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Sample records for aerosol mixing state

  1. 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.

  2. Representation and evaluation of aerosol mixing state in a climate model

    NASA Astrophysics Data System (ADS)

    Bauer, S. E.; Prather, K. A.; Ault, A. P.

    2011-12-01

    Aerosol particles in the atmosphere are composed out of multiple chemical species. The aerosol mixing state is an important aerosol property that will determine the interaction of aerosols with the climate system via radiative forcings and cloud activation. Through the introduction of aerosol microphysics into climate models, aerosol mixing state is by now taken into account to a certain extend in climate models, and evaluation of mixing state is the next challenge. Here we use data from the Aerosol Time of Flight Mass Spectrometer (ATOFMS) and compare the results to the GISS-modelE-MATRIX model, a global climate model including a detailed aerosol micro-physical scheme. We use data from various field campaigns probing, urban, rural and maritime air masses and compare those to climatological and nudged simulations for the years 2005 to 2009. ATOFMS provides information about the size distributions of several mixing state classes, including the chemical components of black and organic carbon, sulfates, dust and salts. MATRIX simulates 16 aerosol populations, which definitions are based on mixing state. We have grouped ATOFMS and MATRIX data into similar mixing state classes and compare the size resolved number concentrations against each other. As a first result we find that climatological simulations are rather difficult to evaluate with field data, and that nudged simulations give a much better agreement. However this is not just caused by the better fit of natural - meteorological driven - aerosol components, but also due to the interaction between meteorology and aerosol formation. The model seems to get the right amount of mixing state of black carbon material with sulfate and organic components, but seems to always overestimate the fraction of black carbon that is externally mixed. In order to understand this bias between model and the ATOFMS data, we will look into microphysical processes near emission sources and investigate the climate relevance of these sub

  3. Calculation of aerosol optical properties under different assumptions on mixing state, refractive index, density and hygroscopicity: uncertainties and importance of representation of aerosol mixing state

    NASA Astrophysics Data System (ADS)

    Curci, Gabriele

    2015-04-01

    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. We used the FlexAOD post-processing tool to calculate the optical properties (aerosol optical depth (AOD), single scattering albedo (SSA) and asymmetry parameter (g)) from chemistry-transport model aerosol profiles, using a wide range of assumptions on aerosol chemical and physical properties. We calculated that the most important factor of uncertainty is the assumption about the mixing state, for which we estimate an uncertainty of 30-35% on the simulated aerosol optical depth (AOD) and single scattering albedo (SSA). The choice of the core composition in the core-shell representation is of minor importance for calculation of AOD, while it is critical for the SSA. Other factors of uncertainty tested here have a maximum average impact of 10% each on calculated AOD, and an impact of a few percent on SSA and g. We then tested simple parameterizations of the aerosol mixing state, expressed as a function of the aerosol aging, and verified that they may be helpful in reducing the uncertainty when comparing simulations with AERONET retrievals.

  4. 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

  5. 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.

  6. MATRIX (Multiconfiguration Aerosol TRacker of mIXing state): an aerosol microphysical module for global atmospheric models

    NASA Astrophysics Data System (ADS)

    Bauer, S. E.; Wright, D.; Koch, D.; Lewis, E. R.; McGraw, R.; Chang, L.-S.; Schwartz, S. E.; Ruedy, R.

    2008-05-01

    A new aerosol microphysical module MATRIX, the Multiconfiguation Aerosol TRacker of mIXing state, and its application in the Goddard Institute for Space Studies (GISS) climate model (ModelE) is described. This module, which is based on the quadrature method of moments (QMOM), represents nucleation, condensation, coagulation, internal and external mixing, and cloud-drop activation and provides aerosol particle mass and number concentration and particle size information for up to 16 mixed-mode aerosol populations. Internal and external mixing among aerosol components sulfate, nitrate, ammonium, carbonaceous aerosols, dust and sea-salt particles are represented. The solubility of each aerosol mode, which is explicitly calculated based on its soluble and insoluble components, enables calculation of the dependence of cloud drop activation on the microphysical characterization of multiple soluble modes. A detailed model description and results of box-model simulations of various mode configurations are presented. The number concentration of aerosol particles activated to cloud drops depends on the mode configuration. Simulations on the global scale with the GISS climate model are evaluated against aircraft and station measurements of aerosol mass and number concentration and particle size. The model accurately captures the observed size distributions in the aitken and accumulation modes up to particle diameter 1 μm, in which sulfate, nitrate, black and organic carbon are predominantly located; however the model underestimates coarse-mode number concentration and size, especially in the marine environment.

  7. MATRIX (Multiconfiguration Aerosol TRacker of mIXing state): an aerosol microphysical module for global atmospheric models

    NASA Astrophysics Data System (ADS)

    Bauer, S. E.; Wright, D. L.; Koch, D.; Lewis, E. R.; McGraw, R.; Chang, L.-S.; Schwartz, S. E.; Ruedy, R.

    2008-10-01

    A new aerosol microphysical module MATRIX, the Multiconfiguration Aerosol TRacker of mIXing state, and its application in the Goddard Institute for Space Studies (GISS) climate model (ModelE) are described. This module, which is based on the quadrature method of moments (QMOM), represents nucleation, condensation, coagulation, internal and external mixing, and cloud-drop activation and provides aerosol particle mass and number concentration and particle size information for up to 16 mixed-mode aerosol populations. Internal and external mixing among aerosol components sulfate, nitrate, ammonium, carbonaceous aerosols, dust and sea-salt particles are represented. The solubility of each aerosol population, which is explicitly calculated based on its soluble and insoluble components, enables calculation of the dependence of cloud drop activation on the microphysical characterization of multiple soluble aerosol populations. A detailed model description and results of box-model simulations of various aerosol population configurations are presented. The box model experiments demonstrate the dependence of cloud activating aerosol number concentration on the aerosol population configuration; comparisons to sectional models are quite favorable. MATRIX is incorporated into the GISS climate model and simulations are carried out primarily to assess its performance/efficiency for global-scale atmospheric model application. Simulation results were compared with aircraft and station measurements of aerosol mass and number concentration and particle size to assess the ability of the new method to yield data suitable for such comparison. The model accurately captures the observed size distributions in the Aitken and accumulation modes up to particle diameter 1 μm, in which sulfate, nitrate, black and organic carbon are predominantly located; however the model underestimates coarse-mode number concentration and size, especially in the marine environment. This is more likely due to

  8. 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.

  9. Black carbon mixing state impacts on cloud microphysical properties: effects of aerosol plume and environmental conditions

    SciTech Connect

    Ching, Ping Pui; Riemer, Nicole; West, Matthew

    2016-05-27

    Black carbon (BC) is usually mixed with other aerosol species within individual aerosol particles. This mixture, along with the particles' size and morphology, determines the particles' optical and cloud condensation nuclei properties, and hence black carbon's climate impacts. In this study the particle-resolved aerosol model PartMC-MOSAIC was used to quantify the importance of black carbon mixing state for predicting cloud microphysical quantities. Based on a set of about 100 cloud parcel simulations a process level analysis framework was developed to attribute the response in cloud microphysical properties to changes in the underlying aerosol population ("plume effect") and the cloud parcel cooling rate ("parcel effect"). It shows that the response of cloud droplet number concentration to changes in BC emissions depends on the BC mixing state. When the aerosol population contains mainly aged BC particles an increase in BC emission results in increasing cloud droplet number concentrations ("additive effect"). In contrast, when the aerosol population contains mainly fresh BC particles they act as sinks for condensable gaseous species, resulting in a decrease in cloud droplet number concentration as BC emissions are increased ("competition effect"). Additionally, we quantified the error in cloud microphysical quantities when neglecting the information on BC mixing state, which is often done in aerosol models. The errors ranged from -12% to +45% for the cloud droplet number fraction, from 0% to +1022% for the nucleation-scavenged black carbon (BC) mass fraction, from -12% to +4% for the effective radius, and from -30% to +60% for the relative dispersion.

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

    SciTech Connect

    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) 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. 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.

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

    DOE PAGES

    Willis, Megan D.; Healy, Robert M.; Riemer, Nicole; ...

    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

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

    DOE PAGES

    O'Brien, Rachel E.; Wang, Bingbing; Laskin, Alexander; ...

    2015-08-26

    In this study, 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 themore » 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.« less

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

    SciTech Connect

    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.

    2015-08-26

    In this study, 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.

  14. 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

  15. 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.

  16. 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.

  17. Influence of the external mixing state of atmospheric aerosol on derived CCN number concentrations

    NASA Astrophysics Data System (ADS)

    Wex, H.; McFiggans, G.; Henning, S.; Stratmann, F.

    2010-05-01

    We derived the range of particle hygroscopicities ($\\kappa$) that occurs in the atmosphere, based on literature data of measured hygroscopic growth or based on chemical composition. The derived $\\kappa$-values show that the atmospheric aerosol often is an external mixture with respect to hygroscopicity. Mean $\\kappa$ were derived for urban, rural, and marine aerosols for the different hygroscopic modes. Using these $\\kappa$ and exemplary particle number size distributions for the different aerosols, the number concentration of cloud condensation nuclei (NCCN) was derived for two cases, (1) accounting for the less hygroscopic fraction of particles and (2) assuming all particles to have $\\kappa$ of the more hygroscopic mode. NCCN derived from measured particle hygroscopicity is overestimated for case (2). Overestimation of NCCN is largest for fresh continental aerosol and less pronounced for marine aerosol. With $\\kappa$ derived from bulk aerosol composition data, only the hygroscopicity of more soluble aerosol particles is captured. Bulk or even size-resolved composition data will be insufficient to predict NCCN under many conditions unless independent information about particle mixing state is available.

  18. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2011-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  1. Impact of mixing state and hygroscopicity on CCN activity of biomass burning aerosol in Amazonia

    NASA Astrophysics Data System (ADS)

    Sánchez Gácita, Madeleine; Longo, Karla M.; Freire, Julliana L. M.; Freitas, Saulo R.; Martin, Scot T.

    2017-02-01

    Smoke aerosols prevail throughout Amazonia because of widespread biomass burning during the dry season, and external mixing, low variability in the particle size distribution and low particle hygroscopicity are typical. There can be profound effects on cloud properties. This study uses an adiabatic cloud model to simulate the activation of smoke particles as cloud condensation nuclei (CCN) for three hypothetical case studies, chosen as to resemble biomass burning aerosol observations in Amazonia. The relative importance of variability in hygroscopicity, mixing state, and activation kinetics for the activated fraction and maximum supersaturation is assessed. For a population with κp = 0.04, an overestimation of the cloud droplet number concentration Nd for the three selected case studies between 22.4 ± 1.4 and 54.3 ± 3.7 % was obtained when assuming a hygroscopicity parameter κp = 0.20. Assuming internal mixing of the aerosol population led to overestimations of up to 20 % of Nd when a group of particles with medium hygroscopicity was present in the externally mixed population cases. However, the overestimations were below 10 % for external mixtures between very low and low-hygroscopicity particles, as seems to be the case for Amazon smoke particles. Kinetic limitations were significant for medium- and high-hygroscopicity particles, and much lower for very low and low-hygroscopicity particles. When particles were assumed to be at equilibrium and to respond instantly to changes in the air parcel supersaturation, the overestimation of the droplet concentration was up to ˜ 100 % in internally mixed populations, and up to ˜ 250 % in externally mixed ones, being larger for the higher values of hygroscopicity. In addition, a perceptible delay between the times when maximum supersaturation and maximum aerosol activated fraction are reached was noticed and, for aerosol populations with effective hygroscopicity κpeff higher than a certain threshold value, the delay in

  2. 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

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

    NASA Astrophysics Data System (ADS)

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

    2011-12-01

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

  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.

    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

  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.

    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

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

    NASA Astrophysics Data System (ADS)

    Cahill, J. F.; Suski, K.; Seinfeld, J. H.; Zaveri, R. A.; Prather, K. A.

    2012-11-01

    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 influences their optical properties, hygroscopicity, and atmospheric lifetime, thus impacting climate forcing. 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 are internally mixed and the variability of their mixing state in California during the Carbonaceous Aerosols 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 in California are internally mixed and are heavily influenced by secondary species that are most prevalent in the particular 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

  9. The mixing state of carbonaceous aerosol particles in Northern and Southern California measured during CARES and CalNex 2010

    NASA Astrophysics Data System (ADS)

    Cahill, J. F.; Suski, K.; Seinfeld, J. H.; Zaveri, R. A.; Prather, K. A.

    2012-07-01

    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 influences their optical properties, hygroscopicity, and atmospheric lifetime, thus impacting climate forcing. 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 are internally mixed and the variability of their mixing state in California during the Carbonaceous Aerosols 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 in California are internally mixed and are heavily influenced by secondary species that are most prevalent in the particular 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

  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. A three-dimensional sectional representation of aerosol mixing state for simulating optical properties and cloud condensation nuclei

    SciTech Connect

    Ching, Ping Pui; Zaveri, Rahul A.; Easter, Richard C.; Riemer, Nicole; Fast, Jerome D.

    2016-05-27

    Light absorption by black carbon (BC) particles emitted from fossil fuel combustion depends on the how thickly they are coated with non-refractory species such as ammonium, sulfate, nitrate, organics, and water. The cloud condensation nuclei (CCN) activation property of a particle depends on its dry size and the hygroscopicities of all the individual species mixed together. It is therefore necessary to represent both size and mixing state of aerosols to reliably predict their climate-relevant properties in atmospheric models. Here we describe and evaluate a novel sectional framework in the Model for Simulating Aerosol Interactions and Chemistry, referred to as MOSAIC-mix, that represents the mixing state by resolving aerosol dry size (Ddry), BC dry mass fraction (wBC), and hygroscopicity (κ). Using ten idealized urban plume scenarios in which different types of aerosols evolve over 24 hours under a range of atmospherically relevant environmental conditions, we examine errors in CCN concentrations and optical properties with respect to a more explicit aerosol mixing state representation. We find that only a small number of wBC and κ bins are needed to achieve significant reductions in the errors, and propose a configuration consisting of 24 Ddry bins, 2 wBC bins, and 2 κ bins that gives 24-hour average errors of about 5% or less in CCN concentrations and optical properties, 3-4 times lower than those from size-only-resolved simulations. These results show that MOSAIC-mix is suitable for use in regional and global models to examine the effects of evolving aerosol mixing states on aerosol-radiation-cloud feedbacks.

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

    NASA Astrophysics Data System (ADS)

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

    2016-05-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2014-05-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2014-04-01

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

  15. 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. The importance of aerosol mixing state and size-resolved composition on CCN concentration and the variation of the importance with atmospheric aging of aerosols

    SciTech Connect

    Wang, J.; Cubison, M. J.; Aiken, A. C.; Jimenez, J. L.; Collins, D. R.

    2010-05-01

    Aerosol microphysics, chemical composition, and CCN concentrations were measured at the T0 urban supersite in Mexico City during Megacity Initiative: Local and Global Research Observations (MILAGRO) in March 2006. The aerosol size distribution and composition often showed strong diurnal variation associated with traffic emissions and aging of aerosols through coagulation and local photochemical production of secondary aerosol species. CCN concentrations (N{sub CCN}) are derived using Kohler theory from the measured aerosol size distribution and various simplified aerosol mixing state and chemical composition, and are compared to concurrent measurements at five supersaturations ranging from 0.11% to 0.35%. The influence of assumed mixing state on calculated N{sub CCN} is examined using both aerosols observed during MILAGRO and representative aerosol types. The results indicate that while ambient aerosols often consist of particles with a wide range of compositions at a given size, N{sub CCN} may be derived within {approx}20% assuming an internal mixture (i.e., particles at a given size are mixtures of all participating species, and have the identical composition) if great majority of particles has an overall {kappa} (hygroscopicity parameter) value greater than 0.1. For a non-hygroscopic particle with a diameter of 100 nm, a 3 nm coating of sulfate or nitrate is sufficient to increase its {kappa} from 0 to 0.1. The measurements during MILAGRO suggest that the mixing of non-hygroscopic primary organic aerosol (POA) and black carbon (BC) particles with photochemically produced hygroscopic species and thereby the increase of their {kappa} to 0.1 take place in a few hours during daytime. This rapid process suggests that during daytime, a few tens of kilometers away for POA and BC sources, N{sub CCN} may be derived with sufficient accuracy by assuming an internal mixture, and using bulk chemical composition. The rapid mixing also indicates that, at least for very active

  17. 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

  18. 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.

  19. 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.

  20. 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.

  1. 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.

  2. 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

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

    NASA Astrophysics Data System (ADS)

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

    2010-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2016-11-01

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

  5. Effects of turbulence on mixed-phase deep convective clouds under different basic-state winds and aerosol concentrations

    NASA Astrophysics Data System (ADS)

    Lee, Hyunho; Baik, Jong-Jin; Han, Ji-Young

    2014-12-01

    The effects of turbulence-induced collision enhancement (TICE) on mixed-phase deep convective clouds are numerically investigated using a 2-D cloud model with bin microphysics for uniform and sheared basic-state wind profiles and different aerosol concentrations. Graupel particles account for the most of the cloud mass in all simulation cases. In the uniform basic-state wind cases, graupel particles with moderate sizes account for some of the total graupel mass in the cases with TICE, whereas graupel particles with large sizes account for almost all the total graupel mass in the cases without TICE. This is because the growth of ice crystals into small graupel particles is enhanced due to TICE. The changes in the size distributions of graupel particles due to TICE result in a decrease in the mass-averaged mean terminal velocity of graupel particles. Therefore, the downward flux of graupel mass, and thus the melting of graupel particles, is reduced due to TICE, leading to a decrease in the amount of surface precipitation. Moreover, under the low aerosol concentration, TICE increases the sublimation of ice particles, consequently playing a partial role in reducing the amount of surface precipitation. The effects of TICE are less pronounced in the sheared basic-state wind cases than in the uniform basic-state wind cases because the number of ice crystals is much smaller in the sheared basic-state wind cases than in the uniform basic-state wind cases. Thus, the size distributions of graupel particles in the cases with and without TICE show little difference.

  6. 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

  7. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2011-12-01

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

  9. 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

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

    NASA Astrophysics Data System (ADS)

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

    2009-04-01

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

  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. Using Retrieved Aerosol Spectral Properties to Characterize Aerosol Composition and Mixing

    NASA Astrophysics Data System (ADS)

    Li, J.

    2015-12-01

    The spectral dependence of aerosol properties, such as aerosol absorption optical depth (AAOD) and single scattering albedo (SSA), can be used to infer aerosol composition. In particular, aerosol mixtures dominated by dust absorption will have monotonically increasing SSA with wavelength while that dominated by black carbon absorption has monotonically decreasing SSA spectra. However, spectral AAOD and SSA measured in reality may differ from these extreme cases, due to the complicated composition and mixing states. In this study, we use spectral SSA and AAOD retrieved from AERONET measurements, assisted by CALIPSO aerosol type product and Mie calculations, to characterize aerosol mixtures over representative regions. Moreover, in addition to the monotonically increasing or decreasing AAOD and SSA spectra, we find the spectral dependence of these two parameters are frequently peaked (at 675 nm or 870 nm) over several places including East Asia, India, West Africa and South America. We thus suggest that SSA spectral curvature, defined as the negative of the second derivative of SSA as a function of wavelength, can provide additional information on the composition of these aerosol mixtures. Further analysis indicates that moderate mixing of black carbon with dust or organic carbon is mainly responsible for producing the SSA curvature. An optimization scheme was developed to match the observed AAOD and SSA spectra with Mie calculations assuming different aerosol composition and mixing states. Results suggest that while external mixing can explain most of the observed AAOD and SSA spectral dependence, internal mixing or core-shell mode is also likely under many circumstances, such as East Asia during winter and post-monsoon and winter seasons over India. This method offers the potential to quantitatively infer aerosol composition from these spectral measurements of aerosol optical properties.

  15. A conceptual framework for mixing structures in individual aerosol particles

    NASA Astrophysics Data System (ADS)

    Li, Weijun; Sun, Jiaxing; Xu, Liang; Shi, Zongbo; Riemer, Nicole; Sun, Yele; Fu, Pingqing; Zhang, Jianchao; Lin, Yangting; Wang, Xinfeng; Shao, Longyi; Chen, Jianmin; Zhang, Xiaoye; Wang, Zifa; Wang, Wenxing

    2016-11-01

    This study investigated the particle size- and age-dependent mixing structures of individual particles in clean and polluted air. Aerosols were classified into eight components: sea salt, mineral dust, fly ash, metal, soot, sulfates, nitrates, and organic matter (OM). Based on our aerosol classification, a particle that consists of two or more aerosol components can be defined as an internally mixed particle. Otherwise, it is considered to be an externally mixed particle. Within the internally mixed particle class, we identified four heterogeneous mixing structures: core-shell, dumbbell, OM coating, and dispersed OM, as well as one homogeneous-like mixing structure. Homogeneous-like mixing mainly occurred in fine particles (<1 µm), while the frequency of heterogeneously mixed particles increased with particle size. Our study demonstrated that particle mixing structures depend on particle size and location and evolve with time. OM-coating and core-shell structures are important indicators for particle aging in air as long as they are distant from specific emission sources. Long-range transported particles tended to have core-shell and OM-coating structures. We found that secondary aerosol components (e.g., sulfates, nitrates, and organics) determined particle mixing structures, because their phases change following particle hydration and dehydration under different relative humidities. Once externally mixed particles are transformed into internally mixed particles, they cannot revert to their former state, except when semivolatile aerosol components are involved. Categorizing mixing structures of individual particles is essential for studying their optical and hygroscopic properties and for tracing the development of their physical or chemical properties over time.

  16. 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).

  17. 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

  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. On the mixing and evaporation of secondary organic aerosol components.

    PubMed

    Loza, Christine L; Coggon, Matthew M; Nguyen, Tran B; Zuend, Andreas; Flagan, Richard C; Seinfeld, John H

    2013-06-18

    The physical state and chemical composition of an organic aerosol affect its degree of mixing and its interactions with condensing species. We present here a laboratory chamber procedure for studying the effect of the mixing of organic aerosol components on particle evaporation. The procedure is applied to the formation of secondary organic aerosol (SOA) from α-pinene and toluene photooxidation. SOA evaporation is induced by heating the chamber aerosol from room temperature (25 °C) to 42 °C over 7 h and detected by a shift in the peak diameter of the SOA size distribution. With this protocol, α-pinene SOA is found to be more volatile than toluene SOA. When SOA is formed from the two precursors sequentially, the evaporation behavior of the SOA most closely resembles that of SOA from the second parent hydrocarbon, suggesting that the structure of the mixed SOA resembles a core of SOA from the initial precursor coated by a layer of SOA from the second precursor. Such a core-and-shell configuration of the organic aerosol phases implies limited mixing of the SOA from the two precursors on the time scale of the experiments, consistent with a high viscosity of at least one of the phases.

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

    NASA Astrophysics Data System (ADS)

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

    2014-06-01

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

  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. Dependence of Ice Formation in Sierra Winter Orographic Clouds on the Mixing State of Aerosols Serving as Ice Nuclei

    NASA Astrophysics Data System (ADS)

    DeMott, P. J.; Prather, K. A.; Sullivan, R. C.; Suski, K.; Comstock, J. M.; Tomlinson, J. M.; Rosenfeld, D.; Prenni, A. J.; Cazorla, A.

    2011-12-01

    The CalWater study of February to March 2011 offered the opportunity for observations of aerosols from local, regional and long distance sources as they were integrated into clouds and precipitation in the Sierra Nevada. Single particle chemical analysis of cloud particle residual nuclei and surface precipitation, and their association with changes in cloud microphysical differences, suggest that ice initiation and precipitation formation were strongly affected by intrusions of Asian dust. This is consistent with coincident processing of aerosols present in ambient air and cloud particle residuals as ice nuclei. Elevated ice nuclei concentrations were associated with the presence of dust detected in cloud particle residuals, and dust particles dominated ice nuclei chemical compositions assessed by transmission electron microscopy x-ray analyses at these same times. Evidence of the role of Asian dust as ice nuclei during 2011 are consistent with back trajectory analyses and with recently published observational findings from CalWater Early Start data from 2009. The relative roles of aerosols from the marine boundary layer, biomass burning, and pollution as ice nuclei will also be discussed.

  4. Shaken, not Stirred: Mixing Organic Aerosol

    NASA Astrophysics Data System (ADS)

    Donahue, N. M.; Robinson, E.; Trump, E. R.; Saleh, R.

    2013-12-01

    For organic vapors to condense onto or into existing particles in the atmosphere, the compounds must have a positive thermodynamic driving force. Their activity (saturation ratio) in the gas phase must exceed their activity (modified mole fraction) at the particle surface. Organic-aerosol production rates are generally quite small -- a few μg m-3 per hour at most -- and thus gas-phase saturation ratios are correspondingly small. Most experiments are conducted with far higher production rates and thus far higher saturation ratios. Consequently, experiments may or may not constrain whether organics coat particles in the real world. In addition, surface activity is often assumed to equal bulk activity for most species, meaning that particles are well mixed. However, if particles are viscous and coating rates high, diffusion through the bulk of even 100 nm particles may be slow. Again, matching experimental timescales to real-world timescales is important. Here we describe organic particle mixing experiments in which two organic particle populations are prepared separately and then intermingled by transferring the contents of one preparation chamber into another. Constituents of one population are isotopically labeled, making the mass spectra of the two particle types completely orthogonal. Following the intermingling, single-particle mass spectra allow us to track individual particle composition as the populations mix via gas-phase exchange. This allows us to explore the mixing and coating behavior of organic-aerosol populations under conditions much closer to concentrations found in the real world.

  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. Effect of relative humidity on mixed aerosols in atmosphere.

    PubMed

    Lee, W M; Huang, W M; Chen, Y Y

    2001-01-01

    In this study, the effects of relative humidity on the deliquescent point and size of internally mixed aerosols diameter, NH4NO3 and (NH4)2SO4 were investigated using a Tandem Differential Mobility Analyzer (TDMA) with a relative humidity conditioner. The growth of mixed aerosols appears to have two deliquescent steps. The first one was at about 61.2-61.3%, but the second one was at around 77-78%. At the first deliquescence point, growth ratio at phase change was 7.5%, which agrees with the growth ratio of ammonium nitrate aerosol. Growth ratio of phase change at the second deliquescence point was about 20%, lower than the growth ratio of ammonium sulfate aerosol. In the relative humidity range of 80-85%, the growth ratio of the mixed aerosols reached 60%. In other words, it appears that growth ratio increases with the size of aerosol. Furthermore, a theoretical growth model of mixed aerosols was developed and applied to estimate the amount of composition of the mixed aerosols dissolved at each deliquescence point. The results also show that some of ammonium sulfate already dissolved at the first deliquescence point according to the theoretical growth model.

  7. 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.

  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, 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.

  9. Study of atmospheric aerosols and mixing layer by LIDAR.

    PubMed

    Angelini, Federico; Barnaba, Francesca; Landi, Tony Christian; Caporaso, Luca; Gobbi, Gian Paolo

    2009-12-01

    The LIDAR (laser radar) is an active remote sensing technique, which allows for the altitude-resolved observation of several atmospheric constituents. A typical application is the measurement of the vertically resolved aerosol optical properties. By using aerosol particles as a marker, continuous determination of the mixing layer height (MLH) can also be obtained by LIDAR. Some examples of aerosol extinction coefficient profiles and MLH extracted from a 1-year LIDAR data set collected in Milan (Italy) are discussed and validated against in situ data (from a balloon-borne optical particle counter). Finally a comparison of the observation-based MLH with relevant numerical simulations (mesoscale model MM5) is provided.

  10. 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.

  11. Seasonality of Aerosols the Southeastern United States

    NASA Astrophysics Data System (ADS)

    Ford, B. J.; Heald, C. L.

    2012-12-01

    Previous studies have suggested that increases in atmospheric aerosols of biogenic origin may have caused regional cooling over the southeastern United States in recent decades. Understanding the sources and behaviors of these aerosols is important for determining their role in a changing climate and managing their air quality impacts. In this study, we investigate the strong seasonality in aerosol optical depth (AOD) observed by MODIS, MISR, and CALIOP instruments over the southeastern United States and show that this is not simulated by a chemical transport model (GEOS-Chem). However, the model does reproduce surface PM 2.5 concentrations in the region as reported by the IMPROVE and Southeastern Aerosol Research and Characterization (SEARCH) networks, as well as the muted seasonality of these concentrations. In addition, these surface measurements show that organic aerosol makes up a small fraction of total PM 2.5 and has relatively little seasonality, which calls into question the importance of biogenic aerosol as a driver for climate change in the region. Sounding profiles and ground observations of relative humidity suggest that the magnitude of seasonality in AOD cannot be explained by seasonal differences in the hygroscopic growth of aerosols. CALIOP measurements of the vertical profile of aerosol extinction confirm that the likely reconciliation of the differences in seasonality between the surface PM 2.5 and AOD observations is the formation of aerosol aloft, a process not captured by the model. These findings provide initial insights for the Southern Oxidant and Aerosol Study (SOAS) campaign in 2013 which aims to investigate the anthropogenic influence on biogenic aerosol formation in the Southeastern US and elucidate the impact on regional climate and air quality.

