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Sample records for aerosol liquid water

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

    EPA Science Inventory

    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 org...

  2. 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

  3. 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

  4. 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...

  5. Reconciling satellite aerosol optical thickness and surface fine particle mass through aerosol liquid water

    NASA Astrophysics Data System (ADS)

    Nguyen, Thien Khoi V.; Ghate, Virendra P.; Carlton, Annmarie G.

    2016-11-01

    Summertime aerosol optical thickness (AOT) over the southeast U.S. is sharply enhanced over wintertime values. This seasonal pattern is unique and of particular interest because temperatures there have not warmed over the past 100 years. Patterns in surface fine particle mass are inconsistent with satellite reported AOT. In this work, we attempt to reconcile the spatial and temporal distribution of AOT over the U.S. with particle mass measurements at the surface by examining trends in aerosol liquid water (ALW), a particle constituent that scatters radiation and affects satellite AOT but is removed in mass measurements at routine surface monitoring sites. We employ the thermodynamic model ISORROPIAv2.1 to estimate ALW mass concentrations at Interagency Monitoring of PROtected Visual Environments sites using measured ion mass concentrations and North American Regional Reanalysis meteorological data. Excellent agreement between Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations AOT and estimated ALW provides a plausible explanation for the discrepancies in the geographical patterns of AOT and aerosol mass measurements.

  6. Role of Aerosol Liquid Water in Secondary Organic Aerosol Formation from Volatile Organic Compounds.

    PubMed

    Faust, Jennifer A; Wong, Jenny P S; Lee, Alex K Y; Abbatt, Jonathan P D

    2017-02-07

    A key mechanism for atmospheric secondary organic aerosol (SOA) formation occurs when oxidation products of volatile organic compounds condense onto pre-existing particles. Here, we examine effects of aerosol liquid water (ALW) on relative SOA yield and composition from α-pinene ozonolysis and the photooxidation of toluene and acetylene by OH. Reactions were conducted in a room-temperature flow tube under low-NOx conditions in the presence of equivalent loadings of deliquesced (∼20 μg m(-3) ALW) or effloresced (∼0.2 μg m(-3) ALW) ammonium sulfate seeds at exactly the same relative humidity (RH = 70%) and state of wall conditioning. We found 13% and 19% enhancements in relative SOA yield for the α-pinene and toluene systems, respectively, when seeds were deliquesced rather than effloresced. The relative yield doubled in the acetylene system, and this enhancement was partially reversible upon drying the prepared SOA, which reduced the yield by 40% within a time scale of seconds. We attribute the high relative yield of acetylene SOA on deliquesced seeds to aqueous partitioning and particle-phase reactions of the photooxidation product glyoxal. The observed range of relative yields for α-pinene, toluene, and acetylene SOA on deliquesced and effloresced seeds suggests that ALW plays a complicated, system-dependent role in SOA formation.

  7. On the Implications of aerosol liquid water and phase separation for modeled organic aerosol mass

    EPA Science Inventory

    Current chemical transport models assume that organic aerosol (OA)-forming compounds partition mostly to a water-poor, organic-rich phase in accordance with their vapor pressures. However, in the southeast United States, a significant fraction of ambient organic compounds are wat...

  8. Potential of Aerosol Liquid Water to Facilitate Organic Aerosol Formation: Assessing Knowledge Gaps about Precursors and Partitioning.

    PubMed

    Sareen, Neha; Waxman, Eleanor M; Turpin, Barbara J; Volkamer, Rainer; Carlton, Annmarie G

    2017-03-06

    Isoprene epoxydiol (IEPOX), glyoxal, and methylglyoxal are ubiquitous water-soluble organic gases (WSOGs) that partition to aerosol liquid water (ALW) and clouds to form aqueous secondary organic aerosol (aqSOA). Recent laboratory-derived Setschenow (or salting) coefficients suggest glyoxal's potential to form aqSOA is enhanced by high aerosol salt molality, or "salting-in". In the southeastern U.S., aqSOA is responsible for a significant fraction of ambient organic aerosol, and correlates with sulfate mass. However, the mechanistic explanation for this correlation remains elusive, and an assessment of the importance of different WSOGs to aqSOA is currently missing. We employ EPA's CMAQ model to the continental U.S. during the Southern Oxidant and Aerosol Study (SOAS) to compare the potential of glyoxal, methylglyoxal, and IEPOX to partition to ALW, as the initial step toward aqSOA formation. Among these three studied compounds, IEPOX is a dominant contributor, ∼72% on average in the continental U.S., to potential aqSOA mass due to Henry's Law constants and molecular weights. Glyoxal contributes significantly, and application of the Setschenow coefficient leads to a greater than 3-fold model domain average increase in glyoxal's aqSOA mass potential. Methylglyoxal is predicted to be a minor contributor. Acid or ammonium - catalyzed ring-opening IEPOX chemistry as well as sulfate-driven ALW and the associated molality may explain positive correlations between SOA and sulfate during SOAS and illustrate ways in which anthropogenic sulfate could regulate biogenic aqSOA formation, ways not presently included in atmospheric models but relevant to development of effective control strategies.

  9. IMPACT OF AEROSOL LIQUID WATER ON SECONDARY ORGANIC AEROSOL YIELDS OF IRRADIATED TOLUENE/PROPYLENE/NOX/(NH4)2SO4/AIR MIXUTRES

    EPA Science Inventory

    Laboratory experiments were conducted to assess whether the presence of liquid water on pre-existing submicron ammonium sulfate aerosols affects yields of condensible organic compounds. Toluene/propylene/NOX/air mixtures were irradiated in the presence of submicron ammonium su...

  10. High-Resolution Electrospray Ionization Mass Spectrometry Analysis of Water- Soluble Organic Aerosols Collected with a Particle into Liquid Sampler

    SciTech Connect

    Bateman, Adam P.; Nizkorodov, Serguei; Laskin, Julia; Laskin, Alexander

    2010-10-01

    This work demonstrates the utility of a particle-into-liquid sampler (PILS) a technique traditionally used for identification of inorganic ions present in ambient or laboratory aerosols for the analysis of water soluble organic aerosol (OA) using high resolution electrospray ionization mass spectrometry (HR ESI-MS). Secondary organic aerosol (SOA) was produced from 0.5 ppm mixing ratios of limonene and ozone in a 5 m3 Teflon chamber. SOA was collected simultaneously using a traditional filter sampler and a PILS. The filter samples were later extracted with either water or acetonitrile, while the aqueous PILS samples were analyzed directly. In terms of peak intensities, types of detectable compounds, average O:C ratios, and organic mass to organic carbon ratios, the resulting high resolution mass spectra were essentially identical for the PILS and filter based samples. SOA compounds extracted from both filter/acetonitrile extraction and PILS/water extraction accounted for >95% of the total ion current in ESI mass spectra. This similarity was attributed to high solubility of limonene SOA in water. In contrast, significant differences in detected ions and peak abundances were observed for pine needle biomass burning organic aerosol (BBOA) collected with PILS and filter sampling. The water soluble fraction of BBOA is considerably smaller than for SOA, and a number of unique peaks were detectable only by the filter/acetonitrile method. The combination of PILS collection with HR-ESI-MS analysis offers a new approach for molecular analysis of the water-soluble organic fraction in biogenic SOA, aged photochemical smog, and BBOA.

  11. Estimate of the Impact of Absorbing Aerosol Over Cloud on the MODIS Retrievals of Cloud Optical Thickness and Effective Radius Using Two Independent Retrievals of Liquid Water Path

    NASA Technical Reports Server (NTRS)

    Wilcox, Eric M.; Harshvardhan; Platnick, Steven

    2009-01-01

    Two independent satellite retrievals of cloud liquid water path (LWP) from the NASA Aqua satellite are used to diagnose the impact of absorbing biomass burning aerosol overlaying boundary-layer marine water clouds on the Moderate Resolution Imaging Spectrometer (MODIS) retrievals of cloud optical thickness (tau) and cloud droplet effective radius (r(sub e)). In the MODIS retrieval over oceans, cloud reflectance in the 0.86-micrometer and 2.13-micrometer bands is used to simultaneously retrieve tau and r(sub e). A low bias in the MODIS tau retrieval may result from reductions in the 0.86-micrometer reflectance, which is only very weakly absorbed by clouds, owing to absorption by aerosols in cases where biomass burning aerosols occur above water clouds. MODIS LWP, derived from the product of the retrieved tau and r(sub e), is compared with LWP ocean retrievals from the Advanced Microwave Scanning Radiometer-EOS (AMSR-E), determined from cloud microwave emission that is transparent to aerosols. For the coastal Atlantic southern African region investigated in this study, a systematic difference between AMSR-E and MODIS LWP retrievals is found for stratocumulus clouds over three biomass burning months in 2005 and 2006 that is consistent with above-cloud absorbing aerosols. Biomass burning aerosol is detected using the ultraviolet aerosol index from the Ozone Monitoring Instrument (OMI) on the Aura satellite. The LWP difference (AMSR-E minus MODIS) increases both with increasing tau and increasing OMI aerosol index. During the biomass burning season the mean LWP difference is 14 g per square meters, which is within the 15-20 g per square meter range of estimated uncertainties in instantaneous LWP retrievals. For samples with only low amounts of overlaying smoke (OMI AI less than or equal to 1) the difference is 9.4, suggesting that the impact of smoke aerosols on the mean MODIS LWP is 5.6 g per square meter. Only for scenes with OMI aerosol index greater than 2 does the

  12. Cloud droplet size and liquid water path retrievals from zenith radiance measurements: examples from the Atmospheric Radiation Measurement Program and the Aerosol Robotic Network

    NASA Astrophysics Data System (ADS)

    Chiu, J. C.; Marshak, A.; Huang, C.-H.; Várnai, T.; Hogan, R. J.; Giles, D. M.; Holben, B. N.; O'Connor, E. J.; Knyazikhin, Y.; Wiscombe, W. J.

    2012-11-01

    The ground-based Atmospheric Radiation Measurement Program (ARM) and NASA Aerosol Robotic Network (AERONET) routinely monitor clouds using zenith radiances at visible and near-infrared wavelengths. Using the transmittance calculated from such measurements, we have developed a new retrieval method for cloud effective droplet size and conducted extensive tests for non-precipitating liquid water clouds. The underlying principle is to combine a liquid-water-absorbing wavelength (i.e., 1640 nm) with a non-water-absorbing wavelength for acquiring information on cloud droplet size and optical depth. For simulated stratocumulus clouds with liquid water path less than 300 g m-2 and horizontal resolution of 201 m, the retrieval method underestimates the mean effective radius by 0.8 μm, with a root-mean-squared error of 1.7 μm and a relative deviation of 13%. For actual observations with a liquid water path less than 450 g m-2 at the ARM Oklahoma site during 2007-2008, our 1.5-min-averaged retrievals are generally larger by around 1 μm than those from combined ground-based cloud radar and microwave radiometer at a 5-min temporal resolution. We also compared our retrievals to those from combined shortwave flux and microwave observations for relatively homogeneous clouds, showing that the bias between these two retrieval sets is negligible, but the error of 2.6 μm and the relative deviation of 22% are larger than those found in our simulation case. Finally, the transmittance-based cloud effective droplet radii agree to better than 11% with satellite observations and have a negative bias of 1 μm. Overall, the retrieval method provides reasonable cloud effective radius estimates, which can enhance the cloud products of both ARM and AERONET.

  13. Cloud droplet size and liquid water path retrievals from zenith radiance measurements: examples from the Atmospheric Radiation Measurement Program and the Aerosol Robotic Network

    NASA Astrophysics Data System (ADS)

    Chiu, J. C.; Marshak, A.; Huang, C.-H.; Várnai, T.; Hogan, R. J.; Giles, D. M.; Holben, B. N.; O'Connor, E. J.; Knyazikhin, Y.; Wiscombe, W. J.

    2012-08-01

    The ground-based Atmospheric Radiation Measurement Program (ARM) and NASA Aerosol Robotic Network (AERONET) routinely monitor clouds using zenith radiances at visible and near-infrared wavelengths. Using the transmittance calculated from such measurements, we have developed a new retrieval method for cloud effective droplet size and conducted extensive tests for non-precipitating liquid water clouds. The underlying principle is to combine a water-absorbing wavelength (i.e. 1640 nm) with a non-water-absorbing wavelength for acquiring information on cloud droplet size and optical depth. For simulated stratocumulus clouds with liquid water path less than 300 g m-2 and horizontal resolution of 201 m, the retrieval method underestimates the mean effective radius by 0.8 μm, with a root-mean-squared error of 1.7 μm and a relative deviation of 13%. For actual observations with a liquid water path less than 450 g m-2 at the ARM Oklahoma site during 2007-2008, our 1.5 min-averaged retrievals are generally larger by around 1 μm than those from combined ground-based cloud radar and microwave radiometer at a 5 min temporal resolution. We also compared our retrievals to those from combined shortwave flux and microwave observations for relatively homogeneous clouds, showing that the bias between these two retrieval sets is negligible, but the error of 2.6 μm and the relative deviation of 22% are larger than those found in our simulation case. Finally, the transmittance-based cloud effective droplet radii agree to better than 11% with satellite observations and have a negative bias of 1 μm. Overall, the retrieval method provides reasonable cloud effective radius estimates, which can enhance the cloud products of both ARM and AERONET.

  14. Determination of water-soluble vitamins in infant milk and dietary supplement using a liquid chromatography on-line coupled to a corona-charged aerosol detector.

    PubMed

    Márquez-Sillero, Isabel; Cárdenas, Soledad; Valcárcel, Miguel

    2013-10-25

    A simple and rapid method for the simultaneous determination of seven water-soluble vitamins (thiamine, folic acid, nicotinic acid, ascorbic acid, pantothenic acid, pyridoxine and biotin) was developed by high performance liquid chromatographic separation and corona-charged aerosol detection. The water-soluble vitamins were separated on a Lichrosorb RP-C18 column under isocratic conditions with a mobile phase consisting of 0.05 M ammonium acetate:methanol 90:10 (v/v) at the flow rate 0.5 mL min(-1). The vitamins were extracted from the infant milk (liquid and powder format) using a precipitation step with 2.5 M acetic acid remaining the analyte in the supernatant. As far as dietary supplements are concerned, only a dilution with distilled water was required. The detection limits ranged from 0.17 to 0.62 mg L(-1) for dietary supplements and 1.7 to 6.5 mg L(-1) for milk samples. The precision of the method was evaluated in terms of relative standard deviation (%, RSD) under repeatability and reproducibility conditions, being the average values for each parameter 2.6 and 2.7 for dietary supplements and 4.3 and 4.6 for milk samples. The optimized method was applied to different infant milk samples and dietary supplements. The results of the analysis were in good agreement with the declared values.

  15. Cloud Droplet Size and Liquid Water Path Retrievals From Zenith Radiance Measurements: Examples From the Atmospheric Radiation Measurement Program and the Aerosol Robotic Network

    NASA Technical Reports Server (NTRS)

    Chiu, J. C.; Marshak, A.; Huang, C.-H.; Varnai, T.; Hogan, R. J.; Giles, D. M.; Holben, B. N.; Knyazikhin, Y.; O'Connor, E. J.; Wiscombe, W. J.

    2012-01-01

    The ground-based Atmospheric Radiation Measurement Program (ARM) and NASA Aerosol Robotic Network (AERONET) routinely monitor clouds using zenith radiances at visible and near-infrared wavelengths. Using the transmittance calculated from such measurements, we have developed a new retrieval method for cloud effective droplet size and conducted extensive tests for non-precipitating liquid water clouds. The underlying principle is to combine a water-absorbing wavelength (i.e. 1640 nm) with a nonwater-absorbing wavelength for acquiring information on cloud droplet size and optical depth. For simulated stratocumulus clouds with liquid water path less than 300 g/sq m and horizontal resolution of 201m, the retrieval method underestimates the mean effective radius by 0.8 m, with a root-mean-squared error of 1.7 m and a relative deviation of 13 %. For actual observations with a liquid water path less than 450 gm.2 at the ARM Oklahoma site during 2007-2008, our 1.5 min-averaged retrievals are generally larger by around 1 m than those from combined ground-based cloud radar and microwave radiometer at a 5min temporal resolution. We also compared our retrievals to those from combined shortwave flux and microwave observations for relatively homogeneous clouds, showing that the bias between these two retrieval sets is negligible, but the error of 2.6 m and the relative deviation of 22% are larger than those found in our simulation case. Finally, the transmittance-based cloud effective droplet radii agree to better than 11% with satellite observations and have a negative bias of 1 m. Overall, the retrieval method provides reasonable cloud effective radius estimates, which can enhance the cloud products of both ARM and AERONET.

  16. Aerosol indirect effect dictated by liquid clouds

    NASA Astrophysics Data System (ADS)

    Christensen, Matthew W.; Chen, Yi-Chun; Stephens, Graeme L.

    2016-12-01

    Anthropogenic aerosols have been shown to enhance the solar reflection from warm liquid clouds and mask part of the warming due to the buildup of greenhouse gases. However, very little is known about the effects of aerosol on mixed-phase stratiform clouds as well as other cloud regimes including cumulus, altocumulus, nimbostratus, deep convection, and anvil cirrus. These additional cloud categories are ubiquitous and typically overlooked in satellite-based assessments of the global aerosol indirect forcing. Here we provide their contribution to the aerosol indirect forcing estimate using satellite data collected from several colocated sensors in the A-train for the period 2006-2010. Cloud type is determined according to the 2B-CLDCLASS-LIDAR CloudSat product, and the observations are matched to the radiative flux measurements from CERES (Clouds and the Earth's Radiant Energy System) and aerosol retrievals from MODIS (MODerate resolution Imaging Spectroradiometer). The oceanic mean aerosol indirect forcing is estimated to be -0.20 ± 0.31 W m-2 with warm low-level cloud largely dictating the strength of the response (-0.36 ± 0.21 W m-2) due to their abundance and strong cloud albedo effect. Contributions from mixed-phase low-level cloud (0.01 ± 0.06 W m-2) and convective cloud (0.15 ± 0.23 W m-2) are positive and buffer the system due to strong aerosol-cloud feedbacks that reduce the cloud albedo effect and/or lead to convective invigoration causing a countering positive longwave warming response. By combining all major cloud categories together, aerosol indirect forcing decreases and now contains positive values in the uncertainty estimate.

  17. Aerosol water parameterisation: a single parameter framework

    NASA Astrophysics Data System (ADS)

    Metzger, Swen; Steil, Benedikt; Abdelkader, Mohamed; Klingmüller, Klaus; Xu, Li; Penner, Joyce E.; Fountoukis, Christos; Nenes, Athanasios; Lelieveld, Jos

    2016-06-01

    We introduce a framework to efficiently parameterise the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, based on the coefficient, νi. This solute-specific coefficient was introduced in Metzger et al. (2012) to accurately parameterise the single solution hygroscopic growth, considering the Kelvin effect - accounting for the water uptake of concentrated nanometer-sized particles up to dilute solutions, i.e. from the compounds relative humidity of deliquescence (RHD) up to supersaturation (Köhler theory). Here we extend the νi parameterisation from single to mixed solutions. We evaluate our framework at various levels of complexity, by considering the full gas-liquid-solid partitioning for a comprehensive comparison with reference calculations using the E-AIM, EQUISOLV II and ISORROPIA II models as well as textbook examples. We apply our parameterisation in the EQuilibrium Simplified Aerosol Model V4 (EQSAM4clim) for climate simulations, implemented in a box model and in the global chemistry-climate model EMAC. Our results show (i) that the νi approach enables one to analytically solve the entire gas-liquid-solid partitioning and the mixed solution water uptake with sufficient accuracy, (ii) that ammonium sulfate mixtures can be solved with a simple method, e.g. pure ammonium nitrate and mixed ammonium nitrate and (iii) that the aerosol optical depth (AOD) simulations are in close agreement with remote sensing observations for the year 2005. Long-term evaluation of the EMAC results based on EQSAM4clim and ISORROPIA II will be presented separately.

  18. Aerosol water parameterization: a single parameter framework

    NASA Astrophysics Data System (ADS)

    Metzger, S.; Steil, B.; Abdelkader, M.; Klingmüller, K.; Xu, L.; Penner, J. E.; Fountoukis, C.; Nenes, A.; Lelieveld, J.

    2015-11-01

    We introduce a framework to efficiently parameterize the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, based on the coefficient, νi. This solute specific coefficient was introduced in Metzger et al. (2012) to accurately parameterize the single solution hygroscopic growth, considering the Kelvin effect - accounting for the water uptake of concentrated nanometer sized particles up to dilute solutions, i.e., from the compounds relative humidity of deliquescence (RHD) up to supersaturation (Köhler-theory). Here we extend the νi-parameterization from single to mixed solutions. We evaluate our framework at various levels of complexity, by considering the full gas-liquid-solid partitioning for a comprehensive comparison with reference calculations using the E-AIM, EQUISOLV II, ISORROPIA II models as well as textbook examples. We apply our parameterization in EQSAM4clim, the EQuilibrium Simplified Aerosol Model V4 for climate simulations, implemented in a box model and in the global chemistry-climate model EMAC. Our results show: (i) that the νi-approach enables to analytically solve the entire gas-liquid-solid partitioning and the mixed solution water uptake with sufficient accuracy, (ii) that, e.g., pure ammonium nitrate and mixed ammonium nitrate - ammonium sulfate mixtures can be solved with a simple method, and (iii) that the aerosol optical depth (AOD) simulations are in close agreement with remote sensing observations for the year 2005. Long-term evaluation of the EMAC results based on EQSAM4clim and ISORROPIA II will be presented separately.

  19. Water uptake impedance of glassy organic aerosols

    NASA Astrophysics Data System (ADS)

    Peter, T.; Zobrist, B.; Krieger, U. K.; Luo, B. P.; Soonsin, V.; Marcolli, C.; Koop, T.

    2009-04-01

    Depending on their concentration and composition, aerosols affect various atmospheric properties and processes, such as atmospheric chemistry and Earth's radiative budget. The atmospheric aerosol itself is a complex mixture of various inorganic and organic components, whereas the organic fraction can represent more than 50% of the total aerosol mass. It was recently shown that aerosols high in organics may be present in a glassy state (Zobrist et al., ACP, 8, 5221-5244, 2008). The glassy nature of the aerosols may influence their properties and restrict their functionalities severely, e.g. their water uptake, heterogeneous chemical reactions in their bulk or on their surfaces, as well as ice nucleation and ice crystal growth. Here, we present the first experiments on the water uptake by single levitated glassy aerosol particles using an electrodynamic balance (EDB). Sucrose was chosen as a model substance, which comprises functional groups typical of organic species in the atmosphere. In addition we developed a microphysical model, which enables us to calculate the liquid diffusion inside a glassy particle using water diffusion coefficients in aqueous sucrose particles adapted from the literature. As the diffusion coefficient of water in the particle, D(cH2O), depends on the water concentration cH2O itself, the solution of the diffusion equation presents an interesting non-linear problem. The combined experimental and modelling approach allows describing in detail the water uptake by glassy aerosols at atmospherically relevant temperatures and relative humidities (RH). Hygroscopicity cycles were perfomed in the EDB starting from a crystalline (non-spherical) sucrose particle at 291 K. No water uptake was observed while RH was increased until the particle deliquesces at roughly 85% RH leading to a liquid (spherical) particle. In the subsequent drying cycle, surprisingly no efflorescence was observed when the particle was dried to below 5% and it remained spherical

  20. Raman lidar observations of cloud liquid water.

    PubMed

    Rizi, Vincenzo; Iarlori, Marco; Rocci, Giuseppe; Visconti, Guido

    2004-12-10

    We report the design and the performances of a Raman lidar for long-term monitoring of tropospheric aerosol backscattering and extinction coefficients, water vapor mixing ratio, and cloud liquid water. We focus on the system's capabilities of detecting Raman backscattering from cloud liquid water. After describing the system components, along with the current limitations and options for improvement, we report examples of observations in the case of low-level cumulus clouds. The measurements of the cloud liquid water content, as well as the estimations of the cloud droplet effective radii and number densities, obtained by combining the extinction coefficient and cloud water content within the clouds, are critically discussed.

  1. High air volume to low liquid volume aerosol collector

    DOEpatents

    Masquelier, Donald A.; Milanovich, Fred P.; Willeke, Klaus

    2003-01-01

    A high air volume to low liquid volume aerosol collector. A high volume flow of aerosol particles is drawn into an annular, centripetal slot in a collector which directs the aerosol flow into a small volume of liquid pool contained is a lower center section of the collector. The annular jet of air impinges into the liquid, imbedding initially airborne particles in the liquid. The liquid in the pool continuously circulates in the lower section of the collector by moving to the center line, then upwardly, and through assistance by a rotating deflector plate passes back into the liquid at the outer area adjacent the impinging air jet which passes upwardly through the liquid pool and through a hollow center of the collector, and is discharged via a side outlet opening. Any liquid droplets escaping with the effluent air are captured by a rotating mist eliminator and moved back toward the liquid pool. The collector includes a sensor assembly for determining, controlling, and maintaining the level of the liquid pool, and includes a lower centrally located valve assembly connected to a liquid reservoir and to an analyzer for analyzing the particles which are impinged into the liquid pool.

  2. Evaluation of liquid aerosol transport through porous media

    NASA Astrophysics Data System (ADS)

    Hall, R.; Murdoch, L.; Falta, R.; Looney, B.; Riha, B.

    2016-07-01

    Application of remediation methods in contaminated vadose zones has been hindered by an inability to effectively distribute liquid- or solid-phase amendments. Injection as aerosols in a carrier gas could be a viable method for achieving useful distributions of amendments in unsaturated materials. The objectives of this work were to characterize radial transport of aerosols in unsaturated porous media, and to develop capabilities for predicting results of aerosol injection scenarios at the field-scale. Transport processes were investigated by conducting lab-scale injection experiments with radial flow geometry, and predictive capabilities were obtained by developing and validating a numerical model for simulating coupled aerosol transport, deposition, and multi-phase flow in porous media. Soybean oil was transported more than 2 m through sand by injecting it as micron-scale aerosol droplets. Oil saturation in the sand increased with time to a maximum of 0.25, and decreased with radial distance in the experiments. The numerical analysis predicted the distribution of oil saturation with only minor calibration. The results indicated that evolution of oil saturation was controlled by aerosol deposition and subsequent flow of the liquid oil, and simulation requires including these two coupled processes. The calibrated model was used to evaluate field applications. The results suggest that amendments can be delivered to the vadose zone as aerosols, and that gas injection rate and aerosol particle size will be important controls on the process.

  3. Soft Ionization of Thermally Evaporated Hypergolic Ionic Liquid Aerosols

    SciTech Connect

    Koh, Christine J.; Liu, Chen-Lin; Harmon, Christopher W.; Strasser, Daniel; Golan, Amir; Kostko, Oleg; Chambreau, Steven D.; Vaghjiani, Ghanshyam L.; Leone, Stephen R.

    2011-04-20

    Isolated ion pairs of a conventional ionic liquid, 1-Ethyl-3-Methyl-Imidazolium Bis(trifluoromethylsulfonyl)imide ([Emim+][Tf2N–]), and a reactive hypergolic ionic liquid, 1-Butyl-3-Methyl-Imidazolium Dicyanamide ([Bmim+][Dca–]), are generated by vaporizing ionic liquid submicrometer aerosol particles for the first time; the vaporized species are investigated by dissociative ionization with tunable vacuum ultraviolet (VUV) light, exhibiting clear intact cations, Emim+ and Bmim+, presumably originating from intact ion pairs. Mass spectra of ion pair vapor from an effusive source of the hypergolic ionic liquid show substantial reactive decomposition due to the internal energy of the molecules emanating from the source. Also, hotoionization efficiency curves in the near threshold ionization region of isolated ion pairs of [Emim+][Tf2N] ionic liquid vapor are compared for an aerosol source and an effusive source, revealing changes in the appearance energy due to the amount of internal energy in the ion pairs. The aerosol source has a shift to higher threshold energy (~0.3 eV), attributed to reduced internal energy of the isolated ion pairs. Lastly, the method of ionic liquid submicrometer aerosol particle vaporization, for reactive ionic liquids such as hypergolic species, is a convenient, thermally “cooler” source of isolated intact ion pairs in the gas phase compared to effusive sources.

  4. Soft ionization of thermally evaporated hypergolic ionic liquid aerosols

    SciTech Connect

    University of California; ERC, Incorporated, Edwards Air Force Base; Air Force Research Laboratory, Edwards Air Force Base; National Synchrotron Radiation Research Center; Institute of Chemistry, Hebrew University; Koh, Christine J.; Liu, Chen-Lin; Harmon, Christopher W.; Strasser, Daniel; Golan, Amir; Kostko, Oleg; Chambreau, Steven D.; Vaghjiani, Ghanshyam L.; Leone, Stephen R.

    2011-07-19

    Isolated ion pairs of a conventional ionic liquid, 1-Ethyl-3-Methyl-Imidazolium Bis(trifluoromethylsulfonyl)imide ([Emim+][Tf2N?]), and a reactive hypergolic ionic liquid, 1-Butyl-3-Methyl-Imidazolium Dicyanamide ([Bmim+][Dca?]), are generated by vaporizing ionic liquid submicron aerosol particles for the first time; the vaporized species are investigated by dissociative ionization with tunable vacuum ultraviolet (VUV) light, exhibiting clear intact cations, Emim+ and Bmim+, presumably originating from intact ion pairs. Mass spectra of ion pair vapor from an effusive source of the hypergolic ionic liquid show substantial reactive decomposition due to the internal energy of the molecules emanating from the source. Photoionization efficiency curves in the near threshold ionization region of isolated ion pairs of [Emim+][Tf2N?]ionic liquid vapor are compared for an aerosol source and an effusive source, revealing changes in the appearance energy due to the amount of internal energy in the ion pairs. The aerosol source has a shift to higher threshold energy (~;;0.3 eV), attributed to reduced internal energy of the isolated ion pairs. The method of ionic liquid submicron aerosol particle vaporization, for reactive ionic liquids such as hypergolic species, is a convenient, thermally ?cooler? source of isolated intact ion pairs in the gas phase compared to effusive sources.

  5. Soft Ionization of Thermally Evaporated Hypergolic Ionic Liquid Aerosols

    DTIC Science & Technology

    2011-03-04

    NOTES For publication in J. Phys. Chem. A in March 2011 14. ABSTRACT Isolated ion pairs of a conventional ionic liquid, 1-Ethyl-3-Methyl- Imidazolium ...Bis(trifluoromethylsulfonyl)imide ([Emim+][Tf2N−]), and a reactive hypergolic ionic liquid, 1-Butyl-3-Methyl- Imidazolium Dicyanamide ([Bmim+][Dca...2011 TITLE RUNNING HEAD: Soft ionization of evaporated IL aerosols Isolated ion pairs of a conventional ionic liquid, 1-Ethyl-3-Methyl- Imidazolium

  6. Water: The Strangest Liquid

    SciTech Connect

    Nilsson, Anders

    2009-02-24

    Water, H2O, is familiar to everyone - it shapes our bodies and our planet. But despite its abundance, water has remained a mystery, exhibiting many strange properties that are still not understood. Why does the liquid have an unusually large capacity to store heat? And why is it denser than ice? Now, using the intense X-ray beams from particle accelerators, investigations into water are leading to fundamental discoveries about the structure and arrangement of water molecules. This lecture will elucidate the many mysteries of water and discuss current studies that are revolutionizing the way we see and understand one of the most fundamental substances of life.

  7. Mars: occurrence of liquid water.

    PubMed

    Ingersoll, A P

    1970-05-22

    In the absence of juvenile liquid water, condensation of water vapor to ice and subsequent melting of ice are the only means of producing liquid water on the martian surface. However, the evaporation rate is so high that the available heat sources cannot melt pure ice. Liquid water is therefore limited to concentrated solutions of strongly deliquescent salts.

  8. Aerosol size distribution and aerosol water content measurements during Atlantic Stratocumulus Transition Experiment/Marine Aerosol and Gas Exchange

    NASA Astrophysics Data System (ADS)

    Kim, Y.; Sievering, H.; Boatman, J.; Wellman, D.; Pszenny, A.

    1995-11-01

    Aerosol size distribution data measured during the June 1992 Marine Aerosol and Gas Exchange experiment are analyzed to investigate the characteristics of fine marine aerosol particles measured over the North Atlantic near the Azores Islands. Measured aerosol size distribution data were corrected using the corrected size calibration data based on the optical properties of particles being measured. The corrected size distribution data were then approximated with either one or two lognormal size distributions, depending on air mass conditions. Under clean air mass conditions <3 μm diameter aerosol size distributions typically exhibited two modes, consisting of an accumulation mode and the small end of the sea-salt particle mode. However, under the influence of continental polluted air masses, the aerosol size distribution was dominated by <1 μm diameter particles in a single mode with an increased aerosol concentration. Aerosol water content of accumulation mode marine aerosols was estimated from differences between several series of ambient and dried aerosol size distributions. The average aerosol water fraction was 0.31, which is in good agreement with an empirical aerosol growth model estimate. The average rate of SO4= production in the accumulation mode aerosol water by H2O2 oxidation was estimated to be <7×10-10 mol L-1 s-1, which is an insignificant contributor to the observed non-sea-salt SO4= in the accumulation mode.

  9. Water absorption by secondary organic aerosol and its effect on inorganic aerosol behavior

    SciTech Connect

    Ansari, A.S.; Pandis, S.N.

    2000-01-01

    The hygroscopic nature of atmospheric aerosol has generally been associated with its inorganic fraction. In this study, a group contribution method is used to predict the water absorption of secondary organic aerosol (SOA). Compared against growth measurements of mixed inorganic-organic particles, this method appears to provide a first-order approximation in predicting SOA water absorption. The growth of common SOA species is predicted to be significantly less than common atmospheric inorganic salts such as (NH{sub 4}){sub 2}SO{sub 4} and NaCl. Using this group contribution method as a tool in predicting SOA water absorption, an integrated modeling approach is developed combining available SOA and inorganic aerosol models to predict overall aerosol behavior. The effect of SOA on water absorption and nitrate partitioning between the gas and aerosol phases is determined. On average, it appears that SOA accounts for approximately 7% of total aerosol water and increases aerosol nitrate concentrations by approximately 10%. At high relative humidity and low SOA mass fractions, the role of SOA in nitrate partitioning and its contribution to total aerosol water is negligible. However, the water absorption of SOA appears to be less sensitive to changes in relative humidity than that of inorganic species, and thus at low relative humidity and high SOA mass fraction concentrations, SOA is predicted to account for approximately 20% of total aerosol water and a 50% increase in aerosol nitrate concentrations. These findings could improve the results of modeling studies where aerosol nitrate has often been underpredicted.

  10. 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

  11. Effect of nitrate and sulfate relative abundance in PM2.5 on liquid water content explored through half-hourly observations of inorganic soluble aerosols at a polluted receptor site

    NASA Astrophysics Data System (ADS)

    Xue, Jian; Griffith, Stephen M.; Yu, Xin; Lau, Alexis K. H.; Yu, Jian Zhen

    2014-12-01

    Liquid water content (LWC) is the amount of liquid water on aerosols. It contributes to visibility degradation, provides a surface for gas condensation, and acts as a medium for heterogeneous gas/particle reactions. In this study, 520 half-hourly measurements of ionic chemical composition in PM2.5 at a receptor site in Hong Kong are used to investigate the dependence of LWC on ionic chemical composition, particularly on the relative abundance of sulfate and nitrate. LWC was estimated using a thermodynamic model (AIM-III). Within this data set of PM2.5 ionic compositions, LWC was highly correlated with the multivariate combination of sulfate and nitrate concentrations and RH (R2 = 0.90). The empirical linear regression result indicates that LWC is more sensitive to nitrate mass than sulfate. During a nitrate episode, the highest LWC (80.6 ± 17.9 μg m-3) was observed and the level was 70% higher than that during a sulfate episode despite a similar ionic PM2.5 mass concentration. A series of sensitivity tests were conducted to study LWC change as a function of the relative nitrate and sulfate abundance, the trend of which is expected to shift to more nitrate in China as a result of SO2 reduction and increase in NOx emission. Starting from a base case that uses the average of measured PM2.5 ionic chemical composition (63% SO42-, 11% NO3-, 19% NH4+, and 7% other ions) and an ionic equivalence ratio, [NH4+]/(2[SO42-] + [NO3-]), set constant to 0.72, the results show LWC would increase by 204% at RH = 40% when 50% of the SO42- is replaced by NO3- mass concentration. This is largely due to inhibition of (NH4)3H(SO4)2 crystallization while PM2.5 ionic species persist in the aqueous phase. At RH = 90%, LWC would increase by 12% when 50% of the SO42- is replaced by NO3- mass concentration. The results of this study highlight the important implications to aerosol chemistry and visibility degradation associated with LWC as a result of a shift in PM2.5 ionic chemical

  12. Aerosols, light, and water: Measurements of aerosol optical properties at different relative humidities

    NASA Astrophysics Data System (ADS)

    Orozco, Daniel

    The Earth's atmosphere is composed of a large number of different gases as well as tiny suspended particles, both in solid and liquid state. These tiny particles, called atmospheric aerosols, have an immense impact on our health and on our global climate. Atmospheric aerosols influence the Earth's radiation budget both directly and indirectly. In the direct effect, aerosols scatter and absorb sunlight changing the radiative balance of the Earth-atmosphere system. Aerosols indirectly influence the Earth's radiation budget by modifying the microphysical and radiative properties of clouds as well as their water content and lifetime. In ambient conditions, aerosol particles experience hygroscopic growth due to the influence of relative humidity (RH), scattering more light than when the particles are dry. The quantitative knowledge of the RH effect and its influence on the light scattering coefficient and, in particular, on the phase function and polarization of aerosol particles is of substantial importance when comparing ground based observations with other optical aerosol measurements techniques such satellite and sunphotometric retrievals of aerosol optical depth and their inversions. This dissertation presents the aerosol hygroscopicity experiment investigated using a novel dryer-humidifier system, coupled to a TSI-3563 nephelometer, to obtain the light scattering coefficient (sp) as a function of relative humidity (RH) in hydration and dehydration modes. The measurements were performed in Porterville, CA (Jan 10-Feb 6, 2013), Baltimore, MD (Jul 3-30, 2013), and Golden, CO (Jul 12-Aug 10, 2014). Observations in Porterville and Golden were part of the NASA-sponsored DISCOVER-AQ project. The measured sp under varying RH in the three sites was combined with ground aerosol extinction, PM2:5mass concentrations, particle composition measurements, and compared with airborne observations performed during campaigns. The enhancement factor, f(RH), defined as the ratio of sp

  13. Condensational growth and trace species scavenging in stratospheric sulfuric acid/water aerosol droplets

    NASA Technical Reports Server (NTRS)

    Tompson, Robert V., Jr.

