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Sample records for aerosol mixing state

  1. 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.

  2. [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

  3. 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.

  4. Mixing states of aerosols over four environmentally distinct atmospheric regimes in Asia: coastal, urban, and industrial locations influenced by dust.

    PubMed

    Ramachandran, S; Srivastava, Rohit

    2016-06-01

    Mixing can influence the optical, physical, and chemical characteristics of aerosols, which in turn can modify their life cycle and radiative effects. Assumptions on the mixing state can lead to uncertain estimates of aerosol radiative effects. To examine the effect of mixing on the aerosol characteristics, and their influence on radiative effects, aerosol mixing states are determined over four environmentally distinct locations (Karachi, Gwangju, Osaka, and Singapore) in Asia, an aerosol hot spot region, using measured spectral aerosol optical properties and optical properties model. Aerosol optical depth (AOD), single scattering albedo (SSA), and asymmetry parameter (g) exhibit spectral, spatial, and temporal variations. Aerosol mixing states exhibit large spatial and temporal variations consistent with aerosol characteristics and aerosol type over each location. External mixing of aerosol species is unable to reproduce measured SSA over Asia, thus providing a strong evidence that aerosols exist in mixed state. Mineral dust (MD) (core)-Black carbon (BC) (shell) is one of the most preferred aerosol mixing states. Over locations influenced by biomass burning aerosols, BC (core)-water soluble (WS, shell) is a preferred mixing state, while dust gets coated by anthropogenic aerosols (BC, WS) over urban regions influenced by dust. MD (core)-sea salt (shell) mixing is found over Gwangju corroborating the observations. Aerosol radiative forcing exhibits large seasonal and spatial variations consistent with features seen in aerosol optical properties and mixing states. TOA forcing is less negative/positive for external mixing scenario because of lower SSA. Aerosol radiative forcing in Karachi is a factor of 2 higher when compared to Gwangju, Osaka, and Singapore. The influence of g on aerosol radiative forcing is insignificant. Results emphasize that rather than prescribing one single aerosol mixing state in global climate models regionally and temporally varying aerosol

  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. Impact of Mixing State on Anthropogenic Aerosol Radiative Forcing and Associated Climate Response

    NASA Astrophysics Data System (ADS)

    Avramov, A.; Shin, H. J.; Wang, C.

    2014-12-01

    Atmospheric aerosols affect Earth's radiation balance directly by scattering and absorbing solar radiation and, indirectly, by changing the microphysical structure, lifetime and spatial extent of clouds. The aerosol mixing state to a large extent determines not only their optical properties (direct effect) but also their ability to serve as cloud condensation nuclei or ice nuclei (indirect effect). Results from previous research have highlighted the importance of the aerosol mixing assumptions in radiative forcing estimates in model simulations. Here we take a step further to analyze the differences in associated climate responses, using a multimodal, size- and mixing-dependent aerosol model (MARC) incorporated within the Community Earth System Model (CESM). The new model allows for a detailed representation of aerosol-radiation and aerosol-cloud interactions by including an improved treatment of aerosol mixing state and composition. First, we estimate and compare the magnitudes of direct and indirect forcing of anthropogenic aerosols under different mixing assumptions. We then carry out several century-long fully-coupled climate simulations designed to isolate the climate responses to direct and indirect forcings under the same aerosol mixing assumptions. In our analysis, we specifically focus on the following three climate response components: 1) cloud distribution and coverage; 2) precipitation amount and distribution; and 3) changes in circulation patterns.

  7. Strong radiative heating due to the mixing state of black carbon in atmospheric aerosols

    NASA Astrophysics Data System (ADS)

    Jacobson, Mark Z.

    2001-02-01

    Aerosols affect the Earth's temperature and climate by altering the radiative properties of the atmosphere. A large positive component of this radiative forcing from aerosols is due to black carbon-soot-that is released from the burning of fossil fuel and biomass, and, to a lesser extent, natural fires, but the exact forcing is affected by how black carbon is mixed with other aerosol constituents. From studies of aerosol radiative forcing, it is known that black carbon can exist in one of several possible mixing states; distinct from other aerosol particles (externally mixed) or incorporated within them (internally mixed), or a black-carbon core could be surrounded by a well mixed shell. But so far it has been assumed that aerosols exist predominantly as an external mixture. Here I simulate the evolution of the chemical composition of aerosols, finding that the mixing state and direct forcing of the black-carbon component approach those of an internal mixture, largely due to coagulation and growth of aerosol particles. This finding implies a higher positive forcing from black carbon than previously thought, suggesting that the warming effect from black carbon may nearly balance the net cooling effect of other anthropogenic aerosol constituents. The magnitude of the direct radiative forcing from black carbon itself exceeds that due to CH4, suggesting that black carbon may be the second most important component of global warming after CO2 in terms of direct forcing.

  8. Sensitivity of Aerosol Radiative Forcing to Mixing State and Non-Sphericity

    NASA Astrophysics Data System (ADS)

    Srivastava, P.; Dey, S.; Srivastava, A.; Singh, S.; Agarwal, P.

    2014-12-01

    Mixing state and particle non-sphericity of aerosols are two major sources of uncertainties in estimation of aerosol direct radiative forcing (DRF). To examine the sensitivity of optical properties to the mixing state, aerosols were collected on filter papers and analyzed for detailed chemical composition in Delhi national capital region (NCR) during 2007-2008. Black carbon, BC was measured directly by Aethalometer. They are grouped into four major aerosol species - dust, water soluble (WS), water insoluble (WINS) and BC. Eight different mixing cases - external mixing, internal mixing, and six combinations of core-shell type which includes two modes of dust (accumulation and coarse) have been considered for the present study. Core-shell mixing cases are BC over dust, WS over dust, BC over WS and, WS over BC. These core shell mixed components are then externally mixed with rest of the aerosol species. The aerosol optical properties for each of the mixing state cases are utilized to estimate the radiative forcing using a radiative transfer model. The surface-reaching fluxes for each of the cases are compared with measured clear-sky surface radiation. MISR aerosol product were analyzed to understand the seasonal variations of the bulk aerosol properties that may help in interpreting the sensitivity results. We observed that for the winter season (DJF), core-shell mixed case; BC over dust (accumulation) (207.7±4.28 Wm-2) and BC over WS (207.25±8.4 Wm-2) are almost comparable with measured surface flux (206.46±70.06 Wm-2), while for the monsoon season (JAS) external mixing is closest to observations. None of the mixing cases show compatible comparison, for the pre-monsoon (MAMJ) and post-monsoon season (ON). The remaining discrepancy may be attributed to the assumption of uniform vertical distribution (calculated from CALIPSO data) for each individual aerosol species, whereas ideally different vertical profile should be considered. Secondly, dust is assumed to be

  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. PMID:27162963

  10. 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

  11. Aerosol Direct Radiative Forcing over Delhi NCR, India: Sensitivity to Mixing State and Particle Shape

    NASA Astrophysics Data System (ADS)

    Srivastava, Parul; Dey, Sagnik; Srivastava, Atul; Singh, Sachchidanand; Agarwal, Poornima

    2015-04-01

    Aerosol properties changes with the change in mixing state of aerosols and thus aerosol direct radiative forcing (DRF). The problem is important in the Indo-Gangetic Basin, Northern India, where various aerosol types mix and show strong seasonal variations. A detailed chemical composition analysis of aerosols for Delhi National capital region (NCR) is carried out during 2007-2008. These results were used to examine the sensitivity of optical properties to the aerosol mixing state. Black carbon, BC was measured directly by Aethalometer. The species are grouped into four major components; dust, water soluble (WS), water insoluble (WINS) and BC. To infer the probable mixing state of aerosols in the Delhi NCR, eight different mixing cases, external mixing, internal mixing, and six combinations of core- shell type mixing which includes two modes of dust (accumulation and coarse) have been considered. Core-shell mixing cases are considered to be as follows - BC over dust, WS over dust, BC over WS and, WS over BC. These core shell mixed components are then externally mixed with rest of the aerosol species. The spectral aerosol optical properties - extinction coefficient, single scattering albedo (SSA) and asymmetry parameter (g) for each of the mixing state cases are calculated. These optical properties are utilized to estimate the radiative forcing using a radiative transfer model. The surface-reaching fluxes for each of the cases are compared with MERRA downward shortwave surface flux. MISR aerosol products were also analyzed to understand the seasonal variations of the bulk aerosol properties that may help in interpreting the sensitivity results. We observed that for the pre-monsoon season (MAMJ), core shell mixed case; BC coated over WS (surface DRF is -10.52 Wm-2) and BC over coarse dust (surface DRF is -2.81 Wm-2) are the most probable mixing states. For monsoon season (JAS,) BC coated over coarse dust (often referred to as polluted dust) (surface DRF is -0.60 Wm-2

  12. 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.

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

    DOE PAGESBeta

    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

  14. 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.

  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. Studies of the chemical mixing state of sea spray aerosol and associated climate relevant properties (Invited)

    NASA Astrophysics Data System (ADS)

    Prather, K. A.; Bertram, T. H.; Grassian, V. H.; Collins, D. B.; Ault, A. P.; Ruppel, M. J.; Axson, J. L.; Ryder, O. S.; Schill, S.

    2013-12-01

    The ocean plays a large but highly uncertain role in affecting clouds and climate, generating sea spray aerosols that can directly impact climate by scattering solar radiation and indirectly through nucleating clouds. A tremendous amount has been learned about these interactions over decades of marine studies, however the goal of establishing robust relationships between seawater composition and sea spray climate properties has remained elusive. Much of the impediment stems from difficulties associated with unraveling the impacts of nascent sea spray and background marine aerosols which have been shown to dominate field measurements. In an effort to advance our understanding of nascent sea spray properties, we have developed a new approach for studying this issue in a newly developed ocean-atmosphere facility equipped with breaking waves. After establishing extremely low background aerosol concentrations (< 1 per cc), studies have probed the size distribution and chemical mixing state of sea spray aerosols produced by breaking waves in natural seawater. The critical importance of using bubble size distributions representative of real breaking waves to generate sea spray aerosol (SSA) is discussed. Using a combination of techniques probing individual particle composition and morphology including aerosol time-of-flight mass spectrometry (ATOFMS), scanning tunnel x-ray microscopy (STXM), and electron microscopy, four major sea spray particle types are prevalent in all studies, consisting of sea salt, mixed sea salt and biogenic organic species, biogenic organic species, and primary biological aerosol particles (PBAP). Results from studies aimed at probing how changes in seawater composition due to biological activity impact sea spray aerosol composition and climate properties will be discussed.

  2. 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

  3. The importance of aerosol composition and mixing state on predicted CCN concentration and the variation of the importance with atmospheric processing of aerosol

    SciTech Connect

    Wang, J.; Cubison, M.; Aiken, A.; Jimenez, J.; Collins, D.; Gaffney, J.; Marley, N.

    2010-03-15

    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 are complex and heterogeneous mixtures 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 and mixing state are necessary for large-scale models. In this study, aerosol microphysics, CCN concentrations, and chemical composition measured at the T0 urban super-site in Mexico City during MILAGRO are analyzed. 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 biases associated with these simplifications are compared for different supersaturations, and the variation of the biases is examined as a function of aerosol age. The results show that the simplification of internally mixed, size

  4. 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

  5. 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

  6. 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

  7. 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

  8. 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.

  9. 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.

  10. 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

  11. 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

  12. 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

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

    NASA Astrophysics Data System (ADS)

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

    2013-04-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2013-09-01

    Single-particle mixing state information can be a powerful tool for assessing the relative impact of local and regional sources of ambient particulate matter in urban environments. However, quantitative mixing state data are challenging to obtain using single-particle mass spectrometers. In this study, the quantitative chemical composition of carbonaceous single particles has been determined using an aerosol time-of-flight mass spectrometer (ATOFMS) as part of the MEGAPOLI 2010 winter campaign in Paris, France. Relative peak areas of marker ions for elemental carbon (EC), organic aerosol (OA), ammonium, nitrate, sulfate and potassium were compared with concurrent measurements from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a thermal-optical OCEC analyser and a particle into liquid sampler coupled with ion chromatography (PILS-IC). ATOFMS-derived estimated mass concentrations reproduced the variability of these species well (R2 = 0.67-0.78), and 10 discrete mixing states for carbonaceous particles were identified and quantified. The chemical mixing state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix factorisation, was also investigated through comparison with the ATOFMS dataset. The results indicate that hydrocarbon-like OA (HOA) detected in Paris is associated with two EC-rich mixing states which differ in their relative sulfate content, while fresh biomass burning OA (BBOA) is associated with two mixing states which differ significantly in their OA / EC ratios. Aged biomass burning OA (OOA2-BBOA) was found to be significantly internally mixed with nitrate, while secondary, oxidised OA (OOA) was associated with five particle mixing states, each exhibiting different relative secondary inorganic ion content. Externally mixed secondary organic aerosol was not observed. These findings demonstrate the range of primary and secondary organic aerosol mixing states in Paris. Examination of the temporal

  15. 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.

  16. 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.

  17. 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.

  18. 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

  19. 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

  20. 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

  1. 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

  2. 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.

  3. 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.

  4. 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.

  5. 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.

  6. 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

  7. 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.

  8. 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

  9. 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.

  10. 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

  11. 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

  12. 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

  13. 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.

  14. Light absorption of black carbon aerosol and its enhancement by mixing state in an urban atmosphere in South China

    NASA Astrophysics Data System (ADS)

    Lan, Zi-Juan; Huang, Xiao-Feng; Yu, Kuang-You; Sun, Tian-Le; Zeng, Li-Wu; Hu, Min

    2013-04-01

    The effects of black carbon (BC) aerosol on climate warming have been the study focus in the recent decade, and the reduction of BC is now expected to have significant near-term climate change mitigation. Large uncertainties of BC optical properties, however, still exist and seriously restrict the ability to quantify BC's climate effects. In this study, advanced instrumentation (a three-wavelength photoacoustic soot spectrometer (PASS-3) and a single particle soot photometer (SP2)) were used to measure black carbon aerosol and analyze its optical properties in a mega-city in South China, Shenzhen, during the summer of 2011. The results indicated that the average BC mass concentration was 4.0 ± 3.1 μg m-3 during the campaign, accounting for ˜11% of the total PM2.5 mass concentration. The PM2.5 light absorption at 405, 532 and 781 nm was 37.1 ± 28.1, 25.4 ± 19.0 and 17.6 ± 12.9 Mm-1, respectively. The average absorption Angstrom exponent of PM2.5 in visual spectrum (AAE405-781 nm) was 1.1 ± 0.1 during the campaign, indicating that the light absorbing carbon mainly came from vehicular emissions, with little contributions from biomass burning emissions. The mass absorption efficiency (MAE) of BC at 532 nm ranged from 5.0 to 8.5 m2 g-1 during the campaign, with an average of 6.5 ± 0.5 m2 g-1, and showed an obvious diurnal pattern with high values in the daytime. The average percentage of internally mixed BC was 24.3 ± 7.9% during the campaign, showing significant positive correlation relationship with the MAE of BC. More quantitative data analysis indicated that the internally mixed BC would amplify MAE by about 7% during the campaign, which stands in accordance with the new finding of a very recent Science magazine paper (Cappa et al., 2012) that the BC absorption enhancement due to internal mixing in the real atmosphere is relatively low, in apparent contrast to theoretical model predictions.

  15. Hygroscopic mixing state of urban aerosol derived from size-resolved cloud condensation nuclei measurements during the MEGAPOLI campaign in Paris

    NASA Astrophysics Data System (ADS)

    Jurányi, Z.; Tritscher, T.; Gysel, M.; Laborde, M.; Gomes, L.; Roberts, G.; Baltensperger, U.; Weingartner, E.

    2013-07-01

    Ambient aerosols are a complex mixture of particles with different physical and chemical properties and consequently distinct hygroscopic behaviour. The hygroscopicity of a particle determines its water uptake at subsaturated relative humidity (RH) and its ability to form a cloud droplet at supersaturated RH. These processes influence Earth's climate and the atmospheric lifetime of the particles. Cloud condensation nuclei (CCN) number size distributions (i.e. CCN number concentrations as a function of dry particle diameter) were measured close to Paris during the MEGAPOLI campaign in January-February 2010, covering 10 different supersaturations (SS = 0.1-1.0%). The time-resolved hygroscopic mixing state with respect to CCN activation was also derived from these measurements. Simultaneously, a hygroscopicity tandem differential mobility analyser (HTDMA) was used to measure the hygroscopic growth factor (ratio of wet to dry mobility diameter) distributions at RH = 90%. The aerosol was highly externally mixed and its mixing state showed significant temporal variability. The average particle hygroscopicity was relatively low at subsaturation (RH = 90%; mean hygroscopicity parameter κ = 0.12-0.27) and increased with increasing dry diameter in the range 35-265 nm. The mean κ value, derived from the CCN measurements at supersaturation, ranged from 0.08 to 0.24 at SS = 1.0-0.1%. Two types of mixing-state resolved hygroscopicity closure studies were performed, comparing the water uptake ability measured below and above saturation. In the first type the CCN counter was connected in series with the HTDMA and and closure was achieved over the whole range of probed dry diameters, growth factors and supersaturations using the κ-parametrization for the water activity and assuming surface tension of pure water in the Köhler theory. In the second closure type we compared hygroscopicity distributions derived from parallel monodisperse CCN measurements and HTDMA measurements

  16. 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

  17. 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).

  18. 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.

  19. 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.

  20. Optical and radiative-transfer properties of mixed atmospheric aerosols

    NASA Astrophysics Data System (ADS)

    Degheidy, A. R.; Sallah, M.; Elgarayhi, A.; Shaaban, S. M.

    2015-04-01

    The optical and radiative-transfer properties of mixed atmospheric aerosols have been investigated. The aerosol medium is considered as a plane-parallel anisotropic scattering medium with diffusive reflecting boundaries and containing an internal radiation source. The basic components are defined by their complex refractive index, a lognormal size distribution and humidity dependence in hygroscopic particles. The aerosol particles are assumed to be spherical, so the scattering parameters in the form of single scattering albedo, asymmetry factor, scattering, absorption, extinction efficiencies and linear anisotropic coefficient are calculated using the Mie theory. The calculations have been performed for individual aerosol particles, internal and external mixing media. Radiation transfer problem through the considered aerosol medium has been solved in terms of the solution of the corresponding source-free problem with simple boundary conditions. For the solution of the source-free problem, the Variational Pomraning-Eddington technique has been employed. The variation of the radiative-transfer properties (partial radiative fluxes at the medium boundaries) have been calculated and represented graphically for the different aerosols with their different mixing states. A comparison of the obtained results versus available published data has been performed and a very good agreement was observed.

  1. Characterization of aerosol optical properties, chemical composition and mixing states in the winter season in Shanghai, China.

    PubMed

    Tang, Yong; Huang, Yuanlong; Li, Ling; Chen, Hong; Chen, Jianmin; Yang, Xin; Gao, Song; Gross, Deborah S

    2014-12-01

    Physical and chemical properties of ambient aerosols at the single particle level were studied in Shanghai from December 22 to 28, 2009. A Cavity-Ring-Down Aerosol Extinction Spectrometer (CRD-AES) and a nephelometer were deployed to measure aerosol light extinction and scattering properties, respectively. An Aerosol Time-of-Flight Mass Spectrometer (ATOFMS) was used to detect single particle sizes and chemical composition. Seven particle types were detected. Air parcels arrived at the sampling site from the vicinity of Shanghai until mid-day of December 25, when they started to originate from North China. The aerosol extinction, scattering, and absorption coefficients all dropped sharply when this cold, clean air arrived. Aerosol particles changed from a highly aged type before this meteorological shift to a relatively fresh type afterwards. The aerosol optical properties were dependent on the wind direction. Aerosols with high extinction coefficient and scattering Ångström exponent (SAE) were observed when the wind blew from the west and northwest, indicating that they were predominantly fine particles. Nitrate and ammonium correlated most strongly with the change in aerosol optical properties. In the elemental carbon/organic carbon (ECOC) particle type, the diurnal trends of single scattering albedo (SSA) and elemental carbon (EC) signal intensity had a negative correlation. We also found a negative correlation (r=-0.87) between high mass-OC particle number fraction and the SSA in a relatively clean period, suggesting that particulate aromatic components might play an important role in light absorption in urban areas. PMID:25499489

  2. 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.

  3. The physical state of UTLS aerosols

    NASA Astrophysics Data System (ADS)

    Peter, Th.; Colberg, C. A.; Corti, T.; Fueglistaler, S.; Hoyle, C. R.; Koop, T.; Krieger, U. K.; Luo, B. P.; Marcolli, C.

    2003-04-01

    This paper gives an overview of the present knowledge on the physical state of aerosols in the upper troposphere (UT) and lower stratosphere (LS). Are UTLS aerosols liquid, solid or mixed-phase? And how does ice nucleate in/on such aerosols? Good progress has been made towards a quantitative theory of homogeneous nucleation of ice in purely liquid solutions of arbitrary composition and concentration based on a volume-proportional description. Very recently it has been proposed that ice nucleation might be facilitated by the surface of aerosol droplets, rather than starting in the bulk, suggests a reversal of the traditional view. Nucleation rates would then be surface-proportional rather than volume-proportional, with potentially strong effects on cloud formation, ice number densities and dehydration of UT. However, laboratory and theoretical evidence is presented corroborating the traditional picture. Above the frost point UTLS aerosols remain either liquid or mixed-phase, e.g. solid letovicite plus the remaining liquid containing aqueous inorganic acids and organic compounds. Massive deliquescence and efflorescence point reductions are expected to occur upon mixing of miscible organic and inorganic components. Hence, for a reliable prediction of the phase composition of individual aerosol particles, the knowledge of the aerosol's mixing state is indispensable. By now little is known about the morphology of mixed-phase aerosols. Experiments suggest that the solid may be coated by liquid, or conversely that the liquid might be enclosed by the solid, possibly leading to different radiative and heterogeneous chemical properties. Knowledge on the impact of efflorescence or salting out on subsequent ice formation is at its infancy. The relative importance of all these processes, in particular of homogeneous and heterogeneous ice nucleation in the UTLS, depends crucially on gravity-wave-induced small-scale temperature fluctuations with typical amplitudes of 1-2 K and

  4. Summer and winter time heterogeneity in aerosol single scattering albedo over the northwestern Atlantic Ocean during the TCAP field campaign: Relationship to chemical composition and mixing state

    NASA Astrophysics Data System (ADS)

    Berg, L. K.; Chand, D.; Fast, J. D.; Zelenyuk, A.; Wilson, J. M.; Sedlacek, A. J., III; Tomlinson, J. M.; Hubbe, J. M.; Comstock, J. M.; Mei, F.; Kassianov, E.; Schmid, B.

    2015-12-01

    Aerosol play crucial role in earth's radiative budget by scattering and absorbing solar radiation. The impact of aerosol on radiation budget depend on several factors including single scattering albedo (SSA), composition, and the growth processes, like coating or mixing. We describe findings relevant to optical properties of aerosol characterized over the Cape Cod and nearby northwest Atlantic Ocean during the Two Column Aerosol Project (TCAP) during the summer (July 2012) and winter (February 2013) campaigns. The average single scattering albedo (SSA) shows distinctly different vertical profiles during the summer and winter periods. During the summer study period, the average SSA is greater than 0.95 near surface, it increases to 0.97 until an altitude of 2.5 km, and then decreases to 0.94 at top of the column near 4 km. In contrast, during the winter study period the average SSA is less than 0.93 and decreases with height reaching an average value of 0.87 near the top of the column. The large difference in summer and winter time SSA is linked to the presence of biomass burning (BB) aerosol rather than black carbon or soot in both seasons. In our study, the BB on average is factor of two higher in free troposphere (FT) during summer and more than a factor of two higher in the boundary layer during winter. Single particle analysis indicates that the average profiles of refractory black carbon (rBC) mass are similar in both seasons. The average rBC size are similar at all altitudes sampled (0-4 km) in summer time but different during winter time. In addition, the particles sampled in the summertime FT appear to be more aged than those seen during winter. The observed large heterogeneity in SSA and its links to the particle coating and composition highlights the importance of aging and mixing processes of aerosol in this region and represents a challenge for both regional and global scale models.

  5. Aerosol Mass Loading, Mixing State, Size and Number in Present Day (2000) and Future (2100): Study with the Advanced Particle Microphysics (APM) module in the Community Earth System Model (CESM)

    NASA Astrophysics Data System (ADS)

    Luo, G.; Yu, F.

    2014-12-01

    Aerosols affect the global energy budget by scattering and absorbing sunlight (direct effects) and by changing the microphysical properties, lifetime, and coverage of clouds (indirect effects). One of the key challenges in quantifying the aerosol direct and indirect effects is to deep our understanding about the size distribution, size-resolved composition, and mixing state of aerosols. However, detailed information on size distribution and mixing state is often not available or incomplete in current climate models. Here, we incorporated APM into CESM. APM is a multi-type, multi-component (sulfate, nitrate, ammonium, SOA, BC, OC, dust, and sea salt), size-resolved particle microphysics model. Online chemistry, up-to-date nucleation, oxidation aging of medium-volatile and semi-volatile organic gases, aerosol-cloud interaction with stratiform cloud, shallow convection cloud, and deep convection cloud are considered. The amounts of secondary species coated on primary particles, through condensation, coagulation, equilibrium uptake, and aqueous chemistry, are also tracked. Model results are compared with aerosol mass observed by IMPROVE/EMEP, vertical structure of global particle number from aircraft-based field campaigns, particle and cloud condensation nuclei number at ground-based stations, aerosol optical properties retrieved by several satellites. Model results can capture the major characteristics shown in these observations. With this model system, we find that global burdens of sulfate, nitrate, ammonium, BC, OC from 2000 to 2100, under scenario RCP 4.5 where total radiative forcing is stabilized before 2100, are decreased by 44%, 50%, 43%, 40%, 40%, respectively. Dust and sea salt increase slightly. Global burdens of secondary species coated on BCOC, dust, and sea salt are deceased by 34%, 30% and 60%, respectively. Global averaged aerosol number in the lower troposphere (from surface to 3 km) is significantly decreased, especially for particles smaller than

  6. [Mixed states and schizophrenia].

    PubMed

    Fakra, E; Belzeaux, R; Pringuey, D; Cermolacce, M; Corréard, N; Micoulaud-Franchi, J-A; Azorin, J-M

    2013-12-01

    Because of their compilation of contrasted symptoms and their variable clinical presentation, mixed episodes have been withdrawn from the DSM. However, mixed states question not only the bonds between depression and mania, but also the distinction between bipolar disorders and schizophrenia. Indeed, doubts about the dichotomy introduced by Kraepelin between bipolar disorders and schizophrenia is as old as the nosolgy itself, as attest the later works of this author revealing his hesitations on his own classification. But findings here reviewed issued from recent technical advances, particularly in the imaging and genetic fields, offer a better understanding of the boundaries between these two disorders. Yet, when confronted to an acute episode, clinicians may find it challenging to distinguish a mixed state from a schizophrenic relapse. Indeed, there is no pathognomonic manifestation allowing to retain a diagnosis with confidence. The physician will therefore have to identify a pattern of signs, which will orient his assessment with no certainty. Thus, negative rather than affective or psychotic symptomatology appears to be useful in discriminating schizophrenia (or schizoaffective) disorders from mixed mania. However, a conclusion during this acute stage appears in definitive a formal exercise, first because the final diagnosis will only be ascertained once the symptoms are amended, and second because, according to our classifications, a mood episode, including mania and mixed mania, can be observed without ruling out the diagnosis of schizophrenia. PMID:24359851

  7. 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. PMID:24131283

  8. 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, H.-H.; Chen, S.-H.; Kleeman, M. J.; Zhang, H.; DeNero, S. P.; Joe, D. K.

    2015-11-01

    The source-oriented Weather Research and Forecasting chemistry model (SOWC) was modified to include warm cloud processes and applied to investigate how aerosol mixing states influence fog formation and optical properties in the atmosphere. SOWC tracks a 6-dimensional 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 longwave 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 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.

  9. 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.

  10. 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.

  11. CCN activation of fumed silica aerosols mixed with soluble pollutants

    NASA Astrophysics Data System (ADS)

    Dalirian, M.; Keskinen, H.; Ahlm, L.; Ylisirniö, A.; Romakkaniemi, S.; Laaksonen, A.; Virtanen, A.; Riipinen, I.

