HG beam are more sensitive to the change in relative humidity compared with those by the plane wave and the Gaussian beam (GB). The HG beam shows superiority over the plane wave and the GB in detecting changes in the relative humidity of marine atmosphere aerosol. The effects of relative humidity on the polarization of the HG beam have been numerically analyzed in detail.

A Micro Aerosol Sensor for the Measurement of Airborne Ultrafine Particles.

PubMed

Zhang, Chao; Zhu, Rong; Yang, Wenming

2016-03-18

Particle number concentration and particle size are the two key parameters used to characterize exposure to airborne nanoparticles or ultrafine particles that have attracted the most attention. This paper proposes a simple micro aerosol sensor for detecting the number concentration and particle size of ultrafine particles with diameters from 50 to 253 nm based on electrical diffusion charging. The sensor is composed of a micro channel and a couple of planar electrodes printed on two circuit boards assembled in parallel, which thus integrate charging, precipitating and measurement elements into one chip, the overall size of which is 98 × 38 × 25 mm³. The experiment results demonstrate that the sensor is useful for measuring monodisperse aerosol particles with number concentrations from 300 to 2.5 × 10⁴ /cm³ and particle sizes from 50 to 253 nm. The aerosol sensor has a simple structure and small size, which is favorable for use in handheld devices.

A Micro Aerosol Sensor for the Measurement of Airborne Ultrafine Particles

PubMed Central

Zhang, Chao; Zhu, Rong; Yang, Wenming

2016-01-01

Particle number concentration and particle size are the two key parameters used to characterize exposure to airborne nanoparticles or ultrafine particles that have attracted the most attention. This paper proposes a simple micro aerosol sensor for detecting the number concentration and particle size of ultrafine particles with diameters from 50 to 253 nm based on electrical diffusion charging. The sensor is composed of a micro channel and a couple of planar electrodes printed on two circuit boards assembled in parallel, which thus integrate charging, precipitating and measurement elements into one chip, the overall size of which is 98 × 38 × 25 mm3. The experiment results demonstrate that the sensor is useful for measuring monodisperse aerosol particles with number concentrations from 300 to 2.5 × 104 /cm3 and particle sizes from 50 to 253 nm. The aerosol sensor has a simple structure and small size, which is favorable for use in handheld devices. PMID:26999156

Morphology and Optical Properties of Mixed Aerosol Particles

NASA Astrophysics Data System (ADS)

Fard, Mehrnoush M.; Krieger, Ulrich; Rudich, Yinon; Marcolli, Claudia; Peter, Thomas

2015-04-01

Experiments and modeling studies have shown that deliquesced aerosols can be present not only as one-phase system containing organics, inorganic salts and water, but often as two-phase systems consisting of a predominantly organic and a predominantly inorganic aqueous phase 1,2. Recent laboratory studies conducted with model mixtures representing tropospheric aerosols1,2,3, secondary organic aerosol (SOA) from smog chamber experiments4, and field measurements5 suggest that liquid- liquid phase separations (LLPS) is indeed a common phenomenon in mixed organic/ ammonium sulfate (AS) particles. During LLPS, particles may adopt different morphologies mainly core- shell and partially engulfed. A core- shell configuration will have consequences for heterogeneous chemistry and hygroscopicity and as a result will alter the optical properties of the particles since the aqueous inorganic-rich phase will be totally enclosed by a probably highly viscous organic coating with low diffusivity for reactants and water. The primary objective of this project is to establish a method for investigating the morphology of mixed inorganic and absorbing organic compounds of atmospheric relevance and study their radiative properties before, during, and after phase transitions mainly during LLPS. This will be the first study looking into the radiative effect of LLPS in detail. In this first experiment, the behavior of single droplets of carminic acid (CA)/ AS/ H2O mixture was monitored during relative humidity (RH) cycles using optical microscopy. The same mixture particle was levitated in an electrodynamic balance (EDB) and the change in its absorption properties was measured at varying RH. We also intend to determine the occurrence of LLPS in accumulation- sized particles and the change in their absorption using a cavity ring down aerosol spectrometer. If LLPS alters the absorptive properties of the suggested model aerosols significantly, absorption measurements of accumulation mode

Polyhexamethylene guanidine phosphate aerosol particles induce pulmonary inflammatory and fibrotic responses.

PubMed

Kim, Ha Ryong; Lee, Kyuhong; Park, Chang We; Song, Jeong Ah; Shin, Da Young; Park, Yong Joo; Chung, Kyu Hyuck

2016-03-01

Polyhexamethylene guanidine (PHMG) phosphate was used as a disinfectant for the prevention of microorganism growth in humidifiers, without recognizing that a change of exposure route might cause significant health effects. Epidemiological studies reported that the use of humidifier disinfectant containing PHMG-phosphate can provoke pulmonary fibrosis. However, the pulmonary toxicity of PHMG-phosphate aerosol particles is unknown yet. This study aimed to elucidate the toxicological relationship between PHMG-phosphate aerosol particles and pulmonary fibrosis. An in vivo nose-only exposure system and an in vitro air-liquid interface (ALI) co-culture model were applied to confirm whether PHMG-phosphate induces inflammatory and fibrotic responses in the respiratory tract. Seven-week-old male Sprague-Dawley rats were exposed to PHMG-phosphate aerosol particles for 3 weeks and recovered for 3 weeks in a nose-only exposure chamber. In addition, three human lung cells (Calu-3, differentiated THP-1 and HMC-1 cells) were cultured at ALI condition for 12 days and were treated with PHMG-phosphate at set concentrations and times. The reactive oxygen species (ROS) generation, airway barrier injuries and inflammatory and fibrotic responses were evaluated in vivo and in vitro. The rats exposed to PHMG-phosphate aerosol particles in nanometer size showed pulmonary inflammation and fibrosis including inflammatory cytokines and fibronectin mRNA increase, as well as histopathological changes. In addition, PHMG-phosphate triggered the ROS generation, airway barrier injuries and inflammatory responses in a bronchial ALI co-culture model. Those results demonstrated that PHMG-phosphate aerosol particles cause pulmonary inflammatory and fibrotic responses. All features of fibrogenesis by PHMG-phosphate aerosol particles closely resembled the pathology of fibrosis that was reported in epidemiological studies. Finally, we expected that PHMG-phosphate infiltrated into the lungs in the form of

Morphologies of aerosol particles consisting of two liquid phases

NASA Astrophysics Data System (ADS)

Song, Mijung; Marcolli, Claudia; Krieger, Ulrich; Peter, Thomas

2013-04-01

Recent studies have shown that liquid-liquid phase separation (LLPS) might be a common feature in mixed organic/ammonium sulfate (AS)/H2O particles. Song et al. (2012) observed that in atmospheric relevant organic/AS/H2O mixtures LLPS always occurred for organic aerosol compositions with O:C < 0.56, depended on the specific functional groups of organics in the range of 0.56 < O:C < 0.80 and never appeared for O:C > 0.80. The composition of the organic fraction and the mixing state of aerosol particles may influence deliquescence relative humidity (DRH) and efflorescence relative humidity (ERH) of inorganic salts during RH cycles and also aerosol morphology. In order to determine how the deliquescence and efflorescence of AS in mixed organic/AS/H2O particles is influenced by LLPS and to identify the corresponding morphologies of the particles, we subjected organic/AS/H2O particles deposited on a hydrophobically coated substrate to RH cycles and observed the phase transitions using optical microscopy and Raman spectroscopy. In this study, we report results from 21 organic/AS/H2O systems with O:C ranging from 0.55 - 0.85 covering aliphatic and aromatic oxidized compounds. Eight systems did not show LLPS for all investigated organic-to-inorganic ratios, nine showed core-shell morphology when present in a two-liquid-phases state and four showed both, core-shell or partially engulfed configurations depending on the organic-to-inorganic ratio. While AS in aerosol particles with complete LLPS showed almost constant values of ERH = 44 ± 4 % and DRH = 77 ± 2 %, a strong reduction or complete inhibition of efflorescence occurred for mixtures that did not exhibit LLPS. To confirm these findings, we performed supplementary experiments on levitated particles in an electrodynamic balance and compared surface and interfacial tensions of the investigated mixtures. Reference Song, M., C. Marcolli, U. K. Krieger, A. Zuend, and T. Peter (2012), Liquid-liquid phase separation in

Chemical evolution of multicomponent aerosol particles during evaporation

NASA Astrophysics Data System (ADS)

Zardini, Alessandro; Riipinen, Ilona; Pagels, Joakim; Eriksson, Axel; Worsnop, Douglas; Switieckli, Erik; Kulmala, Markku; Bilde, Merete

2010-05-01

Atmospheric aerosol particles have an important but not well quantified effect on climate and human health. Despite the efforts made in the last decades, the formation and evolution of aerosol particles in the atmosphere is still not fully understood. The uncertainty is partly due to the complex chemical composition of the particles which comprise inorganic and organic compounds. Many organics (like dicarboxylic acids) can be present both in the gas and in the condensed phase due to their low vapor pressure. Clearly, an understanding of this partition is crucial to address any other issue in atmospheric physics and chemistry. Moreover, many organics are water soluble, and their influence on the properties of aqueous solution droplets is still poorly characterized. The solid and sub-cooled liquid state vapor pressures of some organic compounds have been previously determined by measuring the evaporation rate of single-compound crystals [1-3] or binary aqueous droplets [4-6]. In this work, we deploy the HTDMA technique (Hygroscopicity Tandem Differential Mobility Analyzer) coupled with a 3.5m laminar flow-tube and an Aerosol Mass Spectrometer (AMS) for determining the chemical evolution during evaporation of ternary droplets made of one dicarboxylic acid (succinic acid, commonly found in atmospheric samples) and one inorganic compound (sodium chloride or ammonium sulfate) in different mixing ratios, in equilibrium with water vapor at a fixed relative humidity. In addition, we investigate the evaporation of multicomponent droplets and crystals made of three organic species (dicarboxylic acids and sugars), of which one or two are semi-volatile. 1. Bilde M. and Pandis, S.N.: Evaporation Rates and Vapor Pressures of Individual Aerosol Species Formed in the Atmospheric Oxidation of alpha- and beta-Pinene. Environmental Science and Technology, 35, 2001. 2. Bilde M., et al.: Even-Odd Alternation of Evaporation Rates and Vapor Pressures of C3-C9 Dicarboxylic Acid Aerosols

Aerosol optical properties in the southeastern United States in summer - Part 1: Hygroscopic growth

NASA Astrophysics Data System (ADS)

Brock, C. A.; Wagner, N. L.; Anderson, B. E.; Attwood, A. R.; Beyersdorf, A.; Campuzano-Jost, P.; Carlton, A. G.; Day, D. A.; Diskin, G. S.; Gordon, T. D.; Jimenez, J. L.; Lack, D. A.; Liao, J.; Markovic, M. Z.; Middlebrook, A. M.; Ng, N. L.; Perring, A. E.; Richardson, M. S.; Schwarz, J. P.; Washenfelder, R. A.; Welti, A.; Xu, L.; Ziemba, L. D.; Murphy, D. M.

2015-09-01

Aircraft observations of meteorological, trace gas, and aerosol properties were made during May-September 2013 in the southeastern United States (US) under fair-weather, afternoon conditions with well-defined planetary boundary layer structure. Optical extinction at 532 nm was directly measured at three relative humidities and compared with extinction calculated from measurements of aerosol composition and size distribution using the κ-Köhler approximation for hygroscopic growth. Using this approach, the hygroscopicity parameter κ for the organic fraction of the aerosol must have been < 0.10 to be consistent with 75 % of the observations within uncertainties. This subsaturated κ value for the organic aerosol in the southeastern US is consistent with several field studies in rural environments. We present a new parameterization of the change in aerosol extinction as a function of relative humidity that better describes the observations than does the widely used power-law (gamma, γ) parameterization. This new single-parameter κext formulation is based upon κ-Köhler and Mie theories and relies upon the well-known approximately linear relationship between particle volume (or mass) and optical extinction (Charlson et al., 1967). The fitted parameter, κext, is nonlinearly related to the chemically derived κ parameter used in κ-Köhler theory. The values of κext we determined from airborne measurements are consistent with independent observations at a nearby ground site.

Composition and formation of organic aerosol particles in the Amazon

NASA Astrophysics Data System (ADS)

Pöhlker, C.; Wiedemann, K.; Sinha, B.; Shiraiwa, M.; Gunthe, S. S.; Artaxo, P.; Gilles, M. K.; Kilcoyne, A. L. D.; Moffet, R. C.; Smith, M.; Weigand, M.; Martin, S. T.; Pöschl, U.; Andreae, M. O.

2012-04-01

We applied scanning transmission X-ray microscopy with near edge X-ray absorption fine structure (STXM-NEXAFS) analysis to investigate the morphology and chemical composition of aerosol samples from a pristine tropical environment, the Amazon Basin. The samples were collected in the Amazonian rainforest during the rainy season and can be regarded as a natural background aerosol. The samples were found to be dominated by secondary organic aerosol (SOA) particles in the fine and primary biological aerosol particles (PBAP) in the coarse mode. Lab-generated SOA-samples from isoprene and terpene oxidation as well as pure organic compounds from spray-drying of aqueous solution were measured as reference samples. The aim of this study was to investigate the microphysical and chemical properties of a tropical background aerosol in the submicron size range and its internal mixing state. The lab-generated SOA and pure organic compounds occurred as spherical and mostly homogenous droplet-like particles, whereas the Amazonian SOA particles comprised a mixture of homogeneous droplets and droplets having internal structures due to atmospheric aging. In spite of the similar morphological appearance, the Amazon samples showed considerable differences in elemental and functional group composition. According to their NEXAFS spectra, three chemically distinct types of organic material were found and could be assigned to the following three categories: (1) particles with a pronounced carboxylic acid (COOH) peak similar to those of laboratory-generated SOA particles from terpene oxidation; (2) particles with a strong hydroxy (COH) signal similar to pure carbohydrate particles; and (3) particles with spectra resembling a mixture of the first two classes. In addition to the dominant organic component, the NEXAFS spectra revealed clearly resolved potassium (K) signals for all analyzed particles. During the rainy season and in the absence of anthropogenic influence, active biota is

Source apportionment of lead-containing aerosol particles in Shanghai using single particle mass spectrometry.

PubMed

Zhang, Yaping; Wang, Xiaofei; Chen, Hong; Yang, Xin; Chen, Jianmin; Allen, Jonathan O

2009-01-01

Lead (Pb) in individual aerosol particles was measured using single particle aerosol mass spectrometer (ATOFMS) in the summer of 2007 in Shanghai, China. Pb was found in 3% of particles with diameters in the range 0.1-2.0 microm. Single particle data were analyzed focusing on the particles with high Pb content which were mostly submicron. Using the ART-2a neural network algorithm, these fine Pb-rich particles were classified into eight main classes by their mass spectral patterns. Based on the size distribution, temporal variation of number density, chemical composition and the correlation between different chemical species for each class, three major emission sources were identified. About 45% of the Pb-rich particles contained organic or elemental carbon and were attributed to the emission from coal combustion; particles with good correlation between Cl and Pb content were mostly attributed to waste incineration. One unique class of particles was identified by strong phosphate and Pb signals, which were assigned to emissions from phosphate industry. Other Pb-rich particles included aged sea salt and particles from metallurgical processes.

Crystallization pathways of sulfate-nitrate-ammonium aerosol particles.

PubMed

Schlenker, Julie C; Martin, Scot T

2005-11-10

Crystallization experiments are conducted for aerosol particles composed of aqueous mixtures of (NH(4))(2)SO(4)(aq) and NH(4)NO(3)(aq), (NH(4))(2)SO(4)(aq) and NH(4)HSO(4)(aq), and NH(4)NO(3)(aq) and NH(4)HSO(4)(aq). Depending on the aqueous composition, crystals of (NH(4))(2)SO(4)(s), (NH(4))(3)H(SO(4))(2)(s), NH(4)HSO(4)(s), NH(4)NO(3)(s), 2NH(4)NO(3) x (NH(4))(2)SO(4)(s), and 3NH(4)NO(3) x (NH(4))(2)SO(4)(s) are formed. Although particles of NH(4)NO(3)(aq) and NH(4)HSO(4)(aq) do not crystallize even at 1% relative humidity, additions of 0.05 mol fraction SO(4)(2-)(aq) or NO(3)(-)(aq) ions promote crystallization, respectively. 2NH(4)NO(3) x (NH(4))(2)SO(4)(s) and (NH(4))(3)H(SO(4))(2)(s) appear to serve as good heterogeneous nuclei for NH(4)NO(3)(s) and NH(4)HSO(4)(s), respectively. 2NH(4)NO(3) x (NH(4))(2)SO(4)(s) crystallizes over a greater range of aqueous compositions than 3NH(4)NO(3) x (NH(4))(2)SO(4)(s). An infrared aerosol spectrum is provided for each solid based upon a linear decomposition analysis of the recorded spectra. Small nonzero residuals occur in the analysis because aerosol spectra depend on particle morphology, which changes slightly across the range of compositions studied. In addition, several of the mixed compositions crystallize with residual aqueous water of up to 5% particle mass. We attribute this water content to enclosed water pockets. The results provide further insights into the nonlinear crystallization pathways of sulfate-nitrate-ammonium aerosol particles.

Inversion of solar extinction data from the Apollo-Soyuz Test Project Stratospheric Aerosol Measurement (ASTP/SAM) experiment

NASA Technical Reports Server (NTRS)

Pepin, T. J.

1977-01-01

The inversion methods are reported that have been used to determine the vertical profile of the extinction coefficient due to the stratospheric aerosols from data measured during the ASTP/SAM solar occultation experiment. Inversion methods include the onion skin peel technique and methods of solving the Fredholm equation for the problem subject to smoothing constraints. The latter of these approaches involves a double inversion scheme. Comparisons are made between the inverted results from the SAM experiment and near simultaneous measurements made by lidar and balloon born dustsonde. The results are used to demonstrate the assumptions required to perform the inversions for aerosols.

Global distribution of secondary organic aerosol particle phase state

NASA Astrophysics Data System (ADS)

Shiraiwa, M.; Li, Y., Sr.; Tsimpidi, A.; Karydis, V.; Berkemeier, T.; Pandis, S. N.; Lelieveld, J.; Koop, T.; Poeschl, U.

2016-12-01

Secondary organic aerosols (SOA) account for a large fraction of submicron particles in the atmosphere and play a key role in aerosol effects on climate, air quality and public health. The formation and aging of SOA proceed through multiple steps of chemical reaction and mass transport in the gas and particle phases, which is challenging for the interpretation of field measurements and laboratory experiments as well as accurate representation of SOA evolution in atmospheric aerosol models. SOA particles can adopt liquid, semi-solid and amorphous solid (glassy) phase states depending on chemical composition, relative humidity and temperature. The particle phase state is crucial for various atmospheric gas-particle interactions, including SOA formation, heterogeneous and multiphase reactions and ice nucleation. We found that organic compounds with a wide variety of functional groups fall into molecular corridors, characterized by a tight inverse correlation between molar mass and volatility. Based on the concept of molecular corridors, we develop a method to estimate glass transition temperatures based on the molar mass and molecular O:C ratio of SOA components, which is a key property for determination of particle phase state. We use the global chemistry climate model EMAC with the organic aerosol module ORACLE to predict the atmospheric SOA phase state. For the planetary boundary layer, global simulations indicate that SOA is mostly liquid in tropical and polar air with high relative humidity, semi-solid in the mid-latitudes, and solid over dry lands. We find that in the middle and upper troposphere (>500 hPa) SOA should be mostly in a glassy solid phase state. Thus, slow diffusion of water, oxidants, and organic molecules could kinetically limit gas-particle interactions of SOA in the free and upper troposphere, promote ice nucleation and facilitate long-range transport of reactive and toxic organic pollutants embedded within SOA.

Total particle, sulfate, and acidic aerosol emissions from kerosene space heaters

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

Leaderer, B.P.; Boone, P.M.; Hammond, S.K.

1990-06-01

Chamber studies were conducted on four unvented kerosene space heaters to assess emissions of total particle, sulfate, and acidic aerosol. The heaters tested represented four burner designs currently in use by the public. Kerosene space heaters are a potential source of fine particles ({<=} 2.5-{mu}m diameter), sulfate, and acidic aerosol indoors. Fine particle concentrations in homes in which the heaters are used may be increased in excess of 20 {mu}g/m{sup 3} over background levels. Sulfate and acidic aerosol levels in such homes could exceed average and peak outdoor concentrations. Maltuned heaters could produce exceptionally high levels of all air contaminantsmore » measured.« less

Total particle, sulfate, and acidic aerosol emissions from kerosene space heaters

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

Leaderer, B.P.; Boone, P.M.; Hammond, S.K.

1990-01-01

The article discusses chamber studies of four unvented kerosene space heaters to assess emissions of total particle, sulfate, and acidic aerosol. The heaters tested represented four burner designs currently in use by the public. Kerosene space heaters are a potential source of fine particles (= or < 2.5 micrometer diameter), sulfate, and acidic aerosol indoors. Fine particle concentrations in houses in which the heaters are used may be increased in excess of 20 micrograms/m3 over background levels. Sulfate and acidic aerosol levels in such houses could exceed average and peak outdoor concentrations. Maltuned heaters could produce exceptionally high levels ofmore » all air contaminants measured.« less

Single-particle characterization of urban aerosol particles collected in three Korean cites using low-Z electron probe X-ray microanalysis.