    1991-01-01

    Stratospheric aerosols play a significant role in the environment. The composition of aerosols is believed to be a liquid solution of sulfuric acid and water with numerous trace species. Of these trace species, ozone in particular was recognized as being very important in its role of shielding the environment from harmful ultraviolet radiation. Also among the trace species are HCl and ClONO2, the so called chlorine reservoir species and various oxides of nitrogen. The quantity of stratospheric aerosol and its particle size distribution determines, to a large degree, the chemistry present in the stratosphere. Aerosols experience 3 types of growth: nucleation, condensation, and coagulation. The application of condensation investigations to the specific problem of stratospheric aerosols is discussed.

  14. Comparative Evaluation of Two Different Ultrasonic Liquid Coolants on Dental Aerosols

    PubMed Central

    Bhandari, Vishnudas; Ugale, Gauri; Taru, Snehal; Khaparde, Surbhi; Kulkarni, Arun; Ardale, Mukesh; Marde, Shraddha

    2016-01-01

    Introduction Dentists are more prone for developing infectious diseases especially related to respiratory system. The ultrasonic scaler which is a major source of dental aerosol production is most frequently used contrivance in a dental set up. Aim The aim of this study was to evaluate the effect of povidone iodine and chlorhexidine gluconate as an ultrasonic liquid coolant on aerosols in comparison with distilled water. The objectives of this study were to compare the potency of povidone iodine and chlorhexidine gluconate on reducing dental aerosols and quantitative assessment of microbial content of dental aerosols at right, left and behind the dental chair. Materials and Methods In this study 30 subjects were selected who fulfilled the inclusion criteria and were divided into three groups. Group 1 (Control group): Ultrasonic scaling with distilled water (10 subjects), Group 2 (Test group): Ultrasonic scaling with 2% povidone iodine (10 subjects), Group 3 (Test group): Ultrasonic scaling with 0.12% chlorhexidine (10 subjects). At the baseline one blood agar plate was kept for 10 minutes in the fumigated chamber before ultrasonic scaling, thereafter three blood agar plates were kept at a distance of 0.4 meters away on either side of the patient and 2 meters behind the patient’s mouth during ultrasonic scaling. Blood agar plates were kept for gravitometric settling of dental aerosols. Results At baseline, no significant numbers of Colony-Forming Units (CFU) were detected. It is found that Group 3 (chlorhexidine gluconate) showed effective CFU reduction (27.17 ±12.5 CFU) when compared to distilled water (124.5 ± 30.08 CFU) and povidone iodine (60.43 ± 33.33 CFU). More CFU were found on blood agar plates which were kept on right side in all the three groups. The results obtained were statistically significant (p< 0.001). Conclusion Chlorhexidine gluconate is more effective in reducing dental aerosols when compared to povidone iodine and distilled water. Povidone

  15. Computation of liquid-liquid equilibria and phase stabilities: implications for RH-dependent gas/particle partitioning of organic-inorganic aerosols

    NASA Astrophysics Data System (ADS)

    Zuend, A.; Marcolli, C.; Peter, T.; Seinfeld, J. H.

    2010-08-01

    Semivolatile organic and inorganic aerosol species partition between the gas and aerosol particle phases to maintain thermodynamic equilibrium. Liquid-liquid phase separation into an organic-rich and an aqueous electrolyte phase can occur in the aerosol as a result of the salting-out effect. Such liquid-liquid equilibria (LLE) affect the gas/particle partitioning of the different semivolatile compounds and might significantly alter both particle mass and composition as compared to a one-phase particle. We present a new liquid-liquid equilibrium and gas/particle partitioning model, using as a basis the group-contribution model AIOMFAC (Zuend et al., 2008). This model allows the reliable computation of the liquid-liquid coexistence curve (binodal), corresponding tie-lines, the limit of stability/metastability (spinodal), and further thermodynamic properties of multicomponent systems. Calculations for ternary and multicomponent alcohol/polyol-water-salt mixtures suggest that LLE are a prevalent feature of organic-inorganic aerosol systems. A six-component polyol-water-ammonium sulphate system is used to simulate effects of relative humidity (RH) and the presence of liquid-liquid phase separation on the gas/particle partitioning. RH, salt concentration, and hydrophilicity (water-solubility) are identified as key features in defining the region of a miscibility gap and govern the extent to which compound partitioning is affected by changes in RH. The model predicts that liquid-liquid phase separation can lead to either an increase or decrease in total particulate mass, depending on the overall composition of a system and the particle water content, which is related to the hydrophilicity of the different organic and inorganic compounds. Neglecting non-ideality and liquid-liquid phase separations by assuming an ideal mixture leads to an overestimation of the total particulate mass by up to 30% for the composition and RH range considered in the six-component system

  16. Computation of liquid-liquid equilibria and phase stabilities: implications for RH-dependent gas/particle partitioning of organic-inorganic aerosols

    NASA Astrophysics Data System (ADS)

    Zuend, A.; Marcolli, C.; Peter, T.; Seinfeld, J. H.

    2010-05-01

    Semivolatile organic and inorganic aerosol species partition between the gas and aerosol particle phases to maintain thermodynamic equilibrium. Liquid-liquid phase separation into an organic-rich and an aqueous electrolyte phase can occur in the aerosol as a result of the salting-out effect. Such liquid-liquid equilibria (LLE) affect the gas/particle partitioning of the different semivolatile compounds and might significantly alter both particle mass and composition as compared to a one-phase particle. We present a new liquid-liquid equilibrium and gas/particle partitioning model, using as a basis the group-contribution model AIOMFAC (Zuend et al., 2008). This model allows the reliable computation of the liquid-liquid coexistence curve (binodal), corresponding tie-lines, the limit of stability/metastability (spinodal), and further thermodynamic properties of the phase diagram. Calculations for ternary and multicomponent alcohol/polyol-water-salt mixtures suggest that LLE are a prevalent feature of organic-inorganic aerosol systems. A six-component polyol-water-ammonium sulphate system is used to simulate effects of relative humidity (RH) and the presence of liquid-liquid phase separation on the gas/particle partitioning. RH, salt concentration, and hydrophilicity (water-solubility) are identified as key features in defining the region of a miscibility gap and govern the extent to which compound partitioning is affected by changes in RH. The model predicts that liquid-liquid phase separation can lead to either an increase or decrease in total particulate mass, depending on the overall composition of a system and the particle water content, which is related to the hydrophilicity of the different organic and inorganic compounds. Neglecting non-ideality and liquid-liquid phase separations by assuming an ideal mixture leads to an overestimation of the total particulate mass by up to 30% for the composition and RH range considered in the six-component system simulation

  17. Hydroxyl radicals from secondary organic aerosol decomposition in water

    NASA Astrophysics Data System (ADS)

    Tong, Haijie; Arangio, Andrea M.; Lakey, Pascale S. J.; Berkemeier, Thomas; Liu, Fobang; Kampf, Christopher. J.; Pöschl, Ulrich; Shiraiwa, Manabu

    2016-04-01

    We found that ambient and laboratory-generated secondary organic aerosols (SOA) form substantial amounts of OH radicals upon interaction with liquid water, which can be explained by the decomposition of organic hydroperoxides. The molar OH yield from SOA formed by ozonolysis of terpenes (α-pinene, β-pinene, and limonene) is ~ 0.1% upon extraction with pure water, and which increases to ~ 1.5% in the presence of iron ions due to Fenton-like reactions. Our findings imply that the chemical reactivity and aging of SOA particles is strongly enhanced upon interaction with water and iron. In cloud droplets under dark conditions, SOA decomposition can compete with the classical hydrogen peroxide Fenton reaction as the source of OH radicals. Also in the human respiratory tract, the inhalation and deposition of SOA particles may lead to a substantial release of OH radicals, which may contribute to oxidative stress and play an important role in the adverse health effects of atmospheric aerosols.

  18. Hydroxyl radicals from secondary organic aerosol decomposition in water

    NASA Astrophysics Data System (ADS)

    Tong, Haijie; Arangio, Andrea M.; Lakey, Pascale S. J.; Berkemeier, Thomas; Liu, Fobang; Kampf, Christopher J.; Brune, William H.; Pöschl, Ulrich; Shiraiwa, Manabu

    2016-02-01

    We found that ambient and laboratory-generated secondary organic aerosols (SOA) form substantial amounts of OH radicals upon interaction with liquid water, which can be explained by the decomposition of organic hydroperoxides. The molar OH yield from SOA formed by ozonolysis of terpenes (α-pinene, β-pinene, limonene) is ˜ 0.1 % upon extraction with pure water and increases to ˜ 1.5 % in the presence of Fe2+ ions due to Fenton-like reactions. Upon extraction of SOA samples from OH photooxidation of isoprene, we also detected OH yields of around ˜ 0.1 %, which increases upon addition of Fe2+. Our findings imply that the chemical reactivity and aging of SOA particles is strongly enhanced upon interaction with water and iron. In cloud droplets under dark conditions, SOA decomposition can compete with the classical H2O2 Fenton reaction as the source of OH radicals. Also in the human respiratory tract, the inhalation and deposition of SOA particles may lead to a substantial release of OH radicals, which may contribute to oxidative stress and play an important role in the adverse health effects of atmospheric aerosols.

  19. Hydroxyl radicals from secondary organic aerosol decomposition in water

    NASA Astrophysics Data System (ADS)

    Tong, H.; Arangio, A. M.; Lakey, P. S. J.; Berkemeier, T.; Liu, F.; Kampf, C. J.; Pöschl, U.; Shiraiwa, M.

    2015-11-01

    We found that ambient and laboratory-generated secondary organic aerosols (SOA) form substantial amounts of OH radicals upon interaction with liquid water, which can be explained by the decomposition of organic hydroperoxides. The molar OH yield from SOA formed by ozonolysis of terpenes (α-pinene, β-pinene, limonene) is ~ 0.1 % upon extraction with pure water and increases to ~ 1.5 % in the presence of Fe2+ ions due to Fenton-like reactions. Our findings imply that the chemical reactivity and aging of SOA particles is strongly enhanced upon interaction with water and iron. In cloud droplets under dark conditions, SOA decomposition can compete with the classical H2O2 Fenton reaction as the source of OH radicals. Also in the human respiratory tract, the inhalation and deposition of SOA particles may lead to a substantial release of OH radicals, which may contribute to oxidative stress and play an important role in the adverse health effects of atmospheric aerosols.

  20. Hospital washbasin water: risk of Legionella-contaminated aerosol inhalation.

    PubMed

    Cassier, P; Landelle, C; Reyrolle, M; Nicolle, M C; Slimani, S; Etienne, J; Vanhems, P; Jarraud, S

    2013-12-01

    The contamination of aerosols by washbasin water colonized by Legionella in a hospital was evaluated. Aerosol samples were collected by two impingement technologies. Legionella was never detected by culture in all the (aerosol) samples. However, 45% (18/40) of aerosol samples were positive for Legionella spp. by polymerase chain reaction, with measurable concentrations in 10% of samples (4/40). Moreover, immunoassay detected Legionella pneumophila serogroup 1 and L. anisa, and potentially viable bacteria were seen on viability testing. These data suggest that colonized hospital washbasins could represent risks of exposure to Legionella aerosol inhalation, especially by immunocompromised patients.

  1. Viscosity and electric properties of water aerosols

    NASA Astrophysics Data System (ADS)

    Shavlov, A. V.; Sokolov, I. V.; Dzhumandzhi, V. A.

    2016-09-01

    The flow of water mist in a narrow duct has been studied experimentally. The profile of the velocity of drops has been measured, and the viscosity of the mist has been calculated using the Navier-Stokes equation. It has been found that at low gradients of the rate of shear the viscosity of the mist can exceed that of clean air by tens and even hundreds of times. The electric charge of the drops has been measured. It has been found that the viscosity of the mist differs from that of clean air at gradients of the rate of shear that are less than the frequency of the establishment of electric equilibrium between the drops. A comparative analysis of the viscosities of the mist and a drop cluster has been carried out, and the dependence of the viscosity of the water aerosol on the radius and the charge of the drops has been predicted. The possible role of aerosols that contain submicron drops in the known "clear air turbulence" problem has been shown.

  2. 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.

  3. Liquid-liquid phase separation in aerosol particles: Dependence on O:C, organic functionalities, and compositional complexity

    NASA Astrophysics Data System (ADS)

    Song, M.; Marcolli, C.; Krieger, U. K.; Zuend, A.; Peter, T.

    2012-10-01

    Atmospheric aerosol particles may undergo liquid-liquid phase separation (LLPS) when exposed to varying relative humidity. In this study we investigated the occurrence of LLPS for mixtures consisting of up to ten organic compounds, ammonium sulfate, and water in relationship with the organic oxygen-to-carbon (O:C) ratio. LLPS always occurred for O:C < 0.56, never occurred for O:C > 0.80, and depended on the specific types and compositions of organic functional groups in the regime 0.56 < O:C < 0.80. In the intermediate regime, mixtures with a high share of aromatic compounds shifted the limit of occurrence of LLPS to lower O:C ratios. The number of mixture components and the spread of the O:C range did not notably influence the conditions for LLPS to occur. Since in ambient aerosols O:C range typically between 0.2 and 1.0, LLPS is expected to be a common feature of tropospheric aerosols.

  4. Evaluating Global Aerosol Models and Aerosol and Water Vapor Properties Near Clouds

    SciTech Connect

    Richard A. Ferrare; David D. Turner

    2011-09-01

    Project goals: (1) Use the routine surface and airborne measurements at the ARM SGP site, and the routine surface measurements at the NSA site, to continue our evaluations of model aerosol simulations; (2) Determine the degree to which the Raman lidar measurements of water vapor and aerosol scattering and extinction can be used to remotely characterize the aerosol humidification factor; (3) Use the high temporal resolution CARL data to examine how aerosol properties vary near clouds; and (4) Use the high temporal resolution CARL and Atmospheric Emitted Radiance Interferometer (AERI) data to quantify entrainment in optically thin continental cumulus clouds.

  5. Evaluating Global Aerosol Models and Aerosol and Water Vapor Properties Near Clouds

    SciTech Connect

    Turner, David, D.; Ferrare, Richard, A.

    2011-07-06

    The 'Evaluating Global Aerosol Models and Aerosol and Water Vapor Properties Near Clouds' project focused extensively on the analysis and utilization of water vapor and aerosol profiles derived from the ARM Raman lidar at the Southern Great Plains ARM site. A wide range of different tasks were performed during this project, all of which improved quality of the data products derived from the lidar or advanced the understanding of atmospheric processes over the site. These activities included: upgrading the Raman lidar to improve its sensitivity; participating in field experiments to validate the lidar aerosol and water vapor retrievals; using the lidar aerosol profiles to evaluate the accuracy of the vertical distribution of aerosols in global aerosol model simulations; examining the correlation between relative humidity and aerosol extinction, and how these change, due to horizontal distance away from cumulus clouds; inferring boundary layer turbulence structure in convective boundary layers from the high-time-resolution lidar water vapor measurements; retrieving cumulus entrainment rates in boundary layer cumulus clouds; and participating in a field experiment that provided data to help validate both the entrainment rate retrievals and the turbulent profiles derived from lidar observations.

  6. Ice crystallization in ultrafine water-salt aerosols: nucleation, ice-solution equilibrium, and internal structure.

    PubMed

    Hudait, Arpa; Molinero, Valeria

    2014-06-04

    Atmospheric aerosols have a strong influence on Earth's climate. Elucidating the physical state and internal structure of atmospheric aqueous aerosols is essential to predict their gas and water uptake, and the locus and rate of atmospherically important heterogeneous reactions. Ultrafine aerosols with sizes between 3 and 15 nm have been detected in large numbers in the troposphere and tropopause. Nanoscopic aerosols arising from bubble bursting of natural and artificial seawater have been identified in laboratory and field experiments. The internal structure and phase state of these aerosols, however, cannot yet be determined in experiments. Here we use molecular simulations to investigate the phase behavior and internal structure of liquid, vitrified, and crystallized water-salt ultrafine aerosols with radii from 2.5 to 9.5 nm and with up to 10% moles of ions. We find that both ice crystallization and vitrification of the nanodroplets lead to demixing of pure water from the solutions. Vitrification of aqueous nanodroplets yields nanodomains of pure low-density amorphous ice in coexistence with vitrified solute rich aqueous glass. The melting temperature of ice in the aerosols decreases monotonically with an increase of solute fraction and decrease of radius. The simulations reveal that nucleation of ice occurs homogeneously at the subsurface of the water-salt nanoparticles. Subsequent ice growth yields phase-segregated, internally mixed, aerosols with two phases in equilibrium: a concentrated water-salt amorphous mixture and a spherical cap-like ice nanophase. The surface of the crystallized aerosols is heterogeneous, with ice and solution exposed to the vapor. Free energy calculations indicate that as the concentration of salt in the particles, the advance of the crystallization, or the size of the particles increase, the stability of the spherical cap structure increases with respect to the alternative structure in which a core of ice is fully surrounded by

  7. Prediction of activity coefficients in liquid aerosol particles containing organic compounds, dissolved inorganic salts, and water—Part 1: Organic compounds and water by consideration of short- and long-range effects using X-UNIFAC.1

    NASA Astrophysics Data System (ADS)

    Erdakos, Garnet B.; Asher, William E.; Seinfeld, John H.; Pankow, James F.

    The semi-empirical group contribution method (GCM) of Kikic et al. [Chem. Eng. Sci. 46 (1991) 2775-2780] for estimating activity coefficient ( ζ) values of neutral organic compounds and water in solutions composed of organic compounds, dissolved inorganic salts, and water is adapted for application to atmospheric particulate matter (PM). It is assumed that ζ values are determined by a combination of short- and long-range interactions. The ζ expression involves conventional UNIFAC terms and a Debye-Hückel term, with the former computed using group-group interaction parameters. Organic-organic interaction parameters are assigned the values from the UNIFAC-LLE model of Magnussen et al. [Ind. Eng. Chem. Process Design Develop. 20 (1981) 331-339]. Forty interaction parameters (ion-solvent group and anion-cation) were obtained from Kikic et al. [Chem. Eng. Sci. 46 (1991) 2775-2780], Achard et al. [Fluid Phase Equilibria 98 (1994) 71-89], and Ming and Russell [Am. Inst. Chem. Eng. J. 48 (2002) 1331-1348]. Twenty additional interaction parameters (ion-solvent group) are estimated based on 879 UNIQUAC-fitted ζ values for organic compounds and water. The fitted ζ values are based on liquid-liquid equilibrium (LLE) data for a range of ternary and quaternary organic/inorganic salt/water mixtures at 293-308 K. The UNIQUAC fits are analogous to those described by Fredenslund et al. [Vapor-Liquid Equilibria Using UNIFAC: A Group-Contribution Method, Elsevier Scientific Publishing, New York, 1977]. The LLE mixture compositions range from primarily organic solutions to primarily aqueous solutions with maximum ionic strengths of ˜5 mol kg -1. The groups characteristic of organic compounds found in atmospheric PM considered here include: CH 3-, -CH 2-, -CH|-, -C||-, -OH, -CH 2CO-, and -COOH. These are: single bonded carbon with three, two, one, and zero hydrogens, respectively, hydroxyl, -CH 2-carbonyl, and carboxyl, respectively. The inorganic salts

  8. New liquid aerosol generation devices: systems that force pressurized liquids through nozzles.

    PubMed

    Geller, David E

    2002-12-01

    Over the past few decades, aerosol delivery devices have been relatively inefficient, wasteful, and difficult for patients to use. These drawbacks have been tolerated because the drugs available for inhalation have wide therapeutic margins and steep dose-response curves at low doses. Recently several forces have converged to drive innovation in the aerosol device industry: the ban on chlorofluorocarbon propellants in metered-dose inhalers, the need for more user-friendly devices, and the invention of expensive inhalable therapies for topical and systemic lung delivery. Numerous devices are in development to improve the efficiency, ease of use, and reproducibility of aerosol delivery to the lung, including systems that force liquid through a nozzle to form the aerosol cloud. The Respimat is a novel, compact, propellant-free, multi-dose inhaler that employs a spring to push drug solution through a nozzle, which generates a slow-moving aerosol. Deposition studies show that the Respimat can deliver 39-44% of a dose to the lungs. Clinical asthma and chronic obstructive pulmonary disease trials with bronchodilators show that the Respimat is 2-8 times as effective as a metered-dose inhaler. Respimat has been tested with bronchodilators and inhaled corticosteroids. The AERx device uses sophisticated electronics to deliver aerosol from a single-dose blister, using an integral, disposable nozzle array. The electronics control dose expression and titration, timing of aerosol generation with the breath, and provide feedback for proper inhalation technique. Lung deposition ranges from 50 to 80% of the loaded dose, with remarkable reproducibility. AERx has been tested with a variety of drugs, for both topical and systemic delivery, including rhDNase (dornase alfa), insulin, and opioids. These novel devices face competition from other technologies as well as financial and regulatory hurdles, but they both offer a marked improvement in the efficiency of pulmonary drug delivery.

  9. Discrimination of water, ice and aerosols by light polarisation in the CLOUD experiment

    NASA Astrophysics Data System (ADS)

    Nichman, L.; Fuchs, C.; Järvinen, E.; Ignatius, K.; Höppel, N. F.; Dias, A.; Heinritzi, M.; Simon, M.; Tröstl, J.; Wagner, A. C.; Wagner, R.; Williamson, C.; Yan, C.; Bianchi, F.; Connolly, P. J.; Dorsey, J. R.; Duplissy, J.; Ehrhart, S.; Frege, C.; Gordon, H.; Hoyle, C. R.; Kristensen, T. B.; Steiner, G.; Donahue, N. M.; Flagan, R.; Gallagher, M. W.; Kirkby, J.; Möhler, O.; Saathoff, H.; Schnaiter, M.; Stratmann, F.; Tomé, A.

    2015-11-01

    Cloud microphysical processes involving the ice phase in tropospheric clouds are among the major uncertainties in cloud formation, weather and General Circulation Models (GCMs). The simultaneous detection of aerosol particles, liquid droplets, and ice crystals, especially in the small cloud-particle size range below 50 μm, remains challenging in mixed phase, often unstable ice-water phase environments. The Cloud Aerosol Spectrometer with Polarisation (CASPOL) is an airborne instrument that has the ability to detect such small cloud particles and measure their effects on the backscatter polarisation state. Here we operate the versatile Cosmics-Leaving-OUtdoor-Droplets (CLOUD) chamber facility at the European Organisation for Nuclear Research (CERN) to produce controlled mixed phase and other clouds by adiabatic expansions in an ultraclean environment, and use the CASPOL to discriminate between different aerosols, water and ice particles. In this paper, optical property measurements of mixed phase clouds and viscous Secondary Organic Aerosol (SOA) are presented. We report observations of significant liquid - viscous SOA particle polarisation transitions under dry conditions using CASPOL. Cluster analysis techniques were subsequently used to classify different types of particles according to their polarisation ratios during phase transition. A classification map is presented for water droplets, organic aerosol (e.g., SOA and oxalic acid), crystalline substances such as ammonium sulphate, and volcanic ash. Finally, we discuss the benefits and limitations of this classification approach for atmospherically relevant concentration and mixtures with respect to the CLOUD 8-9 campaigns and its potential contribution to Tropical Troposphere Layer (TTL) analysis.

  10. Experiments on liquid-metal fast breeder reactor aerosol source terms after severe accidents

    SciTech Connect

    Berthoud, G.; Longest, A.W.; Wright, A.L.; Schutz, W.P.

    1988-05-01

    In the extremely unlikely event of a liquid-metal fast breeder reactor core disruptive accident, expanding core material or sodium vapor inside the sodium pool may cause leaks in the vessel head and transport of radioactive material, mostly aerosols, in one large bubble or several smaller bubbles under energetic conditions to the cover gas and through leaks to the inner containment (''instantaneous source term''). Out-of-pile experiments on bubble expansion from a pressurized source inside a liquid (water or sodium) and related phenomena like heat transfer, condensation, entrainment, rise, and aerosol transport were carried out in France and the United States and are continuing in the Federal Republic of Germany. Parameters and results of these experiments are described and discussed, mainly concerning the aerosol problem. It appears that several mechanisms exist for a very efficient removal of particles from the bubble. Retention factors larger than 10,000 were found in most cases. In addition, a short survey is given of French and German experiments on fuel and fission product release from evaporating or burning sodium pools (delayed source term).

  11. Satellite Remote Sensing of the Liquid Water Sensitivity in Water Clouds

    NASA Technical Reports Server (NTRS)

    Han, Qing-Yuan; Rossow, William B.; Welch, Ronald; Zeng, Jane; Jansen, James E. (Technical Monitor)

    2001-01-01

    In estimation of the aerosol indirect effect, cloud liquid water path is considered either constant (Twomey effect) or increasing with enhanced droplet number concentrations (drizzle-suppression effect, or Albrecht effect) if cloud microphysics is the prevailing mechanism during the aerosol-cloud interactions. On the other hand, if cloud thermodynamics and dynamics are considered, the cloud liquid water path may be decreased with increasing droplet number concentration, which is predicted by model calculations and observed in ship-track and urban influence studies. This study is to examine the different responses of cloud liquid water path to changes of cloud droplet number concentration. Satellite data (January, April, July and October 1987) are used to retrieve the cloud liquid water sensitivity, defined as the changes of liquid water path versus changes of column droplet number concentrations. The results of a global survey reveal that 1) in at least one third of the cases the cloud liquid water sensitivity is negative, and the regional and seasonal variations of the negative liquid water sensitivity are consistent with other observations; 2) cloud droplet sizes are always inversely proportional to column droplet number concentrations. Our results suggest that an increase of cloud droplet number concentration leads to reduced cloud droplet size and enhanced evaporation, which weakens the coupling between water clouds and boundary layer in warm zones, decreases water supply from surface and desiccates cloud liquid water. Our results also suggest that the current evaluations of negative aerosol indirect forcing by global climate models (GCM), which are based on Twomey effect or Albrecht effect, may be overestimated.

  12. Impeded ice nucleation in glassy and highly viscous aerosol particles: the role of water diffusion

    NASA Astrophysics Data System (ADS)

    Marcolli, C.; Peter, T.; Zobrist, B.; Krieger, U. K.; Luo, B. P.; Soonsin, V.; Pedernera, D. A.; Koop, T.

    2010-05-01

    In situ and remote observations in the upper troposphere have disclosed the existence of water vapor pressures up to and even above water saturation. Under such conditions ice particle formation by homogeneous nucleation is expected to set in followed by ice crystal growth until the supersaturation is consumed. While the highest measured water vapor values might not withstand rigorous quality checks, values up to water saturation seem to be occurring. Since air masses appear to contain sufficient numbers of aerosol particles for cloud formation, the question arises why these aerosols are not successful at nucleating ice. The atmospheric aerosol is a complex mixture of various inorganic and organic components, whereas the organic fraction can represent more than 50% of the total aerosol mass. The homogeneous ice nucleation threshold was established for atmospherically relevant salt solutions and sulfuric acid, but only for a few organic species. The organic aerosol fraction tends to remain liquid instead of crystallizing as the temperature is decreased and, thus, organic aerosol particles may form highly viscous liquids. When the viscosity of such liquids reaches values in the order of 1012 Pa s, the molecular motion becomes so slow, that the sample vitrifies at the glass transition temperature Tg. If aerosol particles were present as glasses, this would influence several physical and chemical processes in the atmosphere significantly: Water uptake from the gas phase would be drastically impeded and ice nucleation inhibited. We investigated the glass transition temperature of a series of aqueous organic solutions such as polyols, sugars and dicarboxylic acids as a function of the solute concentration using a differential scanning calorimeter (DSC). These measurements show that the higher the molar mass of the organic solutes, the higher Tg of their respective solutions at a given water activity. Aerosol particles containing larger (≥150 g mol-1) organic molecules

  13. Is Every Transparent Liquid Water?

    NASA Astrophysics Data System (ADS)

    Hugerat, Muhamad; Basheer, Sobhi

    2001-08-01

    The accepted description for water in schools worldwide is a transparent and colorless liquid. Since students in lower grades (ages 8-13) often see warning signs "Do not drink this liquid--it is not water", we believe that presenting experiments that demonstrate the inadequacy of the accepted description for water would be beneficial for teachers and their students to practice in their schools. These activities provide simple experiments that introduce students to important characteristics of different compounds that have similar external appearance. The characteristics presented here include polarity, electric conductivity, color change due to presence of an acid-base indicator, and electrolysis.

  14. Effects of atmospheric dynamics and aerosols on the fraction of supercooled water clouds

    NASA Astrophysics Data System (ADS)

    Li, Jiming; Lv, Qiaoyi; Zhang, Min; Wang, Tianhe; Kawamoto, Kazuaki; Chen, Siyu; Zhang, Beidou

    2017-02-01

    Based on 8 years of (January 2008-December 2015) cloud phase information from the GCM-Oriented Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) Cloud Product (GOCCP), aerosol products from CALIPSO and meteorological parameters from the ERA-Interim products, the present study investigates the effects of atmospheric dynamics on the supercooled liquid cloud fraction (SCF) during nighttime under different aerosol loadings at global scale to better understand the conditions of supercooled liquid water gradually transforming to ice phase. Statistical results indicate that aerosols' effect on nucleation cannot fully explain all SCF changes, especially in those regions where aerosols' effect on nucleation is not a first-order influence (e.g., due to low ice nuclei aerosol frequency). By performing the temporal and spatial correlations between SCFs and different meteorological factors, this study presents specifically the relationship between SCF and different meteorological parameters under different aerosol loadings on a global scale. We find that the SCFs almost decrease with increasing of aerosol loading, and the SCF variation is closely related to the meteorological parameters but their temporal relationship is not stable and varies with the different regions, seasons and isotherm levels. Obviously negative temporal correlations between SCFs versus vertical velocity and relative humidity indicate that the higher vertical velocity and relative humidity the smaller SCFs. However, the patterns of temporal correlation for lower-tropospheric static stability, skin temperature and horizontal wind are relatively more complex than those of vertical velocity and humidity. For example, their close correlations are predominantly located in middle and high latitudes and vary with latitude or surface type. Although these statistical correlations have not been used to establish a certain causal relationship, our results may provide a unique point of view

  15. Tracking Water Diffusion Fronts in a Highly Viscous Aerosol Particle

    NASA Astrophysics Data System (ADS)

    Bastelberger, Sandra; Krieger, Ulrich; Peter, Thomas

    2016-04-01

    Field measurements indicate that atmospheric secondary aerosol particles can be present in a highly viscous, glassy state [1]. In contrast to liquid state particles, the gas phase equilibration is kinetically limited and governed by condensed phase diffusion. In recent water diffusion experiments on highly viscous single aerosol particles levitated in an electrodynamic balance (EDB) we observed a characteristic shift behavior of the Mie whispering gallery modes (WGM) indicative of the changing radial structure of the particle, thus providing us with an experimental method to track the diffusion process inside the particle. When a highly viscous, homogeneous particle is exposed to an abrupt increase in relative humidity, the rapid gas phase diffusion and strong concentration dependence of the diffusion coefficient in the condensed phase lead to extremely steep water concentration gradients inside the particle, reminiscent of diffusion fronts. The resulting quasi step-like concentration profile motivates the introduction of a simple core-shell model describing the morphology of the non-equilibrium particle during humidification. The subsequent particle growth and reduction of the shell refractive index can be observed as red and blueshift behavior of the WGM, respectively. The shift pattern can be attributed to a core-shell radius ratio and particle radius derived from model calculations [2]. If supplemented with growth information obtained from the WGM redshift and thermodynamic equilibrium data, we can infer a comprehensive picture of the time evolution of the diffusion fronts in the framework of our core-shell model. The measured time dependent concentration profile is then compared with simulations solving the non-linear diffusion equation [3] [1] Virtanen, A., et al., Nature, 467, 824-827, 2010 [2] Kaiser, T., Schweiger, G., Computers in Physics, Vol. 7, No. 6, 682-686, Nov/Dec 1993 [3] Zobrist, B., Soonsin, V., Luo, B.P., Peter, T. et al., Phys. Chem. Chem

  16. History of aerosol therapy: liquid nebulization to MDIs to DPIs.

    PubMed

    Anderson, Paula J

    2005-09-01

    Inhaled therapies have been used since ancient times and may have had their origins with the smoking of datura preparations in India 4,000 years ago. In the late 18th and in the 19th century, earthenware inhalers were popular for the inhalation of air drawn through infusions of plants and other ingredients. Atomizers and nebulizers were developed in the mid-1800s in France and were thought to be an outgrowth of the perfume industry as well as a response to the fashion of inhaling thermal waters at spas. Around the turn of the 20th century, combustible powders and cigarettes containing stramonium were popular for asthma and other lung complaints. Following the discovery of the utility of epinephrine for treating asthma, hand-bulb nebulizers were developed, as well as early compressor nebulizers. The marketing of the first pressurized metered-dose inhaler for epinephrine and isoproterenol, by Riker Laboratories in 1956, was a milestone in the development of inhaled drugs. There have been remarkable advances in the technology of devices and formulations for inhaled drugs in the past 50 years. These have been influenced greatly by scientific developments in several areas: theoretical modeling and indirect measures of lung deposition, particle sizing techniques and in vitro deposition studies, scintigraphic deposition studies, pharmacokinetics and pharmacodynamics, and the 1987 Montreal Protocol, which banned chlorofluorocarbon propellants. We are now in an era of rapid technologic progress in inhaled drug delivery and applications of aerosol science, with the use of the aerosolized route for drugs for systemic therapy and for gene replacement therapy, use of aerosolized antimicrobials and immunosuppressants, and interest in specific targeting of inhaled drugs.

  17. Water uptake of clay and desert dust aerosol particles at sub- and supersaturated water vapor conditions

    SciTech Connect

    Herich, Hanna; Tritscher, Torsten; Wiacek, Aldona; Gysel, Martin; Weingartner, E.; Lohmann, U.; Baltensperger, Urs; Cziczo, Daniel J.

    2009-11-01

    Airborne mineral dust particles serve as cloud condensation nuclei (CCN), thereby influencing the formation and properties of warm clouds. It is therefore of particular interest how dust aerosols with different mineralogy behave when exposed to high relative humidity (RH) or supersaturation with respect to liquid water similar to atmospheric conditions. In this study the sub-saturated hygroscopic growth and the supersaturated cloud condensation nucleus activity of pure clays and real desert dust aerosols was determined using a hygroscopicity tandem differential mobility analyzer (HTDMA) and a cloud condensation nuclei counter (CCNC), respectively. Five different illite, montmorillonite and kaolinite clay samples as well as three desert dust samples (Saharan dust (SD), Chinese dust (CD) and Arizona test dust (ATD)) were used. Aerosols were generated both with a wet and a dry disperser and the water uptake was parameterized via the hygroscopicity parameter, κ. The hygroscopicity of dry generated dust aerosols was found to be negligible when compared to processed atmospheric aerosols, with CCNC derived κ values between 0.00 and 0.02. The latter value can be idealized as a particle consisting of 96.7% (by volume) insoluble material and ~3.3% ammonium sulfate. Pure clay aerosols were found to be generally less hygroscopic than real desert dust particles. All illite and montmorillonite samples had κ~0.003, kaolinites were least hygroscopic and had κ=0.001. SD (κ=0.023) was found to be the most hygroscopic dry-generated desert dust followed by CD (κ=0.007) and ATD (κ=0.003). Wet-generated dust showed an increased water uptake when compared to dry-generated samples. This is considered to be an artifact introduced by redistribution of soluble material between the particles while immersed in an aqueous medium during atomization, thus indicating that specification of the generation method is critically important when presenting such data. Any atmospheric processing of

  18. Cloud water measurements of glyoxal and methylglyoxal during the Whistler Aerosol and Cloud Study (WACS)

    NASA Astrophysics Data System (ADS)

    Herckes, P.; Ervens, B.; Wang, Y.; Eagar, J.; Leaitch, R.; Macdonald, A.; Sjostedt, S.; Abbatt, J.

    2011-12-01

    Glyoxal and methylglyoxal are produced in high yields from both anthropogenic (aromatics) and biogenic (isoprene) precursors. The role of glyoxal and methylglyoxal in secondary organic aerosol (SOA) formation in the aqueous phase of cloud water and aerosols has received great attention over the past years. In addition, gas phase oxidation and photolysis of these compounds yield radicals and, thus, impact the oxidant budgets. While the reactivity of methylglyoxal and glyoxal in both the gas and aqueous phases is nearly identical, the much higher solubility of glyoxal leads to its more efficient removal in the presence of clouds. Thus, the amount of cloud water (liquid water content, LWC) and cloud processing time will affect the concentration ratios and thus the reaction rates of oxidation processes in the gas and aqueous phase, respectively. The Whistler Aerosol and Cloud Study (WACS) investigated the interactions between clouds and biogenic aerosol in summer 2010 in Whistler (Canada). During this study, cloud samples were collected at two locations, Whistler peak and a mid mountain station Raven's Nest. Cloud samples were extensively chemically characterized including the measurements of glyoxal and methylglyoxal using liquid chromatography coupled to UV and mass spectrometric detection after derivatization. Concentrations were variable on the order of micromoles, accounting for 1% of the dissolved organic matter in clouds. Glyoxal and methylglyoxal concentrations at both locations are predicted by means of model studies using VOC measurements and liquid water contents as input data. These concentrations and their ratios are compared to those in different regions. It will be discussed how cloud liquid water content, cloud processing time and amount and mixture of precursors (emissions) affect these concentration ratios. Finally, the role of different emission scenarios and the presence of clouds for SOA formation and radical budgets will be briefly assessed.