  12. 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

  13. Optimal broadcasting of mixed states

    SciTech Connect

    Dang Guifang; Fan Heng

    2007-08-15

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

  14. 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...

  15. 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.

  16. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  18. 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

  19. 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

  20. 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.

  1. Optical properties of mixed aerosol layers over Japan derived with multi-wavelength Mie-Raman lidar system

    NASA Astrophysics Data System (ADS)

    Hara, Yukari; Nishizawa, Tomoaki; Sugimoto, Nobuo; Matsui, Ichiro; Pan, Xiaole; Kobayashi, Hiroshi; Osada, Kazuo; Uno, Itsushi

    2017-02-01

    Mixing state of aerosols and optical properties including lidar ratio, particle depolarization ratio, and Ångström exponent were investigated at Fukuoka in western Japan using a multi-wavelength Mie-Raman lidar (MMRL), various aerosol mass-concentration measurements, and a polarization optical particle counter during Winter-Spring 2015. Aerosol extinction coefficient, backscatter coefficient, and depolarization at 355 and 532 nm and attenuated backscatter coefficient at 1064 nm are obtained from the MMRL measurements. Ten aerosol episodes were classified into three categories (air pollution, mineral dust, and marine aerosol) based on aerosol mass-concentration measurements in the fine-mode (particle diameter Dp<2.5 μm) and coarse-mode (2.5 μmmixing of mineral dust and anthropogenic fine-mode aerosols. The lowest lidar ratio was obtained for marine case. Classification of aerosol types using the lidar ratio and particle depolarization ratio was conducted based on the results obtained in this study. The classified aerosol types almost corresponded to aerosol category obtained by previous studies. We found no remarkable correlation between the fraction of black carbon and the lidar ratio: this might be due to the complexity of the mixing state among various aerosols. The obtained lidar ratio was rather correlated with the ratio of PMf to PM10, representing the mixing state of fine- and coarse-mode particles.

  2. 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.

  3. 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.

  4. 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

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

    NASA Astrophysics Data System (ADS)

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

    2008-03-01

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

  6. [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.

  7. 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.

  8. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  10. A study of the mixing state of black carbon in urban zone

    NASA Astrophysics Data System (ADS)

    Mallet, M.; Roger, J. C.; Despiau, S.; Putaud, J. P.; Dubovik, O.

    2004-02-01

    The knowledge of the mixing state of black carbon particle with other aerosol species is critical for adequate simulations of the direct radiative effect of black carbon particles and its effect on climate. This paper reports the investigation of the mixing state of black carbon aerosol in the urban zone. The study uses a combination of in situ and ground-based remote sensing observations conducted during the ESCOMPTE experiment, which took place in industrialized region in France in summer of 2001. The criteria we used for identifying mixing state relies on the known enhancement of absorption for aerosol composed by internal versus external mixtures of black carbon with weakly absorbing aerosol components. First, using in situ aerosol data, we performed Mie computations and reconstructed the single scattering albedo of aerosol for the two different mixing assumptions: black carbon mixed externally or internally with other aerosol species. Then, we compared the obtained values ωo,int and ωo,ext with the retrievals of ωo from independent AERONET Sun-photometric measurements. The aerosol single scattering albedo (ωo,aer.) derived from the AERONET photometer observations (with the mean value equal to 0.84 ± 0.04) was found to be close to ωo,ext reconstructed from in situ observation under assumptions of external mixture. This similarity between AERONET values and external mixture simulations was observed during all the days studied. Our conclusion on external mixture of black carbon aerosol with other particles in urban zone during ESCOMPTE (close to the pollution source) is coherent with observations made during other independent studies reported in a number of recent publications.

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

    NASA Astrophysics Data System (ADS)

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

    2008-09-01

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

  12. 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.

  13. 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.

  14. Mixing and water-soluble characteristics of particulate organic compounds in individual urban aerosol particles

    NASA Astrophysics Data System (ADS)

    Li, Weijun; Shao, Longyi

    2010-01-01

    Particulate organic compounds (POCs) in the atmosphere can alter the morphology and hygroscopicity of inorganic particles by coagulation and mixing. Direct observations can illustrate the mixing of organic and inorganic particles. Compositions, mixing states, and morphologies of 360 aerosol particles from urban Beijing collected on transmission electron microscopy (TEM) grids with Si-O substrate were obtained using TEM coupled with energy-dispersive X ray spectrometry (TEM/EDX). The Si-O substrate used in this study allows TEM/EDX to detect carbonaceous particles internally mixed with inorganic particles. POCs were present in approximately 90% of the nitrate-coated mineral particles on both hazy and clear days. Approximately 73% of K- and S-rich particles contained organic coatings and organic inclusions/aggregations on hazy days, while 53% of S-rich particles on clear days during the Beijing Olympics contained only organic coatings. Water dialysis of individual particles indicated that the organic inclusions/aggregations in the K- and S-rich particles were insoluble in water but that POCs from the coatings of individual particles were soluble. The organic coatings on individual inorganic particles may influence their surface hygroscopicity and optical properties.

  15. Efflorescence upon humidification? X-ray microspectroscopic in situ observation of changes in aerosol microstructure and phase state upon hydration

    NASA Astrophysics Data System (ADS)

    Pöhlker, Christopher; Saturno, Jorge; Krüger, Mira L.; Förster, Jan-David; Weigand, Markus; Wiedemann, Kenia T.; Bechtel, Michael; Artaxo, Paulo; Andreae, Meinrat O.

    2014-05-01

    The phase and mixing state of atmospheric aerosols is a central determinant of their properties and thus their role in atmospheric cycling and climate. Particularly, the hygroscopic response of aerosol particles to relative humidity (RH) variation is a key aspect of their atmospheric life cycle and impacts. Here we applied X-ray microspectroscopy under variable RH conditions to internally mixed aerosol particles from the Amazonian rain forest collected during periods with anthropogenic pollution. Upon hydration, we observed substantial and reproducible changes in particle microstructure, which appear as mainly driven by efflorescence and recrystallization of sulfate salts. Multiple solid and liquid phases were found to coexist, especially in intermediate humidity regimes. We show that X-ray microspectroscopy under variable RH is a valuable technique to analyze the hygroscopic response of individual ambient aerosol particles. Our initial results underline that RH changes can trigger strong particle restructuring, in agreement with previous studies on artificial aerosols.

  16. 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.

    2015-06-01

    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. SP2 is a unique instrument that can give detailed information about mass distributions and mixing state of refractory black carbon (rBC). As expected, 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 log-normally distributed rBC core size was relatively constant with an average geometric mass mean diameter of 194 nm. On the average, the number fraction of particles containing rBC was 0.24 and the average rBC core size in these particles was half of the total size (coated to core diameter ratio was 2.0). These numbers mean that the core was larger and had a significantly thicker coating than in typical particles closer to their source regions. Comparison of the measured rBC mass concentration with that of the optically detected equivalent black carbon (eBC) showed a factor of five difference, which could not be fully explained without assuming that a part of the absorbing material is non-refractory. Finally, climate implications of five different rBC mixing state representations were quantified using the Mie approximation and simple direct radiative forcing efficiency calculations. These calculations showed that the observed mixing state (separate non-absorbing and coated rBC particles) means significantly lower warming effect or even a net cooling effect when compared with that of an homogenous aerosol containing the same amounts of rBC and non-absorbing material.

  17. 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

  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.; 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

  19. Development of the RAQM2 aerosol chemical transport model and predictions of the Northeast Asian aerosol mass, size, chemistry, and mixing type

    NASA Astrophysics Data System (ADS)

    Kajino, M.; Inomata, Y.; Sato, K.; Ueda, H.; Han, Z.; An, J.; Katata, G.; Deushi, M.; Maki, T.; Oshima, N.; Kurokawa, J.; Ohara, T.; Takami, A.; Hatakeyama, S.

    2012-12-01

    A new aerosol chemical transport model, the Regional Air Quality Model 2 (RAQM2), was developed to simulate the Asian air quality. We implemented a simple version of a triple-moment modal aerosol dynamics model (MADMS) and achieved a completely dynamic (non-equilibrium) solution of a gas-to-particle mass transfer over a wide range of aerosol diameters from 1 nm to super-μm. To consider a variety of atmospheric aerosol properties, a category approach was utilized in which the aerosols were distributed into four categories: particles in the Aitken mode (ATK), soot-free particles in the accumulation mode (ACM), soot aggregates (AGR), and particles in the coarse mode (COR). The aerosol size distribution in each category is characterized by a single mode. The condensation, evaporation, and Brownian coagulations for each mode were solved dynamically. A regional-scale simulation (Δx = 60 km) was performed for the entire year of 2006 covering the Northeast Asian region. The modeled PM1/bulk ratios of the chemical components were consistent with observations, indicating that the simulated aerosol mixing types were consistent with those in nature. The non-sea-salt SO42- mixed with ATK + ACM was the largest at Hedo in summer, whereas the SOSO42- was substantially mixed with AGR in the cold seasons. Ninety-eight percent of the modeled NO3- was mixed with sea salt at Hedo, whereas 53.7% of the NO3- was mixed with sea salt at Gosan, which is located upwind toward the Asian continent. The condensation of HNO3 onto sea salt particles during transport over the ocean accounts for the difference in the NO3- mixing type at the two sites. Because the aerosol mixing type alters the optical properties and cloud condensation nuclei activity, its accurate prediction and evaluation are indispensable for aerosol-cloud-radiation interaction studies.

  20. 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.

  1. 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.

  2. 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.

  3. 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.

  4. 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.

  5. 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.

  6. 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.

  7. Geometric uncertainty relation for mixed quantum states

    SciTech Connect

    Andersson, Ole Heydari, Hoshang

    2014-04-15

    In this paper we use symplectic reduction in an Uhlmann bundle to construct a principal fiber bundle over a general space of unitarily equivalent mixed quantum states. The bundle, which generalizes the Hopf bundle for pure states, gives in a canonical way rise to a Riemannian metric and a symplectic structure on the base space. With these we derive a geometric uncertainty relation for observables acting on quantum systems in mixed states. We also give a geometric proof of the classical Robertson-Schrödinger uncertainty relation, and we compare the two. They turn out not to be equivalent, because of the multiple dimensions of the gauge group for general mixed states. We give examples of observables for which the geometric relation provides a stronger estimate than that of Robertson and Schrödinger, and vice versa.

  8. Effects of morphology on the radiative properties of internally mixed light absorbing carbon aerosols with different aging status.

    PubMed

    Cheng, Tianhai; Wu, Yu; Chen, Hao

    2014-06-30

    Light absorbing carbon aerosols play a substantial role in climate change through radiative forcing, which is the dominant absorber of solar radiation. Radiative properties of light absorbing carbon aerosols are strongly dependent on the morphological factors and the mixing mechanism of black carbon with other aerosol components. This study focuses on the morphological effects on the optical properties of internally mixed light absorbing carbon aerosols using the numerically exact superposition T-matrix method. Three types aerosols with different aging status such as freshly emitted BC particles, thinly coated light absorbing carbon aerosols, heavily coated light absorbing carbon aerosols are studied. Our study showed that morphological factors change with the aging of internally mixed light absorbing carbon aerosols to result in a dramatic change in their optical properties. The absorption properties of light absorbing carbon aerosols can be enhanced approximately a factor of 2 at 0.67 um, and these enhancements depend on the morphological factors. A larger shell/core diameter ratio of volume-equivalent shell-core spheres (S/C), which indicates the degree of coating, leads to stronger absorption. The enhancement of absorption properties accompanies a greater enhancement of scattering properties, which is reflected in an increase in single scattering albedo (SSA). The enhancement of single scattering albedo due to the morphological effects can reach a factor of 3.75 at 0.67 μm. The asymmetry parameter has a similar yet smaller enhancement. Moreover, the corresponding optical properties of shell-and-core model determined by using Lorenz -Mie solutions are presented for comparison. We found that the optical properties of internally mixed light absorbing carbon aerosol can differ fundamentally from those calculated for the Mie theory shell-and-core model, particularly for thinly coated light absorbing carbon aerosols. Our studies indicate that the complex morphology

  9. 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.

  10. Quantum Darwinism for mixed-state environment

    NASA Astrophysics Data System (ADS)

    Quan, Haitao; Zwolak, Michael; Zurek, Wojciech

    2009-03-01

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

  11. 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

  12. Optical Properties of Internally Mixed Aerosol Particles Composed of Dicarboxylic Acids and Ammonium Sulfate

    NASA Astrophysics Data System (ADS)

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

    2009-10-01

    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.

  13. Modeling the Thermodynamics of Mixed Organic-Inorganic Aerosols to Predict Water Activities and Phase Equilibria

    NASA Astrophysics Data System (ADS)

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

    2008-12-01

    Tropospheric aerosol particles 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 behavior. While the thermodynamics of aqueous inorganic systems at atmospheric temperatures are well established, little is known about the physicochemistry of mixed organic-inorganic particles. Salting-out and salting-in effects result from organic-inorganic interactions and are used to improve industrial separation processes. In the atmosphere, they may influence the aerosol phases. Liquid-liquid phase separations into a mainly polar (aqueous) and a less polar organic phase may considerably influence the gas/particle partitioning of semi-volatile substances compared to a single phase estimation. Moreover, the phases present in the aerosol define the reaction medium for heterogeneous and multiphase chemistry occurring in aerosol particles. A correct description of these phases is needed when gas- or cloud-phase reaction schemes are adapted to aerosols. Non-ideal thermodynamic behavior in mixtures is usually described by an expression for the excess Gibbs energy. We present the group-contribution model AIOMFAC (Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients), which explicitly accounts for molecular interactions between solution constituents, both organic and inorganic, to calculate activities, chemical potentials and the total Gibbs energy of mixed systems. This model allows to compute vapor-liquid (VLE), liquid-liquid (LLE) and solid-liquid (SLE) equilibria within one framework. Focusing on atmospheric applications we considered eight different cations, five anions and a wide range of alcohols/polyols as organic compounds. With AIOMFAC, the activities of the components within an aqueous electrolyte solution are very well represented up to high ionic strength. We show that the semiempirical middle

  14. 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.

  15. Aging of black carbon in outflow from anthropogenic sources using a mixing state resolved model: Model development and evaluation

    NASA Astrophysics Data System (ADS)

    Oshima, N.; Koike, M.; Zhang, Y.; Kondo, Y.; Moteki, N.; Takegawa, N.; Miyazaki, Y.

    2009-03-01

    The mixing state of black carbon (BC) aerosols, namely, the degree to which BC particles are coated with other aerosol components, has been recognized as important for evaluating aerosol radiative forcing. In order to resolve the BC mixing state explicitly in model simulations, a two-dimensional aerosol representation, in which aerosols are given for individual particle diameters and BC mass fractions, is introduced. This representation was incorporated into an aerosol module, the Model of Aerosol Dynamics, Reaction, Ionization, and Dissolution (MADRID), and a new box model, MADRID-BC, was developed. MADRID-BC can accurately simulate changes in the entire BC mixing state resulting from condensation/evaporation processes. Aircraft observations conducted in March 2004 show that the mass fraction of thickly coated BC particles increased in air horizontally transported out from an urban area in Japan over the ocean. MADRID-BC generally reproduces this feature well when observed bulk aerosol concentrations are used as constraints. The model simulations in this particular case show that for particles with BC core diameters of 100-200 nm, the particle diameters, including both core and coating materials, had already increased by a factor of 1.6 on average when they left the source region and by as large as a factor of 1.9 of the BC core diameters after their transport over the ocean for a half day. The model simulations also show that 58% of the total condensed mass was partitioned onto BC-free particles during transport, indicating their importance for the BC mixing state. Although the model simulations are applied to a limited number of the observations in this study, they clearly show the time evolution of the coating thicknesses of BC-containing particles, which is necessary for calculating aerosol optical properties and cloud condensation nuclei activities.

  16. Cloud condensation nucleus activity of secondary organic aerosol particles mixed with sulfate

    NASA Astrophysics Data System (ADS)

    King, Stephanie M.; Rosenoern, Thomas; Shilling, John E.; Chen, Qi; Martin, Scot T.

    2007-12-01

    The cloud condensation nucleus (CCN) activity of organic-sulfate particles was investigated using a steady-state environmental chamber. The organic component consisted of secondary organic aerosol (SOA) generated in the dark from 24 +/- 2 ppb α-pinene for conditions of 300 +/- 5 ppb ozone, 40 +/- 2% relative humidity, and 25 +/- 1°C, with the organic mass loading in the chamber ranging from 23 to 37 μg m-3. CCN analysis was performed for 80- to 150-nm particles having variable organic-sulfate volume fractions, which were estimated from the diameter of the organic-sulfate particle relative to that of the seed as well as independently from mass spectra. Critical supersaturation, which increased for greater SOA volume fraction and smaller particle diameter, was well predicted by a Köhler model having two components, one for ammonium sulfate and another for SOA. The entire data set could be successfully modeled by a single suite of effective chemical parameters for SOA. The results suggest that the effects of limited organic solubility in mixed SOA-sulfate particles may be reliably omitted in the treatment of cloud droplet formation.

  17. 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.

  18. Oxidative aging of mixed oleic acid/sodium chloride aerosol particles

    NASA Astrophysics Data System (ADS)

    Dennis-Smither, Benjamin J.; Miles, Rachael E. H.; Reid, Jonathan P.

    2012-10-01

    Studies of the oxidative aging of single mixed component aerosol particles formed from oleic acid (OL) and sodium chloride over a range of relative humidities (RH) and ozone concentrations by aerosol optical tweezers are reported. The rate of loss of OL and changes in the organic phase volume are directly measured, comparing particles with effloresced and deliquesced inorganic seeds. The kinetics of the OL loss are analyzed and the value of the reactive uptake coefficient of ozone by OL is compared to previous studies. The reaction of OL is accompanied by a decrease in the particle volume, consistent with the evaporation of semivolatile products over a time scale of tens of thousands of seconds. Measurements of the change in the organic phase volume allow the branching ratio to involatile components to be estimated; between 50 and 85% of the initial organic volume remains involatile, depending on ozone concentration. The refractive index (RI) of the organic phase increases during and after evaporation of volatile products, consistent with aging followed by a slow restructuring in particle morphology. The hygroscopicity of the particle and kinetics of the response of the organic phase to changes in RH are investigated. Both size and RI of unoxidized and oxidized particles respond promptly to RH changes with values of the RI consistent with linear mixing rules. Such studies of the simultaneous changes in composition and size of mixed component aerosol provide valuable data for benchmarking kinetic models of heterogeneous atmospheric aging.

  19. Impact of Asian aerosols on air quality over the United States: A perspective from aerosol-cloud-radiation coupling

    NASA Astrophysics Data System (ADS)

    Tao, Z.; Yu, H.; Chin, M.

    2013-12-01

    It has well been established, through satellite/ground observations, that dust and aerosols from various Asian sources can travel across the Pacific and reach North America (NA) at least on episode bases. Once reaching NA, these inflow aerosols would compete with local emissions to influence atmospheric composition and air quality over the United States (US). The previous studies, typically based on one or multiple satellite measurements in combination with global/regional model simulations, suggest that the impact of Asian dust/aerosols on US air quality tend to be small since most inflow aerosols stay aloft. On the other hand, aerosols affect many key meteorological processes that will ultimately channel down to impact air quality. Aerosols absorb and scatter solar radiation that change the atmospheric stability, thus temperature, wind, and planetary boundary layer structure that would directly alter air quality. Aerosols can serve as cloud condensation nuclei and ice nuclei to modify cloud properties and precipitation that would also affect aerosol removal and concentration. This indirect impact of Asian aerosol inflow on US air quality may be substantial and need to be investigated. This study employs the NASA Unified WRF (NU-WRF) to address the question from the aerosol-radiation-cloud interaction perspective. The simulation period was selected from April to June of 2010 during which the Asian dust continuously reached NA based on CALIPSO satellite observation. The preliminary results show that the directly-transported Asian aerosol increases surface PM2.5 concentration by less than 2 μg/m3 over the west coast areas of US, and the aerosol-radiation-cloud feedback has a profound effect on air quality over the central to eastern US. A more detailed analysis links this finding to a series of meteorological conditions modified by aerosol effects.

  20. 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

  1. Aerosols

    Atmospheric Science Data Center

    2013-04-17

    ... article title:  Aerosols over Central and Eastern Europe     View Larger Image ... last weeks of March 2003, widespread aerosol pollution over Europe was detected by several satellite-borne instruments. The Multi-angle ...

  2. 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.

  3. Dysphoric mania, mixed states, and mania with mixed features specifier: are we mixing things up?

    PubMed

    McElroy, Susan L; Keck, Paul E

    2016-11-21

    Various terms have been used to describe mania when it is accompanied by depressive symptoms. In this article, we attempt to define and discuss 3 of these terms: dysphoric mania, mixed state, and mania with mixed features specifier. We conclude that whatever term is used, it is important to be aware that mania is more often unpleasant than pleasant, and that the unpleasantness is not limited to depression.

  4. 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).

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

    NASA Astrophysics Data System (ADS)

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

    2010-02-01

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

  6. Maximally discordant mixed states of two qubits

    SciTech Connect

    Galve, Fernando; Giorgi, Gian Luca; Zambrini, Roberta

    2011-01-15

    We study the relative strength of classical and quantum correlations, as measured by discord, for two-qubit states. Quantum correlations appear only in the presence of classical correlations, while the reverse is not always true. We identify the family of states that maximize the discord for a given value of the classical correlations and show that the largest attainable discord for mixed states is greater than for pure states. The difference between discord and entanglement is emphasized by the remarkable fact that these states do not maximize entanglement and are, in some cases, even separable. Finally, by random generation of density matrices uniformly distributed over the whole Hilbert space, we quantify the frequency of the appearance of quantum and classical correlations for different ranks.

  7. 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.

  8. 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

  9. 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

  10. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2013-02-01

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

  12. 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

  13. Shapes of internally mixed hygroscopic aerosol particles after deliquescence, and their effect on light scattering

    NASA Astrophysics Data System (ADS)

    Adachi, Kouji; Freney, Evelyn J.; Buseck, Peter R.

    2011-07-01

    Hygroscopic aerosol particles change the magnitude of light scattering through condensation and evaporation of water vapor. We collected aerosol particles from two megacities and observed the particle shapes at various values of relative humidity (RH) using an environmental cell within a transmission electron microscope. Many Mexico City samples had sulfate particles that were embedded within weakly hygroscopic organic aerosol, whereas the Los Angeles samples mainly consisted of externally mixed sulfate particles. For the Mexico City samples, when the RH was increased in the microscope, only the sulfate parts deliquesced, but the entire particle did not become spherical, i.e., particles containing deliquescent phases do not necessarily become spherical upon deliquescence. This result conflicts with the assumption used in many models, i.e., that deliquesced particles become spherical. Using a discrete-dipole approximation to calculate light scattering of simulated particles that resemble the observed ones, we show that, for particles >1.0 μm, the spherical-shape assumption used in Mie theory underestimates the light scattering by ˜50%, with the exact value depending on the sizes and relative volumes of the constituent phases.

  14. Non-steady-state aerosol filtration in nanostructured fibrous media.

    PubMed

    Przekop, Rafal; Gradoń, Leon

    2011-06-28

    The filtration of aerosol particles using composites of nano- and microsized fibrous structures is a promising method for the effective separation of nanoparticles from gases. A multi-scale physical system describing the flow pattern and particle deposition at a non-steady-state condition requires an advanced method of modelling. The combination of lattice Boltzmann and Brownian dynamics was used for analysis of the particle deposition pattern in a fibrous system. The dendritic structures of deposits for neutral and charged fibres and particles are present. The efficiency of deposition, deposit morphology, porosity and fractal dimension were calculated for a selected operational condition of the process.

  15. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2012-08-01

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

  17. Optimal full estimation of qubit mixed states

    SciTech Connect

    Bagan, E.; Monras, A.; Munoz-Tapia, R.; Ballester, M. A.; Gill, R. D.

    2006-03-15

    We obtain the optimal scheme for estimating unknown qubit mixed states when an arbitrary number N of identically prepared copies is available. We discuss the case of states in the whole Bloch sphere as well as the restricted situation where these states are known to lie on the equatorial plane. For the former case we obtain that the optimal measurement does not depend on the prior probability distribution provided it is isotropic. Although the equatorial-plane case does not have this property for arbitrary N, we give a prior-independent scheme which becomes optimal in the asymptotic limit of large N. We compute the maximum mean fidelity in this asymptotic regime for the two cases. We show that within the pointwise estimation approach these limits can be obtained in a rather easy and rapid way. This derivation is based on heuristic arguments that are made rigorous by using van Trees inequalities. The interrelation between the estimation of the purity and the direction of the state is also discussed. In the general case we show that they correspond to independent estimations whereas for the equatorial-plane states this is only true asymptotically.

  18. 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.

  19. 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.

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

    NASA Astrophysics Data System (ADS)

    Slade, Jonathan H.; Knopf, Daniel A.

    2014-07-01

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

  1. 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.

  2. 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.

  3. 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.

  4. 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

  5. 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

  6. 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...

  7. 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

  8. 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.

  9. 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.

  10. 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.

  11. 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

  12. Average subentropy, coherence and entanglement of random mixed quantum states

    NASA Astrophysics Data System (ADS)

    Zhang, Lin; Singh, Uttam; Pati, Arun K.

    2017-02-01

    Compact expressions for the average subentropy and coherence are obtained for random mixed states that are generated via various probability measures. Surprisingly, our results show that the average subentropy of random mixed states approaches the maximum value of the subentropy which is attained for the maximally mixed state as we increase the dimension. In the special case of the random mixed states sampled from the induced measure via partial tracing of random bipartite pure states, we establish the typicality of the relative entropy of coherence for random mixed states invoking the concentration of measure phenomenon. Our results also indicate that mixed quantum states are less useful compared to pure quantum states in higher dimension when we extract quantum coherence as a resource. This is because of the fact that average coherence of random mixed states is bounded uniformly, however, the average coherence of random pure states increases with the increasing dimension. As an important application, we establish the typicality of relative entropy of entanglement and distillable entanglement for a specific class of random bipartite mixed states. In particular, most of the random states in this specific class have relative entropy of entanglement and distillable entanglement equal to some fixed number (to within an arbitrary small error), thereby hugely reducing the complexity of computation of these entanglement measures for this specific class of mixed states.

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

    PubMed

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

    2016-08-27

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

  14. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2016-08-01

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

  16. 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.

  17. 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.

  18. 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.

  19. 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.

  20. Airborne In-Situ Measurements of Aerosol and Cloud Microphysical Properties in Mixed-Phase Clouds Under Varying Conditions

    NASA Astrophysics Data System (ADS)

    Comstock, J. M.; Fan, J.; Tomlinson, J. M.; Mei, F.; Hubbe, J. M.; Schmid, B.

    2014-12-01

    Cloud microphysical properties impact the interaction of clouds and radiation in the atmosphere, and can influence atmospheric circulations through changes in cloud phase. Characterizing the conditions that control phase changes and the microphysical properties of mixed-phase clouds is important for improving understanding of physical processes that influence cloud phase. We characterize the aerosol and cloud microphysical properties in relation to the atmospheric dynamic and thermodynamic conditions observed in mixed-phase clouds during several aircraft-based field experiments. The Department of Energy Atmospheric Radiation Measurement program's Gulfstream-1 aircraft was used to sample aerosol and cloud properties in warm and cold clouds during several recent field experiments. We analyze in-situ observations from the CalWater and TCAP field campaigns to examine the variability of cloud properties (phase, hydrometeor size, ice and liquid water content, particle habit) with changes in aerosol, vertical velocity, and temperature. These measurements indicate that in addition to aerosol concentration, vertical velocity strength has important influence on cloud phase in mixed-phase cloud regimes.

  1. 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.

  2. On quantum coding for ensembles of mixed states

    NASA Astrophysics Data System (ADS)

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

    2001-09-01

    We consider the problem of optimal asymptotically faithful compression for ensembles of mixed quantum states. Although the optimal rate is unknown, we prove upper and lower bounds and describe a series of illustrative examples of compression of mixed states. We also discuss a classical analogue of the problem.

  3. 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

  4. 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.

