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Sample records for aerosol mixing state

  1. 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

  2. Quantifying aerosol mixing state with entropy and diversity measures

    NASA Astrophysics Data System (ADS)

    Riemer, N.; West, M.

    2013-11-01

    This paper presents the first quantitative metric for aerosol population mixing state, defined as the distribution of per-particle chemical species composition. This new metric, the mixing state index χ, is an affine ratio of the average per-particle species diversity Dα and the bulk population species diversity Dγ, both of which are based on information-theoretic entropy measures. The mixing state index χ enables the first rigorous definition of the spectrum of mixing states from so-called external mixture to internal mixture, which is significant for aerosol climate impacts, including aerosol optical properties and cloud condensation nuclei activity. We illustrate the usefulness of this new mixing state framework with model results from the stochastic particle-resolved model PartMC-MOSAIC. These results demonstrate how the mixing state metrics evolve with time for several archetypal cases, each of which isolates a specific process such as coagulation, emission, or condensation. Further, we present an analysis of the mixing state evolution for a complex urban plume case, for which these processes occur simultaneously. We additionally derive theoretical properties of the mixing state index and present a family of generalized mixing state indexes that vary in the importance assigned to low-mass-fraction species.

  3. [Investigation of Aerosol Mixed State and CCN Activity in Nanjing].

    PubMed

    Zhu, Lin; Ma, Yan; Zheng, Jun; Li, Shi-zheng; Wang, Li-peng

    2016-04-15

    During 11-18 September 2014, the size-resolved aerosol Cloud Condensation Nuclei (CCN) activity and mixing state were measured using Cloud Condensation Nuclei Counter (CCNC), Aerosol Particle Mass (APM) and Scanning Mobility Particle Sizer (SMPS). The results showed that aerosols mainly existed as an internal mixture. For 76, 111, 138 and 181 nm particles, black carbon (BC) accounted for 5.4%, 10%, l0.7% and 6.7% of the particle mass, but as high as 51%, 57%, 70% and 59% of the particle number concentrations, respectively, suggesting that BC was a type of important condensation nuclei in the atmosphere and made significant contributions to particle numbers. The occasionally observed external mixtures were mainly present in 111 and 138 nm particles. The critical supersaturation was 0.25%, 0.13%, 0.06% and 0.015% for 76, 111, 138 and 181 nm particles, respectively. Precipitation and haze had significant effects on the particle CCN activity. The hygroscopicity parameter K was 0.37, 0.29 and 0.39 in rainy, clear and hazy days, respectively. Particle density and CCN activity were impacted by chemical compositions. Compared with clear days, higher contents of inorganic salts and lower contents of organics were found on hazy days, accompanied by lower particle density and higher CCN activity. PMID:27548938

  4. Model analysis of influences of aerosol mixing state upon its optical properties in East Asia

    NASA Astrophysics Data System (ADS)

    Han, Xiao; Zhang, Meigen; Zhu, Lingyun; Xu, Liren

    2013-07-01

    The air quality model system RAMS (Regional Atmospheric Modeling System)-CMAQ (Models-3 Community Multi-scale Air Quality) coupled with an aerosol optical/radiative module was applied to investigate the impact of different aerosol mixing states (i.e., externally mixed, half externally and half internally mixed, and internally mixed) on radiative forcing in East Asia. The simulation results show that the aerosol optical depth (AOD) generally increased when the aerosol mixing state changed from externally mixed to internally mixed, while the single scattering albedo (SSA) decreased. Therefore, the scattering and absorption properties of aerosols can be significantly affected by the change of aerosol mixing states. Comparison of simulated and observed SSAs at five AERONET (Aerosol Robotic Network) sites suggests that SSA could be better estimated by considering aerosol particles to be internally mixed. Model analysis indicates that the impact of aerosol mixing state upon aerosol direct radiative forcing (DRF) is complex. Generally, the cooling effect of aerosols over East Asia are enhanced in the northern part of East Asia (Northern China, Korean peninsula, and the surrounding area of Japan) and are reduced in the southern part of East Asia (Sichuan Basin and Southeast China) by internal mixing process, and the variation range can reach ±5 W m-2. The analysis shows that the internal mixing between inorganic salt and dust is likely the main reason that the cooling effect strengthens. Conversely, the internal mixture of anthropogenic aerosols, including sulfate, nitrate, ammonium, black carbon, and organic carbon, could obviously weaken the cooling effect.

  5. Mixing state of aerosols over the Indo-Gangetic Plain: Radiative forcing and heating rate

    NASA Astrophysics Data System (ADS)

    Srivastava, R.; Ramachandran, S.

    2012-12-01

    Aerosols are a major atmospheric variable which perturb the Earth-atmosphere radiation balance by absorbing and scattering the solar and terrestrial radiation. Aerosols are produced by natural and anthropogenic processes. The presence of different types of aerosol over a location and aerosols transported from long-range can give rise to different mixing states because of aging and interaction among the different aerosol species. Knowledge of the mixing state of aerosols is important for an accurate assessment of aerosols in climate forcing, as assumptions regarding the mixing state of aerosol and its effect on optical properties can give rise to uncertainties in modeling their direct and indirect effects [1]. Seasonal variations in mixing states of aerosols over an urban (Kanpur) and a rural location (Gandhi College) in the Indo-Gangetic Plain (IGP) are determined using the measured and modeled aerosol optical properties, and the impact of aerosol mixing state on aerosol radiative forcing are investigated. IGP is one of the most populated and polluted river basins in the world, rich in fertile lands and agricultural production. Kanpur is an urban, industrial and densely populated city, and has several large/small scale industries and vehicles, while Gandhi College in IGP is a rural village, located southeast of Kanpur. Aerosol optical properties obtained from Aerosol Robotic Network sun/sky radiometers [2] over these two environmentally distinct locations in Indo-Gangetic Plain are used in the study, along with aerosol vertical profiles obtained from CALIPSO (Cloud- Aerosol Lidar and Infrared Pathfinder Satellite Observations) lidar observations. Probable mixing state of aerosols is determined utilizing the aerosol optical properties viz., aerosol optical depth, single scattering albedo and asymmetry parameter. The coated-sphere Mie calculation requires the refractive index of core and shell species, and the radius of core and shell particles. Core to shell radius

  6. Mixing-State Sensitivity of Aerosol Absorption in the EMAC Chemistry-Climate Model

    NASA Astrophysics Data System (ADS)

    Klingmueller, Klaus; Steil, Benedikt; Bruehl, Christoph; Tost, Holger; Lelieveld, Jos

    2014-05-01

    The modelling of aerosol radiative forcing is a major cause of uncertainty in the assessment of global and regional atmospheric energy budgets and climate change. One reason is the strong dependence of the aerosol optical properties on the mixing state of aerosol components like black carbon and sulphates. Using the atmospheric chemistry-climate model EMAC, we study the radiative transfer assuming various mixing states. The aerosol optics code we employ builds on the AEROPT submodel which assumes homogeneous internal mixing utilising the volume average refractive index mixing rule. We have extended the submodel to additionally account for external mixing, partial external mixing and multilayered particles. Furthermore, we have implemented the volume average dielectric constant and Maxwell Garnett Mixing rule. We present results from regional case studies employing a new column version of the aerosol optical properties and radiative transfer code of EMAC, considering columns over China, India and Africa. The regional results are complemented by global results from a simulation for the year 2005. Our findings corroborate much stronger absorption by internal than external mixtures. Well mixed aerosol often is a good approximation for particles with a black carbon core, whereas particles with black carbon at the surface absorb significantly less. Therefore, we conclude that it is generally recommended to take the inner structure of internally mixed particles into account.

  7. Spectro-microscopy of Ambient Aerosol Particles: Observational Constraints on Mixing State Parameterization

    NASA Astrophysics Data System (ADS)

    OBrien, R. E.; Wang, B.; Laskin, A.; West, M.; Riemer, N. S.; Gilles, M. K.; Moffet, R.

    2014-12-01

    Individual aerosol particles are often mixtures of multiple components such as inorganic salts, soot or elemental carbon, and organic molecules. The amounts of the different components in each particle and the particle morphologies will impact the CCN activity and the radiative properties of the aerosol population. A recent parameterization of the mixing state developed by Nicole Riemer and Matthew West provides a clear transition between ambient measurements of aerosol components and particle mixing states employed in climate models. Single particle spectro-microscopy techniques including scanning transmission x-ray microscopy/near-edge x-ray absorption fine structure spectroscopy (STXM/NEXAFS) and computer controlled scanning electron microscopy/energy dispersive x-ray spectroscopy (CCSEM/EDX) are used to measure the composition of aerosol particles from the CARES campaign at both T0 and T1. Here, we present results from the application of the per particle composition to a parameterization of the mixing state and provide constraints on the mixing state of ambient aerosol particles. The two microscopy techniques yield complementary information on the mixing state of the aerosol populations; STXM/NEXAFS provides information on the mixing state of the organic fraction while CCSEM/EDX provides information on the inorganic fraction.

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

    PubMed Central

    2015-01-01

    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. PMID:27162963

  9. 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.

  10. 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. PMID:27162963

  11. A strategy for characterizing the mixing state of immiscible aerosol components and the formation of multiphase aerosol particles through coagulation.

    PubMed

    Mitchem, Laura; Buajarern, Jariya; Ward, Andrew D; Reid, Jonathan P

    2006-07-20

    We demonstrate that the coagulation of two aerosol droplets of different chemical composition can be studied directly through the unique combination of optical tweezers and Raman spectroscopy. Multiple optical traps can be established, allowing the manipulation of multiple aerosol droplets. Spontaneous Raman scattering allows the characterization of droplet composition and mixing state, permitting the phase segregation of immiscible components in multiphase aerosol to be investigated with spatial resolution. Stimulated Raman scattering allows the integrity of the droplet and uniformity of refractive index to be probed. The combination of these spectroscopic probes with optical tweezers is shown to yield unprecedented detail in studies of the coagulation of decane and water droplets.

  12. Quantification of black carbon mixing state from traffic: implications for aerosol optical properties

    NASA Astrophysics Data System (ADS)

    Willis, Megan D.; Healy, Robert M.; Riemer, Nicole; West, Matthew; Wang, Jon M.; Jeong, Cheol-Heon; Wenger, John C.; Evans, Greg J.; Abbatt, Jonathan P. D.; Lee, Alex K. Y.

    2016-04-01

    The climatic impacts of black carbon (BC) aerosol, an important absorber of solar radiation in the atmosphere, remain poorly constrained and are intimately related to its particle-scale physical and chemical properties. Using particle-resolved modelling informed by quantitative measurements from a soot-particle aerosol mass spectrometer, we confirm that the mixing state (the distribution of co-emitted aerosol amongst fresh BC-containing particles) at the time of emission significantly affects BC-aerosol optical properties even after a day of atmospheric processing. Both single particle and ensemble aerosol mass spectrometry observations indicate that BC near the point of emission co-exists with hydrocarbon-like organic aerosol (HOA) in two distinct particle types: HOA-rich and BC-rich particles. The average mass fraction of black carbon in HOA-rich and BC-rich particle classes was < 0.1 and 0.8, respectively. Notably, approximately 90 % of BC mass resides in BC-rich particles. This new measurement capability provides quantitative insight into the physical and chemical nature of BC-containing particles and is used to drive a particle-resolved aerosol box model. Significant differences in calculated single scattering albedo (an increase of 0.1) arise from accurate treatment of initial particle mixing state as compared to the assumption of uniform aerosol composition at the point of BC injection into the atmosphere.

  13. Quantification of black carbon mixing state from traffic: implications for aerosol optical properties

    NASA Astrophysics Data System (ADS)

    Willis, M. D.; Healy, R. M.; Riemer, N.; West, M.; Wang, J. M.; Jeong, C.-H.; Wenger, J. C.; Evans, G. J.; Abbatt, J. P. D.; Lee, A. K. Y.

    2015-11-01

    The climatic impacts of black carbon (BC) aerosol, an important absorber of solar radiation in the atmosphere, remain poorly constrained and are intimately related to its particle-scale physical and chemical properties. Using particle-resolved modelling informed by quantitative measurements from a soot-particle aerosol mass spectrometer, we confirm that the mixing state (the distribution of co-emitted aerosol amongst fresh BC-containing particles) at the time of emission significantly affects BC-aerosol optical properties even after a day of atmospheric processing. Both single particle and ensemble aerosol mass spectrometry observations indicate that BC near the point of emission co-exists with hydrocarbon-like organic aerosol in two distinct particle types: HOA-rich and BC-rich particles. The average mass fraction of black carbon in HOA-rich and BC-rich particles was 0.02-0.08 and 0.72-0.93, respectively. Notably, approximately 90 % of BC mass resides in BC-rich particles. This new measurement capability provides quantitative insight into the physical and chemical nature of BC-containing particles and is used to drive a particle-resolved aerosol box model. Significant differences in calculated single scattering albedo (an increase of 0.1) arise from accurate treatment of initial particle mixing state as compared to the assumption of uniform aerosol composition at the point of BC injection into the atmosphere.

  14. Quantification of black carbon mixing state from traffic: Implications for aerosol optical properties

    DOE PAGES

    Willis, Megan D.; Healy, Robert M.; Riemer, Nicole; West, Matthew; Wang, Jon M.; Jeong, Cheol -Heon; Wenger, John C.; Evans, Greg J.; Abbatt, Jonathan P. D.; Lee, Alex K. Y.

    2016-04-14

    The climatic impacts of black carbon (BC) aerosol, an important absorber of solar radiation in the atmosphere, remain poorly constrained and are intimately related to its particle-scale physical and chemical properties. Using particle-resolved modelling informed by quantitative measurements from a soot-particle aerosol mass spectrometer, we confirm that the mixing state (the distribution of co-emitted aerosol amongst fresh BC-containing particles) at the time of emission significantly affects BC-aerosol optical properties even after a day of atmospheric processing. Both single particle and ensemble aerosol mass spectrometry observations indicate that BC near the point of emission co-exists with hydrocarbon-like organic aerosol (HOA) inmore » two distinct particle types: HOA-rich and BC-rich particles. The average mass fraction of black carbon in HOA-rich and BC-rich particle classes was  < 0.1 and 0.8, respectively. Notably, approximately 90 % of BC mass resides in BC-rich particles. This new measurement capability provides quantitative insight into the physical and chemical nature of BC-containing particles and is used to drive a particle-resolved aerosol box model. Lastly, significant differences in calculated single scattering albedo (an increase of 0.1) arise from accurate treatment of initial particle mixing state as compared to the assumption of uniform aerosol composition at the point of BC injection into the atmosphere.« less

  15. Chemical imaging of ambient aerosol particles: Observational constraints on mixing state parameterization

    NASA Astrophysics Data System (ADS)

    O'Brien, Rachel E.; Wang, Bingbing; Laskin, Alexander; Riemer, Nicole; West, Matthew; Zhang, Qi; Sun, Yele; Yu, Xiao-Ying; Alpert, Peter; Knopf, Daniel A.; Gilles, Mary K.; Moffet, Ryan C.

    2015-09-01

    A new parameterization for quantifying the mixing state of aerosol populations has been applied for the first time to samples of ambient particles analyzed using spectro-microscopy techniques. Scanning transmission X-ray microscopy/near edge X-ray absorption fine structure (STXM/NEXAFS) and computer-controlled scanning electron microscopy/energy dispersive X-ray spectroscopy (CCSEM/EDX) were used to probe the composition of the organic and inorganic fraction of individual particles collected on 27 and 28 June during the 2010 Carbonaceous Aerosols and Radiative Effects study in the Central Valley, California. The first field site, T0, was located in downtown Sacramento, while T1 was located near the Sierra Nevada Mountains. Mass estimates of the aerosol particle components were used to calculate mixing state metrics, such as the particle-specific diversity, bulk population diversity, and mixing state index, for each sample. The STXM data showed evidence of changes in the mixing state associated with a buildup of organic matter confirmed by collocated measurements, and the largest impact on the mixing state was due to an increase in soot dominant particles during this buildup. The mixing state from STXM was similar between T0 and T1, indicating that the increased organic fraction at T1 had a small effect on the mixing state of the population. The CCSEM/EDX analysis showed the presence of two types of particle populations: the first was dominated by aged sea-salt particles and had a higher mixing state index (indicating a more homogeneous population); the second was dominated by carbonaceous particles and had a lower mixing state index.

  16. Aerosol mixing state, hygroscopic growth and cloud activation efficiency during MIRAGE 2006

    NASA Astrophysics Data System (ADS)

    Lance, S.; Raatikainen, T.; Onasch, T. B.; Worsnop, D. R.; Yu, X.-Y.; Alexander, M. L.; Stolzenburg, M. R.; McMurry, P. H.; Smith, J. N.; Nenes, A.

    2013-05-01

    Observations of aerosol hygroscopic growth and CCN activation spectra for submicron particles are reported for the T1 ground site outside of Mexico City during the MIRAGE 2006 campaign. κ-Köhler theory is used to evaluate the characteristic hygroscopicity parameter, κ*, for the CCN active aerosol population using both size-resolved HTMDA and size-resolved CCNc measurements. Organic mass fractions (forg) are evaluated from size-resolved aerosol mass spectrometer (AMS) measurements, from which predictions of the hygroscopicity parameter are compared against κ*. Strong diurnal changes in aerosol water uptake parameters and aerosol composition are observed. We find that new particle formation (NPF) events are correlated with an increased κ* and CCN-active fraction during the daytime, with greater impact on smaller particles. During NPF events, the number concentration of 40 nm particles acting as CCN at 0.51% ± 0.06% supersaturation can surpass by more than a factor of two the corresponding concentrations of 100 nm particles. We also find that at 06:00-08:00 LT throughout the campaign, fresh traffic emissions result in substantial changes to the chemical distribution of the aerosol, with on average 65% externally mixed fraction for 40 nm particles and 30% externally mixed fraction for 100 nm particles, whereas at midday nearly all particles of both sizes can be described as "internally mixed". Average activation spectra and growth factor distributions are analyzed for different time periods characterizing the daytime (with and without NPF events), the early morning "rush hour" and the entire campaign. We show that κ* derived from CCNc measurements decreases as a function of size during all time periods, while the CCN-active fraction increases as a function of size. Size-resolved AMS measurements do not predict the observed trend for κ* versus particle size, which can be attributed to unresolved mixing state and the presence of refractory material not measured

  17. Chemical Imaging of Ambient Aerosol Particles: Observational Constraints on Mixing State Parameterization

    SciTech Connect

    O'Brien, Rachel; Wang, Bingbing; Laskin, Alexander; Riemer, Nicole; West, Matthew; Zhang, Qi; Sun, Yele; Yu, Xiao-Ying; Alpert, Peter A.; Knopf, Daniel A.; Gilles, Mary K.; Moffet, Ryan

    2015-09-28

    A new parameterization for quantifying the mixing state of aerosol populations has been applied for the first time to samples of ambient particles analyzed using spectro-microscopy techniques. Scanning transmission x-ray microscopy/near edge x-ray absorption fine structure (STXM/NEXAFS) and computer controlled scanning electron microscopy/energy dispersive x-ray spectroscopy (CCSEM/EDX) were used to probe the composition of the organic and inorganic fraction of individual particles collected on June 27th and 28th during the 2010 Carbonaceous Aerosols and Radiative Effects (CARES) study in the Central Valley, California. The first field site, T0, was located in downtown Sacramento, while T1 was located near the Sierra Nevada Mountains. Mass estimates of the aerosol particle components were used to calculate mixing state metrics, such as the particle-specific diversity, bulk population diversity, and mixing state index, for each sample. Both microscopy imaging techniques showed more changes over these two days in the mixing state at the T0 site than at the T1 site. The STXM data showed evidence of changes in the mixing state associated with a build-up of organic matter confirmed by collocated measurements and the largest impact on the mixing state was due to an increase in soot dominant particles during this build-up. The CCSEM/EDX analysis showed the presence of two types of particle populations; the first was dominated by aged sea salt particles and had a higher mixing state index (indicating a more homogeneous population), the second was dominated by carbonaceous particles and had a lower mixing state index.

  18. Simulating the Evolution of Soot Mixing State with a Particle-Resolved Aerosol Model

    SciTech Connect

    Riemer, Nicole; West, Matt; Zaveri, Rahul A.; Easter, Richard C.

    2009-05-05

    The mixing state of soot particles in the atmosphere is of crucial importance for assessing their climatic impact, since it governs their chemical reactivity, cloud condensation nuclei activity and radiative properties. To improve the mixing state representation in models, we present a new approach, the stochastic particle-resolved model PartMC-MOSAIC, which explicitly resolves the composition of individual particles in a given population of different types of aerosol particles. This approach accurately tracks the evolution of the mixing state of particles due to emission, dilution, condensation and coagulation. To make this direct stochastic particle-based method practical, we implemented a new multiscale stochastic coagulation method. With this method we achieved optimal efficiency for applications when the coagulation kernel is highly non-uniform, as is the case for many realistic applications. PartMC-MOSAIC was applied to an idealized urban plume case representative of a large urban area to simulate the evolution of carbonaceous aerosols of different types due to coagulation and condensation. For this urban plume scenario we quantified the individual processes that contribute to the aging of the aerosol distribution, illustrating the capabilities of our modeling approach. The results showed for the first time the multidimensional structure of particle composition, which is usually lost in internally-mixed sectional or modal aerosol models.

  19. Mixing State and Optical Properties of Biomass Burning Aerosol during the SAMBBA 2012 Campaign

    NASA Astrophysics Data System (ADS)

    Brooke, Jennifer; Brooks, Barbara; McQuaid, Jim; Osborne, Simon

    2013-04-01

    Emissions of black carbon are a global phenomenon associated with combustion activities with an estimated 40 % of global emissions from biomass burning. These emissions are typically dominated in regional hotspots, such as along the edges of the Amazon Basin, and contribute to the regional air quality and have associated health impacts as well as the global climatic impacts of this major source of black carbon as well as other radiatively active species. New airborne measurements will be presented of biomass burning emissions across the Amazon region from the South AMerican Biomass Burning Analysis (SAMBBA) campaign based at Porto Vehlo, Rondônia, Brazil in September 2012. This airborne campaign aboard the FAAM BAe-146 coincided with the seasonal peak in South American biomass burning emissions, which make up the most dominant source of atmospheric pollutants in the region at this time. SAMBBA included dedicated flights involving in-situ measurements and remote sensing of single plume studies through to multi-plume sampling of smouldering and flaming vegetation fires, regional haze sampling, and measurements of biogenic aerosol and gases across Amazonas. This presentation summarises early findings from the SAMBBA aircraft observations focusing on the relationship between biomass burning aerosol properties; size distributions, aerosol mixing state and optical properties from a suite of instruments onboard the FAAM BAe-146. The interplay of these properties influences the regional radiative balance impacting on weather and climate. The Leeds airborne VACC (Volatile Aerosol Concentration and Composition) instrument is designed to investigate the volatility properties of different aerosol species in order to determine aerosol composition; furthermore it can be used to infer the mixing state of the aerosol. Size distributions measured with the volatility system will be compared with ambient size distribution measurements this allows information on organic coating

  20. Aerosol optical properties and mixing state of black carbon in the Pearl River Delta, China

    NASA Astrophysics Data System (ADS)

    Tan, Haobo; Liu, Li; Fan, Shaojia; Li, Fei; Yin, Yan; Cai, Mingfu; Chan, P. W.

    2016-04-01

    Aerosols contribute the largest uncertainty to the total radiative forcing estimate, and black carbon (BC) that absorbs solar radiation plays an important role in the Earth's energy budget. This study analysed the aerosol optical properties from 22 February to 18 March 2014 at the China Meteorological Administration Atmospheric Watch Network (CAWNET) station in the Pearl River Delta (PRD), China. The representative values of dry-state particle scattering coefficient (σsp), hemispheric backscattering coefficient (σhbsp), absorption coefficient (σabsp), extinction coefficient (σep), hemispheric backscattering fraction (HBF), single scattering albedo (SSA), as well as scattering Ångström exponent (α) were presented. A comparison between a polluted day and a clean day shows that the aerosol optical properties depend on particle number size distribution, weather conditions and evolution of the mixing layer. To investigate the mixing state of BC at the surface, an optical closure study of HBF between measurements and calculations based on a modified Mie model was employed for dry particles. The result shows that the mixing state of BC might be between the external mixture and the core-shell mixture. The average retrieved ratio of the externally mixed BC to the total BC mass concentration (rext-BC) was 0.58 ± 0.12, and the diurnal pattern of rext-BC can be found. Furthermore, considering that non-light-absorbing particles measured by a Volatility-Tandem Differential Mobility Analyser (V-TDMA) exist independently with core-shell and homogenously internally mixed BC particles, the calculated optical properties were just slightly different from those based on the assumption that BC exist in each particle. This would help understand the influence of the BC mixing state on aerosol optical properties and radiation budget in the PRD.

  1. Particle-Resolved Modeling of Aerosol Mixing State in an Evolving Ship Plume

    NASA Astrophysics Data System (ADS)

    Riemer, N. S.; Tian, J.; Pfaffenberger, L.; Schlager, H.; Petzold, A.

    2011-12-01

    The aerosol mixing state is important since it impacts the particles' optical and CCN properties and thereby their climate impact. It evolves continuously during the particles' residence time in the atmosphere as a result of coagulation with other particles and condensation of secondary aerosol species. This evolution is challenging to represent in traditional aerosol models since they require the representation of a multi-dimensional particle distribution. While modal or sectional aerosol representations cannot practically resolve the aerosol mixing state for more than a few species, particle-resolved models store the composition of many individual aerosol particles directly. They thus sample the high-dimensional composition state space very efficiently and so can deal with tens of species, fully resolving the mixing state. Here we use the capabilities of the particle-resolved model PartMC-MOSAIC to simulate the evolution of particulate matter emitted from marine diesel engines and compare the results to aircraft measurements made in the English Channel in 2007 as part of the European campaign QUANTIFY. The model was initialized with values of gas concentrations and particle size distributions and compositions representing fresh ship emissions. These values were obtained from a test rig study in the European project HERCULES in 2006 using a serial four-stroke marine diesel engine operating on high-sulfur heavy fuel oil. The freshly emitted particles consisted of sulfate, black carbon, organic carbon and ash. We then tracked the particle population for several hours as it evolved undergoing coagulation, dilution with the background air, and chemical transformations in the aerosol and gas phase. This simulation was used to compute the evolution of CCN properties and optical properties of the plume on a per-particle basis. We compared our results to size-resolved data of aged ship plumes from the QUANTIFY Study in 2007 and showed that the model was able to reproduce

  2. Evaluating the Role of Aerosol Mixing State in Cloud Droplet Nucleation using a New Activation Parameterization

    NASA Astrophysics Data System (ADS)

    Rothenberg, D. A.; Wang, C.

    2013-12-01

    An important source contributing to uncertainty in simulations with global climate models arises from the influence of aerosols on cloud properties. These so-called aerosol indirect effects arise from a single coupling in the model, representing how aerosols activate and serve as cloud condensation nuclei and ultimately cloud droplets. While it is possible to build explicit numerical models which describe this process in detail, these class of tools are untenable for use in global climate models due to their complexity. Instead, physically- or empirically-based parameterizations of activation are used in their place to efficiently approximate cloud droplet nucleation as a function of a few meteorological and aerosol physical/chemical properties. As global climate models are outfitted with more complex, size- and mixing state-resolving aerosol models, activation parameterizations are increasingly called upon to handle aerosol populations against which their performance has not been explicitly benchmarked. Here, a simple scheme is proposed to evaluate the performance of activation parameterizations against a spectrum of mixing states, and two schemes commonly used in global models are studied using this framework. It is shown that each scheme exhibits systematic biases when a complex mixing state is present. To help resolve these issues, a new scheme is derived using Polynomial Chaos Expansion to build meta-models representing a full complexity parcel model. The meta-models are shown to accurately handle activation in both single-mode and mixture cases. In addition, a global sensitivity analysis is applied to benchmark the performance of the meta-models and the activation parameterizations against a detailed parcel model, and it is shown that the meta-models tend to more accurately attribute variability in activation dynamics to each input parameter and their interactions with others when compared to the physically-based parameterizations. A variety of experiments

  3. Black carbon aerosol optical properties are influenced by initial mixing state

    NASA Astrophysics Data System (ADS)

    Willis, M. D.; Healy, R. M.; Riemer, N.; West, M.; Wang, J. M.; Jeong, C. H.; Wenger, J.; Abbatt, J.; Lee, A.

    2015-12-01

    Incomplete combustion emits teragram quantities of black carbon (BC) aerosol to the troposphere each year, resulting in a significant warming effect on climate that may be second only to carbon dioxide. The magnitude of BC impacts on a global scale remains poorly constrained and is intimately related to its particle-scale physical and chemical properties. Using particle-resolved modeling informed by novel quantitative measurements from an Aerodyne soot-particle aerosol mass spectrometer (SP-AMS), we show that initial mixing state (or the distribution of co-emitted components amongst fresh BC-containing particles) significantly affects BC-aerosol optical properties even after a day of atmospheric processing. Both single particle and ensemble observations indicate that BC near emission co-exists with hydrocarbon-like organic aerosol (HOA) in two distinct particle types: HOA-rich and BC-rich particles. The average mass fraction of black carbon (mfBC) in HOA- and BC-rich particle types was 0.02-0.08 and 0.72-0.93, respectively. Notably, positive matrix factorization (PMF) analysis of ensemble SP-AMS measurements indicates that BC-rich particles contribute the majority of BC mass (> 90%) in freshly emitted particles. This new measurement capability provides quantitative insight into the physical and chemical nature of BC-containing particles and is used to drive a particle-resolved aerosol box model. Significant differences in calculated single scattering albedo (an increase of 0.1) arise from accurate treatment of initial particle mixing state as compared to the assumption of uniform aerosol composition at the point of BC injection to the atmosphere.

  4. Mixing state and spectral absorption of atmospheric aerosols observed at a marine background site

    NASA Astrophysics Data System (ADS)

    Cayetano, M. G.; Lee, K. Y.; Kim, Y. J.

    2011-12-01

    Mineral dust and sea salt particles are portions of atmospheric aerosols in Korea due to the periodic transport of loess dust particles from Gobi and Taklimakan deserts in west China, as well as the sea salt enrichment of atmospheric particles from the seas surrounding the Korean peninsula [Kim et al., 2009; Sahu et al., 2009]. Carbonaceous particles and secondary inorganic aerosols (sulphates and nitrates) are ubiquitous due to the proliferating biomass burning [Ryu et al., 2004], as well as the increasing use of fossil fuels locally and by regional transport from neighbouring countries. Collectively, when these aerosols are transported, their compositions are further modified due to the aging process, impacting their physico-chemical properties including spectral absorption. In order to investigate the spectral response of the absorption under different ambient aerosol conditions, measurements have been conducted at a marine background site in Korea (Deokjeok Island. 37° 13' 33" N, 126° 8' 51" E) during the spring (13 days) and fall (8 days) seasons of 2009 using an aethalometer (Magee AE31), a nephelometer (Optec NGN2a) and other supporting instruments (PILS-IC, PM2.5 cyclone samplers for off-line OC/EC measurements). It has been found that spring aerosols were dominated by sulphate-rich and carbonaceous-rich fractions (21.4%±8.0% and 28.8%±7.9%, respectively), with an Angström exponent of absorption, αabs = 1.3±0.1 at 370-950 nm. The fall season aerosols were grouped based on their chemical composition as acidic aerosols, dust-enriched, and seasalt-enriched aerosols. Angström exponent of absorption, αabs for acidic aerosols was obtained to be 1.3±0.2 at 370-950 nm. However, dust enriched aerosols showed increased absorption in the short UV-Vis range (370-590 nm), which can be attributed to their mixing with light absorbing aerosols. Different types of aerosols exhibit different spectral absorption characteristics depending on their composition and

  5. Aerosol mixing-state, hygroscopic growth and cloud activation efficiency during MIRAGE 2006

    NASA Astrophysics Data System (ADS)

    Lance, S.; Raatikainen, T.; Onasch, T.; Worsnop, D. R.; Yu, X.-Y.; Alexander, M. L.; Stolzenburg, M. R.; McMurry, P. H.; Smith, J. N.; Nenes, A.

    2012-06-01

    Observations of aerosol hygroscopic growth and CCN activation spectra for submicron particles are reported for the T1 ground site outside of Mexico City during the MIRAGE 2006 campaign. κ-Köhler theory is used to evaluate the characteristic water uptake coefficient, κ*, for the CCN active aerosol population using both size-resolved HTDMA and size-resolved CCNc measurements. Organic mass fractions, forg, are evaluated from size-resolved aerosol mass spectrometer (AMS) measurements, from which κAMS is inferred and compared against κ*. Strong diurnal profiles of aerosol water uptake parameters and aerosol composition are observed. We find that new particle formation (NPF) events are correlated with an increased κ* and CCN-active fraction during the daytime, with greater impact on smaller particles. During NPF events, the number concentration of 40 nm particles acting as CCN can surpass by more than a factor of two the concentrations of 100 nm particles acting as CCN, at supersaturations of 0.51% ± 0.06%. We also find that at 06:00-08:00 in the morning throughout the campaign, fresh traffic emissions result in substantial changes to the chemical distribution of the aerosol, with on average 65% externally-mixed fraction for 40 nm particles and 30% externally-mixed fraction for 100 nm particles, whereas at midday nearly all particles of both sizes can be described as internally-mixed. Average activation spectra and growth factor distributions are analyzed for different time periods characterizing the daytime (with and without NPF events), the early morning "rush hour", and the entire campaign. We show that κ* derived from CCNc measurements decreases as a function of size during all time periods, while the CCN-active fraction increases as a function of size. Size-resolved AMS measurements do not predict the observed trend for κ* versus particle size, which can be attributed to unresolved mixing-state and the presence of refractory material not measured by the AMS

  6. Influence of particle-phase state on the hygroscopic behavior of mixed organic-inorganic aerosols

    NASA Astrophysics Data System (ADS)

    Hodas, N.; Zuend, A.; Mui, W.; Flagan, R. C.; Seinfeld, J. H.

    2015-05-01

    Recent work has demonstrated that organic and mixed organic-inorganic particles can exhibit multiple phase states depending on their chemical composition and on ambient conditions such as relative humidity (RH). To explore the extent to which water uptake varies with particle-phase behavior, hygroscopic growth factors (HGFs) of nine laboratory-generated, organic and organic-inorganic aerosol systems with physical states ranging from well-mixed liquids to phase-separated particles to viscous liquids or semi-solids were measured with the Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe at RH values ranging from 40 to 90%. Water-uptake measurements were accompanied by HGF and RH-dependent thermodynamic equilibrium calculations using the Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model. In addition, AIOMFAC-predicted growth curves are compared to several simplified HGF modeling approaches: (1) representing particles as ideal, well-mixed liquids; (2) forcing a single phase but accounting for non-ideal interactions through activity coefficient calculations; and (3) a Zdanovskii-Stokes-Robinson-like calculation in which complete separation of the inorganic and organic components is assumed at all RH values, with water uptake treated separately in each of the individual phases. We observed variability in the characteristics of measured hygroscopic growth curves across aerosol systems with differing phase behaviors, with growth curves approaching smoother, more continuous water uptake with decreasing prevalence of liquid-liquid phase separation and increasing oxygen : carbon ratios of the organic aerosol components. We also observed indirect evidence for the dehydration-induced formation of highly viscous semi-solid phases and for kinetic limitations to the crystallization of ammonium sulfate at low RH for sucrose-containing particles. AIOMFAC-predicted growth curves are generally in good agreement with the HGF

  7. Influence of particle phase state on the hygroscopic behavior of mixed organic-inorganic aerosols

    NASA Astrophysics Data System (ADS)

    Hodas, N.; Zuend, A.; Mui, W.; Flagan, R. C.; Seinfeld, J. H.

    2014-12-01

    Recent work has demonstrated that organic and mixed organic-inorganic particles can exhibit multiple phase states depending on their chemical composition and on ambient conditions such as relative humidity (RH). To explore the extent to which water uptake varies with particle phase behavior, hygroscopic growth factors (HGFs) of nine laboratory-generated, organic and organic-inorganic aerosol systems with physical states ranging from well-mixed liquids, to phase-separated particles, to viscous liquids or semi-solids were measured with the Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe at RH values ranging from 40-90%. Water-uptake measurements were accompanied by HGF and RH-dependent thermodynamic equilibrium calculations using the Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model. In addition, AIOMFAC-predicted growth curves are compared to several simplified HGF modeling approaches: (1) representing particles as ideal, well-mixed liquids, (2) forcing a single phase, but accounting for non-ideal interactions through activity coefficient calculations, and (3) a Zdanovskii-Stokes-Robinson-like calculation in which complete separation between the inorganic and organic components is assumed at all RH values, with water-uptake treated separately in each of the individual phases. We observed variability in the characteristics of measured hygroscopic growth curves across aerosol systems with differing phase behaviors, with growth curves approaching smoother, more continuous water uptake with decreasing prevalence of liquid-liquid phase separation and increasing oxygen : carbon ratios of the organic aerosol components. We also observed indirect evidence for the dehydration-induced formation of highly viscous semi-solid phases and for kinetic limitations to the crystallization of ammonium sulfate at low RH for sucrose-containing particles. AIOMFAC-predicted growth curves are generally in good agreement with the HGF

  8. Measurements of the aerosol chemical composition and mixing state in the Po Valley using multiple spectroscopic techniques

    NASA Astrophysics Data System (ADS)

    Decesari, S.; Allan, J.; Plass-Duelmer, C.; Williams, B. J.; Paglione, M.; Facchini, M. C.; O'Dowd, C.; Harrison, R. M.; Gietl, J. K.; Coe, H.; Giulianelli, L.; Gobbi, G. P.; Lanconelli, C.; Carbone, C.; Worsnop, D.; Lambe, A. T.; Ahern, A. T.; Moretti, F.; Tagliavini, E.; Elste, T.; Gilge, S.; Zhang, Y.; Dall'Osto, M.

    2014-11-01

    The use of co-located multiple spectroscopic techniques can provide detailed information on the atmospheric processes regulating aerosol chemical composition and mixing state. So far, field campaigns heavily equipped with aerosol mass spectrometers have been carried out mainly in large conurbations and in areas directly affected by their outflow, whereas lesser efforts have been dedicated to continental areas characterised by a less dense urbanisation. We present here the results obtained at a background site in the Po Valley, Italy, in summer 2009. For the first time in Europe, six state-of-the-art spectrometric techniques were used in parallel: aerosol time-of-flight mass spectrometer (ATOFMS), two aerosol mass spectrometers (high-resolution time-of-flight aerosol mass spectrometer - HR-ToF-AMS and soot particle aerosol mass spectrometer - SP-AMS), thermal desorption aerosol gas chromatography (TAG), chemical ionisation mass spectrometry (CIMS) and (offline) proton nuclear magnetic resonance (1H-NMR) spectroscopy. The results indicate that, under high-pressure conditions, atmospheric stratification at night and early morning hours led to the accumulation of aerosols produced by anthropogenic sources distributed over the Po Valley plain. Such aerosols include primary components such as black carbon (BC), secondary semivolatile compounds such as ammonium nitrate and amines and a class of monocarboxylic acids which correspond to the AMS cooking organic aerosol (COA) already identified in urban areas. In daytime, the entrainment of aged air masses in the mixing layer is responsible for the accumulation of low-volatility oxygenated organic aerosol (LV-OOA) and also for the recycling of non-volatile primary species such as black carbon. According to organic aerosol source apportionment, anthropogenic aerosols accumulating in the lower layers overnight accounted for 38% of organic aerosol mass on average, another 21% was accounted for by aerosols recirculated in

  9. Size, composition, and mixing state of individual aerosol particles in a South China coastal city.

    PubMed

    Li, Weijun; Shao, Longyi; Wang, Zhishi; Shen, Rongrong; Yang, Shusheng; Tang, Uwa

    2010-01-01

    Aerosol samples were collected in summer in Macao, a coastal city of the Pearl River Delta Region in China. Morphology, size, elemental composition, and mixing state of individual aerosol particles were determined by scanning electron microscopy coupled energy dispersive X-ray (SEM/EDX) and transmission electron microscopy (TEM). Based on the morphologies of 5711 aerosol particles, they consist of soot (32%), mineral (17%), secondary (22%), and unknown fine particles (29%). The sizes of these particles were mostly distributed between 0.1 and 0.4 microm. Compositions of 202 mineral particles were obtained by SEM/EDX. Mineral particles were mainly classified into three types: Si-rich, Ca-rich, and Na-rich. The compositions of typical mineral particles can indicate their sources in sampling location. For example, mineral particles, collected along the main street, were associated with trace amounts of heavy metals, such as Zn, Ti, Mn, Ba, Pb, and As. TEM observations indicate that most Na-rich particles were aged sea salt particles (e.g., Na2SO4 and NaNO3) which formed through heterogeneous chemical reactions between sea salt and acidic gases. Additionally, aging time of soot was short in Macao due to high humidity, high temperature, and high levels of sunlight in Macao. Most of soot and fine mineral dust particles were internally mixed with secondary particles.

  10. The mixing state of carbonaceous aerosol particles in northern and southern California measured during CARES and CalNex 2010

    SciTech Connect

    Cahill, John F.; Suski, Kaitlyn; Seinfeld, John H.; Zaveri, Rahul A.; Prather, Kimberly A.

    2012-11-21

    Carbonaceous aerosols impact climate directly by scattering and absorbing radiation, and hence play a major, although highly uncertain, role in global radiative forcing. Commonly, ambient carbonaceous aerosols are internally mixed with secondary species such as nitrate, sulfate, and ammonium, which influence their climate impacts through optical properties, hygroscopicity, and atmospheric lifetime. Aircraft-aerosol time-of-flight mass spectrometry (A-ATOFMS), which measures single-particle mixing state, was used to determine the fraction of organic and soot aerosols that were internally mixed and the variability of their mixing state in California during the Carbonaceous Aerosol and Radiative Effects Study (CARES) and the Research at the Nexus of Air Quality and Climate Change (CalNex) field campaigns in the late spring and early summer of 2010. Nearly 88% of all A-ATOFMS measured particles (100-1000 nm in diameter) were internally mixed with secondary species, with 96% and 75% of particles internally mixed with nitrate and/or sulfate in southern and northern California, respectively. Even though atmospheric particle composition in both regions was primarily influenced by urban sources, the mixing state was found to vary greatly, with nitrate and soot being the dominant species in southern California, and sulfate and organic carbon in northern California. Furthermore, mixing state varied temporally in northern California, with soot becoming the prevalent particle type towards the end of the study as regional pollution levels increased. The results from these studies demonstrate that the majority of ambient carbonaceous particles are internally mixed and are heavily influenced by secondary species that are most predominant in each region. Based on these findings, considerations of regionally dominant sources and secondary species, as well as temporal variations of aerosol physical and optical properties, will be required to obtain more accurate predictions of the

  11. Using the Aerosol Single Scattering Albedo and Angstrom Exponent from AERONET to Determine Aerosol Origins and Mixing States over the Indo-Gangetic Plain

    NASA Astrophysics Data System (ADS)

    Giles, D. M.; Holben, B. N.; Eck, T. F.; Sinyuk, A.; Slutsker, I.; Smirnov, A.; Schafer, J. S.; Dickerson, R. R.; Thompson, A. M.; Tripathi, S. N.; Singh, R. P.; Ghauri, B.

    2012-12-01

    Aerosol mixtures—whether dominated by dust, carbon, sulfates, nitrates, sea salt, or mixtures of them—complicate the retrieval of remotely sensed aerosol properties from satellites and possibly increase the uncertainty of the aerosol radiative impact on climate. Major aerosol source regions in South Asia include the Thar Desert as well as agricultural lands, Himalayan foothills, and large urban centers in and near the Indo-Gangetic Plain (IGP). Over India and Pakistan, seasonal changes in meteorology, including the monsoon (June-September), significantly affect the transport, lifetime, and type of aerosols. Strong monsoonal winds can promote long range transport of dust resulting in mixtures of dust and carbonaceous aerosols, while more stagnant synoptic conditions (e.g., November-January) can prolong the occurrence of urban/industrial pollution, biomass burning smoke, or mixtures of them over the IGP. Aerosol Robotic Network (AERONET) Sun/sky radiometer data are analyzed to show the aerosol optical depth (AOD) seasonality and aerosol dominant mixing states. The Single Scattering Albedo (SSA) and extinction Angstrom exponent (EAE) relationship has been shown to provide sound clustering of dominant aerosol types using long term AERONET site data near known source regions [Giles et al., 2012]. In this study, aerosol type partitioning using the SSA (440 nm) and EAE (440-870 nm) relationship is further developed to quantify the occurrence of Dust, Mixed (e.g., dust and carbonaceous aerosols), Urban/Industrial (U/I) pollution, and Biomass Burning (BB) smoke. Based on EAE thresholds derived from the cluster analysis (for AOD440nm>0.4), preliminary results (2001-2010) for Kanpur, India, show the overall contributions of each dominant particle type (rounded to the nearest 10%): 10% for Dust (EAE≤0.25), 60% for Mixed (0.251.25). In the IGP, BB aerosols may have varying sizes (e.g., corresponding to 1.2

  12. Mixing state of ambient aerosols in Nanjing city by single particle mass spectrometry

    NASA Astrophysics Data System (ADS)

    Wang, Honglei; An, Junlin; Shen, Lijuan; Zhu, Bin; Xia, Li; Duan, Qing; Zou, Jianan

    2016-05-01

    To investigate the mixing state and size-resolved aerosol in Nanjing, measurements were carried out for the period 14th January-1st February 2013 by using a Single Particle Aerosol Mass Spectrometer (SPAMS). A total of 10,864,766 particles were sized with vacuum aerodynamic diameter (dva) in the range of 0.2-2.0 μm. Of which, 1,989,725 particles were successfully ionized. Aerosol particles employed for analyzing SPAMS data utilized 96% of the hit particles to identify 5 main particle groups. The particle classes include: K-rich particles (K-CN, K-Nitrate, K-Sulfate and K-Secondary), sodium particles, ammonium particles, carbon-rich particles (OC, EC and OCEC) and heavy-metal particles (Fe-Secondary, Pb-Nitrate, Cu-Mn-Secondary and V-Secondary). EC was the largest contributor with a fraction of 21.78%, followed by K-Secondary (17.87%), K-Nitrate (12.68%) and K-CN (11.25%). High particle level and high RH (relative humidity) are two important factors decreasing visibility in Nanjing. Different particle classes have distinct extinction effects. It anti-correlated well with visibility for the K-secondary, sodium, ammonium, EC, Fe-Secondary and K-Nitrate particles. The proportion of EC particles at 0.65-1.4 μm was up to 25% on haze days and was below 10% on clean days.

  13. Airborne measurements of hygroscopicity and mixing state of aerosols in the planetary boundary layer during the PEGASOS campaigns

    NASA Astrophysics Data System (ADS)

    Rosati, Bernadette; Weingartner, Ernest; Gysel, Martin; Rubach, Florian; Mentel, Thomas; Baltensperger, Urs

    2014-05-01

    Aerosols interact directly with the incident solar radiation by scattering or absorbing the light. The optical properties of an aerosol particle can strongly be altered at enhanced relative humidity (RH). Depending on the particle's chemical composition, it can experience hygroscopic growth, leading to a change in size and index of refraction compared to the dry particle (Zieger et al., 2011). Besides, aerosols can exist in different mixing states which are usually divided into internal and external mixtures. If all particles of a certain size have the same chemical composition, they are described as internally mixed, whereas if particles of equal size have different chemical composition, they are defined as externally mixed. Depending on the mixture the hygroscopic behavior will change: internally mixed aerosols will grow uniformly with increasing RH, while the different substances in external mixtures will experience different growing behaviors leading to a mode-splitting or broadened size distribution. Laboratory studies are commonly performed at dry conditions but it is known that temperature and RH as well as chemical composition are changing with altitude (Morgan et al., 2010). This further leads to the conclusion that the in-situ measurements of optical properties at different heights are crucial for climate forcing calculations. Within the Pan-European Gas-Aerosols-climate interaction Study (PEGASOS) the white- light humidified optical particle spectrometer (WHOPS) was developed and installed on the Zeppelin to investigate changes of light scattering with regard to water uptake and altitude. This instrument firstly selects a dry monodisperse aerosol by its electrical mobility and then exposes it to a well-defined RH (typically 95%). Alternately, the dry and humidified particles are measured in a white-light optical particle spectrometer (WELAS). In this way it is possible to infer the effective index of refraction of the dry particles, their hygroscopic

  14. Measurements of the aerosol chemical composition and mixing state in the Po Valley using multiple spectroscopic techniques

    NASA Astrophysics Data System (ADS)

    Decesari, S.; Allan, J.; Plass-Duelmer, C.; Williams, B. J.; Paglione, M.; Facchini, M. C.; O'Dowd, C.; Harrison, R. M.; Gietl, J. K.; Coe, H.; Giulianelli, L.; Gobbi, G. P.; Lanconelli, C.; Carbone, C.; Worsnop, D.; Lambe, A. T.; Ahern, A. T.; Moretti, F.; Tagliavini, E.; Elste, T.; Gilde, S.; Zhang, Y.; Dall'Osto, M.

    2014-04-01

    The use of co-located multiple spectroscopic techniques can provide detailed information on the atmospheric processes regulating aerosol chemical composition and mixing state. So far, field campaigns heavily equipped with aerosol mass spectrometers have been carried out mainly in large conurbations and in areas directly affected by their outflow, whereas lesser efforts have been dedicated to continental areas characterized by a less dense urbanization. We present here the results obtained in San Pietro Capofiume, which is located in a sparsely inhabited sector of the Po Valley, Italy. The experiment was carried out in summer 2009 in the framework of the EUCAARI project ("European Integrated Project on Aerosol, Cloud Climate Aerosol Interaction"). For the first time in Europe, six state-of-the-art techniques were used in parallel: (1) on-line TSI aerosol time-of-flight mass spectrometer (ATOFMS), (2) on-line Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS), (3) soot particle aerosol mass spectrometer (SP-AMS), (4) on-line high resolution time-of-flight mass spectrometer-thermal desorption aerosol gas chromatograph (HR-ToFMS-TAG), (5) off-line twelve-hour resolution proton nuclear magnetic resonance (H-NMR) spectroscopy, and (6) chemical ionization mass spectrometry (CIMS) for the analysis of gas-phase precursors of secondary aerosol. Data from each aerosol spectroscopic method were analysed individually following ad-hoc tools (i.e. PMF for AMS, Art-2a for ATOFMS). The results obtained from each techniques are herein presented and compared. This allows us to clearly link the modifications in aerosol chemical composition to transitions in air mass origin and meteorological regimes. Under stagnant conditions, atmospheric stratification at night and early morning hours led to the accumulation of aerosols produced by anthropogenic sources distributed over the Po Valley plain. Such aerosols include primary components such as black carbon (BC

  15. Evidence of the aerosol core-shell mixing state over Europe during the heat wave of summer 2003 by using CHIMERE simulations and AERONET inversions

    NASA Astrophysics Data System (ADS)

    Péré, J. C.; Mallet, M.; Bessagnet, B.; Pont, V.

    2009-05-01

    The aim of this work consists to infer the most probable mixing state of aerosols over the European continent during the heat wave of summer 2003, where large concentrations of biomass burning and anthropogenic aerosols have been observed. The methodology presented here is based on the Single Scattering Albedo (SSA) sensitivity to the mixing state of particles. Three different mixing cases; external mixing, internal mixing, and core-shell type mixing have been considered. Composite SSA has been computed for this intense pollution event over Europe and are compared with the AErosol RObotic NETwork (AERONET) retrieved SSA values. The most probable mixing state seems to be core-shell mixing, with secondary aerosols coating over primary soot and mineral dust. This work underlines clearly that this specific representation should be used in modeling exercises for simulating anthropogenic and/or biomass burning direct and semi-direct aerosol effects and climate impact over the European region.

  16. Providing Size-Resolved Mixing State Inputs to Improve Aerosol Optics Models: Comparison of ACE-Asia Aerosol Chemical Measurements for Different Source Regions With Simultaneous Optical Measurements

    NASA Astrophysics Data System (ADS)

    Sullivan, R. C.; Poon, G.; Guazzotti, S.; Sodeman, D.; Holecek, J.; Spencer, M.; Prather, K.

    2005-12-01

    Measurements made of the aerodynamic size and chemical composition of single aerosol particles on board the R/V Ronald H. Brown sailing between Hawaii and the Sea of Japan during ACE-Asia in 2001 revealed a complex mixture of mineral dust, organic carbon, elemental carbon, sulfates, nitrates, chloride, ammonium, and sea salt. The air mass source regions included influences from the Pacific Ocean, Miyakejima volcano, Gobi and Taklimakan Deserts, Shanghai, Japan, and Korea. The particle composition sampled from each of these regions showed unique changes in the aerosol's mixing state. This complexity presents major challenges in accurately modeling the optical properties of the Asian aerosol. The degree of closure between the measured chemical and optical properties of this aerosol and those predicted by models has been presented by Quinn et al. [JGR, 109, D19S01, doi: 10.1029/2003JD004010, 2004]. Differences between measured and calculated aerosol absorption coefficients were partly attributed to the assumption of internally mixed homogeneous spheres for the aerosol population. Good correlations between measured and calculated aerosol mass and light scattering were found but relied on particle shapes not confirmed by measurements. To better our understanding of the relationship between aerosol chemistry and optical measurements, and provide more detailed inputs to improve the predictions of optical models, we present size-resolved single-particle mixing state results obtained by an ATOFMS for the seven air mass source regions described by Quinn et al. (2004). Our results do not support the assumption of a homogeneous internally mixed aerosol population for many of the source regions. Particular focus is given to the mixing state and chemical associations of sulfate, nitrate, chloride, ammonium, OC, EC, dust, and sea salt. We demonstrate the segregation of ammonium, sulfate, and nitrate within individual particles throughout the study and discuss the different

  17. Importance of aerosol composition, mixing state, and morphology for heterogeneous ice nucleation: A combined field and laboratory approach

    SciTech Connect

    Baustian, Kelly J.; Cziczo, Daniel J.; Wise, M. A.; Pratt, Kerri; Kulkarni, Gourihar R.; Hallar, Anna G.; Tolbert, Margaret A.

    2012-03-30

    In this study chemical compositions of background aerosol and ice nuclei were examined through laboratory investigations using Raman spectroscopy and field measurements by single-particle mass spectrometry. Aerosol sampling took place at Storm Peak Laboratory in Steamboat Springs, Colorado (elevation of 3210 m). A cascade impactor was used to collect coarse-mode aerosol particles for laboratory analysis by Raman spectroscopy; the composition, mixing state, and heterogeneous ice nucleation activity of individual particles were examined. For in situ analysis of fine-mode aerosol, ice nucleation on ambient particles was observed using a compact ice nucleation chamber. Ice crystals were separated from unactivated aerosol using a pumped counterflow virtual impactor, and ice nuclei were analyzed using particle analysis by laser mass spectrometry. For both fine and coarse modes, the ice nucleating particle fractions were enriched in minerals and depleted in sulfates and nitrates, compared to the background aerosol sampled. The vast majority of particles in both the ambient and ice active aerosol fractions contained a detectable amount of organic material. Raman spectroscopy showed that organic material is sometimes present in the form of a coating on the surface of inorganic particles. We find that some organic-containing particles serve as efficient ice nuclei while others do not. For coarse-mode aerosol, organic particles were only observed to initiate ice formation when oxygen signatures were also present in their spectra.

  18. Importance of aerosol composition, mixing state, and morphology for heterogeneous ice nucleation: A combined field and laboratory approach

    NASA Astrophysics Data System (ADS)

    Baustian, Kelly J.; Cziczo, Daniel J.; Wise, Matthew E.; Pratt, Kerri A.; Kulkarni, Gourihar; Hallar, A. Gannet; Tolbert, Margaret A.

    2012-03-01

    In this study chemical compositions of background aerosol and ice nuclei were examined through laboratory investigations using Raman spectroscopy and field measurements by single-particle mass spectrometry. Aerosol sampling took place at Storm Peak Laboratory in Steamboat Springs, Colorado (elevation of 3210 m). A cascade impactor was used to collect coarse-mode aerosol particles for laboratory analysis by Raman spectroscopy; the composition, mixing state, and heterogeneous ice nucleation activity of individual particles were examined. For in situ analysis of fine-mode aerosol, ice nucleation on ambient particles was observed using a compact ice nucleation chamber. Ice crystals were separated from unactivated aerosol using a pumped counterflow virtual impactor, and ice nuclei were analyzed using particle analysis by laser mass spectrometry. For both fine and coarse modes, the ice nucleating particle fractions were enriched in minerals and depleted in sulfates and nitrates, compared to the background aerosol sampled. The vast majority of particles in both the ambient and ice active aerosol fractions contained a detectable amount of organic material. Raman spectroscopy showed that organic material is sometimes present in the form of a coating on the surface of inorganic particles. We find that some organic-containing particles serve as efficient ice nuclei while others do not. For coarse-mode aerosol, organic particles were only observed to initiate ice formation when oxygen signatures were also present in their spectra.

  19. Discrete dipole approximation for black carbon-containing aerosols in arbitrary mixing state: A hybrid discretization scheme

    NASA Astrophysics Data System (ADS)

    Moteki, Nobuhiro

    2016-07-01

    An accurate and efficient simulation of light scattering by an atmospheric black carbon (BC)-containing aerosol-a fractal-like cluster of hundreds of carbon monomers that is internally mixed with other aerosol compounds such as sulfates, organics, and water-remains challenging owing to the enormous diversities of such aerosols' size, shape, and mixing state. Although the discrete dipole approximation (DDA) is theoretically an exact numerical method that is applicable to arbitrary non-spherical inhomogeneous targets, in practice, it suffers from severe granularity-induced error and degradation of computational efficiency for such extremely complex targets. To solve this drawback, we propose herein a hybrid DDA method designed for arbitrary BC-containing aerosols: the monomer-dipole assumption is applied to a cluster of carbon monomers, whereas the efficient cubic-lattice discretization is applied to the remaining particle volume consisting of other materials. The hybrid DDA is free from the error induced by the surface granularity of carbon monomers that occurs in conventional cubic-lattice DDA. In the hybrid DDA, we successfully mitigate the artifact of neglecting the higher-order multipoles in the monomer-dipole assumption by incorporating the magnetic dipole in addition to the electric dipole into our DDA formulations. Our numerical experiments show that the hybrid DDA method is an efficient light-scattering solver for BC-containing aerosols in arbitrary mixing states. The hybrid DDA could be also useful for a cluster of metallic nanospheres associated with other dielectric materials.

  20. Comparison of aerosol hygroscopicity and mixing state between winter and summer seasons in Pearl River Delta region, China

    NASA Astrophysics Data System (ADS)

    Jiang, Rongxin; Tan, Haobo; Tang, Lili; Cai, Mingfu; Yin, Yan; Li, Fei; Liu, Li; Xu, Hanbing; Chan, P. W.; Deng, Xuejiao; Wu, Dui

    2016-03-01

    Hygroscopic properties of aerosol particles are important for determining aerosol size distributions, and thus determining scattering and absorption coefficients at ambient atmospheric conditions. In this study, hygroscopic properties of aerosol particles at an urban site in Guangzhou, China, were measured using a Hygroscopic Tandem Differential Mobility Analyzer (H-TDMA) system during the winter and the summer. The results show that the urban aerosols were composed of more-hygroscopic, less-hygroscopic and non-hygroscopic particles. For less-hygroscopic particles of 40-200 nm in diameter, the hygroscopic parameter κLH was around 0.15. For more-hygroscopic particles, the κMH was from 0.290 to 0.339 with a particle size from 40 to 200 nm. For non-hygroscopic particles, the κNH was about 0.015. It was found that the number fraction of less-hygroscopic particles (NFLH) was correlated with the atmospheric oxidation which can be presented by OC/EC. This paper attributed the larger NFLH in winter to the higher value of OC/EC (3.0). Such conditions may lead to more formation of less-hygroscopic particles. Backward trajectories cluster analysis shows that there is a certain link between air mass origin and aerosol hygroscopicity, but it seems to be independent of the level of pollution. The difference of NFNH indicates that the mixing state of aerosol particles can also be affected by air mass origin. Diurnal variations in aerosol hygroscopic parameters in both seasons show that during daytime, aerosol particles tend to have a low degree of external mixing or quasi-internal mixing, resulting in a higher NFMH and a larger κmean; during nighttime and early mornings, they tend to be mixed externally, resulting in a lower NFMH and a smaller κmean. This can be attributed to atmospheric aging effect and evolution of mixing layer height and implies that soot (non-hygroscopic) particles present to a large extent as internal mixtures by the time they leave the urban

  1. Mixing State and Aging of Biomass Burning Aerosols During the 2007 San Diego Wildfires

    NASA Astrophysics Data System (ADS)

    Zauscher, M. D.; Wang, Y.; Moore, M. J.; Gaston, C. J.; Prather, K. A.

    2011-12-01

    Biomass burning aerosols (BBA) significantly affect regional and global air quality, health and climate, yet their mixing state is not fully characterized. Specifically, aerosols from burning land dominated by chaparral shrubs, such as in Southern California, are less characterized than other BBA, although fires in this area have been increasing in frequency since 1980s. During the 2007 San Diego Wildfires the size-resolved chemistry of 100-400 nm single particles was determined in real-time with an ultra-fine aerosol time of flight mass spectrometer (UF-ATOFMS). BBA, identified by having a strong potassium peak and smaller carbonaceous markers present in the mass spectra, made up 84% of all particles measured between 10/22/07 and 11/1/07. Even though levoglucosan is known as a good biomass burning tracer, only 36% of all BBA in this study had this tracer present. Positive Matrix Factorization (PMF) analysis was utilized to group different BBA chemical markers, such as potassium salts, sulfate, ammonium, oxalate and levoglucosan. A spike in ammonium was observed with the increase in relative humidity on 10/25/07 and correlated with nitric acid and nitrate, indicating that the majority of ammonium was present as NH4NO3. The presence of different potassium salts were used to identify the age of BBA. K2Cl+, indicative of fresh BBA, was only seen at the beginning of the wildfires when the size mode of particles was ~<120 nm. K2NO3+ and K3SO4+ spiked at different times, with K2NO3+ peaking before K3SO4+. Particles with K3SO4+ had larger sizes than those with K2NO3+, thus K2NO3+ represents slightly aged whereas K3SO4+ represents moderately aged BBA. The largest BBA observed, and hence the most aged, were those characterized by the lack of potassium salts and the presence of secondary markers, such as sulfate and oxalate. In summary, we observed the evolution of BBA undergoing four distinct aging steps based on particle size and composition: slightly fresh, slightly aged

  2. Deriving aerosol hygroscopic mixing state from size-resolved CCN activity and HR-ToF-AMS measurements

    NASA Astrophysics Data System (ADS)

    Bhattu, Deepika; Tripathi, S. N.; Chakraborty, Abhishek

    2016-10-01

    The ability of a particle to uptake water and form a cloud droplet depends on its hygroscopicity. To understand its impact on cloud properties and ultimately radiative forcing, knowledge of chemically-resolved mixing state information or the one based on hygroscopic growth is crucial. Typically, global models assume either pure internal or external mixing state which might not be true for all conditions and sampling locations. To investigate into this, the current study employed an indirect approach to infer the probable mixing state. The hygroscopic parameters derived from κ-Kohler theory using size-resolved CCN measurements (κCCN) and bulk/size-resolved aerosol mass spectrometer (AMS) measurements (κAMS) were compared. The accumulation mode particles were found to be more hygroscopic (κCCN = 0.24) than Aitken mode (κCCN = 0.13), perhaps due to increased ratio of inorganic to organic mass fraction. The activation diameter calculated from size-resolved CCN activity measurements at 5 different supersaturation (SS) levels varied in the range of 115 nm-42 nm with κCCN = 0.13-0.23 (avg = 0.18 ± 0.10 (±1σ)). Further, κAMS>κCCN was observed possibly due to the fact that organic and inorganic mass present in the Aitken mode was not correctly represented by bulk chemical composition and size-resolved fractional contribution of oxidized OA was not accurately accounted. Better correlation of organic fraction (forg) and κCCN at lower SS explained this behaviour. The decrease in κCCN with the time of the day was more pronounced at lower SS because of the relative mass reduction of soluble inorganic species by ∼17%. Despite the large differences between κ measured from two approaches, less over-prediction (up to 18%) between measured and predicted CCN concentration suggested lower impact of chemical composition and mixing state at higher SS. However, at lower SS, presences of externally mixed CCN-inactive aerosols lead to CCN over-prediction reflecting the

  3. Wintertime Experimental investigation of Morphology, Mixing States and Columnar Optical Properties of Aerosols over a Desert location in India

    NASA Astrophysics Data System (ADS)

    Mishra, S.; Kumar, T.; Sharma, C.; Prasad, M. V. S. N.; Singh, S.; Agnihotri, R.; Arya, B. C.; Gupta, B.; Naaraayanan, T.; Gautam, S.; Kumar, D.; Sood, K. N.; Tawale, J. S.; Sharma, A. K.; Mitra, A. K.

    2014-12-01

    Indian Desert (The Thar Desert) is considered as the source of mineral dust in the Indo-Gangetic Plain (IGP) especially in pre-monsoon period due to large scale convective activities during hot summer. To study the physico-chemical characteristics of aerosols over the Thar Desert (Jaisalmer, Rajasthan) during winter (December, 2013), a field campaign has been carried out in Jaisalmer in Rajasthan state. Experiments were conducted inside the city as well as far from the city. The faraway location is close to international border of another country i.e. Pakistan. PM2.5 and PM10 were collected within the city while PM5 was collected far from the city. Particles were collected on Teflon filters for bulk analysis with Fourier Transform Infrared Spectroscopy (FTIR), on Tin substrate for individual particle morphology and elemental composition analysis with Scanning Electron Microscope (SEM) equipped with Energy Dispersive Spectrometer (EDS) and on the Cu-TEM grid for individual particle morphology and mixing state characterization using High Resolution-Transmission Electron Microscope (HRTEM). Together with this, aerosol size distribution observation and columnar spectral aerosol optical properties have been carried out with OPC (Optical Particle Counter, GRIMM Model 1.108) and hand held Microtops-II, respectively. HRTEM analysis reveals occurrence of carbonaceous fractals found in various mixing states 1) aged with some hygroscopic species 2) embedded in sulfate host 3) semi-externally mixed with sulfate and other species. Core-shell particles were also observed with varying core composition (carbon, typical mineral dust, and calcite) and shell thickness (shell comprising of water). The back trajectory analysis reveals the source of wind from Karachi and Islamabad from Pakistan which may be the potential source of carbonaceous species over the sampling site. SEM-EDS analysis reveals occurrence of mineral dust 1) pure mineral dust (Ca and Si rich) 2) polluted mineral

  4. Evaluation of Aerosol Mixing State Classes in the GISS Modele-matrix Climate Model Using Single-particle Mass Spectrometry Measurements

    NASA Technical Reports Server (NTRS)

    Bauer, Susanne E.; Ault, Andrew; Prather, Kimberly A.

    2013-01-01

    Aerosol particles in the atmosphere are composed of multiple chemical species. The aerosol mixing state, which describes how chemical species are mixed at the single-particle level, provides critical information on microphysical characteristics that determine the interaction of aerosols with the climate system. The evaluation of mixing state has become the next challenge. This study uses aerosol time-of-flight mass spectrometry (ATOFMS) data and compares the results to those of the Goddard Institute for Space Studies modelE-MATRIX (Multiconfiguration Aerosol TRacker of mIXing state) model, a global climate model that includes a detailed aerosol microphysical scheme. We use data from field campaigns that examine a variety of air mass regimens (urban, rural, and maritime). At all locations, polluted areas in California (Riverside, La Jolla, and Long Beach), a remote location in the Sierra Nevada Mountains (Sugar Pine) and observations from Jeju (South Korea), the majority of aerosol species are internally mixed. Coarse aerosol particles, those above 1 micron, are typically aged, such as coated dust or reacted sea-salt particles. Particles below 1 micron contain large fractions of organic material, internally-mixed with sulfate and black carbon, and few external mixtures. We conclude that observations taken over multiple weeks characterize typical air mass types at a given location well; however, due to the instrumentation, we could not evaluate mass budgets. These results represent the first detailed comparison of single-particle mixing states in a global climate model with real-time single-particle mass spectrometry data, an important step in improving the representation of mixing state in global climate models.

  5. Evaluation of aerosol mixing state classes in the GISS modelE-MATRIX climate model using single-particle mass spectrometry measurements

    NASA Astrophysics Data System (ADS)

    Bauer, Susanne E.; Ault, Andrew; Prather, Kimberly A.

    2013-09-01

    Aerosol particles in the atmosphere are composed of multiple chemical species. The aerosol mixing state, which describes how chemical species are mixed at the single-particle level, provides critical information on microphysical characteristics that determine the interaction of aerosols with the climate system. The evaluation of mixing state has become the next challenge. This study uses aerosol time-of-flight mass spectrometry (ATOFMS) data and compares the results to those of the Goddard Institute for Space Studies modelE-MATRIX (Multiconfiguration Aerosol TRacker of mIXing state) model, a global climate model that includes a detailed aerosol microphysical scheme. We use data from field campaigns that examine a variety of air mass regimens (urban, rural, and maritime). At all locations, polluted areas in California (Riverside, La Jolla, and Long Beach), a remote location in the Sierra Nevada Mountains (Sugar Pine) and observations from Jeju (South Korea), the majority of aerosol species are internally mixed. Coarse aerosol particles, those above 1 µm, are typically aged, such as coated dust or reacted sea-salt particles. Particles below 1 µm contain large fractions of organic material, internally mixed with sulfate and black carbon, and few external mixtures. We conclude that observations taken over multiple weeks characterize typical air mass types at a given location well; however, due to the instrumentation, we could not evaluate mass budgets. These results represent the first detailed comparison of single-particle mixing states in a global climate model with real-time single-particle mass spectrometry data, an important step in improving the representation of mixing state in global climate models.

  6. Optical Properties and Mixing State of Aerosols from Residential Wood Burning and Vehicle Emissions in Central and Southern California

    NASA Astrophysics Data System (ADS)

    Zhang, X.; Cappa, C. D.; Collier, S.; Zhang, Q.; Williams, L. R.; Lee, A.; Abbatt, J.; Russell, L. M.; Liu, J.; Chen, C. L.; Betha, R.

    2015-12-01

    Light-absorbing materials such as black carbon (BC) and brown carbon (BrC) in atmospheric aerosols play important roles in regulating the earth's radiative budget and climate. However, the representations of BC and BrC in state-of-the-art climate models remain highly uncertain, in part due to the poor understanding of their microphysical and optical properties. Direct observations and characterizations of the mixing state and absorption enhancement of ambient aerosols could provide invaluable constraints for current model representations of aerosol radiative effects. Here, we will discuss results from measurements of aerosol light absorption and absorption enhancement (Eabs), using a thermodenuder-absorption method, made during two recent field studies in central and southern California. The winter study took place in Dec/Jan of 2014/2015 in Fresno, CA. This region is severely impacted by particulate matter from local and regional residential biomass burning. The summer study took place in July 2015 in Fontana, CA, a region ~80 km downwind of Los Angeles and strongly impacted by vehicular emissions, and thus provides a sharp contrast to the Fresno study. Eabs of BC particles due to the "lensing" effect from coatings to BC core and/or the presence of BrC will be quantified and compared between the two studies. Additionally, the chemical composition of bulk and the BC-containing particles are determined via a HR-ToF-AMS and a SP-AMS, respectively. Variations in the composition and mixing state of the ambient particles and how these affect the observed Eabs will be examined. The overall measurements suggest a relatively small role for lensing-induced absorption enhancements for ambient particles in these regions.

  7. Importance of aerosol composition and mixing state for cloud droplet activation in the high Arctic

    NASA Astrophysics Data System (ADS)

    Leck, C.; Svensson, E.

    2014-08-01

    Concentrations of cloud condensation nuclei (CCN) were measured throughout an expedition by icebreaker around the central Arctic Ocean, including a 3 week ice drift operation at 87° N, from 3 August to 9 September 2008. In agreement with previous observations in the area and season median daily CCN concentrations at 0.2% water vapor supersaturation were typically in the range of 15 to 30 cm-3, but concentrations varied by two to three orders of magnitude over the expedition and were occasionally below 1 cm-3. The CCN concentrations were highest near the ice edge and fell by a factor of three in the first 48 h of transport from the open sea into the pack ice region. For longer transport times they increased again indicating a local source over the pack ice, suggested to be polymer gels, via drops injected into the air by bubbles bursting on open leads. By assuming Köhler theory and simulating the cloud nucleation process using a Lagrangian adiabatic air parcel model that solves the kinetic formulation for condensation of water on size resolved aerosol particles we inferred the properties of the unexplained non-water soluble aerosol fraction that is necessary for reproducing the observed concentrations of CCN. We propose that the portion of the internally/externally mixed water insoluble particles was larger in the corresponding smaller aerosol sizes ranges. These particles were physically and chemically behaving as polymer gels: the interaction of the hydrophilic and hydrophobic entities on the structures of polymer gels during cloud droplet activation would at first only show a partial wetting character and only weak hygroscopic growth. Given time, a high CCN activation efficiency is achieved, which is promoted by the hydrophilicity or surface-active properties of the gels. Thus the result in this study argues for that the behavior of the high Arctic aerosol in CCN-counters operating at water vapor supersaturations > 0.4% (high relative humidities) may not be

  8. Mixing state of particles with secondary species by single particle aerosol mass spectrometer in an atmospheric pollution event

    NASA Astrophysics Data System (ADS)

    Xu, Lingling; Chen, Jinsheng

    2016-04-01

    Single particle aerosol mass spectrometer (SPAMS) was used to characterize size distribution, chemical composition, and mixing state of particles in an atmospheric pollution event during 20 Oct. - 5 Nov., 2015 in Xiamen, Southeast China. A total of 533,012 particle mass spectra were obtained and clustered into six groups, comprising of industry metal (4.5%), dust particles (2.6%), carbonaceous species (70.7%), K-Rich particles (20.7%), seasalt (0.6%) and other particles (0.9%). Carbonaceous species were further divided into EC (70.6%), OC (28.5%), and mixed ECOC (0.9%). There were 61.7%, 58.3%, 4.0%, and 14.6% of particles internally mixed with sulfate, nitrate, ammonium and C2H3O, respectively, indicating that these particles had undergone significant aging processing. Sulfate was preferentially mixed with carbonaceous particles, while nitrate tended to mix with metal-containing and dust particles. Compared to clear days, the fractions of EC-, metal- and dust particles remarkably increased, while the fraction of OC-containing particles decreased in pollution days. The mixing state of particles, excepted for OC-containing particles with secondary species was much stronger in pollution days than that in clear days, which revealed the significant influence of secondary particles in atmospheric pollution. The different activity of OC-containing particles might be related to their much smaller aerodynamic diameter. These results could improve our understanding of aerosol characteristics and could be helpful to further investigate the atmospheric process of particles.