    2015-04-01

    Particle-water interactions of completely soluble or insoluble particles are fairly well understood but less is known of aerosols consisting of mixtures of soluble and insoluble components. In this study, laboratory measurements were performed to investigate cloud condensation nuclei (CCN) activity of silica particles mixed with ammonium sulfate (a salt), sucrose (a sugar) and bovine serum albumin known as BSA (a protein). The agglomerated structure of the silica particles was investigated using measurements with a differential mobility analyser (DMA) and an aerosol particle mass analyser (APM). Based on these data, the particles were assumed to be compact agglomerates when studying their CCN activation capabilities. Furthermore, the critical supersaturations of particles consisting of pure and mixed soluble and insoluble compounds were explored using existing theoretical frameworks. These results showed that the CCN activation of single-component particles was in good agreement with Köhler- and adsorption theory based models when the agglomerated structure was accounted for. For mixed particles the CCN activation was governed by the soluble components, and the soluble fraction varied considerably with particle size for our wet-generated aerosols. Our results confirm the hypothesis that knowing the soluble fraction is the key parameter needed for describing the CCN activation of mixed aerosols, and highlight the importance of controlled coating techniques for acquiring a detailed understanding of the CCN activation of atmospheric insoluble particles mixed with soluble pollutants.

  12. Aerosol Production in a Mixed Deciduous/Coniferous Forest

    NASA Astrophysics Data System (ADS)

    Slade, N.; Mielke, L.; Alaghmand, M.; Galloway, M.; Kammrath, A.; Keutsch, F.; Hansen, R.; Griffith, S.; Dusanter, S.; Stevens, P.; Carroll, M.; Bertman, S.; Shepson, P.

    2008-12-01

    Aerosols are of fundamental concern because of their impacts on air quality, human health and radiative forcing. Recent studies have focused on secondary organic aerosol (SOA) production due to oxidation of volatile organic compounds (VOCs), and more importantly biogenic-VOCs (BVOCs), in particular, isoprene. However, the SOA precursors are not well understood because the mechanisms have shown that isoprene oxidation can contribute to aerosol production through multiple generation oxidation products. For terpenes, it is more likely that primary or secondary oxidation products lead to particle formation. In the present study, we measured the aerosol size distribution, along with O3, HOx, NOx, NOy and BVOCs, in a mixed deciduous forest that is undergoing successional transition to a conifer-dominated species mix. This study was conducted in a rural forest environment in northern Michigan as a part of the summer 2008 PROPHET campaign at the University of Michigan Biological Station (UMBS). We examine here the potential BVOC contribution to aerosol formation. A TSI, inc. Scanning Mobility Particle Sizer (SMPS) was used to measure aerosol number density in the size range, 15 nm < x < 711 nm and a Proton Transfer Reaction - Linear Ion Trap (PTR-LIT) mass spectrometer for quantifying isoprene and other BVOCs, including methyl vinyl ketone and methacrolein, and total monoterpenes. Preliminary results show periods of new particle production. Here we use a unique set of BVOC, HOx, NOx, NOy, O3 and meteorological data to examine conditions leading to new particle production.

  13. Anthropogenic Aerosol Effects on Sea Surface Temperatures: Mixed-Layer Ocean Experiments with Explicit Aerosol Representation

    NASA Astrophysics Data System (ADS)

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

    2014-05-01

    Anthropogenic aerosols affect the Earth's radiative balance both through direct and indirect effects. These effects can lead to a reduction of the incoming solar radiation at the surface, i.e. dimming, which may lead to a change in sea surface temperatures (SST) or SST pattern. This, in turn, may affect precipitation patterns. The goal of the present work is to achieve an estimate of the equilibrium SST changes under anthropogenic aerosol forcing since industrialisation. We show preliminary results from mixed-layer ocean (MLO) experiments with explicit aerosol representation performed with ECHAM6-HAM. The (fixed) MLO heat flux into the deep ocean was derived from atmosphere only runs with fixed climatological SSTs (1961-1990 average) and present day (year 2000) aerosols and GHG burdens. Some experiments we repeated with an alternative MLO deep ocean heat flux (based on pre-industrial conditions) to test the robustness of our results with regard to this boundary condition. The maximum surface temperature responses towards anthropogenic aerosol and GHG forcing (separately and combined) were derived on a global and regional scale. The same set of experiments was performed with aerosol and GHG forcings representative of different decades over the past one and a half centuries. This allows to assess how SST patterns at equilibrium changed with changing aerosol (and GHG) forcing. Correlating SST responses with the change in downward clear-sky and all-sky shortwave radiation provides a first estimate of the response to anthropogenic aerosols. Our results show a clear contrast in hemispheric surface temperature response, as expected from the inter-hemispheric asymmetry of aerosol forcing The presented work is part of a project aiming at quantifying the effect of anthropogenic aerosol forcing on SSTs and the consequences for global precipitation patterns. Results from this study will serve as a starting point for further experiments involving a dynamic ocean model, which

  14. CCN activation of fumed silica aerosols mixed with soluble pollutants

    NASA Astrophysics Data System (ADS)

    Dalirian, M.; Keskinen, H.; Ahlm, L.; Ylisirniö, A.; Romakkaniemi, S.; Laaksonen, A.; Virtanen, A.; Riipinen, I.

    2014-09-01

    Particle-water interactions of completely soluble or insoluble particles are fairly well understood but less is known of aerosols consisting of mixtures of soluble and insoluble components. In this study, laboratory measurements were performed to investigate cloud condensation nuclei (CCN) activity of silica particles coated with ammonium sulphate (a salt), sucrose (a sugar) and bovine serum albumin known as BSA (a protein). In addition, the agglomerated structure of the silica particles was investigated by estimating the surface equivalent diameter based on measurements with a Differential Mobility Analyzer (DMA) and an Aerosol Particle Mass Analyzer (APM). By using the surface equivalent diameter the non-sphericity of the particles containing silica was accounted for when estimating CCN activation. Furthermore, characterizing critical supersaturations of particles consisting of pure soluble on insoluble compounds using existing frameworks showed that the CCN activation of single component particles was in good agreement with Köhler and adsorption theory based models when the agglomerated structure was accounted for. For mixed particles the CCN activation was governed by the soluble components, and the soluble fraction varied considerably with particle size for our wet-generated aerosols. Our results confirm the hypothesis that knowing the soluble fraction is the key parameter needed for describing the CCN activation of mixed aerosols, and highlight the importance of controlled coating techniques for acquiring a detailed understanding of the CCN activation of atmospheric insoluble particles mixed with soluble pollutants.

  15. 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...

  16. A size-composition resolved aerosol model for simulating the dynamics of externally mixed particles: SCRAM (v 1.0)

    NASA Astrophysics Data System (ADS)

    Zhu, S.; Sartelet, K. N.; Seigneur, C.

    2015-06-01

    The Size-Composition Resolved Aerosol Model (SCRAM) for simulating the dynamics of externally mixed atmospheric particles is presented. This new model classifies aerosols by both composition and size, based on a comprehensive combination of all chemical species and their mass-fraction sections. All three main processes involved in aerosol dynamics (coagulation, condensation/evaporation and nucleation) are included. The model is first validated by comparison with a reference solution and with results of simulations using internally mixed particles. The degree of mixing of particles is investigated in a box model simulation using data representative of air pollution in Greater Paris. The relative influence on the mixing state of the different aerosol processes (condensation/evaporation, coagulation) and of the algorithm used to model condensation/evaporation (bulk equilibrium, dynamic) is studied.

  17. 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

  18. Quantification of Feedbacks in Aerosol-Cloud-Precipitation Interactions of Mixed-Phase Clouds

    NASA Astrophysics Data System (ADS)

    Glassmeier, F.; Herger, N.; Ramelli, F.; Lohmann, U.

    2014-12-01

    The notion of clouds as buffered or resilient systems implies that generalized feedback processes unaccounted for in climate simulations may lead to an overestimation of the effective radiative forcing due to aerosol-cloud interactions, i.e. cloud lifetime effects. In this contribution, we study the importance of microphysical feedback processes in response to anthropogenic aerosols in orographic mixed-phase clouds. Our methods can be extended to other cloud regimes as well as dynamical and thermodynamical feedbacks. For our simulations, we use the regional atmospheric model COSMO-ART-M7 in a 2D setup with an idealized mountain. To capture major processes from aerosol emission to precipitation, the model is coupled to a modal aerosol scheme and includes aerosol activation and heterogeneous freezing as well as two-moment cold and warm cloud microphysics. We perform simulations with aerosol conditions that vary in amount and chemical composition and thus perturb the warm- and ice-phase pathways of precipitation formation and their mixed-phase interactions. Our analysis is based on quantifying the interaction strength between aerosol, cloud and precipitation variables by susceptibilities, i.e. relative sensitivities d ln(Y) / d ln(X), where the change in variable Y is a response to a perturbation in variable X. We describe how to decompose susceptibilities into a direct response expected from the parameterization and a contribution from feedbacks. Resilience features similar magnitudes but opposite signs for those contributions, resulting in an overall small susceptibility. We find considerable contributions from feedbacks, which appear more important for warm-phase than for cold-phase processes. We do not observe, however, a trend for resilience in mixed-phase cloud microphysics. Moreover, feedback contributions seem of secondary importance when compared to the strong dependence of susceptibilities on the microphysical state of the cloud.

  19. 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. PMID:25758418

  20. [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

  1. Mixed states in ferromagnetic superconductors

    SciTech Connect

    Matsumoto, H.; Teshima, R.; Umezawa, H.; Tachiki, M.

    1983-01-01

    A detailed study of the mixed state of the ferromagnetic rare-earth compounds RRh/sub 4/B/sub 4/, R/sub x/Mo/sub 6/S/sub 8/, and R/sub x/Mo/sub 6/Se/sub 6/ is presented. The saturation effect of the magnetic moments is taken into account. Depending on the parameters, there are many types of phase transitions between the type-II/2, type-II/1, and type-I mixed states and the paramagnetic Meissner state, ferromagnetic Meissner state, spin-periodic Meissner state, and the self-induced vortex state. It is predicted that the magnetization can exhibit a variety of unusual modes.

  2. Mechanisms for indirect effects from aerosol pollution on mixed-phase clouds

    NASA Astrophysics Data System (ADS)

    Phillips, Vaughan

    2015-04-01

    Aerosol pollution can have various effects on mixed-phase clouds. They can alter coalescence and raindrop-freezing for droplet activation by CCN aerosols. They can alter aggregation of ice crystals and snow formation. This can alter the lifetime of mixed-phase clouds, as well as the reflectivity for solar radiation. Simulations of observed cases of mixed-phase clouds have been performed to examine the mechanisms for effects from aerosol pollution on them. Such mechanisms are discussed in the presentation.

  3. 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

  4. 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.

  5. 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

  6. 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.

  7. 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.

  8. 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.

  9. 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.

  10. 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.

  11. Aerosols in the study of convective acinar mixing

    PubMed Central

    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 μm-diameter particles were inhaled at penetration volumes (Vp) 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. PMID:15890563

  12. 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.

  13. 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

  14. Vertical aerosol structure and aerosol mixed layer heights determined with scanning shipborne lidars during the TexAQS II study

    NASA Astrophysics Data System (ADS)

    McCarty, B. J.; Senff, C. J.; Tucker, S. C.; Eberhard, W. L.; Marchbanks, R. D.; Machol, J.; Brewer, W. A.

    2007-12-01

    The NOAA Earth Systems Research Laboratory (ESRL) deployed the Ozone Profiling Atmospheric LIDAR (OPAL) on the R/V Ronald H. Brown during the summer of 2006 for the Texas Air Quality Study (TEXAQS II). Calibrated aerosol backscatter profiles were determined from data collected at the 355 nm wavelength using a modified Klett retrieval method. OPAL employs a unique scan sequence that consists of staring at multiple elevation angles between 2 and 90 degrees, which is repeated approx. every 90 sec. Blending the data from the various elevation angles allows to extend the aerosol backscatter profiles down to near the surface (approximately 10 meters ASL), while maintaining a high spatial resolution (5 meters). Successful application of this technique requires the aerosol distribution to be sufficiently horizontally homogeneous over several kilometers. Estimates of aerosol mixed layer height were determined by applying a Haar wavelet transform method to detect the gradient that is often present at the top of the boundary layer. Co-located on the R/V Ronald H. Brown, was NOAA/ESRL's High Resolution Doppler LIDAR (HRDL). Aerosol mixed layer heights were also estimated using the data from the 2 micron Doppler LIDAR. A comparison of the mixed layer heights as determined from each LIDAR's observations was used to choose the height of the layer likely connected with the surface. The vertical structure of aerosols in the lower troposphere, in particular the presence of aerosol layers above the boundary layer, is important in understanding radiative effects of aerosols. We will present aerosol backscatter structure in the lower troposphere encountered during the TexAQS II study as well as a comparison of relative aerosol content in the free troposphere compared to that within the boundary layer.

  15. [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

  16. Enhanced light absorption and scattering by carbon soot aerosol internally mixed with sulfuric acid.

    PubMed

    Khalizov, Alexei F; Xue, Huaxin; Wang, Lin; Zheng, Jun; Zhang, Renyi

    2009-02-12

    Light absorption by carbon soot increases when the particles are internally mixed with nonabsorbing materials, leading to increased radiative forcing, but the magnitude of this enhancement is a subject of great uncertainty. We have performed laboratory experiments of the optical properties of fresh and internally mixed carbon soot aerosols with a known particle size, morphology, and the mixing state. Flame-generated soot aerosol is size-selected with a double-differential mobility analyzer (DMA) setup to eliminate multiply charged particle modes and then exposed to gaseous sulfuric acid (10(9)-10(10) molecule cm(-3)) and water vapor (5-80% relative humidity, RH). Light extinction and scattering by fresh and internally mixed soot aerosol are measured at 532 nm wavelength using a cavity ring-down spectrometer and an integrating nephelometer, respectively, and the absorption is derived as the difference between extinction and scattering. The optical properties of fresh soot are independent of RH, whereas soot internally mixed with sulfuric acid exhibits significant enhancement in light absorption and scattering, increasing with the mass fraction of sulfuric acid coating and relative humidity. For soot particles with an initial mobility diameter of 320 nm and a 40% H(2)SO(4) mass coating fraction, absorption and scattering are increased by 1.4- and 13-fold at 80% RH, respectively. Also, the single scattering albedo of soot aerosol increases from 0.1 to 0.5 after coating and humidification. Additional measurements with soot particles that are first coated with sulfuric acid and then heated to remove the coating show that both scattering and absorption are enhanced by irreversible restructuring of soot aggregates to more compact globules. Depending on the initial size and density of soot aggregates, restructuring acts to increase or decrease the absorption cross-section, but the combination of restructuring and encapsulation always results in an increased absorption for

  17. 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.

  18. In situ vertical profiles of aerosol extinction, mass, and composition over the southeast United States during SENEX and SEAC4RS: observations of a modest aerosol enhancement aloft

    NASA Astrophysics Data System (ADS)

    Wagner, N. L.; Brock, C. A.; Angevine, W. M.; Beyersdorf, A.; Campuzano-Jost, P.; Day, D. A.; de Gouw, J. A.; Diskin, G. S.; Gordon, T. D.; Graus, M. G.; Huey, G.; Jimenez, J. L.; Lack, D. A.; Liao, J.; Liu, X.; Markovic, M. Z.; Middlebrook, A. M.; Mikoviny, T.; Peischl, J.; Perring, A. E.; Richardson, M. S.; Ryerson, T. B.; Schwarz, J. P.; Warneke, C.; Welti, A.; Wisthaler, A.; Ziemba, L. D.; Murphy, D. M.

    2015-02-01

    Vertical profiles of submicron aerosol over the southeastern United States (SEUS) during the summertime from in situ aircraft-based measurements were used to construct aggregate profiles of chemical, microphysical, and optical properties. Shallow cumulus convection was observed during many profiles. These conditions enhance vertical transport of trace gases and aerosol and create a cloudy transition layer on top of the sub-cloud mixed layer. The trace gas and aerosol concentrations in the transition layer were modeled as a mixture with contributions from the mixed layer below and the free troposphere above. The amount of vertical mixing, or entrainment of air from the free troposphere, was quantified using the observed mixing ratio of carbon monoxide (CO). Although the median aerosol mass, extinction, and volume decreased with altitude in the transition layer, they were ~10% larger than expected from vertical mixing alone. This enhancement was likely due to secondary aerosol formation in the transition layer. Although the transition layer enhancements of the particulate sulfate and organic aerosol (OA) were both similar in magnitude, only the enhancement of sulfate was statistically significant. The column integrated extinction, or aerosol optical depth (AOD), was calculated for each individual profile, and the transition layer enhancement of extinction typically contributed less than 10% to the total AOD. Our measurements and analysis were motivated by two recent studies that have hypothesized an enhanced layer of secondary organic aerosol (SOA) aloft to explain the summertime enhancement of AOD (2-3 times greater than winter) over the southeastern United States. In contrast to this hypothesis, the modest enhancement we observed in the transition layer was not dominated by OA and was not a large fraction of the summertime AOD.

  19. Effect of aggregation, morphology and mixing state on optical properties of bare and internally mixed Black Carbon particles

    NASA Astrophysics Data System (ADS)

    Scarnato, Barbara; China, Swarup; Mazzoleni, Claudio

    2014-05-01

    Black carbon (BC) is a small, dark particle that warms Earth's climate. BC is a distinct type of carbonaceous aerosol particle, product of combustion of fossil and biomass fuels. Upon emission into the atmosphere, BC internally mixes with other aerosol compounds. According to recent studies, internal mixing of BC with other aerosol materials in the atmosphere alters its aggregate shape, absorption of solar radiation, and radiative forcing. These mixing state effects are not yet fully understood. Laboratory and field studies have identified a strong variability in the observed absorption efficiencies of internally mixed BC. Additionally, there is a discrepancy between modeled and measured values using traditional modeling approaches. This talk will investigate the central role of parameterization of light interaction by BC particles in the assessment of its radiative forcing and present a sensitivity study of the effect of aggregation, morphology and mixing state on optical properties of bare and internally mixed BC with mineral dust, ammonium sulfate, sodium chloride and others. Optical properties of the different mixtures, sampled both in field campaigns and laboratory environment, are computed using Discrete Dipole Approximation model in accordance with BC aggregation, morphology and mixing observed at microscopes. The results of this work are relevant for several applications in atmospheric science, including but not limited to radiative transfer calculations, regional and global climate modeling and, the interpretation of remote sensing measurements.

  20. Chemical composition and mixing-state of ice residuals sampled within mixed phase clouds

    NASA Astrophysics Data System (ADS)

    Ebert, M.; Worringen, A.; Benker, N.; Mertes, S.; Weingartner, E.; Weinbruch, S.

    2011-03-01

    During an intensive campaign at the high alpine research station Jungfraujoch, Switzerland, in February/March 2006 ice particle residuals within mixed-phase clouds were sampled using the Ice-counterflow virtual impactor (Ice-CVI). Size, morphology, chemical composition, mineralogy and mixing state of the ice residual and the interstitial (i.e., non-activated) aerosol particles were analyzed by scanning and transmission electron microscopy. Ice nuclei (IN) were identified from the significant enrichment of particle groups in the ice residual (IR) samples relative to the interstitial aerosol. In terms of number lead-bearing particles are enriched by a factor of approximately 25, complex internal mixtures with silicates or metal oxides as major components by a factor of 11, and mixtures of secondary aerosol and carbonaceous material (C-O-S particles) by a factor of 2. Other particle groups (sulfates, sea salt, Ca-rich particles, external silicates) observed in the ice-residual samples cannot be assigned unambiguously as IN. Between 9 and 24% of all IR are Pb-bearing particles. Pb was found as major component in around 10% of these particles (PbO, PbCl2). In the other particles, Pb was found as some 100 nm sized agglomerates consisting of 3-8 nm sized primary particles (PbS, elemental Pb). C-O-S particles are present in the IR at an abundance of 17-27%. The soot component within these particles is strongly aged. Complex internal mixtures occur in the IR at an abundance of 9-15%. Most IN identified at the Jungfraujoch station are internal mixtures containing anthropogenic components (either as main or minor constituent), and it is concluded that admixture of the anthropogenic component is responsible for the increased IN efficiency within mixed phase clouds. The mixing state appears to be a key parameter for the ice nucleation behaviour that cannot be predicted from the sole knowledge of the main component of an individual particle.

  1. Mixing state of atmospheric particles over the North China Plain

    NASA Astrophysics Data System (ADS)

    Zhang, S. L.; Ma, N.; Kecorius, S.; Wang, P. C.; Hu, M.; Wang, Z. B.; Größ, J.; Wu, Z. J.; Wiedensohler, A.

    2016-01-01

    In this unique processing study, the mixing state of ambient submicron aerosol particles in terms of hygroscopicity and volatility was investigated with a Hygroscopicity Tandem Differential Mobility Analyzer and a Volatility Tandem Differential Mobility Analyzer. The measurements were conducted at a regional atmospheric observational site in the North China Plain (NCP) from 8 July to 9 August, 2013. Multimodal patterns were observed in the probability density functions of the hygroscopicity parameter κ and the shrink factor, indicating that ambient particles are mostly an external mixture of particles with different hygroscopicity and volatility. Linear relationships were found between the number fraction of hydrophobic and non-volatile populations, reflecting the dominance of soot in hydrophobic and non-volatile particles. The number fraction of non-volatile particles is lower than that of hydrophobic particles in most cases, indicating that a certain fraction of hydrophobic particles is volatile. Distinct diurnal patterns were found for the number fraction of the hydrophobic and non-volatile particles, with a higher level at nighttime and a lower level during the daytime. The result of air mass classification shows that aerosol particles in air masses coming from north with high moving speed have a high number fraction of hydrophobic/non-volatile population, and are more externally mixed. Only minor differences can be found between the measured aerosol properties for the rest of the air masses. With abundant precursor in the NCP, no matter where the air mass originates, as far as it stays in the NCP for a certain time, aerosol particles may get aged and mixed with newly emitted particles in a short time.

  2. SLOCC invariants for multipartite mixed states

    NASA Astrophysics Data System (ADS)

    Jing, Naihuan; Li, Ming; Li-Jost, Xianqing; Zhang, Tinggui; Fei, Shao-Ming

    2014-05-01

    We construct a nontrivial set of invariants for any multipartite mixed states under the stochastic local operations and classical communication symmetry. These invariants are given by hyperdeterminants and independent of basis change. In particular, a family of d2 invariants for arbitrary d-dimensional even partite mixed states are explicitly given.

  3. Effect of Aerosol Size and Hygroscopicity on Aerosol Optical Depth in the Southeastern United States

    NASA Astrophysics Data System (ADS)

    Brock, Charles; Wagner, Nick; Gordon, Timothy

    2016-04-01

    Aerosol optical depth (AOD) is affected by the size, optical characteristics, and hygroscopicity of particles, confounding attempts to link remote sensing observations of AOD to measured or modeled aerosol mass concentrations. In situ airborne observations of aerosol optical, chemical, microphysical and hygroscopic properties were made in the southeastern United States in the daytime in summer 2013. We use these observations to constrain a simple model that is used to test the sensitivity of AOD to the various measured parameters. As expected, the AOD was found to be most sensitive to aerosol mass concentration and to aerosol water content, which is controlled by aerosol hygroscopicity and the ambient relative humidity. However, AOD was also fairly sensitive to the mean particle diameter and the width of the size distribution. These parameters are often prescribed in global models that use simplified modal parameterizations to describe the aerosol, suggesting that the values chosen could substantially bias the calculated relationship between aerosol mass and optical extinction, AOD, and radiative forcing.

  4. 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.}

  5. 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

  6. 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.

  7. Compressibility of Quantum Mixed-State Signals

    SciTech Connect

    Koashi, Masato; Imoto, Nobuyuki

    2001-07-02

    We present a formula that determines the optimal number of qubits per message that allows asymptotically faithful compression of the quantum information carried by an ensemble of mixed states. The set of mixed states determines a decomposition of the Hilbert space into the redundant part and the irreducible part. After removing the redundancy, the optimal compression rate is shown to be given by the von Neumann entropy of the reduced ensemble.

  8. 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.

  9. Aerosol Nucleation Frequency and Hygroscopicity at a Forested Site in the Southeastern United States

    NASA Astrophysics Data System (ADS)

    O'Halloran, T. L.; Fuentes, J. D.; Collins, D. R.; Cleveland, M. J.

    2007-12-01

    This paper examines how aerosol hygroscopicity and nucleation frequency, measured with a tandem differential mobility analyzer (TDMA) at a rural site in the southeastern United States, vary with air mass source regions and transport pathways. We also examine an observed enhancement in aerosol hygroscopicity during nucleation events. During October through December, 2006, a TDMA was used to measure submicron aerosol size distributions and size-resolved hygroscopicity at a forested site in the southeastern U.S. Measurements were conducted above a mixed deciduous forest at the Virginia Forest Research Facility, a newly operational permanent micrometeorological facility located approximately 20 km east of the foothills of the Blue Ridge Mountains. The site features a 40-m walkup scaffolding tower above a 20-m mixed deciduous forest with excellent fetch, and a climate controlled lab for housing instruments and data acquisition systems. Hygroscopic growth factor distributions were measured for eight dry diameters between 0.013 and 0.400 μm. Cluster analysis of back trajectories was applied to identify characteristic source regions and air mass pathways during the study period. Significant differences were found in the frequency of aerosol nucleation events and hygroscopicity amongst the five distinct pathways identified by the cluster analysis. Nucleation occurred most frequently when fast moving air masses originated from the northern central U.S. and lower central Canada. In these cases existing aerosol surface area was low, and the majority of trajectories passed directly over the Ohio River valley. Hygroscopicity generally increased with increasing dry diameter, except for the largest size bin, which had a slightly lower hygroscopicity than the next smallest size. Two clusters with short, stagnant trajectories contained aerosols with enhanced hygroscopicity at dry diameters less than 0.100 μm. Aerosol hygroscopicity was significantly enhanced, especially at small

  10. Mixed-Symmetry States in ^93Nb

    NASA Astrophysics Data System (ADS)

    McKay, C. J.; Bandyopadhyay, D.; Lesher, S. R.; Mynk, M.; Orce, J.; McEllistrem, M. T.; Yates, S. W.

    2003-10-01

    The neutron-proton version of the interacting boson model predicts the existence of mixed-symmetry collective excitations. In an even-even nucleus the 2^+_ms state has the distinctive signature of a strong M1 transition to the first 2^+ state and a weak E2 transiton to the ground state. Previous investigations of the N=52 isotones ^92Zr, ^94Mo and ^96Ru have have led to the identification of mixed-symmetry states. It is expected that odd-A nuclei will also display states with mixed-symmetry character. Therefore, excitation function and angular distibution measurements have been performed on ^93Nb, the lone stable odd-A N=52 isotone, using the (n,n^'γ) reaction at the University of Kentucky. Lifetimes were determined with the Doppler-shift attenuation method. This work was supported by the U.S. National Science Foundation under grant No. PHY-0098813

  11. In situ vertical profiles of aerosol extinction, mass, and composition over the southeast United States during SENEX and SEAC4RS: observations of a modest aerosol enhancement aloft

    NASA Astrophysics Data System (ADS)

    Wagner, N. L.; Brock, C. A.; Angevine, W. M.; Beyersdorf, A.; Campuzano-Jost, P.; Day, D.; de Gouw, J. A.; Diskin, G. S.; Gordon, T. D.; Graus, M. G.; Holloway, J. S.; Huey, G.; Jimenez, J. L.; Lack, D. A.; Liao, J.; Liu, X.; Markovic, M. Z.; Middlebrook, A. M.; Mikoviny, T.; Peischl, J.; Perring, A. E.; Richardson, M. S.; Ryerson, T. B.; Schwarz, J. P.; Warneke, C.; Welti, A.; Wisthaler, A.; Ziemba, L. D.; Murphy, D. M.

    2015-06-01

    Vertical profiles of submicron aerosol from in situ aircraft-based measurements were used to construct aggregate profiles of chemical, microphysical, and optical properties. These vertical profiles were collected over the southeastern United States (SEUS) during the summer of 2013 as part of two separate field studies: the Southeast Nexus (SENEX) study and the Study of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS). Shallow cumulus convection was observed during many profiles. These conditions enhance vertical transport of trace gases and aerosol and create a cloudy transition layer on top of the sub-cloud mixed layer. The trace gas and aerosol concentrations in the transition layer were modeled as a mixture with contributions from the mixed layer below and the free troposphere above. The amount of vertical mixing, or entrainment of air from the free troposphere, was quantified using the observed mixing ratio of carbon monoxide (CO). Although the median aerosol mass, extinction, and volume decreased with altitude in the transition layer, they were ~10 % larger than expected from vertical mixing alone. This enhancement was likely due to secondary aerosol formation in the transition layer. Although the transition layer enhancements of the particulate sulfate and organic aerosol (OA) were both similar in magnitude, only the enhancement of sulfate was statistically significant. The column integrated extinction, or aerosol optical depth (AOD), was calculated for each individual profile, and the transition layer enhancement of extinction typically contributed less than 10 % to the total AOD. Our measurements and analysis were motivated by two recent studies that have hypothesized an enhanced layer of secondary aerosol aloft to explain the summertime enhancement of AOD (2-3 times greater than winter) over the southeastern United States. The first study attributes the layer aloft to secondary organic aerosol (SOA) while

  12. 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.