  5. Average coherence and its typicality for random mixed quantum states

    NASA Astrophysics Data System (ADS)

    Zhang, Lin

    2017-04-01

    The Wishart ensemble is a useful and important random matrix model used in diverse fields. By realizing induced random mixed quantum states as a Wishart ensemble with fixed unit trace, using matrix integral technique we give a fast track to the average coherence for random mixed quantum states induced via partial-tracing of the Haar-distributed bipartite pure states. As a direct consequence of this result, we get a compact formula for the average subentropy of random mixed states. These compact formulae extend our previous work.

  6. 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.

  7. Modelling the chemically aged and mixed aerosols over the eastern central Atlantic Ocean - potential impacts

    NASA Astrophysics Data System (ADS)

    Astitha, M.; Kallos, G.; Spyrou, C.; O'Hirok, W.; Lelieveld, J.; Denier van der Gon, H. A. C.

    2010-07-01

    Detailed information on the chemical and physical properties of aerosols is important for assessing their role in air quality and climate. This work explores the origin and fate of continental aerosols transported over the Central Atlantic Ocean, in terms of chemical composition, number and size distribution, using chemistry-transport models, satellite data and in situ measurements. We focus on August 2005, a period with intense hurricane and tropical storm activity over the Atlantic Ocean. A mixture of anthropogenic (sulphates, nitrates), natural (desert dust, sea salt) and chemically aged (sulphate and nitrate on dust) aerosols is found entering the hurricane genesis region, most likely interacting with clouds in the area. Results from our modelling study suggest rather small amounts of accumulation mode desert dust, sea salt and chemically aged dust aerosols in this Atlantic Ocean region. Aerosols of smaller size (Aitken mode) are more abundant in the area and in some occasions sulphates of anthropogenic origin and desert dust are of the same magnitude in terms of number concentrations. Typical aerosol number concentrations are derived for the vertical layers near shallow cloud formation regimes, indicating that the aerosol number concentration can reach several thousand particles per cubic centimetre. The vertical distribution of the aerosols shows that the desert dust particles are often transported near the top of the marine cloud layer as they enter into the region where deep convection is initiated. The anthropogenic sulphate aerosol can be transported within a thick layer and enter the cloud deck through multiple ways (from the top, the base of the cloud, and by entrainment). The sodium (sea salt related) aerosol is mostly found below the cloud base. The results of this work may provide insights relevant for studies that consider aerosol influences on cloud processes and storm development in the Central Atlantic region.

  8. Chemically aged and mixed aerosols over the Central Atlantic Ocean - potential impacts

    NASA Astrophysics Data System (ADS)

    Astitha, M.; Kallos, G.; Spyrou, C.; O'Hirok, W.; Lelieveld, J.; Denier van der Gon, H. A. C.

    2010-02-01

    Detailed information on the chemical and physical properties of aerosols is important for assessing their role in air quality and climate. This work explores the origin and fate of continental aerosols transported over the Central Atlantic Ocean, in terms of chemical composition, number and size distribution, using chemistry-transport models, satellite data and in situ measurements. We focus on August 2005, a period with intense hurricane and tropical storm activity over the Atlantic Ocean. A mixture of anthropogenic (sulphates, nitrates), natural (desert dust, sea salt) and chemically aged (sulphate and nitrate on dust) aerosols is found entering the hurricane genesis region, most likely interacting with clouds in the area. Results from our modelling study suggest rather small amounts of accumulation mode desert dust, sea salt and chemically aged dust aerosols in this Atlantic Ocean region. Aerosols of smaller size (Aitken mode) are more abundant in the area and in some occasions sulphates of anthropogenic origin and desert dust are of the same magnitude in terms of number concentrations. Typical aerosol number concentrations are derived for the vertical layers near shallow cloud formation regimes, designating that the aerosol number concentration can reach several thousand particles per cubic centimetre. The vertical distribution of the aerosols indicates that the desert dust particles are often transported near the top of the marine cloud layer as they enter into the region where deep convection is initiated. The anthropogenic sulphate aerosol can be transported within a thick layer and enter the cloud deck through multiple ways (from the top, the base of the cloud and entrainment). The sodium (sea salt related) aerosol is mostly found below the cloud base. The results of this work may provide insights relevant for studies that consider aerosol influences on cloud processes and storm development in the Central Atlantic region.

  9. Mixed States in Bipolar Disorder: Etiology, Pathogenesis and Treatment

    PubMed Central

    2017-01-01

    Many bipolar disorder patients exhibit mixed affective states, which portend a generally more severe illness course and treatment resistance. In the previous renditions of Diagnostic and Statistical Manual mixed states were narrowly defined in the context of bipolar I disorder, but with the advent of DSM-5 the term “mixed episode” was dropped and replaced by “mixed features” specifier which could be broadly applied to manic, hypomanic and depressive episodes in both the bipolar spectrum and major depressive disorders. This paradigm shift reflected their significance in the prognosis and overall management of mood disorders, so that the clinicians should thoroughly familiarize themselves with the contemporary notions surrounding these conditions. The purpose of this manuscript is to bring to light the current conceptualizations regarding the etiology, pathogenesis and treatment of mixed states. To achieve this goal, in June 2016 an extensive literature search was undertaken using the PubMed database. Some exploratory terms utilized included “mixed states”, “mixed episodes”, “switching”, “rapid cycling” cross referenced with “bipolar disorder”. Focusing on the most relevant and up to date studies, it was revealed that mixed states result from genetic susceptibility in the circadian and dopamine neurotransmission apparatuses and disturbance in the intricate catecholamine-acetylcholine neurotransmission balance which leads to mood fluctuations. The management of mixed states is challenging with atypical antipsychotics, newer anticonvulsants and electroconvulsive therapy emerging as the foremost treatment options. In conclusion, while progress has been made in the neurobiological understanding of mixed states, the currently available therapeutic modalities have only shown limited effectiveness. PMID:28184334

  10. 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.

  11. 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

  12. 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

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

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

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

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

    PubMed

    Verstraete, Frank; Verschelde, Henri

    2003-03-07

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

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

    PubMed

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

    2011-02-01

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

  16. 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 ...

  17. 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 ...

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

    PubMed

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

    2015-09-01

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

  19. 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.

  20. 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.

  1. 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.

  2. 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.

  3. 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).

  4. Cloud droplet activation through oxidation of organic aerosol influenced by temperature and particle phase state

    NASA Astrophysics Data System (ADS)

    Slade, Jonathan H.; Shiraiwa, Manabu; Arangio, Andrea; Su, Hang; Pöschl, Ulrich; Wang, Jian; Knopf, Daniel A.

    2017-02-01

    Chemical aging of organic aerosol (OA) through multiphase oxidation reactions can alter their cloud condensation nuclei (CCN) activity and hygroscopicity. However, the oxidation kinetics and OA reactivity depend strongly on the particle phase state, potentially influencing the hydrophobic-to-hydrophilic conversion rate of carbonaceous aerosol. Here, amorphous Suwannee River fulvic acid (SRFA) aerosol particles, a surrogate humic-like substance (HULIS) that contributes substantially to global OA mass, are oxidized by OH radicals at different temperatures and phase states. When oxidized at low temperature in a glassy solid state, the hygroscopicity of SRFA particles increased by almost a factor of two, whereas oxidation of liquid-like SRFA particles at higher temperatures did not affect CCN activity. Low-temperature oxidation appears to promote the formation of highly-oxygenated particle-bound fragmentation products with lower molar mass and greater CCN activity, underscoring the importance of chemical aging in the free troposphere and its influence on the CCN activity of OA.

  5. A study of the aerosol radiative properties needed to compute direct aerosol forcing in the southeastern United States

    NASA Astrophysics Data System (ADS)

    Yu, Shaocai; Saxena, V. K.; Wenny, B. N.; Deluisi, J. J.; Yue, G. K.; Petropavlovskikh, I. V.

    2000-10-01

    To assess the direct radiative forcing due to aerosols in southeastern United States where a mild cooling is under way, an accurate set of data describing the aerosol radiative properties are needed. We report here aerosol optical depth (AOD) and diffuse to-direct solar irradiance ratio (DDR) at three operational wavelengths (415, 500, 673 nm) determined by using Multifilter Rotating Shadowband Radiometers (MFRSR) at two sites (a mountain top site: Mount Gibbes, 35.78°N, 82.29°W, 2006 m mean sea level (msl); a valley site: Black Mountain, 35.66°N, 82.38°W, 951 m msl), which are separated horizontally by 10 km and vertically by 1 km. The characteristics AOD and DDR were determined from the field measurements obtained during 1995. It was found that the representative total AOD values at 500 nm at the valley site for highly polluted (HP), marine (M) and continental (C) air masses were 0.68±0.33, 0.29±0.19, and 0.10±0.04, respectively. The fact that the ratio of the mean 1 km layer optical depth to total mean optical depth at 500 nm from the valley site was 71% indicates that the major portion of the atmospheric aerosol was located in the lowest 1 km surface boundary layer (SBL). There was a significant linear correlation between the DDR and the total AOD at both sites. A simple, fast, and operative search-graph method was used to retrieve the columnar size distribution (number concentration N effective radius reff, and geometric standard deviation σg) from the optical depth observations at the three operational wavelengths. The ground albedo, single-scattering albedo, and imaginary part of the refractive index are calculated using a mathematically unique procedure involving a Mie code and a radiative transfer code in conjunction with the retrieved aerosol size distribution, AOD, and DDR. It was found that N, reff, and σg were in the range of 1.9×10 to 1.7×104 cm-3, 0.09-0.68 μm, and 1.12-2.70, respectively. The asymmetry factor and single-scattering albedo

  6. 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.

  7. Secondary organic aerosol formation during June 2010 in Central Europe: measurements and modelling studies with a mixed thermodynamic-kinetic approach

    NASA Astrophysics Data System (ADS)

    Langmann, B.; Sellegri, K.; Freney, E.

    2013-10-01

    Until recently secondary organic carbon (SOC) aerosol mass concentrations have been systematically underestimated by three-dimensional atmospheric-chemistry-aerosol models. With a newly proposed concept of aging of organic vapours more realistic model results for organic carbon aerosol mass concentrations could be achieved. Applying a mixed thermodynamic-kinetic approach for SOC aerosol formation shifted the aerosol size distribution towards particles in the cloud condensation nuclei size range, thereby emphasising the importance of SOC aerosol formation schemes for modelling realistic cloud and precipitation formation. The additional importance of hetero-molecular nucleation between H2SO4 and organic vapours remains to be evaluated in three-dimensional atmospheric-chemistry-aerosol models. Here a case study is presented focusing on Puy-de-Dôme, France in June 2010. Even though nucleation events at Puy-de-Dôme were rare during the chosen period of investigation a weak event in the boundary layer could be reproduced by the model when nucleation of low-volatile secondary organic vapour is included. Differences in the model results with and without nucleation of organic vapour are visible in the lower free troposphere over several days of the period. Taking into account nucleation of organic vapour leads to an increase in accumulation mode particles due to coagulation of nucleation and aitken mode particles. Moreover, the measurements indicate a considerable increase in SOC aerosol mass concentration during the measurement campaign, which could be reproduced by modelling using a simplified thermodynamic-kinetic approach for SOC aerosol formation and increased biogenic VOC precursor emissions. Comparison with a thermodynamic SOC aerosol formation approach shows a huge improvement in modelled SOC aerosol mass concentration with the thermodynamic-kinetic approach for SOC aerosol formation and a slight improvement of modelled particle size distribution.

  8. 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

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

    PubMed

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

    2012-06-21

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

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

    NASA Astrophysics Data System (ADS)

    China, Swarup

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

  11. 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.

  12. 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.

  13. Sources and Distributions of Secondary Aerosols over the Northeastern United States during the WINTER Aircraft Campaign.

    NASA Astrophysics Data System (ADS)

    Shah, V.; Jaegle, L.; Haskins, J.; Campuzano Jost, P.; Schroder, J. C.; Jimenez, J. L.; Sullivan, A.; Weber, R. J.; Dibb, J. E.; Green, J. R.; Fiddler, M. N.; Bililign, S.; Lopez-Hilfiker, F.; Lee, B. H.; Veres, P. R.; Thornton, J. A.

    2015-12-01

    Atmospheric aerosols harm public health, reduce visibility, and alter the Earth's climate. A significant fraction of the aerosol burden is composed of secondary aerosols formed from gas-phase precursors such as SO2, NOx, NH3, and VOC's. The formation and composition of secondary aerosols depends on precursor abundance, oxidant availability, and the thermodynamic properties of the semi-volatile species. The oxidation and thermodynamic processes are strongly dependent on the available sunlight, temperature, and humidity, and produce large seasonal shifts in the aerosol characteristics. While most previous aircraft campaigns have studied these processes during summer, the Wintertime INvestigation of Transport, Emissions, and Reactivity (WINTER) campaign focuses on the wintertime chemical processes over the northeastern United States. A comprehensive dataset of gas- and particle-phase species was collected during the campaign using the NSF/NCAR C-130 aircraft in February-March 2015. We interpret these observations using the GEOS-Chem chemical transport model with a 1/4 degree latitude by 5/16 degree longitude nested-grid over North America. We present a comparison of the model results with the aircraft measurements, and examine the sources of secondary inorganic and organic aerosols observed during the campaign. We use the model results to investigate the consistency between the aircraft, surface and satellite observations of aerosol concentrations and optical depths. Furthermore, we use multi-year model simulations to understand the effect of the unusually cold weather in 2015 over the northeastern United States on the chemical environment observed during the campaign.

  14. 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.

  15. 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.

  16. Peltier effect in the mixed state of high- Tc superconductors

    NASA Astrophysics Data System (ADS)

    Logvenov, G. Yu.; Ryazanov, V. V.; Ustinov, A. V.; Huebener, R. P.

    1991-04-01

    The Peltier and Seebeck effects in the mixed state of high- Tc superconductors are proportional to the resistivity due to flux motion. Therefore, both effects also show the broadening of the transition regime characteristic for these superconductors. The origin of the Peltier effect is discussed in detail, and the validity of the Thomson relation is confirmed, as expected.

  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. 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.

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

    PubMed

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

    2014-11-06

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

  20. 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

  1. Studies on the equation of state of mixed carbide fuel

    NASA Astrophysics Data System (ADS)

    Joseph, M.; Mathews, C. K.; Rao, P. Bhaskar

    1989-12-01

    The equation of state of reactor fuels is required up to very high temperatures in order to assess the energy release in hypothetical core disruptive accidents (HCM). Though the mixed carbide of uranium and plutonium is a candidate fuel material for fast breeder reactors, much information is not available on its equation of state. This paper reports the results of our studies to obtain the equilibrium vapour pressures of uranium carbide and uranium-plutonium mixed carbide of varying compositions in the temperature range of 1300-9000 K. An extrapolation method based on the principles of equilibrium thermodynamics has been used as also the principle of corresponding states. The agreement between the different results are discussed and their implications in HCDA calculations brought out.

  2. 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.

  3. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2016-09-01

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

  5. 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

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

    NASA Astrophysics Data System (ADS)

    Park, R. J.; Jacob, D. J.; Logan, J. A.

    2006-12-01

    Fires are a potentially major but poorly quantified factor for air quality degradation in the United States. Although episodic effects are well established, little attention has been paid to the more diffuse, nationwide effects of fires on seasonal and annual aerosol concentrations of relevance for air quality and visibility standards. Effects of biofuel use, both residential and industrial, have also received little attention. We use here correlations with non-soil potassium (ns-K) at the nationwide IMPROVE network of surface sites for 2001- 2004 to estimate total contributions to total carbonaceous (TC) aerosol concentrations from wildfires, prescribed fires, and residential and industrial biofuels. We find that the year-to-year variation of fires largely drives the observed interannual variability in TC. We present estimates of biomass burning contributions to regional aerosol concentrations in the western and eastern United States and further examine their implications for the national ambient air quality standard of fine aerosol concentrations and for the application of natural visibility condition by the U.S. EPA Regional Haze Rule.

  7. 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.

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

    PubMed

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

    2014-04-09

    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.

  9. 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

  10. 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.

  11. Nondestructive Estimation of the Eigenvectors of Mixed State

    NASA Astrophysics Data System (ADS)

    Gao, Jingliang

    2017-02-01

    Given n qubits prepared according to the same mixed state ρ, we propose a measuring scheme which approximately yields the eigenvectors of ρ. By performing a sequence of measurements, we can scan the Bloch sphere like radar to search for the eigenvectors. It is shown that this scheme is nondestructive when n is large. This result is based on the quantum typical subspace theory and it actually reveals an interesting mathematical structure of the n-fold Hilbert space.

  12. 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.

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

    PubMed Central

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

    2010-01-01

    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 α-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 α-pinene products on size-selected DOP particles and by condensation of DOP on size-selected α-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 ∼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

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

    PubMed

    Rouvière, Aurélie; Sosedova, Yulia; Ammann, Markus

    2010-07-08

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

  15. Separable balls around the maximally mixed multipartite quantum states

    NASA Astrophysics Data System (ADS)

    Gurvits, Leonid; Barnum, Howard

    2003-10-01

    We show that for an m-partite quantum system, there is a ball of radius 2-(m/2-1) in Frobenius norm, centered at the identity matrix, of separable (unentangled) positive semidefinite matrices. This can be used to derive an ɛ below which mixtures of ɛ of any density matrix with 1-ɛ of the maximally mixed state will be separable. The ɛ thus obtained is exponentially better (in the number of systems) than existing results. This gives a number of qubits below which nuclear magnetic resonance with standard pseudopure-state preparation techniques can access only unentangled states; with parameters realistic for current experiments, this is 23 qubits (compared to 13 qubits via earlier results). A ball of radius 1 is obtained for multipartite states separable over the reals.

  16. Asian aerosols in North America: Extracting the chemical composition and mass concentration of the Asian continental aerosol plume from long-term aerosol records in the western United States

    NASA Astrophysics Data System (ADS)

    Vancuren, Richard A.

    2003-10-01

    Empirical assessment of the frequency and intensity of dust transport from Asia to North America has found that the dust regularly impacts elevated sites in the western United States, revealing a pattern of consistent, frequent transport above the marine boundary layer. Using the dust as a marker for Asian transport, a subset of Asian-influenced samples was identified within a decade of routine aerosol samples from two sites in the western cordillera of North America: Crater Lake, Oregon, and Mount Lassen, California. This subset was used to guide a statistical analysis to isolate Asian aerosol against the "background" of local contaminants. The analysis was then generalized to all samples during the transport season (March-October) for 1989-1999. A mixture of dust and combustion products dominates the Asian aerosol with typical concentration around 5 μg/m3 and mass median diameter between 2 and 3 μm. Major fine particle (<2.5 μm diameter) constituent fractions are ˜30% mineral, 28% organic compounds, 4% elemental carbon, 10% sulfate, <5% nitrate, and <1% sea salt. A second, possibly Asian, component of aged biomass smoke and sea salt is also present, with typical concentration (when present) around 1.5 μg/m3. Averaged over the transport season the dusty Asian aerosol and the smoky aerosol comprise 60 and 6%, respectively, of total particle mass (<10 μm diameter) and 72 and 13% of fine particle mass at these sites. These data indicate that the Asian continental plume is a significant contributor to aerosol loading at remote high-altitude sites across western North America. This implies a significant influence for Asian emissions on free troposphere aerosols over North America and suggests that they need to be explicitly accounted for in aerosol analyses ranging from climate studies to aerosol regulatory programs.

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

    PubMed

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

    2012-11-06

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

  18. Lidar observations of long-range transported Saharan dust over Sofia, Bulgaria: a case study of dust mixed with local aerosols

    NASA Astrophysics Data System (ADS)

    Peshev, Zahary Y.; Dreischuh, Tanja N.; Evgenieva, Tsvetina T.; Deleva, Atanaska D.; Tonev, Dimitar; Stoyanov, Dimitar V.

    2016-07-01

    Two-wavelength (1064/532 nm) lidar observations of long-range transported Saharan dust present in the atmosphere over Sofia, Bulgaria, during a 4-day dust intrusion event in winter 2010, are reported. Aged desert aerosols are detected at altitudes up to 4 km above the sea level, within and above the boundary layer as mixed with other aerosols-representing the particular case under consideration. Optical, microphysical, and dynamical properties of dust aerosols are obtained and analyzed. Special attention is paid to retrieving and vertical profiling of dust backscatter-related Ångström exponents (BAEs), as well as to determining their frequency-count distributions. Obtained BAE values in the range 0.3 to 0.6 (±0.2) indicate domination of coarse particles in the near overmicron size range. Reasonability of coarse-mode-dominated dust size composition is substantiated, based on measurement and transportation-history analysis. The performed frequency-count statistics reveals dust BAE distributions asymmetrically extended to multimode distribution shapes, resulting from dust mixing with finer local aerosol fractions. Peculiarities and patterns of the aerosol dynamics at different stages of dust-loading event are revealed and discussed.

  19. Explicit Simulation of Aerosol Physics in a Cloud-Resolving Model: Aerosol Transport and Processing in the Free Troposphere.

    NASA Astrophysics Data System (ADS)

    Ekman, Annica M. L.; Wang, Chien; Ström, Johan; Krejci, Radovan

    2006-02-01

    Large concentrations of small aerosols have been previously observed in the vicinity of anvils of convective clouds. A 3D cloud-resolving model (CRM) including an explicit size-resolving aerosol module has been used to examine the origin of these aerosols. Five different types of aerosols are considered: nucleation mode sulfate aerosols (here defined by 0 d 5.84 nm), Aitken mode sulfate aerosols (here defined by 5.84 nm d 31.0 nm), accumulation mode sulfate aerosols (here defined by d 31.0 nm), mixed aerosols, and black carbon aerosols.The model results suggest that approximately 10% of the initial boundary layer number concentration of Aitken mode aerosols and black carbon aerosols are present at the top of the convective cloud as the cloud reaches its decaying state. The simulated average number concentration of Aitken mode aerosols in the cloud anvil (1.6 × 104 cm-3) is in the same order of magnitude as observations. Thus, the model results strongly suggest that vertical convective transport, particularly during the active period of the convection, is responsible for a major part of the appearance of high concentrations of small aerosols (corresponding to the Aitken mode in the model) observed in the vicinity of cloud anvils.There is some formation of new aerosols within the cloud, but the formation is small. Nucleation mode aerosols are also efficiently scavenged through impaction scavenging by precipitation. Accumulation mode and mixed mode aerosols are efficiently scavenged through nucleation scavenging and their concentrations in the cloud anvil are either very low (mixed mode) or practically zero (accumulation mode).In addition to the 3D CRM, a box model, including important features of the aerosol module of the 3D model, has been used to study the formation of new aerosols after the cloud has evaporated. The possibility of these aerosols to grow to suitable cloud condensation or ice nuclei size is also examined. Concentrations of nucleation mode aerosols

  20. 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.

  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. 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.

  4. 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.

  5. Cloud droplet activation through oxidation of organic aerosol influenced by temperature and particle phase state

    DOE PAGES

    Slade, Jonathan H.; Shiraiwa, Manabu; Arangio, Andrea; ...

    2017-01-27

    Chemical aging of organic aerosol (OA) through multiphase oxidation reactions can alter their cloud condensation nuclei (CCN) activity and hygroscopicity. However, the oxidation kinetics and OA reactivity depend strongly on the particle phase state, potentially influencing the hydrophobic-to-hydrophilic conversion rate of carbonaceous aerosol. Here, amorphous Suwannee River fulvic acid (SRFA) aerosol particles, a surrogate humic-like substance (HULIS) that contributes substantially to global OA mass, are oxidized by OH radicals at different temperatures and phase states. When oxidized at low temperature in a glassy solid state, the hygroscopicity of SRFA particles increased by almost a factor of two, whereas oxidation ofmore » liquid-like SRFA particles at higher temperatures did not affect CCN activity. Low-temperature oxidation appears to promote the formation of highly-oxygenated particle-bound fragmentation products with lower molar mass and greater CCN activity, underscoring the importance of chemical aging in the free troposphere and its influence on the CCN activity of OA.« less

  6. 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.

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

    DOE PAGES

    Kercher, Andrew K.; Kolopus, James A.; Carroll, Kyler; ...

    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

  8. 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.

  9. Pharmacotherapy of depression and mixed states in bipolar disorder.

    PubMed

    Montgomery, S A; Schatzberg, A F; Guelfi, J D; Kasper, S; Nemeroff, C; Swann, A; Zajecka, J

    2000-09-01

    The treatment of bipolar depression requires the resolution of depression and the establishment of mood stability. A basic problem is that the treatments used in treating bipolar depression were developed and proven effective for other disease states: antidepressants for unipolar depression, and mood stabilizers for mania. The panel addressed four unresolved questions regarding depression in relation to bipolar disorder: (1) the relative effectiveness of different antidepressant treatments; (2) the relative likelihood of mood destabilization with different antidepressant treatments; (3) the effectiveness and role of mood-stabilizing medicines as antidepressants; and (4) the optimal approach to mixed states. The selection of an antidepressant depends both on its relative lack of mania- or hypomania-provoking potential and on its effectiveness against bipolar depression. There is little definitive evidence distinguishing effectiveness of the major groups of antidepressive agents, so side-effect profiles and pharmacokinetics are major considerations. The underlying bipolar disorder should be treated with mood stabilizers started simultaneously with any antidepressive treatments. Lithium, divalproex sodium and carbamazepine have all been found to be helpful, to some extent, in treating bipolar depressive episodes as well as for long-term mood stabilization. There is little evidence for long-term benefits of antidepressive agents in bipolar disorder, and some evidence that they may destabilize the disorder. Therefore, in contrast to the long-term use of mood-stabilizers, antidepressant use is recommended on a temporary basis. The duration of antidepressant treatment is determined by past history in terms of liability for mood destabilization, and by the ability of the patient to tolerate gradual antidepressant discontinuation without return of depression. Mixed states, where symptoms of depression and mania coexist, are regarded as a predictor of relatively poor

  10. 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

  11. 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.

  12. 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.

  13. 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.

  14. 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

  15. 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.

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

    PubMed

    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. 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...

  18. Size-selected black carbon mass distributions and mixing state in polluted and clean environments of northern India

    NASA Astrophysics Data System (ADS)

    Raatikainen, Tomi; Brus, David; Hooda, Rakesh K.; Hyvärinen, Antti-Pekka; Asmi, Eija; Sharma, Ved P.; Arola, Antti; Lihavainen, Heikki

    2017-01-01

    We have measured black carbon properties by using a size-selected single-particle soot photometer (SP2). The measurements were conducted in northern India at two sites: Gual Pahari is located at the Indo-Gangetic Plain (IGP) and Mukteshwar at the Himalayan foothills. Northern India is known as one of the absorbing aerosol hot spots, but detailed information about absorbing aerosol mixing state is still largely missing. Previous equivalent black carbon (eBC) mass concentration measurements are available for this region, and these are consistent with our observations showing that refractory black carbon (rBC) concentrations are about 10 times higher in Gual Pahari than those at Mukteshwar. Also, the number fraction of rBC-containing particles is higher in Gual Pahari, but individual rBC-containing particles and their size distributions are fairly similar. These findings indicate that particles at both sites have similar local and regional emission sources, but aerosols are also transported from the main source regions (IGP) to the less polluted regions (Himalayan foothills). Detailed examination of the rBC-containing particle properties revealed that they are most likely irregular particles such as fractal aggregates, but the exact structure remains unknown.

  19. Phase state is a limiting factor in hygroscopic growth of secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Pajunoja, Aki; Virtanen, Annele

    2014-05-01

    Secondary organic aerosol (SOA) particles formed from oxidation products of volatile organic compounds (VOC) form a significant fraction of the total atmospheric particulate matter affecting climate both directly and indirectly. The dependence of hygroscopicity on particle composition is often represented with the single parameter κ, commonly used in global models to describe the hygroscopic properties of atmospheric aerosol particles. The physical phase state of SOA particles affects the partitioning of organic vapors and also may affect the uptake of water vapor and particle activation into cloud droplets. Thus, hygroscopic behaviour of SOA particles is affected by composition (i.e. oxidation state and molecular size) but also by phase of particles. In this study the following three distinct studies were performed: (1) particle bounced fraction (BF) measurements, which are qualitatively related to particle phase, as a function of relative humidity using an Aerosol Bounce Instrument (ABI). We assume that the particles with BF > 0 are solid or semisolid, and that particles with BF = 0 behave mechanically as liquids (2) water uptake measured in the sub-saturated region using hygroscopicity tandem differential mobility analyzer (HTDMA) by measuring the ratio of wet to dry particle diameter following exposure to water vapor at a controlled RH (3) cloud droplet formation in the supersaturated region using a cloud condensation nuclei counter (CCNc). Particle composition and oxidation state was measured with a compact time of flight aerosol mass spectrometer (c-ToF-AMS). In this study we show that at sub-saturation conditions water uptake by SOA particles is restricted due to the kinetic limitations. Diffusion and solubility limitations inhibit water uptake until the humidity is high enough for dissolution to occur. Our studies show that this 'threshold' humidity is dependent on particle composition, oxidation state, and average molecular size. Our laboratory results

  20. 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%.