  19. Connecting Water Quality With Air Quality Through Microbial Aerosols

    NASA Astrophysics Data System (ADS)

    Dueker, M. Elias

    Aerosol production from surface waters results in the transfer of aquatic materials (including nutrients and bacteria) to air. These materials can then be transported by onshore winds to land, representing a biogeochemical connection between aquatic and terrestrial systems not normally considered. In urban waterfront environments, this transfer could result in emissions of pathogenic bacteria from contaminated waters. Despite the potential importance of this link, sources, near-shore deposition, identity and viability of microbial aerosols are largely uncharacterized. This dissertation focuses on the environmental and biological mechanisms that define this water-air connection, as a means to build our understanding of the biogeochemical, biogeographical, and public health implications of the transfer of surface water materials to the near-shore environment in both urban and non-urban environments. The effects of tidal height, wind speed and fog on coastal aerosols and microbial content were first quantified on a non-urban coast of Maine, USA. Culture-based, culture-independent, and molecular methods were used to simultaneously sample microbial aerosols while monitoring meteorological parameters. Aerosols at this site displayed clear marine influence and high concentrations of ecologically-relevant nutrients. Coarse aerosol concentrations significantly increased with tidal height, onshore wind speed, and fog presence. Tidal height and fog presence did not significantly influence total microbial aerosol concentrations, but did have a significant effect on culturable microbial aerosol fallout. Molecular analyses of the microbes settling out of near-shore aerosols provided further evidence of local ocean to terrestrial transport of microbes. Aerosol and surface ocean bacterial communities shared species and in general were dominated by organisms previously sampled in marine environments. Fog presence strengthened the microbial connection between water and land through

  20. Static heterogeneities in liquid water

    NASA Astrophysics Data System (ADS)

    Stanley, H. Eugene; Buldyrev, Sergey V.; Giovambattista, Nicolas

    2004-10-01

    The thermodynamic behavior of water seems to be closely related to static heterogeneities. These static heterogeneities are related to the local structure of water molecules, and when properly characterized, may offer an economical explanation of thermodynamic data. The key feature of liquid water is not so much that the existence of hydrogen bonds, first pointed out by Linus Pauling, but rather the local geometry of the liquid molecules is not spherical or oblong but tetrahedral. In the consideration of static heterogeneities, this local geometry is critical. Recent experiments suggested more than one phase of amorphous solid water, while simulations suggest that one of these phases is metastable with respect to another, so that in fact there are only two stable phases.

  1. Aircraft observations of water-soluble dicarboxylic acids in the aerosols over China

    NASA Astrophysics Data System (ADS)

    Zhang, Yan-Lin; Kawamura, Kimitaka; Qing Fu, Ping; Boreddy, Suresh K. R.; Watanabe, Tomomi; Hatakeyama, Shiro; Takami, Akinori; Wang, Wei

    2016-05-01

    Vertical profiles of dicarboxylic acids, related organic compounds and secondary organic aerosol (SOA) tracer compounds in particle phase have not yet been simultaneously explored in East Asia, although there is growing evidence that aqueous-phase oxidation of volatile organic compounds may be responsible for the elevated organic aerosols (OA) in the troposphere. Here, we found consistently good correlation of oxalic acid, the most abundant individual organic compounds in aerosols globally, with its precursors as well as biogenic-derived SOA compounds in Chinese tropospheric aerosols by aircraft measurements. Anthropogenically derived dicarboxylic acids (i.e., C5 and C6 diacids) at high altitudes were 4-20 times higher than those from surface measurements and even occasionally dominant over oxalic acid at altitudes higher than 2 km, which is in contrast to the predominance of oxalic acid previously reported globally including the tropospheric and surface aerosols. This indicates an enhancement of tropospheric SOA formation from anthropogenic precursors. Furthermore, oxalic acid-to-sulfate ratio maximized at altitudes of ˜ 2 km, explaining aqueous-phase SOA production that was supported by good correlations with predicted liquid water content, organic carbon and biogenic SOA tracers. These results demonstrate that elevated oxalic acid and related SOA compounds from both the anthropogenic and biogenic sources may substantially contribute to tropospheric OA burden over polluted regions of China, implying aerosol-associated climate effects and intercontinental transport.

  2. A spectroscopic tour through the liquid aerosol interface: Implications for atmospheric chemistry

    NASA Astrophysics Data System (ADS)

    Zhang, Jian-Xiang; Aiello, Denise; Aker, Pamela M.

    1994-12-01

    A novel nonlinear Raman spectroscopic technique has been used to image the extent of hydrogen bonding at water aerosol interfaces. The aerosols probed were generated in the laboratory using the vibrating orifice technique. The spectroscopic results show that the aerosols suffer severe hydrogen bond disruption and that the structural impairment is more pronounced at the surface. Laboratory aerosols generated this way do not mimic those found naturally. Thus mass accommodation coefficients measured using such aerosols should not be used in global climate modeling calculations.

  3. Adsorptive uptake of water by semisolid secondary organic aerosols

    NASA Astrophysics Data System (ADS)

    Pajunoja, Aki; Lambe, Andrew T.; Hakala, Jani; Rastak, Narges; Cummings, Molly J.; Brogan, James F.; Hao, Liqing; Paramonov, Mikhail; Hong, Juan; Prisle, Nønne L.; Malila, Jussi; Romakkaniemi, Sami; Lehtinen, Kari E. J.; Laaksonen, Ari; Kulmala, Markku; Massoli, Paola; Onasch, Timothy B.; Donahue, Neil M.; Riipinen, Ilona; Davidovits, Paul; Worsnop, Douglas R.; Petäjä, Tuukka; Virtanen, Annele

    2015-04-01

    Aerosol climate effects are intimately tied to interactions with water. Here we combine hygroscopicity measurements with direct observations about the phase of secondary organic aerosol (SOA) particles to show that water uptake by slightly oxygenated SOA is an adsorption-dominated process under subsaturated conditions, where low solubility inhibits water uptake until the humidity is high enough for dissolution to occur. This reconciles reported discrepancies in previous hygroscopicity closure studies. We demonstrate that the difference in SOA hygroscopic behavior in subsaturated and supersaturated conditions can lead to an effect up to about 30% in the direct aerosol forcing—highlighting the need to implement correct descriptions of these processes in atmospheric models. Obtaining closure across the water saturation point is therefore a critical issue for accurate climate modeling.

  4. Comparison of the water vapor and aerosol profiles

    NASA Astrophysics Data System (ADS)

    Penner, I. E.; Arshinov, M. Yu.; Balin, Yu. S.; Belan, B. D.; Voronin, B. A.; Kokhanenko, G. P.

    2014-11-01

    Analysis of the contents of water vapor and aerosol in the atmosphere measured by means of different instruments was performed based on the results of the comprehensive aerosol experiment carried out at the Institute of Atmospheric optics in May 2012. The data obtained using remote (lidar) and contact (balloon) methods were used. They are capable of obtaining the vertical profiles of the measured parameters with high spatial resolution. Lidar measurements of the water vapor content in the boundary layer of the atmosphere by Raman method have shown very good agreement with the data of measurements by balloon. Simultaneous lidar measurements of backscattering and mixing ratio of water vapor in the atmosphere give significant positive correlation of the contents of water vapor and aerosol in the layers.

  5. Comparison of activity coefficient models for atmospheric aerosols containing mixtures of electrolytes, organics, and water

    NASA Astrophysics Data System (ADS)

    Tong, Chinghang; Clegg, Simon L.; Seinfeld, John H.

    Atmospheric aerosols generally comprise a mixture of electrolytes, organic compounds, and water. Determining the gas-particle distribution of volatile compounds, including water, requires equilibrium or mass transfer calculations, at the heart of which are models for the activity coefficients of the particle-phase components. We evaluate here the performance of four recent activity coefficient models developed for electrolyte/organic/water mixtures typical of atmospheric aerosols. Two of the models, the CSB model [Clegg, S.L., Seinfeld, J.H., Brimblecombe, P., 2001. Thermodynamic modelling of aqueous aerosols containing electrolytes and dissolved organic compounds. Journal of Aerosol Science 32, 713-738] and the aerosol diameter dependent equilibrium model (ADDEM) [Topping, D.O., McFiggans, G.B., Coe, H., 2005. A curved multi-component aerosol hygroscopicity model framework: part 2—including organic compounds. Atmospheric Chemistry and Physics 5, 1223-1242] treat ion-water and organic-water interactions but do not include ion-organic interactions; these can be referred to as "decoupled" models. The other two models, reparameterized Ming and Russell model 2005 [Raatikainen, T., Laaksonen, A., 2005. Application of several activity coefficient models to water-organic-electrolyte aerosols of atmospheric interest. Atmospheric Chemistry and Physics 5, 2475-2495] and X-UNIFAC.3 [Erdakos, G.B., Change, E.I., Pandow, J.F., Seinfeld, J.H., 2006. Prediction of activity coefficients in liquid aerosol particles containing organic compounds, dissolved inorganic salts, and water—Part 3: Organic compounds, water, and ionic constituents by consideration of short-, mid-, and long-range effects using X-UNIFAC.3. Atmospheric Environment 40, 6437-6452], include ion-organic interactions; these are referred to as "coupled" models. We address the question—Does the inclusion of a treatment of ion-organic interactions substantially improve the performance of the coupled models over

  6. Liquid-liquid phase separation in aerosol particles: Imaging at the Nanometer Scale

    SciTech Connect

    O'Brien, Rachel; Wang, Bingbing; Kelly, Stephen T.; Lundt, Nils; You, Yuan; Bertram, Allan K.; Leone, Stephen R.; Laskin, Alexander; Gilles, Mary K.

    2015-04-21

    Atmospheric aerosols can undergo phase transitions including liquid-liquid phase separation (LLPS) while responding to changes in the ambient relative humidity (RH). Here, we report results of chemical imaging experiments using environmental scanning electron microscopy (ESEM) and scanning transmission x-ray microscopy (STXM) to investigate the LLPS of micron sized particles undergoing a full hydration-dehydration cycle. Internally mixed particles composed of ammonium sulfate (AS) and either: limonene secondary organic carbon (LSOC), a, 4-dihydroxy-3-methoxybenzeneaceticacid (HMMA), or polyethylene glycol (PEG-400) were studied. Events of LLPS with apparent core-shell particle morphology were observed for all samples with both techniques. Chemical imaging with STXM showed that both LSOC/AS and HMMA/AS particles were never homogeneously mixed for all measured RH’s above the deliquescence point and that the majority of the organic component was located in the shell. The shell composition was estimated as 65:35 organic: inorganic in LSOC/AS and as 50:50 organic: inorganic for HMMA/AS. PEG-400/AS particles showed fully homogeneous mixtures at high RH and phase separated below 89-92% RH with an estimated 50:50% organic to inorganic mix in the shell. These two chemical imaging techniques are well suited for in-situ analysis of the hygroscopic behavior, phase separation, and surface composition of collected ambient aerosol particles.

  7. Effects of long-range aerosol transport on the microphysical properties of low-level liquid clouds in the Arctic

    NASA Astrophysics Data System (ADS)

    Coopman, Quentin; Garrett, Timothy J.; Riedi, Jérôme; Eckhardt, Sabine; Stohl, Andreas

    2016-04-01

    The properties of low-level liquid clouds in the Arctic can be altered by long-range pollution transport to the region. Satellite, tracer transport model, and meteorological data sets are used here to determine a net aerosol-cloud interaction (ACInet) parameter that expresses the ratio of relative changes in cloud microphysical properties to relative variations in pollution concentrations while accounting for dry or wet scavenging of aerosols en route to the Arctic. For a period between 2008 and 2010, ACInet is calculated as a function of the cloud liquid water path, temperature, altitude, specific humidity, and lower tropospheric stability. For all data, ACInet averages 0.12 ± 0.02 for cloud-droplet effective radius and 0.16 ± 0.02 for cloud optical depth. It increases with specific humidity and lower tropospheric stability and is highest when pollution concentrations are low. Carefully controlling for meteorological conditions we find that the liquid water path of arctic clouds does not respond strongly to aerosols within pollution plumes. Or, not stratifying the data according to meteorological state can lead to artificially exaggerated calculations of the magnitude of the impacts of pollution on arctic clouds.

  8. THERMODYNAMIC MODELING OF LIQUID AEROSOLS CONTAINING DISSOLVED ORGANICS AND ELECTROLYTES

    EPA Science Inventory

    Many tropospheric aerosols contain large fractions of soluble organic material, believed to derive from the oxidation of precursors such alpha-pinene. The chemical composition of aerosol organic matter is complex and not yet fully understood.

    The key properties of solu...

  9. Infrared spectroscopy of sulfuric acid/water aerosols: Freezing characteristics

    NASA Astrophysics Data System (ADS)

    Clapp, M. L.; Niedziela, R. F.; Richwine, L. J.; Dransfield, T.; Miller, R. E.; Worsnop, D. R.

    1997-04-01

    A low-temperature flow cell has been used in conjunction with a Fourier transform infrared (FT-IR) spectrometer to study sulfuric acid/water aerosols. The aerosols were generated with a wide range of composition (28 to 85 wt%), including those characteristic of stratospheric sulfate aerosols, and studied over the temperature range from 240 K to 160 K. The particles exhibited deep supercooling, by as much as 100 K below the freezing point in some cases. Freezing of water ice was observed in the more dilute (<40 wt% sulfuric acid) particles, in agreement with the predictions of Jensen et al. and recent observations by Bertram et al. In contrast with theoretical predictions, however, the entire particle often does not immediately freeze, at least on the timescale of the present experiments (seconds to minutes). Freezing of the entire particle is observed at lower temperatures, well below that characteristic of the polar stratosphere.

  10. Water soluble organic constituents in Arctic aerosols and snow pack

    SciTech Connect

    Li, Shaomeng ); Winchester, J.W. )

    1993-01-08

    Eight water-soluble organic anions were measured in 70 aerosol samples and 10 snow samples at Barrow, Alaska in March-April, 1989. The ranking of the ions in aerosols according to total (coarse + fine aerosol) median concentrations was acetate (44 ng m[sup [minus]3]), oxalate (27), benzoate (23), formate (22), propionate (6), methanesulfonate (5), lactate (4), and pyruvate (4). When added up, the median organic anion mass was 156 ng m[sup [minus]3]. The organic anions/nssSO[sub 4][sup =] mass ratio had a median of 0.18 and 0.07 in the coarse (>1 [mu]m) and fine (<1 [mu]m) size fractions, respectively, but can be very high on occasions. On average, the organic anions made up more than 10% of the water-soluble aerosol mass. A similar ranking in concentration was also found for the organic ions in the snow pack samples. The organic anion/nssSO[sub 4][sup =] mass ratio in these samples was >0.5, substantially higher than in aerosols. 18 refs., 2 tabs.

  11. Modeling aerosol-water interactions in subsaturated and supersaturated environments

    NASA Astrophysics Data System (ADS)

    Fountoukis, Christos

    The current dissertation is motivated by the need for an improved understanding of aerosol - water interactions both in subsaturated and supersaturated atmospheric conditions with a strong emphasis on air pollution and climate change modeling. A cloud droplet formation parameterization was developed to (i) predict droplet formation from a lognormal representation of aerosol size distribution and composition, and, (ii) include a size-dependant mass transfer coefficient for the growth of water droplets which explicitly accounts for the impact of organics on droplet growth kinetics. The parameterization unravels most of the physics of droplet formation and is in remarkable agreement with detailed numerical parcel model simulations, even for low values of the accommodation coefficient. The parameterization offers a much needed rigorous and computationally inexpensive framework for directly linking complex chemical effects on aerosol activation in global climate models. The new aerosol activation parameterization was also tested against observations from highly polluted clouds (within the vicinity of power plant plumes). Remarkable closure was achieved (much less than the 20% measurement uncertainty). The error in predicted cloud droplet concentration was mostly sensitive to updraft velocity. Optimal closure is obtained if the water vapor uptake coefficient is equal to 0.06. These findings can serve as much needed constraints in modeling of aerosol-cloud interactions in the North America. Aerosol-water interactions in ambient relative humidities less than 100% were studied using a thermodynamic equilibrium model for inorganic aerosol and a three dimensional air quality model. We developed a new thermodynamic equilibrium model, ISORROPIA-II, which predicts the partitioning of semi-volatiles and the phase state of K+/Ca2+/M g2+ /NH4+/Na+/SO4 2-/NO3-/Cl-/H2O aerosols. A comprehensive evaluation of its performance was conducted over a wide range of atmospherically relevant

  12. Density Fluctuations in Liquid Water

    NASA Astrophysics Data System (ADS)

    English, Niall J.; Tse, John S.

    2011-01-01

    The density distributions and fluctuations in grids of varying size in liquid water at ambient pressure, both above the freezing point and in the supercooled state, are analyzed from the trajectories obtained from large-scale molecular dynamics simulations. It is found that the occurrence of low- and high-density regions (LDL and HDL) is transient and their respective residence times are dependent on the size of the simulated system. The spatial extent of density-density correlation is found to be within 7 Å or less. The temporal existence of LDL and HDL arises as a result of natural density fluctuations of an equilibrium system. The density of bulk water at ambient conditions is homogenous.

  13. Geomorphologic evidence for liquid water

    USGS Publications Warehouse

    Masson, P.; Carr, M.H.; Costard, F.; Greeley, R.; Hauber, E.; Jaumann, R.

    2001-01-01

    Besides Earth, Mars is the only planet with a record of resurfacing processes and environmental circumstances that indicate the past operation of a hydrologic cycle. However the present-day conditions on Mars are far apart of supporting liquid water on the surface. Although the large-scale morphology of the Martian channels and valleys show remarkable similarities with fluid-eroded features on Earth, there are major differences in their size, small-scale morphology, inner channel structure and source regions indicating that the erosion on Mars has its own characteristic genesis and evolution. The different landforms related to fluvial, glacial and periglacial activities, their relations with volcanism, and the chronology of water-related processes, are presented.

  14. Molecular dynamics simulations of the water adsorption around malonic acid aerosol models.

    PubMed

    Darvas, Maria; Picaud, Sylvain; Jedlovszky, Pál

    2013-07-14

    Water nucleation around a malonic acid aggregate has been studied by means of molecular dynamics simulations in the temperature and pressure range relevant for atmospheric conditions. Systems of different water contents have been considered and a large number of simulations have allowed us to determine the phase diagram of the corresponding binary malonic acid-water systems. Two phases have been evidenced in the phase diagrams corresponding either to water adsorption on a large malonic acid grain at low temperatures, or to the formation of a liquid-like mixed aggregate of the two types of molecules, at higher temperatures. Finally, the comparison between the phase diagrams simulated for malonic acid-water and oxalic acid-water mixtures emphasizes the influence of the O : C ratio on the hydrophilic behavior of the aerosol, and thus on its ability to act as a cloud condensation nucleus, in accordance with recent experimental conclusions.

  15. Liquid-liquid phase separation in atmospheric aerosol particles: dependence on organic functionalities and mixture complexity

    NASA Astrophysics Data System (ADS)

    Song, M.; Marcolli, C.; Krieger, U. K.; Zuend, A.; Peter, T.

    2012-04-01

    In the troposphere, aerosol particles undergo phase transitions such as deliquescence and efflorescence during humidity cycles (Marcolli and Krieger, 2006). In addition, interactions between organic and inorganic compounds lead to liquid-liquid phase separation (LLPS) (Ciobanu et al., 2009). Recent studies on a limited number of model systems have shown that oxygen-to-carbon ratios (O:C) of the organic aerosol fraction might be a good predictor for LLPS in mixed organic/ammonium sulfate (AS) particles (Bertram et al., 2011; Song et al., 2011). However, in order to corroborate this hypothesis experiments with an organic fraction that consists of a higher number of components with different O:C ratios and functional groups are needed. In order to determine the influence of O:C ratio, the specific organic functionalities and the mixture complexity on LLPS, we subjected organic/AS particles deposited on a hydrophobically coated substrate to relative humidity (RH) cycles and observed phase changes using optical microscopy and micro-Raman spectroscopy. To determine the influence of mixture complexity, we mixed together up to 10 organic compounds. We also prepared mixtures that were rich in different types of functional groups like polyols, aromatics and dicarboxylic acids which were identified from field measurements. We screened for a miscibility gap by varying the organic-to-inorganic ratio from 2:1 to 1:6. AS in the investigated single particles effloresced at 27 - 50 %RH and deliquesced at 72 - 79 %RH during humidity cycles. The occurrence of LLPS is determined to a high degree by the O:C of the organics: there was no LLPS for mixtures with O:C > 0.8 and there was always LLPS for mixtures with O:C < 0.57. In the range in between, we observed a dependence on the specific functional groups: a high share of aromatic functionalities shifts the range of O:C for which LLPS occurs to lower values. A correlation was also found for the onset RH of LLPS as a function of O

  16. Depolarization of water in protic ionic liquids.

    PubMed

    Zahn, Stefan; Wendler, Katharina; Delle Site, Luigi; Kirchner, Barbara

    2011-09-07

    A mixture of the protic ionic liquid mono-methylammonium nitrate with 1.6 wt% water was investigated from Car-Parrinello molecular dynamics simulations. In contrast to imidazolium-based ionic liquids, the cation possesses strong directional hydrogen bonds to water and all hydrogen bonds in the mixture have a comparable strength. This results in a good incorporation of water into the hydrogen bond network of mono-methylammonium nitrate and a tetrahedral hydrogen bond coordination of water. Hence, one might expect a larger dipole moment of water in the investigated mixture compared to neat water due to the good hydrogen bond network incorporation and the charged vicinity of water in the protic ionic liquid. However, the opposite is observed pointing to strong electrostatic screening in protic ionic liquids. Additionally, the influence of water on the properties of the protic ionic liquid is discussed.

  17. CRISM Limb Observations of Aerosols and Water Vapor

    NASA Technical Reports Server (NTRS)

    Smith, Michael D.; Wolff, M.J.; Clancy, R.T.; Seelos, F.; Murchie, S.L.

    2009-01-01

    Near-infrared spectra taken in a limb-viewing geometry by the Compact Reconnaissance Imaging Spectrometer for Mars (CRISM) on-board the Mars Reconnaissance Orbiter (MRO) provide a useful tool for probing atmospheric structure. Here we describe preliminary work on the retrieval of vertical profiles of aerosols and water vapor from the CRISM limb observations. The first full set of CRISM limb observations was taken in July 2009, with subsequent limb observations planned once every two months. Each set of limb observations contains about four dozen scans across the limb giving pole-to-pole coverage for two orbits at roughly 100 and 290 W longitude. Radiative transfer modeling taking account of aerosol scattering in the limb-viewing geometry is used to model the observations. The retrievals show the height to which dust and water vapor extend and the location and height of water ice clouds. Results from the First set of CRISM limb observations (July 2009, Ls=300) show dust aerosol well-mixed to about three scale heights above the surface with thin water ice clouds above the dust near the equator and at mid-northern latitudes. Water vapor is concentrated at high southern latitudes.

  18. Mass Spectrometry of Liquid Aniline Aerosol Particles by IR/UV Laser Irradiation.

    PubMed

    Zelenyuk, A; Cabalo, J; Baer, T; Miller, R E

    1999-05-01

    The first results are reported from a new single-particle two-color laser time-of-flight mass spectrometer, incorporating a combination of infrared (CO(2)) and UV (excimer) laser irradiation. This combination of lasers has the capability to effectively separate the desorption or evaporation step from the ionization step, thereby greatly improving the analytical capabilities of such an instrument. The results on liquid aerosols, such as aniline, show that prior evaporation of the aerosol particle with the IR laser increases the ion signal produced by the excimer laser by more than 2 orders of magnitude. In the case of nitrobenzene aerosols, the excimer laser alone produces no ions, while a very large signal is observed when the aerosol is first irradiated with the CO(2) laser. A simple model, based on the Coulomb explosion of the ionized aerosol, is used to estimate the number of ions generated by the excimer laser (∼10(5) ions). Experimental evidence based on the observed time delay of protonated aniline parent ions indicates that the laser irradiation of the liquid aerosol results in a stable neutral plasma which separates into positive and negative charges only after a 100-500-ns delay.

  19. 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 ...

  20. Seasonal differences in aerosol water may reconcile AOT and surface mass measurements in the Southeast U.S.

    NASA Astrophysics Data System (ADS)

    Nguyen, T. K. V.; Ghate, V. P.; Carlton, A. M. G.

    2015-12-01

    Summertime aerosol optical thickness (AOT) in the Southeast U.S. is high and sharply enhanced (2-3 times) compared to wintertime AOT. This seasonal pattern is unique to the Southeast U.S. and is of particular interest because temperatures there have not warmed over the past 100 years, contrasting with trends in other U.S. regions. Some investigators hypothesize the Southeast temperature trend is due to secondary organic aerosols (SOA) formed from interactions of biogenic volatile organic compounds (BVOCs) and anthropogenic emissions that create a cooling haze. However, aerosol measurements made at the surface do not exhibit strong seasonal differences in mass or organic fraction to support this hypothesis. In this work, we attempt to reconcile the spatial and temporal distribution of AOT over the U.S. with surface mass measurements by examining trends in particle-phase liquid water, an aerosol constituent that effectively scatters radiation and is removed from aerosols in mass measurements at routine surface monitoring sites. We employ the thermodynamic model ISORROPIA (v2.1) to estimate surface and aloft aerosol water mass concentrations at locations of Interagency Monitoring of Protected Visual Environments (IMPROVE) sites using measured speciated ion mass concentrations and NCEP North American Regional Reanalysis (NARR) meteorological data. Results demonstrate strong seasonal differences in aerosol water in the eastern compared to the western part of the U.S., consistent with geographic patterns in AOT. The highest mean regional seasonal difference from 2000 to 2007 is 5.5 μg m-3 and occurs the Southeast, while the lowest is 0.44 μg m-3 and occurs in the dry Mountain West. Our findings suggest 1) similarity between spatial trends in aerosol water in the U.S. and previously published AOT data from the MODIS-TERRA instrument and 2) similar interannual trends in mean aerosol water and previously published interannual AOT trends from MISR, MODIS-TERRA, MODIS

  1. Water Activity Limits the Hygroscopic Growth Factor of Organic Aerosols

    NASA Astrophysics Data System (ADS)

    Rodriguez, L. I.; Cabrera, J. A.; Golden, D.; Tabazadeh, A.

    2007-12-01

    In this work we study the hygroscopic behavior of organic aerosols, which has important implications for Earth's climate. The hygroscopic growth factor (HGF) is defined as the ratio of the diameter of a spherical particle when it is exposed to dry conditions to that at humid conditions. We present a new formulation to express the HGF of an aerosol particle as a function of water activity (aw) in the aqueous phase. This new formulation matches reported HGFs for common inorganic salts and water-miscible organic particles that are known to deliquesce into aqueous drops at high relative humidities (RH). Many studies use tandem differential mobility analyzers (TDMA) to determine the HGF of organic aerosols. For example, Brooks et al. used a TDMA to measure a HGF of 1.2 for 2 μm phthalic acid (PA) particles at 90% RH (aw= 0.9). However, water activity limits the growth of a particle that can be attributed to water uptake. We have assembled a vapor pressure apparatus to measure aw of aqueous solutions at room temperature. Measured water activities for PA, used in our growth formulation, yield a HGF of ~ 1.0005 for 2 μm PA particles at 90% RH. Comparing our results against Brooks et al. suggests that TDMA experiments may grossly overestimate the HGF of PA particles since water activity limits this growth to below 1.0005. Alternatively, we suggest that the adsorption of a negligible mass of water by a highly porous PA particle can lead to an apparent growth in particle size by changing its morphology. Other studies also use TDMAs to measure HGFs of secondary organic aerosols (SOAs). HGFs reported for SOAs are very similar to PA, suggesting that the observed growth may be due to morphological changes in particle size rather than water uptake as commonly assumed. We built a smog chamber where an organic precursor, such as d-limonene, reacts with nitrogen oxides under UV radiation to produce SOAs. We compare the HGFs for SOAs obtained with our method to those obtained with

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  3. Dipolar correlations in liquid water

    SciTech Connect

    Zhang, Cui; Galli, Giulia

    2014-08-28

    We present an analysis of the dipolar correlations in water as a function of temperature and density and in the presence of simple ionic solutes, carried out using molecular dynamics simulations and empirical potentials. We show that the dipole-dipole correlation function of the liquid exhibits sizable oscillations over nanodomains of about 1.5 nm radius, with several isosbestic points as a function of temperature; the size of the nanodomains is nearly independent on temperature and density, between 240 and 400 K and 0.9 and 1.3 g/cm{sup 3}, but it is substantially affected by the presence of solvated ions. In the same range of thermodynamic conditions, the decay time (τ) of the system dipole moment varies by a factor of about 30 and 1.5, as a function of temperature and density, respectively. At 300 K, we observed a maximum in τ as a function of density, and a corresponding shallow maximum in the tetrahedral order parameter, in a range where the diffusion coefficient, the pressure and the dielectric constant increase monotonically.

  4. Water Uptake and Hygroscopic Growth of Organosulfate Aerosol.

    PubMed

    Estillore, Armando D; Hettiyadura, Anusha P S; Qin, Zhen; Leckrone, Erin; Wombacher, Becky; Humphry, Tim; Stone, Elizabeth A; Grassian, Vicki H

    2016-04-19

    Organosulfates (OS) are important components of secondary organic aerosol (SOA) that have been identified in numerous field studies. This class of compounds within SOA can potentially affect aerosol physicochemical properties such as hygroscopicity because of their polar and hydrophilic nature as well as their low volatility. Currently, there is a dearth of information on how aerosol particles that contain OS interact with water vapor in the atmosphere. Herein we report a laboratory investigation on the hygroscopic properties of a structurally diverse set of OS salts at varying relative humidity (RH) using a Hygroscopicity-Tandem Differential Mobility Analyzer (H-TDMA). The OS studied include the potassium salts of glycolic acid sulfate, hydroxyacetone sulfate, 4-hydroxy-2,3-epoxybutane sulfate, and 2-butenediol sulfate and the sodium salts of benzyl sulfate, methyl sulfate, ethyl sulfate, and propyl sulfate. In addition, mixtures of OS and sodium chloride were also studied. The results showed gradual deliquescence of these aerosol particles characterized by continuous uptake and evaporation of water in both hydration and dehydration processes for the OS, while the mixture showed prompt deliquescence and effloresce transitions, albeit at a lower relative humidity relative to pure sodium chloride. Hygroscopic growth of these OS at 85% RH were also fit to parameterized functional forms. This new information provided here has important implications about the atmospheric lifetime, light scattering properties, and the role of OS in cloud formation. Moreover, results of these studies can ultimately serve as a basis for the development and evaluation of thermodynamic models for these compounds in order to consider their impact on the atmosphere.

  5. On the Physics of Fizziness: How liquid properties control bursting bubble aerosol production?

    NASA Astrophysics Data System (ADS)

    Ghabache, Elisabeth; Antkowiak, Arnaud; Josserand, Christophe; Seon, Thomas

    2014-11-01

    Either in a champagne glass or at the oceanic scales, the tiny capillary bubbles rising at the surface burst in ejecting myriads of droplets. Focusing on the ejected droplets produced by a single bubble, we investigate experimentally how liquid properties and bubble size affect their characteristics: number, ejection velocities, sizes and ejection heights. These results allow us to finely tune the bursting bubble aerosol production. In the context of champagne industry, aerosols play a major role by spreading wine aroma above the glass. We demonstrate that this champagne fizz can be enhanced by selecting the wine viscosity and the bubble size, thanks to specially designed glass.

  6. Removal of Sarin Aerosol and Vapor by Water Sprays

    SciTech Connect

    Brockmann, John E.

    1998-09-01

    Falling water drops can collect particles and soluble or reactive vapor from the gas through which they fall. Rain is known to remove particles and vapors by the process of rainout. Water sprays can be used to remove radioactive aerosol from the atmosphere of a nuclear reactor containment building. There is a potential for water sprays to be used as a mitigation technique to remove chemical or bio- logical agents from the air. This paper is a quick-look at water spray removal. It is not definitive but rather provides a reasonable basic model for particle and gas removal and presents an example calcu- lation of sarin removal from a BART station. This work ~ a starting point and the results indicate that further modeling and exploration of additional mechanisms for particle and vapor removal may prove beneficial.

  7. 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.

  8. Combined Dial Sounding of Ozone, Water Vapour and Aerosol

    NASA Astrophysics Data System (ADS)

    Trickl, Thomas; Vogelmann, Hannes

    2016-06-01

    Routine high-quality lidar measurements of ozone, water vapour and aerosol at Garmisch-Partenkirchen since 2007 have made possible more comprehensive atmospheric studies and lead to a growing insight concerning the most frequently occurring long-range transport pathways. In this contribution we present as examples results on stratospheric layers travelling in the free troposphere for extended periods of time without eroding. In particular, we present a case of an intrusion layer that subsided over as many as fifteen days and survived the interference by strong Canadian fires. These results impose a challenge on atmospheric modelling that grossly overestimates free-tropospheric mixing.

  9. Photoresponsive liquid marbles and dry water.

    PubMed

    Tan, Tristan Tsai Yuan; Ahsan, Aniq; Reithofer, Michael R; Tay, Siok Wei; Tan, Sze Yu; Hor, Tzi Sum Andy; Chin, Jia Min; Chew, Benny Kia Jia; Wang, Xiaobai

    2014-04-01

    Stimuli-responsive liquid marbles for controlled release typically rely on organic moieties that require lengthy syntheses. We report herein a facile, one-step synthesis of hydrophobic and oleophobic TiO2 nanoparticles that display photoresponsive wettability. Water liquid marbles stabilized by these photoresponsive TiO2 particles were found to be stable when shielded from ultraviolet (UV) radiation; however, they quickly collapsed after being irradiated with 302 nm UV light. Oil- and organic-solvent-based liquid marbles could also be fabricated using oleophobic TiO2 nanoparticles and show similar UV-induced collapse. Finally, we demonstrated the formation of the micronized form of water liquid marbles, also known as dry water, by homogenization of the TiO2 nanoparticles with water. The TiO2 dry water displayed a similar photoresponse, whereby the micronized liquid marbles collapsed after irradiation and the dry water turned from a free-flowing powder to a paste. Hence, by exploiting the photoresponsive wettability of TiO2, we fabricated liquid marbles and dry water that display photoresponse and studied the conditions required for their collapse.

  10. Global Cloud Liquid Water Path Simulations(.

    NASA Astrophysics Data System (ADS)

    Lemus, Lilia; Rikus, Lawrie; Martin, C.; Platt, R.

    1997-01-01

    A new parameterization of cloud liquid water and ice content has been included in the Bureau of Meteorology Global Assimilation and Prediction System. The cloud liquid water content is derived from the mean cloud temperatures in the model using an empirical relationship based on observations. The results from perpetual January and July simulations are presented and show that the total cloud water path steadily decreases toward high latitudes, with two relative maxima at midlatitudes and a peak at low latitudes. To validate the scheme, the simulated fields need to be processed to produce liquid water paths that can be directly compared with the corresponding field derived from Special Sensor Microwave/Imager (SSM/I) data. This requires the identification of cloud ice water content within the parameterization and a prescription to account for the treatment of strongly precipitating subgrid-scale cloud. The resultant cloud liquid water paths agree qualitatively with the SSM/I data but show some systematic errors that are attributed to corresponding errors in the model's simulation of cloud amounts. Given that a more quantitative validation requires substantial improvement in the model's diagnostic cloud scheme, the comparison with the SSM/I data indicates that the cloud water path, derived from the cloud liquid water content parameterization introduced in this paper, is consistent with the observations and can be usefully incorporated in the prediction system.

  11. Are There Two Forms of Liquid Water?

    NASA Astrophysics Data System (ADS)

    Stanley, H. E.

    We will introduce some of the 73 documented anomalies of the most complex of liquids, water--focusing on recent progress in understanding these anomalies by combining information provided by recent experiments and simulations on water in bulk, nanoconfined and biological environments designed to test the hypothesis that liquid water has behavior consistent with the novel phenomenon of ``liquid polymorphism'' in that water can exist in two distinct phases [1]. We will also discuss very recent work on nanoconfined water anomalies as well as the apparently related, and highly unusual, behavior of water in biological environments. Finally, we will discuss how the general concept of liquid polymorphism is proving useful in understanding anomalies in other liquids, such as silicon, silica, and carbon, as well as metallic glasses, which have in common that they are characterized by two characteristic length scales in their interactions.This work has been supported by the NSF Chemistry Division grant CHE-1213217 and was performed in collaboration with, among others, C. A. Angell, S. V. Buldyrev, S.-H. Chen, D. Corradini, P. G. Debenedetti, G. Franzese, P. Kumar, E. Lascaris, F. Mallamace, O. Mishima, P. H. Poole, S. Sastry, F. Sciortino, and L. Xu. H. E. Stanley, Editor, Liquid Polymorphism, Vol. 152 in Advances in Chemical Physics, S. A. Rice, Series Editor (Wiley, New York, 2013).

  12. Interfaces Select Specific Stereochemical Conformations: The Isomerization of Glyoxal at the Liquid Water Interface.

    PubMed

    Zhu, Chongqin; Kais, Sabre; Zeng, Xiao Cheng; Francisco, Joseph S; Gladich, Ivan

    2017-01-11

    Interfacial chemistry involving glyoxal at aerosol surfaces is postulated to catalyze aerosol growth. This chemistry remains speculative due to a lack of detailed information concerning the physicochemical behavior of glyoxal at the interface of atmospheric aerosols. Here, we report results from high-level electronic structure calculations as well as both classical and Born-Oppenheimer ab initio molecular dynamics simulations of glyoxal solvation at the air/liquid water interface. When compared to the gas phase, the trans to cis isomerization of glyoxal at the liquid water interface is found to be catalyzed; additionally, the trans conformation is selectively solvated within the bulk to a greater degree than is the cis conformation. These two processes, i.e., the catalytic effect at the water interface and the differentially selective solvation, act to enhance the concentration of the cis isomer of glyoxal at the water interface. This has important consequences for the interpretation of experiments and for the modeling of glyoxal chemistry both at the interface of water clouds and at aerosols. Broader implications of this work relate to describing the role of interfaces in selecting specific stereo molecular structures at interfacial environments.

  13. Self-assembly of new surface active ionic liquids based on Aerosol-OT in aqueous media.

    PubMed

    Rao, K Srinivasa; Gehlot, Praveen Singh; Trivedi, Tushar J; Kumar, Arvind

    2014-08-15

    New anionic ionic liquid surfactants have been synthesized by replacing the sodium cation of Aerosol-OT (sodium dioctylsulfosuccinate, [Na]AOT) with various biocompatible moieties, such as 1-butyl-3-methyl imidazolium ([C4mim]), proliniumisopropylester ([ProC3]), cholinium ([Cho]), and guanidinium ([Gua]). The Aerosol-OT derived ionic liquids (AOT-ILs) were found fairly soluble in water and formed vesicles above a critical vesicle concentration (CVC) which depended upon the nature of cation, and followed the order: [ProC3]<[C4mim]<[Gua]<[Cho]liquids. All the AOT-ILs were found fairly soluble in the hydrophilic IL, ethanolammonium formate (EOAF), whereas only [C4mim]AOT and [ProC3]AOT were found soluble in hydrophobic IL, [C4mim]Tf2N. Such combinations can have potential for construction of stable colloidal formulations or microemulsions in ionic liquid media.

  14. Light water reactor aerosol containment experiment LA4 simulated by JERICHO and AEROSOLS-B2 codes

    SciTech Connect

    Passalacqua, R.; Tarabelli, D.; Renault, C.