  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. Mixed-Symmetry States in 96Mo

    SciTech Connect

    Lesher, S.R.; Bandyopadhyay, D.; Boukharouba, N.; Mynk, M.; McKay, C.J.; McEllistrem, M.T.; Yates, S.W.; Fransen, C.

    2004-09-13

    Mixed-symmetry states in 96Mo have been identified using the (n,n'{gamma}) reaction. From the lifetime measured using the Doppler-shift attenuation method and multipole mixing ratios, B(E2) and B(M1) values were determined. The 2{sub ms}{sup +} state was found at 2095.77 keV with B(M1: 2{sub ms}{sup +} {yields} 2{sub 1}{sup +}) = 0.18{mu}{sub N}{sup 2}, while the 1{sub ms}{sup +} strength lies primarily in states at 2794.45 and 3300.23 keV.

  15. 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.

  16. 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.

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

    2015-11-01

    Biomass burning is a major source of black carbon (BC) and primary organic aerosol globally. In particular, biomass burning organic aerosol (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 aged biomass burning. Cluster analysis of single particle measurements identified five BBOA-related particle types. rBC accounted for 3-14 w.t. % 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.

  18. 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.

  19. 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

  20. Numerical investigation of the coagulation mixing between dust and hygroscopic aerosol particles and its impacts

    NASA Astrophysics Data System (ADS)

    Tsai, I.-Chun; Chen, Jen-Ping; Lin, Yi-Chiu; Chung-Kuang Chou, Charles; Chen, Wei-Nai

    2015-05-01

    A statistical-numerical aerosol parameterization was incorporated into the Community Multiscale Air Quality modeling system to study the coagulation mixing process focusing on a dust storm event that occurred over East Asia. Simulation results show that the coagulation mixing process tends to decrease aerosol mass, surface area, and number concentrations over the dust source areas. Over the downwind oceanic areas, aerosol concentrations generally increased due to enhanced sedimentation as particles became larger upon coagulation. The mixture process can reduce the overall single-scattering albedo by up to 10% as a result of enhanced core with shell absorption by dust and reduction in the number of scattering particles. The enhanced dry deposition speed also altered the vertical distribution. In addition, the ability of aerosol particles to serve as cloud condensation nuclei (CCN) increased from around 107 m-3 to above 109 m-3 over downwind areas because a large amount of mineral dust particles became effective CCN with solute coating, except over the highly polluted areas where multiple collections of hygroscopic particles by dust in effect reduced CCN number. This CCN effect is much stronger for coagulation mixing than by the uptake of sulfuric acid gas on dust, although the nitric acid gas uptake was not investigated. The ability of dust particles to serve as ice nuclei may decrease or increase at low or high subzero temperatures, respectively, due to the switching from deposition nucleation to immersion freezing or haze freezing.

  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. Mixed-symmetry states in ^114Cd

    NASA Astrophysics Data System (ADS)

    Bandyopadhyay, D.; Reynolds, C. C.; Fransen, C.; Boukharouba, N.; McEllistrem, M. T.; Yates, S. W.

    2002-10-01

    In recent years, there has been considerable interest in the properties of a new class of low-lying excitations known as mixed-symmetry states. These states, associated with the isovector part of the boson wave functions and characterized by their strong M1 transitions, have been extensively studied in deformed nuclei; however, for U(5) nuclei these states have rarely been characterized(P. E. Garrett et al., Phy. Rev. C 54). 2259(1996). Therefore, we have examined the low-spin states in ^114Cd, which has long been considered as a good vibrational nucleus(R. F. Casten et al. Phys. Lett. 297B), 19(1992). Levels in ^114Cd were studied at the University of Kentucky 7 MV accelerator facility in measurements of excitation functions and angular distributions of γ-rays emitted in the (n,n^'γ) reaction. The Doppler-shift attenuation method has been used to determine level lifetimes. A strong M1 transition from the 2218.9-keV level (2^+) to the 2_1^+ level indicates that the 2218.9-keV level is a probable candidate for the fundamental mixed-symmetry state. A weak E2 transition from this level to the ground state further supports the assignment of this state as one-phonon mixed-symmetry state. The search for two-phonon mixed-symmetry states is in progress. This work was supported by the U. S. National Science Foundation under grant No. PHY-0098813

  5. Coexisting aggregates in mixed aerosol OT and cholesterol microemulsions.

    PubMed

    Sedgwick, Myles A; Trujillo, Alejandro M; Hendricks, Noah; Levinger, Nancy E; Crans, Debbie C

    2011-02-01

    Dynamic light scattering and NMR spectroscopic experimental evidence suggest the coexistence of two compositionally different self-assembled particles in solution. The self-assembled particles form in solutions containing water, Aerosol OT (AOT, sodium bis(2-ethylhexyl) sulfosuccinate) surfactant, and cholesterol in cyclohexane. In a similar series of studies carried out in 1-octanol only one aggregate type, that is, reverse micelles, is observed. Dynamic light scattering measurements reveal the presence of two different types of aggregates in the microemulsions formed in cyclohexane, demonstrating the coexistence of two compositionally distinct structures with very similar Gibbs energies. One particle type consists of standard AOT reverse micelles while the second type of particle consists of submicellar aggregates including cholesterol as well as small amounts of AOT and water. In microemulsions employing 1-octanol as the continuous medium, AOT reverse micelles form in a dispersed solution of cholesterol in 1-octanol. Although the size distribution of self-assembled particles is well-known for many different systems, evidence for simultaneous formation of two distinctly sized particles in solution that are chemically different is unprecedented. The ability to form microemulsion solutions that contain coexisting particles may have important applications in drug formulation and administration, particularly as applied to drug delivery using cholesterol as a targeting agent. PMID:21188993

  6. Biases in modeled surface snow BC mixing ratios in prescribed-aerosol climate model runs

    NASA Astrophysics Data System (ADS)

    Doherty, S. J.; Bitz, C. M.; Flanner, M. G.

    2014-11-01

    Black carbon (BC) in snow lowers its albedo, increasing the absorption of sunlight, leading to positive radiative forcing, climate warming and earlier snowmelt. A series of recent studies have used prescribed-aerosol deposition flux fields in climate model runs to assess the forcing by black carbon in snow. In these studies, the prescribed mass deposition flux of BC to surface snow is decoupled from the mass deposition flux of snow water to the surface. Here we compare prognostic- and prescribed-aerosol runs and use a series of offline calculations to show that the prescribed-aerosol approach results, on average, in a factor of about 1.5-2.5 high bias in annual-mean surface snow BC mixing ratios in three key regions for snow albedo forcing by BC: Greenland, Eurasia and North America. These biases will propagate directly to positive biases in snow and surface albedo reduction by BC. The bias is shown be due to coupling snowfall that varies on meteorological timescales (daily or shorter) with prescribed BC mass deposition fluxes that are more temporally and spatially smooth. The result is physically non-realistic mixing ratios of BC in surface snow. We suggest that an alternative approach would be to prescribe BC mass mixing ratios in snowfall, rather than BC mass fluxes, and we show that this produces more physically realistic BC mixing ratios in snowfall and in the surface snow layer.

  7. Optical properties of internally mixed aerosol particles composed of dicarboxylic acids and ammonium sulfate.

    PubMed

    Freedman, Miriam A; Hasenkopf, Christa A; Beaver, Melinda R; Tolbert, Margaret A

    2009-12-01

    We have investigated the optical properties of internally mixed aerosol particles composed of dicarboxylic acids and ammonium sulfate using cavity ring-down aerosol extinction spectroscopy at a wavelength of 532 nm. The real refractive indices of these nonabsorbing species were retrieved from the extinction and concentration of the particles using Mie scattering theory. We obtain refractive indices for pure ammonium sulfate and pure dicarboxylic acids that are consistent with literature values, where they exist, to within experimental error. For mixed particles, however, our data deviates significantly from a volume-weighted average of the pure components. Surprisingly, the real refractive indices of internal mixtures of succinic acid and ammonium sulfate are higher than either of the pure components at the highest organic weight fractions. For binary internal mixtures of oxalic or adipic acid with ammonium sulfate, the real refractive indices of the mixtures are approximately the same as ammonium sulfate for all organic weight fractions. Various optical mixing rules for homogeneous and slightly heterogeneous systems fail to explain the experimental real refractive indices. It is likely that complex particle morphologies are responsible for the observed behavior of the mixed particles. Implications of our results for atmospheric modeling and aerosol structure are discussed. PMID:19877658

  8. 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.

  9. 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.

  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. 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.

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

    NASA Astrophysics Data System (ADS)

    Matsui, H.; Koike, M.; Kondo, Y.; Moteki, N.; Fast, J. D.; Zaveri, R. A.

    2013-03-01

    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) with 12 size × 10 mixing state bins, 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. This result shows that the model can simulate realistic BC mixing states in the atmosphere if condensation and coagulation processes are calculated explicitly with the detailed treatment of BC mixing state. 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

  13. Externally mixed aerosol : simulation of ice nucleation in a parcel model

    NASA Astrophysics Data System (ADS)

    Anquetil-Deck, Candy; Hoose, Corinna; Conolly, Paul

    2014-05-01

    The effect of different aerosol (mineral dust, bacteria and soot) acting as immersion ice nuclei is investigated using ACPIM (AerosolCloud Precipitation Interaction Model) [1]. ACPIM is a powerful tool which can be used in two different ways. This box model can be, either, driven by experimental data (experiments carried out at the AIDA cloud chamber facility) or used as an air parcel in order to examine different ice nucleation parameterizations under specific conditions. This adiabatic air parcel model was employed for the simulation of a convective cloud. The study consists here in the investigation of how two externally mixed aerosols interact with one another. The initial study concentrates on mineral dust aerosol and biological aerosol without any background in order to fully understand the interaction between the different types of aerosol. Immersion freezing is described for the mineral dust aerosol by Niemand et al. 's parameterization [2], which was derived from laboratory studies in AIDA and is an extension of surface site density approach suggested by Connolly et al. [1]. Regarding bioaerosol, we introduce Hummel et al. 's parameterization [3] : f(in) = f(max)(1 - exp(- Ap *n(s)(T))) With an empirically fitted ice nucleation active site density n s based on AIDA measurements of Pseudomonas syringae bacteria [4]. This initial study is conducted for different proportion of each aerosol (the total number of aerosol being constant throughout all the simulation runs) at different vertical velocities. We then extented this study with different backgrounds (urban, marine, rural) in order to get a full picture. We found that there is not only a CCN competition but an IN competition as well. References : [1] Connolly, P. J., Möhler O., Field P. R., Saathoff H., Burgess, R., Choularton, T. and Gallagher, M., Atmos. Chem. Phys 9, 2805-2824 (2009). [2] Niemand, M., Möhler, O., Vogel B., Vogel, H., Hoose, C., Connolly, P., Klein, H., Bingemer, H., De

  14. Arctic Cloud-driven Mixed Layers and Surface Coupling State

    NASA Astrophysics Data System (ADS)

    Shupe, M.; Persson, O. P.; Solomon, A.; de Boer, G.

    2013-12-01

    Arctic low-level clouds interact with the atmosphere and underlying surface via many inter-related processes. The balance of cloud radiative warming and cooling effects imparts a strong control on the net surface energy budget. Cloud-driven atmospheric circulations can impact surface turbulent heat fluxes and influence the vertical mixing of atmospheric state parameters and aerosols. Large-scale advection of heat and moisture provides the background context within which these local interactions unfold. Importantly, these radiative, dynamical, and advective processes also contribute to a complex web of self-sustaining cloud processes that can promote cloud maintenance over long periods of time. We examine many of these processes, with a specific focus on the dynamical linkages between Arctic clouds and the surface that influence low-level atmospheric structure and mixing. Comprehensive, ground-based observations from meteorological towers, remote-sensors, and radiosondes are used to simultaneously characterize surface fluxes, atmospheric structure, cloud properties, in-cloud motions, and the depth of the cloud-driven mixed layer in multiple Arctic environments. Relationships among these parameters are explored to elucidate the properties of the system that determine the degree of vertical atmospheric mixing and the coupling state between cloud and surface. The influence of temperature and moisture inversions on this system is also explored. Transitions in the coupling state are utilized to illustrate the relative roles of different processes. Cases from a coastal Arctic site at Barrow, Alaska and a station embedded in the Arctic sea-ice pack are used to contrast conditional influences related to season and surface type. It is found that over sea-ice, where surface turbulent fluxes are weak, the coupling of cloud-level processes to the surface layer is largely due to proximity of the cloud-driven mixed layer to the surface, which appears to be primarily influenced by

  15. Accounting for aerosol scattering in the CLARS retrieval of column averaged CO2 mixing ratios

    NASA Astrophysics Data System (ADS)

    Zhang, Qiong; Natraj, Vijay; Li, King-Fai; Shia, Run-Lie; Fu, Dejian; Pongetti, Thomas J.; Sander, Stanley P.; Roehl, Coleen M.; Yung, Yuk L.

    2015-07-01

    The California Laboratory for Atmospheric Remote Sensing Fourier transform spectrometer (CLARS-FTS) deployed at Mount Wilson, California, has been measuring column abundances of greenhouse gases in the Los Angeles (LA) basin in the near-infrared spectral region since August 2011. CLARS-FTS measures reflected sunlight and has high sensitivity to absorption and scattering in the boundary layer. In this study, we estimate the retrieval biases caused by aerosol scattering and present a fast and accurate approach to correct for the bias in the CLARS column averaged CO2 mixing ratio product, XCO2. The high spectral resolution of 0.06 cm-1 is exploited to reveal the physical mechanism for the bias. We employ a numerical radiative transfer model to simulate the impact of neglecting aerosol scattering on the CO2 and O2 slant column densities operationally retrieved from CLARS-FTS measurements. These simulations show that the CLARS-FTS operational retrieval algorithm likely underestimates CO2 and O2 abundances over the LA basin in scenes with moderate aerosol loading. The bias in the CO2 and O2 abundances due to neglecting aerosol scattering cannot be canceled by ratioing each other in the derivation of the operational product of XCO2. We propose a new method for approximately correcting the aerosol-induced bias. Results for CLARS XCO2 are compared to direct-Sun XCO2 retrievals from a nearby Total Carbon Column Observing Network (TCCON) station. The bias-correction approach significantly improves the correlation between the XCO2 retrieved from CLARS and TCCON, demonstrating that this approach can increase the yield of useful data from CLARS-FTS in the presence of moderate aerosol loading.

  16. 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

  17. 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

  18. Multistability with a metastable mixed state.

    PubMed

    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. PMID:23005273

  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. SAMPLING DURATION DEPENDENCE OF SEMI-CONTINUOUS ORGANIC CARBON MEASUREMENTS ON STEADY STATE SECONDARY ORGANIC AEROSOLS

    EPA Science Inventory

    Semi-continuous organic carbon concentrations were measured through several experiments of statically generated secondary organic aerosol formed by hydrocarbon + NOx irradiations. Repeated, randomized measurements of these steady state aerosols reveal decreases in the observed c...

  1. 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.

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

    2015-11-01

    Aircraft observations of meteorological, trace gas, and aerosol properties were made between May and September 2013. 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 of 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 airmasses in which an accumulation mode between 0.1-0.5 μm diameter dominates aerosol extinction.

  3. Vertical transport and processing of aerosols in a mixed-phase convective cloud and the feedback on cloud development

    NASA Astrophysics Data System (ADS)

    Yin, Y.; Carslaw, K. S.; Feingold, G.

    2005-01-01

    A modelling study of vertical transport and processing of sulphate aerosol by a mixed-phase convective cloud, and the feedback of the cloud-processed aerosols on the development of cloud microphysical properties and precipitation is presented. An axisymmetric dynamic cloud model with bin-resolved microphysics and aqueousphase chemistry is developed and is used to examine the relative importance of microphysical and chemical processes on the aerosol budget, the fate of the aerosol material inside hydrometeors, and the size distributions of cloud-processed sulphate aerosols. Numerical simulations are conducted for a moderately deep convective cloud observed during the Cooperative Convective Precipitation Experiments. The results show that aerosol particles that have been transported from the boundary layer, detrained, and then re-entrained at midcloud levels account for a large fraction of the aerosol inside hydrometeors (~40% by mass). Convective transport by the simulated cloud enhances upper-tropospheric aerosol number and mass concentrations by factors of 2-3 and 3-4, respectively. Sensitivity studies suggest that, for the simulated case, aqueous chemistry does not modify the evolution of the cloud significantly. Finally, ice-phase hydrometeor development is very sensitive to aerosol concentrations at midcloud levels. The latter result suggests that the occurrence of mid-tropospheric aerosol layers that have been advected through long-range transport could strongly affect cloud microphysical processes and precipitation formation.

  4. Mixed-Symmetry States in ^96Mo

    NASA Astrophysics Data System (ADS)

    Lesher, S. R.; Bandyopadhyay, D.; Boukharouba, N.; Fransen, C.; Mynk, M.; McKay, C. J.; McEllistrem, M. T.; Yates, S. W.

    2003-10-01

    Mixed-symmetry states, a new class of low-lying collective excitations, are predicted by the neutron-proton version of the interacting boson model. The signatures for the 2^+_ms excitation in an even-even nucleus are a strong M1 transition to the first 2^+ state and a weak E2 transition to the ground state. Above the 2^+_ms state, the 2^+øtimes2^+_ms coupling will produce 2-phonon states, i.e., a 0^+, 1^+, 2^+, 3^+, 4^+ quintet. Extensive studies have been performed to identify these states in ^94Mo, which is thought to be well understood, and two other N=52 isotones, ^92Zr and ^96Ru. It is interesting to examine the collectivity of these excitations further from the closed N=50 shell. Therefore, we initiated a study of ^96_42Mo_54 using the (n,n^'γ) reaction at the University of Kentucky, including excitation function and angular distribution measurements, to search for these states. Lifetimes were measured using the Doppler-shift attenuation method, and B(E2) and B(M1) values were determined. This work was supported by the U.S. National Science Foundation under grant No. PHY-0098813.

  5. Local Optical Closure Using Single Particle Mixing State Observations during the 2010 DOE CARES Campaign

    NASA Astrophysics Data System (ADS)

    Zaveri, R. A.; Arnott, W. P.; Atkinson, D. B.; Barnard, J.; Beranek, J.; Cappa, C. D.; Chand, D.; Dubey, M. K.; Easter, R. C.; Flowers, B. A.; Gyawali, M. S.; Jobson, B. T.; Pekour, M. S.; Riemer, N. S.; Subramanian, R.; Song, C.; Zelenyuk, A.

    2011-12-01

    Atmospheric black carbon (BC) particles readily absorb both upwelling and downwelling broadband radiation and are thought to be second only to CO2 in contributing to global warming. However large uncertainties still exist in the global estimates of BC radiative forcing, which depend not only on our ability to accurately simulate the global loading and distribution of BC, but also on the precise knowledge of the mixing state and morphology of BC particles due to aging. To this end, one of the objectives of the Carbonaceous Aerosols and Radiative Effects Study (CARES) conducted in Sacramento, CA, during June 2010 was to investigate the evolution of urban BC particles and the associated optical properties, with the overarching goal of improving their process-level model representations. The daytime Sacramento urban plume was routinely transported to the northeast into the Sierra Nevada foothills area rich in biogenic emissions, and the aged aerosols were often recirculated back into the urban area the next morning. The CARES campaign observational strategy was designed to take advantage of this flow pattern by setting up two observation supersites - one located within the Sacramento urban area, referred to as the "T0 site," and another located about 24 km to the northeast in Cool, CA, a small town in the rural foothills area, referred to as the "T1 site." BC size distribution and mixing state were measured at both the sites with single particle soot photometry (SP2). The single particle mass spectrometer SPLAT II was also deployed at the T0 site to characterize the size, composition (mixing state), density, and morphology of BC and non-BC containing particles. Non-refractory aerosol species were measured by Aerodyne aerosol mass spectrometer (AMS). Aerosol light absorption and scattering (or extinction) at multiple wavelengths were measured using several techniques, including photoacoustic, cavity ring-down, nephelometer as well as the filter-based particle

  6. 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

  7. Entangled states close to the maximally mixed state

    SciTech Connect

    Hildebrand, Roland

    2007-06-15

    This paper deals with the radius of the largest ball of separable mixed states around the maximally mixed state for multiqubit systems. This radius determines how close entangled states can be to the maximally mixed state. In Aubrun and Szarek (e-print arXiv:quant-ph/0503221) an upper bound on the radius was given, while in Gurvits and Barnum (e-print arXiv:quant-ph/0409095) a lower bound was provided. In this paper we improve both the upper and the lower bound, bringing the ratio of these bounds down to a constant c={radical}(34/27){approx_equal}1.122, as opposed to a term of order {radical}(m log m) for the best bounds known previously, where m is the number of qubits in the system. We construct concrete examples of separable states on the boundary to entanglement which realize the upper bounds. As a by-product, we compute the radii of the largest balls that fit into the projective tensor product of three and four unit balls in R{sup 3} and in the projective tensor product of an arbitrary number of unit balls in R{sup n} for n=2, 4, and 8.

  8. 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

  9. Mixing state and compositional effects on CCN activity and droplet growth kinetics of size-resolved CCN in an urban environment

    NASA Astrophysics Data System (ADS)

    Padró, L. T.; Moore, R. H.; Zhang, X.; Rastogi, N.; Weber, R. J.; Nenes, A.

    2011-12-01

    Aerosol composition and mixing state near anthropogenic sources can be highly variable and can challenge predictions of cloud condensation nuclei (CCN). We present in-situ size-resolved CCN measurements to quantify this predictive uncertainty, which were carried out during the 2008 summertime August Mini Intensive Gas and Aerosol Study (AMIGAS) campaign in Atlanta, GA. Aerosol chemical composition was measured by two particle-into-liquid samplers measuring water-soluble inorganic ions and total water-soluble organic carbon. Size-resolved CCN data were collected using the Scanning Mobility CCN Analysis (SMCA) method and were used to obtain characteristic aerosol hygroscopicity distributions, whose breadth reflects the aerosol compositional variability and mixing state. We find that knowledge of aerosol mixing state is important for accurate predictions of CCN concentrations and that the influence of an externally-mixed, non-CCN-active aerosol fraction varies with size from 31% for particle diameters less than 40 nm to 93% for accumulation mode aerosol during the day. This is likely indicative of the interactions between biogenic and anthropogenic emissions which contribute to the formation and transformation of aerosols in this heterogeneous environment. Assuming size-dependent aerosol mixing state and size-invariant chemical composition decreased the average CCN concentration overprediction from greater than 50-200% to less than 20%. CCN activity was parameterized using a single hygroscopicity parameter, κ, which averaged 0.16 ± 0.07 for 80 nm particles and exhibited considerable variability (range: 0.03-0.48) throughout the study period.

  10. [Technic of studying microorganism viability in a simulated aerosol state on fiberglass microfilaments].

    PubMed

    Koniukhov, V F; Krasnozhenov, G G; Labushkin, Iu G; Olenichev, A V; Petrosov, V V

    1980-07-01

    A specially developed method of studying the viability of microorganisms in the simulated aerosol state on glass microfibers was used to show that the survival rate of E. coli and F. tularensis on fiber-glass spheres was similar to that in true aerosol, as observed in a static aerosol chamber. The proposed method allows to study the viability of microbial cells after prolonged existence in aerosol under any environmental condition both in open spaces and closed rooms. PMID:7001815

  11. 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.

  12. Quantum Correlations in Mixed-State Metrology

    NASA Astrophysics Data System (ADS)

    Modi, Kavan; Cable, Hugo; Williamson, Mark; Vedral, Vlatko

    2011-10-01

    We analyze the effects of quantum correlations, such as entanglement and discord, on the efficiency of phase estimation by studying four quantum circuits that can be readily implemented using NMR techniques. These circuits define a standard strategy of repeated single-qubit measurements, a classical strategy where only classical correlations are allowed, and two quantum strategies where nonclassical correlations are allowed. In addition to counting space (number of qubits) and time (number of gates) requirements, we introduce mixedness as a key constraint of the experiment. We compare the efficiency of the four strategies as a function of the mixedness parameter. We find that the quantum strategy gives N enhancement over the standard strategy for the same amount of mixedness. This result applies even for highly mixed states that have nonclassical correlations but no entanglement.

  13. Internally mixed soot, sulfates, and organic matter in aerosol particles from Mexico City

    NASA Astrophysics Data System (ADS)

    Adachi, K.; Buseck, P. R.

    2008-05-01

    Soot particles are major aerosol constituents that result from emissions of burning of fossil fuel and biomass. Because they both absorb sunlight and contribute to cloud formation, they are an influence on climate on local, regional, and global scales. It is therefore important to evaluate their optical and hygroscopic properties and those effects on the radiation budget. Those properties commonly change through reaction with other particles or gases, resulting in complex internal mixtures. Using transmission electron microscopy, we measured ~8000 particles (25 samples) with aerodynamic diameters from 0.05 to 0.3 μm that were collected in March 2006 from aircraft over Mexico City (MC) and adjacent areas. More than 50% of the particles consist of internally mixed soot, organic matter, and sulfate. Imaging combined with chemical analysis of individual particles show that many are coated, consist of aggregates, or both. Coatings on soot particles can amplify their light absorption, and coagulation with sulfates changes their hygroscopic properties, resulting in shorter lifetime. Our results suggest that a mixture of materials from multiple sources such as vehicles, power plants, and biomass burning occurs in individual particles, thereby increasing their complexity. Through changes in their optical and hygroscopic properties, internally mixed soot particles have a greater effect on the regional climate than uncoated soot particles. Moreover, soot occurs in more than 60% of all particles in the MC plumes, suggesting its important role in the formation of secondary aerosol particles.

  14. 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.

  15. 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.

  16. In vitro dissolution of respirable aerosols of industrial uranium and plutonium mixed-oxide nuclear fuels.

    PubMed

    Eidson, A F; Mewhinney, J A

    1983-12-01

    Dissolution characteristics of mixed-oxide nuclear fuels are important considerations for prediction of biological behavior of inhaled particles. Four representative industrial mixed-oxide powders were obtained from fuel fabrication enclosures. Studies of the dissolution of Pu, Am and U from aerosol particles of these materials in a serum simulant solution and in 0.1M HCl showed: (1) dissolution occurred at a rapid rate initially and slowed at longer times, (2) greater percentages of U dissolved than Pu or Am: with the dissolution rates of U and Pu generally reflecting the physical nature of the UO2-PuO2 matrix, (3) the temperature history of industrial mixed-oxides could not be reliably related to Pu dissolution except for a 3-5% increase when incorporated into a solid solution by sintering at 1750 degrees C, and (4) dissolution in the serum simulant agreed with the in vivo UO2 dissolution rate and suggested the dominant role of mechanical processes in PuO2 clearance from the lung. The rapid initial dissolution rate was shown to be related, in part, to an altered surface layer. The advantages and uses of in vitro solubility data for estimation of biological behavior of inhaled industrial mixed oxides, such as assessing the use of chelation therapy and interpretation of urinary excretion data, are discussed. It was concluded that in vitro solubility tests were useful, simple and easily applied to individual materials potentially inhaled by humans. PMID:6643070

  17. 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.

  18. 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

  19. 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

  20. 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.

  1. 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.

  2. 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.