  9. Anthropogenic Effects on the Mixing State of Aerosols over Manaus during the Green Ocean Amazon (GoAmazon) Campaign

    NASA Astrophysics Data System (ADS)

    Fraund, M. W.; Pham, D.; Harder, T.; O'Brien, R.; Wang, B.; Laskin, A.; Gilles, M. K.; Moffet, R.

    2015-12-01

    The role that anthropogenic aerosols play in cloud formation is uncertain and contributes largely to the uncertainty in predicting future climate. One region of particular importance is the Amazon rainforest, which accounts for over half of the world's rainforest. During GoAmazon2014/15 IOP2, aerosol samples were collected at multiple sites in and around the rapidly growing industrial city of Manaus in the Amazon basin. Manaus is of scientific interest due to the pristine nature of the surrounding rainforest and the high levels of pollution coming from the city in the form of SO2, NOx, and soot. Some sites, such as the Terrestrial Ecosystem Science center (TES, also designated ZF2) located to the north of Manaus, represent air masses which have not interacted with emissions from the city. The comparison of pristine atmosphere with heavy pollution allows both for the determination of a natural baseline level of pollutants, as well as the study of pollutant's impact on the conversion of biogenic volatile organic compounds to secondary organic aerosols. Towards this goal, samples from ZF2 and other unpolluted sites will be compared to samples from the Atmospheric Radiation Measurement (ARM) climate research facility in Manacapuru (T3), which is southwest (downwind) of Manaus. Spatially resolved spectra were recorded at the sub-particle level using scanning transmission X-ray microscopy (STXM) at the carbon, nitrogen, and oxygen K-absorption edges. Scanning electron microscopy coupled with energy dispersive x-ray spectroscopy (SEM/EDX) was also performed on to characterize higher Z elements. These two techniques together will allow for the mass fraction of atmospherically relevant elements to be determined on a per-particle basis. We will apply established procedures to determine the mixing state index for samples collected at ZF2 and T3 using elemental mass fractions. Preliminary results will be presented which focus on investigating the difference between mixing

  10. Mixing state of aerosols and direct observation of carbonaceous and marine coatings on African dust by individual particle analysis

    NASA Astrophysics Data System (ADS)

    Deboudt, Karine; Flament, Pascal; ChoëL, Marie; Gloter, Alexandre; Sobanska, Sophie; Colliex, Christian

    2010-12-01

    The mixing state of aerosols collected at M'Bour, Senegal, during the Special Observing Period conducted in January-February 2006 (SOP-0) of the African Monsoon Multidisciplinary Analysis project (AMMA), was studied by individual particle analysis. The sampling location on the Atlantic coast is particularly adapted for studying the mixing state of tropospheric aerosols since it is (1) located on the path of Saharan dust plumes transported westward over the northern tropical Atlantic, (2) influenced by biomass burning events particularly frequent from December to March, and (3) strongly influenced by anthropogenic emissions from polluted African cities. Particle size, morphology, and chemical composition were determined for 12,672 particles using scanning electron microscopy (automated SEM-EDX). Complementary analyses were performed using transmission electron microscopy combined with electron energy loss spectrometry (TEM-EELS) and Raman microspectrometry. Mineral dust and carbonaceous and marine compounds were predominantly found externally mixed, i.e., not present together in the same particles. Binary internally mixed particles, i.e., dust/carbonaceous, carbonaceous/marine, and dust/marine mixtures, accounted for a significant fraction of analyzed particles (from 10.5% to 46.5%). Western Sahara was identified as the main source of mineral dust. Two major types of carbonaceous particles were identified: "tar balls" probably coming from biomass burning emissions and soot from anthropogenic emissions. Regarding binary internally mixed particles, marine and carbonaceous compounds generally formed a coating on mineral dust particles. The carbonaceous coating observed at the particle scale on African dust was evidenced by the combined use of elemental and molecular microanalysis techniques, with the identification of an amorphous rather than crystallized carbon structure.

  11. Size distribution and mixing state of refractory black carbon aerosol from a coastal city in South China

    NASA Astrophysics Data System (ADS)

    Wang, Qiyuan; Huang, Ru-Jin; Zhao, Zhuzi; Zhang, Ningning; Wang, Yichen; Ni, Haiyan; Tie, Xuexi; Han, Yongming; Zhuang, Mazhan; Wang, Meng; Zhang, Jieru; Zhang, Xuemin; Dusek, Uli; Cao, Junji

    2016-11-01

    An intensive measurement campaign was conducted in the coastal city of Xiamen, China to investigate the size distribution and mixing state of the refractory black carbon (rBC) aerosol. The average rBC concentration for the campaign, measured with a ground-based single particle soot photometer (SP2), was 2.3 ± 1.7 μg m- 3, which accounted for ~ 4.3% of the PM2.5 mass. A potential source contribution function model indicated that emissions from coastal cities to the southwest were the most important source for the rBC and that shipping traffic was another likely source. The mass size distribution of the rBC particles was mono-modal and approximately lognormal, with a mass median diameter (MMD) of ~ 185 nm. Larger MMDs (~ 195 nm) occurred during polluted conditions compared with non-polluted times (~ 175 nm) due to stronger biomass burning activities during pollution episodes. Uncoated or thinly-coated particles composed the bulk of the rBC aerosol, and on average ~ 31% of the rBC was internally-mixed or thickly-coated. A positive matrix factorization model showed that organic materials were the predominant component of the rBC coatings and that mixing with nitrate increased during pollution conditions. These findings should lead to improvements in the parameterizations used to model the radiative effects of rBC.

  12. Size Resolved measurements of aerosol hygroscopicity and mixing state during Green Ocean Amazon (GoAmazon) 2014

    NASA Astrophysics Data System (ADS)

    Thalman, R. M.; Artaxo, P.; Campuzano Jost, P.; Barbosa, H. M.; Day, D. A.; de Sá, S. S.; Hu, W.; Jimenez, J. L.; Kuang, C.; Palm, B. B.; Krüger, M. L.; Manzi, A. O.; Martin, S. T.; Poeschl, U.; Sedlacek, A. J., III; Senum, G.; Souza, R. A. F. D.; Springston, S. R.; Alexander, M. L.; Watson, T. B.; Wang, J.

    2014-12-01

    Measurements of size-resolved cloud condensation nucleai (CCN) spectra were performed at the T3 site of the Green Ocean Amazon (GoAmazon) field project located near Manacapuru, Brazil during 2014. The T3 site is a receptor site for both polluted urban down-wind (Manaus, BR a city of several million 70 km up wind) and background (Amazon rainforest) air-masses and can provide a contrast between clean and polluted conditions. Particle hygroscopicity (kappa) and mixing state were calculated from the particle activation spectrum measured by size selecting aerosols and exposing them to a wide range of supersaturation in the CCN counter (Droplet Measurement Technologies Continuous-Flow Streamwise Thermal Gradient CCN Chamber). The supersaturation was varied between 0.07 and 1.1% by changing a combination of both total flow rate and temperature gradient in the CCN counter. Measured spectra were examined for air masses with different level of influence from Manaus plume. Particle hygroscopicity generally peaked near noon local time which was broadly consistent with the trend in aerosol sulfate. The average kappa values during the first intensive operation period were 0.14±0.05, 0.14±0.04 and 0.16±0.06 for 75, 112 and 171 nm particles respectively. Evaluation of particle hygroscopicity and dispersion (mixing state) will be presented with respect to size and level of pollution.

  13. Integrated evaluation of aerosols from regional brown hazes over northern China in winter: Concentrations, sources, transformation, and mixing states

    NASA Astrophysics Data System (ADS)

    Li, Weijun; Zhou, Shengzhen; Wang, Xinfeng; Xu, Zheng; Yuan, Chao; Yu, Yangchun; Zhang, Qingzhu; Wang, Wenxing

    2011-05-01

    To evaluate the wintertime regional brown haze in northern China, trace gases and aerosols were measured at an urban site between 9 and 20 November 2009. Ion chromatography and transmission electron microscopy (TEM) were used to investigate soluble ions in PM2.5 and the mixing state of individual particles. The contrasts between clear and hazy days were examined in detail. Concentrations of the primary gases including NO (55.62 ppbv), NO2 (54.86 ppbv), SO2 (83.03 ppbv), and CO (2.07 ppmv) on hazy days were 2 to 6 times higher than those on clear days. In contrast, concentrations of O3 remained low (5.71 ppbv) on hazy days. Mass concentrations of PM2.5 (135.90 μg m-3) and BC (7.85 μg m-3) were 3 times higher on hazy days than on clear days. Based on the estimations from TEM analysis, fractions of both ammoniated sulfate (AS)-soot (20%) and AS-soot/organic matter/fly ash (20%) were larger on hazy days than on clear days (13% and 12%), implying that coagulation is an important mixing process in the polluted air. The SO2 emissions from coal combustion for power plants, industrial activities, and household heating led to high concentrations. Also, high concentrations of secondary sulfates significantly formed in the haze. Therefore, high concentrations of acidic gases contributed to the increased mass and number of secondary aerosols. Our study indicates that metal-catalyzed oxidation in the aqueous phase is a major pathway of sulfate formation. The mixtures of aerosol particles, together with MODIS images, suggest that the hazes covered not only the industrial cities, but extended into the neighboring rural regions.

  14. Modulation of aerosol radiative forcing due to mixing state in clear and cloudy-sky: A case study from Delhi National Capital Region, India

    NASA Astrophysics Data System (ADS)

    Srivastava, Parul; Dey, Sagnik; Srivastava, Atul K.; Singh, Sachchidanand; Tiwari, Suresh; Agarwal, Poornima

    2016-04-01

    Aerosol properties change with the change in mixing state of aerosols and therefore it is a source of uncertainty in estimated aerosol radiative forcing (ARF) from observations or by models assuming a specific mixing state. The problem is important in the Indo-Gangetic Basin, Northern India, where various aerosol types mix and show strong seasonal variations. Quantifying the modulation of ARF by mixing state is hindered by lack of knowledge about proper aerosol composition. Hence, first a detailed chemical composition analysis of aerosols for Delhi National capital region (NCR) is carried out. Aerosol composition is arranged quantitatively into five major aerosol types - accumulation dust, coarse dust, water soluble (WS), water insoluble (WINS), and black carbon (BC) (directly measured by Athelometer). Eight different mixing cases - external mixing, internal mixing, and six combinations of core- shell mixing (BC over dust, WS over dust, WS over BC, BC over WS, WS over WINS, and BC over WINS; each of the combinations externally mixed with other species) have been considered. The spectral aerosol optical properties - extinction coefficient, single scattering albedo (SSA) and asymmetry parameter (g) for each of the mixing cases are calculated and finally 'clear-sky' and 'cloudy-sky' ARF at the top-of-the-atmosphere (TOA) and surface are estimated using a radiative transfer model. Comparison of surface-reaching flux for each of the cases with MERRA downward shortwave surface flux reveals the most likely mixing state. 'BC-WINS+WS+Dust' show least deviation relative to MERRA during the pre-monsoon (MAMJ) and monsoon (JAS) seasons and hence is the most probable mixing states. During the winter season (DJF), 'BC-Dust+WS+WINS' case shows the closest match with MERRA, while external mixing is the most probable mixing state in the post-monsoon season (ON). Lowest values for both TOA and surface 'clear-sky' ARF is observed for 'BC-WINS+WS+ Dust' mixing case. TOA ARF is 0.28±2

  15. Comparative Climate Responses of Anthropogenic Greenhouse Gases, All Major Aerosol Components, Black Carbon, and Methane, Accounting for the Evolution of the Aerosol Mixing State and of Clouds/Precipitation from Multiple Aerosol Size Distributions

    NASA Astrophysics Data System (ADS)

    Jacobson, M. Z.

    2005-12-01

    evolution accounted for the first and second indirect effects and the mixing state of aerosol particles. The optical properties of clouds were found by treating black carbon inclusions surrounded by a shell of water. The albedos of snow, sea ice, and water were calculated with radiative transfer solutions, assuming black carbon inclusions in the case of snow and sea ice. The simulations accounted for 3-D energy diffusion to the deep ocean and 2-D ocean circulation. Major conclusions are (a) the most important constituents of global warming, in terms of climate response, appear to be, in order, carbon dioxide, black carbon, and methane, (b) aerosol particles (all together) appear to act on top of greenhouse gases to enhance extremes in both regional cooling and regional warming, (b) the combination of important greenhouse gases and aerosol particles can explain observed major regions of historic warming and cooling, and (d) eliminating all anthropogenic aerosol emission could more than double current global warming but would have less of an effect than independently doubling carbon dioxide.

  16. Size distribution, mixing state and source apportionment of black carbon aerosol in London during wintertime

    NASA Astrophysics Data System (ADS)

    Liu, D.; Allan, J. D.; Young, D. E.; Coe, H.; Beddows, D.; Fleming, Z. L.; Flynn, M. J.; Gallagher, M. W.; Harrison, R. M.; Lee, J.; Prevot, A. S. H.; Taylor, J. W.; Yin, J.; Williams, P. I.; Zotter, P.

    2014-09-01

    Black carbon aerosols (BC) at a London urban site were characterised in both winter- and summertime 2012 during the Clean Air for London (ClearfLo) project. Positive matrix factorisation (PMF) factors of organic aerosol mass spectra measured by a high-resolution aerosol mass spectrometer (HR-AMS) showed traffic-dominant sources in summer but in winter the influence of additional non-traffic sources became more important, mainly from solid fuel sources (SF). Measurements using a single particle soot photometer (SP2, DMT), showed the traffic-dominant BC exhibited an almost uniform BC core size (Dc) distribution with very thin coating thickness throughout the detectable range of Dc. However, the size distribution of sf (project average mass median Dc = 149 ± 22 nm in winter, and 120 ± 6 nm in summer) and BC coating thickness varied significantly in winter. A novel methodology was developed to attribute the BC number concentrations and mass abundances from traffic (BCtr) and from SF (BCsf), by using a 2-D histogram of the particle optical properties as a function of BC core size, as measured by the SP2. The BCtr and BCsf showed distinctly different sf distributions and coating thicknesses, with BCsf displaying larger Dc and larger coating thickness compared to BCtr. BC particles from different sources were also apportioned by applying a multiple linear regression between the total BC mass and each AMS-PMF factor (BC-AMS-PMF method), and also attributed by applying the absorption spectral dependence of carbonaceous aerosols to 7-wavelength Aethalometer measurements (Aethalometer method). Air masses that originated from westerly (W), southeasterly (SE), and easterly (E) sectors showed BCsf fractions that ranged from low to high, and whose mass median Dc values were 137 ± 10 nm, 143 ± 11 nm and 169 ± 29 nm, respectively. The corresponding bulk relative coating thickness of BC (coated particle size/BC core - Dp/Dc) for these same sectors was 1.28 ± 0.07, 1.45 ± 0

  17. Size distribution, mixing state and source apportionments of black carbon aerosols in London during winter time

    NASA Astrophysics Data System (ADS)

    Liu, D.; Allan, J. D.; Young, D. E.; Coe, H.; Beddows, D.; Fleming, Z. L.; Flynn, M. J.; Gallagher, M. W.; Harrison, R. M.; Lee, J.; Prevot, A. S. H.; Taylor, J. W.; Yin, J.; Williams, P. I.; Zotter, P.

    2014-06-01

    Black carbon aerosols (BC) at a London urban site were characterized in both winter and summer time 2012 during the Clean Air for London (ClearfLo) project. Positive matrix factorization (PMF) factors of organic aerosol mass spectra measured by a high resolution aerosol mass spectrometer (HR-AMS) showed traffic-dominant sources in summer but in winter the influence of additional non-traffic sources became more important, mainly from solid fuel sources (SF). Measurements using a single particle soot photometer (SP2, DMT), showed the traffic-dominant BC exhibited an almost uniform BC core size (Dc) distribution with very thin coating thickness throughout the detectable range of Dc. However the size distribution of Dc (project average mass median Dc = 149 ± 22 nm in winter, and 120 ± 6 nm in summer) and BC coating thickness varied significantly in winter. A novel methodology was developed to attribute the BC number concentrations and mass abundances from traffic (BCtr) and from SF (BCsf), by using a 2-D histogram of the particle optical properties as a function of BC core size, as measured by the SP2. The BCtr and BCsf showed distinctly different Dc distributions and coating thicknesses, with BCsf displaying larger Dc and larger coating thickness compared to BCtr. BC particles from different sources were also apportioned by applying a multiple linear regression between the total BC mass and each AMS-PMF factor (BC-AMS-PMF method), and also attributed by applying the absorption spectral dependence of carbonaceous aerosols to 7-wavelength Aethalometer measurements (Aethalometer method). Air masses that originated from westerly (W), southeasterly (SE), or easterly (E) sectors showed BCsf fractions that ranged from low to high, and whose mass median Dc values were 137 ± 10 nm, 143 ± 11 nm, and 169 ± 29 nm respectively. The corresponding bulk relative coating thickness of BC (coated particle size / BC core - Dp / Dc) for these same sectors was 1.28 ± 0.07, 1.45 ± 0

  18. Probing the impact of different aerosol sources on cloud microphysics and precipitation through in-situ measurements of chemical mixing state

    NASA Astrophysics Data System (ADS)

    Prather, K. A.; Suski, K.; Cazorla, A.; Cahill, J. F.; Creamean, J.; Collins, D. B.; Heymsfield, A.; Roberts, G. C.; DeMott, P. J.; Sullivan, R. C.; Rosenfeld, D.; Comstock, J. M.; Tomlinson, J. M.

    2011-12-01

    Aerosol particles play a crucial role in affecting cloud processes by serving as cloud nuclei. However, our understanding of which particles actually form cloud and ice nuclei limits our ability to treat aerosols properly in climate models. In recent years, it has become possible to measure the chemical composition of individual cloud nuclei within the clouds using on-line mass spectrometry. In-situ high time resolution chemistry can now be compared with cloud physics measurements to directly probe the impact of aerosol chemistry on cloud microphysics. This presentation will describe results from two recent field campaigns, CalWater in northern California and ICE-T in the western Caribbean region. Ground-based and aircraft measurements will be presented of aerosol mixing state, cloud microphysics, and meteorology. Results from single particle mass spectrometry will show the sources of the cloud seeds, including dust, biomass burning, sea spray, and biological particles. Details will be provided on how we are now able to probe the sources and cycling of atmospheric aerosols by measuring individual aerosols, cloud nuclei, and precipitation chemistry. The important role of dust, both Asian and African, and bioparticles in forming ice nuclei will be discussed. Finally, a summary will be provided discussing how these new in-situ measurements are being used to advance our understanding of complex atmospheric processes, and improve our understanding of aerosol impacts on climate.

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

    NASA Astrophysics Data System (ADS)

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

    2009-04-01

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

  20. Evolution of biomass burning aerosol over the Amazon: airborne measurements of aerosol chemical composition, microphysical properties, mixing state and optical properties during SAMBBA

    NASA Astrophysics Data System (ADS)

    Morgan, W.; Allan, J. D.; Flynn, M.; Darbyshire, E.; Hodgson, A.; Liu, D.; O'Shea, S.; Bauguitte, S.; Szpek, K.; Johnson, B.; Haywood, J.; Longo, K.; Artaxo, P.; Coe, H.

    2013-12-01

    Biomass burning represents one of the largest sources of particulate matter to the atmosphere, resulting in a significant perturbation to the Earth's radiative balance coupled with serious impacts on public health. On regional scales, the impacts are substantial, particularly in areas such as the Amazon Basin where large, intense and frequent burning occurs on an annual basis for several months. Absorption by atmospheric aerosols is underestimated by models over South America, which points to significant uncertainties relating to Black Carbon (BC) aerosol properties. Initial results from the South American Biomass Burning Analysis (SAMBBA) field experiment, which took place during September and October 2012 over Brazil on-board the UK Facility for Airborne Atmospheric Measurement (FAAM) BAe-146 research aircraft, are presented here. Aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) and a DMT Single Particle Soot Photometer (SP2). The physical, chemical and optical properties of the aerosols across the region will be characterized in order to establish the impact of biomass burning on regional air quality, weather and climate. The aircraft sampled a range of conditions including sampling of pristine Rainforest, fresh biomass burning plumes, regional haze and elevated biomass burning layers within the free troposphere. The aircraft sampled biomass burning aerosol across the southern Amazon in the states of Rondonia and Mato Grosso, as well as in a Cerrado (Savannah-like) region in Tocantins state. This presented a range of fire conditions, in terms of their number, intensity, vegetation-type and their combustion efficiencies. Near-source sampling of fires in Rainforest environments suggested that smouldering combustion dominated, while flaming combustion dominated in the Cerrado. This led to significant differences in aerosol chemical composition, particularly in terms of the BC content, with BC being enhanced in the Cerrado

  1. On the role of particle inorganic mixing state in the reactive uptake of N2O5 to ambient aerosol particles.

    PubMed

    Ryder, Olivia S; Ault, Andrew P; Cahill, John F; Guasco, Timothy L; Riedel, Theran P; Cuadra-Rodriguez, Luis A; Gaston, Cassandra J; Fitzgerald, Elizabeth; Lee, Christopher; Prather, Kimberly A; Bertram, Timothy H

    2014-01-01

    The rates of heterogeneous reactions of trace gases with aerosol particles are complex functions of particle chemical composition, morphology, and phase state. Currently, the majority of model parametrizations of heterogeneous reaction kinetics focus on the population average of aerosol particle mass, assuming that individual particles have the same chemical composition as the average state. Here we assess the impact of particle mixing state on heterogeneous reaction kinetics using the N2O5 reactive uptake coefficient, γ(N2O5), and dependence on the particulate chloride-to-nitrate ratio (nCl(-)/nNO3(-)). We describe the first simultaneous ambient observations of single particle chemical composition and in situ determinations of γ(N2O5). When accounting for particulate nCl(-)/nNO3(-) mixing state, model parametrizations of γ(N2O5) continue to overpredict γ(N2O5) by more than a factor of 2 in polluted coastal regions, suggesting that chemical composition and physical phase state of particulate organics likely control γ(N2O5) in these air masses. In contrast, direct measurement of γ(N2O5) in air masses of marine origin are well captured by model parametrizations and reveal limited suppression of γ(N2O5), indicating that the organic mass fraction of fresh sea spray aerosol at this location does not suppress γ(N2O5). We provide an observation-based framework for assessing the impact of particle mixing state on gas-particle interactions.

  2. The Pagami Creek smoke plume after long-range transport to the upper troposphere over Europe - aerosol properties and black carbon mixing state

    NASA Astrophysics Data System (ADS)

    Dahlkötter, F.; Gysel, M.; Sauer, D.; Minikin, A.; Baumann, R.; Seifert, P.; Ansmann, A.; Fromm, M.; Voigt, C.; Weinzierl, B.

    2013-11-01

    During the CONCERT~2011 field experiment with the DLR research aircraft Falcon an enhanced aerosol layer with particle linear depolarization ratios of 6-8% at 532 nm has been observed at altitudes above 10 km over northeast Germany on 16 September 2011. Dispersion simulations with HYSPLIT suggest that the elevated aerosol layer originated from the pyro-convective Pagami Creek forest fire in Minnesota, USA. The 3-4 days old smoke plume has high total refractory black carbon (rBC) mass concentrations of 0.03-0.35 μg m-3 at standard temperature and pressure (stp) with rBC mass equivalent diameters predominantly smaller than 130 nm. Assuming a~core-shell particle structure, the BC cores exhibit very thick (median: 105-136 nm) BC-free coatings, which modify the radiative transfer through this layer. A large fraction of the BC-containing particles disintegrate while passing the laser beam of the Single Particle Soot Photometer (SP2). This is shown for the first time for high-altitude aerosol layers in this study, giving evidence for heterogeneous mixing structures and possibly modified light-scattering and light-absorbing properties of the particles. This case study estimates the rBC mass import from the Pagami Creek forest fire into the upper troposphere/lower stratosphere (UTLS) region (best estimate: 25 Mg BC). A comparison to black carbon emission rates from aviation underlines the relevance of the import of forest fire aerosol on the BC load in the UTLS region. Our detailed information on the microphysics and the mixing state of the BC forest fire aerosol layer will help to better understand and investigate its radiative impact.

  3. Importance of aerosol composition and mixing state for cloud droplet activation over the Arctic pack ice in summer

    NASA Astrophysics Data System (ADS)

    Leck, C.; Svensson, E.

    2015-03-01

    Concentrations of cloud condensation nuclei (CCN) were measured throughout an expedition by icebreaker around the central Arctic Ocean, including a 3 week ice drift operation at 87° N, from 3 August to 9 September 2008. In agreement with previous observations in the area and season, median daily CCN concentrations at 0.2% water vapour supersaturation (SS) were typically in the range of 15 to 30 cm-3, but concentrations varied by 2 to 3 orders of magnitude over the expedition and were occasionally below 1 cm-3. The CCN concentrations were highest near the ice edge and fell by a factor of 3 in the first 48 h of transport from the open sea into the pack ice region. For longer transport times they increased again, indicating a local source over the pack ice, suggested to be polymer gels, via drops injected into the air by bubbles bursting on open leads. We inferred the properties of the unexplained non-water soluble aerosol fraction that was necessary for reproducing the observed concentrations of CCN. This was made possible by assuming Köhler theory and simulating the cloud nucleation process using a Lagrangian adiabatic air parcel model that solves the kinetic formulation for condensation of water on size resolved aerosol particles. We propose that the portion of the internally/externally mixed water insoluble particles was larger in the corresponding smaller aerosol size ranges. These particles were physically and chemically behaving as polymer gels: the interaction of the hydrophilic and hydrophobic entities on the structures of polymer gels during cloud droplet activation would at first only show a partial wetting character and only weak hygroscopic growth. Given time, a high CCN activation efficiency is achieved, which is promoted by the hydrophilicity or surface-active properties of the gels. Thus the result in this study argues that the behaviour of the high Arctic aerosol in CCN-counters operating at water vapour SSs > 0.4% (high relative humidities) may not

  4. Black carbon aerosol in winter northeastern Qinghai-Tibetan Plateau, China: the source, mixing state and optical property

    NASA Astrophysics Data System (ADS)

    Wang, Q. Y.; Huang, R.-J.; Cao, J. J.; Tie, X. X.; Ni, H. Y.; Zhou, Y. Q.; Han, Y. M.; Hu, T. F.; Zhu, C. S.; Feng, T.; Li, N.; Li, J. D.

    2015-11-01

    Black carbon (BC) aerosol at high altitudes of the Qinghai-Tibetan Plateau has potential effects on the regional climate and hydrological cycle. An intensive measurement campaign was conducted at Qinghai Lake (~ 3200 m above sea level) at the edge of the northeastern Qinghai-Tibetan Plateau during winter using a ground-based single particle soot photometer (SP2) and a photoacoustic extinctiometer (PAX). The average concentration of refractory BC (rBC) and number fraction of coated rBC were found to be 160 ± 190 ng m-3 and 59 % for the entire campaign, respectively. Significant enhancements of rBC loadings and number fraction of coated rBC were observed during a pollution episode, with an average value of 390 ng m-3 and 65 %, respectively. The mass size distribution of rBC particles showed log-normal distribution, with a peak diameter of ~ 187 nm regardless of the pollution level. Five-day backward trajectory analysis suggests that the air masses from north India contributed to the increased rBC loadings during the campaign. The potential source contribution function (PSCF) model combined with the fire counts map further proves that biomass burning from north India is an important potential source influencing the northeastern Qinghai-Tibetan Plateau during the pollution episode. The rBC mass absorption cross section (MACrBC) at λ = 532 nm was slightly larger in clean days (14.9 m2 g-1) than during the pollution episode (9.3 m2 g-1), likely due to the effects of brown carbon and the uncertainty of the MACrBC calculation. The MACrBC was positively correlated with number fraction of coated rBC during the pollution episode with an increasing rate of 0.18 (m2 g-1) %-1. The number fraction of coated rBC particles showed positive correlation with light absorption, suggesting that the increase of coated rBC particles will enhance the light absorption. Compared to rBC mass concentration, rBC mixing sate is more important in determining absorption during the pollution

  5. Radiative forcing under mixed aerosol conditions

    NASA Astrophysics Data System (ADS)

    GarcíA, O. E.; Expósito, F. J.; DíAz, J. P.; DíAz, A. M.

    2011-01-01

    The mixture of mineral dust with biomass burning or urban-industrial aerosols presents significant differences in optical properties when compared to those of the individual constituents, leading to different impacts on solar radiation levels. This effect is assessed by estimating the direct radiative forcing (ΔF) of these aerosols from solar flux models using the radiative parameters derived from the Aerosol Robotic Network (AERONET). These data reveal that, in oceanic and vegetative covers (surface albedo (SA) < 0.30), the aerosol effect at the top of atmosphere (TOA) is always cooling the Earth-atmosphere system, regardless of the aerosol type. The obtained average values of ΔF range between -27 ± 15 Wm-2 (aerosol optical depth (AOD) at 0.55 μm, 0.3 ± 0.3) for mineral dust mixed with urban-industrial aerosols, registered in the East Asia region, and -34 ± 18 Wm-2 (AOD = 0.8 ± 0.4) for the mixture of the mineral dust and biomass burning particles, observed in the Central Africa region. In the intermediate SA range (0.30-0.50) the TOA radiative effect depends on the aerosol absorption properties. Thus, aerosols with single scattering albedo at 0.55 μm lower than ˜0.88 lead to a warming of the system, with ΔF of 10 ± 11 Wm-2 for the mixture of mineral dust and biomass burning. Cases with SA > 0.30 are not present in East Asia region. At the bottom of atmosphere (BOA) the maximum ΔF values are associated with the highest AOD levels obtained for the mixture of mineral dust and biomass burning aerosols (-130 ± 44 Wm-2 with AOD = 0.8 ± 0.4 for SA < 0.30).

  6. Mixing state and sources of submicron regional background aerosols in the northern Qinghai-Tibet Plateau and the influence of biomass burning

    NASA Astrophysics Data System (ADS)

    Li, W. J.; Chen, S. R.; Xu, Y. S.; Guo, X. C.; Sun, Y. L.; Yang, X. Y.; Wang, Z. F.; Zhao, X. D.; Chen, J. M.; Wang, W. X.

    2015-12-01

    Transmission electron microscopy (TEM) was employed to obtain morphology, size, composition, and mixing state of background aerosols with diameter less than 1 μm in the northern Qinghai-Tibet Plateau (QTP) during 15 September to 15 October 2013. Individual aerosol particles mainly contained secondary inorganic aerosols (SIA - sulfate and nitrate) and organics during clean periods (PM2.5 mass concentration less than 2.5 μg m-3). The presence of K-Na-Cl associated with organics and an increase in soot particles suggest that an intense biomass burning event caused the highest PM2.5 concentrations (> 30 μg m-3) during the study. A large number fraction of the fly-ash-containing particles (21.73 %) suggests that coal combustion emissions in the QTP significantly contributed to air pollutants at the medium pollution level (PM2.5: 10-30 μg m-3). We concluded that emissions from biomass burning and from coal combustion both constantly contribute to anthropogenic particles in the QTP atmosphere. Based on size distributions of individual particles at different pollution levels, we found that gas condensation on existing particles is an important chemical process for the formation of SIA with organic coating. TEM observations show that refractory aerosols (e.g., soot, fly ash, and visible organic particles) likely adhere to the surface of SIA particles larger than 200 nm due to coagulation. Organic coating and soot on surface of the aged particles likely influence their hygroscopic and optical properties, respectively, in the QTP. To our knowledge, this study reports the first microscopic analysis of fine particles in the background QTP air.

  7. Particle-resolved simulation of aerosol size, composition, mixing state, and the associated optical and cloud condensation nuclei activation properties in an evolving urban plume

    SciTech Connect

    Zaveri, Rahul A.; Barnard, James C.; Easter, Richard C.; Riemer, Nicole; West, Matthew

    2010-09-11

    The recently developed particle-resolved aerosol box model PartMC-MOSAIC was used to simulate the evolution of aerosol mixing state and the associated optical and cloud condensation nuclei (CCN) activation properties in an idealized urban plume. The model explicitly resolved the size and composition of individual particles from a number of sources and tracked their evolution due to condensation/evaporation, coagulation, emission, and dilution. The ensemble black carbon (BC) specific absorption cross section increased by 40% over the course of two days as a result of BC aging by condensation and coagulation. Three- and four-fold enhancements in CCN/CN ratios were predicted to occur within 6 hours for 0.2% and 0.5% supersaturations (S), respectively. The particle-resolved results were used to evaluate the errors in the optical and CCN activation properties that would be predicted by a conventional sectional framework that assumes monodisperse, internally-mixed particles within each bin. This assumption artificially increased the ensemble BC specific absorption by 14-30% and decreased the single scattering albedo by 0.03-0.07 while the bin resolution had a negligible effect. In contrast, the errors in CCN/CN ratios were sensitive to the bin resolution, and they depended on the chosen supersaturation. For S = 0.2%, the CCN/CN ratio predicted using 100 internally-mixed bins was up to 25% higher than the particle-resolved results, while it was up to 125% higher using 10 internally-mixed bins. Errors introduced in the predicted optical and CCN properties by neglecting coagulation were also quantified.

  8. Hygroscopic properties and mixing state of aerosol measured at the high altitude site Puy de Dôme (1465 m a.s.l.), France

    NASA Astrophysics Data System (ADS)

    Holmgren, H.; Sellegri, K.; Hervo, M.; Rose, C.; Freney, E.; Villani, P.; Laj, P.

    2014-03-01

    A Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) was used to evaluate the hygroscopic properties of aerosol particles measured at the Puy de Dôme research station in central France from September 2008 to December 2012. This high-altitude site is ideally situated to allow for both the upper part of the planetary boundary layer and the lower free troposphere to be sampled. The aim of the study is to investigate both the influence of year-to-year, seasonal, and diurnal cycles, as well as the influence of air mass type on particle hygroscopicity and mixing state. Results show that particle hygroscopicity increases with particle size and depends both on air mass type and on season. Average growth factor values are lowest in winter (1.21 ± 0.13, 1.23 ± 0.18 and 1.38 ± 0.25 for 25, 50 and 165 nm particles, respectively) and highest in autumn (1.27 ± 0.11, 1.32 ± 0.12 and 1.49 ± 0.15 for 25, 50 and 165 nm particles, respectively). Particles are generally more hygroscopic at night than during the day. The seasonal and diurnal variations are likely to be strongly influenced by boundary layer dynamics. Furthermore, particles originating from oceanic and continental regions tend to be more hygroscopic than those measured in African and local air masses. The high hygroscopicity of marine aerosol may be explained by large proportions of inorganic aerosol and sea salts, and it is speculated that continental particles are more hygroscopic than local and African ones due to ageing of fresh combustion aerosol. Aerosol measured at the Puy de Dôme display a high degree of external mixing, and hygroscopic growth spectra can be divided into three different hygroscopic modes: a less hygroscopic mode (GF < 1.3), a hygroscopic mode (GF 1.3-1.7) and a more hygroscopic mode (GF > 1.7). The majority of particles measured can be classified as being in either the less hygroscopic mode or the hygroscopic mode, and only few of them have more hygroscopic properties. The

  9. Hygroscopic properties and mixing state of aerosol measured at the high-altitude site Puy de Dôme (1465 m a.s.l.), France

    NASA Astrophysics Data System (ADS)

    Holmgren, H.; Sellegri, K.; Hervo, M.; Rose, C.; Freney, E.; Villani, P.; Laj, P.

    2014-09-01

    A Hygroscopicity Tandem Differential Mobility Analyser (HTDMA) was used to evaluate the hygroscopic properties of aerosol particles measured at the Puy de Dôme research station in central France, periodically from September 2008 to January 2010, and almost continuously from October 2010 to December 2012. This high-altitude site is ideally situated to allow for both the upper part of the planetary boundary layer and the lower free troposphere to be sampled. The aim of the study is to investigate both the influence of year-to-year, seasonal and diurnal cycles, as well as the influence of air mass type on particle hygroscopicity and mixing state. Results show that particle hygroscopicity increases with particle size and depends both on air mass type and on season. Average growth factor values, GFs, are lowest in winter (1.21 ± 0.13, 1.23 ± 0.18 and 1.38 ± 0.25 for 25, 50 and 165 nm particles, respectively) and highest in autumn (1.27 ± 0.11, 1.32 ± 0.12 and 1.49 ± 0.15 for 25, 50 and 165 nm particles, respectively). Particles are generally more hygroscopic at night than during the day. The seasonal and diurnal variations are likely to be strongly influenced by boundary layer dynamics. Furthermore, particles originating from oceanic and continental regions tend to be more hygroscopic than those measured in African and local air masses. The high hygroscopicity of oceanic aerosol can be explained by large proportions of inorganic aerosol and sea salts. Aerosols measured at the Puy de Dôme display a high degree of external mixing, and hygroscopic growth spectra can be divided into three different hygroscopic modes: a less-hygroscopic mode (GF < 1.3), a hygroscopic mode (GF 1.3-1.7) and a more-hygroscopic mode (GF > 1.7). The majority of particles measured can be classified as being in either the less-hygroscopic mode or the hygroscopic mode, and only few of them have more-hygroscopic properties. The degree of external mixing, evaluated as the fraction of time when

  10. The Pagami Creek smoke plume after long-range transport to the upper troposphere over Europe - aerosol properties and black carbon mixing state

    NASA Astrophysics Data System (ADS)

    Dahlkötter, F.; Gysel, M.; Sauer, D.; Minikin, A.; Baumann, R.; Seifert, P.; Ansmann, A.; Fromm, M.; Voigt, C.; Weinzierl, B.

    2014-06-01

    During the CONCERT 2011 field experiment with the DLR research aircraft Falcon, an enhanced aerosol layer with particle linear depolarization ratios of 6-8% at 532 nm was observed at altitudes above 10 km over northeast Germany on 16 September 2011. Dispersion simulations with HYSPILT suggest that the elevated aerosol layer originated from the Pagami Creek forest fire in Minnesota, USA, which caused pyro-convective uplift of particles and gases. The 3-4 day-old smoke plume had high total refractory black carbon (rBC) mass concentrations of 0.03-0.35 μg m-3 at standard temperature and pressure (STP) with rBC mass equivalent diameter predominantly smaller than 130 nm. Assuming a core-shell particle structure, the BC cores exhibit very thick (median: 105-136 nm) BC-free coatings. A large fraction of the BC-containing particles disintegrated into a BC-free fragment and a BC fragment while passing through the laser beam of the Single Particle Soot Photometer (SP2). In this study, the disintegration is a result of very thick coatings around the BC cores. This is in contrast to a previous study in a forest-fire plume, where it was hypothesized to be a result of BC cores being attached to a BC-free particle. For the high-altitude forest-fire aerosol layer observed in this study, increased mass specific light-absorption cross sections of BC can be expected due to the very thick coatings around the BC cores, while this would not be the case for the attached-type morphology. We estimate the BC mass import from the Pagami Creek forest fire into the upper troposphere/lower stratosphere (UTLS) region (best estimate: 25 Mg rBC). A comparison to black carbon emission rates from aviation underlines the importance of pyro-convection on the BC load in the UTLS region. Our study provides detailed information on the microphysics and the mixing state of BC in the forest-fire aerosol layer in the upper troposphere that can be used to better understand and investigate the radiative

  11. Mixing state, composition, and sources of fine aerosol particles in the Qinghai-Tibetan Plateau and the influence of agricultural biomass burning

    NASA Astrophysics Data System (ADS)

    Li, W. J.; Chen, S. R.; Xu, Y. S.; Guo, X. C.; Sun, Y. L.; Yang, X. Y.; Wang, Z. F.; Zhao, X. D.; Chen, J. M.; Wang, W. X.

    2015-09-01

    Transmission electron microscopy (TEM) was employed to obtain morphology, size, composition, and mixing state of background fine particles with diameter less than 1 μm in the Qinghai-Tibetan Plateau (QTP) during 15 September to 15 October 2013. Individual aerosol particles mainly contained secondary inorganic aerosols (SIA-sulfate and nitrate) and organics during clean periods (PM2.5: particles less than 2.5 μg m-3). The presence of KCl-NaCl associated with organics and an increase of soot particles suggest that an intense biomass burning event caused the highest PM2.5 concentrations (> 30 μg m-3) during the study. A large number fraction of the fly ash-containing particles (21.73 %) suggests that coal combustion emissions in the QTP significantly contributed to air pollutants at the median pollution level (PM2.5: 10-30 μg m-3). We concluded that emissions from biomass burning and from coal combustion both constantly contribute to anthropogenic particles in the QTP atmosphere. Based on size distributions of individual particles in different pollution levels, we found that gas condensation on existing particles is an important chemical process for the formation of SIA with organic coating. TEM observations show that refractory aerosols (e.g., soot, fly ash, and visible organic particles) likely adhere to the surface of SIA particles larger than 200 nm due to coagulation. Organic coating and soot on surface of the aged particles likely influence their hygroscopic and optical properties in the QTP, respectively. To our knowledge, this study reports the first microscopic analysis of fine particles in the background QTP air.

  12. [Aging and mixing state of particulate matter during aerosol pollution episode in autumn Shanghai using a single particle aerosol mass spectrometer (SPAMS)].

    PubMed

    Mu, Ying-Ying; Lou, Sheng-Rong; Chen, Chang-Hong; Zhou, Min; Wang, Hong-Li; Zhou, Zhen; Qiao, Li-Ping; Huang, Cheng; Li, Mei; Li, Li; Wang, Qian; Huang, Hai-Ying; Zou, Lan-Jun

    2013-06-01

    A single particle aerosol mass spectrometer (SPAMS) was applied to characterize the size distribution (200 nm-2.0 microm) and chemical compositions of ambient particles during a polluted event from 11th to 18th, November 2011. OCEC, METAL, EC, SECONDARY and K-Na types of particulates were the dominant groups observed in hazy day period, which were 27.4%, 3.4%, 7.3% , 45.6% and 5.4% of the overall measured particles, respectively. The observed five types of particles contained the secondary composition such as 18NH4(+), 80SO3(-), 96SO4(-), 97HSO4(-), 46NO2(-), 62NO3(-) and 125H (NO3) -, showing that they probably went through different aging processes, and the increasing of the SECONDARY particles during the event clearly indicated a secondary aerosol pollution. Heterogeneous reactions of SO2 and particles could be the reason of strong 97HSO4(-) signals in the mass spectrums of OCEC type particles while the existence of organic compounds might have an important influence on the aerosol formation with the gas-phase sulfuric acid. Fresh EC particles in the environment tended to be aging with above-mentioned secondary ions by the analysis of particle size distribution and eventually lead to a particle type conversion from EC to SECONDARY. Organic amine in marine environment was brought to the land by the warm, moist marine air mass that dramatically removed atmospheric SECONDARY and OCEC particles from the air with a heavy rain and leading to the observation of amine particles in the clean day period. PMID:23947016

  13. [Aging and mixing state of particulate matter during aerosol pollution episode in autumn Shanghai using a single particle aerosol mass spectrometer (SPAMS)].

    PubMed

    Mu, Ying-Ying; Lou, Sheng-Rong; Chen, Chang-Hong; Zhou, Min; Wang, Hong-Li; Zhou, Zhen; Qiao, Li-Ping; Huang, Cheng; Li, Mei; Li, Li; Wang, Qian; Huang, Hai-Ying; Zou, Lan-Jun

    2013-06-01

    A single particle aerosol mass spectrometer (SPAMS) was applied to characterize the size distribution (200 nm-2.0 microm) and chemical compositions of ambient particles during a polluted event from 11th to 18th, November 2011. OCEC, METAL, EC, SECONDARY and K-Na types of particulates were the dominant groups observed in hazy day period, which were 27.4%, 3.4%, 7.3% , 45.6% and 5.4% of the overall measured particles, respectively. The observed five types of particles contained the secondary composition such as 18NH4(+), 80SO3(-), 96SO4(-), 97HSO4(-), 46NO2(-), 62NO3(-) and 125H (NO3) -, showing that they probably went through different aging processes, and the increasing of the SECONDARY particles during the event clearly indicated a secondary aerosol pollution. Heterogeneous reactions of SO2 and particles could be the reason of strong 97HSO4(-) signals in the mass spectrums of OCEC type particles while the existence of organic compounds might have an important influence on the aerosol formation with the gas-phase sulfuric acid. Fresh EC particles in the environment tended to be aging with above-mentioned secondary ions by the analysis of particle size distribution and eventually lead to a particle type conversion from EC to SECONDARY. Organic amine in marine environment was brought to the land by the warm, moist marine air mass that dramatically removed atmospheric SECONDARY and OCEC particles from the air with a heavy rain and leading to the observation of amine particles in the clean day period.

  14. Glass formation processes in mixed inorganic/organic aerosol particles.

    PubMed

    Dette, Hans P; Koop, Thomas

    2015-05-14

    Recent experiments suggest that organic aerosol particles may transform into a glassy state at room temperature under dry conditions. Information on glass forming processes in mixed inorganic/organic aerosol particles is sparse, however, because inorganic crystal nucleation is usually very likely in such mixtures. Here we investigate the glass transition temperatures Tg of various organics (trehalose, sucrose, citric acid, sorbitol, and glycerol as well as 3-MBTCA) in binary mixtures with either NaNO3 or NH4HSO4 at different mass fractions. The glassy samples were prepared with the MARBLES technique by atomizing dilute aqueous solutions into aerosol particles and subsequent diffusion drying. The resulting aerosol particles were collected and their phase behavior was investigated using differential scanning calorimetry. At small and intermediate inorganic mass fractions salt crystallization did not occur. Instead, the single-phase mixtures remained in an amorphous state upon drying such that determination of their Tg was possible. From these measurements the Tg value of pure NaNO3 and pure NH4HSO4 could be inferred through extrapolation, resulting in values of Tg(NaNO3) ≈ 290 K and Tg(NH4HSO4) ≈ 220 K. Upon drying of NH4HSO4/3-MBTCA mixtures, phase-separated samples formed in which the inorganic-rich and organic-rich phases each show an independent glass transition. Our measurements provide a route toward establishing Tg values of inorganic salts that usually crystallize readily, and they may explain the reported contradicting observations of NaNO3 aerosol particles to either crystallize or remain amorphous upon drying at room temperature. PMID:25490407

  15. Organic aerosol mixing observed by single-particle mass spectrometry.

    PubMed

    Robinson, Ellis Shipley; Saleh, Rawad; Donahue, Neil M

    2013-12-27

    We present direct measurements of mixing between separately prepared organic aerosol populations in a smog chamber using single-particle mass spectra from the high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). Docosane and docosane-d46 (22 carbon linear solid alkane) did not show any signs of mixing, but squalane and squalane-d62 (30 carbon branched liquid alkane) mixed on the time scale expected from a condensational-mixing model. Docosane and docosane-d46 were driven to mix when the chamber temperature was elevated above the melting point for docosane. Docosane vapors were shown to mix into squalane-d62, but not the other way around. These results are consistent with low diffusivity in the solid phase of docosane particles. We performed mixing experiments on secondary organic aerosol (SOA) surrogate systems finding that SOA derived from toluene-d8 (a surrogate for anthropogenic SOA (aSOA)) does not mix into squalane (a surrogate for hydrophobic primary organic aerosol (POA)) but does mix into SOA derived from α-pinene (biogenic SOA (bSOA) surrogate). For the aSOA/POA, the volatility of either aerosol does not limit gas-phase diffusion, indicating that the two particle populations do not mix simply because they are immiscible. In the aSOA/bSOA system, the presence of toluene-d8-derived SOA molecules in the α-pinene-derived SOA provides evidence that the diffusion coefficient in α-pinene-derived SOA is high enough for mixing on the time scale of 1 min. The observations from all of these mixing experiments are generally invisible to bulk aerosol composition measurements but are made possible with single-particle composition data.

  16. Implementation of warm-cloud processes in a source-oriented WRF/Chem model to study the effect of aerosol mixing state on fog formation in the Central Valley of California

    NASA Astrophysics Data System (ADS)

    Lee, Hsiang-He; Chen, Shu-Hua; Kleeman, Michael J.; Zhang, Hongliang; DeNero, Steven P.; Joe, David K.

    2016-07-01

    The source-oriented Weather Research and Forecasting chemistry model (SOWC) was modified to include warm cloud processes and was applied to investigate how aerosol mixing states influence fog formation and optical properties in the atmosphere. SOWC tracks a 6-D chemical variable (X, Z, Y, size bins, source types, species) through an explicit simulation of atmospheric chemistry and physics. A source-oriented cloud condensation nuclei module was implemented into the SOWC model to simulate warm clouds using the modified two-moment Purdue Lin microphysics scheme. The Goddard shortwave and long-wave radiation schemes were modified to interact with source-oriented aerosols and cloud droplets so that aerosol direct and indirect effects could be studied. The enhanced SOWC model was applied to study a fog event that occurred on 17 January 2011, in the Central Valley of California. Tule fog occurred because an atmospheric river effectively advected high moisture into the Central Valley and nighttime drainage flow brought cold air from mountains into the valley. The SOWC model produced reasonable liquid water path, spatial distribution and duration of fog events. The inclusion of aerosol-radiation interaction only slightly modified simulation results since cloud optical thickness dominated the radiation budget in fog events. The source-oriented mixture representation of particles reduced cloud droplet number relative to the internal mixture approach that artificially coats hydrophobic particles with hygroscopic components. The fraction of aerosols activating into cloud condensation nuclei (CCN) at a supersaturation of 0.5 % in the Central Valley decreased from 94 % in the internal mixture model to 80 % in the source-oriented model. This increased surface energy flux by 3-5 W m-2 and surface temperature by as much as 0.25 K in the daytime.

  17. Glass transition measurements in mixed organic and organic/inorganic aerosol particles

    NASA Astrophysics Data System (ADS)

    Dette, Hans Peter; Qi, Mian; Schröder, David; Godt, Adelheid; Koop, Thomas

    2014-05-01

    The recent proposal of a semi-solid or glassy state of secondary organic aerosol (SOA) particles has sparked intense research in that area. In particular, potential effects of a glassy aerosol state such as incomplete gas-to-particle partitioning of semi-volatile organics, inhibited chemical reactions and water uptake, and the potential to act as heterogeneous ice nuclei have been identified so far. Many of these studies use well-studied proxies for oxidized organics such as sugars or other polyols. There are, however, few measurements on compounds that do exist in atmospheric aerosol particles. Here, we have performed studies on the phase state of organics that actually occur in natural SOA particles arising from the oxidation of alpha-pinene emitted in boreal forests. We have investigated the two marker compounds pinonic acid and 3-methylbutane-1,2,3-tricarboxylic acid (3-MBTCA) and their mixtures. 3-MBCTA was synthesized from methyl isobutyrate and dimethyl maleate in two steps. In order to transfer these substances into a glassy state we have developed a novel aerosol spray drying technique. Dilute solutions of the relevant organics are atomized into aerosol particles which are dried subsequently by diffusion drying. The dried aerosol particles are then recollected in an impactor and studied by means of differential scanning calorimetry (DSC), which provides unambiguous information on the aerosols' phase state, i.e. whether the particles are crystalline or glassy. In the latter case DSC is used to determine the glass transition temperature Tg of the investigated samples. Using the above setup we were able to determine Tg of various mixtures of organic aerosol compounds as a function of their dry mass fraction, thus allowing to infer a relation between Tg and the O:C ratio of the aerosols. Moreover, we also studied the glass transition behavior of mixed organic/inorganic aerosol particles, including the effects of liquid-liquid phase separation upon drying.

  18. Optimal broadcasting of mixed states

    SciTech Connect

    Dang Guifang; Fan Heng

    2007-08-15

    The N to M (M{>=}N) universal quantum broadcasting of mixed states {rho}{sup xN} is proposed for a qubit system. The broadcasting of mixed states is universal and optimal in the sense that the shrinking factor is independent of the input state and achieves the upper bound. The quantum broadcasting of mixed qubits is a generalization of the universal quantum cloning machine for identical pure input states. A pure state decomposition of the identical mixed qubits {rho}{sup xN} is obtained.

  19. Aerosol from Organic Nitrogen in the Southeast United States

    EPA Science Inventory

    Biogenic volatile organic compounds (BVOCs) contribute significantly to organic aerosol in the southeastern United States. During the Southern Oxidant and Aerosol Study (SOAS), a portion of ambient organic aerosol was attributed to isoprene oxidation and organic nitrogen from BVO...

  20. Fine Iron Aerosols Are Internally Mixed with Nitrate in the Urban European Atmosphere.

    PubMed

    Dall'Osto, Manuel; Beddows, D C S; Harrison, Roy M; Onat, Burcu

    2016-04-19

    Atmospheric iron aerosol is a bioavailable essential nutrient playing a role in oceanic productivity. Using aerosol time-of-flight mass spectrometry (ATOFMS), the particle size (0.3-1.5 μm), chemical composition and mixing state of Fe-containing particles collected at two European urban sites (London and Barcelona) were characterized. Out of the six particle types accounting for the entire Fe-aerosol population, that arising from long-range transport (LRT) of fine Fe-containing particles (Fe-LRT, 54-82% across the two sites) was predominant. This particle type was found to be internally mixed with nitrate and not with sulfate, and likely mostly associated with urban traffic activities. This is in profound contrast with previous studies carried out in Asia, where the majority of iron-containing particles are mixed with sulfate and are of coal combustion origin. Other minor fine iron aerosol sources included mineral dust (8-11%), traffic brake wear material (1-17%), shipping/oil (1-6%), biomass combustion (4-13%) and vegetative debris (1-3%). Overall, relative to anthropogenic Asian Fe-sulfate dust, anthropogenic European dust internally mixed with additional key nutrients such as nitrate is likely to play a different role in ocean global biogeochemical cycles. PMID:27002272

  1. Mixing properties of individual submicrometer aerosol particles in Vienna

    NASA Astrophysics Data System (ADS)

    Okada, Kikuo; Hitzenberger, Regina M.

    Individual aerosol particles were collected on 5 days with different meteorological conditions in March, April and June 1991 in the urban atmosphere of Vienna in Austria. The samples collected with an impactor were examined by electron microscopy. The mixing properties of submicrometer aerosol particles with radii between 0.1 and 1 μm were studied by using the dialysis (extraction) of water-soluble material. The averaged results showed that more than 85% of particles with radii between 0.1 and 0.7 μm were hygroscopic. However, more than 50% of particles with radii larger than 0.2 μm were mixed particles (hygroscopic particles with water-insoluble inclusions), and they were dominant (80%) in the size range 0.5-0.7 μm radius. The results also showed that the number proportion of mixed particles increased with increasing radius and the abundance increased with increasing particle loading in the atmosphere. The volume fraction of water-soluble material ( ɛ) in mixed particles tended to decrease with increasing radius, implying the formation of mixed particles by heterogeneous processes such as condensation and/or surface reaction. Some results of elemental composition in individual particles analyzed with an energy-dispersive X-ray (EDX) analyzer equipped with an electron microscope are also presented in this paper.

  2. X-Ray Microspectroscopic Investigations of Remote Aerosol Composition and Changes in Aerosol Microstructure and Phase State upon Hydration

    NASA Astrophysics Data System (ADS)

    Andreae, M. O.; Artaxo, P.; Bechtel, M.; Förster, J. D.; Kilcoyne, A. L. D.; Krüger, M. L.; Pöhlker, C.; Saturno, J.; Weigand, M.; Wiedemann, K. T.

    2014-12-01

    Atmospheric aerosols play a crucial role in the Earth's climate system and hydrological cycle by scattering and absorbing sunlight and affecting the formation and development of clouds and precipitation. Our research focuses on aerosols in remote regions, in order to characterize the properties and sources of natural aerosol particles and the extent of human perturbations of the aerosol burden. The phase and mixing state of atmospheric aerosols, and particularly their hygroscopic response to relative humidity (RH) variations, is a central determinant of their atmospheric life cycle and impacts. We present an investigation using X-ray microspectroscopy on submicrometer aerosols under variable RH conditions, showing in situ changes in morphology, microstructure, and phase state upon humidity cycling. We applied Scanning Transmission X-ray Microscopy with Near-Edge X-ray Absorption Fine Structure spectroscopy (STXM-NEXAFS) under variable RH conditions to standard aerosols for a validation of the experimental approach and to internally mixed aerosol particles from the Amazonian rain forest collected during periods with anthropogenic pollution. The measurements were conducted at X-ray microscopes at the synchrotron facilities Advanced Light Source (ALS) in Berkeley, USA, and BESSY II in Berlin, Germany. Upon hydration, we observed substantial and reproducible changes in microstructure of the Amazonian particles (internal mixture of secondary organic material, ammoniated sulfate, and soot), which appear as mainly driven by efflorescence and recrystallization of sulfate salts. Multiple solid and liquid phases were found to coexist, especially in intermediate humidity regimes (60-80% RH). This shows that X-ray microspectroscopy under variable RH is a valuable technique to analyze the hygroscopic response of individual ambient aerosol particles. Our initial results underline that RH changes can trigger strong particle restructuring, in agreement with previous studies on

  3. Study of the carbonaceous aerosol and morphological analysis of fine particles along with their mixing state in Delhi, India: a case study.

    PubMed

    Tiwari, S; Pipal, A S; Hopke, Philip K; Bisht, D S; Srivastava, A K; Tiwari, Shani; Saxena, P N; Khan, A H; Pervez, S

    2015-07-01

    Because of high emissions of anthropogenic as well as natural particles over the Indo-Gangetic Plains (IGP), it is important to study the characteristics of fine (PM2.5) and inhalable particles (PM10), including their morphology, physical and chemical characteristics, etc., in Delhi during winter 2013. The mean mass concentrations of fine (PM2.5) and inhalable (PM10) (continuous) was 117.6 ± 79.1 and 191.0 ± 127.6 μg m(-3), respectively, whereas the coarse mode (PM10-2.5) particle PM mass was 73.38 ± 28.5 μg m(-3). During the same period, offline gravimetric monitoring of PM2.5 was conducted for morphological analysis, and its concentration was ~37 % higher compared to the continuous measurement. Carbonaceous PM such as organic carbon (OC) and elemental carbon (EC) were analyzed on the collected filters, and their mean concentration was respectively 33.8 and 4.0 μg m(-3) during the daytime, while at night it was 41.2 and 10.1 μg m(-3), respectively. The average OC/EC ratio was 8.97 and 3.96 during the day and night, respectively, indicating the formation of secondary organic aerosols during daytime. Effective carbon ratio was studied to see the effect of aerosols on climate, and its mean value was 0.52 and 1.79 during night and day, indicating the dominance of absorbing and scattering types of aerosols respectively into the atmosphere over the study region. Elemental analysis of individual particles indicates that Si is the most abundant element (~37-90 %), followed by O (oxide) and Al. Circularity and aspect ratio was studied, which indicates that particles are not perfectly spherical and not elongated in any direction. Trajectory analysis indicated that in the months of February and March, air masses appear to be transported from the Middle Eastern part along with neighboring countries and over Thar Desert region, while in January it was from the northeast direction which resulted in high concentrations of fine particles.

  4. [Analysis of Single Particle Aging and Mixing State at an Agriculture Site (Quzhou) in the North China Plain in Summer Using a Single Particle Aerosol Mass Spectrometer].

    PubMed

    Huang, Zi-long; Zeng, Li-mm; Dong, I-Iua-Bin; Li, Mei; Zhu, Tong

    2016-04-15

    To characterize the size distribution and chemical ompsitins f abiet prtices t a agicuturesit intheNorh o Chinese Plain, a single particle aerosol mass spectrometer (SPAMS) was deployed from June 30 to July 8, 2013. A total of 230,152 particles in the size range of 0.2-2.0 pm were chemically analyzed with both positive and negative ion spectra. The results revealed that aerosol could he classified into eight dominant groups, including elemental carbon (EC, 55.5%), organic carbon (OC, 10.7%), alkalis (Na-K, 17.4%), other metals (1.7%), Fe-rich (6.3%), Pb-rich (3.1%), dust (4.8%), and other (0.8%). The observed eight types of particles contained secondary components such as 46NO2-, 62NO3-, 96SO3-, 96SO4-, 97HSO4-, showing that they probably went through different aging processes. The analysis of particle size distribution showed that 700-800 nm was the peak value of all particles, and that dust and Fe particles were mainly in the coarse size range. EC particles subtype group research revealed EC particles tended to be aging with the above mentioned secondary ions and eventually led to a particle type conversion from EC to the less aging ECN and the more serious aging ECS, the diurnal variation of which was obviously negatively correlated, and there was a possibility of forming OC/EC mixture with the adsorption of secondary organic matter on EC surface.

  5. [Analysis of Single Particle Aging and Mixing State at an Agriculture Site (Quzhou) in the North China Plain in Summer Using a Single Particle Aerosol Mass Spectrometer].

    PubMed

    Huang, Zi-long; Zeng, Li-mm; Dong, I-Iua-Bin; Li, Mei; Zhu, Tong

    2016-04-15

    To characterize the size distribution and chemical ompsitins f abiet prtices t a agicuturesit intheNorh o Chinese Plain, a single particle aerosol mass spectrometer (SPAMS) was deployed from June 30 to July 8, 2013. A total of 230,152 particles in the size range of 0.2-2.0 pm were chemically analyzed with both positive and negative ion spectra. The results revealed that aerosol could he classified into eight dominant groups, including elemental carbon (EC, 55.5%), organic carbon (OC, 10.7%), alkalis (Na-K, 17.4%), other metals (1.7%), Fe-rich (6.3%), Pb-rich (3.1%), dust (4.8%), and other (0.8%). The observed eight types of particles contained secondary components such as 46NO2-, 62NO3-, 96SO3-, 96SO4-, 97HSO4-, showing that they probably went through different aging processes. The analysis of particle size distribution showed that 700-800 nm was the peak value of all particles, and that dust and Fe particles were mainly in the coarse size range. EC particles subtype group research revealed EC particles tended to be aging with the above mentioned secondary ions and eventually led to a particle type conversion from EC to the less aging ECN and the more serious aging ECS, the diurnal variation of which was obviously negatively correlated, and there was a possibility of forming OC/EC mixture with the adsorption of secondary organic matter on EC surface. PMID:27548937

  6. Collectibility for mixed quantum states

    NASA Astrophysics Data System (ADS)

    Rudnicki, Łukasz; Puchała, Zbigniew; Horodecki, Paweł; Życzkowski, Karol

    2012-12-01

    Bounds analogous to entropic uncertainty relations allow one to design practical tests to detect quantum entanglement by a collective measurement performed on several copies of the state analyzed. This approach, initially worked out for pure states only [Phys. Rev. Lett.PRLTAO0031-900710.1103/PhysRevLett.107.150502 107, 150502 (2011)], is extended here for mixed quantum states. We define collectibility for any mixed states of a multipartite system. Deriving bounds for collectibility for positive partially transposed states of given purity provides insight into the structure of entangled quantum states. In the case of two qubits the application of complementary measurements and coincidence based detections leads to a test of entanglement of pseudopure states.

  7. Aerosol charge state characterisation using an ELPI

    NASA Astrophysics Data System (ADS)

    Matthews, J. C.; Wright, M. D.; Biddiscombe, M. F.; Usmani, O. S.; Henshaw, D. L.

    2011-06-01

    A new technique has been developed to measure the size distribution and charge state of highly charged aerosols using an Electrical Low Pressure Impactor (ELPI). The internal charger was switched alternately on and off and the time between stable charge states found to be ~ 10 s. The size distribution of aerosols was found when the charger was on, from which the charge distribution can be estimated when the charger is off using the current at each impactor stage. This method was tested in background conditions, when a candle was burning and when a negative air ioniser was used. The ELPI electrometers were not sensitive enough to accurately measure the charge state on background and candle air, but gave a value for air charged by an ioniser. Comparing results from the ELPI with other techniques showed inaccuracies in this method that need to be addressed before further use of this technique.

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

    PubMed

    Ramachandran, S; Srivastava, Rohit

    2013-05-01

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

  9. 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

  10. Understanding the Role of Water in Modifying Particle Mixing States for CCN Activity

    NASA Astrophysics Data System (ADS)

    Vu, D. N.; Gao, S.; Pierce, J. R.; Asa-Awuku, A. A.

    2014-12-01

    CCN data sets from ambient and chamber studies, which consist of complex heterogeneous mixtures of organic and inorganic aerosol mixtures, may not show a single activation curve but instead can exhibit multiple activations not associated with doubly charged particles. It has been suggested that these activation curves may be representative of multiple externally mixed compounds, whereas single activation curves are representative of single component or multicomponent internally mixed aerosols. To characterize and modify mixing states, a new laminar flow tube apparatus was developed to control the extent of mixing of organic and inorganic fractions under different environmental conditions such as relative humidity. Data sets yielding multiple activation curves have been recreated by mixing multiple inorganic and organic compounds. Preliminary results suggest that aerosol water is a significant factor; under dry conditions, the aerosols remained externally mixed while humid conditions facilitated internal mixing. For example, ammonium sulfate (inorganic) and succinic acid (organic) when dry, maintained an external mixture and multiple activation curves were observed to be constant. Under humid conditions, external mixing was initially observed; however, the aerosol water promoted internal mixing and the activation curves were observed to converge into a single curve. The data agrees well with Köhler Theory and single parameter (kappa) theory thermodynamic predictions of droplet activation. Data sets are also compared with a diffusion based coagulation particle model to predict mixing behavior. The method of analysis and the effect of mixing states of multiple components on the supersaturated hygroscopic properties of aerosols are presented.

  11. Aerosol optical properties in the southeastern United States in summer - Part 2: Sensitivity of aerosol optical depth to relative humidity and aerosol parameters

    NASA Astrophysics Data System (ADS)

    Brock, Charles A.; Wagner, Nicholas L.; Anderson, Bruce E.; Beyersdorf, Andreas; Campuzano-Jost, Pedro; Day, Douglas A.; Diskin, Glenn S.; Gordon, Timothy D.; Jimenez, Jose L.; Lack, Daniel A.; Liao, Jin; Markovic, Milos Z.; Middlebrook, Ann M.; Perring, Anne E.; Richardson, Matthews S.; Schwarz, Joshua P.; Welti, Andre; Ziemba, Luke D.; Murphy, Daniel M.

    2016-04-01

    Aircraft observations of meteorological, trace gas, and aerosol properties were made between May and September 2013 in the southeastern United States (US). Regionally representative aggregate vertical profiles of median and interdecile ranges of the measured parameters were constructed from 37 individual aircraft profiles made in the afternoon when a well-mixed boundary layer with typical fair-weather cumulus was present (Wagner et al., 2015). We use these 0-4 km aggregate profiles and a simple model to calculate the sensitivity of aerosol optical depth (AOD) to changes in dry aerosol mass, relative humidity, mixed-layer height, the central diameter and width of the particle size distribution, hygroscopicity, and dry and wet refractive index, while holding the other parameters constant. The calculated sensitivity is a result of both the intrinsic sensitivity and the observed range of variation in these parameters. These observationally based sensitivity studies indicate that the relationship between AOD and dry aerosol mass in these conditions in the southeastern US can be highly variable and is especially sensitive to relative humidity (RH). For example, calculated AOD ranged from 0.137 to 0.305 as the RH was varied between the 10th and 90th percentile profiles with dry aerosol mass held constant. Calculated AOD was somewhat less sensitive to aerosol hygroscopicity, mean size, and geometric standard deviation, σg. However, some chemistry-climate models prescribe values of σg substantially larger than we or others observe, leading to potential high biases in model-calculated AOD of ˜ 25 %. Finally, AOD was least sensitive to observed variations in dry and wet aerosol refractive index and to changes in the height of the well-mixed surface layer. We expect these findings to be applicable to other moderately polluted and background continental air masses in which an accumulation mode between 0.1-0.5 µm diameter dominates aerosol extinction.

  12. Three-dimensional modeling of the mixing state of particles over Greater Paris

    NASA Astrophysics Data System (ADS)

    Zhu, Shupeng; Sartelet, Karine; Zhang, Yang; Nenes, Athanasios

    2016-05-01

    A size-composition resolved aerosol model (SCRAM) is coupled to the Polyphemus air quality platform and evaluated over Greater Paris. SCRAM simulates the particle mixing state and solves the aerosol dynamic evolution taking into account the processes of coagulation, condensation/evaporation, and nucleation. Both the size and mass fractions of chemical components of particles are discretized. The performance of SCRAM to model air quality over Greater Paris is evaluated by comparison to PM2.5, PM10, and Aerosol Optical Depth (AOD) measurements. Because air quality models usually assume that particles are internally mixed, the impact of the mixing state on aerosols formation, composition, optical properties, and their ability to be activated as cloud condensation nuclei (CCN) is investigated. The simulation results show that more than half (up to 80% during rush hours) of black carbon particles are barely mixed at the urban site of Paris, while they are more mixed with organic species at a rural site. The comparisons between the internal-mixing simulation and the mixing state-resolved simulation show that the internal-mixing assumption leads to lower nitrate and higher ammonium concentrations in the particulate phase. Moreover, the internal-mixing assumption leads to lower single scattering albedo, and the difference of aerosol optical depth caused by the mixing state assumption can be as high as 72.5%. Furthermore, the internal-mixing assumption leads to lower CCN activation percentage at low supersaturation, but higher CCN activation percentage at high supersaturation.

  13. Aerosol flux measurements above a mixed forest at Borden, Ontario

    NASA Astrophysics Data System (ADS)

    Gordon, M.; Staebler, R. M.; Liggio, J.; Vlasenko, A.; Li, S.-M.; Hayden, K.

    2010-10-01

    Aerosol fluxes were measured above a mixed forest by Eddy Covariance (EC) with a Fast Mobility Particle Sizer (FMPS) at the Borden Forest Research Station in Ontario, Canada between 13 July and 12 August 2009. The FMPS, mounted at a height of 33 m (approximately 10 m above the canopy top) and housed in a temperature controlled enclosure, measured size-resolved particle concentrations for 3 to 410 nm at a rate of 1 Hz. For the size range 20Aerosol Mass Spectrometer (Q-AMS) demonstrate a tendency towards downward fluxes, which may be due to an organic particle component which can not be resolved by the flux mode of the Q-AMS.

  14. Aerosol flux measurements above a mixed forest at Borden, Ontario

    NASA Astrophysics Data System (ADS)

    Gordon, M.; Staebler, R. M.; Liggio, J.; Vlasenko, A.; Li, S.-M.; Hayden, K.

    2011-07-01

    Aerosol fluxes were measured above a mixed forest by Eddy Covariance (EC) with a Fast Mobility Particle Sizer (FMPS) at the Borden Forest Research Station in Ontario, Canada between 13 July and 12 August 2009. Chemically speciated flux measurements were made at a height of 29 m at the same location between 19 July and 2 August, 2006 using a Quadrupole Aerosol Mass Spectrometer (Q-AMS). The Q-AMS measured an average sulphate deposition velocity of 0.3 mm s-1 and an average nitrate deposition velocity of 4.8 mm s-1. The FMPS, mounted at a height of 33 m (approximately 10 m above the canopy top) and housed in a temperature controlled enclosure, measured size-resolved particle concentrations from 3 to 410 nm diameter at a rate of 1 Hz. For the size range 18 < D < 452 nm, 60 % of fluxes were upward. The exchange velocity was between -0.5 and 2.0 mm s-1, with median values near 0.5 mm s-1 for all sizes between 22 and 310 nm. The size distribution of the apparent production rate of particles at 33 m peaked at a diameter of 75 nm. Results indicate a decoupling of the above and below canopy spaces, whereby particles are stored in the canopy space at night, and are then diluted with cleaner air above during the day.

  15. Aerosols in the study of convective acinar mixing

    NASA Technical Reports Server (NTRS)

    Darquenne, Chantal; Prisk, G. Kim

    2005-01-01

    Convective mixing (CM) refers to the different transport mechanisms except Brownian diffusion that irreversibly transfer inspired air into resident air and can be studied using aerosol bolus inhalations. This paper provides a review of the present understanding of how each of these mechanisms contributes to CM. Original data of the combined effect of stretch and fold and gravitational sedimentation on CM are also presented. Boli of 0.5 microm-diameter particles were inhaled at penetration volumes (V(p)) of 300 and 1200 ml in eight subjects. Inspiration was followed by a 10-s breath hold, during which small flow reversals (FR) were imposed, and expiration. There was no physiologically significant dependence in dispersion and deposition with increasing FR. The results were qualitatively similar to those obtained in a previous study in microgravity in which it was speculated that the phenomenon of stretch and fold occurred during the first breathing cycle without the need of any subsequent FR.

  16. Surface tensions, viscosities, and diffusion constants in mixed component single aerosol particles

    NASA Astrophysics Data System (ADS)

    Bzdek, Bryan; Marshall, Frances; Song, Young-Chul; Haddrell, Allen; Reid, Jonathan

    2016-04-01

    Surface tension and viscosity are important aerosol properties but are challenging to measure on individual particles owing to their small size and mass. Aerosol viscosity impacts semivolatile partitioning from the aerosol phase, molecular diffusion in the bulk of the particle, and reaction kinetics. Aerosol surface tension impacts how particles activate to serve as cloud condensation nuclei. Knowledge of these properties and how they change under different conditions hinders accurate modelling of aerosol physical state and atmospheric impacts. We present measurements made using holographic optical tweezers to directly determine the viscosity and surface tension of optically trapped droplets containing ~1-4 picolitres of material (corresponding to radii of ~5-10 micrometres). Two droplets are captured in the experimental setup, equilibrated to a relative humidity, and coalesced through manipulation of the relative trap positions. The moment of coalescence is captured using camera imaging as well as from elastically backscattered light connected to an oscilloscope. For lower viscosity droplets, the relaxation in droplet shape to a sphere follows the form of a damped oscillator and gives the surface tension and viscosity. For high viscosity droplets, the relaxation results in a slow merging of the two droplets to form a sphere and the timescale of that process permits determination of viscosity. We show that droplet viscosity and surface tension can be quantitatively determined to within <10% of the expected value for low viscosity droplets and to better than 1 order of magnitude for high viscosity droplets. Examples illustrating how properties such as surface tension can change in response to environmental conditions will be discussed. Finally, a study of the relationship between viscosity, diffusion constants, vapour pressures, and reactive uptake coefficients for a mixed component aerosol undergoing oxidation and volatilisation will be discussed.