    1996-12-01

    Large-scale experiments show that whenever a loss of coolant accident occurs water pools are generated. Stratification of steam-saturated gas develops above growing water pools causing a different thermal hydraulics in the subcompartment where the water pool is located. Hereafter, the LWR Aerosols Containment Experiment (LACE) LA4 experiment, performed at the Hanford Engineering Development Laboratory, will be studied; this experiment exhibited a strong stratification, at all times, above a growing wade pool. JERICHO and AEROSOLS-B2 are part of the Ensemble de Systemes de Codes d`Analyse d`Accident des Reacteurs a Eau (ESCADRE) code system, a tool for evaluating the response of a nuclear plant to severe accidents. These two codes are used here to simulate respectively the thermal hydraulics and the associated aerosol behavior. Code results have shown that modeling large containment thermal hydraulics without taking into account the stratification phenomenon leads to large overpredictions of containment pressure and temperature. If the stratification, above the water pool, is modeled as a zone with a higher steam condensation rate and a higher thermal resistance (that is acting as a barrier to heat exchanges with the upper and larger compartment), ESCADRE predictions match experimental data quite well. The stratification region is believed to be able to affect aerosol behavior; aerosol settling is improved by steam condensation on particles and by diffusiophoresis and thermophoresis. In addition, the lower aerosol concentration throughout the stratification might cause a nonnegligible aerosol concentration gradient and consequently a driving force for the motion of smaller particles toward the pool.

  15. Properties of Water Confined in Ionic Liquids

    PubMed Central

    Saihara, Koji; Yoshimura, Yukihiro; Ohta, Soichi; Shimizu, Akio

    2015-01-01

    The varying states of water confined in the nano-domain structures of typical room temperature ionic liquids (ILs) were investigated by 1H NMR and by measurements of self-diffusion coefficients while systematically varying the IL cations and anions. The NMR peaks for water in BF4-based ILs were clearly split, indicating the presence of two discrete states of confined water (H2O and HOD). Proton and/or deuterium exchange rate among the water molecules was very slowly in the water-pocket. Notably, no significant changes were observed in the chemical shifts of the ILs. Self-diffusion coefficient results showed that water molecules exhibit a similar degree of mobility, although their diffusion rate is one order of magnitude faster than that of the IL cations and anions. These findings provide information on a completely new type of confinement, that of liquid water in soft matter. PMID:26024339

  16. Liquid chromatographic determination of water

    DOEpatents

    Fortier, Nancy E.; Fritz, James S.

    1990-11-13

    A sensitive method for the determination of water in the presence of common interferences is presented. The detection system is based on the effect of water on the equilibrium which results from the reaction aryl aldehydes, such as cinnamaldehyde and methanol in the eluent to form cinnamaldehyde dimethylacetal, plus water. This equilibrium is shifted in a catalytic atmosphere of a hydrogen ion form past column reactor. The extent of the shift and the resulting change in absorbance are proportional to the amount of water present.

  17. Liquid chromatographic determination of water

    DOEpatents

    Fortier, N.E.; Fritz, J.S.

    1990-11-13

    A sensitive method for the determination of water in the presence of common interferences is presented. The detection system is based on the effect of water on the equilibrium which results from the reaction aryl aldehydes, such as cinnamaldehyde and methanol in the eluent to form cinnamaldehyde dimethylacetal, plus water. This equilibrium is shifted in a catalytic atmosphere of a hydrogen ion form past column reactor. The extent of the shift and the resulting change in absorbance are proportional to the amount of water present. 1 fig.

  18. Liquid Water Oceans in Ice Giants

    NASA Technical Reports Server (NTRS)

    Wiktorowicz, Sloane J.; Ingersoll, Andrew P.

    2007-01-01

    Aptly named, ice giants such as Uranus and Neptune contain significant amounts of water. While this water cannot be present near the cloud tops, it must be abundant in the deep interior. We investigate the likelihood of a liquid water ocean existing in the hydrogen-rich region between the cloud tops and deep interior. Starting from an assumed temperature at a given upper tropospheric pressure (the photosphere), we follow a moist adiabat downward. The mixing ratio of water to hydrogen in the gas phase is small in the photosphere and increases with depth. The mixing ratio in the condensed phase is near unity in the photosphere and decreases with depth; this gives two possible outcomes. If at some pressure level the mixing ratio of water in the gas phase is equal to that in the deep interior, then that level is the cloud base. The gas below the cloud base has constant mixing ratio. Alternately, if the mixing ratio of water in the condensed phase reaches that in the deep interior, then the surface of a liquid ocean will occur. Below this ocean surface, the mixing ratio of water will be constant. A cloud base occurs when the photospheric temperature is high. For a family of ice giants with different photospheric temperatures, the cooler ice giants will have warmer cloud bases. For an ice giant with a cool enough photospheric temperature, the cloud base will exist at the critical temperature. For still cooler ice giants, ocean surfaces will result. A high mixing ratio of water in the deep interior favors a liquid ocean. We find that Neptune is both too warm (photospheric temperature too high) and too dry (mixing ratio of water in the deep interior too low) for liquid oceans to exist at present. To have a liquid ocean, Neptune s deep interior water to gas ratio would have to be higher than current models allow, and the density at 19 kbar would have to be approx. equal to 0.8 g/cu cm. Such a high density is inconsistent with gravitational data obtained during the Voyager

  19. Modeling aerosol water uptake in the arctic based on the κ-Kohler theory

    NASA Astrophysics Data System (ADS)

    Rastak, N.; Ekman, A.; Silvergren, S.; Zieger, P.; Wideqvist, U.; Ström, J.; Svenningsson, B.; Tunved, P.; Riipinen, I.

    2013-05-01

    Water uptake or hygroscopicity is one of the most fundamental properties of atmospheric aerosols. Aerosol particles containing soluble materials can grow in size by absorbing water in ambient atmosphere. This property is measured by a parameter known as growth factor (GF), which is defined as the ratio of the wet diameter to the dry diameter. Hygroscopicity controls the size of an aerosol particle and therefore its optical properties in the atmosphere. Hygroscopic growth depends on the dry size of the particle, its chemical composition and the relative humidity in the ambient air (Fitzgerald, 1975; Pilinis et al., 1995). One of the typical problems in aerosol studies is the lack of measurements of aerosol size distributions and optical properties in ambient conditions. The gap between dry measurements and the real humid atmosphere is filled in this study by utilizing a hygroscopic model which calculates the hygroscopic growth of aerosol particles at Mt Zeppelin station, Ny Ålesund, Svalbard during 2008.

  20. 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.

  1. Aerosol generation and characterization of multi-walled carbon nanotubes exposed to cells cultured at the air-liquid interface.

    PubMed

    Polk, William W; Sharma, Monita; Sayes, Christie M; Hotchkiss, Jon A; Clippinger, Amy J

    2016-04-23

    Aerosol generation and characterization are critical components in the assessment of the inhalation hazards of engineered nanomaterials (NMs). An extensive review was conducted on aerosol generation and exposure apparatus as part of an international expert workshop convened to discuss the design of an in vitro testing strategy to assess pulmonary toxicity following exposure to aerosolized particles. More specifically, this workshop focused on the design of an in vitro method to predict the development of pulmonary fibrosis in humans following exposure to multi-walled carbon nanotubes (MWCNTs). Aerosol generators, for dry or liquid particle suspension aerosolization, and exposure chambers, including both commercially available systems and those developed by independent researchers, were evaluated. Additionally, characterization methods that can be used and the time points at which characterization can be conducted in order to interpret in vitro exposure results were assessed. Summarized below is the information presented and discussed regarding the relevance of various aerosol generation and characterization techniques specific to aerosolized MWCNTs exposed to cells cultured at the air-liquid interface (ALI). The generation of MWCNT aerosols relevant to human exposures and their characterization throughout exposure in an ALI system is critical for extrapolation of in vitro results to toxicological outcomes in humans.

  2. Water Contaminant Mitigation in Ionic Liquid Propellant

    NASA Technical Reports Server (NTRS)

    Conroy, David; Ziemer, John

    2009-01-01

    Appropriate system and operational requirements are needed in order to ensure mission success without unnecessary cost. Purity requirements applied to thruster propellants may flow down to materials and operations as well as the propellant preparation itself. Colloid electrospray thrusters function by applying a large potential to a room temperature liquid propellant (such as an ionic liquid), inducing formation of a Taylor cone. Ions and droplets are ejected from the Taylor cone and accelerated through a strong electric field. Electrospray thrusters are highly efficient, precise, scaleable, and demonstrate low thrust noise. Ionic liquid propellants have excellent properties for use as electrospray propellants, but can be hampered by impurities, owing to their solvent capabilities. Of foremost concern is the water content, which can result from exposure to atmosphere. Even hydrophobic ionic liquids have been shown to absorb water from the air. In order to mitigate the risks of bubble formation in feed systems caused by water content of the ionic liquid propellant, physical properties of the ionic liquid EMI-Im are analyzed. The effects of surface tension, material wetting, physisorption, and geometric details of the flow manifold and electrospray emitters are explored. Results are compared to laboratory test data.

  3. An automated analyzer to measure surface-atmosphere exchange fluxes of water soluble inorganic aerosol compounds and reactive trace gases.

    PubMed

    Thomas, Rick M; Trebs, Ivonne; Otjes, René; Jongejan, Piet A C; Ten Brink, Harry; Phillips, Gavin; Kortner, Michael; Meixner, Franz X; Nemitz, Eiko

    2009-03-01

    Here, we present a new automated instrument for semicontinuous gradient measurements of water-soluble reactive trace gas species (NH3, HNO3, HONO, HCl, and SO2) and their related aerosol compounds (NH4+, NO3-, Cl-, SO4(2-)). Gas and aerosol samples are collected simultaneously at two heights using rotating wet-annular denuders and steam-jet aerosol collectors, respectively. Online (real-time) analysis using ion chromatography (IC) for anions and flow injection analysis (FIA) for NH4+ and NH3 provide a half-hourly averaged gas and aerosol gradients within each hour. Through the use of syringe pumps, IC preconcentration columns, and high-quality purified water, the system achieves detection limits (3sigma-definition) under field conditions of typically: 136/207,135/114, 29/ 22,119/92, and 189/159 ng m(-3) for NH3/NH4+, HNO3/NO3-, HONO/ NO2-, HCl/Cl- and SO2/SO4(2-), respectively. The instrument demonstrates very good linearity and accuracy for liquid and selected gas phase calibrations over typical ambient concentration ranges. As shown by examples from field experiments, the instrument provides sufficient precision (3-9%), even at low ambient concentrations, to resolve vertical gradients and calculate surface-atmosphere exchange fluxes undertypical meteorological conditions of the atmospheric surface layer using the aerodynamic gradient technique.

  4. High performance liquid chromatography study of complex oxygenated alkane mixtures from organic aerosols

    NASA Astrophysics Data System (ADS)

    Kalafut-Pettibone, Alicia J.; Klems, Joseph P.; McGivern, W. Sean

    2013-05-01

    The composition of secondary organic aerosol particles is of primary importance both in identifying particle sources and in determining physical parameters, such as cloud condensation nucleus propensity. Further, measurements of composition are valuable in determining the chemistry of formation and aging. In this work, we describe the application of a recently-developed derivatization technique to a complex synthetic organic aerosol derived from the photolysis of 1-iodooctane. The technique utilizes high-performance liquid chromatography (HPLC) coupled to both ultravioletvisible (UV/VIS) spectroscopy and tandem mass spectrometry (MS-MS) to determine the overall distribution of hydroxyl (OH), non-acid carbonyl (C=O), and carboxylic acid (COOH) moieties as well as the specific identities of chromatographically separated products. This composition data will then be used to constrain models of the particle formation mechanisms.

  5. Global survey of the relationships of cloud albedo and liquid water path with droplet size using ISCCP

    SciTech Connect

    Han, Q.; Chou, J.; Welch, R.M.; Rossow, W.B.

    1998-07-01

    The most common approach used to model the aerosol indirect effect on clouds holds the cloud liquid water path constant. In this case, increasing aerosol concentration increases cloud droplet concentration, decreases cloud droplet size, and increases cloud albedo. The expected decrease in cloud droplet size associated with larger aerosol concentrations has been found to be larger over land than over water and larger in the Northern that in the Southern Hemisphere, but the corresponding cloud albedo increase has not been found. Many previous studies have shown that cloud liquid water path varies with changing cloud droplet size, which may alter the behavior of clouds when aerosols change. This study examines the relationship between geographic and seasonal variations of cloud effective droplet size and cloud albedo, as well as cloud liquid water path, in low-level clouds using International Satellite Cloud Climatology Project data. The results show that cloud albedo increases with decreasing droplet size for most clouds over continental areas and for all optically thicker clouds, but that cloud albedo decreases with decreasing droplet size for optically thinner clouds over most oceans and the tropical rain forest regions. For almost all clouds, the liquid water path increases with increasing cloud droplet size.

  6. Impacts of surface adsorbed catechol on tropospheric aerosol surrogates: heterogeneous ozonolysis and its effects on water uptake.

    PubMed

    Woodill, Laurie A; O'Neill, Erinn M; Hinrichs, Ryan Z

    2013-07-11

    Surface adsorbed organics are ubiquitous components of inorganic tropospheric aerosols and have the potential to alter aerosol chemical and physical properties. To assess the impact of adsorbed organics on water uptake by inorganic substrates, we used diffuse reflectance infrared spectroscopy to compared water adsorption isotherms for uncoated NaCl and α-Al2O3 samples, samples containing a monolayer of adsorbed catechol, and adsorbed catechol samples following ozonolysis. Adsorption of gaseous catechol on to the inorganic substrates produced vibrational features indicating physisorption on NaCl and displacement of surface hydroxyl groups forming binuclear bidentate catecholate on α-Al2O3, with surface concentrations of 2-3 × 10(18) molecules m(-2). Subsequent heterogeneous ozonolysis produced muconic acid at a rate 4-5 times faster on NaCl compared to α-Al2O3, with predicted atmospheric lifetimes of 4.3 and 18 h, respectively, assuming a tropospheric ozone concentration of 40 ppb. Water adsorption isotherms for all NaCl samples were indistinguishable within experimental uncertainty, indicating that these organic monolayers had negligible impact on coadsorbed water surface concentrations for these systems. α-Al2O3-catechol samples exhibited dramatically less water uptake compared to uncoated α-Al2O3, while oxidation of surface adsorbed catechol had no effect on the extent of water uptake. For both substrates, adsorbed organics increased the relative abundance of "ice-like" versus "liquid-like" water, with the effect larger for catechol than oxidized ozonolysis products. These results highlight the importance of aerosol substrate in understanding the heterogeneous ozonolysis of adsorbed polyphenols and suggest such coatings may impair ice nucleation by aluminosilicate mineral aerosol.

  7. Solid versus liquid particle sampling efficiency of three personal aerosol samplers when facing the wind.

    PubMed

    Koehler, Kirsten A; Anthony, T Renee; Van Dyke, Michael; Volckens, John

    2012-03-01

    The objective of this study was to examine the facing-the-wind sampling efficiency of three personal aerosol samplers as a function of particle phase (solid versus liquid). Samplers examined were the IOM, Button, and a prototype personal high-flow inhalable sampler head (PHISH). The prototype PHISH was designed to interface with the 37-mm closed-face cassette and provide an inhalable sample at 10 l min(-1) of flow. Increased flow rate increases the amount of mass collected during a typical work shift and helps to ensure that limits of detection are met, particularly for well-controlled but highly toxic species. Two PHISH prototypes were tested: one with a screened inlet and one with a single-pore open-face inlet. Personal aerosol samplers were tested on a bluff-body disc that was rotated along the facing-the-wind axis to reduce spatiotemporal variability associated with sampling supermicron aerosol in low-velocity wind tunnels. When compared to published data for facing-wind aspiration efficiency for a mouth-breathing mannequin, the IOM oversampled relative to mannequin facing-the-wind aspiration efficiency for all sizes and particle types (solid and liquid). The sampling efficiency of the Button sampler was closer to the mannequin facing-the-wind aspiration efficiency than the IOM for solid particles, but the screened inlet removed most liquid particles, resulting in a large underestimation compared to the mannequin facing-the-wind aspiration efficiency. The open-face PHISH results showed overestimation for solid particles and underestimation for liquid particles when compared to the mannequin facing-the-wind aspiration efficiency. Substantial (and statistically significant) differences in sampling efficiency were observed between liquid and solid particles, particularly for the Button and screened-PHISH, with a majority of aerosol mass depositing on the screened inlets of these samplers. Our results suggest that large droplets have low penetration efficiencies

  8. Water: A Tale of Two Liquids.

    PubMed

    Gallo, Paola; Amann-Winkel, Katrin; Angell, Charles Austen; Anisimov, Mikhail Alexeevich; Caupin, Frédéric; Chakravarty, Charusita; Lascaris, Erik; Loerting, Thomas; Panagiotopoulos, Athanassios Zois; Russo, John; Sellberg, Jonas Alexander; Stanley, Harry Eugene; Tanaka, Hajime; Vega, Carlos; Xu, Limei; Pettersson, Lars Gunnar Moody

    2016-07-13

    Water is the most abundant liquid on earth and also the substance with the largest number of anomalies in its properties. It is a prerequisite for life and as such a most important subject of current research in chemical physics and physical chemistry. In spite of its simplicity as a liquid, it has an enormously rich phase diagram where different types of ices, amorphous phases, and anomalies disclose a path that points to unique thermodynamics of its supercooled liquid state that still hides many unraveled secrets. In this review we describe the behavior of water in the regime from ambient conditions to the deeply supercooled region. The review describes simulations and experiments on this anomalous liquid. Several scenarios have been proposed to explain the anomalous properties that become strongly enhanced in the supercooled region. Among those, the second critical-point scenario has been investigated extensively, and at present most experimental evidence point to this scenario. Starting from very low temperatures, a coexistence line between a high-density amorphous phase and a low-density amorphous phase would continue in a coexistence line between a high-density and a low-density liquid phase terminating in a liquid-liquid critical point, LLCP. On approaching this LLCP from the one-phase region, a crossover in thermodynamics and dynamics can be found. This is discussed based on a picture of a temperature-dependent balance between a high-density liquid and a low-density liquid favored by, respectively, entropy and enthalpy, leading to a consistent picture of the thermodynamics of bulk water. Ice nucleation is also discussed, since this is what severely impedes experimental investigation of the vicinity of the proposed LLCP. Experimental investigation of stretched water, i.e., water at negative pressure, gives access to a different regime of the complex water diagram. Different ways to inhibit crystallization through confinement and aqueous solutions are

  9. Secondary Organic Aerosol Formation over Coastal Ocean: Inferences from Atmospheric Water-Soluble Low Molecular Weight Organic Compounds.

    PubMed

    Bikkina, Srinivas; Kawamura, Kimitaka; Sarin, Manmohan

    2017-04-07

    A lack of consensus on the distributions and formation pathways of secondary organic aerosols (SOA) over oceanic regions downwind of pollution sources limits our ability to assess their climate impact globally. As a case study, we report here on water-soluble SOA components such as dicarboxylic acids, oxocarboxylic acids, and α-dicarbonyls in the continental outflows from the Indo-Gangetic Plain (IGP) and Southeast Asia (SEA) to the Bay of Bengal. Oxalic acid (C2) is the dominant species followed by succinic (C4) and glyoxylic acids (ωC2) in the outflow. Nonsea-salt SO4(2-) also dominates (∼70%) total water-soluble inorganic constituents and correlates well with aerosol liquid water content (LWC) and C2, indicating their production through aqueous phase photochemical reactions. Furthermore, mass ratios of dicarboxylic acids (C2/C4, C2/ωC2), and their relative abundances in water-soluble organic carbon and total organic carbon are quite similar between the two continental (IGP and SEA) outflows, indicating the formation of SOA through aqueous phase photochemical reactions in LWC-enriched aerosols, largely controlled by anthropogenic SO4(2-).

  10. Submicron Aerosol Characterization of Water by a Differential Mobility Particle Sizer.

    DTIC Science & Technology

    1987-02-01

    relevant to modern science and industry. N *% ~ ~ ~?1 *1?%~%~ 0.0 :~. % % his ’i tl’tt Security Classif ication KIEV WORDS Submricron aerosols Water ...7 :-711 no0 StIHICRON AEROSOL CHARACTERIZATION OF WATER DY A vi1 DIFFERENTIAL NOBILITY PA.. (U) DEFENCE RESEARCH ESTABLISHMENT SUFFIELD RALSTON... WATER BY A DIFFERENTIAL MOBILITY PARTICLE SIZER (U) by B. Kournikakis, A. Gunning, J. Fildes and J. Ho Project No. 251SD EL .TE APR 099?07uD February

  11. Discontinuities in hygroscopic growth below and above water saturation for laboratory surrogates of oligomers in organic atmospheric aerosols

    NASA Astrophysics Data System (ADS)

    Hodas, Natasha; Zuend, Andreas; Schilling, Katherine; Berkemeier, Thomas; Shiraiwa, Manabu; Flagan, Richard C.; Seinfeld, John H.

    2016-10-01

    Discontinuities in apparent hygroscopicity below and above water saturation have been observed for organic and mixed organic-inorganic aerosol particles in both laboratory studies and in the ambient atmosphere. However, uncertainty remains regarding the factors that contribute to observations of low hygroscopic growth below water saturation but enhanced cloud condensation nuclei (CCN) activity for a given aerosol population. Utilizing laboratory surrogates for oligomers in atmospheric aerosols, we explore the extent to which such discontinuities are influenced by organic component molecular mass and viscosity, non-ideal thermodynamic interactions between aerosol components, and the combination of these factors. Measurements of hygroscopic growth under subsaturated conditions and the CCN activity of aerosols comprised of polyethylene glycol (PEG) with average molecular masses ranging from 200 to 10 000 g mol-1 and mixtures of PEG with ammonium sulfate (AS) were conducted. Experimental results are compared to calculations of hygroscopic growth at thermodynamic equilibrium conducted with the Aerosol Inorganic Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model, and the potential influence of kinetic limitations on observed water uptake was further explored through estimations of water diffusivity in the PEG oligomers. Particle-phase behavior, including the prevalence of liquid-liquid phase separation (LLPS), was also modeled with AIOMFAC. Under subsaturated relative humidity (RH) conditions, we observed little variability in hygroscopic growth across PEG systems with different molecular masses; however, an increase in CCN activity with increasing PEG molecular mass was observed. This effect is most pronounced for PEG-AS mixtures, and, in fact, an enhancement in CCN activity was observed for the PEG10000-AS mixture as compared to pure AS, as evidenced by a 15 % reduction in critical activation diameter at a supersaturation of 0.8 %. We also

  12. Cloud-Aerosol Interactions: Retrieving Aerosol Ångström Exponents from Calipso Measurements of Opaque Water Clouds

    NASA Astrophysics Data System (ADS)

    Vaughan, Mark; Liu, Zhaoyan; Hu, Yong-Xiang; Powell, Kathleen; Omar, Ali; Rodier, Sharon; Hunt, William; Kar, Jayanta; Tackett, Jason; Getzewich, Brian; Lee, Kam-Pui

    2016-06-01

    Backscatter and extinction from water clouds are well-understood, both theoretically and experimentally, and thus changes to the expected measurement of layer-integrated attenuated backscatter can be used to infer the optical properties of overlying layers. In this paper we offer a first look at a new retrieval technique that uses CALIPSO measurements of opaque water clouds to derive optical depths and Ångström exponents for overlying aerosol layers.

  13. A novel ultrasonic aerosol generator.

    PubMed

    Davies, A; Hudson, N; Pirie, L

    1995-07-01

    An ultrasonic aerosol generator constructed from a domestic humidifier is described which has been used to produce liquid aerosols for physiological investigations. The instrument was constructed from a Pifco domestic humidifier modified to include an energy guide to direct the oscillations of the transducer through the coupling water, which would normally be aerosolized, onto a small membrane based sample chamber containing the liquid to be aerosolized. The size distribution of the aerosol produced was found to be between 2 and 6 mm, optimum for diffuse intrapulmonary deposition. Up to 4 ml/min of aqueous liquid was used; however the sample chamber could be made small enough to contain economic amounts of expensive material to administer by inhalation. The instrument has proved to be reliable over a period of three years.

  14. Liquid-liquid phase transitions and water-like anomalies in liquids

    NASA Astrophysics Data System (ADS)

    Lascaris, Erik

    In this thesis we employ computer simulations and statistical physics to understand the origin of liquid-liquid phase transitions and their relationship with anomalies typical of liquid water. Compared with other liquids, water has many anomalies. For example the density anomaly: when water is cooled below 4 °C the density decreases rather than increases. This and other anomalies have also been found to occur in a few other one-component liquids, sometimes in conjunction with the existence of a liquid-liquid phase transition (LLPT) between a low-density liquid (LDL) and a high-density liquid (HDL). Using simple models we explain how these anomalies arise from the presence of two competing length scales. As a specific example we investigate the cut ramp potential, where we show the importance of "competition" in this context, and how one length scale can sometimes be zero. When there is a clear energetic preference for either LDL or HDL for all pressures and temperatures, then there is insufficient competition between the two liquid structures and no anomalies occur. From the simple models it also follows that anomalies can occur without the presence of a LLPT and vice versa. It remains therefore unclear if water has a LLPT that ends in a liquid-liquid critical point (LLCP), a hypothesis that was first proposed based on simulations of the ST2 water model. We confirm the existence of a LLCP in this model using finite size scaling and the Challa-Landau-Binder parameter, and show that the LLPT is not a liquid-crystal transition, as has recently been suggested. Previous research has indicated the possible existence of a LLCP in liquid silica. We perform a detailed analysis of two different silica models (WAC and BKS) at temperatures much lower than was previously simulated. Within the accessible temperature range we find no LLCP in either model, although in the case of WAC potential it is closely approached. We compare our results with those obtained for other

  15. New technique for online measurement of water-soluble Fe(II) in atmospheric aerosols.

    PubMed

    Rastogi, Neeraj; Oakes, Michelle M; Schauer, James J; Shafer, Martin M; Majestic, Brian J; Weber, Rodney J

    2009-04-01

    A prototype instrument has been developed for online analysis of water-soluble Fe(II) (WS_Fe(II)) in atmospheric aerosols using a particle-into-liquid-sampler (PILS), which concentrates particles into a small flow of purified water, coupled with a liquid waveguide capillary cell (LWCC) and absorbance spectrophotometryto detect iron-ferrozine colored complexes. The analytical method is highly precise (<3% RSD), and the overall measurement uncertainty and limit of detection for the complete PILS-LWCC system are estimated at 12% and 4.6 ng m(-3), respectively. The online measurements compared well with those of 24 h integrated filter samples collected at two different sampling sites (n=27, R2 = 0.82, slope 0.90 +/- 0.08, and intercept 3.08 +/- 1.99 ng m(-3)). In urban Atlanta, fine particle WS_Fe(II) concentrations measured every 12 min exhibited large variability, ranging from below the detection limit (4.6) to 370 ng m(-3) during a 24 day period in June 2008. This instrument provides new capabilities for investigating the sources and atmospheric processing of fine particle WS_Fe(II) and may prove useful in studies ranging from effects of particle WS_Fe(II) on human health to effects of particle WS_Fe(II) on atmospheric chemistry and ocean biogeochemistry.

  16. Updating CMAQ secondary organic aerosol properties relevant for aerosol water interactions

    EPA Science Inventory

    Properties of secondary organic aerosol (SOA) compounds in CMAQ are updated with state-of-the-science estimates from structure activity relationships to provide consistency among volatility, molecular weight, degree of oxygenation, and solubility/hygroscopicity. These updated pro...

  17. Atmospheric aerosol deposition influences marine microbial communities in oligotrophic surface waters of the western Pacific Ocean

    NASA Astrophysics Data System (ADS)

    Maki, Teruya; Ishikawa, Akira; Mastunaga, Tomoki; Pointing, Stephen B.; Saito, Yuuki; Kasai, Tomoaki; Watanabe, Koichi; Aoki, Kazuma; Horiuchi, Amane; Lee, Kevin C.; Hasegawa, Hiroshi; Iwasaka, Yasunobu

    2016-12-01

    Atmospheric aerosols contain particulates that are deposited to oceanic surface waters. These can represent a major source of nutrients, trace metals, and organic compounds for the marine environment. The Japan Sea and the western Pacific Ocean are particularly affected by aerosols due to the transport of desert dust and industrially derived particulate matter with aerodynamic diameter less than 2.5 μm (PM2.5) from continental Asia. We hypothesized that supplementing seawater with aerosol particulates would lead to measurable changes in surface water nutrient composition as well as shifts in the marine microbial community. Shipboard experiments in the Pacific Ocean involved the recovery of oligotrophic oceanic surface water and subsequent supplementation with aerosol particulates obtained from the nearby coastal mountains, to simulate marine particulate input in this region. Initial increases in nitrates due to the addition of aerosol particulates were followed by a decrease correlated with the increase in phytoplankton biomass, which was composed largely of Bacillariophyta (diatoms), including Pseudo-nitzschia and Chaetoceros species. This shift was accompanied by changes in the bacterial community, with apparent increases in the relative abundance of heterotrophic Rhodobacteraceae and Colwelliaceae in aerosol particulate treated seawater. Our findings provide empirical evidence revealing the impact of aerosol particulates on oceanic surface water microbiology by alleviating nitrogen limitation in the organisms.

  18. Comparing the mechanism of water condensation and evaporation in glassy aerosol.

    PubMed

    Bones, David L; Reid, Jonathan P; Lienhard, Daniel M; Krieger, Ulrich K

    2012-07-17

    Atmospheric models generally assume that aerosol particles are in equilibrium with the surrounding gas phase. However, recent observations that secondary organic aerosols can exist in a glassy state have highlighted the need to more fully understand the kinetic limitations that may control water partitioning in ambient particles. Here, we explore the influence of slow water diffusion in the condensed aerosol phase on the rates of both condensation and evaporation, demonstrating that significant inhibition in mass transfer occurs for ultraviscous aerosol, not just for glassy aerosol. Using coarse mode (3-4 um radius) ternary sucrose/sodium chloride/aqueous droplets as a proxy for multicomponent ambient aerosol, we demonstrate that the timescale for particle equilibration correlates with bulk viscosity and can be ≫10(3) s. Extrapolation of these timescales to particle sizes in the accumulation mode (e.g., approximately 100 nm) by applying the Stokes-Einstein equation suggests that the kinetic limitations imposed on mass transfer of water by slow bulk phase diffusion must be more fully investigated for atmospheric aerosol. Measurements have been made on particles covering a range in dynamic viscosity from < 0.1 to > 10(13) Pa s. We also retrieve the radial inhomogeneities apparent in particle composition during condensation and evaporation and contrast the dynamics of slow dissolution of a viscous core into a labile shell during condensation with the slow percolation of water during evaporation through a more homogeneous viscous particle bulk.

  19. Measurements of total column ozone, precipitable water content and aerosol optical depth at Sofia

    NASA Astrophysics Data System (ADS)

    Kaleyna, P.; Kolev, N.; Savov, P.; Evgenieva, Ts.; Danchovski, V.; Muhtarov, P.

    2016-03-01

    This article reports the results of a study related to variations in total ozone content, aerosol optical depth, water vapor content and Ångström coefficients from summer campaign carried out in June-July 2014, at two sites in the city of Sofia (Astronomical Observatory in the Borisova Gradina Park and National Institute of Geophysics, Geodesy and Geography (NIGGG)). The results of data analysis indicate the following: Spectral dependence of aerosol optical depth (AOD); Greater AOD values due to greater portion of aerosols; Inverse relationship between the time variations of AOD or water vapor and ozone.

  20. Enhanced water vapor in Asian dust layer: Entrainment processes and implication for aerosol optical properties

    NASA Astrophysics Data System (ADS)

    Yoon, Soon-Chang; Kim, Sang-Woo; Kim, Jiyoung; Sohn, Byung-Ju; Jefferson, Anne; Choi, Suk-Jin; Cha, Dong-Hyun; Lee, Dong-Kyou; Anderson, Theodore L.; Doherty, Sarah J.; Weber, Rodney J.

    The entrainment process of water vapor into the dust layer during Asian dust events and the effect of water vapor associated with the Asian dust layer (ADL) on aerosol hygroscopic properties are investigated. The entrainment processes of water vapor into the ADL is examined by using a PSU/NCAR MM5 together with the backward trajectory model, radiosonde data, and remotely sensed aerosol vertical distribution data. Two dust events in the spring of 1998 and 2001 are examined in detail. The results reveal that the water vapor mixing ratio (WVMR) derived by the MM5 fits in well with the WVMR observed by radiosonde, and is well coincident with the aerosol extinction coefficient ( σep) measured by the micro-pulse lidar. The temporal evolution of the vertical distributions of WVMR and σep exhibited similar features. On the basis of a well simulation of the enhanced water vapor within the dust layer by the MM5, we trace the dust storms to examine the entrainment mechanism. The enhancement of WVMR within the ADL was initiated over the mountainous areas. The relatively moist air mass in the well-developed mixing layer over the mountainous areas is advected upward from the boundary layer by an ascending motion. However, a large portion of the water vapor within the ADL is enhanced over the edge of a highland and the plains in China. This is well supported by the simulated WVMR and the wind vectors. Aircraft-based in situ measurements of the chemical and optical properties of aerosol enable a quantitative estimation of the effect of the enhanced WVMR on the aerosol hygroscopic properties. The submicron aerosol accompanied by the dust storm caused an increase of aerosol scattering through water uptakes during the transport. This increase could be explained by the chemical fact that water-soluble submicron pollution aerosols are enriched in the ADL.

  1. Influence of organic films on the evaporation and condensation of water in aerosol.

    PubMed

    Davies, James F; Miles, Rachael E H; Haddrell, Allen E; Reid, Jonathan P

    2013-05-28

    Uncertainties in quantifying the kinetics of evaporation and condensation of water from atmospheric aerosol are a significant contributor to the uncertainty in predicting cloud droplet number and the indirect effect of aerosols on climate. The influence of aerosol particle surface composition, particularly the impact of surface active organic films, on the condensation and evaporation coefficients remains ambiguous. Here, we report measurements of the influence of organic films on the evaporation and condensation of water from aerosol particles. Significant reductions in the evaporation coefficient are shown to result when condensed films are formed by monolayers of long-chain alcohols [C(n)H(2n+1)OH], with the value decreasing from 2.4 × 10(-3) to 1.7 × 10(-5) as n increases from 12 to 17. Temperature-dependent measurements confirm that a condensed film of long-range order must be formed to suppress the evaporation coefficient below 0.05. The condensation of water on a droplet coated in a condensed film is shown to be fast, with strong coherence of the long-chain alcohol molecules leading to islanding as the water droplet grows, opening up broad areas of uncoated surface on which water can condense rapidly. We conclude that multicomponent composition of organic films on the surface of atmospheric aerosol particles is likely to preclude the formation of condensed films and that the kinetics of water condensation during the activation of aerosol to form cloud droplets is likely to remain rapid.

  2. Analysis and Calibration of CRF Raman Lidar Cloud Liquid Water Measurements

    SciTech Connect

    Turner, D.D. Whiteman, D.N. Russo, F.

    2007-10-31

    The Atmospheric Radiation Measurement (ARM) Raman lidar (RL), located at the Southern Great Plains (SGP) Climate Research Facility (CRF), is a unique state-of-the-art active remote sensor that is able to measure profiles of water vapor, aerosol, and cloud properties at high temporal and vertical resolution throughout the diurnal cycle. In October 2005, the capability of the RL was extended by the addition of a new detection channel that is sensitive to the Raman scattering of liquid water. This new channel permits the system, in theory, to measure profiles of liquid water content (LWC) by the RL. To our knowledge, the ARM RL is the only operation lidar with this capability. The liquid water Raman backscattering cross-section is a relatively weak and spectrally broad feature, relative to the water vapor Raman backscatter signal. The wide bandpass required to achieve reasonable signal-to-noise in the liquid water channel essentially eliminates the ability to measure LWC profiles during the daytime in the presence of large solar background, and thus all LWC observations are nighttime only. Additionally, the wide bandpass increases the probability that other undesirable signals, such as fluorescence from aerosols, may contaminate the observation. The liquid water Raman cross-section has a small amount of overlap with the water vapor Raman cross-section, and thus there will be a small amount of ‘cross-talk’ between the two signals, with water vapor contributing a small amount of signal to the LWC observation. And finally, there is significant uncertainty in the actual strength of the liquid water Raman cross-section in the literature. The calibrated LWC profiles, together with the coincident cloud backscatter observations also made by the RL, can be used to derive profiles of cloud droplet effective radius. By combining these profiles of effective radius in the lower portion of the cloud with the aerosol extinction measurements made below the cloud by the RL, the

  3. Response of North Pacific eastern subtropical mode water to greenhouse gas versus aerosol forcing

    NASA Astrophysics Data System (ADS)

    Li, Xiang; Luo, Yiyong

    2016-04-01

    Mode water is a distinct water mass characterized by a near vertical homogeneous layer or low potential vorticity, and is considered essential for understanding ocean climate variability. Based on the output of GFDL CM3, this study investigates the response of eastern subtropical mode water (ESTMW) in the North Pacific to two different single forcings: greenhouse gases (GHGs) and aerosol. Under GHG forcing, ESTMW is produced on lighter isopycnal surfaces and is decreased in volume. Under aerosol forcing, in sharp contrast, it is produced on denser isopycnal surfaces and is increased in volume. The main reason for the opposite response is because surface ocean-to-atmosphere latent heat flux change over the ESTMW formation region shoals the mixed layer and thus weakens the lateral induction under GHG forcing, but deepens the mixed layer and thus strengthens the lateral induction under aerosol forcing. In addition, local wind changes are also favorable to the opposite response of ESTMW production to GHG versus aerosol.

  4. Liquid water habitats on early Mars

    NASA Technical Reports Server (NTRS)

    Mckay, Christopher P.; Davis, Wanda L.

    1992-01-01

    Although the Viking results may indicate that Mars has no life today, the possibility exists that Mars may hold the best record of the events that led to the origin of life. There is direct geomorphological evidence that in the past Mars had large amounts of liquid water on its surface. Atmospheric models would suggest that this early period of hydrological activity was due to the presence of a thick atmosphere and the resulting warmer temperatures. From a biological perspective the existence of liquid water by itself motivates the question of the origin of life on Mars. From studies of the Earth's earliest biosphere, we know that by 3.5 Gyr ago life had originated on Earth and reached a fair degree of biological sophistication. Surface activity and erosion on Earth make it difficult to trace the history of life before the 3.5 Gyr timeframe. If Mars did maintain a clement environment for longer than it took for life to originate on Earth, then the question of the origin of life on Mars follows naturally. Based upon simple models of the evolution of the Martian climate, we divide the history of liquid water habitats on the Martian surface into four epochs based upon the atmospheric temperature and pressure.