  3. Source contributions to organic aerosol in the eastern United States

    NASA Astrophysics Data System (ADS)

    Lane, Timothy Edward

    emitted into the troposphere, has generally not been considered a major source of SOA due to the relatively high volatility of its oxidation products. The variability of the measured SOA yields in the available smog chamber studies is captured by combining the base case scenario with upper and lower bound estimates of the measurements. For the base case simulation, the predicted annual average isoprene SOA concentration in the southeast is 0.09 mug m-3 (bounds 0.04-0.23 mug m-3). PMCAMx predictions are compared to available measurements of some isoprene SOA components in North Carolina and New York State. These modeling results suggest that on an annual basis isoprene oxidation is a small but non-negligible organic aerosol source in the eastern U.S. Its contribution is relatively more important during the summer and in the southeast U.S. Afterward, an updated SOA module based on laboratory results from recent smog chamber experiments is implemented in PMCAMx. A new modeling framework is implemented based on the SOA volatility basis-set approach instead of the two-product approach used in existing models. The role of chemical aging is investigated by adding to the base case parameterization gas-phase reactions oxidizing the semi-volatile SOA compounds to lower volatility products. The predicted OA concentrations are compared to the available ambient measurements from the EPA Speciation Trends Network (STN) and the Interagency Monitoring of Protected Visual Environments (IMPROVE). The base case OA simulation slightly overpredicts the ambient measured OA concentrations at the rural IMPROVE sites with a bias of 0.33 mug m-3. The base case underpredicts the measured OA at urban STN sites but is performing significantly better than the two-product module in PMCAMx compared to observations. The contribution of biogenic and anthropogenic SOA to the predicted organic aerosol concentrations and the potential role of chemical aging are discussed. Finally, the secondary organic

  4. 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...

  5. Single biphoton ququarts as either pure or mixed states

    SciTech Connect

    Fedorov, M. V.; Volkov, P. A.; Mikhailova, J. M.

    2011-09-15

    We analyze features of mixed biphoton polarization states, which arise from pure states of polarization-frequency biphoton ququarts after averaging over frequencies of photons. For mixed states, we find their concurrence C, Schmidt parameter K, degree of polarization P, as well as the von Neumann mutual information I. In some simple cases, we also find the relative entropy S{sub rel} and the degree of classical correlations C{sub cl}. In mixed states, the Schmidt parameter does not characterize the degree of entanglement anymore, as it does in pure states. Nevertheless, the Schmidt parameter remains useful even in the case of mixed states because it remains directly related to the degree of polarization. We compare results occurring in the cases of full pure polarization-frequency states of ququarts and mixed states (averaged over frequencies). Differences between these results can be seen in experiments with and without frequency filters in front of a detector.

  6. Mixing of Asian dust with pollution aerosol and the transformation of aerosol components during the dust storm over China in spring 2007

    NASA Astrophysics Data System (ADS)

    Huang, Kan; Zhuang, Guoshun; Li, Juan; Wang, Qiongzhen; Sun, Yele; Lin, Yanfen; Fu, Joshua S.

    2010-04-01

    An intensive spring aerosol sampling campaign over northwestern and northern China and a megacity in eastern China was conducted in the spring of 2007 to investigate the mixing of Asian dust with pollution aerosol during its long-range transport. On the basis of the results of the three sites near dust source regions (Tazhong, Yulin, and Duolun) and a metropolitan city (Shanghai), three dust sources, i.e., the western high-Ca dust in the Taklimakan Desert, the northwestern high-Ca dust and the northeastern low-Ca dust in Mongolia Gobi, were identified on the basis of the air mass trajectories and the elemental tracer analysis (e.g., Ca/Al, SO42-/S, Ca2+/Ca, and Na+/Na). The western dust was least polluted in comparison to the other two dust sources. The results evidently indicated that the dust could have already mixed with pollution aerosol even in near dust source regions. The concentrations of As, Cd, Cu, Pb, Zn, and S were elevated several times at all sites during dust days, showing the entrainment of pollution elements by dust. The secondary SO42- was observed to show much higher concentration due to the heterogeneous reaction on the alkaline dust during dust storm, while the concentrations of NO3- and NH4+ decreased owing to the dilution of the local pollution by the invaded dust. The western dust contained relatively low anthropogenic aerosols, and it mainly derived from the Taklimakan Desert, a paleomarine source. The northwestern dust had a considerable chemical reactivity and mixing with sulfur precursors emitted from the coal mines on the pathway of the long-range transport of dust. The northeastern dust reached Shanghai with high acidity, and it became the mixed aerosol with the interaction among dust, local pollutants, and sea salts. Comparison of the speciation of the water-soluble ions on both nondust and dust days at all sites illustrated the evolution of major ion species from different dust sources during the long-range transport of dust. The

  7. 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

  8. 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.

  9. Investigating hygroscopic behavior and phase separation of organic/inorganic mixed phase aerosol particles with FTIR spectroscopy

    NASA Astrophysics Data System (ADS)

    Zawadowicz, M. A.; Cziczo, D. J.

    2013-12-01

    Atmospheric aerosol particles can be composed of inorganic salts, such as ammonium sulfate and sodium chloride, and therefore exhibit hygroscopic properties. Many inorganic salts have very well-defined deliquescence and efflorescence points at which they take up and lose water, respectively. For example, the deliquescence relative humidity of pure ammonium sulfate is about 80% and its efflorescence point is about 35%. This behavior of ammonium sulfate is important to atmospheric chemistry because some reactions, such as the hydrolysis of nitrogen pentoxide, occur on aqueous but not crystalline surfaces. Deliquescence and efflorescence of simple inorganic salt particles have been investigated by a variety of methods, such as IR spectroscopy, tandem mobility analysis and electrodynamic balance. Field measurements have shown that atmospheric aerosol are not typically a single inorganic salt, instead they often contain organic as well as inorganic species. Mixed inorganic/organic aerosol particles, while abundant in the atmosphere, have not been studied as extensively. Many recent studies have focused on microscopy techniques that require deposition of the aerosol on a glass slide, possibly changing its surface properties. This project investigates the deliquescence and efflorescence points, phase separation and ability to exchange gas-phase components of mixed organic and inorganic aerosol using a flow tube coupled with FTIR spectroscopy. Ammonium sulfate aerosol mixed with organic polyols with different O:C ratios, including glycerol, 1,2,6-hexanetriol, 1,4-butanediol and 1,5-pentanediol have been investigated. This project aims to study gas-phase exchange in these aerosol systems to determine if exchange is impacted when phase separation occurs.

  10. Mixing state and compositional effects on CCN activity and droplet growth kinetics of size-resolved CCN in an urban environment

    NASA Astrophysics Data System (ADS)

    Padró, L. T.; Moore, R. H.; Zhang, X.; Rastogi, N.; Weber, R. J.; Nenes, A.

    2012-11-01

    Aerosol composition and mixing state near anthropogenic sources can be highly variable and can challenge predictions of cloud condensation nuclei (CCN). The impacts of chemical composition on CCN activation kinetics is also an important, but largely unknown, aspect of cloud droplet formation. Towards this, we present in-situ size-resolved CCN measurements carried out during the 2008 summertime August Mini Intensive Gas and Aerosol Study (AMIGAS) campaign in Atlanta, GA. Aerosol chemical composition was measured by two particle-into-liquid samplers measuring water-soluble inorganic ions and total water-soluble organic carbon. Size-resolved CCN data were collected using the Scanning Mobility CCN Analysis (SMCA) method and were used to obtain characteristic aerosol hygroscopicity distributions, whose breadth reflects the aerosol compositional variability and mixing state. Knowledge of aerosol mixing state is important for accurate predictions of CCN concentrations and that the influence of an externally-mixed, CCN-active aerosol fraction varies with size from 31% for particle diameters less than 40 nm to 93% for accumulation mode aerosol during the day. Assuming size-dependent aerosol mixing state and size-invariant chemical composition decreases the average CCN concentration overprediction (for all but one mixing state and chemical composition scenario considered) from over 190-240% to less than 20%. CCN activity is parameterized using a single hygroscopicity parameter, κ, which averages to 0.16 ± 0.07 for 80 nm particles and exhibits considerable variability (from 0.03 to 0.48) throughout the study period. Particles in the 60-100 nm range exhibited similar hygroscopicity, with a κ range for 60 nm between 0.06-0.076 (mean of 0.18 ± 0.09). Smaller particles (40 nm) had on average greater κ, with a range of 0.20-0.92 (mean of 0.3 ± 0.12). Analysis of the droplet activation kinetics of the aerosol sampled suggests that most of the CCN activate as rapidly as

  11. 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.

  12. 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

  13. 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

  14. Changes of ns-soot mixing states and shapes in an urban area during CalNex

    NASA Astrophysics Data System (ADS)

    Adachi, Kouji; Buseck, Peter R.

    2013-05-01

    Aerosol particles from megacities influence the regional and global climate as well as the health of their occupants. We used transmission electron microscopes (TEMs) to study aerosol particles collected from the Los Angeles area during the 2010 CalNex campaign. We detected major amounts of ns-soot, defined as consisting of carbon nanospheres, sulfate, sea salt, and organic aerosol (OA) and lesser amounts of brochosome particles from leaf hoppers. Ns-soot-particle shapes, mixing states, and abundances varied significantly with sampling times and days. Within plumes having high CO2 concentrations, much ns-soot was compacted and contained a relatively large number of carbon nanospheres. Ns-soot particles from both CalNex samples and Mexico City, the latter collected in 2006, had a wide range of shapes when mixed with other aerosol particles, but neither sets showed spherical ns-soot nor the core-shell configuration that is commonly used in optical calculations. Our TEM observations and light-absorption calculations of modeled particles indicate that, in contrast to ns-soot particles that are embedded within other materials or have the hypothesized core-shell configurations, those attached to other aerosol particles hardly enhance their light absorption. We conclude that the ways in which ns-soot mixes with other particles explain the observations of smaller light amplification by ns-soot coatings than model calculations during the CalNex campaign and presumably in other areas.

  15. In situ measurement of cloud condensation nuclei activation of black carbon particles in dependence of their mixing state

    NASA Astrophysics Data System (ADS)

    Gysel, M.; Laborde, M.; Bukowiecki, N.; Juranyi, Z.; Hammer, E.; Zieger, P.; Baltensperger, U.; Weingartner, E.

    2012-12-01

    Black carbon (BC) emitted from combustion sources is the major absorbing component of atmospheric aerosols. The Earth's climate can be influenced by BC particles in several ways, e.g. through absorption of solar radiation or through decreasing the surface albedo of glaciers due to deposited BC particles. Cloud droplets only form on cloud condensation nuclei (CCN). The CCN activation behaviour of BC particles is important for their atmospheric life cycle as wet removal is an important sink. Several laboratory and field studies have shown that BC is less hygroscopic and less CCN active than inorganic or water-soluble organic aerosol components. The goal of this study was to investigate the CCN activation behaviour of BC-containing particles in dependence of their mixing state and compared to non-BC containing particles. In situ measurements of the cloud droplet activation behaviour of aerosol particles were done in winter 2010 at the high-alpine research station Jungfraujoch (3580 m asl), Switzerland. Two different inlets were employed during cloud episodes to selectively collect the interstitial aerosol (all particles that did not form cloud droplets) as well as the total aerosol (interstitial aerosol plus cloud droplet residuals). Both types of aerosol samples were characterized using a Single Particle Soot Photometer (SP2), providing quantitative measurement of BC mass in individual particles as well as information on the mixing state of BC, and further aerosol measurement techniques. Outdoor measurements of microphysical cloud properties were also available. Comparison of the aerosol samples from the interstitial and total inlets makes it possible to determine the properties of the CCN active aerosol as opposed to the interstitial aerosol. The analysis of several cloud events revealed that coated BC particles are more readily activated to CCN compared to uncoated BC particles with equal BC mass. This can actually be expected even for non-hygroscopic coatings due

  16. Aerosol Processing in Mixed-Phase Clouds in ECHAM5-HAM: Comparison of Single-Column Model Simulations to Observations

    NASA Astrophysics Data System (ADS)

    Hoose, C.; Lohmann, U.; Stier, P.; Verheggen, B.; Weingartner, E.; Herich, H.

    2007-12-01

    The global aerosol-climate model ECHAM5-HAM (Stier et al., 2005) has been extended by an explicit treatment of cloud-borne particles. Two additional modes for in-droplet and in-crystal particles are introduced, which are coupled to the number of cloud droplet and ice crystal concentrations simulated by the ECHAM5 double-moment cloud microphysics scheme (Lohmann et al., 2007). Transfer, production and removal of cloud-borne aerosol number and mass by cloud droplet activation, collision scavenging, aqueous-phase sulfate production, freezing, melting, evaporation, sublimation and precipitation formation are taken into account. The model performance is demonstrated and validated with observations of the evolution of total and interstitial aerosol concentrations and size distributions during three different mixed-phase cloud events at the alpine high-altitude research station Jungfraujoch (Switzerland) (Verheggen et al, 2007). Although the single-column simulations can not be compared one-to-one with the observations, the governing processes in the evolution of the cloud and aerosol parameters are captured qualitatively well. High scavenged fractions are found during the presence of liquid water, while the release of particles during the Bergeron-Findeisen process results in low scavenged fractions after cloud glaciation. The observed coexistence of liquid and ice, which might be related to cloud heterogeneity at subgrid scales, can only be simulated in the model when forcing non-equilibrium conditions. References: U. Lohmann et al., Cloud microphysics and aerosol indirect effects in the global climate model ECHAM5-HAM, Atmos. Chem. Phys. 7, 3425-3446 (2007) P. Stier et al., The aerosol-climate model ECHAM5-HAM, Atmos. Chem. Phys. 5, 1125-1156 (2005) B. Verheggen et al., Aerosol partitioning between the interstitial and the condensed phase in mixed-phase clouds, Accepted for publication in J. Geophys. Res. (2007)

  17. 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.

  18. 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.

  19. 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

  20. Sub-Planck structure in a mixed state

    NASA Astrophysics Data System (ADS)

    Kumari, Asmita; Pan, Alok Kumar; Panigrahi, Prasanta K.

    2015-11-01

    The persistence of sub-Planck structure in phase space with loss of coherence is demonstrated in a mixed state, which comprises two terms in the density matrix. Its utility in carrying out Heisenberg-limited measurement and quantum parameter estimation have been shown. It is also shown that the mixed state performs equally well as the compass state for carrying out precision measurements. The advantage of using mixed state relies on the fact that such a state can be easier to prepare and may appear from pure states after partial loss of coherence. We explicate the effect of environment on these sub-Planck structures in the mixed state and estimates the time scale of complete decoherence.

  1. 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.

  2. Aerosol black carbon characteristics over Central India: Temporal variation and its dependence on mixed layer height

    NASA Astrophysics Data System (ADS)

    Kompalli, Sobhan Kumar; Babu, S. Suresh; Moorthy, K. Krishna; Manoj, M. R.; Kumar, N. V. P. Kiran; Shaeb, K. Hareef Baba; Joshi, Ashok Kumar

    2014-10-01

    In a first of its kind study over the Indian region, concurrent and extensive measurements of black carbon (BC) concentration and atmospheric boundary layer parameters are used to quantify the role of atmospheric boundary layer in producing temporal changes in BC. During this study, 18 months (2011-12) data of continuous measurements of BC aerosols, made over a semi-urban location, Nagpur, in Central India are used along with concurrent measurements of vertical profiles of atmospheric thermodynamics, made using weekly ascents of GPS aided Radiosonde for a period of 1 year. From the balloon data, mixed layer heights and ventilation coefficients are estimated, and the monthly and seasonal changes in BC mass concentration are examined in the light of the boundary layer changes. Seasonally, the BC mass concentration was highest (~ 4573 ± 1293 ng m- 3) in winter (December-February), and lowest (~ 1588 ± 897 ng m- 3) in monsoon (June-September), while remained moderate (~ 3137 ± 1446 ng m- 3) in pre-monsoon (March-May), and post-monsoon (~ 3634 ± 813 ng m- 3) (October-November) seasons. During the dry seasons, when the rainfall is scanty or insignificantly small, the seasonal variations in BC concentrations have a strong inverse relationship with mixed layer height and ventilation coefficient. However, the lowest BC concentrations do not occur during the season when the mixed layer height (MLH) is highest or the ventilation coefficient is the highest; rather it occurs when the rainfall is strong (during summer monsoon season) and airmass changes to primarily of marine origin.

  3. Cardiogenic mixing increases aerosol deposition in the human lung in the absence of gravity

    PubMed Central

    Prisk, G. Kim; Sá, Rui Carlos; Darquenne, Chantal

    2012-01-01

    Rationale Exposure to extraterrestrial dusts is an almost inevitable consequence of any proposed planetary exploration. Previous studies in humans showed reduced deposition in low-gravity compared with normal gravity (1G). However, the reduced sedimentation means that fewer particles deposit in the airways, increasing the number of particles transported to the lung periphery where they eventually deposit albeit at a smaller rate than in 1G. In this study, we determined the role that gravity and other mechanisms such as cardiogenic mixing play in peripheral lung deposition during breath holds. Methods Eight healthy subjects inhaled boluses of 0.5 μm-diameter particles to penetration volumes (Vp) of 300 and 1200ml that were followed by breath holds of up to 10 sec. Tests were performed in 1G and during short periods of microgravity (μG) aboard the NASA Microgravity Research Aircraft. Aerosol deposition and dispersion were calculated from these data. Results Results show that, for both Vp, deposition in 1G was significantly higher than in μG. In contrast, while dispersion was significantly higher in 1G compared to μG at Vp=1200ml, there was no significant gravitational effect on dispersion at Vp=300ml. Finally, for each G level and Vp, deposition and dispersion significantly increased with increasing breath-hold time. Conclusion The most important finding of this study is that, even in the absence of gravity, aerosol deposition in the lung periphery increased with increasing residence time. Because the particles used in this study were too large to be significantly affected by Brownian diffusion, the increase in deposition is likely due to cardiogenic motion effects. PMID:23976801

  4. 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.

  5. New ARM Measurements of Clouds, Aerosols, and the Atmospheric State

    NASA Astrophysics Data System (ADS)

    Mather, J.

    2012-04-01

    The DOE Atmospheric Radiation Measurement (ARM) program has recently enhanced its observational capabilities at its fixed and mobile sites as well as its aerial facility. New capabilities include scanning radars, several types of lidars, an array of aerosol instruments, and in situ cloud probes. All ARM sites have been equipped with dual frequency scanning cloud radars that will provide three-dimensional observations of cloud fields for analysis of cloud field evolution. Sites in Oklahoma, Alaska, and Papua New Guinea have also received scanning centimeter wavelength radars for observing precipitation fields. This combination of radars will provide the means to study the interaction of clouds and precipitation. New lidars include a Raman lidar in Darwin, Australia and High Spectral Resolution Lidars in Barrow and with the second ARM Mobile Facility. Each of these lidars will provide profiles of aerosol extinction while the Raman will also measure profiles of water vapor. ARM has also expanded its capabilities in the realm of aerosol observations. ARM is adding Aerosol Observing Systems to its sites in Darwin and the second mobile facility. These aerosol systems principally provided measurements of aerosol optical properties. In addition, a new Mobile Aerosol Observing System has been developed that includes a variety of instruments to provide information about aerosol chemistry and size distributions. Many of these aerosol instruments are also available for the ARM Aerial Facility. The Aerial Facility also now includes a variety of cloud probes for measuring size distribution and water content. The new array of ARM instruments is intended to build upon the existing ARM capabilities to better study the interactions among aerosol, clouds, and precipitation. Data from these instruments are now available and development of advanced data products is underway.

  6. Grover's quantum search algorithm for an arbitrary initial mixed state

    SciTech Connect

    Biham, Eli; Kenigsberg, Dan

    2002-12-01

    The Grover quantum search algorithm is generalized to deal with an arbitrary mixed initial state. The probability to measure a marked state as a function of time is calculated, and found to depend strongly on the specific initial state. The form of the function, though, remains as it is in the case of initial pure state. We study the role of the von Neumann entropy of the initial state, and show that the entropy cannot be a measure for the usefulness of the algorithm. We give few examples and show that for some extremely mixed initial states (carrying high entropy), the generalized Grover algorithm is considerably faster than any classical algorithm.

  7. Retrieval of CO2 Mixing Ratios from CLARS Measurements: Correcting Aerosol Induced Biases

    NASA Astrophysics Data System (ADS)

    Zhang, Q.; Natraj, V.; Shia, R. L.; Roehl, C. M.; Yung, Y. L.; Sander, S. P.

    2014-12-01

    A Fourier transform spectrometer at the California Laboratory for Atmospheric Remote Sensing (CLARS) on the top of Mt Wilson, California, measures greenhouse gas concentrations in the Los Angeles basin using reflected sun light. Observations include those with large viewing zenith angles (up to 83.1), making the measurements very sensitive to aerosol scattering. A previous study by the authors shows the ratioing of CO2 and O2 slant column densities (SCDs) can largely cancel the effect of aerosol scattering, but biases still exist due to the wavelength dependence of aerosol scattering.In this study, biases caused by different types of aerosols are analyzed. Preliminary results indicate that the information from CLARS-FTS spectra is not sufficient to constrain all the free parameters, including the aerosol single scattering albedo (SSA), aerosol optical depth, surface albedo, etc. In order to mitigate the influence of aerosol scattering, a few effective aerosol parameters are retrieved simultaneously with absorbing gas abundances. The corrected SCDs show reasonable variabilities from the morning to the afternoon in the presence of aerosols. The column-averaged dry air mole fraction of CO2 (XCO2) products are compared to measurements from the Total Carbon Column Observing Network (TCCON) at Caltech. By retrieving aerosol parameters in the CO2 and O2 absorption bands, biases in XCO2 caused by wavelength dependence of aerosol scattering can be considerably reduced.

  8. 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.

  9. Mixing state of individual submicron carbon-containing particles and their seasonal variation in urban Guangzhou, China

    NASA Astrophysics Data System (ADS)

    Zhang, G.; Bi, X.; Li, L.; Chan, L. Y.; Li, M.; Wang, X.; Sheng, G.; Fu, J.; Zhou, Z.

    2012-12-01

    Growing evidence suggests that size-resolved mixing state of carbon-containing particles is very critical in determining their optical properties, atmospheric lifetime, and impact on the environment. However, still little is known about the mixing state of particles in urban area of Pearl River Delta (PRD) region, China. To investigate the mixing state of submicron carbon-containing particles, measurements were carried out during spring and fall periods of 2010 using a single particle aerosol mass spectrometer (SPAMS). Approximate 700 000 particles for each period were detected. This is the first report on the size-resolved mixing state of carbon-containing particles by direct observations in PRD region. Cluster analysis of single particle mass spectra was applied to identify carbon-containing particle classes. These classes represented ~80% and ~90% of all the detected particles for spring and fall periods, respectively. Carbon-containing particle classes mainly consisted of biomass/biofuel burning particles (Biomass), organic carbon (OC), fresh elemental carbon (EC-fresh), internally mixed OC and EC (ECOC), internally mixed EC with sulfate (EC-Sulfate), vanadium-containing ECOC (V-ECOC), and amines-containing particles (Amine). In spring, the top three ranked carbon-containing particle classes were ECOC (26.1%), Biomass (23.6%) and OC (10%), respectively. However, the fraction of Biomass particles increased remarkably and predominated (61.0%), while the fraction of ECOC (3.0%) and V-ECOC (0.1%) significantly decreased in fall. To highlight the influence of monsoon on the properties of carbon-containing particles in urban Guangzhou, their size distribution, mixing state, and aerosol acidity were compared between spring and fall seasons. In addition, a case study was also performed to investigate how the formation of fog and haze influenced the mixing state of carbon-containing particles. These results are of importance in understanding atmospheric chemistry and

  10. 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

  11. Mixed-state sensitivity of several quantum-information benchmarks

    SciTech Connect

    Peters, Nicholas A.; Wei, T.-C.; Kwiat, Paul G.

    2004-11-01

    We investigate an imbalance between the sensitivity of the common state measures - fidelity, trace distance, concurrence, tangle, von Neumann entropy, and linear entropy - when acted on by a depolarizing channel. Further, in this context we explore two classes of two-qubit entangled mixed states. Specifically, we illustrate a sensitivity imbalance between three of these measures for depolarized (i.e., Werner-state-like) nonmaximally entangled and maximally entangled mixed states, noting that the size of the imbalance depends on the state's tangle and linear entropy.

  12. 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.

  13. A Classification of Correlations of Tripartite Mixed States

    NASA Astrophysics Data System (ADS)

    Guo, Zhihua; Cao, Huaixin

    2013-06-01

    To obtain a classification of correlations of tripartite mixed states, various correlated states are introduced by using measurement-induced disturbance, including CCC, QC, GQC, CCX, CXC, XCC, CXX, XCX and XXC-states. Standard forms of them are established and equivalent characterizations of them are obtained in terms of normality and commutativity of the associated component operators.

  14. Uncertainty, entropy, and non-Gaussianity for mixed states

    NASA Astrophysics Data System (ADS)

    Mandilara, Aikaterini; Karpov, Evgueni; Cerf, Nicolas J.

    2010-06-01

    In the space of mixed states the Schrödinger-Robertson uncertainty relation holds though it can never be saturated. Two tight extensions of this relation in the space of mixed states exist; one proposed by Dodonov and Man'ko, where the lower limit on the uncertainty depends on the purity of the state, and another where the uncertainty is bounded by the von Neumann entropy of the state proposed by Bastiaans. Driven by the needs that have emerged in the field of quantum information, in a recent work we have extended the puritybounded uncertainty relation by adding an additional parameter characterizing the state, namely its degree of non-Gaussianity. In this work we alternatively present a extension of the entropy-bounded uncertainty relation. The common points and differences between the two extensions of the uncertainty relation help us to draw more general conclusions concerning the bounds on the non-Gaussianity of mixed states.

  15. Mixed-mode oscillation suppression states in coupled oscillators

    NASA Astrophysics Data System (ADS)

    Ghosh, Debarati; Banerjee, Tanmoy

    2015-11-01

    We report a collective dynamical state, namely the mixed-mode oscillation suppression state where the steady states of the state variables of a system of coupled oscillators show heterogeneous behaviors. We identify two variants of it: The first one is a mixed-mode death (MMD) state, which is an interesting oscillation death state, where a set of variables show dissimilar values, while the rest arrive at a common value. In the second mixed death state, bistable and monostable nontrivial homogeneous steady states appear simultaneously to a different set of variables (we refer to it as the MNAD state). We find these states in the paradigmatic chaotic Lorenz system and Lorenz-like system under generic coupling schemes. We identify that while the reflection symmetry breaking is responsible for the MNAD state, the breaking of both the reflection and translational symmetries result in the MMD state. Using a rigorous bifurcation analysis we establish the occurrence of the MMD and MNAD states, and map their transition routes in parameter space. Moreover, we report experimental observation of the MMD and MNAD states that supports our theoretical results. We believe that this study will broaden our understanding of oscillation suppression states; subsequently, it may have applications in many real physical systems, such as laser and geomagnetic systems, whose mathematical models mimic the Lorenz system.

  16. 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.

  17. Measurement of Optical Properties of Organic and Mixed Organic/ Inorganic Laboratory Aerosols at Relative Humidities between 8 and 95%

    NASA Astrophysics Data System (ADS)

    Brem, B.; Mena, F. C.; Chen, Y.; Bond, T. C.; Rood, M. J.

    2011-12-01

    Relative humidity (RH) affects the liquid water content of an aerosol, altering its scattering and absorption of visible light, which is important for aerosol effects on visibility and climate. Particle light extinction, light scattering and light absorption coefficient values are reported here for laboratory-generated inorganic and organic carbon (OC) aerosols at RH values between 8% and 95%. Light scattering was measured with a nephelometer, light extinction was measured with an extinction cell and light absorption was determined based on the difference between those two values at three visible wavelengths (467 nm, 530 nm and 660 nm). The instrumentation was benchmarked with non-absorbing ammonium sulfate, absorbing polystyrene microspheres (PSMs) and absorbing nigrosin aerosol under controlled RH conditions. Agreement between dry measured scattering and extinction coefficients for ammonium sulfate was achieved within 3%. Optical closure with modeled scattering values based on measured ammonium sulfate particle size distributions was achieved within 7%. Measured single scattering albedo for dry absorbing PSMs agreed within 0.02 with the literature value. Light absorption by nigrosin increased by a factor of 1.24 +/-0.06 at all wavelengths as RH increased from 38 to 95%. Light absorption of OC aerosol that was generated from wood pyrolysis demonstrated enhancements of 2.2 +/- 0.7 and 2.7 +/- 1.2 between 32 and 95% RH at the wavelengths of 467 and 530 nm, but no absorption was detected at 660 nm. A spectral dependence of light absorption by OC was observed with absorption increasing from 530 nm towards the 467 nm wavelength, consistent with previously reported ex situ measurements of filter extracts. Current work focuses on the measurement of optical properties as a function of RH for OC wood pyrolysis aerosol mixed with ammonium sulfate. Additionally optical closure is evaluated between measured and modeled results.

  18. 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.

  19. 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.

  20. 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.