  17. 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

  18. Phases and Phase Changes of Mixed Organic/Inorganic Model Systems of Tropospheric Aerosols

    NASA Astrophysics Data System (ADS)

    Marcolli, C.; Krieger, U. K.; Zardini, A. A.; Zobrist, B.; Zuend, A.; Luo, B. P.; Peter, T.

    2006-12-01

    Knowledge of the physical state of tropospheric aerosols is important for an adequate description of cloud formation, heterogeneous and multiphase chemistry, and the aerosol's radiative properties. We will present and discuss laboratory experiments on bulk aerosol model mixtures and micron-sized particles consisting of polyols, polyethylene glycol or dicarboxylic acids mixed with ammonium sulfate. Depending on the exact composition and relative humidity, these mixtures form liquid-one-phase or two-phase systems plus additional solid phases. Whilst the organic matter in ambient aerosols is expected to be predominantly present in the form of liquid or amorphous phases, the inorganic salts may still undergo deliquescence and efflorescence as a function of relative humidity. Moreover, they may induce phase separations into a predominantly organic and an inorganic aqueous phase. In the absence of solid phases, the water uptake and release of the investigated micron-sized particles was usually well described by the Zdanovskii-Stokes-Robinson (ZSR) approach. However, this model became inaccurate when solid phases were present. Moreover, it is not able to account for liquid-liquid phase separations due to the salting-out effects of the investigated inorganic salts. While most organics participate in liquid phases some organic substances are abundant enough in the particles to form crystalline solids that might act as ice nuclei. We show that this is the case for oxalic acid.

  19. A combined particle trap/HTDMA hygroscopicity study of mixed inorganic/organic aerosol particles

    NASA Astrophysics Data System (ADS)

    Zardini, A. A.; Sjogren, S.; Marcolli, C.; Krieger, U. K.; Gysel, M.; Weingartner, E.; Baltensperger, U.; Peter, T.

    2008-03-01

    Atmospheric aerosols are often mixtures of inorganic and organic material. Organics can represent a large fraction of the total aerosol mass and are comprised of water-soluble and insoluble compounds. Increasing attention was paid in the last decade to the capability of mixed inorganic/organic aerosol particles to take up water (hygroscopicity). We performed hygroscopicity measurements of internally mixed particles containing ammonium sulfate and carboxylic acids (citric, glutaric, adipic acid) in parallel with an electrodynamic balance (EDB) and a hygroscopicity tandem differential mobility analyzer (HTDMA). The organic compounds were chosen to represent three distinct physical states. During hygroscopicity cycles covering hydration and dehydration measured by the EDB and the HTDMA, pure citric acid remained always liquid, adipic acid remained always solid, while glutaric acid could be either. We show that the hygroscopicity of mixtures of the above compounds is well described by the Zdanovskii-Stokes-Robinson (ZSR) relationship as long as the two-component particle is completely liquid in the ammonium sulfate/citric acid and in the ammonium sulfate/glutaric acid cases. However, we observe significant discrepancies compared to what is expected from bulk thermodynamics when a solid component is present. We explain this in terms of a complex morphology resulting from the crystallization process leading to veins, pores, and grain boundaries which allow for water sorption in excess of bulk thermodynamic predictions caused by the inverse Kelvin effect on concave surfaces.

  20. The Mixing State of Black Carbon in Asian Outflow (Invited)

    NASA Astrophysics Data System (ADS)

    Kondo, Y.; Moteki, N.; Takegawa, N.; Oshima, N.; Sahu, L. K.

    2009-12-01

    Black carbon (BC) aerosol efficiently absorbs visible sunlight and heats the atmosphere. The magnitude of the photo-absorption of BC depends on its particle size distribution and mixing state (coating thickness or shell/core diameter ratio). In addition, the efficiency of wet removal of BC is sensitive to mixing state. Therefore, it is critically important to understand the evolution of the mixing state of BC, especially in Asia, where BC emissions are largest. The size distribution and mixing state of BC were measured by an SP2 instrument over the East China Sea and Yellow Sea in March-April 2009 during the A-FORCE (Aerosol-Radiative Forcing in East Asia) aircraft campaign. Aircraft sampling was made in air masses strongly influenced by emissions from China, Korea, and Japan in the latitude region between 27 and 37N. In the boundary layer, the mass median diameter of BC was stable at about 200 nm in air masses with ages exceeding 1 day. BC in these air masses was thickly coated even over the Yellow Sea at distances of only a few hundred km from the coastlines of China and Korea. Thinly coated (shell/core diameter ratio < 1.2) BC was observed only in the vicinity of urban areas of Korea and Japan. The dominance of thickly coated BC in the moderately aged outflow is consistent with our previous ground-based and aircraft measurements showing that BC coating proceeds within 24 hours in the outflow of urban air. The variability of the observed BC mixing state is interpreted in terms of available volatile aerosol compounds.

  1. [Mixed states: evolution of classifications].

    PubMed

    Pringuey, D; Cherikh, F; Giordana, B; Fakra, E; Dassa, D; Cermolacce, M; Belzeaux, R; Maurel, M; Azorin, J-M

    2013-12-01

    The nosological position of mixed states has followed the course of classifying methods in psychiatry, the steps of the invention of the clinic, progress in the organization of care, including the discoveries of psychopharmacology. The clinical observation of a mixture of symptoms emerging from usually opposite clinical conditions is classical. In the 70s, a syndromic specification fixed the main symptom combinations but that incongruous assortment failed to stabilize the nosological concept. Then stricter criteriology was proposed. To be too restrictive, a consensus operates a dimensional opening that attempts to meet the pragmatic requirements of nosology validating the usefulness of the class system. This alternation between rigor of categorization and return to a more flexible criteriological option reflects the search for the right balance between nosology and diagnosis. The definition of mixed states is best determined by their clinical and prognostic severity, related to the risk of suicide, their lower therapeutic response, the importance of their psychiatric comorbidities, anxiety, emotional lability, alcohol abuse. Trying to compensate for the lack of categorical definitions and better reflecting the clinical field problems, new definitions complement criteriology with dimensional aspects, particularly taking into account temperaments. PMID:24359850

  2. A simple method for estimation of coagulation efficiency in mixed aerosols. [environmental pollution control

    NASA Technical Reports Server (NTRS)

    Dimmick, R. L.; Boyd, A.; Wolochow, H.

    1975-01-01

    Aerosols of KBr and AgNO3 were mixed, exposed to light in a glass tube and collected in the dark. About 15% of the collected material was reduced to silver upon development. Thus, two aerosols of particles that react to form a photo-reducible compound can be used to measure coagulation efficiency.

  3. Volatility and mixing states of ultrafine particles from biomass burning.

    PubMed

    Maruf Hossain, A M M; Park, Seungho; Kim, Jae-Seok; Park, Kihong

    2012-02-29

    Fine and ultrafine carbonaceous aerosols produced from burning biomasses hold enormous importance in terms of assessing radiation balance and public health hazards. As such, volatility and mixing states of size-selected ultrafine particles (UFP) emitted from rice straw, oak, and pine burning were investigated by using volatility tandem differential mobility analyzer (VTDMA) technique in this study. Rice straw combustion produced unimodal size distributions of emitted aerosols, while bimodal size distributions from combustions of oak (hardwood) and pine (softwood) were obtained. A nearness of flue gas temperatures and a lower CO ratio of flaming combustion (FC) to smoldering combustion (SC) were characteristic differences found between softwood and hardwood. SC emitted larger mode particles in higher numbers than smaller mode particles, while the converse was true for FC. Rice straw open burning UFPs exhibited a volatilization behavior similar to that between FC and SC. In addition, internal mixing states were observed for size-selected UFPs in all biomasses for all combustion conditions, while external mixing states were only observed for rice straw combustion. Results for FC and open burning suggested there was an internal mixing of volatile organic carbon (OC) and non-volatile core (e.g., black carbon (BC)), while the SC in rice straw produced UFPs devoid of non-volatile core. Also, it was found that volatility of constituting OC in FC and SC particles was different.

  4. Effect of relative humidity on soot - secondary organic aerosol mixing: A case study from the Soot Aerosol Aging Study (PNNL-SAAS)

    NASA Astrophysics Data System (ADS)

    Sharma, N.; China, S.; Zaveri, R. A.; Shilling, J. E.; Pekour, M. S.; Liu, S.; Aiken, A. C.; Dubey, M. K.; Wilson, J. M.; Zelenyuk, A.; OBrien, R. E.; Moffet, R.; Gilles, M. K.; Gourihar, K.; Chand, D.; Sedlacek, A. J., III; Subramanian, R.; Onasch, T. B.; Laskin, A.; Mazzoleni, C.

    2014-12-01

    Atmospheric processing of fresh soot particles emitted by anthropogenic as well as natural sources alters their physical and chemical properties. For example, fresh and aged soot particles interact differently with incident solar radiation, resulting in different overall radiation budgets. Varying atmospheric chemical and meteorological conditions can result in complex soot mixing states. The Soot Aerosol Aging Study (SAAS) was conducted at the Pacific Northwest National Laboratory in November 2013 and January 2014 as a step towards understanding the evolution of mixing state of soot and its impact on climate-relevant properties. Aging experiments on diesel soot were carried out in a controlled laboratory chamber, and the effects of condensation and coagulation processes were systematically explored in separate sets of experiments. In addition to online measurement of aerosol properties, aerosol samples were collected for offline single particle analysis to investigate the evolution of the morphology, elemental composition and fine structure of sample particles from different experiments. Condensation experiments focused on the formation of α-pinene secondary organic aerosol on diesel soot aerosol seeds. Experiments were conducted to study the aging of soot under dry (RH < 2%) and humid conditions (RH ~ 80%). We present an analysis of the morphology of soot, its evolution, and its correlation with optical properties, as the condensation of α-pinene SOA is carried out for the two different RH conditions. The analysis was performed by using scanning electron microscopy, transmission electron microscopy, scanning transmission x-ray microscopy and atomic force microscopy for single particle characterization. In addition, particle size, mass, composition, shape, and density were characterized in-situ, as a function of organics condensed on soot seeds, using single particle mass spectrometer.

  5. A combined particle trap/HTDMA hygroscopicity study of mixed inorganic/organic aerosol particles

    NASA Astrophysics Data System (ADS)

    Zardini, A. A.; Sjogren, S.; Marcolli, C.; Krieger, U. K.; Gysel, M.; Weingartner, E.; Baltensperger, U.; Peter, T.

    2008-09-01

    Atmospheric aerosols are often mixtures of inorganic and organic material. Organics can represent a large fraction of the total aerosol mass and are comprised of water-soluble and insoluble compounds. Increasing attention was paid in the last decade to the capability of mixed inorganic/organic aerosol particles to take up water (hygroscopicity). We performed hygroscopicity measurements of internally mixed particles containing ammonium sulfate and carboxylic acids (citric, glutaric, adipic acid) in parallel with an electrodynamic balance (EDB) and a hygroscopicity tandem differential mobility analyzer (HTDMA). The organic compounds were chosen to represent three distinct physical states. During hygroscopicity cycles covering hydration and dehydration measured by the EDB and the HTDMA, pure citric acid remained always liquid, adipic acid remained always solid, while glutaric acid could be either. We show that the hygroscopicity of mixtures of the above compounds is well described by the Zdanovskii-Stokes-Robinson (ZSR) relationship as long as the two-component particle is completely liquid in the ammonium sulfate/glutaric acid system; deviations up to 10% in mass growth factor (corresponding to deviations up to 3.5% in size growth factor) are observed for the ammonium sulfate/citric acid 1:1 mixture at 80% RH. We observe even more significant discrepancies compared to what is expected from bulk thermodynamics when a solid component is present. We explain this in terms of a complex morphology resulting from the crystallization process leading to veins, pores, and grain boundaries which allow for water sorption in excess of bulk thermodynamic predictions caused by the inverse Kelvin effect on concave surfaces.

  6. Numerical simulations of mixing conditions and aerosol dynamics in the CERN CLOUD chamber

    NASA Astrophysics Data System (ADS)

    Voigtländer, J.; Duplissy, J.; Rondo, L.; Kürten, A.; Stratmann, F.

    2012-02-01

    To study the effect of galactic cosmic rays on aerosols and clouds, the Cosmics Leaving OUtdoor Droplets (CLOUD) project was established. Experiments are carried out at a 26.1 m3 tank at CERN (Switzerland). In the experiments, the effect of ionizing radiation on H2SO4 particle formation and growth is investigated. To evaluate the experimental configuration, the experiment was simulated using a coupled multidimensional computational fluid dynamics (CFD) - particle model. In the model the coupled fields of gas/vapor species, temperature, flow velocity and particle properties were computed to investigate mixing state and mixing times of the CLOUD tank's contents. Simulation results show that a 1-fan configuration, as used in first experiments, may not be sufficient to ensure a homogeneously mixed chamber. To mix the tank properly, two fans and sufficiently high fan speeds are necessary. The 1/e response times for instantaneous changes of wall temperature and saturation ratio were found to be in the order of few minutes. Particle nucleation and growth was also simulated and particle number size distribution properties of the freshly nucleated particles (particle number, mean size, standard deviation of the assumed log-normal distribution) were found to be distributed over the tank's volume similar to the gas species.

  7. Aerosol optical properties over the midcontinental United States

    SciTech Connect

    Halthore, R.N. ); Markham, B.L.; Ferrare, R.A. ); Aro, T.O. )

    1992-11-30

    This work is part of the First International Satellite Land Surface Climatology Project (ISLSCP) Field Experiment (FIFE), an international land-surface-atmosphere experiment aimed at improving the way climate models represent energy, water, heat, and carbon exchanges, and improving the utilization of satellite based remote sensing to monitor such parameters. Here the authors report on measurements of aerosol optical depth over the FIFE site, making use of a calibrated Sun photometer. Aerosols are relevant for the impact they have on remotely sensed measurements of radiation effects on the earth. They also play a major role in cloud formation, and can impact the atmospheric concentration of minor species gases. Here the authors look at the meteorological effects on aerosols in the troposphere. Wavelength dependence gives information on the size distributions within the aerosols. During 1987 they observe mixing of gulf air with continental air over the site. They report on correlation with surface values of pressure, temperature, specific, and relative humidity.

  8. Modeling Gas-Particle Partitioning of SOA: Effects of Aerosol Physical State and RH

    NASA Astrophysics Data System (ADS)

    Zuend, A.; Seinfeld, J.

    2011-12-01

    Aged tropospheric aerosol particles contain mixtures of inorganic salts, acids, water, and a large variety of organic compounds. In liquid aerosol particles non-ideal mixing of all species determines whether the condensed phase undergoes liquid-liquid phase separation or whether it is stable in a single mixed phase, and whether it contains solid salts in equilibrium with their saturated solution. The extended thermodynamic model AIOMFAC is able to predict such phase states by representing the variety of organic components using functional groups within a group-contribution concept. The number and composition of different condensed phases impacts the diversity of reaction media for multiphase chemistry and the gas-particle partitioning of semivolatile species. Recent studies show that under certain conditions biogenic and other organic-rich particles can be present in a highly viscous, semisolid or amorphous solid physical state, with consequences regarding reaction kinetics and mass transfer limitations. We present results of new gas-particle partitioning computations for aerosol chamber data using a model based on AIOMFAC activity coefficients and state-of-the-art vapor pressure estimation methods. Different environmental conditions in terms of temperature, relative humidity (RH), salt content, amount of precursor VOCs, and physical state of the particles are considered. We show how modifications of absorptive and adsorptive gas-particle mass transfer affects the total aerosol mass in the calculations and how the results of these modeling approaches compare to data of aerosol chamber experiments, such as alpha-pinene oxidation SOA. For a condensed phase in a mixed liquid state containing ammonium sulfate, the model predicts liquid-liquid phase separation up to high RH in case of, on average, moderately hydrophilic organic compounds, such as first generation oxidation products of alpha-pinene. The computations also reveal that treating liquid phases as ideal

  9. Noncommuting mixed states cannot be broadcast

    SciTech Connect

    Barnum, H.; Caves, C.M.; Fuchs, C.A.; Jozsa, R.; Schumacher, B.

    1996-04-01

    We show that, given a general mixed state for a quantum system, there are no physical means for {ital broadcasting} that state onto two separate quantum systems, even when the state need only be reproduced marginally on the separate systems. This result extends the standard no-cloning theorem for pure states. {copyright} {ital 1996 The American Physical Society.}

  10. Noncommuting Mixed States Cannot Be Broadcast

    NASA Astrophysics Data System (ADS)

    Barnum, Howard; Caves, Carlton M.; Fuchs, Christopher A.; Jozsa, Richard; Schumacher, Benjamin

    1996-04-01

    We show that, given a general mixed state for a quantum system, there are no physical means for broadcasting that state onto two separate quantum systems, even when the state need only be reproduced marginally on the separate systems. This result extends the standard no-cloning theorem for pure states.

  11. Engineering arbitrary pure and mixed quantum states

    SciTech Connect

    Pechen, Alexander

    2011-10-15

    Controlled manipulation by atomic- and molecular-scale quantum systems has attracted a lot of research attention in recent years. A fundamental problem is to provide deterministic methods for controlled engineering of arbitrary quantum states. This work proposes a deterministic method for engineering arbitrary pure and mixed states of a wide class of quantum systems. The method exploits a special combination of incoherent and coherent controls (incoherent and coherent radiation) and has two properties which are specifically important for manipulating by quantum systems: it realizes the strongest possible degree of their state control, complete density matrix controllability, meaning the ability to steer arbitrary pure and mixed initial states into any desired pure or mixed final state, and it is all-to-one, such that each particular control transfers all initial system states into one target state.

  12. Nonadditive Mixed State Phases in Neutron Optics

    SciTech Connect

    Klepp, J.; Sponar, S.; Filipp, S.; Lettner, M.; Badurek, G.; Hasegawa, Y.

    2009-03-10

    In a neutron polarimetry experiment mixed neutron spin phases are determined. We consider evolutions leading to purely geometric, purely dynamical and combined phases. It is experimentally demonstrated that the sum of the geometric and dynamical phases--both obtained in separate measurements--is not equal to the associated total phase as obtained from a third measurement, unless the system is in a pure state. In this sense, mixed state phases are not additive.

  13. Characterisation of regional ambient biomass burning organic aerosol mixing ratios

    NASA Astrophysics Data System (ADS)

    Jolleys, M.; Coe, H.; McFiggans, G.; Capes, G.; Allan, J. D.; Crosier, J.; Williams, P.; Allen, G.; Bower, K.; Jimenez, J. L.; Russell, L. M.; Grutter, M.; Baumgardner, D.

    2012-12-01

    No evidence for a regional additional source of secondary organic aerosol (SOA) has been identified in measurements of biomass burning-influenced ambient air masses. Measurements included in this study were obtained from the deployment of an Aerodyne Quadrupole Aerosol Mass Spectrometer during four field campaigns, involving both research aircraft flights and ground-based measurements. OA concentrations normalised to excess CO (OA/dCO) show strong regional and local scale variability, with a difference of almost a factor of five across fresh OA emissions between campaigns. Average OA/dCO is typically higher in the near-field than at a greater distance from source, indicating an absence of significant SOA formation, despite evidence to suggest OA becomes increasingly oxidized with age. This trend is in contrast with observations of anthropogenic OA in urban environments, where OA/dCO is consistently shown to increase with distance from source. There is no such agreement in the case of biomass burning OA (BBOA) amongst the literature base, with conflicting examples relating to the influence of SOA on aerosol loadings. A wide range of average initial emission ratios (ERs) close to source are observed both within the datasets analysed here and within the literature, together with considerable variability in individual OA/dCO values throughout fresh biomass burning plumes. The extent of this variability far outweighs any increase in OA/dCO in the few instances it is observed here, suggesting that source conditions are of greater importance for the propagation of BBOA loadings within the ambient atmosphere. However, the implications of ageing on OA/dCO variability appear to be highly uncertain, with little consistency between observed trends for different locations. Furthermore, the exact effects of the fire conditions influencing emissions from biomass burning events remain poorly constrained. These uncertainties regarding the evolution of biomass burning emissions

  14. Mixing-Height Time Series from Operational Ceilometer Aerosol-Layer Heights

    NASA Astrophysics Data System (ADS)

    Lotteraner, Christoph; Piringer, Martin

    2016-07-01

    A new method is described to derive mixing-height time series directly from aerosol-layer height data available from a Vaisala CL51 ceilometer. As complete as possible mixing-height time series are calculated by avoiding outliers, filling data gaps by linear interpolation, and smoothing. In addition, large aerosol-layer heights at night that can be interpreted as residual layers are not assigned as mixing heights. The resulting mixing-height time series, converted to an appropriate data format, can be used as input for dispersion calculations. Two case examples demonstrate in detail how the method works. The mixing heights calculated using ceilometer data are compared with values determined from radiosounding data at Vienna by applying the parcel, Heffter, and Richardson methods. The results of the parcel method, obtained from radiosonde profiles at noon, show the best fit to the ceilometer-derived mixing heights. For midnight radiosoundings, larger deviations between mixing heights from the ceilometer and those deduced from the potential temperature profiles of the soundings are found. We use data from two Vaisala CL51 ceilometers, operating in the Vienna area at an urban and rural site, respectively, during an overlapping period of about 1 year. In addition to the case studies, the calculated mixing-height time series are also statistically evaluated and compared, demonstrating that the ceilometer-based mixing height follows an expected daily and seasonal course.

  15. Mixing-Height Time Series from Operational Ceilometer Aerosol-Layer Heights

    NASA Astrophysics Data System (ADS)

    Lotteraner, Christoph; Piringer, Martin

    2016-11-01

    A new method is described to derive mixing-height time series directly from aerosol-layer height data available from a Vaisala CL51 ceilometer. As complete as possible mixing-height time series are calculated by avoiding outliers, filling data gaps by linear interpolation, and smoothing. In addition, large aerosol-layer heights at night that can be interpreted as residual layers are not assigned as mixing heights. The resulting mixing-height time series, converted to an appropriate data format, can be used as input for dispersion calculations. Two case examples demonstrate in detail how the method works. The mixing heights calculated using ceilometer data are compared with values determined from radiosounding data at Vienna by applying the parcel, Heffter, and Richardson methods. The results of the parcel method, obtained from radiosonde profiles at noon, show the best fit to the ceilometer-derived mixing heights. For midnight radiosoundings, larger deviations between mixing heights from the ceilometer and those deduced from the potential temperature profiles of the soundings are found. We use data from two Vaisala CL51 ceilometers, operating in the Vienna area at an urban and rural site, respectively, during an overlapping period of about 1 year. In addition to the case studies, the calculated mixing-height time series are also statistically evaluated and compared, demonstrating that the ceilometer-based mixing height follows an expected daily and seasonal course.

  16. Multipartite entangled states in particle mixing

    SciTech Connect

    Blasone, M.; Dell'Anno, F.; De Siena, S.; Di Mauro, M.; Illuminati, F.

    2008-05-01

    In the physics of flavor mixing, the flavor states are given by superpositions of mass eigenstates. By using the occupation number to define a multiqubit space, the flavor states can be interpreted as multipartite mode-entangled states. By exploiting a suitable global measure of entanglement, based on the entropies related to all possible bipartitions of the system, we analyze the correlation properties of such states in the instances of three- and four-flavor mixing. Depending on the mixing parameters, and, in particular, on the values taken by the free phases, responsible for the CP-violation, entanglement concentrates in certain bipartitions. We quantify in detail the amount and the distribution of entanglement in the physically relevant cases of flavor mixing in quark and neutrino systems. By using the wave packet description for localized particles, we use the global measure of entanglement, suitably adapted for the instance of multipartite mixed states, to analyze the decoherence, induced by the free evolution dynamics, on the quantum correlations of stationary neutrino beams. We define a decoherence length as the distance associated with the vanishing of the coherent interference effects among massive neutrino states. We investigate the role of the CP-violating phase in the decoherence process.

  17. Weekly patterns of aerosol in the United States

    NASA Astrophysics Data System (ADS)

    Murphy, D. M.; Capps, S. L.; Daniel, J. S.; Frost, G. J.; White, W. H.

    2008-05-01

    Data from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network of aerosol samplers and NOAA monitoring sites are examined for weekly cycles. At remote and rural sites, fine particle elemental carbon, crustal elements, and coarse particle mass had pronounced (up to 20%) weekly cycles with minima on Sunday or Monday. Fine particle organic carbon and mass had smaller amplitude cycles, also with Sunday or Monday minima. There was no statistically significant weekly cycle in fine particle sulfate despite a 5 to 15% weekly cycle in power plant SO2 emissions. Although results for nitrate may be more susceptible to sampling artifacts, nitrate also showed a pronounced weekly cycle with an amplitude similar to elemental carbon. The only species found with a weekend maximum was Pb, probably from general aviation on weekends. Aerosol optical properties at NOAA monitoring sites were consistent with the IMPROVE chemical data, with significant weekly cycles in aerosol light absorption but not light scattering. These results support a large role of diesel emissions in elemental carbon aerosol over the entire United States and suggest that a large fraction of the airborne soil dust is anthropogenic. They also suggest that studies of weekly cycles in temperature, cloudiness, precipitation, or other meteorological variables should look for causes more in light-absorbing particles and possible ice nucleation by dust rather than sulfate or total aerosol. There are also implications for personal exposure and epidemiological studies of aerosol health effects.

  18. Hardy's criterion of nonlocality for mixed states

    SciTech Connect

    Ghirardi, GianCarlo; Marinatto, Luca

    2006-03-15

    We generalize Hardy's proof of nonlocality to the case of bipartite mixed statistical operators, and we exhibit a necessary condition which has to be satisfied by any given mixed state {sigma} in order that a local and realistic hidden variable model exists which accounts for the quantum mechanical predictions implied by {sigma}. Failure of this condition will imply both the impossibility of any local explanation of certain joint probability distributions in terms of hidden variables and the nonseparability of the considered mixed statistical operator. Our result can be also used to determine the maximum amount of noise, arising from imperfect experimental implementations of the original Hardy's proof of nonlocality, in presence of which it is still possible to put into evidence the nonlocal features of certain mixed states.

  19. Purification of Gaussian maximally mixed states

    NASA Astrophysics Data System (ADS)

    Jeong, Kabgyun; Lim, Youngrong

    2016-10-01

    We find that the purifications of several Gaussian maximally mixed states (GMMSs) correspond to some Gaussian maximally entangled states (GMESs) in the continuous-variable regime. Here, we consider a two-mode squeezed vacuum (TMSV) state as a purification of the thermal state and construct a general formalism of the Gaussian purification process. Moreover, we introduce other kind of GMESs via the process. All of our purified states of the GMMSs exhibit Gaussian profiles; thus, the states show maximal quantum entanglement in the Gaussian regime.

  20. Quantum Darwinism for mixed-state environment

    NASA Astrophysics Data System (ADS)

    Quan, Haitao; Zwolak, Michael; Zurek, Wojciech

    2009-03-01

    We exam quantum darwinism when a system is in the presence of a mixed environment, and we find a general relation between the mutual information for the mixed-state environment and the change of the entropy of the fraction of the environment. We then look at a particular solvable model, and we numerically exam the time evolution of the ``mutual information" for large environment. Finally we discuss about the exact expressions for all entropies and the mutual information at special time.

  1. Observed aerosol-induced radiative effect on plant productivity in the eastern United States

    NASA Astrophysics Data System (ADS)

    Strada, S.; Unger, N.; Yue, X.

    2015-12-01

    We apply satellite observations of aerosol optical depth (AOD) in conjunction with flux tower-derived estimates of gross primary productivity (GPP) to probe the relationship between atmospheric aerosol loading and carbon uptake rate at 10 select sites (4 deciduous broadleaf, 3 cropland, 1 evergreen needle leaf, 1 mixed forest and 1 grassland) on hourly time scales in the growing season in the eastern United States. For deciduous and mixed forests, the aerosol light scattering increases GPP with a maximum effect observed under polluted conditions (AOD >0.6), when diffuse radiation is 40-60%. During midday hours, high AOD conditions (>0.4) enhance plant productivity by ∼13% in deciduous forests. In contrast, we find that high diffuse light fraction does not increase the carbon uptake rate in croplands and grasslands; for these ecosystems, we estimate that high AOD conditions reduce GPP by ∼17% during midday hours. Our findings are consistent with previous studies that have attributed these contrasting response sensitivities to the complex and closed canopy architecture of forests versus crops and grasslands. C4 but not C3 crops may benefit from pollution-induced changes in diffuse and direct light. Further research is needed to investigate the role of local meteorology as a possible confounder in the connection between atmospheric aerosols and plant productivity.

  2. Mixed-layer ocean responses to anthropogenic aerosol dimming from 1870 to 2000

    NASA Astrophysics Data System (ADS)

    Dallafior, T. N.; Folini, D.; Knutti, R.; Wild, M.

    2016-01-01

    It is debated to what extent surface solar radiation (SSR) changes through varying anthropogenic aerosol emissions since industrialization affected surface temperatures (tsurf). We use mixed-layer ocean experiments with the general circulation model ECHAM6.1 and explicit aerosols (HAM2.2) to identify regions where this effect is discernible. For each decade from 1870 to 2000 we derive three equilibria: anthropogenic aerosol emissions and greenhouse gas concentrations at the respective decade's levels (ALL), either aerosols or greenhouse gases fixed at year 1850 levels (GHG and AERO). We duplicated parts of the experiments with different prescribed divergence of ocean heat transport (Q_ALL, Q_AERO, and Q_GHG). Comparing year 2000 with year 1870 equilibria, we find global average cooling of -1.4 K for AERO and warming of 1.4 K for GHG. ALL and Q_ALL warm by 0.6 K and 0.4 K, respectively. The way divergence of ocean heat transport is prescribed thus matters. Pattern correlations of year 2000 tsurf responses in ALL with the sum of AERO and GHG are higher (0.88) than with Q_ALL (0.71) confirming additivity of global patterns, but not of global means. The imprint of anthropogenic aerosols on tsurf response patterns in ALL is distinct, thus potentially detectable. Over the decades, ocean fractions affected by either changing aerosol optical depth or all-sky SSR vary in concert, supporting linkage between anthropogenic aerosols and all-sky SSR. SSR changes and tsurf responses are marginally collocated. Oceanic regions with strongest tsurf response to aerosol-induced SSR changes are the northern midlatitudes and North Pacific with tsurf sensitivities up to -0.7 K W m-2 SSR change.

  3. Mixed-layer ocean responses to anthropogenic aerosol dimming from 1870 to 2000

    NASA Astrophysics Data System (ADS)

    Dallafior, Tanja; Folini, Doris; Knutti, Reto; Wild, Martin

    2016-04-01

    It is still debated, to what extent anthropogenic aerosol-induced changes in surface solar radiation (SSR) since industrialization affected surface temperatures (tsurf). We use mixed-layer ocean (MLO) experiments with the general circulation model ECHAM6.1 and explicit aerosols (HAM2.2) to identify regions where this effect is discernible. For each decade from 1870 to 2000 we derive three equilibria: anthropogenic aerosol emissions and greenhouse gas concentrations at the respective decade's levels (ALL), either aerosols or greenhouse gases fixed at year 1850 levels (GHG and AERO). We duplicated parts of the experiments with different prescribed divergence of ocean heat transport (Q_ALL, Q_AERO, Q_GHG). Comparing year 2000 with year 1870 equilibria, we find global average cooling of -1.4K for AERO, and warming of 1.4K for GHG. ALL and Q_ALL warm by 0.6K and 0.4K, respectively. The way divergence of ocean heat transport is prescribed thus matters. Pattern correlations of year 2000 tsurf responses in ALL with the sum of AERO and GHG are higher (0.88) than with Q_ALL (0.71) confirming additivity of global patterns, but not of global means. The imprint of anthropogenic aerosols on tsurf response patterns in ALL is distinct, thus potentially detectable. Over the decades, ocean fractions affected by either changing aerosol optical depth or all-sky SSR vary in concert, supporting linkage between anthropogenic aerosols and all-sky SSR. SSR changes and tsurf responses are marginally collocated. Oceanic regions with strongest tsurf response to aerosol-induced SSR changes are the northern mid-latitudes and North Pacific with tsurf sensitivities up to -0.7K per Wm-2 SSR change. Results presented have been published under the same title in the Journal of Geophysical Research, Volume 121, DOI 10.1002/2015JD024070.

  4. Black carbon concentrations and mixing state in the Finnish Arctic

    NASA Astrophysics Data System (ADS)

    Raatikainen, T.; Brus, D.; Hyvärinen, A.-P.; Svensson, J.; Asmi, E.; Lihavainen, H.

    2015-09-01

    Atmospheric aerosol composition was measured using a Single Particle Soot Photometer (SP2) in the Finnish Arctic during winter 2011-2012. The Sammaltunturi measurement site at the Pallas GAW (Global Atmosphere Watch) station receives air masses from different source regions including the Arctic Ocean and continental Europe. The SP2 provides detailed information about mass distributions and mixing state of refractory black carbon (rBC). The measurements showed widely varying rBC mass concentrations (0-120 ng m-3), which were related to varying contributions of different source regions and aerosol removal processes. The rBC mass was log-normally distributed showing a relatively constant rBC core mass mean diameter with an average of 194 nm (75-655 nm sizing range). On average, the number fraction of particles containing rBC was 0.24 (integrated over 350-450 nm particle diameter range) and the average particle diameter to rBC core volume equivalent diameter ratio was 2.0 (averaged over particles with 150-200 nm rBC core volume equivalent diameters). These average numbers mean that the observed rBC core mass mean diameter is similar to those of aged particles, but the observed particles seem to have unusually high particle to rBC core diameter ratios. Comparison of the measured rBC mass concentration with that of the optically detected equivalent black carbon (eBC) using an Aethalometer and a MAAP showed that eBC was larger by a factor of five. The difference could not be fully explained without assuming that only a part of the optically detected light absorbing material is refractory and absorbs light at the wavelength used by the SP2. Finally, climate implications of five different black carbon mixing state representations were compared using the Mie approximation and simple direct radiative forcing efficiency calculations. These calculations showed that the observed mixing state means significantly lower warming effect or even a net cooling effect when compared with

  5. Entanglement of spin coherent mixed states

    NASA Astrophysics Data System (ADS)

    Mansour, Mostafa; Hassouni, Yassine

    2016-04-01

    In this paper, we quantify the amount of entanglement of bipartite mixed states represented by a statistical mixture of the more general type of two-qubit non-orthogonal states of the form: |ψi>=ui|χi>⊗|ηi>+vi|χi>⊗|ηi‧>+wi|χi‧>⊗|ηi>+zi|χi‧>⊗|ηi‧>, constructed by linearly independent spin coherent states. We use the concurrence as a measure of entanglement and we study its behavior in terms of the amplitudes of SU(2) coherent states.

  6. Modeling immersion freezing with aerosol-dependent prognostic ice nuclei in Arctic mixed-phase clouds

    NASA Astrophysics Data System (ADS)

    Paukert, M.; Hoose, C.

    2014-07-01

    While recent laboratory experiments have thoroughly quantified the ice nucleation efficiency of different aerosol species, the resulting ice nucleation parameterizations have not yet been extensively evaluated in models on different scales. Here the implementation of an immersion freezing parameterization based on laboratory measurements of the ice nucleation active surface site density of mineral dust and ice nucleation active bacteria, accounting for nucleation scavenging of ice nuclei, into a cloud-resolving model with two-moment cloud microphysics is presented. We simulated an Arctic mixed-phase stratocumulus cloud observed during Flight 31 of the Indirect and Semi-Direct Aerosol Campaign near Barrow, Alaska. Through different feedback cycles, the persistence of the cloud strongly depends on the ice number concentration. It is attempted to bring the observed cloud properties, assumptions on aerosol concentration, and composition and ice formation parameterized as a function of these aerosol properties into agreement. Depending on the aerosol concentration and on the ice crystal properties, the simulated clouds are classified as growing, dissipating, and quasi-stable. In comparison to the default ice nucleation scheme, the new scheme requires higher aerosol concentrations to maintain a quasi-stable cloud. The simulations suggest that in the temperature range of this specific case, mineral dust can only contribute to a minor part of the ice formation. The importance of ice nucleation active bacteria and possibly other ice formation modes than immersion freezing remains poorly constrained in the considered case, since knowledge on local variations in the emissions of ice nucleation active organic aerosols in the Arctic is scarce.

  7. The ASTAR 2007 April 14 haze layer: The radiative effect of an aged and internally mixed aerosol in the Arctic

    NASA Astrophysics Data System (ADS)

    Engvall, A.-C.; Ström, J.; Tunved, P.; Schlager, H.; Minikin, A.

    2009-04-01

    the mixing state of the aerosol in the size range between 17 and 239 nm obtained from a volatility DMPS (V-DMPS). Information about the light-absorbing properties of the aerosol was obtained from a custom-built particle soot absorption photometer (PSAP), which provided the particle light-absorption coefficient sp at a wavelength of 525 nm. From this we estimated the black carbon mass concentration (BC, ng m-3) by using the commonly employed specific absorption coefficient 10 m2 g-1 [Petzold, et al., 1997]. As a part of the quality control, an intercomparison was made with measurements from the Zeppelin station (474 m.a.s.l.) at Ny-Ålesund [Ström, et al., 2003; Engvall, et al., 2008]. This indicated good agreement between the airborne and the ground-based size-distribution results for particles of diameter smaller than approximately 200 nm. To investigate the radiative effects of the enhanced aerosol layer a one-dimensional radiation model was used to simulate the amplified heating rate (K day-1). The calculations were based on in-situ measurements of the input variables, viz. relative humidity (RH), temperature (T), pressure (p), aerosol size distribution, and the scattering and absorption properties of the aerosols, for more details see [Treffeisen, et al., 2007]. CONCLUSIONS Transport of pollutants from the mid-latitudes into the Arctic free troposphere may give rise to a heating rate within the plume of up to 1.3 K day-1, dependent on the properties of the plume and the surface albedo. The surface properties, in this study ice/snow covered or ice-free ocean, are of importance since the latter case with a low albedo shows a 25-30% decrease of the heating rate compared to the snow/ice case. These results can be compared to those obtained by [Treffeisen, et al., 2007], who estimated a heating rate of 1.7 K day-1 at an altitude of 0.5 km based on the observed concentrations of particles, soot, and aerosol scattering during the highest pollution event ever recorded

  8. Iron Speciation and Mixing in Single Aerosol Particles from the Asian Continental Outflow

    SciTech Connect

    Moffet, Ryan C.; Furutani, Hiroshi; Rodel, Tobias; Henn, Tobias R.; Sprau, Peter; Laskin, Alexander; Uematsu, Mitsuo; Gilles, Marry K.

    2012-04-04

    Bioavailable iron from atmospheric aerosol is an essential nutrient that can control oceanic productivity, thereby impacting the global carbon budget and climate. Particles collected on Okinawa Island during an atmospheric pollution transport event from China were analyzed using complementary single particle techniques to determine the iron source and speciation. Comparing the spatial distribution of iron within ambient particles and standard Asian mineral dust, it was determined that field-collected atmospheric Fe-containing particles have numerous sources, including anthropogenic sources such as coal combustion. Fe-containing particles were found to be internally mixed with secondary species such as sulfate, soot, and organic carbon. The mass weighted average Fe(II) fraction (defined as Fe(II)/[Fe(II)+Fe(III)]) was determined to be 0.33 {+-} 0.08. Within the experimental uncertainty, this value lies close to the range of 0.26-0.30 determined for representative Asian mineral dust. Previous studies have indicated that the solubility of iron from combustion is much higher than that from mineral dust. Therefore, chemical and/or physical differences other than oxidation state may help explain the higher solubility of iron in atmospheric particles.

  9. Experimental Evidence for Mixed Reality States

    NASA Astrophysics Data System (ADS)

    Gintautas, Vadas; Hubler, Alfred

    2008-03-01

    We present experimental data on the limiting behavior of an inter-reality system: a virtual pendulum with a bi-directional instantaneous coupling to its real-world counterpart [Gintautas & Hubler, Phys.Rev.E 75, 057201 (2007)]. The data show that if the physical parameters of the simplified virtual system are close to the parameters of the real system, there is a phase transition from an uncorrelated dual reality state to a mixed reality state in which the motion of the two pendulums is highly correlated. As virtual systems better approximate real ones, even weak couplings in inter-reality systems may induce sudden transitions to mixed reality states. This phenomenon may be typical for systems with instantaneous coupling and was recently featured on the tip sheet of the American Physical Society [http://www.aps.org/about/tipsheets/tip68.cfm ]. We show that mixed reality states in physical systems are related to out-of- body experiences of humans in 3D-video feedback systems [H. H. Ehrsson, The Experimental Induction of Out-of-Body Experiences. Science 317, 1048 (2007)].

  10. Fidelity between Gaussian mixed states with quantum state quadrature variances

    NASA Astrophysics Data System (ADS)

    Hai-Long, Zhang; Chun, Zhou; Jian-Hong, Shi; Wan-Su, Bao

    2016-04-01

    In this paper, from the original definition of fidelity in a pure state, we first give a well-defined expansion fidelity between two Gaussian mixed states. It is related to the variances of output and input states in quantum information processing. It is convenient to quantify the quantum teleportation (quantum clone) experiment since the variances of the input (output) state are measurable. Furthermore, we also give a conclusion that the fidelity of a pure input state is smaller than the fidelity of a mixed input state in the same quantum information processing. Project supported by the National Basic Research Program of China (Grant No. 2013CB338002) and the Foundation of Science and Technology on Information Assurance Laboratory (Grant No. KJ-14-001).

  11. Fidelity between Gaussian mixed states with quantum state quadrature variances

    NASA Astrophysics Data System (ADS)

    Hai-Long, Zhang; Chun, Zhou; Jian-Hong, Shi; Wan-Su, Bao

    2016-04-01

    In this paper, from the original definition of fidelity in a pure state, we first give a well-defined expansion fidelity between two Gaussian mixed states. It is related to the variances of output and input states in quantum information processing. It is convenient to quantify the quantum teleportation (quantum clone) experiment since the variances of the input (output) state are measurable. Furthermore, we also give a conclusion that the fidelity of a pure input state is smaller than the fidelity of a mixed input state in the same quantum information processing. Project supported by the National Basic Research Program of China (Grant No. 2013CB338002) and the Foundation of Science and Technology on Information Assurance Laboratory (Grant No. KJ-14-001).

  12. FESEM Analysis showing evidence of aerosol Mixing over Indo-Gangetic Plains

    NASA Astrophysics Data System (ADS)

    Singh, R. P.; Huth, J.; Wagner, T.; Sharma, M.; Chauhan, A.; Singh, S.; Pandey, S. N.

    2012-12-01

    Kanpur AERONET deployed in January 2001 has provided a long-term dataset which has been used to understand the aerosol properties and aerosol long term trend in the Indo-Gangetic Plains (IGP). Recent studies have revealed higher black carbon (BC) mass concentrations in the IGP, home to 900 million people. We present analysis of black carbon mass concentrations obtained from several locations in the IGP - namely Varanasi, Lucknow, Kanpur, Greater Noida and Delhi. Measurements show significant diurnal variation with higher BC concentrations in the morning hours and low concentrations during afternoon and evening time. Seasonally, BC concentrations are generally found to be higher during winter months compared to spring and summer monsoon season showing high seasonal variability. The higher winter-time BC is associated with a stable and shallow boundary layer which favors accumulation of pollutants over the IGP, resulting in dense haze conditions. Filter-based analysis, obtained from samples used in Aethalometer and high vacuum sampler, were analyzed to study aerosol surface characteristics and size of particles. Additionally, FESEM (Field Emission Scanning Electron Microscope) analysis show many dust minerals (Na, Al, Si, K, Fe), biogenic substances, fly ash of varying sizes 15 nanometer to 5 micron. The SEM imagery also show heterogeneous aerosol particles, sometimes these mineral grains are seen separately and sometime coating of fly ash and mineral particles are clearly seen. Similarly, Kanpur AERONET data is analyzed during winter and pre-monsoon season, contrasting aerosol properties (SSA, Refractive index and Size distribution) are found that are associated with large aerosol mixing, also supported from the FESEM analysis.

  13. Optimal cloning of mixed Gaussian states

    SciTech Connect

    Guta, Madalin; Matsumoto, Keiji

    2006-09-15

    We construct the optimal one to two cloning transformation for the family of displaced thermal equilibrium states of a harmonic oscillator, with a fixed and known temperature. The transformation is Gaussian and it is optimal with respect to the figure of merit based on the joint output state and norm distance. The proof of the result is based on the equivalence between the optimal cloning problem and that of optimal amplification of Gaussian states which is then reduced to an optimization problem for diagonal states of a quantum oscillator. A key concept in finding the optimum is that of stochastic ordering which plays a similar role in the purely classical problem of Gaussian cloning. The result is then extended to the case of n to m cloning of mixed Gaussian states.

  14. Measurement of mixed biomass burning and mineral dust aerosol in the thermal infrared

    NASA Astrophysics Data System (ADS)

    Koehler, C. H.; Trautmann, T.; Lindermeir, E.

    2009-03-01

    From January 19th to February 7th, 2008, we installed a Fourier transform infrared spectrometer (FTIR) at Praia Airport on the island of Santiago, Cape Verde. Our goal was to measure the combined radiative effect of biomass burning aerosol and mineral dust usually observed there during that time of the year, when mineral dust emerging from the Sahara mixes with biomass burning aerosol transported north-westwards from the Sahelian region. Our measurements were part of the Saharan Mineral Dwst Experiment 2 (SAMUM 2) funded by the German Research Foundation (DFG) as continuation of the SAMUM field experiment in Morocco in 2006. SAMUM 2 is a joint venture of several German research institutes and universities and included both ground based as well as airborne measurements with the DLR Falcon research aircraft. The ground based instrumentation included spectrometers for visible and thermal infrared downwelling radiation, sun photometers, LIDAR and particle impactors while the Falcon was equipped with LIDAR and several instruments for aerosol analysis and sample return. A comparison of the FTIR measurements with radiative transfer simulations yields the expected aerosol forcing in the atmospheric window region after application of a suitable calibration method.

  15. Fast mental states decoding in mixed reality.

    PubMed

    De Massari, Daniele; Pacheco, Daniel; Malekshahi, Rahim; Betella, Alberto; Verschure, Paul F M J; Birbaumer, Niels; Caria, Andrea

    2014-01-01

    The combination of Brain-Computer Interface (BCI) technology, allowing online monitoring and decoding of brain activity, with virtual and mixed reality (MR) systems may help to shape and guide implicit and explicit learning using ecological scenarios. Real-time information of ongoing brain states acquired through BCI might be exploited for controlling data presentation in virtual environments. Brain states discrimination during mixed reality experience is thus critical for adapting specific data features to contingent brain activity. In this study we recorded electroencephalographic (EEG) data while participants experienced MR scenarios implemented through the eXperience Induction Machine (XIM). The XIM is a novel framework modeling the integration of a sensing system that evaluates and measures physiological and psychological states with a number of actuators and effectors that coherently reacts to the user's actions. We then assessed continuous EEG-based discrimination of spatial navigation, reading and calculation performed in MR, using linear discriminant analysis (LDA) and support vector machine (SVM) classifiers. Dynamic single trial classification showed high accuracy of LDA and SVM classifiers in detecting multiple brain states as well as in differentiating between high and low mental workload, using a 5 s time-window shifting every 200 ms. Our results indicate overall better performance of LDA with respect to SVM and suggest applicability of our approach in a BCI-controlled MR scenario. Ultimately, successful prediction of brain states might be used to drive adaptation of data representation in order to boost information processing in MR.

  16. Fast mental states decoding in mixed reality

    PubMed Central

    De Massari, Daniele; Pacheco, Daniel; Malekshahi, Rahim; Betella, Alberto; Verschure, Paul F. M. J.; Birbaumer, Niels; Caria, Andrea

    2014-01-01

    The combination of Brain-Computer Interface (BCI) technology, allowing online monitoring and decoding of brain activity, with virtual and mixed reality (MR) systems may help to shape and guide implicit and explicit learning using ecological scenarios. Real-time information of ongoing brain states acquired through BCI might be exploited for controlling data presentation in virtual environments. Brain states discrimination during mixed reality experience is thus critical for adapting specific data features to contingent brain activity. In this study we recorded electroencephalographic (EEG) data while participants experienced MR scenarios implemented through the eXperience Induction Machine (XIM). The XIM is a novel framework modeling the integration of a sensing system that evaluates and measures physiological and psychological states with a number of actuators and effectors that coherently reacts to the user's actions. We then assessed continuous EEG-based discrimination of spatial navigation, reading and calculation performed in MR, using linear discriminant analysis (LDA) and support vector machine (SVM) classifiers. Dynamic single trial classification showed high accuracy of LDA and SVM classifiers in detecting multiple brain states as well as in differentiating between high and low mental workload, using a 5 s time-window shifting every 200 ms. Our results indicate overall better performance of LDA with respect to SVM and suggest applicability of our approach in a BCI-controlled MR scenario. Ultimately, successful prediction of brain states might be used to drive adaptation of data representation in order to boost information processing in MR. PMID:25505878

  17. Fast mental states decoding in mixed reality.

    PubMed

    De Massari, Daniele; Pacheco, Daniel; Malekshahi, Rahim; Betella, Alberto; Verschure, Paul F M J; Birbaumer, Niels; Caria, Andrea

    2014-01-01

    The combination of Brain-Computer Interface (BCI) technology, allowing online monitoring and decoding of brain activity, with virtual and mixed reality (MR) systems may help to shape and guide implicit and explicit learning using ecological scenarios. Real-time information of ongoing brain states acquired through BCI might be exploited for controlling data presentation in virtual environments. Brain states discrimination during mixed reality experience is thus critical for adapting specific data features to contingent brain activity. In this study we recorded electroencephalographic (EEG) data while participants experienced MR scenarios implemented through the eXperience Induction Machine (XIM). The XIM is a novel framework modeling the integration of a sensing system that evaluates and measures physiological and psychological states with a number of actuators and effectors that coherently reacts to the user's actions. We then assessed continuous EEG-based discrimination of spatial navigation, reading and calculation performed in MR, using linear discriminant analysis (LDA) and support vector machine (SVM) classifiers. Dynamic single trial classification showed high accuracy of LDA and SVM classifiers in detecting multiple brain states as well as in differentiating between high and low mental workload, using a 5 s time-window shifting every 200 ms. Our results indicate overall better performance of LDA with respect to SVM and suggest applicability of our approach in a BCI-controlled MR scenario. Ultimately, successful prediction of brain states might be used to drive adaptation of data representation in order to boost information processing in MR. PMID:25505878

  18. Two extreme types of mixing of dust with urban aerosols observed in Kosa particles: ‘After’ mixing and ‘on-the-way’ mixing

    NASA Astrophysics Data System (ADS)

    Suzuki, Issei; Igarashi, Yasuhito; Dokiya, Yukiko; Akagi, Tasuku

    2010-02-01

    Besides well-known episodic Kosa during spring, high concentrations of Ca 2+ in aerosols were observed early in summer as well as in the semi-continuous data of the aerosols at the summit of Mt. Fuji. We further analysed the data to study the chemical characteristics of the high calcium event during early summer. The back trajectory analyses of the event indicated that Ca was transported from arid and semi-arid regions (e.g. the Taklamakan desert) through the westerly-dominated troposphere higher than the height of the summit of Fuji. The amount of SO 42- was always equivalent to that of NH 4+ unlike the case of the normal Kosa period where SO 42- is in excess with respect to NH 4+. This shows the 'after' mixing of unreacted CaCO 3 of Kosa origin with (NH 4) 2SO 4, which was only realized by the downward injection of Kosa particles from higher altitudes to the air masses of different origin. In the case of normal Kosa, the air bearing Kosa particles passed through the polluted area to absorb unneutralized acids ('on-the-way' mixing), whereas in the case of the Kosa-like phenomena in summer, the acids from the polluted area have been neutralized by NH 4+ and become inactive before mixing with CaCO 3 ("after" mixing). We have simplified the chemistry of aerosols using their three major components, Ca 2+, SO 42- and NH 4+, and introduced a new triangle diagram with the three assumed end-members of CaCO 3, CaSO 4 and (NH 4) 2SO 4 to quantify the contribution of the 'after' mixing to the aerosols (AMI; 'after' mixing index). Based on the back trajectories of some high AMI cases, CaCO 3 in Kosa particles was transported through the middle troposphere (5000-7000 m) and descended to meet another air mass where SO 42- had been already neutralized by NH 3.

  19. Multistability with a Metastable Mixed State

    NASA Astrophysics Data System (ADS)

    Sneppen, Kim; Mitarai, Namiko

    2012-09-01

    Complex dynamical systems often show multiple metastable states. In macroevolution, such behavior is suggested by punctuated equilibrium and discrete geological epochs. In molecular biology, bistability is found in epigenetics and in the many mutually exclusive states that a human cell can take. Sociopolitical systems can be single-party regimes or a pluralism of balancing political fractions. To introduce multistability, we suggest a model system of D mutually exclusive microstates that battle for dominance in a large system. Assuming one common intermediate state, we obtain D+1 metastable macrostates for the system, one of which is a self-reinforced mixture of all D+1 microstates. Robustness of this metastable mixed state increases with diversity D.

  20. Simulation of nitrate, sulfate, and ammonium aerosols over the United States

    NASA Astrophysics Data System (ADS)

    Walker, J. M.; Philip, S.; Martin, R. V.; Seinfeld, J. H.

    2012-11-01

    Atmospheric concentrations of inorganic gases and aerosols (nitrate, sulfate, and ammonium) are simulated for 2009 over the United States using the chemical transport model GEOS-Chem. Predicted aerosol concentrations are compared with surface-level measurement data from the Interagency Monitoring of Protected Visual Environments (IMPROVE), the Clean Air Status and Trends Network (CASTNET), and the California Air Resources Board (CARB). Sulfate predictions nationwide are in reasonably good agreement with observations, while nitrate and ammonium are over-predicted in the East and Midwest, but under-predicted in California, where observed concentrations are the highest in the country. Over-prediction of nitrate in the East and Midwest is consistent with results of recent studies, which suggest that nighttime nitric acid formation by heterogeneous hydrolysis of N2O5 is over-predicted based on current values of the N2O5 uptake coefficient, γ, onto aerosols. After reducing the value of γ by a factor of 10, predicted nitrate levels in the US Midwest and East still remain higher than those measured, and over-prediction of nitrate in this region remains unexplained. Comparison of model predictions with satellite measurements of ammonia from the Tropospheric Emissions Spectrometer (TES) indicates that ammonia emissions in GEOS-Chem are underestimated in California and that the nationwide seasonality applied to ammonia emissions in GEOS-Chem does not represent California very well, particularly underestimating winter emissions. An ammonia sensitivity study indicates that GEOS-Chem simulation of nitrate is ammonia-limited in southern California and much of the state, suggesting that an underestimate of ammonia emissions is likely the main cause for the under-prediction of nitrate aerosol in many areas of California. An approximate doubling of ammonia emissions is needed to reproduce observed nitrate concentrations in southern California and in other ammonia sensitive areas

  1. A numerical study of aerosol influence on mixed-phase stratiform clouds through modulation of the liquid phase

    NASA Astrophysics Data System (ADS)

    de Boer, G.; Hashino, T.; Tripoli, G. J.; Eloranta, E. W.

    2013-02-01

    Numerical simulations were carried out in a high-resolution two-dimensional framework to increase our understanding of aerosol indirect effects in mixed-phase stratiform clouds. Aerosol characteristics explored include insoluble particle type, soluble mass fraction, influence of aerosol-induced freezing point depression and influence of aerosol number concentration. Simulations were analyzed with a focus on the processes related to liquid phase microphysics, and ice formation was limited to droplet freezing. Of the aerosol properties investigated, aerosol insoluble mass type and its associated freezing efficiency was found to be most relevant to cloud lifetime. Secondary effects from aerosol soluble mass fraction and number concentration also alter cloud characteristics and lifetime. These alterations occur via various mechanisms, including changes to the amount of nucleated ice, influence on liquid phase precipitation and ice riming rates, and changes to liquid droplet nucleation and growth rates. Alteration of the aerosol properties in simulations with identical initial and boundary conditions results in large variability in simulated cloud thickness and lifetime, ranging from rapid and complete glaciation of liquid to the production of long-lived, thick stratiform mixed-phase cloud.

  2. High Spectral Resolution Lidar (HSRL)-2 Observations of Aerosol Variability and Mixing during Boundary Layer Evolution in Houston

    NASA Astrophysics Data System (ADS)

    Burton, S. P.; Scarino, A. J.; Rogers, R. R.; Hostetler, C. A.; Ferrare, R. A.; Sawamura, P.; Berkoff, T.; Harper, D. B.; Cook, A. L.; Saide, P. E.

    2014-12-01

    The NASA Langley airborne multi-wavelength High Spectral Resolution Lidar (HSRL-2) provides the vertical distribution of aerosol optical properties as "curtains" of aerosol extinction, backscatter and depolarization along the flight track, plus intensive properties that are used to infer aerosol type and external mixing of types. Deployed aboard the NASA Langley King Air on the DISCOVER-AQ field mission in Houston in September 2013, HSRL-2 flew a pattern that included 18 ground sites, repeated four times a day, coordinated with a suite of airborne in situ measurements. The horizontally and vertically resolved curtains of HSRL-2 measurements give an unparalleled view of the spatial and temporal variability of aerosol, which provide broad context for interpreting other measurements and models. In Houston, HSRL-2 generally observed significant variability with distinct layering: boundary layer, residual layer, and frequent upper layers of smoke transported from the Mississippi Valley. The period from Sep. 11-14 is notable for a large aerosol build-up and persistent layers in the free troposphere. We investigate the aerosol properties and evolution using the vertically resolved HSRL-2 measurements, typing and mixture analysis techniques, and boundary layer detection. Between morning and afternoon overpasses, as the boundary layer grows, many distinctions between the layers are lost as the aerosols become mixed. As the boundary layer collapses overnight, the aerosols are cut off and are observed in a distinct residual layer the following morning. HSRL-2 measurements of the upper smoke layers suggest slightly different properties each day as new smoke enters the region, while the morning boundary layer indicates more similarity in local emissions day-to-day. HSRL-2 intensive variables (indicators of aerosol type) reflect complex yet predictable mixing. We will present the analysis of aerosol mixtures, and explore the WRF-Chem chemical transport model along the HSRL-2

  3. Aerosol Inflluence on Ice Nucleation via the Immersion Mode in Mixed-Phase Arctic Stratiform Clouds

    NASA Astrophysics Data System (ADS)

    de Boer, G.; Hashino, T.; Tripoli, G. J.; Eloranta, E. W.

    2009-12-01

    Mixed-phase stratiform clouds are commonly observed at high latitudes (e.g. Shupe et al., 2006; de Boer et al., 2009a). Herman and Goody (1976), as well as Curry et al. (1996) present summaries of Arctic cloud climatologies that show low altitude stratus frequencies of up to 70% during transitional seasons. In addition to their frequent occurrence, these clouds have significant impacts on the near-surface atmospheric radiative budget, with estimates of wintertime reductions in net surface cooling of 40-50 Wm-2 (Curry et al., 1996) due predominantly to liquid in the mixed-phase layer. Both observational and modeling studies (e.g. Harrington et al., 1999; Jiang et al., 2000; Shupe et al., 2008; Klein et al., 2008) show a strong connection between the amount of ice present and the lifetime of the liquid portion of the cloud layer. This is thought to occur via the Bergeron-Findeissen mechanism (Pruppacher and Klett, 1997) in which ice grows at the expense of liquid due to its lower saturation vapor pressure. Unfortunately, the mechanisms by which ice is nucleated within these mixed-phase layers are not yet fully understood, and therefore an accurate depiction of this process for mixed-phase stratiform clouds has not yet been characterized. The nucleation mechanisms that are active in a given environment are sensitive to aerosol properties. Insoluble particles are typically good nuclei for ice particle formation, while soluble particles are typically better at nucleating water droplets. Aerosol observations from the Arctic often show mixed aerosol particles that feature both soluble and insoluble mass (Leaitch et al., 1984). Soluble mass fractions for these particles have been shown to be high, with estimates of 60-80% and are often made up of sulfates (Zhou et al., 2001; Bigg and Leck, 2001). It is believed that a significant portion of this sulfate mass comes from dimethyl sulfide (DMS) production in the Arctic Ocean and subsequent atmospheric oxidation. Since these

  4. OH-initiated heterogeneous oxidation of internally-mixed squalane and secondary organic aerosol.

    PubMed

    Kolesar, Katheryn R; Buffaloe, Gina; Wilson, Kevin R; Cappa, Christopher D

    2014-03-18

    Recent work has established that secondary organic aerosol (SOA) can exist as an amorphous solid, leading to various suggestions that the addition of SOA coatings to existing particles will decrease the reactivity of those particles toward common atmospheric oxidants. Experimental evidence suggests that O3 is unable to physically diffuse through an exterior semisolid or solid layer thus inhibiting reaction with the core. The extent to which this suppression in reactivity occurs for OH has not been established, nor has this been demonstrated specifically for SOA. Here, measurements of the influence of adding a coating of α-pinene+O3 SOA onto squalane particles on the OH-initiated heterogeneous oxidation rate are reported. The chemical composition of the oxidized internally mixed particles was monitored online using a vacuum ultraviolet-aerosol mass spectrometer. Variations in the squalane oxidation rate with particle composition were quantified by measurement of the effective uptake coefficient, γeff, which is the loss rate of a species relative to the oxidant-particle collision rate. Instead of decreasing, the measured γeff increased continuously as the SOA coating thickness increased, by a factor of ∼2 for a SOA coating thickness of 42 nm (corresponding to ca. two-thirds of the particle mass). These results indicate that heterogeneous oxidation of ambient aerosol by OH radicals is not inhibited by SOA coatings, and further that condensed phase chemical pathways and rates in organic particles depend importantly on composition.

  5. New Examination of the Traditional Raman Lidar Technique II: Temperature Dependence Aerosol Scattering Ratio and Water Vapor Mixing Ratio Equations

    NASA Technical Reports Server (NTRS)

    Whiteman, David N.; Abshire, James B. (Technical Monitor)

    2002-01-01

    In a companion paper, the temperature dependence of Raman scattering and its influence on the Raman water vapor signal and the lidar equations was examined. New forms of the lidar equation were developed to account for this temperature sensitivity. Here we use those results to derive the temperature dependent forms of the equations for the aerosol scattering ratio, aerosol backscatter coefficient, extinction to backscatter ratio and water vapor mixing ratio. Pertinent analysis examples are presented to illustrate each calculation.

  6. A numerical study of aerosol influence on mixed-phase stratiform clouds through modulation of the liquid phase

    NASA Astrophysics Data System (ADS)

    de Boer, G.; Hashino, T.; Tripoli, G. J.; Eloranta, E. W.

    2012-08-01

    Numerical simulations were carried out in a high-resolution two dimensional framework to increase our understanding of aerosol indirect effects in mixed-phase stratiform clouds. Aerosol characteristics explored include insoluble particle type, soluble mass fraction, the influence of aerosol-induced freezing point depression and the influence of aerosol number concentration. These experiments were completed with an emphasis on the liquid phase, with droplet freezing the mechanism for ice production. Of the aerosol properties investigated, aerosol insoluble mass type and its associated freezing efficiency was found to be most relevant to cloud lifetime. Secondary effects from aerosol soluble mass fraction and number concentration also alter cloud characteristics and lifetime. These alterations occur via various mechanisms, including changes to the amount of nucleated ice, influence on liquid phase precipitation and ice riming rates, and changes to liquid droplet growth rates. Simulation of the same environment leads to large variability of cloud thickness and lifetime, ranging from rapid and complete glaciation of the cloud to the production of a long-lived, thick stratiform mixed-phase cloud. In the end, these processes are summarized into a diagram that includes internal feedback loops that act within the cloud system.

  7. Formation of secondary aerosols from gasoline vehicle exhausts when mixing with SO2

    NASA Astrophysics Data System (ADS)

    Liu, T.; Wang, X.; Hu, Q.; Deng, W.; Zhang, Y.; Ding, X.; Fu, X.; Bernard, F.; Zhang, Z.; Lü, S.; He, Q.; Bi, X.; Chen, J.; Sun, Y.; Yu, J.; Peng, P.; Sheng, G.; Fu, J.

    2015-09-01

    Sulfur dioxide (SO2) can enhance the formation of secondary aerosols from biogenic volatile organic compounds (VOCs), but its influence on secondary aerosol formation from anthropogenic VOCs, particularly complex mixtures like vehicle exhausts, is still poorly understood. Here we directly co-introduced gasoline vehicles exhausts (GVE) and SO2, a typical pollutant from coal burning, into a smog chamber to investigate the formation of secondary organic aerosols (SOA) and sulfate aerosols through photooxidation. In the presence of high concentration of SO2, new particle formation was enhanced while substantial sulfate was formed through the oxidation of SO2. The homogenous oxidation by OH radicals contributed a negligible fraction to the conversion of SO2 to sulfate, and instead the oxidation by stabilized Criegee intermediates (sCIs), formed from alkenes in the exhaust reacting with ozone, dominated the conversion of SO2. After 5 h of photochemical aging, GVE's SOA production factor revealed an increase by 60-200 % in the presence of high concentration of SO2. This increase could largely be attributed to acid-catalyzed SOA formation, which was evidenced by the strong positive linear correlation (R2 = 0.97) between the SOA production factor and in-situ particle acidity calculated by AIM-II model. A high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) resolved OA's relatively lower oxygen-to-carbon (O : C) and higher hydrogen-to-carbon (H : C) molar ratios for the GVE/SO2 mixture, with a much lower estimated average carbon oxidation state (OSc) of -0.51 ± 0.06 than that of -0.19 ± 0.08 for GVE alone. The relative higher mass loading of OA in the experiments with SO2 might be the major reason for the lower oxidation degree of SOA.

  8. Formation of secondary aerosols from gasoline vehicle exhaust when mixing with SO2

    NASA Astrophysics Data System (ADS)

    Liu, T.; Wang, X.; Hu, Q.; Deng, W.; Zhang, Y.; Ding, X.; Fu, X.; Bernard, F.; Zhang, Z.; Lü, S.; He, Q.; Bi, X.; Chen, J.; Sun, Y.; Yu, J.; Peng, P.; Sheng, G.; Fu, J.

    2016-01-01

    Sulfur dioxide (SO2) can enhance the formation of secondary aerosols from biogenic volatile organic compounds (VOCs), but its influence on secondary aerosol formation from anthropogenic VOCs, particularly complex mixtures like vehicle exhaust, remains uncertain. Gasoline vehicle exhaust (GVE) and SO2, a typical pollutant from coal burning, are directly co-introduced into a smog chamber, in this study, to investigate the formation of secondary organic aerosols (SOA) and sulfate aerosols through photooxidation. New particle formation was enhanced, while substantial sulfate was formed through the oxidation of SO2 in the presence of high concentration of SO2. Homogenous oxidation by OH radicals contributed a negligible fraction to the conversion of SO2 to sulfate, and instead the oxidation by stabilized Criegee intermediates (sCIs), formed from alkenes in the exhaust reacting with ozone, dominated the conversion of SO2. After 5 h of photochemical aging, GVE's SOA production factor revealed an increase by 60-200 % in the presence of high concentration of SO2. The increase could principally be attributed to acid-catalyzed SOA formation as evidenced by the strong positive linear correlation (R2 = 0.97) between the SOA production factor and in situ particle acidity calculated by the AIM-II model. A high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) resolved OA's relatively lower oxygen-to-carbon (O : C) (0.44 ± 0.02) and higher hydrogen-to-carbon (H : C) (1.40 ± 0.03) molar ratios for the GVE / SO2 mixture, with a significantly lower estimated average carbon oxidation state (OSc) of -0.51 ± 0.06 than -0.19 ± 0.08 for GVE alone. The relative higher mass loading of OA in the experiments with SO2 might be a significant explanation for the lower SOA oxidation degree.

  9. Parallel Simulated Annealing by Mixing of States

    NASA Astrophysics Data System (ADS)

    Chu, King-Wai; Deng, Yuefan; Reinitz, John

    1999-01-01

    We report the results of testing the performance of a new, efficient, and highly general-purpose parallel optimization method, based upon simulated annealing. This optimization algorithm was applied to analyze the network of interacting genes that control embryonic development and other fundamental biological processes. We found several sets of algorithmic parameters that lead to optimal parallel efficiency for up to 100 processors on distributed-memory MIMD architectures. Our strategy contains two major elements. First, we monitor and pool performance statistics obtained simultaneously on all processors. Second, we mix states at intervals to ensure a Boltzmann distribution of energies. The central scientific issue is the inverse problem, the determination of the parameters of a set of nonlinear ordinary differential equations by minimizing the total error between the model behavior and experimental observations.

  10. Multiphase OH oxidation kinetics of organic aerosol: The role of particle phase state and relative humidity

    NASA Astrophysics Data System (ADS)

    Slade, Jonathan H.; Knopf, Daniel A.

    2014-07-01

    Organic aerosol can exhibit different phase states in response to changes in relative humidity (RH), thereby influencing heterogeneous reaction rates with trace gas species. OH radical uptake by laboratory-generated levoglucosan and methyl-nitrocatechol particles, serving as surrogates for biomass burning aerosol, is determined as a function of RH. Increasing RH lowers the viscosity of amorphous levoglucosan aerosol particles enabling enhanced OH uptake. Conversely, OH uptake by methyl-nitrocatechol aerosol particles is suppressed at higher RH as a result of competitive coadsorption of H2O that occupies reactive sites. This is shown to have substantial impacts on organic aerosol lifetimes with respect to OH oxidation. The results emphasize the importance of organic aerosol phase state to accurately describe the multiphase chemical kinetics and thus chemical aging process in atmospheric models to better represent the evolution of organic aerosol and its role in air quality and climate.

  11. Hygroscopicity of internally mixed multi-component aerosol particles of atmospheric relevance

    NASA Astrophysics Data System (ADS)

    Liu, Qifan; Jing, Bo; Peng, Chao; Tong, Shengrui; Wang, Weigang; Ge, Maofa

    2016-01-01

    The hygroscopic properties of two water-soluble organic compounds (WSOCs) relevant to urban haze pollution (phthalic acid and levoglucosan) and their internally mixtures with inorganic salts (ammonium sulfate and ammonium nitrate) are investigated using a hygroscopicity tandem differential mobility analyzer (H-TDMA) system. The multi-component particles uptake water gradually in the range 5-90% relative humidity (RH). The experimental results are compared with the thermodynamic model predictions. For most mixtures, Extended Aerosol Inorganic Model (E-AIM) predictions agree well with the measured growth factors. The hygroscopic growth of mixed particles can be well described by the Zdanovskii-Stokes-Robinson (ZSR) relation as long as the mixed particles are completely liquid. ZSR calculations underestimate the water uptake of mixed particles at moderate RH due to the partial dissolution of ammonium sulfate in the organic and ammonium nitrate solution in this RH region. The phase of ammonium nitrate in the initial dry particles changes dramatically with the composition of mixtures. The presence of organics in the mixed particles can inhibit the crystallization of ammonium nitrate during the drying process and results in water uptake at low RH (RH < 60%). These results demonstrate that certain representative WSOCs can substantially influence the hygroscopicity of inorganic salts and overall water uptake of particles.

  12. Transport and Mixing Patterns over Central California during the Carbonaceous Aerosol and Radiative Effects Study (CARES)

    SciTech Connect

    Fast, Jerome D.; Gustafson, William I.; Berg, Larry K.; Shaw, William J.; Pekour, Mikhail S.; Shrivastava, ManishKumar B.; Barnard, James C.; Ferrare, R.; Hostetler, Chris A.; Hair, John; Erickson, Matthew H.; Jobson, Tom; Flowers, Bradley; Dubey, Manvendra K.; Springston, Stephen R.; Pirce, Bradley R.; Dolislager, Leon; Pederson, J. R.; Zaveri, Rahul A.

    2012-02-17

    We describe the synoptic and regional-scale meteorological conditions that affected the transport and mixing of trace gases and aerosols in the vicinity of Sacramento, California during June 2010 when the Carbonaceous Aerosol and Radiative Effects Study (CARES) was conducted. The meteorological measurements collected by various instruments deployed during the campaign and the performance of the chemistry version of the Weather Research and Forecasting model (WRF-Chem) are both discussed. WRF-Chem was run daily during the campaign to forecast the spatial and temporal variation of carbon monoxide emitted from 20 anthropogenic source regions in California to guide aircraft sampling. The model is shown to reproduce the overall circulations and boundary-layer characteristics in the region, although errors in the upslope wind speed and boundary-layer depth contribute to differences in the observed and simulated carbon monoxide. Thermally-driven upslope flows that transported pollutants from Sacramento over the foothills of the Sierra Nevada occurred every afternoon, except during three periods when the passage of mid-tropospheric troughs disrupted the regional-scales flow patterns. The meteorological conditions after the passage of the third trough were the most favorable for photochemistry and likely formation of secondary organic aerosols. Meteorological measurements and model forecasts indicate that the Sacramento pollutant plume was likely transported over a downwind site that collected trace gas and aerosol measurements during 23 periods; however, direct transport occurred during only eight of these periods. The model also showed that emissions from the San Francisco Bay area transported by intrusions of marine air contributed a large fraction of the carbon monoxide in the vicinity of Sacramento, suggesting that this source likely affects local chemistry. Contributions from other sources of pollutants, such as those in the Sacramento Valley and San Joaquin Valley

  13. Transport and mixing patterns over Central California during the carbonaceous aerosol and radiative effects study (CARES)

    SciTech Connect

    Fast J. D.; Springston S.; Gustafson Jr., W. I.; Berg, L. K.; Shaw, W. J.; Pekour, M.; Shrivastava, M.; Barnard, J. C.; Ferrare, R. A.; Hostetler, C. A.; Hair, J. A.; Erickson, M.; Jobson, B. T.; Flowers, B.; Dubey, M. K.; Pierce, R. B.; Dolislager, L.; Pederson, J.; Zaveri, R. A.