  1. Maximally entangled mixed states for qubit-qutrit systems

    NASA Astrophysics Data System (ADS)

    Mendonça, Paulo E. M. F.; Marchiolli, Marcelo A.; Hedemann, Samuel R.

    2017-02-01

    We consider the problems of maximizing the entanglement negativity of X-form qubit-qutrit density matrices with (i) a fixed spectrum and (ii) a fixed purity. In the first case, the problem is solved in full generality whereas, in the latter, partial solutions are obtained by imposing extra spectral constraints such as rank deficiency and degeneracy, which enable a semidefinite programming treatment for the optimization problem at hand. Despite the technically motivated assumptions, we provide strong numerical evidence that threefold degenerate X states of purity P reach the highest entanglement negativity accessible to arbitrary qubit-qutrit density matrices of the same purity, hence characterizing a sparse family of likely qubit-qutrit maximally entangled mixed states.

  2. 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.

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

    NASA Astrophysics Data System (ADS)

    Tonchev, N. S.

    2014-11-01

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

  4. 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.

  5. 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.

  6. 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.

  7. 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

  8. 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

  9. 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

  10. 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

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

    NASA Astrophysics Data System (ADS)

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

    2015-08-01

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

  12. The Houston Urban Heat Island: Surface Temperature, Aerosol Mixing Layer Height, and Surface Wind Field Relationships

    NASA Astrophysics Data System (ADS)

    Darby, L. S.; Senff, C. J.

    2007-12-01

    Both Dallas and Houston, Texas have comprehensive networks of surface meteorology and chemistry sensors. The similarities of the networks and lack of terrain in Dallas and Houston allow for the comparison of their urban heat islands (UHI). The Dallas UHI, unperturbed by thermal flows driven by the land/sea temperature difference, is a well-defined phenomenon over the summers of 2000-2006. Including all weather conditions, the average nighttime T(urban) - T(rural) temperature difference was between 1.5° and 2.0° C and the average daytime difference was ~ 1.0° C. Analysis of Houston temperature data, however, revealed a different picture due to the bay and gulf breezes. While the Houston UHI was a distinct phenomenon, even when including all weather conditions, the bay or gulf breeze modified the Houston UHI by cooling the city. Average nighttime T(urban) - T(rural) temperature differences in Houston were between 1.75° and 2.75° C. However, during the day, the rural areas to the north and west of the city were often warmer than the downtown area during afternoon hours as a result of the sea breeze. Averaging the Houston T(urban) - T(rural) temperature differences over the summers of 2000-2006 indicated a very small urban-rural temperature difference between 1400 to 1600 LST. In some individual years, such as 2000, 2003, 2005 and 2006, the urban areas were actually cooler than the rural areas, on average, in the mid-afternoon. These years had more bay breeze/gulf breeze activity to cool the urban area. We will also look at how land use, the UHI, and boundary-layer winds impact the horizontal distribution of boundary layer heights over the Houston area, as calculated from backscatter measurements from TOPAZ, an ozone and aerosol profiling lidar deployed on a NOAA Twin Otter in the summer of 2006 during the Texas Air Quality Study II.

  13. 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

  14. MATRIX-VBS (v1.0): implementing an evolving organic aerosol volatility in an aerosol microphysics model

    NASA Astrophysics Data System (ADS)

    Gao, Chloe Y.; Tsigaridis, Kostas; Bauer, Susanne E.

    2017-02-01

    The gas-particle partitioning and chemical aging of semi-volatile organic aerosol are presented in a newly developed box model scheme, where its effect on the growth, composition, and mixing state of particles is examined. The volatility-basis set (VBS) framework is implemented into the aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state), which resolves mass and number aerosol concentrations and in multiple mixing-state classes. The new scheme, MATRIX-VBS, has the potential to significantly advance the representation of organic aerosols in Earth system models by improving upon the conventional representation as non-volatile particulate organic matter, often also with an assumed fixed size distribution. We present results from idealized cases representing Beijing, Mexico City, a Finnish forest, and a southeastern US forest, and investigate the evolution of mass concentrations and volatility distributions for organic species across the gas and particle phases, as well as assessing their mixing state among aerosol populations. Emitted semi-volatile primary organic aerosols evaporate almost completely in the intermediate-volatility range, while they remain in the particle phase in the low-volatility range. Their volatility distribution at any point in time depends on the applied emission factors, oxidation by OH radicals, and temperature. We also compare against parallel simulations with the original scheme, which represented only the particulate and non-volatile component of the organic aerosol, examining how differently the condensed-phase organic matter is distributed across the mixing states in the model. The results demonstrate the importance of representing organic aerosol as a semi-volatile aerosol, and explicitly calculating the partitioning of organic species between the gas and particulate phases.

  15. MATRIX-VBS (v1.0): Implementing an Evolving Organic Aerosol Volatility in an Aerosol Microphysics Model

    NASA Technical Reports Server (NTRS)

    Gao, Chloe Y.; Tsigaridis, Kostas; Bauer, Susanne E.

    2017-01-01

    The gas-particle partitioning and chemical aging of semi-volatile organic aerosol are presented in a newly developed box model scheme, where its effect on the growth, composition, and mixing state of particles is examined. The volatility-basis set (VBS) framework is implemented into the aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state), which resolves mass and number aerosol concentrations and in multiple mixing-state classes. The new scheme, MATRIX-VBS, has the potential to significantly advance the representation of organic aerosols in Earth system models by improving upon the conventional representation as non-volatile particulate organic matter, often also with an assumed fixed size distribution. We present results from idealized cases representing Beijing, Mexico City, a Finnish forest, and a southeastern US forest, and investigate the evolution of mass concentrations and volatility distributions for organic species across the gas and particle phases, as well as assessing their mixing state among aerosol populations. Emitted semi-volatile primary organic aerosols evaporate almost completely in the intermediate-volatility range, while they remain in the particle phase in the low-volatility range. Their volatility distribution at any point in time depends on the applied emission factors, oxidation by OH radicals, and temperature. We also compare against parallel simulations with the original scheme, which represented only the particulate and non-volatile component of the organic aerosol, examining how differently the condensed-phase organic matter is distributed across the mixing states in the model. The results demonstrate the importance of representing organic aerosol as a semi-volatile aerosol, and explicitly calculating the partitioning of organic species between the gas and particulate phases.

  16. Deliquescence behavior of internally mixed clay and salt aerosols by optical extinction measurements.

    PubMed

    Attwood, Alexis Rae; Greenslade, Margaret E

    2012-05-10

    Internal mixtures of montmorillonite, a clay component of mineral dust, with sodium chloride or ammonium sulfate were studied optically using cavity ring down spectroscopy. The effects of the addition of the clay to the optically observed deliquescence relative humidity (DRH) and water uptake of these salts were considered by investigating a series of different salt mass fractions. In most cases, montmorillonite alters the hygroscopic properties, lowering the DRH in comparison to the pure salt, and causes the particles to transition from solid to liquid at a lower relative humidity than is expected based on the salt alone. Predictions based on volume-weighted mixing rules were not accurate for most measurements around the DRH. We attribute deviations from theory to changes in the Gibbs free energy of the system caused by disturbances in the ion-ion interactions and lattice structure allowing water uptake prior to the DRH of the salt. Our optical results contradict some current measurements in the literature that suggest little change in the hygroscopic behavior of salts when insoluble mineral dust components are added.

  17. 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

  18. 30-year lidar observations of the stratospheric aerosol layer state over Tomsk (Western Siberia, Russia)

    NASA Astrophysics Data System (ADS)

    Zuev, Vladimir V.; Burlakov, Vladimir D.; Nevzorov, Aleksei V.; Pravdin, Vladimir L.; Savelieva, Ekaterina S.; Gerasimov, Vladislav V.

    2017-02-01

    There are only four lidar stations in the world which have almost continuously performed observations of the stratospheric aerosol layer (SAL) state over the last 30 years. The longest time series of the SAL lidar measurements have been accumulated at the Mauna Loa Observatory (Hawaii) since 1973, the NASA Langley Research Center (Hampton, Virginia) since 1974, and Garmisch-Partenkirchen (Germany) since 1976. The fourth lidar station we present started to perform routine observations of the SAL parameters in Tomsk (56.48° N, 85.05° E, Western Siberia, Russia) in 1986. In this paper, we mainly focus on and discuss the stratospheric background period from 2000 to 2005 and the causes of the SAL perturbations over Tomsk in the 2006-2015 period. During the last decade, volcanic aerosol plumes from tropical Mt. Manam, Soufrière Hills, Rabaul, Merapi, Nabro, and Kelut and extratropical (northern) Mt. Okmok, Kasatochi, Redoubt, Sarychev Peak, Eyjafjallajökull, and Grímsvötn were detected in the stratosphere over Tomsk. When it was possible, we used the NOAA HYSPLIT trajectory model to assign aerosol layers observed over Tomsk to the corresponding volcanic eruptions. The trajectory analysis highlighted some surprising results. For example, in the cases of the Okmok, Kasatochi, and Eyjafjallajökull eruptions, the HYSPLIT air mass backward trajectories, started from altitudes of aerosol layers detected over Tomsk with a lidar, passed over these volcanoes on their eruption days at altitudes higher than the maximum plume altitudes given by the Smithsonian Institution Global Volcanism Program. An explanation of these facts is suggested. The role of both tropical and northern volcanic eruptions in volcanogenic aerosol loading of the midlatitude stratosphere is also discussed. In addition to volcanoes, we considered other possible causes of the SAL perturbations over Tomsk, i.e., the polar stratospheric cloud (PSC) events and smoke plumes from strong forest fires. At least

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

    NASA Astrophysics Data System (ADS)

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

    2016-08-01

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

  20. Cloud droplet activation through oxidation of organic aerosol influenced by temperature and particle phase state: CLOUD ACTIVATION BY AGED ORGANIC AEROSOL

    DOE PAGES

    Slade, Jonathan H.; Shiraiwa, Manabu; Arangio, Andrea; ...

    2017-02-04

    Chemical aging of organic aerosol (OA) through multiphase oxidation reactions can alter their cloud condensation nuclei (CCN) activity and hygroscopicity. However, the oxidation kinetics and OA reactivity depend strongly on the particle phase state, potentially influencing the hydrophobic-to-hydrophilic conversion rate of carbonaceous aerosol. Here, amorphous Suwannee River fulvic acid (SRFA) aerosol particles, a surrogate humic-like substance (HULIS) that contributes substantially to global OA mass, are oxidized by OH radicals at different temperatures and phase states. When oxidized at low temperature in a glassy solid state, the hygroscopicity of SRFA particles increased by almost a factor of two, whereas oxidation ofmore » liquid-like SRFA particles at higher temperatures did not affect CCN activity. Low-temperature oxidation appears to promote the formation of highly-oxygenated particle-bound fragmentation products with lower molar mass and greater CCN activity, underscoring the importance of chemical aging in the free troposphere and its influence on the CCN activity of OA.« less

  1. 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

  2. Secondary organic aerosol production from aqueous reactions of atmospheric phenols with an organic triplet excited state.

    PubMed

    Smith, Jeremy D; Sio, Vicky; Yu, Lu; Zhang, Qi; Anastasio, Cort

    2014-01-21

    Condensed-phase chemistry plays a significant role in the formation and evolution of atmospheric organic aerosols. Past studies of the aqueous photoformation of secondary organic aerosol (SOA) have largely focused on hydroxyl radical oxidation, but here we show that triplet excited states of organic compounds ((3)C*) can also be important aqueous oxidants. We studied the aqueous photoreactions of three phenols (phenol, guaiacol, and syringol) with the aromatic carbonyl 3,4-dimethoxybenzaldehyde (DMB); all of these species are emitted by biomass burning. Under simulated sunlight, DMB forms a triplet excited state that rapidly oxidizes phenols to form low-volatility SOA. Rate constants for these reactions are fast and increase with decreasing pH and increasing methoxy substitution of the phenols. Mass yields of aqueous SOA are near 100% for all three phenols. For typical ambient conditions in areas with biomass combustion, the aqueous oxidation of phenols by (3)C* is faster than by hydroxyl radical, although rates depend strongly on pH, oxidant concentrations, and the identity of the phenol. Our results suggest that (3)C* can be the dominant aqueous oxidant of phenols in areas impacted by biomass combustion and that this is a significant pathway for forming SOA.

  3. 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.

    2014-05-01

    Hygroscopic behavior of organic compounds, including levoglucosan, 4-hydroxybenzoic acid and humic acid, and 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 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-hydrobenxybenzoic 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 effects), which are not

  4. 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

  5. Condensing Organic Aerosols in a Microphysical Model

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

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

    DOE PAGES

    Willis, M. D.; Lee, A. K. Y.; Onasch, T. B.; ...

    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

  7. 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

  8. Secondary organic aerosol formation during June 2010 in Central Europe: measurements and modelling studies with a mixed thermodynamic-kinetic approach

    NASA Astrophysics Data System (ADS)

    Langmann, B.; Sellegri, K.; Freney, E.

    2014-04-01

    Until recently secondary organic carbon aerosol (SOA) mass concentrations have been systematically underestimated by three-dimensional atmospheric-chemistry-aerosol models. With a newly proposed concept of aging of organic vapours, more realistic model results for organic carbon aerosol mass concentrations can be achieved. Applying a mixed thermodynamic-kinetic approach for SOA formation shifted the aerosol size distribution towards particles in the cloud condensation nuclei size range, thereby emphasising the importance of SOA formation schemes for modelling realistic cloud and precipitation formation. The additional importance of hetero-molecular nucleation between H2SO4 and organic vapours remains to be evaluated in three-dimensional atmospheric-chemistry-aerosol models. Here a case study is presented focusing on Puy-de-Dôme, France in June 2010. The measurements indicate a considerable increase in SOA mass concentration during the measurement campaign, which could be reproduced by modelling using a simplified thermodynamic-kinetic approach for SOA formation and increased biogenic volatile organic compound (VOC) precursor emissions. Comparison with a thermodynamic SOA formation approach shows a huge improvement in modelled SOA mass concentration with the thermodynamic-kinetic approach for SOA formation. SOA mass concentration increases by a factor of up to 6 accompanied by a slight improvement of modelled particle size distribution. Even though nucleation events at Puy-de-Dôme were rare during the chosen period of investigation, a weak event in the boundary layer could be reproduced by the model in a sensitivity study when nucleation of low-volatile secondary organic vapour is included. Differences in the model results with and without nucleation of organic vapour are visible in the lower free troposphere over several days. Taking into account the nucleation of organic vapour leads to an increase in accumulation mode particles due to coagulation and

  9. 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.

  10. 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.

  11. Characterization of Black Carbon Mixing State Field Campaign Report

    SciTech Connect

    Sedlacek, A.; Davidovits, P.; Lewis, E. R.; Onasch, T. B.

    2016-04-01

    Interpreting the temporal relationship between the scattering and incandescence signals recorded by the Single Particle Soot Photometer (SP2), Sedlacek et al. (2012) reported that 60% of the refractory black carbon containing particles in a plume containing biomass burning tracers exhibited non-core-shell structure. Because the relationship between the rBC (refractory black carbon) incandescence and the scattering signals had not been reported in the peer-reviewed literature, and to further evaluate the initial interpretation by Sedlacek et al., a series of experiments was undertaken to investigate black carbon-containing particles of known morphology using Regal black (RB), a proxy for collapsed soot, as the light-absorbing substance to characterize this signal relationship. Particles were formed by coagulation of RB with either a solid substance (sodium chloride or ammonium sulfate) or a liquid substance (dioctyl sebacate), and by condensation with dioctyl sebacate, the latter experiment forming particles in a core-shell configuration. Each particle type experienced fragmentation (observed as negative lagtimes), and each yielded similar lagtime responses in some instances, confounding attempts to differentiate particle morphology using current SP2 lagtime analysis. SP2 operating conditions, specifically laser power and sample flow rate, which in turn affect the particle heating and dissipation rates, play an important role in the behavior of particles in the SP2, including probability of fragmentation. This behavior also depended on the morphology of the particles and on the thermochemical properties of the non-RB substance. Although these influences cannot currently be unambiguously separated, the SP2 analysis may still provide useful information on particle mixing states and black carbon particle sources. This work was communicated in a 2015 publication (Sedlacek et al. 2015)

  12. 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

  13. Water soluble organic carbon in aerosols (PM1, PM2.5, PM10) and various precipitation forms (rain, snow, mixed) over the southern Baltic Sea station.

    PubMed

    Witkowska, Agnieszka; Lewandowska, Anita U

    2016-12-15

    In the urbanized coastal zone of the Southern Baltic, complex measurements of water soluble organic carbon (WSOC) were conducted between 2012 and 2015, involving atmospheric precipitation in its various forms (rain, snow, mixed) and PM1, PM2.5 and PM10 aerosols. WSOC constituted about 60% of the organic carbon mass in aerosols of various sizes. The average concentration of WSOC was equal to 2.6μg∙m(-3) in PM1, 3.6μg∙m(-3) in PM2.5 and 4.4μg∙m(-3) in PM10. The lowest concentration of WSOC was noted in summer as a result of effective removal of this compound with rainfall. The highest WSOC concentrations in PM2.5 and PM10 aerosols were measured in spring, which should be associated with developing vegetation on land and in the sea. On the other hand, the highest WSOC concentrations in PM1 occurred in winter at low air temperatures and greatest atmospheric stability, when there were increased carbon emissions from fuel combustion in the communal-utility sector and from transportation. WSOC concentrations in precipitation were determined by its form. Mixed precipitation turned out to be the richest in soluble organic carbon (5.1mg·dm(-3)), while snow contained the least WSOC (1.7mg·dm(-3)). Snow and rain cleaned carbon compounds from the atmosphere more effectively when precipitation lasted longer than 24h, while in the case of mixed precipitation WSOC was removed most effectively within the first 24h.

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

    SciTech Connect

    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.

    2016-01-01

    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

  15. 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.

  16. MATRIX-VBS Condensing Organic Aerosols in an Aerosol Microphysics Model

    NASA Technical Reports Server (NTRS)

    Gao, Chloe Y.; Tsigaridis, Konstas; Bauer, Susanne E.

    2015-01-01

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

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

    PubMed Central

    Ferraris, Chiara F.

    2001-01-01

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

  18. Mixed-valence states of 11, 1111-dialkyl- and 11, 1111-bis(methylbenzyl)biferrocenium triiodides

    NASA Astrophysics Data System (ADS)

    Nakashima, Satoru; Masuda, Yuichi; Motoyama, Izumi; Sano, Hirotoshi

    1988-02-01

    It was found that the packing of cations and anions influences the electronic structures of mixed-valence binuclear ferrocene derivatives. Temperature-dependence of the mixed-valence state of 11, 1111-diisobutylbiferrocenium triiodide was observed in a crystalline state, whereas only a trapped-valence state was found in a dispersed state. The packing effect was also observed for a series of 11, 1111-dialkyl- and 11, 1111-bis(methylbenzyl)biferrocenium triiodides by means of ESR spectroscopy.

  19. 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.

  20. “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...

  1. 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

  2. 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.

  3. Mixed LICORS: A Nonparametric Algorithm for Predictive State Reconstruction

    PubMed Central

    Goerg, Georg M.; Shalizi, Cosma Rohilla

    2015-01-01

    We introduce mixed LICORS, an algorithm for learning nonlinear, high-dimensional dynamics from spatio-temporal data, suitable for both prediction and simulation. Mixed LICORS extends the recent LICORS algorithm (Goerg and Shalizi, 2012) from hard clustering of predictive distributions to a non-parametric, EM-like soft clustering. This retains the asymptotic predictive optimality of LICORS, but, as we show in simulations, greatly improves out-of-sample forecasts with limited data. The new method is implemented in the publicly-available R package LICORS. PMID:26279743

  4. Charge state distribution studies of pure and oxygen mixed krypton ECR plasma - signature of isotope anomaly and gas mixing effect.

    PubMed

    Kumar, Pravin; Mal, Kedar; Rodrigues, G

    2016-11-01

    We report the charge state distributions of the pure, 25% and 50% oxygen mixed krypton plasma to shed more light on the understanding of the gas mixing and the isotope anomaly [A. G. Drentje, Rev. Sci. Instrum. 63 (1992) 2875 and Y Kawai, D Meyer, A Nadzeyka, U Wolters and K Wiesemann, Plasma Sources Sci. Technol. 10 (2001) 451] in the electron cyclotron resonance (ECR) plasmas. The krypton plasma was produced using a 10 GHz all-permanent-magnet ECR ion source. The intensities of the highly abundant four isotopes, viz. (82) Kr (~11.58%), (83) Kr (~11.49%), (84) Kr (~57%) and (86) Kr (17.3%) up to ~ +14 charge state have been measured by extracting the ions from the plasma and analysing them in the mass and the energy using a large acceptance analyzer-cum-switching dipole magnet. The influence of the oxygen gas mixing on the isotopic krypton ion intensities is clearly evidenced beyond +9 charge state. With and without oxygen mixing, the charge state distribution of the krypton ECR plasma shows the isotope anomaly with unusual trends. The anomaly in the intensities of the isotopes having quite closer natural abundance, viz. (82) Kr, (86) Kr and (83) Kr, (86) Kr is prominent, whereas the intensity ratio of (86) Kr to (84) Kr shows a weak signature of it. The isotope anomaly tends to disappear with increasing oxygen mixing in the plasma. The observed trends in the intensities of the krypton isotopes do not follow the prediction of linear Landau wave damping in the plasma. Copyright © 2016 John Wiley & Sons, Ltd.

  5. 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.

  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. 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.

  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.

    2014-06-01

    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.

  9. 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.

  10. 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.

  11. 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.

  12. 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

  13. 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

  14. Effect of Aggregation and Mixing on optical properties of Black Carbon

    NASA Astrophysics Data System (ADS)

    Scarnato, B. V.; Nielsen, K.; Vahidinia, S.; Richard, D.

    2013-12-01

    According to recent studies, internal mixing of black carbon (BC) with other aerosol materials in the atmosphere alters its aggregate shape, absorption and scattering of solar radiation, and then radiative forcing. These mixing state effects are not yet fully understood. Multiple studies have demonstrated a strong variability in the observed mass absorption efficiency of BC, when it becomes internally mixed with non-absorbing organic compounds. Recent modeling studies show that BC absorption enhancement depends strongly on the BC aggregate compactness and on the resulting mixing with other aerosol compounds. The impact of morphology and mixing state on aerosol optical properties is a relevant topic, as well, for interpretation of remote sensing measurements. In radiative transfer calculations, that are also used to interpret space or ground-based observations of Earth, it is common to approximate aerosol shape to homogeneous spherical or spheroidal particles, ignoring the effect of realistic morphology and realistic mixing with other aerosol compounds, which can lead to significant errors in retrieved parameters, such as the aerosol type, optical thickness, particle size distributions and composition, and so forth. This paper will present a sensitivity study of the effect of the BC aggregate morphology and the mixing state on optical properties, when BC is mixed with ammonium sulfate, sodium chloride, dust and others. Optical properties are computed, using a discrete dipole approximation model (DDSCAT), in accordance with observed BC morphology and mixing state published in literature.

  15. 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.

  16. Nuclear structure of 96,98Mo: Shape coexistence and mixed-symmetry states

    NASA Astrophysics Data System (ADS)

    Thomas, T.; Werner, V.; Jolie, J.; Nomura, K.; Ahn, T.; Cooper, N.; Duckwitz, H.; Fitzler, A.; Fransen, C.; Gade, A.; Hinton, M.; Ilie, G.; Jessen, K.; Linnemann, A.; Petkov, P.; Pietralla, N.; Radeck, D.

    2016-03-01

    Excited low-spin states in 96Mo and 98Mo have been studied in γγ angular correlation experiments in order to determine spins and multipole mixing ratios. Furthermore, from a Doppler lineshape analysis effective lifetimes τ in the femtosecond range were obtained. The experimental data show a complex spectrum due to configuration mixing, which is confirmed by Interacting Boson Model calculations based on a Skyrme energy density functional. The M1-transition strengths of transitions depopulating excited 2+ states to the first 2+ state are discussed in terms of the proton-neutron mixed symmetry.

  17. Hydration State of the Ambient Aerosol in the North Pacific Ocean from Controlled Relative Humidity Light Scattering Measurements

    NASA Astrophysics Data System (ADS)

    Rood, M. J.; Carrico, K.; Kus, P.; Quinn, T.; Bates, T.

    2002-12-01

    The hydration state of the ambient aerosol over the North Pacific was studied onboard the R/V Ronald Brown during ACE-Asia in spring 2001. Determination of whether ambient aerosols exist in a "dry" state, "hydrated" state, or a mixture of both states is important in determining the radiative effects of aerosols and their influence on heterogeneous atmospheric chemistry. Three nephelometers measured aerosol light scattering coefficients as a function of controlled relative humidity (20% < RH < 85%), wavelength of light (450, 550, and 700 nm), and particle diameter (Dp) <10 um and 1 um. One nephelometer was at "dry" conditions (RH = 19 +/- 5%) while a second downstream nephelometer was operated with RH scanning between 35% and 85%, while alternating the scans so they start at the low RH "dry" condition or the high RH "hydrated" condition. A third nephelometer was operated at an intermediate RH of 50 +/- 8%. In the latter, the aerosol only experienced decreasing RH conditions from their ambient state. The intermediate RH light scattering measurement was made because it likely did not perturb the aerosol from its ambient hydration state as the aerosol generally would not have deliquesced or crystallized for such a change in RH conditions (i.e. changed phase from a solution drop to a dry crystal). Light scattering values vs. RH (f(RH)) provides humidograms that were classified and fit to functions according to whether the structure followed a smooth monotonic function or deliquescent behavior (step changes in f(RH) with a possible hysteresis loop). Deliquescent behavior was observed 40% of the time with Dp < 1 um and 56% of the time with Dp < 10 um, likely due to the influence of coarse mode seasalt aerosol. The deliquescence RH was 77 +/- 2% while the efflorescence RH was 41 +/- 2% for all humidograms demonstrating deliquescence. The intermediate RH nephelometer measured light scattering values on the lower "dry" branch of the hysteresis loop 9% of the time, in between

  18. Mixed-state form factors of U(1) twist fields in the Dirac theory

    NASA Astrophysics Data System (ADS)

    Chen, Yixiong

    2016-08-01

    Using the ‘Liouville space’ (the space of operators) of the massive Dirac theory, we define mixed-state form factors of U(1) twist fields. We consider mixed states with density matrices diagonal in the asymptotic particle basis. This includes the thermal Gibbs state as well as all generalized Gibbs ensembles of the Dirac theory. When the mixed state is specialized to a thermal Gibbs state, using a Riemann-Hilbert problem and low-temperature expansion, we obtain finite-temperature form factors of U(1) twist fields. We then propose the expression for form factors of U(1) twist fields in general diagonal mixed states. We verify that these form factors satisfy a system of nonlinear functional differential equations, which is derived from the trace definition of mixed-state form factors. At last, under weak analytic conditions on the eigenvalues of the density matrix, we write down the large distance form factor expansions of two-point correlation functions of these twist fields. Using the relation between the Dirac and Ising models, this provides the large-distance expansion of the Rényi entropy (for integer Rényi parameter) in the Ising model in diagonal mixed states.

  19. Seasonal variations in Titan's stratosphere observed with Cassini/CIRS: temperature, trace molecular gas and aerosol mixing ratio profiles

    NASA Astrophysics Data System (ADS)

    Vinatier, S.; Bézard, B.; Lebonnois, S.; Teanby, N. A.; Rannou, P.; Anderson, C. M.; Achterberg, R. K.

    2013-12-01

    Titan's northern spring equinox occurred in August 2009. General Circulation Models 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. 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 between 2009 and 2013 that we used to monitor the seasonal evolution of the vertical profiles of temperature, molecular (C2H2, C2H6, HCN, ...) and aerosol abundances.

  20. 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.

  1. High-NOON states by mixing quantum and classical light.

    PubMed

    Afek, Itai; Ambar, Oron; Silberberg, Yaron

    2010-05-14

    Precision measurements can be brought to their ultimate limit by harnessing the principles of quantum mechanics. In optics, multiphoton entangled states, known as NOON states, can be used to obtain high-precision phase measurements, becoming more and more advantageous as the number of photons grows. We generated "high-NOON" states (N = 5) by multiphoton interference of quantum down-converted light with a classical coherent state in an approach that is inherently scalable. Super-resolving phase measurements with up to five entangled photons were produced with a visibility higher than that obtainable using classical light only.