  5. Photoelectron Emission Spectroscopy of Liquid Water.

    DTIC Science & Technology

    1981-04-01

    correlated to solvation free energies for H2O+(aq) and OH (aq)., DD ,FO*M 1473 EDITIOOF INOV so iS OBSOLETE Unclassified SECURITY CLASSIFICATION OF THIS PAGE...Photoelectron spectroscopy Reorganization free energy Water, liquid 20. ABSTRACT (Chlnw am ef We, aid* it nooe"mr and 1iEru’h hr 190k le 6) The threshold... energy Et a 10.06 eV (0.002 @V standard deviation) is detemined for phot~oelectron emission by litquid water and is correlated with Et a 8.45 eV for

  6. Influence of aqueous chemistry on the chemical composition of fog water and interstitial aerosol in Fresno

    NASA Astrophysics Data System (ADS)

    Kim, Hwajin; Ge, Xinlei; Collier, Sonya; Xu, Jianzhong; Sun, Yele; Wang, Youliang; Herckes, Pierre; Zhang, Qi

    2015-04-01

    A measurement study was conducted in the Central Valley (Fresno) of California in January 2010, during which radiation fog events were frequently observed. Fog plays important roles in atmospheric chemistry by scavenging aerosol particles and trace gases and serving as a medium for various aqueous-phase reactions. Understanding the effects of fog on the microphysical and chemical processing of aerosol particles requires detailed information on their chemical composition. In this study, we characterized the chemical composition of fog water and interstitial aerosol particles to study the effects of fog processing on aerosol properties. Fog water samples were collected during the 2010 Fresno campaigns with a Caltech Active Strand Cloud water Collector (CASCC) while interstitial submicron aerosols were characterized in real time with an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and a scanning Mobility Particle Sizer (SMPS). The fog water samples were later analyzed using the HR-ToF-AMS, ion chromatography, and a total carbon analyzer. The chemical composition and characteristics of interstitial particles during the fog events were compared to those of dissolved inorganic and organic matter in fog waters. Compared to interstitial aerosols, fog water is composed of a higher fraction of ammonium nitrate and oxygenated organics, due to aqueous formation of secondary aerosol species as well as enhanced gas-to-particle partitioning of water soluble species under water rich conditions. Sulfate is formed most efficiently in fog water although its contribution to total dissolved mass is relatively low. The HR-ToF-AMS mass spectra of organic matter in fog water (FOM) are very similar to that of oxygenated organic aerosols (OOA) derived from positive matrix factorization (PMF) of the HR-ToF-AMS spectra of ambient aerosol (r2 = 0.96), but FOM appears to contain a large fraction of acidic functional groups than OOA. FOM is also enriched of

  7. 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.

  8. Separation of THF and water by room temperature ionic liquids.

    PubMed

    Hu, X; Yu, J; Liu, H

    2006-01-01

    Liquid-liquid equilibrium data are presented for mixtures of 1-(2-hydroxyethyl)-3-methylimidazolium chloride or tetrafluoroborate + tetrahydrofuran(THF) + water at 293.15 K. The data presented provides a valuable insight into how the environmentally friendly ionic liquid solvent can have the separation power of THF-water azeotropic systems. The sloping of the tie lines towards the THF vertex is investigated for mixtures of 1-(2-hydroxyethyl)-3-methylimidazolium chloride (or tetrafluoroborate) + THF + water. Selectivity values, derived from the tie line data, indicate that these two ionic liquids are suitable solvents for the liquid-liquid extraction of water from THF.

  9. Liquid water and active resurfacing on Europa

    NASA Technical Reports Server (NTRS)

    Squyres, S. W.; Reynolds, R. T.; Cassen, P. M.; Peale, S. J.

    1983-01-01

    Arguments for recent resurfacing of Europa by H2O from a liquid layer are presented, based on new interpretations of recent spacecraft and earth-based observations and revised theoretical calculations. The heat flow in the core and shell due to tidal forces is discussed, and considerations of viscosity and convection in the interior are found to imply water retention in the outer 60 km or so of the silicates, forming a layer of water/ice many tens of km thick. The outer ice crust is considered to be too thin to support heat transport rates sufficient to freeze the underlying water. Observational evidence for the calculations would consist of an insulating layer of frosts derived from water boiling up between cracks in the surface crust. Evidence for the existence of such a frost layer, including the photometric function of Europa and the deposits of sulfur on the trailing hemisphere, is discussed.

  10. Near-global survey of effective droplet radii in liquid water clouds using ISCCP data

    NASA Technical Reports Server (NTRS)

    Han, Qingyan; Rossow, William B.; Lacis, Andrew B.

    1994-01-01

    A global survey of cloud particle size variations can provide crucial constraints on how cloud processes determine cloud liquid water contents and their variation with temperature, and further, may indicate the magnitude of aerosol effects on clouds. A method, based on a complete radiative transfer model for Advanced Very High Resolution Radiometer (AVHRR)-measured radiances, is described for retrieving cloud particle radii in liquid water clouds from satellite data currently available from the International Satellite Cloud Climatology Project. Results of sensitivity tests and validation studies provide error estimates. AVHRR data from NOAA-9 and NOAA-10 have been analyzed for January, April, July and October in 1987 and 1988. The results of this first survey reveal systematic continental and maritime differences and hemispheric contrasts that are indicative of the effects of associated aerosol concentration differences: cloud droplet radii in continental water clouds are about 2-3 micrometers smaller than in marine clouds, and droplet radii are about 1 micrometer smaller in marine clouds of the Northern Hemisphere than in the Southern Hemisphere. The height dependencies of cloud droplet radii in continental and marine clouds are also consistent with differences in the vertical profiles of aerosol concentration. Significant seasonal and diurnal variations of effective droplet radii are also observed, particularly at lower latitudes. Variations of the relationship between cloud optical thickness and droplet radii may indicate variations in cloud microphysical regimes.

  11. Aerosol-Water Cycle Interaction: A New Challenge in Monsoon Climate Research

    NASA Technical Reports Server (NTRS)

    Lau, William K. M.

    2006-01-01

    Long recognized as a major environmental hazard, aerosol is now known to have strong impacts on both regional and global climate. It has been estimated that aerosol may reduce by up to 10% of the seasonal mean solar radiation reaching the earth surface, producing a global cooling effect that opposes global warming (Climate Change 2001). This means that the potential perils that humans have committed to global warming may be far greater than what we can detect at the present. As a key component of the Earth climate system, the water cycle is profoundly affected by the presence of aerosols in the atmosphere. Through the so-called direct effect , aerosol scatters and/or absorbs solar radiation, thus cooling the earth surface and changing the horizontal and vertical radiational heating contrast in the atmosphere. The heating contrast drives anomalous atmospheric circulation, resulting in changes in convection, clouds, and rainfall. Another way aerosol can affect the water cycle is through the so-called indirect effects, whereby aerosol increases the number of cloud condensation nuclei, prolongs life time of clouds, and inhibits the growth of cloud drops to raindrops. This leads to more clouds, and increased reflection of solar radiation, and further cooling at the earth surface. In monsoon regions, the response of the water cycle to aerosol forcing is especially complex, not only because of presence of diverse mix of aerosol species with vastly different radiative properties, but also because the monsoon is strongly influenced by ocean and land surface processes, land use, land change, as well as regional and global greenhouse warming effects. Thus, sorting out the impacts of aerosol forcing, and interaction with the monsoon water cycle is a very challenging problem. In this talk, I will offer some insights into how aerosols may impact the Asian monsoon based on preliminary results from satellite observations and climate model experiments. Specifically, I will discuss

  12. Aerosol-Water Cycle Interaction: A New Challenge in Monsoon Climate Research

    NASA Technical Reports Server (NTRS)

    Lau, William K. M.

    2006-01-01

    Long recognized as a major environmental hazard, aerosol is now known to have strong impacts on both regional and global climate. It has been estimated that aerosol may reduce by up to 10% of the seasonal mean solar radiation reaching the earth surface, producing a global cooling effect that opposes global warming (Climate Change 2001). This means that the potential perils that humans have committed to global warming may be far greater than what we can detect at the present. As a key component of the Earth climate system, the water cycle is profoundly affected by the presence of aerosols in the atmosphere. Through the so-called "direct effect", aerosol scatters and/or absorbs solar radiation, thus cooling the earth surface and changing the horizontal and vertical radiational heating contrast in the atmosphere. The heating contrast drives anomalous atmospheric circulation, resulting in changes in convection, clouds, and rainfall. Another way aerosol can affect the water cycle is through the so-called "indirect effects", whereby aerosol increases the number of cloud condensation nuclei, prolongs life time of clouds, and inhibits the growth of cloud drops to raindrops. This leads to more clouds, and increased reflection of solar radiation, and further cooling at the earth surface. In monsoon regions, the response of the water cycle to aerosol forcing is especially complex, not only because of presence of diverse mix of aerosol species with vastly different radiative properties, but also because the monsoon is strongly influenced by ocean and land surface processes, land use, land change, as well as regional and global greenhouse warming effects. Thus, sorting out the impacts of aerosol forcing, and interaction with the monsoon water cycle is a very challenging problem. In this talk, I will offer some insights into how aerosols may impact the Asian monsoon based on preliminary results from satellite observations and climate model experiments. Specifically, I will

  13. Experimental evidence supporting the insensitivity of cloud droplet formation to the mass accommodation coefficient for condensation of water vapor to liquid water

    NASA Astrophysics Data System (ADS)

    Langridge, Justin M.; Richardson, Mathews S.; Lack, Daniel A.; Murphy, Daniel M.

    2016-06-01

    The mass accommodation coefficient for uptake of water vapor to liquid water, αM, has been constrained using photoacoustic measurements of aqueous absorbing aerosol. Measurements performed over a range of relative humidities and pressures were compared to detailed model calculations treating coupled heat and mass transfer occurring during photoacoustic laser heating cycles. The strengths and weaknesses of this technique are very different to those for droplet growth/evaporation experiments that have typically been applied to these measurements, making this a useful complement to existing studies. Our measurements provide robust evidence that αM is greater than 0.1 for all humidities tested and greater than 0.3 for data obtained at relative humidities greater than 88% where the aerosol surface was most like pure water. These values of αM are above the threshold at which kinetic limitations are expected to impact the activation and growth of aerosol particles in warm cloud formation.

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

    NASA Astrophysics Data System (ADS)

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

    2016-01-01

    In order to utilize satellite-based aerosol measurements for the determination of air quality, the relationship between aerosol optical properties (wavelength-dependent, column-integrated extinction measured by satellites) and mass measurements of aerosol loading (PM2.5 used for air quality monitoring) must be understood. This connection varies with many factors including those specific to the aerosol type - such as composition, size, and hygroscopicity - and to the surrounding atmosphere, such as temperature, relative humidity (RH), and altitude, all of which can vary spatially and temporally. During the DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality) project, extensive in situ atmospheric profiling in the Baltimore, MD-Washington, D.C. region was performed during 14 flights in July 2011. Identical flight plans and profile locations throughout the project provide meaningful statistics for determining the variability in and correlations between aerosol loading, composition, optical properties, and meteorological conditions. Measured water-soluble aerosol mass was composed primarily of ammonium sulfate (campaign average of 32 %) and organics (57 %). A distinct difference in composition was observed, with high-loading days having a proportionally larger percentage of sulfate due to transport from the Ohio River Valley. This composition shift caused a change in the aerosol water-uptake potential (hygroscopicity) such that higher relative contributions of inorganics increased the bulk aerosol hygroscopicity. These days also tended to have higher relative humidity, causing an increase in the water content of the aerosol. Conversely, low-aerosol-loading days had lower sulfate and higher black carbon contributions, causing lower single-scattering albedos (SSAs). The average black carbon concentrations were 240 ng m-3 in the lowest 1 km, decreasing to 35 ng m-3 in the free troposphere (above

  15. Satellite-Based Assessment of Possible Dust Aerosols Semi-Direct Effect on Cloud Water Path over East Asia

    NASA Technical Reports Server (NTRS)

    Huang, Jianping; Lin, Bing; Minnis, Patrick; Wang, Tainhe; Wang, Xin; Hu, Yongxiang; Yi, Yuhong; Ayers, J. Kirk

    2006-01-01

    The semi-direct effects of dust aerosols are analyzed over eastern Asia using 2 years (June 2002 to June 2004) of data from the Clouds and the Earth s Radiant Energy System (CERES) scanning radiometer and MODerate Resolution Imaging Spectroradiometer (MODIS) on the Aqua satellite, and 18 years (1984 to 2001) of International Satellite Cloud Climatology Project (ISCCP) data. The results show that the water path of dust-contaminated clouds is considerably smaller than that of dust-free clouds. The mean ice water path (IWP) and liquid water path (LWP) of dusty clouds are less than their dust-free counterparts by 23.7% and 49.8%, respectively. The long-term statistical relationship derived from ISCCP also confirms that there is significant negative correlation between dust storm index and ISCCP cloud water path. These results suggest that dust aerosols warm clouds, increase the evaporation of cloud droplets and further reduce cloud water path, the so-called semi-direct effect. The semi-direct effect may play a role in cloud development over arid and semi-arid areas of East Asia and contribute to the reduction of precipitation.

  16. Thermodynamics of ice nucleation in liquid water.

    PubMed

    Wang, Xin; Wang, Shui; Xu, Qinzhi; Mi, Jianguo

    2015-01-29

    We present a density functional theory approach to investigate the thermodynamics of ice nucleation in supercooled water. Within the theoretical framework, the free-energy functional is constructed by the direct correlation function of oxygen-oxygen of the equilibrium water, and the function is derived from the reference interaction site model in consideration of the interactions of hydrogen-hydrogen, hydrogen-oxygen, and oxygen-oxygen. The equilibrium properties, including vapor-liquid and liquid-solid phase equilibria, local structure of hexagonal ice crystal, and interfacial structure and tension of water-ice are calculated in advance to examine the basis for the theory. The predicted phase equilibria and the water-ice surface tension are in good agreement with the experimental data. In particular, the critical nucleus radius and free-energy barrier during ice nucleation are predicted. The critical radius is similar to the simulation value, suggesting that the current theoretical approach is suitable in describing the thermodynamic properties of ice crystallization.

  17. The Interaction of Water and Aerosols in the Marine Boundary Layer: A Study of Selected Processes Impacting Radiative Transfer and Cloudiness

    DTIC Science & Technology

    2013-01-01

    cumulus (moderatus) clouds . Theoretical work centered around exercising the NAAPS model with various altered parameteric inputs to test the accuracy of...inversion mixing and sub- cloud aerosol on cloud thickness and cloud base height, 3) quantify and parameterize the impact of precipitation scavenging on...below cloud radiative transfer and cloud liquid water path. However, in the course of obtaining the measurements and analyzing them, our goals evolved

  18. Metastable liquid-liquid transition in a molecular model of water.

    PubMed

    Palmer, Jeremy C; Martelli, Fausto; Liu, Yang; Car, Roberto; Panagiotopoulos, Athanassios Z; Debenedetti, Pablo G

    2014-06-19

    Liquid water's isothermal compressibility and isobaric heat capacity, and the magnitude of its thermal expansion coefficient, increase sharply on cooling below the equilibrium freezing point. Many experimental, theoretical and computational studies have sought to understand the molecular origin and implications of this anomalous behaviour. Of the different theoretical scenarios put forward, one posits the existence of a first-order phase transition that involves two forms of liquid water and terminates at a critical point located at deeply supercooled conditions. Some experimental evidence is consistent with this hypothesis, but no definitive proof of a liquid-liquid transition in water has been obtained to date: rapid ice crystallization has so far prevented decisive measurements on deeply supercooled water, although this challenge has been overcome recently. Computer simulations are therefore crucial for exploring water's structure and behaviour in this regime, and have shown that some water models exhibit liquid-liquid transitions and others do not. However, recent work has argued that the liquid-liquid transition has been mistakenly interpreted, and is in fact a liquid-crystal transition in all atomistic models of water. Here we show, by studying the liquid-liquid transition in the ST2 model of water with the use of six advanced sampling methods to compute the free-energy surface, that two metastable liquid phases and a stable crystal phase exist at the same deeply supercooled thermodynamic condition, and that the transition between the two liquids satisfies the thermodynamic criteria of a first-order transition. We follow the rearrangement of water's coordination shell and topological ring structure along a thermodynamically reversible path from the low-density liquid to cubic ice. We also show that the system fluctuates freely between the two liquid phases rather than crystallizing. These findings provide unambiguous evidence for a liquid-liquid transition in

  19. Metastable liquid-liquid transition in a molecular model of water

    NASA Astrophysics Data System (ADS)

    Palmer, Jeremy C.; Martelli, Fausto; Liu, Yang; Car, Roberto; Panagiotopoulos, Athanassios Z.; Debenedetti, Pablo G.

    2014-06-01

    Liquid water's isothermal compressibility and isobaric heat capacity, and the magnitude of its thermal expansion coefficient, increase sharply on cooling below the equilibrium freezing point. Many experimental, theoretical and computational studies have sought to understand the molecular origin and implications of this anomalous behaviour. Of the different theoretical scenarios put forward, one posits the existence of a first-order phase transition that involves two forms of liquid water and terminates at a critical point located at deeply supercooled conditions. Some experimental evidence is consistent with this hypothesis, but no definitive proof of a liquid-liquid transition in water has been obtained to date: rapid ice crystallization has so far prevented decisive measurements on deeply supercooled water, although this challenge has been overcome recently. Computer simulations are therefore crucial for exploring water's structure and behaviour in this regime, and have shown that some water models exhibit liquid-liquid transitions and others do not. However, recent work has argued that the liquid-liquid transition has been mistakenly interpreted, and is in fact a liquid-crystal transition in all atomistic models of water. Here we show, by studying the liquid-liquid transition in the ST2 model of water with the use of six advanced sampling methods to compute the free-energy surface, that two metastable liquid phases and a stable crystal phase exist at the same deeply supercooled thermodynamic condition, and that the transition between the two liquids satisfies the thermodynamic criteria of a first-order transition. We follow the rearrangement of water's coordination shell and topological ring structure along a thermodynamically reversible path from the low-density liquid to cubic ice. We also show that the system fluctuates freely between the two liquid phases rather than crystallizing. These findings provide unambiguous evidence for a liquid-liquid transition in

  20. LASE Measurements of Water Vapor, Aerosol, and Cloud Distributions in Saharan Air Layers and Tropical Disturbances

    NASA Technical Reports Server (NTRS)

    Ismail, Syed; Ferrare, Richard A.; Browell, Edward V.; Kooi, Susan A.; Dunion, Jason P.; Heymsfield, Gerry; Notari, Anthony; Butler, Carolyn F.; Burton, Sharon; Fenn, Marta; Krishnamurti, T. N.; Chen, Gao; Anderson, Bruce

    2010-01-01

    LASE (Lidar Atmospheric Sensing Experiment) on-board the NASA DC-8 measured high resolution profiles of water vapor and aerosols, and cloud distributions in 14 flights over the eastern North Atlantic during the NAMMA (NASA African Monsoon Multidisciplinary Analyses) field experiment. These measurements were used to study African easterly waves (AEWs), tropical cyclones (TCs), and the Saharan Air Layer(s) (SAL). Interactions between the SAL and tropical air were observed during the early stages of the TC development. These LASE measurements represent the first simultaneous water vapor and aerosol lidar measurements to study the SAL and its impact on AEWs and TCs. Examples of profile measurements of aerosol scattering ratios, aerosol extinction coefficients, aerosol optical thickness, water vapor mixing ratios, RH, and temperature are presented to illustrate their characteristics in SAL, convection, and clear air regions. LASE data suggest that the SAL suppresses low-altitude convection at the convection-SAL interface region. Mid-level convection associated with the AEW and transport are likely responsible for high water vapor content observed in the southern regions of the SAL on August 20, 2008. This interaction is responsible for the transfer of about 7 x 10(exp 15) J latent heat energy within a day to the SAL. Measurements of lidar extinction-to-backscatter ratios in the range 36+/-5 to 45+/-5 are within the range of measurements from other lidar measurements of dust. LASE aerosol extinction and water vapor profiles are validated by comparison with onboard in situ aerosol measurements and GPS dropsonde water vapor soundings, respectively.

  1. Sensitivity of the remote sensing reflectance of ocean and coastal waters to uncertainties in aerosol characteristics

    NASA Astrophysics Data System (ADS)

    Seidel, F. C.; Garay, M. J.; Zhai, P.; Kalashnikova, O. V.; Diner, D. J.

    2015-12-01

    Remote sensing is a powerful tool for optical oceanography and limnology to monitor and study ocean, coastal, and inland water ecosystems. However, the highly spatially and temporally variable nature of water conditions and constituents, as well as atmospheric conditions are challenging factors, especially for spaceborne observations.Here, we study the quantitative impact of uncertainties in the spectral aerosol optical and microphysical properties, namely aerosol optical depth (AOD), spectral absorption, and particle size, on the remote sensing reflectance (Rrs) of simulated typical open ocean and coastal waters. Rrs is related to the inherent optical properties of the water column and is a fundamental parameter in ocean optics retrievals. We use the successive order of scattering (SOS) method to perform radiative transfer calculations of the coupled system of atmosphere and water. The optics of typical open ocean and coastal waters are simulated with bio-optical models. We derive sensitivities by comparing spectral SOS calculations of Rrs with a reference aerosol model against similar calculations performed using a different aerosol model. One particular focus of this study lies on the impact of the spectral absorption of dust and brown carbon, or similar particles with greater absorption at short wavelengths on Rrs. The results are presented in terms of the minimum expected error in Rrs due to the choice of an incorrect aerosol model during the atmospheric correction of ocean color remote sensing data from space. This study is independent of errors related to observational data or retrieval techniques.The results are relevant for quantifying requirements of aerosol retrievals to derive accurate Rrs from spaceborne observations, such as NASA's future Pre-Aerosol, Clouds, and ocean Ecosystem (PACE) mission.

  2. Factors influencing the microphysics and radiative properties of liquid-dominated Arctic clouds: insight from observations of aerosol and clouds during ISDAC

    SciTech Connect

    Earle, Michael; Liu, Peter S.; Strapp, J. Walter; Zelenyuk, Alla; Imre, D.; McFarquhar, Greg; Shantz, Nicole C.; Leaitch, W. R.

    2011-11-04

    Aircraft measurements during the Indirect and Semi-Direct Aerosol Campaign (ISDAC) in April 2008 are used to investigate aerosol indirect effects in Arctic clouds. Two aerosol-cloud regimes are considered in this analysis: single-layer stratocumulus cloud with below-cloud aerosol concentrations (N{sub a}) below 300 cm{sup -3} on April 8 and April 26-27 (clean cases); and inhomogeneous layered cloud with N{sub a} > 500 cm{sup -3} below cloud base on April 19-20, concurrent with a biomass burning episode (polluted cases). Vertical profiles through cloud in each regime are used to determine average cloud microphysical and optical properties. Positive correlations between the cloud droplet effective radius (Re) and cloud optical depth ({tau}) are observed for both clean and polluted cases, which are characteristic of optically-thin, non-precipitating clouds. Average Re values for each case are {approx} 6.2 {mu}m, despite significantly higher droplet number concentrations (Nd) in the polluted cases. The apparent independence of Re and Nd simplifies the description of indirect effects, such that {tau} and the cloud albedo (A) can be described by relatively simple functions of the cloud liquid water path. Adiabatic cloud parcel model simulations show that the marked differences in Na between the regimes account largely for differences in droplet activation, but that the properties of precursor aerosol also play a role, particularly for polluted cases where competition for vapour amongst the more numerous particles limits activation to larger and/or more hygroscopic particles. The similarity of Re for clean and polluted cases is attributed to compensating droplet growth processes for different initial droplet size distributions.

  3. Triplet correlation functions in liquid water

    NASA Astrophysics Data System (ADS)

    Dhabal, Debdas; Singh, Murari; Wikfeldt, Kjartan Thor; Chakravarty, Charusita

    2014-11-01

    Triplet correlations have been shown to play a crucial role in the transformation of simple liquids to anomalous tetrahedral fluids [M. Singh, D. Dhabal, A. H. Nguyen, V. Molinero, and C. Chakravarty, Phys. Rev. Lett. 112, 147801 (2014)]. Here we examine triplet correlation functions for water, arguably the most important tetrahedral liquid, under ambient conditions, using configurational ensembles derived from molecular dynamics (MD) simulations and reverse Monte Carlo (RMC) datasets fitted to experimental scattering data. Four different RMC data sets with widely varying hydrogen-bond topologies fitted to neutron and x-ray scattering data are considered [K. T. Wikfeldt, M. Leetmaa, M. P. Ljungberg, A. Nilsson, and L. G. M. Pettersson, J. Phys. Chem. B 113, 6246 (2009)]. Molecular dynamics simulations are performed for two rigid-body effective pair potentials (SPC/E and TIP4P/2005) and the monatomic water (mW) model. Triplet correlation functions are compared with other structural measures for tetrahedrality, such as the O-O-O angular distribution function and the local tetrahedral order distributions. In contrast to the pair correlation functions, which are identical for all the RMC ensembles, the O-O-O triplet correlation function can discriminate between ensembles with different degrees of tetrahedral network formation with the maximally symmetric, tetrahedral SYM dataset displaying distinct signatures of tetrahedrality similar to those obtained from atomistic simulations of the SPC/E model. Triplet correlations from the RMC datasets conform closely to the Kirkwood superposition approximation, while those from MD simulations show deviations within the first two neighbour shells. The possibilities for experimental estimation of triplet correlations of water and other tetrahedral liquids are discussed.

  4. Triplet correlation functions in liquid water

    SciTech Connect

    Dhabal, Debdas; Chakravarty, Charusita; Singh, Murari; Wikfeldt, Kjartan Thor

    2014-11-07

    Triplet correlations have been shown to play a crucial role in the transformation of simple liquids to anomalous tetrahedral fluids [M. Singh, D. Dhabal, A. H. Nguyen, V. Molinero, and C. Chakravarty, Phys. Rev. Lett. 112, 147801 (2014)]. Here we examine triplet correlation functions for water, arguably the most important tetrahedral liquid, under ambient conditions, using configurational ensembles derived from molecular dynamics (MD) simulations and reverse Monte Carlo (RMC) datasets fitted to experimental scattering data. Four different RMC data sets with widely varying hydrogen-bond topologies fitted to neutron and x-ray scattering data are considered [K. T. Wikfeldt, M. Leetmaa, M. P. Ljungberg, A. Nilsson, and L. G. M. Pettersson, J. Phys. Chem. B 113, 6246 (2009)]. Molecular dynamics simulations are performed for two rigid-body effective pair potentials (SPC/E and TIP4P/2005) and the monatomic water (mW) model. Triplet correlation functions are compared with other structural measures for tetrahedrality, such as the O–O–O angular distribution function and the local tetrahedral order distributions. In contrast to the pair correlation functions, which are identical for all the RMC ensembles, the O–O–O triplet correlation function can discriminate between ensembles with different degrees of tetrahedral network formation with the maximally symmetric, tetrahedral SYM dataset displaying distinct signatures of tetrahedrality similar to those obtained from atomistic simulations of the SPC/E model. Triplet correlations from the RMC datasets conform closely to the Kirkwood superposition approximation, while those from MD simulations show deviations within the first two neighbour shells. The possibilities for experimental estimation of triplet correlations of water and other tetrahedral liquids are discussed.

  5. Liquid-liquid transition in ST2 water

    NASA Astrophysics Data System (ADS)

    Liu, Yang; Palmer, Jeremy C.; Panagiotopoulos, Athanassios Z.; Debenedetti, Pablo G.

    2012-12-01

    We use the weighted histogram analysis method [S. Kumar, D. Bouzida, R. H. Swendsen, P. A. Kollman, and J. M. Rosenberg, J. Comput. Chem. 13, 1011 (1992), 10.1002/jcc.540130812] to calculate the free energy surface of the ST2 model of water as a function of density and bond-orientational order. We perform our calculations at deeply supercooled conditions (T = 228.6 K, P = 2.2 kbar; T = 235 K, P = 2.2 kbar) and focus our attention on the region of bond-orientational order that is relevant to disordered phases. We find a first-order transition between a low-density liquid (LDL, ρ ≈ 0.9 g/cc) and a high-density liquid (HDL, ρ ≈ 1.15 g/cc), confirming our earlier sampling of the free energy surface of this model as a function of density [Y. Liu, A. Z. Panagiotopoulos, and P. G. Debenedetti, J. Chem. Phys. 131, 104508 (2009), 10.1063/1.3229892]. We demonstrate the disappearance of the LDL basin at high pressure and of the HDL basin at low pressure, in agreement with independent simulations of the system's equation of state. Consistency between directly computed and reweighted free energies, as well as between free energy surfaces computed using different thermodynamic starting conditions, confirms proper equilibrium sampling. Diffusion and structural relaxation calculations demonstrate that equilibration of the LDL phase, which exhibits slow dynamics, is attained in the course of the simulations. Repeated flipping between the LDL and HDL phases in the course of long molecular dynamics runs provides further evidence of a phase transition. We use the Ewald summation with vacuum boundary conditions to calculate long-ranged Coulombic interactions and show that conducting boundary conditions lead to unphysical behavior at low temperatures.

  6. Secondary organic aerosol formation from cyclohexene ozonolysis in the presence of water vapor and dissolved salts

    NASA Astrophysics Data System (ADS)

    Warren, Bethany; Malloy, Quentin G. J.; Yee, Lindsay D.; Cocker, David R.

    A series of 90 experiments were conducted in the UC Riverside/CE-CERT environmental chamber to evaluate the impact of water vapor and dissolved salts on secondary organic aerosol formation for cyclohexene ozonolysis. Water vapor (low - 30 ± 2% RH, medium - 46 ± 2% RH, high - 63 ± 2% RH) was found to directly participate in the atmospheric chemistry altering the composition of the condensing species, thus increasing total organic aerosol formation by ˜22% as compared to the system under dry (<0.1% RH) conditions. Hygroscopicity measurements also indicate that the organic aerosol composition is altered in the presence of gaseous water. These results are consistent with water vapor reacting with the crigee intermediate in the gas phase resulting in increased aldehyde formation. The addition of dissolved salts ((NH 4) 2SO 4, NH 4HSO 4, CaCl 2, NaCl) had minimal effect; only the (NH 4) 2SO 4 and NaCl were found to significantly impact the system with ˜10% increase in total organic aerosol formation. These results indicate that the organics may be partitioning to an outer organic shell as opposed to into the aqueous salt. Hygroscopicity measurements indicate that the addition of salts does not alter the aerosol composition for the dry or water vapor system.

  7. Vertical Distribution of Dust and Water Ice Aerosols from CRISM Limb-geometry Observations

    NASA Technical Reports Server (NTRS)

    Smith, Michael Doyle; Wolff, Michael J.; Clancy, Todd; Kleinbohl, Armin; Murchie, Scott L.

    2013-01-01

    [1] Near-infrared spectra taken in a limb-viewing geometry by the Compact Reconnaissance Imaging Spectrometer for Mars (CRISM) on board the Mars Reconnaissance Orbiter provide a useful tool for probing atmospheric structure. Specifically, the observed radiance as a function of wavelength and height above the limb enables the vertical distribution of both dust and water ice aerosols to be retrieved. More than a dozen sets of CRISM limb observations have been taken so far providing pole-to-pole cross sections, spanning more than a full Martian year. Radiative transfer modeling is used to model the observations taking into account multiple scattering from aerosols and the spherical geometry of the limb observations. Both dust and water ice vertical profiles often show a significant vertical structure for nearly all seasons and latitudes that is not consistent with the well-mixed or Conrath-v assumptions that have often been used in the past for describing aerosol vertical profiles for retrieval and modeling purposes. Significant variations are seen in the retrieved vertical profiles of dust and water ice aerosol as a function of season. Dust typically extends to higher altitudes (approx. 40-50km) during the perihelion season than during the aphelion season (<20km), and the Hellas region consistently shows more dust mixed to higher altitudes than other locations. Detached water ice clouds are common, and water ice aerosols are observed to cap the dust layer in all seasons.

  8. Aerosol absorption measurement at SWIR with water vapor interference using a differential photoacoustic spectrometer.

    PubMed

    Zhu, Wenyue; Liu, Qiang; Wu, Yi

    2015-09-07

    Atmospheric aerosol plays an important role in atmospheric radiation balance through absorbing and scattering the solar radiation, which changes local weather and global climate. Accurate measurement is highly requested to estimate the radiative effects and climate effects of atmospheric aerosol. Photoacoustic spectroscopy (PAS) technique, which observes the aerosols on their natural suspended state and is insensitive to light scattering, is commonly recognized as one of the best candidates to measure the optical absorption coefficient (OAC) of aerosols. In the present work, a method of measuring aerosol OAC at the wavelength where could also be absorbed by water vapor was proposed and corresponding measurements of the absorption properties of the atmospheric aerosol at the short wave infrared (SWIR, 1342 nm) wavelength were carried out. The spectrometer was made up of two high performance homemade photoacoustic cells. To improve the sensitivity, several methods were presented to control the noise derived from gas flow and vibration from the sampling pump. Calibration of the OAC and properties of the system were also studied in detail. Using the established PAS instrument, measurement of the optical absorption properties of the atmospheric aerosol were carried out in laboratory and field environment.

  9. Determination of four heterocyclic insecticides by ionic liquid dispersive liquid-liquid microextraction in water samples.

    PubMed

    Liu, Yu; Zhao, Ercheng; Zhu, Wentao; Gao, Haixiang; Zhou, Zhiqiang

    2009-02-06

    A novel microextraction method termed ionic liquid dispersive liquid-liquid microextraction (IL-DLLME) combining high-performance liquid chromatography with diode array detection (HPLC-DAD) was developed for the determination of insecticides in water samples. Four heterocyclic insecticides (fipronil, chlorfenapyr, buprofezin, and hexythiazox) were selected as the model compounds for validating this new method. This technique combines extraction and concentration of the analytes into one step, and the ionic liquid was used instead of a volatile organic solvent as the extraction solvent. Several important parameters influencing the IL-DLLME extraction efficiency such as the volume of extraction solvent, the type and volume of disperser solvent, extraction time, centrifugation time, salt effect as well as acid addition were investigated. Under the optimized conditions, good enrichment factors (209-276) and accepted recoveries (79-110%) were obtained for the extraction of the target analytes in water samples. The calibration curves were linear with correlation coefficient ranged from 0.9947 to 0.9973 in the concentration level of 2-100 microg/L, and the relative standard deviations (RSDs, n=5) were 4.5-10.7%. The limits of detection for the four insecticides were 0.53-1.28 microg/L at a signal-to-noise ratio (S/N) of 3.

  10. Liquid water sill emplacement on Europa?

    NASA Astrophysics Data System (ADS)

    Craft, K.; Patterson, G. W.; Lowell, R. P.

    2013-12-01

    Recent work has suggested that lithospheric flexure and flanking fractures observed along some ridges on Europa are best explained by the initial presence of a shallow liquid water sill. The emplacement of a sill suggests certain conditions existed that were favorable to water flow from the ocean to the subsurface, stresses that allowed horizontal fracturing for sill emplacement, and liquid water replenishment to enable a sill lifetime of ~ 1000s of years. Here, we investigate whether these conditions could occur and result in sill formation. Previous models of the stresses resulting from ice shell thickening on Europa indicated that fractures can initiate within the shell and propagate both upward toward the surface and downward to the ice-ocean interface. For an ~10 km thick ice shell, we determined that flow velocities for ocean water driven up a vertical fracture by the release of lithostatic pressures are adequate for reaching the subsurface before freezing occurs (LPSC #3033). We propose the next step for sill emplacement could occur through horizontal fracturing. Nominally, the stress field in a material under lithostatic load is conducive to vertical crack propagation. However, factors exist that can cause the stress field to change and propagate cracks horizontally. Seismically imaged terrestrial sills beneath mid-ocean ridges often occur in areas with extensive cracking and/or faulting, suggesting crack interactions may play a key role. Through application of a finite element program, we modeled four stress changing mechanisms and the resulting fracture propagation in a 10 km thick ice shell on Europa: (1) mechanical layering, (2) shallow cracks to the surface, (3) deep cracks from the ocean-ice interface and (4) shallow and deep cracks combined. Results determined that all mechanisms cause some turn in propagation direction, with Model 4 (both shallow and deep cracks) enabling the greatest turn to ~ horizontal. The horizontal extent of the fracture

  11. Polarized View of Supercooled Liquid Water Clouds

    NASA Technical Reports Server (NTRS)

    Alexandrov, Mikhail D.; Cairns, Brian; Van Diedenhoven, Bastiaan; Ackerman, Andrew S.; Wasilewski, Andrzej P.; McGill, Matthew J.; Yorks, John E.; Hlavka, Dennis L.; Platnick, Steven E.; Arnold, G. Thomas

    2016-01-01

    Supercooled liquid water (SLW) clouds, where liquid droplets exist at temperatures below 0 C present a well known aviation hazard through aircraft icing, in which SLW accretes on the airframe. SLW clouds are common over the Southern Ocean, and climate-induced changes in their occurrence is thought to constitute a strong cloud feedback on global climate. The two recent NASA field campaigns POlarimeter Definition EXperiment (PODEX, based in Palmdale, California, January-February 2013) and Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS, based in Houston, Texas in August- September 2013) provided a unique opportunity to observe SLW clouds from the high-altitude airborne platform of NASA's ER-2 aircraft. We present an analysis of measurements made by the Research Scanning Polarimeter (RSP) during these experiments accompanied by correlative retrievals from other sensors. The RSP measures both polarized and total reflectance in 9 spectral channels with wavelengths ranging from 410 to 2250 nm. It is a scanning sensor taking samples at 0.8deg intervals within 60deg from nadir in both forward and backward directions. This unique angular resolution allows for characterization of liquid water droplet size using the rainbow structure observed in the polarized reflectances in the scattering angle range between 135deg and 165deg. Simple parametric fitting algorithms applied to the polarized reflectance provide retrievals of the droplet effective radius and variance assuming a prescribed size distribution shape (gamma distribution). In addition to this, we use a non-parametric method, Rainbow Fourier Transform (RFT),which allows retrieval of the droplet size distribution without assuming a size distribution shape. We present an overview of the RSP campaign datasets available from the NASA GISS website, as well as two detailed examples of the retrievals. In these case studies we focus on cloud fields with spatial features

  12. Liquid penetration inside glass nozzle during bubble departures in water

    NASA Astrophysics Data System (ADS)

    Dzienis, P.; Mosdorf, R.; Augustyniak, J.