PubMed

Ro, Chul-Un; Kim, HyeKyeong; Oh, Keun-Young; Yea, Sun Kyung; Lee, Chong Bum; Jang, Meongdo; Van Grieken, René

2002-11-15

A recently developed single-particle analytical technique, called low-Z electron probe X-ray microanalysis (low-Z EPMA), was applied to characterize urban aerosol particles collected in three cities of Korea (Seoul, CheongJu, and ChunCheon) on single days in the winter of 1999. In this study, it is clearly demonstrated that the low-Z EPMA technique can provide detailed and quantitative information on the chemical composition of particles in the urban atmosphere. The collected aerosol particles were analyzed and classified on the basis of their chemical species. Various types of particles were identified, such as soil-derived, carbonaceous, marine-originated, and anthropogenic particles. In the sample collected in Seoul, carbonaceous, aluminosilicates, silicon dioxide, and calcium carbonate aerosol particles were abundantly encountered. In the CheongJu and ChunCheon samples, carbonaceous, aluminosilicates, reacted sea salts, and ammonium sulfate aerosol particles were often seen. However, in the CheongJu sample, ammonium sulfate particles were the most abundant in the fine fraction. Also, calcium sulfate and nitrate particles were significantly observed. In the ChunCheon sample, organic particles were the most abundant in the fine fraction. Also, sodium nitrate particles were seen at high levels. The ChunCheon sample seemed to be strongly influenced by sea-salt aerosols originating from the Yellow Sea, which is located about 115 km away from the city.

Formation of Oxidized Organic Aerosol (OOA) through Fog Processing in the Po Valley

NASA Astrophysics Data System (ADS)

Gilardoni, S.; Paglione, M.; Rinaldi, M.; Giulianelli, L.; Massoli, P.; Hillamo, R. E.; Carbone, S.; Lanconelli, C.; Laaksonen, A. J.; Russell, L. M.; Poluzzi, V.; Fuzzi, S.; Facchini, C.

2014-12-01

Aqueous phase chemistry might be responsible for the formation of a significant fraction of the organic aerosol (OA) observed in the atmosphere, and could explain some of the discrepancies between OA concentration and properties predicted by models and observed in the environment. Aerosol - fog interaction and its effect on submicron aerosol properties were investigated in the Po Valley (northern Italy) during fall 2011, in the framework of the Supersite project (ARPA Emilia Romagna). Composition and physical properties of submicron aerosol were measured online by a High Resolution- Time of Flight - Aerosol Mass Spectrometer (HR-TOF-AMS), a Soot Photometer - Aerosol Mass Spectrometer (SP-AMS), and a Tandem Differential Mobility Particle Sizer (TDMPS). Organic functional group analysis was performed off-line by Hydrogen - Nuclear Magnetic Resonance (H-NMR) spectrometry and by Fourier Transform Infrared (FTIR) spectrometry. Aerosol absorption, scattering, and total extinction were measured simultaneously with a Particle Soot Absorption Photometer (PSAP), a Nephelometer, and a Cavity Attenuated Phase Shift Spectrometer particle extinction monitor (CAPS PMex), respectively. Water-soluble organic carbon in fog-water was characterized off-line by HR-TOF-AMS. Fourteen distinct fog events were observed. Fog dissipation left behind an aerosol enriched in particles larger than 400 nm, typical of fog and cloud processing, and dominated by secondary species, including ammonium nitrate, ammonium sulfate and oxidized OA (OOA). Source apportionment of OA allowed us to identify OOA as the difference between total OA and primary OA (hydrocarbon like OA and biomass burning OA). The formation of OOA through fog processing is proved by the correlation of OOA concentration with hydroxyl methyl sulfonate signal and by the similarity of OOA spectra with organic mass spectra obtained by re-aerosolization of fog water samples. The oxygen to carbon ratio and the hydrogen to carbon ratio of

Morphology and Optical Properties of Mixed Aerosol Particles

NASA Astrophysics Data System (ADS)

Fard, Mehrnoush M.; Krieger, Ulrich; Rudich, Yinon; Marcolli, Claudia; Peter, Thomas

2016-04-01

Experiments and modeling studies have shown that deliquesced aerosols can exist not only as one-phase system containing organics, inorganic salts and water, but often as two-phase systems consisting of a predominantly organic and a predominantly inorganic aqueous phase (1,2). Recent laboratory studies conducted with model mixtures representing tropospheric aerosols (1,2,3), secondary organic aerosol (SOA) from smog chamber experiments (4), and field measurements (5) suggest that liquid-liquid phase separations (LLPS) is indeed a common phenomenon in mixed organic/ inorganic particles. During LLPS, particles may adopt different morphologies mainly core-shell and partially engulfed. A core-shell configuration will have consequences for heterogeneous chemistry and hygroscopicity and as a result will alter the optical properties of the particles in particular for organic phases containing absorbing molecules, e.g. brown carbon. The primary objective of this project is to establish a method for investigating the morphology of mixed inorganic and absorbing organic compounds of atmospheric relevance and study their radiative properties before, during, and after phase transitions mainly during LLPS. This will be the first study looking into the radiative effect of LLPS in detail. Our ternary model system consist of ammonium sulfate (AS)/ Polyethylene Glycol (PEG)/ and water (H2O). Carminic acid (CA) was added as a proxy for an absorbing organic compound to the system. The behavior of single droplets of above ternary mixture was monitored during relative humidity (RH) cycles using optical microscopy. The same ternary mixture particle was levitated in an electrodynamic balance (EDB) and the change in its absorption properties was measured at varying RH. In addition, Mie-code modeling is used to predict the absorption efficiency of the same ternary system and the result will be compared with the data obtained from EDB experiment. We also intend to determine the occurrence of

Wintertime water-soluble aerosol composition and particle water content in Fresno, California

NASA Astrophysics Data System (ADS)

Parworth, Caroline L.; Young, Dominique E.; Kim, Hwajin; Zhang, Xiaolu; Cappa, Christopher D.; Collier, Sonya; Zhang, Qi

2017-03-01

The composition and concentrations of water-soluble gases and ionic aerosol components were measured from January to February 2013 in Fresno, CA, with a particle-into-liquid sampler with ion chromatography and annular denuders. The average (±1σ) ionic aerosol mass concentration was 15.0 (±9.4) µg m-3, and dominated by nitrate (61%), followed by ammonium, sulfate, chloride, potassium, nitrite, and sodium. Aerosol-phase organic acids, including formate and glycolate, and amines including methylaminium, triethanolaminium, ethanolaminium, dimethylaminium, and ethylaminium were also detected. Although the dominant species all came from secondary aerosol formation, there were primary sources of ionic aerosols as well, including biomass burning for potassium and glycolate, sea spray for sodium, chloride, and dimethylamine, and vehicles for formate. Particulate methanesulfonic acid was also detected and mainly associated with terrestrial sources. On average, the molar concentration of ammonia was 49 times greater than nitric acid, indicating that ammonium nitrate formation was limited by nitric acid availability. Particle water was calculated based on the Extended Aerosol Inorganics Model (E-AIM) thermodynamic prediction of inorganic particle water and κ-Köhler theory approximation of organic particle water. The average (±1σ) particle water concentration was 19.2 (±18.6) µg m-3, of which 90% was attributed to inorganic species. The fractional contribution of particle water to total fine particle mass averaged at 36% during this study and was greatest during early morning and night and least during the day. Based on aqueous-phase concentrations of ions calculated by using E-AIM, the average (±1σ) pH of particles in Fresno during the winter was estimated to be 4.2 (±0.2).

Aerosol Abundances and Optical Characteristics in the Pacific Basin Free Troposphere

NASA Technical Reports Server (NTRS)

Pueschel, R. F.; Livingston, J. M.; Ferry, G. V.; deFelice, T. E.

1994-01-01

During NASA's Global Backscatter Experiment (GLOBE) mission flights in November 1989 and May 1990, a DC-8 research aircraft probed the Pacific Basin free troposphere for about 90 flight hours in each month between +72 and -62 degrees latitude, +130 and -120 degrees longitude, and up to 39,000 feet pressure altitudes. Aerosols were sampled continuously in situ by optical particle counters to measure concentration and particle size, and during 48 10-min intervals during each mission by wire impactors for concentration, size, composition, phase and shape analyses. The optical particle counters cover a particle diameter range between 0.3 and 20 microns; wire impactors extend the range down to 0.03 microns. Results of particle number, size, shape, together with the assumption of a refractive index corresponding to (NH4)2SO4 to account for the prevalence of aerosol sulfur, were utilized in a Mie algorithm to calculate aerosol extinction and backscatter for a range of wavelengths (0.385 less than lambda less than 10.64 microns). Computations for 22 randomly selected size distributions yield coefficients of extinction E(0.525) = (2.03 +/- 1.20) x 10(exp -4) km(exp -1) and backscatter beta(0.525) = (6.45 +/- 3.49) x 10(exp -6) km(exp -1) sr(exp -1) in the visible, and E(10.64) = (8.13 +/- 6.47) x 10(exp -6) km(exp -1) and beta(10.64) = (9.98 +/- 10.69) x 10(exp -8) km(exp -1) sr(exp -1) in the infrared, respectively. Large particles (D greater than 0.3 microns) contribute two-thirds to the total extinction in the visible (lambda = 0.525 microns), and almost 100% in the infrared (lambda = 10.64 microns). These results have been used to define an IR optical aerosol climatology of the Pacific Basin free troposphere, from which it follows that the infrared backscatter coefficient at lambda = 9.25 microns wavelength fluctuates between 5.0 x 10(exp -10) and 2.0 x 10(exp -7) km(exp -1) sr(exp -1) with a modal value 2.0 x 10(exp -8) km(exp -1) sr(exp -1).

Adhesion of Mineral and Soot Aerosols can Strongly Affect their Scattering and Absorption Properties

NASA Technical Reports Server (NTRS)

Mishchenko, Michael I.; Dlugach, Jana M.

2012-01-01

We use the numerically exact superposition T-matrix method to compute the optical cross sections and the Stokes scattering matrix for polydisperse mineral aerosols (modeled as homogeneous spheres) covered with a large number of much smaller soot particles. These results are compared with the Lorenz-Mie results for a uniform external mixture of mineral and soot aerosols. We show that the effect of soot particles adhering to large mineral particles can be to change the extinction and scattering cross sections and the asymmetry parameter quite substantially. The effect on the phase function and degree of linear polarization can be equally significant.

Experimental demonstration that a free-falling aerosol particle obeys a fluctuation theorem

NASA Astrophysics Data System (ADS)

Wong, Chun-Shang; Goree, J.; Gopalakrishnan, Ranganathan

2018-05-01

We investigate the fluctuating motion of an aerosol particle falling in air. Using a Millikan-like setup, we tracked a 1-μ m sphere falling at its terminal velocity. We observe occurrences of particles undergoing upward displacements against the force of gravity, so that negative work is done briefly. These negative-work events have a probability that is shown to obey the work fluctuation theorem. This experimental confirmation of the theorem's applicability to aerosols leads us to develop and demonstrate an application: an in situ measurement of an aerosol particle's mass.

Novel Measurements of Aerosol Particle Interfaces Using Biphasic Microfluidics

NASA Astrophysics Data System (ADS)

Metcalf, A. R.; Dutcher, C. S.

2014-12-01

Secondary organic aerosol (SOA) particles are nearly ubiquitous in the atmosphere and yet there remains large uncertainties in their formation processes and ambient properties. These particles are complex microenvironments, which can contain multiple interfaces due to internal aqueous-organic phase partitioning and to the external liquid-vapor surface. These aerosol interfaces can profoundly affect the fate of condensable organic compounds emitted into the atmosphere by altering the way in which organic vapors interact with the ambient aerosol. Aerosol interfaces affect particle internal structure, species uptake, equilibrium partitioning, activation to cloud condensation or ice nuclei, and optical properties. For example, organic thin films can shield the core of the aerosol from the ambient environment, which may disrupt equilibrium partitioning and mass transfer. To improve our ability to accurately predict the fate of SOA in the atmosphere, we must improve our knowledge of aerosol interfaces and their interactions with the ambient environment. Few technologies exist to accurately probe aerosol interfaces at atmospherically-relevant conditions. In this talk, a novel method using biphasic microscale flows will be introduced for generating, trapping, and perturbing complex interfaces at atmospherically relevant conditions. These microfluidic experiments utilize high-speed imaging to monitor interfacial phenomena at the microscale and are performed with phase contrast and fluorescence microscopy on a temperature-controlled inverted microscope stage. From these experiments, interfacial thermodynamic properties such as surface tension, rheological properties such as interfacial moduli, and kinetic properties such as mass transfer coefficients can be measured or inferred. Chemical compositions of the liquid phases studied here span a range of viscosities and include electrolyte and water soluble organic acid species often observed in the atmosphere, such as mixtures

In Situ Single Particle Measurement of Atmospheric Aging of Carbonaceous Aerosols During CARES

NASA Astrophysics Data System (ADS)

Cahill, J. F.; Suski, K.; Hubbe, J.; Shilling, J.; Zaveri, R. A.; Springston, S. R.; Prather, K. A.

2011-12-01

Atmospheric aging of aerosols through photochemistry, heterogeneous reactions and aqueous processing can change their physical and chemical properties, impacting their gas uptake, radiative forcing, and activation of cloud nuclei. Understanding the timescale and magnitude of this aging process is essential for accurate aerosol-climate modeling and predictions. An aircraft aerosol time-of-flight mass spectrometer (A-ATOFMS) measured single particle mixing state during the Carbonaceous Aerosols and Radiative Effects Study (CARES) in the summer of 2010 over Sacramento, CA. On 6/23/10, flights in the morning and afternoon performed pseudo-Lagrangian sampling of the Sacramento urban plume. Carbonaceous particles from these flights were classified into 'aged' and 'fresh' classes based on their mixing state, with aged particles having more secondary species, such as nitrate and sulfate. In the morning flight, a clear decreasing trend in the ratio of fresh/aged particle types was seen as the flight progressed, whereas in the afternoon flight, the ratio was essentially constant. These data show that in the morning carbonaceous aerosols can become heavily oxidized in a few hours. Further analysis of particle mixing state and the timescale of carbonaceous aerosol aging will be presented

Impact of aerosol particle sources on optical properties in urban, regional and remote areas in the north-western Mediterranean

NASA Astrophysics Data System (ADS)

Ealo, Marina; Alastuey, Andrés; Pérez, Noemí; Ripoll, Anna; Querol, Xavier; Pandolfi, Marco

2018-01-01

Further research is needed to reduce the existing uncertainties on the effect that specific aerosol particle sources have on light extinction and consequently on climate. This study presents a new approach that aims to quantify the mass scattering and absorption efficiencies (MSEs and MAEs) of different aerosol sources at urban (Barcelona - BCN), regional (Montseny - MSY) and remote (Montsec - MSA) background sites in the north-western (NW) Mediterranean. An analysis of source apportionment to the measured multi-wavelength light scattering (σsp) and absorption (σap) coefficients was performed by means of a multilinear regression (MLR) model for the periods 2009-2014, 2010-2014 and 2011-2014 at BCN, MSY and MSA respectively. The source contributions to PM10 mass concentration, identified by means of the positive matrix factorization (PMF) model, were used as dependent variables in the MLR model. With this approach we addressed both the effect that aerosol sources have on air quality and their potential effect on light extinction through the determination of their MSEs and MAEs. An advantage of the presented approach is that the calculated MSEs and MAEs take into account the internal mixing of atmospheric particles. Seven aerosol sources were identified at MSA and MSY, and eight sources at BCN. Mineral, aged marine, secondary sulfate, secondary nitrate and V-Ni bearing sources were common at the three sites. Traffic, industrial/metallurgy and road dust resuspension sources were isolated at BCN, whereas mixed industrial/traffic and aged organics sources were identified at MSY and MSA. The highest MSEs were observed for secondary sulfate (4.5 and 10.7 m2 g-1, at MSY and MSA), secondary nitrate (8.8 and 7.8 m2 g-1) and V-Ni bearing source (8 and 3.5 m2 g-1). These sources dominated the scattering throughout the year with marked seasonal trends. The V-Ni bearing source, originating mainly from shipping in the area under study, simultaneously contributed to both �

A numerical determination of the evolution of cloud drop spectra due to condensation on natural aerosol particles

NASA Technical Reports Server (NTRS)

Lee, I. Y.; Haenel, G.; Pruppacher, H. R.

1980-01-01

The time variation in size of aerosol particles growing by condensation is studied numerically by means of an air parcel model which allows entrainment of air and aerosol particles. Particles of four types of aerosols typically occurring in atmospheric air masses were considered. The present model circumvents any assumption about the size distribution and chemical composition of the aerosol particles by basing the aerosol particle growth on actually observed size distributions and on observed amounts of water taken up under equilibrium by a deposit of the aerosol particles. Characteristic differences in the drop size distribution, liquid water content and supersaturation were found for the clouds which evolved from the four aerosol types considered.

Identifying Metals as Marker for Waste Burning Aerosol Particles in New Delhi

NASA Astrophysics Data System (ADS)

Kumar, Sudhanshu

2012-07-01

{Identifying Metals as Marker for Waste Burning Aerosol Particles in New Delhi } Tracing of aerosol sources is an important task helpful for making control strategy, and for climate change study. However, it is a difficult job as aerosols have several sources, involve in complex atmospheric processing, degradation and removal processes. Several approaches have been used for this task, e.g., models, which are based on the input of chemical species; stable- and radio-isotope compositions of certain species; chemical markers in which trace metals are the better options because they persist in atmosphere until the life of a particle. For example, K and Hg are used for biomass and coal burning tracings, respectively. Open waste burning has recently been believed to be a considerable source of aerosols in several mega cities in India and China. To better understand this source contribution in New Delhi aerosols, we have conducted aerosol sampling at a landfill site (Okhla), and in proximity (within 1 km distance) of this site. Aerosol filter samples were acid digested in microwave digestion system and analyzed using inductively coupled plasma -- high resolution mass spectrometry (ICP-HRMS) for getting metal signatures in particles. The metals, e.g., Sn, Sb and As those are found almost negligible in remote aerosols, are maximized in these waste burning aerosols. Sample collected in other location of New Delhi also shows the considerable presence of these metals in particles. Preliminary studies of isotopic ratios of these metals suggested that these metals, especially Sn can be used as marker for tracing the open waste burning sources of aerosols in New Delhi.

Endotoxin in Size-Separated Metal Working Fluid Aerosol Particles.

PubMed

Dahlman-Höglund, Anna; Lindgren, Åsa; Mattsby-Baltzer, Inger

2016-08-01

Patients with airway symptoms working in metal working industries are increasing, despite efforts to improve the environmental air surrounding the machines. Our aim was to analyse the amount of endotoxin in size-separated airborne particles of metal working fluid (MWF) aerosol, by using the personal sampler Sioutas cascade impactor, to compare filter types, and to compare the concentration of airborne endotoxin to that of the corresponding MWFs. In a pilot field study, aerosols were collected in two separate machine halls on totally 10 occasions, using glass fibre and polytetrafluoroethylene (PTFE) filters in parallel at each station. Airborne endotoxin was distributed over all size fractions. While a major part was found in the largest size fraction (72%, 2.5-10 µm), up to 8% of the airborne endotoxin was detected in the smallest size fraction (<0.25 µm). Comparing the efficiency of the filter types, a significantly higher median endotoxin level was found with glass fibres filters collecting the largest particle-size fraction (1.2-fold) and with PTFE filters collecting the smallest ones (5-fold). The levels of endotoxin in the size-separated airborne particle fractions correlated to those of the MWFs supporting the aerosol-generating machines. Our study indicates that a significant part of inhalable aerosols of MWFs consists of endotoxin-containing particles below the size of intact bacteria, and thus small enough to readily reach the deepest part of the lung. Combined with other chemical irritants of the MWF, exposure to MWF aerosols containing endotoxin pose a risk to respiratory health problems. © The Author 2016. Published by Oxford University Press on behalf of the British Occupational Hygiene Society.