  1. Effect of small flow reversals on aerosol mixing in the alveolar region of the human lung.

    PubMed

    Darquenne, Chantal; Prisk, G Kim

    2004-12-01

    It has been suggested that irreversibility of alveolar flow combined with a stretched and folded pattern of streamlines can lead to a sudden increase in mixing in the lung. To determine whether this phenomenon is operative in the human lung in vivo, we performed a series of bolus studies with a protocol designed to induce complex folding patterns. Boli of 0.5- and 1-microm-diameter particles were inhaled at penetration volumes (V(p)) of 300 and 1,200 ml in eight subjects during short periods of microgravity aboard the National Aeronautics and Space Administration Microgravity Research Aircraft. Inspiration was from residual volume to 1 liter above 1 G functional residual capacity. This was followed by a 10-s breathhold, during which up to seven 100-ml flow reversals (FR) were imposed at V(p) = 300 ml and up to four 500-ml FR at V(p) = 1,200 ml, and by an expiration to residual volume. Bolus dispersion and deposition were calculated from aerosol concentration and flow rate continuously monitored at the mouth. There was no significant increase in dispersion and deposition with increasing FR except for dispersion between 0 and 7 FR at V(p) = 300 ml with 0.5-microm-diameter particles, and this increase was small. This suggested that either the phenomenon of stretch and fold did not occur within the number of FR we performed or that it had already occurred during the one breathing cycle included in the basic maneuver. We speculate that the phenomenon occurred during the basic maneuver, which is consistent with the high degree of dispersion and deposition observed previously in microgravity. PMID:15298988

  2. Hygroscopicity of organic compounds from biomass burning and their influence on the water uptake of mixed organic ammonium sulfate aerosols

    NASA Astrophysics Data System (ADS)

    Lei, T.; Zuend, A.; Wang, W. G.; Zhang, Y. H.; Ge, M. F.

    2014-10-01

    Hygroscopic behavior of organic compounds, including levoglucosan, 4-hydroxybenzoic acid, and humic acid, as well as their effects on the hygroscopic properties of ammonium sulfate (AS) in internally mixed particles are studied by a hygroscopicity tandem differential mobility analyzer (HTDMA). The organic compounds used represent pyrolysis products of wood that are emitted from biomass burning sources. It is found that humic acid aerosol particles only slightly take up water, starting at RH (relative humidity) above ~70%. This is contrasted by the continuous water absorption of levoglucosan aerosol particles in the range 5-90% RH. However, no hygroscopic growth is observed for 4-hydroxybenzoic acid aerosol particles. Predicted water uptake using the ideal solution theory, the AIOMFAC model and the E-AIM (with UNIFAC) model are consistent with measured hygroscopic growth factors of levoglucosan. However, the use of these models without consideration of crystalline organic phases is not appropriate to describe the hygroscopicity of organics that do not exhibit continuous water uptake, such as 4-hydroxybenzoic acid and humic acid. Mixed aerosol particles consisting of ammonium sulfate and levoglucosan, 4-hydroxybenzoic acid, or humic acid with different organic mass fractions, take up a reduced amount of water above 80% RH (above AS deliquescence) relative to pure ammonium sulfate aerosol particles of the same mass. Hygroscopic growth of mixtures of ammonium sulfate and levoglucosan with different organic mass fractions agree well with the predictions of the thermodynamic models. Use of the Zdanovskii-Stokes-Robinson (ZSR) relation and AIOMFAC model lead to good agreement with measured growth factors of mixtures of ammonium sulfate with 4-hydroxybenzoic acid assuming an insoluble organic phase. Deviations of model predictions from the HTDMA measurement are mainly due to the occurrence of a microscopical solid phase restructuring at increased humidity (morphology

  3. Aerosol processing in mixed-phase clouds in ECHAM5-HAM: Model description and comparison to observations

    NASA Astrophysics Data System (ADS)

    Hoose, C.; Lohmann, U.; Stier, P.; Verheggen, B.; Weingartner, E.

    2008-04-01

    The global aerosol-climate model ECHAM5-HAM has been extended by an explicit treatment of cloud-borne particles. Two additional modes for in-droplet and in-crystal particles are introduced, which are coupled to the number of cloud droplet and ice crystal concentrations simulated by the ECHAM5 double-moment cloud microphysics scheme. Transfer, production, and removal of cloud-borne aerosol number and mass by cloud droplet activation, collision scavenging, aqueous-phase sulfate production, freezing, melting, evaporation, sublimation, and precipitation formation are taken into account. The model performance is demonstrated and validated with observations of the evolution of total and interstitial aerosol concentrations and size distributions during three different mixed-phase cloud events at the alpine high-altitude research station Jungfraujoch (Switzerland). Although the single-column simulations cannot be compared one-to-one with the observations, the governing processes in the evolution of the cloud and aerosol parameters are captured qualitatively well. High scavenged fractions are found during the presence of liquid water, while the release of particles during the Bergeron-Findeisen process results in low scavenged fractions after cloud glaciation. The observed coexistence of liquid and ice, which might be related to cloud heterogeneity at subgrid scales, can only be simulated in the model when assuming nonequilibrium conditions.

  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. 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

  6. Influence of mineral dust mixing-state and reaction probabilities on size-resolved sulfate formation in Northeast Asia

    NASA Astrophysics Data System (ADS)

    Song, C. H.; Nam, J. E.; Han, K. M.; Lee, M. K.; Woo, J. H.; Han, J. S.

    2012-10-01

    Significant differences were found between two particulate sulfate size-distributions measured using a MOUDI impactor at Gosan, Jeju Island, Korea, and simulated via the Lagrangian photochemical model under a condition of aerosol internal mixing between mineral dust and urban pollution particles. It was suspected that these differences might have resulted from: (1) the assumption of aerosol internal mixing and (2) the uses of identical reaction probabilities (γ) of the gaseous sulfate precursors (SO2 and H2SO4) onto both urban pollution particles and mineral dust in the Lagrangian photochemical model simulations. In this study; therefore, some cases of aerosol external mixing between urban-derived pollution aerosols and mineral dust were investigated, with different magnitudes of γ for the gas-phase sulfate precursors onto the two different condensing media. The model simulations under the external mixing condition, with different magnitudes of the reaction probabilities (γi,urban and γi,dust) onto urban pollution particles and mineral dust, successfully reproduced the size-dependent particulate sulfate formation measured at the Gosan station. Further attempts were made to approximate the magnitudes of γSO2,urban and γH2SO4,dust under external mixing state conditions with the fixed γSO2,dust and γH2SO2,urban values of 10-4 and 1.0. The best-estimates of γSO2,urban and γH2SO4,dust found in this study were in the orders of 10-4-10-5 and 10-2-10-3, respectively.

  7. Entanglement under restricted operations: Analogy to mixed-state entanglement

    SciTech Connect

    Bartlett, Stephen D.; Doherty, Andrew C.; Spekkens, Robert W.; Wiseman, H. M.

    2006-02-15

    We show that the classification of bipartite pure entangled states when local quantum operations are restricted yields a structure that is analogous in many respects to that of mixed-state entanglement. Specifically, we develop this analogy by restricting operations through local superselection rules, and show that such exotic phenomena as bound entanglement and activation arise using pure states in this setting. This analogy aids in resolving several conceptual puzzles in the study of entanglement under restricted operations. In particular, we demonstrate that several types of quantum optical states that possess confusing entanglement properties are analogous to bound entangled states. Also, the classification of pure-state entanglement under restricted operations can be much simpler than for mixed-state entanglement. For instance, in the case of local Abelian superselection rules all questions concerning distillability can be resolved.

  8. 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.

  9. 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.

  10. Ergodicity, mixing, and time reversibility for atomistic nonequilibrium steady states

    SciTech Connect

    Hoover, W.G.; Kum, O.

    1997-11-01

    Ergodic mixing is prerequisite to any statistical-mechanical calculation of properties derived from atomistic dynamical simulations. Thus the time-reversible thermostats and ergostats used in simulating Gibbsian equilibrium dynamics or nonequilibrium steady-state dynamics should impose ergodicity and mixing. Though it is hard to visualize many-dimensional phase-space distributions, recent developments provide several practical numerical approaches to the problem of ergodic mixing. Here we apply three of these approaches to a useful nonequilibrium test problem, an oscillator in a temperature gradient. {copyright} {ital 1997} {ital The American Physical Society}

  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. 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.

  13. Non-refractory Submicron Aerosol Aging Processes in the Rural Southeastern United States

    NASA Astrophysics Data System (ADS)

    Karakurt Cevik, B.; Leong, Y. J.; Hernandez, C.; Griffin, R. J.

    2014-12-01

    The Southern Oxidant and Aerosol Study (SOAS) took place over a six-week period and included ground and elevated measurements that aimed to improve the understanding of biosphere-atmosphere interactions and their impacts on air quality and climate. As part of SOAS, an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed at the rural ground site in Centreville, AL, from 1 June to 15 July 2013. The HR-ToF-AMS provided quantitative measurement of non-refractory submicron aerosol composition and size distribution with high temporal resolution. Time series of mass concentrations of organic material, sulfate, ammonium, and nitrate (in order of average relative importance) and the changes in the concentrations of each component with respect to a photochemical airmass age metric (based on oxidation of nitrogen oxides) are reported. The relative importance of secondary ammonium and sulfate increases with values of the airmass age metric. While the contributions of organic and nitrate aerosol to total particle concentration decrease with increasing airmass age, organic aerosol concentration normalized by carbon monoxide (CO) constantly increases with age. However, the nitrate concentration normalized by CO appears relatively independent of the age metric. For a better understanding of organic aerosol processing, atomic ratio (oxygen/carbon and hydrogen/carbon) and carbon oxidation state (OSc) analyses of bulk organic aerosol are investigated.

  14. 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.

  15. Operational entanglement families of symmetric mixed N -qubit states

    NASA Astrophysics Data System (ADS)

    Bastin, T.; Mathonet, P.; Solano, E.

    2015-02-01

    We introduce an operational entanglement classification of symmetric mixed states for an arbitrary number of qubits based on stochastic local operations assisted with classical communication (SLOCC operations). We define families of SLOCC entanglement classes successively embedded into each other, we prove that they are of nonzero measure, and we construct witness operators to distinguish them. Moreover, we discuss how arbitrary symmetric mixed states can be realized in the laboratory via a one-to-one correspondence between well-defined sets of controllable parameters and the corresponding entanglement families.

  16. 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.

  17. 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.

  18. 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

  19. 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 ...

  20. A sea spray aerosol flux parameterization encapsulating wave state

    NASA Astrophysics Data System (ADS)

    Ovadnevaite, J.; Manders, A.; de Leeuw, G.; Ceburnis, D.; Monahan, C.; Partanen, A.-I.; Korhonen, H.; O'Dowd, C. D.

    2014-02-01

    A new sea spray source function (SSSF), termed Oceanflux Sea Spray Aerosol or OSSA, was derived based on in-situ sea spray aerosol measurements along with meteorological/physical parameters. Submicron sea spray aerosol fluxes derived from particle number concentration measurements at the Mace Head coastal station, on the west coast of Ireland, were used together with open-ocean eddy correlation flux measurements from the Eastern Atlantic Sea Spray, Gas Flux, and Whitecap (SEASAW) project cruise. In the overlapping size range, the data for Mace Head and SEASAW were found to be in a good agreement, which allowed deriving the new SSSF from the combined dataset spanning the dry diameter range from 15 nm to 6 μm. The OSSA source function has been parameterized in terms of five lognormal modes and the Reynolds number instead of the more commonly used wind speed, thereby encapsulating important influences of wave height, wind history, friction velocity, and viscosity. This formulation accounts for the different flux relationships associated with rising and waning wind speeds since these are included in the Reynolds number. Furthermore, the Reynolds number incorporates the kinematic viscosity of water, thus the SSSF inherently includes dependences on sea surface temperature and salinity. The temperature dependence of the resulting SSSF is similar to that of other in-situ derived source functions and results in lower production fluxes for cold waters and enhanced fluxes from warm waters as compared with SSSF formulations that do not include temperature effects.

  1. Modeling of Biomass Burning Aerosols over Southeastern United States

    NASA Astrophysics Data System (ADS)

    Ivey, C.; Lavoue, D.; Davis, A.; Hu, Y.; Russell, A. G.

    2014-12-01

    The U.S. National Emissions Inventory (NEI) for area sources such as biomass burning have uncertainties in temporal variability due to temporal averaging of the final inventories. The Fire Inventory of NCAR (FINN) provides detailed emissions estimates of gaseous and aerosol emissions from individual wildland, prescribed, and open fires over North America. In an effort to improve PM2.5 source impact estimates from fire activity over Southeastern U.S., the Community Multi-Scale Air Quality (CMAQ) model is used to simulate PM2.5 concentrations and source impacts for fires during May of 2012. In this work, FINN emissions estimates replace NEI fire emissions estimates for more precise estimation of fire impact on air quality. Modeled results are evaluated using observations from monitoring networks such as the Chemical Speciation Network and the Southeastern Aerosol Research and Characterization network. Aircraft measurements from the Deep Convective Cloud and Chemistry (DC3) flight campaign and the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) are also used to evaluate modeled simulations of aerosol concentrations.

  2. 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 ...

  3. Simulated Transport and Mixing of Anthropogenic and Biogenic Aerosol and Their Entrainment into Clouds during the Goamazon Campaign

    NASA Astrophysics Data System (ADS)

    Fast, J. D.; Shrivastava, M. B.; Fan, J.; Berg, L. K.; Chand, D.; Fortner, E.; Mei, F.; Pekour, M. S.; Shilling, J. E.; Springston, S. R.; Tomlinson, J. M.; Wang, J.

    2014-12-01

    Several recent studies have suggested that anthropogenic emissions enhance the production of biogenic secondary organic aerosol (SOA). Because Manaus, Brazil is an isolated large city within the Amazon rainforest, measurements collected within and outside of the downwind urban plume during the 2014 Green Ocean Amazon (GoAmazon) campaign (supported by the U.S. Department of Energy's Atmospheric Radiation and Measurement program) will provide valuable information needed by regional and global models to evaluate parameterizations of SOA. The isolated urban plume should also provide distinct patterns of mixing with biogenic emissions and eliminate complications of multiple anthropogenic sources found in most other regions of the world. The objective of this study is to evaluate the performance of preliminary simulations of the transport, mixing, and chemical evolution of the Manaus urban plume from the chemistry version of the Weather Research and Forecasting model (WRF-Chem) using the available surface and aircraft measurements collected during the first intensive observation period (IOP) of GoAmazon. Simulations are performed using both a 10 km or 2 km grid spacing as well as a newly developed treatment that couples a sectional aerosol model and its parameterization of SOA using a volatility basis set approach with resolved clouds and a sub-grid scale cloud parameterization. Since the first IOP of GoAmazon was conducted during the wet season, shallow and deep convection were observed on most days and likely impacts the transport and vertical mixing of the Manaus plume. Therefore, we are using the available field campaign cloud measurements to evaluate the impact of sub-grid scale clouds on the horizontal and vertical distribution of aerosols. Satellite data is also used to assess the regional variability in simulated clouds and precipitation. Analyses of the simulations during the first IOP will be presented. Simulations with and without anthropogenic emissions will

  4. 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.

  5. 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

  6. Characterization and deposition of aerosol organic matter in the eastern United States

    NASA Astrophysics Data System (ADS)

    Wozniak, Andrew S.

    Aerosol organic carbon (OC) was characterized in two eastern United States watersheds to investigate the potential importance of aerosol OC in watershed OC budgets and cycling. Fluxes of 1.7 and 2.1 mg aerosol OC m-2 d-1 were measured for aerosol samples in Harcum, VA and Millbrook, NY, respectively. Scaled to the area of nearby watersheds (York River watershed, VA and Hudson River watershed, NY) these fluxes are similar in magnitude or greater than the magnitude of riverine OC exported by corresponding rivers indicating that aerosols must be taken into account when thinking about biogeochemical exchanges between the atmospheric, terrestrial, and aquatic realms. Fossil fuel and contemporary biomass emissions are the major sources of aerosol total OC (TOC) to the eastern United States, and radiocarbon signatures were used to estimate the relative contributions from these two sources. On average 33% of aerosol TOC could be attributed to fossil sources throughout the year with mean seasonal fossil TOC contributions (11% to 57% fossil) revealing significant heterogeneity in the relative magnitude of anthropogenic fossil and contemporary biomass TOC sources throughout the year. The 33% fossil aerosol TOC corresponds to a human-derived, 50% increase in aerosol TOC delivered to watersheds and aquatic systems above pre-industrial levels. The effects of such an increase in the delivery of TOC to watersheds are unknown and warrant further investigation. Further radiocarbon analyses on aerosol TOC sub-fractions showed the water-soluble component of aerosol OC (WSOC) to contain significantly more contemporary-aged OC than either bulk aerosol OC or its water-insoluble components. These differences represent a fundamental partitioning in the solubility of fossil and contemporary-derived aerosol OC, and its potential post-depositional fate in watersheds and soils. Fossil OC remains in the less bioavailable particulate phase and its transport is dependent on the erodibility of

  7. 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.

  8. Quantum uncertainty of mixed states based on skew information

    SciTech Connect

    Luo Shunlong

    2006-02-15

    The uncertainty of a mixed state has two quite different origins: classical mixing and quantum randomness. While the classical aspect (mixedness) is significantly quantified by the von Neumann entropy, it seems that we still do not have a well accepted measure of quantum uncertainty. In terms of the skew information introduced by Wigner and Yanase in 1963 in the context of quantum measurements, we will propose an intrinsic measure for synthesizing quantum uncertainty of a mixed state and investigate its fundamental properties. We illustrate how it arises naturally from a naive hidden-variable approach to entanglement and how it exhibits a simple relation to the notion of negativity, which is an entanglement monotone introduced quite recently. We further show that it has a dramatic nonextensive feature resembling the probability law relating operations of two events. This measure of quantum uncertainty provides an alternative quantity complementary to the von Neumann entropy for studying mixedness and quantum correlations.

  9. 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.

  10. 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).

  11. 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

  12. Seasonal comparisons of single-particle chemical mixing state in Riverside, CA

    NASA Astrophysics Data System (ADS)

    Qin, Xueying; Pratt, Kerri A.; Shields, Laura G.; Toner, Stephen M.; Prather, Kimberly A.

    2012-11-01

    The Study of Organic Aerosols in Riverside, CA (SOAR) field campaign, conducted in the summer and fall of 2005, focused on developing a stronger understanding of seasonal influences on the sources and processes contributing to some of the highest levels of particulate matter in the United States. On-line single-particle mass spectrometry measurements showed that carbonaceous particles generally dominated the submicron size range (>75% by number), compared to primarily aged sea salt and dust in the supermicron size range. During periods with high PM2.5 (particulate matter <2.5 μm) mass and number concentrations, hygroscopic water-containing carbonaceous particles internally mixed with sulfate and nitrate extended up into the supermicron size mode. The mixing state of carbonaceous particles changed with season. In the summer, carbonaceous particles were primarily mixed with secondary (oxidized) organic carbon and sulfate; whereas in the fall, they were mixed mostly with ammonium nitrate. During each season, different processes contributed to the highest pollution levels. In the summer, photochemical production of highly aged secondary organic carbon resulted in daily peaks in both number and mass particle concentrations, followed by removal in the afternoon by the arrival of the clean marine air masses from the coast. In contrast, cooler, more stagnant meteorological conditions in the fall season resulted in the buildup over several days of submicron carbonaceous particles mixed with semivolatile ammonium, nitrate, and amines. In addition, Santa Ana wind events in the fall led to dust and biomass burning particles dominating both the submicron and supermicron size ranges.

  13. 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

  14. 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.

  15. 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.

  16. Black carbon simulations using a size- and mixing-state-resolved three-dimensional model: 1. Radiative effects and their uncertainties

    NASA Astrophysics Data System (ADS)

    Matsui, H.

    2016-02-01

    This study quantifies how uncertainties in the size distribution and mixing state parameters of black carbon (BC) emissions translate into the uncertainties in BC radiative effects by using a particle-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 can explicitly calculate BC processes in the atmosphere, such as BC aging due to condensation and coagulation and the resulting enhancement of absorption and cloud condensation nuclei activity, with 12 size and 10 BC mixing state bins (128 bins in total). Fifteen model simulations perturbing the emission parameters within their uncertainties are conducted over East Asia (spring 2009) to understand which parameters and processes are important and which are associated with the uncertainty in evaluating BC radiative effects. The simulations reveal a large variability (uncertainty) of BC optical and radiative variables over the East Asian region (the variability is 58-99%), which corresponds to ranges of BC radiative effect of 1.6-2.8 W m-2 at the top of the atmosphere and from -5.2 to -2.1 W m-2 at the surface over East Asia. BC optical and radiative variables are 3 to 5 times sensitive to the size and the mixing state in emissions than BC mass concentrations (the variability is 20%). The two main causes of the difference in sensitivity are the reduction of the variability of BC mass concentrations by coagulation and the enhancement of the variability of BC absorption by resolving BC mixing state. These complicated responses of aerosol processes can be calculated for the first time using a detailed aerosol model such as ATRAS. The results suggest that the following two points are important in the estimation of BC radiative effects: (1) reduction of the

  17. 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.

  18. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

    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 relative humidities (RHs) of ˜ 15, ˜ 70, and ˜ 90 % and compared with extinction calculated from measurements of aerosol composition and size distribution using the κ-Köhler approximation for hygroscopic growth. The calculated enhancement in hydrated aerosol extinction with relative humidity, f(RH), calculated by this method agreed well with the observed f(RH) at ˜ 90 % RH. The dominance of organic aerosol, which comprised 65 ± 10 % of particulate matter with aerodynamic diameter < 1 µm in the planetary boundary layer, resulted in relatively low f(RH) values of 1.43 ± 0.67 at 70 % RH and 2.28 ± 1.05 at 90 % RH. The subsaturated κ-Köhler 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, with a best estimate of κ = 0.05. This subsaturated κ value for the organic aerosol in the southeastern US is broadly consistent with field studies in rural environments. A new, physically based, single-parameter representation was developed that better described f(RH) than did the widely used gamma power-law approximation.

  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. 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.

  2. Efficient Quantum Compression for Ensembles of Identically Prepared Mixed States

    NASA Astrophysics Data System (ADS)

    Yang, Yuxiang; Chiribella, Giulio; Ebler, Daniel

    2016-02-01

    We present one-shot compression protocols that optimally encode ensembles of N identically prepared mixed states into O (log N ) qubits. In contrast to the case of pure-state ensembles, we find that the number of encoding qubits drops down discontinuously as soon as a nonzero error is tolerated and the spectrum of the states is known with sufficient precision. For qubit ensembles, this feature leads to a 25% saving of memory space. Our compression protocols can be implemented efficiently on a quantum computer.

  3. Aerosol Precursor Emissions, Secondary Aerosol Production, and Climate-Forcing Gas Exchange in the Midwestern United States

    NASA Astrophysics Data System (ADS)

    Doskey, P. V.

    2009-12-01

    Aerosol precursors in the Midwest are generated from a myriad of sources including biogenic emissions of terpenes from the Ozarks region, anthropogenic emissions of volatile and semivolatile aliphatic and aromatic hydrocarbons from the St. Louis airshed, and agricultural emissions of ammonia (NH3), amines, and nitrogen oxides (NOx) from animal husbandry and cropping systems of the Midwest Corn Belt. The deciduous and coniferous forests of the Ozarks region are significant sources of isoprene, monoterpenes, and sesquiterpenes that are sensitive to rising CO2 levels and temperature and generate light-scattering, secondary organic aerosol (SOA). Application of nitrogen fertilizers stimulates emissions of ammonia (NH3), nitric oxide (NO), and nitrous oxide (N2O) from agricultural soils and crops. Nitric acid, generated through photooxidation of NO emissions from fossil fuel combustion in urban air and from soil emissions in agroecosystems, reacts rapidly with NH3 to generate light-scattering, secondary inorganic aerosol (SIA). The atmospheric lifetime of N2O is about 120 years, making the substance a potent greenhouse gas with a global warming potential of 290 for a time horizon of 20 years relative to CO2. Emissions of CO2, N2O, and SIA precursors from the Midwest Corn Belt and surrounding areas are likely to increase in the near future as pastureland and prairie is converted to grow corn and other biofuel crops to meet the demand for renewable fuels. Several large river systems transport nutrients from fertilized fields of the Midwest agroecosystem to the Gulf of Mexico where plankton growth is accelerated. Microbial decomposition of plankton detritus consumes oxygen and creates a hypoxic zone, which might be a significant source of N2O.The presentation will discuss gaps in our knowledge of the production of climate-forcing species in the Midwestern United States.

  4. 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.

  5. 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.

  6. 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.

  7. 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

  8. 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

  9. 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...

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

    PubMed

    Moffet, Ryan C; Prather, Kimberly A

    2009-07-21

    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/m(2), making soot second only to CO(2) 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 1.6x 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

  11. 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

  12. 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.

  13. 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.

  14. 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.

  15. 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.

  16. 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

  17. 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.

  18. 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

  19. 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.

  20. A sea spray aerosol flux parameterization encapsulating wave state

    NASA Astrophysics Data System (ADS)

    Ovadnevaite, J.; Manders, A.; de Leeuw, G.; Monahan, C.; Ceburnis, D.; O'Dowd, C. D.

    2013-09-01

    A new sea spray source function (SSSF), termed Oceanflux Sea Spray Aerosol or OSSA, was derived based on in-situ sea spray measurements along with meteorological/physical parameters. Submicron sea spray fluxes derived from particle number concentration measurements at the Mace Head coastal station, on the west coast of Ireland, were used together with open-ocean eddy correlation flux measurements from the Eastern Atlantic (SEASAW cruise). In the overlapping size range, the data for Mace Head and SEASAW were found to be in a good agreement, which allowed deriving the new SSSF from the combined dataset spanning the dry diameter range from 15 nm to 6 μm. The sea spray production was parameterized in terms of 5 log-normal modes and the Reynolds number instead of the more commonly used wind speed, thereby encapsulating important influences of wave height and history, friction velocity and viscosity. This formulation accounts for the different flux relationships associated with rising and waning wind speeds since these are included in the Reynolds number. Furthermore, the Reynolds number incorporates the kinematic viscosity of water, thus the SSSF inherently includes a sea surface temperature dependence. The temperature dependence of the resulting SSSF is similar to that of other in-situ derived source functions and results in lower production fluxes for cold waters and enhanced fluxes from warm waters as compared with SSSF formulations that do not include temperature effects.

  1. 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.

  2. The Potential Importance of the Cloud Processing of Aerosol in Mesoscale Simulations of Mixed-Phase Arctic Stratus

    NASA Astrophysics Data System (ADS)

    Avramov, A.; Harrington, J. Y.; Yannuzi, V.; Prenni, A.; Demott, P.

    2005-12-01

    Mixed-phase arctic stratus clouds are the predominant cloud type in the Arctic . Perhaps one of the most intriguing of their features is that they tend to have liquid tops that precipitate ice. Despite the fact that this situation is colloidally unstable, these cloud systems are quite long lived - from a few days to over a couple of weeks. Previous studies have suggested that this longevity may be due to a paucity of ice nucleating aerosols (ice nuclei, or IN) in the arctic. Such studies have shown that small changes in IN concentrations can cause large changes in the amount of liquid water within a mixed-phase stratus deck. We use the Regional Atmospheric Modeling System (RAMS) to simulate the time period of October 9-11 from the Mixed-Phase Arctic Cloud Experiment (M-PACE) which was conducted in October of 2004. During this period the North Slope of Alaska and Arctic Ocean were covered by an extensive mixed-phase straus deck. Using heterogeneous ice nucleation parameterizations typical of most models (e.g. Meyers et al., (1992)), the simulated clouds rapidly glaciate. Unlike the observed clouds, very little liquid remains and most of the region is covered by thin ice clouds in the simulations. Measurements during M-PACE suggest that the IN concentrations predicted by typical parameterizations are, perhaps, an order of magnitude too large for the Arctic. Using data taken during M-PACE, the existing IN parameterizations in RAMS were modified. Simulations using the new parameterizations illustrate that arctic mixed-phase clouds can maintain large amounts of liquid water because of the following: (1) IN concentrations are particularly low in the Arctic, leading to a weak glaciation process. (2) Cloud processing of IN, whereby ice nucleation removes IN from the pool of available nuclei, effectively reduces IN concentrations leading to larger liquid amounts. (3) If IN concentrations are too large, cloud

  3. 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

  4. Source and mixing state of iron-containing particles in Shanghai by individual particle analysis.

    PubMed

    Zhang, Guohua; Bi, Xinhui; Lou, Shengrong; Li, Lei; Wang, Hongli; Wang, Xinming; Zhou, Zhen; Sheng, Guoying; Fu, Jiamo; Chen, Changhong

    2014-01-01

    Bioavailable iron (Fe) is an essential nutrient that can control oceanic productivity, thereby impacting the global carbon budget and climate. Therefore it is of vital importance to identify chemical species and mixing state of Fe-containing particles in the air, which are demonstrated to pose substantial impact on bioavailability of Fe. Using a single particle aerosol mass spectrometer (SPAMS), ~2,000,000 individual particles with mass spectra were collected in Shanghai for nearly 22d during the winter of 2011. Number fraction of Fe-containing particles (NfFe) varied in a wide range (<1-15%) throughout the measurement. Fe-containing particles were mainly clustered into four chemical groups, comprising of Fe-rich, K-rich, Dust and V-containing particle types. Analysis of mass spectra and mixing state suggests that Fe-containing particles correspond to various sources in Shanghai, especially anthropogenic sources iron/steel industrial activities, and fly ashes from both biomass burning and coal combustion, accounting for ~55% and ~18%, respectively. However, invasion of dust from northern desert areas is suspected to be more responsible for the spikes of NfFe (>10%), when Dust particle type contributed to >50% of Fe-containing particles. It is also revealed that Fe-containing particles were internally mixed with secondary species (e.g., sulfate and nitrate). Anthropogenic K-rich and Fe-rich particles tended to associate with both sulfate and nitrate, and thus might lead to more fraction of soluble Fe, compared to Dust particles. These results imply that atmospheric processing of Fe-containing particles from various sources might vary and thus would change the bioavailability of atmospheric Fe. PMID:23719486

  5. 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.