    2016-09-01

    Liquid penetration into the glass nozzle with inner diameter of 1 mm during the bubble, departures in distilled (surface tension = 65 mN/m) and not distilled (surface tension = 72 mN/m), water was investigated. It has been shown that dynamics of liquid movement inside the nozzle depend on the water surface tension. Maximum value of liquid penetration inside the nozzle is different for distilled and not distilled water. In not distilled water the depth of liquid penetration into the nozzle depends on air volume flow rate. For desilted water this value is constant.

  13. Ab Initio Quantum Simulations of Liquid Water

    NASA Astrophysics Data System (ADS)

    Gergely, John; Ceperley, David; Gygi, Francois

    2007-03-01

    Some recent efforts at simulating liquid water have employed ``ab initio'' molecular dynamics (AIMD) methods with forces from a version of density functional theory (DFT) and, in some cases, imaginary-time path integrals (PI) to study quantum effects of the protons. Although AIMD methods have met with many successes, errors introduced by the approximations and choices of simulation parameters are not fully understood. We report on path integral Monte Carlo (PIMC) studies of liquid water using DFT energies that provide quantitative benchmarks for PI-AIMD work. Specifically, we present convergence studies of the path integrals and address whether the Trotter number can be reduced by improving the form of the (approximate) action. Also, we assess 1) whether typical AIMD simulations are sufficiently converged in simulation time, i.e., if there is reason to suspect that nonergodic behavior in PI-AIMD methods leads to poor convergence, and 2) the relative efficiency of the methods. E. Schwegler, J.C. Grossman, F. Gygi, G. Galli, J. Chem. Phys 121, 5400 (2004).

  14. Monitoring of Sahelian aerosol and Atmospheric water vapor content characteristics from sun photometer measurements

    NASA Astrophysics Data System (ADS)

    Faizoun, C. A.; Podaire, A.; Dedieu, G.

    1994-11-01

    Atmospheric measurements in two Sahelian sites in West Africa are presented and analyzed. The measurements were performed using a sun photometer with five bands in the visible and near-infrared range of the solar spectrum. This instrument measures spectral values of the solar irradiances that are used to derive the aerosol optical thickness in three bands; the two other bands are used to derive the integrated atmospheric water vapor content using a differential absorption method. The Angstroem exponent, which is an estimate of the aerosol particle size, is derived from the spectral dependence of the optical thickness. Although the sites were located far from Sahara Desert aerosol sources, the observed aerosol optical thicknesses were high, with a mean annual value of 0.5 at 550 nm. The spectral dependence of aerosol optical thickness is generally low, with a mean annual value of Angstroem exponent of 0.4. The aerosol optical thickness and the atmosphereic water vapor content are both characterized by high temporal variability and exhibit seasonal cycles. From these measurements, climatological values and associated probability distribution laws are proposed.

  15. Aerosol contributions to speleothem geochemistry

    NASA Astrophysics Data System (ADS)

    Dredge, J. A.; Fairchild, I. J.; Harrison, R.; Woodhead, J. D.; Hellstrom, J.

    2011-12-01

    The term "aerosols" encompasses the suspension of both fine solid or liquid particles within a gaseous medium. Aerosols become suspended into the earth's atmosphere through a multitude of processes both natural and anthropogenic. Atmospheric aerosols enter cave networks as a result of cave ventilation processes and are either deposited, or cycled and removed from the system. Speleothem offer a multiproxy palaeoclimate resource; many of the available proxies have been extensively investigated and utilised for palaeoclimatic reconstructions in a range of studies. The potential contribution of aerosols to speleothem chemistry and their applicability for palaeoenvironmental reconstructions remains untested and the extent of their value as an addition to palaeoclimate sciences unknown. Aerosols through incorporation into speleothem may provide a novel palaeoenvironmental resource. The aerosol component of interest is that which is transported into the cave atmosphere and deposited and are available for incorporation into precipitated calcite. Aerosol deposition and therefore distribution in the cave has shown to be a complex function of ventilation and changing environmental factors. Through detailed monitoring aerosols have been detected, identified, characterised and quantified to determine their prominence in the cave system. Investigations are on a case study basis, searching for suitable aerosol proxies of environmentally significant emission processes. Case studies include: Palaeofires at Yarrangobilly Caves, Australia; anthropogenic emissions at St Michaels Cave, Gibraltar and Cheddar gorge, UK; and drip water aerosol production and geochemical addition in Obir cave, Austria. Monitoring has allowed for the temporal and spatial determination of aerosols in karst networks. Speleothem samples will be analysed in combination with in-situ monitoring to determine incorporation factors and record preservation. By understanding how aerosols are transmitted within the

  16. Fundamental studies with a monodisperse aerosol-based liquid chromatography/mass spectrometry interface (MAGIC-LC/MS)

    SciTech Connect

    Browner, R.F.

    1990-10-01

    Accomplishments on the fundamental studies with a monodisperse aerosol-based liquid chromatography/mass spectrometry (LC/MS) interface during the period 1 December 1989 to 30 November 1990 are summarized. In order to determine the influence of temperature on the vaporization and decomposition properties of molecules, test have been carried out on both thermally stable and thermally labile molecules. The test compounds used were a series of polynuclear aromatic (PAH) compounds covering a wide range of molecular weights from two-ring naphthalene to twelve-ring perylene. The less thermally stable species examined were aldicarb, a highly thermally labile pesticide, and cholesterol, which readily loses water when subjected to high temperatures. A new, externally heated probe, which can be raised to temperatures as high as 500{degree}C was also used. Matrix loading effects for a range of surface active and non-surface active compounds in three different matrices: glycerol, 3-nitrobenzyl alcohol, and thioglycerol for fast atom bombardment (FAB) particle beam LC/MS have been studied. The time dependence of FAB spectra generation in the particle beam system has been examined and contrasted with ion generation in normal probe FAB work. Future FAB LC/MS research is outlined. 3 refs. (BM)

  17. The Liquid Treasure Water History Trunk: Learning from the Past.

    ERIC Educational Resources Information Center

    Kesselheim, Alan S.; And Others

    This document is a guide to building a Liquid Treasure Water History Trunk that allows educators and students of all ages to learn about water from a historical perspective. By assembling historical water related items into a meaningful and interesting learning format--The Liquid Treasure Trunk--teachers and students of all ages can gain a glimpse…

  18. Evidence for Recent Liquid Water on Mars

    NASA Technical Reports Server (NTRS)

    2000-01-01

    Newton Crater is a large basin formed by an asteroid impact that probably occurred more than 3 billion years ago. It is approximately 287 kilometers (178 miles) across. The picture shown here (top) highlights the north wall of a specific, smaller crater located in the southwestern quarter of Newton Crater (above). The crater of interest was also formed by an impact; it is about 7 km (4.4 mi) across, which is about 7 times bigger than the famous Meteor Crater in northern Arizona in North America. The north wall of the small crater has many narrow gullies eroded into it. These are hypothesized to have been formed by flowing water and debris flows. Debris transported with the water created lobed and finger-like deposits at the base of the crater wall where it intersects the floor (bottom center top image). Many of the finger-like deposits have small channels indicating that a liquid, most likely water, flowed in these areas. Hundreds of individual water and debris flow events might have occurred to create the scene shown here. Each outburst of water from higher up on the crater slopes would have constituted a competition between evaporation, freezing, and gravity. The individual deposits at the ends of channels in this MOC image mosaic were used to get a rough estimate of the minimum amount of water that might be involved in each flow event. This is done first by assuming that the deposits are like debris flows on Earth. In a debris flow, no less than about 10% (and no more than 30%) of their volume is water. Second, the volume of an apron deposit is estimated by measuring the area covered in the MOC image and multiplying it by a conservative estimate of thickness, 2 meters (6.5 feet). For a flow containing only 10% water, these estimates conservatively suggest that about 2.5 million liters (660,000 gallons) of water are involved in each event; this is enough to fill about 7 community-sized swimming pools or enough to supply 20 people with their water needs for a year

  19. Reactivity of liquid and semisolid secondary organic carbon with chloride and nitrate in atmospheric aerosols

    SciTech Connect

    Wang, Bingbing; O'Brien, Rachel E.; Kelly, Stephen T.; Shilling, John E.; Moffet, Ryan C.; Gilles, Mary K.; Laskin, Alexander

    2015-05-14

    Constituents of secondary organic carbon (SOC) in atmospheric aerosols are often mixed with inorganic components and compose a significant mass fraction of fine particulate matter in the atmosphere. Interactions between SOC and other condensed-phase species are not well understood. Here, we investigate the reactions of liquid-like and semi-solid SOC from ozonolysis of limonene (LSOC) and α-pinene (PSOC) with NaCl using a set of complementary micro-spectroscopic analyses. These reactions result in chloride depletion in the condensed phase, release of gaseous HCl, and formation of organic salts. The reactions attributed to acid displacement by SOC acidic components are driven by the high volatility of HCl. Similar reactions can take place in SOC/NaNO₃ particles. The results show that an increase in SOC mass fraction in the internally mixed SOC/NaCl particles leads to higher chloride depletion. Glass transition temperatures and viscosity of PSOC were estimated for atmospherically relevant conditions. Data show that the reaction extent depends on SOC composition, particle phase state and viscosity, mixing state, temperature, relative humidity (RH), and reaction time. LSOC shows slightly higher potential to deplete chloride than PSOC. Higher particle viscosity at low temperatures and RH can hinder these acid displacement reactions. Formation of organic salts from these overlooked reactions can alter particle physiochemical properties and may affect their reactivity and ability to act as cloud condensation and ice nuclei. The release and potential recycling of HCl and HNO₃ from reacted aerosol particles may have important implications for atmospheric chemistry.

  20. CART Raman Lidar Aerosol and Water Vapor Measurements in the Vicinity of Clouds

    NASA Technical Reports Server (NTRS)

    Clayton, Marian B.; Ferrare, Richard A.; Turner, David; Newsom, Rob; Sivaraman, Chitra

    2008-01-01

    Aerosol and water vapor profiles acquired by the Raman lidar instrument located at the Climate Research Facility (CRF) at Southern Great Plains (SGP) provide data necessary to investigate the atmospheric variability in the vicinity of clouds near the top of the planetary boundary layer (PBL). Recent CARL upgrades and modifications to the routine processing algorithms afforded the necessarily high temporal and vertical data resolutions for these investigations. CARL measurements are used to investigate the behavior of aerosol backscattering and extinction and their correlation with water vapor and relative humidity.

  1. Optical Fluorescence Detected from X-ray Irradiated Liquid Water.

    PubMed

    Hans, Andreas; Ozga, Christian; Seidel, Robert; Schmidt, Philipp; Ueltzhöffer, Timo; Holzapfel, Xaver; Wenzel, Philip; Reiß, Philipp; Pohl, Marvin N; Unger, Isaak; Aziz, Emad F; Ehresmann, Arno; Slavíček, Petr; Winter, Bernd; Knie, André

    2017-03-16

    Despite its importance, the structure and dynamics of liquid water are still poorly understood in many apsects. Here, we report on the observation of optical fluorescence upon soft X-ray irradiation of liquid water. Detection of spectrally resolved fluorescence was achieved by a combination of the liquid microjet technique and fluorescence spectroscopy. We observe a genuine liquid-phase fluorescence manifested by a broad emission band in the 170-340 nm (4-7 eV) photon wavelength range. In addition, another narrower emission near 300 nm can be assigned to the fluorescence of OH (A state) in the gas phase, the emitting species being formed by Auger electrons escaping from liquid water. We argue that the newly observed broad-band emission of liquid water is relevant in search of extraterrestrial life, and we also envision the observed electron-ejection mechanism to find application for exploring solutes at liquid-vapor interfaces.

  2. Organic peroxide and OH formation in aerosol and cloud water: laboratory evidence for this aqueous chemistry

    NASA Astrophysics Data System (ADS)

    Lim, Y. B.; Turpin, B. J.

    2015-06-01

    Aqueous chemistry in atmospheric waters (e.g., cloud droplets or wet aerosols) is well accepted as an atmospheric pathway to produce secondary organic aerosol (SOAaq). Water-soluble organic compounds with small carbon numbers (C2-C3) are precursors for SOAaq and products include organic acids, organic sulfates, and high molecular weight compounds/oligomers. Fenton reactions and the uptake of gas-phase OH radicals are considered to be the major oxidant sources for aqueous organic chemistry. However, the sources and availability of oxidants in atmospheric waters are not well understood. The degree to which OH is produced in the aqueous phase affects the balance of radical and non-radical aqueous chemistry, the properties of the resulting aerosol, and likely its atmospheric behavior. This paper demonstrates organic peroxide formation during aqueous photooxidation of methylglyoxal using ultra high resolution Fourier Transform Ion Cyclotron Resonance electrospray ionization mass spectrometry (FTICR-MS). Organic peroxides are known to form through gas-phase oxidation of volatile organic compounds. They contribute secondary organic aerosol (SOA) formation directly by forming peroxyhemiacetals, and epoxides, and indirectly by enhancing gas-phase oxidation through OH recycling. We provide simulation results of organic peroxide/peroxyhemiacetal formation in clouds and wet aerosols and discuss organic peroxides as a source of condensed-phase OH radicals and as a contributor to aqueous SOA.

  3. Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China

    PubMed Central

    Cheng, Yafang; Zheng, Guangjie; Wei, Chao; Mu, Qing; Zheng, Bo; Wang, Zhibin; Gao, Meng; Zhang, Qiang; He, Kebin; Carmichael, Gregory; Pöschl, Ulrich; Su, Hang

    2016-01-01

    Fine-particle pollution associated with winter haze threatens the health of more than 400 million people in the North China Plain. Sulfate is a major component of fine haze particles. Record sulfate concentrations of up to ~300 μg m−3 were observed during the January 2013 winter haze event in Beijing. State-of-the-art air quality models that rely on sulfate production mechanisms requiring photochemical oxidants cannot predict these high levels because of the weak photochemistry activity during haze events. We find that the missing source of sulfate and particulate matter can be explained by reactive nitrogen chemistry in aerosol water. The aerosol water serves as a reactor, where the alkaline aerosol components trap SO2, which is oxidized by NO2 to form sulfate, whereby high reaction rates are sustained by the high neutralizing capacity of the atmosphere in northern China. This mechanism is self-amplifying because higher aerosol mass concentration corresponds to higher aerosol water content, leading to faster sulfate production and more severe haze pollution. PMID:28028539

  4. Airborne water vapor DIAL system and measurements of water and aerosol profiles

    NASA Technical Reports Server (NTRS)

    Higdon, Noah S.; Browell, Edward V.

    1991-01-01

    The Lidar Applications Group at NASA Langley Research Center has developed a differential absorption lidar (DIAL) system for the remote measurement of atmospheric water vapor (H2O) and aerosols from an aircraft. The airborne H2O DIAL system is designed for extended flights to perform mesoscale investigations of H2O and aerosol distributions. This DIAL system utilizes a Nd:YAG-laser-pumped dye laser as the off-line transmitter and a narrowband, tunable Alexandrite laser as the on-line transmitter. The dye laser has an oscillator/amplifier configuration which incorporates a grating and prism in the oscillator cavity to narrow the output linewidth to approximately 15 pm. This linewidth can be maintained over the wavelength range of 725 to 730 nm, and it is sufficiently narrow to satisfy the off-line spectral requirements. In the Alexandrite laser, three intracavity tuning elements combine to produce an output linewidth of 1.1 pm. These spectral devices include a five-plate birefringent tuner, a 1-mm thick solid etalon and a 1-cm air-spaced etalon. A wavelength stability of +/- 0.35 pm is achieved by active feedback control of the two Fabry-Perot etalons using a frequency stabilized He-Ne laser as a wavelength reference. The three tuning elements can be synchronously scanned over a 150 pm range with microprocessor-based scanning electronics. Other aspects of the DIAL system are discussed.

  5. Contrasting the Evaporation and Condensation of Water from Glassy and Amorphous Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Reid, J. P.; Bones, D. L.; Power, R.; Lienhard, D.; Krieger, U. K.

    2012-04-01

    The partitioning of water between the condensed and gas phases in atmospheric aerosol is usually assumed to occur instantaneously and to be regulated by solution thermodynamics. However, the persistence of high viscosity, glassy and amorphous aerosol to low relative humidity without crystallisation occurring is now widely recognised, suggesting that the timescale for water transport to or from the particle during condensation or evaporation may be significant. A kinetic limitation on water transport could have important implications for understanding hygroscopic growth measurements made on ambient particles, the ability of particles to act as ice nuclei or cloud condensation nuclei, the kinetics of chemical aging/heterogeneous chemistry, and the rate or condensation/evaporation of semi-volatile organic components. In this study we will report on measurements of the timescale of water transport to and from glassy aerosol and ultra-high viscosity solution droplets using aerosol optical tweezers to investigate the time-response of single particles to changes in relative humidity. As a benchmark system, mixed component aerosol particles containing sucrose and sodium chloride have been used; varying the mole fractions of the two solutes allows a wide range of solution viscosities to be studied. We will show that coarse particles can take many thousands of seconds to equilibrate in size and that the timescale correlates with the estimated bulk viscosity of the particle. We will also confirm that significant inhomogeneities in particle composition can be established during evaporation or condensation. Using the experimental data to benchmark a model for equilibration time, predictions can be made of the timescale for the equilibration of accumulation mode particles during water condensation or evaporation and these predictions will be described and their significance explored. Finally, the coalescence dynamics of highly viscous aerosol particles will be reported

  6. Liquid-liquid transition without macroscopic phase separation in a water-glycerol mixture

    NASA Astrophysics Data System (ADS)

    Murata, Ken-Ichiro; Tanaka, Hajime

    2012-05-01

    The existence of more than two liquid states in a single-component substance and the ensuing liquid-liquid transitions (LLTs) has attracted considerable attention because of its counterintuitive nature and its importance in the fundamental understanding of the liquid state. Here we report direct experimental evidence for a genuine (isocompositional) LLT without macroscopic phase separation in an aqueous solution of glycerol. We show that liquid I transforms into liquid II by way of two types of kinetics: nucleation and growth, and spinodal decomposition. Although liquid II is metastable against crystallization, we could access both its static and dynamical properties experimentally. We find that liquids I and II differ in density, refractive index, structure, hydrogen bonding state, glass transition temperature and fragility, and that the transition between the two liquids is mainly driven by the local structuring of water rather than of glycerol, suggesting a link to a plausible LLT inpure water.

  7. Modulated exponential films generated by surface acoustic waves and their role in liquid wicking and aerosolization at a pinned drop

    NASA Astrophysics Data System (ADS)

    Taller, Daniel; Go, David B.; Chang, Hsueh-Chia

    2013-05-01

    The exponentially decaying acoustic pressure of scattered surface acoustic waves (SAWs) at the contact line of a liquid film pinned to filter paper is shown to sustain a high curvature conic tip with micron-sized modulations whose dimension grows exponentially from the tip. The large negative capillary pressure in the film, necessary for offsetting the large positive acoustic pressure at the contact line, also creates significant negative hydrodynamic pressure and robust wicking action through the paper. An asymptotic analysis of this intricate pressure matching between the quasistatic conic film and bulk drop shows that the necessary SAW power to pump liquid from the filter paper and aerosolize, expressed in terms of the acoustic pressure scaled by the drop capillary pressure, grows exponentially with respect to twice the acoustic decay constant multiplied by the drop length, with a universal preexponential coefficient. Global rapid aerosolization occurs at a SAW power twice as high, beyond which the wicking rate saturates.

  8. Modulated exponential films generated by surface acoustic waves and their role in liquid wicking and aerosolization at a pinned drop.

    PubMed

    Taller, Daniel; Go, David B; Chang, Hsueh-Chia

    2013-05-01

    The exponentially decaying acoustic pressure of scattered surface acoustic waves (SAWs) at the contact line of a liquid film pinned to filter paper is shown to sustain a high curvature conic tip with micron-sized modulations whose dimension grows exponentially from the tip. The large negative capillary pressure in the film, necessary for offsetting the large positive acoustic pressure at the contact line, also creates significant negative hydrodynamic pressure and robust wicking action through the paper. An asymptotic analysis of this intricate pressure matching between the quasistatic conic film and bulk drop shows that the necessary SAW power to pump liquid from the filter paper and aerosolize, expressed in terms of the acoustic pressure scaled by the drop capillary pressure, grows exponentially with respect to twice the acoustic decay constant multiplied by the drop length, with a universal preexponential coefficient. Global rapid aerosolization occurs at a SAW power twice as high, beyond which the wicking rate saturates.

  9. Air and water stable ionic liquids in physical chemistry.

    PubMed

    Endres, Frank; Zein El Abedin, Sherif

    2006-05-14

    Ionic liquids are defined today as liquids which solely consist of cations and anions and which by definition must have a melting point of 100 degrees C or below. Originating from electrochemistry in AlCl(3) based liquids an enormous progress was made during the recent 10 years to synthesize ionic liquids that can be handled under ambient conditions, and today about 300 ionic liquids are already commercially available. Whereas the main interest is still focussed on organic and technical chemistry, various aspects of physical chemistry in ionic liquids are discussed now in literature. In this review article we give a short overview on physicochemical aspects of ionic liquids, such as physical properties of ionic liquids, nanoparticles, nanotubes, batteries, spectroscopy, thermodynamics and catalysis of/in ionic liquids. The focus is set on air and water stable ionic liquids as they will presumably dominate various fields of chemistry in future.

  10. Aerosol scattering effects on water vapor retrievals over the Los Angeles Basin

    NASA Astrophysics Data System (ADS)

    Zeng, Zhao-Cheng; Zhang, Qiong; Natraj, Vijay; Margolis, Jack S.; Shia, Run-Lie; Newman, Sally; Fu, Dejian; Pongetti, Thomas J.; Wong, Kam W.; Sander, Stanley P.; Wennberg, Paul O.; Yung, Yuk L.

    2017-02-01

    In this study, we propose a novel approach to describe the scattering effects of atmospheric aerosols in a complex urban environment using water vapor (H2O) slant column measurements in the near infrared. This approach is demonstrated using measurements from the California Laboratory for Atmospheric Remote Sensing Fourier Transform Spectrometer on the top of Mt. Wilson, California, and a two-stream-exact single scattering (2S-ESS) radiative transfer (RT) model. From the spectral measurements, we retrieve H2O slant column density (SCD) using 15 different absorption bands between 4000 and 8000 cm-1. Due to the wavelength dependence of aerosol scattering, large variations in H2O SCD retrievals are observed as a function of wavelength. Moreover, the variations are found to be correlated with aerosol optical depths (AODs) measured at the AERONET-Caltech station. Simulation results from the RT model reproduce this correlation and show that the aerosol scattering effect is the primary contributor to the variations in the wavelength dependence of the H2O SCD retrievals. A significant linear correlation is also found between variations in H2O SCD retrievals from different bands and corresponding AOD data; this correlation is associated with the asymmetry parameter, which is a first-order measure of the aerosol scattering phase function. The evidence from both measurements and simulations suggests that wavelength-dependent aerosol scattering effects can be derived using H2O retrievals from multiple bands. This understanding of aerosol scattering effects on H2O retrievals suggests a promising way to quantify the effect of aerosol scattering on greenhouse gas retrievals and could potentially contribute towards reducing biases in greenhouse gas retrievals from space.

  11. Physics-Based Modeling of Permeation: Simulation of Low-Volatility Agent Permeation and Aerosol Vapor Liquid Assessment Group Experiments

    DTIC Science & Technology

    2015-06-01

    PHYSICS-BASED MODELING OF PERMEATION: SIMULATION OF LOW-VOLATILITY AGENT PERMEATION AND AEROSOL VAPOR LIQUID...REPORT TYPE Final 3. DATES COVERED (From - To) Jan 2014 – Sep 2014 4. TITLE AND SUBTITLE Physics-Based Modeling of Permeation: Simulation of Low...Approved for public release; distribution is unlimited. 13. SUPPLEMENTARY NOTES 14. ABSTRACT: Physics-based models were developed to predict agent

  12. Size matters in the water uptake and hygroscopic growth of atmospherically relevant multicomponent aerosol particles.

    PubMed

    Laskina, Olga; Morris, Holly S; Grandquist, Joshua R; Qin, Zhen; Stone, Elizabeth A; Tivanski, Alexei V; Grassian, Vicki H

    2015-05-14

    Understanding the interactions of water with atmospheric aerosols is crucial for determining the size, physical state, reactivity, and climate impacts of this important component of the Earth's atmosphere. Here we show that water uptake and hygroscopic growth of multicomponent, atmospherically relevant particles can be size dependent when comparing 100 nm versus ca. 6 μm sized particles. It was determined that particles composed of ammonium sulfate with succinic acid and of a mixture of chlorides typical of the marine environment show size-dependent hygroscopic behavior. Microscopic analysis of the distribution of components within the aerosol particles show that the size dependence is due to differences in the mixing state, that is, whether particles are homogeneously mixed or phase separated, for different sized particles. This morphology-dependent hygroscopicity has consequences for heterogeneous atmospheric chemistry as well as aerosol interactions with electromagnetic radiation and clouds.

  13. Tropospheric aerosols remote sensing over the water surface of Penang Island

    NASA Astrophysics Data System (ADS)

    Hashim, S. A.; MatJafri, M. Z.; Abdullah, K.; Lim, H. S.; Wong, C. J.; Salleh, N. Mohd.

    2006-05-01

    Tropospheric aerosols play an important role in climate change. Aerosols are typically studied over deep clear water, due to the relatively constant reflectance of water and the ability to easily separate surface and atmospheric contributions on the satellite signal. A methodology based on multi-spectral approach was employed to map tropospheric aerosols concentrations over the water areas surrounding Penang Island. The aim of this study was to estimate the pollutants concentrations using remote sensing techniques. In this study, we attempted to derive AOT (Aerosol Optical Thickness) values from the sky transmittance measurements in the visible spectrum. The transmittance values were measured at the sea surface using a handheld spectroradiometer. The correspond PM10 readings were taken simultaneously during the transmittance measurements acquisition of the imageries using a Dust Trak meter. The PCI Geomatica version 9.1 digital image processing software was used in all image-processing analyses. The results produced a linear relationship between PM10 and AOT values over the water surface of Penang Island. Finally, The PM10 concentration map over the water surface of Penang Island was generated using Kriging interpolation technique. This study has indicated the potential use of a handheld spectroradiometer for air quality study.

  14. Dissolved organic matter in sea spray: a transfer study from marine surface water to aerosols

    NASA Astrophysics Data System (ADS)

    Schmitt-Kopplin, P.; Liger-Belair, G.; Koch, B. P.; Flerus, R.; Kattner, G.; Harir, M.; Kanawati, B.; Lucio, M.; Tziotis, D.; Hertkorn, N.; Gebefügi, I.

    2012-04-01

    Atmospheric aerosols impose direct and indirect effects on the climate system, for example, by absorption of radiation in relation to cloud droplets size, on chemical and organic composition and cloud dynamics. The first step in the formation of Organic primary aerosols, i.e. the transfer of dissolved organic matter from the marine surface into the atmosphere, was studied. We present a molecular level description of this phenomenon using the high resolution analytical tools of Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) and nuclear magnetic resonance spectroscopy (NMR). Our experiments confirm the chemoselective transfer of natural organic molecules, especially of aliphatic compounds from the surface water into the atmosphere via bubble bursting processes. Transfer from marine surface water to the atmosphere involves a chemical gradient governed by the physicochemical properties of the involved molecules when comparing elemental compositions and differentiating CHO, CHNO, CHOS and CHNOS bearing compounds. Typical chemical fingerprints of compounds enriched in the aerosol phase were CHO and CHOS molecular series, smaller molecules of higher aliphaticity and lower oxygen content, and typical surfactants. A non-targeted metabolomics analysis demonstrated that many of these molecules corresponded to homologous series of oxo-, hydroxy-, methoxy-, branched fatty acids and mono-, di- and tricarboxylic acids as well as monoterpenes and sugars. These surface active biomolecules were preferentially transferred from surface water into the atmosphere via bubble bursting processes to form a significant fraction of primary organic aerosols. This way of sea spray production leaves a selective biological signature of the surface water in the corresponding aerosol that may be transported into higher altitudes up to the lower atmosphere, thus contributing to the formation of secondary organic aerosol on a global scale or transported laterally with

  15. Modeling Aerosol Effects on Clouds and Precipitation: Insights from CalWater 2015

    NASA Astrophysics Data System (ADS)

    Leung, L. R.; Lim, K. S. S.; Fan, J.; Prather, K. A.; DeMott, P. J.; Spackman, J. R.; Ralph, F. M.

    2015-12-01

    The CalWater 2015 field campaign took place in northern California from mid January through early March of 2015. The field campaign, including collaborations between CalWater 2 and ACAPEX, aims to improve understanding and modeling of large-scale dynamics and cloud and precipitation processes associated with atmospheric rivers (ARs) and aerosol-cloud interactions that influence precipitation variability and extremes in the western U.S. An observational strategy was employed using land and offshore assets to monitor (1) the evolution and structure of ARs from near their regions of development, (2) long range transport of aerosols in eastern North Pacific and potential interactions with ARs, and (3) how aerosols from long-range transport and local sources influence cloud and precipitation in the U.S. During the field campaign, an AR developed in the Northeast Pacific Ocean in early February and made landfall in northern California. In-situ aerosol and cloud measurements from the G-1 aircraft; remote sensing data of clouds and aerosols; and meteorological measurements from aircraft, ship, and ground-based instruments collected from February 5 - 8, 2015 are analyzed to characterize the large-scale environment and cloud and precipitation forming processes. Modeling experiments are designed using a regional model for simulations with a cloud resolving limited area domain and quasi-global coarser resolution domain to evaluate the impacts of aerosols on clouds and precipitation, and to explore the relative contributions of long-range transported and regional aerosols that interacted with the clouds before, during, and after AR landfall. Preliminary results will be discussed in the context of the field data as well as a multi-year simulation of the climatological contributions of long-range transported dust during AR landfall in California.

  16. Techniques of Validation of Aerosol and Water Vapor Retrievals From MODIS

    NASA Technical Reports Server (NTRS)

    Ichoku, Charles; Chu, Allen; Mattoo, Shana; Kaufman, Yoram; Remer, Lorraine; Tanre, Didier; Slutsker, Ilya; Holben, Brent N.; Einaudi, Franco (Technical Monitor)

    2001-01-01

    Aerosols are extremely important for global climate studies and modeling in the quest to characterize the global radiation budget and forcing. The physical characteristics, composition, abundance, and spatial distribution and dynamics of aerosols are still very poorly known. Aerosol column optical thickness and other parameters as well as column precipitable water vapor amount are some of the main atmospheric parameters retrieved from the MODIS instrument on board the Terra satellite. To ensure the reliability of these parameters, we have embarked on a very massive validation effort. This involves cross correlation between the retrievals from the satellite data and those obtained from sunphotometer measurements at a large number of ground stations spread throughout the globe. Notable among these ground stations is a large network of over 100 stations coordinated under the Aerosol Robotic Network (AERONET) project. Whereas MODIS retrieves the aerosol parameters throughout the globe once or twice a day during the daytime, the ground measurements cover only discrete locations of the earth, though the retrievals are done several times a day. We have devised a method to. match the MODIS and ground retrievals through spatial statistics for the MODIS data and temporal statistics for the ground data. This has produced good comparisons and has enabled the validation of MODIS aerosol and water vapor retrievals at over 100 discrete locations in various parts of the earth both over the land and over the ocean. Currently, the validation statistical data is produced routinely by the MODIS aerosol group and is even available not only for validation but also for use by the science community for short and long term studies at various parts of the earth. One important advantage is that the system can be expanded to incorporate more locations where ground measurements and other studies may be conducted at any time during the lifetime of MODIS.

  17. Solid/liquid phase diagram of the ammonium sulfate/succinic acid/water system.

    PubMed

    Pearson, Christian S; Beyer, Keith D

    2015-05-14

    We have studied the low-temperature phase diagram and water activities of the ammonium sulfate/succinic acid/water system using differential scanning calorimetry and infrared spectroscopy of thin films. Using the results from our experiments, we have mapped the solid/liquid ternary phase diagram, determined the water activities based on the freezing point depression, and determined the ice/succinic acid phase boundary as well as the ternary eutectic composition and temperature. We also compared our results to the predictions of the extended AIM aerosol thermodynamics model (E-AIM) and found good agreement for the ice melting points in the ice primary phase field of this system; however, differences were found with respect to succinic acid solubility temperatures. We also compared the results of this study with those of previous studies that we have published on ammonium sulfate/dicarboxylic acid/water systems.

  18. Interactions between water and 1-butyl-1-methylpyrrolidinium ionic liquids

    NASA Astrophysics Data System (ADS)

    Fadeeva, Tatiana A.; Husson, Pascale; DeVine, Jessalyn A.; Costa Gomes, Margarida F.; Greenbaum, Steven G.; Castner, Edward W.

    2015-08-01

    We report experimental results on the diffusivity of water in two ionic liquids obtained using the pulsed-gradient spin-echo NMR method. Both ionic liquids have the same cation, 1-butyl-1-methylpyrrolidinium, but different trifluoromethyl-containing anions. One has a strongly hydrophobic anion, bis(trifluoromethylsulfonyl)amide, while the second has a hydrophilic anion, trifluoromethylsulfonate. Transport of water in these ionic liquids is much faster than would be predicted from hydrodynamic laws, indicating that the neutral water molecules experience a very different friction than the anions and cations at the molecular level. Temperature-dependent viscosities, conductivities, and densities are reported as a function of water concentration to further analyze the properties of the ionic liquid-water mixtures. These results on the properties of water in ionic liquids should be of interest to researchers in diverse areas ranging from separations, solubilizing biomass and energy technologies.

  19. Interactions between water and 1-butyl-1-methylpyrrolidinium ionic liquids.

    PubMed

    Fadeeva, Tatiana A; Husson, Pascale; DeVine, Jessalyn A; Costa Gomes, Margarida F; Greenbaum, Steven G; Castner, Edward W

    2015-08-14

    We report experimental results on the diffusivity of water in two ionic liquids obtained using the pulsed-gradient spin-echo NMR method. Both ionic liquids have the same cation, 1-butyl-1-methylpyrrolidinium, but different trifluoromethyl-containing anions. One has a strongly hydrophobic anion, bis(trifluoromethylsulfonyl)amide, while the second has a hydrophilic anion, trifluoromethylsulfonate. Transport of water in these ionic liquids is much faster than would be predicted from hydrodynamic laws, indicating that the neutral water molecules experience a very different friction than the anions and cations at the molecular level. Temperature-dependent viscosities, conductivities, and densities are reported as a function of water concentration to further analyze the properties of the ionic liquid-water mixtures. These results on the properties of water in ionic liquids should be of interest to researchers in diverse areas ranging from separations, solubilizing biomass and energy technologies.

  20. Interactions between water and 1-butyl-1-methylpyrrolidinium ionic liquids

    SciTech Connect

    Fadeeva, Tatiana A.; DeVine, Jessalyn A.; Castner, Edward W.; Husson, Pascale; Costa Gomes, Margarida F.; Greenbaum, Steven G.

    2015-08-14

    We report experimental results on the diffusivity of water in two ionic liquids obtained using the pulsed-gradient spin-echo NMR method. Both ionic liquids have the same cation, 1-butyl-1-methylpyrrolidinium, but different trifluoromethyl-containing anions. One has a strongly hydrophobic anion, bis(trifluoromethylsulfonyl)amide, while the second has a hydrophilic anion, trifluoromethylsulfonate. Transport of water in these ionic liquids is much faster than would be predicted from hydrodynamic laws, indicating that the neutral water molecules experience a very different friction than the anions and cations at the molecular level. Temperature-dependent viscosities, conductivities, and densities are reported as a function of water concentration to further analyze the properties of the ionic liquid-water mixtures. These results on the properties of water in ionic liquids should be of interest to researchers in diverse areas ranging from separations, solubilizing biomass and energy technologies.

  1. 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.

  2. 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

  3. Some results of water vapor, ozone and aerosol balloon borne measurements during EASOE

    NASA Astrophysics Data System (ADS)

    Khattatov, V.; Yushkov, V.; Khaplanov, M.; Zaitzev, I.; Rosen, J.; Kjome, N.

    As part of the European Arctic Stratospheric Ozone Experiment (EASOE) in the northern winter of 1991/92, regular measurements of the vertical distribution of ozone and aerosols were carried out from two Russian polar stations, Heiss Island (81N, 58E) and Dikson Island (73N, 81E). In addition measurements of the vertical distribution of water vapor and aerosols were made from Esrange (68N, 21E), near Kiruna in Sweden. The instruments used were electrochemical ozone sondes (ECC-4A), a fluorescence hygrometer, and the University of Wyoming backscattersonde. Following the eruption of Mt.Pinatubo, in the Philippines, in June 1991, volcanic aerosol had reached Arctic latitudes at altitudes below 19 km by September. At all three sites it was observed on every flight. Polar stratospheric clouds were encountered above the volcanic aerosol on two flights from Esrange. There were no indications of dehydration in the Arctic stratosphere. On all flights the minimum mixing ratio of water vapor was observed 2 to 3 km above the tropopause. Total ozone was much lower than the climatological mean, over Dikson Island from the January 27, and over Heiss Island from mid-February, until the end of EASOE. Ozone profiles over these stations showed rapid increases in partial pressure immediately above the peak values of backscatter ratio when the volcanic aerosol was especially dense.

  4. First lidar measurements of water vapor and aerosols from a high-altitude aircraft

    NASA Technical Reports Server (NTRS)

    Browell, Edward V.; Ismail, Syed

    1995-01-01

    Water vapor plays an important role in many atmospheric processes related to radiation, climate change, atmospheric dynamics, meteorology, the global hydrologic cycle, and atmospheric chemistry, and yet our knowledge of the global distribution of water vapor is very limited. The differential absorption lidar (DIAL) technique has the potential of providing needed high resolution water vapor measurements from aircraft and from space, and the Lidar Atmospheric Sensing Experiment (LASE) is a key step in the development of this capability. The LASE instrument is the first fully engineered, autonomous DIAL system, and it is designed to operate from a high-altitude aircraft (ER-2) and to make water vapor and aerosol profile measurements across the troposphere. The LASE system was flown from the NASA Wallops Flight Facility in a series of engineering flights during September 1994. This paper discusses the characteristics of the LASE system and presents the first LASE measurements of water vapor and aerosol profiles.

  5. Speciation and water soluble fraction of iron in aerosols from various sources

    NASA Astrophysics Data System (ADS)

    Takahashi, Y.; Kurisu, M.; Uematsu, M.