Elucidating determinants of aerosol composition through particle-type-based receptor modeling

NASA Astrophysics Data System (ADS)

McGuire, M. L.; Jeong, C.-H.; Slowik, J. G.; Chang, R. Y.-W.; Corbin, J. C.; Lu, G.; Mihele, C.; Rehbein, P. J. G.; Sills, D. M. L.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

2011-03-01

An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed at a semi-rural site in Southern Ontario to characterize the size and chemical composition of individual particles. Particle-type-based receptor modelling of these data was used to investigate the determinants of aerosol chemical composition in this region. Individual particles were classified into particle-types and positive matrix factorization (PMF) was applied to their temporal trends to separate and cross-apportion particle-types to factors. The extent of chemical processing for each factor was assessed by evaluating the internal and external mixing state of the characteristic particle-types. The nine factors identified helped to elucidate the coupled interactions of these determinants. Nitrate-laden dust was found to be the dominant type of locally emitted particles measured by ATOFMS. Several factors associated with aerosol transported to the site from intermediate local-to-regional distances were identified: the Organic factor was associated with a combustion source to the north-west; the ECOC Day factor was characterized by nearby local-to-regional carbonaceous emissions transported from the south-west during the daytime; and the Fireworks factor consisted of pyrotechnic particles from the Detroit region following holiday fireworks displays. Regional aerosol from farther emissions sources were reflected through three factors: two biomass burning factors and a highly chemically processed long range transport factor. The biomass burning factors were separated by PMF due to differences in chemical processing which were caused in part by the passage of two thunderstorm gust fronts with different air mass histories. The remaining two factors, ECOC Night and Nitrate Background, represented the night-time partitioning of nitrate to pre-existing particles of different origins. The distinct meteorological conditions observed during this month-long study in the summer of 2007 provided a unique range

Elucidating determinants of aerosol composition through particle-type-based receptor modeling

NASA Astrophysics Data System (ADS)

McGuire, M. L.; Jeong, C.-H.; Slowik, J. G.; Chang, R. Y.-W.; Corbin, J. C.; Lu, G.; Mihele, C.; Rehbein, P. J. G.; Sills, D. M. L.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

2011-08-01

An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed at a semi-rural site in southern Ontario to characterize the size and chemical composition of individual particles. Particle-type-based receptor modelling of these data was used to investigate the determinants of aerosol chemical composition in this region. Individual particles were classified into particle-types and positive matrix factorization (PMF) was applied to their temporal trends to separate and cross-apportion particle-types to factors. The extent of chemical processing for each factor was assessed by evaluating the internal and external mixing state of the characteristic particle-types. The nine factors identified helped to elucidate the coupled interactions of these determinants. Nitrate-laden dust was found to be the dominant type of locally emitted particles measured by ATOFMS. Several factors associated with aerosol transported to the site from intermediate local-to-regional distances were identified: the Organic factor was associated with a combustion source to the north-west; the ECOC Day factor was characterized by nearby local-to-regional carbonaceous emissions transported from the south-west during the daytime; and the Fireworks factor consisted of pyrotechnic particles from the Detroit region following holiday fireworks displays. Regional aerosol from farther emissions sources was reflected through three factors: two Biomass Burning factors and a highly chemically processed Long Range Transport factor. The Biomass Burning factors were separated by PMF due to differences in chemical processing which were in part elucidated by the passage of two thunderstorm gust fronts with different air mass histories. The remaining two factors, ECOC Night and Nitrate Background, represented the night-time partitioning of nitrate to pre-existing particles of different origins. The distinct meteorological conditions observed during this month-long study in the summer of 2007 provided a unique

Measurements of the evaporation and hygroscopic response of single fine-mode aerosol particles using a Bessel beam optical trap.

PubMed

Cotterell, Michael I; Mason, Bernard J; Carruthers, Antonia E; Walker, Jim S; Orr-Ewing, Andrew J; Reid, Jonathan P

2014-02-07

A single horizontally-propagating zeroth order Bessel laser beam with a counter-propagating gas flow was used to confine single fine-mode aerosol particles over extended periods of time, during which process measurements were performed. Particle sizes were measured by the analysis of the angular variation of light scattered at 532 nm by a particle in the Bessel beam, using either a probe beam at 405 nm or 633 nm. The vapour pressures of glycerol and 1,2,6-hexanetriol particles were determined to be 7.5 ± 2.6 mPa and 0.20 ± 0.02 mPa respectively. The lower volatility of hexanetriol allowed better definition of the trapping environment relative humidity profile over the measurement time period, thus higher precision measurements were obtained compared to those for glycerol. The size evolution of a hexanetriol particle, as well as its refractive index at wavelengths 532 nm and 405 nm, were determined by modelling its position along the Bessel beam propagation length while collecting phase functions with the 405 nm probe beam. Measurements of the hygroscopic growth of sodium chloride and ammonium sulfate have been performed on particles as small as 350 nm in radius, with growth curves well described by widely used equilibrium state models. These are the smallest particles for which single-particle hygroscopicity has been measured and represent the first measurements of hygroscopicity on fine mode and near-accumulation mode aerosols, the size regimes bearing the most atmospheric relevance in terms of loading, light extinction and scattering. Finally, the technique is contrasted with other single particle and ensemble methods, and limitations are assessed.

SAGE Aerosol Measurements. Volume 2: 1 January - 31 December 1980

NASA Technical Reports Server (NTRS)

Mccormick, M. P.

1986-01-01

The stratospheric Aerosol and Gas Experiment (SAGE) satellite system, launched on February 18, 1979, provides profiles of aerosol extinction at wavelengths of 1.00 and 0.45 micron, ozone concentration, and nitrogen dioxide concentration. Data taken during sunset events in the form of zonal averages and seasonal averages of the aerosol extinction at 1.00 and 0.45 micron, ratios of the aerosol extinction to the molecular extinction at 1.00 micron, and ratios of the aerosol extinction at 0.45 micron to the aerosol extinction at 1.00 micron are presented. The averages for l980 are shown in tables and in profile and contour plots (as a function of altitude and latitude). In addition, temperature data provided by the National Oceanic and Atmospheric Administration (NOAA) for the time and location of each SAGE measurement are averaged and shown in a similar format.

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.

Characterization of a Quadrotor Unmanned Aircraft System for Aerosol-Particle-Concentration Measurements.

PubMed

Brady, James M; Stokes, M Dale; Bonnardel, Jim; Bertram, Timothy H

2016-02-02

High-spatial-resolution, near-surface vertical profiling of atmospheric chemical composition is currently limited by the availability of experimental platforms that can sample in constrained environments. As a result, measurements of near-surface gradients in trace gas and aerosol particle concentrations have been limited to studies conducted from fixed location towers or tethered balloons. Here, we explore the utility of a quadrotor unmanned aircraft system (UAS) as a sampling platform to measure vertical and horizontal concentration gradients of trace gases and aerosol particles at high spatial resolution (1 m) within the mixed layer (0-100 m). A 3D Robotics Iris+ autonomous quadrotor UAS was outfitted with a sensor package consisting of a two-channel aerosol optical particle counter and a CO2 sensor. The UAS demonstrated high precision in both vertical (±0.5 m) and horizontal positions (±1 m), highlighting the potential utility of quadrotor UAS drones for aerosol- and trace-gas measurements within complex terrain, such as the urban environment, forest canopies, and above difficult-to-access areas such as breaking surf. Vertical profiles of aerosol particle number concentrations, acquired from flights conducted along the California coastline, were used to constrain sea-spray aerosol-emission rates from coastal wave breaking.

Seasonal aerosol characteristics in the Amazon rain forest

NASA Astrophysics Data System (ADS)

Baars, H.; Althausen, D.; Ansmann, A.; Engelmann, R.; Heese, B.; Müller, D.; Pauliquevis, T.; Souza, R.; Artaxo, P.

2012-04-01

For the first time in Amazonia, continuous measurements of the vertical aerosol structure were carried out in the framework of EUCAARI (European Integrated Project on Aerosol, Cloud, Climate, Air Quality Interactions) and AMAZE-08 (Amazonian Aerosol Characterization Experiment). The observations were performed 60 km north of Manaus, Brazil (at 2° 35.5' S and 60° 2.3' W) in the central northern part of the Amazon rain forest from January to November 2008 with the automated multi-wavelength-Raman-polarization-lidar PollyXT. With this instrument, vertical profiles of the particle backscatter coefficient at 355, 532, and 1064 nm, of the particle extinction coefficient at 355 and 532 nm, and of the particle linear depolarization ratio at 355 nm can be determined. During the 10-months observational period, measurements were performed on 211 days resulting in more than 2500 hours of tropospheric aerosol and cloud profile observations. The analysis of the long-term data set revealed strong differences in the aerosol characteristics between the wet and the dry season. In the wet season, very clean atmospheric conditions occurred in ca. 50% of all observation cases. During these clean conditions, the aerosol optical depth (AOD) at 532 nm was less than 0.05 and the aerosol was trapped in the lowermost 2 km of the troposphere. However, also intrusions of Saharan dust and African biomass-burning aerosol (BBA) - characterized by a significantly increased AOD and particle depolarization ratio - were observed in about one third (32%) of all lidar observations. These African aerosol plumes extended usually from the surface up to about 3.5 km agl. During the dry season, BBA from fires on the South American continent was the dominant aerosol species. The mean AOD of the dry season was found to be a factor of 3 higher than the mean AOD of the wet season (0.26 compared to 0.08 at 532 nm). This is due to the high BBA concentration in the atmosphere. Maximum AOD values were less than 0

Optical properties of aerosols at Grand Canyon National Park

NASA Astrophysics Data System (ADS)

Malm, William C.; Day, Derek E.

Visibility in the United States is expected to improve over the next few decades because of reduced emissions, especially sulfur dioxide. In the eastern United States, sulfates make up about 60-70% of aerosol extinction, while in the inner mountain west that fraction is only about 30%. In the inner mountain west, carbon aerosols make up about 35% of extinction, while coarse mass contributes between 15 and 25% depending on how absorption is estimated. Although sulfur dioxide emissions are projected to decrease, carbon emissions due to prescribed fire activity will increase by factors of 5-10, and while optical properties of sulfates have been extensively studied, similar properties of carbon and coarse particles are less well understood. The inability to conclusively apportion about 50% of the extinction budget motivated a study to examine aerosol physio-chemical-optical properties at Grand Canyon, Arizona during the months of July and August. Coarse particle mass has usually been assumed to consist primarily of wind-blown dust, with a mass-scattering efficiency between about 0.4 and 0.6 m 2 g -1. Although there were episodes where crustal material made up most of the coarse mass, on the average, organics and crustal material mass were about equal. Furthermore, about one-half of the sampling periods had coarse-mass-scattering efficiencies greater than 0.6 m 2 g -1 and at times coarse-mass-scattering efficiencies were near 1.0 m 2 g -1. It was shown that absorption by coarse- and fine-particle absorption were about equal and that both fine organic and sulfate mass-scattering efficiencies were substantially less than the nominal values of 4.0 and 3.0 m 2 g -1 that have typically been used.

Resolving the Aerosol Piece of the Global Climate Picture

NASA Astrophysics Data System (ADS)

Kahn, R. A.

2017-12-01

Factors affecting our ability to calculate climate forcing and estimate model predictive skill include direct radiative effects of aerosols and their indirect effects on clouds. Several decades of Earth-observing satellite observations have produced a global aerosol column-amount (AOD) record, but an aerosol microphysical property record required for climate and many air quality applications is lacking. Surface-based photometers offer qualitative aerosol-type classification, and several space-based instruments map aerosol air-mass types under favorable conditions. However, aerosol hygroscopicity, mass extinction efficiency (MEE), and quantitative light absorption, must be obtained from in situ measurements. Completing the aerosol piece of the climate picture requires three elements: (1) continuing global AOD and qualitative type mapping from space-based, multi-angle imagers and aerosol vertical distribution from near-source stereo imaging and downwind lidar, (2) systematic, quantitative in situ observations of particle properties unobtainable from space, and (3) continuing transport modeling to connect observations to sources, and extrapolate limited sampling in space and time. At present, the biggest challenges to producing the needed aerosol data record are: filling gaps in particle property observations, maintaining global observing capabilities, and putting the pieces together. Obtaining the PDFs of key particle properties, adequately sampled, is now the leading observational deficiency. One simplifying factor is that, for a given aerosol source and season, aerosol amounts often vary, but particle properties tend to be repeatable. SAM-CAAM (Systematic Aircraft Measurements to Characterize Aerosol Air Masses), a modest aircraft payload deployed frequently could fill this gap, adding value to the entire satellite data record, improving aerosol property assumptions in retrieval algorithms, and providing MEEs to translate between remote-sensing optical constraints

Simulation of the influence of aerosol particles on Stokes parameters of polarized skylight

NASA Astrophysics Data System (ADS)

Li, L.; Li, Z. Q.; Wendisch, M.

2014-03-01

Microphysical properties and chemical compositions of aerosol particles determine polarized radiance distribution in the atmosphere. In this paper, the influences of different aerosol properties (particle size, shape, real and imaginary parts of refractive index) on Stokes parameters of polarized skylight in the solar principal and almucantar planes are studied by using vector radiative transfer simulations. The results show high sensitivity of the normalized Stokes parameters due to fine particle size, shape and real part of refractive index of aerosols. It is possible to utilize the strength variations at the peak positions of the normalized Stokes parameters in the principal and almucantar planes to identify aerosol types.

Spatio-temporal aerosol particle distributions in the UT/LMS measured by the IAGOS-CARIBIC Observatory

NASA Astrophysics Data System (ADS)

Assmann, Denise; Hermann, Markus; Weigelt, Andreas; Martinsson, Bengt; Brenninkmeijer, Carl; Rauthe-Schöch, Armin; van Velthoven, Peter; Bönisch, Harald; Zahn, Andreas

2017-04-01

Submicrometer aerosol particles in the upper troposphere and lowermost stratosphere (UT/LMS) influence the Earth`s radiation budget directly and, more important, indirectly, by acting as cloud condensation nuclei and by changing trace gas concentrations through heterogeneous chemical processes. Since 1997, regular in situ UT/LMS aerosol particle measurements have been conducted by the Leibniz Institute for Tropospheric Research, Leipzig, Germany and the University of Lund, Sweden, using the the CARIBIC (now IAGOS-CARIBIC) observatory (www.caribic-atmospheric.com) onboard a passenger aircraft. Submicrometer aerosol particle number concentrations and the aerosol particle size distribution are measured using three condensation particle counters and one optical particle size spectrometer. Moreover, particle elemental composition is determined using an aerosol impactor sampler and post-flight ion beam analysis (PIXE, PESA) of the samples in the laboratory. Based on this unique data set, including meteorological analysis, we present representative spatio-temporal distributions of particle number, surface, volume and elemental concentrations in an altitude of 8-12 km covering a large fraction of the northern hemisphere. We discuss the measured values in the different size regimes with respect to sources and sinks in different regions. Additionally, we calculated highly resolved latitudinal and longitudinal cross sections of the particle number size distribution, probability density functions and trends in particle number concentrations, but also in elemental composition, determined from our regular measurements over more than a decade. Moreover, we generated seasonal contour plots for particle number concentrations, the potential temperature, and the equivalent latitude. The results are interpreted with respect to aerosol microphysics and transport using CARIBIC trace gas data like ozone and water vapour. The influence of clouds in the troposphere and the different

OMPS Limb Profiler: Extending SAGE and CALIPSO Stratospheric Aerosol Records

NASA Astrophysics Data System (ADS)

Taha, G.; Bhartia, P. K.; Chen, Z.; Xu, P.; Loughman, R. P.; Jaross, G.

2017-12-01

The OMPS LP instrument is designed to provide high vertical resolution ozone and aerosol profiles from measurements of the scattered solar radiation in the 290-1000 nm spectral range. It collected its first Earth limb measurement in January 10, 2012, and continues to provide daily global measurements of ozone and aerosol profiles from the cloud top up to 60 km and 40 km respectively. The relatively high vertical and spatial sampling allow detection and tracking periodic events when aerosol particles are injected into the stratosphere, such as volcanic eruptions or meteor explosions. OMPS LP can extend the long-term records of stratospheric aerosol at high vertical resolution produced by variety of sensors, such as SAGEII, GOMOS, OSIRIS and CALIPSO. Most of these instruments ceased to operate or well beyond their designed lifetime. After an absence of over a decade, SAGE III/ISS was launched earlier this year and expected to resume the high quality aerosol data record. OMPS LP is also schedule to fly on JPSS-2 and 3. In this study we will examine the suitability of using LP profiles to continue the stratospheric aerosol records beyond SAGE, OSIRIS, and CALIPSO. We will compare OMPS LP released V1.0 aerosol extinction measurements to OSIRIS and CALIPSO. Initial results shows good agreement with OSIRIS measurements to within 20%, with larger bias in the southern hemisphere. To test the effect of the assumed aerosol size model (ASD) and phase function, we compare measurements taken at similar location and time with different viewing geometry. Comparison of ascending and descending aerosol extinction daily zonal means at high latitudes shows systematic bias that is well correlated with the solar scattering angle, indicating ASD uncertainties up to 30%. In addition, results showing latitudinal, and temporal variability of stratospheric aerosol extinction and optical depth for the three instruments will also be presented and compared. We will also present OMPS LP aerosol

The rate of equilibration of viscous aerosol particles

NASA Astrophysics Data System (ADS)

O'Meara, Simon; Topping, David O.; McFiggans, Gordon

2016-04-01

The proximity of atmospheric aerosol particles to equilibrium with their surrounding condensable vapours can substantially impact their transformations, fate and impacts and is the subject of vibrant research activity. In this study we first compare equilibration timescales estimated by three different models for diffusion through aerosol particles to assess any sensitivity to choice of model framework. Equilibration times for diffusion coefficients with varying dependencies on composition are compared for the first time. We show that even under large changes in the saturation ratio of a semi-volatile component (es) of 1-90 % predicted equilibration timescales are in agreement, including when diffusion coefficients vary with composition. For condensing water and a diffusion coefficient dependent on composition, a plasticising effect is observed, leading to a decreased estimated equilibration time with increasing final es. Above 60 % final es maximum equilibration times of around 1 s are estimated for comparatively large particles (10 µm) containing a relatively low diffusivity component (1 × 10-25 m2 s-1 in pure form). This, as well as other results here, questions whether particle-phase diffusion through water-soluble particles can limit hygroscopic growth in the ambient atmosphere. In the second part of this study, we explore sensitivities associated with the use of particle radius measurements to infer diffusion coefficient dependencies on composition using a diffusion model. Given quantified similarities between models used in this study, our results confirm considerations that must be taken into account when designing such experiments. Although quantitative agreement of equilibration timescales between models is found, further work is necessary to determine their suitability for assessing atmospheric impacts, such as their inclusion in polydisperse aerosol simulations.

Size distribution and scattering phase function of aerosol particles retrieved from sky brightness measurements

NASA Technical Reports Server (NTRS)

Kaufman, Y. J.; Gitelson, A.; Karnieli, A.; Ganor, E. (Editor); Fraser, R. S.; Nakajima, T.; Mattoo, S.; Holben, B. N.

1994-01-01

Ground-based measurements of the solar transmission and sky radiance in a horizontal plane through the Sun are taken in several geographical regions and aerosol types: dust in a desert transition zone in Israel, sulfate particles in Eastern and Western Europe, tropical aerosol in Brazil, and mixed continental/maritime aerosol in California. Stratospheric aerosol was introduced after the eruption of Mount Pinatubo in June 1991. Therefore measurements taken before the eruption are used to analyze the properties of tropospheric aerosol; measurements from 1992 are also used to detect the particle size and concentration of stratospheric aerosol. The measurements are used to retrieve the size distribution and the scattering phase function at large scattering angles of the undisturbed aerosol particles. The retrieved properties represent an average on the entire atmospheric column. A comparison between the retrieved phase function for a scattering angle of 120 deg, with phase function predicted from the retrieved size distribution, is used to test the assumption of particle homogeneity and sphericity in radiative transfer models (Mie theory). The effect was found to be small (20% +/- 15%). For the stratospheric aerosol (sulfates), as expected, the phase function was very well predicted using the Mie theory. A model with a power law distribution, based on the spectral dependence of the optical thickness, alpha, cannot estimate accurately the phase function (up to 50% error for lambda = 0.87 microns). Before the Pinatubo eruption the ratio between the volumes of sulfate and coarse particles was very well correlated with alpha. The Pinatubo stratospheric aerosol destroyed this correlation. The aerosol optical properties are compared with analysis of the size, shape, and composition of the individual particles by electron microscopy of in situ samples. The measured volume size distribution before the injection of stratospheric aerosol consistently show two modes, sulfate

Oxalate metal complexes in aerosol particles: implications for the hygroscopicity of oxalate-containing particles

NASA Astrophysics Data System (ADS)

Furukawa, T.; Takahashi, Y.

2011-05-01

Atmospheric aerosols have both a direct and an indirect cooling effect that influences the radiative balance at the Earth's surface. It has been estimated that the degree of cooling is large enough to weaken the warming effect of carbon dioxide. Among the cooling factors, secondary organic aerosols (SOA) play an important role in the solar radiation balance in the troposphere as SOA can act as cloud condensation nuclei (CCN) and extend the lifespan of clouds because of their high hygroscopic and water soluble nature. Oxalic acid is an important component of SOA, and is produced via several formation pathways in the atmosphere. However, it is not certain whether oxalic acid exists as free oxalic acid or as metal oxalate complexes in aerosols, although there is a marked difference in their solubility in water and their hygroscopicity. We employed X-ray absorption fine structure spectroscopy to characterize the calcium (Ca) and zinc (Zn) in aerosols collected at Tsukuba in Japan. Size-fractionated aerosol samples were collected for this purpose using an impactor aerosol sampler. It was shown that 10-60% and 20-100% of the total Ca and Zn in the finer particles (<2.1 μm) were present as Ca and Zn oxalate complexes, respectively. Oxalic acid is hygroscopic and can thus increase the CCN activity of aerosol particles, while complexes with various polyvalent metal ions such as Ca and Zn are not hygroscopic, which cannot contribute to the increase of the CCN activity of aerosols. Based on the concentrations of noncomplexed and metal-complexed oxalate species, we found that most of the oxalic acid is present as metal oxalate complexes in the aerosols, suggesting that oxalic acid does not always increase the hygroscopicity of aerosols in the atmosphere. Similar results are expected for other dicarboxylic acids, such as malonic and succinic acids. Thus, it is advisable that the cooling effect of organic aerosols should be estimated by including the information on metal

Study of the chemical composition of atmospheric aerosol particles in Hungary: a review

NASA Astrophysics Data System (ADS)

Mészáros, E.