  2. 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.

  3. 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.

  4. Aerosolization properties, surface composition and physical state of spray-dried protein powders.

    PubMed

    Bosquillon, Cynthia; Rouxhet, Paul G; Ahimou, François; Simon, Denis; Culot, Christine; Préat, Véronique; Vanbever, Rita

    2004-10-19

    Powder aerosols made of albumin, dipalmitoylphosphatidylcholine (DPPC) and a protein stabilizer (lactose, trehalose or mannitol) were prepared by spray-drying and analyzed for aerodynamic behavior, surface composition and physical state. The powders exited a Spinhaler inhaler as particle aggregates, the size of which depending on composition, spray-drying parameters and airflow rate. However, due to low bulk powder tap density (<0.15 g/cm3), the aerodynamic size of a large fraction of aggregates remained respirable (<5 microm). Fine particle fractions ranged between 21% and 41% in an Andersen cascade impactor operated at 28.3 l/min, with mannitol and lactose providing the most cohesive and free-flowing powders, respectively. Particle surface analysis by X-ray photoelectron spectroscopy (XPS) revealed a surface enrichment with DPPC relative to albumin for powders prepared under certain spray-drying conditions. DPPC self-organized in a gel phase in the particle and no sugar or mannitol crystals were detected by X-ray diffraction. Water sorption isotherms showed that albumin protected lactose from moisture-induced crystallization. In conclusion, a proper combination of composition and spray-drying parameters allowed to obtain dry powders with elevated fine particle fractions (FPFs) and a physical environment favorable to protein stability.

  5. Control aspects of quantum computing using pure and mixed states.

    PubMed

    Schulte-Herbrüggen, Thomas; Marx, Raimund; Fahmy, Amr; Kauffman, Louis; Lomonaco, Samuel; Khaneja, Navin; Glaser, Steffen J

    2012-10-13

    Steering quantum dynamics such that the target states solve classically hard problems is paramount to quantum simulation and computation. And beyond, quantum control is also essential to pave the way to quantum technologies. Here, important control techniques are reviewed and presented in a unified frame covering quantum computational gate synthesis and spectroscopic state transfer alike. We emphasize that it does not matter whether the quantum states of interest are pure or not. While pure states underly the design of quantum circuits, ensemble mixtures of quantum states can be exploited in a more recent class of algorithms: it is illustrated by characterizing the Jones polynomial in order to distinguish between different (classes of) knots. Further applications include Josephson elements, cavity grids, ion traps and nitrogen vacancy centres in scenarios of closed as well as open quantum systems.

  6. 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...

  7. Dynamic terahertz spectroscopy of gas molecules mixed with unwanted aerosol under atmospheric pressure using fibre-based asynchronous-optical-sampling terahertz time-domain spectroscopy.

    PubMed

    Hsieh, Yi-Da; Nakamura, Shota; Abdelsalam, Dahi Ghareab; Minamikawa, Takeo; Mizutani, Yasuhiro; Yamamoto, Hirotsugu; Iwata, Tetsuo; Hindle, Francis; Yasui, Takeshi

    2016-06-15

    Terahertz (THz) spectroscopy is a promising method for analysing polar gas molecules mixed with unwanted aerosols due to its ability to obtain spectral fingerprints of rotational transition and immunity to aerosol scattering. In this article, dynamic THz spectroscopy of acetonitrile (CH3CN) gas was performed in the presence of smoke under the atmospheric pressure using a fibre-based, asynchronous-optical-sampling THz time-domain spectrometer. To match THz spectral signatures of gas molecules at atmospheric pressure, the spectral resolution was optimized to 1 GHz with a measurement rate of 1 Hz. The spectral overlapping of closely packed absorption lines significantly boosted the detection limit to 200 ppm when considering all the spectral contributions of the numerous absorption lines from 0.2 THz to 1 THz. Temporal changes of the CH3CN gas concentration were monitored under the smoky condition at the atmospheric pressure during volatilization of CH3CN droplets and the following diffusion of the volatilized CH3CN gas without the influence of scattering or absorption by the smoke. This system will be a powerful tool for real-time monitoring of target gases in practical applications of gas analysis in the atmospheric pressure, such as combustion processes or fire accident.

  8. 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

  9. 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.

  10. 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.

  11. 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

  12. Largest separable balls around the maximally mixed bipartite quantum state

    NASA Astrophysics Data System (ADS)

    Gurvits, Leonid; Barnum, Howard

    2002-12-01

    For finite-dimensional bipartite quantum systems, we find the exact size of the largest balls, in spectral lp norms for 1<=p<=∞, of separable (unentangled) matrices around the identity matrix. This implies a simple and intuitively meaningful geometrical sufficient condition for separability of bipartite density matrices: that their purity tr ρ2 not be too large. Theoretical and experimental applications of these results include algorithmic problems such as computing whether or not a state is entangled, and practical ones such as obtaining information about the existence or nature of entanglement in states reached by nuclear magnetic resonance quantum computation implementations or other experimental situations.

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

    PubMed

    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.

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

    PubMed Central

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

    2015-01-01

    Abstract A sectional aerosol model (CARMA) has been developed and coupled with the Community Earth System Model (CESM1). Aerosol microphysics, radiative properties, and interactions with clouds are simulated in the size‐resolving model. The model described here uses 20 particle size bins for each aerosol component including freshly nucleated sulfate particles, as well as mixed particles containing sulfate, primary organics, black carbon, dust, and sea salt. The model also includes five types of bulk secondary organic aerosols with four volatility bins. The overall cost of CESM1‐CARMA is approximately ∼2.6 times as much computer time as the standard three‐mode aerosol model in CESM1 (CESM1‐MAM3) and twice as much computer time as the seven‐mode aerosol model in CESM1 (CESM1‐MAM7) using similar gas phase chemistry codes. Aerosol spatial‐temporal distributions are simulated and compared with a large set of observations from satellites, ground‐based measurements, and airborne field campaigns. Simulated annual average aerosol optical depths are lower than MODIS/MISR satellite observations and AERONET observations by ∼32%. This difference is within the uncertainty of the satellite observations. CESM1/CARMA reproduces sulfate aerosol mass within 8%, organic aerosol mass within 20%, and black carbon aerosol mass within 50% compared with a multiyear average of the IMPROVE/EPA data over United States, but differences vary considerably at individual locations. Other data sets show similar levels of comparison with model simulations. The model suggests that in addition to sulfate, organic aerosols also significantly contribute to aerosol mass in the tropical UTLS, which is consistent with limited data. PMID:27668039

  15. 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

    2012-04-03

    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.

  16. Particle bound black carbon size distribution and mixing state in urban environments using a novel tandem differential mobility analyzer and aethalometer

    NASA Astrophysics Data System (ADS)

    Ning, Zhi; Westerdahl, Dane; Wong, Ka-Chun; Chan, Ka-Lok

    2013-04-01

    Particle bound black carbon (BC) has dominant anthropogenic origins from fossil fuel combustion and biomass burning sources. It is an important component of the light absorbing aerosols in the atmosphere, playing a role in the earth's radiative balance and climate change. While the mixing states of the BC largely determine the coating on the particles, knowledge of the size distribution of BC is key to the accurate modelling of their absorption of solar radiation. Also, BC is a major component of the diesel PM emissions, recently classified by World Health Organization as Class I carcinogen, and has been widely documented with association of a variety of adverse health effects. Their sizes also determine the fraction of lung deposition. Due to the limited information of the mixing state and size distribution of BC, there still exists large uncertainty of the role of BC in climate change modelling. This study presents a novel approach of the direct and continuous measurement of atmospheric BC size distribution and coating by tandem operation of a differential mobility analyzer and a modified aethalometer. A condensation particle counter was deployed concurrently with the aethalometer to determine the particle number size distribution. Particle coating on BC was further estimated. A wide range of particle sizes (15-700nm) was investigated to determine the BC mass size distribution in fresh diesel engine tailpipe emissions and different ambient environments including urban and roadside. The results showed the evolution of BC mixing state and size distribution from fresh engine emissions to the roadside and urban ambient environments. The results provide important references for climate modelling to better determine the effect of radiative forcing from urban aerosols.

  17. 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

  18. 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.

  19. 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.

  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. 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.

  2. 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.

  3. Continuum of depressive and manic mixed states in patients with bipolar disorder: quantitative measurement and clinical features.

    PubMed

    Swann, Alan C; Steinberg, Joel L; Lijffijt, Marijn; Moeller, Gerard F

    2009-10-01

    Bipolar mixed states combine depressive and manic features, presenting diagnostic and treatment challenges and reflecting a severe form of the illness. DSM-IV criteria for a mixed state require combined depressive and manic syndromes, but a range of mixed states has been described clinically. A unified definition of mixed states would be valuable in understanding their diagnosis, mechanism and treatment implications. We investigated the manner in which depressive and manic features combine to produce a continuum of mixed states. In 88 subjects with bipolar disorder (DSM-IV), we evaluated symptoms and clinical characteristics, and compared depression-based, mania-based, and other published definitions of mixed states. We developed an index of the extent to which symptoms were mixed (Mixed State Index, MSI) and characterized its relationship to clinical state. Predominately manic and depressive mixed states using criteria from recent literature, as well as Kraepelinian mixed states, had similar symptoms and MSI scores. Anxiety correlated significantly with depression scores in manic subjects and with mania scores in depressed subjects. Discriminant function analysis associated mixed states with symptoms of hyperactivity and negative cognitions, but not subjective depressive or elevated mood. High MSI scores were associated with severe course of illness. For depressive or manic episodes, characteristics of mixed states emerged with two symptoms of the opposite polarity. This was a cross-sectional study. Mixed states appear to be a continuum. An index of the degree to which depressive and manic symptoms combine appears useful in identifying and characterizing mixed states. We propose a depressive or manic episode with three or more symptoms of the opposite polarity as a parsimonious definition of a mixed state.

  4. Quantum correlations of two-qubit states with one maximally mixed marginal

    NASA Astrophysics Data System (ADS)

    Milne, Antony; Jennings, David; Jevtic, Sania; Rudolph, Terry

    2014-08-01

    We investigate the entanglement, CHSH nonlocality, fully entangled fraction, and symmetric extendibility of two-qubit states that have a single maximally mixed marginal. Within this set of states, the steering ellipsoid formalism has recently highlighted an interesting family of so-called maximally obese states. These are found to have extremal quantum correlation properties that are significant in the steering ellipsoid picture and for the study of two-qubit states in general.

  5. 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

  6. A revisit to non-maximally entangled mixed states: teleportation witness, noisy channel and discord

    NASA Astrophysics Data System (ADS)

    Roy, Sovik; Ghosh, Biplab

    2017-04-01

    We constructed a class of non-maximally entangled mixed states (Adhikari et al. in Quantum Inf Comput 10:0398, 2010) and extensively studied their entanglement properties and also their usefulness as teleportation channels. In this article, we have revisited our constructed state and have studied it from three different perspectives. Since every entangled state is associated with a witness operator, we have found a suitable entanglement as well as teleportation witness operator for our non-maximally entangled mixed states. We considered the noisy channel's effects on our constructed states to see how much it affects the states' capacities as teleportation channels. For this purpose, we have mainly focussed on amplitude damping channel. A comparative study on concurrence and quantum discord of our constructed state of Adhikari et al. (2010) has also been carried out here.

  7. 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.

  8. Morphology and mixing state of individual freshly emitted wildfire carbonaceous particles.

    PubMed

    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.

  9. 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

  10. Rotational State Microwave Mixing for Laser Cooling of Complex Diatomic Molecules

    NASA Astrophysics Data System (ADS)

    Yeo, Mark; Hummon, Matthew T.; Collopy, Alejandra L.; Yan, Bo; Hemmerling, Boerge; Chae, Eunmi; Doyle, John M.; Ye, Jun

    2015-06-01

    We demonstrate the mixing of rotational states in the ground electronic state using microwave radiation to enhance optical cycling in the molecule yttrium (II) monoxide (YO). This mixing technique is used in conjunction with a frequency modulated and chirped continuous wave laser to slow longitudinally a cryogenic buffer-gas beam of YO. We generate a flux of YO below 10 m /s , directly loadable into a three-dimensional magneto-optical trap. This technique opens the door for laser cooling of diatomic molecules with more complex loss channels due to intermediate states.

  11. Hall Crystal States at ν = 2 and Moderate Landau Level Mixing

    NASA Astrophysics Data System (ADS)

    Murthy, Ganpathy

    2000-08-01

    The ν = 2 quantum Hall state at low Zeeman coupling is well known to be a translationally invariant singlet if Landau level mixing is small. At zero Zeeman interaction, as Landau level mixing increases, the translationally invariant state becomes unstable to an inhomogeneous state. This is the first realistic example of a full Hall crystal, which shows the coexistence of quantum Hall order and density wave order. The full Hall crystal differs from the more familiar Wigner crystal by a topological property, which results in it having only linearly dispersing collective modes at small q, and no q3/2 magnetophonon. I present calculations of the topological number and the collective modes.

  12. 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.

  13. Geometric phase of mixed states for three-level open systems

    NASA Astrophysics Data System (ADS)

    Jiang, Yanyan; Ji, Y. H.; Xu, Hualan; Hu, Li-Yun; Wang, Z. S.; Chen, Z. Q.; Guo, L. P.

    2010-12-01

    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.

  14. ModelE2-TOMAS development and evaluation using aerosol optical depths, mass and number concentrations

    NASA Astrophysics Data System (ADS)

    Lee, Y. H.; Adams, P. J.; Shindell, D. T.

    2014-09-01

    The TwO-Moment Aerosol Sectional microphysics model (TOMAS) has been integrated into the state-of-the-art general circulation model, GISS ModelE2. TOMAS has the flexibility to select a size resolution as well as the lower size cutoff. A computationally efficient version of TOMAS is used here, which has 15 size bins covering 3 nm to 10 μm aerosol dry diameter. For each bin, it simulates the total aerosol number concentration and mass concentrations of sulphate, pure elementary carbon (hydrophobic), mixed elemental carbon (hydrophilic), hydrophobic organic matter, hydrophilic organic matter, sea salt, mineral dust, ammonium, and aerosol-associated water. This paper provides a detailed description of the ModelE2-TOMAS model and evaluates the model against various observations including aerosol precursor gas concentrations, aerosol mass and number concentrations, and aerosol optical depths. Additionally, global budgets in ModelE2-TOMAS are compared with those of other global aerosol models, and the TOMAS model is compared to the default aerosol model in ModelE2, which is a bulk aerosol model. Overall, the ModelE2-TOMAS predictions are within the range of other global aerosol model predictions, and the model has a reasonable agreement with observations of sulphur species and other aerosol components as well as aerosol optical depth. However, ModelE2-TOMAS (as well as the bulk aerosol model) cannot capture the observed vertical distribution of sulphur dioxide over the Pacific Ocean possibly due to overly strong convective transport. The TOMAS model successfully captures observed aerosol number concentrations and cloud condensation nuclei concentrations. Anthropogenic aerosol burdens in the bulk aerosol model running in the same host model as TOMAS (ModelE2) differ by a few percent to a factor of 2 regionally, mainly due to differences in aerosol processes including deposition, cloud processing, and emission parameterizations. Larger differences are found for naturally

  15. 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.

  16. 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.

  17. 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

  18. On the implications of aerosol liquid water and phase separation for organic aerosol mass

    NASA Astrophysics Data System (ADS)

    Pye, Havala O. T.; Murphy, Benjamin N.; Xu, Lu; Ng, Nga L.; Carlton, Annmarie G.; Guo, Hongyu; Weber, Rodney; Vasilakos, Petros; Wyat Appel, K.; Hapsari Budisulistiorini, Sri; Surratt, Jason D.; Nenes, Athanasios; Hu, Weiwei; Jimenez, Jose L.; Isaacman-VanWertz, Gabriel; Misztal, Pawel K.; Goldstein, Allen H.

    2017-01-01

    Organic compounds and liquid water are major aerosol constituents in the southeast United States (SE US). Water associated with inorganic constituents (inorganic water) can contribute to the partitioning medium for organic aerosol when relative humidities or organic matter to organic carbon (OM / OC) ratios are high such that separation relative humidities (SRH) are below the ambient relative humidity (RH). As OM / OC ratios in the SE US are often between 1.8 and 2.2, organic aerosol experiences both mixing with inorganic water and separation from it. Regional chemical transport model simulations including inorganic water (but excluding water uptake by organic compounds) in the partitioning medium for secondary organic aerosol (SOA) when RH > SRH led to increased SOA concentrations, particularly at night. Water uptake to the organic phase resulted in even greater SOA concentrations as a result of a positive feedback in which water uptake increased SOA, which further increased aerosol water and organic aerosol. Aerosol properties, such as the OM / OC and hygroscopicity parameter (κorg), were captured well by the model compared with measurements during the Southern Oxidant and Aerosol Study (SOAS) 2013. Organic nitrates from monoterpene oxidation were predicted to be the least water-soluble semivolatile species in the model, but most biogenically derived semivolatile species in the Community Multiscale Air Quality (CMAQ) model were highly water soluble and expected to contribute to water-soluble organic carbon (WSOC). Organic aerosol and SOA precursors were abundant at night, but additional improvements in daytime organic aerosol are needed to close the model-measurement gap. When taking into account deviations from ideality, including both inorganic (when RH > SRH) and organic water in the organic partitioning medium reduced the mean bias in SOA for routine monitoring networks and improved model performance compared to observations from SOAS. Property updates from

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

    NASA Astrophysics Data System (ADS)

    Curci, G.; Hogrefe, C.; Bianconi, R.; Im, U.; Balzarini, A.; Baró, R.; Brunner, D.; Forkel, R.; Giordano, L.; Hirtl, M.; Honzak, L.; Jiménez-Guerrero, P.; Knote, C.; Langer, M.; Makar, P. A.; Pirovano, G.; Pérez, J. L.; San José, R.; Syrakov, D.; Tuccella, P.; Werhahn, J.; Wolke, R.; Žabkar, R.; Zhang, J.; Galmarini, S.

    2015-08-01

    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 intercomparison, we used the bulk mass profiles of aerosol chemical species sampled over the locations of AERONET stations across Europe and North America to calculate the aerosol optical properties under a range of common assumptions for all models. Several simulations with parameters perturbed within a range of observed values are carried out for July 2010 and compared in order to infer the assumptions that have the largest impact on the calculated aerosol optical properties. We calculate that the most important factor of uncertainty is the assumption about the mixing state, for which we estimate an uncertainty of 30-35% on the simulated aerosol optical depth (AOD) and single scattering albedo (SSA). The choice of the core composition in the core-shell representation is of minor importance for calculation of AOD, while it is critical for the SSA. The uncertainty introduced by the choice of mixing state choice on the calculation of the asymmetry parameter is the order of 10%. Other factors of uncertainty tested here have a maximum average impact of 10% each on calculated AOD, and an impact of a few percent on SSA and g. It is thus recommended to focus further research on a more accurate representation of the aerosol mixing state in models, in order to have a less uncertain simulation of the related optical properties.

  20. Exact spin-cluster ground states in a mixed diamond chain

    NASA Astrophysics Data System (ADS)

    Takano, Ken'Ichi; Suzuki, Hidenori; Hida, Kazuo

    2009-09-01

    The mixed diamond chain is a frustrated Heisenberg chain composed of successive diamond-shaped units with two kinds of spins of magnitudes S and S/2 ( S : integer). Ratio λ of two exchange parameters controls the strength of frustration. With varying λ , the Haldane state and several spin-cluster states appear as the ground state. A spin-cluster state is a tensor product of exact local eigenstates of cluster spins. We prove that a spin-cluster state is the ground state in a finite interval of λ . For S=1 , we numerically determine the total phase diagram consisting of five phases.

  1. Economic and Deterministic Quantum Teleportation of Arbitrary Bipartite Pure and Mixed State with Shared Cluster Entanglement

    NASA Astrophysics Data System (ADS)

    Zhang, Binbin; Liu, Yu

    2009-09-01

    We present a novel protocol for teleportation of arbitrary bipartite pure and mixed state with shared cluster entanglement in this paper. By employing Bell-state measurement on the teleported state and the shared cluster state twice, a sender could transmit the arbitrary bipartite state to a distant receiver. We show the good feature of the cluster state channel, with which it can realize the deterministic teleportation rather than probabilistic one. Moreover, since we require less particles to be shared and need no auxiliary qubit in our protocol, it is more efficient and applicable than the previous schemes.

  2. 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.

  3. 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...

  4. Reactive bromine chemistry in Mount Etna's volcanic plume: the influence of total Br, high-temperature processing, aerosol loading and plume-air mixing

    NASA Astrophysics Data System (ADS)

    Roberts, T. J.; Martin, R. S.; Jourdain, L.

    2014-10-01

    Volcanic emissions present a source of reactive halogens to the troposphere, through rapid plume chemistry that converts the emitted HBr to more reactive forms such as BrO. The nature of this process is poorly quantified, yet is of interest in order to understand volcanic impacts on the troposphere, and infer volcanic activity from volcanic gas measurements (i.e. BrO / SO2 ratios). Recent observations from Etna report an initial increase and subsequent plateau or decline in BrO / SO2 ratios with distance downwind. We present daytime PlumeChem model simulations that reproduce and explain the reported trend in BrO / SO2 at Etna including the initial rise and subsequent plateau. Suites of model simulations also investigate the influences of volcanic aerosol loading, bromine emission, and plume-air mixing rate on the downwind plume chemistry. Emitted volcanic HBr is converted into reactive bromine by autocatalytic bromine chemistry cycles whose onset is accelerated by the model high-temperature initialisation. These rapid chemistry cycles also impact the reactive bromine speciation through inter-conversion of Br, Br2, BrO, BrONO2, BrCl, HOBr. We predict a new evolution of Br speciation in the plume. BrO, Br2, Br and HBr are the main plume species near downwind whilst BrO and HOBr are present further downwind (where BrONO2 and BrCl also make up a minor fraction). BrNO2 is predicted to be only a relatively minor plume component. The initial rise in BrO / SO2 occurs as ozone is entrained into the plume whose reaction with Br promotes net formation of BrO. Aerosol has a modest impact on BrO / SO2 near-downwind (< ~6 km, ~10 min) at the relatively high loadings considered. The subsequent decline in BrO / SO2 occurs as entrainment of oxidants HO2 and NO2 promotes net formation of HOBr and BrONO2, whilst the plume dispersion dilutes volcanic aerosol so slows the heterogeneous loss rates of these species. A higher volcanic aerosol loading enhances BrO / SO2 in the (> 6 km

  5. 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.

  6. Interpretation of unusual absorption bandwidths and resonance Raman intensities in excited state mixed valence.

    PubMed

    Lockard, Jenny V; Valverde, Guadalupe; Neuhauser, Daniel; Zink, Jeffrey I; Luo, Yun; Weaver, Michael N; Nelsen, Stephen F

    2006-01-12

    Excited state mixed valence (ESMV) occurs in molecules in which the ground state has a symmetrical charge distribution but the excited state possesses two or more interchangeably equivalent sites that have different formal oxidation states. Although mixed valence excited states are relatively common in both organic and inorganic molecules, their properties have only recently been explored, primarily because their spectroscopic features are usually overlapped or obscured by other transitions in the molecule. The mixed valence excited state absorption bands of 2,3-di-p-anisyl-2,3-diazabicyclo[2.2.2]octane radical cation are well-separated from others in the absorption spectrum and are particularly well-suited for detailed analysis using the ESMV model. Excited state coupling splits the absorption band into two components. The lower energy component is broader and more intense than the higher energy component. The absorption bandwidths are caused by progressions in totally symmetric modes, and the difference in bandwidths is caused by the coordinate dependence of the excited state coupling. The Raman intensities obtained in resonance with the high and low energy components differ significantly from those expected based on the oscillator strengths of the bands. This unexpected observation is a result of the excited state coupling and is explained by both the averaging of the transition dipole moment orientation over all angles for the two types of spectroscopies and the coordinate-dependent coupling. The absorption spectrum is fit using a coupled two-state model in which both symmetric and asymmetric coordinates are included. The physical meaning of the observed resonance Raman intensity trends is discussed along with the origin of the coordinate-dependent coupling. The well-separated mixed valence excited state spectroscopic components enable detailed electronic and resonance Raman data to be obtained from which the model can be more fully developed and tested.

  7. 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

  8. 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.

  9. Mixed-symmetry 2 sup + state of sup 56 Fe in realistic shell model

    SciTech Connect

    Nakada, H. ); Otsuka, T. ); Sebe, T. )

    1991-08-26

    The mixed-symmetry 2{sup +} state of {sup 56}Fe is investigated by a large-scale shell-model calculation. We can reproduce the experimental energy levels by the Kuo-Brown interaction, as well as the {ital E}2 and {ital M}1 transition probabilities. The ({ital e},{ital e}{prime}) form factors are also reproduced by including the core-polarization effect. By inspecting the shell-model wave functions thus tested, it is found that the 2{sub 2}{sup +} and 2{sub 4}{sup +} states share a large fraction of the mixed-symmetry component.

  10. 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.

  11. Mixing in the spiral roll state in heat convection between concentric double spherical boundaries

    NASA Astrophysics Data System (ADS)

    Itano, Tomoaki; Ninomiya, Takahiro; Iida, Kohei; Sugihara-Seki, Masako

    2015-11-01

    Recent studies have indicated that the spherical Rayleigh Bénard convection provides a variety of non-trivial (convective) flow states bifurcating from the (conductive) static state at the onset of instability. In the present study, focusing on one of them, ''spiral roll state'', which was originally explored by Zhang et al. (2002), we elucidated the following three points of the state; (1) the state exists even in a fairly thicker gap than expected in the previous study, and (2) it is an exact autonomously rotating wave solution, and (3) the state bifurcates directly from the static state at the onset of instability. It is of great interest that this state involves globally mixing through the whole domain beyond a cell which would be formed by the other highly-symmetric nontrivial steady states bifurcating at the onset. ORDIST of Kansai Univ., KAKENHI(23760164).

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

    NASA Technical Reports Server (NTRS)

    Schmid, B.; Ferrare, R.; Flynn, C.; Elleman, R.; Covert, D.; Strawa, A.; Welton, E.; Turner, D.; Jonsson, H.; Redemann, J.; Eilers, J.; Ricci, K.; Hallar, A. G.; Clayton, M.; Michalsky, J.; Smirnov, A.; Holben, B.; Barnard, J.

    2006-01-01

    with measuring the tropospheric vertical profile of the ambient aerosol extinction with current state-of-the-art instrumentation is 15-20% at visible wavelengths and potentially larger in the UV and near-infrared.

  13. 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

  14. Role of clouds, aerosols, and aerosol-cloud interaction in 20th century simulations with GISS ModelE2

    NASA Astrophysics Data System (ADS)

    Nazarenko, L.; Rind, D. H.; Bauer, S.; Del Genio, A. D.