    2015-12-01

    Iron (Fe) is an essential micronutrient and has been identified as a limiting factor for phytoplankton growth in high-nitrate low-chlorophyll (HNLC) regions of the ocean. In the North Pacific, three sources of iron (Fe) transported via. atmosphere can be suggested: (i) mineral dust from East Asia, (ii) anthropogenic Fe, and (iii) aerosols from volcanic origin. Considering these different sources, Fe can be found and transported in a variety of chemical forms, both water-soluble and -insoluble. It is generally believed that only the soluble fraction of Fe can be considered as bioavailable for phytoplankton. To assess the biogeochemical impact of the atmospheric input, attempt was made to determine Fe species by X-ray absorption spectroscopy (XAS) and its water solubility, in particular to compare the three sources. Iron species, chemical composition, and soluble Fe concentration in aerosol collected at Tsukuba (Japan) through a year were investigated to compare the contributions of mineral dust and anthropogenic components. It was found that the concentration of soluble Fe in aerosol is correlated with those of sulfate and oxalate which originate from anthropogenic sources, suggesting that soluble Fe is mainly derived from anthropogenic sources. XAS analysis showed that main Fe species in aerosols in Tsukuba were illite, ferrihydrite, hornblende, and Fe(III) sulfate. Moreover, soluble Fe fraction is closely correlated with that of Fe(III) sulfate. In spite of supply of high concentrations of Fe in mineral dust from East Asia, it was found that anthropogenic fraction is important due to its high water solubility by the presence of Fe(III) sulfate. Marine aerosol samples originated from volcanic ash were collected in the western North Pacific during KH-08-2 cruise (August, 2008). XAS analysis suggested that Fe species of volcanic ashes changed during the long-range transport, while dissolution experiment showed that Fe solubility of the marine aerosol is larger than

  6. Formation mechanisms of water-soluble organic compounds in atmospheric aerosols

    NASA Astrophysics Data System (ADS)

    Huang, Xiaofeng

    Water-soluble organic compounds (WSOCs) are abundant in atmospheric aerosols, typically accounting for 20˜80% of particulate organic matter mass. Due to their affinity for water, WSOCs play an active role in aerosol-water interaction, and thus influence hygroscopic properties of aerosols, which in turn affect cloud formation processes and earth's radiation balance. Despite their abundance and significance, the sources of WSOCs are not well understood. Some primary sources (e.g., biomass burning) are known to emit WSOCs. It is also known from smog chamber experiments that photochemical oxidation of volatile organic compounds lead to less volatile oxygenated compounds that reside in the aerosol phase and are water-soluble because of the presence of polar functional groups. More recent work points to in-cloud/fog processes as a potentially important source for WSOCs. Work in this thesis aims to improve our understanding of the sources and formation mechanisms of WSOCs in atmospheric aerosols. Multiple approaches have been taken, including field measurements and controlled laboratory experiments. The thesis consists of the following four parts: (1) The formation mechanism of the most abundant WSOC species, oxalate, was investigated by synthesizing field measurement data obtained by our group and those available in the literature. Our measurements of aerosol sulfate and oxalate across a wide geographical span in the East Asia region, up to Beijing in the north and down to Hong Kong in the south, indicated that the two species were highly correlated. This good correlation was also found in measurements made elsewhere in the world by other researchers. Through a detailed analysis of factors influencing ambient oxalate, it can be argued that a common dominant formation pathway, likely in-cloud processing, explains the close tracking of the two chemically distinct species. This result also highlights the potential importance of in-cloud processing as a pathway leading to

  7. Raman lidar and sun photometer measurements of aerosols and water vapor during the ARM RCS experiment

    NASA Technical Reports Server (NTRS)

    Ferrare, R. A.; Whiteman, D. N.; Melfi, S. H.; Evans, K. D.; Holben, B. N.

    1995-01-01

    The first Atmospheric Radiation Measurement (ARM) Remote Cloud Study (RCS) Intensive Operations Period (IOP) was held during April 1994 at the Southern Great Plains (SGP) Cloud and Radiation Testbed (CART) site near Lamont, Oklahoma. This experiment was conducted to evaluate and calibrate state-of-the-art, ground based remote sensing instruments and to use the data acquired by these instruments to validate retrieval algorithms developed under the ARM program. These activities are part of an overall plan to assess general circulation model (GCM) parameterization research. Since radiation processes are one of the key areas included in this parameterization research, measurements of water vapor and aerosols are required because of the important roles these atmospheric constituents play in radiative transfer. Two instruments were deployed during this IOP to measure water vapor and aerosols and study their relationship. The NASA/Goddard Space Flight Center (GSFC) Scanning Raman Lidar (SRL) acquired water vapor and aerosol profile data during 15 nights of operations. The lidar acquired vertical profiles as well as nearly horizontal profiles directed near an instrumented 60 meter tower. Aerosol optical thickness, phase function, size distribution, and integrated water vapor were derived from measurements with a multiband automatic sun and sky scanning radiometer deployed at this site.

  8. 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.

  9. Hydrogen bonding in protic ionic liquids: reminiscent of water.

    PubMed

    Fumino, Koichi; Wulf, Alexander; Ludwig, Ralf

    2009-01-01

    Similarities and differences: Far-infrared spectra of protic ionic liquids could be assigned to intermolecular bending and stretching modes of hydrogen bonds. The characteristics of the low-frequency spectra resemble those of water. Both liquids form three-dimensional network structures, but only water is capable of building tetrahedral configurations. EAN: ethylammonium nitrate, PAN: propylammonium nitrate, DMAN: dimethylammonium nitrate.

  10. Light absorption properties of water soluble organic aerosol from Residential Wood Burning in Fresno, CA: Results from 2013 NASA DISCOVER-AQ Campaign

    NASA Astrophysics Data System (ADS)

    Kim, H.; Zhang, Q.; Young, D. E.; Parworth, C.

    2015-12-01

    Light absorption properties of water soluble organic aerosol were investigated at Fresno, CA from 13 January to 11 February, 2013 as part of the NASA DISCOVER-AQ campaign. The light absorption spectra of water soluble organic aerosol in PM2.5 was measured using a UV/vis diode array detector (DAD) coupled with a particle into liquid sampler (PILS) that sampled downstream of a PM2.5 cyclone (URG). The PILS was also coupled with two ion chromatographs (IC) to measure inorganic and organic ionic species in PM2.5. In addition, an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed at the same site to measure size-resolved chemical composition of submicrometer aerosol (PM1) in real time during this study. Light absorption at 365 nm (Abs365), which is typically used as a proxy of water-soluble brown carbon (BrC), showed strong enhancement during night time and appeared to correlate well (r = 0.71) with biomass burning organic aerosol (BBOA) from residential wood burning for heating in the Fresno area. The tight correlations between Abs365 and biomass burning relevant tracers such as acetonitrile (r = 0.69), AMS-signature ions for phenolic compounds (r = 0.52-0.71), PAH (r = 0.74), and potassium (r = 0.67) further confirm that biomass burning contributed significantly to water soluble brown carbon during this study. The absorption angstrom exponent (Åa) values fitted between 300 and 700 nm wavelength were 3.3 ± 1.1, 2.0 ± 0.9 and 4.0 ± 0.8, respectively, in the morning, afternoon and nighttime, indicating that BrC is prevalent at night in Fresno during wintertime. However, there are also indications that small amount of BrC existed during the daytime as well, likely due to daytime wood burning and other sources such as the formation of light-absorbing secondary organic aerosol (SOA). Finally, light absorption at 300 nm, 330 nm, and 390 nm were found to correlate tightly with BBOA, which indicate that biomass burning also emits

  11. Water Soluble Organic Nitrogen in atmospheric aerosol samples from urban, sub-urban and pristine areas of Venezuela

    NASA Astrophysics Data System (ADS)

    Canelon, R.; Giuliante, A.; Aguiar, G.; Ghneim, T.; Perez, T.

    2007-12-01

    Concentrations of water soluble organic nitrogen (WSON) were determined in atmospheric total suspended particles (TSP) collected between September of 2005 and May of 2006, in an urban continental (Caracas, 10° 29' 09'' N, 66° 53' 48'' W), an urban coastal (Catia la mar, 10° 35' 47'' N, 67° 01' 45'' W), a sub-urban coastal (Osma, 10° 32' N, 67° 28' W), a suburban continental (Altos de Pipe, 10° 23' 41'' N, 63° 59' 10'' W), a pristine coastal (Isla de Aves, 15° 40' N, 63° 36' W) and a pristine continental (La Gran Sabana National Park, 5° 41' 30'' N, 61° 34' 20'' W) areas of Venezuela. TSP samples were collected using a Hi-Vol airborne particle sampler. TSP were impacted on a fiberglass filter pretreated under 400° C for 4 hours to minimize organic nitrogen contamination. Ultra sound water extractions of the sample filters were performed and their NH4+, NO2- and NO3- concentrations were determined by ion exchange liquid chromatography. The water extracts were UV digested and the nitrogen inorganic ions were analyzed after the UV exposure. WSON concentrations were calculated by the difference between the inorganic nitrogen concentrations before and after UV digestion. Ninety five percent of the aerosol samples collected in the suburban and pristine areas showed a WSON concentration range from 0.03 to 0.6 μg/m3 whereas in urban areas the range was 0.21 to 1.09 μg/m3. These concentration values are on the same order of magnitude than the previously found in other tropical and subtropical areas. The contribution of aerosol WSON to the total soluble nitrogen in the coastal urban, sub-urban and pristine areas ranged from 23 to 67%, while in Caracas was smaller (38±8%, n=5). Therefore, aerosol WSON provides an important source of nitrogen to these pristine and suburban ecosystems, which could potentially have implications on the nutrient cycling. There was a statistically significant linear correlation between the aerosol WSON and the water soluble inorganic

  12. Clearing of a polydisperse water aerosol by a laser pulse in the diffusive-convective regime

    SciTech Connect

    Kucherov, Arkadii N

    2006-04-30

    The propagation of an IR laser pulse through a water aerosol layer (fog, clouds) is studied. The relative motion of the beam and medium, the diffraction spread, thermal self-action of the laser beam, absorption and scattering of radiation by particles, evaporation of particles (aerosol clearing), and the size distribution of particles were taken into account. The propagation problem was solved numerically at a macroscopic scale of the order of the beam transverse size, and the action of radiation on drops was considered at a microscopic scale of the order of the particle radius. A satisfactory agreement was obtained between theoretical and experimental results. (interaction of laser radiation with matter)

  13. Water-soluble material on aerosols collected within volcanic eruption clouds ( Fuego, Pacaya, Santiaguito, Guatamala).

    USGS Publications Warehouse

    Smith, D.B.; Zielinski, R.A.; Rose, W.I.; Huebert, B.J.

    1982-01-01

    In Feb. and March of 1978, filter samplers mounted on an aircraft were used to collect the aerosol fraction of the eruption clouds from three active Guatemalan volcanoes (Fuego, Pacaya, and Santiaguito). The elements dissolved in the aqueous extracts represent components of water-soluble material either formed directly in the eruption cloud or derived from interaction of ash particles and aerosol components of the plume. Calculations of enrichment factors, based upon concentration ratios, showed the elements most enriched in the extracts relative to bulk ash composition were Cd, Cu, V, F, Cl, Zn, and Pb.-from Authors

  14. The glass-liquid transition of water on hydrophobic surfaces.

    PubMed

    Souda, Ryutaro

    2008-09-28

    Interactions of thin water films with surfaces of graphite and vitrified room-temperature ionic liquid [1-butyl-3-methylimidazolium hexafluorophosphate ([bmim][PF(6)])] were investigated using time-of-flight secondary ion mass spectrometry as a function of temperature and annealing time to elucidate the glass-liquid transition of water at the molecular level. Surface diffusion of water occurs at temperatures higher than 120 K, thereby forming three-dimensional clusters (a two-dimensional layer) on the [bmim][PF(6)] (graphite) surface. The hydrophobic effect of the surface decreases with increasing coverage of water; the bulklike properties evolve up to 40 ML, as evidenced by the occurrence of film dewetting at around the conventional glass transition temperature (140 K). Results also showed that aging is necessary for the water monolayer (a 40 ML water film) to dewet the graphite ([bmim][PF(6)]) surface. The occurrence of aging is explainable by the successive evolution of two distinct liquids during the glass-liquid transition: low density liquid is followed by supercooled liquid water. The water monolayer on graphite is characterized by the preferred orientation of unpaired OH groups toward the surface; this structure is arrested during the aging time despite the occurrence of surface diffusion. However, the water monolayer formed on the [bmim][PF(6)] surface agglomerates immediately after the commencement of surface diffusion. The structure of low density liquid tends to be arrested by the attractive interaction with the neighbors.

  15. Aerosols and water vapor dynamics over the Kingdom of Saudi Arabia

    NASA Astrophysics Data System (ADS)

    Farahat, Ashraf; El-Askary, Hesham; Al-Shaibani, Abdulaziz; Dogan, Umran

    2014-05-01

    The Kingdom of Saudi Arabia contains a vast desert area and the home of some of the largest deserts worldwide. This nature subjects the area to numerous dust storms. This is in addition to local emissions transported from industrial activities. The Arabian Peninsula dust storms have a major impact on air quality and affects dust cycle around the world. The nature of dust also affects air, ground traffics, and human health. Aerosols play a pivotal role in global climate change through their effects on the hydrological cycle and solar energy budget. Recently there have been some trials to study the nature of dust over the kingdom using satellite remote sensing and modeling to investigate the impact of aerosols of natural and anthropogenic origins from both local emissions and long-range transport on the air quality and atmospheric composition, yet a lot more needs to be done. In this study, data obtained from the Moderate Resolution Imaging Spectroradiometer (MODIS) on board of Terra and Aqua satellites are used to analyze aerosols properties over the thirteen provinces of the Kingdom of Saudi Arabia from April 2003 to January 2012. This analysis will help to characterize aerosol and cloud properties, and the seasonal hydrological factors to establish the relative contributions of aerosols derived from different regions to the different Saudi provinces and their impacts on local atmospheric composition and air quality. During this period, we have examined possible nature and anthropogenic/natural aerosols/dust sources. The analysis is based on important parameters including the aerosol optical depth (AOD), fine mode fraction (FMF), cloud properties including cloud top temperature (CTT), cloud top pressure (CTP) and the water vapor column. Correlation between water vapor and AOD was observed over three provinces which could be a result of pollution aerosols rather than dust and is, hence, acting as cloud condensation nuclei (CCN). Increasing anomalous aerosols pattern

  16. Column atmospheric water vapor and vegetation liquid water retrievals from Airborne Imaging Spectrometer data

    NASA Astrophysics Data System (ADS)

    Gao, Bo-Cai; Goetz, Alexander F. H.

    1990-03-01

    High spatial resolution column atmospheric water vapor amounts were derived from spectral data collected by the airborne visible-infrared imaging spectrometer (AVIRIS), which covers the spectral region from 0.4 to 2.5 μm in 10-nm bands and has a ground instantaneous field of view of 20×20 m from an altitude of 20 km. The quantitative derivation is made by curve fitting observed spectra with calculated spectra in the 1.14-μm and 0.94-μm water vapor band absorption regions using an atmospheric model, a narrowband spectral model, and a nonlinear least squares fitting technique. The derivation makes use of the facts that (1) the reflectances of many ground targets vary approximately linearly with wavelength in the 0.94- and 1.14-μm water vapor band absorption regions, (2) the scattered radiation near 1 μm is small compared with the directly reflected radiation when the atmospheric aerosol concentrations are low, and (3) the scattered radiation in the lower part of the atmosphere is subjected to the water vapor absorption. The technique is directly applicable for retrieving column water vapor amounts from AVIRIS spectra measured on clear days with visibilities 20 km or greater. The precision of the retrieved column water vapor amounts from several data sets is 5% or better. Based on the analyses of an AVIRIS data set that was acquired within an hour of radiosonde launch, it appears that the accuracy approaches the precision. The derived column water vapor amounts are independent of the absolute surface reflectances. It now appears feasible to derive high spatial resolution column water vapor amounts over land areas from satellite altitude with the proposed high resolution imaging spectrometer (HIRIS). Curve fitting of spectra near 1 μm from areas covered with vegetation, using an atmospheric model and a simplified vegetation reflectance model, indicates that both the amount of atmospheric water vapor and the moisture content of vegetation can be retrieved

  17. Evaluation of Daytime Measurements of Aerosols and Water Vapor made by an Operational Raman Lidar over the Southern Great Plains

    NASA Technical Reports Server (NTRS)

    Ferrare, Richard; Turner, David; Clayton, Marian; Schmid, Beat; Covert, David; Elleman, Robert; Orgren, John; Andrews, Elisabeth; Goldsmith, John E. M.; Jonsson, Hafidi

    2006-01-01

    Raman lidar water vapor and aerosol extinction profiles acquired during the daytime over the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site in northern Oklahoma (36.606 N, 97.50 W, 315 m) are evaluated using profiles measured by in situ and remote sensing instruments deployed during the May 2003 Aerosol Intensive Operations Period (IOP). The automated algorithms used to derive these profiles from the Raman lidar data were first modified to reduce the adverse effects associated with a general loss of sensitivity of the Raman lidar since early 2002. The Raman lidar water vapor measurements, which are calibrated to match precipitable water vapor (PWV) derived from coincident microwave radiometer (MWR) measurements were, on average, 5-10% (0.3-0.6 g/m(exp 3) higher than the other measurements. Some of this difference is due to out-of-date line parameters that were subsequently updated in the MWR PWV retrievals. The Raman lidar aerosol extinction measurements were, on average, about 0.03 km(exp -1) higher than aerosol measurements derived from airborne Sun photometer measurements of aerosol optical thickness and in situ measurements of aerosol scattering and absorption. This bias, which was about 50% of the mean aerosol extinction measured during this IOP, decreased to about 10% when aerosol extinction comparisons were restricted to aerosol extinction values larger than 0.15 km(exp -1). The lidar measurements of the aerosol extinction/backscatter ratio and airborne Sun photometer measurements of the aerosol optical thickness were used along with in situ measurements of the aerosol size distribution to retrieve estimates of the aerosol single scattering albedo (omega(sub o)) and the effective complex refractive index. Retrieved values of omega(sub o) ranged from (0.91-0.98) and were in generally good agreement with omega(sub o) derived from airborne in situ measurements of scattering and absorption. Elevated aerosol

  18. Aerosol Impacts on Cloud Properties Observed during CalWater 2011

    NASA Astrophysics Data System (ADS)

    Suski, K.; Prather, K. A.; Hubbe, J.; Kluzek, C.; Jonsson, H.

    2011-12-01

    In February and March of 2011, an aircraft aerosol time-of-flight mass spectrometer (A-ATOFMS) was deployed on the DOE G-1 during CalWater, a multiyear field campaign aimed at understanding the effects of aerosols and atmospheric rivers on precipitation in California. Flights were conducted out of Sacramento and traversed the western coast of California to the eastern edge of the Sierra Nevada Mountain Range. Initial results show that when heavily processed Asian dust was present, clouds contained more ice than when dust wasn't present, showing that cloud processed Asian dust acts as an efficient ice nucleus. In one particular cloud, salty, processed dust was at the core of most cloud droplets, while aged soot remained unactivated in the interstitial aerosol. These results show that atmospheric aging can have varying effects on CCN and IN abilities. Further analysis of chemical mixing state and atmospheric aging effects on cloud properties are presented.

  19. Physicochemical Characterization of Lake Spray Aerosol Generated from Great Lakes Water Samples

    NASA Astrophysics Data System (ADS)

    Ault, A. P.; Axson, J. L.; May, N.; Pratt, K.

    2014-12-01

    Wave breaking across bodies of water releases particles into the air which can impact climate and human health. Similar to sea spray aerosols formed through marine wave breaking, freshwater lakes generate lake spray aerosol (LSA). LSA can impact climate directly through scattering/absorption and indirectly through cloud nucleation. In addition, these LSA are suggested to impact human health through inhalation of these particles during algal bloom periods characterized by toxic cyanobacteria. Few studies have been conducted to assess the physical and chemical properties of freshwater LSA. Herein, we discuss constructing a LSA generation system and preliminary physical and chemical characterization of aerosol generated from water samples collected at various sites across Lake Erie, Lake Huron, Lake Superior, and Lake Michigan. Information on aerosol size distributions, number concentrations, and chemical composition will be discussed as a function of lake water blue-green algae concentration, dissolved organic carbon concentration, temperature, conductivity, and dissolved oxygen concentration. These studies represent a first step towards evaluating the potential for LSA to impact climate and health in the Great Lakes region.

  20. A comparative assessment of cigarette smoke aerosols using an in vitro air–liquid interface cytotoxicity test

    PubMed Central

    Thorne, David; Dalrymple, Annette; Dillon, Deborah; Duke, Martin; Meredith, Clive

    2015-01-01

    Abstract This study describes the evaluation of a modified air-liquid interface BALB/c 3T3 cytotoxicity method for the assessment of smoke aerosols in vitro. The functionality and applicability of this modified protocol was assessed by comparing the cytotoxicity profiles from eight different cigarettes. Three reference cigarettes, 1R5F, 3R4F and CORESTA Monitor 7 were used to put the data into perspective and five bespoke experimental products were manufactured, ensuring a balanced and controlled study. Manufactured cigarettes were matched for key variables such as nicotine delivery, puff number, pressure drop, ventilation, carbon monoxide, nicotine free dry particulate matter and blend, but significantly modified for vapor phase delivery, via the addition of two different types and quantities of adsorptive carbon. Specifically manufacturing products ensures comparisons can be made in a consistent manner and allows the research to ask targeted questions, without confounding product variables. The results demonstrate vapor-phase associated cytotoxic effects and clear differences between the products tested and their cytotoxic profiles. This study has further characterized the in vitro vapor phase biological response relationship and confirmed that the biological response is directly proportional to the amount of available vapor phase toxicants in cigarette smoke, when using a Vitrocell® VC 10 exposure system. This study further supports and strengthens the use of aerosol based exposure options for the appropriate analysis of cigarette smoke induced responses in vitro and may be especially beneficial when comparing aerosols generated from alternative tobacco aerosol products. PMID:26339773

  1. Liquid-liquid equilibria of water + methanol + 1-octanol and water + ethanol + 1-octanol at various temperatures

    SciTech Connect

    Arce, A.; Blanco, A.; Souza, P.; Vidal, I. . Dept. of Chemical Engineering)

    1994-04-01

    This study is part of a wider program of research on the recovery of light alcohols from dilute aqueous solutions using high molecular weight solvents. The authors report liquid-liquid equilibrium data and binodal curves for the systems water + methanol + 1-octanol and water + ethanol + 1-octanol at 25, 35, and 45 C. The data were fitted to the NRTL and UNIQUAC equations.

  2. Evidence for Recent Liquid Water on Mars

    NASA Technical Reports Server (NTRS)

    2000-01-01

    This image, acquired by the Mars Global Surveyor (MGS) Mars Orbiter Camera (MOC) in May 2000 shows numerous examples of martian gullies that all start--or head--in a specific layer roughly a hundred meters beneath the surface of Mars. These features are located on the south-facing wall of a trough in the Gorgonum Chaos region, an area found to have many examples of gullies proposed to have formed by seepage and runoff of liquid water in recent martian times. The layer from which the gullies emanate has recessed backward to form an overhang beneath a harder layer of rock. The larger gullies have formed an alcove--an area above the overhang from which debris has collapsed to leave a dark-toned scar. Below the layer of seepage is found a dark, narrow channel that runs down the slope to an apron of debris. The small, bright, parallel features at the base of the cliff at the center-right of the picture is a series of large windblown ripples. Although the dark tone of the alcoves and channels in this image is not likely to be the result of wet ground (the contrast in this image has been enhanced), it does suggest that water has seeped out of the ground and moved down the slope quite recently. Sharp contrasts between dark and light areas are hard to maintain on Mars for very long periods of time because dust tends to coat surfaces and reduce brightness differences. To keep dust from settling on a surface, it has to have undergone some process of erosion (wind, landslides, water runoff) relatively recently. There is no way to know how recent this activity was, but educated guesses center between a few to tens of years, and it is entirely possible that the area shown in this image has water seeping out of the ground today. Centered near 37.9S, 170.2W, sunlight illuminates the MOC image from the upper left, north is toward the upper right. The context view above is from the Viking 1 orbiter and was acquired in 1977. The Viking picture is illuminated from the upper right

  3. Infrared spectroscopy of aerosols

    NASA Astrophysics Data System (ADS)

    Mentel, Th.; Sebald, H.

    2003-04-01

    In our large Aerosol Chamber at the FZ Jülich we apply HR FTIR absorption spectroscopy for the determination of trace gases. In the FTIR spectra we also observe broad absorptions of several 10 to a few 100 cm-1 widths that arise from species in the condensed aerosol phase: liquid H_2O, NO_3^-, SO_42-, HSO_4^-, or dicarboxylic acids. Moreover, the aerosol droplets caused extinctions over several 1000 cm-1 by IR scattering. This allows for in-situ observation of changes in the condensed aerosol phase e.g. on HNO_3 uptake, like the shift of the sulfate/bisulfate equilibrium or the growth by water condensation. The IR absorptions of the condensed aerosol phase provide useful extra information in process studies, if they can be quantified. Therefore the absorption cross section, respective, the absorption index which is the imaginary part of the complex refractive index is needed. We set up an aerosol flow tube in which IR spectroscopy on a 8 m light path and aerosol size distribution measurements in the range from 20 nm - 10 μm can be performed simultaneously. We measured sulfate aerosols at several relative humidities (dry, metastable, deliquescent). We will demonstrate an iterative procedure based on Mie calculations and Kramers Kronig transformation to retrieve the absorption index from the observed IR spectra and the corresponding size distribution (for dry ammonium sulfate). We will compare resulting absorption indices for aqueous sodium bisulfate aerosols at several relative humidties with thermodynamic model calculations for the Na^+/H^+/HSO_4^-/SO_42-/H_2O system.

  4. Solid/Liquid phase diagram of the ammonium sulfate/maleic acid/water system.

    PubMed

    Beyer, Keith D; Schroeder, Jason R; Pearson, Christian S

    2011-12-01

    We have studied the low temperature phase diagram and water activities of the ammonium sulfate/maleic acid/water system using differential scanning calorimetry and infrared spectroscopy of thin films. Using the results from our experiments, we have mapped the solid/liquid ternary phase diagram, determined the water activities based on the freezing point depression, and determined the ice/maleic acid phase boundary as well as the ternary eutectic composition and temperature. We also compare our results to the predictions of the extended AIM aerosol thermodynamics model and find good agreement for the ice melting points in the ice primary phase field of this system; however significant differences were found with respect to phase boundaries, maleic acid dissolution, and ammonium sulfate dissolution.

  5. A novel Aerosol-Into-Liquid Collector for online measurements of trace metal and elements in ambient particulate matter (PM)

    NASA Astrophysics Data System (ADS)

    Wang, Dongbin; Shafer, Martin; Schauer, James; Sioutas, Constantinos

    2015-04-01

    A novel monitor for online, in-situ measurement of several important metal species (i.e. Fe, Mn and Cr) in ambient fine and ultrafine particulate matter (PM) is developed based on a recent published high flow rate Aerosol-Into-Liquid Collector. This Aerosol-Into-Liquid Collector collects particles directly as highly concentrated slurry samples, and the concentrations of target metals in slurry samples are subsequently determined in a Micro Volume Flow Cell (MVFC) coupled with absorbance spectrophotometry to detect colored complexes coming from the reactions between target metals and specific reagents. Laboratory tests are conducted to evaluate the performance of the MVFC-absorbance system. The calibration curves of the system are determined using standard solutions prepared by serial dilution. As part of the evaluation, the effects of reaction time, reagent amount and interference on the system are also evaluated. Field evaluations of the online monitor will be performed to validate the ability of this new online sampler in near-continuous collection and measurements. Both laboratory and field evaluations of the novel monitor will indicate that it is an effective and valuable technology for PM collection and characterization of important metal species in ambient aerosols.

  6. Reformulating Aerosol Thermodynamics and Cloud Microphysics

    NASA Astrophysics Data System (ADS)

    Metzger, S.

    2006-12-01

    Modeling aerosol composition and cloud microphysics is rather complex due to the required thermodynamics, even if chemical and thermodynamical equilibrium is assumed. We show, however, that for deliquescent atmospheric aerosols thermodynamics can be considerably simplified, if we reformulate chemical equilibrium to include water purely based on thermodynamic principles. In chemical and thermodynamical equilibrium, the relative humidity (RH) fixes the molality of atmospheric aerosols. Although this fact is in theory well known, it has hardly been utilized in aerosol modeling nor has been the fact that for the same reason also the aerosol activity (including activity coefficients) and water content are fixed (by RH) for a given aerosol concentration and type. The only model that successfully utilizes this fact is the computationally very efficient EQuilibrium Simplified thermodynamic gas/Aerosol partitioning Model, EQSAM (Metzger et al., 2002a), EQSAM2 (Metzger et al., 2006). In both versions the entire gas/liquid/solid aerosol equilibrium partitioning is solved analytically and hence non-iteratively a substantial advantage in aerosol composition modeling. Here we briefly present the theoretical framework of EQSAM2, which differs from EQSAM in a way that the calculation of the water activity of saturated binary or mixed inorganic/organic salt solutions of multi-component aerosols has been generalized by including the Kelvin-term, thus allowing for any solute activity above the deliquescence relative humidity, including supersaturation. With application of our new concept to a numerical whether prediction (NWP) model, we demonstrate its wide implications for the computation of various aerosol and cloud properties, as our new concept allows to consistently and efficiently link the modeling of aerosol thermodynamics and cloud microphysics through the aerosol water mass, which therefore deserves special attention in atmospheric chemistry, air pollution, NWP and climate

  7. The CalWater 2 - ARM Cloud Aerosol Precipitation Experiment (ACAPEX)

    NASA Astrophysics Data System (ADS)

    Leung, L. Y.; Prather, K. A.; Ralph, F. M.; Rosenfeld, D.; Spackman, J. R.; Fairall, C. W.; DeMott, P. J.; Fan, J.; Zhao, C.

    2014-12-01

    The western U.S. receives precipitation predominantly during the cold season when storms approach from the Pacific Ocean. The snowpack that accumulates during winter storms provides about 70-90% of water supply for the region. Two elements of significant importance in predicting precipitation variability in the western U.S. are atmospheric rivers and aerosols. Atmospheric rivers (ARs) are narrow bands of enhanced water vapor associated with the warm sector of extratropical cyclones over the Pacific and Atlantic oceans. While ARs are responsible for a large fraction of heavy precipitation in the western U.S. during winter, much of the rest of the orographic precipitation occurs in post-frontal clouds, which are typically quite shallow, with tops just high enough to pass the mountain barrier. Such clouds are inherently quite susceptible to aerosol effects on both warm rain and ice precipitation-forming processes. In January - March 2015, the ARM Cloud Aerosol Precipitation Experiment (ACAPEX) field campaign will take place in northern California. Joined with CalWater 2, the field campaign aims to improve understanding and modeling of large-scale dynamics and cloud and precipitation processes associated with ARs and aerosol-cloud interactions that influence precipitation variability and extremes in the western U.S. We will implement an observational strategy consisting of the use of land and offshore assets to monitor (1) the evolution and structure of ARs from near their regions of development, (2) long range transport of aerosols in eastern North Pacific and potential interactions with ARs, and (3) how aerosols from long-range transport and local sources influence cloud and precipitation in the U.S. West Coast where ARs make landfall and post-frontal clouds are frequent. This presentation will provide an overview of the science questions and hypotheses to be addressed by CalWater 2/ACAPEX, review key results from prior studies, and discuss recent findings from

  8. Quantification of individual phenolic compounds' contribution to antioxidant capacity in apple: a novel analytical tool based on liquid chromatography with diode array, electrochemical, and charged aerosol detection.

    PubMed

    Plaza, Merichel; Kariuki, James; Turner, Charlotta

    2014-01-15

    Phenolics, particularly from apples, hold great interest because of their antioxidant properties. In the present study, the total antioxidant capacity of different apple extracts obtained by pressurized hot water extraction (PHWE) was determined by cyclic voltammetry (CV), which was compared with the conventional antioxidant assays. To measure the antioxidant capacity of individual antioxidants present in apple extracts, a novel method was developed based on high-performance liquid chromatography (HPLC) with photodiode array (DAD), electrochemical (ECD), and charged aerosol (CAD) detection. HPLC-DAD-ECD-CAD enabled rapid, qualitative, and quantitative determination of antioxidants in the apple extracts. The main advantage of using CAD was that this detector enabled quantification of a large number of phenolics using only a few standards. The results showed that phenolic acids and flavonols were mainly responsible for the total antioxidant capacity of apple extracts. In addition, protocatechuic acid, chlorogenic acid, hyperoside, an unidentified phenolic acid, and a quercetin derivative presented the highest antioxidant capacities.

  9. The influence of small aerosol particles on the properties of water and ice clouds.

    PubMed

    Choularton, T W; Bower, K N; Weingartner, E; Crawford, I; Coe, H; Gallagher, M W; Flynn, M; Crosier, J; Connolly, P; Targino, A; Alfarra, M R; Baltensperger, U; Sjogren, S; Verheggen, B; Cozic, J; Gysel, M

    2008-01-01

    In this paper, results are presented of the influence of small organic- and soot-containing particles on the formation of water and ice clouds. There is strong evidence that these particles have grown from nano particle seeds produced by the combustion of oil products. Two series of field experiments are selected to represent the observations made. The first is the CLoud-Aerosol Characterisation Experiment (CLACE) series of experiments performed at a high Alpine site (Jungfraujoch), where cloud was in contact with the ground and the measuring station. Both water and ice clouds were examined at different times of the year. The second series of experiments is the CLOud Processing of regional Air Pollution advecting over land and sea (CLOPAP) series, where ageing pollution aerosol from UK cities was observed, from an airborne platform, to interact with warm stratocumulus cloud in a cloud-capped atmospheric boundary layer. Combining the results it is shown that aged pollution aerosol consists of an internal mixture of organics, sulfate, nitrate and ammonium, the organic component is dominated by highly oxidized secondary material. The relative contributions and absolute loadings of the components vary with location and season. However, these aerosols act as Cloud Condensation Nuclei (CCN) and much of the organic material, along with the other species, is incorporated into cloud droplets. In ice and mixed phase cloud, it is observed that very sharp transitions (extending over just a few metres) are present between highly glaciated regions and regions consisting of supercooled water. This is a unique finding; however, aircraft observations in cumulus suggest that this kind of structure may be found in these cloud types too. It is suggested that this sharp transition is caused by ice nucleation initiated by oxidised organic aerosol coated with sulfate in more polluted regions of cloud, sometimes enhanced by secondary ice particle production in these regions.

  10. Observed reflectivities and liquid water content for marine stratocumulus

    NASA Technical Reports Server (NTRS)

    Coakley, J. A., Jr.; Snider, J. B.

    1989-01-01

    Simultaneous observations of cloud liquid water content and cloud reflectivity are used to verify their parametric relationship in a manner consistent with simple parameterizations often used in general-circulation climate models. The column amount of cloud liquid water was measured with a microwave radiometer on San Nicolas Island as described by Hogg et al., (1983). Cloud reflectivity was obtained through spatial coherence analysis of AVHRR imagery data as per Coakley and Baldwin (1984) and Coakley and Beckner (1988). The dependence of the observed reflectivity on the observed liquid water is discussed, and this empirical relationship is compared with the parameterization proposed by Stephens (1978).

  11. Thermoluminescence dosimetry measurements of brachytherapy sources in liquid water

    SciTech Connect

    Tailor, Ramesh; Tolani, Naresh; Ibbott, Geoffrey S.

    2008-09-15

    Radiation therapy dose measurements are customarily performed in liquid water. The characterization of brachytherapy sources is, however, generally based on measurements made with thermoluminescence dosimeters (TLDs), for which contact with water may lead to erroneous readings. Consequently, most dosimetry parameters reported in the literature have been based on measurements in water-equivalent plastics, such as Solid Water. These previous reports employed a correction factor to transfer the dose measurements from a plastic phantom to liquid water. The correction factor most often was based on Monte Carlo calculations. The process of measuring in a water-equivalent plastic phantom whose exact composition may be different from published specifications, then correcting the results to a water medium leads to increased uncertainty in the results. A system has been designed to enable measurements with TLDs in liquid water. This system, which includes jigs to support water-tight capsules of lithium fluoride in configurations suitable for measuring several dosimetric parameters, was used to determine the correction factor from water-equivalent plastic to water. Measurements of several {sup 125}I and {sup 131}Cs prostate brachytherapy sources in liquid water and in a Solid Water phantom demonstrated a correction factor of 1.039{+-}0.005 at 1 cm distance. These measurements are in good agreement with a published value of this correction factor for an {sup 125}I source.

  12. In situ measurements of water uptake by black carbon-containing aerosol in wildfire plumes

    NASA Astrophysics Data System (ADS)

    Perring, Anne E.; Schwarz, Joshua P.; Markovic, Milos Z.; Fahey, David W.; Jimenez, Jose L.; Campuzano-Jost, Pedro; Palm, Brett D.; Wisthaler, Armin; Mikoviny, Tomas; Diskin, Glenn; Sachse, Glen; Ziemba, Luke; Anderson, Bruce; Shingler, Taylor; Crosbie, Ewan; Sorooshian, Armin; Yokelson, Robert; Gao, Ru-Shan

    2017-01-01

    Water uptake by black carbon (BC)-containing aerosol was quantified in North American wildfire plumes of varying age (1 to 40 h old) sampled during the SEAC4RS mission (2013). A Humidified Dual SP2 (HD-SP2) is used to optically size BC-containing particles under dry and humid conditions from which we extract the hygroscopicity parameter, κ, of materials internally mixed with BC. Instrumental variability and the uncertainty of the technique are briefly discussed. An ensemble average κ of 0.04 is found for the set of plumes sampled, consistent with previous estimates of bulk aerosol hygroscopicity from biomass burning sources. The temporal evolution of κ in the Yosemite Rim Fire plume is explored to constrain the rate of conversion of BC-containing aerosol from hydrophobic to more hydrophilic modes in these emissions. A BC-specific κ increase of 0.06 over 40 h is found, fit well with an exponential curve corresponding to a transition from a κ of 0 to a κ of 0.09 with an e-folding time of 29 h. Although only a few percent of wildfire particles contain BC, a similar κ increase is estimated for bulk aerosol and the measured aerosol composition is used to infer that the observed κ change is driven by a combination of incorporation of ammonium sulfate and oxidation of existing organic materials. Finally, a substantial fraction of wildfire-generated BC-containing aerosol is calculated to be active as cloud condensation nuclei shortly after emission likely indicating efficient wet removal. These results can constrain model treatment of BC from wildfire sources.