The methods used in Hungarian laboratories to study the chemical composition of atmospheric aerosol particles over the last 30 years are reviewed. Individual particles were identified by topochemical techniques and morphological identification with an electron microscope. Bulk analyses were also carried out by applying wet chemical methods, and more recently by the PIXE procedure. The results gained are summarized in connection with the general development of atmospheric aerosol science during the last decades. These studies demonstrated that cloud condensation nuclei are water soluble Aitken sized particles which are composed of sulfates. Neutralized and acidic sulfate particles constitute the main class of fine aerosol particles under continental and oceanic background conditions. Coarse particles contain mostly sodium, silicon and aluminium. The formation and origin of particles in different size ranges are also discussed.

Relating Aerosol Mass and Optical Depth in the Summertime Continental Boundary Layer

NASA Astrophysics Data System (ADS)

Brock, C. A.; Wagner, N.; Middlebrook, A. M.; Attwood, A. R.; Washenfelder, R. A.; Brown, S. S.; McComiskey, A. C.; Gordon, T. D.; Welti, A.; Carlton, A. G.; Murphy, D. M.

2014-12-01

Aerosol optical depth (AOD), the column-integrated ambient aerosol light extinction, is determined from satellite and ground-based remote sensing measurements. AOD is the parameter most often used to validate earth system model simulations of aerosol mass. Relating aerosol mass to AOD, however, is problematic due to issues including aerosol water uptake as a function of relative humidity (RH) and the complicated relationship between aerosol physicochemical properties and light extinction. Measurements of aerosol microphysical, chemical, and optical properties help to constrain the relationship between aerosol mass and optical depth because aerosol extinction at ambient RH is a function of the abundance, composition and size distribution of the aerosol. We use vertical profiles of humidity and dry aerosol extinction observed in the southeastern United States (U.S.) to examine the relationship between submicron aerosol mass concentration and extinction at ambient RH. We show that the κ-Köhler parameterization directly, and without additional Mie calculations, describes the change in extinction with varying RH as a function of composition for both aged aerosols typical of the polluted summertime continental boundary layer and the biomass burning aerosols we encountered. We calculate how AOD and the direct radiative effect in the eastern U.S. have likely changed due to trends in aerosol composition in recent decades. We also examine the sensitivity of AOD to the RH profile and to aerosol composition, size distribution and abundance.

Radial inhomogeneities in particle composition of single, levitated aerosol particles observed by Mie resonance spectroscopy (Invited)

NASA Astrophysics Data System (ADS)

Krieger, U. K.; Steimer, S.; Lienhard, D.; Bastelberger, S.

2013-12-01

Recent observations have indicated that organic aerosol particles in the atmosphere may exist in an amorphous semi-solid or even solid (i.e. glassy) state, e.g. [1]. The influence of highly viscous and glassy states on the timescale of aerosol particle equilibration with respect to water vapor have been investigated for some model systems of atmospheric aerosol, e.g. [2,3]. In particular, it has been shown that the kinetics of the water absorption/desorption process is controlled entirely by liquid-phase diffusion of water molecules for a highly viscous aerosol particle. A liquid phase diffusion model based on numerically solving the non-linear diffusion equation predicts strong internal gradients in water concentration when condensed phase diffusion impedes the water uptake from the gas phase [2]. Here we observe and quantify the internal concentration gradients in single, levitated, micron size aerosol particles of aqueous MBTCA (3-methyl-1,2,3-Butanetricarboxylic acid) and shikimic acid using elastic Mie resonance spectroscopy. A single, aqueous particle is levitated in an electro-dynamic balance (for details see [2]), dried for several days at room temperature, cooled to the target temperature and exposed to a rapid change in relative humidity. In addition to measuring the elastically backscattered light of a 'white light ' LED source and recording the full spectrum with a spectrograph as in [2], we use a tunable diode laser (TDL) to scan high resolution TE- and TM spectra. This combination allows observing various Mie resonance mode orders simultaneously. Since we perform the experiment at low temperatures and low humidities the changes in the Mie-spectra due to water uptake are sufficiently slow to resolve the kinetics. Experimental Mie resonance spectra are inverted to concentration profiles of water within the particle by applying the numerical diffusion model [2] in conjunction with Mie calculations of multilayered spheres [4]. Potential implications for

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.

Improved identification of primary biological aerosol particles using single-particle mass spectrometry

DOE PAGES

Zawadowicz, Maria A.; Froyd, Karl D.; Murphy, Daniel M.; ...

2017-06-16

Measurements of primary biological aerosol particles (PBAP), especially at altitudes relevant to cloud formation, are scarce. Single-particle mass spectrometry (SPMS) has been used to probe aerosol chemical composition from ground and aircraft for over 20 years. Here we develop a method for identifying bioaerosols (PBAP and particles containing fragments of PBAP as part of an internal mixture) using SPMS. Here, we show that identification of bioaerosol using SPMS is complicated because phosphorus-bearing mineral dust and phosphorus-rich combustion by-products such as fly ash produce mass spectra with peaks similar to those typically used as markers for bioaerosol. We have developed a methodologymore » to differentiate and identify bioaerosol using machine learning statistical techniques applied to mass spectra of known particle types. This improved method provides far fewer false positives compared to approaches reported in the literature. The new method was then applied to two sets of ambient data collected at Storm Peak Laboratory and a forested site in Central Valley, California to show that 0.04–2 % of particles in the 200–3000 nm aerodynamic diameter range were identified as bioaerosol. In addition, 36–56 % of particles identified as biological also contained spectral features consistent with mineral dust, suggesting internal dust–biological mixtures.« less

Improved identification of primary biological aerosol particles using single-particle mass spectrometry

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

Zawadowicz, Maria A.; Froyd, Karl D.; Murphy, Daniel M.

Measurements of primary biological aerosol particles (PBAP), especially at altitudes relevant to cloud formation, are scarce. Single-particle mass spectrometry (SPMS) has been used to probe aerosol chemical composition from ground and aircraft for over 20 years. Here we develop a method for identifying bioaerosols (PBAP and particles containing fragments of PBAP as part of an internal mixture) using SPMS. Here, we show that identification of bioaerosol using SPMS is complicated because phosphorus-bearing mineral dust and phosphorus-rich combustion by-products such as fly ash produce mass spectra with peaks similar to those typically used as markers for bioaerosol. We have developed a methodologymore » to differentiate and identify bioaerosol using machine learning statistical techniques applied to mass spectra of known particle types. This improved method provides far fewer false positives compared to approaches reported in the literature. The new method was then applied to two sets of ambient data collected at Storm Peak Laboratory and a forested site in Central Valley, California to show that 0.04–2 % of particles in the 200–3000 nm aerodynamic diameter range were identified as bioaerosol. In addition, 36–56 % of particles identified as biological also contained spectral features consistent with mineral dust, suggesting internal dust–biological mixtures.« less

Improved identification of primary biological aerosol particles using single-particle mass spectrometry

NASA Astrophysics Data System (ADS)

Zawadowicz, Maria A.; Froyd, Karl D.; Murphy, Daniel M.; Cziczo, Daniel J.

2017-06-01

Measurements of primary biological aerosol particles (PBAP), especially at altitudes relevant to cloud formation, are scarce. Single-particle mass spectrometry (SPMS) has been used to probe aerosol chemical composition from ground and aircraft for over 20 years. Here we develop a method for identifying bioaerosols (PBAP and particles containing fragments of PBAP as part of an internal mixture) using SPMS. We show that identification of bioaerosol using SPMS is complicated because phosphorus-bearing mineral dust and phosphorus-rich combustion by-products such as fly ash produce mass spectra with peaks similar to those typically used as markers for bioaerosol. We have developed a methodology to differentiate and identify bioaerosol using machine learning statistical techniques applied to mass spectra of known particle types. This improved method provides far fewer false positives compared to approaches reported in the literature. The new method was then applied to two sets of ambient data collected at Storm Peak Laboratory and a forested site in Central Valley, California to show that 0.04-2 % of particles in the 200-3000 nm aerodynamic diameter range were identified as bioaerosol. In addition, 36-56 % of particles identified as biological also contained spectral features consistent with mineral dust, suggesting internal dust-biological mixtures.

Spatial Variability of CCN Sized Aerosol Particles

NASA Astrophysics Data System (ADS)

Asmi, A.; Väänänen, R.

2014-12-01

The computational limitations restrict the grid size used in GCM models, and for many cloud types they are too large when compared to the scale of the cloud formation processes. Several parameterizations for e.g. convective cloud formation exist, but information on spatial subgrid variation of the cloud condensation nuclei (CCNs) sized aerosol concentration is not known. We quantify this variation as a function of the spatial scale by using datasets from airborne aerosol measurement campaigns around the world including EUCAARI LONGREX, ATAR, INCA, INDOEX, CLAIRE, PEGASOS and several regional airborne campaigns in Finland. The typical shapes of the distributions are analyzed. When possible, we use information obtained by CCN counters. In some other cases, we use particle size distribution measured by for example SMPS to get approximated CCN concentration. Other instruments used include optical particle counters or condensational particle counters. When using the GCM models, the CCN concentration used for each the grid-box is often considered to be either flat, or as an arithmetic mean of the concentration inside the grid-box. However, the aircraft data shows that the concentration values are often lognormal distributed. This, combined with the subgrid variations in the land use and atmospheric properties, might cause that the aerosol-cloud interactions calculated by using mean values to vary significantly from the true effects both temporary and spatially. This, in turn, can cause non-linear bias into the GCMs. We calculate the CCN aerosol concentration distribution as a function of different spatial scales. The measurements allow us to study the variation of these distributions within from hundreds of meters up to hundreds of kilometers. This is used to quantify the potential error when mean values are used in GCMs.

Broadband optical extinction measurements and complex refractive indices in the ultraviolet spectral region for biogenic secondary organic aerosol exposed to ammonia

NASA Astrophysics Data System (ADS)

Flores, J.; Washenfelder, R. A.; Lee, H.; Segev, L.; Nizkorodov, S.; Brown, S. S.; Rudich, Y.

2013-12-01

The interaction between aerosols and sunlight plays an important role in the radiative balance of Earth's atmosphere. Aerosols can both scatter and absorb solar radiation causing surface cooling and heating of the atmosphere. These interactions depend on the optical properties of the aerosols (i.e., complex refractive index). Secondary organic aerosol (SOA) account for a significant fraction of the tropospheric aerosol. However, their chemical, physical, and optical properties, especially as they are processed in the atmosphere (aging), are still poorly understood. In this study, SOA formed by the ozonolysis of various biogenic volatile organic compound (BVOC) precursors (α-pinene, limonene, and α-humulene) were exposed to humid air containing various concentrations of gaseous ammonia which has been shown to cause the biogenic SOA to ';brown' on filters. The extent of absorption of the SOA in the aerosol phase cause by the exposure to gaseous ammonia was measured by a newly developed instrument to measure aerosol extinction as a function of wavelength using Broadband Cavity Enhanced Spectroscopy (BBCES) with a broadband light source. Size-selected measurements of the humid SOA exposed to NH3 for about 1.5 hours were used to derive complex refractive indices (RI) as a function of wavelength in the UV spectral region (from 360 - 420nm). The imaginary part of the refractive index did not exceed 0.05 in the 360 - 420 nm range for SOA formed from the three BVOCs even at high concentrations of NH3 (>1ppm), allowing to place an upper limit of k = 0.05. Furthermore, the small k values are consistent with bulk UV-VIS measurements. However, for the α-pinene SOA, the real part of the RI slightly increased from n = 1.49 to n = 1.55 with negligible spectral dependence. For limonene and α-humulene the real part remind constant within error calculations. Based on these observations, reactive uptake of gaseous ammonia is not expected to significantly affect absorption and

Characterization of aerosol particles from grass mowing by joint deployment of ToF-AMS and ATOFMS instruments

NASA Astrophysics Data System (ADS)

Drewnick, Frank; Dall'Osto, Manuel; Harrison, Roy

During a measurement campaign at a semi-urban/industrial site a grass-cutting event was observed, when the lawn in the immediate surrounding of the measurement site was mowed. Using a wide variety of state-of-the-art aerosol measurement technology allowed a broad characterization of the aerosol generated by the lawn mowing. The instrumentation included two on-line aerosol mass spectrometers: an Aerodyne Time-of-Flight Aerosol Mass Spectrometer (ToF-AMS) and a TSI Aerosol Time-of-Flight Mass Spectrometer (ATOFMS); in addition, a selection of on-line aerosol concentration and size distribution instruments (OPC, APS, SMPS, CPC, FDMS-TEOM, MAAP) was deployed. From comparison of background aerosol measurements during most of the day with the aerosol measured during the lawn mowing, the grass cutting was found to generate mainly two different types of aerosol particles: an intense ultrafine particle mode (1 h average: 4 μg m -3) of almost pure hydrocarbon-like organics and a distinct particle mode in the upper sub-micrometer size range containing particles with potassium and nitrogen-organic compounds. The ultrafine particles are probably lubricating oil particles from the lawn mower exhaust; the larger particles are swirled-up plant debris particles from the mowing process. While these particle types were identified in the data from the two mass spectrometers, the on-line aerosol concentration and size distribution data support these findings. The results presented here show that the combination of quantitative aerosol particle ensemble mass spectrometry (ToF-AMS) and single particle mass spectrometry (ATOFMS) provides much deeper insights into the nature of the aerosol properties than each of the instruments could do alone. Therefore a combined deployment of both types of instruments is strongly recommended.

Extrinsic extinction cross-section in the multiple acoustic scattering by fluid particles

NASA Astrophysics Data System (ADS)

Mitri, F. G.

2017-04-01

Cross-sections (and their related energy efficiency factors) are physical parameters used in the quantitative analysis of different phenomena arising from the interaction of waves with a particle (or multiple particles). Earlier works with the acoustic scattering theory considered such quadratic (i.e., nonlinear) quantities for a single scatterer, although a few extended the formalism for a pair of scatterers but were limited to the scattering cross-section only. Therefore, the standard formalism applied to viscous particles is not suitable for the complete description of the cross-sections and energy balance of the multiple-particle system because both absorption and extinction phenomena arise during the multiple scattering process. Based upon the law of the conservation of energy, this work provides a complete comprehensive analysis for the extrinsic scattering, absorption, and extinction cross-sections (i.e., in the far-field) of a pair of viscous scatterers of arbitrary shape, immersed in a nonviscous isotropic fluid. A law of acoustic extinction taking into consideration interparticle effects in wave propagation is established, which constitutes a generalized form of the optical theorem in multiple scattering. Analytical expressions for the scattering, absorption, and extinction cross-sections are derived for plane progressive waves with arbitrary incidence. The mathematical expressions are formulated in partial-wave series expansions in cylindrical coordinates involving the angle of incidence, the addition theorem for the cylindrical wave functions, and the expansion coefficients of the scatterers. The analysis shows that the multiple scattering cross-section depends upon the expansion coefficients of both scatterers in addition to an interference factor that depends on the interparticle distance. However, the extinction cross-section depends on the expansion coefficients of the scatterer located in a particular system of coordinates, in addition to the

Comparison of mineral dust and droplet residuals measured with two single particle aerosol mass spectrometers

NASA Astrophysics Data System (ADS)

Wonaschütz, Anna; Ludwig, Wolfgang; Zawadowicz, Maria; Hiranuma, Naruki; Hitzenberger, Regina; Cziczo, Daniel; DeMott, Paul; Möhler, Ottmar

2017-04-01

Single Particle mass spectrometers are used to gain information on the chemical composition of individual aerosol particles, aerosol mixing state, and other valuable aerosol characteristics. During the Mass Spectrometry Intercomparison at the Fifth Ice Nucleation (FIN-01) Workshop, the new LAAPTOF single particle aerosol mass spectrometer (AeroMegt GmbH) was conducting simultaneous measurements together with the PALMS (Particle Analysis by Laser Mass Spectrometry) instrument. The aerosol particles were sampled from the AIDA chamber during ice cloud expansion experiments. Samples of mineral dust and ice droplet residuals were measured simultaneously. In this work, three expansion experiments are chosen for a comparison between the two mass spectrometers. A fuzzy clustering routine is used to group the spectra. Cluster centers describing the ensemble of particles are compared. First results show that while differences in the peak heights are likely due to the use of an amplifier in PALMS, cluster centers are comparable.

Formation characteristics of aerosol particles from pulverized coal pyrolysis in high-temperature environments.

PubMed

Chen, Wei-Hsin; Du, Shan-Wen; Yang, Hsi-Hsien; Wu, Jheng-Syun

2008-05-01

The formation characteristics of aerosol particles from pulverized coal pyrolysis in high temperatures are studied experimentally. By conducting a drop-tube furnace, fuel pyrolysis processes in industrial furnaces are simulated in which three different reaction temperatures of 1000, 1200, and 1400 degrees C are considered. Experimental observations indicate that when the reaction temperature is 1000 degrees C, submicron particles are produced, whereas the particle size is dominated by nanoscale for the temperature of 1400 degrees C. Thermogravimetric analysis of the aerosol particles stemming from the pyrolysis temperature of 1000 degrees C reveals that the thermal behavior of the aerosol is characterized by a three-stage reaction with increasing heating temperature: (1) a volatile-reaction stage, (2) a weak-reaction stage, and (3) a soot-reaction stage. However, with the pyrolysis temperature of 1400 degrees C, the volatile- and weak-reaction stages almost merge together and evolve into a chemical-frozen stage. The submicron particles (i.e., 1000 degrees C) are mainly composed of volatiles, tar, and soot, with the main component of the nanoscale particles (i.e., 1400 degrees C) being soot. The polycyclic aromatic hydrocarbons (PAHs) contained in the aerosols are also analyzed. It is found that the PAH content in generated aerosols decreases dramatically as the pyrolysis temperature increases.

The Impact of Aerosol Microphysical Representation in Models on the Direct Radiative Effect

NASA Astrophysics Data System (ADS)

Ridley, D. A.; Heald, C. L.

2017-12-01

Aerosol impacts the radiative balance of the atmosphere both directly and indirectly. There is considerable uncertainty remaining in the aerosol direct radiative effect (DRE), hampering understanding of the present magnitude of anthropogenic aerosol forcing and how future changes in aerosol loading will influence climate. Computationally expensive explicit aerosol microphysics are usually reserved for modelling of the aerosol indirect radiative effects that depend upon aerosol particle number. However, the direct radiative effects of aerosol are also strongly dependent upon the aerosol size distribution, especially particles between 0.2µm - 2µm diameter. In this work, we use a consistent model framework and consistent emissions to explore the impact of prescribed size distributions (bulk scheme) relative to explicit microphysics (sectional scheme) on the aerosol radiative properties. We consider the difference in aerosol burden, water uptake, and extinction efficiency resulting from the two representations, highlighting when and where the bulk and sectional schemes diverge significantly in their estimates of the DRE. Finally, we evaluate the modelled size distributions using in-situ measurements over a range of regimes to provide constraints on both the accumulation and coarse aerosol sizes.

AEROSOL PARTICLE COLLECTOR DESIGN STUDY

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

Lee, S; Richard Dimenna, R

2007-09-27

A computational evaluation of a particle collector design was performed to evaluate the behavior of aerosol particles in a fast flowing gas stream. The objective of the work was to improve the collection efficiency of the device while maintaining a minimum specified air throughput, nominal collector size, and minimal power requirements. The impact of a range of parameters was considered subject to constraints on gas flow rate, overall collector dimensions, and power limitations. Potential improvements were identified, some of which have already been implemented. Other more complex changes were identified and are described here for further consideration. In addition, fruitfulmore » areas for further study are proposed.« less

SAGE aerosol measurements. Volume 1: February 21, 1979 to December 31, 1979

NASA Technical Reports Server (NTRS)

Mccormick, M. P.

1985-01-01

The Stratospheric Aerosol and Gas Experiment (SAGE) satellite system, launched on February 18, 1979, provides profiles of aerosol extinction, ozone concentration, and nitrogen dioxide concentration between about 80 N and 80 S. Zonal averages, separated into sunrise and sunset events, and seasonal averages of the aerosol extinction at 1.00 microns and 0.45 microns ratios of the aerosol extinction to the molecular extinction at 1.00 microns, and ratios of the aerosol extinction at 0.45 microns to the aerosol extinction at 1.00 microns are given. The averages for 1979 are shown in tables and in profile and contour plots (as a function of altitude and latitude). In addition, temperature data provided by the National Oceanic and Atmospheric Administration (NOAA) for the time and location of each SAGE measurement are averaged and shown in a similar format. Typical values of the peak aerosol extinction were 0.0001 to 0.0002 km at 1.00 microns depth values for the 1.00 microns channel varied between 0.001 and 0.002 over all latitudes.