    2012-02-17

    We describe the synoptic and regional-scale meteorological conditions that affected the transport and mixing of trace gases and aerosols in the vicinity of Sacramento, California during June 2010 when the Carbonaceous Aerosol and Radiative Effects Study (CARES) was conducted. The meteorological measurements collected by various instruments deployed during the campaign and the performance of the chemistry version of the Weather Research and Forecasting model (WRF-Chem) are both discussed. WRF-Chem was run daily during the campaign to forecast the spatial and temporal variation of carbon monoxide emitted from 20 anthropogenic source regions in California to guide aircraft sampling. The model is shown to reproduce the overall circulations and boundary-layer characteristics in the region, although errors in the upslope wind speed and boundary-layer depth contribute to differences in the observed and simulated carbon monoxide. Thermally-driven upslope flows that transported pollutants from Sacramento over the foothills of the Sierra Nevada occurred every afternoon, except during three periods when the passage of mid-tropospheric troughs disrupted the regional-scale flow patterns. The meteorological conditions after the passage of the third trough were the most favorable for photochemistry and likely formation of secondary organic aerosols. Meteorological measurements and model forecasts indicate that the Sacramento pollutant plume was likely transported over a downwind site that collected trace gas and aerosol measurements during 23 time periods; however, direct transport occurred during only eight of these periods. The model also showed that emissions from the San Francisco Bay area transported by intrusions of marine air contributed a large fraction of the carbon monoxide in the vicinity of Sacramento, suggesting that this source likely affects local chemistry. Contributions from other sources of pollutants, such as those in the Sacramento Valley and San Joaquin

  14. A smog chamber study coupling a photoionization aerosol electron/ion spectrometer to VUV synchrotron radiation: organic and inorganic-organic mixed aerosol analysis

    NASA Astrophysics Data System (ADS)

    Baeza-Romero, María Teresa; Gaie-Levrel, Francois; Mahjoub, Ahmed; López-Arza, Vicente; Garcia, Gustavo A.; Nahon, Laurent

    2016-07-01

    A reaction chamber was coupled to a photoionization aerosol time-of-flight mass spectrometer based on an electron/ion coincidence scheme and applied for on-line analysis of organic and inorganic-organic mixed aerosols using synchrotron tunable vacuum ultraviolet (VUV) photons as the ionization source. In this proof of principle study, both aerosol and gas phase were detected simultaneously but could be differentiated. Present results and perspectives for improvement for this set-up are shown in the study of ozonolysis ([O3] = 0.13-3 ppm) of α-pinene (2-3 ppm), and the uptake of glyoxal upon ammonium sulphate. In this work the ozone concentration was monitored in real time, together with the particle size distributions and chemical composition, the latter taking advantage of the coincidence spectrometer and the tuneability of the synchrotron radiation as a soft VUV ionization source.

  15. AEROSOL GROWTH IN A STEADY-STATE, CONTINUOUS FLOW CHAMBER: APPLICATION TO STUDIES OF SECONDARY AEROSOL FORMATION

    EPA Science Inventory

    An analytical solution for the steady-state aerosol size distribution achieved in a steady-state, continuous flow chamber is derived, where particle growth is occurring by gas-to-particle conversion and particle loss is occurring by deposition to the walls of the chamber. The s...

  16. Mixed entangled states with two or more common stabilizers

    SciTech Connect

    Hsu, L.-Y.

    2007-08-15

    We investigate a family of mixed entangled states wherein there exist common stabilizers among the mixtures of the corresponding density matrix. The nonlocality of these mixed entangled states can be verified by the maximal violation of stabilizer-based Bell-type inequalities. Some of these states with specific probability distributions are bound entangled, which can be superactivated. Potential applications of these mixed states in quantum key distribution and quantum repeaters are also introduced.

  17. Generalized geometric measure of entanglement for multiparty mixed states

    NASA Astrophysics Data System (ADS)

    Das, Tamoghna; Roy, Sudipto Singha; Bagchi, Shrobona; Misra, Avijit; SenDe, Aditi; Sen, Ujjwal

    2016-08-01

    Computing entanglement of an arbitrary bipartite or multipartite mixed state is in general not an easy task as it usually involves complex optimization. Here we show that, exploiting symmetries of certain multiqudit mixed states, we can compute a genuine multiparty entanglement measure, the generalized geometric measure, for these classes of mixed states. The chosen states have different ranks and consist of an arbitrary number of parties.

  18. Single-particle characterization of biomass burning organic aerosol (BBOA): evidence for non-uniform mixing of high molecular weight organics and potassium

    NASA Astrophysics Data System (ADS)

    Lee, Alex K. Y.; Willis, Megan D.; Healy, Robert M.; Wang, Jon M.; Jeong, Cheol-Heon; Wenger, John C.; Evans, Greg J.; Abbatt, Jonathan P. D.

    2016-05-01

    Biomass burning organic aerosol (BBOA) can be emitted from natural forest fires and human activities such as agricultural burning and domestic energy generation. BBOA is strongly associated with atmospheric brown carbon (BrC) that absorbs near-ultraviolet and visible light, resulting in significant impacts on regional visibility degradation and radiative forcing. The mixing state of BBOA can play a critical role in the prediction of aerosol optical properties. In this work, single-particle measurements from a Soot-Particle Aerosol Mass Spectrometer coupled with a light scattering module (LS-SP-AMS) were performed to examine the mixing state of BBOA, refractory black carbon (rBC), and potassium (K, a tracer for biomass burning aerosol) in an air mass influenced by wildfire emissions transported from northern Québec to Toronto, representing aged biomass burning plumes. Cluster analysis of single-particle measurements identified five BBOA-related particle types. rBC accounted for 3-14 wt % of these particle types on average. Only one particle type exhibited a strong ion signal for K+, with mass spectra characterized by low molecular weight organic species. The remaining four particle types were classified based on the apparent molecular weight of the BBOA constituents. Two particle types were associated with low potassium content and significant amounts of high molecular weight (HMW) organic compounds. Our observations indicate non-uniform mixing of particles within a biomass burning plume in terms of molecular weight and illustrate that HMW BBOA can be a key contributor to low-volatility BrC observed in BBOA particles. The average mass absorption efficiency of low-volatility BBOA is about 0.8-1.1 m2 g-1 based on a theoretical closure calculation. Our estimates indicate that low-volatility BBOA contributes ˜ 33-44 % of thermo-processed particle absorption at 405 nm; and almost all of the BBOA absorption was associated with low-volatility organics.

  19. Development and validation of a black carbon mixing state resolved three-dimensional model: Aging processes and radiative impact

    SciTech Connect

    Matsui, H.; Koike, Makoto; Kondo, Yutaka; Moteki, N.; Fast, Jerome D.; Zaveri, Rahul A.

    2013-03-16

    : A new two-dimensional aerosol bin scheme, which resolves both aerosol size and black carbon (BC) mixing state for BC aging processes (e.g., condensation and coagulation), has been developed and implemented into the WRF-chem model (MS-resolved WRF-chem). The mixing state of BC simulated by this model is compared with direct measurements over the East Asian region in spring 2009. Model simulations generally reproduce the observed features of the BC mixing state, such as the size-dependent number fractions of BC-containing and BC-free particles and the coating thickness of BC-containing particles. Sensitivity simulations show that the condensation process is dominant for the growth of thinly coated BC particles, while the coagulation process is necessary to produce thickly coated BC particles. Off-line optical and radiative calculations assuming an average mixing state for each size bin show that the domain- and period-averaged absorption coefficient and heating rate by aerosols are overestimated by 30 – 40% in the boundary layer compared with a benchmark simulation with the detailed treatment of mixing state. The absolute value of aerosol radiative forcing is also overestimated (10%, 3 W m-2) at the surface. However, these overestimations are reduced considerably when all the parameters (including mass and number concentration) are calculated with the simple treatment of mixing state. This is because the overestimation of radiative parameters due to higher absorption efficiency (compared with the benchmark simulation) is largely canceled by the underestimation of BC concentrations due to efficient wet removal processes. The overall errors in radiative forcing can be much smaller because of this cancellation but for the wrong reasons.

  20. An amorphous solid state of biogenic secondary organic aerosol particles.

    PubMed

    Virtanen, Annele; Joutsensaari, Jorma; Koop, Thomas; Kannosto, Jonna; Yli-Pirilä, Pasi; Leskinen, Jani; Mäkelä, Jyrki M; Holopainen, Jarmo K; Pöschl, Ulrich; Kulmala, Markku; Worsnop, Douglas R; Laaksonen, Ari

    2010-10-14

    Secondary organic aerosol (SOA) particles are formed in the atmosphere from condensable oxidation products of anthropogenic and biogenic volatile organic compounds (VOCs). On a global scale, biogenic VOCs account for about 90% of VOC emissions and of SOA formation (90 billion kilograms of carbon per year). SOA particles can scatter radiation and act as cloud condensation or ice nuclei, and thereby influence the Earth's radiation balance and climate. They consist of a myriad of different compounds with varying physicochemical properties, and little information is available on the phase state of SOA particles. Gas-particle partitioning models usually assume that SOA particles are liquid, but here we present experimental evidence that they can be solid under ambient conditions. We investigated biogenic SOA particles formed from oxidation products of VOCs in plant chamber experiments and in boreal forests within a few hours after atmospheric nucleation events. On the basis of observed particle bouncing in an aerosol impactor and of electron microscopy we conclude that biogenic SOA particles can adopt an amorphous solid-most probably glassy-state. This amorphous solid state should provoke a rethinking of SOA processes because it may influence the partitioning of semi-volatile compounds, reduce the rate of heterogeneous chemical reactions, affect the particles' ability to accommodate water and act as cloud condensation or ice nuclei, and change the atmospheric lifetime of the particles. Thus, the results of this study challenge traditional views of the kinetics and thermodynamics of SOA formation and transformation in the atmosphere and their implications for air quality and climate.

  1. An amorphous solid state of biogenic secondary organic aerosol particles.

    PubMed

    Virtanen, Annele; Joutsensaari, Jorma; Koop, Thomas; Kannosto, Jonna; Yli-Pirilä, Pasi; Leskinen, Jani; Mäkelä, Jyrki M; Holopainen, Jarmo K; Pöschl, Ulrich; Kulmala, Markku; Worsnop, Douglas R; Laaksonen, Ari

    2010-10-14

    Secondary organic aerosol (SOA) particles are formed in the atmosphere from condensable oxidation products of anthropogenic and biogenic volatile organic compounds (VOCs). On a global scale, biogenic VOCs account for about 90% of VOC emissions and of SOA formation (90 billion kilograms of carbon per year). SOA particles can scatter radiation and act as cloud condensation or ice nuclei, and thereby influence the Earth's radiation balance and climate. They consist of a myriad of different compounds with varying physicochemical properties, and little information is available on the phase state of SOA particles. Gas-particle partitioning models usually assume that SOA particles are liquid, but here we present experimental evidence that they can be solid under ambient conditions. We investigated biogenic SOA particles formed from oxidation products of VOCs in plant chamber experiments and in boreal forests within a few hours after atmospheric nucleation events. On the basis of observed particle bouncing in an aerosol impactor and of electron microscopy we conclude that biogenic SOA particles can adopt an amorphous solid-most probably glassy-state. This amorphous solid state should provoke a rethinking of SOA processes because it may influence the partitioning of semi-volatile compounds, reduce the rate of heterogeneous chemical reactions, affect the particles' ability to accommodate water and act as cloud condensation or ice nuclei, and change the atmospheric lifetime of the particles. Thus, the results of this study challenge traditional views of the kinetics and thermodynamics of SOA formation and transformation in the atmosphere and their implications for air quality and climate. PMID:20944744

  2. Vertical profiles of cloud condensation nuclei, aerosol hygroscopicity, water uptake, and scattering across the United States

    NASA Astrophysics Data System (ADS)

    Lin, J. J.; Bougiatioti, A.; Nenes, A.; Anderson, B. E.; Beyersdorf, A. J.; Brock, C. A.; Gordon, T. D.; Lack, D.; Law, D. C.; Liao, J.; Middlebrook, A. M.; Richardson, M.; Thornhill, K. L., II; Winstead, E.; Wagner, N. L.; Welti, A.; Ziemba, L. D.

    2014-12-01

    The evolutions of vertical distributions of aerosol chemical, microphysical, hygroscopic, and optical properties present fundamental challenges to the understanding of ground-level air quality and radiative transfer, and few datasets exist to date for evaluation of atmospheric models. Data collected from recent NASA and NOAA field campaigns in the California Central Valley (DISCOVER-AQ), southeast United States (SENEX, SEAC4RS) and Texas (DISCOVER-AQ) allow for a unique opportunity to constrain vertical profiles of climate-relevant aerosol properties. This work presents in-situ aircraft measurements of cloud condensation nuclei (CCN) concentration and derivations of aerosol hygroscopicity, water uptake, and light scattering. Aerosol hygroscopicity is derived from CCN and aerosol measurements. Inorganic water uptake is calculated from aerosol composition using ISORROPIA, a chemical thermodynamic model, while organic water uptake is calculated from organic hygroscopicity. Aerosol scattering closure is performed between scattering from water uptake calculations and in-situ scattering measurements.

  3. State transformations and ice nucleation in amorphous (semi-)solid organic aerosol

    NASA Astrophysics Data System (ADS)

    Baustian, K. J.; Wise, M. E.; Jensen, E. J.; Schill, G. P.; Freedman, M. A.; Tolbert, M. A.

    2013-06-01

    Amorphous (semi-)solid organic aerosol particles have the potential to serve as surfaces for heterogeneous ice nucleation in cirrus clouds. Raman spectroscopy and optical microscopy have been used in conjunction with a cold stage to examine water uptake and ice nucleation on individual amorphous (semi-)solid particles at atmospherically relevant temperatures (200-273 K). Three organic compounds considered proxies for atmospheric secondary organic aerosol (SOA) were used in this investigation: sucrose, citric acid and glucose. Internally mixed particles consisting of each organic and ammonium sulfate were also investigated. Results from water uptake experiments followed the shape of a humidity-induced glass transition (Tg(RH)) curve and were used to construct state diagrams for each organic and corresponding mixture. Experimentally derived Tg(RH) curves are in good agreement with theoretical predictions of Tg(RH) following the approach of Koop et al. (2011). A unique humidity-induced glass transition point on each state diagram, Tg'(RH), was used to quantify and compare results from this study to previous works. Values of Tg'(RH) determined for sucrose, glucose and citric acid glasses were 236, 230 and 220 K, respectively. Values of Tg'(RH) for internally mixed organic/sulfate particles were always significantly lower; 210, 207 and 215 K for sucrose/sulfate, glucose/sulfate and citric acid/sulfate, respectively. All investigated SOA proxies were observed to act as heterogeneous ice nuclei at tropospheric temperatures. Heterogeneous ice nucleation on pure organic particles occurred at Sice = 1.1-1.4 for temperatures below 235 K. Particles consisting of 1:1 organic-sulfate mixtures took up water over a greater range of conditions but were in some cases also observed to heterogeneously nucleate ice at temperatures below 202 K (Sice= 1.25-1.38). Polynomial curves were fitted to experimental water uptake data and then incorporated into the Community Aerosol Radiation

  4. Sensitive and direct determination of lithium by mixed-mode chromatography and charged aerosol detection.

    PubMed

    Dai, Lulu; Wigman, Larry; Zhang, Kelly

    2015-08-21

    A sensitive analytical method using mixed mode HPLC separation coupled with charged aerosol detection (CAD) was developed for quantitative analysis of lithium. The method is capable of separating lithium ion from different drug matrices and other ions in a single run thus eliminating the organic matrix and ionic analyte interferences without extensive sample preparation such as derivatization and extraction. The separation space and chromatographic conditions are defined by systematic studies of the retention behaviors of lithium and potential interfering ions and different type of pharmaceutical APIs (active pharmaceutical ingredients) under reversed-phase, HILIC and cation/anion exchange mechanisms. Compared to other current analytical techniques for lithium analysis, the presented method provides a new approach and demonstrates high sensitivity (0.02ng for LOD and 0.08ng for LOQ in both standard and sample solution). The method has been validated for pharmaceutical samples and can be potentially applied to biological, food and environmental samples.

  5. Detection of internally mixed Asian dust with air pollution aerosols using a polarization optical particle counter and a polarization-sensitive two-wavelength lidar

    NASA Astrophysics Data System (ADS)

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

    2015-01-01

    East Asia is a unique region where mineral dust (Asian dust) sources are located near urban and industrial areas. Asian dust is often mixed with air pollution aerosols during transportation. It is important to understand the mixing states of Asian dust and other aerosols, because the effects on the environment and human health differ depending on the mixing state. We studied the mixing states of Asian dust using a polarization particle counter (POPC) that measures the forward scattering and the two polarization components of backscattering for single particles and a polarization-sensitive (532 nm) two-wavelength (1064 nm and 532 nm) lidar. We conducted the simultaneous observations using the POPC and the lidar in Seoul from March to December 2013 and captured the characteristics of pure Asian dust and internally mixed polluted Asian dust. POPC measurements indicated that the density of large particles was lower in polluted Asian dust that transported slowly over the polluted areas than in pure Asian dust that transported quickly from the dust source region. Moreover, the backscattering depolarization ratio was smaller for all particle sizes in polluted dust. The optical characteristics measured using the lidar were consistent with the POPC measurements. The backscattering color ratio of polluted dust was comparable to that of pure dust, but the depolarization ratio was lower for polluted dust. In addition, coarse non-spherical particles (Asian dust) almost always existed in the background, and the depolarization ratio had seasonal variation with a lower depolarization ratio in the summer. These results suggest background Asian dust particles are internally mixed in the summer.

  6. Vertical Structure, Transport, and Mixing of Ozone and Aerosols Observed During NEAQS/ICARTT 2004

    NASA Astrophysics Data System (ADS)

    Senff, C. J.; Hardesty, R. M.; Brewer, W. A.; Alvarez, R. J.; Sandberg, S. P.; Tucker, S. C.; Intrieri, J. M.; Marchbanks, R. D.; McCarty, B. J.; Banta, R. M.; Darby, L. S.; White, A. B.

    2005-12-01

    During the 2004 New England Air Quality Study (NEAQS), which was conducted within the framework of the International Consortium for Atmospheric Research on Transport and Transformation (ICARTT) field experiment, airborne and shipborne lidar remote sensing instruments were deployed to characterize the 3-dimensional structure of ozone, aerosol, and low-level wind fields in the New England region. The 2004 measurements confirmed findings from the smaller-scale NEAQS 2002 experiment: the vertical structure and transport patterns of pollutant plumes from the Boston and New York City urban areas are strongly modified when they are advected over the Gulf of Maine. Because of strong vertical wind shear and a very stable atmosphere over the cold ocean water the plumes tend to get sheared apart and the resulting pieces of the plumes stay confined in layers aloft, isolated from the surface. Most notably, ozone concentrations aloft are very often significantly higher than ozone levels near the ocean surface. These elevated pollution plumes over the Gulf of Maine can affect air quality in coastal New England only when they are transported back over land. This can be accomplished by the large-scale flow or by local circulations such as the sea breeze. Once over land the elevated plumes may impact surface air quality by direct transport to higher terrain (e.g., Cadillac Mountain, ME) or by being fumigated down to the surface. Alternatively, but probably more rarely, an elevated pollution plume over the ocean may be mixed down to the surface by mechanically generated turbulence and then transported back to land within the marine boundary layer. We will use airborne and shipborne lidar remote sensing data to characterize the vertical distribution of ozone and aerosols over coastal New England, in particular the difference in plume structure over land and water. We will also show observational evidence for several of the processes described above that may mix down and transport

  7. Aerosol lidar observations of atmospheric mixing in Los Angeles: Climatology and implications for greenhouse gas observations

    NASA Astrophysics Data System (ADS)

    Ware, John; Kort, Eric A.; DeCola, Phil; Duren, Riley

    2016-08-01

    Atmospheric observations of greenhouse gases provide essential information on sources and sinks of these key atmospheric constituents. To quantify fluxes from atmospheric observations, representation of transport—especially vertical mixing—is a necessity and often a source of error. We report on remotely sensed profiles of vertical aerosol distribution taken over a 2 year period in Pasadena, California. Using an automated analysis system, we estimate daytime mixing layer depth, achieving high confidence in the afternoon maximum on 51% of days with profiles from a Sigma Space Mini Micropulse LiDAR (MiniMPL) and on 36% of days with a Vaisala CL51 ceilometer. We note that considering ceilometer data on a logarithmic scale, a standard method, introduces, an offset in mixing height retrievals. The mean afternoon maximum mixing height is 770 m Above Ground Level in summer and 670 m in winter, with significant day-to-day variance (within season σ = 220m≈30%). Taking advantage of the MiniMPL's portability, we demonstrate the feasibility of measuring the detailed horizontal structure of the mixing layer by automobile. We compare our observations to planetary boundary layer (PBL) heights from sonde launches, North American regional reanalysis (NARR), and a custom Weather Research and Forecasting (WRF) model developed for greenhouse gas (GHG) monitoring in Los Angeles. NARR and WRF PBL heights at Pasadena are both systematically higher than measured, NARR by 2.5 times; these biases will cause proportional errors in GHG flux estimates using modeled transport. We discuss how sustained lidar observations can be used to reduce flux inversion error by selecting suitable analysis periods, calibrating models, or characterizing bias for correction in post processing.

  8. Impact of transpacific aerosol on air quality over the United States: A perspective from aerosol-cloud-radiation interactions

    NASA Astrophysics Data System (ADS)

    Tao, Zhining; Yu, Hongbin; Chin, Mian

    2016-01-01

    Observations have well established that aerosols from various sources in Asia, Europe, and Africa can travel across the Pacific and reach the contiguous United States (U.S.) at least on episodic bases throughout a year, with a maximum import in spring. The imported aerosol not only can serve as an additional source to regional air pollution (e.g., direct input), but also can influence regional air quality through the aerosol-cloud-radiation (ACR) interactions that change local and regional meteorology. This study assessed impacts of the transpacific aerosol on air quality, focusing on surface ozone and PM2.5, over the U.S. using the NASA Unified Weather Research Forecast model. Based on the results of 3-month (April to June of 2010) simulations, the impact of direct input (as an additional source) of transpacific aerosol caused an increase of surface PM2.5 concentration by approximately 1.5 μg m-3 over the west coast and about 0.5 μg m-3 over the east coast of the U.S. By influencing key meteorological processes through the ACR interactions, the transpacific aerosol exerted a significant effect on both surface PM2.5 (±6 μg m-3) and ozone (±12 ppbv) over the central and eastern U.S. This suggests that the transpacific transport of aerosol could either improve or deteriorate local air quality and complicate local effort toward the compliance with the U.S. National Ambient Air Quality Standards.

  9. Estimated SAGE II ozone mixing ratios in early 1993 and comparisons with Stratospheric Photochemistry, Aerosols and Dynamic Expedition measurements

    NASA Technical Reports Server (NTRS)

    Yue, G. K.; Veiga, R. E.; Poole, L. R.; Zawodny, J. M.; Proffitt, M. H.

    1994-01-01

    An empirical time-series model for estimating ozone mixing ratios based on Stratospheric Aerosols and Gas Experiment II (SAGE II) monthly mean ozone data for the period October 1984 through June 1991 has been developed. The modeling results for ozone mixing ratios in the 10- to 30- km region in early months of 1993 are presented. In situ ozone profiles obtained by a dual-beam UV-absorption ozone photometer during the Stratospheric Photochemistry, Aerosols and Dynamics Expedition (SPADE) campaign, May 1-14, 1993, are compared with the model results. With the exception of two profiles at altitudes below 16 km, ozone mixing ratios derived by the model and measured by the ozone photometer are in relatively good agreement within their individual uncertainties. The identified discrepancies in the two profiles are discussed.

  10. Origin and development of concepts of bipolar mixed states.

    PubMed

    Marneros, A

    2001-12-01

    This paper reviews the historical origins of the contemporaneous resurgence of interest in mixed states. This is a classical concept whose origins can be traced back to ancient times. In more modern times, already in the pre-Kraepelinian era we can find descriptions and classifications of "mixed states". For example, in his classification of mental disorders described "mixtures of exaltations and depression", and he distinguished among "mixed mood disorders", "mixed mental disorders", and "mixed volition disorders". Subsequently, (the father of empirical and biological psychiatric research in Germany) described the "mid-forms". Half a century later we encounter the crucial role of Emil Kraepelin and the development and systemization of his views between 1899 and 1913--leading to the characterization of such conditions as "depressive-anxious mania", "excited depression", and "stuporous mania". The remainder of this article focuses on the essential points of the first book on mixed states in the psychiatric literature: On The Mixed States of Manic-Depressive Insanity by. For much of the present 20th century nothing new emerges, followed by a contemporary renaissance of mixed states, particularly in the United States. The paper concludes with proposal of mixed states as temperament intruding into an episode of opposite polarity.

  11. Influence of the vertical absorption profile of mixed Asian dust plumes on aerosol direct radiative forcing over East Asia

    NASA Astrophysics Data System (ADS)

    Noh, Young Min; Lee, Kwonho; Kim, Kwanchul; Shin, Sung-Kyun; Müller, Detlef; Shin, Dong Ho

    2016-08-01

    We estimate the aerosol direct radiative forcing (ADRF) and heating rate profiles of mixed East Asian dust plumes in the solar wavelength region ranging from 0.25 to 4.0 μm using the Santa Barbara Discrete Ordinate Atmospheric Radiative Transfer (SBDART) code. Vertical profiles of aerosol extinction coefficients and single-scattering albedos (SSA) were derived from measurements with a multi-wavelength Raman lidar system. The data are used as input parameters for our radiative transfer calculations. We considered four cases of radiative forcing in SBDART: 1. dust, 2. pollution, 3. mixed dust plume and the use of vertical profiles of SSA, and 4. mixed dust plumes and the use of column-averaged values of SSA. In our sensitivity study we examined the influence of SSA and aerosol layer height on our results. The ADRF at the surface and in the atmosphere shows a small dependence on the specific shape of the aerosol extinction vertical profile and its light-absorption property for all four cases. In contrast, at the top of the atmosphere (TOA), the ADRF is largely affected by the vertical distribution of the aerosols extinction. This effect increases if the light-absorption capacity (decrease of SSA) of the aerosols increases. We find different radiative effects in situations in which two layers of aerosols had different light-absorption properties. The largest difference was observed at the TOA for an absorbing aerosol layer at high altitude in which we considered in one case the vertical profile of SSA and in another case the column-averaged SSA only. The ADRF at the TOA increases when the light-absorbing aerosol layer is located above 3 km altitude. The differences between height-resolved SSA, which can be obtained from lidar data, and total layer-mean SSA indicates that the use of a layer-mean SSA can be rather misleading as it can induce a large error in the calculation of the ADRF at the TOA, which in turn may cause errors in the vertical profiles of heating rates.

  12. Entangled State Representation for Four-Wave Mixing

    NASA Astrophysics Data System (ADS)

    Ma, Shan-Jun; Lu, Hai-Liang; Fan, Hong-Yi

    2008-08-01

    We introduce the entangled state representation to describe the four-wave mixing. We find that the four-wave mixing operator, which engenders the correct input-output field transformation, has a natural representation in the entangled state representation. In this way, we see that the four-wave mixing process not only involves squeezing but also is an entanglement process. This analysis brings convenience to the calculation of quadrature-amplitude measurement for the output state of four-wave mixing process.

  13. A high-resolution study of surfactant partitioning and kinetic limitations for two-component internally mixed aerosols

    NASA Astrophysics Data System (ADS)

    Suda, S. R.; Petters, M. D.

    2013-12-01

    Atmospheric aerosols serve as cloud condensation nuclei (CCN), altering cloud properties and ultimately affecting climate through their effect on the radiative balance. Aerosol CCN activity depends in part on aerosol composition and surfactant compounds are of particular interest because surfactants are enriched at the water/air interface, resulting in a radial concentration gradient within the aqueous droplet. Accurate treatment of the surfactant concentration gradient complicates the otherwise straightforward predictions of CCN activity for aerosols of known composition. To accurately evaluate predictions made by theory, laboratory studies investigating the relationship between critical supersaturation and dry diameter of particles that include surfactants require significant reduction in measurement uncertainty for both water-uptake and CCN measurements. Furthermore, uncertainties remain regarding kinetic limitations to surfactant partitioning that could result in deviation from predictions based on equilibrium thermodynamics. This study attempts to address some of these issues through high-resolution analysis of CCN activity of two-component mixed surfactant/non-surfactant aerosols at different internal mixing ratios performed with and without a water-uptake time delay to ascertain whether or not the observed effects are kinetically limited. We present new data for the aerosols consisting of 1) the ionic surfactant sodium dodecyl sulfate (SDS) with ammonium sulfate, 2) SDS with sodium chloride and 3) the strong non-ionic fluorosurfactant Zonyl with an organic proxy glucose. As a point of reference we also evaluated the mixture of ammonium sulfate with glucose. Aerosol activation diameters were determined using CCN analysis in conjunction with scanning mobility size classification and high sheath-to-aerosol flow ratios. This resulted in CCN-derived kappa values that could be determined within +/-5% relative error. To test whether dynamic surfactant partitioning

  14. A method to resolve the phase state of aerosol particles

    NASA Astrophysics Data System (ADS)

    Saukko, E.; Kuuluvainen, H.; Virtanen, A.

    2012-01-01

    The phase state of atmospheric aerosols has an impact on their chemical aging and their deliquescence and thus their ability to act as cloud condensation nuclei (CCN). The phase change of particles can be induced by the deliquescence or efflorescence of water or by chemical aging. Existing methods, such as tandem differential mobility analysis rely on the size change of particles related to the water uptake or release. To address the need to study the phase change induced by mass-preserving and nearly mass-preserving processes a new method has been developed. The method relies on the physical impaction of particles on a smooth substrate and subsequent counting of bounced particles by a condensation particle counter (CPC). The connection between the bounce probability and physical properties of particles is so far qualitative. To evaluate the performance of this method, the phase state of ammonium sulfate and levoglucosan, crystalline and amorphous solid, in the presence of water vapor was studied. The results show a marked difference in particle bouncing properties between substances - not only at the critical relative humidity level, but also on the slope of the bouncing probability with respect to humidity. This suggests that the method can be used to differentiate between amorphous and crystalline substances as well as to differentiate between liquid and solid phases.

  15. A method to resolve the phase state of aerosol particles

    NASA Astrophysics Data System (ADS)

    Saukko, E.; Kuuluvainen, H.; Virtanen, A.

    2011-10-01

    The phase state of atmospheric aerosols has impact on their chemical aging and their deliquescence and thus their ability to act as cloud condensation nuclei (CCN). The phase change of particles can be induced by the deliquescence or efflorescence of water or by chemical aging. Existing methods, such as tandem differential mobility analysis rely on the size change of particles related to the water uptake or release related to deliquescence and efflorescence. To address the need to study the phase change induced by mass-preserving and nearly mass-preserving processes a new method has been developed. The method relies on the physical impaction of particles on a smooth substrate and subsequent counting of bounced particles by condensation particle counter (CPC). The connection between the bounce probability and physical properties of particles is so far qualitative. To evaluate the performance of this method, the phase state of ammonium sulfate and levoglucosan, crystalline and amorphous solid, in the presence of water vapor was studied. The results show a marked difference in particle bouncing properties between substances - not only at the critical relative humidity level, but also on the slope of the bouncing probability with respect to humidity. This suggests that the method can be used to differentiate between amorphous and crystalline substances as well as to differentiate between liquid and solid phases.

  16. Maximal entanglement versus entropy for mixed quantum states

    SciTech Connect

    Wei, T.-C.; Goldbart, Paul M.; Kwiat, Paul G.; Nemoto, Kae; Munro, William J.; Verstraete, Frank

    2003-02-01

    Maximally entangled mixed states are those states that, for a given mixedness, achieve the greatest possible entanglement. For two-qubit systems and for various combinations of entanglement and mixedness measures, the form of the corresponding maximally entangled mixed states is determined primarily analytically. As measures of entanglement, we consider entanglement of formation, relative entropy of entanglement, and negativity; as measures of mixedness, we consider linear and von Neumann entropies. We show that the forms of the maximally entangled mixed states can vary with the combination of (entanglement and mixedness) measures chosen. Moreover, for certain combinations, the forms of the maximally entangled mixed states can change discontinuously at a specific value of the entropy. Along the way, we determine the states that, for a given value of entropy, achieve maximal violation of Bell's inequality.

  17. Water uptake by organic aerosol and its influence on gas/particle partitioning of secondary organic aerosol in the United States

    NASA Astrophysics Data System (ADS)

    Jathar, Shantanu H.; Mahmud, Abdullah; Barsanti, Kelley C.; Asher, William E.; Pankow, James F.; Kleeman, Michael J.

    2016-03-01

    Organic aerosol (OA) is at least partly hygroscopic, i.e., water partitions into the organic phase to a degree determined by the relative humidity (RH), the organic chemical composition, and the particle size. This organic-phase water increases the aerosol mass and provides a larger absorbing matrix while decreasing its mean molecular weight, which can encourage additional condensation of semi-volatile organic compounds. Most regional and global atmospheric models account for water uptake by inorganic salts but do not explicitly account for organic-phase water and its subsequent impact on gas/particle partitioning of semi-volatile OA. In this work, we incorporated the organic-phase water model described by Pankow et al. (2015) into the UCD/CIT air quality model to simulate water uptake by OA and assessed its influence on total OA mass concentrations. The model was run for one summer month over two distinct regions: South Coast Air Basin (SoCAB) surrounding Los Angeles, California and the eastern United States (US). In SoCAB where the OA was dominated by non-hygroscopic primary OA (POA), there was very little organic-phase water uptake (0.1-0.2 μg m-3) and consequently very little enhancement (or growth) in total OA concentrations (OA + organic-phase water): a 3% increase in total OA mass was predicted for a 0.1 increase in relative humidity. In contrast, in the eastern US where secondary OA (SOA) from biogenic sources dominated the OA, substantial organic-phase water uptake and enhancement in total OA concentrations was predicted, even in urban locations. On average, the model predicted a 20% growth in total OA mass for a 0.1 increase in relative humidity; the growth was equivalent to a 250 nm particle with a hygroscopicity parameter (κ) of 0.15. Further, for the same relative humidity, the exact extent of organic-phase water uptake and total OA enhancement was found to be dependent on the particle mixing state. When the source-oriented mixing state of aerosols

  18. Reconciling Organic Aerosol Volatility, Hygroscopicity, and Oxidation State During the Colorado DISCOVER-AQ Deployment

    NASA Astrophysics Data System (ADS)

    Hite, J. R.; Moore, R.; Martin, R.; Thornhill, K. L., II; Winstead, E.; Anderson, B. E.; Nenes, A.

    2014-12-01

    The organic fraction of submicron aerosol can profoundly impact radiative forcing on climate directly, through enhancement of extinction, or indirectly through modulation of cloud formation. Semi-volatile constituents of organic ambient aerosol are of particular interest as their partitioning between the vapor and aerosol phases is not well constrained by current atmospheric models and appears to play an important role in the formation of cloud condensation nuclei (CCN) as suggested by recent research. An experimental setup consisting of a DMT CCN counter and SMPS downstream of a custom-built thermodenuder assembly was deployed during the summer 2014 DISCOVER-AQ field campaign to retrieve simultaneous, size-resolved volatility and hygroscopicity - through the use of scanning mobility CCN analysis (SMCA). Housed in the NASA Langley mobile laboratory, a suite of complimentary measurements were made available onboard including submicron aerosol composition and oxidation state provided by an HR-ToF-AMS, and aerosol optical properties provided by a range of other instruments including an SP2. Air masses sampled from locations across the Central Colorado region include influences from regional aerosol nucleation/growth events, long-range transport of Canadian biomass burning aerosols, cattle feedlot emissions and influences of the Denver urban plume - amidst a backdrop of widespread oil and gas exploration. The analysis focuses on the reconciliation of the retrieved aerosol volatility distributions and corresponding hygroscopicity and oxidation state observations, including the use of AMS factor analysis.

  19. Thermomagnetic phenomena in the mixed state of high temperature superconductors

    NASA Technical Reports Server (NTRS)

    Meilikhov, E. Z.

    1995-01-01

    Galvano- and thermomagnetic-phenomena in high temperature superconductors, based on kinetic coefficients, are discussed, along with a connection between the electric field and the heat flow in superconductor mixed state. The relationship that determines the transport coefficients of high temperature superconductors in the mixed state based on Seebeck and Nernst effects is developed. It is shown that this relationship is true for a whole transition region of the resistive mixed state of a superconductor. Peltier, Ettingshausen and Righi-Leduc effects associated with heat conductivity as related to high temperature superconductors are also addressed.

  20. Multidecadal solar radiation trends in the United States and Germany and direct tropospheric aerosol forcing

    NASA Astrophysics Data System (ADS)

    Liepert, Beate; Tegen, Ina

    2002-06-01

    In recent studies, anthropogenic aerosols have been recognized as important radiative forcing factors of climate because of their ability to scatter and/or absorb sunlight. At clear-sky conditions the direct aerosol forcing at ground is negative and implies less solar heating of the surface because of aerosols. In this study, an intensified direct aerosol forcing of -7 to -8 W/m2 has been detected in the United States for the interval from 1960 to 1990. In Germany a weakened aerosol forcing of +3 W/m2 was observed during the same time period. Even though the aerosol forcing is stronger in the eastern United States compared to the western United States, the positive trend is almost equal. We attained these results by scrutinizing clear-sky global solar radiation recordings for these regions and this time period. Additionally, the diurnal cycle and the direct to diffuse ratio of solar radiation were used for constraining the observed trends. Increased absorption and declined light scattering are presumably responsible for the intensified direct aerosol forcing in the United States. While at the same time in Germany, both aerosol absorption and scattering must have declined to explain the parallel weakened aerosol forcing and the increased direct/diffuse ratio. To estimate the possible anthropogenic portion of these observed changes, we compared the observational results with modeled aerosol forcing scenarios retrieved from the Goddard Institute for Space Studies general circulation model (GISS GCM). Modeled surface solar radiation, aerosol optical thickness, and single-scattering albedo are derived from emission trends of anthropogenic sulfate and carbonaceous aerosols. The emission distributions are calculated from fossil fuel consumption databases. On the basis of these simulations we suspect that the declining trend of sulfate burden over Germany between 1960 and 1990 was stronger than estimated with the model. Over the United States the simulated small increase

  1. Optical Properties of Mixed Black Carbon, Inorganic and Secondary Organic Aerosols

    SciTech Connect

    Paulson, S E

    2012-05-30

    Summarizes the achievements of the project, which are divided into four areas: 1) Optical properties of secondary organic aerosols; 2) Development and of a polar nephelometer to measure aerosol optical properties and theoretical approaches to several optical analysis problems, 3) Studies on the accuracy of measurements of absorbing carbon by several methods, and 4) Environmental impacts of biodiesel.

  2. The Sensitivity of Multiangle Imaging to Natural Mixes of Aerosols Over Ocean

    NASA Technical Reports Server (NTRS)

    Kahn, R.; Banerjee, P.; McDonald, D.

    1999-01-01

    Multiangle, multispectral remote sensing observations, such as those anticipated from the Earth Observing System (EOS) Multi-angle Imaging SpectroRadiomenter (MISR), can significantly improve our ability to constrain aerosol properties based on a generic retrieval approach; top-of-atmosphere radiances were interpreted in terms of a single, average aerosol population having unimodal size distribution and uniform composition.

  3. Optimal teleportation with a mixed state of two qubits.

    PubMed

    Verstraete, Frank; Verschelde, Henri

    2003-03-01

    We consider a single copy of a mixed state of two qubits and derive the optimal trace-preserving local operations assisted by classical communication such as to maximize the fidelity of teleportation that can be achieved with this state. These optimal local operations turn out to be implementable by one-way communication and always yield a teleportation fidelity larger than 2/3 if the original state is entangled. This maximal achievable fidelity is an entanglement measure and turns out quantifying the minimal amount of mixing required to destroy the entanglement in a quantum state.

  4. Tropospheric Vertical Profiles of Aerosol Optical, Microphysical and Concentration Properties in the Frame of the Hygra-CD Campaign (Athens, Greece 2014): A Case Study of Long-Range Transport of Mixed Aerosols

    NASA Astrophysics Data System (ADS)

    Papayannis, Alexandros; Argyrouli, Athina; Müller, Detlef; Tsaknakis, Georgios; Kokkalis, Panayotis; Binietoglou, Ioannis; Kazadzis, Stelios; Solomos, Stavros; Amiridis, Vassilis

    2016-06-01

    Combined multi-wavelength aerosol Raman lidar and sun photometry measurements were performed during the HYGRA-CD campaign over Athens, Greece during May-June 2014. The retrieved aerosol optical properties (3 aerosol backscatter at 355-532-1064 nm and 2 aerosol extinction profiles at 355-532 nm) were used as input to an inversion code to retrieve the aerosol microphysical properties (effective radius reff and number concentration N) using regularization techniques. Additionally, the volume concentration profile was derived for fine particles using the LIRIC code. In this paper we selected a complex case study of long-range transport of mixed aerosols (biomass burning particles mixed with dust) arriving over Athens between 10-12 June 2014 in the 1.5-4 km height. Between 2-3 km height we measured mean lidar ratios (LR) ranging from 45 to 58 sr (at 355 and 532 nm), while the Ångström exponent (AE) aerosol extinction-related values (355nm/532nm) ranged between 0.8-1.3. The retrieved values of reff and N ranged from 0.19±0.07 to 0.22±0.07 μm and 460±230 to 2200±2800 cm-3, respectively. The aerosol linear depolarization ratio (δ) at 532 nm was lower than 5-7% (except for the Saharan dust cases, where δ~10-15%).

  5. Faithful Transfer Arbitrary Pure States with Mixed Resources

    NASA Astrophysics Data System (ADS)

    Luo, Ming-Xing; Li, Lin; Ma, Song-Ya; Chen, Xiu-Bo; Yang, Yi-Xian

    2013-09-01

    In this paper, we show that some special mixed quantum resource experience the same property of pure entanglement such as Bell state for quantum teleportation. It is shown that one mixed state and three bits of classical communication cost can be used to teleport one unknown qubit compared with two bits via pure resources. The schemes are easily implement with model physical techniques. Moreover, these resources are also optimal and typical for faithfully remotely prepare an arbitrary qubit, two-qubit and three-qubit states with mixed quantum resources. Our schemes are completed as same as those with pure quantum entanglement resources except only 1 bit additional classical communication cost required. The success probability is independent of the form of the mixed resources.

  6. Long-range transport and mixing of aerosol sources during the 2013 North American biomass burning episode: analysis of multiple lidar observations in the western Mediterranean basin

    NASA Astrophysics Data System (ADS)

    Ancellet, Gerard; Pelon, Jacques; Totems, Julien; Chazette, Patrick; Bazureau, Ariane; Sicard, Michaël; Di Iorio, Tatiana; Dulac, Francois; Mallet, Marc

    2016-04-01

    Long-range transport of biomass burning (BB) aerosols between North America and the Mediterranean region took place in June 2013. A large number of ground-based and airborne lidar measurements were deployed in the western Mediterranean during the Chemistry-AeRosol Mediterranean EXperiment (ChArMEx) intensive observation period. A detailed analysis of the potential North American aerosol sources is conducted including the assessment of their transport to Europe using forward simulations of the FLEXPART Lagrangian particle dispersion model initialized using satellite observations by MODIS and CALIOP. The three-dimensional structure of the aerosol distribution in the ChArMEx domain observed by the ground-based lidars (Minorca, Barcelona and Lampedusa), a Falcon-20 aircraft flight and three CALIOP tracks, agrees very well with the model simulation of the three major sources considered in this work: Canadian and Colorado fires, a dust storm from western US and the contribution of Saharan dust streamers advected from the North Atlantic trade wind region into the westerlies region. Four aerosol types were identified using the optical properties of the observed aerosol layers (aerosol depolarization ratio, lidar ratio) and the transport model analysis of the contribution of each aerosol source: (i) pure BB layer, (ii) weakly dusty BB, (iii) significant mixture of BB and dust transported from the trade wind region, and (iv) the outflow of Saharan dust by the subtropical jet and not mixed with BB aerosol. The contribution of the Canadian fires is the major aerosol source during this episode while mixing of dust and BB is only significant at an altitude above 5 km. The mixing corresponds to a 20-30 % dust contribution in the total aerosol backscatter. The comparison with the MODIS aerosol optical depth horizontal distribution during this episode over the western Mediterranean Sea shows that the Canadian fire contributions were as large as the direct northward dust outflow

  7. Nonlocality in pure and mixed n-qubit X states

    NASA Astrophysics Data System (ADS)

    Batle, J.; Ooi, C. H. Raymond; Farouk, Ahmed; Abdalla, S.

    2016-04-01

    Nonlocality for general multiqubit X states is studied in detail. Pure and mixed states are analyzed as far as their maximum amount of nonlocality is concerned, and analytic results are obtained for important families of these states. The particular form of nonzero diagonal and antidiagonal matrix elements makes the corresponding study easy enough to obtain exact results. We also provide a numerical recipe to randomly generate an important family of X states endowed with a given degree of mixture.

  8. Investigations of boundary layer structure, cloud characteristics and vertical mixing of aerosols at Barbados with large eddy simulations

    NASA Astrophysics Data System (ADS)

    Jähn, Michael; Muñoz-Esparza, Domingo; Chouza, Fernando; Reitebuch, Oliver; Knoth, Oswald; Haarig, Moritz; Ansmann, Albert; Tegen, Ina

    2016-04-01

    Large eddy simulations (LESs) with ASAM (All Scale Atmospheric Model) are performed for the area of the Caribbean island Barbados to investigate island effects on boundary layer modification, cloud generation and vertical mixing of aerosols. In order to generate inflow turbulence consistent with the upstream marine boundary layer forcing, we use the cell perturbation method based on finite amplitude potential temperature perturbations. This method is now also validated for moist boundary layer simulations with open lateral boundary conditions. Observational data obtained from the SALTRACE (Saharan Aerosol Long-range Transport and Aerosol-Cloud-Interaction Experiment) field campaign is used for both model initialization and comparisons. Several sensitivity tests are carried out to demonstrate the problems related to "gray zone modeling" or when the turbulent marine boundary layer flow is replaced by laminar winds. Additional simulation cases deal with modified surface characteristics and their impacts on the simulation results. Saharan dust layers that reach Barbados via long-range transport over the North Atlantic are included as passive tracers in the model. Effects of layer thinning, subsidence and turbulent downward transport near the layer bottom at z ≈ 1800 m become apparent. The exact position of these layers and strength of downward mixing is found to be mainly controlled atmospheric stability (especially inversion strength) and wind shear. Comparisons of LES model output with lidar data show similarities in the downwind vertical wind structure and accurately reproduces the development of the daytime convective boundary layer measured by the Raman lidar.

  9. Diagnosis, Epidemiology and Management of Mixed States in Bipolar Disorder.

    PubMed

    Fagiolini, Andrea; Coluccia, Anna; Maina, Giuseppe; Forgione, Rocco N; Goracci, Arianna; Cuomo, Alessandro; Young, Allan H

    2015-09-01

    Approximately 40% of patients with bipolar disorder experience mixed episodes, defined as a manic state with depressive features, or manic symptoms in a patient with bipolar depression. Compared with bipolar patients without mixed features, patients with bipolar mixed states generally have more severe symptomatology, more lifetime episodes of illness, worse clinical outcomes and higher rates of comorbidities, and thus present a significant clinical challenge. Most clinical trials have investigated second-generation neuroleptic monotherapy, monotherapy with anticonvulsants or lithium, combination therapy, and electroconvulsive therapy (ECT). Neuroleptic drugs are often used alone or in combination with anticonvulsants or lithium for preventive treatment, and ECT is an effective treatment for mixed manic episodes in situations where medication fails or cannot be used. Common antidepressants have been shown to worsen mania symptoms during mixed episodes without necessarily improving depressive symptoms; thus, they are not recommended during mixed episodes. A greater understanding of pathophysiological processes in bipolar disorder is now required to provide a more accurate diagnosis and new personalised treatment approaches. Targeted, specific treatments developed through a greater understanding of bipolar disorder pathophysiology, capable of affecting the underlying disease processes, could well prove to be more effective, faster acting, and better tolerated than existing therapies, therefore providing better outcomes for individuals affected by bipolar disorder. Until such time as targeted agents are available, second-generation neuroleptics are emerging as the treatment of choice in the management of mixed states in bipolar disorder.

  10. Diagnosis, Epidemiology and Management of Mixed States in Bipolar Disorder.

    PubMed

    Fagiolini, Andrea; Coluccia, Anna; Maina, Giuseppe; Forgione, Rocco N; Goracci, Arianna; Cuomo, Alessandro; Young, Allan H

    2015-09-01

    Approximately 40% of patients with bipolar disorder experience mixed episodes, defined as a manic state with depressive features, or manic symptoms in a patient with bipolar depression. Compared with bipolar patients without mixed features, patients with bipolar mixed states generally have more severe symptomatology, more lifetime episodes of illness, worse clinical outcomes and higher rates of comorbidities, and thus present a significant clinical challenge. Most clinical trials have investigated second-generation neuroleptic monotherapy, monotherapy with anticonvulsants or lithium, combination therapy, and electroconvulsive therapy (ECT). Neuroleptic drugs are often used alone or in combination with anticonvulsants or lithium for preventive treatment, and ECT is an effective treatment for mixed manic episodes in situations where medication fails or cannot be used. Common antidepressants have been shown to worsen mania symptoms during mixed episodes without necessarily improving depressive symptoms; thus, they are not recommended during mixed episodes. A greater understanding of pathophysiological processes in bipolar disorder is now required to provide a more accurate diagnosis and new personalised treatment approaches. Targeted, specific treatments developed through a greater understanding of bipolar disorder pathophysiology, capable of affecting the underlying disease processes, could well prove to be more effective, faster acting, and better tolerated than existing therapies, therefore providing better outcomes for individuals affected by bipolar disorder. Until such time as targeted agents are available, second-generation neuroleptics are emerging as the treatment of choice in the management of mixed states in bipolar disorder. PMID:26369921

  11. Raman Spectroscopy of Isotopic Water Diffusion in Ultraviscous, Glassy, and Gel States in Aerosol by Use of Optical Tweezers.

    PubMed

    Davies, James F; Wilson, Kevin R

    2016-02-16

    The formation of ultraviscous, glassy, and amorphous gel states in aqueous aerosol following the loss of water results in nonequilibrium dynamics due to the extended time scales for diffusive mixing. Existing techniques for measuring water diffusion by isotopic exchange are limited by contact of samples with the substrate, and methods applied to infer diffusion coefficients from mass transport in levitated droplets requires analysis by complex coupled differential equations to derive diffusion coefficients. We present a new technique that combines contactless levitation with aerosol optical tweezers with isotopic exchange (D2O/H2O) to measure the water diffusion coefficient over a broad range (Dw ≈ 10(-12)-10(-17) m(2)·s(-1)) in viscous organic liquids (citric acid, sucrose, and shikimic acid) and inorganic gels (magnesium sulfate, MgSO4). For the organic liquids in binary and ternary mixtures, Dw depends on relative humidity and follows a simple compositional Vignes relationship. In MgSO4 droplets, water diffusivity decreases sharply with water activity and is consistent with predictions from percolation theory. These measurements show that, by combining micrometer-sized particle levitation (a contactless measurement with rapid mixing times) with an established probe of water diffusion, Dw can be simply and directly quantified for amorphous and glassy states that are inaccessible to existing methods. PMID:26751163

  12. Symmetry conserving configuration mixing method with cranked states

    NASA Astrophysics Data System (ADS)

    Borrajo, Marta; Rodríguez, Tomás R.; Luis Egido, J.

    2015-06-01

    We present the first calculations of a symmetry conserving configuration mixing method (SCCM) using time-reversal symmetry breaking Hartree-Fock-Bogoliubov (HFB) states with the Gogny D1S interaction. The method includes particle number and tridimensional angular momentum symmetry restorations as well as configuration mixing within the generator coordinate method (GCM) framework. The nucleus 32Mg is chosen to show the performance and reliability of the calculations. Additionally, 01+, 21+ and 41+ states are computed for the magnesium isotopic chain, where a noticeable compression of the spectrum is obtained by including cranked states, leading to a very good agreement with the known experimental data.

  13. Maximally entangled mixed-state generation via local operations

    SciTech Connect

    Aiello, A.; Puentes, G.; Voigt, D.; Woerdman, J. P.

    2007-06-15

    We present a general theoretical method to generate maximally entangled mixed states of a pair of photons initially prepared in the singlet polarization state. This method requires only local operations upon a single photon of the pair and exploits spatial degrees of freedom to induce decoherence. We report also experimental confirmation of these theoretical results.

  14. Universal and phase-covariant superbroadcasting for mixed qubit states

    SciTech Connect

    Buscemi, Francesco; D'Ariano, Giacomo Mauro; Macchiavello, Chiara; Perinotti, Paolo

    2006-10-15

    We describe a general framework to study covariant symmetric broadcasting maps for mixed qubit states. We explicitly derive the optimal N{yields}M superbroadcasting maps, achieving optimal purification of the single-site output copy, in both the universal and phase-covariant cases. We also study the bipartite entanglement properties of the superbroadcast states.

  15. Population of mixed-symmetry states via {alpha} transfer reactions

    SciTech Connect

    Alonso, C. E.; Arias, J. M.; Fortunato, L.; Vitturi, A.; Pietralla, N.

    2008-07-15

    Within the neutron-proton interacting boson model we study the population of mixed-symmetry states via {alpha} transfer processes. Closed expressions are deduced in the case of the limiting U{sub {pi}}{sub +{nu}}(5) and SU{sub {pi}}{sub +{nu}}(3). We find that the population of the lowest mixed-symmetry 2{sup +} state, vanishing along the N{sub {pi}}=N{sub {nu}} line, depends on the number of active bosons and is normally smaller than that of the lowest full symmetric 2{sup +} state. In particular, for deformed nuclei where the number of bosons is normally large, the relative population of the mixed-symmetry 2{sup +} state is of the order of a few percent. More favorable cases can be found near shell closures, as in the case of {alpha} transfer leading to {sup 140}Ba.

  16. Carbon oxidation state as a metric for describing the chemistry of atmospheric organic aerosol.

    PubMed

    Kroll, Jesse H; Donahue, Neil M; Jimenez, Jose L; Kessler, Sean H; Canagaratna, Manjula R; Wilson, Kevin R; Altieri, Katye E; Mazzoleni, Lynn R; Wozniak, Andrew S; Bluhm, Hendrik; Mysak, Erin R; Smith, Jared D; Kolb, Charles E; Worsnop, Douglas R

    2011-02-01

    A detailed understanding of the sources, transformations and fates of organic species in the environment is crucial because of the central roles that they play in human health, biogeochemical cycles and the Earth's climate. However, such an understanding is hindered by the immense chemical complexity of environmental mixtures of organics; for example, atmospheric organic aerosol consists of at least thousands of individual compounds, all of which likely evolve chemically over their atmospheric lifetimes. Here, we demonstrate the utility of describing organic aerosol (and other complex organic mixtures) in terms of average carbon oxidation state, a quantity that always increases with oxidation, and is readily measured using state-of-the-art analytical techniques. Field and laboratory measurements of the average carbon oxidation state, using several such techniques, constrain the chemical properties of the organics and demonstrate that the formation and evolution of organic aerosol involves simultaneous changes to both carbon oxidation state and carbon number.

  17. Coherent-state transfer via highly mixed quantum spin chains

    SciTech Connect

    Cappellaro, Paola; Viola, Lorenza; Ramanathan, Chandrasekhar

    2011-03-15

    Spin chains have been proposed as quantum wires in many quantum-information processing architectures. Coherent transmission of quantum information in spin chains over short distances is enabled by their internal dynamics, which drives the transport of single-spin excitations in perfectly polarized chains. Given the practical challenge of preparing the chain in a pure state, we propose to use a chain that is initially in the maximally mixed state. We compare the transport properties of pure and mixed-state chains and find similarities that enable the experimental study of pure-state transfer via mixed-state chains. We also demonstrate protocols for the perfect transfer of quantum information in these chains. Remarkably, mixed-state chains allow the use of Hamiltonians that do not preserve the total number of single-spin excitations and are more readily obtainable from the naturally occurring magnetic dipolar interaction. We discuss experimental implementations using solid-state nuclear magnetic resonance and defect centers in diamond.

  18. Long range transport and mixing of aerosol sources during the 2013 North American biomass burning episode: analysis of multiple lidar observations in the Western Mediterranean basin

    NASA Astrophysics Data System (ADS)

    Ancellet, G.; Pelon, J.; Totems, J.; Chazette, P.; Bazureau, A.; Sicard, M.; Di Iorio, T.; Dulac, F.; Mallet, M.

    2015-11-01

    Long range transport of biomass burning (BB) aerosols between North America and the Mediterranean region took place in June 2013. A large number of ground based and airborne lidar measurements were deployed in the Western Mediterranean during the Chemistry-AeRosol Mediterranean EXperiment (ChArMEx) intensive observation period. A detailed analysis of the potential North American aerosol sources is conducted including the assessment of their transport to Europe using forward simulations of the FLEXPART Lagrangian particle dispersion model initialized using satellite observations by MODIS and CALIOP. The three dimensional structure of the aerosol distribution in the ChArMEx domain observed by the ground-based lidars (Menorca, Barcelona and Lampedusa), a Falcon-20 aircraft flight and three CALIOP tracks, agree very well with the model simulation of the three major sources considered in this work: Canadian and Colorado fires, a dust storm from Western US and the contribution of Saharan dust streamers advected from the North Atlantic trade wind region into the Westerlies region. Four aerosol types were identified using the optical properties of the observed aerosol layers (aerosol depolarization ratio, lidar ratio) and the transport model analysis of the contribution of each aerosol source: (I) pure BB layer, (II) weakly dusty BB, (III) significant mixture of BB and dust transported from the trade wind region (IV) the outflow of Saharan dust by the subtropical jet and not mixed with BB aerosol. The contribution of the Canadian fires is the major aerosol source during this episode while mixing of dust and BB is only significant at altitude above 5 km. The mixing corresponds to a 20-30 % dust contribution in the total aerosol backscatter. The comparison with the MODIS AOD horizontal distribution during this episode over the Western Mediterranean sea shows that the Canadian fires contribution were as large as the direct northward dust outflow from Sahara.

  19. Examining the role of NOx and acidity on organic aerosol formation through predictions of key isoprene aerosol species in the United States

    EPA Science Inventory

    Isoprene is a significant contributor to organic aerosol in the Southeastern United States. Later generation isoprene products, specifically isoprene epoxydiols (IEPOX) and methacryloylperoxynitrate (MPAN), have been identified as SOA precursors. The contribution of each pathway ...

  20. Ice and liquid partitioning in mid-latitude and artic mixed-phase clouds: how common is the real mixed-phase state

    NASA Astrophysics Data System (ADS)

    Meyer, Jessica; Krämer, Martina; Afchine, Armin; Gallagher, Martin; Dorsey, James; Brown, Phil; Woolley, Alan; Bierwirth, Eike; Ehrlich, Andre; Wendisch, Manfred; Gehrmann, Martin

    2013-04-01

    The influence of mixed-phase clouds on the radiation budget of the earth is largely unknown. One of the key parameters to determine mixed-phase cloud radiative properties however is the fraction of ice particles and liquid droplets in these clouds. The separate detection of liquid droplets and ice crystals especially in the small cloud particle size range below 50 µm remains challenging though. Here, we present airborne NIXE-CAPS mixed-phase cloud particle measurements observed in mid-latitude and Arctic low-level mixed-phase clouds during the COALESC field campaign in 2011 and the Arctic field campaign VERDI in 2012. NIXE-CAPS (Novel Ice EXpEriment - Cloud and Aerosol Particle Spectrometer, manufactured by DMT) is a cloud particle spectrometer which measures the cloud particle number, size as well as their phase for each cloud particle in the diameter range 0.6 to 945 µm. The common understanding in mixed-phase cloud research is that liquid droplets and ice crystals in the same cloud volume are rather sparse, but instead either liquid droplets or ice crystals are present. However, recently published model studies (e.g. Korolev, A. & Field, P., The effect of dynamics on mixed-phase clouds: Theoretical considerations. J. Atmos. Sci. 65, 66-86, 2008) indicate that a cloud state containing both liquid droplets and ice crystals can be kept up by turbulence. Indeed, our particle by particle analyses of the observed mixed-phase clouds during COALESC and VERDI indicate that the real mixed-phase state is rather common in the atmosphere. The spatial distribution of the mixed-phase ice fraction and the size of the droplets and ice crystals however vary substantially from case to case. The latter parameters seem to be influenced not only by concentration of ice nuclei but also - to a large degree - by cloud dynamics.

  1. Epoxide pathways improve model predictions of isoprene markers and reveal key role of acidity in aerosol formation

    EPA Science Inventory

    Isoprene significantly contributes to organic aerosol in the southeastern United States where biogenic hydrocarbons mix with anthropogenic emissions. In this work, the Community Multiscale Air Quality model is updated to predict isoprene aerosol from epoxides produced under both ...

  2. Morphology of Mixed Primary and Secondary Organic Particles and the Adsorption of Spectator Organic Gases during Aerosol Formation

    SciTech Connect

    Vaden, Timothy D.; Song, Chen; Zaveri, Rahul A.; Imre, D.; Zelenyuk, Alla

    2010-04-13

    Traditional semi-empirical secondary organic aerosol (SOA) models assume that SOA mixes well with primary organic aerosols (POA), which significantly enhances the modeled SOA yields. These models further assume that the organic compounds in the gas phase do no condense on SOA as it forms. These assumptions were challenged through a detailed experimental investigation of the compositions and morphologies of SOA particles formed during ozonolysis of α-pinene in the presence of dioctyl phthalate (DOP) particles and DOP gas phase component using a single particle mass spectrometer. Ultraviolet (UV) laser depth-profiling experiments were used to characterize different types of mixed SOA/DOP particles: those formed by condensation of the oxidized α-pinene products on size-selected DOP particles and by condensation of DOP on size-selected α-pinene SOA particles. The results of these measurements conclusively show that the hydrophilic SOA and hydrophobic DOP do not mix, but instead form distinct phases. An examination of homogeneously-nucleated SOA particles formed in the presence of DOP shows them to be encapsulated by a thin DOP layer. Thus SOA can adsorb gas-phase DOP even though it has an extremely low vapor pressure (1.3×10-7 Torr), which has significant implications for SOA formation and fate in the atmosphere, where numerous organic compounds with various volatilities are present.

  3. Parameterization of the Cloud Nucleating Activity of Fresh, Aged, and Internally-Mixed Organic Aerosols

    NASA Astrophysics Data System (ADS)

    Kreidenweis, S.; Petters, M.; Demott, P.; Prenni, A.; Ziemann, P.

    2006-12-01

    Carbonaceous particle types affect global climate, visibility, and human health, but their primary and secondary sources, sinks, and tropospheric lifetimes are highly uncertain. The size and hygroscopicity of particles, and in particular their activity as cloud condensation nuclei (CCN), plays a large role in determining their atmospheric impacts and lifetimes. However, hygroscopicity is difficult to parameterize for many organic species for which no thermodynamic data exist, and for complex, multicomponent aerosols of undefined composition. We propose a simple method to describe the relationship between dry particle diameter and CCN activity using a single hygroscopicity parameter, κ. We derive values of κ from fitting of experimental CCN-activity data from the literature and from recent experiments, including oxidation-aged organic particles and secondary organic aerosols. Values of κ are between 0.5 and 2 for highly-CCN- active salts such as sodium chloride, between 0.01 and 0.5 for slightly to very hygroscopic organic aerosols such as those produced in biomass burning and as secondary organic aerosols, and 0 for nonhygroscopic components. The hygroscopicity of internal mixtures can be calculated as a volume fraction weighted average of the hygroscopicity parameters of the individual species comprising the mixture. Aging of aerosol, understood as changes in hygroscopicity due to condensation of hydrophilic species, coagulation of aerosol populations, or heterogeneous chemical reactions, are described conveniently by changes in κ. Our studies show that oxidative aging that proceeds by addition of functional groups to the CHx carbon backbone leads to only small changes in κ, and thus the process alone is inefficient at rendering small, initially- hydrophobic primary organic particles capable of being scavenged by cloud-drop nucleation. Other processes, such as coagulation and condensation, control the rate of hydrophobic-to-hydrophilic conversion of primary

  4. Carbon oxidation state as a metric for describing the chemistry of atmospheric organic aerosol

    SciTech Connect

    Massachusetts Institute of Technology; Kroll, Jesse H.; Donahue, Neil M.; Jimenez, Jose L.; Kessler, Sean H.; Canagaratna, Manjula R.; Wilson, Kevin R.; Altieri, Katye E.; Mazzoleni, Lynn R.; Wozniak, Andrew S.; Bluhm, Hendrik; Mysak, Erin R.; Smith, Jared D.; Kolb, Charles E.; Worsnop, Douglas R.

    2010-11-05

    A detailed understanding of the sources, transformations, and fates of organic species in the environment is crucial because of the central roles that organics play in human health, biogeochemical cycles, and Earth's climate. However, such an understanding is hindered by the immense chemical complexity of environmental mixtures of organics; for example, atmospheric organic aerosol consists of at least thousands of individual compounds, all of which likely evolve chemically over their atmospheric lifetimes. Here we demonstrate the utility of describing organic aerosol (and other complex organic mixtures) in terms of average carbon oxidation state (OSC), a quantity that always increases with oxidation, and is readily measured using state-of-the-art analytical techniques. Field and laboratory measurements of OSC , using several such techniques, constrain the chemical properties of the organics and demonstrate that the formation and evolution of organic aerosol involves simultaneous changes to both carbon oxidation state and carbon number (nC).

  5. Impacts of Venturi Turbulent Mixing on the Size Distribution of Sodium Chloride and Dioctyl-Phthalate Aerosols

    SciTech Connect

    Cheng, M.-D.; Wainman, T.; Storey, J.

    2000-08-01

    Internal combustion engines are a major source of airborne particulate matter (PM). The size of the engine PM is in the sub-micrometer range. The number of engine particles per unit volume is high, normally in the range of 10{sup 12} to 10{sup 14}. To measure the size distribution of the engine particles dilution of an aerosol sample is required. A diluter utilizing a venturi ejector mixing technique is commercially available and tested. The purpose of this investigation was to determine if turbulence created by the ejector in the mini-dilutor changes the size of particles passing through it.

  6. Spatial Variability in Black Carbon Mixing State Observed During The Multi-City NASA DISCOVER-AQ Field Campaign

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

    Light absorbing carbonaceous aerosols are known to be an important climatic driver with a global radiative forcing of about half (IPCC, 2013) to two-thirds (Bond et al., 2013) that of the dominant greenhouse gas, carbon dioxide. While the mass absorption coefficient of pure black carbon (BC) is fairly well known, observational evidence suggests that BC rapidly mixes with other aerosol chemical components within hours of emission (Moffet and Prather, 2009; Moteki et al., 2007). These other components may include predominantly scattering organic, sulfate, and nitrate species, as well as light-absorbing, so-called "brown carbon" (BrC). It has been suggested that the presence of these BC-mixed components may induce mixing-state-dependent lensing effects that could potentially double the BC direct radiative forcing (Jacobson, 2001). The key to better understanding how BC-rich aerosols are distributed in the atmosphere is to examine an unbiased set of measurements covering broad spatial and temporal coverage; however, many past airborne field campaigns have specifically targeted source plumes or other scientifically-relevant emissions sources. The recent NASA DISCOVER-AQ campaign is unique in that approximately the same flight pattern was performed over a month-long period in each of four different U.S. metropolitan areas, ensuring an unbiased, or at least less biased, data set with both wide horizontal and vertical (surface to 5 km altitude) coverage. We present a statistical analysis of BC-rich particle mixing state measured during DISCOVER-AQ by a DMT Single Particle Soot Photometer (SP2). The SP2 measures the BC mass distribution via laser incandescence, and the non-BC coating thickness is inferred from the light scattering signal of particles greater than 200 nm in diameter (Gao et al., 2007; Moteki and Kondo, 2008). The SP2-derived size distributions are compared to optical scattering size distributions measured by an UHSAS in order determine 1) the externally

  7. Entangled mixed-state generation by twin-photon scattering

    SciTech Connect

    Puentes, G.; Aiello, A.; Woerdman, J. P.; Voigt, D.

    2007-03-15

    We report experimental results on mixed-state generation by multiple scattering of polarization-entangled photon pairs created from parametric down-conversion. By using a large variety of scattering optical systems we have experimentally obtained entangled mixed states that lie upon and below the Werner curve in the linear entropy-tangle plane. We have also introduced a simple phenomenological model built on the analogy between classical polarization optics and quantum maps. Theoretical predictions from such a model are in full agreement with our experimental findings.

  8. Morphology and mixing state of atmospheric particles: Links to optical properties and cloud processing

    NASA Astrophysics Data System (ADS)

    China, Swarup

    Atmospheric particles are ubiquitous in Earth's atmosphere and impact the environment and the climate while affecting human health and Earth's radiation balance, and degrading visibility. Atmospheric particles directly affect our planet's radiation budget by scattering and absorbing solar radiation, and indirectly by interacting with clouds. Single particle morphology (shape, size and internal structure) and mixing state (coating by organic and inorganic material) can significantly influence the particle optical properties as well as various microphysical processes, involving cloud-particle interactions and including heterogeneous ice nucleation and water uptake. Conversely, aerosol cloud processing can affect the morphology and mixing of the particles. For example, fresh soot has typically an open fractal-like structure, but aging and cloud processing can restructure soot into more compacted shapes, with different optical and ice nucleation properties. During my graduate research, I used an array of electron microscopy and image analysis tools to study morphology and mixing state of a large number of individual particles collected during several field and laboratory studies. To this end, I investigated various types of particles such as tar balls (spherical carbonaceous particles emitted during biomass burning) and dust particles, but with a special emphasis on soot particles. In addition, I used the Stony Brook ice nucleation cell facility to investigate heterogeneous ice nucleation and water uptake by long-range transported particles collected at the Pico Mountain Observatory, in the Archipelago of the Azores. Finally, I used ice nucleation data from the SAAS (Soot Aerosol Aging Study) chamber study at the Pacific Northwest National Laboratory to understand the effects that ice nucleation and supercooled water processing has on the morphology of residual soot particles. Some highlights of our findings and implications are discussed next. We found that the

  9. Characterizing the aging of biomass burning organic aerosol by use of mixing ratios: a meta-analysis of four regions.

    PubMed

    Jolleys, Matthew D; Coe, Hugh; McFiggans, Gordon; Capes, Gerard; Allan, James D; Crosier, Jonathan; Williams, Paul I; Allen, Grant; Bower, Keith N; Jimenez, Jose L; Russell, Lynn M; Grutter, Michel; Baumgardner, Darrel

    2012-12-18

    Characteristic organic aerosol (OA) emission ratios (ERs) and normalized excess mixing ratios (NEMRs) for biomass burning (BB) events have been calculated from ambient measurements recorded during four field campaigns. Normalized OA mass concentrations measured using Aerodyne Research Inc. quadrupole aerosol mass spectrometers (Q-AMS) reveal a systematic variation in average values between different geographical regions. For each region, a consistent, characteristic ratio is seemingly established when measurements are collated from plumes of all ages and origins. However, there is evidence of strong regional and local-scale variability between separate measurement periods throughout the tropical, subtropical, and boreal environments studied. ERs close to source typically exceed NEMRs in the far-field, despite apparent compositional change and increasing oxidation with age. The absence of any significant downwind mass enhancement suggests no regional net source of secondary organic aerosol (SOA) from atmospheric aging of BB sources, in contrast with the substantial levels of net SOA formation associated with urban sources. A consistent trend of moderately reduced ΔOA/ΔCO ratios with aging indicates a small net loss of OA, likely as a result of the evaporation of organic material from initial fire emissions. Variability in ERs close to source is shown to substantially exceed the magnitude of any changes between fresh and aged OA, emphasizing the importance of fuel and combustion conditions in determining OA loadings from biomass burning. PMID:23163290

  10. The effects of marine primary biogenic organic aerosols as heterogeneous ice nuclei in mixed-phase clouds

    NASA Astrophysics Data System (ADS)

    Yun, Y.; Penner, J. E.

    2012-12-01

    There have been reports in the literature about marine primary biogenic organic aerosols (marine POA) acting as ice nuclei. These marine POA can be transported to the atmosphere through the bursting of air bubbles by breaking waves. In this study, we add marine POA as heterogeneous ice nuclei in mixed-phase clouds in a coupled general circulation model and aerosol transport model (CAM-IMPACT). The emission of the marine POA is determined by the sea salt emissions and a sea spray organic fraction function. The wet and dry deposition scheme in the CAM-IMPACT model will be extended to treat marine POA. The ice nucleation ability of the marine POA will be determined according to the in situ observation of the surface ice nuclei ratio, as well as the simulated surface concentration of marine POA and other aerosols. Several sensitivity tests will be performed on the sea salt emission flux, the sea spray organic fraction function, as well as the freezing efficiency of marine POA. The simulated ice water amount will be compared to satellite observations. This study attempts to evaluate the effect of marine biological organics as ice nuclei on a global scale.

  11. Phase, morphology, and hygroscopicity of mixed oleic acid/sodium chloride/water aerosol particles before and after ozonolysis.

    PubMed

    Dennis-Smither, Benjamin J; Hanford, Kate L; Kwamena, Nana-Owusua A; Miles, Rachael E H; Reid, Jonathan P

    2012-06-21

    Aerosol optical tweezers are used to probe the phase, morphology, and hygroscopicity of single aerosol particles consisting of an inorganic component, sodium chloride, and a water insoluble organic component, oleic acid. Coagulation of oleic acid aerosol with an optically trapped aqueous sodium chloride droplet leads to formation of a phase-separated particle with two partially engulfed liquid phases. The dependence of the phase and morphology of the trapped particle with variation in relative humidity (RH) is investigated by cavity enhanced Raman spectroscopy over the RH range <5% to >95%. The efflorescence and deliquescence behavior of the inorganic component is shown to be unaffected by the presence of the organic phase. Whereas efflorescence occurs promptly (<1 s), the deliquescence process requires both dissolution of the inorganic component and the adoption of an equilibrium morphology for the resulting two phase particle, occurring on a time-scale of <20 s. Comparative measurements of the hygroscopicity of mixed aqueous sodium chloride/oleic acid droplets with undoped aqueous sodium chloride droplets show that the oleic acid does not impact on the equilibration partitioning of water between the inorganic component and the gas phase or the time response of evaporation/condensation. The oxidative aging of the particles through reaction with ozone is shown to increase the hygroscopicity of the organic component.