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

    DOE PAGESBeta

    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

  7. Maximally coherent mixed states: Complementarity between maximal coherence and mixedness

    NASA Astrophysics Data System (ADS)

    Singh, Uttam; Bera, Manabendra Nath; Dhar, Himadri Shekhar; Pati, Arun Kumar

    2015-05-01

    Quantum coherence is a key element in topical research on quantum resource theories and a primary facilitator for design and implementation of quantum technologies. However, the resourcefulness of quantum coherence is severely restricted by environmental noise, which is indicated by the loss of information in a quantum system, measured in terms of its purity. In this work, we derive the limits imposed by the mixedness of a quantum system on the amount of quantum coherence that it can possess. We obtain an analytical trade-off between the two quantities that upperbound the maximum quantum coherence for fixed mixedness in a system. This gives rise to a class of quantum states, "maximally coherent mixed states," whose coherence cannot be increased further under any purity-preserving operation. For the above class of states, quantum coherence and mixedness satisfy a complementarity relation, which is crucial to understand the interplay between a resource and noise in open quantum systems.

  8. 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.

  9. Modelled radiative effects of sea spray aerosol using a source function encapsulating wave state

    NASA Astrophysics Data System (ADS)

    Partanen, Antti-Ilari; Dunne, Eimear M.; Bergman, Tommi; Laakso, Anton; Kokkola, Harri; Ovadnevaite, Jurgita; Sogacheva, Larisa; Baisnée, Dominique; Sciare, Jean; Manders, Astrid; O'Dowd, Colin; de Leeuw, Gerrit; Korhonen, Hannele

    2014-05-01

    Sea spray aerosol particles have significant effects on global climate by scattering solar radiation (direct effect) and modifying cloud properties (indirect effect). Sea spray consists mainly of sea salt, but in biologically active regions, major fraction of sea spray may come in the form of primary marine organic matter (PMOM). Traditionally, sea spray flux has been parameterized in global models in terms of wind speed, and organic fraction of sea spray in terms of chlorophyll-a concentration. In this study, we have incorporated recently developed parameterizations for the sea spray aerosol source flux into the global aerosol-climate model ECHAM-HAMMOZ. The parameterizations encapsulate the wave state via Reynolds number, and predict the organic fraction of the sea spray aerosol source flux. The model was then used to investigate the direct and indirect effects of sea spray aerosol particles. We compared simulated sea spray concentrations with in-situ measurements from Mace Head (North Atlantic), Point Reyes (North Pacific), and Amsterdam Island (Southern Indian Ocean). Aerosol optical depth (AOD) was compared with satellite measurements from PARASOL. Modelled annual mean global emissions of sea salt and PMOM were 805 Tg yr-1 (uncertainty range of 378-1233 Tg yr-1) and 1.1 Tg yr-1 (0.5-1.8 Tg yr-1), respectively. Sea salt emissions were considerably lower than the majority of previous estimates, but PMOM was in the range of previous studies. The model captured sea salt concentrations fairly well in the smaller size ranges at Mace Head (annual normalized mean bias of -13% for particles with vacuum aerodynamic diameter Dva

  10. Geometric phases for mixed states of the Kitaev chain.

    PubMed

    Andersson, Ole; Bengtsson, Ingemar; Ericsson, Marie; Sjöqvist, Erik

    2016-05-28

    The Berry phase has found applications in building topological order parameters for certain condensed matter systems. The question whether some geometric phase for mixed states can serve the same purpose has been raised, and proposals are on the table. We analyse the intricate behaviour of Uhlmann's geometric phase in the Kitaev chain at finite temperature, and then argue that it captures quite different physics from that intended. We also analyse the behaviour of a geometric phase introduced in the context of interferometry. For the Kitaev chain, this phase closely mirrors that of the Berry phase, and we argue that it merits further investigation. PMID:27091168

  11. Glass transition and phase state of organic compounds: dependency on molecular properties and implications for secondary organic aerosols in the atmosphere.

    PubMed

    Koop, Thomas; Bookhold, Johannes; Shiraiwa, Manabu; Pöschl, Ulrich

    2011-11-21

    Recently, it has been proposed that organic aerosol particles in the atmosphere can exist in an amorphous semi-solid or solid (i.e. glassy) state. In this perspective, we analyse and discuss the formation and properties of amorphous semi-solids and glasses from organic liquids. Based on a systematic survey of a wide range of organic compounds, we present estimates for the glass forming properties of atmospheric secondary organic aerosol (SOA). In particular we investigate the dependence of the glass transition temperature T(g) upon various molecular properties such as the compounds' melting temperature, their molar mass, and their atomic oxygen-to-carbon ratios (O:C ratios). Also the effects of mixing different compounds and the effects of hygroscopic water uptake depending on ambient relative humidity are investigated. In addition to the effects of temperature, we suggest that molar mass and water content are much more important than the O:C ratio for characterizing whether an organic aerosol particle is in a liquid, semi-solid, or glassy state. Moreover, we show how the viscosity in liquid, semi-solid and glassy states affect the diffusivity of those molecules constituting the organic matrix as well as that of guest molecules such as water or oxidants, and we discuss the implications for atmospheric multi-phase processes. Finally, we assess the current state of knowledge and the level of scientific understanding, and we propose avenues for future studies to resolve existing uncertainties. PMID:21993380

  12. A thermodynamic model of mixed organic-inorganic aerosols to predict activity coefficients

    NASA Astrophysics Data System (ADS)

    Zuend, A.; Marcolli, C.; Luo, B. P.; Peter, T.

    2008-08-01

    Tropospheric aerosols contain mixtures of inorganic salts, acids, water, and a large variety of organic compounds. Interactions between these substances in liquid mixtures lead to discrepancies from ideal thermodynamic behaviour. By means of activity coefficients, non-ideal behaviour can be taken into account. We present here a thermodynamic model named AIOMFAC (Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients) that is able to calculate activity coefficients covering inorganic, organic, and organic-inorganic interactions in aqueous solutions over a wide concentration range. This model is based on the activity coefficient model LIFAC by Yan et al. (1999) that we modified and reparametrised to better describe atmospherically relevant conditions and mixture compositions. Focusing on atmospheric applications we considered H+, Li+, Na+, K+, NH+4, Mg2+, Ca2+, Cl-, Br-, NO-3, HSO-4, and SO2-4 as cations and anions and a wide range of alcohols/polyols composed of the functional groups CHn and OH as organic compounds. With AIOMFAC, the activities of the components within an aqueous electrolyte solution are well represented up to high ionic strength. Most notably, a semi-empirical middle-range parametrisation of direct organic-inorganic interactions in alcohol+water+salt solutions strongly improves the agreement between experimental and modelled activity coefficients. At room temperature, this novel thermodynamic model offers the possibility to compute equilibrium relative humidities, gas/particle partitioning and liquid-liquid phase separations with high accuracy. In further studies, other organic functional groups will be introduced. The model framework is not restricted to specific ions or organic compounds and is therefore also applicable for other research topics.

  13. A thermodynamic model of mixed organic-inorganic aerosols to predict activity coefficients

    NASA Astrophysics Data System (ADS)

    Zuend, A.; Marcolli, C.; Luo, B. P.; Peter, Th.

    2008-03-01

    Tropospheric aerosols contain mixtures of inorganic salts, acids, water, and a large variety of organic compounds. Interactions between these substances in liquid mixtures lead to discrepancies from ideal thermodynamic behaviour. By means of activity coefficients, non-ideal behaviour can be taken into account. We present here a thermodynamic model named AIOMFAC (Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients) that is able to calculate activity coefficients covering inorganic, organic, and organic-inorganic interactions in aqueous solutions over a wide concentration range. This model is based on the activity coefficient model LIFAC by Yan et al. (1999) that we modified and reparametrised to better describe atmospherically relevant conditions and mixture compositions. Focusing on atmospheric applications we considered H+, Li+, Na+, K+, NH4+, Mg2+, Ca2+, Cl-, Br-, NO3-, HSO4-, and SO42- as cations and anions and a wide range of alcohols/polyols composed of the functional groups CHn and OH as organic compounds. With AIOMFAC, the activities of the components within an aqueous electrolyte solution are well represented up to high ionic strength. Most notably, a semi-empirical middle-range parametrisation of direct organic-inorganic interactions in alcohol + water + salt solutions strongly improves the agreement between experimental and modelled activity coefficients. At room temperature, this novel thermodynamic model offers the possibility to compute equilibrium relative humidities, gas/particle partitioning and liquid-liquid phase separations with high accuracy. In further studies, other organic functional groups will be introduced. The model framework is not restricted to specific ions or organic compounds and is therefore also applicable for other research topics.

  14. 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.

  15. 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

  16. Simulation of particle diversity and mixing state over Greater Paris: a model-measurement inter-comparison.

    PubMed

    Zhu, Shupeng; Sartelet, Karine N; Healy, Robert M; Wenger, John C

    2016-07-18

    Air quality models are used to simulate and forecast pollutant concentrations, from continental scales to regional and urban scales. These models usually assume that particles are internally mixed, i.e. particles of the same size have the same chemical composition, which may vary in space and time. Although this assumption may be realistic for continental-scale simulations, where particles originating from different sources have undergone sufficient mixing to achieve a common chemical composition for a given model grid cell and time, it may not be valid for urban-scale simulations, where particles from different sources interact on shorter time scales. To investigate the role of the mixing state assumption on the formation of particles, a size-composition resolved aerosol model (SCRAM) was developed and coupled to the Polyphemus air quality platform. Two simulations, one with the internal mixing hypothesis and another with the external mixing hypothesis, have been carried out for the period 15 January to 11 February 2010, when the MEGAPOLI winter field measurement campaign took place in Paris. The simulated bulk concentrations of chemical species and the concentrations of individual particle classes are compared with the observations of Healy et al. (Atmos. Chem. Phys., 2013, 13, 9479-9496) for the same period. The single particle diversity and the mixing-state index are computed based on the approach developed by Riemer et al. (Atmos. Chem. Phys., 2013, 13, 11423-11439), and they are compared to the measurement-based analyses of Healy et al. (Atmos. Chem. Phys., 2014, 14, 6289-6299). The average value of the single particle diversity, which represents the average number of species within each particle, is consistent between simulation and measurement (2.91 and 2.79 respectively). Furthermore, the average value of the mixing-state index is also well represented in the simulation (69% against 59% from the measurements). The spatial distribution of the mixing-state

  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. 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

  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. Determining Boundary Layer Mixing State based on NASA DISCOVER-AQ Airborne Soundings over the Baltimore/Washington Area

    NASA Astrophysics Data System (ADS)

    Chen, G.; Crawford, J. H.; Silverman, M. L.; Anderson, B. E.; Barrick, J. D.; Diskin, G. S.; Fried, A.; Yang, M. M.; Weinheimer, A. J.; Lenschow, D. H.

    2012-12-01

    The DISCOVER-AQ (Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality) mission conducted its first field deployment in the Washington D.C./Baltimore region during July 2011. The overarching goal is to better understand how remotely-sensed column measurements can be used to diagnose near-surface air quality. To achieve this objective, the DISCOVER-AQ sampling strategy requires extensive probing of the vertical structure of the lower troposphere as it relates to both trace gases and aerosols. This strategy was implemented by using the NASA P-3B aircraft to spiral from 0.3 to ~3 km over 6 MDE (Maryland Department of the Environment) ground monitoring sites. A total of 254 spirals were flown which generated detailed vertical distributions for a large variety of trace gases, aerosol properties, and meteorological variables. This data set allows a detailed assessment of vertical mixing state, which can be estimated by the changes of the measured variables with height within the boundary layer. The data set was further filtered to minimize the influence of the horizontal inhomogeneity. To be presented are cases under different atmospheric stability classes to show the actual observed atmospheric structure and vertical distributions of the aerosols and trace gases which have a wide range of lifetimes.

  1. 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...

  2. 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.

  3. 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).

  4. Impacts of black carbon mixing state on black carbon nucleation scavenging: Insights from a particle-resolved model

    NASA Astrophysics Data System (ADS)

    Ching, J.; Riemer, N.; West, M.

    2012-12-01

    This paper presents an advancement of the recently developed particle-resolved aerosol model PartMC-MOSAIC (Particle Monte Carlo-Model for Simulating Aerosol Interactions and Chemistry) to investigate the impacts of mixing state on cloud droplet formation and to provide a tool for the quantification of errors in cloud properties introduced by simplifying mixing state assumptions. We coupled PartMC-MOSAIC with a cloud parcel model. We initialized the cloud parcel simulation with hourly PartMC-MOSAIC model output from a 48-hour urban plume simulation. The cloud parcel model then explicitly simulated activation and condensational growth of the particles as the parcel underwent cooling at a specified rate and the particles of the aerosol population competed for water vapor. We used this capability to quantify the relative importance of size information versus composition information for the prediction of the cloud droplet number fraction, mass fraction of black carbon that is nucleation-scavenged, cloud droplet effective radius, and relative dispersion of the droplet size distribution by introducing averaging of particle-resolved information within prescribed bins. For the cloud droplet number fraction, both composition averaging and size-bin averaging individually led to an error of less than 25% for all cloud parcel simulations, while averaging in both size bins and composition resulted in errors of up to 34% for the base case cooling rate of 0.5 K/min. In contrast, for the nucleation-scavenged black carbon mass fraction, the results for size-bin averaging tracked the reference case well, while composition averaging, with or without size-bin averaging, led to overestimation of this quantity by up to 600%.

  5. 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.

  6. 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. PMID:20699696

  7. Fire and biofuel contributions to annual mean aerosol mass concentrations in the United States

    NASA Astrophysics Data System (ADS)

    Park, Rokjin J.; Jacob, Daniel J.; Logan, Jennifer A.

    We estimate the contributions from biomass burning (summer wildfires, other fires, residential biofuel, and industrial biofuel) to seasonal and annual aerosol concentrations in the United States. Our approach is to use total carbonaceous (TC) and non-soil potassium (ns-K) aerosol mass concentrations for 2001-2004 from the nationwide IMPROVE network of surface sites, together with satellite fire data. We find that summer wildfires largely drive the observed interannual variability of TC aerosol concentrations in the United States. TC/ns-K mass enhancement ratios from fires range from 10 for grassland and shrub fires in the south to 130 for forest fires in the north. The resulting summer wildfire contributions to annual TC aerosol concentrations for 2001-2004 are 0.26 μg C m -3 in the west and 0.14 μg C m -3 in the east; Canadian fires are a major contributor in the east. Non-summer wildfires and prescribed burns contribute on an annual mean basis 0.27 and 0.31 μg C m -3 in the west and the east, highest in the southeast because of prescribed burning. Residential biofuel is a large contributor in the northeast with annual mean concentration of up to 2.2 μg C m -3 in Maine. Industrial biofuel (mainly paper and pulp mills) contributes up to 0.3 μg C m -3 in the southeast. Total annual mean fine aerosol concentrations from biomass burning average 1.2 and 1.6 μg m -3 in the west and east, respectively, contributing about 50% of observed annual mean TC concentrations in both regions and accounting for 30% (west) and 20% (east) of total observed fine aerosol concentrations. Our analysis supports bottom-up source estimates for the contiguous United States of 0.7-0.9 Tg C yr -1 from open fires (climatological) and 0.4 Tg C yr -1 from biofuel use. Biomass burning is thus an important contributor to US air quality degradation, which is likely to grow in the future.

  8. 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.

  9. 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.

  10. Mixing state of individual submicron carbon-containing particles during spring and fall seasons in urban Guangzhou, China: a case study

    NASA Astrophysics Data System (ADS)

    Zhang, G.; Bi, X.; Li, L.; Chan, L. Y.; Li, M.; Wang, X.; Sheng, G.; Fu, J.; Zhou, Z.

    2013-05-01

    Growing evidence suggests that the size-resolved mixing state of carbon-containing particles is very critical in determining their optical properties, atmospheric lifetime, and impact on the environment. However, still little is known about the mixing state of particles in the urban area of the Pearl River Delta (PRD) region, China. To investigate the mixing state of submicron carbon-containing particles, measurements were carried out during spring and fall periods of 2010 using a single-particle aerosol mass spectrometer (SPAMS). Approximately 700 000 particles for each period were detected. This is the first report on the size-resolved mixing state of carbon-containing particles by direct observations in the PRD region. Cluster analysis of single-particle mass spectra was applied to identify carbon-containing particle classes. These classes represented ~80% and ~90% of all the detected particles for spring and fall periods, respectively. Carbon-containing particle classes mainly consisted of biomass/biofuel burning particles (Biomass), organic carbon (OC), fresh elemental carbon (EC-fresh), internally mixed OC and EC (ECOC), internally mixed EC with sulfate (EC-Sulfate), vanadium-containing ECOC (V-ECOC), and amines-containing particles (Amine). In spring, the top three ranked carbon-containing particle classes were ECOC (26.1%), Biomass (23.6%) and OC (10%), respectively. However, the fraction of Biomass particles increased remarkably and predominated (61.0%), while the fraction of ECOC (3.0%) and V-ECOC (0.1%) significantly decreased in fall. To highlight the influence of monsoon on the properties of carbon-containing particles in urban Guangzhou, their size distributions, mixing state, and aerosol acidity were compared between spring and fall seasons. In addition, a case study was also performed to investigate how the formation of fog and haze influenced the mixing state of carbon-containing particles. These results could improve our understanding of the

  11. Simulations of aerosol, microphysical and coastal influences on Arctic mixed-phase clouds

    NASA Astrophysics Data System (ADS)

    Avramov, Alexander Elkov

    Mixed-phase stratus clouds are the prevalent cloud type in the Arctic during the winter and transition seasons. Despite their important role in various climate feedback mechanisms they are still not well understood and are difficult to represent accurately in large-scale models. In this study the role of ice nucleation mechanisms, the influence of the coastally-generated circulations and parameterized ice crystal habit on the longevity and structure of Arctic mixed-phase clouds were examined using detailed mesoscale, cloud- and eddy-resolving model simulations. The structure and the lifetime of simulated Arctic mixed-phase clouds were found to be highly sensitive to the concentration of ice-nuclei (IN) acting in deposition/condensation-freezing nucleation mode. Contact nucleation could not produce significant ice amounts unless the contact IN concentrations were increased to unrealistically high values. Local, coastally induced circulations were found to be responsible for maintaining the continuous ice precipitation along the coastline through transport of deposition/condensation-freezing IN from above the cloud layer. It was demonstrated that incorrect partitioning of the liquid and ice phase can produce errors in the surface radiative budget of up to 90 Wm-2. Simulated IN sensitivity and liquid/ice phase partitioning were found to depend critically on the assumed ice crystal habit. It was demonstrated that a large range of liquid or ice water path can be produced by reasonable changes in ice crystal habit mass-dimensional and terminal fall-speed relations based on data reported in the literature. The changes in ice crystal habit were shown to be related to liquid layer formation, splitting of liquid layers, and cloud dissipation mechanisms in multi-layered Arctic mixed-phase clouds. These results suggest that predicting changes in crystal habit is of significant importance for correct model representation of mixed-phase clouds. Three additional ice nucleation

  12. 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

  13. 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

  14. 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

  15. 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.

  16. 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.

  17. 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

  18. Mixing of dust with pollution on the transport path of Asian dust--revealed from the aerosol over Yulin, the north edge of Loess Plateau.

    PubMed

    Wang, Qiongzhen; Zhuang, Guoshun; Li, Juan; Huang, Kan; Zhang, Rong; Jiang, Yilun; Lin, Yanfen; Fu, Joshua S

    2011-01-01

    Both PM(2.5) and TSP were monitored in the spring from 2006 to 2008 in an intensive ground monitoring network of five sites (Tazhong, Yulin, Duolun, Beijing, and Shanghai) along the pathway of Asian dust storm across China to investigate the mixing of dust with pollution on the pathway of the long-range transport of Asian dust. Mineral was found to be the most loading component of aerosols both in dust event days and non-dust days. The concentrations of those pollution elements, As, Cd, Pb, Zn, and S in aerosol were much higher than their mean abundances in the crust even in dust event days. The high concentration of SO(4)(2-) could be from both sources: one from the transformation of the local emitted SO(2) and the other from the sulfate that existed in primary dust, which was transported to Yulin. Na(+), Ca(2+), and Mg(2+) were mainly from the crustal source, while NO(3)(-) and NH(4)(+) were from the local pollution sources. The mixing of dust with pollution aerosol over Yulin in dust event day was found to be ubiquitous, and the mixing extent could be expressed by the ratio of NO(3)(-)/Al in dust aerosol. The ratio of Ca/Al was used as a tracer to study the dust source. The comparison of the ratios of Ca/Al together with back trajectory analysis indicated that the sources of the dust aerosol that invaded Yulin could be from the northwestern desert in China and Mongolia Gobi. PMID:21075425

  19. 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...

  20. 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.

  1. Simulation of the effects of aerosol on mixed-phase orographic clouds using the WRF model with a detailed bin microphysics scheme

    NASA Astrophysics Data System (ADS)

    Xiao, Hui; Yin, Yan; Jin, Lianji; Chen, Qian; Chen, Jinghua

    2015-08-01

    The Weather Research Forecast (WRF) mesoscale model coupled with a detailed bin microphysics scheme is used to investigate the impact of aerosol particles serving as cloud condensation nuclei and ice nuclei on orographic clouds and precipitation. A mixed-phase orographic cloud developed under two scenarios of aerosol (a typical continental background and a relatively polluted urban condition) and ice nuclei over an idealized mountain is simulated. The results show that, when the initial aerosol condition is changed from the relatively clean case to the polluted scenario, more droplets are activated, leading to a delay in precipitation, but the precipitation amount over the terrain is increased by about 10%. A detailed analysis of the microphysical processes indicates that ice-phase particles play an important role in cloud development, and their contribution to precipitation becomes more important with increasing aerosol particle concentrations. The growth of ice-phase particles through riming and Wegener-Bergeron-Findeisen regime is more effective under more polluted conditions, mainly due to the increased number of droplets with a diameter of 10-30 µm. Sensitivity tests also show that a tenfold increase in the concentration of ice crystals formed from ice nucleation leads to about 7% increase in precipitation, and the sensitivity of the precipitation to changes in the concentration and size distribution of aerosol particles is becoming less pronounced when the concentration of ice crystals is also increased.

  2. 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

  3. Temperature and Precipitation Extremes in the United States: Quantifying the Responses to Aerosols and Greenhouse Gases

    NASA Astrophysics Data System (ADS)

    Mascioli, N. R.; Fiore, A. M.; Previdi, M. J.; Correa, G. J. P.

    2014-12-01

    Changes in extreme temperatures, heat waves, heavy rainfall events, and precipitation frequency can have adverse impacts on human health, air quality, agricultural productivity, and water resources. Using the aerosol only (AER) and greenhouse gas only (GHG) "single forcing" simulations (3 ensemble members each) from the GFDL CM3 chemistry-climate model, we investigate aerosol- versus greenhouse gas-induced changes in high temperature and precipitation extremes over the United States. We identify changes in these events from 1860 to 2005 and the associated large-scale dynamical conditions. Small changes in these extremes in the "all forcing" simulations reflect cancellations between the individual, opposite-signed effects of increasing anthropogenic aerosols and greenhouse gases. In AER, aerosols lead to lower extreme high temperatures and fewer warm spells over the western US (-2.1 K regional average; -20 days/year) and over the central and northeast US (-1.5 K; -12 days/year). In GHG, a similar but opposite-signed response pattern occurs (+2.7 K and +14 days/year over the western US; +2.5 K and +10 days/year in the central and northeast US). The similar spatial response patterns in AER versus GHG suggest a preferred regional mode of response that is largely independent of the regional distribution of the forcing agent. The influence of both greenhouse gases and aerosols on extreme high temperature is weakest in the southeast US, collocated with the observed "warming hole". No statistically significant change occurs in AER, and a warming of only +1.8 K occurs in GHG. Warming in this region continues to be muted over the 21st century under the RCP 8.5 scenario, with increases in extreme temperatures more than 1 K smaller than elsewhere. Aerosols induce decreases in the number of days per year with at least 10mm of precipitation (R10mm) over the eastern US in summer and winter and over the southern US in spring of roughly 1 day/year. In contrast, greenhouse gases

  4. GCM simulations of volcanic aerosol forcing. I - Climate changes induced by steady-state perturbations

    NASA Technical Reports Server (NTRS)

    Pollack, James B.; Rind, David; Lacis, Andrew; Hansen, James E.; Sato, Makiko; Ruedy, Reto

    1993-01-01

    The response of the climate system to a temporally and spatially constant amount of volcanic particles is simulated using a general circulation model (GCM). The optical depth of the aerosols is chosen so as to produce approximately the same amount of forcing as results from doubling the present CO2 content of the atmosphere and from the boundary conditions associated with the peak of the last ice age. The climate 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. The simulations indicate 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. 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.

  5. 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.

  6. Hygroscopicity of mineral dust particles: Roles of chemical mixing state and hygroscopic conversion timescale

    NASA Astrophysics Data System (ADS)

    Sullivan, R. C.; Moore, M. J.; Petters, M. D.; Laskin, A.; Roberts, G. C.; Kreidenweis, S. M.; Prather, K. A.