    2015-12-01

    Simulations of aerosols, clouds and their interaction contribute to the major source of uncertainty in predicting the changing Earth's energy and in estimating future climate. Anthropogenic contribution of aerosols affects the properties of clouds through aerosol indirect effects. Three different versions of NASA GISS global climate model are presented for simulation of the twentieth century climate change. All versions have fully interactive tracers of aerosols and chemistry in both the troposphere and stratosphere. All chemical species are simulated prognostically consistent with atmospheric physics in the model and the emissions of short-lived precursors [Shindell et al., 2006]. One version does not include the aerosol indirect effect on clouds. The other two versions include a parameterization of the interactive first indirect aerosol effect on clouds following Menon et al. [2010]. One of these two models has the Multiconfiguration Aerosol Tracker of Mixing state (MATRIX) that permits detailed treatment of aerosol mixing state, size, and aerosol-cloud activation. The main purpose of this study is evaluation of aerosol-clouds interactions and feedbacks, as well as cloud and aerosol radiative forcings, for the twentieth century climate under different assumptions and parameterizations for aerosol, clouds and their interactions in the climate models. The change of global surface air temperature based on linear trend ranges from +0.8°C to +1.2°C between 1850 and 2012. Water cloud optical thickness increases with increasing temperature in all versions with the largest increase in models with interactive indirect effect of aerosols on clouds, which leads to the total (shortwave and longwave) cloud radiative cooling trend at the top of the atmosphere. Menon, S., D. Koch, G. Beig, S. Sahu, J. Fasullo, and D. Orlikowski (2010), Black carbon aerosols and the third polar ice cap, Atmos. Chem. Phys., 10,4559-4571, doi:10.5194/acp-10-4559-2010. Shindell, D., G. Faluvegi

  15. On the implications of aerosol liquid water and phase ...

    EPA Pesticide Factsheets

    Organic compounds and liquid water are major aerosol constituents in the southeast United States (SE US). Water associated with inorganic constituents (inorganic water) can contribute to the partitioning medium for organic aerosol when relative humidities or organic matter to organic carbon (OM ∕ OC) ratios are high such that separation relative humidities (SRH) are below the ambient relative humidity (RH). As OM ∕ OC ratios in the SE US are often between 1.8 and 2.2, organic aerosol experiences both mixing with inorganic water and separation from it. Regional chemical transport model simulations including inorganic water (but excluding water uptake by organic compounds) in the partitioning medium for secondary organic aerosol (SOA) when RH  >  SRH led to increased SOA concentrations, particularly at night. Water uptake to the organic phase resulted in even greater SOA concentrations as a result of a positive feedback in which water uptake increased SOA, which further increased aerosol water and organic aerosol. Aerosol properties, such as the OM ∕ OC and hygroscopicity parameter (κorg), were captured well by the model compared with measurements during the Southern Oxidant and Aerosol Study (SOAS) 2013. Organic nitrates from monoterpene oxidation were predicted to be the least water-soluble semivolatile species in the model, but most biogenically derived semivolatile species in the Community Multiscale Air Quality (CMAQ) model were hig

  16. The Two-Column Aerosol Project: Phase I—Overview and impact of elevated aerosol layers on aerosol optical depth

    NASA Astrophysics Data System (ADS)

    Berg, Larry K.; Fast, Jerome D.; Barnard, James C.; Burton, Sharon P.; Cairns, Brian; Chand, Duli; Comstock, Jennifer M.; Dunagan, Stephen; Ferrare, Richard A.; Flynn, Connor J.; Hair, Johnathan W.; Hostetler, Chris A.; Hubbe, John; Jefferson, Anne; Johnson, Roy; Kassianov, Evgueni I.; Kluzek, Celine D.; Kollias, Pavlos; Lamer, Katia; Lantz, Kathleen; Mei, Fan; Miller, Mark A.; Michalsky, Joseph; Ortega, Ivan; Pekour, Mikhail; Rogers, Ray R.; Russell, Philip B.; Redemann, Jens; Sedlacek, Arthur J.; Segal-Rosenheimer, Michal; Schmid, Beat; Shilling, John E.; Shinozuka, Yohei; Springston, Stephen R.; Tomlinson, Jason M.; Tyrrell, Megan; Wilson, Jacqueline M.; Volkamer, Rainer; Zelenyuk, Alla; Berkowitz, Carl M.

    2016-01-01

    The Two-Column Aerosol Project (TCAP), conducted from June 2012 through June 2013, was a unique study designed to provide a comprehensive data set that can be used to investigate a number of important climate science questions, including those related to aerosol mixing state and aerosol radiative forcing. The study was designed to sample the atmosphere between and within two atmospheric columns; one fixed near the coast of North America (over Cape Cod, MA) and a second moveable column over the Atlantic Ocean several hundred kilometers from the coast. The U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) was deployed at the base of the Cape Cod column, and the ARM Aerial Facility was utilized for the summer and winter intensive observation periods. One important finding from TCAP is that four of six nearly cloud-free flight days had aerosol layers aloft in both the Cape Cod and maritime columns that were detected using the nadir pointing second-generation NASA high-spectral resolution lidar (HSRL-2). These layers contributed up to 60% of the total observed aerosol optical depth (AOD). Many of these layers were also intercepted by the aircraft configured for in situ sampling, and the aerosol in the layers was found to have increased amounts of biomass burning material and nitrate compared to aerosol found near the surface. In addition, while there was a great deal of spatial and day-to-day variability in the aerosol chemical composition and optical properties, no systematic differences between the two columns were observed.

  17. The Two-Column Aerosol Project: Phase I-Overview and impact of elevated aerosol layers on aerosol optical depth

    DOE PAGES

    Berg, Larry K.; Fast, Jerome D.; Barnard, James C.; ...

    2016-01-08

    The Two-Column Aerosol Project (TCAP), conducted from June 2012 through June 2013, was a unique study designed to provide a comprehensive data set that can be used to investigate a number of important climate science questions, including those related to aerosol mixing state and aerosol radiative forcing. The study was designed to sample the atmosphere between and within two atmospheric columns; one fixed near the coast of North America (over Cape Cod, MA) and a second moveable column over the Atlantic Ocean several hundred kilometers from the coast. The U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) Mobile Facilitymore » (AMF) was deployed at the base of the Cape Cod column, and the ARM Aerial Facility was utilized for the summer and winter intensive observation periods. One important finding from TCAP is that four of six nearly cloud-free flight days had aerosol layers aloft in both the Cape Cod and maritime columns that were detected using the nadir pointing second-generation NASA high-spectral resolution lidar (HSRL-2). In addition, these layers contributed up to 60% of the total observed aerosol optical depth (AOD). Many of these layers were also intercepted by the aircraft configured for in situ sampling, and the aerosol in the layers was found to have increased amounts of biomass burning material and nitrate compared to aerosol found near the surface. Lastly, while there was a great deal of spatial and day-to-day variability in the aerosol chemical composition and optical properties, no systematic differences between the two columns were observed.« less

  18. The Two-Column Aerosol Project: Phase I-Overview and impact of elevated aerosol layers on aerosol optical depth

    SciTech Connect

    Berg, Larry K.; Fast, Jerome D.; Barnard, James C.; Burton, Sharon P.; Cairns, Brian; Chand, Duli; Comstock, Jennifer M.; Dunagan, Stephen; Ferrare, Richard A.; Flynn, Connor J.; Hair, Johnathan W.; Hostetler, Chris A.; Hubbe, John; Jefferson, Anne; Johnson, Roy; Kassianov, Evgueni I.; Kluzek, Celine D.; Kollias, Pavlos; Lamer, Katia; Lantz, Kathleen; Mei, Fan; Miller, Mark A.; Michalsky, Joseph; Ortega, Ivan; Pekour, Mikhail; Rogers, Ray R.; Russell, Philip B.; Redemann, Jens; Sedlacek III, Arthur J.; Segal-Rosenheimer, Michal; Schmid, Beat; Shilling, John E.; Shinozuka, Yohei; Springston, Stephen R.; Tomlinson, Jason M.; Tyrrell, Megan; Wilson, Jacqueline M.; Volkamer, Rainer; Zelenyuk, Alla; Berkowitz, Carl M.

    2016-01-08

    The Two-Column Aerosol Project (TCAP), conducted from June 2012 through June 2013, was a unique study designed to provide a comprehensive data set that can be used to investigate a number of important climate science questions, including those related to aerosol mixing state and aerosol radiative forcing. The study was designed to sample the atmosphere between and within two atmospheric columns; one fixed near the coast of North America (over Cape Cod, MA) and a second moveable column over the Atlantic Ocean several hundred kilometers from the coast. The U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) was deployed at the base of the Cape Cod column, and the ARM Aerial Facility was utilized for the summer and winter intensive observation periods. One important finding from TCAP is that four of six nearly cloud-free flight days had aerosol layers aloft in both the Cape Cod and maritime columns that were detected using the nadir pointing second-generation NASA high-spectral resolution lidar (HSRL-2). In addition, these layers contributed up to 60% of the total observed aerosol optical depth (AOD). Many of these layers were also intercepted by the aircraft configured for in situ sampling, and the aerosol in the layers was found to have increased amounts of biomass burning material and nitrate compared to aerosol found near the surface. Lastly, while there was a great deal of spatial and day-to-day variability in the aerosol chemical composition and optical properties, no systematic differences between the two columns were observed.

  19. The Two-Column Aerosol Project: Phase I - Overview and Impact of Elevated Aerosol Layers on Aerosol Optical Depth

    SciTech Connect

    Berg, Larry K.; Fast, Jerome D.; Barnard, James C.; Burton, Sharon; Cairns, Brian; Chand, Duli; Comstock, Jennifer M.; Dunagan, Stephen; Ferrare, Richard A.; Flynn, Connor J.; Hair, John; Hostetler, Chris A.; Hubbe, John M.; Jefferson, Anne; Johnson, Roy; Kassianov, Evgueni I.; Kluzek, Celine D.; Kollias, Pavlos; Lamer, Katia; Lantz, K.; Mei, Fan; Miller, Mark A.; Michalsky, Joseph; Ortega, Ivan; Pekour, Mikhail S.; Rogers, Ray; Russell, P.; Redemann, Jens; Sedlacek, Art; Segal Rozenhaimer, Michal; Schmid, Beat; Shilling, John E.; Shinozuka, Yohei; Springston, Stephen R.; Tomlinson, Jason M.; Tyrrell, Megan; Wilson, Jacqueline; Volkamer, Rainer M.; Zelenyuk, Alla; Berkowitz, Carl M.

    2016-01-08

    The Two-Column Aerosol Project (TCAP), which was conducted from June 2012 through June 2013, was a unique field study that was designed to provide a comprehensive data set that can be used to investigate a number of important climate science questions, including those related to aerosol mixing state and aerosol radiative forcing. The study was designed to sample the atmosphere at a number of altitudes, from near the surface to as high as 8 km, within two atmospheric columns; one located near the coast of North America (over Cape Cod, MA) and a second over the Atlantic Ocean several hundred kilometers from the coast. TCAP included the yearlong deployment of the U.S. Department of Energy’s (DOE) Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) that was located at the base of the Cape Cod column, as well as summer and winter aircraft intensive observation periods of the ARM Aerial Facility. One important finding from TCAP is the relatively common occurrence (on four of six nearly cloud-free flights) of elevated aerosol layers in both the Cape Cod and maritime columns that were detected using the nadir pointing second-generation NASA high-spectral resolution lidar (HSRL-2). These layers contributed up to 60% of the total aerosol optical depth (AOD) observed in the column. Many of these layers were also intercepted by the aircraft configured for in situ sampling, and the aerosol in the layers was found to have increased amounts of biomass burning aerosol and nitrate compared to the aerosol found near the surface.

  20. Airborne observations of regional variation in fluorescent aerosol across the United States

    NASA Astrophysics Data System (ADS)

    Perring, A. E.; Schwarz, J. P.; Baumgardner, D.; Hernandez, M. T.; Spracklen, D. V.; Heald, C. L.; Gao, R. S.; Kok, G.; McMeeking, G. R.; McQuaid, J. B.; Fahey, D. W.

    2015-02-01

    Airborne observations of fluorescent aerosol were made aboard an airship during CloudLab, a series of flights that took place in September and October of 2013 and covered a wideband of longitude across the continental U.S. between Florida and California and between 28 and 37 N latitudes. Sampling occurred from near the surface to 1000 m above the ground. A Wideband Integrated Bioaerosol Sensor (WIBS-4) measured average concentrations of supermicron fluorescent particles aloft (1 µm to 10 µm), revealing number concentrations ranging from 2.1 ± 0.8 to 8.7 ± 2.2 × 104 particles m-3 and representing up to 24% of total supermicron particle number. We observed distinct variations in size distributions and fluorescent characteristics in different regions, and attribute these to geographically diverse bioaerosol. Fluorescent aerosol detected in the east is largely consistent with mold spores observed in a laboratory setting, while a shift to larger sizes associated with different fluorescent patterns is observed in the west. Fluorescent bioaerosol loadings in the desert west were as high as those near the Gulf of Mexico, suggesting that bioaerosol is a substantial component of supermicron aerosol both in humid and arid environments. The observations are compared to model fungal and bacterial loading predictions, and good agreement in both particle size and concentrations is observed in the east. In the west, the model underestimated observed concentrations by a factor between 2 and 4 and the prescribed particle sizes are smaller than the observed fluorescent aerosol. A classification scheme for use with WIBS data is also presented.

  1. Chemical Characterization of Aerosols on the East Coast of the United States Using Aircraft and Ground-Based Stations during the CLAMS Experiment.

    NASA Astrophysics Data System (ADS)

    de Almeida Castanho, Andréa D.; Vanderlei Martins, J.; Hobbs, Peter V.; Artaxo, Paulo; Remer, Lorraine; Yamasoe, Marcia; Colarco, Peter R.

    2005-04-01

    The Chesapeake Lighthouse and Aircraft Measurements for Satellites (CLAMS) experiment was carried out off the central East Coast of the United States in July 2001. During CLAMS, aerosol particle mass was measured at two ground stations and on the University of Washington's Convair 580 research aircraft. Physical and chemical characteristics of the aerosols were identified and quantified. Three main aerosol regimes were identified in the region and are discussed in this work: local pollution/sea salt background, long-range transported dust, and long-range transported pollution. The major component measured in the fine mode of the aerosol on the ground at Wallops Island, Virginia, was sulfate, estimated as NH4HSO4, which accounted for 55% ± 9% on average of the fine particle mass (FPM) during the experiment period. Black carbon concentrations accounted for 3% ± 1% of FPM; soil dust was also present, representing on average 6% ± 8% of FPM. The difference between the sum of the masses of the measured compounds and the total fine particle mass was 36% ± 10% of FPM, which is attributed primarily to nitrates and organic carbon that were not measured. Aerosol chemical composition in the atmospheric column is also discussed and compared with ground-based measurements. Aerosol dust concentration reached 40% of FPM during an incursion of Saharan dust between 24 and 26 July. Sulfate aerosol reached 70% of FPM during the transport of regional pollution on 17 July. Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol optical thickness, coupled with air parcel back trajectories, supported the conclusion of episodes of long-range transport of dust from the Sahara Desert and pollutants from the continental United States.

  2. Theory of degenerate three-wave mixing using circuit QED in solid-state circuits

    NASA Astrophysics Data System (ADS)

    Cao, Ye; Huo, Wen Yi; Ai, Qing; Long, Gui Lu

    2011-11-01

    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.

  3. Quasi-biennial oscillation of the tropical stratospheric aerosol layer

    NASA Astrophysics Data System (ADS)

    Hommel, R.; Timmreck, C.; Giorgetta, M. A.; Graf, H. F.

    2015-05-01

    This study describes how aerosol in an aerosol-coupled climate model of the middle atmosphere is influenced by the quasi-biennial oscillation (QBO) during times when the stratosphere is largely unperturbed by volcanic material. In accordance with satellite observations, the vertical extent of the stratospheric aerosol layer in the tropics is modulated by the QBO by up to 6 km, or ~ 35% of its mean vertical extent between 100-7 hPa (about 16-33 km). Its largest vertical extent lags behind the occurrence of strongest QBO westerlies. The largest reduction lags behind maximum QBO easterlies. Strongest QBO signals in the aerosol surface area (30 %) and number densities (up to 100% e.g. in the Aitken mode) are found in regions where aerosol evaporates, that is above the 10 hPa pressure level (~ 31 km). Positive modulations are found in the QBO easterly shear, negative modulations in the westerly shear. Below 10 hPa, in regions where the aerosol mixing ratio is largest (50-20 hPa, or ~ 20-26 km), in most of the analysed parameters only moderate statistically significant QBO signatures (< 10%) have been found. QBO signatures in the model prognostic aerosol mixing ratio are significant at the 95% confidence level throughout the tropical stratosphere where modelled mixing ratios exceed 0.1 ppbm. In some regions of the tropical lower stratosphere the QBO signatures in other analysed parameters are partly not statistically significant. Peak-to-peak amplitudes of the QBO signature in the prognostic mixing ratios are up to twice as large as seasonal variations in the region where aerosols evaporate and between 70-30 hPa. Between the tropical tropopause and 70 hPa the QBO signature is relatively weak and seasonal variations dominate the variability of the simulated Junge layer. QBO effects on the upper lid of the tropical aerosol layer turn the quasi-static balance between processes maintaining the layer's vertical extent into a cyclic balance when considering this dominant mode

  4. The optical manipulation and characterisation of aerosol particles

    NASA Astrophysics Data System (ADS)

    Reid, Jonathan P.

    2008-08-01

    Aerosols play a crucial role in many areas of science, ranging from atmospheric chemistry and physics, to pharmaceutical aerosols and drug delivery to the lungs, to combustion science and spray drying. The development of new methods for characterising the properties and dynamics of aerosol particles is of crucial importance if the complex role that particles play is to be more fully understood. Optical tweezers provide a valuable new tool to address fundamental questions in aerosol science. Single or multiple particles 1-15 μm in diameter can be manipulated for indefinite timescales. Linear and non-linear Raman and fluorescence spectroscopies can be used to probe particle composition, phase, component mixing state, and size. In particular, size can be determined with nanometre accuracy, allowing accurate measurements of the thermodynamic properties of aerosols, the kinetics of particle transformation and of light absorption. Further, the simultaneous manipulation of multiple particles in parallel optical traps provides a method for performing comparative measurements on particles of different composition. We will present some latest work in which optical tweezers are used to characterise aerosol dynamics, demonstrating that optical tweezers can find application in studies of hygroscopicity, the mixing state of different chemical components, including the phase separation of immiscible phases, and the kinetics of chemical transformation.

  5. Aerosol effects on the anvil characteristics of mesoscale convective systems

    NASA Astrophysics Data System (ADS)

    Saleeby, S. M.; Heever, S. C.; Marinescu, P. J.; Kreidenweis, S. M.; DeMott, P. J.

    2016-09-01

    Simulations of two mesoscale convective systems (MCSs) that occurred during the Midlatitude Continental Convective Clouds Experiment were performed to examine the impact of aerosol number concentration on the vertical distributions of liquid and ice condensate and the macrophysical, microphysical, and radiative properties of the cirrus-anvil cloud shield. Analyses indicate that for an increase in aerosol concentration from a clean continental to a highly polluted state, there was an increase in the rime collection rate of cloud water, which led to less lofted cloud water. Aerosol-induced trends in the cloud mixing ratio profiles were, however, nonmonotonic in the mixed phase region, such that a moderate increase in aerosol concentration produced the greatest reduction in cloud water. Generally, less lofted cloud water led to less anvil ice mixing ratio but more numerous, small ice crystals within the anvil. In spite of reduced anvil ice mixing ratio, the anvil clouds exhibited greater areal coverage, increased albedo, reduced cloud top cooling, and reduced net radiative flux, which led to an aerosol-induced warming (reduced cooling) effect in these squall lines.

  6. Radiative Impacts of Elevated Aerosol Layers from Different Origins

    NASA Astrophysics Data System (ADS)

    Sauer, D. N.; Weinzierl, B.; Gasteiger, J.; Heimerl, K.

    2014-12-01

    Aerosol particles are omnipresent in the Earth's atmosphere and have important impacts on weather and climate by their effects on the atmospheric radiative balance. With the advent of more and more sophisticated representations of atmospheric processes in earth system models, the lack of reliable input data on aerosols leads to significant uncertainties in the prediction of future climate scenarios. In recent years large discrepancies in radiative forcing estimates from aerosol layers in modeling studies have been revealed emphasizing the need for detailed and systematic observations of aerosols. Airborne in-situ measurements represent an important pillar for validating both model results and retrievals of aerosol distributions and properties from remote sensing methods on global scales. However, detailed observations are challenging and therefore are subject to substantial uncertainties themselves. Here we use data from airborne in-situ measurements of elevated aerosol layers from various field experiments in different regions of the world. The data set includes Saharan mineral dust layers over Africa, the Atlantic Ocean and the Caribbean from the SALTRACE and the SAMUM campaigns as well as long-range transported biomass burning aerosol layers from wild fires in the Sahel region and North America measured over the tropical Atlantic Ocean, Europe and the Arctic detected during SAMUM2, CONCERT2011, DC3 and ACCESS 2012. We aim to characterize the effects of the measured aerosol layers, in particular with respect to ageing, mixing state and vertical structure, on the overall atmospheric radiation budget as well as local heating and cooling rates. We use radiative transfer simulations of short and long-wave radiation and aerosol optical properties derived in a consistent way from the in-situ observations of microphysical properties using T-matrix calculations. The results of this characterization will help to improve the parameterization of the effects of elevated

  7. 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

  8. Mixed-effects state-space models for analysis of longitudinal dynamic systems.

    PubMed

    Liu, Dacheng; Lu, Tao; Niu, Xu-Feng; Wu, Hulin

    2011-06-01

    The rapid development of new biotechnologies allows us to deeply understand biomedical dynamic systems in more detail and at a cellular level. Many of the subject-specific biomedical systems can be described by a set of differential or difference equations that are similar to engineering dynamic systems. In this article, motivated by HIV dynamic studies, we propose a class of mixed-effects state-space models based on the longitudinal feature of dynamic systems. State-space models with mixed-effects components are very flexible in modeling the serial correlation of within-subject observations and between-subject variations. The Bayesian approach and the maximum likelihood method for standard mixed-effects models and state-space models are modified and investigated for estimating unknown parameters in the proposed models. In the Bayesian approach, full conditional distributions are derived and the Gibbs sampler is constructed to explore the posterior distributions. For the maximum likelihood method, we develop a Monte Carlo EM algorithm with a Gibbs sampler step to approximate the conditional expectations in the E-step. Simulation studies are conducted to compare the two proposed methods. We apply the mixed-effects state-space model to a data set from an AIDS clinical trial to illustrate the proposed methodologies. The proposed models and methods may also have potential applications in other biomedical system analyses such as tumor dynamics in cancer research and genetic regulatory network modeling.

  9. Two-photon-state generation via four-wave mixing in optical fibers

    SciTech Connect

    Chen Jun; Li Xiaoying; Kumar, Prem

    2005-09-15

    A quantum theory of two-photon-state generation via four-wave mixing in optical fibers is studied, with emphasis on the case where the pump is a classical, narrow (picosecond-duration) pulse. One of the experiments performed in our lab is discussed and analyzed. Numerical predictions from the theory are shown to be in good agreement with the experimental results.

  10. Characterization of submicron particles influenced by mixed biogenic and anthropogenic emissions using high-resolution aerosol mass spectrometry: results from CARES

    SciTech Connect

    Setyan, Ari; Zhang, Qi; Merkel, M.; Knighton, Walter B.; Sun, Y.; Song, Chen; Shilling, John E.; Onasch, Timothy B.; Herndon, Scott C.; Worsnop, Douglas R.; Fast, Jerome D.; Zaveri, Rahul A.; Berg, Larry K.; Wiedensohler, A.; Flowers, B. A.; Dubey, Manvendra K.; Subramanian, R.

    2012-09-11

    The Carbonaceous Aerosols and Radiative Effects Study (CARES) took place in the Sacramento Valley of California in summer 2010. We present results obtained at Cool, CA, the T1 site of the project ({approx}40 km downwind of urban emissions from Sacramento), where we deployed an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) in parallel with complementary instrumentation to characterize the sources and processes of submicron particles (PM1). Cool is located at the foothill of the Sierra Nevada Mountains, where intense biogenic emissions are periodically mixed with urban outflow transported by daytime southwesterly winds from the Sacramento metropolitan area. The particle mass loading was low (3.0 {micro}gm{sup -3} on average) and dominated by organics (80% of the PM1 mass) followed by sulfate (9.9 %). Organics and sulfate appeared to be externally mixed, as suggested by their different time series (r2 = 0.13) and size distributions. Sulfate showed a bimodal distribution with a droplet mode peaking at {approx}400nm in vacuum aerodynamic diameter (Dva), and a condensation mode at {approx}150 nm, while organics generally displayed a broad distribution in 60-600nm (Dva). New particle formation and growth events were observed almost every day, emphasizing the roles of organics and sulfate in new particle growth, especially that of organics. The organic aerosol (OA) had a nominal formula of C{sub 1}H{sub 1.38}N{sub 0.004}O{sub 0.44}, thus an average organic mass-to-carbon (OM/OC) ratio of 1.70. Two different oxygenated OA (OOA, 90% of total OA mass) and a hydrocarbon-like OA (HOA, 10 %) were identified by Positive matrix factorization (PMF) of the high resolution mass spectra. The more oxidized MO-OOA (O/C = 0.54) corresponded to secondary OA (SOA) primarily influenced by biogenic emissions, while the less oxidized LO-OOA (O/C = 0.42) corresponded to SOA associated with urban transport. The HOA factor corresponded to primary emissions mainly

  11. Excited electronic state mixing in 7-azaindole. Quantitative measurements using the Stark effect.

    PubMed

    Young, Justin W; Pozun, Zachary D; Jordan, Kenneth D; Pratt, David W

    2013-12-12

    Stark effect measurements of the +280 cm(-1) vibronic band at ∼286 nm in the high resolution S1-S0 fluorescence excitation spectrum of 7-azaindole (7AI) in a molecular beam show that the permanent (electric) dipole moment (PDM) of the upper state vibrational level reached in this transition is 4.6 D, twice as large as the PDM of the zero-point level of the S1 state. This large difference is attributed to state mixing with a more polar state. EOM-CSSD calculations suggest that this more polar state is σπ* in nature and that it crosses the ππ* state in energy along the coordinate connecting the two potential energy minima. Such state mixing apparently provides more facile access to conical intersections with the ground state, and subsequent hydrogen atom detachment reactions, since independent studies by Sakota and Sekiya have shown that the N-H stretching frequency of 7AI is significantly reduced when it is excited to the +280 cm(-1) vibrational level of the S1 state.

  12. Unspeciated organic emissions from combustion sources and their influence on the secondary organic aerosol budget in the United States

    EPA Science Inventory

    Secondary organic aerosol (SOA) formed from the atmospheric oxidation of nonmethane organic gases (NMOG) is a major contributor to atmospheric aerosol mass. Emissions and smog chamber experiments were performed to investigate SOA formation from gasoline vehicles, diesel vehicles,...

  13. Aerosol processing in stratiform clouds in ECHAM6-HAM

    NASA Astrophysics Data System (ADS)

    Neubauer, David; Lohmann, Ulrike; Hoose, Corinna

    2013-04-01

    Aerosol processing in stratiform clouds by uptake into cloud particles, collision-coalescence, chemical processing inside the cloud particles and release back into the atmosphere has important effects on aerosol concentration, size distribution, chemical composition and mixing state. Aerosol particles can act as cloud condensation nuclei. Cloud droplets can take up further aerosol particles by collisions. Atmospheric gases may also be transferred into the cloud droplets and undergo chemical reactions, e.g. the production of atmospheric sulphate. Aerosol particles are also processed in ice crystals. They may be taken up by homogeneous freezing of cloud droplets below -38° C or by heterogeneous freezing above -38° C. This includes immersion freezing of already immersed aerosol particles in the droplets and contact freezing of particles colliding with a droplet. Many clouds do not form precipitation and also much of the precipitation evaporates before it reaches the ground. The water soluble part of the aerosol particles concentrates in the hydrometeors and together with the insoluble part forms a single, mixed, larger particle, which is released. We have implemented aerosol processing into the current version of the general circulation model ECHAM6 (Stevens et al., 2013) coupled to the aerosol module HAM (Stier et al., 2005). ECHAM6-HAM solves prognostic equations for the cloud droplet number and ice crystal number concentrations. In the standard version of HAM, seven modes are used to describe the total aerosol. The modes are divided into soluble/mixed and insoluble modes and the number concentrations and masses of different chemical components (sulphate, black carbon, organic carbon, sea salt and mineral dust) are prognostic variables. We extended this by an explicit representation of aerosol particles in cloud droplets and ice crystals in stratiform clouds similar to Hoose et al. (2008a,b). Aerosol particles in cloud droplets are represented by 5 tracers for the

  14. A note on the effects of inorganic seed aerosol on the oxidation state of secondary organic aerosol—α-Pinene ozonolysis

    NASA Astrophysics Data System (ADS)

    Huang, Dan Dan; Zhang, Xuan; Dalleska, Nathan F.; Lignell, Hanna; Coggon, Matthew M.; Chan, Chi-Ming; Flagan, Richard C.; Seinfeld, John H.; Chan, Chak K.

    2016-10-01

    We compare the oxidation state and molecular composition of α-pinene-derived secondary organic aerosol (SOA) by varying the types and surface areas of inorganic seed aerosol that are used to promote the condensation of SOA-forming vapors. The oxidation state of α-pinene SOA is found to increase with inorganic seed surface area, likely a result of enhanced condensation of low-volatility organic compounds on particles versus deposition on the chamber wall. α-Pinene SOA is more highly oxygenated in the presence of sodium nitrate (SN) seed than ammonium sulfate seed. The relative abundance of semivolatile monomers and low-volatility dimer components that account for more than half of α-pinene SOA mass is not significantly affected by the composition of seed aerosol. Enhanced uptake of highly oxidized small carboxylic acids onto SN seed particles is observed, which could potentially explain the observed higher SOA oxidation state in the presence of SN seed aerosol. Overall, our results demonstrate that a combined effect of seed aerosol composition and surface area leads to an increase in the O:C atomic ratio of α-pinene SOA by as much as a factor of 2.