A rocket-borne mass analyzer for charged aerosol particles in the mesosphere

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

Knappmiller, Scott; Robertson, Scott; Sternovsky, Zoltan

2008-10-15

An electrostatic mass spectrometer for nanometer-sized charged aerosol particles in the mesosphere has been developed and tested. The analyzer is mounted on the forward end of a rocket and has a slit opening for admitting a continuous sample of air that is exhausted through ports at the sides. Within the instrument housing are two sets of four collection plates that are biased with positive and negative voltages for the collection of negative and positive aerosol particles, respectively. Each collection plate spans about an order of magnitude in mass which corresponds to a factor of 2 in radius. The number densitymore » of the charge is calculated from the current collected by the plates. The mean free path for molecular collisions in the mesosphere is comparable to the size of the instrument opening; thus, the analyzer performance is modeled by a Monte Carlo computer code that finds the aerosol particles trajectories within the instrument including both the electrostatic force and the forces from collisions of the aerosol particles with air molecules. Mass sensitivity curves obtained using the computer models are near to those obtained in the laboratory using an ion source. The first two flights of the instrument returned data showing the charge number densities of both positive and negative aerosol particles in four mass ranges.« less

Seasonal variability of aerosol vertical profiles over east US and west Europe: GEOS-Chem/APM simulation and comparison with CALIPSO observations

NASA Astrophysics Data System (ADS)

Ma, Xiaoyan; Yu, Fangqun

2014-04-01

In this study, we employed 5 years (2007-2011) of the CALIPSO level-3 monthly aerosol extinction product to compare with the GEOS-Chem/APM simulations for the same time period over two major industrial regions (east US and west Europe). The objective is to understand which aerosol types or species significantly determine the vertical profiles by comparing the seasonal variability between the simulations and observations. Our study shows that the model successfully produces the magnitude of aerosol extinction, profile shape, and their seasonal variability observed by CALIPSO over both east US (EUS) and west Europe (WEU). The extinctions below 1 km make up 44-79% to the total, from either the model simulations or satellite retrievals, with larger percentages in winter seasons (62-79%) and smaller percentages in summer seasons (44-57%) associated with the strength of vertical transport. The shape of the vertical profiles has, therefore, a distinct seasonal variability, with a more like quasi-exponential shape in DJF (December, January, and February) and SON (September, October, and November) than in MAM (March, April, and May) and JJA (June, July, and August), which have been discerned from both measurements and simulations. Analysis of modeled aerosol species indicates that secondary particles (SP), containing sulfate, ammonia, nitrate, and secondary organic aerosols (SOAs), predominantly determine the total aerosol vertical profiles while black carbon (BC), primary organic carbon (OC), and sea salt (SS), only account for a small fraction and are also limited near the surface. Mineral dust (DS) contributes more to the total extinction over WEU than over EUS, particularly in MAM, a result of being adjacent to the North Africa desert. Secondary inorganic aerosol (SIA, i.e. sulfate, ammonia, and nitrate) contributes most of the total SP mass in DJF and SON while SOA is particularly important in MAM and JJA when the emissions from leafed plants are active. Our study also

Inside versus Outside: Ion Redistribution in Nitric Acid Reacted Sea Spray Aerosol Particles as Determined by Single Particle Analysis (Invited)

NASA Astrophysics Data System (ADS)

Ault, A. P.; Guasco, T.; Ryder, O. S.; Baltrusaitis, J.; Cuadra-Rodriguez, L. A.; Collins, D. B.; Ruppel, M. J.; Bertram, T. H.; Prather, K. A.; Grassian, V. H.

2013-12-01

Sea spray aerosol (SSA) particles were generated under real-world conditions using natural seawater and a unique ocean-atmosphere facility equipped with actual breaking waves or a marine aerosol reference tank (MART) that replicates those conditions. The SSA particles were exposed to nitric acid in situ in a flow tube and the well-known chloride displacement and nitrate formation reaction was observed. However, as discussed here, little is known about how this anion displacement reaction affects the distribution of cations and other chemical constituents within and phase state of individual SSA particles. Single particle analysis of individual SSA particles shows that cations (Na+, K+, Mg2+ and Ca2+) within individual particles undergo a spatial redistribution after heterogeneous reaction with nitric acid, along with a more concentrated layer of organic matter at the surface of the particle. These data suggest that specific ion and aerosol pH effects play an important role in aerosol particle structure in ways that have not been previously recognized. The ordering of organic coatings can impact trace gas uptake, and subsequently impact trace gas budgets of O3 and NOx.

Wintertime hygroscopicity and volatility of ambient urban aerosol particles

NASA Astrophysics Data System (ADS)

Enroth, Joonas; Mikkilä, Jyri; Németh, Zoltán; Kulmala, Markku; Salma, Imre

2018-04-01

Hygroscopic and volatile properties of atmospheric aerosol particles with dry diameters of (20), 50, 75, 110 and 145 nm were determined in situ by using a volatility-hygroscopicity tandem differential mobility analyser (VH-TDMA) system with a relative humidity of 90 % and denuding temperature of 270 °C in central Budapest during 2 months in winter 2014-2015. The probability density function of the hygroscopic growth factor (HGF) showed a distinct bimodal distribution. One of the modes was characterised by an overall mean HGF of approximately 1.07 (this corresponds to a hygroscopicity parameter κ of 0.033) independently of the particle size and was assigned to nearly hydrophobic (NH) particles. Its mean particle number fraction was large, and it decreased monotonically from 69 to 41 % with particle diameter. The other mode showed a mean HGF increasing slightly from 1.31 to 1.38 (κ values from 0.186 to 0.196) with particle diameter, and it was attributed to less hygroscopic (LH) particles. The mode with more hygroscopic particles was not identified. The probability density function of the volatility GF (VGF) also exhibited a distinct bimodal distribution with an overall mean VGF of approximately 0.96 independently of the particle size, and with another mean VGF increasing from 0.49 to 0.55 with particle diameter. The two modes were associated with less volatile (LV) and volatile (V) particles. The mean particle number fraction for the LV mode decreased from 34 to 21 % with particle diameter. The bimodal distributions indicated that the urban atmospheric aerosol contained an external mixture of particles with a diverse chemical composition. Particles corresponding to the NH and LV modes were assigned mainly to freshly emitted combustion particles, more specifically to vehicle emissions consisting of large mass fractions of soot likely coated with or containing some water-insoluble organic compounds such as non-hygroscopic hydrocarbon-like organics. The hygroscopic

Measurements of phoretic velocities of aerosol particles in microgravity conditions

NASA Astrophysics Data System (ADS)

Prodi, F.; Santachiara, G.; Travaini, S.; Vedernikov, A.; Dubois, F.; Minetti, C.; Legros, J. C.

2006-11-01

Measurements of thermo- and diffusio-phoretic velocities of aerosol particles (carnauba wax, paraffin and sodium chloride) were performed in microgravity conditions (Drop Tower facility, in Bremen, and Parabolic Flights, in Bordeaux). In the case of thermophoresis, a temperature gradient was obtained by heating the upper plate of the cell, while the lower one was maintained at environmental temperature. For diffusiophoresis, the water vapour gradient was obtained with sintered plates imbued with a water solution of MgCl 2 and distilled water, at the top and at the bottom of the cell, respectively. Aerosol particles were observed through a digital holographic velocimeter, a device allowing the determination of 3-D coordinates of particles from the observed volume. Particle trajectories and consequently particle velocities were reconstructed through the analysis of the sequence of particle positions. The experimental values of reduced thermophoretic velocities are between the theoretical values of Yamamoto and Ishihara [Yamamoto, K., Ishihara, Y., 1988. Thermophoresis of a spherical particle in a rarefied gas of a transition regime. Phys. Fluids. 31, 3618-3624] and Talbot et al. [Talbot, L., Cheng, R.K., Schefer, R.W., Willis, D.R., 1980. Thermophoresis of particles in a heated boundary layer. J. Fluid Mech. 101, 737-758], and do not show a clear dependence on the thermal conductivity of the aerosol. The existence of negative thermophoresis is not confirmed in our experiments. Concerning diffusiophoretic experiments, the results obtained show a small increase of reduced diffusiophoretic velocity with the Knudsen number.

Particle deposition in human respiratory system: deposition of concentrated hygroscopic aerosols.

PubMed

Varghese, Suresh K; Gangamma, S

2009-06-01

In the nearly saturated human respiratory tract, the presence of water-soluble substances in the inhaled aerosols can cause change in the size distribution of the particles. This consequently alters the lung deposition profiles of the inhaled airborne particles. Similarly, the presence of high concentration of hygroscopic aerosols also affects the water vapor and temperature profiles in the respiratory tract. A model is presented to analyze these effects in human respiratory system. The model solves simultaneously the heat and mass transfer equations to determine the size evolution of respirable particles and gas-phase properties within human respiratory tract. First, the model predictions for nonhygroscopic aerosols are compared with experimental results. The model results are compared with experimental results of sodium chloride particles. The model reproduces the major features of the experimental data. The water vapor profile is significantly modified only when a high concentration of particles is present. The model is used to study the effect of equilibrium assumptions on particle deposition. Simulations show that an infinite dilution solution assumption to calculate the saturation equilibrium over droplet could induce errors in estimating particle growth. This error is significant in the case of particles of size greater than 1 mum and at number concentrations higher than 10(5)/cm(3).

Investigation of Aerosol Surface Area Estimation from Number and Mass Concentration Measurements: Particle Density Effect.

PubMed

Ku, Bon Ki; Evans, Douglas E

2012-04-01

For nanoparticles with nonspherical morphologies, e.g., open agglomerates or fibrous particles, it is expected that the actual density of agglomerates may be significantly different from the bulk material density. It is further expected that using the material density may upset the relationship between surface area and mass when a method for estimating aerosol surface area from number and mass concentrations (referred to as "Maynard's estimation method") is used. Therefore, it is necessary to quantitatively investigate how much the Maynard's estimation method depends on particle morphology and density. In this study, aerosol surface area estimated from number and mass concentration measurements was evaluated and compared with values from two reference methods: a method proposed by Lall and Friedlander for agglomerates and a mobility based method for compact nonspherical particles using well-defined polydisperse aerosols with known particle densities. Polydisperse silver aerosol particles were generated by an aerosol generation facility. Generated aerosols had a range of morphologies, count median diameters (CMD) between 25 and 50 nm, and geometric standard deviations (GSD) between 1.5 and 1.8. The surface area estimates from number and mass concentration measurements correlated well with the two reference values when gravimetric mass was used. The aerosol surface area estimates from the Maynard's estimation method were comparable to the reference method for all particle morphologies within the surface area ratios of 3.31 and 0.19 for assumed GSDs 1.5 and 1.8, respectively, when the bulk material density of silver was used. The difference between the Maynard's estimation method and surface area measured by the reference method for fractal-like agglomerates decreased from 79% to 23% when the measured effective particle density was used, while the difference for nearly spherical particles decreased from 30% to 24%. The results indicate that the use of particle density

Chemical Composition and Oxidation State of Iron-Containing Aerosol Particles Over West Antarctic Peninsula

NASA Astrophysics Data System (ADS)

Fan, S.; Yu, S.; Lai, B.; Gao, Y.

2017-12-01

Iron is a limiting micronutrient element critical for the marine ecosystem. In the extensive high-nutrient low-chlorophyll (HNLC) regions of the Southern Ocean, the activities of phytoplankton are partly controlled by iron (Fe) from different sources, including atmospheric deposition. Among important properties of atmospheric Fe are the elemental composition and Fe oxidation state of Fe-containing aerosol particles, as these properties affect aerosol Fe solubility. To explore these issues, aerosol samples were collected at Palmer Station in West Antarctic Peninsula. Samples were analyzed by submicron synchrotron-based X-ray fluorescence (XRF) and X-ray absorption near edge structure (XANES) spectroscopy for the Fe oxidation state and elemental composition of aerosol particles. The morphological information of aerosol particles was also observed by the high-resolution fluorescence microscopy, revealing possible sources and formation processes of iron-containing particles. More detailed results will be discussed in this presentation.

Particle interactions of fluticasone propionate and salmeterol xinafoate detected with single particle aerosol mass spectrometry (SPAMS).

PubMed

Jetzer, Martin W; Morrical, Bradley D; Fergenson, David P; Imanidis, Georgios

2017-10-30

Particle co-associations between the active pharmaceutical ingredients fluticasone propionate and salmeterol xinafoate were examined in dry powder inhaled (DPI) and metered dose inhaled (MDI) combination products. Single Particle Aerosol Mass Spectrometry was used to investigate the particle interactions in Advair Diskus ® (500/50 mcg) and Seretide ® (125/25 mcg). A simple rules tree was used to identify each compound, either alone or co-associated at the level of the individual particle, using unique marker peaks in the mass spectra for the identification of each drug. High levels of drug particle co-association (fluticasone-salmeterol) were observed in the aerosols emitted from Advair Diskus ® and Seretide ® . The majority of the detected salmeterol particles were found to be in co-association with fluticasone in both tested devices. Another significant finding was that rather coarse fluticasone particles (in DPI) and fine salmeterol particles (both MDI and DPI) were forming the particle co-associations. Copyright © 2017 Elsevier B.V. All rights reserved.

Trends in sulfate and organic aerosol mass in the Southeast U.S.: Impact on aerosol optical depth and radiative forcing

NASA Astrophysics Data System (ADS)

Attwood, A. R.; Washenfelder, R. A.; Brock, C. A.; Hu, W.; Baumann, K.; Campuzano-Jost, P.; Day, D. A.; Edgerton, E. S.; Murphy, D. M.; Palm, B. B.; McComiskey, A.; Wagner, N. L.; Sá, S. S.; Ortega, A.; Martin, S. T.; Jimenez, J. L.; Brown, S. S.

2014-11-01

Emissions of SO2 in the United States have declined since the early 1990s, resulting in a decrease in aerosol sulfate mass in the Southeastern U.S. of -4.5(±0.9)% yr-1 between 1992 and 2013. Organic aerosol mass, the other major aerosol component in the Southeastern U.S., has decreased more slowly despite concurrent emission reductions in anthropogenic precursors. Summertime measurements in rural Alabama quantify the change in aerosol light extinction as a function of aerosol composition and relative humidity. Application of this relationship to composition data from 2001 to 2013 shows that a -1.1(±0.7)% yr-1 decrease in extinction can be attributed to decreasing aerosol water mass caused by the change in aerosol sulfate/organic ratio. Calculated reductions in extinction agree with regional trends in ground-based and satellite-derived aerosol optical depth. The diurnally averaged summertime surface radiative effect has changed by 8.0 W m-2, with 19% attributed to the decrease in aerosol water.

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.

Spatio-temporal aerosol particle distributions in the UT/LMS measured by the IAGOS-CARIBIC Observatory

NASA Astrophysics Data System (ADS)

Assmann, D. N.; Hermann, M.; Weigelt, A.; Martinsson, B. G.; Brenninkmeijer, C. A. M.; Rauthe-Schoech, A.; van Velthoven, P. J. F.; Boenisch, H.; Zahn, A.

2016-12-01

Submicrometer aerosol particles in the upper troposphere and lowermost stratosphere (UT/LMS) influence the Earth`s radiation budget directly and, more important, indirectly, by acting as cloud condensation nuclei and by changing trace gas concentrations through heterogeneous chemical processes. Since 1997, regular in situ UT/LMS aerosol particle measurements have been conducted by the Leibniz Institute for Tropospheric Research, Leipzig, Germany and the University of Lund, Sweden, using the the CARIBIC (now IAGOS-CARIBIC) observatory (www.caribic-atmospheric.com) onboard a passenger aircraft. Submicrometer aerosol particle number concentrations and the aerosol particle size distribution are measured using three condensation particle counters and one optical particle size spectrometer. Moreover, particle elemental composition is determined using an aerosol impactor sampler and post-flight ion beam analysis (PIXE, PESA) of the samples in the laboratory. Based on this unique data set, including meteorological analysis, we present representative spatio-temporal distributions of particle number, surface, volume, and elemental concentrations in an altitude of 8-12 km covering a large fraction of the northern hemisphere. We discuss the measured values in the different size regimes with respect to sources and sinks in different regions. Additionally, we calculated highly resolved latitudinal and longitudinal cross sections of the particle number size distribution, probability density functions and trends in particle number concentrations, but also in elemental composition, determined from our regular measurements over more than a decade. Moreover, we present the seasonality of particle number concentration in an equivelent latitude - potential temperature coordinate framework (see figure). The results are interpreted with respect to aerosol microphysics and transport using CARIBIC trace gas data like ozone and water vapour. The influence of clouds in the troposphere and

Processing of aerosol particles within the Habshan pollution plume

NASA Astrophysics Data System (ADS)

Semeniuk, T. A.; Bruintjes, R.; Salazar, V.; Breed, D.; Jensen, T.; Buseck, P. R.

2015-03-01

The Habshan industrial site in the United Arab Emirates produces a regional-scale pollution plume associated with oil and gas processing, discharging high loadings of sulfates and chlorides into the atmosphere, which interact with the ambient aerosol population. Aerosol particles and trace gas chemistry at this site were studied on two flights in the summer of 2002. Measurements were collected along vertical plume profiles to show changes associated with atmospheric processing of particle and gas components. Close to the outlet stack, particle concentrations were over 10,000 cm-3, dropping to <2000 cm-3 in more dilute plume around 1500 m above the stack. Particles collected close to the stack and within the dilute plume were individually measured for size, morphology, composition, and mixing state using transmission electron microscopy coupled with energy-dispersive X-ray spectroscopy. Close to the stack, most coarse particles consisted of mineral dust and NaCl crystals from burning oil brines, while sulfate droplets dominated the fine mode. In more dilute plume, at least 1500 m above the stack, the particle spectrum was more diverse, with a significant increase in internally mixed particle types. Dilute plume samples consisted of coarse NaCl/silicate aggregates or NaCl-rich droplets, often with a sulfate component, while fine-fraction particles were of mixed cation sulfates, also internally mixed with nanospherical soot or silicates. Thus, both chloride and sulfate components of the pollution plume rapidly reacted with ambient mineral dust to form coated and aggregate particles, enhancing particle size, hygroscopicity, and reactivity of the coarse mode. The fine-fraction sulfate-bearing particles formed in the plume contribute to regional transport of sulfates, while coarse sulfate-bearing fractions locally reduced the SO2 loading through sedimentation. The chloride- and sulfate-bearing internally mixed particles formed in the plume markedly changed the

Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation

PubMed Central

Shiraiwa, Manabu; Yee, Lindsay D.; Schilling, Katherine A.; Loza, Christine L.; Craven, Jill S.; Zuend, Andreas; Ziemann, Paul J.; Seinfeld, John H.

2013-01-01

Organic aerosols are ubiquitous in the atmosphere and play a central role in climate, air quality, and public health. The aerosol size distribution is key in determining its optical properties and cloud condensation nucleus activity. The dominant portion of organic aerosol is formed through gas-phase oxidation of volatile organic compounds, so-called secondary organic aerosols (SOAs). Typical experimental measurements of SOA formation include total SOA mass and atomic oxygen-to-carbon ratio. These measurements, alone, are generally insufficient to reveal the extent to which condensed-phase reactions occur in conjunction with the multigeneration gas-phase photooxidation. Combining laboratory chamber experiments and kinetic gas-particle modeling for the dodecane SOA system, here we show that the presence of particle-phase chemistry is reflected in the evolution of the SOA size distribution as well as its mass concentration. Particle-phase reactions are predicted to occur mainly at the particle surface, and the reaction products contribute more than half of the SOA mass. Chamber photooxidation with a midexperiment aldehyde injection confirms that heterogeneous reaction of aldehydes with organic hydroperoxides forming peroxyhemiacetals can lead to a large increase in SOA mass. Although experiments need to be conducted with other SOA precursor hydrocarbons, current results demonstrate coupling between particle-phase chemistry and size distribution dynamics in the formation of SOAs, thereby opening up an avenue for analysis of the SOA formation process. PMID:23818634

Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation.

PubMed

Shiraiwa, Manabu; Yee, Lindsay D; Schilling, Katherine A; Loza, Christine L; Craven, Jill S; Zuend, Andreas; Ziemann, Paul J; Seinfeld, John H

2013-07-16

Organic aerosols are ubiquitous in the atmosphere and play a central role in climate, air quality, and public health. The aerosol size distribution is key in determining its optical properties and cloud condensation nucleus activity. The dominant portion of organic aerosol is formed through gas-phase oxidation of volatile organic compounds, so-called secondary organic aerosols (SOAs). Typical experimental measurements of SOA formation include total SOA mass and atomic oxygen-to-carbon ratio. These measurements, alone, are generally insufficient to reveal the extent to which condensed-phase reactions occur in conjunction with the multigeneration gas-phase photooxidation. Combining laboratory chamber experiments and kinetic gas-particle modeling for the dodecane SOA system, here we show that the presence of particle-phase chemistry is reflected in the evolution of the SOA size distribution as well as its mass concentration. Particle-phase reactions are predicted to occur mainly at the particle surface, and the reaction products contribute more than half of the SOA mass. Chamber photooxidation with a midexperiment aldehyde injection confirms that heterogeneous reaction of aldehydes with organic hydroperoxides forming peroxyhemiacetals can lead to a large increase in SOA mass. Although experiments need to be conducted with other SOA precursor hydrocarbons, current results demonstrate coupling between particle-phase chemistry and size distribution dynamics in the formation of SOAs, thereby opening up an avenue for analysis of the SOA formation process.