  12. Y(3940) as a mixed charmonium-molecule state

    NASA Astrophysics Data System (ADS)

    Albuquerque, R. M.; Dias, J. M.; Nielsen, M.; Zanetti, C. M.

    2014-04-01

    Using the QCD sum rules approach, we study the mass and the decay widths of the Y(3940) state, assuming that it can be described by a mixed charmonium-molecule scalar state, i.e., a mixture between the χc0 charmonium and D*D ¯* molecule. Using a current with JPC=0++, we estimate for the mixing angle, θ =(76.0±5.0)°, resulting in a mass value of MY=(3.95±0.11) GeV, which is in reasonable agreement with the experimental mass of the Y(3940) state. For the decay width, we evaluate the channels Y→J/ψω and Y→γγ. We find the values ΓY→J/ψω≈(1.7±0.6) MeV and ΓY→γγ≈(1.6±1.3) KeV, respectively. We also study the decay process of this state into channels containing DD ¯ mesons in the final state. The result for the order of magnitude of the product ΓY→γγ×ΓY→J/ψω˜O(103) KeV2 is also in reasonable agreement with the experimental data. We thus conclude that the present description of the Y(3940) as a mixed charmonium-molecule state is a possible scenario to explain the structure of such a state.

  13. Airborne Lidar measurements of aerosols, mixed layer heights, and ozone during the 1980 PEPE/NEROS summer field experiment

    NASA Technical Reports Server (NTRS)

    Browell, E. V.; Shipley, S. T.; Butler, C. F.; Ismail, S.

    1985-01-01

    A detailed summary of the NASA Ultraviolet Differential Absorption Lidar (UV DIAL) data archive obtained during the EPA Persistent Elevated Pollution Episode/Northeast Regional Oxidant Study (PEPE/NEROS) Summer Field Experiment Program (July through August 1980) is presented. The UV dial data set consists of remote measurements of mixed layer heights, aerosol backscatter cross sections, and sequential ozone profiles taken during 14 long-range flights onboard the NASA Wallops Flight Center Electra aircraft. These data are presented in graphic and tabular form, and they have been submitted to the PEPE/NEROS data archive on digital magnetic tape. The derivation of mixing heights and ozone profiles from UV Dial signals is discussed, and detailed intercomparisons with measurements obtained by in situ sensors are presented.

  14. Mixed Charmonium-Molecule Interpretation for the Y (3940) State

    NASA Astrophysics Data System (ADS)

    Albuquerque, R. M.; Dias, J. M.; Nielsen, M.; Zanetti, C. M.

    2015-07-01

    QCD sum rules are used to study the mass and the decay widths of the Y(3940) state. We assume that it can be described by a mixed charmonium-molecule scalar current with JPC = 0++. Using a mixing angle θ = (76.0±5.0)°, we obtain MY = (3.95±0.11) GeV, which is in good agreement with the experimental mass of the Y(3940) state. We also evaluate the decay width in the channels Y → J/ψω and Y → γγ obtaining the values ΓY → j/ψω ≈ (1.7± 0.6) MeV and ΓY→γγ ≈ (1.6 ± 1.3) KeV, respectively. We also study the decay process of this state into channels containing DD mesons in the final state.

  15. Spin relaxation of iron in mixed state hemoproteins.

    PubMed Central

    Wajnberg, E; Kalinowski, H J; Bemski, G; Helman, J S

    1986-01-01

    In hemoproteins the relaxation mechanism of iron is Orbach for high spin (HS) and Raman for low spin (LS). We found that in met-hemoglobin and met-myoglobin, under conditions in which the two spin states coexist, both the HS and the LS states relax to the lattice through Orbach-like processes. Alos, very short (approximately 1 ns) and temperature independent transverse relaxation times T2 were estimated. This may result from the unusual electronic structure of mixed states hemoproteins that allows thermal equilibrium and interconversion of the spin states. PMID:3013333

  16. The Optimal Cloner for Mixed States as a Quantum Operation

    NASA Astrophysics Data System (ADS)

    Gardiner, John G.; van Huele, Jean-Francois S.

    2012-10-01

    The no-cloning theorem in quantum information says that it is impossible to produce two copies of an arbitrary quantum state. This precludes the possibility of a perfect universal quantum cloner, a process that could copy any quantum state perfectly. It is possible, however, to find optimal approximations of such a cloner. Using the formalism of quantum operations we obtain the optimal quantum cloner for arbitrary mixed states of a given purity and find that it is equivalent to the Buzek-Hillery optimal cloner for pure states. We also find the fidelity of this cloner as a function of the chosen purity.

  17. Nonlinear Guided Wave Mixing for Localized Material State Characterization

    NASA Astrophysics Data System (ADS)

    Lissenden, Cliff J.; Liu, Yang; Chillara, Vamshi K.; Choi, Gloria; Cho, Hwanjeong

    Material state characterization methods sensitive to incipient damage provide new opportunities for managing the life cycle of structures. Finite element simulations of ultrasonic guided waves show the potential of nonlinear wave mixing to detect localized degradation invisible to both linear elastic stress-strain response and the eye. Correlation of material degradation to the generation of higher harmonics or combinational harmonics makes estimation of remaining life possible from material state data early in the service life.

  18. Search for mixed-symmetry states in 212Po

    NASA Astrophysics Data System (ADS)

    Kocheva, D.; Rainovski, G.; Jolie, J.; Pietralla, N.; Stahl, C.; Petkov, P.; Blazhev, A.; Hennig, A.; Astier, A.; Braunroth, Th.; Cortes, L.; Dewald, A.; Djongolov, M.; Fransen, C.; Gladnishki, K.; Karayonchev, V.; Litzinger, J.; Müller-Gatermann, C.; Scheck, M.; Scholz, Ph.; Schramm, C.; Tölle, P.; Werner, V.; Witt, W.; Wölk, D.; Van Isacker, P.

    2016-06-01

    In this work we present an experiment dedicated to searching for quarupole- collective isovector valence-shell excitation — the states with so-called mixed proton-neutron symmetry (MSSs), in the nucleus 212Po. The states of interest were populated and studied by an α-transfer reaction. The experiment provides indication for existence of one-phonon MSS in the nucleus 212Po which is the first experimentally identified MSS in the region around double magic nucleus 208Pb.

  19. Photonic states mixing beyond the plasmon hybridization model

    NASA Astrophysics Data System (ADS)

    Suryadharma, Radius N. S.; Iskandar, Alexander A.; Tjia, May-On

    2016-07-01

    A study is performed on a photonic-state mixing-pattern in an insulator-metal-insulator cylindrical silver nanoshell and its rich variations induced by changes in the geometry and dielectric media of the system, representing the combined influences of plasmon coupling strength and cavity effects. This study is performed in terms of the photonic local density of states (LDOS) calculated using the Green tensor method, in order to elucidate those combined effects. The energy profiles of LDOS inside the dielectric core are shown to exhibit consistently growing number of redshifted photonic states due to an enhanced plasmon coupling induced state mixing arising from decreased shell thickness, increased cavity size effect, and larger symmetry breaking effect induced by increased permittivity difference between the core and the background media. Further, an increase in cavity size leads to increased additional peaks that spread out toward the lower energy regime. A systematic analysis of those variations for a silver nanoshell with a fixed inner radius in vacuum background reveals a certain pattern of those growing number of redshifted states with an analytic expression for the corresponding energy downshifts, signifying a photonic state mixing scheme beyond the commonly adopted plasmon hybridization scheme. Finally, a remarkable correlation is demonstrated between the LDOS energy profiles outside the shell and the corresponding scattering efficiencies.

  20. Race-mixing and science in the United States.

    PubMed

    Farber, Paul

    2003-12-01

    Scientific racism was widely used as a justification to oppose race-mixing in the United States. Historians have justly criticized this abuse of science, but have overlooked some of the important ways in which science was used in the 1930s and 1940s to overturn scientific racism and opposition to race-mixing. Of particular importance was the cultural anthropology of Franz Boas and the evolutionary biology of Theodosius Dobzhansky, which supplied arguments against racism and fundamentally altered the scientific understanding of race. PMID:14652040

  1. Race-mixing and science in the United States.

    PubMed

    Farber, Paul

    2003-12-01

    Scientific racism was widely used as a justification to oppose race-mixing in the United States. Historians have justly criticized this abuse of science, but have overlooked some of the important ways in which science was used in the 1930s and 1940s to overturn scientific racism and opposition to race-mixing. Of particular importance was the cultural anthropology of Franz Boas and the evolutionary biology of Theodosius Dobzhansky, which supplied arguments against racism and fundamentally altered the scientific understanding of race.

  2. Measurement of the topological charge of mixed OAM states

    NASA Astrophysics Data System (ADS)

    Shutova, Mariia; Zhdanova, Alexandra; Sokolov, Alexei

    2016-05-01

    In the current work, we investigate how the technique of measuring the topological charge of an optical vortex by using a tilted convex lens (tilted lens technique) works for optical vortices in mixed orbital angular momentum (OAM) states (i.e. the case when one beam contains several components with different values of topological charge). A mixed OAM state may occur, for example, because of perturbations in the optical devices used to generate the state, such as spatial light modulators or spiral phase plates. Hence, we present experimental results and theoretical simulations for the measurement of the topological charge of mixed states with variable amounts of each component contributing to the total beam intensity. We also investigate two different cases: first, when interference between components is present (coherent addition of component OAM states), and second, when interference is absent (incoherent addition). We conclude that in both cases the results of the tilted lens technique are valid for that component of light which is dominant (i.e. the component that contributes to more than 50% of the beam's total intensity). Presenter is supported by the Herman F. Heep and Minnie Belle Heep Texas A&M University Endowed Fund administered by the Texas A&M Foundation.

  3. AGRICULTURAL AMMONIA EMISSIONS AND AMMONIUM CONCENTRATIONS ASSOCIATED WITH AEROSOLS AND PRECIPITATION IN THE SOUTHEAST UNITED STATES

    EPA Science Inventory

    Temporal and spatial variations in ammonia (NH3) emissions and ammonium (NH4+) concentrations associated with aerosols and volume-weighted NH4+ concentration in precipitation are investigated over the period 1990-1998 in the southeast United States (Alabama, Florida, Georgia, Ken...

  4. Random Bures mixed states and the distribution of their purity

    NASA Astrophysics Data System (ADS)

    Osipov, V. Al; Sommers, H.-J.; Życzkowski, K.

    2010-02-01

    Ensembles of random density matrices determined by various probability measures are analysed. A simple and efficient algorithm to generate at random density matrices distributed according to the Bures measure is proposed. This procedure may serve as an initial step in performing the Bayesian approach to quantum state estimation based on the Bures prior. We study the distribution of purity of random mixed states. The moments of the distribution of purity are determined for quantum states generated with respect to the Bures measure. This calculation serves as an exemplary application of the 'deform-and-study' approach in the theory of integrable systems leading to one of Painlevés transcendents.

  5. The dependence of ice microphysics on aerosol concentration in arctic mixed-phase stratus clouds during ISDAC and M-PACE

    SciTech Connect

    Jackson, Robert C.; McFarquhar, Greg; Korolev, Alexei; Earle, Michael; Liu, Peter S.; Lawson, R. P.; Brooks, Sarah D.; Wolde, Mengistu; Laskin, Alexander; Freer, Matthew

    2012-08-14

    Cloud and aerosol data acquired by the National Research Council of Canada (NRC) Convair-580 aircraft in, above, and below single-layer arctic stratocumulus cloud during the Indirect and Semi-Direct Aerosol Campaign (ISDAC) in April 2008 were used to test three aerosol indirect effects hypothesized to act in mixed-phase clouds: the riming indirect effect, the glaciation indirect effect, and the cold second indirect effect. The data showed a correlation of R= 0.75 between liquid drop number concentration, Nliq, inside cloud and ambient aerosol number concentration NPCASP below cloud. This, combined with increasing liquid water content LWC with height above cloud base and the nearly constant profile of Nliq, suggested that liquid drops were nucleated from aerosol at cloud base. No strong evidence of a riming indirect effect was observed, but a strong correlation of R = 0.69 between ice crystal number concentration Ni and NPCASP above cloud was noted. Increases in ice nuclei (IN) concentration with NPCASP above cloud combined with the subadiabatic LWC profiles suggest possible mixing of IN from cloud top consistent with the glaciation indirect effect. The higher Nice and lower effective radius rel for the more polluted ISDAC cases compared to data collected in cleaner single-layer stratocumulus conditions during the Mixed-Phase Arctic Cloud Experiment is consistent with the operation of the cold second indirect effect. However, more data in a wider variety of meteorological and surface conditions, with greater variations in aerosol forcing, are required to identify the dominant aerosol forcing mechanisms in mixed-phase arctic clouds.

  6. Existence and construction of simultaneous cloning machines for mixed states

    NASA Astrophysics Data System (ADS)

    Guo, ZhiHua; Cao, HuaiXin; Qu, ShiXian

    2015-04-01

    It is a well-known fact that the no-cloning theorem forbids the creation of identical copies of an arbitrary unknown quantum state. In other words, there does not exist a quantum cloning machine that can clone all quantum states. However, it is possible to clone given quantum states under certain conditions, for instance, k distinct pure states | Ψ 1>, | Ψ 2>, …, | Ψ k > can be cloned simultaneously if and only if they are orthogonal. This paper discusses the existence and construction of simultaneous cloning machines for mixed states. It is proved that k distinct mixed states ρ 1, ρ 2, …, ρ k of the n-dimensional quantum system ℂ n can be cloned simultaneously, that is, there exists a quantum channel Φ on M n ⊗ M n and a state Σ in M n , such that Φ( ρ i ⊗ Σ) = ρ i ⊗ ρ i for all i, if and only if ρ i ρ j = 0 ( i ≠ j). Also, the constructing procedure of the desired simultaneous cloning machine is given.

  7. Attribution of the United States "warming hole": aerosol indirect effect and precipitable water vapor.

    PubMed

    Yu, Shaocai; Alapaty, Kiran; Mathur, Rohit; Pleim, Jonathan; Zhang, Yuanhang; Nolte, Chris; Eder, Brian; Foley, Kristen; Nagashima, Tatsuya

    2014-11-06

    Aerosols can influence the climate indirectly by acting as cloud condensation nuclei and/or ice nuclei, thereby modifying cloud optical properties. In contrast to the widespread global warming, the central and south central United States display a noteworthy overall cooling trend during the 20(th) century, with an especially striking cooling trend in summertime daily maximum temperature (Tmax) (termed the U.S. "warming hole"). Here we used observations of temperature, shortwave cloud forcing (SWCF), longwave cloud forcing (LWCF), aerosol optical depth and precipitable water vapor as well as global coupled climate models to explore the attribution of the "warming hole". We find that the observed cooling trend in summer Tmax can be attributed mainly to SWCF due to aerosols with offset from the greenhouse effect of precipitable water vapor. A global coupled climate model reveals that the observed "warming hole" can be produced only when the aerosol fields are simulated with a reasonable degree of accuracy as this is necessary for accurate simulation of SWCF over the region. These results provide compelling evidence of the role of the aerosol indirect effect in cooling regional climate on the Earth. Our results reaffirm that LWCF can warm both winter Tmax and Tmin.

  8. 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.

  9. Attribution of the United States "warming hole": aerosol indirect effect and precipitable water vapor.

    PubMed

    Yu, Shaocai; Alapaty, Kiran; Mathur, Rohit; Pleim, Jonathan; Zhang, Yuanhang; Nolte, Chris; Eder, Brian; Foley, Kristen; Nagashima, Tatsuya

    2014-01-01

    Aerosols can influence the climate indirectly by acting as cloud condensation nuclei and/or ice nuclei, thereby modifying cloud optical properties. In contrast to the widespread global warming, the central and south central United States display a noteworthy overall cooling trend during the 20(th) century, with an especially striking cooling trend in summertime daily maximum temperature (Tmax) (termed the U.S. "warming hole"). Here we used observations of temperature, shortwave cloud forcing (SWCF), longwave cloud forcing (LWCF), aerosol optical depth and precipitable water vapor as well as global coupled climate models to explore the attribution of the "warming hole". We find that the observed cooling trend in summer Tmax can be attributed mainly to SWCF due to aerosols with offset from the greenhouse effect of precipitable water vapor. A global coupled climate model reveals that the observed "warming hole" can be produced only when the aerosol fields are simulated with a reasonable degree of accuracy as this is necessary for accurate simulation of SWCF over the region. These results provide compelling evidence of the role of the aerosol indirect effect in cooling regional climate on the Earth. Our results reaffirm that LWCF can warm both winter Tmax and Tmin. PMID:25373416

  10. Attribution of the United States “warming hole”: Aerosol indirect effect and precipitable water vapor

    NASA Astrophysics Data System (ADS)

    Yu, Shaocai; Alapaty, Kiran; Mathur, Rohit; Pleim, Jonathan; Zhang, Yuanhang; Nolte, Chris; Eder, Brian; Foley, Kristen; Nagashima, Tatsuya

    2014-11-01

    Aerosols can influence the climate indirectly by acting as cloud condensation nuclei and/or ice nuclei, thereby modifying cloud optical properties. In contrast to the widespread global warming, the central and south central United States display a noteworthy overall cooling trend during the 20th century, with an especially striking cooling trend in summertime daily maximum temperature (Tmax) (termed the U.S. ``warming hole''). Here we used observations of temperature, shortwave cloud forcing (SWCF), longwave cloud forcing (LWCF), aerosol optical depth and precipitable water vapor as well as global coupled climate models to explore the attribution of the ``warming hole''. We find that the observed cooling trend in summer Tmax can be attributed mainly to SWCF due to aerosols with offset from the greenhouse effect of precipitable water vapor. A global coupled climate model reveals that the observed ``warming hole'' can be produced only when the aerosol fields are simulated with a reasonable degree of accuracy as this is necessary for accurate simulation of SWCF over the region. These results provide compelling evidence of the role of the aerosol indirect effect in cooling regional climate on the Earth. Our results reaffirm that LWCF can warm both winter Tmax and Tmin.

  11. Attribution of the United States “warming hole”: Aerosol indirect effect and precipitable water vapor

    PubMed Central

    Yu, Shaocai; Alapaty, Kiran; Mathur, Rohit; Pleim, Jonathan; Zhang, Yuanhang; Nolte, Chris; Eder, Brian; Foley, Kristen; Nagashima, Tatsuya

    2014-01-01

    Aerosols can influence the climate indirectly by acting as cloud condensation nuclei and/or ice nuclei, thereby modifying cloud optical properties. In contrast to the widespread global warming, the central and south central United States display a noteworthy overall cooling trend during the 20th century, with an especially striking cooling trend in summertime daily maximum temperature (Tmax) (termed the U.S. “warming hole”). Here we used observations of temperature, shortwave cloud forcing (SWCF), longwave cloud forcing (LWCF), aerosol optical depth and precipitable water vapor as well as global coupled climate models to explore the attribution of the “warming hole”. We find that the observed cooling trend in summer Tmax can be attributed mainly to SWCF due to aerosols with offset from the greenhouse effect of precipitable water vapor. A global coupled climate model reveals that the observed “warming hole” can be produced only when the aerosol fields are simulated with a reasonable degree of accuracy as this is necessary for accurate simulation of SWCF over the region. These results provide compelling evidence of the role of the aerosol indirect effect in cooling regional climate on the Earth. Our results reaffirm that LWCF can warm both winter Tmax and Tmin. PMID:25373416

  12. Single point aerosol sampling: Evaluation of mixing and probe performance in a nuclear stack

    SciTech Connect

    Rodgers, J.C.; Fairchild, C.I.; Wood, G.O.; Ortiz, C.A.; Muyshondt, A.; McFarland, A.R. |

    1994-12-31

    Alternative Reference Methodologies (ARMS) have been developed for sampling of radionuclide; from stacks and ducts that differ from the methods required by the US EPA. The EPA methods are prescriptive in selection of sampling locations and in design of sampling probes whereas the alternative methods are performance driven. Tests were conducted in a stack at Los Alamos National Laboratory to demonstrate the efficacy of the ARMS. Coefficients of variation of the velocity tracer gas, and aerosol particle profiles were determined at three sampling locations. Results showed numerical criteria placed upon the coefficients of variation by the ARMs were met at sampling stations located 9 and 14 stack diameters from flow entrance, but not at a location that is 1.5 diameters downstream from the inlet. Experiments were conducted to characterize the transmission of 10 {mu}m aerodynamic equivalent diameter liquid aerosol particles through three types of sampling probes. The transmission ratio (ratio of aerosol concentration at the probe exit plane to the concentration in the free stream) was 107% for a 113 L/min (4-cfm) an isokinetic shrouded probe, but only 20% for an isokinetic probe that follows the EPA requirements. A specially designed isokinetic probe showed a transmission ratio of 63%. The shrouded probe performance would conform to the ARM criteria; however, the isokinetic probes would not.

  13. Single point aerosol sampling: Evaluation of mixing and probe performance in a nuclear stack

    SciTech Connect

    Rodgers, J.C.; Fairchild, C.I.; Wood, G.O.

    1995-02-01

    Alternative Reference Methodologies (ARMs) have been developed for sampling of radionuclides from stacks and ducts that differ from the methods required by the U.S. EPA. The EPA methods are prescriptive in selection of sampling locations and in design of sampling probes whereas the alternative methods are performance driven. Tests were conducted in a stack at Los Alamos National Laboratory to demonstrate the efficacy of the ARMs. Coefficients of variation of the velocity tracer gas, and aerosol particle profiles were determined at three sampling locations. Results showed numerical criteria placed upon the coefficients of variation by the ARMs were met at sampling stations located 9 and 14 stack diameters from flow entrance, but not at a location that is 1.5 diameters downstream from the inlet. Experiments were conducted to characterize the transmission of 10 {mu}m aerodynamic equivalent diameter liquid aerosol particles through three types of sampling probes. The transmission ratio (ratio of aerosol concentration at the probe exit plane to the concentration in the free stream) was 107% for a 113 L/min (4-cfm) anisokinetic shrouded probe, but only 20% for an isokinetic probe that follows the EPA requirements. A specially designed isokinetic probe showed a transmission ratio of 63%. The shrouded probe performance would conform to the ARM criteria; however, the isokinetic probes would not.

  14. Biomass burning aerosol in the State of São Paulo (Southeastern Brazil)

    NASA Astrophysics Data System (ADS)

    Lara, L. L. S.; Artaxo, P.; Martinelli, L. A.; Camargo, P. B.; Ferraz, E. S. B.

    2003-04-01

    A detailed aerosol source apportionment study has been performed in three sites in State of São Paulo with different land-use: sugarcane crops, cattle, urban area and forest. During the summer and winter, the period when sugarcane is burned every year, PM10 has been sampled during day and night in a period of 48 hours, using stacked filters units collecting fine and coarse particulate mode, providing mass, BC and elemental concentration for each aerosol mode. The concentrations of around 20 elements were determined using particle induced X-ray emission technique (PIXE). Ion chromatography was used to determine up to 11 water-soluble ion components. Highest levels of pollutants have been measured around the sugarcane crops, where the annual PM10 concentration (57.1"45.2µgm-3) exceeds of the other urban and industrialized areas and the BC concentration is significantly higher during the sugarcane burning period (4.2"2.2 µgm-3) than the rest of the year (2.0"1.0 µgm-3). The main sources of the aerosol are correlated to the land cover. Factor and cluster analysis showed the main source int the State of São Paulo is biomass burning, followed by soil dust, biogenic emissions and industrial emissions. The sampling and analytical procedures applied in this study showed the sugarcane burning and agricultural practices are the main source of inhalable particulate, possibly altering the aerosol concentration in some places of the State of São Paulo.

  15. Robust quantum state recovery from amplitude damping within a mixed states framework

    NASA Astrophysics Data System (ADS)

    Shahrokh Esfahani, Saeideh; Liao, Zeyang; Zubairy, M. Suhail

    2016-08-01

    Due to interaction with the environment, a quantum state is subjected to decoherence which becomes one of the major problems in many quantum systems. Amplitude damping is one of the most important decoherence processes. Here, we show that general two-qubit mixed states undergoing amplitude damping can be almost completely restored using a reversal procedure. This reversal procedure through CNOT and Hadamard gates could also protect the entanglement of two-qubit mixed states from general amplitude damping. We also propose a robust recovery scheme to protect the quantum states when the decay parameters or the input quantum states are not completely known.

  16. In-situ measurements of the mixing state and optical properties of soot with implications for radiative forcing estimates

    PubMed Central

    Moffet, Ryan C.; Prather, Kimberly A.

    2009-01-01

    Our ability to predict how global temperatures will change in the future is currently limited by the large uncertainties associated with aerosols. Soot aerosols represent a major research focus as they influence climate by absorbing incoming solar radiation resulting in a highly uncertain warming effect. The uncertainty stems from the fact that the actual amount soot warms our atmosphere strongly depends on the manner and degree in which it is mixed with other species, a property referred to as mixing state. In global models and inferences from atmospheric heating measurements, soot radiative forcing estimates currently differ by a factor of 6, ranging between 0.2–1.2 W/m2, making soot second only to CO2 in terms of global warming potential. This article reports coupled in situ measurements of the size-resolved mixing state, optical properties, and aging timescales for soot particles. Fresh fractal soot particles dominate the measured absorption during peak traffic periods (6–9 AM local time). Immediately after sunrise, soot particles begin to age by developing a coating of secondary species including sulfate, ammonium, organics, nitrate, and water. Based on these direct measurements, the core-shell arrangement results in a maximum absorption enhancement of 1.6× over fresh soot. These atmospheric observations help explain the larger values for soot forcing measured by others and will be used to obtain closure in optical property measurements to reduce one of the largest remaining uncertainties in climate change. PMID:19581581

  17. Aerosol optical properties over the midcontinental United States

    NASA Technical Reports Server (NTRS)

    Halthore, Rangasayi N.; Markham, Brian L.; Ferrare, Richard A.; Aro, Theo. O.

    1992-01-01

    Solar and sky radiation measurements were analyzed to obtain aerosol properties such as the optical thickness and the size distribution. The measurements were conducted as part of the First International Satellite Land Surface Climatology Project Field Experiment during the second intensive field campaign (IFC) from June 25 to July 14, 1987, and the fifth IFC from July 25 to August 12, 1989, on the Konza Prairie near Manhattan, Kansas. Correlations with climatological and meteorological parameters show that during the period of observations in 1987, two types of air masses dominated the area: an air mass with low optical thickness and low temperature air associated with a northerly breeze, commonly referred to as the continental air, and an air mass with a higher optical thickness and higher temperature air associated with a southerly wind which we call 'Gulf air'. The size distributions show a predominance of the larger size particles in 'Gulf air'. Because of the presence of two contrasting air masses, correlations with parameters such as relative humidity, specific humidity, pressure, temperature, and North Star sky radiance reveal some interesting aspects. In 1989, clear distinctions between continental and Gulf air cannot be made; the reason for this will be discussed.

  18. Nonlocal memory effects allow perfect teleportation with mixed states.

    PubMed

    Laine, Elsi-Mari; Breuer, Heinz-Peter; Piilo, Jyrki

    2014-01-01

    One of the most striking consequences of quantum physics is quantum teleportation - the possibility to transfer quantum states over arbitrary distances. Since its theoretical introduction, teleportation has been demonstrated experimentally up to the distance of 143 km. In the original proposal two parties share a maximally entangled quantum state acting as a resource for the teleportation task. If, however, the state is influenced by decoherence, perfect teleportation can no longer be accomplished. Therefore, one of the current major challenges in accomplishing teleportation over long distances is to overcome the limitations imposed by decoherence and the subsequent mixedness of the resource state. Here we show that, in the presence of nonlocal memory effects, perfect quantum teleportation can be achieved even with mixed photon polarisation states. Our results imply that memory effects can be exploited in harnessing noisy quantum systems for quantum communication and that non-Markovianity is a resource for quantum information tasks. PMID:24714695

  19. Nonlocal memory effects allow perfect teleportation with mixed states

    PubMed Central

    Laine, Elsi-Mari; Breuer, Heinz-Peter; Piilo, Jyrki

    2014-01-01

    One of the most striking consequences of quantum physics is quantum teleportation – the possibility to transfer quantum states over arbitrary distances. Since its theoretical introduction, teleportation has been demonstrated experimentally up to the distance of 143 km. In the original proposal two parties share a maximally entangled quantum state acting as a resource for the teleportation task. If, however, the state is influenced by decoherence, perfect teleportation can no longer be accomplished. Therefore, one of the current major challenges in accomplishing teleportation over long distances is to overcome the limitations imposed by decoherence and the subsequent mixedness of the resource state. Here we show that, in the presence of nonlocal memory effects, perfect quantum teleportation can be achieved even with mixed photon polarisation states. Our results imply that memory effects can be exploited in harnessing noisy quantum systems for quantum communication and that non-Markovianity is a resource for quantum information tasks. PMID:24714695

  20. Nonlocal memory effects allow perfect teleportation with mixed states.

    PubMed

    Laine, Elsi-Mari; Breuer, Heinz-Peter; Piilo, Jyrki

    2014-01-01

    One of the most striking consequences of quantum physics is quantum teleportation - the possibility to transfer quantum states over arbitrary distances. Since its theoretical introduction, teleportation has been demonstrated experimentally up to the distance of 143 km. In the original proposal two parties share a maximally entangled quantum state acting as a resource for the teleportation task. If, however, the state is influenced by decoherence, perfect teleportation can no longer be accomplished. Therefore, one of the current major challenges in accomplishing teleportation over long distances is to overcome the limitations imposed by decoherence and the subsequent mixedness of the resource state. Here we show that, in the presence of nonlocal memory effects, perfect quantum teleportation can be achieved even with mixed photon polarisation states. Our results imply that memory effects can be exploited in harnessing noisy quantum systems for quantum communication and that non-Markovianity is a resource for quantum information tasks.

  1. Free energy surfaces in the superconducting mixed state

    NASA Technical Reports Server (NTRS)

    Finnemore, D. K.; Fang, M. M.; Bansal, N. P.; Farrell, D. E.

    1989-01-01

    The free energy surface for Tl2Ba2Ca2Cu3O1O has been measured as a function of temperature and magnetic field to determine the fundamental thermodynamic properties of the mixed state. The change in free energy, G(H)-G(O), is found to be linear in temperature over a wide range indicating that the specific heat is independent of field.

  2. Probing the quantumness of channels with mixed states

    SciTech Connect

    Haeseler, Hauke; Luetkenhaus, Norbert

    2009-10-15

    We present an alternative approach to the derivation of benchmarks for quantum channels, such as memory or teleportation channels. Using the concept of effective entanglement and the verification thereof, a testing procedure is derived which demands very few experimental resources. The procedure is generalized by allowing for mixed test states. By constructing optimized measure and reprepare channels, the benchmarks are found to be very tight in the considered experimental regimes.

  3. Phase state of ambient aerosol linked with water uptake and chemical aging in the southeastern US

    NASA Astrophysics Data System (ADS)

    Pajunoja, Aki; Hu, Weiwei; Leong, Yu J.; Taylor, Nathan F.; Miettinen, Pasi; Palm, Brett B.; Mikkonen, Santtu; Collins, Don R.; Jimenez, Jose L.; Virtanen, Annele

    2016-09-01

    During the summer 2013 Southern Aerosol and Oxidant Study (SOAS) field campaign in a rural site in the southeastern United States, the effect of hygroscopicity and composition on the phase state of atmospheric aerosol particles dominated by the organic fraction was studied. The analysis is based on hygroscopicity measurements by a Hygroscopic Tandem Differential Mobility Analyzer (HTDMA), physical phase state investigations by an Aerosol Bounce Instrument (ABI) and composition measurements using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). To study the effect of atmospheric aging on these properties, an OH-radical oxidation flow reactor (OFR) was used to simulate longer atmospheric aging times of up to 3 weeks. Hygroscopicity and bounce behavior of the particles had a clear relationship showing higher bounce at elevated relative humidity (RH) values for less hygroscopic particles, which agrees well with earlier laboratory studies. Additional OH oxidation of the aerosol particles in the OFR increased the O : C and the hygroscopicity resulting in liquefying of the particles at lower RH values. At the highest OH exposures, the inorganic fraction starts to dominate the bounce process due to production of inorganics and concurrent loss of organics in the OFR. Our results indicate that at typical ambient RH and temperature, organic-dominated particles stay mostly liquid in the atmospheric conditions in the southeastern US, but they often turn semisolid when dried below ˜ 50 % RH in the sampling inlets. While the liquid phase state suggests solution behavior and equilibrium partitioning for the SOA particles in ambient air, the possible phase change in the drying process highlights the importance of thoroughly considered sampling techniques of SOA particles.

  4. Anthropogenic Aerosols and Tropical Precipitation

    NASA Astrophysics Data System (ADS)

    Wang, C.; Kim, D.; Ekman, A. M. L.; Barth, M. C.; Rasch, P. J.

    2009-04-01

    Anthropogenic aerosols can affect the radiative balance of the Earth-atmosphere system and precipitation by acting as cloud condensation nuclei (CCN) or ice nuclei (IN) and thus modifying the optical and microphysical properties as well as lifetimes of clouds. Recent studies have also suggested that the direct radiative effect of anthropogenic aerosols, particularly absorbing aerosols, can perturb the large-scale circulation and cause a significant change in both quantity and distribution of critical tropical precipitation systems ranging from Pacific and Indian to Atlantic Oceans. This effect of aerosols on precipitation often appears in places away from aerosol-concentrated regions and current results suggest that the precipitation changes caused by it could be much more substantial than that by the microphysics-based aerosol effect. To understand the detailed mechanisms and strengths of such a "remote impact" and the climate response/feedback to anthropogenic aerosols in general, an interactive aerosol-climate model has been developed based on the Community Climate System Model (CCSM) of NCAR. Its aerosol module describes size, chemical composition, and mixing states of various sulfate and carbonaceous aerosols. Several model processes are derived based on 3D cloud-resolving model simulations. We have conducted a set of long integrations using the model driven by radiative effects of different combinations of various carbonaceous and sulfate aerosols and their mixtures. The responses of tropical precipitation systems to the forcing of these aerosols are analyzed using both model and observational data. Detailed analyses on the aerosol-precipitation causal relations of two systems: i.e., the Indian summer monsoon and Pacific ITCZ will be specifically presented.

  5. Aerosol products, mechanisms, and kinetics of heterogeneous reactions of ozone with oleic acid in pure and mixed particles.

    PubMed

    Ziemann, Paul J

    2005-01-01

    Reactions of O3 with pure and mixed oleic acid particles and bulk solutions were investigated using a thermal desorption particle beam mass spectrometer. The results provide information on the effect of particle matrix on reaction products, mechanisms, and kinetics. The major aerosol products are alpha-acyloxyalkyl hydroperoxides, secondary ozonides, alpha-alkoxyalkyl hydroperoxides, and oxocarboxylic acids formed primarily through reactions of Criegee intermediates with products or with particle matrix compounds. For example, it is estimated that for the reaction of pure oleic acid particles with O3 the aerosol products consist of approximately 68% organic peroxides, 28% 9-oxononanoic acid, and 4% azelaic acid. Although the reaction rate of pure oleic acid particles corresponds to an atmospheric lifetime of minutes, reactions in liquid/solid particle matrices can be orders of magnitude slower. The peroxide products are relatively stable when exposed to matrices typical of atmospheric particles, indicating that the lifetimes of these compounds in the atmosphere may be long enough to allow for long-range transport.

  6. Laboratory measurements of the angular light-scattering properties of internally mixed organic and sea-salt aerosol particles using polar nephelometry

    NASA Astrophysics Data System (ADS)

    Curtis, D. B.; Tinilau, S. S.

    2013-12-01

    Aerosol particles play an important, but relatively poorly understood, role in Earth's climate. Sea-salt aerosol is one of the most prevalent naturally occurring aerosols and is therefore expected to have a large effect on climate by scattering incoming solar radiation back to space. While sea-salt aerosol has been thought to be mainly composed of sodium chloride and other salts, measurements have shown the presence of biogenic organic compounds, such as glucose, in primary sea-salt aerosol particles. In addition, the sea-salt aerosol particles can become coated by secondary organics from anthropogenic activities. In order to better understand the potential climate effects of internally mixed organic and sea-salt particles, the angular scattering properties of laboratory-generated aerosols were measured at a wavelength of 532 nm using polar nephelometry. The polar nephelometer collected scattered light with an elliptical mirror and focused it across a linear CCD detector. The instrument was therefore capable of measuring the scattering intensity as a function of scattering angle (the phase function). Two incident polarizations were studied, parallel and perpendicular to the scattering plane, which were then used to calculate the degree of linear polarization. The scattering measurements along with size distribution measurements were used to retrieve the refractive index of the particles by comparison with Mie theory. Particles were generated from solutions of sodium chloride with varying concentrations of organics such as glucose and oxalic acid. In addition, particles generated from authentic sea-water were studied for comparison. Preliminary results indicate that the effective refractive indices of the mixed particles differ significantly from pure sodium chloride and do not follow simple mixing rules used to calculate refractive index from individual components.

  7. Surface and Column Aerosol Impacts of the United States' Natural Gas Transition

    NASA Astrophysics Data System (ADS)

    Burney, J. A.

    2015-12-01

    This paper quantifies the air pollution and climate impacts of the natural gas transition over the past decade in the United States. We integrate satellite and ground measurements with chemical transport modeling to understand the impact of of the large-scale shift from coal to natural gas on the quantity and chemical composition of column aerosol and surface particulate matter. We leverage the natural experiment of individual units that changed technologies (a sharp discontinuity) as well as state-level changes from old plants being taken offline and new ones being brought online (a soft discontinuity) and connect technology changes to emissions changes to detected aerosol / particulate matter changes. We use this methodology to estimate the size of the 'sulfate' mask due to coal consumption in the United States and understand more fully the climate implications of energy technology changes.

  8. Morphology of mixed primary and secondary organic particles and the adsorption of spectator organic gases during aerosol formation.

    PubMed

    Vaden, Timothy D; Song, Chen; Zaveri, Rahul A; Imre, Dan; Zelenyuk, Alla

    2010-04-13

    Primary organic aerosol (POA) and associated vapors can play an important role in determining the formation and properties of secondary organic aerosol (SOA). If SOA and POA are miscible, POA will significantly enhance SOA formation and some POA vapor will incorporate into SOA particles. When the two are not miscible, condensation of SOA on POA particles forms particles with complex morphology. In addition, POA vapor can adsorb to the surface of SOA particles increasing their mass and affecting their evaporation rates. To gain insight into SOA/POA interactions we present a detailed experimental investigation of the morphologies of SOA particles formed during ozonolysis of alpha-pinene in the presence of dioctyl phthalate (DOP) particles, serving as a simplified model of hydrophobic POA, using a single-particle mass spectrometer. Ultraviolet laser depth-profiling experiments were used to characterize two different types of mixed SOA/DOP particles: those formed by condensation of the oxidized alpha-pinene products on size-selected DOP particles and by condensation of DOP on size-selected alpha-pinene SOA particles. The results show that the hydrophilic SOA and hydrophobic DOP do not mix but instead form layered phases. In addition, an examination of homogeneously nucleated SOA particles formed in the presence of DOP vapor shows them to have an adsorbed DOP coating layer that is approximately 4 nm thick and carries 12% of the particles mass. These results may have implications for SOA formation and behavior in the atmosphere, where numerous organic compounds with various volatilities and different polarities are present.

  9. Morphology of mixed primary and secondary organic particles and the adsorption of spectator organic gases during aerosol formation.

    PubMed

    Vaden, Timothy D; Song, Chen; Zaveri, Rahul A; Imre, Dan; Zelenyuk, Alla

    2010-04-13

    Primary organic aerosol (POA) and associated vapors can play an important role in determining the formation and properties of secondary organic aerosol (SOA). If SOA and POA are miscible, POA will significantly enhance SOA formation and some POA vapor will incorporate into SOA particles. When the two are not miscible, condensation of SOA on POA particles forms particles with complex morphology. In addition, POA vapor can adsorb to the surface of SOA particles increasing their mass and affecting their evaporation rates. To gain insight into SOA/POA interactions we present a detailed experimental investigation of the morphologies of SOA particles formed during ozonolysis of alpha-pinene in the presence of dioctyl phthalate (DOP) particles, serving as a simplified model of hydrophobic POA, using a single-particle mass spectrometer. Ultraviolet laser depth-profiling experiments were used to characterize two different types of mixed SOA/DOP particles: those formed by condensation of the oxidized alpha-pinene products on size-selected DOP particles and by condensation of DOP on size-selected alpha-pinene SOA particles. The results show that the hydrophilic SOA and hydrophobic DOP do not mix but instead form layered phases. In addition, an examination of homogeneously nucleated SOA particles formed in the presence of DOP vapor shows them to have an adsorbed DOP coating layer that is approximately 4 nm thick and carries 12% of the particles mass. These results may have implications for SOA formation and behavior in the atmosphere, where numerous organic compounds with various volatilities and different polarities are present. PMID:20194795

  10. Uptake of ozone to deliquesced KI and mixed KI/NaCl aerosol particles.

    PubMed

    Rouvière, Aurélie; Sosedova, Yulia; Ammann, Markus

    2010-07-01

    The kinetics of uptake of ozone to deliquesced potassium iodide (KI) aerosol particles has been investigated in an aerosol flow tube at 72-75% relative humidity, room temperature, and atmospheric pressure. The observed loss of ozone was further analyzed in terms of a numeric model to explicitly track the iodide concentration in the particles. This allowed retrieving a value alpha(b) = 0.6 +/- (0.5)(0.4) for the bulk accommodation coefficient (alpha(b)). The second order rate constant in the bulk phase agreed with available literature (k(b) = (1.0 +/- 0.3) x 10(9) M(-1) s(-1)) even for the high ionic strength conditions of the present experiments. As long as iodide remained in excess, the average uptake coefficient was gamma = (1.10 +/- 0.20) x 10(-2). Different experiments were performed where the iodide to chloride ratio, the ozone concentration, and the surface to volume ratio of particles were varied. In combination, the results obtained indicate that uptake was driven by fast bulk accommodation and reaction in the bulk for all conditions investigated. The results further suggest that ozone uptake is not limited by the bulk accommodation coefficient alpha(b) under atmospheric conditions.

  11. Mixed polyanion glass cathodes: Glass-state conversion reactions

    SciTech Connect

    Kercher, Andrew K.; Kolopus, James A.; Carroll, Kyler; Unocic, Raymond R.; Kirklin, S.; Wolverton, C.; Stooksbury, Shelby L.; Boatner, Lynn A.; Dudney, Nancy J.

    2015-01-01

    Mixed polyanion (MP) glasses can undergo glass-state conversion (GSC) reactions to provide an alternate class of high-capacity cathode materials. GSC reactions have been demonstrated in phosphate/vanadate glasses with Ag, Co, Cu, Fe, and Ni cations. These MP glasses provided high capacity and good high power performance, but suffer from moderate voltages, large voltage hysteresis, and significant capacity fade with cycling. Details of the GSC reaction have been revealed by x-ray absorption spectroscopy, electron microscopy, and energy dispersive x-ray spectroscopy of ex situ cathodes at key states of charge. Using the Open Quantum Materials Database (OQMD), a computational thermodynamic model has been developed to predict the near-equilibrium voltages of glass-state conversion reactions in MP glasses.

  12. Mixed polyanion glass cathodes: Glass-state conversion reactions

    DOE PAGES

    Kercher, Andrew K.; Kolopus, James A.; Carroll, Kyler; Unocic, Raymond R.; Kirklin, S.; Wolverton, C.; Stooksbury, Shelby L.; Boatner, Lynn A.; Dudney, Nancy J.

    2015-01-01

    Mixed polyanion (MP) glasses can undergo glass-state conversion (GSC) reactions to provide an alternate class of high-capacity cathode materials. GSC reactions have been demonstrated in phosphate/vanadate glasses with Ag, Co, Cu, Fe, and Ni cations. These MP glasses provided high capacity and good high power performance, but suffer from moderate voltages, large voltage hysteresis, and significant capacity fade with cycling. Details of the GSC reaction have been revealed by x-ray absorption spectroscopy, electron microscopy, and energy dispersive x-ray spectroscopy of ex situ cathodes at key states of charge. Using the Open Quantum Materials Database (OQMD), a computational thermodynamic model hasmore » been developed to predict the near-equilibrium voltages of glass-state conversion reactions in MP glasses.« less

  13. Aerosols from fires: an examination of the effects on ozone photochemistry in the Western United States.

    PubMed

    Jiang, Xiaoyan; Wiedinmyer, Christine; Carlton, Annmarie G

    2012-11-01

    This study presents a first attempt to investigate the roles of fire aerosols in ozone (O(3)) photochemistry using an online coupled meteorology-chemistry model, the Weather Research and Foresting model with Chemistry (WRF-Chem). Four 1-month WRF-Chem simulations for August 2007, with and without fire emissions, were carried out to assess the sensitivity of O(3) predictions to the emissions and subsequent radiative feedbacks associated with large-scale fires in the Western United States (U.S.). Results show that decreases in planetary boundary layer height (PBLH) resulting from the radiative effects of fire aerosols and increases in emissions of nitrogen oxides (NO(x)) and volatile organic compounds (VOCs) from the fires tend to increase modeled O(3) concentrations near the source. Reductions in downward shortwave radiation reaching the surface and surface temperature due to fire aerosols cause decreases in biogenic isoprene emissions and J(NO(2)) photolysis rates, resulting in reductions in O(3) concentrations by as much as 15%. Thus, the results presented in this study imply that considering the radiative effects of fire aerosols may reduce O(3) overestimation by traditional photochemical models that do not consider fire-induced changes in meteorology; implementation of coupled meteorology-chemistry models are required to simulate the atmospheric chemistry impacted by large-scale fires.

  14. MODELING THE EFFECT OF CHLORINE EMISSIONS ON ATMOSPHERIC OZONE AND SECONDARY ORGANIC AEROSOL CONCENTRATIONS ACROSS THE UNITED STATES

    EPA Science Inventory

    This paper presents the modeled effects of natural and anthropogenic chlorine emissions on the atmospheric concentrations of ozone and secondary organic aerosol across the United States. The model calculations include anthropogenic molecular chlorine emissions, anthropogenic hypo...

  15. Regional Warming from Aerosol Removal over the United States: Results from a Transient 2010-2050 Climate Simulation

    NASA Technical Reports Server (NTRS)

    Mickley, L. J.; Leibensperger, E. M.; Jacob, D. J.; Rind, D.

    2012-01-01

    We use a general circulation model (NASA Goddard Institute for Space Studies GCM 3) to investigate the regional climate response to removal of aerosols over the United States. We perform a pair of transient 2010e2050 climate simulations following a scenario of increasing greenhouse gas concentrations, with and without aerosols over the United States and with present-day aerosols elsewhere. We find that removing U.S. aerosol significantly enhances the warming from greenhouse gases in a spatial pattern that strongly correlates with that of the aerosol. Warming is nearly negligible outside the United States, but annual mean surface temperatures increase by 0.4e0.6 K in the eastern United States. Temperatures during summer heat waves in the Northeast rise by as much as 1e2 K due to aerosol removal, driven in part by positive feedbacks involving soil moisture and low cloud cover. Reducing U.S. aerosol sources to achieve air quality objectives could thus have significant unintended regional warming consequences.

  16. Optics of water cloud droplets mixed with black-carbon aerosols.

    PubMed

    Mishchenko, Michael I; Liu, Li; Cairns, Brian; Mackowski, Daniel W

    2014-05-01

    We use the recently extended superposition T-matrix method to calculate scattering and absorption properties of micrometer-sized water droplets contaminated by black carbon. Our numerically exact results reveal that, depending on the mode of soot-water mixing, the soot specific absorption can vary by a factor exceeding 6.5. The specific absorption is maximized when the soot material is quasi-uniformly distributed throughout the droplet interior in the form of numerous small monomers. The range of mixing scenarios captured by our computations implies a wide range of remote sensing and radiation budget implications of the presence of black carbon in liquid-water clouds. We show that the popular Maxwell-Garnett effective-medium approximation can be used to calculate the optical cross sections, single-scattering albedo, and asymmetry parameter for the quasi-uniform mixing scenario, but is likely to fail in application to other mixing scenarios and in computations of the elements of the scattering matrix.

  17. Optics of Water Cloud Droplets Mixed with Black-Carbon Aerosols

    NASA Technical Reports Server (NTRS)

    Mishchenko, Michael I.; Liu, Li; Cairns, Brian; Mackowski, Daniel W.

    2014-01-01

    We use the recently extended superposition T-matrix method to calculate scattering and absorption properties of micrometer-sized water droplets contaminated by black carbon. Our numerically exact results reveal that, depending on the mode of soot-water mixing, the soot specific absorption can vary by a factor exceeding 6.5. The specific absorption is maximized when the soot material is quasi-uniformly distributed throughout the droplet interior in the form of numerous small monomers. The range of mixing scenarios captured by our computations implies a wide range of remote sensing and radiation budget implications of the presence of black carbon in liquid-water clouds. We show that the popular Maxwell-Garnett effective-medium approximation can be used to calculate the optical cross sections, single-scattering albedo, and asymmetry parameter for the quasi-uniform mixing scenario, but is likely to fail in application to other mixing scenarios and in computations of the elements of the scattering matrix.

  18. Long-term dust climatology in the western United States reconstructed from routine aerosol ground monitoring

    NASA Astrophysics Data System (ADS)

    Tong, D. Q.; Dan, M.; Wang, T.; Lee, P.

    2012-06-01

    This study introduces an observation-based dust identification approach and applies it to reconstruct long-term dust climatology in the western United States. Long-term dust climatology is important for quantifying the effects of atmospheric aerosols on regional and global climate. Although many routine aerosol monitoring networks exist, it is often difficult to obtain dust records from these networks, because these monitors are either deployed far away from dust active regions (most likely collocated with dense population) or contaminated by anthropogenic sources and other natural sources, such as wildfires and vegetation detritus. Here we propose an approach to identify local dust events relying solely on aerosol mass and composition from general-purpose aerosol measurements. Through analyzing the chemical and physical characteristics of aerosol observations during satellite-detected dust episodes, we select five indicators to be used to identify local dust records: (1) high PM10 concentrations; (2) low PM2.5/PM10 ratio; (3) higher concentrations and percentage of crustal elements; (4) lower percentage of anthropogenic pollutants; and (5) low enrichment factors of anthropogenic elements. After establishing these identification criteria, we conduct hierarchical cluster analysis for all validated aerosol measurement data over 68 IMPROVE sites in the western United States. A total of 182 local dust events were identified over 30 of the 68 locations from 2000 to 2007. These locations are either close to the four US Deserts, namely the Great Basin Desert, the Mojave Desert, the Sonoran Desert, and the Chihuahuan Desert, or in the high wind power region (Colorado). During the eight-year study period, the total number of dust events displays an interesting four-year activity cycle (one in 2000-2003 and the other in 2004-2007). The years of 2003, 2002 and 2007 are the three most active dust periods, with 46, 31 and 24 recorded dust events, respectively, while the years

  19. Complex vertical layering and mixing of aerosols over the eastern Mediterranean: active and passive remote sensing at the Cyprus University of Technology

    NASA Astrophysics Data System (ADS)

    Mamouri, R.-E.; Nisantzi, A.; Hadjimitsis, D. G.; Ansmann, A.; Schwarz, A.; Basart, S.; Baldasano, J. M.

    2013-08-01

    Aerosols can have a complicated influence on climate conditions, directly as well as indirectly via cloud formation. The southeastern Mediterranean region can be characterized as a cross road of aerosols originating from European, Asian and African continents. Complex vertical aerosol distributions are frequently detected over Cyprus by means of active remote sensing. Observations of such complex aerosol layering and comparison of the measurements with aerosol products of regional and global atmospheric transport models are required to improve our understanding of life cycles of aerosol mixtures and their impact on climate as well as on satellite remote sensing products. In this study, a case of an intense desert dust outbreak from Syria and Saudi Arabia towards the eastern Mediterranean in September 2011 is presented. The observations used in this study were performed with a 532-nm polarization Lidar and a sun/sky AERONET photometer operated at 8 channels from 340 to 1640 nm wavelength. Both instruments belong to remote sensing station of the Cyprus Technical University at Limassol, Cyprus (34°N, 33°E). The lofted dust plume was doped with air masses that crossed sources of biomass burning smoke and anthropogenic pollution. In addition, the shallow marine boundary layer over the Mediterranean Sea and over Limassol became mixed with the anthropogenic haze by sea breeze circulations. The case study demonstrates the potential of combined lidar/photometer observations to deliver detailed vertically resolved information of the aerosol characteristics in terms of particle optical and microphysical properties, separately for the spherical particle fraction as well as for the non-spherical aerosol mode.

  20. Simulation of nitrate, sulfate, and ammonium aerosols over the United States

    NASA Astrophysics Data System (ADS)

    Walker, J. M.; Seinfeld, J. H.; Clarisse, L.; Coheur, P.-F.; Clerbaux, C.; Van Damme, M.

    2012-08-01

    Atmospheric concentrations of inorganic gases and aerosols (nitrate, sulfate, and ammonium) are simulated for 2009 over the United States using the chemical transport model GEOS-Chem. This work is motivated, in part, by the inability of previous modeling studies to reproduce observed high nitrate aerosol concentrations in California. Nitrate aerosol concentrations over most of the US are over-predicted relative to Interagency Monitoring of Protected Visual Environments (IMPROVE) and Clean Air Status and Trends Network (CASTNET) data. In California, on the other hand, nitrate and ammonium are under-predicted as compared to California Air Resources Board (CARB) measurements. Over-prediction of nitrate in the East and Midwest is consistent with results of recent studies, which have suggested that nighttime nitric acid formation by heterogeneous hydrolysis of N2O5 is over-predicted with current values of the N2O5 uptake coefficient, γ, onto aerosols. Accordingly, the value of γ is reduced here by a factor of 10. Despite this, predicted nitrate levels in the US Midwest remain higher than those measured and over-prediction of nitrate in this region remains to be explained. Data from the Infrared Atmospheric Sounding Interferometer (IASI) onboard the MetOp-A satellite indicate the presence of a strong ammonia maximum in central and southern California that is not present in the simulations, which are based on the EPA National Emissions Inventory (NEI) NH3 emission inventory. In order to predict ammonia columns similar to the satellite measurements in the San Joaquin Valley, CA and Riverside, CA, the current ammonia emission inventory in California would need to be increased substantially. Based on the sensitivity of ammonium nitrate formation to the availability of ammonia, the present results suggest that under-prediction of ammonia emissions is likely the main cause for the under-prediction of nitrate aerosol in California.

  1. Final Technical Report for "Ice nuclei relation to aerosol properties: Data analysis and model parameterization for IN in mixed-phase clouds" (DOE/SC00002354)

    SciTech Connect

    Anthony Prenni; Kreidenweis, Sonia M.

    2012-09-28

    Clouds play an important role in weather and climate. In addition to their key role in the hydrologic cycle, clouds scatter incoming solar radiation and trap infrared radiation from the surface and lower atmosphere. Despite their importance, feedbacks involving clouds remain as one of the largest sources of uncertainty in climate models. To better simulate cloud processes requires better characterization of cloud microphysical processes, which can affect the spatial extent, optical depth and lifetime of clouds. To this end, we developed a new parameterization to be used in numerical models that describes the variation of ice nuclei (IN) number concentrations active to form ice crystals in mixed-phase (water droplets and ice crystals co-existing) cloud conditions as these depend on existing aerosol properties and temperature. The parameterization is based on data collected using the Colorado State University continuous flow diffusion chamber in aircraft and ground-based campaigns over a 14-year period, including data from the DOE-supported Mixed-Phase Arctic Cloud Experiment. The resulting relationship is shown to more accurately represent the variability of ice nuclei distributions in the atmosphere compared to currently used parameterizations based on temperature alone. When implemented in one global climate model, the new parameterization predicted more realistic annually averaged cloud water and ice distributions, and cloud radiative properties, especially for sensitive higher latitude mixed-phase cloud regions. As a test of the new global IN scheme, it was compared to independent data collected during the 2008 DOE-sponsored Indirect and Semi-Direct Aerosol Campaign (ISDAC). Good agreement with this new data set suggests the broad applicability of the new scheme for describing general (non-chemically specific) aerosol influences on IN number concentrations feeding mixed-phase Arctic stratus clouds. Finally, the parameterization was implemented into a regional

  2. Vertical Profiles of Aerosol Optical and Microphysical Properties During a Rare Case of Long-range Transport of Mixed Biomass Burning-polluted Dust Aerosols from the Russian Federation-kazakhstan to Athens, Greece

    NASA Astrophysics Data System (ADS)

    Papayannis, Alexandros; Argyrouli, Athina; Kokkalis, Panayotis; Tsaknakis, Georgios; Binietoglou, Ioannis; Solomos, Stavros; Kazadzis, Stylianos; Samaras, Stefanos; Böckmann, Christine; Raptis, Panagiotis; Amiridis, Vassilis

    2016-06-01

    Multi-wavelength aerosol Raman lidar measurements with elastic depolarization at 532 nm were combined with sun photometry during the HYGRA-CD campaign over Athens, Greece, on May-June 2014. We retrieved the aerosol optical [3 aerosol backscatter profiles (baer) at 355-532-1064 nm, 2 aerosol extinction (aaer) profiles at 355-532 nm and the aerosol linear depolarization ratio (δ) at 532 nm] and microphysical properties [effective radius (reff), complex refractive index (m), single scattering albedo (ω)]. We present a case study of a long distance transport (~3.500-4.000 km) of biomass burning particles mixed with dust from the Russian Federation-Kazakhstan regions arriving over Athens on 21-23 May 2014 (1.7-3.5 km height). On 23 May, between 2-2.75 km we measured mean lidar ratios (LR) of 35 sr (355 nm) and 42 sr (532 nm), while the mean Ångström exponent (AE) aerosol backscatter-related values (355nm/532nm and 532nm/1064nm) were 2.05 and 1.22, respectively; the mean value of δ at 532 nm was measured to be 9%. For that day the retrieved mean aerosol microphysical properties at 2-2.75 km height were: reff=0.26 μm (fine mode), reff=2.15 μm (coarse mode), m=1.36+0.00024i, ω=0.999 (355 nm, fine mode), ω=0.992(355 nm, coarse mode), ω=0.997 (532 nm, fine mode), and ω=0.980 (532 nm, coarse mode).

  3. Mixed-state fidelity susceptibility through iterated commutator series expansion

    NASA Astrophysics Data System (ADS)

    Tonchev, N. S.

    2014-11-01

    We present a perturbative approach to the problem of computation of mixed-state fidelity susceptibility (MFS) for thermal states. The mathematical techniques used provide an analytical expression for the MFS as a formal expansion in terms of the thermodynamic mean values of successively higher commutators of the Hamiltonian with the operator involved through the control parameter. That expression is naturally divided into two parts: the usual isothermal susceptibility and a constituent in the form of an infinite series of thermodynamic mean values which encodes the noncommutativity in the problem. If the symmetry properties of the Hamiltonian are given in terms of the generators of some (finite-dimensional) algebra, the obtained expansion may be evaluated in a closed form. This issue is tested on several popular models, for which it is shown that the calculations are much simpler if they are based on the properties from the representation theory of the Heisenberg or SU(1, 1) Lie algebra.

  4. Mixed-state fidelity susceptibility through iterated commutator series expansion.

    PubMed

    Tonchev, N S

    2014-11-01

    We present a perturbative approach to the problem of computation of mixed-state fidelity susceptibility (MFS) for thermal states. The mathematical techniques used provide an analytical expression for the MFS as a formal expansion in terms of the thermodynamic mean values of successively higher commutators of the Hamiltonian with the operator involved through the control parameter. That expression is naturally divided into two parts: the usual isothermal susceptibility and a constituent in the form of an infinite series of thermodynamic mean values which encodes the noncommutativity in the problem. If the symmetry properties of the Hamiltonian are given in terms of the generators of some (finite-dimensional) algebra, the obtained expansion may be evaluated in a closed form. This issue is tested on several popular models, for which it is shown that the calculations are much simpler if they are based on the properties from the representation theory of the Heisenberg or SU(1, 1) Lie algebra. PMID:25493736

  5. Late-occurring pulmonary pathologies following inhalation of mixed oxide (uranium + plutonium oxide) aerosol in the rat.

    PubMed

    Griffiths, N M; Van der Meeren, A; Fritsch, P; Abram, M-C; Bernaudin, J-F; Poncy, J L

    2010-09-01

    Accidental exposure by inhalation to alpha-emitting particles from mixed oxide (MOX: uranium and plutonium oxide) fuels is a potential long-term health risk to workers in nuclear fuel fabrication plants. For MOX fuels, the risk of lung cancer development may be different from that assigned to individual components (plutonium, uranium) given different physico-chemical characteristics. The objective of this study was to investigate late effects in rat lungs following inhalation of MOX aerosols of similar particle size containing 2.5 or 7.1% plutonium. Conscious rats were exposed to MOX aerosols and kept for their entire lifespan. Different initial lung burdens (ILBs) were obtained using different amounts of MOX. Lung total alpha activity was determined by external counting and at autopsy for total lung dose calculation. Fixed lung tissue was used for anatomopathological, autoradiographical, and immunohistochemical analyses. Inhalation of MOX at ILBs ranging from 1-20 kBq resulted in lung pathologies (90% of rats) including fibrosis (70%) and malignant lung tumors (45%). High ILBs (4-20 kBq) resulted in reduced survival time (N = 102; p < 0.05) frequently associated with lung fibrosis. Malignant tumor incidence increased linearly with dose (up to 60 Gy) with a risk of 1-1.6% Gy for MOX, similar to results for industrial plutonium oxide alone (1.9% Gy). Staining with antibodies against Surfactant Protein-C, Thyroid Transcription Factor-1, or Oct-4 showed differential labeling of tumor types. In conclusion, late effects following MOX inhalation result in similar risk for development of lung tumors as compared with industrial plutonium oxide.

  6. Arctic organic aerosol measurements show particles from mixed combustion in spring haze and from frost flowers in winter

    NASA Astrophysics Data System (ADS)

    Shaw, P. M.; Russell, L. M.; Jefferson, A.; Quinn, P. K.

    2010-05-01

    Submicron atmospheric aerosol particles were collected between 1 March 2008 and 1 March 2009 at Barrow, Alaska, to characterize the organic mass (OM) in the Arctic aerosol. Organic functional group concentrations and trace metals were measured with FTIR on submicron particles collected on Teflon filters. The OM varied from 0.07 μg m-3 in summer to 0.43 μg m-3 in winter, and 0.35 μg m-3 in spring, showing a transition in OM composition between spring and winter. Most of the OM in spring could be attributed to anthropogenic sources, consisting primarily of alkane and carboxylic acid functional groups and correlated to elemental tracers of industrial pollution, biomass burning, and shipping emissions. PMF analysis associated OM with two factors, a Mixed Combustion factor (MCF) and an Ocean-derived factor (ODF). Back trajectory analysis revealed that the highest fractions of the MCF were associated with air masses that had originated from northeastern Asia and the shipping lanes south of the Bering Straits. The ODF consisted of organic hydroxyl groups and correlated with organic and inorganic seawater components. The ODF accounted for more than 55% of OM in winter when the sampled air masses originated along the coastal and lake regions of the Northwest Territories of Canada. Frost flowers with organic-salt coatings that arise by brine rejection during sea ice formation may account for this large source of carbohydrate-like OM during the ice-covered winter season. While the anthropogenic sources contributed more than 0.3 μg m-3 of the springtime haze OM, ocean-derived particles provided comparable OM sources in winter.

  7. Salting Constants of Small Organic Molecules in Aerosol-Relevant Salts and Application to Aerosol Formation in the Southeastern United States

    NASA Astrophysics Data System (ADS)

    Waxman, E.; Carlton, A. M. G.; Ziemann, P. J.; Volkamer, R. M.

    2014-12-01

    Secondary organic aerosol (SOA) formation from small water-soluble molecules such as glyoxal and methyl glyoxal is a topic of emerging interest. Results from recent field campaigns, e.g. Waxman et al. (2013, GRL) and Knote et al. (2014, ACP), show that these molecules can form significant SOA mass as a result of 'salting-in'. Salting-in happens when a molecule's solubility increases with salt concentration and salting-out is the reverse. Salting effects modify the solubility exponentially with increasing salt concentration, and thus the effective Henry's law constant can strongly modify partitioning, and multiphase chemical reaction rates in aerosol water. Moreover, the solubility in aerosol water cannot easily inferred based on the solubility in cloud water, as the salting effects could change the solubility by a factor of 104 or more. In this work, we have devised and applied a novel experimental setup to measure salting constants using an ion trap mass spectrometer. We focus on small, water soluble molecules like methyl glyoxal and similar compounds and measure salting constants for aerosol-relevant salts including ammonium sulfate, ammonium nitrate, and sodium chloride. The Setschenow salting-constant values are then used to parameterize the effects of salting in CMAQ. We present a series of sensitivity studies of the effects that inorganic aerosols have on the SOA formation from small soluble molecules in the southeastern United States.

  8. Non-sulfate sulfur in fine aerosols across the United States: Insight for organosulfate prevalence

    NASA Astrophysics Data System (ADS)

    Shakya, Kabindra M.; Peltier, Richard E.

    2015-01-01

    We investigated the discrepancies in long-term sulfur measurements from 2000 to 2012 by two separate speciation methods, X-ray fluorescence (XRF) spectroscopy and ion chromatography (IC) across the United States (334 sites). Overall, there was a good correlation between sulfur measurements by XRF spectroscopy and IC (R ≥ 0.90 for most of the sites). However, the inorganic sulfate measured by ion chromatography was not sufficient to account for all the sulfur measured by XRF spectroscopy at many of the sites. Discrepancies were observed with the high ratios of sulfur measured by XRF spectroscopy to that by IC. Such high ratios also exhibited seasonal variation, and differed across land use types; significant differences occurred at locations classified as forest, agriculture, and mobile, but not in locations classified as commercial, desert, industrial, and residential. On average, the excess, or non-sulfate, sulfur (unmeasured organic sulfur or other inorganic species of sulfur) was variable and observed as high as ∼13% of organic carbon and ∼2% of PM2.5. The contribution of such assumed organosulfur was larger in the eastern region than other geographical locations in the United States. Besides the temporal and spatial trends, the additional sulfur was found to be related to other factors such as aerosol acidity and emission sources. The results suggest that these unmeasured sulfur species could have significant contribution to aerosol burden, and the understanding of these could help to control PM2.5 levels and to assess other effects of sulfur aerosols.

  9. Non-sulfate sulfur in fine aerosols across the United States: Insight for organosulfate prevalence

    PubMed Central

    Shakya, Kabindra M.; Peltier, Richard E.

    2014-01-01

    We investigated the discrepancies in long-term sulfur measurements from 2000 to 2012 by two separate speciation methods, X-ray fluorescence (XRF) spectroscopy and ion chromatography (IC) across the United States (334 sites). Overall, there was a good correlation between sulfur measurements by XRF spectroscopy and IC (R ≥ 0.90 for most of the sites). However, the inorganic sulfate measured by ion chromatography was not sufficient to account for all the sulfur measured by XRF spectroscopy at many of the sites. Discrepancies were observed with the high ratios of sulfur measured by XRF spectroscopy to that by IC. Such high ratios also exhibited seasonal variation, and differed across land use types; significant differences occurred at locations classified as forest, agriculture, and mobile, but not in locations classified as commercial, desert, industrial, and residential. On average, the excess, or non-sulfate, sulfur (unmeasured organic sulfur or other inorganic species of sulfur) was variable and observed as high as ~13% of organic carbon and ~2% of PM2.5. The contribution of such assumed organosulfur was larger in the eastern region than other geographical locations in the United States. Besides the temporal and spatial trends, the additional sulfur was found to be related to other factors such as aerosol acidity and emission sources. The results suggest that these unmeasured sulfur species could have significant contribution to aerosol burden, and the understanding of these could help to control PM2.5 levels and to assess other effects of sulfur aerosols. PMID:25620874

  10. Mixed configuration ground state in iron(II) phthalocyanine

    NASA Astrophysics Data System (ADS)

    Fernández-Rodríguez, Javier; Toby, Brian; van Veenendaal, Michel

    2015-06-01

    We calculate the angular dependence of the x-ray linear and circular dichroism at the L2 ,3 edges of α -Fe(II) Phthalocyanine (FePc) thin films using a ligand-field model with full configuration interaction. We find the best agreement with the experimental spectra for a mixed ground state of 3Eg(a1g 2eg3b2g 1) and 3B2 g(a1g 1eg4b2g 1) with the two configurations coupled by the spin-orbit interaction. The 3Eg(b ) and 3B2 g states have easy-axis and easy-plane anisotropies, respectively. Our model accounts for an easy-plane magnetic anisotropy and the measured magnitudes of the in-plane orbital and spin moments. The proximity in energy of the two configurations allows a switching of the magnetic anisotropy from easy plane to easy axis with a small change in the crystal field, as recently observed for FePc adsorbed on an oxidized Cu surface. We also discuss the possibility of a quintet ground state (5A1 g is 250 meV above the ground state) with planar anisotropy by manipulation of the Fe-C bond length by depositing the complex on a substrate that is subjected to a mechanical strain.

  11. Comparison of the mixing state of long-range transported Asian and African mineral dust

    NASA Astrophysics Data System (ADS)

    Fitzgerald, Elizabeth; Ault, Andrew P.; Zauscher, Melanie D.; Mayol-Bracero, Olga L.; Prather, Kimberly A.

    2015-08-01

    Mineral dust from arid regions represents the second largest global source of aerosols to the atmosphere. Dust strongly impacts the radiative balance of the earth's atmosphere by directly scattering solar radiation and acting as nuclei for the formation of liquid droplets and ice nuclei within clouds. The climate effects of mineral dust aerosols are poorly understood, however, due to their complex chemical and physical properties, which continuously evolve during atmospheric transport. This work focuses on characterizing atmospheric mineral dust from the two largest global dust sources: the Sahara Desert in Africa and the Gobi and Taklamakan Deserts in Asia. Measurements of individual aerosol particle size and chemical mixing state were made at El Yunque National Forest, Puerto Rico, downwind of the Sahara Desert, and Gosan, South Korea, downwind of the Gobi and Taklamakan Deserts. In general, the chemical characterization of the individual dust particles detected at these two sites reflected the dominant mineralogy of the source regions; aluminosilicate-rich dust was more common at El Yunque (∼91% of El Yunque dust particles vs. ∼69% of Gosan dust particles) and calcium-rich dust was more common at Gosan (∼22% of Gosan dust particles vs. ∼2% of El Yunque dust particles). Furthermore, dust particles from Africa and Asia were subjected to different transport conditions and atmospheric processing; African dust showed evidence of cloud processing, while Asian dust was modified via heterogeneous chemistry and direct condensation of secondary species. A larger fraction of dust detected at El Yunque contained the cloud-processing marker oxalate ion compared to dust detected at Gosan (∼20% vs ∼9%). Additionally, nearly 100% of dust detected at Gosan contained nitrate, showing it was aged via heterogeneous reactions with nitric acid, compared to only ∼60% of African dust. Information on the distinct differences in the chemical composition of mineral dust

  12. Aqueous secondary organic aerosol (SOA) production from the oxidation of phenols by triplet excited state organics

    NASA Astrophysics Data System (ADS)

    Smith, J.; Yu, L.; Zhang, Q.; Anastasio, C.

    2011-12-01

    Recent literature has shown that atmospheric condensed-phase chemistry can play a significant role in the evolution of organic aerosols, including the formation of secondary organic aerosol (SOA). SOA formation from the oxidation of volatile organic compounds (VOCs) in the aqueous phase has largely focused on oxidations involving the hydroxyl radical and other oxidants, such as photochemically created triplet excited states, have not been fully investigated. Phenolic compounds are one of the primary carbon emission classes from biomass and wood combustion and have significant water solubility. Once in the aqueous phase, phenolic compounds can react with the triplet excited states of non-phenolic aromatic carbonyls (NPCs), particle-bound organics that are also emitted in large quantities from wood combustion. The oxidation of phenolic species in the condensed phase by triplet excited states can result in the production of SOA. A main goal of this study was to investigate bulk solution reaction kinetics under atmospherically relevant conditions in order to ascertain how these reactions can impact aqueous-phase SOA production. In our experiments, we studied the reactions of five phenols (phenol, guaiacol, syringol, catechol, and resorcinol) with the triplet state of 3,4-dimethoxybenzaldehyde (34-DMB) during simulated solar radiation. We have characterized the impacts of pH, ionic strength and reactant concentrations on the reaction behavior of this system. In addition, we analyzed the SOA formed using high-resolution aerosol mass spectrometry, ion chromatography, and liquid chromatography-mass spectrometry to infer the reaction mechanisms. Our evidence suggests that under atmospherically relevant conditions, triplet excited states can be the dominant oxidant of phenolics and contribute significantly to the total SOA budget.

  13. Uncertainties of simulated aerosol optical properties induced by assumptions on aerosol physical and chemical properties: an AQMEII-2 perspective

    EPA Science Inventory

    The calculation of aerosol optical properties from aerosol mass is a process subject to uncertainty related to necessary assumptions on the treatment of the chemical species mixing state, density, refractive index, and hygroscopic growth. In the framework of the AQMEII-2 model in...

  14. Sources and mixing state of size-resolved elemental carbon particles in a European megacity: Paris

    NASA Astrophysics Data System (ADS)

    Healy, R. M.; Sciare, J.; Poulain, L.; Kamili, K.; Merkel, M.; Müller, T.; Wiedensohler, A.; Eckhardt, S.; Stohl, A.; Sarda-Estève, R.; McGillicuddy, E.; O'Connor, I. P.; Sodeau, J. R.; Wenger, J. C.