    2009-05-01

    Our laboratory investigations of mineral dust particle hygroscopicity are motivated by field observations of the atmospheric processing of dust. During ACE-Asia we observed sulphate and nitrate to be strongly segregated from each other in individual aged Asian dust particles. CCN activation curves of pure calcium minerals as proxies for fresh (calcium carbonate) and aged (calcium sulphate, nitrate, chloride) dust indicate that this mixing state would cause a large fraction of aged dust particles to remain poor warm cloud nucleation potential, contrary to previous assumptions. The enrichment of oxalic acid in calcium-rich dust particles could have similar effects due to the formation of insoluble calcium oxalate. Soluble calcium nitrate and chloride reaction products are hygroscopic and will transform mineral dust into excellent CCN. Generating insoluble mineral particles wet by atomization produced particles with much higher hygroscopicity then when resuspended dry. The atomized particles are likely composed of dissolved residuals and do not properly reflect the chemistry of dry mineral powders. Aerosol flow tube experiments were employed to study the conversion of calcium carbonate into calcium nitrate via heterogeneous reaction with nitric acid, with simultaneous measurements of the reacted particles' chemistry and hygroscopicity. The timescale for this hygroscopic conversion was found to occur on the order of a few hours under tropospheric conditions. This implies that the conversion of non-hygroscopic calcite- containing dust into hygroscopic particles will be controlled by the availability of nitric acid, and not by the atmospheric residence time. Results from recent investigations of the effect of secondary coatings on the ice nucleation properties of dust particles will also be presented. The cloud formation potential of aged dust particles depends on both the quantity and form of the secondary species that have reacted or mixed with the dust. These results

  7. 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

  8. Significant Contributions of Isoprene to Summertime Secondary Organic Aerosol in Eastern United States.

    PubMed

    Ying, Qi; Li, Jingyi; Kota, Sri Harsha

    2015-07-01

    A modified SAPRC-11 (S11) photochemical mechanism with more detailed treatment of isoprene oxidation chemistry and additional secondary organic aerosol (SOA) formation through surface-controlled reactive uptake of dicarbonyls, isoprene epoxydiol and methacrylic acid epoxide was incorporated in the Community Multiscale Air Quality Model (CMAQ) to quantitatively determine contributions of isoprene to summertime ambient SOA concentrations in the eastern United States. The modified model utilizes a precursor-origin resolved approach to determine secondary glyoxal and methylglyoxal produced by oxidation of isoprene and other major volatile organic compounds (VOCs). Predicted OC concentrations show good agreement with field measurements without significant bias (MFB ∼ 0.07 and MFE ∼ 0.50), and predicted SOA reproduces observed day-to-day and diurnal variation of Oxygenated Organic Aerosol (OOA) determined by an aerosol mass spectrometer (AMS) at two locations in Houston, Texas. On average, isoprene SOA accounts for 55.5% of total predicted near-surface SOA in the eastern U.S., followed by aromatic compounds (13.2%), sesquiterpenes (13.0%) and monoterpenes (10.9%). Aerosol surface uptake of isoprene-generated glyoxal, methylglyoxal and epoxydiol accounts for approximately 83% of total isoprene SOA or more than 45% of total SOA. A domain wide reduction of NOx emissions by 40% leads to a slight decrease of domain average SOA by 3.6% and isoprene SOA by approximately 2.6%. Although most of the isoprene SOA component concentrations are decreased, SOA from isoprene epoxydiol is increased by ∼16%. PMID:26029963

  9. 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

  10. Investigating Primary Marine Aerosol Properties: CCN Activity of Sea Salt and Mixed Inorganic–Organic Particles

    PubMed Central

    2012-01-01

    Sea spray particles ejected as a result of bubbles bursting from artificial seawater containing salt and organic matter in a stainless steel tank were sampled for size distribution, morphology, and cloud condensation nucleus (CCN) activity. Bubbles were generated either by aeration through a diffuser or by water jet impingement on the seawater surface. Three objectives were addressed in this study. First, CCN activities of NaCl and two types of artificial sea salt containing only inorganic components were measured to establish a baseline for further measurements of mixed organic–inorganic particles. Second, the effect of varying bubble residence time in the bulk seawater solution on particle size and CCN activity was investigated and was found to be insignificant for the organic compounds studied. Finally, CCN activities of particles produced from jet impingement were compared with those produced from diffuser aeration. Analyses indicate a considerable amount of organic enrichment in the jet-produced particles relative to the bulk seawater composition when sodium laurate, an organic surfactant, is present in the seawater. In this case, the production of a thick foam layer during impingement may explain the difference in activation and supports hypotheses that particle production from the two methods of generating bubbles is not equal. PMID:22809370

  11. 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

  12. 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

  13. Biogenic secondary organic aerosol over the United States: Comparison of climatological simulations with observations

    NASA Astrophysics Data System (ADS)

    Liao, Hong; Henze, Daven K.; Seinfeld, John H.; Wu, Shiliang; Mickley, Loretta J.

    2007-03-01

    Understanding the effects of global climate change on regional air quality is central in future air quality planning. We report here on the use of the Goddard Institute for Space Studies (GISS) general circulation model (GCM) III to drive the GEOS-CHEM global atmospheric chemical transport model to simulate climatological present-day aerosol levels over the United States. Evaluation of model predictions using surface measurements from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network indicates that the GISS GCM III/GEOS-CHEM model is a suitable tool for simulating aerosols over the United States in the present climate. The model reproduces fairly well the concentrations of sulfate (mean bias of -0.36 μg m-3, normalized mean bias (NMB) of -25.9%), black carbon (-0.004 μg m-3, -1.9%), organic carbon that comprises primary and secondary components (-0.56 μg m-3, -34.2%), and PM2.5 (-0.87 μg m-3, -20.4%). Nitrate concentrations are overpredicted in the western United States (west of 95°W) with a NMB of +75.6% and underestimated in the eastern United States with a NMB of -54.4%. Special attention is paid to biogenic secondary organic aerosol (SOA). The highest predicted seasonal mean SOA concentrations of 1-2 μg m-3 and 0.5-1.5 μg m-3 are predicted over the northwestern and southeastern United States, respectively, in the months of June-July-August. Isoprene is predicted to contribute 49.5% of the biogenic SOA burden over the United States, with the rest explained by the oxidation of terpenes. Predicted biogenic SOA concentrations are in reasonable agreement with inferred SOA levels from IMPROVE measurements. On an annual basis, SOA is predicted to contribute 10-20% of PM2.5 mass in the southeastern United States, as high as 38% in the northwest and about 5-15% in other regions, indicating the important role of SOA in understanding air quality and visibility over the United States.

  14. 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.

  15. 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

  16. A Survey of Airborne Observations of Biological Aerosol over the Continental United States during NASA SEAC4RS

    NASA Astrophysics Data System (ADS)

    Ziemba, L. D.; Venkateswaran, K.; Froyd, K.; Dibb, J. E.; Beyersdorf, A. J.; Chen, G.; Crumeyrolle, S.; Hudgins, C.; Lin, J. J.; Moore, R.; Thornhill, K. L.; Winstead, E.; Anderson, B. E.

    2013-12-01

    Aerosols play a significant role in regulating Earth's climate. Biological aerosols exist in the atmosphere in many forms including bacteria, fungal spores, pollens, viruses, and plant detritus. While laboratory studies have illustrated the potential for biological aerosol to act as efficient ice nuclei, ambient observations do not clearly show the significance of this mechanism for ice formation. Particularly lacking for assessing the role of biological aerosol on cloud processes are observations of the vertical extent of biological aerosol, especially in conjunction with strong convection as a pathway for redistributing particles from surface sources to the free troposphere. An extensive suite of instrumentation measuring aerosol chemical, physical, and optical properties was deployed aboard the NASA DC-8 aircraft during the SEAC4RS campaign (Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys) in August/September of 2013. Flights were focused on characterizing emissions and transport of aerosols in the Southeast United States, a region characterized by strong biogenic activity. Additionally, convection associated with the North American Monsoon and Atlantic-basin hurricanes was targeted. Airborne biological aerosol was specifically measured during SEAC4RS with a Wideband Integrated Bioaerosol Sensor (WIBS-4A, Droplet Measurement Technologies). WIBS-4A utilizes a single-particle laser-induced fluorescence technique at two excitation wavelengths (280nm and 370nm) to identify biological aerosol, in addition to simultaneous determination of optical size and asymmetry factor for particles with diameter greater than 800nm. Single-particle mass spectrometry coupled with filter-based chemical composition and bacterial speciation analyses will be used to assess relationships with co-emitted mineral dusts. Vertical profiles for the background atmosphere will be compared to profiles influenced by convective storms to assess

  17. 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

  18. 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

  19. 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

  20. 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.

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

    DOE PAGESBeta

    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

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

    DOE PAGESBeta

    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

  3. Pseudosteady-state mixed convection inside rotating spherical containers

    SciTech Connect

    Khodadadi, J.M.; Li, W.; Shi, X.

    1999-07-01

    A computational study of the pseudosteady-state two-dimensional mixed convection within rotating spherical containers is presented. The computations are based on an iterative, finite-volume numerical procedure using primitive dependent variables, whereby the time-dependent continuity, momentum and energy equations in the spherical coordinate system are solved. Natural convection effect is modeled via the Boussinesq approximation. For a fixed Prandtl number of 4.62, parametric studies were performed by varying the Rayleigh number in order to cover the laminar regime adequately. For a given Rayleigh number, the ratio of Gr/Re{sup 2} was varied between 0.1 and 10. Given a Rayleigh number, the streamline patterns maintain their general shape with a dominant rotating vortex. As the forced convection effect becomes less marked, the streamlines exhibit less pronounced gradients near the surface of the sphere. As the rotational effect become more marked, the extent of the deviation from the limiting case of non-rotating spheres becomes more noticed. However, the bottom of the sphere still remains to be the region with enhanced heat transfer. Given a rotational Reynolds number, the streamline patterns are not affected greatly as the natural convection is promoted, however the temperature gradients near the surface are markedly enhanced. It is noticed that as natural convection effects are promoted, the greater portion of the sphere's surface experiences enhanced heat transfer rates. Given a Rayleigh number, the contours of the azimuthal velocity exhibit a nearly vertical equally-spaced pattern suggesting that solid-body rotation for high rotational Reynolds numbers. However, as the natural convection effects are enhanced, the contours become more slanted. The variation of the mean Nusselt number with the Reynolds and Rayleigh numbers is also quantified.

  4. Inversion of tropospheric profiles of aerosol extinction and HCHO and NO2 mixing ratios from MAX-DOAS observations in Milano during the summer of 2003 and comparison with independent data sets

    NASA Astrophysics Data System (ADS)

    Wagner, T.; Beirle, S.; Brauers, T.; Deutschmann, T.; Frieß, U.; Hak, C.; Halla, J. D.; Heue, K. P.; Junkermann, W.; Li, X.; Platt, U.; Pundt-Gruber, I.

    2011-12-01

    We present aerosol and trace gas profiles derived from MAX-DOAS observations. Our inversion scheme is based on simple profile parameterisations used as input for an atmospheric radiative transfer model (forward model). From a least squares fit of the forward model to the MAX-DOAS measurements, two profile parameters are retrieved including integrated quantities (aerosol optical depth or trace gas vertical column density), and parameters describing the height and shape of the respective profiles. From these results, the aerosol extinction and trace gas mixing ratios can also be calculated. We apply the profile inversion to MAX-DOAS observations during a measurement campaign in Milano, Italy, September 2003, which allowed simultaneous observations from three telescopes (directed to north, west, south). Profile inversions for aerosols and trace gases were possible on 23 days. Especially in the middle of the campaign (17-20 September 2003), enhanced values of aerosol optical depth and NO2 and HCHO mixing ratios were found. The retrieved layer heights were typically similar for HCHO and aerosols. For NO2, lower layer heights were found, which increased during the day. The MAX-DOAS inversion results are compared to independent measurements: (1) aerosol optical depth measured at an AERONET station at Ispra; (2) near-surface NO2 and HCHO (formaldehyde) mixing ratios measured by long path DOAS and Hantzsch instruments at Bresso; (3) vertical profiles of HCHO and aerosols measured by an ultra light aircraft. Depending on the viewing direction, the aerosol optical depths from MAX-DOAS are either smaller or larger than those from AERONET observations. Similar comparison results are found for the MAX-DOAS NO2 mixing ratios versus long path DOAS measurements. In contrast, the MAX-DOAS HCHO mixing ratios are generally higher than those from long path DOAS or Hantzsch instruments. The comparison of the HCHO and aerosol profiles from the aircraft showed reasonable agreement with

  5. Inversion of tropospheric profiles of aerosol extinction and HCHO and NO2 mixing ratios from MAX-DOAS observations in Milano during the summer of 2003 and comparison with independent data sets

    NASA Astrophysics Data System (ADS)

    Wagner, T.; Beirle, S.; Brauers, T.; Deutschmann, T.; Frieß, U.; Hak, C.; Halla, J. D.; Heue, K. P.; Junkermann, W.; Li, X.; Platt, U.; Pundt-Gruber, I.

    2011-06-01

    We present aerosol and trace gas profiles derived from MAX-DOAS observations. Our inversion scheme is based on simple profile parameterisations used as input for an atmospheric radiative transfer model (forward model). From a least squares fit of the forward model to the MAX-DOAS measurements, two profile parameters are retrieved including integrated quantities (aerosol optical depth or trace gas vertical column density), and parameters describing the height and shape of the respective profiles. From these results, the aerosol extinction and trace gas mixing ratios can also be calculated. We apply the profile inversion to MAX-DOAS observations during a measurement campaign in Milano, Italy, September 2003, which allowed simultaneous observations from three telescopes (directed to north, west, south). Profile inversions for aerosols and trace gases were possible on 23 days. Especially in the middle of the campaign (17-20 September 2003), enhanced values of aerosol optical depth and NO2 and HCHO mixing ratios were found. The retrieved layer heights were typically similar for HCHO and aerosols. For NO2, lower layer heights were found, which increased during the day. The MAX-DOAS inversion results are compared to independent measurements: (1) aerosol optical depth measured at an AERONET station at Ispra; (2) near-surface NO2 and HCHO (formaldehyde) mixing ratios measured by long path DOAS and Hantzsch instruments at Bresso; (3) vertical profiles of HCHO and aerosols measured by an ultra light aircraft. Depending on the viewing direction, the aerosol optical depths from MAX-DOAS are either smaller or larger than those from AERONET observations. Similar comparison results are found for the MAX-DOAS NO2 mixing ratios versus long path DOAS measurements. In contrast, the MAX-DOAS HCHO mixing ratios are generally higher than those from long path DOAS or Hantzsch instruments. The comparison of the HCHO and aerosol profiles from the aircraft showed reasonable agreement with

  6. 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).

  7. 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

  8. Aerosols in the arid southwestern United States - Measurements of mass loading, volatility, size distribution, absorption characteristics, black carbon content, and vertical structure to 7 km above sea level

    NASA Astrophysics Data System (ADS)

    Pinnick, R. G.; Fernandez, G.; Martinez-Andazola, E.; Hinds, B. D.; Hansen, A. D. A.; Fuller, K.

    1993-02-01

    A variety of methods and sensors including quartz fiber filter samplers, hi-vol samplers, ground-based and aircraft-mounted light-scattering aerosol counters, an aerosol counter equipped with a heated inlet, and an aethalometer are used to determine near-surface and lower tropospheric aerosol characteristics at several remote sites near Orogrande, New Mexico. The results of these measurements, which were taken sporadically over the last 15 yr, suggest that regardless of season, aerosol consists of two modes - a submicron fraction composed primarily of ammonium/acid sulfates and elemental black carbon and a supermicron fraction composed mainly of quartz and clay minerals of soil origin. Limited aircraft measurements in the lowest few kilometers of the troposphere reveal a well-mixed aerosol for a neutral atmospheric condition, and a significant decrease in aerosol concentration with altitude for a stable atmospheric condition.

  9. 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. PMID:27500029

  10. 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.

  11. Uranium oxide and sodium oxide aerosol experiments: NSPP mixed-oxide tests 303-307, data record report. [LMFBR

    SciTech Connect

    Adams, R.E.; Kress, T.S.; Tobias, M.L.

    1982-10-01

    This data record report summarizes five tests, involving mixtures of uranium oxide and sodium oxide aerosols, conducted in the Nuclear Safety Pilot Plant project at Oak Ridge National Laboratory. The goal of this project is to establish the validity (or level of conservatism) of the aerosol behavioral code, HAARM-3, and follow-on codes under development at Battelle Columbus Laboratories for the US Nuclear Regulatory Commission. Descriptions of the five tests with tables and graphs summarizing the results are included.

  12. 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.

  13. Optical-chemical-microphysical relationships and closure studies for mixed carbonaceous aerosols observed at Jeju Island; 3-laser photoacoustic spectrometer, particle sizing, and filter analysis

    NASA Astrophysics Data System (ADS)

    Flowers, B. A.; Dubey, M. K.; Mazzoleni, C.; Stone, E. A.; Schauer, J. J.; Kim, S.-W.; Yoon, S. C.

    2010-11-01

    Transport of aerosols in pollution plumes from the mainland Asian continent was observed in situ at Jeju, South Korea during the Cheju Asian Brown Cloud Plume-Asian Monsoon Experiment (CAPMEX) field campaign throughout August and September 2008 using a 3-laser photoacoustic spectrometer (PASS-3), chemical filter analysis, and size distributions. The PASS-3 directly measures the effects of morphology (e.g. coatings) on light absorption that traditional filter-based instruments are unable to address. Transport of mixed sulfate, carbonaceous, and nitrate aerosols from various Asian pollution plumes to Jeju accounted for 74% of the deployment days, showing large variations in their measured chemical and optical properties. Analysis of eight distinct episodes, spanning wide ranges of chemical composition, optical properties, and source regions, reveals that episodes with higher organic carbon (OC)/sulfate (SO42-) and nitrate (NO3-)/SO42- composition ratios exhibit lower single scatter albedo at shorter wavelengths (ω405). We infer complex refractive indices (n-ik) as a function of wavelength for the high, intermediate, and low OC/SO42- pollution episodes by using the observed particle size distributions and the measured optical properties. The smallest mean particle diameter corresponds to the high OC/SO42- aerosol episode. The imaginary part of the refractive index (k) is greater for the high OC/SO42- episode at all wavelengths. A distinct, sharp increase in k at short wavelength implies enhanced light absorption by OC, which accounts for 50% of the light absorption at 405 nm, in the high OC/SO42- episode. Idealized analysis indicates increased absorption at 781 nm by factors greater than 3 relative to denuded black carbon in the laboratory. We hypothesize that coatings of black carbon cores are the mechanism of this enhancement. This implies that climate warming and atmospheric heating rates from black carbon particles can be significantly larger than have been

  14. 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

  15. Effects of cloudy/clear air mixing and droplet pH on sulfate aerosol formation in a coupled chemistry/climate global model

    SciTech Connect

    Molenkamp, C.R.; Atherton, C.A.; Penner, J.E.; Walton, J.J.

    1996-10-01

    In this paper we will briefly describe our coupled ECHAM/GRANTOUR model, provide a detailed description of our atmospheric chemistry parameterizations, and discuss a couple of numerical experiments in which we explore the influence of assumed pH and rate of mixing between cloudy and clear air on aqueous sulfate formation and concentration. We have used our tropospheric chemistry and transport model, GRANTOUR, to estimate the life cycle and global distributions of many trace species. Recently, we have coupled GRANTOUR with the ECHAM global climate model, which provides several enhanced capabilities in the representation of aerosol interactions.

  16. 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.

  17. Aerosol spectral optical depths of the South Asian winter haze at a tropical coastal site in India under background state of the stratospheric aerosol

    NASA Astrophysics Data System (ADS)

    Balla, M.

    2012-12-01

    Every year during the South Asian winter and pre-monsoon periods most of the Indian subcontinent, the Bay of Bengal and the adjoining tropical Indian Ocean are affected by a synoptic transport of polluted aerosol from the continent in the northern hemisphere, known as the South Asian Winter Haze (SAWH). Visakhapatnam (17.7 deg N, 83.3 deg E), a tropical coastal station in India, is also affected by this anthropogenic regional haze. In spite of the usual clear blue skies and clean maritime airmasses hazy skies associated with public health effects, and higher values of spectral optical depths and near-surface aerosol mass concentrations have become a regular scenario at Visakhapatnam and its environs during wintertime. For an accurate assessment of the possible direct and indirect effects aerosol spectral optical depth of this lower atmospheric haze must be obtained. The problem of retrieving spectral optical depths of the SAWH from atmospheric optical depths by ground-based solar radiometry and inter-channel correlations was discussed in our recent article [Rao, B.M. and Niranjan, K., 2012. Optical properties of the South Asian winter haze at a tropical coastal site in India, Atmos. Environ. 54, 449-455]. The present work is concerned with the retrieval of SAWH AOD at Visakhapatnam under background state of the stratospheric aerosol. The SAWH AODs (spectral values) obtained for two successive winter seasons during the years 2002, 2003 and 2004 are compared with their columnar counterparts (obtained by a conventional method) and the results are discussed.

  18. Neutrino production states in oscillation phenomena—are they pure or mixed?

    NASA Astrophysics Data System (ADS)

    Ochman, Michał; Szafron, Robert; Zrałek, Marek

    2008-06-01

    General quantum mechanical states of neutrinos produced by mechanisms outside the Standard Model are discussed. The neutrino state is described by the Maki-Nakagawa-Sakata-Pontecorvo unitary mixing matrix only in the case of relativistic neutrinos and Standard Model left-handed charge-current interaction. The problem of Wigner spin rotation caused by Lorentz transformation from the rest production frame to the laboratory frame is considered. Moreover, the mixture of the neutrino states as a function of their energy and parameters from the extension of the Standard Model are investigated. Two sources of mixture, the appearance of subdominant helicity states and mass mixing with several different mixing matrices are studied.

  19. 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.

  20. 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.

  1. 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.

  2. 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.

  3. 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

  4. 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.

  5. 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.

  6. 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.

  7. 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.

  8. 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.

  9. 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.

  10. 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

  11. State-Mixing of nS Rydberg Atoms in an External Electric Field

    NASA Astrophysics Data System (ADS)

    Jiao, Yuechun; Wang, Limei; Zhang, Hao; Zhang, Linjie; Zhao, Jianming; Jia, Suotang

    2015-09-01

    State-mixing effect of ultracold nS cesium Rydberg atoms in an external electric field is investigated in a magneto-optical trap. Populated high-l Rydberg atoms due to the state-mixing through avoided crossings are measured with a state-selective field ionization technique. The measured transfer rates of high-l states increase with the electric field and get to the maximum at the field of about 3.0 V/cm for 49S1/2 Rydberg state, and show decrease behavior when the electric field increases further. The decrease behavior of the transfer rate is explained with the slower m-mixing effect caused by decreasing dipole-dipole interactions between high-l Rydberg atoms. During the m-mixing process the ultracold plasma is formed by the Penning ionization.

  12. Coupling aerosol optics to the chemical transport model MATCH (v5.5.0) and aerosol dynamics module SALSA (v1)

    NASA Astrophysics Data System (ADS)

    Andersson, E.; Kahnert, M.

    2015-12-01

    Modelling aerosol optical properties is a notoriously difficult task due to the particles' complex morphologies and compositions. Yet aerosols and their optical properties are important for Earth system modelling and remote sensing applications. Operational optics models often make drastic and non realistic approximations regarding morphological properties, which can introduce errors. In this study a new aerosol optics model is implemented, in which more realistic morphologies and mixing states are assumed, especially for black carbon aerosols. 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 radiative fluxes, backscattering coefficients and the Ångström exponent from the new optics model are compared with results from another model simulating particles as externally mixed homogeneous spheres. To gauge the impact on the optical properties from the new optics model, the known and important effects from using aerosol dynamics serves as a reference. The results show that using a more detailed description of particle morphology and mixing states influences the optical properties to the same degree as aerosol dynamics. This is an important finding suggesting that over-simplified optics models coupled to a chemical transport model can introduce considerable errors; this can strongly effect simulations of radiative fluxes in Earth-system models, and it can compromise the use of remote sensing observations of aerosols in model evaluations and chemical data assimilation.

  13. 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

  14. 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.

  15. “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...

  16. 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.

  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

    NASA Astrophysics Data System (ADS)

    Zhang, Cheng-Jie; Han, Yong-Jian; Zhang, Yong-Sheng; Wu, Yu-Chun; Zhou, Xiang-Fa; Guo, Guang-Can

    2010-12-01

    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. 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.

  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. Symmetric mixed states of n qubits: Local unitary stabilizers and entanglement classes

    SciTech Connect

    Lyons, David W.; Walck, Scott N.

    2011-10-15

    We classify, up to local unitary equivalence, local unitary stabilizer Lie algebras for symmetric mixed states of n qubits into six classes. These include the stabilizer types of the Werner states, the Greenberger-Horne-Zeilinger state and its generalizations, and Dicke states. For all but the zero algebra, we classify entanglement types (local unitary equivalence classes) of symmetric mixed states that have those stabilizers. We make use of the identification of symmetric density matrices with polynomials in three variables with real coefficients and apply the representation theory of SO(3) on this space of polynomials.

  2. Separability criteria for mixed three-qubit states

    SciTech Connect

    Szalay, Szilard

    2011-06-15

    We study the noisy GHZ-W mixture (where GHZ denotes Greenberger-Horne-Zeilinger). We demonstrate some necessary but not sufficient criteria for different classes of separability of these states. It turns out that the partial transposition criterion of Peres [Phys. Rev. Lett. 77, 1413 (1996)] and the criteria of Guehne and Seevinck [New J. Phys. 12, 053002 (2010)] dealing with matrix elements are the strongest ones for different separability classes of this two-parameter state. As a result, we determine a set of entangled states of positive partial transpose.

  3. 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.

  4. 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

  5. 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...

  6. 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...

  7. 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.

  8. The impact of aerosol optical depth assimilation on aerosol forecasts and radiative effects during a wild fire event over the United States

    NASA Astrophysics Data System (ADS)

    Chen, D.; Liu, Z.; Schwartz, C. S.; Lin, H.-C.; Cetola, J. D.; Gu, Y.; Xue, L.

    2014-11-01

    The Gridpoint Statistical Interpolation three-dimensional variational data assimilation (DA) system coupled with the Weather Research and Forecasting/Chemistry (WRF/Chem) model was utilized to improve aerosol forecasts and study aerosol direct and semi-direct radiative feedbacks during a US wild fire event. Assimilation of MODIS total 550 nm aerosol optical depth (AOD) retrievals clearly improved WRF/Chem forecasts of surface PM2.5 and organic carbon (OC) compared to the corresponding forecasts without aerosol data assimilation. The scattering aerosols in the fire downwind region typically cooled layers both above and below the aerosol layer and suppressed convection and clouds, which led to an average of 2% precipitation decrease during the fire week. This study demonstrated that, even with no input of fire emissions, AOD DA improved the aerosol forecasts and allowed a more realistic model simulation of aerosol radiative effects.

  9. The impact of aerosol optical depth assimilation on aerosol forecasts and radiative effects during a wild fire event over the United States

    NASA Astrophysics Data System (ADS)

    Chen, D.; Liu, Z.; Schwartz, C. S.; Lin, H.-C.; Cetola, J. D.; Gu, Y.; Xue, L.

    2014-06-01

    The Gridpoint Statistical Interpolation three-dimensional variational data assimilation (DA) system coupled with the Weather Research and Forecasting/Chemistry (WRF/Chem) model was utilized to improve aerosol forecasts and study aerosol direct and semi-direct radiative feedbacks during a US wild fire event. Assimilation of MODIS total 550 nm aerosol optical depth (AOD) retrievals clearly improved WRF/Chem forecasts of surface PM2.5 and organic carbon (OC) compared to the corresponding forecasts without aerosol data assimilation. The scattering aerosols in the fire downwind region typically cooled layers both above and below the aerosol layer and suppressed convection and clouds, which led to an average 2% precipitation decease during the fire week. This study demonstrated that even with no input of fire emissions, AOD DA improved the aerosol forecasts and allowed a more realistic model simulation of aerosol radiative effects.

  10. 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.

  11. An Upper Bound of Fully Entangled Fraction of Mixed States

    NASA Astrophysics Data System (ADS)

    Huang, Xiao-Fen; Jing, Nai-Huan; Zhang, Ting-Gui

    2016-06-01

    We study the fully entangled fraction of a quantum state. An upper bound is obtained for arbitrary bipartite system. This upper bound only depends on the Frobenius norm of the state. Supported by the National Natural Science Foundation of China under Grant Nos. 11401032, 11501153, 11271138, and 11531004; the Natural Science Foundation of Hainan Province under Grant Nos. 20151010, 114006 and 20161006; and the Scientific Research Foundation for Colleges of Hainan Province under Grant No. Hnky2015-18 and Simons Foundation under Grant No. 198129

  12. Coupling of four-wave mixing and Raman scattering by ground-state atomic coherence

    NASA Astrophysics Data System (ADS)

    Parniak, Michał; Leszczyński, Adam; Wasilewski, Wojciech

    2016-05-01

    We demonstrate coupling of light resonant to transition between two excited states of rubidium and long-lived ground-state atomic coherence. In our proof-of-principle experiment a nonlinear process of four-wave mixing is used to achieve light emission proportional to independently prepared ground-state atomic coherence. Strong correlations between stimulated Raman-scattering light heralding the generation of ground-state coherence and the four-wave mixing signal are measured and shown to survive the storage period, which is promising in terms of quantum memory applications. The process is characterized as a function of laser detunings.