Demonstration of Aerosol Property Profiling by Multi-wavelength Lidar Under Varying Relative Humidity Conditions

NASA Technical Reports Server (NTRS)

Whiteman, D.N.; Veselovskii, I.; Kolgotin, A.; Korenskii, M.; Andrews, E.

2008-01-01

The feasibility of using a multi-wavelength Mie-Raman lidar based on a tripled Nd:YAG laser for profiling aerosol physical parameters in the planetary boundary layer (PBL) under varying conditions of relative humidity (RH) is studied. The lidar quantifies three aerosol backscattering and two extinction coefficients and from these optical data the particle parameters such as concentration, size and complex refractive index are retrieved through inversion with regularization. The column-integrated, lidar-derived parameters are compared with results from the AERONET sun photometer. The lidar and sun photometer agree well in the characterization of the fine mode parameters, however the lidar shows less sensitivity to coarse mode. The lidar results reveal a strong dependence of particle properties on RH. The height regions with enhanced RH are characterized by an increase of backscattering and extinction coefficient and a decrease in the Angstrom exponent coinciding with an increase in the particle size. We present data selection techniques useful for selecting cases that can support the calculation of hygroscopic growth parameters using lidar. Hygroscopic growth factors calculated using these techniques agree with expectations despite the lack of co-located radiosonde data. Despite this limitation, the results demonstrate the potential of multi-wavelength Raman lidar technique for study of aerosol humidification process.

Particle size distribution of aerosols sprayed from household hand-pump sprays containing fluorine-based and silicone-based compounds.

PubMed

Kawakami, Tsuyoshi; Isama, Kazuo; Ikarashi, Yoshiaki

2015-01-01

Japan has published safety guideline on waterproof aerosol sprays. Furthermore, the Aerosol Industry Association of Japan has adopted voluntary regulations on waterproof aerosol sprays. Aerosol particles of diameter less than 10 µm are considered as "fine particles". In order to avoid acute lung injury, this size fraction should account for less than 0.6% of the sprayed aerosol particles. In contrast, the particle size distribution of aerosols released by hand-pump sprays containing fluorine-based or silicone-based compounds have not been investigated in Japan. Thus, the present study investigated the aerosol particle size distribution of 16 household hand-pump sprays. In 4 samples, the ratio of fine particles in aerosols exceeded 0.6%. This study confirmed that several hand-pump sprays available in the Japanese market can spray fine particles. Since the hand-pump sprays use water as a solvent and their ingredients may be more hydrophilic than those of aerosol sprays, the concepts related to the safety of aerosol-sprays do not apply to the hand pump sprays. Therefore, it may be required for the hand-pump spray to develop a suitable method for evaluating the toxicity and to establish the safety guideline.

Aerosol reduction/expansion synthesis (A-RES) for zero valent metal particles

DOEpatents

Leseman, Zayd; Luhrs, Claudia; Phillips, Jonathan; Soliman, Haytham

2016-04-12

Various embodiments provide methods of forming zero valent metal particles using an aerosol-reductive/expansion synthesis (A-RES) process. In one embodiment, an aerosol stream including metal precursor compound(s) and chemical agent(s) that produces reducing gases upon thermal decomposition can be introduced into a heated inert atmosphere of a RES reactor to form zero valent metal particles corresponding to metals used for the metal precursor compound(s).

In-Situ Measurements of Aerosol Optical Properties using New Cavity Ring-Down and Photoacoustics Instruments and Comparison with more Traditional Techniques

NASA Technical Reports Server (NTRS)

Strawa, A. W.; Arnott, P.; Covert, D.; Elleman, R.; Ferrare, R.; Hallar, A. G.; Jonsson, H.; Kirchstetter, T. W.; Luu, A. P.; Ogren, J.

2004-01-01

Carbonaceous species (BC and OC) are responsible for most of the absorption associated with aerosol particles. The amount of radiant energy an aerosol absorbs has profound effects on climate and air quality. It is ironic that aerosol absorption coefficient is one of the most difficult aerosol properties to measure. A new cavity ring-down (CRD) instrument, called Cadenza (NASA-ARC), measures the aerosol extinction coefficient for 675 nm and 1550 nm light, and simultaneously measures the scattering coefficient at 675 nm. Absorption coefficient is obtained from the difference of measured extinction and scattering within the instrument. Aerosol absorption coefficient is also measured by a photoacoustic (PA) instrument (DRI) that was operated on an aircraft for the first time during the DOE Aerosol Intensive Operating Period (IOP). This paper will report on measurements made with this new instrument and other in-situ instruments during two field recent field studies. The first field study was an airborne cam;oaign, the DOE Aerosol Intensive Operating Period flown in May, 2003 over northern Oklahoma. One of the main purposes of the IOP was to assess our ability to measure extinction and absorption coefficient in situ. This paper compares measurements of these aerosol optical properties made by the CRD, PA, nephelometer, and Particle Soot Absorption Photometer (PSAP) aboard the CIRPAS Twin-Otter. During the IOP, several significant aerosol layers were sampled aloft. These layers are identified in the remote (AATS-14) as well as in situ measurements. Extinction profiles measured by Cadenza are compared to those derived from the Ames Airborne Tracking Sunphotometer (AATS-14, NASA-ARC). The regional radiative impact of these layers is assessed by using the measured aerosol optical properties in a radiative transfer model. The second study was conducted in the Caldecott Tunnel, a heavily-used tunnel located north of San Francisco, Ca. The aerosol sampled in this study was

Reduced anthropogenic aerosol radiative forcing caused by biogenic new particle formation

NASA Astrophysics Data System (ADS)

Gordon, Hamish; Sengupta, Kamalika; Rap, Alexandru; Duplissy, Jonathan; Frege, Carla; Williamson, Christina; Heinritzi, Martin; Simon, Mario; Yan, Chao; Almeida, João; Tröstl, Jasmin; Nieminen, Tuomo; Ortega, Ismael K.; Wagner, Robert; Dunne, Eimear M.; Adamov, Alexey; Amorim, Antonio; Bernhammer, Anne-Kathrin; Bianchi, Federico; Breitenlechner, Martin; Brilke, Sophia; Chen, Xuemeng; Craven, Jill S.; Dias, Antonio; Ehrhart, Sebastian; Fischer, Lukas; Flagan, Richard C.; Franchin, Alessandro; Fuchs, Claudia; Guida, Roberto; Hakala, Jani; Hoyle, Christopher R.; Jokinen, Tuija; Junninen, Heikki; Kangasluoma, Juha; Kim, Jaeseok; Kirkby, Jasper; Krapf, Manuel; Kürten, Andreas; Laaksonen, Ari; Lehtipalo, Katrianne; Makhmutov, Vladimir; Mathot, Serge; Molteni, Ugo; Monks, Sarah A.; Onnela, Antti; Peräkylä, Otso; Piel, Felix; Petäjä, Tuukka; Praplan, Arnaud P.; Pringle, Kirsty J.; Richards, Nigel A. D.; Rissanen, Matti P.; Rondo, Linda; Sarnela, Nina; Schobesberger, Siegfried; Scott, Catherine E.; Seinfeld, John H.; Sharma, Sangeeta; Sipilä, Mikko; Steiner, Gerhard; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Virtanen, Annele; Vogel, Alexander Lucas; Wagner, Andrea C.; Wagner, Paul E.; Weingartner, Ernest; Wimmer, Daniela; Winkler, Paul M.; Ye, Penglin; Zhang, Xuan; Hansel, Armin; Dommen, Josef; Donahue, Neil M.; Worsnop, Douglas R.; Baltensperger, Urs; Kulmala, Markku; Curtius, Joachim; Carslaw, Kenneth S.

2016-10-01

The magnitude of aerosol radiative forcing caused by anthropogenic emissions depends on the baseline state of the atmosphere under pristine preindustrial conditions. Measurements show that particle formation in atmospheric conditions can occur solely from biogenic vapors. Here, we evaluate the potential effect of this source of particles on preindustrial cloud condensation nuclei (CCN) concentrations and aerosol-cloud radiative forcing over the industrial period. Model simulations show that the pure biogenic particle formation mechanism has a much larger relative effect on CCN concentrations in the preindustrial atmosphere than in the present atmosphere because of the lower aerosol concentrations. Consequently, preindustrial cloud albedo is increased more than under present day conditions, and therefore the cooling forcing of anthropogenic aerosols is reduced. The mechanism increases CCN concentrations by 20-100% over a large fraction of the preindustrial lower atmosphere, and the magnitude of annual global mean radiative forcing caused by changes of cloud albedo since 1750 is reduced by 0.22 W m-2 (27%) to -0.60 W m-2. Model uncertainties, relatively slow formation rates, and limited available ambient measurements make it difficult to establish the significance of a mechanism that has its dominant effect under preindustrial conditions. Our simulations predict more particle formation in the Amazon than is observed. However, the first observation of pure organic nucleation has now been reported for the free troposphere. Given the potentially significant effect on anthropogenic forcing, effort should be made to better understand such naturally driven aerosol processes.

Aircraft- and ground-based assessment of the CCN-AOD relationship and implications on model analysis of ACI and underlying aerosol processes

NASA Astrophysics Data System (ADS)

Shinozuka, Y.; Clarke, A. D.; Nenes, A.; Lathem, T. L.; Redemann, J.; Jefferson, A.; Wood, R.

2014-12-01

Contrary to common assumptions in satellite-based modeling of aerosol-cloud interactions, ∂logCCN/∂logAOD is less than unity, i.e., the number concentration of cloud condensation nuclei (CCN) less than doubles as aerosol optical depth (AOD) doubles. This can be explained by omnipresent aerosol processes. Condensation, coagulation and cloud processing, for example, generally make particles scatter more light while hardly increasing their number. This paper reports on the relationship in local air masses between CCN concentration, aerosol size distribution and light extinction observed from aircraft and the ground at diverse locations. The CCN-to-local-extinction relationship, when averaged over ~1 km distance and sorted by the wavelength dependence of extinction, varies approximately by a factor of 2, reflecting the variability in aerosol intensive properties. This, together with retrieval uncertainties and the variability in aerosol spatio-temporal distribution and hygroscopic growth, challenges satellite-based CCN estimates. However, the large differences in estimated CCN may correspond to a considerably lower uncertainty in cloud drop number concentration (CDNC), given the sublinear response of CDNC to CCN. Overall, our findings from airborne and ground-based observations call for model-based reexamination of aerosol-cloud interactions and underlying aerosol processes.

Individual Aerosol Particles from Biomass Burning in Southern Africa Compositions and Aging of Inorganic Particles. 2; Compositions and Aging of Inorganic Particles

NASA Technical Reports Server (NTRS)

Li, Jia; Posfai, Mihaly; Hobbs, Peter V.; Buseck, Peter R.

2003-01-01

Individual aerosol particles collected over southern Africa during the SAFARI 2000 field study were studied using transmission electron microscopy and field-emission scanning electron microscopy. The sizes, shapes, compositions, mixing states, surface coatings, and relative abundances of aerosol particles from biomass burning, in boundary layer hazes, and in the free troposphere were compared, with emphasis on aging and reactions of inorganic smoke particles. Potassium salts and organic particles were the predominant species in the smoke, and most were internally mixed. More KCl particles occur in young smoke, whereas more K2SO4 and KNO3 particles were present in aged smoke. This change indicates that with the aging of the smoke, KCl particles from the fires were converted to K2SO4 and KNO3 through reactions with sulfur- and nitrogen- bearing species from biomass burning as well as other sources. More soot was present in smoke from flaming grass fires than bush and wood fires, probably due to the predominance of flaming combustion in grass fires. The high abundance of organic particles and soluble salts can affect the hygroscopic properties of biomass-burning aerosols and therefore influence their role as cloud condensation nuclei. Particles from biomass burning were important constituents of the regional hazes.

Microspectroscopic Analysis of Anthropogenic- and Biogenic-Influenced Aerosol Particles during the SOAS Field Campaign

NASA Astrophysics Data System (ADS)

Ault, A. P.; Bondy, A. L.; Nhliziyo, M. V.; Bertman, S. B.; Pratt, K.; Shepson, P. B.

2013-12-01

During the summer, the southeastern United States experiences a cooling haze due to the interaction of anthropogenic and biogenic aerosol sources. An objective of the summer 2013 Southern Oxidant and Aerosol Study (SOAS) was to improve our understanding of how trace gases and aerosols are contributing to this relative cooling through light scattering and absorption. To improve understanding of biogenic-anthropogenic interactions through secondary organic aerosol (SOA) formation on primary aerosol cores requires detailed physicochemical characterization of the particles after uptake and processing. Our measurements focus on single particle analysis of aerosols in the accumulation mode (300-1000 nm) collected using a multi orifice uniform deposition impactor (MOUDI) at the Centreville, Alabama SEARCH site. Particles were characterized using an array of microscopic and spectroscopic techniques, including: scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy dispersive X-ray analysis (EDX), and Raman microspectroscopy. These analyses provide detailed information on particle size, morphology, elemental composition, and functional groups. This information is combined with mapping capabilities to explore individual particle spatial patterns and how that impacts structural characteristics. The improved understanding will be used to explore how sources and processing (such as SOA coating of soot) change particle structure (i.e. core shell) and how the altered optical properties impact air quality/climate effects on a regional scale.

Thermophoretic separation of aerosol particles from a sampled gas stream

DOEpatents

Postma, A.K.

1984-09-07

This disclosure relates to separation of aerosol particles from gas samples withdrawn from within a contained atmosphere, such as containment vessels for nuclear reactors or other process equipment where remote gaseous sampling is required. It is specifically directed to separation of dense aerosols including particles of any size and at high mass loadings and high corrosivity. The United States Government has rights in this invention pursuant to Contract DE-AC06-76FF02170 between the US Department of Energy and Westinghouse Electric Corporation.

Gas-particle partitioning of alcohol vapors on organic aerosols.

PubMed

Chan, Lap P; Lee, Alex K Y; Chan, Chak K

2010-01-01

Single particle levitation using an electrodynamic balance (EDB) has been found to give accurate and direct hygroscopic measurements (gas-particle partitioning of water) for a number of inorganic and organic aerosol systems. In this paper, we extend the use of an EDB to examine the gas-particle partitioning of volatile to semivolatile alcohols, including methanol, n-butanol, n-octanol, and n-decanol, on levitated oleic acid particles. The measured K(p) agreed with Pankow's absorptive partitioning model. At high n-butanol vapor concentrations (10(3) ppm), the uptake of n-butanol reduced the average molecular-weight of the oleic acid particle appreciably and hence increased the K(p) according to Pankow's equation. Moreover, the hygroscopicity of mixed oleic acid/n-butanol particles was higher than the predictions given by the UNIFAC model (molecular group contribution method) and the ZSR equation (additive rule), presumably due to molecular interactions between the chemical species in the mixed particles. Despite the high vapor concentrations used, these findings warrant further research on the partitioning of atmospheric organic vapors (K(p)) near sources and how collectively they affect the hygroscopic properties of organic aerosols.

The physico-chemical evolution of atmospheric aerosols and the gas-particle partitioning of inorganic aerosol during KORUS-AQ

NASA Astrophysics Data System (ADS)

Lee, T.; Park, T.; Lee, J. B.; Lim, Y. J.; Ahn, J.; Park, J. S.; Soo, C. J.; Desyaterik, Y.; Collett, J. L., Jr.

2017-12-01

Aerosols influence climate change directly by scattering and absorption and indirectly by acting as cloud condensation nuclei and some of the effects of aerosols are reduction in visibility, deterioration of human health, and deposition of pollutants to ecosystems. Urban area is large source of aerosols and aerosol precursors. Aerosol sources are both local and from long-range transport. Long-range transport processed aerosol are often dominant sources of aerosol pollution in Korea. To improve our knowledge of aerosol chemistry, Korea and U.S-Air Quality (KORUS-AQ) of Aircraft-based aerosol measurement took place in and around Seoul, Korea during May and June 2016. KORUS-AQ campaigns were conducted to study the chemical characterization and processes of pollutants in the Seoul Metropolitan area to regional scales of Korean peninsula. Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed on aircraft platforms on-board DC-8 (NASA) aircraft. We characterized aerosol chemical properties and mass concentrations of sulfate, nitrate, ammonium and organics in polluted air plumes and investigate the spatial and vertical distribution of the species. The results of studies show that organics is predominant in Aerosol and a significant fraction of the organics is oxygenated organic aerosol (OOA) at the high altitude. Both Nitrate and sulfate can partition between the gas and particle phases. The ratios for HNO3/(N(V) (=gaseous HNO3 + particulate Nitrate) and SO2/(SO2+Sulfate) were found to exhibit quite different distributions between the particles and gas phase for the locations during KORUS-AQ campaign, representing potential for formation of additional particulate nitrate and sulfate. The results of those studies can provide highly resolved temporal and spatial air pollutant, which are valuable for air quality model input parameters for aerosol behaviour.

Stratospheric Aerosol Measurements

NASA Technical Reports Server (NTRS)

Pueschel, Rudolf, F.; Gore, Warren J. (Technical Monitor)

1998-01-01

Stratospheric aerosols affect the atmospheric energy balance by scattering and absorbing solar and terrestrial radiation. They also can alter stratospheric chemical cycles by catalyzing heterogeneous reactions which markedly perturb odd nitrogen, chlorine and ozone levels. Aerosol measurements by satellites began in NASA in 1975 with the Stratospheric Aerosol Measurement (SAM) program, to be followed by the Stratospheric Aerosol and Gas Experiment (SAGE) starting in 1979. Both programs employ the solar occultation, or Earth limb extinction, techniques. Major results of these activities include the discovery of polar stratospheric clouds (PSCs) in both hemispheres in winter, illustrations of the impacts of major (El Chichon 1982 and Pinatubo 1991) eruptions, and detection of a negative global trend in lower stratospheric/upper tropospheric aerosol extinction. This latter result can be considered a triumph of successful worldwide sulfur emission controls. The SAGE record will be continued and improved by SAGE III, currently scheduled for multiple launches beginning in 2000 as part of the Earth Observing System (EOS). The satellite program has been supplemented by in situ measurements aboard the ER-2 (20 km ceiling) since 1974, and from the DC-8 (13 km ceiling) aircraft beginning in 1989. Collection by wire impactors and subsequent electron microscopic and X-ray energy-dispersive analyses, and optical particle spectrometry have been the principle techniques. Major findings are: (1) The stratospheric background aerosol consists of dilute sulfuric acid droplets of around 0.1 micrometer modal diameter at concentration of tens to hundreds of monograms per cubic meter; (2) Soot from aircraft amounts to a fraction of one percent of the background total aerosol; (3) Volcanic eruptions perturb the sulfuric acid, but not the soot, aerosol abundance by several orders of magnitude; (4) PSCs contain nitric acid at temperatures below 195K, supporting chemical hypotheses

Glyoxal and Methylglyoxal in Atlantic Seawater and marine Aerosol Particles

NASA Astrophysics Data System (ADS)

van Pinxteren, Manuela; Herrmann, Hartmut

2014-05-01

The two α-dicarbonyls glyoxal (CHOCHO; GLY) and methylglyoxal (CH3COCHO; MGLY) have attracted increasing attention over the past years because of their potential role in secondary organic aerosol formation. Recently Sinreich et al. (2010) suggested the open ocean as an important (so far unknown) source for GLY in the atmosphere. To date, there are few available field data of these compounds in the marine area. In this study we present measurements of GLY and MGLY in seawater and marine aerosol particles sampled during a transatlantic Polarstern cruise in spring 2011. In seawater we especially investigated the sea surface microlayer (sampled with the glass plate technique) as it is the direct interface between ocean and atmosphere. Analytical measurements were based on derivatisation with o-(2,3,4,5,6-Pentafluorobenzyl)-hydroxylamine reagent, solvent extraction and GC-MS (SIM) analysis. The results show that GLY and MGLY are present in the sea surface microlayer of the ocean and corresponding bulkwater with average concentrations of 228 ng L-1 (GLY) and 196 ng L-1 (MGLY). Significant enrichment (factor of 4) of GLY and MGLY in the sea surface microlayer was found implying photochemical production of the two carbonyls though a clear connection to global radiation was not observed. On aerosol particles, both carbonyls were detected (average concentration 0.2 ng m-3) and are strongly connected to each other, suggesting similar formation mechanisms. Both carbonyls show a very good correlation with particulate oxalate, supporting the idea of a secondary formation of oxalic acid via GLY and MGLY. A slight correlation of the two carbonyls in the sea surface microlayer and in the aerosol particles was found at co-located sampling areas. In summary, the results of GLY and MGLY in marine aerosol particles and in the oceanic water give first insights towards interaction processes of these alpha dicarbonyls between ocean and atmosphere (van Pinxteren and Herrmann (2013

Aerosol Particle Interfacial Thermodynamics and Phase Partitioning Measurements Using Biphasic Microfluidics

NASA Astrophysics Data System (ADS)

Dutcher, Cari; Metcalf, Andrew

2015-03-01

Secondary organic aerosol particles are nearly ubiquitous in the atmosphere and yet there remain large uncertainties in their formation processes and ambient properties. These particles are complex microenvironments, which can contain multiple interfaces due to internal aqueous-organic phase partitioning and to the external liquid-vapor surface. Interfacial properties affect the ambient aerosol morphology, or internal structure of the particle, which in turn can affect the way a particle interacts with an environment of condensable clusters and organic vapors. To improve our ability to accurately predict ambient aerosol morphology, we must improve our knowledge of aerosol interfaces and their interactions with the ambient environment. Unfortunately, many techniques employed to measure interfacial properties do so in bulk solutions or in the presence of a ternary (e.g. solid) phase. In this talk, a novel method using biphasic microscale flows will be introduced for generating, trapping, and perturbing complex interfaces at atmospherically relevant conditions. These microfluidic experiments utilize high-speed imaging to monitor interfacial phenomena at the microscale and are performed with phase contrast and fluorescence microscopy on a temperature-controlled inverted microscope stage. From these experiments, interfacial thermodynamic properties such as surface or interfacial tension, rheological properties such as interfacial moduli, and kinetic properties such as mass transfer coefficients can be measured or inferred.