    2011-11-01

    An Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS) was deployed to investigate the size-resolved chemical composition of single particles at an urban background site in Paris, France, as part of the MEGAPOLI winter campaign in January/February 2010. ATOFMS particle counts were scaled to match coincident Twin Differential Mobility Particle Sizer (TDMPS) data in order to generate hourly size-resolved mass concentrations for the single particle classes observed. The total scaled ATOFMS particle mass concentration in the size range 150-1067 nm was found to agree very well with the sum of concurrent High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and Multi-Angle Absorption Photometer (MAAP) mass concentration measurements of organic carbon (OC), inorganic ions and black carbon (BC) (R2 = 0.91). Clustering analysis of the ATOFMS single particle mass spectra allowed the separation of elemental carbon (EC) particles into four classes: (i) EC attributed to biomass burning (ECbiomass), (ii) EC attributed to traffic (ECtraffic), (iii) EC internally mixed with OC and ammonium sulfate (ECOCSOx), and (iv) EC internally mixed with OC and ammonium nitrate (ECOCNOx). Average hourly mass concentrations for EC-containing particles detected by the ATOFMS were found to agree reasonably well with semi-continuous quantitative thermal/optical EC and optical BC measurements (r2 = 0.61 and 0.65-0.68, respectively, n = 552). The EC particle mass assigned to fossil fuel and biomass burning sources also agreed reasonably well with BC mass fractions assigned to the same sources using seven-wavelength aethalometer data (r2 = 0.60 and 0.48, respectively, n = 568). Agreement between the ATOFMS and other instrumentation improved noticeably when a period influenced by significantly aged, internally mixed EC particles was removed from the intercomparison. 88 % and 12 % of EC particle mass was apportioned to fossil fuel and biomass burning respectively using the ATOFMS data

  15. Sources and mixing state of size-resolved elemental carbon particles in a European megacity: Paris

    NASA Astrophysics Data System (ADS)

    Healy, R. M.; Sciare, J.; Poulain, L.; Kamili, K.; Merkel, M.; Müller, T.; Wiedensohler, A.; Eckhardt, S.; Stohl, A.; Sarda-Estève, R.; McGillicuddy, E.; O'Connor, I. P.; Sodeau, J. R.; Wenger, J. C.

    2012-02-01

    An Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS) was deployed to investigate the size-resolved chemical composition of single particles at an urban background site in Paris, France, as part of the MEGAPOLI winter campaign in January/February 2010. ATOFMS particle counts were scaled to match coincident Twin Differential Mobility Particle Sizer (TDMPS) data in order to generate hourly size-resolved mass concentrations for the single particle classes observed. The total scaled ATOFMS particle mass concentration in the size range 150-1067 nm was found to agree very well with the sum of concurrent High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and Multi-Angle Absorption Photometer (MAAP) mass concentration measurements of organic carbon (OC), inorganic ions and black carbon (BC) (R2 = 0.91). Clustering analysis of the ATOFMS single particle mass spectra allowed the separation of elemental carbon (EC) particles into four classes: (i) EC attributed to biomass burning (ECbiomass), (ii) EC attributed to traffic (ECtraffic), (iii) EC internally mixed with OC and ammonium sulfate (ECOCSOx), and (iv) EC internally mixed with OC and ammonium nitrate (ECOCNOx). Average hourly mass concentrations for EC-containing particles detected by the ATOFMS were found to agree reasonably well with semi-continuous quantitative thermal/optical EC and optical BC measurements (r2 = 0.61 and 0.65-0.68 respectively, n = 552). The EC particle mass assigned to fossil fuel and biomass burning sources also agreed reasonably well with BC mass fractions assigned to the same sources using seven-wavelength aethalometer data (r2 = 0.60 and 0.48, respectively, n = 568). Agreement between the ATOFMS and other instrumentation improved noticeably when a period influenced by significantly aged, internally mixed EC particles was removed from the intercomparison. 88% and 12% of EC particle mass was apportioned to fossil fuel and biomass burning respectively using the ATOFMS data

  16. Ambient black carbon particle hygroscopic properties controlled by mixing state and composition

    NASA Astrophysics Data System (ADS)

    Liu, D.; Allan, J.; Whitehead, J.; Young, D.; Flynn, M.; Coe, H.; McFiggans, G.; Fleming, Z. L.; Bandy, B.

    2013-02-01

    The wet removal of black carbon aerosol (BC) in the atmosphere is a crucial factor in determining its atmospheric lifetime and thereby the vertical and horizontal distributions, dispersion on local and regional scales, and the direct, semi-direct and indirect radiative forcing effects. The in-cloud scavenging and wet deposition rate of freshly emitted hydrophobic BC will be increased on acquisition of more-hydrophilic components by coagulation or coating processes. The lifetime of BC is still subject to considerable uncertainty for most of the model inputs, which is largely due to the insufficient constraints on the BC hydrophobic-to-hydrophilic conversion process from observational field data. This study was conducted at a site along UK North Norfolk coastline, where the BC particles were transported from different regions within Western Europe. A hygroscopicity tandem differential mobility analyser (HTDMA) was coupled with a single particle soot photometer (SP2) to measure the hygroscopic properties of BC particles and associated mixing state in real time. In addition, a Soot Particle AMS (SP-AMS) measured the chemical compositions of additional material associated with BC particles. The ensemble of BC particles persistently contained a less-hygroscopic mode at a growth factor (gf) of around 1.05 at 90% RH (dry diameter 163 nm). Importantly, a more-hygroscopic mode of BC particles was observed throughout the experiment, the gf of these BC particles extended up to ~1.4-1.6 with the minimum between this and the less hygroscopic mode at a gf ~1.25, or equivalent effective hygroscopicity parameter κ ~0.1. The gf of BC particles (gfBC) was highly influenced by the composition of associated soluble material: increases of gfBC were associated with secondary inorganic components, and these increases were more pronounced when ammonium nitrate was in the BC particles; however the presence of secondary organic matter suppressed the gfBC below that of pure inorganics. The

  17. Ambient black carbon particle hygroscopic properties controlled by mixing state and composition

    NASA Astrophysics Data System (ADS)

    Liu, D.; Allan, J.; Whitehead, J.; Young, D.; Flynn, M.; Coe, H.; McFiggans, G.; Fleming, Z.; Bandy, B.

    2012-11-01

    The wet removal of black carbon aerosol (BC) in the atmosphere is a crucial factor in determining its atmospheric lifetime and thereby the vertical and horizontal distributions, dispersion on local and regional scales, and the direct, semi-direct and indirect radiative forcing effects. The in-cloud scavenging and wet deposition rate of freshly emitted hydrophobic BC will be increased on acquisition of more-hydrophilic components by coagulation or coating processes. The lifetime of BC is still subject to considerable uncertainty for most of the model inputs, which is largely due to the insufficient constraints on the BC hydrophobic-to-hydrophilic conversion process from observational field data. This study was conducted at a site along UK North Norfolk coastline, where the BC particles were transported from different regions within Western Europe. A hygroscopicity tandem differential mobility analyser (HTDMA) was coupled with a single particle soot photometer (SP2) to measure the hygroscopic properties of BC particles and associated mixing state in real time. In addition, a Soot Particle AMS (SP-AMS) measured the chemical compositions of additional material associated with BC particles. The ensemble of BC particles persistently contained a less-hygroscopic mode at a growth factor (gf) of around 1.05 at 90% RH (dry diameter 163 nm). Importantly, a more-hygroscopic mode of BC particles was observed throughout the experiment, the gf of these BC particles extended up to ~1.4-1.6 with the minimum between this and the less hygroscopic mode at a gf ~1.25, or equivalent effective hygroscopicity parameter κ = ~0.1. The gf of BC particles (gfBC) was highly influenced by the composition of associated soluble material: increases of gfBC were associated with secondary inorganic components, and these increases were more pronounced when ammonium nitrate was in the BC particles; however the presence of secondary organic matter suppressed the gfBC below that of pure inorganics. The

  18. A State-of-the-Art Experimental Laboratory for Cloud and Cloud-Aerosol Interaction Research

    NASA Technical Reports Server (NTRS)

    Fremaux, Charles M.; Bushnell, Dennis M.

    2011-01-01

    The state of the art for predicting climate changes due to increasing greenhouse gasses in the atmosphere with high accuracy is problematic. Confidence intervals on current long-term predictions (on the order of 100 years) are so large that the ability to make informed decisions with regard to optimum strategies for mitigating both the causes of climate change and its effects is in doubt. There is ample evidence in the literature that large sources of uncertainty in current climate models are various aerosol effects. One approach to furthering discovery as well as modeling, and verification and validation (V&V) for cloud-aerosol interactions is use of a large "cloud chamber" in a complimentary role to in-situ and remote sensing measurement approaches. Reproducing all of the complex interactions is not feasible, but it is suggested that the physics of certain key processes can be established in a laboratory setting so that relevant fluid-dynamic and cloud-aerosol phenomena can be experimentally simulated and studied in a controlled environment. This report presents a high-level argument for significantly improved laboratory capability, and is meant to serve as a starting point for stimulating discussion within the climate science and other interested communities.

  19. Collection efficiency of the soot-particle aerosol mass spectrometer (SP-AMS) for internally mixed particulate black carbon

    NASA Astrophysics Data System (ADS)

    Willis, M. D.; Lee, A. K. Y.; Onasch, T. B.; Fortner, E. C.; Williams, L. R.; Lambe, A. T.; Worsnop, D. R.; Abbatt, J. P. D.

    2014-12-01

    The soot-particle aerosol mass spectrometer (SP-AMS) uses an intra-cavity infrared laser to vaporize refractory black carbon (rBC) containing particles, making the particle beam-laser beam overlap critical in determining the collection efficiency (CE) for rBC and associated non-refractory particulate matter (NR-PM). This work evaluates the ability of the SP-AMS to quantify rBC and NR-PM mass in internally mixed particles with different thicknesses of organic coating. Using apparent relative ionization efficiencies for uncoated and thickly coated rBC particles, we report measurements of SP-AMS sensitivity to NR-PM and rBC, for Regal Black, the recommended particulate calibration material. Beam width probe (BWP) measurements are used to illustrate an increase in sensitivity for highly coated particles due to narrowing of the particle beam, which enhances the CE of the SP-AMS by increasing the laser beam-particle beam overlap. Assuming complete overlap for thick coatings, we estimate CE for bare Regal Black particles of 0.6 ± 0.1, which suggests that previously measured SP-AMS sensitivities to Regal Black were underestimated by up to a factor of 2. The efficacy of the BWP measurements is highlighted by studies at a busy road in downtown Toronto and at a non-roadside location, which show particle beam widths similar to, but greater than that of bare Regal Black and coated Regal Black, respectively. Further BWP measurements at field locations will help to constrain the range of CE for fresh and aged rBC-containing particles. The ability of the SP-AMS to quantitatively assess the composition of internally mixed particles is validated through measurements of laboratory-generated organic coated particles, which demonstrate that the SP-AMS can quantify rBC and NR-PM over a wide range of particle compositions and rBC core sizes.

  20. Investigations of boundary layer structure, cloud characteristics and vertical mixing of aerosols at Barbados with large eddy simulations

    NASA Astrophysics Data System (ADS)

    Jähn, M.; Muñoz-Esparza, D.; Chouza, F.; Reitebuch, O.

    2015-08-01

    Large eddy simulations (LES) are performed for the area of the Caribbean island Barbados to investigate island effects on boundary layer modification, cloud generation and vertical mixing of aerosols. Due to the presence of a topographically structured island surface in the domain center, the model setup has to be designed with open lateral boundaries. In order to generate inflow turbulence consistent with the upstream marine boundary layer forcing, we use the cell perturbation method based on finite amplitude perturbations. In this work, this method is for the first time tested and validated for moist boundary layer simulations with open lateral boundary conditions. Observational data obtained from the SALTRACE field campaign is used for both model initialization and a comparison with Doppler wind lidar data. Several numerical sensitivity tests are carried out to demonstrate the problems related to "gray zone modeling" when using coarser spatial grid spacings beyond the inertial subrange of three-dimensional turbulence or when the turbulent marine boundary layer flow is replaced by laminar winds. Especially cloud properties in the downwind area west of Barbados are markedly affected in these kinds of simulations. Results of an additional simulation with a strong trade-wind inversion reveal its effect on cloud layer depth and location. Saharan dust layers that reach Barbados via long-range transport over the North Atlantic are included as passive tracers in the model. Effects of layer thinning, subsidence and turbulent downward transport near the layer bottom at z ~ 1800 m become apparent. The exact position of these layers and strength of downward mixing is found to be mainly controlled atmospheric stability (especially inversion strength) and wind shear. Comparisons of LES model output with wind lidar data show similarities in the formation of the daytime convective plume and the mean vertical wind structure.

  1. Investigations of boundary layer structure, cloud characteristics and vertical mixing of aerosols at Barbados with large eddy simulations

    NASA Astrophysics Data System (ADS)

    Jähn, M.; Muñoz-Esparza, D.; Chouza, F.; Reitebuch, O.; Knoth, O.; Haarig, M.; Ansmann, A.

    2016-01-01

    Large eddy simulations (LESs) are performed for the area of the Caribbean island Barbados to investigate island effects on boundary layer modification, cloud generation and vertical mixing of aerosols. Due to the presence of a topographically structured island surface in the domain center, the model setup has to be designed with open lateral boundaries. In order to generate inflow turbulence consistent with the upstream marine boundary layer forcing, we use the cell perturbation method based on finite amplitude potential temperature perturbations. In this work, this method is for the first time tested and validated for moist boundary layer simulations with open lateral boundary conditions. Observational data obtained from the SALTRACE field campaign is used for both model initialization and a comparison with Doppler wind and Raman lidar data. Several numerical sensitivity tests are carried out to demonstrate the problems related to "gray zone modeling" when using coarser spatial grid spacings beyond the inertial subrange of three-dimensional turbulence or when the turbulent marine boundary layer flow is replaced by laminar winds. Especially cloud properties in the downwind area west of Barbados are markedly affected in these kinds of simulations. Results of an additional simulation with a strong trade-wind inversion reveal its effect on cloud layer depth and location. Saharan dust layers that reach Barbados via long-range transport over the North Atlantic are included as passive tracers in the model. Effects of layer thinning, subsidence and turbulent downward transport near the layer bottom at z ≈ 1800 m become apparent. The exact position of these layers and strength of downward mixing is found to be mainly controlled atmospheric stability (especially inversion strength) and wind shear. Comparisons of LES model output with wind lidar data show similarities in the downwind vertical wind structure. Additionally, the model results accurately reproduce the

  2. Effects of anthropogenic emissions on aerosol formation from isoprene and monoterpenes in the southeastern United States

    PubMed Central

    Xu, Lu; Guo, Hongyu; Boyd, Christopher M.; Klein, Mitchel; Bougiatioti, Aikaterini; Cerully, Kate M.; Hite, James R.; Kreisberg, Nathan M.; Knote, Christoph; Olson, Kevin; Koss, Abigail; Goldstein, Allen H.; Hering, Susanne V.; de Gouw, Joost; Baumann, Karsten; Lee, Shan-Hu; Nenes, Athanasios; Weber, Rodney J.; Ng, Nga Lee

    2015-01-01

    Secondary organic aerosol (SOA) constitutes a substantial fraction of fine particulate matter and has important impacts on climate and human health. The extent to which human activities alter SOA formation from biogenic emissions in the atmosphere is largely undetermined. Here, we present direct observational evidence on the magnitude of anthropogenic influence on biogenic SOA formation based on comprehensive ambient measurements in the southeastern United States (US). Multiple high-time-resolution mass spectrometry organic aerosol measurements were made during different seasons at various locations, including urban and rural sites in the greater Atlanta area and Centreville in rural Alabama. Our results provide a quantitative understanding of the roles of anthropogenic SO2 and NOx in ambient SOA formation. We show that isoprene-derived SOA is directly mediated by the abundance of sulfate, instead of the particle water content and/or particle acidity as suggested by prior laboratory studies. Anthropogenic NOx is shown to enhance nighttime SOA formation via nitrate radical oxidation of monoterpenes, resulting in the formation of condensable organic nitrates. Together, anthropogenic sulfate and NOx can mediate 43–70% of total measured organic aerosol (29–49% of submicron particulate matter, PM1) in the southeastern US during summer. These measurements imply that future reduction in SO2 and NOx emissions can considerably reduce the SOA burden in the southeastern US. Updating current modeling frameworks with these observational constraints will also lead to more accurate treatment of aerosol formation for regions with substantial anthropogenic−biogenic interactions and consequently improve air quality and climate simulations. PMID:25535345

  3. Effects of anthropogenic emissions on aerosol formation from isoprene and monoterpenes in the southeastern United States.

    PubMed

    Xu, Lu; Guo, Hongyu; Boyd, Christopher M; Klein, Mitchel; Bougiatioti, Aikaterini; Cerully, Kate M; Hite, James R; Isaacman-VanWertz, Gabriel; Kreisberg, Nathan M; Knote, Christoph; Olson, Kevin; Koss, Abigail; Goldstein, Allen H; Hering, Susanne V; de Gouw, Joost; Baumann, Karsten; Lee, Shan-Hu; Nenes, Athanasios; Weber, Rodney J; Ng, Nga Lee

    2015-01-01

    Secondary organic aerosol (SOA) constitutes a substantial fraction of fine particulate matter and has important impacts on climate and human health. The extent to which human activities alter SOA formation from biogenic emissions in the atmosphere is largely undetermined. Here, we present direct observational evidence on the magnitude of anthropogenic influence on biogenic SOA formation based on comprehensive ambient measurements in the southeastern United States (US). Multiple high-time-resolution mass spectrometry organic aerosol measurements were made during different seasons at various locations, including urban and rural sites in the greater Atlanta area and Centreville in rural Alabama. Our results provide a quantitative understanding of the roles of anthropogenic SO2 and NOx in ambient SOA formation. We show that isoprene-derived SOA is directly mediated by the abundance of sulfate, instead of the particle water content and/or particle acidity as suggested by prior laboratory studies. Anthropogenic NOx is shown to enhance nighttime SOA formation via nitrate radical oxidation of monoterpenes, resulting in the formation of condensable organic nitrates. Together, anthropogenic sulfate and NOx can mediate 43-70% of total measured organic aerosol (29-49% of submicron particulate matter, PM1) in the southeastern US during summer. These measurements imply that future reduction in SO2 and NOx emissions can considerably reduce the SOA burden in the southeastern US. Updating current modeling frameworks with these observational constraints will also lead to more accurate treatment of aerosol formation for regions with substantial anthropogenic-biogenic interactions and consequently improve air quality and climate simulations. PMID:25535345

  4. The Effect of Recent Aerosol Trends on Solar Radiation in the Central and Southeastern United States: Implications for Regional Hydrology.

    NASA Astrophysics Data System (ADS)

    Cusworth, D.; Mickley, L. J.; Leibensperger, E. M.; Iacono, M. J.

    2015-12-01

    Observations show large increases in summertime (JJA) surface solar radiation (SWdn) over the central and southeastern United States during the last 20 years, as much as a +40 Wm-2 at midday. At the same time, in response to environmental regulations in the early 1990s, emissions of U.S. aerosol precursors have decreased by as much as 60%. Detecting a possible connection between these two trends has been difficult due to the secondary effects of aerosols on cloud concentration and lifetime, and previous efforts have failed to find a direct link. Here we investigate the clear-sky direct effect of decreasing U.S. aerosols on climate, using a radiative transfer model (RRTMG) driven by 1997-2014 measurements of aerosol optical depth at Surface Radiation Budget Network (SURFRAD) sites in the central and southeastern United States. We impose aerosol asymmetry parameters and single scattering albedos from nearby Aerosol Robotic Network (AERONET) sites. Preliminary results indicate that declining aerosols drive a summer noontime change in clear-sky SWdn of +25 Wm-2 since 1997 at Goodwin Creek, MS, accounting for 56% of the observed increase in SWdn at that site. Similarly, we find that aerosols increase clear-sky SWdn by +6.5 Wm-2 in Bondville, IL, which accounts for 21% of the observed SWdn trend there. These results suggest that the climate in these regions of the U.S. may be sensitive to recent reductions in aerosol concentrations, especially during summer months. We also analyze in situ soil measurements from the Illinois Climate Network from 1990-present, and find that a significant decrease in soil moisture (-0.6 m3 m-3 a-1) accompanies the increase in SWdn, implying a link between aerosol trends and regional hydrology. Aerosol reductions are expected to continue in the United States and may further influence regional climate including hydrological factors. Our work has implications for polluted regions outside the U.S., where future reductions in the aerosol burden

  5. Comparison of MADE3-simulated and observed aerosol distributions with a focus on aerosol vertical profiles

    NASA Astrophysics Data System (ADS)

    Kaiser, Christopher; Hendricks, Johannes; Righi, Mattia; Jöckel, Patrick

    2016-04-01

    The reliability of aerosol radiative forcing estimates from climate models depends on the accuracy of simulated global aerosol distribution and composition, as well as on the models' representation of the aerosol-cloud and aerosol-radiation interactions. To help improve on previous modeling studies, we recently developed the new aerosol microphysics submodel MADE3 that explicitly tracks particle mixing state in the Aitken, accumulation, and coarse mode size ranges. We implemented MADE3 into the global atmospheric chemistry general circulation model EMAC and evaluated it by comparison of simulated aerosol properties to observations. Compared properties include continental near-surface aerosol component concentrations and size distributions, continental and marine aerosol vertical profiles, and nearly global aerosol optical depth. Recent studies have shown the specific importance of aerosol vertical profiles for determination of the aerosol radiative forcing. Therefore, our focus here is on the evaluation of simulated vertical profiles. The observational data is taken from campaigns between 1990 and 2011 over the Pacific Ocean, over North and South America, and over Europe. The datasets include black carbon and total aerosol mass mixing ratios, as well as aerosol particle number concentrations. Compared to other models, EMAC with MADE3 yields good agreement with the observations - despite a general high bias of the simulated mass mixing ratio profiles. However, BC concentrations are generally overestimated by many models in the upper troposphere. With MADE3 in EMAC, we find better agreement of the simulated BC profiles with HIPPO data than the multi-model average of the models that took part in the AeroCom project. There is an interesting difference between the profiles from individual campaigns and more "climatological" datasets. For instance, compared to spatially and temporally localized campaigns, the model simulates a more continuous decline in both total

  6. Impacts of Venturi Turbulent Mixing on the Size Distributions of Sodium Chloride and Dioctyl-Phthalate Aerosols

    SciTech Connect

    Cheng, M-D.

    2000-08-23

    Internal combustion engines are a major source of airborne particulate matter (PM). The size of the engine PM is in the sub-micrometer range. The number of engine particles per unit volume is high, normally in the range of 10{sup 12} to 10{sup 14}. To measure the size distribution of the engine particles dilution of an aerosol sample is required. A diluter utilizing a venturi ejector mixing technique is commercially available and tested. The purpose of this investigation was to determine if turbulence created by the ejector in the mini-dilutor changes the size of particles passing through it. The results of the NaCl aerosol experiments show no discernible difference in the geometric mean diameter and geometric standard deviation of particles passing through the ejector. Similar results were found for the DOP particles. The ratio of the total number concentrations before and after the ejector indicates that a dilution ratio of approximately 20 applies equally for DOP and NaCl particles. This indicates the dilution capability of the ejector is not affected by the particle composition. The statistical analysis results of the first and second moments of a distribution indicate that the ejector may not change the major parameters (e.g., the geometric mean diameter and geometric standard deviation) characterizing the size distributions of NaCl and DOP particles. However, when the skewness was examined, it indicates that the ejector modifies the particle size distribution significantly. The ejector could change the skewness of the distribution in an unpredictable and inconsistent manner. Furthermore, when the variability of particle counts in individual size ranges as a result of the ejector is examined, one finds that the variability is greater for DOP particles in the size range of 40-150 nm than for NaCl particles in the size range of 30 to 350 nm. The numbers or particle counts in this size region are high enough that the Poisson counting errors are small (<10

  7. Mixing states of light-absorbing particles measured using a transmission electron microscope and a single-particle soot photometer in Tokyo, Japan

    NASA Astrophysics Data System (ADS)

    Adachi, Kouji; Moteki, Nobuhiro; Kondo, Yutaka; Igarashi, Yasuhito

    2016-08-01

    Light-absorbing atmospheric aerosols such as carbonaceous particles influence the climate through absorbing sunlight. The mixing states of these aerosol particles affect their optical properties. This study examines the changes in the mixing states and abundance of strongly light absorbing carbonaceous particles by using transmission electron microscopy (TEM) and single-particle soot photometer (SP2), as well as of iron oxide particles, in Tokyo, Japan. TEM and SP2 use fundamentally different detection techniques for the same light-absorbing particles. TEM allows characterization of the morphological, chemical, and structural features of individual particles, whereas SP2 optically measures the number, size, and mixing states of black carbon (BC). A comparison of the results obtained using these two techniques indicates that the peaks of high soot (nanosphere soot (ns-soot)) concentration periods agree with those of the BC concentrations determined by SP2 and that the high Fe-bearing particle fraction periods measured by TEM agree with that of high number concentrations of iron oxide particles measured using SP2 during the first half of the observation campaign. The results also show that the changes in the ns-soot/BC mixing states primarily correlate with the air mass sources, wind speed, precipitation, and photochemical processes. Nano-sized, aggregated, iron oxide particles mixed with other particles were commonly observed by using TEM during the high iron oxide particle periods. We conclude that although further quantitative comparison between TEM and SP2 data will be needed, the morphologically and optically defined ns-soot and BC, respectively, are essentially the same substance and that their mixing states are generally consistent across the techniques.

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

    NASA Astrophysics Data System (ADS)

    Giles, David M.

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

  9. Observed dimming effect during a forest fire in the southeastern United States and the role of aerosols

    NASA Astrophysics Data System (ADS)

    Prabha, Thara V.; Hoogenboom, Gerrit

    2009-06-01

    A surface dimming effect during a forest fire was observed in the incoming solar radiation measurements of the Georgia Automated Environmental Monitoring Network (AEMN). A combination of in situ AEMN and Moderate Resolution Imaging Spectroradiometer (MODIS) datasets were used to demonstrate the implications on the forecasts when aerosol radiative effects are not included in the Weather Research and Forecasting (WRF) model. The clear sky incoming radiative flux predicted by the model at the surface was overestimated when aerosol optical depths (AODs) exceeded 0.2, which in turn caused a positive temperature bias and a negative mixing ratio bias at the surface. These biases resulted from differences in the energy partitioning at the surface, where the main contribution was from enhanced sensible heat flux. The model atmosphere was also cooler and drier than the MODIS profiles, indicative of the aerosol induced warming below 6 km.

  10. Study on optical and microphysical properties of mixed aerosols from lidar during the EMEP 2012 summer campaign at 45oN 26oE

    NASA Astrophysics Data System (ADS)

    Talianu, Camelia; Nicolae, Doina; Belegante, Livio; Marmureanu, Luminita

    2013-04-01

    Aerosols optical and chemical properties in the upper layers of the atmosphere and near ground are variable, as function of the different mixtures of aerosol components resulting from their origin and transport over polluted areas. Due to a complex dynamics of air masses, the Romanian atmosphere has strong influences from dust and biomass-burning transported from South, West or East Europe. The dominant transport, and consequently the dominant aerosol type, depends on the season. As a result of the transport distance from the source and depending on the chemical and physical characteristics of the particles, tropospheric aerosols detected at Magurele, Romania, show different optical and microphysical properties than at the originating source. The differences are caused by the mixing with local particles, and also by the ageing processes and hygroscopic growth during the transport. This paper presents a statistical analysis of tropospheric aerosol optical properties during the EMEP (European Monitoring and Evaluation Programme) summer campaign (08 June - 17 July 2012), as retrieved from multiwavelength Raman and depolarization lidar data. Three elastic (1064, 532 and 355 nm), two Raman (607 and 387 nm) and one depolarization channel (532 nm parallel / 532 nm cross) are used to independently retrieve the backscatter coefficient, extinction coefficient and linear particle depolarization ratio of aerosols between 0.8 and 10 km altitude. Intensive optical parameters (Angstrom exponent, color ratios and color indexes) and microphysical parameters (effective radius, complex refractive index) from multiwavelength optical data inversion of the layer mean values are obtained. During the campaign, aerosol profiles were measured daily around sunset, following EARLINET standards. An intensive 3-days continuous measurements exercise was also performed. Layers were generally present above 2 km and bellow 6 km altitude, but descent of air masses from the free troposphere to the

  11. Abundance of fluorescent biological aerosol particles at temperatures conducive to the formation of mixed-phase and cirrus clouds

    NASA Astrophysics Data System (ADS)

    Twohy, Cynthia H.; McMeeking, Gavin R.; DeMott, Paul J.; McCluskey, Christina S.; Hill, Thomas C. J.; Burrows, Susannah M.; Kulkarni, Gourihar R.; Tanarhte, Meryem; Kafle, Durga N.; Toohey, Darin W.

    2016-07-01

    Some types of biological particles are known to nucleate ice at warmer temperatures than mineral dust, with the potential to influence cloud microphysical properties and climate. However, the prevalence of these particle types above the atmospheric boundary layer is not well known. Many types of biological particles fluoresce when exposed to ultraviolet light, and the Wideband Integrated Bioaerosol Sensor takes advantage of this characteristic to perform real-time measurements of fluorescent biological aerosol particles (FBAPs). This instrument was flown on the National Center for Atmospheric Research Gulfstream V aircraft to measure concentrations of fluorescent biological particles from different potential sources and at various altitudes over the US western plains in early autumn. Clear-air number concentrations of FBAPs between 0.8 and 12 µm diameter usually decreased with height and generally were about 10-100 L-1 in the continental boundary layer but always much lower at temperatures colder than 255 K in the free troposphere. At intermediate temperatures where biological ice-nucleating particles may influence mixed-phase cloud formation (255 K ≤ T ≤ 270 K), concentrations of fluorescent particles were the most variable and were occasionally near boundary-layer concentrations. Predicted vertical distributions of ice-nucleating particle concentrations based on FBAP measurements in this temperature regime sometimes reached typical concentrations of primary ice in clouds but were often much lower. If convection was assumed to lift boundary-layer FBAPs without losses to the free troposphere, better agreement between predicted ice-nucleating particle concentrations and typical ice crystal concentrations was achieved. Ice-nucleating particle concentrations were also measured during one flight and showed a decrease with height, and concentrations were consistent with a relationship to FBAPs established previously at the forested surface site below. The vertical

  12. Aerosol optical absorption measurements with photoacoustic spectroscopy

    NASA Astrophysics Data System (ADS)

    Liu, Kun; Wang, Lei; Liu, Qiang; Wang, Guishi; Tan, Tu; Zhang, Weijun; Chen, Weidong; Gao, Xiaoming

    2015-04-01

    Many parameters related to radiative forcing in climate research are known only with large uncertainties. And one of the largest uncertainties in global radiative forcing is the contribution from aerosols. Aerosols can scatter or absorb the electromagnetic radiation, thus may have negative or positive effects on the radiative forcing of the atmosphere, respectively [1]. And the magnitude of the effect is directly related to the quantity of light absorbed by aerosols [2,3]. Thus, sensitivity and precision measurement of aerosol optical absorption is crucial for climate research. Photoacoustic spectroscopy (PAS) is commonly recognized as one of the best candidates to measure the light absorption of aerosols [4]. A PAS based sensor for aerosol optical absorption measurement was developed. A 532 nm semiconductor laser with an effective power of 160 mW was used as a light source of the PAS sensor. The PAS sensor was calibrated by using known concentration NO2. The minimum detectable optical absorption coefficient (OAC) of aerosol was determined to be 1 Mm-1. 24 hours continues measurement of OAC of aerosol in the ambient air was carried out. And a novel three wavelength PAS aerosol OAC sensor is in development for analysis of aerosol wavelength-dependent absorption Angstrom coefficient. Reference [1] U. Lohmann and J. Feichter, Global indirect aerosol effects: a review, Atmos. Chem. Phys. 5, 715-737 (2005) [2] M. Z. Jacobson, Strong radiative heating due to the mixing state of black carbon in atmospheric aerosols, Nature 409, 695-697 (2001) [3] V. Ramanathan and G. Carmichae, Global and regional climate changes due to black carbon, nature geoscience 1, 221-227 (2008) [4] W.P Arnott, H. Moosmuller, C. F. Rogers, T. Jin, and R. Bruch, Photoacoustic spectrometer for measuring light absorption by aerosol: instrument description. Atmos. Environ. 33, 2845-2852 (1999).

  13. Collection efficiency of the Soot-Particle Aerosol Mass Spectrometer (SP-AMS) for internally mixed particulate black carbon

    DOE PAGES

    Willis, M. D.; Lee, A. K. Y.; Onasch, T. B.; Fortner, E. C.; Williams, L. R.; Lambe, A. T.; Worsnop, D. R.; Abbatt, J. P. D.

    2014-05-26

    The soot-particle aerosol mass spectrometer (SP-AMS) uses an intra-cavity infrared laser to vaporize refractory black carbon (rBC) containing particles, making the particle beam–laser beam overlap critical in determining the collection efficiency (CE) for rBC and associated non-refractory particulate matter (NR-PM). This work evaluates the ability of the SP-AMS to quantify rBC and NR-PM mass in internally mixed particles with different thicknesses of organic coating. Using apparent relative ionization efficiencies for uncoated and thickly coated rBC particles, we report measurements of SP-AMS sensitivity to NR-PM and rBC, for Regal Black, the recommended particulate calibration material. Beam width probe (BWP) measurements aremore » used to illustrate an increase in sensitivity for highly coated particles due to narrowing of the particle beam, which enhances the CE of the SP-AMS by increasing the laser beam–particle beam overlap. Assuming complete overlap for thick coatings, we estimate CE for bare Regal Black particles of 0.6 ± 0.1, which suggests that previously measured SP-AMS sensitivities to Regal Black were underestimated by up to a factor of two. The efficacy of the BWP measurements is highlighted by studies at a busy road in downtown Toronto and at a non-roadside location, which show particle beam widths similar to, but greater than that of bare Regal Black and coated Regal Black, respectively. Further BWP measurements at field locations will help to constrain the range of CE for fresh and aged rBC-containing particles. The ability of the SP-AMS to quantitatively assess the composition of internally mixed particles is validated through measurements of laboratory-generated organic coated particles, which demonstrate that the SP-AMS can quantify rBC and NR-PM over a wide range of particle compositions and rBC core sizes.« less

  14. Collection efficiency of the soot-particle aerosol mass spectrometer (SP-AMS) for internally mixed particulate black carbon

    DOE PAGES

    Willis, M. D.; Lee, A. K. Y.; Onasch, T. B.; Fortner, E. C.; Williams, L. R.; Lambe, A. T.; Worsnop, D. R.; Abbatt, J. P. D.

    2014-12-18

    The soot-particle aerosol mass spectrometer (SP-AMS) uses an intra-cavity infrared laser to vaporize refractory black carbon (rBC) containing particles, making the particle beam–laser beam overlap critical in determining the collection efficiency (CE) for rBC and associated non-refractory particulate matter (NR-PM). This work evaluates the ability of the SP-AMS to quantify rBC and NR-PM mass in internally mixed particles with different thicknesses of organic coating. Using apparent relative ionization efficiencies for uncoated and thickly coated rBC particles, we report measurements of SP-AMS sensitivity to NR-PM and rBC, for Regal Black, the recommended particulate calibration material. Beam width probe (BWP) measurements aremore » used to illustrate an increase in sensitivity for highly coated particles due to narrowing of the particle beam, which enhances the CE of the SP-AMS by increasing the laser beam–particle beam overlap. Assuming complete overlap for thick coatings, we estimate CE for bare Regal Black particles of 0.6 ± 0.1, which suggests that previously measured SP-AMS sensitivities to Regal Black were underestimated by up to a factor of 2. The efficacy of the BWP measurements is highlighted by studies at a busy road in downtown Toronto and at a non-roadside location, which show particle beam widths similar to, but greater than that of bare Regal Black and coated Regal Black, respectively. Further BWP measurements at field locations will help to constrain the range of CE for fresh and aged rBC-containing particles. The ability of the SP-AMS to quantitatively assess the composition of internally mixed particles is validated through measurements of laboratory-generated organic coated particles, which demonstrate that the SP-AMS can quantify rBC and NR-PM over a wide range of particle compositions and rBC core sizes.« less

  15. Laboratory-generated mixtures of mineral dust particles with biological substances: characterization of the particle mixing state and immersion freezing behavior

    NASA Astrophysics Data System (ADS)

    Augustin-Bauditz, Stefanie; Wex, Heike; Denjean, Cyrielle; Hartmann, Susan; Schneider, Johannes; Schmidt, Susann; Ebert, Martin; Stratmann, Frank

    2016-05-01

    Biological particles such as bacteria, fungal spores or pollen are known to be efficient ice nucleating particles. Their ability to nucleate ice is due to ice nucleation active macromolecules (INMs). It has been suggested that these INMs maintain their nucleating ability even when they are separated from their original carriers. This opens the possibility of an accumulation of such INMs in soils, resulting in an internal mixture of mineral dust and INMs. If particles from such soils which contain biological INMs are then dispersed into the atmosphere due to wind erosion or agricultural processes, they could induce ice nucleation at temperatures typical for biological substances, i.e., above -20 up to almost 0 °C, while they might be characterized as mineral dust particles due to a possibly low content of biological material. We conducted a study within the research unit INUIT (Ice Nucleation research UnIT), where we investigated the ice nucleation behavior of mineral dust particles internally mixed with INM. Specifically, we mixed a pure mineral dust sample (illite-NX) with ice active biological material (birch pollen washing water) and quantified the immersion freezing behavior of the resulting particles utilizing the Leipzig Aerosol Cloud Interaction Simulator (LACIS). A very important topic concerning the investigations presented here as well as for atmospheric application is the characterization of the mixing state of aerosol particles. In the present study we used different methods like single-particle aerosol mass spectrometry, Scanning Electron Microscopy (SEM), Energy Dispersive X-ray analysis (EDX), and a Volatility-Hygroscopicity Tandem Differential Mobility Analyser (VH-TDMA) to investigate the mixing state of our generated aerosol. Not all applied methods performed similarly well in detecting small amounts of biological material on the mineral dust particles. Measuring the hygroscopicity/volatility of the mixed particles with the VH-TDMA was the most

  16. Student ability to distinguish between superposition states and mixed states in quantum mechanics

    NASA Astrophysics Data System (ADS)

    Passante, Gina; Emigh, Paul J.; Shaffer, Peter S.

    2015-12-01

    Superposition gives rise to the probabilistic nature of quantum mechanics and is therefore one of the concepts at the heart of quantum mechanics. Although we have found that many students can successfully use the idea of superposition to calculate the probabilities of different measurement outcomes, they are often unable to identify the experimental implications of a superposition state. In particular, they fail to recognize how a superposition state and a mixed state (sometimes called a "lack of knowledge" state) can produce different experimental results. We present data that suggest that superposition in quantum mechanics is a difficult concept for students enrolled in sophomore-, junior-, and graduate-level quantum mechanics courses. We illustrate how an interactive lecture tutorial can improve student understanding of quantum mechanical superposition. A longitudinal study suggests that the impact persists after an additional quarter of quantum mechanics instruction that does not specifically address these ideas.

  17. Ice formation in Arctic mixed-phase clouds: Insights from a 3-D cloud-resolving model with size-resolved aerosol and cloud microphysics

    NASA Astrophysics Data System (ADS)

    Fan, Jiwen; Ovtchinnikov, Mikhail; Comstock, Jennifer M.; McFarlane, Sally A.; Khain, Alexander

    2009-02-01

    The single-layer mixed-phase clouds observed during the Atmospheric Radiation Measurement (ARM) program's Mixed-Phase Arctic Cloud Experiment (MPACE) are simulated with a three-dimensional cloud-resolving model, the System for Atmospheric Modeling (SAM), coupled with an explicit bin microphysics scheme and a radar simulator. By implementing an aerosol-dependent and a temperature- and supersaturation-dependent ice nucleation scheme and treating IN size distribution prognostically, the link between ice crystal and aerosol properties is established to study aerosol indirect effects. Two possible ice enhancement mechanisms, activation of droplet evaporation residues by condensation followed by freezing and droplet evaporation freezing by contact freezing inside out, are scrutinized by extensive comparisons with the in situ and remote sensing measurements. Simulations with either mechanism agree well with the in situ and remote sensing measurements of ice microphysical properties but liquid water content is slightly underpredicted. These two mechanisms give similar cloud properties, although ice nucleation occurs at very different rates and locations. Ice nucleation from activation of evaporation nuclei occurs mostly near cloud top areas, while ice nucleation from the drop freezing during evaporation has no significant location preference. Both ice enhancement mechanisms contribute dramatically to ice formation with ice particle concentration of 10-15 times higher relative to the simulation without either of them. Ice nuclei (IN) recycling from ice sublimation contributes significantly to maintaining concentrations of IN and ice particles in this case, implying an important role to maintain the observed long-term existence of mixed-phase clouds. Cloud can be very sensitive to IN initially but become much less sensitive as cloud evolves to a steady mixed-phase condition.

  18. Condensing Organic Aerosols in a Microphysical Model

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

    The condensation of organic aerosols is represented in a newly developed box-model scheme, where its effect on the growth and composition of particles are examined. We implemented the volatility-basis set (VBS) framework into the aerosol mixing state resolving microphysical scheme Multiconfiguration Aerosol TRacker of mIXing state (MATRIX). This new scheme is unique and advances the representation of organic aerosols in models in that, contrary to the traditional treatment of organic aerosols as non-volatile in most climate models and in the original version of MATRIX, this new scheme treats them as semi-volatile. Such treatment is important because low-volatility organics contribute significantly to the growth of particles. The new scheme includes several classes of semi-volatile organic compounds from the VBS framework that can partition among aerosol populations in MATRIX, thus representing the growth of particles via condensation of low volatility organic vapors. Results from test cases representing Mexico City and a Finish forrest condistions show good representation of the time evolutions of concentration for VBS species in the gas phase and in the condensed particulate phase. Emitted semi-volatile primary organic aerosols evaporate almost completely in the high volatile range, and they condense more efficiently in the low volatility range.

  19. Aerosol Optical Thickness Patterns and their Trend in the Southeastern United States

    NASA Astrophysics Data System (ADS)

    Reid, J. S.; Holben, B. N.; Zhang, J.; Campbell, J. R.; Edgerton, E.; De Gouw, J. A.; Eloranta, E. W.; Hand, J. L.; Holz, R.; Hyer, E. J.; Jacob, D. J.; Kaku, K.; kuang, S.; Lynch, P.; Newchurch, M.; Schichtel, B. A.; Shaw, S. L.; Shi, Y.; Toon, O. B.; Trepte, C. R.

    2013-12-01

    The Southeastern United States (SEUS) has long been known for its large scale regional hazes, fueled by a complex interaction of anthropogenic and biogenic emissions. Chemically, strong zonal gradients in organic to inorganic ratio coupled with high humidity also likely lead to microphysically induced variability in ambient light extinction to dry mass ratios. As part of the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) and the Southeast Nexus (SENEX) campaigns, a mesonet of Aerosol Robotic Network (AERONET) sun photometers was deployed across the SEUS in the summer of 2013. The University of Wisconsin HSRL lidar was also placed alongside an Ozone Dial lidar at the University of Alabama Huntsville. We present early results from the 2013 aerosol ground network deployment and relate findings to previous years. AERONET data is combined with MODIS and MISR satellite data along with surface particulate matter measurements to understand the regional extent of the SEUS haze and its relationship to surface particulate matter concentrations. We further examine the apparent downward trend in regional AOT. Special emphasis is placed on applying ground network data to issues of satellite data quality assurance, data assimilation and large scale modeling.

  20. Aerosol characterization over the southeastern United States using high resolution aerosol mass spectrometry: spatial and seasonal variation of aerosol composition, sources, and organic nitrates

    NASA Astrophysics Data System (ADS)

    Xu, L.; Suresh, S.; Guo, H.; Weber, R. J.; Ng, N. L.

    2015-04-01

    We deployed a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Aerosol Chemical Speciation Monitor (ACSM) to characterize the chemical composition of submicron non-refractory particles (NR-PM1) in the southeastern US. Measurements were performed in both rural and urban sites in the greater Atlanta area, GA and Centreville, AL for approximately one year, as part of Southeastern Center of Air Pollution and Epidemiology study (SCAPE) and Southern Oxidant and Aerosol Study (SOAS). Organic aerosol (OA) accounts for more than half of NR1 mass concentration regardless of sampling sites and seasons. Positive matrix factorization (PMF) analysis of HR-ToF-AMS measurements identified various OA sources, depending on location and season. Hydrocarbon-like OA (HOA) and cooking OA (COA) have important but not dominant contributions to total OA in urban sites. Biomass burning OA (BBOA) concentration shows a distinct seasonal variation with a larger enhancement in winter than summer. We find a good correlation between BBOA and brown carbon, indicating biomass burning is an important source for brown carbon, although an additional, unidentified brown carbon source is likely present at the rural Yorkville site. Isoprene-derived OA (Isoprene-OA) is only deconvolved in warmer months and contributes 18-36% of total OA. The presence of Isoprene-OA factor in urban sites is more likely from local production in the presence of NOx than transport from rural sites. More-oxidized and less-oxidized oxygenated organic aerosol (MO-OOA and LO-OOA, respectively) are dominant fractions (47-79%) of OA in all sites. MO-OOA correlates well with ozone in summer, but not in winter, indicating MO-OOA sources may vary with seasons. LO-OOA, which reaches a daily maximum at night, correlates better with estimated nitrate functionality from organic nitrates than total nitrates. Based on the HR-ToF-AMS measurements, we estimate that the nitrate functionality from organic nitrates

  1. In-line mixing states monitoring of suspensions using ultrasonic reflection technique.

    PubMed

    Zhan, Xiaobin; Yang, Yili; Liang, Jian; Zou, Dajun; Zhang, Jiaqi; Feng, Luyi; Shi, Tielin; Li, Xiwen

    2016-02-01

    Based on the measurement of echo signal changes caused by different concentration distributions in the mixing process, a simple ultrasonic reflection technique is proposed for in-line monitoring of the mixing states of suspensions in an agitated tank in this study. The relation between the echo signals and the concentration of suspensions is studied, and the mixing process of suspensions is tracked by in-line measurement of ultrasonic echo signals using two ultrasonic sensors. Through the analysis of echo signals over time, the mixing states of suspensions are obtained, and the homogeneity of suspensions is quantified. With the proposed technique, the effects of impeller diameter and agitation speed on the mixing process are studied, and the optimal agitation speed and the minimum mixing time to achieve the maximum homogeneity are acquired under different operating conditions and design parameters. The proposed technique is stable and feasible and shows great potential for in-line monitoring of mixing states of suspensions. PMID:26548526

  2. Concrete Mixing Methods and Concrete Mixers: State of the Art.

    PubMed

    Ferraris, C F

    2001-01-01

    As for all materials, the performance of concrete is determined by its microstructure. Its microstructure is determined by its composition, its curing conditions, and also by the mixing method and mixer conditions used to process the concrete. This paper gives an overview of the various types of mixing methods and concrete mixers commercially available used by the concrete industry. There are two main types of mixers used: batch mixers and continuous mixers. Batch mixers are the most common. To determine the mixing method best suited for a specific application, factors to be considered include: location of the construction site (distance from the batching plant), the amount of concrete needed, the construction schedule (volume of concrete needed per hour), and the cost. Ultimately, the quality of the concrete produced determines its performance after placement. An important measure of the quality is the homogeneity of the material after mixing. This paper will review mixing methods in regards to the quality of the concrete produced. Some procedures used to determine the effectiveness of the mixing will be examined.

  3. Concrete Mixing Methods and Concrete Mixers: State of the Art

    PubMed Central

    Ferraris, Chiara F.

    2001-01-01

    As for all materials, the performance of concrete is determined by its microstructure. Its microstructure is determined by its composition, its curing conditions, and also by the mixing method and mixer conditions used to process the concrete. This paper gives an overview of the various types of mixing methods and concrete mixers commercially available used by the concrete industry. There are two main types of mixers used: batch mixers and continuous mixers. Batch mixers are the most common. To determine the mixing method best suited for a specific application, factors to be considered include: location of the construction site (distance from the batching plant), the amount of concrete needed, the construction schedule (volume of concrete needed per hour), and the cost. Ultimately, the quality of the concrete produced determines its performance after placement. An important measure of the quality is the homogeneity of the material after mixing. This paper will review mixing methods in regards to the quality of the concrete produced. Some procedures used to determine the effectiveness of the mixing will be examined. PMID:27500029

  4. Background Southeast United States Aerosol Optical Properties and Their Dependence Upon Meteorology

    NASA Astrophysics Data System (ADS)

    Pawlyszyn, C.; West, M.; Sherman, J. P.; Link, M.; Zhou, Y.

    2015-12-01

    Aerosol effects on SE U.S. radiation budget are highly-seasonal. Aerosol loading is much higher in summer, due largely to high levels of biogenic secondary organic aerosol and sulfates. Aerosol loading is lowest in winter. Aerosol optical properties relevant to radiative forcing have been measured continuously at the Appalachian Atmospheric Interdisciplinary Research facility (AppalAIR) since the summer of 2009. AppalAIR is the only site in the eastern US to house co-located NOAA ESRL and NASA AeroNET instrumentation and is located in the mountains of Boone, NC. Lower tropospheric sub-micron (PM1) light scattering and absorption coefficients measured over seven summers and six winters are presented here, in addition to PM1 organic and sulfate aerosol mass concentrations measured during summers 2012-2013 as well as winter 2013. The objective is to determine the influence of aerosol sources and meteorology along the air mass back-trajectories on aerosol loading and composition. PM1 aerosol mass was dominated by organic aerosol and sulfate during the periods measured. Aerosol light scattering and organic aerosol concentrations were positively correlated during summer with temperature and solar flux along the parcel back-trajectory and negatively-correlated with rainfall along the back-trajectory. Wet deposition was a major factor in the difference between the upper and lower scattering coefficient quartiles for both summer and winter. Summer PM1 light scattering coefficient declined by approximately 30-40% since 2009, with smaller decreases during winter months. Long-term studies of aerosol optical properties from the regionally-representative AppalAIR site are necessary to determine the relationships between changing SE U.S. air quality and aerosol effects on regional climate and weather.

  5. Agricultural ammonia emissions and ammonium concentrations associated with aerosols and precipitation in the southeast United States

    NASA Astrophysics Data System (ADS)

    Aneja, Viney P.; Nelson, Dena R.; Roelle, Paul A.; Walker, John T.; Battye, William

    2003-02-01

    Temporal and spatial variations in ammonia (NH3) emissions and ammonium (NH4+) concentrations associated with aerosols and volume-weighted NH4+ concentration in precipitation are investigated over the period 1990-1998 in the southeast United States (Alabama, Florida, Georgia, Kentucky, North Carolina, South Carolina, Mississippi, and Tennessee). These variations were analyzed using an NH3 emissions inventory developed for the southeast United States and ambient NH4+ data from the various Clean Air Status and Trends Network (CASTNet) and the National Atmospheric Deposition Program/National Trends Network (NADP/NTN). Results show that natural log-transformed annual NH4+ concentration associated with aerosols increases with natural log-transformed annual NH3 emission density within the same county (R2 = 0.86, p < 0.0001, N = 12). Natural log-transformed annual volume-weighted average NH4+ concentration in precipitation shows only a very weak positive correlation with natural log-transformed annual NH3 emission densities within the corresponding county (R2 = 0.12, p = 0.04, N = 29). Analysis of NH4+ concentration associated with aerosols at CASTNet sites revealed that temperature, precipitation amount, and relative humidity are the most statistically significant (p < 0.05) parameters in predicting the weekly concentrations of NH4+ during the period 1990-1998. Wind speed and wind direction were also statistically significant (p < 0.05) at several CASTNet sites, but the results were less consistent. Investigation into wet NH4+ concentration in precipitation consistently yielded temperature as a statistically significant (p < 0.05) parameter at individual sites. Trends over the period 1990-1998 revealed a slight decrease in NH4+ concentration at CASTNet site SPD, Claiborne County, Tennessee (2.14-1.88 μg m-3), while positive trends in NH4+ concentration in precipitation were evident at NADP sites NC35, Sampson County, North Carolina (0.2-0.48 mg L-1) and KY35, Rowan

  6. Radiative Effects of Aerosol in the Marine Environment: Tales from the Two-Column Aerosol Project

    NASA Astrophysics Data System (ADS)

    Berg, L. K.; Fast, J. D.; Barnard, J.; Chand, D.; Chapman, E. G.; Comstock, J. M.; Ferrare, R. A.; Flynn, C. J.; Hair, J. W.; Hostetler, C. A.; Hubbe, J.; Johnson, R.; Kassianov, E.; Kluzek, C.; Laskin, A.; Lee, Y.; Mei, F.; Michalsky, J. J.; Redemann, J.; Rogers, R. R.; Russell, P. B.; Sedlacek, A. J.; Schmid, B.; Shilling, J. E.; Shinozuka, Y.; Springston, S. R.; Tomlinson, J. M.; Wilson, J. M.; Zelenyuk, A.; Berkowitz, C. M.

    2013-12-01

    single scattering albedo) as a function of height, and changes in aerosol loading, chemical composition, and mixing state with height and distance from the coast.

  7. Organic nitrate aerosol formation via NO3 + biogenic volatile organic compounds in the southeastern United States

    NASA Astrophysics Data System (ADS)

    Ayres, B. R.; Allen, H. M.; Draper, D. C.; Brown, S. S.; Wild, R. J.; Jimenez, J. L.; Day, D. A.; Campuzano-Jost, P.; Hu, W.; de Gouw, J.; Koss, A.; Cohen, R. C.; Duffey, K. C.; Romer, P.; Baumann, K.; Edgerton, E.; Takahama, S.; Thornton, J. A.; Lee, B. H.; Lopez-Hilfiker, F. D.; Mohr, C.; Wennberg, P. O.; Nguyen, T. B.; Teng, A.; Goldstein, A. H.; Olson, K.; Fry, J. L.

    2015-12-01

    Gas- and aerosol-phase measurements of oxidants, biogenic volatile organic compounds (BVOCs) and organic nitrates made during the Southern Oxidant and Aerosol Study (SOAS campaign, Summer 2013) in central Alabama show that a nitrate radical (NO3) reaction with monoterpenes leads to significant secondary aerosol formation. Cumulative losses of NO3 to terpenes are correlated with increase in gas- and aerosol-organic nitrate concentrations made during the campaign. Correlation of NO3 radical consumption to organic nitrate aerosol formation as measured by aerosol mass spectrometry and thermal dissociation laser-induced fluorescence suggests a molar yield of aerosol-phase monoterpene nitrates of 23-44 %. Compounds observed via chemical ionization mass spectrometry (CIMS) are correlated to predicted nitrate loss to BVOCs and show C10H17NO5, likely a hydroperoxy nitrate, is a major nitrate-oxidized terpene product being incorporated into aerosols. The comparable isoprene product C5H9NO5 was observed to contribute less than 1 % of the total organic nitrate in the aerosol phase and correlations show that it is principally a gas-phase product from nitrate oxidation of isoprene. Organic nitrates comprise between 30 and 45 % of the NOy budget during SOAS. Inorganic nitrates were also monitored and showed that during incidents of increased coarse-mode mineral dust, HNO3 uptake produced nitrate aerosol mass loading at a rate comparable to that of organic nitrate produced via NO3 + BVOCs.

  8. Retrieval of aerosol composition using ground-based remote sensing measurements

    NASA Astrophysics Data System (ADS)

    Xie, Yisong; Li, Zhengqiang; Zhang, Ying; Li, Donghui; Li, Kaitao

    2016-04-01

    The chemical composition and mixing states of ambient aerosol are the main factors deciding aerosol microphysical and optical properties, and thus have significant impacts on regional or global climate change and air quality. Traditional approaches to detect atmospheric aerosol composition include sampling with laboratory analysis and in-situ measurements. They can accurately acquire aerosol components, however, the sampling or air exhausting could change the status of ambient aerosol or lead to some mass loss. Additionally, aerosol is usually sampled at the surface level so that it is difficult to detect the columnar aerosol properties. Remote sensing technology, however, can overcome these problems because it is able to detect aerosol information of entire atmosphere by optical and microphysical properties without destructing the natural status of ambient aerosol. This paper introduces a method to acquire aerosol composition by the remote sensing measurements of CIMEL CE318 ground-based sun-sky radiometer. A six component aerosol model is used in this study, including one strong absorbing component Black Carbon (BC), two partly absorbing components Brown Carbon (BrC) and Mineral Dust (MD), two scattering components Ammonia Sulfate-like (AS) and Sea Salt (SS), and Aerosol Water uptake (AW). Sensitivity analysis are performed to find the most sensitive parameters to each component and retrieval method for each component is accordingly developed. Different mixing models such as Maxwell-Garnett (MG), Bruggeman (BR) and Volume Average (VA) are also studied. The residual minimization method is used by comparing remote sensing measurements and simulation outputs to find the optimization of aerosol composition (including volume fraction and mass concentration of each component). This method is applied to measurements obtained from Beijing site under different weather conditions, including polluted haze, dust storm and clean days, to investigate the impacts of mixing

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

    NASA Technical Reports Server (NTRS)

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

    2003-01-01

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

  10. Aerosol Sources, Absorption, and Intercontinental Transport: Synergies among Models, Remote Sensing, and Atmospheric Measurements

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Ginoux, Paul; Dubovik, Oleg; Holben, Brent; Kaufman, Yoram; chu, Allen; Anderson, Tad; Quinn, Patricia

    2003-01-01

    Aerosol climate forcing is one of the largest uncertainties in assessing the anthropogenic impact on the global climate system. This uncertainty arises from the poorly quantified aerosol sources, especially black carbon emissions, our limited knowledge of aerosol mixing state and optical properties, and the consequences of intercontinental transport of aerosols and their precursors. Here we use a global model GOCART to simulate atmospheric aerosols, including sulfate, black carbon, organic carbon, dust, and sea salt, from anthropogenic, biomass burning, and natural sources. We compare the model calculated aerosol extinction and absorption with those quantities from the ground-based sun photometer measurements from AERONET at several different wavelengths and the field observations from ACE-Asia, and model calculated total aerosol optical depth and fine mode fractions with the MODIS satellite retrieval. We will also estimate the intercontinental transport of pollution and dust aerosols from their source regions to other areas in different seasons.

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

    NASA Technical Reports Server (NTRS)

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

    2004-01-01

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

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

    NASA Technical Reports Server (NTRS)

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

    2004-01-01

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

  13. Aerosol Sources, Absorption, and Intercontinental Transport: Synergies Among Models, Remote Sensing, and Atmospheric Measurements

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Chu, Allen; Levy, Robert; Remer, Lorraine; Kaufman, Yoram; Dubovik, Oleg; Holben, Brent; Eck, Tom; Anderson, Tad; Quinn, Patricia

    2004-01-01

    Aerosol climate forcing is one of the largest uncertainties in assessing the anthropogenic impact on the global climate system. This uncertainty arises from the poorly quantified aerosol sources, especially black carbon emissions, our limited knowledge of aerosol mixing state and optical properties, and the consequences of intercontinental transport of aerosols and their precursors. Here we use a global model GOCART to simulate atmospheric aerosols, including sulfate, black carbon, organic carbon, dust, and sea salt, from anthropogenic, .biomass burning, and natural sources. We compare the model calculated aerosol extinction and absorption with those quantities from the ground-based sun photometer measurements from AERON" at several different wavelengths and the field observations from ACE-Asia, and model calculated total aerosol optical depth and fine mode fractions with the MODIS satellite retrieval. We will also estimate the intercontinental transport of pollution and dust aerosols from their source regions to other areas in different seasons.

  14. Sources of carbonaceous aerosols over the United States and implications for natural visibility

    NASA Astrophysics Data System (ADS)

    Park, Rokjin J.; Jacob, Daniel J.; Chin, Mian; Martin, Randall V.

    2003-06-01

    We use a global three-dimensional model (GEOS-CHEM) to better quantify the sources of elemental carbon (EC) and organic carbon (OC) aerosols in the United States through simulation of year-round observations for 1998 at a network of 45 sites (Interagency Monitoring of Protected Visual Environments (IMPROVE)). Simulation with our best a priori understanding of sources, including global satellite data to constrain fire emissions, captures most of the variance in the observations (R2 = 0.84 for EC, 0.67 for OC) with a low bias of 15% for EC and 26% for OC. Multiple linear regression to fit the IMPROVE data yields best estimates of 1998 U.S. sources of 0.60 Tg year-1 EC and 0.52 Tg year-1 OC from fossil fuel; 0.07 Tg year-1 EC and 0.89 Tg year-1 OC from biofuel; 0.08 Tg year-1 EC and 0.60 Tg year-1 OC from wildfires; and 1.10 Tg year-1 OC from vegetation. We find that fires in Mexico and Canada contributed 40-70% of annual mean natural EC in the United States for 1998 and 20-30% of annual mean natural OC. Transpacific transport from Asian pollution sources amounted to less than 10% of the natural EC and less than 2% of the natural OC; in contrast to ozone, we find that intercontinental transport of anthropogenic carbonaceous aerosols does not enhance significantly the natural background. IMPROVE observations and model simulations for the summer of 1995 show that Canadian fire emissions can produce large events of elevated EC and OC in the southeastern United States. Our best estimates of mean natural concentrations of EC and OC in the United States, using a model simulation with climatological monthly mean fire emissions, are 2-3 times higher than the default values recommended by the U.S. Environmental Protection Agency for visibility calculations, except for OC in the eastern United States (16% lower).

  15. Hygroscopic growth of size-resolved, emission-source classified, aerosol particles sampled across the United States

    NASA Astrophysics Data System (ADS)

    Shingler, T.; Crosbie, E. C.; Ziemba, L. D.; Anderson, B. E.; Campuzano Jost, P.; Jimenez, J. L.; Mikoviny, T.; Wisthaler, A.; Sorooshian, A.

    2014-12-01

    The hygroscopic growth of atmospheric aerosol particles is a key air quality parameter, impacting the radiation budget, visibility, and cloud formation. During the DC3 and SEAC4RS field campaigns (>300 total flight hours), measurements were made over 32 US states, Canada, the Pacific Ocean, and the Gulf of Mexico, between the surface and 41,000 feet ASL. The aircraft research payloads included a suite of in-situ aerosol and gas phase instruments. The Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe (DASH-SP) and the Langley Aerosol Research Group Experiment (LARGE) humidified nephelometer instrument applied different techniques to measure water uptake by aerosol particles at prescribed relative humidity values. Size-resolved growth factor (GF ≡ Dp,wet/Dp,dry) measurements by the DASH-SP are compared to bulk scattering measurements (f(RH) ≡ σscat,wet/σscat,dry) by the LARGE instrument. Spatial location and volatile organic compound tracers such as isoprene and acetonitrile are used to classify the origin of distinct air masses, including: forest fires, biogenic-emitting forests, agricultural use lands, marine boundary layer, urban, and rural background. Analyses of GF results by air mass origin are reported and results are compared with f(RH) measurements. A parameterization between the f(RH) and GF measurements and its potential uses are discussed.

  16. MATRIX-VBS Condensing Organic Aerosols in an Aerosol Microphysics Model

    NASA Technical Reports Server (NTRS)

    Gao, Chloe Y.; Tsigaridis, Konstas; Bauer, Susanne E.

    2015-01-01

    The condensation of organic aerosols is represented in a newly developed box-model scheme, where its effect on the growth and composition of particles are examined. We implemented the volatility-basis set (VBS) framework into the aerosol mixing state resolving microphysical scheme Multiconfiguration Aerosol TRacker of mIXing state (MATRIX). This new scheme is unique and advances the representation of organic aerosols in models in that, contrary to the traditional treatment of organic aerosols as non-volatile in most climate models and in the original version of MATRIX, this new scheme treats them as semi-volatile. Such treatment is important because low-volatility organics contribute significantly to the growth of particles. The new scheme includes several classes of semi-volatile organic compounds from the VBS framework that can partition among aerosol populations in MATRIX, thus representing the growth of particles via condensation of low volatility organic vapors. Results from test cases representing Mexico City and a Finish forrest condistions show good representation of the time evolutions of concentration for VBS species in the gas phase and in the condensed particulate phase. Emitted semi-volatile primary organic aerosols evaporate almost completely in the high volatile range, and they condense more efficiently in the low volatility range.

  17. Energy shift and state mixing of Rydberg atoms in ponderomotive optical traps

    NASA Astrophysics Data System (ADS)

    Wang, Xiao; Robicheaux, F.

    2016-08-01

    We present a degenerate perturbation analysis in the spin–orbit coupled basis for Rydberg atoms in an optical trap. The perturbation matrix is found to be nearly the same for two states with the same total angular momentum j, and orbital angular momentum number l differing by 1, The same perturbation matrices result in the same state-mixing and energy shift. We also study the dependence of state mixing and energy shift on the periodicity and symmetry of the ponderomotive potentials induced by different optical traps. State mixing in a one-dimensional lattice formed with two counterpropagating Gaussian beams is studied and yields a state-dependent trap depth. We also calculate the state-mixing in an optical trap formed by four parallel, separated and highly focused Gaussian beams.

  18. Aerosol and precipitation chemistry in the southwestern United States: spatiotemporal trends and interrelationships

    PubMed Central

    Sorooshian, A.; Shingler, T.; Harpold, A.; Feagles, C. W.; Meixner, T.; Brooks, P. D.

    2013-01-01

    This study characterizes the spatial and temporal patterns of aerosol and precipitation composition at six sites across the United States Southwest between 1995 and 2010. Precipitation accumulation occurs mostly during the wintertime (December–February) and during the monsoon season (July–September). Rain and snow pH levels are usually between 5–6, with crustal-derived species playing a major role in acid neutralization. These species (Ca2+, Mg2+, K+, Na+) exhibit their highest concentrations between March and June in both PM2.5 and precipitation due mostly to dust. Crustal-derived species concentrations in precipitation exhibit positive relationships with SO42−, NO3−, and Cl–, suggesting that acidic gases likely react with and partition to either crustal particles or hydrometeors enriched with crustal constituents. Concentrations of particulate SO42− show a statistically significant correlation with rain SO42− unlike snow SO42−, which may be related to some combination of the vertical distribution of SO42− (and precursors) and the varying degree to which SO42−-enriched particles act as cloud condensation nuclei versus ice nuclei in the region. The coarse : fine aerosol mass ratio was correlated with crustal species concentrations in snow unlike rain, suggestive of a preferential role of coarse particles (mainly dust) as ice nuclei in the region. Precipitation NO3− : SO42− ratios exhibit the following features with potential explanations discussed: (i) they are higher in precipitation as compared to PM2.5; (ii) they exhibit the opposite annual cycle compared to particulate NO3− : SO42− ratios; and (iii) they are higher in snow relative to rain during the wintertime. Long-term trend analysis for the monsoon season shows that the NO3− : SO42− ratio in rain increased at the majority of sites due mostly to air pollution regulations of SO42− precursors. PMID:24432030

  19. Aerosol and precipitation chemistry in the southwestern United States: spatiotemporal trends and interrelationships.

    PubMed

    Sorooshian, A; Shingler, T; Harpold, A; Feagles, C W; Meixner, T; Brooks, P D

    2013-08-01

    This study characterizes the spatial and temporal patterns of aerosol and precipitation composition at six sites across the United States Southwest between 1995 and 2010. Precipitation accumulation occurs mostly during the wintertime (December-February) and during the monsoon season (July-September). Rain and snow pH levels are usually between 5-6, with crustal-derived species playing a major role in acid neutralization. These species (Ca(2+), Mg(2+), K(+), Na(+)) exhibit their highest concentrations between March and June in both PM2.5 and precipitation due mostly to dust. Crustal-derived species concentrations in precipitation exhibit positive relationships with [Formula: see text], [Formula: see text], and Cl(-), suggesting that acidic gases likely react with and partition to either crustal particles or hydrometeors enriched with crustal constituents. Concentrations of particulate [Formula: see text] show a statistically significant correlation with rain [Formula: see text] unlike snow [Formula: see text], which may be related to some combination of the vertical distribution of [Formula: see text] (and precursors) and the varying degree to which [Formula: see text]-enriched particles act as cloud condensation nuclei versus ice nuclei in the region. The coarse : fine aerosol mass ratio was correlated with crustal species concentrations in snow unlike rain, suggestive of a preferential role of coarse particles (mainly dust) as ice nuclei in the region. Precipitation [Formula: see text] : [Formula: see text] ratios exhibit the following features with potential explanations discussed: (i) they are higher in precipitation as compared to PM2.5; (ii) they exhibit the opposite annual cycle compared to particulate [Formula: see text] : [Formula: see text] ratios; and (iii) they are higher in snow relative to rain during the wintertime. Long-term trend analysis for the monsoon season shows that the [Formula: see text] : [Formula: see text] ratio in rain increased at the

  20. GCM simulations of volcanic aerosol forcing. Part I: Climate changes induced by stead-state perturbations

    SciTech Connect

    Pollack, J.B. ); Rind, D.; Lacis, A.; Hansen, J.E.; Sato, M.; Ruedy, R. )

    1993-09-01

    The Goddard Institute for Space Studies Climate Model II was used to simulate the response of the climate system to a spatially and temporally constant forcing by volcanic aerosols. The climatic changes produced by differencing this simulation and one made for the present climate with no volcanic aerosol forcing. These climatic changes are also compared with those obtained when CO[sub 2] in the atmosphere was doubled and when the boundary conditions associated with the peak of the last ice age. In all three cases, the absolute magnitude of the change in the globally averaged air temperature at the surface is approximately 5K. The simulations imply a significant cooling of the troposphere and surface can occur at times of closely spaced, multiple, sulfur-rich volcanic explosions that span time scales of decades to centuries, such as occurred at the end of the nineteenth and beginning of the twentieth centuries. The steady-state climate response to volcanic forcing includes a expansion of sea ice, especially Southern Hemisphere; a large increase in surface and planetary albedo at high latitudes; and sizable changes in the annually and zonally averaged air temperature. The climate response to three different forcings is similar in 3 ways: direct radiative forcing accounts for 30% and 25% of the total [delta]T[sub s]; Changes in atmospheric water vapor are the most important positive feedback; Albedo feedback is significant, positive at high latitudes. The climate response to the three forcings also differs. The latitudinal profiles of [delta]T[sub s] differ, reflecting significant variations in the latitudinal profiles of the primary radiative forcing. Changes in eddy kinetic energy, heat transport by atmospheric eddies, and total atmospheric heat transport are quite different. These results raise questions about the ease with which atmospheric heat transport can be parameterized in a simple way in energy climate models. 44 refs., 32 figs.

  1. Aerosol and precipitation chemistry in the southwestern United States: spatiotemporal trends and interrelationships

    NASA Astrophysics Data System (ADS)

    Sorooshian, A.; Shingler, T.; Harpold, A.; Feagles, C. W.; Meixner, T.; Brooks, P. D.

    2013-04-01

    This study characterizes the spatial and temporal patterns of aerosol and precipitation composition at six sites across the United States Southwest between 1995 and 2010. Precipitation accumulation occurs mostly during the wintertime (December-February) and during the monsoon season (July-September). Rain and snow pH levels are usually between 5-6, with crustal-derived species playing a major role in acid neutralization. These species (Ca2+, Mg2+, K+,Na+) exhibit their highest concentrations between March and June in both PM2.5 and precipitation due mostly to dust. Crustal-derived species concentrations in precipitation exhibit positive relationships with SO42-, NO3-, and Cl-, suggesting that acidic gases likely react with and partition to either crustal particles or hydrometeors enriched with crustal constituents. Concentrations of particulate SO42- show a statistically significant correlation with rain SO42- unlike snow SO42-, which may be related to some combination of the vertical distribution of SO42- (and precursors) and the varying degree to which SO42--enriched particles act as cloud condensation nuclei versus ice nuclei in the region. The coarse : fine aerosol mass ratio was correlated with crustal species concentrations in snow unlike rain, suggestive of a preferential role of coarse particles (mainly dust) as ice nuclei in the region. Precipitation NO3- : SO42- ratios exhibit the following features with potential explanations discussed: (i) they are higher in precipitation as compared to PM2.5; (ii) they exhibit the opposite annual cycle compared to particulate NO3- : SO42- ratios; and (iii) they are higher in snow relative to rain during the wintertime. Long-term trend analysis for the monsoon season shows that the NO3- : SO42- ratio in rain decreased at the majority of sites due mostly to air pollution regulations of SO42- precursors.

  2. Aerosol and precipitation chemistry in the southwestern United States: spatiotemporal trends and interrelationships

    NASA Astrophysics Data System (ADS)

    Sorooshian, A.; Shingler, T.; Harpold, A.; Feagles, C. W.; Meixner, T.; Brooks, P. D.

    2013-08-01

    This study characterizes the spatial and temporal patterns of aerosol and precipitation composition at six sites across the United States Southwest between 1995 and 2010. Precipitation accumulation occurs mostly during the wintertime (December-February) and during the monsoon season (July-September). Rain and snow pH levels are usually between 5-6, with crustal-derived species playing a major role in acid neutralization. These species (Ca2+, Mg2+, K+, Na+) exhibit their highest concentrations between March and June in both PM2.5 and precipitation due mostly to dust. Crustal-derived species concentrations in precipitation exhibit positive relationships with SO42-, NO3-, and Cl-, suggesting that acidic gases likely react with and partition to either crustal particles or hydrometeors enriched with crustal constituents. Concentrations of particulate SO42- show a statistically significant correlation with rain SO42- unlike snow SO42-, which may be related to some combination of the vertical distribution of SO42- (and precursors) and the varying degree to which SO42--enriched particles act as cloud condensation nuclei versus ice nuclei in the region. The coarse : fine aerosol mass ratio was correlated with crustal species concentrations in snow unlike rain, suggestive of a preferential role of coarse particles (mainly dust) as ice nuclei in the region. Precipitation NO3- : SO42- ratios exhibit the following features with potential explanations discussed: (i) they are higher in precipitation as compared to PM2.5; (ii) they exhibit the opposite annual cycle compared to particulate NO3- : SO42- ratios; and (iii) they are higher in snow relative to rain during the wintertime. Long-term trend analysis for the monsoon season shows that the NO3- : SO42- ratio in rain increased at the majority of sites due mostly to air pollution regulations of SO42- precursors.