  15. Monodisperse aerosol generator

    DOEpatents

    Ortiz, Lawrence W.; Soderholm, Sidney C.

    1990-01-01

    An aerosol generator is described which is capable of producing a monodisperse aerosol within narrow limits utilizing an aqueous solution capable of providing a high population of seed nuclei and an organic solution having a low vapor pressure. The two solutions are cold nebulized, mixed, vaporized, and cooled. During cooling, particles of the organic vapor condense onto the excess seed nuclei, and grow to a uniform particle size.

  16. Fine Aerosol Bulk Composition Measured on WP-3D Research Aircraft in Vicinity of the Northeastern United States - Results from NEAQS

    NASA Technical Reports Server (NTRS)

    Peltier, R. E.; Sullivan, A. P.; Weber, R. J.; Brock, C. A.; Wollny, A. G.; Holloway, J. S.; deGouw, J. A.; Warneke, C.

    2007-01-01

    During the New England Air Quality Study (NEAQS) in the summer of 2004, airborne measurements were made of the major inorganic ions and the water-soluble organic carbon (WSOC) of the submicron (PM(sub 1.0)) aerosol. These and ancillary data are used to describe the overall aerosol chemical characteristics encountered during the study. Fine particle mass was estimated from particle volume and a calculated density based on measured particle composition. Fine particle organic matter (OM) was estimated from WSOC and a mass balance analysis. The aerosol over the northeastern United States (U.S.) and Canada was predominantly sulfate and associated ammonium, and organic components, although in unique plumes additional ionic components were also periodically above detection limits. In power generation regions, and especially in the Ohio River Valley region, the aerosol tended to be predominantly sulfate (approximately 60% micro gram /micro gram) and apparently acidic, based on an excess of measured anions compared to cations. In all other regions where sulfate concentrations were lower and a smaller fraction of overall mass, the cations and anions were balanced suggesting a more neutral aerosol. In contrast, the WSOC and estimated OM were more spatially uniform and the fraction of OM relative to PM mass was largely influenced by sources of sulfate. The study median OM mass fraction was 40%. Throughout the study region, sulfate and organic aerosol mass were highest near the surface and decreased rapidly with increasing altitude. The relative fraction of organic mass to sulfate was similar throughout all altitudes within the boundary layer (altitude less than 2.5 km), but was significantly higher at altitude layers in the free troposphere (above 2.5 km). A number of distinct biomass burning plumes from fires in Alaska and the Yukon were periodically intercepted, mostly at altitudes between 3 and 4 km. These plumes were associated with highest aerosol concentrations of the

  17. Fine aerosol bulk composition measured on WP-3D research aircraft in vicinity of the Northeastern United States - results from NEAQS

    NASA Astrophysics Data System (ADS)

    Peltier, R. E.; Sullivan, A. P.; Weber, R. J.; Brock, C. A.; Wollny, A. G.; Holloway, J. S.; de Gouw, J. A.; Warneke, C.

    2007-06-01

    During the New England Air Quality Study (NEAQS) in the summer of 2004, airborne measurements were made of the major inorganic ions and the water-soluble organic carbon (WSOC) of the submicron (PM1.0) aerosol. These and ancillary data are used to describe the overall aerosol chemical characteristics encountered during the study. Fine particle mass was estimated from particle volume and a calculated density based on measured particle composition. Fine particle organic matter (OM) was estimated from WSOC and a mass balance analysis. The aerosol over the northeastern United States (U.S.) and Canada was predominantly sulfate and associated ammonium, and organic components, although in unique plumes additional ionic components were also periodically above detection limits. In power generation regions, and especially in the Ohio River Valley region, the aerosol tended to be predominantly sulfate (~60% μg μg-1) and apparently acidic, based on an excess of measured anions compared to cations. In all other regions where sulfate concentrations were lower and a smaller fraction of overall mass, the cations and anions were balanced suggesting a more neutral aerosol. In contrast, the WSOC and estimated OM were more spatially uniform and the fraction of OM relative to PM mass was largely influenced by sources of sulfate. The study median OM mass fraction was 40%. Throughout the study region, sulfate and organic aerosol mass were highest near the surface and decreased rapidly with increasing altitude. The relative fraction of organic mass to sulfate was similar throughout all altitudes within the boundary layer (altitude less than 2.5 km), but was significantly higher at altitude layers in the free troposphere (above 2.5 km). A number of distinct biomass burning plumes from fires in Alaska and the Yukon were periodically intercepted, mostly at altitudes between 3 and 4 km. These plumes were associated with highest aerosol concentrations of the study and were largely comprised

  18. Fine aerosol bulk composition measured on WP-3D research aircraft in vicinity of the Northeastern United States - results from NEAQS

    NASA Astrophysics Data System (ADS)

    Peltier, R. E.; Sullivan, A. P.; Weber, R. J.; Brock, C. A.; Wollny, A. G.; Holloway, J. S.; de Gouw, J. A.; Warneke, C.

    2007-02-01

    During the New England Air Quality Study (NEAQS) in the summer of 2004, airborne measurements were made of the major inorganic ions and the water-soluble organic carbon (WSOC) of the submicron (PM1.0) aerosol. These and ancillary data are used to describe the overall aerosol chemical characteristics encountered during the study. Fine particle mass was estimated from particle volume and a calculated density based on measured particle composition. Fine particle organic matter (OM) was estimated from WSOC and a mass balance analysis. The aerosol over the northeastern United States (U.S.) and Canada was predominately sulfate and associated ammonium, and organic components, although in unique plumes additional ionic components were also periodically above detection limits. In power generation regions, and especially in the Ohio River Valley region, the aerosol tended to be predominantly sulfate (~60% μg μg-1) and apparently acidic, based on an excess of measured anions compared to cations. In all other regions where sulfate concentrations were lower and a smaller fraction of overall mass, the cations and anions were balanced suggesting a more neutral aerosol. In contrast, the WSOC and estimated OM were more spatially uniform and the fraction of OM relative to PM mass largely influenced by sources of sulfate. The study median OM mass fraction was 40%. Throughout the study region, sulfate and organic aerosol mass were highest near the surface and decreased rapidly with increasing altitude. The relative fraction of organic mass to sulfate was similar within the boundary layer (altitude less than ~2.5 km), but was significantly higher in the free troposphere (above ~2.5 km). A number of distinct biomass burning plumes from fires in Alaska and the Yukon were periodically intercepted, mostly at altitudes between 3 and 4 km. These plumes were associated with highest aerosol concentrations of the study and were largely comprised of organic aerosol components (~60%).

  19. Mixing of quantum states: A new route to creating optical activity.

    PubMed

    Baimuratov, Anvar S; Tepliakov, Nikita V; Gun'ko, Yurii K; Baranov, Alexander V; Fedorov, Anatoly V; Rukhlenko, Ivan D

    2016-12-01

    The ability to induce optical activity in nanoparticles and dynamically control its strength is of great practical importance due to potential applications in various areas, including biochemistry, toxicology, and pharmaceutical science. Here we propose a new method of creating optical activity in originally achiral quantum nanostructures based on the mixing of their energy states of different parities. The mixing can be achieved by selective excitation of specific states or via perturbing all the states in a controllable fashion. We analyze the general features of the so produced optical activity and elucidate the conditions required to realize the total dissymmetry of optical response. The proposed approach is applicable to a broad variety of real systems that can be used to advance chiroptical devices and methods.

  20. Distillation of mixed-state continuous-variable entanglement by photon subtraction

    SciTech Connect

    Zhang Shengli; Loock, Peter van

    2010-12-15

    We present a detailed theoretical analysis for the distillation of one copy of a mixed two-mode continuous-variable entangled state using beam splitters and coherent photon-detection techniques, including conventional on-off detectors and photon-number-resolving detectors. The initial Gaussian mixed-entangled states are generated by transmitting a two-mode squeezed state through a lossy bosonic channel, corresponding to the primary source of errors in current approaches to optical quantum communication. We provide explicit formulas to calculate the entanglement in terms of logarithmic negativity before and after distillation, including losses in the channel and the photon detection, and show that one-copy distillation is still possible even for losses near the typical fiber channel attenuation length. A lower bound for the transmission coefficient of the photon-subtraction beam splitter is derived, representing the minimal value that still allows to enhance the entanglement.

  1. Modeling aerosols and their interactions with shallow cumuli during the 2007 CHAPS field study

    SciTech Connect

    Shrivastava, ManishKumar B.; Berg, Larry K.; Fast, Jerome D.; Easter, Richard C.; Laskin, Alexander; Chapman, Elaine G.; Gustafson, William I.; Liu, Ying; Berkowitz, Carl M.

    2013-02-07

    The Weather Research and Forecasting model coupled with chemistry (WRF-Chem) is used to simulate relationships between aerosols and clouds in the vicinity of Oklahoma City during the June 2007 Cumulus Humilis Aerosol Processing Study (CHAPS). The regional scale simulation completed using 2 km horizontal grid spacing evaluates four important relationships between aerosols and shallow cumulus clouds observed during CHAPS. First, the model reproduces the trends of higher nitrate volume fractions in cloud droplet residuals compared to interstitial non-activated aerosols, as measured using the Aerosol Mass Spectrometer. Comparing simulations with cloud chemistry turned on and off, we show that nitric acid vapor uptake by cloud droplets explains the higher nitrate content of cloud droplet residuals. Second, as documented using an offline code, both aerosol water and other inorganics (OIN), which are related to dust and crustal emissions, significantly affect predicted aerosol optical properties. Reducing the OIN content of wet aerosols by 50% significantly improves agreement of model predictions with measurements of aerosol optical properties. Third, the simulated hygroscopicity of aerosols is too high as compared to their hygroscopicity derived from cloud condensation nuclei and particle size distribution measurements, indicating uncertainties associated with simulating size-dependent chemical composition and treatment of aerosol mixing state within the model. Fourth, the model reasonably represents the observations of the first aerosol indirect effect where pollutants in the vicinity of Oklahoma City increase cloud droplet number concentrations and decrease the droplet effective radius. While previous studies have often focused on cloud-aerosol interactions in stratiform and deep convective clouds, this study highlights the ability of regional-scale models to represent some of the important aspects of cloud-aerosol interactions associated with fields of short

  2. Chemical, physical, and optical evolution of biomass burning aerosols: a case study

    NASA Astrophysics Data System (ADS)

    Adler, G.; Flores, J. M.; Abo Riziq, A.; Borrmann, S.; Rudich, Y.

    2011-02-01

    In-situ chemical composition measurements of ambient aerosols have been used for characterizing the evolution of submicron aerosols from a large anthropogenic biomass burning (BB) event in Israel. A high resolution Time of Flight Aerosol Mass Spectrometer (HR-RES-TOF-AMS) was used to follow the chemical evolution of BB aerosols during a night-long, extensive nationwide wood burning event and during the following day. While these types of extensive BB events are not common in this region, burning of agricultural waste is a common practice. The aging process of the BB aerosols was followed through their chemical, physical and optical properties. Mass spectrometric analysis of the aerosol organic component showed that aerosol aging is characterized by shifting from less oxidized fresh BB aerosols to more oxidized aerosols. Evidence for aerosol aging during the day following the BB event was indicated by an increase in the organic mass, its oxidation state, the total aerosol concentration, and a shift in the modal particle diameter. The effective broadband refractive index (EBRI) was derived using a white light optical particle counter (WELAS). The average EBRI for a mixed population of aerosols dominated by open fires was m = 1.53(±0.03) + 0.07i(±0.03), during the smoldering phase of the fires we found the EBRI to be m = 1.54(±0.01) + 0.04i(±0.01) compared to m = 1.49(±0.01) + 0.02i(±0.01) of the aged aerosols during the following day. This change indicates a decrease in the overall aerosol absorption and scattering. Elevated levels of particulate Polycyclic Aromatic Hydrocarbons (PAHs) were detected during the entire event, which suggest possible implications for human health during such extensive event.

  3. GENERAL: Thermal entanglement and teleportation of a thermally mixed entangled state of a Heisenberg chain through a Werner state

    NASA Astrophysics Data System (ADS)

    Huang, Li-Yuan; Fang, Mao-Fa

    2008-07-01

    The thermal entanglement and teleportation of a thermally mixed entangled state of a two-qubit Heisenberg XXX chain under the Dzyaloshinski-Moriya (DM) anisotropic antisymmetric interaction through a noisy quantum channel given by a Werner state is investigated. The dependences of the thermal entanglement of the teleported state on the DM coupling constant, the temperature and the entanglement of the noisy quantum channel are studied in detail for both the ferromagnetic and the antiferromagnetic cases. The result shows that a minimum entanglement of the noisy quantum channel must be provided in order to realize the entanglement teleportation. The values of fidelity of the teleported state are also studied for these two cases. It is found that under certain conditions, we can transfer an initial state with a better fidelity than that for any classical communication protocol.

  4. Long-term impacts of aerosols on vertical development of cloud and precipitation

    SciTech Connect

    Li Z.; Liu Y.; Niu, F.; Fan, J.; Rosenfeld, D.; Ding, Y.

    2011-11-13

    Aerosols alter cloud density and the radiative balance of the atmosphere. This leads to changes in cloud microphysics and atmospheric stability, which can either suppress or foster the development of clouds and precipitation. The net effect is largely unknown, but depends on meteorological conditions and aerosol properties. Here, we examine the long-term impact of aerosols on the vertical development of clouds and rainfall frequencies, using a 10-year dataset of aerosol, cloud and meteorological variables collected in the Southern Great Plains in the United States. We show that cloud-top height and thickness increase with aerosol concentration measured near the ground in mixed-phase clouds-which contain both liquid water and ice-that have a warm, low base. We attribute the effect, which is most significant in summer, to an aerosol-induced invigoration of upward winds. In contrast, we find no change in cloud-top height and precipitation with aerosol concentration in clouds with no ice or cool bases. We further show that precipitation frequency and rain rate are altered by aerosols. Rain increases with aerosol concentration in deep clouds that have a high liquid-water content, but declines in clouds that have a low liquid-water content. Simulations using a cloud-resolving model confirm these observations. Our findings provide unprecedented insights of the long-term net impacts of aerosols on clouds and precipitation.

  5. Reactive bromine chemistry in Mt. Etna's volcanic plume: the influence of total Br, high temperature processing, aerosol loading and plume-air mixing

    NASA Astrophysics Data System (ADS)

    Roberts, T. J.; Martin, R. S.; Jourdain, L.

    2014-03-01

    Volcanic emissions present a source of reactive halogens to the troposphere, through rapid plume chemistry that converts the emitted HBr to more reactive forms such as BrO. The nature of this process is poorly quantified, yet is of interest to understand volcanic impacts on the troposphere, and infer volcanic activity from volcanic gas measurements (i.e. BrO / SO2 ratios). Recent observations from Etna report an initial increase and subsequent plateau or decline in BrO / SO2 ratios with distance downwind. We present daytime PlumeChem model simulations that reproduce and explain the reported trend in BrO / SO2 at Etna including the initial rise and subsequent plateau. Through suites of model simulations we also investigate the influences of volcanic aerosol loading, bromine emission, and plume-air mixing rate on the downwind plume chemistry. Emitted volcanic HBr is converted into reactive bromine by autocatalytic bromine chemistry cycles whose onset is accelerated by the model high-temperature initialisation. These rapid chemistry cycles also impact the reactive bromine speciation through inter-conversion of Br, Br2, BrO, BrONO2, BrCl, HOBr. Formation of BrNO2 is also discussed. We predict a new evolution of Br-speciation in the plume, with BrO, Br2, Br and HBr as the main plume species in the near downwind plume whilst BrO, and HOBr are present in significant quantities further downwind (where BrONO2 and BrCl also make up a minor fraction). The initial rise in BrO / SO2 occurs as ozone is entrained into the plume whose reaction with Br promotes net formation of BrO. Aerosol has a modest impact on BrO / SO2 near-downwind (< 6 km) at the relatively high loadings considered. The subsequent decline in BrO / SO2 occurs as entrainment of oxidants HO2 and NO2 promotes net formation of HOBr and BrONO2, whilst the plume dispersion dilutes volcanic aerosol so slows the heterogeneous loss rates of these species. A higher volcanic aerosol loading enhances BrO / SO2 in the (> 6

  6. Single-cell analysis of mixed-lineage states leading to a binary cell fate choice.

    PubMed

    Olsson, Andre; Venkatasubramanian, Meenakshi; Chaudhri, Viren K; Aronow, Bruce J; Salomonis, Nathan; Singh, Harinder; Grimes, H Leighton

    2016-09-29

    Delineating hierarchical cellular states, including rare intermediates and the networks of regulatory genes that orchestrate cell-type specification, are continuing challenges for developmental biology. Single-cell RNA sequencing is greatly accelerating such research, given its power to provide comprehensive descriptions of genomic states and their presumptive regulators. Haematopoietic multipotential progenitor cells, as well as bipotential intermediates, manifest mixed-lineage patterns of gene expression at a single-cell level. Such mixed-lineage states may reflect the molecular priming of different developmental potentials by co-expressed alternative-lineage determinants, namely transcription factors. Although a bistable gene regulatory network has been proposed to regulate the specification of either neutrophils or macrophages, the nature of the transition states manifested in vivo, and the underlying dynamics of the cell-fate determinants, have remained elusive. Here we use single-cell RNA sequencing coupled with a new analytic tool, iterative clustering and guide-gene selection, and clonogenic assays to delineate hierarchical genomic and regulatory states that culminate in neutrophil or macrophage specification in mice. We show that this analysis captured prevalent mixed-lineage intermediates that manifested concurrent expression of haematopoietic stem cell/progenitor and myeloid progenitor cell genes. It also revealed rare metastable intermediates that had collapsed the haematopoietic stem cell/progenitor gene expression programme, instead expressing low levels of the myeloid determinants, Irf8 and Gfi1 (refs 9, 10, 11, 12, 13). Genetic perturbations and chromatin immunoprecipitation followed by sequencing revealed Irf8 and Gfi1 as key components of counteracting myeloid-gene-regulatory networks. Combined loss of these two determinants 'trapped' the metastable intermediate. We propose that mixed-lineage states are obligatory during cell-fate specification

  7. Unambiguous discrimination of mixed states: A description based on system-ancilla coupling

    SciTech Connect

    Zhou, Xiang-Fa; Zhang, Yong-Sheng; Guo, Guang-Can

    2007-05-15

    We propose a general description for the unambiguous discrimination of mixed states according to the system-environment coupling, and present a procedure to reduce this to a standard semidefinite programming problem. In the two-state case, we introduce the canonical vectors and partly simplify the problem to the case of discrimination between pairs of canonical vectors. By considering the positivity of the 2x2 matrices, we obtain a series of new upper bounds for the total success probability, which depends on both the prior probabilities and specific state structures.

  8. Resonant purification of mixed states for closed and open quantum systems

    SciTech Connect

    Romano, Raffaele

    2007-02-15

    Pure states are fundamental for the implementation of quantum technologies, and several methods for the purification of the state of a quantum system S have been developed in the past years. In this work we describe a mechanism leading to purification of mixed states, based on the interaction of S with an auxiliary system P. Considering two-level systems and assuming a particular interaction between them, we study how the dynamical parameters of the system P affect the purification of S. By using analytical and numerical tools, we show that the purification process exhibits a resonant behavior in both the cases of system isolated from the external environment or not.

  9. Donor/Acceptor Mixed Self-Assembled Monolayers for Realising a Multi-Redox-State Surface.

    PubMed

    Casado-Montenegro, Javier; Marchante, Elena; Crivillers, Núria; Rovira, Concepció; Mas-Torrent, Marta

    2016-06-17

    Mixed molecular self-assembled monolayers (SAMs) on gold, based on two types of electroactive molecules, that is, electron-donor (ferrocene) and electron-acceptor (anthraquinone) molecules, are prepared as an approach to realise surfaces exhibiting multiple accessible redox states. The SAMs are investigated in different electrolyte media. The nature of these media has a strong impact on the types of redox processes that take place and on the redox potentials. Under optimised conditions, surfaces with three redox states are achieved. Such states are accessible in a relatively narrow potential window in which the SAMs on gold are stable. This communication elucidates the key challenges in fabricating bicomponent SAMs as electrochemical switches.

  10. Unspeciated organic emissions from combustion sources and their influence on the secondary organic aerosol budget in the United States.

    PubMed

    Jathar, Shantanu H; Gordon, Timothy D; Hennigan, Christopher J; Pye, Havala O T; Pouliot, George; Adams, Peter J; Donahue, Neil M; Robinson, Allen L

    2014-07-22

    Secondary organic aerosol (SOA) formed from the atmospheric oxidation of nonmethane organic gases (NMOG) is a major contributor to atmospheric aerosol mass. Emissions and smog chamber experiments were performed to investigate SOA formation from gasoline vehicles, diesel vehicles, and biomass burning. About 10-20% of NMOG emissions from these major combustion sources are not routinely speciated and therefore are currently misclassified in emission inventories and chemical transport models. The smog chamber data demonstrate that this misclassification biases model predictions of SOA production low because the unspeciated NMOG produce more SOA per unit mass than the speciated NMOG. We present new source-specific SOA yield parameterizations for these unspeciated emissions. These parameterizations and associated source profiles are designed for implementation in chemical transport models. Box model calculations using these new parameterizations predict that NMOG emissions from the top six combustion sources form 0.7 Tg y(-1) of first-generation SOA in the United States, almost 90% of which is from biomass burning and gasoline vehicles. About 85% of this SOA comes from unspeciated NMOG, demonstrating that chemical transport models need improved treatment of combustion emissions to accurately predict ambient SOA concentrations.

  11. Re-creation of aerosol charge state found near HV power lines using a high voltage corona charger

    NASA Astrophysics Data System (ADS)

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

    2015-10-01

    Corona ionisation from AC HV power lines (HVPL) can release ions into the environment, which have the potential to electrically charge pollutant aerosol in the atmosphere. It has been hypothesised that these charged particles have an enhanced probability of being deposited in human airways upon inhalation due to electrostatic attraction by image charge within the lung, with implications for human health. Carbonaceous aerosol particles from a Technegas generator were artificially charge-enhanced using a corona charger. Once generated, particles were passed through the charger, which was either on or off, and stored in a 15 litre conducting bag for ∼20 minutes to observe size and charge distribution changes over time. Charge states were estimated using two Sequential Mobility Particle Sizers measuring the size and mobility distributions. Charge-neutral particles were measured 7 times and positive particles 9 times, the average charge-neutral value of x was 1.00 (sd = 0.06) while the average positive value was 4.60 (0.72). The system will be used to generate positive or charge neutral particles for delivery to human volunteers in an inhalation study to assess the impact of charge on ultrafine (size < 100 nm) particle deposition.

  12. Optical, size and mass properties of mixed type aerosols in Greece and Romania as observed by synergy of lidar and sunphotometers in combination with model simulations: a case study.

    PubMed

    Papayannis, A; Nicolae, D; Kokkalis, P; Binietoglou, I; Talianu, C; Belegante, L; Tsaknakis, G; Cazacu, M M; Vetres, I; Ilic, L

    2014-12-01

    A coordinated experimental campaign aiming to study the aerosol optical, size and mass properties was organized in September 2012, in selected sites in Greece and Romania. It was based on the synergy of lidar and sunphotometers. In this paper we focus on a specific campaign period (23-24 September), where mixed type aerosols (Saharan dust, biomass burning and continental) were confined from the Planetary Boundary Layer (PBL) up to 4-4.5 km height. Hourly mean linear depolarization and lidar ratio values were measured inside the dust layers, ranging from 13 to 29 and from 44 to 65sr, respectively, depending on their mixing status and the corresponding air mass pathways over Greece and Romania. During this event the columnar Aerosol Optical Depth (AOD) values ranged from 0.13 to 0.26 at 532 nm. The Lidar/Radiometer Inversion Code (LIRIC) and the Polarization Lidar Photometer Networking (POLIPHON) codes were used and inter-compared with regards to the retrieved aerosol (fine and coarse spherical/spheroid) mass concentrations, showing that LIRIC generally overestimates the aerosol mass concentrations, in the case of spherical particles. For non-spherical particles the difference in the retrieved mass concentration profiles from these two codes remained smaller than ±20%. POLIPHON retrievals showed that the non-spherical particles reached concentrations of the order of 100-140 μg/m(3) over Romania compared to 50-75 μg/m(3) over Greece. Finally, the Dust Regional Atmospheric Model (DREAM) model was used to simulate the dust concentrations over the South-Eastern Europe.

  13. Eliciting positive, negative and mixed emotional states: A film library for affective scientists.

    PubMed

    Samson, Andrea C; Kreibig, Sylvia D; Soderstrom, Blake; Wade, A Ayanna; Gross, James J

    2016-08-01

    We describe the creation of a film library designed for researchers interested in positive (amusing), negative (repulsive), mixed (amusing and repulsive) and neutral emotional states. Three hundred 20- to 33-second film clips videotaped by amateurs were selected from video-hosting websites and screened in laboratory studies by 75 female participants on self-reported amusement and repulsion (Experiments 1 and 2). On the basis of pre-defined cut-off values, 51 positive, 39 negative, 59 mixed and 50 neutral film clips were selected. These film clips were then presented to 411 male and female participants in a large online study to identify film clips that reliably induced the target emotions (Experiment 3). Depending on the goal of the study, researchers may choose positive, negative, mixed or neutral emotional film clips on the basis of Experiments 1 and 2 or Experiment 3 ratings.

  14. Mixed s -sourcery: Building many-body states using bubbles of nothing

    NASA Astrophysics Data System (ADS)

    Swingle, Brian; McGreevy, John

    2016-10-01

    We recently introduced the idea of s -sourcery [B. Swingle and J. McGreevy, Phys. Rev. B 93, 045127 (2016), 10.1103/PhysRevB.93.045127], a general formalism for building many-body quantum ground states using renormalization-group-inspired quantum circuits. Here we define a generalized notion of s -sourcery that applies to mixed states and study its properties and applicability. For our examples we focus on thermal states of local Hamiltonians. We prove a number of theorems establishing the prevalence of mixed s -source fixed points, giving results for free fermion models, conformal field theories, holographic models, and topological phases. Thermal double states (also called thermofield double states) and the machinery of approximate conditional independence are used heavily in the constructions. For a large class of models we provide an information theoretic argument for the existence of a local Hamiltonian whose ground state is the thermal double state, and in some cases we construct such a Hamiltonian.

  15. Shallow Cumulus Sensitivity to Aerosol within a Fixed Meteorology Framework (Invited)

    NASA Astrophysics Data System (ADS)

    Seigel, R. B.

    2013-12-01

    Shallow cumulus clouds are critically important to the global energy budget and the general circulation of the earth. These clouds occupy up to a quarter of the global cloud fraction and they play a crucial role in mixing boundary layer properties with the free troposphere. As such, shallow cumulus clouds have a large effect on the vertical thermodynamic structure of the lower atmosphere, which then directly impacts larger scale circulations. Therefore, changes to the vertical mixing rates of cumulus clouds by forcing mechanisms such as aerosol loading can result in significant consequences for the general circulation of the Earth. This study aims to isolate changes in cumulus vertical mixing by a single forcing mechanism - aerosol loading. In order to isolate aerosol induced changes in cumulus mixing that are solely due to microphysical-dynamical interactions and not from mean-state thermodynamic instability changes caused by aerosol-cloud-precipitation feedbacks, this study uses a new approach of forcing shallow cumulus clouds in large eddy simulations (LESs). Nine (9) LESs with systematic variations in aerosol concentration and model domain size are initialized with the well-studied trade cumulus regime of the Barbados Oceanographic and Meteorological Experiment (BOMEX). However, rather than using the standard BOMEX forcing functions for each of the nine (9) simulations, which can result in different mean thermodynamic states when variations in aerosol concentration are imposed, the horizontal mean states of the following four (4) model prognosed variables are held fixed: liquid potential temperature (θl), total water (qt), zonal wind (u) and meridional wind (v). This guarantees that all variations of the cloud populations and their role in mixing are strictly the result of local microphysical-dynamical changes that result from changes in aerosol concentrations and not from changes to bulk conditional instability. Results from the nine (9) simulations show

  16. Stratus: An interactive steady state mixed layer model for personal computers

    NASA Technical Reports Server (NTRS)

    Guinn, Thomas A.; Schubert, Wayne H.