Optical and chemical properties of wildland biomass burning particles measured downwind during the BBOP study

NASA Astrophysics Data System (ADS)

Onasch, Timothy; Wormhoudt, Jody; Sedlacek, Arthur; Chand, Duli; Freedman, Andrew

2017-04-01

Rapid physical, chemical and optical changes in biomass burning particles were measured downwind (< 3 hours temporally) from wildland fires. The Biomass Burning Observation Project (BBOP), sponsored by the U.S. Department of Energy (DOE), involved the measurement of emissions from wildland fires in the Pacific Northwest and agricultural burns in the Central Southeastern United States observed from the DOE Gulfstream-1 airborne platform over a four month period in 2013. Optical instrumentation included a CAPS PMex particle extinction monitor operating at 630 nm (Aerodyne Research), a photothermal interferometer (Brookhaven National Laboratory) measuring particle absorption at 632 nm and a 3 wavelength nephelometer (TSI). Information about the chemical evolution of the plumes was obtained primarily using a SP-AMS (Aerodyne Research) and a Single Particle Soot Photometer (SP2, Droplet Measurements). The chemical composition of the particulate emissions were characterized in the context of the fire location, combustion conditions, and optical property measurements, including extinction and single scattering albedos. The chemical composition of organic aerosol was found to be rapidly changing as a function of downwind location, with oxygen to carbon ratios increasing as a results of atmospheric aging processes (e.g., dilution, photochemistry). The single scattering albedo, (SSA) of plume aerosols increases downwind as the ratio of total particle extinction to carbon monoxide concentration (a marker for the plume dilution) increases, a finding that is related to changes in organic aerosol chemistry.

Improved solution of the lidar equation utilizing particle counter measurements

NASA Technical Reports Server (NTRS)

Jaeger, H.; Hofmann, D. J.; Jaeger, H.; Hofmann, D. J.

1986-01-01

The extraction of particle backscattering from incoherent lidar measurements poses some problems. In the case of measurements of the stratospheric aerosol layer the solution of the lidar equation is based on two assumptions which are necessary to normalize the measured signal and to correct it with the two-way transmission of the laser pulse. Normalization and transmission are tackled by adding the information contained in aerosol particle counter measurements of the University of Wyoming to the ruby lidar measurements at Garmisch-Partenkirchen. Calculated backscattering from height levels above 25 km for the El Chichon period will be compared with lidar measurements and necessary corrections. The calculated backscatter-to-extinction ratios are compared to those, which were derived from a comparison of published extinction values to measured lidar backscattering at Garmisch. These ratios were used to calculate the Garmisch lidar returns. For the period 4 to 12 months after the El Chichon eruption a backscater-to-extinction ratio of 0.026 1/sr was applied with smaller values before and after that time.

Particle Size Distribution of Serratia marcescens Aerosols Created During Common Laboratory Procedures and Simulated Laboratory Accidents

PubMed Central

Kenny, Michael T.; Sabel, Fred L.

1968-01-01

Andersen air samplers were used to determine the particle size distribution of Serratia marcescens aerosols created during several common laboratory procedures and simulated laboratory accidents. Over 1,600 viable particles per cubic foot of air sampled were aerosolized during blending operations. More than 98% of these particles were less than 5 μ in size. In contrast, 80% of the viable particles aerosolized by handling lyophilized cultures were larger than 5 μ. Harvesting infected eggs, sonic treatment, centrifugation, mixing cultures, and dropping infectious material produced aerosols composed primarily of particles in the 1.0- to 7.5-μ size range. Images Fig. 1 PMID:4877498

Comparisons of Airborne HSRL and Modeled Aerosol Profiles

NASA Astrophysics Data System (ADS)

Ferrare, R. A.; Burton, S. P.; Hostetler, C. A.; Hair, J. W.; Ismail, S.; Rogers, R. R.; Notari, A.; Berkoff, T.; Butler, C. F.; Collins, J. E., Jr.; Fenn, M. A.; Scarino, A. J.; Clayton, M.; Mueller, D.; Chemyakin, E.; Fast, J. D.; Berg, L. K.; Randles, C. A.; Colarco, P. R.; daSilva, A.

2014-12-01

Aerosol profiles derived from a regional and a global model are compared with aerosol profiles acquired by NASA Langley Research Center (LaRC) airborne High Spectral Resolution Lidars (HSRLs) during recent field missions. We compare simulated aerosol profiles obtained from the WRF-Chem regional model with those measured by the airborne HSRL-2 instrument over the Atlantic Ocean east of Cape Cod in July 2012 during the Department of Energy Two-Column Aerosol Project (TCAP). While deployed on the LaRC King Air during TCAP, HSRL-2 acquired profiles of aerosol extinction at 355 and 532 nm, as well as aerosol backscatter and depolarization at 355, 532, and 1064 nm. Additional HSRL-2 data products include profiles of aerosol type, mixed layer depth, and aerosol microphysical parameters (e.g. effective radius, concentration). The HSRL-2 and WRF-Chem aerosol profiles are compared along the aircraft flight tracks. HSRL-2 profiles acquired during the NASA Deriving Information on Surface Conditions from COlumn and VERtically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) mission over Houston during September 2013 are compared with the NASA Goddard Earth Observing System global model, version 5 (GEOS-5) profiles. In addition to comparing backscatter and extinction profiles, the fraction of aerosol extinction and optical thickness from various aerosol species from GEOS-5 are compared with aerosol extinction and optical thickness contributed by aerosol types derived from HSRL-2 data. We also compare aerosol profiles modeled by GEOS-5 with those measured by the airborne LaRC DIAL/HSRL instrument during August and September 2013 when it was deployed on the NASA DC-8 for the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) mission. DIAL/HSRL measured extinction (532 nm), backscatter (532 and 1064 nm), and depolarization profiles (532 and 1064 nm) in both nadir and zenith directions during long transects over the

Decomposition of Atmospheric Aerosol Phase Function by Particle Size and Morphology via Single Particle Scattering Measurements

NASA Astrophysics Data System (ADS)

Aptowicz, K. B.; Pan, Y.; Martin, S.; Fernandez, E.; Chang, R.; Pinnick, R. G.

2013-12-01

We report upon an experimental approach that provides insight into how particle size and shape affect the scattering phase function of atmospheric aerosol particles. Central to our approach is the design of an apparatus that measures the forward and backward scattering hemispheres (scattering patterns) of individual atmospheric aerosol particles in the coarse mode range. The size and shape of each particle is discerned from the corresponding scattering pattern. In particular, autocorrelation analysis is used to differentiate between spherical and non-spherical particles, the calculated asphericity factor is used to characterize the morphology of non-spherical particles, and the integrated irradiance is used for particle sizing. We found the fraction of spherical particles decays exponentially with particle size, decreasing from 11% for particles on the order of 1 micrometer to less than 1% for particles over 5 micrometer. The average phase functions of subpopulations of particles, grouped by size and morphology, are determined by averaging their corresponding scattering patterns. The phase functions of spherical and non-spherical atmospheric particles are shown to diverge with increasing size. In addition, the phase function of non-spherical particles is found to vary little as a function of the asphericity factor.

Seasonal variations of aerosol optical properties, vertical distribution and associated radiative effects in the Yangtze Delta Region of China

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

Liu, Jianjun; Zheng, Youfei; Li, Zhanqing

2012-02-09

Four years of columnar aerosol particle optical properties (2006 to 2009) and one year database worth of aerosol particle vertical profile of 527 nm extinction coefficient (June 2008 to May 2009) are analyzed at Taihu in the central Yangtze Delta region in eastern China. Seasonal variations of aerosol optical properties, vertical distribution, and influence on shortwave radiation and heating rates were investigated. Multiyear variations of aerosol optical depths (AOD), Angstrom exponents, single scattering albedo (SSA) and asymmetry factor (ASY) are analyzed, together with the vertical profile of aerosol extinction. AOD is largest in summer and smallest in winter. SSAs exhibitmore » weak seasonal variation with the smallest values occurring during winter and the largest during summer. The vast majority of aerosol particles are below 2 km, and about 62%, 67%, 67% and 83% are confined to below 1 km in spring, summer, autumn and winter, respectively. Five-day back trajectory analyses show that the some aerosols aloft are traced back to northern/northwestern China, as far as Mongolia and Siberia, in spring, autumn and winter. The presence of dust aerosols were identified based on the linear depolarization measurements together with other information (i.e., back trajectory, precipitation, aerosol index). Dust strongly impacts the vertical particle distribution in spring and autumn, with much smaller effects in winter. The annual mean aerosol direct shortwave radiative forcing (efficiency) at the bottom, top and within the atmosphere are -34.8 {+-} 9.1 (-54.4 {+-} 5.3), -8.2 {+-} 4.8 (-13.1 {+-} 1.5) and 26.7 {+-} 9.4 (41.3 {+-} 4.6) W/m{sup 2} (Wm{sup -2} T{sup -1}), respectively. The mean reduction in direct and diffuse radiation reaching surface amount to 109.2 {+-} 49.4 and 66.8 {+-} 33.3 W/m{sup 2}, respectively. Aerosols significantly alter the vertical profile of solar heating, with great implications for atmospheric stability and dynamics within the lower

Particle Effects On The Extinction And Ignition Of Flames In Normal- And Micro-Gravity

NASA Technical Reports Server (NTRS)

Andac, M. G.; Egolfopoulos, F. N.; Campbell, C. S.

2003-01-01

Reacting dusty flows have been studied to lesser extent than pure gas phase flows and sprays. Particles can significantly alter the ignition, burning and extinction characteristics of the gas phase due to the dynamic, thermal, and chemical couplings between the phases. The understanding of two-phase flows can be attained in stagnation flow configurations, which have been used to study spray combustion [e.g. 1] as well as reacting dusty flows [e.g. 2]. The thermal coupling between inert particles and a gas, as well as the effect of gravity, were studied in Ref. 3. It was also shown that the gravity can substantially affect parameters such as the particle velocity, number density, mass flux, and temperature. In Refs. 4 and 5, the effects of inert particles on the extinction of strained premixed and nonpremixed flames were studied both experimentally and numerically at 1-g and m-g. It was shown that large particles can cool flames more effectively than smaller particles. The effects of flame configuration and particle injection orientation were also addressed. It was shown that it was not possible to obtain a simple and still meaningful scaling that captured all the pertinent physics due to the complexity of the couplings between parameters. Also, the cooling by particles is more profound in the absence of gravity as gravity works to reduce the particle number density in the neighborhood of the flame. The efforts were recently shifted towards the understanding of the effects of combustible particles on extinction [6], the gas-phase ignition by hot particle injection [7], and the hot gas ignition of flames in the presence of particles that are not hot enough to ignite the gas phase by themselves.

Investigation of Aerosol Surface Area Estimation from Number and Mass Concentration Measurements: Particle Density Effect

PubMed Central

Ku, Bon Ki; Evans, Douglas E.

2015-01-01

For nanoparticles with nonspherical morphologies, e.g., open agglomerates or fibrous particles, it is expected that the actual density of agglomerates may be significantly different from the bulk material density. It is further expected that using the material density may upset the relationship between surface area and mass when a method for estimating aerosol surface area from number and mass concentrations (referred to as “Maynard’s estimation method”) is used. Therefore, it is necessary to quantitatively investigate how much the Maynard’s estimation method depends on particle morphology and density. In this study, aerosol surface area estimated from number and mass concentration measurements was evaluated and compared with values from two reference methods: a method proposed by Lall and Friedlander for agglomerates and a mobility based method for compact nonspherical particles using well-defined polydisperse aerosols with known particle densities. Polydisperse silver aerosol particles were generated by an aerosol generation facility. Generated aerosols had a range of morphologies, count median diameters (CMD) between 25 and 50 nm, and geometric standard deviations (GSD) between 1.5 and 1.8. The surface area estimates from number and mass concentration measurements correlated well with the two reference values when gravimetric mass was used. The aerosol surface area estimates from the Maynard’s estimation method were comparable to the reference method for all particle morphologies within the surface area ratios of 3.31 and 0.19 for assumed GSDs 1.5 and 1.8, respectively, when the bulk material density of silver was used. The difference between the Maynard’s estimation method and surface area measured by the reference method for fractal-like agglomerates decreased from 79% to 23% when the measured effective particle density was used, while the difference for nearly spherical particles decreased from 30% to 24%. The results indicate that the use of

Hygrosopicity measurements of aerosol particles in the San Joaquin Valley, CA, Baltimore, MD, and Golden, CO

NASA Astrophysics Data System (ADS)

Orozco, Daniel; Beyersdorf, A. J.; Ziemba, L. D.; Berkoff, T.; Zhang, Q.; Delgado, R.; Hennigan, C. J.; Thornhill, K. L.; Young, D. E.; Parworth, C.; Kim, H.; Hoff, R. M.

2016-06-01

Aerosol hygroscopicity was investigated using a novel dryer-humidifier system, coupled to a TSI-3563 nephelometer, to obtain the light scattering coefficient (σscat) as a function of relative humidity (RH) in hydration and dehydration modes. The measurements were performed in Porterville, CA (10 January to 6 February 2013), Baltimore, MD (3-30 July 2013), and Golden, CO (12 July to 10 August 2014). Observations in Porterville and Golden were part of the NASA-sponsored Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality project. The measured σscat under varying RH in the three sites was combined with ground aerosol extinction, PM2.5 mass concentrations, and particle composition measurements and compared with airborne observations performed during campaigns. The enhancement factor, f(RH), defined as the ratio of σscat(RH) at a certain RH divided by σscat at a dry value, was used to evaluate the aerosol hygroscopicity. Particles in Porterville showed low average f(RH = 80%) (1.42) which was attributed to the high carbonaceous loading in the region where residential biomass burning and traffic emissions contribute heavily to air pollution. In Baltimore, the high average f(RH = 80%) (2.06) was attributed to the large contribution of SO42- in the region. The lowest water uptake was observed in Golden, with an average f(RH = 80%) = 1.24 where organic carbon dominated the particle loading. Different empirical fits were evaluated using the f(RH) data. The widely used Kasten (gamma) model was found least satisfactory, as it overestimates f(RH) for RH < 75%. A better empirical fit with two power law curve fitting parameters c and k was found to replicate f(RH) accurately from the three sites. The relationship between the organic carbon mass and the species that are affected by RH and f(RH) was also studied and categorized.

T-matrix Study of Scattering and Absorption of Light by Biomass Burning Aerosols

NASA Astrophysics Data System (ADS)

Poudel, Samin

The uncertainty in the measurements of aerosol optical properties has made it difficult to quantify the global impact of aerosols on Earth's climate and limits our ability to predict future climate changes. Morphology, size, volume, shape, fuel type, burning conditions, aging, and changes in chemical composition due to atmospheric processing of soot play a significant part in determining the optical properties of aerosols. The T-matrix method has been successfully used to reproduce experimental results of optical properties of spherical and non-spherical particles. In this work we applied the T-matrix method to extract the refractive index of biomass burning soot (burning pine tree) by reproducing experimentally determined single scattering albedo (SSA), scattering and extinction cross section values obtained by burning pine and collecting aerosols in two different ways: (1) from an outdoor burn drum to burn pine and collect soot in distilled water using an impinger and re-aerosolized the soot after several days to measure extinction and scattering cross sections using cavity ring down spectroscopy and nephelometry and (2) from a tube furnace in the lab to burn pine and the soot was introduced into an indoor smog chamber and soot particles sampled directly into the cavity ring down system and the nephelometer to measure extinction and scattering cross sections. Filter samples were also collected from both types of burning and electron microscopy images were used to obtain morphology and size information to conduct T-Matrix calculations. The experimentally measured optical properties from the impinger samples were reproduced using a refractive index of 1.345 + i0.096 for 300 and 400nm particles, while the results from the tube furnace samples were reproduced using 1.88 + i0.024 for 200 nm particles and 1.47 + i0.047 for 300 nm particles. This suggests that the impinger samples do not represent fresh soot since they are more absorbing and have lower SSA values

Satellite stratospheric aerosol measurement validation

NASA Technical Reports Server (NTRS)

Russell, P. B.; Mccormick, M. P.

1984-01-01

The validity of the stratospheric aerosol measurements made by the satellite sensors SAM II and SAGE was tested by comparing their results with each other and with results obtained by other techniques (lider, dustsonde, filter, and impactor). The latter type of comparison required the development of special techniques that convert the quantity measured by the correlative sensor (e.g. particle backscatter, number, or mass) to that measured by the satellite sensor (extinction) and quantitatively estimate the uncertainty in the conversion process. The results of both types of comparisons show agreement within the measurement and conversion uncertainties. Moreover, the satellite uncertainty is small compared to aerosol natural variability (caused by seasonal changes, volcanoes, sudden warmings, and vortex structure). It was concluded that the satellite measurements are valid.

Characterizing the Vertical Distribution of Aerosols Over the ARM SGP Site

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

Richard Ferrare, Connor Flynn, David Turner

This project focused on: 1) evaluating the performance of the DOE ARM SGP Raman lidar system in measuring profiles of water vapor and aerosols, and 2) the use of the Raman lidar measurements of aerosol and water vapor profiles for assessing the vertical distribution of aerosols and water vapor simulated by global transport models and examining diurnal variability of aerosols and water vapor. The highest aerosol extinction was generally observed close to the surface during the nighttime just prior to sunrise. The high values of aerosol extinction are most likely associated with increased scattering by hygroscopic aerosols, since the correspondingmore » average relative humidity values were above 70%. After sunrise, relative humidity and aerosol extinction below 500 m decreased with the growth in the daytime convective boundary layer. The largest aerosol extinction for altitudes above 1 km occurred during the early afternoon most likely as a result of the increase in relative humidity. The water vapor mixing ratio profiles generally showed smaller variations with altitude between day and night. We also compared simultaneous measurements of relative humidity, aerosol extinction, and aerosol optical thickness derived from the ARM SGP Raman lidar and in situ instruments on board a small aircraft flown routinely over the ARM SGP site. In contrast, the differences between the CARL and IAP aerosol extinction measurements are considerably larger. Aerosol extinction derived from the IAP measurements is, on average, about 30-40% less than values derived from the Raman lidar. The reasons for this difference are not clear, but may be related to the corrections for supermicron scattering and relative humidity that were applied to the IAP data. The investigators on this project helped to set up a major field mission (2003 Aerosol IOP) over the DOE ARM SGP site. One of the goals of the mission was to further evaluate the aerosol and water vapor retrievals from this lidar system

Potential of polarization lidar to provide profiles of CCN- and INP-relevant aerosol parameters

NASA Astrophysics Data System (ADS)

Mamouri, R. E.; Ansmann, A.