  3. Multiqubit symmetric states with maximally mixed one-qubit reductions

    NASA Astrophysics Data System (ADS)

    Baguette, D.; Bastin, T.; Martin, J.

    2014-09-01

    We present a comprehensive study of maximally entangled symmetric states of arbitrary numbers of qubits in the sense of the maximal mixedness of the one-qubit reduced density operator. A general criterion is provided to easily identify whether given symmetric states are maximally entangled in that respect or not. We show that these maximally entangled symmetric (MES) states are the only symmetric states for which the expectation value of the associated collective spin of the system vanishes, as well as in corollary the dipole moment of the Husimi function. We establish the link between this kind of maximal entanglement, the anticoherence properties of spin states, and the degree of polarization of light fields. We analyze the relationship between the MES states and the classes of states equivalent through stochastic local operations with classical communication (SLOCC). We provide a nonexistence criterion of MES states within SLOCC classes of qubit states and show in particular that the symmetric Dicke state SLOCC classes never contain such MES states, with the only exception of the balanced Dicke state class for even numbers of qubits. The 4-qubit system is analyzed exhaustively and all MES states of this system are identified and characterized. Finally the entanglement content of MES states is analyzed with respect to the geometric and barycentric measures of entanglement, as well as to the generalized N-tangle. We show that the geometric entanglement of MES states is ensured to be larger than or equal to 1/2, but also that MES states are not in general the symmetric states that maximize the investigated entanglement measures.

  4. Assessing Aerosol Mixed Layer Heights from the NASA Larc Airborne High Spectral Resolution Lidar (HSRL) during the Discover-AQ Field Campaigns

    NASA Astrophysics Data System (ADS)

    Scarino, A. J.; Ferrare, R. A.; Burton, S. P.; Hostetler, C. A.; Hair, J. W.; Rogers, R. R.; Berkoff, T.; Sawamura, P.; Collins, J. E., Jr.; Seaman, S. T.; Cook, A. L.; Harper, D. B.; Follette-Cook, M. B.; daSilva, A.; Randles, C. A.

    2014-12-01

    The first- and second-generation NASA airborne High Spectral Resolution Lidars (HSRL-1 and HSRL-2) have been deployed on board the NASA Langley Research Center King Air aircraft during the Deriving Information on Surface Conditions from Column and VERtically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) field campaigns. These included deployments during July 2011 over Washington, D.C. and Baltimore, MD, during January and February 2013 over the San Joaquin Valley of California, during September 2013 over Houston, TX and during July and August 2014 over Denver, CO. Measurements of aerosol extinction, backscatter, and depolarization are available from both HSRL-1 and HSRL-2 in coordination with other participating research aircraft and ground sites. These measurements constitute a diverse data set for use in characterizing the spatial and temporal distribution of aerosols, aerosol optical thickness (AOT), as well as the mixed layer (ML) height. Analysis of the ML height at these four locations is presented, including temporal and horizontal variability and comparisons between land and water, including the Chesapeake Bay and Galveston Bay. Using the ML heights, the distribution of AOT relative to the ML heights is determined, which is relevant for assessing the long-range transport of aerosols. The ML heights are also used to help relate column AOT measurements and extinction profiles to surface PM2.5 concentrations. The HSRL ML heights are also used to evaluate the performance in simulating the temporal and spatial variability of ML heights from both chemical regional models and global forecast models.

  5. Uncertainty relation of mixed states by means of Wigner-Yanase-Dyson information

    SciTech Connect

    Li, D.; Li, X.; Wang, F.; Huang, H.; Li, X.; Kwek, L. C.

    2009-05-15

    The variance of an observable in a quantum state is usually used to describe Heisenberg uncertainty relation. For mixed states, the variance includes quantum and classical uncertainties. By means of the skew information and the decomposition of the variance, a stronger uncertainty relation was presented by Luo [ Phys. Rev. A 72, 042110 (2005)]. In this paper, by using Wigner-Yanase-Dyson information which is a generalization of the skew information, we propose a general uncertainty relation of mixed states.

  6. “A significant source of isoprene aerosol controlled by acidity”

    EPA Science Inventory

    “A significant source of isoprene aerosol controlled by acidity” by Pye et al.Abstract: Isoprene is a significant contributor to organic aerosol in the southeastern United States where biogenic hydrocarbons mix with anthropogenic emissions. In this work, CMAQ provides explicit p...

  7. Teleportation and entanglement distillation in the presence of correlation among bipartite mixed states

    SciTech Connect

    Hamada, Mitsuru

    2003-07-01

    The teleportation channel associated with an arbitrary bipartite state denotes the map that represents the change suffered by a teleported state when the bipartite state is used instead of the ideal maximally entangled state for teleportation. This work presents and proves an explicit expression of the teleportation channel for teleportation using Weyl's projective unitary representation of (Z/dZ){sup 2n} for integers d{>=}2, n{>=}1, which has been known for n=1. This formula allows any correlation among the n bipartite mixed states, and an application shows the existence of reliable schemes for distillation of entanglement from a sequence of mixed states with correlation.

  8. 1 Mixing state and absorbing properties of black carbon during Arctic haze

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

    The Arctic atmosphere is periodically affected by the Arctic haze occurring in spring. One of its particulate components is the black carbon (BC), which is considered to be an important contributor to climate change in the Arctic region. Beside BC-cloud interaction and albedo reduction of snow, BC may influence Arctic climate interacting directly with the solar radiation, warming the corresponding aerosol layer (Flanner, 2013). Such warming depends on BC atmospheric burden and also on the efficiency of BC to absorb light, in fact the light absorption is enhanced by mixing of BC with other atmospheric non-absorbing materials (lensing effect) (Bond et al., 2013). The BC reaching the Arctic is evilly processed, due to long range transport. Aging promote internal mixing and thus absorption enhancement. Such modification of mixing and is quantification after long range transport have been observed in the Atlantic ocean (China et al., 2015) but never investigated in the Arctic. During field experiments conducted at the Zeppelin research site in Svalbard during the 2012 Arctic spring, we investigated the relative precision of different BC measuring techniques; a single particle soot photometer was then used to assess the coating of Arctic black carbon. This allowed quantifying the absorption enhancement induced by internal mixing via optical modelling; the optical assessment of aged black carbon in the arctic will be of major interest for future radiative forcing assessment.Optical characterization of the total aerosol indicated that in 2012 no extreme smoke events took place and that the aerosol population was dominated by fine and non-absorbing particles. Low mean concentration of rBC was found (30 ng m-3), with a mean mass equivalent diameter above 200 nm. rBC concentration detected with the continuous soot monitoring system and the single particle soot photometer was agreeing within 15%. Combining absorption coefficient observed with an aethalometer and rBC mass

  9. THE EFFECT OF METASTABLE EQUILIBRIUM STATES ON THE PARTITIONING OF NITRATE BETWEEN THE GAS AND AEROSOL PHASES. (R826371C005)

    EPA Science Inventory

    With the aid of three atmospheric aerosol equilibrium models, we quantify the effect of metastable equilibrium states (efflorescence branch) in comparison to stable (deliquescence branch) on the partitioning of total nitrate between the gas and aerosol phases. On average, effl...

  10. Experimental Test of Residual Error-Disturbance Uncertainty Relations for Mixed Spin-1/2 States

    NASA Astrophysics Data System (ADS)

    Demirel, Bülent; Sponar, Stephan; Sulyok, Georg; Ozawa, Masanao; Hasegawa, Yuji

    2016-09-01

    The indeterminacy inherent in quantum measurements is an outstanding character of quantum theory, which manifests itself typically in the uncertainty principle. In the last decade, several universally valid forms of error-disturbance uncertainty relations were derived for completely general quantum measurements for arbitrary states. Subsequently, Branciard established a form that is optimal for spin measurements for some pure states. However, the bound in his inequality is not stringent for mixed states. One of the present authors recently derived a new bound tight in the corresponding mixed state case. Here, a neutron-optical experiment is carried out to investigate this new relation: it is tested whether error and disturbance of quantum measurements disappear or persist in mixing up the measured ensemble. The attainability of the new bound is experimentally observed, falsifying the tightness of Branciard's bound for mixed spin states.

  11. ASSESSMENT OF THE LIQUID WATER CONTENT OF SUMMERTIME AEROSOL IN THE SOUTHEAST UNITED STATES

    EPA Science Inventory

    The concentration of aerosol liquid water mass represents an important parameter for understanding the physical properties of PM2.5 in the atmosphere. Increases in ambient relative humidity can increase aerosol liquid water and thus the composite particle mass and particle volu...

  12. High-NOON states by mixing quantum and classical light.

    PubMed

    Afek, Itai; Ambar, Oron; Silberberg, Yaron

    2010-05-14

    Precision measurements can be brought to their ultimate limit by harnessing the principles of quantum mechanics. In optics, multiphoton entangled states, known as NOON states, can be used to obtain high-precision phase measurements, becoming more and more advantageous as the number of photons grows. We generated "high-NOON" states (N = 5) by multiphoton interference of quantum down-converted light with a classical coherent state in an approach that is inherently scalable. Super-resolving phase measurements with up to five entangled photons were produced with a visibility higher than that obtainable using classical light only.

  13. Quantum teleportation of composite systems via mixed entangled states

    SciTech Connect

    Bandyopadhyay, Somshubhro; Sanders, Barry C.

    2006-09-15

    We analyze quantum teleportation for composite systems, specifically for concatenated teleporation (decomposing a large composite state into smaller states of dimension commensurate with the channel) and partial teleportation (teleporting one component of a larger quantum state). We obtain an exact expression for teleportation fidelity that depends solely on the dimension and singlet fraction for the entanglement channel and entanglement (measures by I concurrence) for the state; in fact quantum teleportation for composite systems provides an operational interpretation for I concurrence. In addition we obtain tight bounds on teleportation fidelity and prove that the average fidelity approaches the lower bound of teleportation fidelity in the high-dimension limit.

  14. Mixed-state form factors of U(1) twist fields in the Dirac theory

    NASA Astrophysics Data System (ADS)

    Chen, Yixiong

    2016-08-01

    Using the ‘Liouville space’ (the space of operators) of the massive Dirac theory, we define mixed-state form factors of U(1) twist fields. We consider mixed states with density matrices diagonal in the asymptotic particle basis. This includes the thermal Gibbs state as well as all generalized Gibbs ensembles of the Dirac theory. When the mixed state is specialized to a thermal Gibbs state, using a Riemann-Hilbert problem and low-temperature expansion, we obtain finite-temperature form factors of U(1) twist fields. We then propose the expression for form factors of U(1) twist fields in general diagonal mixed states. We verify that these form factors satisfy a system of nonlinear functional differential equations, which is derived from the trace definition of mixed-state form factors. At last, under weak analytic conditions on the eigenvalues of the density matrix, we write down the large distance form factor expansions of two-point correlation functions of these twist fields. Using the relation between the Dirac and Ising models, this provides the large-distance expansion of the Rényi entropy (for integer Rényi parameter) in the Ising model in diagonal mixed states.

  15. Mixed boundary states from 1-loop bosonic closed strings

    NASA Astrophysics Data System (ADS)

    Nardi, R.

    2013-03-01

    We analyze in a simple calculation the way 2-dimensional moduli induce a noise-like mixing between the right and left sectors of the 1-loop partition function of bosonic closed strings. As it is a direct consequence of string interactions, we argue it must be taken as a renormalization to the tree-level dynamics as far as the Wilsonian view on renormalization group is kept. We also highlight the way this noise effect brings a thermodynamical meaning to space-filling D-branes.

  16. Aerosol synthesis and electrochemical analysis of niobium mixed-metal oxides for the ethanol oxidation reaction in acid and alkaline electrolyte

    NASA Astrophysics Data System (ADS)

    Konopka, Daniel A.

    Direct ethanol fuel cells are especially important among emerging electrochemical power systems with the potential to offset a great deal of the energy demand currently met through the use of fossil fuels. Ethanol can be refined from petroleum sources or attained from renewable biomass, and is more easily and safely stored and transported than hydrogen, methanol or gasoline. The full energy potential of ethanol in fuel cells can only be realized if the reaction follows a total oxidation pathway to produce CO2. This must be achieved by the development of advanced catalysts that are electrically conductive, stable in corrosive environments, contain a high surface area on which the reaction can occur, and exhibit a bi-functional effect for the ethanol oxidation reaction (EOR). The latter criterion is achievable in mixed-metal systems. Platinum is an effective metal for catalyzing surface reactions of many adsorbates and is usually implemented in the form of Pt nanoparticles supported on inexpensive carbon. This carbon is believed to be neutral in the catalysis of Pt. Instead, carbon can be replaced with carefully designed metals and metal oxides as co-catalysis or support structures that favorably alter the electronic structure of Pt slightly through a strong metal support interaction, while also acting as an oxygen source near adsorbates to facilitate the total oxidation pathway. Niobium mixed-metal-oxides were explored in this study as bi-functional catalyst supports to Pt nanoparticles. We developed a thermal aerosol synthesis process by which mesoporous powders of mixed-metal-oxides decorated with Pt nanoparticles could be obtained from liquid precursors within ˜5 seconds or less, followed by carefully refined chemical and thermal post-treatments. Exceptionally high surface areas of 170--180m2/g were achieved via a surfactant-templated 3D wormhole-type porosity, comparable on a per volume basis to commercial carbon blacks and high surface area silica supports

  17. Entanglement and measurement-induced nonlocality of mixed maximally entangled states in multipartite dynamics

    NASA Astrophysics Data System (ADS)

    Wang, Li-Die; Wang, Li-Tao; Yang, Mou; Xu, Jing-Zhou; Wang, Z. D.; Bai, Yan-Kui

    2016-06-01

    The maximally entangled state can be in a mixed state as well as the well-known pure state. Taking the negativity as a measure of entanglement, we study the entanglement dynamics of bipartite, mixed maximally entangled states (MMESs) in multipartite cavity-reservoir systems. It is found that the MMES can exhibit the phenomenon of entanglement sudden death, which is quite different from the asymptotic decay of the pure-Bell-state case. We also find that maximal entanglement cannot guarantee maximal nonlocality, and the MMES does not correspond to the state with maximal measurement-induced nonlocality (MIN). In fact, the value and dynamic behavior of the MIN for the MMESs are dependent on the mixed-state probability. In addition, we investigate the distributions of negativity and the MIN in a multipartite system, where the two types of correlations have different monogamous properties.

  18. Negative entanglement measure for bipartite separable mixed states

    SciTech Connect

    Zhang Chengjie; Han Yongjian; Zhang Yongsheng; Wu Yuchun; Zhou Xiangfa; Guo Guangcan

    2010-12-15

    We define a negative entanglement measure for separable states which shows how much entanglement one should compensate the unentangled state, at the least, to change it into an entangled state. For two-qubit systems and some special classes of states in higher-dimensional systems, the explicit formula and the lower bounds for the negative entanglement measure (NEM) have been presented, and it always vanishes for bipartite separable pure states. The negative entanglement measure can be used as a useful quantity to describe the entanglement dynamics and the quantum phase transition. In the transverse Ising model, the first derivatives of negative entanglement measure diverge on approaching the critical value of the quantum phase transition, although these two-site reduced density matrices have no entanglement at all. In the one-dimensional (1D) Bose-Hubbard model, the NEM as a function of t/U changes from zero to negative on approaching the critical point of quantum phase transition.

  19. Control aspects of quantum computing using pure and mixed states.

    PubMed

    Schulte-Herbrüggen, Thomas; Marx, Raimund; Fahmy, Amr; Kauffman, Louis; Lomonaco, Samuel; Khaneja, Navin; Glaser, Steffen J

    2012-10-13

    Steering quantum dynamics such that the target states solve classically hard problems is paramount to quantum simulation and computation. And beyond, quantum control is also essential to pave the way to quantum technologies. Here, important control techniques are reviewed and presented in a unified frame covering quantum computational gate synthesis and spectroscopic state transfer alike. We emphasize that it does not matter whether the quantum states of interest are pure or not. While pure states underly the design of quantum circuits, ensemble mixtures of quantum states can be exploited in a more recent class of algorithms: it is illustrated by characterizing the Jones polynomial in order to distinguish between different (classes of) knots. Further applications include Josephson elements, cavity grids, ion traps and nitrogen vacancy centres in scenarios of closed as well as open quantum systems.

  20. Control aspects of quantum computing using pure and mixed states

    PubMed Central

    Schulte-Herbrüggen, Thomas; Marx, Raimund; Fahmy, Amr; Kauffman, Louis; Lomonaco, Samuel; Khaneja, Navin; Glaser, Steffen J.

    2012-01-01

    Steering quantum dynamics such that the target states solve classically hard problems is paramount to quantum simulation and computation. And beyond, quantum control is also essential to pave the way to quantum technologies. Here, important control techniques are reviewed and presented in a unified frame covering quantum computational gate synthesis and spectroscopic state transfer alike. We emphasize that it does not matter whether the quantum states of interest are pure or not. While pure states underly the design of quantum circuits, ensemble mixtures of quantum states can be exploited in a more recent class of algorithms: it is illustrated by characterizing the Jones polynomial in order to distinguish between different (classes of) knots. Further applications include Josephson elements, cavity grids, ion traps and nitrogen vacancy centres in scenarios of closed as well as open quantum systems. PMID:22946034

  1. Mixing state of regionally transported soot particles and the coating effect on their size and shape at a mountain site in Japan

    NASA Astrophysics Data System (ADS)

    Adachi, Kouji; Zaizen, Yuji; Kajino, Mizuo; Igarashi, Yasuhito

    2014-05-01

    Soot particles influence the global climate through interactions with sunlight. A coating on soot particles increases their light absorption by increasing their absorption cross section and cloud condensation nuclei activity when mixed with other hygroscopic aerosol components. Therefore, it is important to understand how soot internally mixes with other materials to accurately simulate its effects in climate models. In this study, we used a transmission electron microscope (TEM) with an auto particle analysis system, which enables more particles to be analyzed than a conventional TEM. Using the TEM, soot particle size and shape (shape factor) were determined with and without coating from samples collected at a remote mountain site in Japan. The results indicate that ~10% of aerosol particles between 60 and 350 nm in aerodynamic diameters contain or consist of soot particles and ~75% of soot particles were internally mixed with nonvolatile ammonium sulfate or other materials. In contrast to an assumption that coatings change soot shape, both internally and externally mixed soot particles had similar shape and size distributions. Larger aerosol particles had higher soot mixing ratios, i.e., more than 40% of aerosol particles with diameters >1 µm had soot inclusions, whereas <20% of aerosol particles with diameters <1 µm included soot. Our results suggest that climate models may use the same size distributions and shapes for both internally and externally mixed soot; however, changing the soot mixing ratios in the different aerosol size bins is necessary.

  2. Quasiparticle-phonon model and quadrupole mixed-symmetry states of 96Ru

    NASA Astrophysics Data System (ADS)

    Stoyanov, Ch.; Pietralla, N.

    2016-01-01

    The structure of low-lying quadrupole states of 96Ru was calculated within the Quasiparticle-Phonon Model. It is shown that symmetric and mixed-symmetry properties manifest themselves via the structure of the excited states. The first 2+ state is collective and neutron and proton transition matrix elements Mn and Mp are in-phase, while the neutron and proton transition matrix elements Mn and Mp have opposite signs for the third 2+ state. This property of the third 2+ state leads to a large M1 transition between the first and third 2+ states. It is an unambigous demonstration of the mixed-symmetry nature of the third 2+ state. The structure of the first 1+ state is calculated. The state is a member of the two-phonon multiplet generated by the coupling of the [21+]QRPA and the [22+]QRPA states.

  3. Theory of CW lidar aerosol backscatter measurements and development of a 2.1 microns solid-state pulsed laser radar for aerosol backscatter profiling

    NASA Technical Reports Server (NTRS)

    Kavaya, Michael J.; Henderson, Sammy W.; Frehlich, R. G.

    1991-01-01

    The performance and calibration of a focused, continuous wave, coherent detection CO2 lidar operated for the measurement of atmospheric backscatter coefficient, B(m), was examined. This instrument functions by transmitting infrared (10 micron) light into the atmosphere and collecting the light which is scattered in the rearward direction. Two distinct modes of operation were considered. In volume mode, the scattered light energy from many aerosols is detected simultaneously, whereas in the single particle mode (SPM), the scattered light energy from a single aerosol is detected. The analysis considered possible sources of error for each of these two cases, and also considered the conditions where each technique would have superior performance. The analysis showed that, within reasonable assumptions, the value of B(m) could be accurately measured by either the VM or the SPM method. The understanding of the theory developed during the analysis was also applied to a pulsed CO2 lidar. Preliminary results of field testing of a solid state 2 micron lidar using a CW oscillator is included.

  4. Seasonal variations in Titan's stratosphere observed with Cassini/CIRS: temperature, trace molecular gas and aerosol mixing ratio profiles

    NASA Astrophysics Data System (ADS)

    Vinatier, S.; Bézard, B.; Anderson, C.; Teanby, N.; Lebonnois, S.; Rannou, P.; de Kok, R.; T. CIRS Team

    2013-09-01

    Titan's northern spring equinox occurred in August 2009. General Circulation Models (e.g. [1]) predict strong modifications of the global circulation in this period, with formation of two circulation cells instead of the pole-to-pole cell that occurred during northern winter. This winter single cell, which had its descending branch at the north pole, was at the origin of the enrichment of molecular abundances and high stratopause temperatures observed by Cassini/CIRS at high northern latitudes (e.g., [2], [3], [4], [5]). The predicted dynamical seasonal variations after the equinox have strong impact on the spatial distributions of trace gas, temperature and aerosol abundances. We will present here an analysis of CIRS limbgeometry datasets acquired in 2010, 2011 and 2012 that we used to monitor the seasonal evolution of the vertical profiles of temperature, molecular (C2H2, C2H6, HCN, ...) and aerosol abundances.

  5. Characteristics of Chinese aerosols determined by individual-particle analysis

    NASA Astrophysics Data System (ADS)

    Gao, Yuan; Anderson, James R.

    2001-08-01

    Tropospheric aerosols that originate in China and are transported over the North Pacific Ocean have potentially significant impacts on regional and global climate. These aerosols are complex mixtures of soil dust and anthropogenic particles from a variety of sources, including fossil fuel combustion, biomass burning, mining, smelting, and other industrial processes, plus reaction products of heterogeneous processes that affect these particles during transport. In the coastal marine atmosphere, these particles could be further mixed with marine aerosols. To provide examples of the diversity of chemical and physical properties of east Asian aerosols in the spring, individual aerosol particle samples were collected in April and May 1999 in three different environments in China: Qingdao on the coast of the East China Sea, Beijing in the northeast interior, and Mount Waliguan in remote northwestern China. Results reveal that aerosols in this region are complex and heterogeneous. In addition to significant differences in aerosol composition and size distributions among the samples, each sample contains a large number of polyphase aggregates. Many of the particles also have irregular shapes; for a number of the particle types, the irregular shapes should persist even at high ambient RH. Because composition, degree and nature of polyphase aggregation, and shape all effect aerosol radiative properties, the complex state of east Asian aerosols presents a challenge for the modeling of aerosol radiative forcing in the region.

  6. LASE measurements of aerosols and water vapor during TARFOX

    NASA Technical Reports Server (NTRS)

    Ferrare, Richard A.; Ismail, Syed; Browell, Edward V.; Brackett, Vincent G.; Kooi, Susan A.; Clayton, Marian B.; Melfi, Harvey; Whiteman, David N.; Schwenner, Geary; Evans, Keith D.; Hobbs, Peter V.; Veefkind, J. Pepijn; Russell, Philip B.; Livingston, John M.; Hignett, Philip; Holben, Brent N.; Remer, Lorraine A.

    1998-01-01

    The TARFOX (Tropospheric Aerosol Radiative Forcing Observational Experiment) intensive field campaign was designed to reduce uncertainties in estimates of the effects of anthropogenic aerosols on climate by measuring direct radiative effects and the optical, physical, and chemical properties of aerosols [1]. TARFOX was conducted off the East Coast of the United States between July 10-31, 1996. Ground, aircraft, and satellite-based sensors measured the sensitivity of radiative fields at various atmospheric levels to aerosol optical properties (i.e., optical thickness, phase function, single-scattering albedo) and to the vertical profile of aerosols. The LASE (Lidar Atmospheric Sensing Experiment) instrument, which was flown on the NASA ER-2 aircraft, measured vertical profiles of total scattering ratio and water vapor during a series of 9 flights. These profiles were used in real-time to help direct the other aircraft to the appropriate altitudes for intensive sampling of aerosol layers. We have subsequently used the LASE aerosol data to derive aerosol backscattering and extinction profiles. Using these aerosol extinction profiles, we derived estimates of aerosol optical thickness (AOT) and compared these with measurements of AOT from both ground and airborne sun photometers and derived from the ATSR-2 (Along Track and Scanning Radiometer 2) sensor on ERS-2 (European Remote Sensing Satellite-2). We also used the water vapor mixing ratio profiles measured simultaneously by LASE to derive precipitable water vapor and compare these to ground based measurements.

  7. Role of aerosols on the Indian Summer Monsoon variability, as simulated by state-of-the-art global climate models

    NASA Astrophysics Data System (ADS)

    Cagnazzo, Chiara; Biondi, Riccardo; D'Errico, Miriam; Cherchi, Annalisa; Fierli, Federico; Lau, William K. M.

    2016-04-01

    Recent observational and modeling analyses have explored the interaction between aerosols and the Indian summer monsoon precipitation on seasonal-to-interannual time scales. By using global scale climate model simulations, we show that when increased aerosol loading is found on the Himalayas slopes in the premonsoon period (April-May), intensification of early monsoon rainfall over India and increased low-level westerly flow follow, in agreement with the elevated-heat-pump (EHP) mechanism. The increase in rainfall during the early monsoon season has a cooling effect on the land surface that may also be amplified through solar dimming (SD) by more cloudiness and aerosol loading with subsequent reduction in monsoon rainfall over India. We extend this analyses to a subset of CMIP5 climate model simulations. Our results suggest that 1) absorbing aerosols, by influencing the seasonal variability of the Indian summer monsoon with the discussed time-lag, may act as a source of predictability for the Indian Summer Monsoon and 2) if the EHP and SD effects are operating also in a number of state-of-the-art climate models, their inclusion could potentially improve seasonal forecasts.

  8. Purification of mixed states with closed timelike curve is not possible

    SciTech Connect

    Pati, Arun K.; Chakrabarty, Indranil; Agrawal, Pankaj

    2011-12-15

    In ordinary quantum theory, any mixed state can be purified in an enlarged Hilbert space by adding an ancillary system. The purified state does not depend on the state of any extraneous system with which the mixed state is going to interact or on the physical interaction. Here, we prove that it is not possible to purify a mixed state that traverses a closed timelike curve (CTC) and is allowed to interact in a consistent way with a causality-respecting (CR) quantum system in the same manner. In other words, if a CTC quantum system with a mixed state has to undergo an arbitrary interaction with an arbitrary CR system then it has to be in a ''proper'' mixture, as it cannot be regarded as a subsystem of a pure entangled state. Thus, in general for arbitrary interactions between CR and CTC systems, there is no universal purification by embedding in a larger Hilbert space for mixed states with CTCs. This shows that in quantum theory with CTCs there can exist proper and improper mixtures.

  9. GCM Simulations of Volcanic Aerosol Forcing. Part I: Climate Changes Induced by Steady-State Perturbations.

    NASA Astrophysics Data System (ADS)

    Pollack, James B.; Rind, David; Lacis, Andrew; Hansen, James E.; Sato, Makiko; Ruedy, Reto

    1993-09-01

    The authors have used the Goddard Institute for Space Studies Climate Model II to simulate the response of the climate system to a spatially and temporally constant forcing by volcanic aerosols having an optical depth of 0.15. The climatic changes produced by long-term volcanic aerosol forcing are obtained by differencing this simulation and one made for the present climate with no volcanic aerosol forcing. These climatic changes are compared with those obtained with the same climate model when the C02 content of the atmosphere was doubled (2×C02) and when the boundary conditions associated with the peak of the last ice age were used (18 K). In all three cases, the absolute magnitude of the change in the globally averaged air temperature at the surface is approximately the same, 5 K.The simulations imply that a significant cooling of the troposphere and surface can occur at times of closely spaced, multiple, sulfur-rich volcanic explosions that span time scales of decades to centuries, such as occurred at the end of the nineteenth and beginning of the twentieth centuries. The steady-state climate response to volcanic forcing includes a large expansion of sea ice, especially in the Southern Hemisphere; a resultant large increase in surface and planetary albedo at high latitudes; and sizable changes in the annually and zonally averaged air temperature, T; T at the surface (Ts) does not sharply increase with increasing latitude, while T in the lower stratosphere is positive at low latitudes and negative at high latitudes.In certain ways, the climate response to the three different forcings is similar. Direct radiative forcing accounts for 30% and 25% of the total Ts in the volcano and 2×C02 runs, respectively. Changes in atmospheric water vapor act as the most important feedback, and are positive in all three cases. Albedo feedback is a significant, positive feedback at high latitudes in all three simulations, although the land ice feedback is prominent only in the

  10. Aerosols in clean and smoky air at Bozeman, Montana

    NASA Astrophysics Data System (ADS)

    Shaw, J. A.; Thomas, M.; Lathem, T. L.; Shaw, G. E.; Nenes, A.; Pust, N.; Repasky, K. S.

    2010-12-01

    The northern Rocky Mountain region of the United States is a natural laboratory for studying aerosols in a relatively uncontaminated environment punctuated by episodes of wildfire smoke. In autumn 2009, we conducted a field experiment at Montana State University in Bozeman, Montana to characterize the boundary layer aerosols as they transition from smoky periods to relatively clean background air. Physical and chemical properties of the aerosols were conducted, including high time resolution of Cloud Condensation Nuclei and inter comparison with AERONET data during times of deep atmospheric mixing. The key results of this experiment are: 1) the air in this northern Rocky Mountain location is surprisingly pristine with frequent aerosol size distributions devoid of a an accumulation mode; 2) periods of night-time growth of Aitken-mode aerosols were observed; 3) a persistent diurnal variation occurred, with upslope daytime winds bringing aerosols exhibiting moderate anthropogenic influence , and down slope nighttime winds bringing aerosols with weak accumulation mode; 4) the smoke aerosol was weakly soluble; and 5) satisfactory agreement was found between the inverted estimate of the fine mode aerosol from AERONET solar radiometry with that measured in situ.

  11. Analysis of the chemical and physical properties of combustion aerosols: State of the art.

    EPA Science Inventory

    The impact of combustion aerosols on human health is well documented byepidemiological studies, however the effect of low concentrations of ultrafineparticles on the human lung are not yet fully understood. With the advent ofnovel measurement technologies for simultaneous charact...

  12. Development of a United States - Mexico emissions inventory for the Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study

    SciTech Connect

    Hampden Kuhns; Eladio M. Knipping; Jeffrey M. Vukovich,

    2005-05-01

    The Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study investigated the sources of haze at Big Bend National Park in southwest Texas. The modeling domain includes most of the continental United States and Mexico. The BRAVO emissions inventory was constructed from the 1999 National Emission Inventory for the United States, modified to include finer-resolution data for Texas and 13 U.S. states in close proximity. The inventory includes emissions for CO, nitrogen oxides, sulfur dioxide, volatile organic compounds (VOCs), ammonia, particulate matter (PM) {lt}10 {mu}m in aerodynamic diameter, and PM {lt}2.5 {mu}m in aerodynamic diameter. The SMOKE modeling system was used to generate gridded emissions fields for use with the Regional Modeling System for Aerosols and Deposition (REMSAD) and the Community Multiscale Air Quality model modified with the Model of Aerosol Dynamics, Reaction, Ionization and Dissolution (CMAQ-MADRID). The compilation of the inventory, supporting model input data, and issues encountered during the development of the inventory are documented. A comparison of the BRAVO emissions inventory for Mexico with other emerging Mexican emission inventories illustrates their uncertainty. 65 refs., 4 figs., 9 tabs.

  13. [Cytologic parameters of broncho-alveolar lavage state in experimental animals exposed to mechanical rubber aerosol].

    PubMed

    Zhumabekova, B K; Sraubayev, E N; Gazalieva, M A; Akhmetova, S B

    2015-01-01

    Cytologic studies covered broncho-alveolar lavage in animals exposed to mechanical rubber aerosol in subacute (2 months) and chronic (5 months) experiments. Under exposure to mechanical rubber aerosol the experimental animals developed disorders of lung protective mechanisms. Subacute dust inhalation in the experimental animals caused higher counts of neutrophils and degeneratively changed cells with increased functional activity of alveolar macrophages and neutrophils. Chronic dust inhalation in the experimental animals proved lower functional activity alveolar macrophages and neutrophils.

  14. Dynamic terahertz spectroscopy of gas molecules mixed with unwanted aerosol under atmospheric pressure using fibre-based asynchronous-optical-sampling terahertz time-domain spectroscopy.

    PubMed

    Hsieh, Yi-Da; Nakamura, Shota; Abdelsalam, Dahi Ghareab; Minamikawa, Takeo; Mizutani, Yasuhiro; Yamamoto, Hirotsugu; Iwata, Tetsuo; Hindle, Francis; Yasui, Takeshi

    2016-06-15

    Terahertz (THz) spectroscopy is a promising method for analysing polar gas molecules mixed with unwanted aerosols due to its ability to obtain spectral fingerprints of rotational transition and immunity to aerosol scattering. In this article, dynamic THz spectroscopy of acetonitrile (CH3CN) gas was performed in the presence of smoke under the atmospheric pressure using a fibre-based, asynchronous-optical-sampling THz time-domain spectrometer. To match THz spectral signatures of gas molecules at atmospheric pressure, the spectral resolution was optimized to 1 GHz with a measurement rate of 1 Hz. The spectral overlapping of closely packed absorption lines significantly boosted the detection limit to 200 ppm when considering all the spectral contributions of the numerous absorption lines from 0.2 THz to 1 THz. Temporal changes of the CH3CN gas concentration were monitored under the smoky condition at the atmospheric pressure during volatilization of CH3CN droplets and the following diffusion of the volatilized CH3CN gas without the influence of scattering or absorption by the smoke. This system will be a powerful tool for real-time monitoring of target gases in practical applications of gas analysis in the atmospheric pressure, such as combustion processes or fire accident.

  15. Dynamic terahertz spectroscopy of gas molecules mixed with unwanted aerosol under atmospheric pressure using fibre-based asynchronous-optical-sampling terahertz time-domain spectroscopy

    PubMed Central

    Hsieh, Yi-Da; Nakamura, Shota; Abdelsalam, Dahi Ghareab; Minamikawa, Takeo; Mizutani, Yasuhiro; Yamamoto, Hirotsugu; Iwata, Tetsuo; Hindle, Francis; Yasui, Takeshi

    2016-01-01

    Terahertz (THz) spectroscopy is a promising method for analysing polar gas molecules mixed with unwanted aerosols due to its ability to obtain spectral fingerprints of rotational transition and immunity to aerosol scattering. In this article, dynamic THz spectroscopy of acetonitrile (CH3CN) gas was performed in the presence of smoke under the atmospheric pressure using a fibre-based, asynchronous-optical-sampling THz time-domain spectrometer. To match THz spectral signatures of gas molecules at atmospheric pressure, the spectral resolution was optimized to 1 GHz with a measurement rate of 1 Hz. The spectral overlapping of closely packed absorption lines significantly boosted the detection limit to 200 ppm when considering all the spectral contributions of the numerous absorption lines from 0.2 THz to 1 THz. Temporal changes of the CH3CN gas concentration were monitored under the smoky condition at the atmospheric pressure during volatilization of CH3CN droplets and the following diffusion of the volatilized CH3CN gas without the influence of scattering or absorption by the smoke. This system will be a powerful tool for real-time monitoring of target gases in practical applications of gas analysis in the atmospheric pressure, such as combustion processes or fire accident. PMID:27301319

  16. Dynamic terahertz spectroscopy of gas molecules mixed with unwanted aerosol under atmospheric pressure using fibre-based asynchronous-optical-sampling terahertz time-domain spectroscopy.

    PubMed

    Hsieh, Yi-Da; Nakamura, Shota; Abdelsalam, Dahi Ghareab; Minamikawa, Takeo; Mizutani, Yasuhiro; Yamamoto, Hirotsugu; Iwata, Tetsuo; Hindle, Francis; Yasui, Takeshi

    2016-01-01

    Terahertz (THz) spectroscopy is a promising method for analysing polar gas molecules mixed with unwanted aerosols due to its ability to obtain spectral fingerprints of rotational transition and immunity to aerosol scattering. In this article, dynamic THz spectroscopy of acetonitrile (CH3CN) gas was performed in the presence of smoke under the atmospheric pressure using a fibre-based, asynchronous-optical-sampling THz time-domain spectrometer. To match THz spectral signatures of gas molecules at atmospheric pressure, the spectral resolution was optimized to 1 GHz with a measurement rate of 1 Hz. The spectral overlapping of closely packed absorption lines significantly boosted the detection limit to 200 ppm when considering all the spectral contributions of the numerous absorption lines from 0.2 THz to 1 THz. Temporal changes of the CH3CN gas concentration were monitored under the smoky condition at the atmospheric pressure during volatilization of CH3CN droplets and the following diffusion of the volatilized CH3CN gas without the influence of scattering or absorption by the smoke. This system will be a powerful tool for real-time monitoring of target gases in practical applications of gas analysis in the atmospheric pressure, such as combustion processes or fire accident. PMID:27301319

  17. Dynamic terahertz spectroscopy of gas molecules mixed with unwanted aerosol under atmospheric pressure using fibre-based asynchronous-optical-sampling terahertz time-domain spectroscopy

    NASA Astrophysics Data System (ADS)

    Hsieh, Yi-Da; Nakamura, Shota; Abdelsalam, Dahi Ghareab; Minamikawa, Takeo; Mizutani, Yasuhiro; Yamamoto, Hirotsugu; Iwata, Tetsuo; Hindle, Francis; Yasui, Takeshi

    2016-06-01

    Terahertz (THz) spectroscopy is a promising method for analysing polar gas molecules mixed with unwanted aerosols due to its ability to obtain spectral fingerprints of rotational transition and immunity to aerosol scattering. In this article, dynamic THz spectroscopy of acetonitrile (CH3CN) gas was performed in the presence of smoke under the atmospheric pressure using a fibre-based, asynchronous-optical-sampling THz time-domain spectrometer. To match THz spectral signatures of gas molecules at atmospheric pressure, the spectral resolution was optimized to 1 GHz with a measurement rate of 1 Hz. The spectral overlapping of closely packed absorption lines significantly boosted the detection limit to 200 ppm when considering all the spectral contributions of the numerous absorption lines from 0.2 THz to 1 THz. Temporal changes of the CH3CN gas concentration were monitored under the smoky condition at the atmospheric pressure during volatilization of CH3CN droplets and the following diffusion of the volatilized CH3CN gas without the influence of scattering or absorption by the smoke. This system will be a powerful tool for real-time monitoring of target gases in practical applications of gas analysis in the atmospheric pressure, such as combustion processes or fire accident.

  18. Investigation of the chemical mixing state of individual Asian dust particles by the combined use of electron probe X-ray microanalysis and Raman microspectrometry.

    PubMed

    Sobanska, Sophie; Hwang, HeeJin; Choël, Marie; Jung, Hae-Jin; Eom, Hyo-Jin; Kim, HyeKeong; Barbillat, Jacques; Ro, Chul-Un

    2012-04-01

    In this work, quantitative electron probe X-ray microanalysis (EPMA) and Raman microspectrometry (RMS) were applied in combination for the first time to characterize the complex internal structure and physicochemical properties of the same ensemble of Asian dust particles. The analytical methodology to obtain the chemical composition, mixing state, and spatial distribution of chemical species within single particles through the combined use of the two techniques is described. Asian dust aerosol particles collected in Incheon, Korea, during a moderate dust storm event were examined to assess the applicability of the methodology to resolve internal mixtures within single particles. Among 92 individual analyzed particles, EPMA and RMS identified 53% of the particles to be internally mixed with two or more chemical species. Information on the spatial distribution of chemical compounds within internally mixed individual particles can be useful for deciphering the particle aging mechanisms and sources. This study demonstrates that the characterization of individual particles, including chemical speciation and mixing state analysis, can be performed more in detail using EPMA and RMS in combination than with the two single-particle techniques alone. PMID:22380789

  19. Global modelling of direct and indirect effects of sea spray aerosol using a source function encapsulating wave state

    NASA Astrophysics Data System (ADS)

    Partanen, A.-I.; Dunne, E. M.; Bergman, T.; Laakso, A.; Kokkola, H.; Ovadnevaite, J.; Sogacheva, L.; Baisnée, D.; Sciare, J.; Manders, A.; O'Dowd, C.; de Leeuw, G.; Korhonen, H.

    2014-11-01

    Recently developed parameterizations for the sea spray aerosol source flux, encapsulating wave state, and its organic fraction were incorporated into the aerosol-climate model ECHAM-HAMMOZ to investigate the direct and indirect radiative effects of sea spray aerosol particles. Our simulated global sea salt emission of 805 Tg yr-1 (uncertainty range 378-1233 Tg yr-1) was much lower than typically found in previous studies. Modelled sea salt and sodium ion concentrations agreed relatively well with measurements in the smaller size ranges at Mace Head (annual normalized mean model bias -13% for particles with vacuum aerodynamic diameter Dva < 1 μm), Point Reyes (-29% for particles with aerodynamic diameter Da < 2.5 μm) and Amsterdam Island (-52% for particles with Da < 1 μm) but the larger sizes were overestimated (899% for particles with 2.5 μm < Da < 10 μm) at Amsterdam Island. This suggests that at least the high end of the previous estimates of sea spray mass emissions is unrealistic. On the other hand, the model clearly underestimated the observed concentrations of organic or total carbonaceous aerosol at Mace Head (-82%) and Amsterdam Island (-68%). The large overestimation (212%) of organic matter at Point Reyes was due to the contribution of continental sources. At the remote Amsterdam Island site, the organic concentration was underestimated especially in the biologically active months, suggesting a need to improve the parameterization of the organic sea spray fraction. Globally, the satellite-retrieved AOD over the oceans, using PARASOL data, was underestimated by the model (means over ocean 0.16 and 0.10, respectively); however, in the pristine region around Amsterdam Island the measured AOD fell well within the simulated uncertainty range. The simulated sea spray aerosol contribution to the indirect radiative effect was positive (0.3 W m-2), in contrast to previous studies. This positive effect was ascribed to the tendency of sea salt aerosol to

  20. Global modelling of direct and indirect effects of sea spray aerosol using a source function encapsulating wave state

    NASA Astrophysics Data System (ADS)

    Partanen, A.-I.; Dunne, E. M.; Bergman, T.; Laakso, A.; Kokkola, H.; Ovadnevaite, J.; Sogacheva, L.; Baisnée, D.; Sciare, J.; Manders, A.; O'Dowd, C.; de Leeuw, G.; Korhonen, H.

    2014-02-01

    Recently developed parameterizations for the sea spray aerosol source flux, encapsulating wave state, and its organic fraction were incorporated into the aerosol-climate model ECHAM-HAMMOZ to investigate the direct and indirect radiative effects of sea spray aerosol particles. Our simulated global sea salt emission of 805 Tg yr-1 (uncertainty range 378-1233 Tg yr-1) was much lower than typically found in previous studies. Modelled sea salt and sodium ion concentrations agreed relatively well with measurements in the smaller size ranges at Mace Head (annual normalized mean model bias -13% for particles with vacuum aerodynamic diameter Dva < 1 μm), Point Reyes (-29% for particles with aerodynamic diameter Da < 2.5 μm) and Amsterdam Island (-52% for particles with Da < 1 μm) but the larger sizes were overestimated (899% for particles with 2.5 μm aerosol at Mace Head (-82%) and Amsterdam Island (-68%). The large overestimation (212%) of organic matter at Point Reyes was due to the contribution of continental sources. At the remote Amsterdam Island site, the organic concentration was underestimated especially in the biologically active months, suggesting a need to improve the parameterization of the organic sea spray fraction. Globally, the satellite-retrieved AOD over the oceans, using PARASOL data, was underestimated by the model (means over ocean 0.16 and 0.10, respectively); however, in the pristine region around Amsterdam Island the measured AOD fell well within the simulated uncertainty range. The simulated sea spray aerosol contribution to the indirect radiative effect was positive (0.3 W m-2), in contrast to previous studies. This positive effect was ascribed to the tendency of sea salt aerosol to

  1. Particle bound black carbon size distribution and mixing state in urban environments using a novel tandem differential mobility analyzer and aethalometer

    NASA Astrophysics Data System (ADS)

    Ning, Zhi; Westerdahl, Dane; Wong, Ka-Chun; Chan, Ka-Lok

    2013-04-01

    Particle bound black carbon (BC) has dominant anthropogenic origins from fossil fuel combustion and biomass burning sources. It is an important component of the light absorbing aerosols in the atmosphere, playing a role in the earth's radiative balance and climate change. While the mixing states of the BC largely determine the coating on the particles, knowledge of the size distribution of BC is key to the accurate modelling of their absorption of solar radiation. Also, BC is a major component of the diesel PM emissions, recently classified by World Health Organization as Class I carcinogen, and has been widely documented with association of a variety of adverse health effects. Their sizes also determine the fraction of lung deposition. Due to the limited information of the mixing state and size distribution of BC, there still exists large uncertainty of the role of BC in climate change modelling. This study presents a novel approach of the direct and continuous measurement of atmospheric BC size distribution and coating by tandem operation of a differential mobility analyzer and a modified aethalometer. A condensation particle counter was deployed concurrently with the aethalometer to determine the particle number size distribution. Particle coating on BC was further estimated. A wide range of particle sizes (15-700nm) was investigated to determine the BC mass size distribution in fresh diesel engine tailpipe emissions and different ambient environments including urban and roadside. The results showed the evolution of BC mixing state and size distribution from fresh engine emissions to the roadside and urban ambient environments. The results provide important references for climate modelling to better determine the effect of radiative forcing from urban aerosols.

  2. Continuum of depressive and manic mixed states in patients with bipolar disorder: quantitative measurement and clinical features.

    PubMed

    Swann, Alan C; Steinberg, Joel L; Lijffijt, Marijn; Moeller, Gerard F

    2009-10-01

    Bipolar mixed states combine depressive and manic features, presenting diagnostic and treatment challenges and reflecting a severe form of the illness. DSM-IV criteria for a mixed state require combined depressive and manic syndromes, but a range of mixed states has been described clinically. A unified definition of mixed states would be valuable in understanding their diagnosis, mechanism and treatment implications. We investigated the manner in which depressive and manic features combine to produce a continuum of mixed states. In 88 subjects with bipolar disorder (DSM-IV), we evaluated symptoms and clinical characteristics, and compared depression-based, mania-based, and other published definitions of mixed states. We developed an index of the extent to which symptoms were mixed (Mixed State Index, MSI) and characterized its relationship to clinical state. Predominately manic and depressive mixed states using criteria from recent literature, as well as Kraepelinian mixed states, had similar symptoms and MSI scores. Anxiety correlated significantly with depression scores in manic subjects and with mania scores in depressed subjects. Discriminant function analysis associated mixed states with symptoms of hyperactivity and negative cognitions, but not subjective depressive or elevated mood. High MSI scores were associated with severe course of illness. For depressive or manic episodes, characteristics of mixed states emerged with two symptoms of the opposite polarity. This was a cross-sectional study. Mixed states appear to be a continuum. An index of the degree to which depressive and manic symptoms combine appears useful in identifying and characterizing mixed states. We propose a depressive or manic episode with three or more symptoms of the opposite polarity as a parsimonious definition of a mixed state.

  3. Measuring and modeling the hygroscopic growth of two humic substances in mixed aerosol particles of atmospheric relevance

    NASA Astrophysics Data System (ADS)

    Zamora, I. R.; Jacobson, M. Z.

    2013-09-01

    The hygroscopic growth of atmospheric particles affects atmospheric chemistry and Earth's climate. Water-soluble organic carbon (WSOC) constitutes a significant fraction of the dry submicron mass of atmospheric aerosols, thus affecting their water uptake properties. Although the WSOC fraction is comprised of many compounds, a set of model substances can be used to describe its behavior. For this study, mixtures of Nordic aquatic fulvic acid reference (NAFA) and Fluka humic acid (HA), with various combinations of inorganic salts (sodium chloride and ammonium sulfate) and other representative organic compounds (levoglucosan and succinic acid), were studied. We measured the equilibrium water vapor pressure over bulk solutions of these mixtures as a function of temperature and solute concentration. New water activity (aw) parameterizations and hygroscopic growth curves at 25 °C were calculated from these data for particles of equivalent composition. We examined the effect of temperature on the water activity and found a maximum variation of 9% in the 0-30 °C range, and 2% in the 20-30 °C range. Five two-component mixtures were studied to understand the effect of adding a humic substance (HS), such as NAFA and HA, to an inorganic salt or a saccharide. The deliquescence point at 25 °C for HS-inorganic mixtures did not change significantly from that of the pure inorganic species. However, the hygroscopic growth of HA / inorganic mixtures was lower than that exhibited by the pure salt, in proportion to the added mass of HA. The addition of NAFA to a highly soluble solute (ammonium sulfate, sodium chloride or levoglucosan) in water had the same effect as the addition of HA to the inorganic species for most of the water activity range studied. Yet, the water uptake of these NAFA mixtures transitioned to match the growth of the pure salt or saccharide at high aw values. The remaining four mixtures were based on chemical composition data for different aerosol types. As

  4. Retrieval of aerosol composition using ground-based remote sensing measurements

    NASA Astrophysics Data System (ADS)

    Xie, Y.; Li, Z.; Xu, H.; Chen, X.; Li, K.; Lv, Y.; Li, D.; Zhang, Y.

    2015-12-01

    The chemical composition and mixing status of ambient aerosol are the main factors deciding aerosol microphysical and optical properties, and thus have significant impacts on regional or global climate change and air quality. Traditional approaches to detect atmospheric aerosol composition include sampling with laboratory analysis and in-situ measurement. They can accurately acquire aerosol components, however, the sampling or air exhausting could change the status of aerosol or have some mass loss. Additionally, aerosol is usually sampled at the surface level so that it is difficult to detect the columnar aerosol properties. Remote sensing technology, however, can overcome these problems because it investigate aerosol information by optical and microphysical properties without destructing the natural status of ambient aerosol. This paper introduce a method to acquire aerosol composition by the remote sensing measurements of CIMEL CE318 ground-based sun-sky radiometer. A six component aerosol model is used in this study, including one strong absorbing component Black Carbon (BC), two partly absorbing components Brown Carbon (BrC) and Mineral Dust (MD), two scattering components Ammonia Sulfate-like (AS) and Sea Salt (SS), and Aerosol Water uptake (AW). Sensitivity analysis are performed to find the most sensitive parameters to each component and retrieval method for each component is accordingly developed. The residual minimization method is used by comparing remote sensing measurements and simulation outputs to find the optimization of aerosol composition (including volume fraction and mass concentration of each component). This method is applied to real measurements obtained from Beijing site under different weather conditions, including polluted haze, dust storm and clean days, to investigate the impacts of mixing states of aerosol particles on aerosol composition retrieval.

  5. A sea-state based source function for size and composition resolved marine aerosol

    SciTech Connect

    Long, Michael S; Keene, William C; Erickson III, David J

    2011-01-01

    A parameterization for the size- and composition-resolved production fluxes of nascent marine aerosol was developed from prior experimental observations and extrapolated to ambient conditions based on estimates of air entrainment by the breaking of wind-driven ocean waves. Production of particulate organic carbon (OC{sub aer}) was parameterized based on Langmuir equilibrium-type association of organic matter to bubble plumes in seawater and resulting aerosol as constrained by measurements of aerosol produced from productive and oligotrophic seawater. This novel approach is the first to parameterize size- and composition-resolved aerosol production based on explicit evaluation of wind-driven air entrainment/detrainment fluxes and chlorophyll-a as a proxy for surfactants in surface seawater. Production fluxes were simulated globally with an eight aerosol-size-bin version of the NCAR Community Atmosphere Model (CAM v3.5.07). Simulated production fluxes fell within the range of published estimates based on observationally constrained parameterizations. Because the parameterization does not consider contributions from spume drops, the simulated global mass flux (1.5 x 10{sup 3} Tg y{sup -1}) is near the lower end of published estimates. The simulated production of aerosol number (1.4 x 10{sup 6} m{sup -2} s{sup -1}) and OC{sub aer} (29 Tg C y{sup -1}) fall near the upper end of published estimates and suggest that primary marine aerosols may have greater influences on the physicochemical evolution of the troposphere, radiative transfer and climate, and associated feedbacks on the surface ocean than suggested by previous model studies.

  6. A review of changes in composition of hot mix asphalt in the United States.

    PubMed

    Mundt, Diane J; Marano, Kristin M; Nunes, Anthony P; Adams, Robert C

    2009-11-01

    This review researched the materials, methods, and practices in the hot mix asphalt industry that might impact future exposure assessments and epidemiologic research on road paving workers. Since World War II, the U.S. interstate highway system, increased traffic volume, transportation speeds, and vehicle axle loads have necessitated an increase in demand for hot mix asphalt for road construction and maintenance, while requiring a consistent road paving product that meets state-specific physical performance specifications. We reviewed typical practices in hot mix asphalt paving in the United States to understand the extent to which materials are and have been added to hot mix asphalt to meet specifications and how changes in practices and technology could affect evaluation of worker exposures for future research. Historical documents were reviewed, and industry experts from 16 states were interviewed to obtain relevant information on industry practices. Participants from all states reported additive use, with most being less than 2% by weight. Crumb rubber and recycled asphalt pavement were added in concentrations approximately 10% per unit weight of the mix. The most frequently added materials included polymers and anti-stripping agents. Crumb rubber, sulfur, asbestos, roofing shingles, slag, or fly ash have been used in limited amounts for short periods of time or in limited geographic areas. No state reported using coal tar as an additive to hot mix asphalt or as a binder alternative in hot mix pavements for high-volume road construction. Coal tar may be present in recycled asphalt pavement from historical use, which would need to be considered in future exposure assessments of pavers. Changes in hot mix asphalt production and laydown emission control equipment have been universally implemented over time as the technology has become available to reduce potential worker exposures. This work is a companion review to a study undertaken in the petroleum refining

  7. Highly efficient inelastic four-wave mixing using dual induced transparency and coherently prepared states

    NASA Astrophysics Data System (ADS)

    Payne, M. G.; Jiang, Kaijun; Deng, L.

    2006-09-01

    We investigate a life time broadened and coherently prepared five-state system for multi-wave mixing processes. We show that very efficient wave mixing occurs, producing an unconventional mixing wave that has the characteristics of both conventional four-wave mixing (FWM) and stimulated hyper-Raman (SHR) emission. In addition, we show interesting multiple simultaneous multi-photon interference effects at large propagation distances and demonstrate more than 10 orders of magnitude suppression of populations of the probe wave terminal state and the near three-photon resonance mixing wave generating state. These new type of multi-photon interference based induced transparency effects, which are critically dependent on two distinctive relaxation processes involving both an external supplied and an internally generated fields, are fundamentally different from the conventional three-state electromagnetically induced transparency effect which does not depend on propagation. As a consequence, both the probe and the wave-mixing field to propagate nearly free of absorption and distortions in a highly dispersive medium.

  8. Seasonal Variations in Titan's Stratosphere Observed with Cassini/CIRS: Temperature, Trace Molecular Gas and Aerosol Mixing Ratio Profiles

    NASA Technical Reports Server (NTRS)

    Vinatier, S.; Bezard, B.; Anderson, C. M.; Coustenis, A.; Teanby, N.

    2012-01-01

    Titan's northern spring equinox occurred in August 2009. General Circulation Models (e.g. Lebonnois et al., 2012) predict strong modifications of the global circulation in this period, with formation of two circulation cells instead of the pole-to-pole cell that occurred during northern winter. This winter single cell, which had its descending branch at the north pole, was at the origin of the enrichment of molecular abundances and high stratopause temperatures observed by Cassini/CIRS at high northern latitudes (e.g. Achterberg et al., 2011, Coustenis et al., 2010, Teanby et al., 2008, Vinatier et al., 2010). The predicted dynamical seasonal variations after the equinox have strong impact on the spatial distributions of trace gas, temperature and aerosol abundances. We will present here an analysis of CIRS limb-geometry datasets acquired in 2010 and 2011 that we used to monitor the seasonal evolution of the vertical profiles of temperature, molecular (C2H2, C2H6, HCN, ..) and aerosol abundances.

  9. Aerosols and environmental pollution

    NASA Astrophysics Data System (ADS)

    Colbeck, Ian; Lazaridis, Mihalis

    2010-02-01

    The number of publications on atmospheric aerosols has dramatically increased in recent years. This review, predominantly from a European perspective, summarizes the current state of knowledge of the role played by aerosols in environmental pollution and, in addition, highlights gaps in our current knowledge. Aerosol particles are ubiquitous in the Earth’s atmosphere and are central to many environmental issues; ranging from the Earth’s radiative budget to human health. Aerosol size distribution and chemical composition are crucial parameters that determine their dynamics in the atmosphere. Sources of aerosols are both anthropogenic and natural ranging from vehicular emissions to dust resuspension. Ambient concentrations of aerosols are elevated in urban areas with lower values at rural sites. A comprehensive understanding of aerosol ambient characteristics requires a combination of measurements and modeling tools. Legislation for ambient aerosols has been introduced at national and international levels aiming to protect human health and the environment.

  10. Aerosols and environmental pollution.

    PubMed

    Colbeck, Ian; Lazaridis, Mihalis

    2010-02-01

    The number of publications on atmospheric aerosols has dramatically increased in recent years. This review, predominantly from a European perspective, summarizes the current state of knowledge of the role played by aerosols in environmental pollution and, in addition, highlights gaps in our current knowledge. Aerosol particles are ubiquitous in the Earth's atmosphere and are central to many environmental issues; ranging from the Earth's radiative budget to human health. Aerosol size distribution and chemical composition are crucial parameters that determine their dynamics in the atmosphere. Sources of aerosols are both anthropogenic and natural ranging from vehicular emissions to dust resuspension. Ambient concentrations of aerosols are elevated in urban areas with lower values at rural sites. A comprehensive understanding of aerosol ambient characteristics requires a combination of measurements and modeling tools. Legislation for ambient aerosols has been introduced at national and international levels aiming to protect human health and the environment.

  11. Black carbon simulations using a size- and mixing-state-resolved three-dimensional model: 2. Aging timescale and its impact over East Asia

    NASA Astrophysics Data System (ADS)

    Matsui, H.

    2016-02-01

    This study evaluates the aging timescale and the cloud condensation nuclei (CCN) activity of black carbon (BC) over East Asia and its outflow region using a size- and mixing-state-resolved three-dimensional model, the Weather Research and Forecasting model with chemistry (WRF-chem) with the Aerosol Two-dimensional bin module for foRmation and Aging Simulation (ATRAS) and the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC). The WRF-chem/ATRAS-MOSAIC model explicitly calculates BC aging (condensation and coagulation) and removal processes, with 12 size and 10 BC mixing state bins (128 bins in total). The model reveals large spatial and temporal variability of the BC aging timescale and the CCN activity of BC-containing particles over East Asia (spring 2009) with their strong size and supersaturation dependence. The BC aging timescale differs from 0.19 to 3.1 days (period and domain average at an altitude of 1 km), depending on the choice of size (mass or number) and supersaturation (1.0% or 0.1%). As a result, almost 100% of BC-containing particles are CCN-active at a supersaturation of 1.0%, whereas 20-50% of BC-containing particles are CCN-inactive at a supersaturation of 0.1%, with a strong size dependence. These results show the importance of resolving BC aging processes and their dependence on size and supersaturation in models for more accurate simulations of BC concentrations and their distribution and lifetime. A sensitivity simulation without resolving BC mixing state shows the underestimation of total BC mass concentrations by 5-10% and the BC mass concentrations in the CCN-inactive particles (at a supersaturation of 0.1%) by 40-60% over the outflow region (at 150°E), compared with the simulation resolving BC mixing state. Because BC aging speed is very slow at 150°E and eastward, the change in BC mass and its CCN activity by resolving BC mixing state will continue over long distances and may have a large impact on BC transport from East

  12. Development of a United States-Mexico Emissions Inventory for the Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study.

    PubMed

    Kuhns, Hampden; Knipping, Eladio M; Vukovich, Jeffrey M

    2005-05-01

    The Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study was commissioned to investigate the sources of haze at Big Bend National Park in southwest Texas. The modeling domain of the BRAVO Study includes most of the continental United States and Mexico. The BRAVO emissions inventory was constructed from the 1999 National Emission Inventory for the United States, modified to include finer-resolution data for Texas and 13 U.S. states in close proximity. The first regional-scale Mexican emissions inventory designed for air-quality modeling applications was developed for 10 northern Mexican states, the Tula Industrial Park in the state of Hidalgo, and the Popocatépetl volcano in the state of Puebla. Emissions data were compiled from numerous sources, including the U.S. Environmental Protection Agency (EPA), the Texas Natural Resources Conservation Commission (now Texas Commission on Environmental Quality), the Eastern Research Group, the Minerals Management Service, the Instituto Nacional de Ecología, and the Instituto Nacional de Estadistica Geografía y Informática. The inventory includes emissions for CO, nitrogen oxides, sulfur dioxide, volatile organic compounds (VOCs), ammonia, particulate matter (PM) < 10 microm in aerodynamic diameter, and PM < 2.5 microm in aerodynamic diameter. Wind-blown dust and biomass burning were not included in the inventory, although high concentrations of dust and organic PM attributed to biomass burning have been observed at Big Bend National Park. The SMOKE modeling system was used to generate gridded emissions fields for use with the Regional Modeling System for Aerosols and Deposition (REMSAD) and the Community Multiscale Air Quality model modified with the Model of Aerosol Dynamics, Reaction, Ionization and Dissolution (CMAQ-MADRID). The compilation of the inventory, supporting model input data, and issues encountered during the development of the inventory are documented. A comparison of the BRAVO emissions

  13. Development of a United States-Mexico Emissions Inventory for the Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study.

    PubMed

    Kuhns, Hampden; Knipping, Eladio M; Vukovich, Jeffrey M

    2005-05-01

    The Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study was commissioned to investigate the sources of haze at Big Bend National Park in southwest Texas. The modeling domain of the BRAVO Study includes most of the continental United States and Mexico. The BRAVO emissions inventory was constructed from the 1999 National Emission Inventory for the United States, modified to include finer-resolution data for Texas and 13 U.S. states in close proximity. The first regional-scale Mexican emissions inventory designed for air-quality modeling applications was developed for 10 northern Mexican states, the Tula Industrial Park in the state of Hidalgo, and the Popocatépetl volcano in the state of Puebla. Emissions data were compiled from numerous sources, including the U.S. Environmental Protection Agency (EPA), the Texas Natural Resources Conservation Commission (now Texas Commission on Environmental Quality), the Eastern Research Group, the Minerals Management Service, the Instituto Nacional de Ecología, and the Instituto Nacional de Estadistica Geografía y Informática. The inventory includes emissions for CO, nitrogen oxides, sulfur dioxide, volatile organic compounds (VOCs), ammonia, particulate matter (PM) < 10 microm in aerodynamic diameter, and PM < 2.5 microm in aerodynamic diameter. Wind-blown dust and biomass burning were not included in the inventory, although high concentrations of dust and organic PM attributed to biomass burning have been observed at Big Bend National Park. The SMOKE modeling system was used to generate gridded emissions fields for use with the Regional Modeling System for Aerosols and Deposition (REMSAD) and the Community Multiscale Air Quality model modified with the Model of Aerosol Dynamics, Reaction, Ionization and Dissolution (CMAQ-MADRID). The compilation of the inventory, supporting model input data, and issues encountered during the development of the inventory are documented. A comparison of the BRAVO emissions

  14. Structural-phase state and creep of mixed nitride fuel

    NASA Astrophysics Data System (ADS)

    Konovalov, I. I.; Tarasov, B. A.; Glagovsky, E. M.

    2016-04-01

    By the analysis of thermal creep data in conjunction with structural-phase state the most likely mechanisms of UN creep are considered. An equation relating the thermal and radiation creep of nitride fuel with such important parameters as plutonium content, porosity, grain size, the content of impurities of transition metals and oxygen, the carbon content has been suggested. At stationary operating parameters in reactor the creep of nitride fuel with technical purity is defined by the thermal component at mechanism of intergranular slip and by the radiation component, which plays a significant role at temperatures below 1100°C. Both types of creep in a first approximation have a linear dependence on the stress.

  15. Rotational State Microwave Mixing for Laser Cooling of Complex Diatomic Molecules

    NASA Astrophysics Data System (ADS)

    Yeo, Mark; Hummon, Matthew T.; Collopy, Alejandra L.; Yan, Bo; Hemmerling, Boerge; Chae, Eunmi; Doyle, John M.; Ye, Jun

    2015-06-01

    We demonstrate the mixing of rotational states in the ground electronic state using microwave radiation to enhance optical cycling in the molecule yttrium (II) monoxide (YO). This mixing technique is used in conjunction with a frequency modulated and chirped continuous wave laser to slow longitudinally a cryogenic buffer-gas beam of YO. We generate a flux of YO below 10 m /s , directly loadable into a three-dimensional magneto-optical trap. This technique opens the door for laser cooling of diatomic molecules with more complex loss channels due to intermediate states.

  16. Experimental detection of nonclassical correlations in mixed-state quantum computation

    SciTech Connect

    Passante, G.; Moussa, O.; Trottier, D. A.; Laflamme, R.

    2011-10-15

    We report on an experiment to detect nonclassical correlations in a highly mixed state. The correlations are characterized by the quantum discord and are observed using four qubits in a liquid-state nuclear magnetic resonance quantum information processor. The state analyzed is the output of a DQC1 computation, whose input is a single quantum bit accompanied by n maximally mixed qubits. This model of computation outperforms the best known classical algorithms and, although it contains vanishing entanglement, it is known to have quantum correlations characterized by the quantum discord. This experiment detects nonvanishing quantum discord, ensuring the existence of nonclassical correlations as measured by the quantum discord.

  17. Geometric phase of mixed states for three-level open systems

    SciTech Connect

    Jiang Yanyan; Ji, Y. H.; Wang, Z. S.; Xu Hualan; Hu Liyun; Chen, Z. Q.; Guo, L. P.

    2010-12-15

    Geometric phase of mixed state for three-level open system is defined by establishing in connecting density matrix with nonunit vector ray in a three-dimensional complex Hilbert space. Because the geometric phase depends only on the smooth curve on this space, it is formulated entirely in terms of geometric structures. Under the limiting of pure state, our approach is in agreement with the Berry phase, Pantcharatnam phase, and Aharonov and Anandan phase. We find that, furthermore, the Berry phase of mixed state correlated to population inversions of three-level open system.

  18. Greenberger-Horne-Zeilinger argument of nonlocality without inequalities for mixed states

    SciTech Connect

    Ghirardi, Gian Carlo; Marinatto, Luca

    2006-08-15

    We generalize the Greenberger-Horne-Zeilinger nonlocality without inequalities argument to cover the case of arbitrary mixed statistical operators associated to three-qubits quantum systems. More precisely, we determine the radius of a ball (in the trace distance topology) surrounding the pure GHZ state and containing arbitrary mixed statistical operators which cannot be described by any local and realistic hidden variable model and which are, as a consequence, noncompletely separable. As a practical application, we focus on certain one-parameter classes of mixed states which are commonly considered in the experimental realization of the original GHZ argument and which result from imperfect preparations of the pure GHZ state. In these cases we determine for which values of the parameter measuring the noise a nonlocality argument can still be exhibited, despite the mixedness of the considered states. Moreover, the effect of the imperfect nature of measurement processes is discussed.

  19. Morphology and mixing state of individual freshly emitted wildfire carbonaceous particles

    PubMed Central

    China, Swarup; Mazzoleni, Claudio; Gorkowski, Kyle; Aiken, Allison C.; Dubey, Manvendra K.

    2013-01-01

    Biomass burning is one of the largest sources of carbonaceous aerosols in the atmosphere, significantly affecting earth’s radiation budget and climate. Tar balls, abundant in biomass burning smoke, absorb sunlight and have highly variable optical properties, typically not accounted for in climate models. Here we analyse single biomass burning particles from the Las Conchas fire (New Mexico, 2011) using electron microscopy. We show that the relative abundance of tar balls (80%) is 10 times greater than soot particles (8%). We also report two distinct types of tar balls; one less oxidized than the other. Furthermore, the mixing of soot particles with other material affects their optical, chemical and physical properties. We quantify the morphology of soot particles and classify them into four categories: ~50% are embedded (heavily coated), ~34% are partly coated, ~12% have inclusions and~4% are bare. Inclusion of these observations should improve climate model performances. PMID:23824042

  20. Evaluations of tropospheric aerosol properties simulated by the community earth system model with a sectional aerosol microphysics scheme

    PubMed Central

    Toon, Owen B.; Bardeen, Charles G.; Mills, Michael J.; Fan, Tianyi; English, Jason M.; Neely, Ryan R.

    2015-01-01

    Abstract A sectional aerosol model (CARMA) has been developed and coupled with the Community Earth System Model (CESM1). Aerosol microphysics, radiative properties, and interactions with clouds are simulated in the size‐resolving model. The model described here uses 20 particle size bins for each aerosol component including freshly nucleated sulfate particles, as well as mixed particles containing sulfate, primary organics, black carbon, dust, and sea salt. The model also includes five types of bulk secondary organic aerosols with four volatility bins. The overall cost of CESM1‐CARMA is approximately ∼2.6 times as much computer time as the standard three‐mode aerosol model in CESM1 (CESM1‐MAM3) and twice as much computer time as the seven‐mode aerosol model in CESM1 (CESM1‐MAM7) using similar gas phase chemistry codes. Aerosol spatial‐temporal distributions are simulated and compared with a large set of observations from satellites, ground‐based measurements, and airborne field campaigns. Simulated annual average aerosol optical depths are lower than MODIS/MISR satellite observations and AERONET observations by ∼32%. This difference is within the uncertainty of the satellite observations. CESM1/CARMA reproduces sulfate aerosol mass within 8%, organic aerosol mass within 20%, and black carbon aerosol mass within 50% compared with a multiyear average of the IMPROVE/EPA data over United States, but differences vary considerably at individual locations. Other data sets show similar levels of comparison with model simulations. The model suggests that in addition to sulfate, organic aerosols also significantly contribute to aerosol mass in the tropical UTLS, which is consistent with limited data.

  1. Evaluations of tropospheric aerosol properties simulated by the community earth system model with a sectional aerosol microphysics scheme

    PubMed Central

    Toon, Owen B.; Bardeen, Charles G.; Mills, Michael J.; Fan, Tianyi; English, Jason M.; Neely, Ryan R.

    2015-01-01

    Abstract A sectional aerosol model (CARMA) has been developed and coupled with the Community Earth System Model (CESM1). Aerosol microphysics, radiative properties, and interactions with clouds are simulated in the size‐resolving model. The model described here uses 20 particle size bins for each aerosol component including freshly nucleated sulfate particles, as well as mixed particles containing sulfate, primary organics, black carbon, dust, and sea salt. The model also includes five types of bulk secondary organic aerosols with four volatility bins. The overall cost of CESM1‐CARMA is approximately ∼2.6 times as much computer time as the standard three‐mode aerosol model in CESM1 (CESM1‐MAM3) and twice as much computer time as the seven‐mode aerosol model in CESM1 (CESM1‐MAM7) using similar gas phase chemistry codes. Aerosol spatial‐temporal distributions are simulated and compared with a large set of observations from satellites, ground‐based measurements, and airborne field campaigns. Simulated annual average aerosol optical depths are lower than MODIS/MISR satellite observations and AERONET observations by ∼32%. This difference is within the uncertainty of the satellite observations. CESM1/CARMA reproduces sulfate aerosol mass within 8%, organic aerosol mass within 20%, and black carbon aerosol mass within 50% compared with a multiyear average of the IMPROVE/EPA data over United States, but differences vary considerably at individual locations. Other data sets show similar levels of comparison with model simulations. The model suggests that in addition to sulfate, organic aerosols also significantly contribute to aerosol mass in the tropical UTLS, which is consistent with limited data. PMID:27668039

  2. Climate implications of carbonaceous aerosols: An aerosol microphysical study using the GISS/MATRIX climate model

    SciTech Connect

    Bauer, Susanne E.; Menon, Surabi; Koch, Dorothy; Bond, Tami; Tsigaridis, Kostas

    2010-04-09

    Recently, attention has been drawn towards black carbon aerosols as a likely short-term climate warming mitigation candidate. However the global and regional impacts of the direct, cloud-indirect and semi-direct forcing effects are highly uncertain, due to the complex nature of aerosol evolution and its climate interactions. Black carbon is directly released as particle into the atmosphere, but then interacts with other gases and particles through condensation and coagulation processes leading to further aerosol growth, aging and internal mixing. A detailed aerosol microphysical scheme, MATRIX, embedded within the global GISS modelE includes the above processes that determine the lifecycle and climate impact of aerosols. This study presents a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative forcing. Our best estimate for net direct and indirect aerosol radiative forcing change is -0.56 W/m{sup 2} between 1750 and 2000. However, the direct and indirect aerosol effects are very sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative forcing change can vary between -0.32 to -0.75 W/m{sup 2} depending on these carbonaceous particle properties. Assuming that sulfates, nitrates and secondary organics form a coating shell around a black carbon core, rather than forming a uniformly mixed particles, changes the overall net radiative forcing from a negative to a positive number. Black carbon mitigation scenarios showed generally a benefit when mainly black carbon sources such as diesel emissions are reduced, reducing organic and black carbon sources such as bio-fuels, does not lead to reduced warming.