  13. Mixed Exciton–Charge-Transfer States in Photosystem II: Stark Spectroscopy on Site-Directed Mutants

    PubMed Central

    Romero, Elisabet; Diner, Bruce A.; Nixon, Peter J.; Coleman, Wiliam J.; Dekker, Jan P.; van Grondelle, Rienk

    2012-01-01

    We investigated the electronic structure of the photosystem II reaction center (PSII RC) in relation to the light-induced charge separation process using Stark spectroscopy on a series of site-directed PSII RC mutants from the cyanobacterium Synechocystis sp. PCC 6803. The site-directed mutations modify the protein environment of the cofactors involved in charge separation (PD1, PD2, ChlD1, and PheD1). The results demonstrate that at least two different exciton states are mixed with charge-transfer (CT) states, yielding exciton states with CT character: (PD2δ+PD1δ−ChlD1)∗673nm and (ChlD1δ+PheD1δ−)∗681nm (where the subscript indicates the wavelength of the electronic transition). Moreover, the CT state PD2+PD1− acquires excited-state character due to its mixing with an exciton state, producing (PD2+PD1−)δ∗684nm. We conclude that the states that initiate charge separation are mixed exciton-CT states, and that the degree of mixing between exciton and CT states determines the efficiency of charge separation. In addition, the results reveal that the pigment-protein interactions fine-tune the energy of the exciton and CT states, and hence the mixing between these states. This mixing ultimately controls the selection and efficiency of a specific charge separation pathway, and highlights the capacity of the protein environment to control the functionality of the PSII RC complex. PMID:22853895

  14. 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.

  15. 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.

  16. 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.

  17. 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

  18. Chemical composition, mixing state, size and morphology of Ice nucleating particles at the Jungfraujoch research station, Switzerland

    NASA Astrophysics Data System (ADS)

    Ebert, Martin; Worringen, Annette; Kandler, Konrad; Weinbruch, Stephan; Schenk, Ludwig; Mertes, Stephan; Schmidt, Susan; Schneider, Johannes; Frank, Fabian; Nilius, Björn; Danielczok, Anja; Bingemer, Heinz

    2014-05-01

    An intense field campaign from the Ice Nuclei Research Unit (INUIT) was performed in January and February of 2013 at the High-Alpine Research Station Jungfraujoch (3580 m a.s.l., Switzerland). Main goal was the assessment of microphysical and chemical properties of free-tropospheric ice-nucelating particles. The ice-nucleating particles were discriminated from the total aerosol with the 'Fast Ice Nucleation CHamber' (FINCH; University Frankfurt) and the 'Ice-Selective Inlet' (ISI, Paul Scherer Institute) followed by a pumped counter-stream virtual impactor. The separated ice-nucleating particles were then collected with a nozzle-type impactor. With the 'FRankfurt Ice nuclei Deposition freezinG Experiment' (FRIDGE), aerosol particles are sampled on a silicon wafer, which is than exposed to ice-activating conditions in a static diffusion chamber. The locations of the growing ice crystals are recorded for later analysis. Finally, with the ICE Counter-stream Virtual Impactor (ICE-CVI) atmospheric ice crystals are separated from the total aerosol and their water content is evaporated to retain the ice residual particles, which are then collected also by impactor sampling. All samples were analyzed in a high-resolution scanning electron microscope. By this method, for each particle its size, morphology, mixing-state and chemical composition is obtained. In total approximately 1700 ice nucleating particles were analyzed. Based on their chemical composition, the particles were classified into seven groups: silicates, metal oxides, Ca-rich particles, (aged) sea-salt, soot, sulphates and carbonaceous matter. Sea-salt is considered as artifact and is not regarded as ice nuclei here. The most frequent ice nucleating particles/ice residuals at the Jungfraujoch station are silicates > carbonaceous particles > metal oxides. Calcium-rich particles and soot play a minor role. Similar results are obtained by quasi-parallel measurements with an online single particle laser ablation

  19. 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

  20. 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.

  1. 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

  2. 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...

  3. 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

  4. 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.

  5. Simulated annealing and entanglement of formation for (n ⊗m ) -dimensional mixed states

    NASA Astrophysics Data System (ADS)

    Allende, S.; Altbir, D.; Retamal, J. C.

    2015-08-01

    The simulated annealing algorithm, a method commonly used to calculate properties of condensed-matter systems, is used to calculate entanglement of formation for higher-dimensional mixed states. The method relies on representing a mixed state as a pure state in an enlarged Hilbert space, and on the search for the extension minimizing the convex roof of entanglement of formation. Exact results are found, and predictions for system reservoir dynamics in higher dimensions are confirmed. These findings open the way for new applications of the method in quantum information.

  6. 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.

  7. 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.

  8. 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.

  9. 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

  10. 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

  11. Radiative absorption enhancements due to the mixing state of atmospheric black carbon

    SciTech Connect

    Cappa, Christopher D.; Onasch, Timothy B.; Massoli, Paola; Worsnop, Douglas R.; Bates, Timothy S.; Cross, Eben S.; Davidovits, Paul; Hakala, Jani; Hayden, Katherine; Jobson, Bertram Thomas; Kolesar, K. R.; Lack, D. A.; Lerner, Brian M.; Li, Shao-Meng; Mellon, Daniel; Nuaaman, Ibraheem; Olfert, Jason; Petaja, Tuukka; Quinn, P. K.; Song, Chen; Subramanian, R.; Williams, Eric; Zaveri, Rahul A.

    2012-08-30

    Atmospheric particulate black carbon (BC) leads to warming of the Earth's climate. Many models that include forcing by BC assume that non-BC aerosol species internally mixed with BC enhance BC absorption, often by a factor of {approx}2. However, such model estimates have yet to be clearly validated through atmospheric observations. Here, we report on direct measurements of the absorption enhancement (Eabs) of BC in the atmosphere around California and find that it is negligible at 532 nm and much smaller than predicted from theoretical calculations that are uniquely constrained by observations, suggesting that the warming by BC may be significantly overestimated (factor of 2) in many climate models. Additionally, non-BC particulate matter is found to contribute {approx}10% to the total absorption at 405 nm.

  12. 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

  13. 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

  14. The Effect of State Medicaid Case-Mix Payment on Nursing Home Resident Acuity

    PubMed Central

    Feng, Zhanlian; Grabowski, David C; Intrator, Orna; Mor, Vincent

    2006-01-01

    Objective To examine the relationship between Medicaid case-mix payment and nursing home resident acuity. Data Sources Longitudinal Minimum Data Set (MDS) resident assessments from 1999 to 2002 and Online Survey Certification and Reporting (OSCAR) data from 1996 to 2002, for all freestanding nursing homes in the 48 contiguous U.S. states. Study Design We used a facility fixed-effects model to examine the effect of introducing state case-mix payment on changes in nursing home case-mix acuity. Facility acuity was measured by aggregating the nursing case-mix index (NCMI) from the MDS using the Resource Utilization Group (Version III) resident classification system, separately for new admits and long-stay residents, and by an OSCAR-derived index combining a range of activity of daily living dependencies and special treatment measures. Data Collection/Extraction Methods We followed facilities over the study period to create a longitudinal data file based on the MDS and OSCAR, respectively, and linked facilities with longitudinal data on state case-mix payment policies for the same period. Principal Findings Across three acuity measures and two data sources, we found that states shifting to case-mix payment increased nursing home acuity levels over the study period. Specifically, we observed a 2.5 percent increase in the average acuity of new admits and a 1.3 to 1.4 percent increase in the acuity of long-stay residents, following the introduction of case-mix payment. Conclusions The adoption of case-mix payment increased access to care for higher acuity Medicaid residents. PMID:16899009

  15. 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.

  16. Surface Tension and Critical Supersaturations for Mixed Aerosol Particles Composed of Inorganic and Organic Compounds of Atmospheric Relevance

    NASA Astrophysics Data System (ADS)

    Zamora, I. R.; Jacobson, M. Z.

    2012-12-01

    The interaction between water vapor and aerosol particles in the atmosphere has implications on important processes. Among these are cloud droplet formation and growth, which impact cloud properties and therefore have an indirect effect on climate. A significant fraction of the dry submicron mass of atmospheric aerosols is composed of water-soluble organic carbon (WSOC). Although the WSOC fraction contains a large amount of compounds, most yet unidentified, it can be partitioned into three main categories in order to use a set of model substances to reproduce its behavior. In this study, we chose levoglucosan, succinic acid and Nordic Reference fulvic acid (NRFA) to represent the WSOC categories of neutral compounds, mono-/di-carboxylic acids, and polycarboxylic acids, respectively. We measured the surface tension of aqueous pure NRFA and of five of its mixtures at 298 K using the Wilhemy plate method. Langmuir adsorption parameters for the organic mixtures were extracted by fitting the surface tension measurements and corresponding solute concentrations to the Szyszkowski-Langmuir equation. The measured surface tension as a function of aqueous NRFA concentration was identical to that of Suwannee River (SR) and Waskish Peat fulvic acids below 0.02 g/L but up to 12% and 15% higher, respectively, at higher concentrations. Similar to previous findings by Aumann et al. (2010) with SRFA, the surface tension of a NRFA/inorganic salt solution was mainly controlled by the organic compound even when the salt comprised 75% of the added solute mass. This effect was observed for mixtures of NRFA with both sodium chloride and ammonium sulfate salts up to 5 g/L of NRFA. From 5 g/L to about 50 g/L of NRFA, the surface tension for both NRFA/salt mixtures stopped decreasing, remained constant at 52-53 mN/m and then started slowly increasing indicating that the salt component might start dominating at higher concentrations. For a solution of 25% NRFA / 75% levoglucosan, the surface

  17. 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.

  18. 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.

  19. 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.

  20. 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

  1. Carbonaceous aerosol at two rural locations in New York State: Characterization and behavior

    NASA Astrophysics Data System (ADS)

    Sunder Raman, Ramya; Hopke, Philip K.; Holsen, Thomas M.

    2008-06-01

    Fine particle samples were collected to determine the chemical constituents in PM2.5 at two rural background sites (Potsdam and Stockton, N. Y.) in the northeastern United States from November 2002 to August 2005. Samples were collected every third day for 24 h with a speciation network sampler. The measured carbonaceous species included thermal-optical organic carbon (OC), elemental carbon (EC), pyrolytic carbon (OP), black carbon (BC), and water-soluble, short-chain (WSSC) organic acids. Concentration time series, autocorrelations, and seasonal variations of the carbonaceous species were examined. During this multiyear period, the contributions of the total carbon (OC + EC) to the measured fine particle mass were 31.2% and 31.1% at Potsdam and Stockton, respectively. The average sum of the WSSC acids carbon accounted for approximately 2.5% of the organic carbon at Potsdam and 3.0% at Stockton. At Potsdam, the seasonal differences in the autocorrelation function (ACF) and partial autocorrelation function (PACF) values for carbonaceous species suggest that secondary formation may be an important contributor to the observed concentrations of species likely to be secondary in origin, particularly during the photochemically active time of the year (May to October). This study also investigated the relationships between carbonaceous species to better understand the behavior of carbonaceous aerosol and to assess the contribution of secondary organic carbon (SOC) to the total organic carbon mass (the EC tracer method was used to estimate SOC). At Potsdam the average SOC contribution to total OC varied between 66% and 72%, while at Stockton it varied between 58% and 64%.

  2. 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.

  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. Evaluations of tropospheric aerosol properties simulated by the community earth system model with a sectional aerosol microphysics scheme

    NASA Astrophysics Data System (ADS)

    Yu, Pengfei; Toon, Owen B.; Bardeen, Charles G.; Mills, Michael J.; Fan, Tianyi; English, Jason M.; Neely, Ryan R.

    2015-06-01

    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.

  5. Characterization of polar organic components in fine aerosols in the southeastern United States: Identity, origin, and evolution

    NASA Astrophysics Data System (ADS)

    Gao, Song; Surratt, Jason D.; Knipping, Eladio M.; Edgerton, Eric S.; Shahgholi, Mona; Seinfeld, John H.

    2006-07-01

    Filter samples of fine aerosols collected in the Southeastern United States in June 2004 were analyzed for the characterization of polar organic components. Four analytical techniques, liquid chromatography -mass spectrometry, ion trap mass spectrometry, laser desorption ionization mass spectrometry, and high-resolution mass spectrometry, were used for identification and quantification. Forty distinct species were detected, comprising on average 7.2% and 1.1% of the total particulate organic mass at three inland sites and a coastal site, respectively. The relative abundance of these species displays a rather consistent distribution pattern in the inland region, whereas a different pattern is found at the coastal site. Chemical and correlation analyses suggest that the detected species are secondary in nature and originate from terpene oxidation, with possible participation of NOx and SO2. It is estimated that polar, acidic components in fine aerosols in the Southeastern United States cover a molecular weight range of 150-400 Da and do not appear to be oligomeric. Other components with MW up to 800 Da may also be present. The detected polar organic species are similar to humic-like substances (HULIS) commonly found in fine aerosols in other rural areas. We present the first, direct evidence that atmospheric processing of biogenic emissions can lead to the formation of certain HULIS species in fine aerosols, and that this may be a typical pathway in the background atmosphere in continental regions; nevertheless, a natural source for HULIS, such as from aquatic and/or terrestrial humic/fulvic acids and their degradation products, cannot be precluded.

  6. 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.

  7. 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.

  8. 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

  9. 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

  10. The State of the Art of the DSM-5 "with Mixed Features" Specifier.

    PubMed

    Verdolini, Norma; Agius, Mark; Ferranti, Laura; Moretti, Patrizia; Piselli, Massimiliano; Quartesan, Roberto

    2015-01-01

    The new DSM-5 "with mixed features" specifier (MFS) has renewed the interest of the scientific community in mixed states, leading not only to new clinical studies but also to new criticisms of the current nosology. Consequently, in our paper we have reviewed the latest literature, trying to understand the reactions of psychiatrists to the new nosology and its epidemiological, prognostic, and clinical consequences. It seems that the most widespread major criticism is the exclusion from the DSM-5 MFS of overlapping symptoms (such as psychomotor agitation, irritability, and distractibility), with a consequent reduction in diagnostic power. On the other hand, undoubtedly the new DSM-5 classification has helped to identify more patients suffering from a mixed state by broadening the narrow DSM-IV-TR criteria. As for the clinical presentation, the epidemiological data, and the therapeutic outcomes, the latest literature does not point out a univocal point of view and further research is needed to fully assess the implications of the new DSM-5 MFS. It is our view that a diagnostic category should be preferred to a specifier and mixed states should be better considered as a spectrum of states, according to what was stated many years ago by Kraepelin. PMID:26380368

  11. The State of the Art of the DSM-5 “with Mixed Features” Specifier

    PubMed Central

    Verdolini, Norma; Agius, Mark; Ferranti, Laura; Moretti, Patrizia; Piselli, Massimiliano; Quartesan, Roberto

    2015-01-01

    The new DSM-5 “with mixed features” specifier (MFS) has renewed the interest of the scientific community in mixed states, leading not only to new clinical studies but also to new criticisms of the current nosology. Consequently, in our paper we have reviewed the latest literature, trying to understand the reactions of psychiatrists to the new nosology and its epidemiological, prognostic, and clinical consequences. It seems that the most widespread major criticism is the exclusion from the DSM-5 MFS of overlapping symptoms (such as psychomotor agitation, irritability, and distractibility), with a consequent reduction in diagnostic power. On the other hand, undoubtedly the new DSM-5 classification has helped to identify more patients suffering from a mixed state by broadening the narrow DSM-IV-TR criteria. As for the clinical presentation, the epidemiological data, and the therapeutic outcomes, the latest literature does not point out a univocal point of view and further research is needed to fully assess the implications of the new DSM-5 MFS. It is our view that a diagnostic category should be preferred to a specifier and mixed states should be better considered as a spectrum of states, according to what was stated many years ago by Kraepelin. PMID:26380368

  12. 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.

  13. Development of dry powder inhaler formulation loaded with alendronate solid lipid nanoparticles: solid-state characterization and aerosol dispersion performance.

    PubMed

    Ezzati Nazhad Dolatabadi, Jafar; Hamishehkar, Hamed; Valizadeh, Hadi

    2015-01-01

    Alendronate sodium is a bisphosphonate drug used for the treatment of osteoporosis and acts as a specific inhibitor of osteoclast-mediated bone resorption. Inhalable solid lipid nanoparticles (SLNs) of the alendronate were successfully designed and developed by spray-dried and co-spray dried inhalable mannitol from aqueous solution. Emulsification technique using a simple homogenization method was used for preparation of SLNs. In vitro deposition of the aerosolized drug was studied using a Next Generation Impactor at 60 L/min following the methodology described in the European and United States Pharmacopeias. The Carr's Index, Hausner ratio and angle of repose were calculated as suitable criteria for estimation of the flow behavior of solids. Scanning electron microscopy showed spherical particle morphology of the respirable particles. The proposed spray-dried nanoparticulate-on-microparticles dry powders displayed good aerosol dispersion performance as dry powder inhalers with high values in emitted dose, fine particle fraction and mass median aerodynamic diameter. These results indicate that this novel inhalable spray-dried nanoparticulate-on-microparticles aerosol platform has great potential in systemic delivery of the drug. PMID:25220930

  14. 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.

  15. Spatial variability of carbonaceous aerosols and associated source tracers in two cites in the Midwestern United States

    NASA Astrophysics Data System (ADS)

    Snyder, David C.; Rutter, Andrew P.; Worley, Chris; Olson, Mike; Plourde, Anthony; Bader, Rebecca C.; Dallmann, Timothy; Schauer, James J.

    2010-05-01

    Semi-continuous and 24-h averaged measurements of fine carbonaceous aerosols were made concurrently at three sites within each of two U.S. Midwestern Cities; Detroit, Michigan and Cleveland, Ohio; during two, one-month intensive campaigns conducted in July of 2007 and January & February of 2008. A comparison of 24-h measurements revealed substantial intra-urban variability in carbonaceous aerosols consistent with the influence of local sources, and excesses in both PM 2.5 organic carbon (OC) and elemental carbon (EC) were identified at individual sites within each city. High time-resolved black carbon (BC) measurements indicated that elemental carbon concentrations were higher at sites adjacent to freeways and busy surface streets, and temporal patterns suggested that excess EC at sites adjacent to freeways was dominated by mobile source emissions while excesses in EC away from traffic corridors was dominated by point/area source emissions. The site-to-site variability in OC concentrations was approximately 7% within the neighborhood scale (0.5-4 km) and between 4 and 27% at the urban scale (4-100 km). In contrast, measurements of organic source tracers, in conjunction with a Chemical Mass Balance (CMB) source-apportionment model, indicated that the spatial variation in the contribution of both mobile and stationary sources to PM 2.5 OC often exceeded the variation in OC mass concentration by a factor of 3 or more. Markers for mobile sources, biomass smoke, natural gas, and coal combustion differed by as much as 60% within the neighborhood scale and by greater than 200% within the urban scale. The observations made during this study suggest that the urban excess of carbonaceous aerosols is much more complex than has been previously reported and that a more rigorous, source-oriented approach should be taken in order to assess the risk associated with exposure to carbonaceous aerosols within the industrialized environments of the Midwestern United States.

  16. 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.

  17. An Examination of Carbon Monoxide and Organic Aerosol Mass Sources in the Southeastern United States during the SENEX Project

    NASA Astrophysics Data System (ADS)

    Middlebrook, A. M.; Angevine, W. M.; Brioude, J. F.; Brock, C. A.; De Gouw, J. A.; Gilman, J.; Graus, M.; Hanisco, T. F.; Holloway, J. S.; Horowitz, L. W.; Kaiser, J.; Keutsch, F. N.; Lerner, B. M.; Liao, J.; Mao, J.; Trainer, M.; Warneke, C.; Welti, A.; Wolfe, G. M., Jr.

    2014-12-01

    The NOAA Southeast Nexus (SENEX) project occurred during the summer of 2013 over the southeastern United States and involved studying the interactions between natural and anthropogenic emissions at the nexus of climate change and air quality. As part of the project, a suite of instruments for aerosol and gas-phase species was deployed on the NOAA WP-3D aircraft and models were used to calculate trace gas and aerosol species in the region and along the aircraft flight tracks. Throughout the study, the measured non-refractory submicron aerosol mass was dominated by organic material (58% +/- 9%) with smaller contributions from sulfate (27% +/- 8%), ammonium (10% +/- 3%), nitrate (3% +/- 1%), and chloride (0.1% +/- 0.1%). Here we examine the influence of urban emissions on the organic aerosol (OA) mass in regions characterized by higher and lower biogenic emissions. For the air around and downwind of urban areas, OA mass is highly correlated with carbon monoxide (CO), a tracer of anthropogenic emissions as well as an oxidation product of isoprene, a biogenic species. The slope of this correlation is roughly 0.15 micrograms per standard cubic meter per ppbv, which is significantly higher than observed in prior studies downwind of urban areas. The enhancement in OA mass relative to the enhancement in CO is independent of the concentration of biogenic species. In contrast, formaldehyde enhancements are clearly higher in the presence of biogenic species in agreement with the NOAA GFDL AM3 model. Downwind from the urban areas, CO and OA mass were not strongly enhanced relatively to a region-wide enhancement in these species that can only be explained from the accumulation of emissions in the eastern U.S. for several days. Back-trajectories of air parcels with emissions from biogenic and anthropogenic sources will be examined to elucidate the impact of both sources on CO and OA mass.

  18. NMOC, ozone, and organic aerosol in the southeastern United States, 1999-2007: 3. Origins of organic aerosol in Atlanta, Georgia, and surrounding areas

    NASA Astrophysics Data System (ADS)

    Blanchard, C. L.; Hidy, G. M.; Tanenbaum, S.; Edgerton, E. S.

    2011-02-01

    Carbonaceous compounds constitute a major fraction of the fine particle mass at locations throughout North America; much of the condensed-phase organic carbon (OC) is produced in the atmosphere from NMOC reactions as "secondary" OC (SOC). Ten years of particulate carbon and speciated non-methane organic compound (NMOC) data combined with other measurements from Southeastern Aerosol Research and Characterization (SEARCH) and other sites provide insight into the association between elemental carbon (EC), OC and NMOCs. Data are analyzed to characterize the OC and SOC contrasts between urban Atlanta, Georgia, and nearby non-urban conditions in the Southeast. Analysis of the monitoring record indicates that the mean Atlanta urban excess of total carbon (TC) is 2.1-2.8 μg m -3. The OC/EC ratio of the Atlanta urban excess is in the range 1.3 to 1.8, consistent with OC/EC ratios observed in motor vehicle emissions and a fossil carbon source of urban excess TC. Carbon isotope analysis of a subset of particle samples demonstrates that the urban excess is mainly fossil in origin, even though the majority of the TC is modern at both urban and non-urban sites. Temperature-dependent partitioning of OC between gas and condensed phases cannot explain the observed diurnal and seasonal variations of OC/CO, EC/CO, and OC/EC ratios. Alternatively, a hypothesis involving vertical mixing of OC-enriched air from aloft is supported by the seasonal and diurnal OC, isopentane, aromatic and isoprene observations at the ground. A statistical model is applied to indicate the relative significance of aerometric factors affecting OC and EC concentrations, including meteorological and pollutant associations. The model results demonstrate strong linkages between fine particle carbon and pollutant indicators of source emissions compared with meteorological factors; the model results show weaker dependence of OC on meteorological factors than is the case for ozone (O 3) concentrations.

  19. 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...

  20. Detection and quantification of 2-methyltetrols in ambient aerosol in the southeastern United States

    NASA Astrophysics Data System (ADS)

    Clements, Andrea L.; Seinfeld, John H.

    Filters collected from the Southeastern Aerosol Research and Characterization (SEARCH) air monitoring network were analyzed for the presence of 2-methyltetrols, namely 2-methylthreitol and 2-methylerythritol, two compounds that are products of the photooxidation of isoprene and have been detected in aerosol at a variety of sites around the globe. The 2-methytetrols were detected in ambient filter samples collected at the four SEARCH sites, Birmingham, AL, Centreville, AL, Pensacola, FL, and at Jefferson Street in Atlanta, GA, in late June 2004. Average atmospheric concentrations of 11.9 and 4.8 ng m -3 were measured for 2-methylerythritol and 2-methylthreitol, respectively, at the inland sampling sites, whereas average concentrations of 4.9 and 1.6 ng m -3 were measured at the coastal sampling location (Pensacola). On average, the aerosol loading from these two compounds accounts for approximately 0.42% and 0.21% of the organic mass collected on a given sampling day at the inland and coastal sites, respectively. The present data on these compounds, which are particulate-phase fingerprints of isoprene photooxidation, add to the growing body of ambient data on secondary organic aerosol from isoprene.

  1. 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...

  2. 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

  3. 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.

  4. Using the Mixed Effect Model as an Alternative Approach to Improve Correlation between Satellite Derived Aerosol Optical Depth (MISR & MODIS) and Ground Measured PM2.5 Data

    NASA Astrophysics Data System (ADS)

    Cabanes, H. V. O.; Lagrosas, N.

    2014-12-01

    The study seeks to determine the efficacy of using aerosol optical depth (AOD) data from MISR and MODIS as a surrogate for ground-based particulate matter (PM2.5) data by using AOD as an input for various computational methods. The data set used in the study ranged from January 2011 to December 2012. The advantage of the mixed effects model is in its ability to consider temporally changing attributes through the inclusion of random effects in the regression model. The study first established that MISR and MODIS AOD has a correlation with ground measured PM2.5 through regression analysis thereby providing rationale for further analysis. The regression analyses resulted in an R2 of 0.7513 and 0.7536 for MODIS and MISR, respectively. With the rationale established, data quality improvement measures were carried out through data screening and empirical correction. The data screening process involved the removal of data entries in which the absolute difference of MODIS and MISR AOD values deviated far more than the average of the data set. On the other hand, empirical correction was done by developing correction equations through multivariate regression with ground parameters such as AERONET AOD, relative humidity, and wind speed. Both methods were found to yield marked improvement in the correlation of satellite-derived AOD with PM2.5. After data quality had been improved, several computational methods are assessed by solving for the R2 and absolute error percentage. The methods are simple linear regression with MODIS (R2 = 0.7764, 18.43%) and MISR (R2 = 0.7614, 17.99%), multivariate linear regression with MODIS and MISR together (R2 = 0.8721, 13.63%), artificial neural network with MODIS and MISR as inputs (R2 = 0.8764, 13.45%), and the mixed effects model with MODIS and MISR as predictors (R2 = 0.9793, 5.20%). Among these, the mixed effects model performed the best and further error analysis showing an error that was independent on seasonality and dependent on the PM

  5. 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

  6. 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.

  7. Aerosol effects on cloud cover as evidenced by ground-based and space-based observations at five rural sites in the United States

    NASA Astrophysics Data System (ADS)

    Ten Hoeve, John E.; Augustine, John A.

    2016-01-01

    Previous studies of the second aerosol indirect (lifetime) effect on cloud cover have estimated the strength of the effect without correcting for near-cloud contamination and other confounding factors. Here we combine satellite-based observations with a multiyear ground-based data set across five rural locations in the United States to more accurately constrain the second indirect aerosol effect and quantify aerosol effects on radiative forcing. Results show that near-cloud contamination accounts for approximately 40% of the satellite-derived aerosol-cloud relationship. When contamination is removed and the effect of meteorological covariation is minimized, a strong physical aerosol effect on cloud cover remains. Averaged over all stations and after correcting for contamination, the daytime solar and total (solar + IR) radiative forcing is -52 W/m2 and -19 W/m2, respectively, due to both direct and indirect aerosol effects for aerosol optical depths (τ) between 0 and 0.3. Averaged diurnally, the average total radiative forcing is +16 W/m2.

  8. 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.

    2015-04-01

    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 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 (internal, 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 +1.2 W m-2. The global-mean cloud-albedo aerosol indirect effect 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 effects is unclear due to uncertainties

  9. Optical studies of photoactive states in mixed organic-inorganic hybrid perovskites stabilized in polymers

    NASA Astrophysics Data System (ADS)

    Kardynal, Beata; Xi, Lifei; Salim, Teddy; Borghardt, Sven; Stoica, Toma; Lam, Yeng Ming

    2015-03-01

    Mixed organic-inorganic hybrid perovskites MAX-PbY2(X,Y =I, Br,Cl) have been demonstrated as very attractive materials for absorbers of solar cells and active layers of light emitting diodes and optically driven lasers. The bandgap of the perovskites can be tuned by mixing halogen atoms in different ratios. In this presentation we study mixed MAX-PbY2(X,Y =I, Br, Cl) particles synthesized directly in protective polymer matrices as light emitters. Both, time integrated and time resolved photoluminescence have been used to study the materials. So synthesized MAX-PbX2 are very stable when measured at room temperature and in air with radiative recombination of photogenerated carriers as the main decay path. In contrast, MAX-PbY2 with mixed halogen atoms display luminescence from sub-bandgap states which saturate at higher excitation levels. The density of these states depends on the used polymer matrix and increases upon illumination. We further compare the MAX-PbY2 synthesized in polymers and as films and show that these states are inherent to the material rather than its microstructure. This works has been supported by EU NWs4LIGHT grant.

  10. 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 entangl