    1990-01-01

    A steady-state, horizontally homogeneous, cloud-topped marine boundary layer model based primarily on the work of Lilly (1968) and Schubert et al., (1979) is presented. The conservative thermodynamic variables are equivalent potential temperature, theta(sub e), and total water mixing ratio, q + l. Some of the differences between this and Lilly's (1968) model are: radiation is allowed to penetrate into the boundary layer; cloud top values of longwave radiation, equivalent potential temperature, and water vapor mixing ratio are linear functions of height derived from climatological data at California coastal stations; and the closure assumption assumes a weighted average of Lilly's (1968) maximum and minimum entrainment theories. This model was programmed in FORTRAN and will run interactively on an IBM-compatible personal computer. The program allows the user to specify the geographical location, the wind speed, the sea-surface temperature, the large scale horizontal divergence, and the initial guess for cloud top height. Output includes the steady state values of cloud top and cloud base height, mixed layer equivalent potential temperature and total water mixing ratio, and the associated convective and radiative fluxes.

  17. Local source impacts on primary and secondary aerosols in the Midwestern United States

    NASA Astrophysics Data System (ADS)

    Jayarathne, Thilina; Rathnayake, Chathurika M.; Stone, Elizabeth A.

    2016-04-01

    Atmospheric particulate matter (PM) exhibits heterogeneity in composition across urban areas, leading to poor representation of outdoor air pollutants in human exposure assessments. To examine heterogeneity in PM composition and sources across an urban area, fine particulate matter samples (PM2.5) were chemically profiled in Iowa City, IA from 25 August to 10 November 2011 at two monitoring stations. The urban site is the federal reference monitoring (FRM) station in the city center and the peri-urban site is located 8.0 km to the west on the city edge. Measurements of PM2.5 carbonaceous aerosol, inorganic ions, molecular markers for primary sources, and secondary organic aerosol (SOA) tracers were used to assess statistical differences in composition and sources across the two sites. PM2.5 mass ranged from 3 to 26 μg m-3 during this period, averaging 11.2 ± 4.9 μg m-3 (n = 71). Major components of PM2.5 at the urban site included organic carbon (OC; 22%), ammonium (14%), sulfate (13%), nitrate (7%), calcium (2.9%), and elemental carbon (EC; 2.2%). Periods of elevated PM were driven by increases in ammonium, sulfate, and SOA tracers that coincided with hot and dry conditions and southerly winds. Chemical mass balance (CMB) modeling was used to apportion OC to primary sources; biomass burning, vegetative detritus, diesel engines, and gasoline engines accounted for 28% of OC at the urban site and 24% of OC at the peri-urban site. Secondary organic carbon from isoprene and monoterpene SOA accounted for an additional 13% and 6% of OC at the urban and peri-urban sites, respectively. Differences in biogenic SOA across the two sites were associated with enhanced combustion activities in the urban area and higher aerosol acidity at the urban site. Major PM constituents (e.g., OC, ammonium, sulfate) were generally well-represented by a single monitoring station, indicating a regional source influence. Meanwhile, nitrate, biomass burning, food cooking, suspended dust, and

  18. Characterization of Ambient Black Carbon Aerosols

    NASA Astrophysics Data System (ADS)

    Zhang, R.; Levy, M. E.; Zheng, J.; Molina, L. T.

    2013-12-01

    Because of the strong absorption over a broad range of the electromagnetic spectra, black carbon (BC) is a key short-lived climate forcer, which contributes significantly to climate change by direct radiative forcing and is the second most important component causing global warming after carbon dioxide. The impact of BC on the radiative forcing of the Earth-Atmosphere system is highly dependent of the particle properties. In this presentation, emphasis will be placed on characterizing BC containing aerosols in at the California-Mexico border to obtain a greater understanding of the atmospheric aging and properties of ambient BC aerosols. A comprehensive set of directly measured aerosol properties, including the particle size distribution, effective density, hygroscopicity, volatility, and several optical properties, will be discussed to quantify the mixing state and composition of ambient particles. In Tijuana, Mexico, submicron aerosols are strongly influenced by vehicle emissions; subsequently, the BC concentration in Tijuana is considerably higher than most US cities with an average BC concentration of 2.71 × 2.65 g cm-3. BC accounts for 24.75 % × 9.44 of the total submicron concentration on average, but periodically accounts for over 50%. This high concentration of BC strongly influences many observed aerosol properties such as single scattering albedo, hygroscopicity, effective density, and volatility.

  19. Excited-state mixed-valence distortions in a diisopropyl diphenyl hydrazine cation.

    PubMed

    Lockard, Jenny V; Zink, Jeffrey I; Luo, Yun; Weaver, Michael N; Konradsson, Asgeir E; Fowble, Joseph W; Nelsen, Stephen F

    2006-12-27

    Excited-state mixed valence (ESMV) occurs in the 1,2-diphenyl-1,2-diisopropyl hydrazine radical cation, a molecule in which the ground state has a symmetrical charge distribution localized primarily on the hydrazine, but the phenyl to hydrazine charge-transfer excited state has two interchangeably equivalent phenyl groups that have different formal oxidation states. Electronic absorption and resonance Raman spectra are presented. The neighboring orbital model is employed to interpret the absorption spectrum and coupling. Resonance Raman spectroscopy is used to determine the excited-state distortions. The frequencies of the enhanced modes from the resonance Raman spectra are used together with the time-dependent theory of spectroscopy to fit the two observed absorption bands that have resolved vibronic structure. The origins of the vibronic structure and relationships with the neighboring orbital model are discussed.

  20. Development of an aerosol microphysical module: Aerosol Two-dimensional bin module for foRmation and Aging Simulation (ATRAS)

    SciTech Connect

    Matsui, H.; Koike, Makoto; Kondo, Yutaka; Fast, Jerome D.; Takigawa, M.

    2014-09-30

    Number concentrations, size distributions, and mixing states of aerosols are essential parameters for accurate estimation of aerosol direct and indirect effects. In this study, we developed an aerosol module, designated Aerosol Two-dimensional bin module for foRmation and Aging Simulation (ATRAS), that can represent these parameters explicitly by considering new particle formation (NPF), black carbon (BC) aging, and secondary organic aerosol (SOA) processes. A two-dimensional bin representation is used for particles with dry diameters from 40 nm to 10 µm to resolve both aerosol size (12 bins) and BC mixing state (10 bins) for a total of 120 bins. The particles with diameters from 1 to 40 nm are resolved using an additional 8 size bins to calculate NPF. The ATRAS module was implemented in the WRF-chem model and applied to examine the sensitivity of simulated mass, number, size distributions, and optical and radiative parameters of aerosols to NPF, BC aging and SOA processes over East Asia during the spring of 2009. BC absorption enhancement by coating materials was about 50% over East Asia during the spring, and the contribution of SOA processes to the absorption enhancement was estimated to be 10 – 20% over northern East Asia and 20 – 35% over southern East Asia. A clear north-south contrast was also found between the impacts of NPF and SOA processes on cloud condensation nuclei (CCN) concentrations: NPF increased CCN concentrations at higher supersaturations (smaller particles) over northern East Asia, whereas SOA increased CCN concentrations at lower supersaturations (larger particles) over southern East Asia. Application of ATRAS to East Asia also showed that the impact of each process on each optical and radiative parameter depended strongly on the process and the parameter in question. The module can be used in the future as a benchmark model to evaluate the accuracy of simpler aerosol models and examine interactions between NPF, BC aging, and SOA

  1. Development of an aerosol microphysical module: Aerosol Two-dimensional bin module for foRmation and Aging Simulation (ATRAS)

    NASA Astrophysics Data System (ADS)

    Matsui, H.; Koike, M.; Kondo, Y.; Fast, J. D.; Takigawa, M.

    2014-09-01

    Number concentrations, size distributions, and mixing states of aerosols are essential parameters for accurate estimations of aerosol direct and indirect effects. In this study, we develop an aerosol module, designated the Aerosol Two-dimensional bin module for foRmation and Aging Simulation (ATRAS), that can explicitly represent these parameters by considering new particle formation (NPF), black carbon (BC) aging, and secondary organic aerosol (SOA) processes. A two-dimensional bin representation is used for particles with dry diameters from 40 nm to 10 μm to resolve both aerosol sizes (12 bins) and BC mixing states (10 bins) for a total of 120 bins. The particles with diameters between 1 and 40 nm are resolved using additional eight size bins to calculate NPF. The ATRAS module is implemented in the WRF-Chem model and applied to examine the sensitivity of simulated mass, number, size distributions, and optical and radiative parameters of aerosols to NPF, BC aging, and SOA processes over East Asia during the spring of 2009. The BC absorption enhancement by coating materials is about 50% over East Asia during the spring, and the contribution of SOA processes to the absorption enhancement is estimated to be 10-20% over northern East Asia and 20-35% over southern East Asia. A clear north-south contrast is also found between the impacts of NPF and SOA processes on cloud condensation nuclei (CCN) concentrations: NPF increases CCN concentrations at higher supersaturations (smaller particles) over northern East Asia, whereas SOA increases CCN concentrations at lower supersaturations (larger particles) over southern East Asia. The application of ATRAS in East Asia also shows that the impact of each process on each optical and radiative parameter depends strongly on the process and the parameter in question. The module can be used in the future as a benchmark model to evaluate the accuracy of simpler aerosol models and examine interactions between NPF, BC aging, and SOA

  2. Development of an aerosol microphysical module: Aerosol Two-dimensional bin module for foRmation and Aging Simulation (ATRAS)

    NASA Astrophysics Data System (ADS)

    Matsui, H.; Koike, M.; Kondo, Y.; Fast, J. D.; Takigawa, M.

    2014-04-01

    Number concentrations, size distributions, and mixing states of aerosols are essential parameters for accurate estimation of aerosol direct and indirect effects. In this study, we develop an aerosol module, designated Aerosol Two-dimensional bin module for foRmation and Aging Simulation (ATRAS), that can represent these parameters explicitly by considering new particle formation (NPF), black carbon (BC) aging, and secondary organic aerosol (SOA) processes. A two-dimensional bin representation is used for particles with dry diameters from 40 nm to 10 μm to resolve both aerosol size (12 bins) and BC mixing state (10 bins) for a total of 120 bins. The particles with diameters from 1 to 40 nm are resolved using an additional 8 size bins to calculate NPF. The ATRAS module is implemented in the WRF-chem model and applied to examine the sensitivity of simulated mass, number, size distributions, and optical and radiative parameters of aerosols to NPF, BC aging and SOA processes over East Asia during the spring of 2009. BC absorption enhancement by coating materials is about 50% over East Asia during the spring, and the contribution of SOA processes to the absorption enhancement is estimated to be 10-20% over northern East Asia and 20-35% over southern East Asia. A clear north-south contrast is also found between the impacts of NPF and SOA processes on cloud condensation nuclei (CCN) concentrations: NPF increases CCN concentrations at higher supersaturations (smaller particles) over northern East Asia, whereas SOA increases CCN concentrations at lower supersaturations (larger particles) over southern East Asia. Application of ATRAS to East Asia also shows that the impact of each process on each optical and radiative parameter depends strongly on the process and the parameter in question. The module can be used in the future as a benchmark model to evaluate the accuracy of simpler aerosol models and examine interactions between NPF, BC aging, and SOA processes under

  3. Spectroscopic consequences of a mixed valence excited state: quantitative treatment of a dihydrazine diradical dication.

    PubMed

    Lockard, Jenny V; Zink, Jeffrey I; Konradsson, Asgeir E; Weaver, Michael N; Nelsen, Stephen F

    2003-11-05

    A model for the quantitative treatment of molecular systems possessing mixed valence excited states is introduced and used to explain observed spectroscopic consequences. The specific example studied in this paper is 1,4-bis(2-tert-butyl-2,3-diazabicyclo[2.2.2]oct-3-yl)-2,3,5,6-tetramethylbenzene-1,4-diyl dication. The lowest energy excited state of this molecule arises from a transition from the ground state where one positive charge is associated with each of the hydrazine units, to an excited state where both charges are associated with one of the hydrazine units, that is, a Hy-to-Hy charge transfer. The resulting excited state is a Class II mixed valence molecule. The electronic emission and absorption spectra, and resonance Raman spectra, of this molecule are reported. The lowest energy absorption band is asymmetric with a weak low-energy shoulder and an intense higher energy peak. Emission is observed at low temperature. The details of the absorption and emission spectra are calculated for the coupled surfaces by using the time-dependent theory of spectroscopy. The calculations are carried out in the diabatic basis, but the nuclear kinetic energy is explicitly included and the calculations are exact quantum calculations of the model Hamiltonian. Because the transition involves the transfer of an electron from the hydrazine on one side of the molecule to the hydrazine on the other side and vice versa, the two transitions are antiparallel and the transition dipole moments have opposite signs. Upon transformation to the adiabatic basis, the dipole moment for the transition to the highest energy adiabatic surface is nonzero, but that for the transition to the lowest surface changes sign at the origin. The energy separation between the two components of the absorption spectrum is twice the coupling between the diabatic basis states. The bandwidths of the electronic spectra are caused by progressions in totally symmetric modes as well as progressions in the modes

  4. Unspeciated Organic Emissions From Combustion Sources And Their Influence On The Secondary Organic Aerosol Budget In The United States

    NASA Astrophysics Data System (ADS)

    Jathar, S.; Gordon, T.; Hennigan, C. J.; Pye, H. O.; Donahue, N. M.; Adams, P. J.; Robinson, A. L.

    2012-12-01

    Combustion sources are a major source of organic emissions and therefore a potentially important source for secondary organic aerosol (SOA) formation in the atmosphere. Although speciated organic emissions from combustion sources are considered in models to form SOA, a large fraction of the organics are unspeciated. In this work, we analyze data from numerous smog chamber experiments, which photo-oxidized dilute emissions from different combustion sources (on-road gasoline vehicles, aircraft, on-road diesel vehicles, wood burning and open biomass burning), to determine the contribution that unspeciated emissions make to SOA formation. An SOA model based on speciated organics is able to explain, on average, 8-31% of the SOA measured in the experiments. We hypothesize that the remainder results from the gas-phase oxidation of unspeciated emissions, which account on average for 25-75% of the non-methane organic gas (NMOG) emissions. Using the SOA data, we develop, for the first time, source-specific parameterizations to model SOA from unspeciated emissions; all sources seem to have median SOA yields similar to large n-alkanes (C12+). To assess the influence of unspeciated emissions on SOA formation regionally, we use the parameterization to predict SOA production in the United States. Using emissions data collected during the smog chamber experiments and data available in literature, we build a gross inventory for unspeciated emissions in the United States. We discover that unspeciated organics might be included in the current generation of SOA models but misallocated in terms of its SOA potential. The top six combustion sources (on- and off-road gasoline, on- and off-road diesel, open biomass and wood burning) emit 2.61 Tg yr-1 of unspeciated emissions (20% of US anthropogenic VOC emissions from combustion sources) and are estimated to form a minimum of 0.68 Tg yr-1 of SOA; the estimate is a third of the biogenic SOA produced in the US. We predict that accounting for

  5. Application of muon spin relaxation experiment to the mixed state superconductors

    SciTech Connect

    Inui, M. ); Harshman, D.R. )

    1991-05-09

    We discuss the use of muon spin relaxation ({mu}{sup +}SR) technique to study the mixed state of superconductors. Besides the application for static vortex configurations, we argue that large vortex motion can manifest itself as a narrowed time-averaged field distribution, which in turn results in a smaller relaxation rate. A static but disordered vortex configuration can also reduce the relaxation. We summarize these arguments. 7 refs.

  6. Quantum-enhanced protocols with mixed states using cold atoms in dipole traps

    NASA Astrophysics Data System (ADS)

    Krzyzanowska, K.; Copley-May, M.; Romain, R.; MacCormick, C.; Bergamini, S.

    2017-01-01

    We discuss the use of cold atoms in dipole traps to demonstrate experimentally a particular class of protocols for computation and metrology based on mixed states. Modelling of the system shows that, for a specific class of problems (tracing, phase estimation), a quantum advantage can be achieved over classical algorithms for very realistic conditions and strong decoherence. We discuss the results of the models and the experimental implementation.

  7. Simulation of the Indirect Radiative Forcing of Climate Due to Aerosols by the Two-Way Coupled WRF-CMAQ over the Eastern United States

    EPA Science Inventory

    In this study, the shortwave cloud forcing (SWCF) and longwave cloud forcing (LWCF) are estimated with the newly developed two-way coupled WRF-CMAQ over the eastern United States. Preliminary indirect aerosol forcing has been successfully implemented in WRF-CMAQ. The comparisons...

  8. Characterising the influence of atmospheric mixing state on Urban Heat Island Intensity using Radon-222

    NASA Astrophysics Data System (ADS)

    Chambers, Scott D.; Podstawczyńska, Agnieszka; Williams, Alastair G.; Pawlak, Włodzimierz

    2016-12-01

    Characterisation of the effects of varying atmospheric mixing states (stability) in urban climate studies has historically been hampered by problems associated with the complexity of the urban environment, representativity of measurement techniques, and the logistical and financial burdens of maintaining multiple long-term comprehensive measurement sites. These shortcomings, together with a lack of a consistent measurement approach, have limited our ability to understand the physical processes contributing to the urban heat island effect. In this study, we analyse 4 years of continuous hourly near-surface meteorological and atmospheric radon data from an urban-rural site pair in central Poland. A recently-developed radon-based stability classification technique, previously developed for urban pollution characterisation, is employed to characterise the Urban Heat Island Intensity (UHII) and other climatic factors over the full diurnal cycle by season and atmospheric mixing state. By characterising the UHII over a range of atmospheric mixing states in a statistically robust way, this technique provides an effective tool for assessing the efficacy of mitigation measures for urban climate effects in a consistent way over timescales of years to decades. The consistency of approach, ease of application, and unprecedented clarity of findings, provide a strong argument for atmospheric radon observations to be included as part of the 'standard measurement suite' for urban climate monitoring networks for non-coastal cities.

  9. An evaluation of the impact of aerosol particles on weather forecasts from a biomass burning aerosol event over the Midwestern United States: observational-based analysis of surface temperature

    NASA Astrophysics Data System (ADS)

    Zhang, Jianglong; Reid, Jeffrey S.; Christensen, Matthew; Benedetti, Angela

    2016-05-01

    A major continental-scale biomass burning smoke event from 28-30 June 2015, spanning central Canada through the eastern seaboard of the United States, resulted in unforecasted drops in daytime high surface temperatures on the order of 2-5 °C in the upper Midwest. This event, with strong smoke gradients and largely cloud-free conditions, provides a natural laboratory to study how aerosol radiative effects may influence numerical weather prediction (NWP) forecast outcomes. Here, we describe the nature of this smoke event and evaluate the differences in observed near-surface air temperatures between Bismarck (clear) and Grand Forks (overcast smoke), to evaluate to what degree solar radiation forcing from a smoke plume introduces daytime surface cooling, and how this affects model bias in forecasts and analyses. For this event, mid-visible (550 nm) smoke aerosol optical thickness (AOT, τ) reached values above 5. A direct surface cooling efficiency of -1.5 °C per unit AOT (at 550 nm, τ550) was found. A further analysis of European Centre for Medium-Range Weather Forecasts (ECMWF), National Centers for Environmental Prediction (NCEP), United Kingdom Meteorological Office (UKMO) near-surface air temperature forecasts for up to 54 h as a function of Moderate Resolution Imaging Spectroradiometer (MODIS) Dark Target AOT data across more than 400 surface stations, also indicated the presence of the daytime aerosol direct cooling effect, but suggested a smaller aerosol direct surface cooling efficiency with magnitude on the order of -0.25 to -1.0 °C per unit τ550. In addition, using observations from the surface stations, uncertainties in near-surface air temperatures from ECMWF, NCEP, and UKMO model runs are estimated. This study further suggests that significant daily changes in τ550 above 1, at which the smoke-aerosol-induced direct surface cooling effect could be comparable in magnitude with model uncertainties, are rare events on a global scale. Thus, incorporating

  10. Residential Care Supply, Nursing Home Licensing, and Case Mix in Four States

    PubMed Central

    Swan, James; Newcomer, Robert

    2000-01-01

    Simulation analyses quantify admission and continuing physical and cognitive impairment patient case-mix changes under two scenarios: with increases in residential care supply and with all nursing homes licensed only as skilled care facilities. Findings raise caution about the assumed interplay between residential care supply and nursing home use. The proportion of nursing home patients with only physical and cognitive impairment likely to be affected by current and emerging long-term care (LTC) policy was well under 25 percent of the nursing home population in each of the four study States. States varied in LTC supply and utilization controls. PMID:11481756

  11. Change of surface critical current in the surface superconductivity and mixed states of superconducting niobium

    NASA Astrophysics Data System (ADS)

    Aburas, Muhamad; Pautrat, Alain; Bellido, Natalia

    2017-01-01

    A systematic study of irreversible magnetization was performed in bulk niobium after different surface treatments. Starting with smooth surfaces and abrading them, a strong increase of the critical current is observed up to an apparent limiting value. An impressive change of the critical current is also observed in the surface superconductivity (SSC) state, reaching values of the same order of magnitude as in the mixed state. We explain also the observation of strong SSC for magnetic fields perpendicular to large facets in terms of nucleation of superconductivity along bumps of a corrugated surface.

  12. Measurement-induced qubit state mixing in circuit QED from up-converted dephasing noise.

    PubMed

    Slichter, D H; Vijay, R; Weber, S J; Boutin, S; Boissonneault, M; Gambetta, J M; Blais, A; Siddiqi, I

    2012-10-12

    We observe measurement-induced qubit state mixing in a transmon qubit dispersively coupled to a planar readout cavity. Our results indicate that dephasing noise at the qubit-readout detuning frequency is up-converted by readout photons to cause spurious qubit state transitions, thus limiting the nondemolition character of the readout. Furthermore, we use the qubit transition rate as a tool to extract an equivalent flux noise spectral density at f~1 GHz and find agreement with values extrapolated from a 1/f(α) fit to the measured flux noise spectral density below 1 Hz.

  13. Final Report: Process Models of the Equilibrium Size & State of Organic/Inorganic Aerosols for the Development of Large Scale Atmospheric Models & the Analysis of Field Data

    SciTech Connect

    Wexler, Anthony Stein; Clegg, Simon Leslie

    2013-10-26

    Our work addressed the following elements of the Call for Proposals: (i) “to improve the theoretical representation of aerosol processes studied in ASP laboratory or field studies”, (ii) “to enhance the incorporation of aerosol process information into modules suitable for large-scale or global atmospheric models”, and (iii) “provide systematic experimental validation of process model predictions ... using data from targeted laboratory and field experiments”. Achievements to the end of 2012 are described in four previous reports, and include: new models of densities and surface tensions of pure (single solute) and mixed aqueous solutions of typical aerosol composition under all atmospheric conditions (0 to 100% RH and T > 150 K); inclusion of these models into the widely used Extended Aerosol Inorganics model (E-AIM, http://www.aim.env.uea.ac.uk/aim/aim.php); the addition of vapor pressure calculators for organic compounds to the E-AIM website; the ability of include user-defined organic compounds and/or lumped surrogates in gas/aerosol partitioning calculations; the development of new equations to represent the properties of soluble aerosols over the entire concentration range (using methods based upon adsorption isotherms, and derived using statistical mechanics), including systems at close to zero RH. These results are described in publications 1-6 at the end of this report, and on the “News” page of the E-AIM website (http://www.aim.env.uea.ac.uk/aim/info/news.html). During 2012 and 2013 we have collaborated in a combined observation and lab-based study of the water uptake of the organic component of atmospheric aerosols (PI Gannet Hallar, of the Desert Research Institute). The aerosol samples were analyzed using several complementary techniques (GC/MS, FT-ICR MS, and ion chromatography) to produce a very complete organic “speciation” including both polar and non-polar compounds. Hygroscopic growth factors of the samples were measured, and

  14. A Study of Cloud Processing of Organic Aerosols Using Models and CHAPS Data

    SciTech Connect

    Ervens, Barbara

    2012-01-17

    The main theme of our work has been the identification of parameters that mostly affect the formation and modification of aerosol particles and their interaction with water vapor. Our detailed process model studies led to simplifications/parameterizations of these effects that bridge detailed aerosol information from laboratory and field studies and the need for computationally efficient expressions in complex atmospheric models. One focus of our studies has been organic aerosol mass that is formed in the atmosphere by physical and/or chemical processes (secondary organic aerosol, SOA) and represents a large fraction of atmospheric particulate matter. Most current models only describe SOA formation by condensation of low volatility (or semivolatile) gas phase products and neglect processes in the aqueous phase of particles or cloud droplets that differently affect aerosol size and vertical distribution and chemical composition (hygroscopicity). We developed and applied models of aqueous phase SOA formation in cloud droplets and aerosol particles (aqSOA). Placing our model results into the context of laboratory, model and field studies suggests a potentially significant contribution of aqSOA to the global organic mass loading. The second focus of our work has been the analysis of ambient data of particles that might act as cloud condensation nuclei (CCN) at different locations and emission scenarios. Our model studies showed that the description of particle chemical composition and mixing state can often be greatly simplified, in particular in aged aerosol. While over the past years many CCN studies have been successful performed by using such simplified composition/mixing state assumptions, much more uncertainty exists in aerosol-cloud interactions in cold clouds (ice or mixed-phase). Therefore we extended our parcel model that describes warm cloud formation by ice microphysics and explored microphysical parameters that determine the phase state and lifetime of

  15. Seasonal characterization of submicron aerosol chemical composition and organic aerosol sources in the southeastern United States: Atlanta, Georgia,and Look Rock, Tennessee

    NASA Astrophysics Data System (ADS)

    Hapsari Budisulistiorini, Sri; Baumann, Karsten; Edgerton, Eric S.; Bairai, Solomon T.; Mueller, Stephen; Shaw, Stephanie L.; Knipping, Eladio M.; Gold, Avram; Surratt, Jason D.

    2016-04-01

    A year-long near-real-time characterization of non-refractory submicron aerosol (NR-PM1) was conducted at an urban (Atlanta, Georgia, in 2012) and rural (Look Rock, Tennessee, in 2013) site in the southeastern US using the Aerodyne Aerosol Chemical Speciation Monitor (ACSM) collocated with established air-monitoring network measurements. Seasonal variations in organic aerosol (OA) and inorganic aerosol species are attributed to meteorological conditions as well as anthropogenic and biogenic emissions in this region. The highest concentrations of NR-PM1 were observed during winter and fall seasons at the urban site and during spring and summer at the rural site. Across all seasons and at both sites, NR-PM1 was composed largely of OA (up to 76 %) and sulfate (up to 31 %). Six distinct OA sources were resolved by positive matrix factorization applied to the ACSM organic mass spectral data collected from the two sites over the 1 year of near-continuous measurements at each site: hydrocarbon-like OA (HOA), biomass burning OA (BBOA), semi-volatile oxygenated OA (SV-OOA), low-volatility oxygenated OA (LV-OOA), isoprene-derived epoxydiols (IEPOX) OA (IEPOX-OA) and 91Fac (a factor dominated by a distinct ion at m/z 91 fragment ion previously observed in biogenic influenced areas). LV-OOA was observed throughout the year at both sites and contributed up to 66 % of total OA mass. HOA was observed during the entire year only at the urban site (on average 21 % of OA mass). BBOA (15-33 % of OA mass) was observed during winter and fall, likely dominated by local residential wood burning emission. Although SV-OOA contributes quite significantly ( ˜ 27 %), it was observed only at the urban site during colder seasons. IEPOX-OA was a major component (27-41 %) of OA at both sites, particularly in spring and summer. An ion fragment at m/z 75 is well correlated with the m/z 82 ion associated with the aerosol mass spectrum of IEPOX-derived secondary organic aerosol (SOA). The

  16. An Automated Method of MFRSR Calibration for Aerosol Optical Depth Analysis with Application to an Asian Dust Outbreak over the United States.

    NASA Astrophysics Data System (ADS)

    Augustine, John A.; Cornwall, Christopher R.; Hodges, Gary B.; Long, Charles N.; Medina, Carlos I.; Deluisi, John J.

    2003-02-01

    Over the past decade, networks of Multifilter Rotating Shadowband Radiometers (MFRSR) and automated sun photometers have been established in the United States to monitor aerosol properties. The MFRSR alternately measures diffuse and global irradiance in six narrow spectral bands and a broadband channel of the solar spectrum, from which the direct normal component for each may be inferred. Its 500-nm channel mimics sun photometer measurements and thus is a source of aerosol optical depth information. Automatic data reduction methods are needed because of the high volume of data produced by the MFRSR. In addition, these instruments are often not calibrated for absolute irradiance and must be periodically calibrated for optical depth analysis using the Langley method. This process involves extrapolation to the signal the MFRSR would measure at the top of the atmosphere (I0). Here, an automated clear-sky identification algorithm is used to screen MFRSR 500-nm measurements for suitable calibration data. The clear-sky MFRSR measurements are subsequ