  3. Coupling aerosol optics to the MATCH (v5.5.0) chemical transport model and the SALSA (v1) aerosol microphysics module

    NASA Astrophysics Data System (ADS)

    Andersson, Emma; Kahnert, Michael

    2016-05-01

    A new aerosol-optics model is implemented in which realistic morphologies and mixing states are assumed, especially for black carbon particles. The model includes both external and internal mixing of all chemical species, it treats externally mixed black carbon as fractal aggregates, and it accounts for inhomogeneous internal mixing of black carbon by use of a novel "core-grey-shell" model. Simulated results of aerosol optical properties, such as aerosol optical depth, backscattering coefficients and the Ångström exponent, as well as radiative fluxes are computed with the new optics model and compared with results from an older optics-model version that treats all particles as externally mixed homogeneous spheres. The results show that using a more detailed description of particle morphology and mixing state impacts the aerosol optical properties to a degree of the same order of magnitude as the effects of aerosol-microphysical processes. For instance, the aerosol optical depth computed for two cases in 2007 shows a relative difference between the two optics models that varies over the European region between -28 and 18 %, while the differences caused by the inclusion or omission of the aerosol-microphysical processes range from -50 to 37 %. This is an important finding, suggesting that a simple optics model coupled to a chemical transport model can introduce considerable errors affecting radiative fluxes in chemistry-climate models, compromising comparisons of model results with remote sensing observations of aerosols, and impeding the assimilation of satellite products for aerosols into chemical-transport models.

  4. Redox state of plutonium in irradiated mixed oxide fuels

    NASA Astrophysics Data System (ADS)

    Degueldre, C.; Pin, S.; Poonoosamy, J.; Kulik, D. A.

    2014-03-01

    Nowadays, MOX fuels are used in about 20 nuclear power plants around the world. After irradiation, plutonium co-exists with uranium oxide. Due to the redox sensitive nature of UO2 other plutonium oxides than PuO2 potentially present in the fuel may interact with the matrix. The aim of this study is to determine which plutonium species are present in heterogeneous and homogeneous MOX. The results provided by X-ray Absorption Near Edge Spectroscopy (XANES) for non-irradiated as well as irradiated (center and periphery) homogeneous MOX fuel were published earlier and are completed by Extended X-ray Fine Structure (EXAFS) analysis in this work. The EXAFS signals have been extracted using the ATHENA code and the analyses were carried using EXCURE98 as performed earlier for an analogous element. EXAFS shows that plutonium redox state remains tetravalent in the solid solution and that the minor fraction of trivalent Pu must be below 10%. Independently, the study of homogeneous MOX was also approached by thermodynamics of solid solution of (U,Pu)O2. Such solid solutions were modeled using the Gibbs Energy Minimisation (GEM)-Selektor code (developed at LES, NES, PSI) supported by the literature data on such solid solutions. A comparative study was performed showing which plutonium oxides in their respective mole fractions are more likely to occur in (U,Pu)O2. In the modeling, these oxides were set as ideal and non-ideal solid solutions, as well as separate pure phases. Pu exists mainly as PuO2 in the case of separate phases, but can exist under its reduced forms, PuO1.61 and PuO1.5 in minor fraction i.e. ~15% in ideal solid solution (unlikely) and ~10% in non-ideal solid solution (likely) and at temperature around 1300 K. This combined thermodynamic and EXAFS studies confirm independently the results obtained so far by Pu XANES for the same MOX samples.

  5. Uncertainties in global aerosols and climate effects due to biofuel emissions

    NASA Astrophysics Data System (ADS)

    Kodros, J. K.; Scott, C. E.; Farina, S. C.; Lee, Y. H.; L'Orange, C.; Volckens, J.; Pierce, J. R.

    2015-08-01

    Aerosol emissions from biofuel combustion impact both health and climate; however, while reducing emissions through improvements to combustion technologies will improve health, the net effect on climate is largely unconstrained. In this study, we examine sensitivities in global aerosol concentration, direct radiative climate effect, and cloud-albedo aerosol indirect climate effect to uncertainties in biofuel emission factors, optical mixing state, and model nucleation and background secondary organic aerosol (SOA). We use the Goddard Earth Observing System global chemical-transport model (GEOS-Chem) with TwO Moment Aerosol Sectional (TOMAS) microphysics. The emission factors include amount, composition, size, and hygroscopicity, as well as optical mixing-state properties. We also evaluate emissions from domestic coal use, which is not biofuel but is also frequently emitted from homes. We estimate the direct radiative effect assuming different mixing states (homogeneous, core-shell, and external) with and without absorptive organic aerosol (brown carbon). We find the global-mean direct radiative effect of biofuel emissions ranges from -0.02 to +0.06 W m-2 across all simulation/mixing-state combinations with regional effects in source regions ranging from -0.2 to +0.8 W m-2. The global-mean cloud-albedo aerosol indirect effect (AIE) ranges from +0.01 to -0.02 W m-2 with regional effects in source regions ranging from -1.0 to -0.05 W m-2. The direct radiative effect is strongly dependent on uncertainties in emissions mass, composition, emissions aerosol size distributions, and assumed optical mixing state, while the indirect effect is dependent on the emissions mass, emissions aerosol size distribution, and the choice of model nucleation and secondary organic aerosol schemes. The sign and magnitude of these effects have a strong regional dependence. We conclude that the climate effects of biofuel aerosols are largely unconstrained, and the overall sign of the aerosol

  6. Characteristics of PM2.5 Carbonaceous Aerosol in Urban New York State

    NASA Astrophysics Data System (ADS)

    Khwaja, H. A.; Dutkiewicz, V.; Briggs, R.; Siddique, A.; Regan, J.

    2008-12-01

    In order to investigate the characteristics of carbonaceous fine aerosols, PM2.5 and size-segregated particulate samples (< 2.5 um, 2.5 - 4.2 um, 4.2 - 10 um, and 10 um) were collected during the summer in two urban sites of New York State viz., Botanical Garden (BTG), New York City and Empire State Plaza (ESP), Albany. Gas phase organic compounds were sampled with polyurethane foam (PUF) plugs. Particulate samples were acquired on quartz fiber filters using a high-volume air sampler (Hi-Vol) attached with a slotted impactor. Filters were sonicated in dichloromethane:methanol (9:1); extracts concentrated. A suite of more than 200 individual organic compounds was identified in the PM2.5 samples. Molecular markers, homologous compound series, and non-polar and polar organic compounds were detected at ng/m3 ambient concentrations using gas chromatography/mass spectrometry (GC/MS). Measurements of the organic carbon (OC) and elemental carbon (EC) were also made. Organic compounds detected in the size-segregated samples were grouped into different classes including phthalates and adipates, n-alkanes, alkanoic acids, cyclic siloxanes, waxes, benzoates, polyethylene glycols, squalene, and 4-nitro-butylated phenol. Results indicated that these organic species were predominantly associated in the fine particle mode (< 2.5 um). Gaseous organic compounds trapped in the PUF appeared rich in phenol, 4-nitro-2,6-ditertbutylphenol, pentachlorophenol, benzoic acid, alkanoic acids (C6 - C16 ), PAHs (naphthalene to pyrene), and phthalates. The major part of the extractable and elutable organic carbon was found to correspond to a complex mixture of phthalates and adipates, benzoate esters, n-alkanes, methyl silicates, phosphate esters, aldehydes and ketones, alcohols, alkyl amines, nitrosamines, formamides, amides, morpholines, carboxylic acids, methyl and isopropyl esters, dicarboxylic acids, waxes, lactones, hopanes, ionol 2, and PAHs. The most abundant classes of compounds are

  7. What is the "Clim-Likely" aerosol product?

    Atmospheric Science Data Center

    2014-12-08

    ... model were medium and coarse mode mineral dust, sulfate, sea salt, black carbon, and carbonaceous aerosols. Five aerosol air mass "Mixing ... component particles in the column for climatologically common aerosol air masses. Each sub-group identifies the dominant particles ...

  8. Natural and transboundary pollution influences on sulfate-nitrate-ammonium aerosols in the United States: Implications for policy

    NASA Astrophysics Data System (ADS)

    Park, Rokjin J.; Jacob, Daniel J.; Field, Brendan D.; Yantosca, Robert M.; Chin, Mian

    2004-08-01

    We use a global three-dimensional coupled oxidant-aerosol model (GEOS-CHEM) to estimate natural and transboundary pollution influences on sulfate-nitrate-ammonium aerosol concentrations in the United States. This work is motivated in part by the Regional Haze Rule of the U.S. Environmental Protection Agency (EPA), which requires immediate action to improve visibility in U.S. wilderness areas along a linear trajectory toward an endpoint of "natural visibility conditions" by 2064. We present full-year simulations for 1998 and 2001 and evaluate them with nationwide networks of observations in the United States and Europe (Interagency Monitoring of Protected Visual Environments (IMPROVE), Clean Air Status and Trends Network (CASTNET), National Atmospheric Deposition Program (NADP), European Monitoring and Evaluation Programme (EMEP)) and with Asian outflow observations from the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft mission. Shutting off U.S. anthropogenic emissions in the model defines "background" aerosol concentrations representing contributions from both natural and transboundary pollution sources. We find that transboundary transport of pollution from Canada, Mexico, and Asia dominates over natural influences for both sulfate and nitrate. Trans-Pacific transport of Asian pollution accounts for 30% of background sulfate in both the western and eastern United States. Our best estimates of natural concentrations for ammonium sulfate and ammonium nitrate in the United States are either consistent with or lower than the default values recommended by EPA for natural visibility calculations. However, the large transboundary pollution influence in our calculation suggests that a natural visibility objective cannot be approached without international emission controls.

  9. Aerosol Optical Depth (AOD) Retrieval using GOES-East and GOES-West Reflected Radiances over the Western United States

    NASA Astrophysics Data System (ADS)

    Zhang, H.; Hoff, R. M.; Kondragunta, S.; Laszlo, I.; Lyapustin, A.

    2012-12-01

    The western United States is observed by both GOES-East and GOES-West imagers. The TOA reflectance measured from the two satellites has different sensitivity to AOD variations due to the different observation geometries. The GASP (GOES Aerosol/Smoke Product) aerosol optical depth retrieval algorithm only applies to single satellite data and thus obtains two separate aerosol optical depth values at the same time for the same location. In order to fully exploit the simultaneous observations and generate consistent AOD retrievals from the two satellites, we develop a new aerosol optical depth retrieval algorithm that uses data from both satellites. The algorithm uses combined GOES-East and GOES-West visible channel TOA reflectance and daily average AOD from GOES Multi-Angle Implementation of Atmospheric Correction (MAIAC) on clear days (AOD less than 0.3), when diurnal variation of AOD is low, to retrieve surface BRDF. The known BRDF shape is applied on the follow-on days to retrieve BRDF and AOD. The algorithm is validated at three AERONET sites over the western US. The AOD retrieval accuracy from two satellites is similar to that from one satellite, with correlation coefficients ranging from 0.71 to 0.81 for the three sites. However, the new algorithm has more data coverage compared to the single satellite retrievals. The number of coincidences with AERONET observations increases from the single satellite algorithm by 20 - 70% for the three sites. With the application of the new algorithm, we can provide consistent AOD retrievals with better retrieval coverage using the two GOES satellite imagers.

  10. Tropospheric Aerosols

    NASA Astrophysics Data System (ADS)

    Buseck, P. R.; Schwartz, S. E.

    2003-12-01

    anthropogenic aerosols are thought to be of comparable magnitude to the positive forcings resulting from incremental concentrations of greenhouse gases.The magnitudes and estimated uncertainties of the several forcings over the industrial period are summarized in Figure 2, which was prepared as part of the recent assessment of climate change by the Intergovernmental Panel on Climate Change (IPCC, 2001). This figure shows for each forcing a best estimate of its magnitude and of the associated uncertainty. The uncertainty associated with forcing by the long-lived greenhouse gases is relatively small, reflective of the rather high level of understanding of both the magnitude of the incremental concentrations of these species and of the radiative perturbation per incremental concentration. In marked contrast, the uncertainties associated with the several aerosol forcings are much greater, indicative of a much lesser understanding of the controlling quantities. For direct forcing by dust aerosols, which may be positive or negative, and for indirect radiative forcing by anthropogenic aerosols the IPCC working groups ( Penner et al., 2001; Ramaswamy et al., 2001) declined to present best estimates but indicated only possible ranges. This situation is unsatisfying but unavoidable, given the current state of knowledge. Other reviews of aerosol forcings are provided by Ramanathan et al. (2001a), Haywood and Boucher (2000), Shine and Forster (1999), Schwartz (1996), and Schwartz and Slingo (1996). Hobbs (1993) provides an introduction to aerosol-cloud interactions. (9K)Figure 2. The effects of various anthropogenic constituents of the atmosphere on the global climate system for the year 2000 relative to 1750 as estimated by the Intergovernmental Panel on Climate Change (IPCC, 2001). The effects are expressed as forcings, which in this case are changes in global mean radiative flux components arising from the indicated perturbing influence. Best estimates are indicated by the bars and

  11. Geometric approach to non-relativistic quantum dynamics of mixed states

    NASA Astrophysics Data System (ADS)

    Gimeno, Vicent; Sotoca, Jose M.

    2013-05-01

    In this paper we propose a geometrization of the non-relativistic quantum mechanics for mixed states. Our geometric approach makes use of the Uhlmann's principal fibre bundle to describe the space of mixed states and as a novelty tool, to define a dynamic-dependent metric tensor on the principal manifold, such that the projection of the geodesic flow to the base manifold gives the temporal evolution predicted by the von Neumann equation. Using that approach we can describe every conserved quantum observable as a Killing vector field, and provide a geometric proof for the Poincaré quantum recurrence in a physical system with finite energy levels.

  12. Electrodynamic field equations for composite superconducting structures in the mixed state

    SciTech Connect

    Coffey, M.W.

    1997-08-01

    Governing vector partial differential equations for the linear electrodynamic response of an isotropic type-II superconductor in the mixed state are derived. A continuum theory of vortex motion is used, and two-fluid effects are also accounted for. The governing equation is sufficiently general to reduce to either normal metal or dielectric material results in special limits. The complex-valued conductivity tensor of the mixed state is made explicit, and is also discussed for an anisotropic superconductor. The theory is illustrated with a planar superconducting waveguide problem, wherein the complex propagation constant, phase velocity, and surface impedance are obtained.

  13. Attribution of the United States “warming hole”: Aerosol indirect effect andprecipitable water vapor

    EPA Science Inventory

    Aerosols can influence the climate indirectly by acting as cloud condensation nuclei and /or ice nuclei, thereby modifying cloud optical properties. Observations show a striking cooling trend in summertime daily maximum temperature (Tmax) in the central and...

  14. SOURCE APPORTIONMENT OF PRIMARY AND SECONDARY CARBONACEOUS AEROSOL IN THE UNITED STATES USING MODELS AND MEASUREMENTS

    EPA Science Inventory

    In this presentation, three diagnostic evaluation methods of model performance for carbonaceous aerosol are reviewed. The EC-tracer method is used to distinguish primary and secondary carbon, radiocarbon data are used to distinguish fossil-fuel and contemporary carbon, and organ...

  15. Automated Chemical Analysis of Internally Mixed Aerosol Particles Using X-ray Spectromicroscopy at the Carbon K-Edge

    SciTech Connect

    Gilles, Mary K; Moffet, R.C.; Henn, T.; Laskin, A.

    2011-01-20

    We have developed an automated data analysis method for atmospheric particles using scanning transmission X-ray microscopy coupled with near edge X-ray fine structure spectroscopy (STXM/NEXAFS). This method is applied to complex internally mixed submicrometer particles containing organic and inorganic material. Several algorithms were developed to exploit NEXAFS spectral features in the energy range from 278 to 320 eV for quantitative mapping of the spatial distribution of elemental carbon, organic carbon, potassium, and noncarbonaceous elements in particles of mixed composition. This energy range encompasses the carbon K-edge and potassium L2 and L3 edges. STXM/NEXAFS maps of different chemical components were complemented with a subsequent analysis using elemental maps obtained by scanning electron microscopy coupled with energy dispersive X-ray analysis (SEM/EDX). We demonstrate the application of the automated mapping algorithms for data analysis and the statistical classification of particles.

  16. Mixing of anthropogenic dust and carbonaceous aerosols in seasonal snow on snow albedo reduction in 2014 China survey

    NASA Astrophysics Data System (ADS)

    Wang, Xin; Huang, Jianping; Pu, Wei

    2016-04-01

    Anthropogenic dusts produced from the affected by human activities derived from the industrial areas and carbonaceous aerosols (black carbon and organic carbon) deposited into snow or ice core via wet and dry deposition play key roles to the regional and global climate. Recently, a China survey was performed to measure the concentrations of insoluble light-absorbing particles (ILAP) in seasonal snow across northern China in January and February of 2014. The results indicate that the higher concentration of NO3- and SO42- and heavy metals of Zn, Pb, Cd, Ni, and Cu are likely to be attributed to enhanced local industrial emissions due to human activities. The emissions from fossil fuel combustion and biomass burning are likely to be important for the chemical elements in the seasonal snow with long-range transport, while medium enrichment factors of Mg, Ca, and Al were predominantly associated with soil dust, which is the most important natural source. There are large ranges of the BC and AD in seasonal snow over northeast China because of the anthropogenic emissions, which are caused by human activities. In addition, although the values of the snow albedo by model simulations are little higher in the visible to near-infrared wavelength than that during the China survey, the surface snow albedo by field campaign measurements have good agreement with the model simulations in the visible wavelength.

  17. Determination of external and internal mixing of organic and inorganic aerosol components from equilibrium water uptake by sub-micrometer particles.

    NASA Astrophysics Data System (ADS)

    Aklilu, Y.; Mozurkewich, M.

    2002-12-01

    The ability of a particle to gain and lose water with changes in relative humidity is fundamental to particle's effectiveness as a cloud condensation nucleus, chemical reactivity, atmospheric residence time and influence on global radiation balance. We describe a method developed to measure particle hygroscopicity over a range of relative humidities (RH) from 50% to 85%. Ambient aerosol particles were dried, monodisperse particles with diameters of usually 50 and 114 nm were selected, and their size distribution following humidification was measured. We measured particle hygroscopicity at Golden Ears Provincial Park and Eagle Ridge Mountain as part of the Pacific 2001 field study in the lower Fraser Valley in August of 2001. The humidified size distributions were sometimes monomodal and sometimes bimodal distribution with less and more hygroscopic peaks. The hygroscopicity of the monomodal particles varied between that of the less and more hygroscopic particles. The less hygroscopic particles were probably almost entirely organic in composition; they had consistent growth curves with wet/dry diameter ratios that increased from 1.04 at 50% relative humidity to 1.09 at 80% RH. These less hygroscopic particles constituted almost all the sampled aerosol at the forested site in Golden Ears Park and during the rainy periods at Eagle Ridge. At other times there were more hygroscopic particles, either as a single mixed mode or as a distinct mode in addition to the less hygroscopic particles. These showed little growth below 70% RH and pronounced growth above 70%. The increased water sorption above 70% RH is likely due to the particles containing (NH4)3H(SO4)2 or (NH4)2(SO4), as these salts deliquesce at 70% and 80% RH, respectively. Since the growth of these particles was less than expected for the pure salts, we conclude that these particles consisted of a mixture of the organic and inorganic components. An estimate of the relative organic fraction was made using the

  18. Theory of degenerate three-wave mixing using circuit QED in solid-state circuits

    SciTech Connect

    Cao, Ye; Huo, Wen Yi; Ai, Qing; Long, Gui Lu

    2011-11-15

    We study the theory of degenerate three-wave mixing and the generation of squeezed microwaves using circuit quantum electrodynamics in solid state circuits. The Hamiltonian for degenerate three-wave mixing, which seemed to be given phenomenologically in quantum optics, is derived by quantum mechanical calculations. The nonlinear medium needed in three-wave mixing is composed of a series of superconducting charge qubits which are located inside two superconducting transmission-line resonators. Here, the multiqubit ensemble is present to enhance the effective coupling constant between the two modes in the transmission-line resonators. In the squeezing process, the qubits are kept in their ground states so that their decoherence does not corrupt the squeezing. The main obstacle preventing a large squeezing efficiency is the decay rate of the transmission-line resonator.

  19. Communication: state mixing by spin-orbit coupling in the anionic chloroiodine dissociations.

    PubMed

    Xia, L; Wang, X-D; Xuan, C-J; Zeng, X-J; Li, H-K; Tian, S X; Pan, Y; Lau, K-C

    2014-01-28

    Three spin-orbit states, 1(2)Π1/2, 2(2)Π3/2, and 2(2)Π1/2, of chloroiodine anion (ICl(-)) formed by low-energy electron attachment in the Franck-Condon region are associated with the dissociative limits of I(-) ((1)S0) and Cl ((2)P3/2) or Cl(*) ((2)P1/2) fragments. Within the adiabatic scheme, the presumptive Π-symmetry of the fragment angular distributions is dramatically changed to be the Π-Σ mixing symmetry, due to the significant spin-orbit interaction effect on the electronic state couplings of ICl(-). The present experimental approach also enables us to separate the contributions of different electronic states from the mixed states, providing a crucial method for quantitatively evaluating the configuration-interaction wavefunctions. PMID:25669497

  20. Sensitivity of the Ocean State to Internal Lee Wave Driven Mixing

    NASA Astrophysics Data System (ADS)

    Melet, A. V.; Hallberg, R.; Legg, S.; Nikurashin, M.

    2012-12-01

    Diapycnal mixing plays a key role in maintaining the ocean stratification and meridional overturning circulation. In the ocean interior, diapycnal mixing is mainly sustained by the breaking of internal gravity waves which are generated by abyssal flows interacting with rough topography. Two classes of topographic internal waves in the ocean are: internal tides, generated by barotropic tides, and lee waves, generated by geostrophic flows over rough topography. Currently, climate models include only a parameterization of mixing due to local dissipation of internal tides, using the scheme of St Laurent et al. (2002). In this study, we explore the combined effect of internal tide and lee wave driven mixing on the ocean state. We performed a series of sensitivity experiments using two models, developed at GFDL and configured for global simulations at one degree resolution: the GOLD isopycnal ocean model and the CM2G ocean-atmosphere coupled model. In these models, internal-tide driven mixing is parameterized using the St Laurent et al. (2002) scheme. We added a parameterization of lee wave driven mixing by using a recently estimated global map of energy conversion into lee waves (Nikurashin and Ferrari, 2011) in the St Laurent et al. (2002) scheme, with varying fraction of local dissipation and vertical decay scale. We show that although the global energy input into lee waves (0.2 TW) is small compared to that into internal tides (1 TW), lee wave driven mixing makes a significant impact on the ocean state. Notably, the addition of lee wave driven mixing impacts the thermal structure of the ocean, water mass transformation rates and the meridional overturning circulation. The vertically-integrated circulation is also impacted, notably in the Southern Ocean which accounts for half the lee-wave energy flux. Finally, we show that the different spatial distribution of the internal tide and lee wave energy input impacts the sensitivity described in this study. Our modeling

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

    SciTech Connect

    Schmid, Beat; Ferrare, Richard; Flynn, Connor M.; Elleman, Robert; Covert, David; Strawa, A.; Welton, E J.; Turner, David D.; Jonsson, Haf; Redemann, Jens; Eilers, J.; Ricci, K.; Hallar, A. G.; Clayton, M. B.; Michalsky, Joseph J.; Smirnov, A.; Holben, B. N.; Barnard, James C.

    2006-02-01

    The recent U.S. Department of Energy Atmospheric Radiation Measurements (ARM) Aerosol Intensive Observation Period (AIOP, 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. 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 instruments: airborne Sun photometer, airborne nephelometer/absorption photometer, airborne cavity ring-down system, ground-based Raman lidar and two ground-based elastic backscatter lidars. We find the in situ measurements to be biased low (2 - 4 Mm 1 equivalent to 12-17% in the visible, or 45% in the near-infrared) when compared to airborne sunphotometer extinction. On the other hand, we find that with respect to AATS-14, the lidar ?ep(?) are biased high. Bias differences are 0.004 Km-1 (13%) and 0.007 Km-1 (24%) for the two elastic back-scatter lidars (MPLARM and MPLNET, ? = 523 nm) and 0.029 Km-1 (54%) for the Raman lidar (? = 355 nm). 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 six field campaigns conducted since 1996, airborne in situ measurements of extinction tend to be biased slightly low (17% at visible wavelengths) when compared to airborne sunphotometer extinction. On the other hand, extinction derived from lidars tend to have no or positive biases. We conclude that the 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

  2. 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.; Eilers, J.; Ricci, K.; Hallar, A. G.; Clayton, M.; Michalsky, J.; Smirnov, A.; Holben, B.; Barnard, J.

    2006-01-01

    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 the UV and near-infrared.

  3. Self-Mixing Thin-Slice Solid-State Laser Metrology

    PubMed Central

    Otsuka, Kenju

    2011-01-01

    This paper reviews the dynamic effect of thin-slice solid-state lasers subjected to frequency-shifted optical feedback, which led to the discovery of the self-mixing modulation effect, and its applications to quantum-noise-limited versatile laser metrology systems with extreme optical sensitivity. PMID:22319406

  4. Self-mixing thin-slice solid-state laser metrology.

    PubMed

    Otsuka, Kenju

    2011-01-01

    This paper reviews the dynamic effect of thin-slice solid-state lasers subjected to frequency-shifted optical feedback, which led to the discovery of the self-mixing modulation effect, and its applications to quantum-noise-limited versatile laser metrology systems with extreme optical sensitivity.

  5. Quantum metrology with mixed states: When recovering lost information is better than never losing it

    NASA Astrophysics Data System (ADS)

    Haine, Simon A.; Szigeti, Stuart S.

    2015-09-01

    Quantum-enhanced metrology can be achieved by entangling a probe with an auxiliary system, passing the probe through an interferometer, and subsequently making measurements on both the probe and auxiliary system. Conceptually, this corresponds to performing metrology with the purification of a (mixed) probe state. We demonstrate via the quantum Fisher information how to design mixed states whose purifications are an excellent metrological resource. In particular, we give examples of mixed states with purifications that allow (near) Heisenberg-limited metrology and provide examples of entangling Hamiltonians that can generate these states. Finally, we present the optimal measurement and parameter-estimation procedure required to realize these sensitivities (i.e., that saturate the quantum Cramér-Rao bound). Since pure states of comparable metrological usefulness are typically challenging to generate, it may prove easier to use this approach of entanglement and measurement of an auxiliary system. An example where this may be the case is atom interferometry, where entanglement with optical systems is potentially easier to engineer than the atomic interactions required to produce nonclassical atomic states.

  6. Aerosol emissions from prescribed fires in the United States: A synthesis of laboratory and aircraft measurements

    NASA Astrophysics Data System (ADS)

    May, A. A.; McMeeking, G. R.; Lee, T.; Taylor, J. W.; Craven, J. S.; Burling, I.; Sullivan, A. P.; Akagi, S.; Collett, J. L.; Flynn, M.; Coe, H.; Urbanski, S. P.; Seinfeld, J. H.; Yokelson, R. J.; Kreidenweis, S. M.

    2014-10-01

    Aerosol emissions from prescribed fires can affect air quality on regional scales. Accurate representation of these emissions in models requires information regarding the amount and composition of the emitted species. We measured a suite of submicron particulate matter species in young plumes emitted from prescribed fires (chaparral and montane ecosystems in California; coastal plain ecosystem in South Carolina) and from open burning of over 15 individual plant species in the laboratory. We report emission ratios and emission factors for refractory black carbon (rBC) and submicron nonrefractory aerosol and compare field and laboratory measurements to assess the representativeness of our laboratory-measured emissions. Laboratory measurements of organic aerosol (OA) emission factors for some fires were an order of magnitude higher than those derived from any of our aircraft observations; these are likely due to higher-fuel moisture contents, lower modified combustion efficiencies, and less dilution compared to field studies. Nonrefractory inorganic aerosol emissions depended more strongly on fuel type and fuel composition than on combustion conditions. Laboratory and field measurements for rBC were in good agreement when differences in modified combustion efficiency were considered; however, rBC emission factors measured both from aircraft and in the laboratory during the present study using the Single Particle Soot Photometer were generally higher than values previously reported in the literature, which have been based largely on filter measurements. Although natural variability may account for some of these differences, an increase in the BC emission factors incorporated within emission inventories may be required, pending additional field measurements for a wider variety of fires.

  7. Airborne observations of regional variation in fluorescent aerosol across the United States

    NASA Astrophysics Data System (ADS)

    Perring, A. E.; Schwarz, J. P.; Baumgardner, D.; Hernandez, M. T.; Spracklen, D. V.; Heald, C. L.; Gao, R. S.; Kok, G.; McMeeking, G. R.; McQuaid, J. B.; Fahey, D. W.

    2015-02-01

    Airborne observations of fluorescent aerosol were made aboard an airship during CloudLab, a series of flights that took place in September and October of 2013 and covered a wideband of longitude across the continental U.S. between Florida and California and between 28 and 37 N latitudes. Sampling occurred from near the surface to 1000 m above the ground. A Wideband Integrated Bioaerosol Sensor (WIBS-4) measured average concentrations of supermicron fluorescent particles aloft (1 µm to 10 µm), revealing number concentrations ranging from 2.1 ± 0.8 to 8.7 ± 2.2 × 104 particles m-3 and representing up to 24% of total supermicron particle number. We observed distinct variations in size distributions and fluorescent characteristics in different regions, and attribute these to geographically diverse bioaerosol. Fluorescent aerosol detected in the east is largely consistent with mold spores observed in a laboratory setting, while a shift to larger sizes associated with different fluorescent patterns is observed in the west. Fluorescent bioaerosol loadings in the desert west were as high as those near the Gulf of Mexico, suggesting that bioaerosol is a substantial component of supermicron aerosol both in humid and arid environments. The observations are compared to model fungal and bacterial loading predictions, and good agreement in both particle size and concentrations is observed in the east. In the west, the model underestimated observed concentrations by a factor between 2 and 4 and the prescribed particle sizes are smaller than the observed fluorescent aerosol. A classification scheme for use with WIBS data is also presented.

  8. Excited electronic state mixing in 7-azaindole. Quantitative measurements using the Stark effect.

    PubMed

    Young, Justin W; Pozun, Zachary D; Jordan, Kenneth D; Pratt, David W

    2013-12-12

    Stark effect measurements of the +280 cm(-1) vibronic band at ∼286 nm in the high resolution S1-S0 fluorescence excitation spectrum of 7-azaindole (7AI) in a molecular beam show that the permanent (electric) dipole moment (PDM) of the upper state vibrational level reached in this transition is 4.6 D, twice as large as the PDM of the zero-point level of the S1 state. This large difference is attributed to state mixing with a more polar state. EOM-CSSD calculations suggest that this more polar state is σπ* in nature and that it crosses the ππ* state in energy along the coordinate connecting the two potential energy minima. Such state mixing apparently provides more facile access to conical intersections with the ground state, and subsequent hydrogen atom detachment reactions, since independent studies by Sakota and Sekiya have shown that the N-H stretching frequency of 7AI is significantly reduced when it is excited to the +280 cm(-1) vibrational level of the S1 state.

  9. Sources of Water-soluble Organic Aerosol in the Southeastern United States - Evidence of SOA Formed Through Heterogeneous Reactions

    NASA Astrophysics Data System (ADS)

    Zhang, X.; Weber, R. J.

    2010-12-01

    . Weber (2010), Water-soluble organic aerosol material and the light-absorption characteristics of aqueous extracts measured over the southeastern United States, Atm. Chem. Phys., 10, 5965-5977. Hennigan, C. J., M. H. Bergin, J. E. Dibb, and R. J. Weber (2008a), Enhanced secondary organic aerosol formation due to water uptake by fine particles, Geophys. Res. Lett., 35, L18801, 18810.11029/12008GL035046. Hennigan, C. J., M. H. Bergin, and R. J. Weber (2008b), Correlations between water-soluble organic aerosol and water vapor: A synergistic effect from biogenic emissions?, Environ. Sci. Tech., 42(24), 9079-9085. Hennigan, C. J., et al. (2008c), On the volatility and production mechanisms of newly formed nitrate and water soluble organic aerosol in Mexico City, Atm. Chem. Phys., 8, 3761-3768. Hennigan, C. J., M. H. Bergin, A. G. Russell, A. Nenes, and R. J. Weber (2009), Gas/particle partitioning of water-soluble organic aerosol in Atlanta, Atm. Chem. Phys., 9, 3613-3628. Zhang, X., A. Hecobian, M. Zheng, N. Frank, and R. J. Weber (2010), Biomass buring impact on PM2.5 over the southeastern U.S.: Intgrating chemically speciated FRM filter measurements, MODIS fire counts and PMF analysis, Atm. Chem. Phys., 10, 6839-6853.

  10. Role of clouds, aerosols, and aerosol-cloud interaction in 20th century simulations with GISS ModelE2

    NASA Astrophysics Data System (ADS)

    Nazarenko, L.; Rind, D. H.; Bauer, S.; Del Genio, A. D.

    2015-12-01

    Simulations of aerosols, clouds and their interaction contribute to the major source of uncertainty in predicting the changing Earth's energy and in estimating future climate. Anthropogenic contribution of aerosols affects the properties of clouds through aerosol indirect effects. Three different versions of NASA GISS global climate model are presented for simulation of the twentieth century climate change. All versions have fully interactive tracers of aerosols and chemistry in both the troposphere and stratosphere. All chemical species are simulated prognostically consistent with atmospheric physics in the model and the emissions of short-lived precursors [Shindell et al., 2006]. One version does not include the aerosol indirect effect on clouds. The other two versions include a parameterization of the interactive first indirect aerosol effect on clouds following Menon et al. [2010]. One of these two models has the Multiconfiguration Aerosol Tracker of Mixing state (MATRIX) that permits detailed treatment of aerosol mixing state, size, and aerosol-cloud activation. The main purpose of this study is evaluation of aerosol-clouds interactions and feedbacks, as well as cloud and aerosol radiative forcings, for the twentieth century climate under different assumptions and parameterizations for aerosol, clouds and their interactions in the climate models. The change of global surface air temperature based on linear trend ranges from +0.8°C to +1.2°C between 1850 and 2012. Water cloud optical thickness increases with increasing temperature in all versions with the largest increase in models with interactive indirect effect of aerosols on clouds, which leads to the total (shortwave and longwave) cloud radiative cooling trend at the top of the atmosphere. Menon, S., D. Koch, G. Beig, S. Sahu, J. Fasullo, and D. Orlikowski (2010), Black carbon aerosols and the third polar ice cap, Atmos. Chem. Phys., 10,4559-4571, doi:10.5194/acp-10-4559-2010. Shindell, D., G. Faluvegi

  11. Characterization of submicron particles influenced by mixed biogenic and anthropogenic emissions using high-resolution aerosol mass spectrometry: results from CARES

    SciTech Connect

    Setyan, Ari; Zhang, Qi; Merkel, M.; Knighton, Walter B.; Sun, Y.; Song, Chen; Shilling, John E.; Onasch, Timothy B.; Herndon, Scott C.; Worsnop, Douglas R.; Fast, Jerome D.; Zaveri, Rahul A.; Berg, Larry K.; Wiedensohler, A.; Flowers, B. A.; Dubey, Manvendra K.; Subramanian, R.

    2012-09-11

    The Carbonaceous Aerosols and Radiative Effects Study (CARES) took place in the Sacramento Valley of California in summer 2010. We present results obtained at Cool, CA, the T1 site of the project ({approx}40 km downwind of urban emissions from Sacramento), where we deployed an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) in parallel with complementary instrumentation to characterize the sources and processes of submicron particles (PM1). Cool is located at the foothill of the Sierra Nevada Mountains, where intense biogenic emissions are periodically mixed with urban outflow transported by daytime southwesterly winds from the Sacramento metropolitan area. The particle mass loading was low (3.0 {micro}gm{sup -3} on average) and dominated by organics (80% of the PM1 mass) followed by sulfate (9.9 %). Organics and sulfate appeared to be externally mixed, as suggested by their different time series (r2 = 0.13) and size distributions. Sulfate showed a bimodal distribution with a droplet mode peaking at {approx}400nm in vacuum aerodynamic diameter (Dva), and a condensation mode at {approx}150 nm, while organics generally displayed a broad distribution in 60-600nm (Dva). New particle formation and growth events were observed almost every day, emphasizing the roles of organics and sulfate in new particle growth, especially that of organics. The organic aerosol (OA) had a nominal formula of C{sub 1}H{sub 1.38}N{sub 0.004}O{sub 0.44}, thus an average organic mass-to-carbon (OM/OC) ratio of 1.70. Two different oxygenated OA (OOA, 90% of total OA mass) and a hydrocarbon-like OA (HOA, 10 %) were identified by Positive matrix factorization (PMF) of the high resolution mass spectra. The more oxidized MO-OOA (O/C = 0.54) corresponded to secondary OA (SOA) primarily influenced by biogenic emissions, while the less oxidized LO-OOA (O/C = 0.42) corresponded to SOA associated with urban transport. The HOA factor corresponded to primary emissions mainly

  12. The Two-Column Aerosol Project: Phase I—Overview and impact of elevated aerosol layers on aerosol optical depth

    NASA Astrophysics Data System (ADS)

    Berg, Larry K.; Fast, Jerome D.; Barnard, James C.; Burton, Sharon P.; Cairns, Brian; Chand, Duli; Comstock, Jennifer M.; Dunagan, Stephen; Ferrare, Richard A.; Flynn, Connor J.; Hair, Johnathan W.; Hostetler, Chris A.; Hubbe, John; Jefferson, Anne; Johnson, Roy; Kassianov, Evgueni I.; Kluzek, Celine D.; Kollias, Pavlos; Lamer, Katia; Lantz, Kathleen; Mei, Fan; Miller, Mark A.; Michalsky, Joseph; Ortega, Ivan; Pekour, Mikhail; Rogers, Ray R.; Russell, Philip B.; Redemann, Jens; Sedlacek, Arthur J.; Segal-Rosenheimer, Michal; Schmid, Beat; Shilling, John E.; Shinozuka, Yohei; Springston, Stephen R.; Tomlinson, Jason M.; Tyrrell, Megan; Wilson, Jacqueline M.; Volkamer, Rainer; Zelenyuk, Alla; Berkowitz, Carl M.

    2016-01-01

    The Two-Column Aerosol Project (TCAP), conducted from June 2012 through June 2013, was a unique study designed to provide a comprehensive data set that can be used to investigate a number of important climate science questions, including those related to aerosol mixing state and aerosol radiative forcing. The study was designed to sample the atmosphere between and within two atmospheric columns; one fixed near the coast of North America (over Cape Cod, MA) and a second moveable column over the Atlantic Ocean several hundred kilometers from the coast. The U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) was deployed at the base of the Cape Cod column, and the ARM Aerial Facility was utilized for the summer and winter intensive observation periods. One important finding from TCAP is that four of six nearly cloud-free flight days had aerosol layers aloft in both the Cape Cod and maritime columns that were detected using the nadir pointing second-generation NASA high-spectral resolution lidar (HSRL-2). These layers contributed up to 60% of the total observed aerosol optical depth (AOD). Many of these layers were also intercepted by the aircraft configured for in situ sampling, and the aerosol in the layers was found to have increased amounts of biomass burning material and nitrate compared to aerosol found near the surface. In addition, while there was a great deal of spatial and day-to-day variability in the aerosol chemical composition and optical properties, no systematic differences between the two columns were observed.

  13. Aircraft observations of aerosol composition and ageing in New England and Mid-Atlantic States during the summer 2002 New England Air Quality Study field campaign

    NASA Astrophysics Data System (ADS)

    Kleinman, Lawrence I.; Daum, Peter H.; Lee, Yin-Nan; Senum, Gunnar I.; Springston, Stephen R.; Wang, Jian; Berkowitz, Carl; Hubbe, John; Zaveri, Rahul A.; Brechtel, Fred J.; Jayne, John; Onasch, Timothy B.; Worsnop, Douglas

    2007-05-01

    Aerosol chemical composition, size distribution, and optical properties were measured during 17 aircraft flights in New England and Middle Atlantic States as part of the summer 2002 New England Air Quality Study field campaign. An Aerodyne aerosol mass spectrometer (AMS) was operated with a measurement cycle of 30 s, about an order of magnitude faster than used for ground-based measurements. Noise levels within a single measurement period were sub μg m-3. Volume data derived from the AMS were compared with volume measurements from a Passive Cavity Aerosol Spectrometer (PCASP) optical particle detector and a Twin Scanning Electrical Mobility Spectrometer (TSEMS); calculated light scattering was compared with measured values from an integrating nephelometer. The median ratio for AMS/TSEMS volume was 1.25 (1.33 with an estimated refractory component); the median ratio for AMS/nephelometer scattering was 1.18. A dependence of the AMS collection efficiency on aerosol acidity was quantified by a comparison between AMS and PCASP volumes in two high sulfate plumes. For the entire field campaign, the average aerosol concentration was 11 μg m-3. Compared with monitoring data from the IMPROVE network, the organic component made up a large fraction of total mass, varying from 70% in clean air to 40% in high concentration sulfate plumes. In combination with other optical and chemical measurements, the AMS gave information on secondary organic aerosol (SOA) production and the time evolution of aerosol light absorption. CO is taken as a conservative tracer of urban emissions and the ratios of organic aerosol and aerosol light absorption to CO examined as a function of photochemical age. Comparisons were made to ratios determined from surface measurements under conditions of minimal atmospheric processing. In air masses in which the NOx to NOy ratio has decreased to 10%, the ratio of organic aerosol to CO has quadrupled indicating that 75% of the organic aerosol is secondary

  14. Distillation of mixed-state continuous-variable entanglement by photon subtraction

    SciTech Connect

    Zhang Shengli; Loock, Peter van

    2010-12-15

    We present a detailed theoretical analysis for the distillation of one copy of a mixed two-mode continuous-variable entangled state using beam splitters and coherent photon-detection techniques, including conventional on-off detectors and photon-number-resolving detectors. The initial Gaussian mixed-entangled states are generated by transmitting a two-mode squeezed state through a lossy bosonic channel, corresponding to the primary source of errors in current approaches to optical quantum communication. We provide explicit formulas to calculate the entanglement in terms of logarithmic negativity before and after distillation, including losses in the channel and the photon detection, and show that one-copy distillation is still possible even for losses near the typical fiber channel attenuation length. A lower bound for the transmission coefficient of the photon-subtraction beam splitter is derived, representing the minimal value that still allows to enhance the entanglement.

  15. GENERAL: Thermal entanglement and teleportation of a thermally mixed entangled state of a Heisenberg chain through a Werner state

    NASA Astrophysics Data System (ADS)

    Huang, Li-Yuan; Fang, Mao-Fa

    2008-07-01

    The thermal entanglement and teleportation of a thermally mixed entangled state of a two-qubit Heisenberg XXX chain under the Dzyaloshinski-Moriya (DM) anisotropic antisymmetric interaction through a noisy quantum channel given by a Werner state is investigated. The dependences of the thermal entanglement of the teleported state on the DM coupling constant, the temperature and the entanglement of the noisy quantum channel are studied in detail for both the ferromagnetic and the antiferromagnetic cases. The result shows that a minimum entanglement of the noisy quantum channel must be provided in order to realize the entanglement teleportation. The values of fidelity of the teleported state are also studied for these two cases. It is found that under certain conditions, we can transfer an initial state with a better fidelity than that for any classical communication protocol.

  16. CCN Study at Urban Supersite (T0) During MILAGRO: the Essential Information for Prediction of Aerosol CCN Concentrations

    NASA Astrophysics Data System (ADS)

    Wang, J.; Cubison, M.; Aiken, A. C.; Jimenez, J. L.; Collins, D. R.

    2009-12-01

    The influences of atmospheric aerosols on cloud properties (i.e., aerosol indirect effects) strongly depend on the aerosol CCN concentrations, which can be effectively predicted from detailed aerosol size distribution, mixing state, and chemical composition using Köhler theory. However, atmospheric aerosols often consist of a large number of species that cannot be individually simulated in global or regional models due to computational constraints. Furthermore, the thermodynamic properties or even the molecular identities of many organic species present in ambient aerosols are often not known to predict their cloud-activation behavior using Köhler theory. As a result, simplified presentations of aerosol composition are necessary for large-scale models. In this study, aerosol microphysics, CCN concentrations, and chemical composition measured at the T0 urban supersite in Mexico City during MILAGRO are analyzed and the degree of closure is evaluated. During the campaign in March 2006, aerosol size distribution and composition often showed strong diurnal variation as a result of both primary emissions and aging of aerosols through coagulation and local photochemical production of secondary aerosol species. The submicron aerosol composition was ~1/2 organic species. Closure analysis is first carried out by comparing CCN concentrations calculated from the measured aerosol size distribution, mixing state, and chemical composition using extended Köhler theory to concurrent CCN measurements at five supersaturations ranging from 0.11% to 0.35%. The closure agreement and its diurnal variation are studied. CCN concentrations are also derived using various simplifications of the measured aerosol mixing state and chemical composition. The uncertainties associated with these simplifications are compared for different supersaturations and the variation of the uncertainties is examined as a function of aerosol age. The results show that the simplification of internally mixed

  17. Quasi-biennial oscillation of the tropical stratospheric aerosol layer

    NASA Astrophysics Data System (ADS)

    Hommel, R.; Timmreck, C.; Giorgetta, M. A.; Graf, H. F.

    2015-05-01

    This study describes how aerosol in an aerosol-coupled climate model of the middle atmosphere is influenced by the quasi-biennial oscillation (QBO) during times when the stratosphere is largely unperturbed by volcanic material. In accordance with satellite observations, the vertical extent of the stratospheric aerosol layer in the tropics is modulated by the QBO by up to 6 km, or ~ 35% of its mean vertical extent between 100-7 hPa (about 16-33 km). Its largest vertical extent lags behind the occurrence of strongest QBO westerlies. The largest reduction lags behind maximum QBO easterlies. Strongest QBO signals in the aerosol surface area (30 %) and number densities (up to 100% e.g. in the Aitken mode) are found in regions where aerosol evaporates, that is above the 10 hPa pressure level (~ 31 km). Positive modulations are found in the QBO easterly shear, negative modulations in the westerly shear. Below 10 hPa, in regions where the aerosol mixing ratio is largest (50-20 hPa, or ~ 20-26 km), in most of the analysed parameters only moderate statistically significant QBO signatures (< 10%) have been found. QBO signatures in the model prognostic aerosol mixing ratio are significant at the 95% confidence level throughout the tropical stratosphere where modelled mixing ratios exceed 0.1 ppbm. In some regions of the tropical lower stratosphere the QBO signatures in other analysed parameters are partly not statistically significant. Peak-to-peak amplitudes of the QBO signature in the prognostic mixing ratios are up to twice as large as seasonal variations in the region where aerosols evaporate and between 70-30 hPa. Between the tropical tropopause and 70 hPa the QBO signature is relatively weak and seasonal variations dominate the variability of the simulated Junge layer. QBO effects on the upper lid of the tropical aerosol layer turn the quasi-static balance between processes maintaining the layer's vertical extent into a cyclic balance when considering this dominant mode

  18. Unambiguous discrimination of mixed states: A description based on system-ancilla coupling

    SciTech Connect

    Zhou, Xiang-Fa; Zhang, Yong-Sheng; Guo, Guang-Can

    2007-05-15

    We propose a general description for the unambiguous discrimination of mixed states according to the system-environment coupling, and present a procedure to reduce this to a standard semidefinite programming problem. In the two-state case, we introduce the canonical vectors and partly simplify the problem to the case of discrimination between pairs of canonical vectors. By considering the positivity of the 2x2 matrices, we obtain a series of new upper bounds for the total success probability, which depends on both the prior probabilities and specific state structures.

  19. Resonant purification of mixed states for closed and open quantum systems

    SciTech Connect

    Romano, Raffaele

    2007-02-15

    Pure states are fundamental for the implementation of quantum technologies, and several methods for the purification of the state of a quantum system S have been developed in the past years. In this work we describe a mechanism leading to purification of mixed states, based on the interaction of S with an auxiliary system P. Considering two-level systems and assuming a particular interaction between them, we study how the dynamical parameters of the system P affect the purification of S. By using analytical and numerical tools, we show that the purification process exhibits a resonant behavior in both the cases of system isolated from the external environment or not.

  20. Fast Airborne Size Distribution Measurements of an Aerosol Processes and Aging

    NASA Astrophysics Data System (ADS)

    Kapustin, V.; Clarke, A. D.; Zhou, J.; Brekhovskikh, V.; McNaughton, C. S.; Howell, S.

    2009-12-01

    During MILAGRO/INTEX experiment the Hawaii Group for Environmental Aerosol Research (HIGEAR) deployed a wide range of aerosol instrumentation aboard NSF C-130 and NASA DC-8. These were designed to provide rapid information on aerosol composition, state of mixing (internal or external), spectral optical properties (scattering and absorption), the humidity dependence of light scattering - f(RH), and the role of condensed species in changing the absorption properties of black carbon (BC) and inferred properties of organic carbon (OC). We also flew the Fast Mobility Particle Spectrometer (FMPS, TSI Inc.) to measure aerosol size distributions in a range 5.6 - 560 nm. For all our flights around Mexico City, an aerosol number concentration usually was well above the nominal FMPS sensitivity (from ~100 particles/cc @ Dp = 5.6 nm to 1 part/cc @ 560nm), providing us with reliable size distributions even at 1 sec resolution. FMPS measurements revealed small scale structure of an aerosol and allowed us to examine size distributions varying over space and time associated with mixing processes previously unresolved. These 1-Hz measurements during aircraft profiles captured variations in size distributions within shallow layers. Other dynamic processes observed included orography induced aerosol layers and evolution of the nanoparticles formed by nucleation. We put FMPS high resolution size distribution data in a context of aerosol evolution and aging, using a range of established (for MIRAGE/INTEX) chemical, aerosol and transport aging parameters.

  1. Calculation of mass of Y(4140) by introducing mixed molecule state in quark model

    NASA Astrophysics Data System (ADS)

    Chen, Xiaozhao; Lü, Xiaofu; Shi, Renbin; Guo, Xiurong

    2016-08-01

    Using the general form of the Bethe-Salpeter wave functions for the bound states consisting of two vector fields given in our previous work, we investigate the molecular state composed of Ds*+ Ds*-. However, for the SU(3) symmetry the component Ds*+ Ds*- is coupled with the other components D*0D bar * 0 and D*+D*-. Then we interpret the internal structure of the observed Y (4140) state as a mixed state of pure molecule states D*0D bar * 0, D*+D*- and Ds*+ Ds*-with quantum numbers JP =0+. In this paper, the operator product expansion is used to introduce the nonperturbative contribution from the vacuum condensates into the interaction between two heavy mesons. The calculated mass of Y (4140) is consistent with the experimental value, and we conclude that it is a more reasonable scenario to explain the structure of Y (4140) as a mixture of pure molecule states.

  2. Radiative Impacts of Elevated Aerosol Layers from Different Origins

    NASA Astrophysics Data System (ADS)

    Sauer, D. N.; Weinzierl, B.; Gasteiger, J.; Heimerl, K.

    2014-12-01

    Aerosol particles are omnipresent in the Earth's atmosphere and have important impacts on weather and climate by their effects on the atmospheric radiative balance. With the advent of more and more sophisticated representations of atmospheric processes in earth system models, the lack of reliable input data on aerosols leads to significant uncertainties in the prediction of future climate scenarios. In recent years large discrepancies in radiative forcing estimates from aerosol layers in modeling studies have been revealed emphasizing the need for detailed and systematic observations of aerosols. Airborne in-situ measurements represent an important pillar for validating both model results and retrievals of aerosol distributions and properties from remote sensing methods on global scales. However, detailed observations are challenging and therefore are subject to substantial uncertainties themselves. Here we use data from airborne in-situ measurements of elevated aerosol layers from various field experiments in different regions of the world. The data set includes Saharan mineral dust layers over Africa, the Atlantic Ocean and the Caribbean from the SALTRACE and the SAMUM campaigns as well as long-range transported biomass burning aerosol layers from wild fires in the Sahel region and North America measured over the tropical Atlantic Ocean, Europe and the Arctic detected during SAMUM2, CONCERT2011, DC3 and ACCESS 2012. We aim to characterize the effects of the measured aerosol layers, in particular with respect to ageing, mixing state and vertical structure, on the overall atmospheric radiation budget as well as local heating and cooling rates. We use radiative transfer simulations of short and long-wave radiation and aerosol optical properties derived in a consistent way from the in-situ observations of microphysical properties using T-matrix calculations. The results of this characterization will help to improve the parameterization of the effects of elevated

  3. Eliciting positive, negative and mixed emotional states: A film library for affective scientists.

    PubMed

    Samson, Andrea C; Kreibig, Sylvia D; Soderstrom, Blake; Wade, A Ayanna; Gross, James J

    2016-08-01

    We describe the creation of a film library designed for researchers interested in positive (amusing), negative (repulsive), mixed (amusing and repulsive) and neutral emotional states. Three hundred 20- to 33-second film clips videotaped by amateurs were selected from video-hosting websites and screened in laboratory studies by 75 female participants on self-reported amusement and repulsion (Experiments 1 and 2). On the basis of pre-defined cut-off values, 51 positive, 39 negative, 59 mixed and 50 neutral film clips were selected. These film clips were then presented to 411 male and female participants in a large online study to identify film clips that reliably induced the target emotions (Experiment 3). Depending on the goal of the study, researchers may choose positive, negative, mixed or neutral emotional film clips on the basis of Experiments 1 and 2 or Experiment 3 ratings.

  4. Unspeciated organic emissions from combustion sources and their influence on the secondary organic aerosol budget in the United States

    EPA Science Inventory

    Secondary organic aerosol (SOA) formed from the atmospheric oxidation of nonmethane organic gases (NMOG) is a major contributor to atmospheric aerosol mass. Emissions and smog chamber experiments were performed to investigate SOA formation from gasoline vehicles, diesel vehicles,...

  5. Parameterization of the cloud-mediated radiative forcing of climate due to aerosols in the two-way coupled WRF-CMAQ over the continental United States

    NASA Astrophysics Data System (ADS)

    Yu, S.; Mathur, R.; Pleim, J.; Wong, D.; Carlton, A. G.; Roselle, S. J.; Rao, S.

    2010-12-01

    Atmospheric emissions resulting from consumption of fossil fuels by human activities contribute to global warming and degrade air quality. The IPCC (2007) concludes that the total direct aerosol radiative forcing is estimated to be -0.5 [±0.4] W m-2, with a medium-low level of scientific understanding, while the radiative forcing due to the cloud albedo effect (also referred to as first indirect), is estimated to be -0.7 [-1.1, +0.4] W m-2, with a low level of scientific understanding. For a given cloud liquid water content, an increase in the cloud droplet number concentration implies a decrease in the effective radius, thus increasing the cloud reflectivity; this is know as the first indirect aerosol effect. The second indirect aerosol effect is based on the idea that decreasing the mean droplet size in the presence of enhanced aerosols decreases the cloud precipitation efficiency, producing clouds with a larger liquid water content and longer lifetime. In this study, the indirect aerosol effect is estimated with the newly developed two-way coupled WRF-CMAQ over the continental United States. The cloud droplet number concentrations are diagnosed from the activation of CMAQ-predicted aerosol. The resulting cloud droplet number is used to calculate variations in droplet effective radius, which in turn allows us to estimate aerosol effects on cloud optical depth and microphysical processes using a two-moment treatment of cloud water (cloud water mass and cloud droplet number) to model effects on precipitation. With the satellite observation data such as CERES, MODIS and CALIPSO, we will evaluate the cloud properties such as cloud optical depth, cloud droplet effective radius, and liquid water content and indirect aerosol forcing in the newly-developed coupled WRF-CMAQ.

  6. Fine Aerosol Bulk Composition Measured on WP-3D Research Aircraft in Vicinity of the Northeastern United States - Results from NEAQS

    NASA Technical Reports Server (NTRS)

    Peltier, R. E.; Sullivan, A. P.; Weber, R. J.; Brock, C. A.; Wollny, A. G.; Holloway, J. S.; deGouw, J. A.; Warneke, C.

    2007-01-01

    During the New England Air Quality Study (NEAQS) in the summer of 2004, airborne measurements were made of the major inorganic ions and the water-soluble organic carbon (WSOC) of the submicron (PM(sub 1.0)) aerosol. These and ancillary data are used to describe the overall aerosol chemical characteristics encountered during the study. Fine particle mass was estimated from particle volume and a calculated density based on measured particle composition. Fine particle organic matter (OM) was estimated from WSOC and a mass balance analysis. The aerosol over the northeastern United States (U.S.) and Canada was predominantly sulfate and associated ammonium, and organic components, although in unique plumes additional ionic components were also periodically above detection limits. In power generation regions, and especially in the Ohio River Valley region, the aerosol tended to be predominantly sulfate (approximately 60% micro gram /micro gram) and apparently acidic, based on an excess of measured anions compared to cations. In all other regions where sulfate concentrations were lower and a smaller fraction of overall mass, the cations and anions were balanced suggesting a more neutral aerosol. In contrast, the WSOC and estimated OM were more spatially uniform and the fraction of OM relative to PM mass was largely influenced by sources of sulfate. The study median OM mass fraction was 40%. Throughout the study region, sulfate and organic aerosol mass were highest near the surface and decreased rapidly with increasing altitude. The relative fraction of organic mass to sulfate was similar throughout all altitudes within the boundary layer (altitude less than 2.5 km), but was significantly higher at altitude layers in the free troposphere (above 2.5 km). A number of distinct biomass burning plumes from fires in Alaska and the Yukon were periodically intercepted, mostly at altitudes between 3 and 4 km. These plumes were associated with highest aerosol concentrations of the

  7. Influence of Serum and Glucose Additives on Survival of Actinobacillus pleuropneumoniae Aerosolized from the Freeze-Dried State.

    PubMed

    Hensel, A

    1994-06-01

    Serum and/or glucose added to Actinobacillus pleuropneumoniae suspensions before freeze-drying significantly increased survival rates of bacteria in aerosols. Aerosols with predictable numbers of viable bacteria can be made as required in an aerosol infection model. Sucrose supplementation of impinger fluids increased recovery of viable A. pleuropneumoniae.

  8. Stratus: An interactive steady state mixed layer model for personal computers

    NASA Technical Reports Server (NTRS)

    Guinn, Thomas A.; Schubert, Wayne H.

    1990-01-01

    A steady-state, horizontally homogeneous, cloud-topped marine boundary layer model based primarily on the work of Lilly (1968) and Schubert et al., (1979) is presented. The conservative thermodynamic variables are equivalent potential temperature, theta(sub e), and total water mixing ratio, q + l. Some of the differences between this and Lilly's (1968) model are: radiation is allowed to penetrate into the boundary layer; cloud top values of longwave radiation, equivalent potential temperature, and water vapor mixing ratio are linear functions of height derived from climatological data at California coastal stations; and the closure assumption assumes a weighted average of Lilly's (1968) maximum and minimum entrainment theories. This model was programmed in FORTRAN and will run interactively on an IBM-compatible personal computer. The program allows the user to specify the geographical location, the wind speed, the sea-surface temperature, the large scale horizontal divergence, and the initial guess for cloud top height. Output includes the steady state values of cloud top and cloud base height, mixed layer equivalent potential temperature and total water mixing ratio, and the associated convective and radiative fluxes.

  9. Monodisperse aerosol generator

    DOEpatents

    Ortiz, Lawrence W.; Soderholm, Sidney C.

    1990-01-01

    An aerosol generator is described which is capable of producing a monodisperse aerosol within narrow limits utilizing an aqueous solution capable of providing a high population of seed nuclei and an organic solution having a low vapor pressure. The two solutions are cold nebulized, mixed, vaporized, and cooled. During cooling, particles of the organic vapor condense onto the excess seed nuclei, and grow to a uniform particle size.

  10. Aerosol processing in stratiform clouds in ECHAM6-HAM

    NASA Astrophysics Data System (ADS)

    Neubauer, David; Lohmann, Ulrike; Hoose, Corinna

    2013-04-01

    Aerosol processing in stratiform clouds by uptake into cloud particles, collision-coalescence, chemical processing inside the cloud particles and release back into the atmosphere has important effects on aerosol concentration, size distribution, chemical composition and mixing state. Aerosol particles can act as cloud condensation nuclei. Cloud droplets can take up further aerosol particles by collisions. Atmospheric gases may also be transferred into the cloud droplets and undergo chemical reactions, e.g. the production of atmospheric sulphate. Aerosol particles are also processed in ice crystals. They may be taken up by homogeneous freezing of cloud droplets below -38° C or by heterogeneous freezing above -38° C. This includes immersion freezing of already immersed aerosol particles in the droplets and contact freezing of particles colliding with a droplet. Many clouds do not form precipitation and also much of the precipitation evaporates before it reaches the ground. The water soluble part of the aerosol particles concentrates in the hydrometeors and together with the insoluble part forms a single, mixed, larger particle, which is released. We have implemented aerosol processing into the current version of the general circulation model ECHAM6 (Stevens et al., 2013) coupled to the aerosol module HAM (Stier et al., 2005). ECHAM6-HAM solves prognostic equations for the cloud droplet number and ice crystal number concentrations. In the standard version of HAM, seven modes are used to describe the total aerosol. The modes are divided into soluble/mixed and insoluble modes and the number concentrations and masses of different chemical components (sulphate, black carbon, organic carbon, sea salt and mineral dust) are prognostic variables. We extended this by an explicit representation of aerosol particles in cloud droplets and ice crystals in stratiform clouds similar to Hoose et al. (2008a,b). Aerosol particles in cloud droplets are represented by 5 tracers for the

  11. Evolution of Soot Particle Morphology and Mixing State in the Atmosphere

    NASA Astrophysics Data System (ADS)

    Mazzoleni, C.; China, S.; Sharma, N.; Gorkowski, K.; Dubey, M.; Aiken, A. C.; Zaveri, R. A.; Salvadori, N.; Chakrabarty, R. K.; Moosmuller, H.; Onasch, T. B.; Herndon, S.; Williams, L. R.; Liu, S.; Dzepina, K.; Helmig, D.; Hueber, J.; Fialho, P. J.; Mazzoleni, L. R.; kumar, S.; Dziobak, M.; Wright, K.

    2013-12-01

    Soot particles (aka black carbon) impact the environment and climate by affecting Earth's radiation balance, cloud microphysics, and atmospheric chemistry. The complex morphology and mixing state of soot particles influence their optical properties and therefore their radiative forcing, the particles' transport, lifecycle, and heterogeneous chemistry. How soot morphology and mixing state alter during transport from the source to remote areas is still not well understood. While aging, soot particles can change shape, oxidize and mix, and become coated by organic and inorganic materials. In this study, we investigate the morphological and mixing state evolution of single soot particles in different stages of their 'life' in the atmosphere. This analysis will include an overview of several samples collected in various locations and atmospheric conditions: 1) particles freshly emitted near freeway on-ramps in Southern Michigan (USA); 2) particles emitted in two biomass burning events in New Mexico (USA), one close to the sampling location and another hundreds of miles away; 3) particles in the urban atmosphere of Mexico City and in the uplifted boundary layer captured on the top of the Pico de Tres Padres Mountain (on the north edge of Mexico City); 4) particles collected in the Sacramento urban area and the Sierra Nevada foothills (CA, USA); 5) particles collected in Detling (UK), and mostly transported from London, and 6) long-range transported particles in the free troposphere and collected at the Pico Mountain Observatory, located near the top of the Pico Volcano in the Azores (Portugal). We analyzed a large number of individual particles using electron microscopy and X-ray spectroscopy followed by image analysis. The projected structural properties of soot particles were characterized using size (maximum length, maximum width, and area equivalent diameter) and shape descriptors (e.g., aspect ratio, roundness, and convexity). The particle mass-fractal dimensions

  12. Re-creation of aerosol charge state found near HV power lines using a high voltage corona charger

    NASA Astrophysics Data System (ADS)

    Matthews, J. C.; Wright, M. D.; Biddiscombe, M. F.; Underwood, R.; Usmani, O. S.; Shallcross, D. E.; Henshaw, D. L.

    2015-10-01

    Corona ionisation from AC HV power lines (HVPL) can release ions into the environment, which have the potential to electrically charge pollutant aerosol in the atmosphere. It has been hypothesised that these charged particles have an enhanced probability of being deposited in human airways upon inhalation due to electrostatic attraction by image charge within the lung, with implications for human health. Carbonaceous aerosol particles from a Technegas generator were artificially charge-enhanced using a corona charger. Once generated, particles were passed through the charger, which was either on or off, and stored in a 15 litre conducting bag for ∼20 minutes to observe size and charge distribution changes over time. Charge states were estimated using two Sequential Mobility Particle Sizers measuring the size and mobility distributions. Charge-neutral particles were measured 7 times and positive particles 9 times, the average charge-neutral value of x was 1.00 (sd = 0.06) while the average positive value was 4.60 (0.72). The system will be used to generate positive or charge neutral particles for delivery to human volunteers in an inhalation study to assess the impact of charge on ultrafine (size < 100 nm) particle deposition.

  13. Unspeciated organic emissions from combustion sources and their influence on the secondary organic aerosol budget in the United States.

    PubMed

    Jathar, Shantanu H; Gordon, Timothy D; Hennigan, Christopher J; Pye, Havala O T; Pouliot, George; Adams, Peter J; Donahue, Neil M; Robinson, Allen L

    2014-07-22

    Secondary organic aerosol (SOA) formed from the atmospheric oxidation of nonmethane organic gases (NMOG) is a major contributor to atmospheric aerosol mass. Emissions and smog chamber experiments were performed to investigate SOA formation from gasoline vehicles, diesel vehicles, and biomass burning. About 10-20% of NMOG emissions from these major combustion sources are not routinely speciated and therefore are currently misclassified in emission inventories and chemical transport models. The smog chamber data demonstrate that this misclassification biases model predictions of SOA production low because the unspeciated NMOG produce more SOA per unit mass than the speciated NMOG. We present new source-specific SOA yield parameterizations for these unspeciated emissions. These parameterizations and associated source profiles are designed for implementation in chemical transport models. Box model calculations using these new parameterizations predict that NMOG emissions from the top six combustion sources form 0.7 Tg y(-1) of first-generation SOA in the United States, almost 90% of which is from biomass burning and gasoline vehicles. About 85% of this SOA comes from unspeciated NMOG, demonstrating that chemical transport models need improved treatment of combustion emissions to accurately predict ambient SOA concentrations.

  14. Impact of the Manaus urban plume on trace gas mixing ratios near the surface in the Amazon Basin: Implications for the NO-NO2-O3 photostationary state and peroxy radical levels

    NASA Astrophysics Data System (ADS)

    Trebs, Ivonne; Mayol-Bracero, Olga L.; Pauliquevis, Theotonio; Kuhn, Uwe; Sander, Rolf; Ganzeveld, Laurens; Meixner, Franz X.; Kesselmeier, Jürgen; Artaxo, Paulo; Andreae, Meinrat O.

    2012-03-01

    We measured the mixing ratios of NO, NO2, O3, and volatile organic carbon as well as the aerosol light-scattering coefficient on a boat platform cruising on rivers downwind of the city of Manaus (Amazonas State, Brazil) in July 2001 (Large-Scale Biosphere-Atmosphere Experiment in Amazonia-Cooperative LBA Airborne Regional Experiment-2001). The dispersion and impact of the Manaus plume was investigated by a combined analysis of ground-based (boat platform) and airborne trace gas and aerosol measurements as well as by meteorological measurements complemented by dispersion calculations (Hybrid Single-Particle Lagrangian Integrated Trajectory model). For the cases with the least anthropogenic influence (including a location in a so far unexplored region ˜150 km west of Manaus on the Rio Manacapuru), the aerosol scattering coefficient, σs, was below 11 Mm-1, NOx mixing ratios remained below 0.6 ppb, daytime O3 mixing ratios were mostly below 20 ppb and maximal isoprene mixing ratios were about 3 ppb in the afternoon. The photostationary state (PSS) was not established for these cases, as indicated by values of the Leighton ratio, Φ, well above unity. Due to the influence of river breeze systems and other thermally driven mesoscale circulations, a change of the synoptic wind direction from east-northeast to south-southeast in the afternoon often caused a substantial increase of σs and trace gas mixing ratios (about threefold for σs, fivefold for NOx, and twofold for O3), which was associated with the arrival of the Manaus pollution plume at the boat location. The ratio Φ reached unity within its uncertainty range at NOx mixing ratios of about 3 ppb, indicating "steady-state" conditions in cases when radiation variations, dry deposition, emissions, and reactions mostly involving peroxy radicals (XO2) played a minor role. The median midday/afternoon XO2 mixing ratios estimated using the PSS method range from 90 to 120 parts per trillion (ppt) for the remote cases (

  15. Spectroscopic studies of the size and composition of single aerosol droplets

    NASA Astrophysics Data System (ADS)

    Reid, Jonathan P.; Meresman, Helena; Mitchem, Laura; Symes, Rachel

    The characterization of aerosol properties and processes, non-intrusively and directly, poses a severe analytical challenge. In order to understand the role of aerosols in often complex environments, it is necessary to probe the particles in situ and without perturbation. Sampling followed by end-of-line analysis can lead to perturbations in particle composition, morphology and size, particularly when analysing liquid aerosol droplets containing volatile components. Optical spectroscopy can provide a strategy for the direct assessment of particle size, composition and phase. We review here the application of linear and non-linear Raman spectroscopies in the characterization of liquid aerosol droplets. Spontaneous Raman scattering can allow the unambiguous identification of chemical components and the determination of droplet composition. Stimulated Raman spectroscopy can allow the determination of droplet size with nanometre accuracy and can allow the characterization of near-surface composition. When combined, the mixing state and homogeneity in droplet composition can be investigated. We highlight some applications of these spectroscopic techniques in studies of the kinetics of particle transformation, the equilibrium composition of aqueous aerosol droplets, and the coagulation and mixing state of organic and aqueous aerosol components. Specifically, we examine the heat and mass transfer accompanying the evaporation of volatile components from liquid droplets, the equilibrium size of aqueous/sodium chloride droplets with varying relative humidity, and the mixing of the immiscible decane and water components during droplet coagulation. We conclude by considering the potential of these techniques for improving our understanding of aerosol properties and processes.

  16. Optical, size and mass properties of mixed type aerosols in Greece and Romania as observed by synergy of lidar and sunphotometers in combination with model simulations: a case study.

    PubMed

    Papayannis, A; Nicolae, D; Kokkalis, P; Binietoglou, I; Talianu, C; Belegante, L; Tsaknakis, G; Cazacu, M M; Vetres, I; Ilic, L

    2014-12-01

    A coordinated experimental campaign aiming to study the aerosol optical, size and mass properties was organized in September 2012, in selected sites in Greece and Romania. It was based on the synergy of lidar and sunphotometers. In this paper we focus on a specific campaign period (23-24 September), where mixed type aerosols (Saharan dust, biomass burning and continental) were confined from the Planetary Boundary Layer (PBL) up to 4-4.5 km height. Hourly mean linear depolarization and lidar ratio values were measured inside the dust layers, ranging from 13 to 29 and from 44 to 65sr, respectively, depending on their mixing status and the corresponding air mass pathways over Greece and Romania. During this event the columnar Aerosol Optical Depth (AOD) values ranged from 0.13 to 0.26 at 532 nm. The Lidar/Radiometer Inversion Code (LIRIC) and the Polarization Lidar Photometer Networking (POLIPHON) codes were used and inter-compared with regards to the retrieved aerosol (fine and coarse spherical/spheroid) mass concentrations, showing that LIRIC generally overestimates the aerosol mass concentrations, in the case of spherical particles. For non-spherical particles the difference in the retrieved mass concentration profiles from these two codes remained smaller than ±20%. POLIPHON retrievals showed that the non-spherical particles reached concentrations of the order of 100-140 μg/m(3) over Romania compared to 50-75 μg/m(3) over Greece. Finally, the Dust Regional Atmospheric Model (DREAM) model was used to simulate the dust concentrations over the South-Eastern Europe.

  17. Application of muon spin relaxation experiment to the mixed state superconductors

    SciTech Connect

    Inui, M. ); Harshman, D.R. )

    1991-05-09

    We discuss the use of muon spin relaxation ({mu}{sup +}SR) technique to study the mixed state of superconductors. Besides the application for static vortex configurations, we argue that large vortex motion can manifest itself as a narrowed time-averaged field distribution, which in turn results in a smaller relaxation rate. A static but disordered vortex configuration can also reduce the relaxation. We summarize these arguments. 7 refs.

  18. Modeling aerosols and their interactions with shallow cumuli during the 2007 CHAPS field study

    SciTech Connect

    Shrivastava, ManishKumar B.; Berg, Larry K.; Fast, Jerome D.; Easter, Richard C.; Laskin, Alexander; Chapman, Elaine G.; Gustafson, William I.; Liu, Ying; Berkowitz, Carl M.

    2013-02-07

    The Weather Research and Forecasting model coupled with chemistry (WRF-Chem) is used to simulate relationships between aerosols and clouds in the vicinity of Oklahoma City during the June 2007 Cumulus Humilis Aerosol Processing Study (CHAPS). The regional scale simulation completed using 2 km horizontal grid spacing evaluates four important relationships between aerosols and shallow cumulus clouds observed during CHAPS. First, the model reproduces the trends of higher nitrate volume fractions in cloud droplet residuals compared to interstitial non-activated aerosols, as measured using the Aerosol Mass Spectrometer. Comparing simulations with cloud chemistry turned on and off, we show that nitric acid vapor uptake by cloud droplets explains the higher nitrate content of cloud droplet residuals. Second, as documented using an offline code, both aerosol water and other inorganics (OIN), which are related to dust and crustal emissions, significantly affect predicted aerosol optical properties. Reducing the OIN content of wet aerosols by 50% significantly improves agreement of model predictions with measurements of aerosol optical properties. Third, the simulated hygroscopicity of aerosols is too high as compared to their hygroscopicity derived from cloud condensation nuclei and particle size distribution measurements, indicating uncertainties associated with simulating size-dependent chemical composition and treatment of aerosol mixing state within the model. Fourth, the model reasonably represents the observations of the first aerosol indirect effect where pollutants in the vicinity of Oklahoma City increase cloud droplet number concentrations and decrease the droplet effective radius. While previous studies have often focused on cloud-aerosol interactions in stratiform and deep convective clouds, this study highlights the ability of regional-scale models to represent some of the important aspects of cloud-aerosol interactions associated with fields of short

  19. Chemical, physical, and optical evolution of biomass burning aerosols: a case study

    NASA Astrophysics Data System (ADS)

    Adler, G.; Flores, J. M.; Abo Riziq, A.; Borrmann, S.; Rudich, Y.

    2011-02-01

    In-situ chemical composition measurements of ambient aerosols have been used for characterizing the evolution of submicron aerosols from a large anthropogenic biomass burning (BB) event in Israel. A high resolution Time of Flight Aerosol Mass Spectromete