2015-12-01

We investigate the potential of polarization lidar to provide vertical profiles of aerosol parameters from which cloud condensation nucleus (CCN) and ice nucleating particle (INP) number concentrations can be estimated. We show that height profiles of number concentrations of aerosol particles with radius > 50 nm (APC50, reservoir of favorable CCN) and with radius > 250 nm (APC250, reservoir of favorable INP), as well as profiles of the aerosol particle surface area concentration (ASC, used in INP parameterization) can be retrieved from lidar-derived aerosol extinction coefficients (AEC) with relative uncertainties of a factor of around 2 (APC50), and of about 25-50 % (APC250, ASC). Of key importance is the potential of polarization lidar to identify mineral dust particles and to distinguish and separate the aerosol properties of basic aerosol types such as mineral dust and continental pollution (haze, smoke). We investigate the relationship between AEC and APC50, APC250, and ASC for the main lidar wavelengths of 355, 532 and 1064 nm and main aerosol types (dust, pollution, marine). Our study is based on multiyear Aerosol Robotic Network (AERONET) photometer observations of aerosol optical thickness and column-integrated particle size distribution at Leipzig, Germany, and Limassol, Cyprus, which cover all realistic aerosol mixtures of continental pollution, mineral dust, and marine aerosol. We further include AERONET data from field campaigns in Morocco, Cabo Verde, and Barbados, which provide pure dust and pure marine aerosol scenarios. By means of a simple relationship between APC50 and the CCN-reservoir particles (APCCCN) and published INP parameterization schemes (with APC250 and ASC as input) we finally compute APCCCN and INP concentration profiles. We apply the full methodology to a lidar observation of a heavy dust outbreak crossing Cyprus with dust up to 8 km height and to a case during which anthropogenic pollution dominated.

LOAC (Light Optical Particle Counter): a new small aerosol counter with particle characterization capabilities for surface and airborne measurements

NASA Astrophysics Data System (ADS)

Renard, Jean-Baptiste; Berthet, Gwenael; Jégou, Fabrice; Jeannot, Matthieu; Jourdain, Line; Dulac, François; Mallet, Marc; Dupont, Jean-Charles; Thaury, Claire; Tonnelier, Thierry; Verdier, Nicolas; Charpentier, Patrick

2013-04-01

The determination of the size distribution of tropospheric and stratospheric aerosols with conventional optical counters is difficult when different natures of particles are present (droplets, soot, mineral dust, secondary organic or mineral particles...). Also, a light and cheap aerosol counter that can be used at ground, onboard drones or launched under all kinds of atmospheric balloons can be very useful during specific events as volcanic plumes, desert dust transport or local pollution episodes. These goals can be achieved thanks to a new generation of aerosol counter, called LOAC (Light Optical Aerosol Counter). The instrument was developed in the frame of a cooperation between French scientific laboratories (CNRS), the Environnement-SA and MeteoModem companies and the French Space Agency (CNES). LOAC is a small optical particle counter/sizer of ~250 grams, having a low electrical power consumption. The measurements are conducted at two scattering angles. The first one, at 12°, is used to determine the aerosol particle concentrations in 19 size classes within a diameter range of 0.3-100 micrometerers. At such an angle close to forward scattering, the signal is much more intense and the measurements are the least sensitive to the particle nature. The second angle is at 60°, where the scattered light is strongly dependent on the particle refractive index and thus on the nature of the aerosols. The ratio of the measurements at the two angles is used to discriminate between the different types of particles dominating the nature of the aerosol particles in the different size classes. The sensor particularly discriminates wet or liquid particles, soil dust and soot. Since 2011, we have operated LOAC in various environments (Arctic, Mediterranean, urban and peri-urban…) under different kinds of balloons including zero pressure stratospheric, tethered, drifting tropospheric, and meteorological sounding balloons. For the last case, the total weight of the gondola

LASER DESORPTION IONIZATION OF ULTRAFINE AEROSOL PARTICLES. (R823980)

EPA Science Inventory

On-line analysis of ultrafine aerosol particle in the 12 to 150 nm size range is performed by
laser desorption/ionization. Particles are size selected with a differential mobility analyzer and then
sent into a linear time-of-flight mass spectrometer where they are ablated w...

The single scattering properties of the aerosol particles as aggregated spheres

NASA Astrophysics Data System (ADS)

Wu, Y.; Gu, X.; Cheng, T.; Xie, D.; Yu, T.; Chen, H.; Guo, J.

2012-08-01

The light scattering and absorption properties of anthropogenic aerosol particles such as soot aggregates are complicated in the temporal and spatial distribution, which introduce uncertainty of radiative forcing on global climate change. In order to study the single scattering properties of anthorpogenic aerosol particles, the structures of these aerosols such as soot paticles and soot-containing mixtures with the sulfate or organic matter, are simulated using the parallel diffusion limited aggregation algorithm (DLA) based on the transmission electron microscope images (TEM). Then, the single scattering properties of randomly oriented aerosols, such as scattering matrix, single scattering albedo (SSA), and asymmetry parameter (AP), are computed using the superposition T-matrix method. The comparisons of the single scattering properties of these specific types of clusters with different morphological and chemical factors such as fractal parameters, aspect ratio, monomer radius, mixture mode and refractive index, indicate that these different impact factors can respectively generate the significant influences on the single scattering properties of these aerosols. The results show that aspect ratio of circumscribed shape has relatively small effect on single scattering properties, for both differences of SSA and AP are less than 0.1. However, mixture modes of soot clusters with larger sulfate particles have remarkably important effects on the scattering and absorption properties of aggregated spheres, and SSA of those soot-containing mixtures are increased in proportion to the ratio of larger weakly absorbing attachments. Therefore, these complex aerosols come from man made pollution cannot be neglected in the aerosol retrievals. The study of the single scattering properties on these kinds of aggregated spheres is important and helpful in remote sensing observations and atmospheric radiation balance computations.

Chemistry and Composition of Atmospheric Aerosol Particles

NASA Astrophysics Data System (ADS)

Kolb, Charles E.; Worsnop, Douglas R.

2012-05-01

For more than two decades a cadre of physical chemists has focused on understanding the formation processes, chemical composition, and chemical kinetics of atmospheric aerosol particles and droplets with diameters ranging from a few nanometers to ˜10,000 nm. They have adapted or invented a range of fundamental experimental and theoretical tools to investigate the thermochemistry, mass transport, and chemical kinetics of processes occurring at nanoscale gas-liquid and gas-solid interfaces for a wide range of nonideal, real-world substances. State-of-the-art laboratory methods devised to study molecular spectroscopy, chemical kinetics, and molecular dynamics also have been incorporated into field measurement instruments that are deployed routinely on research aircraft, ships, and mobile laboratories as well as at field sites from megacities to the most remote jungle, desert, and polar locations. These instruments can now provide real-time, size-resolved aerosol particle physical property and chemical composition data anywhere in Earth's troposphere and lower stratosphere.

A continuous sampler with background suppression for monitoring alpha-emitting aerosol particles.

PubMed

McFarland, A R; Rodgers, J C; Ortiz, C A; Moore, M E

1992-05-01

A continuous air monitor has been developed that includes provisions for improving the detection of alpha-emitting aerosol particles in the presence of radon/thoron progeny that are unattached to ambient aerosol particles. Wind tunnel tests show that 80% of 10-microns aerodynamic equivalent diameter particles penetrate the flow system from the ambient air to the collection filter when the flow rate is 57 L min-1 (2 cfm) and the wind speed is 1 m s-1. Uniformity of aerosol collection on the filter, as characterized by the coefficient of variation of the areal density deposits, is less than 15% for 10-microns aerodynamic-equivalent-diameter aerosol particles. Tests with unattached radon daughters in a flow-through chamber showed that approximately 99% of the 218Po was removed by an inlet screen that is designed to collect radon daughters that are in the size range of molecular clusters. The inlet screen offers the opportunity to improve the signal-to-noise ratio of energy spectra in the regions of interest (subranges of the energy spectrum) of transuranic elements and thereby enhance the performance of background compensation algorithms.

Scanning proton microprobe applied to analysis of individual aerosol particles from Amazon Basin

NASA Astrophysics Data System (ADS)

Gerab, Fábio; Artaxo, Paulo; Swietlicki, Erik; Pallon, Jan

1998-03-01

The development of the Scanning Proton Microprobe (SPM) offers a new possibility for individual aerosol particle studies. The SPM joins Particle Induced X-ray Emission (PIXE) elemental analysis qualities with micrometric spatial resolution. In this work the Lund University SPM facility was used for elemental characterization of individual aerosol particles emitted to the atmosphere in the Brazilian Amazon Basin, during gold mining activities by the so-called "gold shops".

Quantitative determination of carbonaceous particle mixing state in Paris using single particle mass spectrometer and aerosol mass spectrometer measurements

NASA Astrophysics Data System (ADS)

Healy, R. M.; Sciare, J.; Poulain, L.; Crippa, M.; Wiedensohler, A.; Prévôt, A. S. H.; Baltensperger, U.; Sarda-Estève, R.; McGuire, M. L.; Jeong, C.-H.; McGillicuddy, E.; O'Connor, I. P.; Sodeau, J. R.; Evans, G. J.; Wenger, J. C.

2013-04-01

Single particle mixing state information can be a powerful tool for assessing the relative impact of local and regional sources of ambient particulate matter in urban environments. However, quantitative mixing state data are challenging to obtain using single particle mass spectrometers. In this study, the quantitative chemical composition of carbonaceous single particles has been estimated using an aerosol time-of-flight mass spectrometer (ATOFMS) as part of the MEGAPOLI 2010 winter campaign in Paris, France. Relative peak areas of marker ions for elemental carbon (EC), organic aerosol (OA), ammonium, nitrate, sulphate and potassium were compared with concurrent measurements from an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a thermal/optical OCEC analyser and a particle into liquid sampler coupled with ion chromatography (PILS-IC). ATOFMS-derived mass concentrations reproduced the variability of these species well (R2 = 0.67-0.78), and ten discrete mixing states for carbonaceous particles were identified and quantified. Potassium content was used to identify particles associated with biomass combustion. The chemical mixing state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix factorization, was also investigated through comparison with the ATOFMS dataset. The results indicate that hydrocarbon-like OA (HOA) detected in Paris is associated with two EC-rich mixing states which differ in their relative sulphate content, while fresh biomass burning OA (BBOA) is associated with two mixing states which differ significantly in their OA/EC ratios. Aged biomass burning OA (OOA2-BBOA) was found to be significantly internally mixed with nitrate, while secondary, oxidized OA (OOA) was associated with five particle mixing states, each exhibiting different relative secondary inorganic ion content. Externally mixed secondary organic aerosol was not observed. These findings demonstrate the heterogeneity of primary and

Evaluating Nighttime CALIOP 0.532 micron Aerosol Optical Depth and Extinction Coefficient Retrievals

NASA Technical Reports Server (NTRS)

Campbell, J. R.; Tackett, J. L.; Reid, J. S.; Zhang, J.; Curtis, C. A.; Hyer, E. J.; Sessions, W. R.; Westphal, D. L.; Prospero, J. M.; Welton, E. J.;

Individual aerosol particles in and below clouds along a Mt. Fuji slope: Modification of sea-salt-containing particles by in-cloud processing

NASA Astrophysics Data System (ADS)

Ueda, S.; Hirose, Y.; Miura, K.; Okochi, H.

2014-02-01

Sizes and compositions of atmospheric aerosol particles can be altered by in-cloud processing by absorption/adsorption of gaseous and particulate materials and drying of aerosol particles that were formerly activated as cloud condensation nuclei. To elucidate differences of aerosol particles before and after in-cloud processing, aerosols were observed along a slope of Mt. Fuji, Japan (3776 m a.s.l.) during the summer in 2011 and 2012 using a portable laser particle counter (LPC) and an aerosol sampler. Aerosol samples for analyses of elemental compositions were obtained using a cascade impactor at top-of-cloud, in-cloud, and below-cloud altitudes. To investigate composition changes via in-cloud processing, individual particles (0.5-2 μm diameter) of samples from five cases (days) collected at different altitudes under similar backward air mass trajectory conditions were analyzed using a transmission electron microscope (TEM) equipped with an energy dispersive X-ray analyzer. For most cases (four cases), most particles at all altitudes mainly comprised sea salts: mainly Na with some S and/or Cl. Of those, in two cases, sea-salt-containing particles with Cl were found in below-cloud samples, although sea-salt-containing particles in top-of-cloud samples did not contain Cl. This result suggests that Cl in the sea salt was displaced by other cloud components. In the other two cases, sea-salt-containing particles on samples at all altitudes were without Cl. However, molar ratios of S to Na (S/Na) of the sea-salt-containing particles of top-of-cloud samples were higher than those of below-cloud samples, suggesting that sulfuric acid or sulfate was added to sea-salt-containing particles after complete displacement of Cl by absorption of SO2 or coagulation with sulfate. The additional volume of sulfuric acid in clouds for the two cases was estimated using the observed S/Na values of sea-salt-containing particles. The estimation revealed that size changes by in

Urban organic aerosols measured by single particle mass spectrometry in the megacity of London

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Harrison, R. M.

2012-05-01

During the month of October 2006, as part of the REPARTEE-I experiment (Regent's Park and Tower Environmental Experiment) an Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS) was deployed at an urban background location in the city of London, UK. Fifteen particle types were classified, some of which were already discussed (Dall'Osto et al., 2009a,b; Harrison et al., 2012). In this manuscript the origins and properties of four unreported particle types postulated to be due to locally generated aerosols, independent of the air mass type advected into London, are examined. One particle type, originating from lubricating oil (referred to as Ca-EC), was associated with morning rush hour traffic emissions. A second particle type, composed of both inorganic and organic species (called Na-EC-OC), was found enhanced in particle number concentration during evening time periods, and is likely to originate from a source operating at this time of day, or more probably from condensation of semi-volatile species. A third class, internally mixed with organic carbon and sulphate (called OC), was found to spike both in the morning and evenings although it could not unambiguously associated with a specific source or atmospheric process. The fourth class (Secondary Organic Aerosols - Polycyclic Aromatic Hydrocarbon; SOA-PAH) exhibited maximum frequency during the warmest part of the day, and a number of factors point towards secondary aerosol production from traffic-related volatile aromatic compounds. Single particle mass spectra of this particle type showed an oxidized polycyclic aromatic compound signature. A comparison of ATOFMS particle class data is then made with factors obtained by Positive Matrix Factorization and PAH signatures obtained from Aerosol Mass Spectrometer (AMS) data (Allan et al., 2010). Both the Ca-EC and OC particle types correlate with primary Hydrocarbon-like Organic Aerosol (HOA, R2 = 0.65 and 0.50 respectively), and Na-EC-OC correlates weakly with the AMS

Modelling non-equilibrium secondary organic aerosol formation and evaporation with the aerosol dynamics, gas- and particle-phase chemistry kinetic multilayer model ADCHAM

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

Roldin, P.; Eriksson, A. C.; Nordin, E. Z.

2014-08-11

We have developed the novel Aerosol Dynamics, gas- and particle- phase chemistry model for laboratory CHAMber studies (ADCHAM). The model combines the detailed gas phase Master Chemical Mechanism version 3.2, an aerosol dynamics and particle phase chemistry module (which considers acid catalysed oligomerization, heterogeneous oxidation reactions in the particle phase and non-ideal interactions between organic compounds, water and inorganic ions) and a kinetic multilayer module for diffusion limited transport of compounds between the gas phase, particle surface and particle bulk phase. In this article we describe and use ADCHAM to study: 1) the mass transfer limited uptake of ammonia (NH3)more » and formation of organic salts between ammonium (NH4+) and carboxylic acids (RCOOH), 2) the slow and almost particle size independent evaporation of α-pinene secondary organic aerosol (SOA) particles, and 3) the influence of chamber wall effects on the observed SOA formation in smog chambers.« less

Measurements of the absorption coefficient of stratospheric aerosols

NASA Technical Reports Server (NTRS)

Ogren, J. A.; Ahlquist, N. C.; Clarke, A. D.; Charlson, R. J.

1981-01-01

The absorption coefficients of stratospheric aerosols are measured using a variation on the integrating plate method. The technique is based on the decrease in the transparency of a substrate when an absorbing aerosol is deposited on it. A Lambert scatterer is placed behind the substrate to integrate forward scattered light and minimize the effect of scattering on the measurement. The low pressure in the stratosphere is used for the direct impaction of particles onto a narrow strip of opal glass. The eight samples collected had a median value of 4 x 10 to the -9th m with an uncertainty of + or - 5 x 10 to the -9th m. If this absorption is due to graphitic carbon, then its concentration is estimated at about 0.4 ng/cu m, or about 0.25% of the total aerosol mass concentration. Estimates of the aerosol scattering coefficients based on satellite extinction inversions result in an aerosol single-scattering albedo in the range of 0.96-1.0.

Retrievals of aerosol microphysics from simulations of spaceborne multiwavelength lidar measurements

NASA Astrophysics Data System (ADS)

Whiteman, David N.; Pérez-Ramírez, Daniel; Veselovskii, Igor; Colarco, Peter; Buchard, Virginie

2018-01-01

In support of the Aerosol, Clouds, Ecosystems mission, simulations of a spaceborne multiwavelength lidar are performed based on global model simulations of the atmosphere along a satellite orbit track. The yield for aerosol microphysical inversions is quantified and comparisons are made between the aerosol microphysics inherent in the global model and those inverted from both the model's optical data and the simulated three backscatter and two extinction lidar measurements, which are based on the model's optical data. We find that yield can be significantly increased if inversions based on a reduced optical dataset of three backscatter and one extinction are acceptable. In general, retrieval performance is better for cases where the aerosol fine mode dominates although a lack of sensitivity to particles with sizes less than 0.1 μm is found. Lack of sensitivity to coarse mode cases is also found, in agreement with earlier studies. Surface area is generally the most robustly retrieved quantity. The work here points toward the need for ancillary data to aid in the constraints of the lidar inversions and also for joint inversions involving lidar and polarimeter measurements.

Retrievals of Aerosol Microphysics from Simulations of Spaceborne Multiwavelength Lidar Measurements

NASA Technical Reports Server (NTRS)

Whiteman, David N.; Perez-Ramírez, Daniel; Veselovskii, Igor; Colarco, Peter; Buchard, Virginie

2017-01-01

In support of the Aerosol, Clouds, Ecosystems mission, simulations of a spaceborne multiwavelength lidar are performed based on global model simulations of the atmosphere along a satellite orbit track. The yield for aerosol microphysical inversions is quantified and comparisons are made between the aerosol microphysics inherent in the global model and those inverted from both the model's optical data and the simulated three backscatter and two extinction lidar measurements, which are based on the model's optical data. We find that yield can be significantly increased if inversions based on a reduced optical dataset of three backscatter and one extinction are acceptable. In general, retrieval performance is better for cases where the aerosol fine mode dominates although a lack of sensitivity to particles with sizes less than 0.1 microns is found. Lack of sensitivity to coarse mode cases is also found, in agreement with earlier studies. Surface area is generally the most robustly retrieved quantity. The work here points toward the need for ancillary data to aid in the constraints of the lidar inversions and also for joint inversions involving lidar and polarimeter measurements.

Attenuated total reflectance FT-IR imaging and quantitative energy dispersive-electron probe X-ray microanalysis techniques for single particle analysis of atmospheric aerosol particles.

PubMed

Ryu, JiYeon; Ro, Chul-Un

2009-08-15

This work demonstrates the practical applicability of the combined use of attenuated total reflectance (ATR) FT-IR imaging and low-Z particle electron probe X-ray microanalysis (EPMA) techniques for the characterization of individual aerosol particles. These two single particle analytical techniques provide complementary information on the physicochemical characteristics of the same individual particles, that is, the low-Z particle EPMA for the information on the morphology and elemental concentration and the ATR-FT-IR imaging on the functional group, molecular species, and crystal structure. It was confirmed that the ATR-FT-IR imaging technique can provide sufficient FT-IR absorption signals to perform molecular speciation of individual particles of micrometer size when applied to artificially generated aerosol particles such as ascorbic acid and NaNO(3) aerosols. An exemplar indoor atmospheric aerosol sample was investigated to demonstrate the practical feasibility of the combined application of ATR-FT-IR imaging and low-Z particle EPMA techniques for the characterization of individual airborne particles.

Single particle characterization, source apportionment, and aging effects of ambient aerosols in Southern California

NASA Astrophysics Data System (ADS)

Shields, Laura Grace

Composed of a mixture of chemical species and phases and existing in a variety of shapes and sizes, atmospheric aerosols are complex and can have serious influence on human health, the environment, and climate. In order to better understand the impact of aerosols on local to global scales, detailed measurements on the physical and chemical properties of ambient particles are essential. In addition, knowing the origin or the source of the aerosols is important for policymakers to implement targeted regulations and effective control strategies to reduce air pollution in their region. One of the most ground breaking techniques in aerosol instrumentation is single particle mass spectrometry (SPMS), which can provide online chemical composition and size information on the individual particle level. The primary focus of this work is to further improve the ability of one specific SPMS technique, aerosol time-of-flight mass spectrometry (ATOFMS), for the use of identifying the specific origin of ambient aerosols, which is known as source apportionment. The ATOFMS source apportionment method utilizes a library of distinct source mass spectral signatures to match the chemical information of the single ambient particles. The unique signatures are obtained in controlled source characterization studies, such as with the exhaust emissions of heavy duty diesel vehicles (HDDV) operating on a dynamometer. The apportionment of ambient aerosols is complicated by the chemical and physical processes an individual particle can undergo as it spends time in the atmosphere, which is referred to as "aging" of the aerosol. Therefore, the performance of the source signature library technique was investigated on the ambient dataset of the highly aged environment of Riverside, California. Additionally, two specific subsets of the Riverside dataset (ultrafine particles and particles containing trace metals), which are known to cause adverse health effects, were probed in greater detail. Finally