  13. Characterization of cumulus cloud fields using trajectories in the center of gravity versus water mass phase space: 2. Aerosol effects on warm convective clouds

    NASA Astrophysics Data System (ADS)

    Heiblum, Reuven H.; Altaratz, Orit; Koren, Ilan; Feingold, Graham; Kostinski, Alexander B.; Khain, Alexander P.; Ovchinnikov, Mikhail; Fredj, Erick; Dagan, Guy; Pinto, Lital; Yaish, Ricki; Chen, Qian

    2016-06-01

    In Part I of this work a 3-D cloud tracking algorithm and phase space of center of gravity altitude versus cloud liquid water mass (CvM space) were introduced and described in detail. We showed how new physical insight can be gained by following cloud trajectories in the CvM space. Here this approach is used to investigate aerosol effects on cloud fields of warm cumuli. We show a clear effect of the aerosol loading on the shape and size of CvM clusters. We also find fundamental differences in the CvM space between simulations using bin versus bulk microphysical schemes, with the bin scheme precipitation expressing much higher sensitivity to changes in aerosol concentrations. Using the bin microphysical scheme, we find that the increase in cloud center of gravity altitude with increase in aerosol concentrations occurs for a wide range of cloud sizes. This is attributed to reduced sedimentation, increased buoyancy and vertical velocities, and increased environmental instability, all of which are tightly coupled to inhibition of precipitation processes and subsequent feedbacks of clouds on their environment. Many of the physical processes shown here are consistent with processes typically associated with cloud invigoration.

  14. Quantitative LC-MS for water-soluble heterocyclic amines in fine aerosols (PM2.5) at Duke Forest, USA

    NASA Astrophysics Data System (ADS)

    Samy, Shar; Hays, Michael D.

    2013-06-01

    A quantitative liquid chromatography-mass spectrometry (LC-MS) technique was developed to measure the concentrations of heterocyclic nitrogen compounds in ambient fine aerosols (PM2.5). Quadrupole time-of-flight (Q-TOF) MS technology was used to provide both accurate-mass and MS/MS data for confirmation of chemical formula and nitrogen compound structure. The fine aerosol was collected over the winter and summer seasons at an experimental monitoring station at Duke Forest in North Carolina U.S.A. 3-Hydroxypyridine and two β-carbolines, harmane, and norharmane, were observed in both campaigns at concentrations lower in summer (sum = 332 pg m-3; N = 27) than winter (554 pg m-3; N = 31). Aminopyridines, dimethylpyrazoles, and hydroxymethyl-pyridines were observed in the winter aerosols with a total estimated average concentration of 779 pg m-3. These results demonstrate the possibility of enhanced speciation and provide a first glance at heterocyclic amines in the water-soluble organic nitrogen (ON) fraction of fine aerosols collected from a forest atmosphere.

  15. Examination of the potential impacts of dust and pollution aerosol acting as cloud nucleating aerosol on water resources in the Colorado River Basin

    NASA Astrophysics Data System (ADS)

    Jha, Vandana

    In this study we examine the cumulative effect of dust acting as cloud nucleating aerosol (cloud condensation nuclei (CCN), giant cloud condensation nuclei (GCCN), and ice nuclei (IN)) along with anthropogenic aerosol pollution acting primarily as CCN, over the entire Colorado Rocky Mountains from the months of October to April in the year 2004-2005; the snow year. This ˜6.5 months analysis provides a range of snowfall totals and variability in dust and anthropogenic aerosol pollution. The specific objectives of this research is to quantify the impacts of both dust and pollution aerosols on wintertime precipitation in the Colorado Mountains using the Regional Atmospheric Modeling System (RAMS). In general, dust enhances precipitation primarily by acting as IN, while aerosol pollution reduces water resources in the CRB via the so-called "spill-over" effect, by enhancing cloud droplet concentrations and reducing riming rates. Dust is more episodic and aerosol pollution is more pervasive throughout the winter season. Combined response to dust and aerosol pollution is a net reduction of water resources in the CRB. The question is by how much are those water resources affected? Our best estimate is that total winter-season precipitation loss for for the CRB the 2004-2005 winter season due to the combined influence of aerosol pollution and dust is 5,380,00 acre-feet of water. Sensitivity studies for different cases have also been run for the specific cases in 2004-2005 winter season to analyze the impact of changing dust and aerosol ratios on precipitation in the Colorado River Basin. The dust is varied from 3 to 10 times in the experiments and the response is found to be non monotonic and depends on various environmental factors. The sensitivity studies show that adding dust in a wet system increases precipitation when IN affects are dominant. For a relatively dry system high concentrations of dust can result in over-seeding the clouds and reductions in precipitation

  16. Glass–liquid transition of water at high pressure

    PubMed Central

    Andersson, Ove

    2011-01-01

    The knowledge of the existence of liquid water under extreme conditions and its concomitant properties are important in many fields of science. Glassy water has previously been prepared by hyperquenching micron-sized droplets of liquid water and vapor deposition on a cold substrate (ASW), and its transformation to an ultraviscous liquid form has been reported on heating. A densified amorphous solid form of water, high-density amorphous ice (HDA), has also been made by collapsing the structure of ice at pressures above 1 GPa and temperatures below approximately 140 K, but a corresponding liquid phase has not been detected. Here we report results of heat capacity Cp and thermal conductivity, in situ, measurements, which are consistent with a reversible transition from annealed HDA to ultraviscous high-density liquid water at 1 GPa and 140 K. On heating of HDA, the Cp increases abruptly by (3.4 ± 0.2) J mol-1 K-1 before crystallization starts at (153 ± 1) K. This is larger than the Cp rise at the glass to liquid transition of annealed ASW at 1 atm, which suggests the existence of liquid water under these extreme conditions. PMID:21690361

  17. Isothermal vapor-liquid equilibria for methanol + ethanol + water, methanol + water, and ethanol + water

    SciTech Connect

    Kurihara, Kiyofumi; Takeda, Kouichi; Kojima, Kazuo; Minoura, Tsuyoshi

    1995-05-01

    Isothermal vapor-liquid equilibria were measured for the ternary system methanol + ethanol + water and its constituent binary systems of methanol + water and ethanol + water at 323.15, 328.15, and 333.15 K. The apparatus that was used made it possible to control the measured temperature and total pressure by computer. The experimental binary data were correlated by the NRTL equation. The ternary system was predicted using the binary NRTL parameters with good accuracy.

  18. Primary and Secondary Aerosol Investigation from Different Sea-Waters in the Mediterranean Sea

    NASA Astrophysics Data System (ADS)

    D'anna, B.; Marchand, N.; Sellegri, K.; Sempéré, R.; Mas, S.; George, C.; Meme, A.; Frihi, A.; Pey, J.; Schwier, A.; Delmont, A.

    2014-12-01

    The Mediterranean Sea is a special marine environment characterized by low biological activity and high anthropogenic pressure. It is often difficult to discriminate the contribution of Primary and Secondary Aerosol formed at the sea-air interface from background level of the aerosol. We therefore decided to study the sea-air exchanges in a controlled environment provided by a 2m3simulation chamber, using freshly collected sea-water samples from the SEMEX site (43°15'64 N, 05°20'01 E) near Marseille bay. Two types of experiments were conducted for 4 weeks testing 3 different sea-waters. Primary sea-aerosol was generated by bubble-bursting method, then introduced in the simulation chamber and exposed to atmospheric oxidants (O3, OH) and light to simulated primary aerosol aging. A second set of experiments focused on secondary particle formation upon illumination and/or ozone exposure of the sea-water surface (15l of sea-water were deposited in a pyrex container located inside the simulation chamber). New particle formation was only observed for relatively high DOC level of the sea-water sample. Particles detection and analysis was followed by a PSM (1nm size), a CPC (2.5nm size), a SMPS (granulometry), a CCN chamber for hygroscopicity studies, a TOF-AMS (Aerodyne) for chemical analysis of the sub-micrometer fraction. Off-line analysis included TEM-EDX samples for morphology and size distribution studies and a hybrid quadrupole-orbitrap mass spectrometer (Thermo Fischer) for the molecular identification of the organic fraction. VOCs were measured on-line by PTR-HR-MS. The seawater samples were filtered at 60μm before use and were daily analyzed for chemical (colored dissolved organic matter, particulate matter and related polar compounds, transparent polysaccharides and nutrients concentration) and biological (chlorophyll a, virus, phytoplankton and zooplankton) analyses.

  19. Cloud and Aerosol Properties, Precipitable Water, and Profiles of Temperature and Water Vapor from MODIS

    NASA Technical Reports Server (NTRS)

    King, Michael D.; Menzel, W. Paul; Kaufman, Yoram J.; Tanre, Didier; Gao, Bo-Cai; Platnick, Steven; Ackerman, Steven A.; Remer, Lorraine A.; Pincus, Robert; Hubanks, Paul A.

    2003-01-01

    The Moderate Resolution Imaging Spectroradiometer (MODIS) is an earth-viewing sensor that flies on the Earth Observing System (EOS) Terra and Aqua satellites, launched in 1999 and 2002, respectively. MODIS scans a swath width of 2330 km that is sufficiently wide to provide nearly complete global coverage every two days from a polar-orbiting, sun-synchronous, platform at an altitude of 705 km. MODIS provides images in 36 spectral bands between 0.415 and 14.235 pm with spatial resolutions of 250 m (2 bands), 500 m (5 bands) and 1000 m (29 bands). These bands have been carefully selected to en- able advanced studies of land, ocean, and atmospheric properties. Twenty-six bands are used to derive atmospheric properties such as cloud mask, atmospheric profiles, aerosol properties, total precipitable water, and cloud properties. In this paper we describe each of these atmospheric data products, including characteristics of each of these products such as file size, spatial resolution used in producing the product, and data availability.

  20. Space Station Water Processor Mostly Liquid Separator (MLS)

    NASA Technical Reports Server (NTRS)

    Lanzarone, Anthony

    1995-01-01

    This report presents the results of the development testing conducted under this contract to the Space Station Water Processor (WP) Mostly Liquid Separator (MLS). The MLS units built and modified during this testing demonstrated acceptable air/water separation results in a variety of water conditions with inlet flow rates ranging from 60 - 960 LB/hr.

  1. Liquid-liquid transition in supercooled water suggested by microsecond simulations.

    PubMed

    Li, Yaping; Li, Jicun; Wang, Feng

    2013-07-23

    The putative liquid-liquid phase transition in supercooled water has been used to explain many anomalous behaviors of water. However, no direct experimental verification of such a phase transition has been accomplished, and theoretical studies from different simulations contradict each other. We investigated the putative liquid-liquid phase transition using the Water potential from Adaptive Force Matching for Ice and Liquid (WAIL). The simulation reveals a first-order phase transition in the supercooled regime with the critical point at ~207 K and 50 MPa. Normal water is high-density liquid (HDL). Low-density liquid (LDL) emerges at lower temperatures. The LDL phase has a density only slightly larger than that of the ice-Ih and shows more long-range order than HDL. However, the transformation from LDL to HDL is spontaneous across the first-order phase transition line, suggesting the LDL configuration is not poorly formed nanocrystalline ice. It has been demonstrated in the past that the WAIL potential provides reliable predictions of water properties such as melting temperature and temperature of maximum density. Compared with other simple water potentials, WAIL is not biased by fitting to experimental properties, and simulation with this potential reflects the prediction of a high-quality first-principle potential energy surface.

  2. Liquid water in the domain of cubic crystalline ice Ic

    NASA Technical Reports Server (NTRS)

    Jenniskens, P.; Banham, S. F.; Blake, D. F.; McCoustra, M. R.

    1997-01-01

    Vapor-deposited amorphous water ice when warmed above the glass transition temperature (120-140 K), is a viscous liquid which exhibits a viscosity vs temperature relationship different from that of liquid water at room temperature. New studies of thin water ice films now demonstrate that viscous liquid water persists in the temperature range 140-210 K. where it coexists with cubic crystalline ice. The liquid character of amorphous water above the glass transition is demonstrated by (1) changes in the morphology of water ice films on a nonwetting surface observed in transmission electron microscopy (TEM) at around 175 K during slow warming, (2) changes in the binding energy of water molecules measured in temperature programmed desorption (TPD) studies, and (3) changes in the shape of the 3.07 micrometers absorption band observed in grazing angle reflection-absorption infrared spectroscopy (RAIRS) during annealing at high temperature. whereby the decreased roughness of the water surface is thought to cause changes in the selection rules for the excitation of O-H stretch vibrations. Because it is present over such a wide range of temperatures, we propose that this form of liquid water is a common material in nature. where it is expected to exist in the subsurface layers of comets and on the surfaces of some planets and satellites.

  3. Liquid water in the domain of cubic crystalline ice Ic.

    PubMed

    Jenniskens, P; Banham, S F; Blake, D F; McCoustra, M R

    1997-07-22

    Vapor-deposited amorphous water ice when warmed above the glass transition temperature (120-140 K), is a viscous liquid which exhibits a viscosity vs temperature relationship different from that of liquid water at room temperature. New studies of thin water ice films now demonstrate that viscous liquid water persists in the temperature range 140-210 K. where it coexists with cubic crystalline ice. The liquid character of amorphous water above the glass transition is demonstrated by (1) changes in the morphology of water ice films on a nonwetting surface observed in transmission electron microscopy (TEM) at around 175 K during slow warming, (2) changes in the binding energy of water molecules measured in temperature programmed desorption (TPD) studies, and (3) changes in the shape of the 3.07 micrometers absorption band observed in grazing angle reflection-absorption infrared spectroscopy (RAIRS) during annealing at high temperature. whereby the decreased roughness of the water surface is thought to cause changes in the selection rules for the excitation of O-H stretch vibrations. Because it is present over such a wide range of temperatures, we propose that this form of liquid water is a common material in nature. where it is expected to exist in the subsurface layers of comets and on the surfaces of some planets and satellites.

  4. Water-soluble Organic Components in Aerosols Associated with Savanna Fires in Southern Africa: Identification, Evolution and Distribution

    NASA Technical Reports Server (NTRS)

    Gao, Song; Hegg, Dean A.; Hobbs, Peter V.; Kirchstetter, Thomas W.; Magi, Brian I.; Sadilek, Martin

    2003-01-01

    During the SAFARI 2000 field campaign, both smoke aerosols from savanna fires and haze aerosols in the boundary layer and in the free troposphere were collected from an aircraft in southern Africa. These aerosol samples were analyzed for their water-soluble chemical components, particularly the organic species. A novel technique, electrospray ionization-ion trap mass spectrometry, was used concurrently with an ion chromatography system to analyze for carbohydrate species. Seven carbohydrates, seven organic acids, five metallic elements, and three inorganic anions were identified and quantified. On the average, these 22 species comprised 36% and 27% of the total aerosol mass in haze and smoke aerosols, respectively. For the smoke aerosols, levoglucosan was the most abundant carbohydrate species, while gluconic acid was tentatively identified as the most abundant organic acid. The mass abundance and possible source of each class of identified species are discussed, along with their possible formation pathways. The combustion phase of a fire had an impact on the chemical composition of the emitted aerosols. Secondary formation of sulfate, nitrate, levoglucosan, and several organic acids occurred during the initial aging of smoke aerosols. It is likely that under certain conditions, some carbohydrate species in smoke aerosols, such as levoglucosan, were converted to organic acids during upward transport.

  5. CalWater 2015 — Atmospheric Rivers and Aerosol Impacts on Precipitation

    NASA Astrophysics Data System (ADS)

    Spackman, J. R.; Ralph, F. M.; Prather, K. A.; Cayan, D.; DeMott, P. J.; Dettinger, M. D.; Doyle, J. D.; Fairall, C. W.; Leung, L. R.; Rosenfeld, D.; Rutledge, S. A.; Waliser, D. E.; White, A. B.

    2015-12-01

    The CalWater 2015 field experiment was conducted between January and March and consisted of more than fifty science flights, a major research cruise, and continuous ground-based observations coordinated to study phenomena driving the incidence of extreme precipitation events and the variability of water supply along the West Coast of the United States. CalWater 2015 examined key processes linked to (1) atmospheric rivers (ARs) in delivering much of the precipitation associated with major winter storms, and (2) aerosols, originating from local sources as well as from remote continents, within and between storms and their modulating effects on precipitation on the U.S. West Coast. As part of a large interagency field effort including NOAA, DOE, NASA, NSF, and the Naval Research Laboratory, four research aircraft from three government agencies were deployed in coordination with the oceangoing NOAA Ronald H. Brown and were equipped with meteorological and chemical observing systems in near-shore regions of California and the eastern Pacific. At the same time, ground-based measurements from NOAA's HydroMeteorological Testbed (HMT) network on the U.S. West Coast and a major NSF-supported observing site for aerosols and microphysics at Bodega Bay, California provided continuous near surface-level meteorological and chemical observations, respectively, during CalWater 2015. The DOE-sponsored ARM Cloud Aerosol and Precipitation Experiment (ACAPEX) was executed in close coordination with NOAA and NASA facilities and deployed airborne and ship-based observing systems. This presentation summarizes the objectives, implementation strategy, data acquisitions, and some preliminary results from CalWater 2015 addressing science gaps associated with (1) the evolution and structure of ARs including cloud and precipitation processes and air-sea interaction, and (2) aerosol interaction with ARs and the impact on precipitation, including locally-generated aerosol effects on orographic

  6. Effects of diethylenetriamine and Aerosol OT on the stability of oil-in-water emulsion stabilized by interfacial polyurea film.

    PubMed

    Mikami, T

    1994-01-01

    The stability of oil-in-water emulsions containing a triisocyanate soluble in the oil phase and an amine in the water phase was investigated. The oil component was di-n-butyl phthalate (DBP) containing Aerosol OT as an emulsifier. The time required for the average size parameter to reach a constant value was studied. It was found that the polyurea film produced by an interfacial polymerization reaction between the amine and the triisocyanate contributed to forming a stable emulsion at a lower Aerosol OT concentration, but at a higher Aerosol OT concentration the amine did not show any effect on the emulsion stability.

  7. 2015 AAAR Conference Symposium: "The Role of Water in Aerosol Chemistry"

    SciTech Connect

    McNeill, V. Faye; Weber, Rodney

    2015-10-16

    The DOE-sponsored symposium, "The Role of Water in Aerosol Chemistry" was held at the 2015 Annual meeting of AAAR. The funding supported, in part, travel, lodging, and registration expenses for invited symposium speakers, and travel and lodging expenses allowing students to attend and make presentations at a special conference symposium that focuses on topics of interest to the U.S. DOE Atmospheric System Research (ASR) program.

  8. CalWater 2 - Precipitation, Aerosols, and Pacific Atmospheric Rivers Experiment

    NASA Astrophysics Data System (ADS)

    Spackman, J. R.; Ralph, F. M.; Prather, K. A.; Cayan, D. R.; DeMott, P. J.; Dettinger, M. D.; Fairall, C. W.; Leung, L. R.; Rosenfeld, D.; Rutledge, S. A.; Waliser, D. E.; White, A. B.

    2014-12-01

    Emerging research has identified two phenomena that play key roles in the variability of the water supply and the incidence of extreme precipitation events along the West Coast of the United States. These phenomena include the role of (1) atmospheric rivers (ARs) in delivering much of the precipitation associated with major storms along the U.S. West Coast, and (2) aerosols—from local sources as well as those transported from remote continents—and their modulating effects on western U.S. precipitation. A better understanding of these processes is needed to reduce uncertainties in weather predictions and climate projections of extreme precipitation and its effects, including the provision of beneficial water supply. This presentation summarizes the science objectives and strategies to address gaps associated with (1) the evolution and structure of ARs including cloud and precipitation processes and air-sea interaction, and (2) aerosol interaction with ARs and the impact on precipitation, including locally-generated aerosol effects on orographic precipitation along the U.S. West Coast. Observations are proposed for multiple winter seasons as part of a 5-year broad interagency vision referred to as CalWater 2 to address these science gaps (http://esrl.noaa.gov/psd/calwater). In January-February 2015, a field campaign has been planned consisting of a targeted set of aircraft and ship-based measurements and associated evaluation of data in near-shore regions of California and in the eastern Pacific. In close coordination with NOAA, DOE's Atmospheric Radiation Measurement (ARM) program is also contributing air and shipborne facilities for ACAPEX (ARM Cloud Aerosol and Precipitation Experiment), a DOE-sponsored study complementing CalWater 2. Ground-based measurements from NOAA's HydroMeteorological Testbed (HMT) network in California and aerosol chemical instrumentation at Bodega Bay, California have been designed to add important near surface-level context for the

  9. Tropical intercontinental optical measurement network of aerosol, precipitable water and total column ozone

    NASA Technical Reports Server (NTRS)

    Holben, B. N.; Tanre, D.; Reagan, J. A.; Eck, T. F.; Setzer, A.; Kaufman, Y. A.; Vermote, E.; Vassiliou, G. D.; Lavenu, F.

    1992-01-01

    A new generation of automatic sunphotometers is used to systematically monitor clear sky total column aerosol concentration and optical properties, precipitable water and total column ozone diurnally and annually in West Africa and South America. The instruments are designed to measure direct beam sun, solar aureole and sky radiances in nine narrow spectral bands from the UV to the near infrared on an hourly basis. The instrumentation and the algorithms required to reduce the data for subsequent analysis are described.

  10. 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.

  11. Fluorescent water-soluble organic aerosols in the High Arctic atmosphere

    PubMed Central

    Fu, Pingqing; Kawamura, Kimitaka; Chen, Jing; Qin, Mingyue; Ren, Lujie; Sun, Yele; Wang, Zifa; Barrie, Leonard A.; Tachibana, Eri; Ding, Aijun; Yamashita, Youhei

    2015-01-01

    Organic aerosols are ubiquitous in the earth’s atmosphere. They have been extensively studied in urban, rural and marine environments. However, little is known about the fluorescence properties of water-soluble organic carbon (WSOC) or their transport to and distribution in the polar regions. Here, we present evidence that fluorescent WSOC is a substantial component of High Arctic aerosols. The ratios of fluorescence intensity of protein-like peak to humic-like peak generally increased from dark winter to early summer, indicating an enhanced contribution of protein-like organics from the ocean to Arctic aerosols after the polar sunrise. Such a seasonal pattern is in agreement with an increase of stable carbon isotope ratios of total carbon (δ13CTC) from −26.8‰ to −22.5‰. Our results suggest that Arctic aerosols are derived from a combination of the long-range transport of terrestrial organics and local sea-to-air emission of marine organics, with an estimated contribution from the latter of 8.7–77% (mean 45%). PMID:25920042

  12. Evidence for Recent Liquid Water on Mars

    NASA Technical Reports Server (NTRS)

    2000-01-01

    Gullies eroded into the wall of a meteor impact crater in Noachis Terra. This high resolution view (top left) from the Mars Global Surveyor (MGS) Mars Orbiter Camera (MOC) shows channels and associated aprons of debris that are interpreted to have formed by groundwater seepage, surface runoff, and debris flow. The lack of small craters superimposed on the channels and apron deposits indicates that these features are geologically young. It is possible that these gullies indicate that liquid water is present within the martian subsurface today. The MOC image was acquired on September 28, 1999. The scene covers an area approximately 3 kilometers (1.9 miles) wide by 6.7 km (4.1 mi) high (note, the aspect ratio is 1.5 to 1.0). Sunlight illuminates this area from the upper left. The image is located near 54.8S, 342.5W. The context image (above) shows the location of the MOC image on the south-facing wall of an impact crater approximately 20 kilometers (12 miles) in diameter. The context picture was obtained by the Viking 1 orbiter in 1980 and is illuminated from the upper left. The large mound on the floor of the crater in the context view is a sand dune field. The Mars Orbiter Camera high resolution images are taken black-and-white (grayscale); the color seen here has been synthesized from the colors of Mars observed by the MOC wide angle cameras and by the Viking Orbiters in the late 1970s. A brief description of how the color was generated: The MOC narrow angle camera only takes grayscale (black and white) pictures. To create the color versions seen here, we have taken much lower resolution red and blue images acquired by the MOC's wide angle cameras, and by the Viking Orbiter cameras in the 1970s, synthesized a green image by averaging red and blue, and created a pallete of colors that represent the range of colors on Mars. We then use a relationship that correlates color and brightness to assign a color to each gray level. This is only a crude approximation of

  13. Mobile multi-wavelength polarization Raman lidar for water vapor, cloud and aerosol measurement.

    PubMed

    Wu, Songhua; Song, Xiaoquan; Liu, Bingyi; Dai, Guangyao; Liu, Jintao; Zhang, Kailin; Qin, Shengguang; Hua, Dengxin; Gao, Fei; Liu, Liping

    2015-12-28

    Aiming at the detection of atmospheric water vapor mixing ratio, depolarization ratio, backscatter coefficient, extinction coefficient and cloud information, the Water vapor, Cloud and Aerosol Lidar (WACAL) is developed by the lidar group at Ocean University of China. The lidar consists of transmitter, receiver, data acquisition and auxiliary system. For the measurement of various atmospheric physical properties, three channels including Raman channel, polarization channel and infrared channel are integrated in WACAL. The integration and working principle of these channels are introduced in details. The optical setup, the housekeeping of the system and the data retrieval routines are also presented. After the completion of the construction of the lidar, the WACAL system was installed in Ocean University of China (36.165°N, 120.5°E), Qingdao for the measurement of atmosphere during 2013 and 2014. The measurement principles and some case studies corresponding to various atmospheric physical properties are provided. Finally, the result of one continuous measurement example operated on 13 June 2014 is presented. The WACAL can measure the aerosol and cloud optical properties as well as the water vapor mixing ratio. It is useful for studying the direct and indirect effects of the aerosol on the climate change.

  14. Water: The Liquid of Life. Fifth Grade.

    ERIC Educational Resources Information Center

    Illinois State Environmental Protection Agency, Springfield.

    These materials are for use by elementary and middle school teachers in the state of Illinois. This document contains five modules for teaching water conservation. Topics include: (1) "Life Depends on Water,""What is Water?" and "The Hydrologic Cycle"; (2) "The Treatment of Drinking Water"; (3)…

  15. Importance of Accurate Liquid Water Path for Estimation of Solar Radiation in Warm Boundary Layer Clouds: An Observational Study

    SciTech Connect

    Sengupta, Manajit; Clothiaux, Eugene E.; Ackerman, Thomas P.; Kato, Seiji; Min, Qilong

    2003-09-15

    A one-year observational study of overcast boundary layer stratus at the U.S. Department of Energy Atmospheric Radiation Measurement Program Southern Great Plains site illustrates that surface radiation is primarily sensitive to cloud liquid water path, with cloud drop effective radius having a secondary influence. The mean, median and standard deviation of cloud liquid water path and cloud drop effective radius for the dataset are 0.120 mm, 0.101 mm, 0.108 mm, and 7.38 {micro}m, 7.13 {micro}m, 2.39 {micro}m, respectively. Radiative transfer calculations demonstrate that cloud optical depth and cloud normalized forcing are respectively three and six times as sensitive to liquid water path variations as they are to effective radius variations, when the observed ranges of each of those variables is considered. Overall, there is a 79% correlation between observed and computed surface fluxes when using a fixed effective radius of 7.5 {micro}m and observed liquid water paths in the calculations. One conclusion from this study is that measurement of the indirect aerosol effect will be problematic at the site, as variations in cloud liquid water path will most likely mask effects of variations in particle size.

  16. Process for blending coal with water immiscible liquid

    DOEpatents

    Heavin, Leonard J.; King, Edward E.; Milliron, Dennis L.

    1982-10-26

    A continuous process for blending coal with a water immiscible liquid produces a uniform, pumpable slurry. Pulverized raw feed coal and preferably a coal derived, water immiscible liquid are continuously fed to a blending zone (12 and 18) in which coal particles and liquid are intimately admixed and advanced in substantially plug flow to form a first slurry. The first slurry is withdrawn from the blending zone (12 and 18) and fed to a mixing zone (24) where it is mixed with a hot slurry to form the pumpable slurry. A portion of the pumpable slurry is continuously recycled to the blending zone (12 and 18) for mixing with the feed coal.

  17. Ice-Crystal Fallstreaks from Supercooled Liquid Water Parent Clouds

    NASA Technical Reports Server (NTRS)

    Campbell, James R.; O'C. Starr, David; Welton, Ellsworth J.; Spinhirne, James D.; Ferrare, Richard A.

    2003-01-01

    On 31 December 2001, ice-crystal fallstreaks (e.g., cirrus uncinus, or colloquially "Mare's Tails") from supercooled liquid water parent clouds were observed by ground-based lidars pointed vertically from the Atmospheric Radiation Measurement Southern Great Plains (SGP) facility near Lamont, Oklahoma. The incidence of liquid phase cloud with apparent ice-phase precipitation is investigated. Scenarios for mixed-phase particle nucleation, and fallstreak formation and sustenance are discussed. The observations are unique in the context of the historical reverence given to the commonly observed c h s uncinus fallstreak (wholly ice) versus this seemingly contradictory coincidence of liquid water begetting ice-crystal streaks.

  18. Characterisation of microstructures formed in isopropyl palmitate/water/Aerosol OT:1-butanol (2:1) system.

    PubMed

    Boonme, P; Krauel, K; Graf, A; Rades, T; Junyaprasert, V B

    2006-11-01

    The aim of this work was to determine the type and microstructure of microemulsion samples formed in IPP/water/AerosolOT:1-butanol (2:1) systems as a case study for the investigation of microemulsions. The concentration of the surfactant/cosurfactant mixture was kept constant while the ratio of water to oil was varied. Several techniques were used to investigate the types and phase transitions of the microemulsion formulations. The experimental methods used included visual observation cross-polarized light microscopy (PLM) appearance, conductivity, viscosity, cryo-field emission scanning electron microscopy (cryo-FESEM), differential scanning calorimetry (DSC), nuclear magnetic resonance (NMR), and fluorescence resonance energy transfer (FRET). Taken together, the results of the various techniques imply that the systems investigated are undergoing two transitions as a function of water concentration. Between 10-15%w/w of water, the systems change from headgroup hydrated surfactant solutions in oil (or possibly very small reversed micellar systems) to w/o microemulsions. These systems then change to o/w microemulsions between 25-30%w/w of water. The transitions however, appear to be gradual, as for example the DSC data indicates a transition between 15-20%w/w of water. Furthermore, for some methods the changes observed were very weak, and only with supportive data of other techniques can the phase behaviour of the microemulsion systems be interpreted with confidence. Interestingly, no indication of the presence of a bicontinuous intermediate microstructure was found. Liquid crystal formation was detected in samples containing 55%w/w of water.

  19. Cluster Monte Carlo and numerical mean field analysis for the water liquid-liquid phase transition

    NASA Astrophysics Data System (ADS)

    Mazza, Marco G.; Stokely, Kevin; Strekalova, Elena G.; Stanley, H. Eugene; Franzese, Giancarlo

    2009-04-01

    Using Wolff's cluster Monte Carlo simulations and numerical minimization within a mean field approach, we study the low temperature phase diagram of water, adopting a cell model that reproduces the known properties of water in its fluid phases. Both methods allow us to study the thermodynamic behavior of water at temperatures, where other numerical approaches - both Monte Carlo and molecular dynamics - are seriously hampered by the large increase of the correlation times. The cluster algorithm also allows us to emphasize that the liquid-liquid phase transition corresponds to the percolation transition of tetrahedrally ordered water molecules.

  20. Liquid Water in the Extremely Shallow Martian Subsurface

    NASA Technical Reports Server (NTRS)

    Pavlov, A.; Shivak, J. N.

    2012-01-01

    Availability of liquid water is one of the major constraints for the potential Martian biosphere. Although liquid water is unstable on the surface of Mars due to low atmospheric pressures, it has been suggested that liquid films of water could be present in the Martian soil. Here we explored a possibility of the liquid water formation in the extremely shallow (1-3 cm) subsurface layer under low atmospheric pressures (0.1-10 mbar) and low ("Martian") surface temperatures (approx.-50 C-0 C). We used a new Goddard Martian simulation chamber to demonstrate that even in the clean frozen soil with temperatures as low as -25C the amount of mobile water can reach several percents. We also showed that during brief periods of simulated daylight warming the shallow subsurface ice sublimates, the water vapor diffuses through porous surface layer of soil temporarily producing supersaturated conditions in the soil, which leads to the formation of additional liquid water. Our results suggest that despite cold temperatures and low atmospheric pressures, Martian soil just several cm below the surface can be habitable.

  1. A Simple Model of Global Aerosol Indirect Effects

    SciTech Connect

    Ghan, Steven J.; Smith, Steven J.; Wang, Minghuai; Zhang, Kai; Pringle, K. J.; Carslaw, K. S.; Pierce, Jeffrey; Bauer, Susanne E.; Adams, P. J.

    2013-06-28

    Most estimates of the global mean indirect effect of anthropogenic aerosol on the Earth’s energy balance are from simulations by global models of the aerosol lifecycle coupled with global models of clouds and the hydrologic cycle. Extremely simple models have been developed for integrated assessment models, but lack the flexibility to distinguish between primary and secondary sources of aerosol. Here a simple but more physically-based model expresses the aerosol indirect effect using analytic representations of droplet nucleation, cloud and aerosol vertical structure, and horizontal variability in cloud water and aerosol concentration. Although the simple model is able to produce estimates of aerosol indirect effects that are comparable to those from some global aerosol models using the same global mean aerosol properties, the estimates are found to be sensitive to several uncertain parameters, including the preindustrial cloud condensation nuclei concentration, primary and secondary anthropogenic emissions, the size of the primary particles, the fraction of the secondary anthropogenic emissions that accumulates on the coarse mode, the fraction of the secondary mass that forms new particles, and the sensitivity of liquid water path to droplet number concentration. Aerosol indirect effects are surprisingly linear in emissions. This simple model provides a much stronger physical basis for representing aerosol indirect effects than previous representations in integrated assessment models designed to quickly explore the parameter space of emissions-climate interactions. The model also produces estimates that depend on parameter values in ways that are consistent with results from detailed global aerosol-climate simulation models.

  2. Spatial separation of individual substances in effloresced crystals of ternary ammonium sulphate/dicarboxylic acid/water aerosols.

    PubMed

    Treuel, Lennart; Sandmann, Alice; Zellner, Reinhard

    2011-04-18

    This work examines the crystals resulting from the efflorescence of internally mixed aqueous aerosols comprising ammonium sulphate and different dicarboxylic acids. Most studies on the deliquescence of aerosols use previously effloresced aerosols in their experiments. However, during efflorescence a highly supersaturated solution crystallises in a kinetically controlled way unlike the case of thermodynamically controlled crystallisation. Herein the distribution of individual substances within the effloresced crystals is investigated using Raman scanning experiments. The data presented show an intriguingly complex behaviour of these ternary and quarternary aerosols. A spatial separation of substances in the crystals resulting from the efflorescence of previously internally mixed ternary salt/dicarboxylic acid/water aerosol droplets is demonstrated and mechanistic aspects are discussed.

  3. On the Water Uptake and CCN Activation of Tropospheric Organic Aerosols

    NASA Astrophysics Data System (ADS)

    Rastak, Narges; Pajunoja, Aki; Acosta Navarro, Juan-Camilo; Leong, Yu Jun; Cerully, Kate M.; Nenes, Athanasios; Kirkevåg, Alf; Topping, David; Virtanen, Annele; Riipinen, Ilona

    2016-04-01

    Aerosol particles introduce high uncertainties to radiative climate forcing. If exposed to a given relative humidity (RH), aerosol particles containing soluble material can absorb water and grow in size (hygroscopic growth). If RH is increased further beyond supersaturation (RH >100%) the particles can act as cloud condensation nuclei (CCN). Aerosol particles interactions with water vapour determine to a large extent their influence on climate. Organic aerosols (OA) contribute a large fraction (20-90%) of atmospheric submicron particulate mass, on the other hand they often consist of thousands of compounds with different properties. One of these properties is solubility, which affects the hygroscopic growth and cloud condensation nucleus (CCN) activation of the organic particles. We investigate the hygroscopic behaviour of complex organic aerosols accounting for the distribution of solubilities present in these mixtures. We use the SPARC method to estimate the solubility distributions of isoprene (IP) and monoterpene (MT) SOA based on their chemical composition, as predicted by the Master Chemical Mechanism (MCM). Combining these solubility distributions with the adsorption theory along with the non-ideal behaviour of organic mixtures, we predict the expected hygroscopic growth factors (HGFs), CCN activation behaviour and the related hygroscopicity parameters kappa for these mixtures. The predictions are compared to laboratory measurements as well as field data from MT- and IP-dominated measurement sites. The predicted solubility distributions do a good job in explaining the water uptake of these two mixture types at high relative humidities (RH around 90%), as well as their CCN activation - including the potential differences between the kappa values derived from HGF vs. CCN data. At lower relative humidities, however, the observed water uptake is higher than predicted on solubility alone, particularly for the MT-derived SOA. The data from the low RHs are further

  4. Detection and quantification of water-based aerosols using active open-path FTIR

    NASA Astrophysics Data System (ADS)

    Kira, Oz; Linker, Raphael; Dubowski, Yael

    2016-04-01

    Aerosols have a leading role in many eco-systems and knowledge of their properties is critical for many applications. This study suggests using active Open-Path Fourier Transform Infra-Red (OP-FTIR) spectroscopy for quantifying water droplets and solutes load in the atmosphere. The OP-FTIR was used to measure water droplets, with and without solutes, in a 20 m spray tunnel. Three sets of spraying experiments generated different hydrosols clouds: (1) tap water only, (2) aqueous ammonium sulfate (0.25–3.6%wt) and (3) aqueous ethylene glycol (0.47–2.38%wt). Experiment (1) yielded a linear relationship between the shift of the extinction spectrum baseline and the water load in the line-of-sight (LOS) (R2 = 0.984). Experiment (2) also yielded a linear relationship between the integrated extinction in the range of 880–1150 cm‑1 and the ammonium sulfate load in the LOS (R2 = 0.972). For the semi-volatile ethylene glycol (experiment 3), present in the gas and condense phases, quantification was much more complex and two spectral approaches were developed: (1) according to the linear relationship from the first experiment (determination error of 8%), and (2) inverse modeling (determination error of 57%). This work demonstrates the potential of the OP-FTIR for detecting clouds of water-based aerosols and for quantifying water droplets and solutes at relatively low concentrations.

  5. Review: Drinking water for liquid-fed pigs.

    PubMed

    Meunier-Salaün, M-C; Chiron, J; Etore, F; Fabre, A; Laval, A; Pol, F; Prunier, A; Ramonet, Y; Nielsen, B L

    2016-11-07

    Liquid feeding has the potential to provide pigs with sufficient water to remain hydrated and prevent prolonged thirst. However, lack of permanent access to fresh water prevents animals from drinking when they are thirsty. Moreover, individual differences between pigs in a pen may result in uneven distribution of the water provided by the liquid feed, leading to some pigs being unable to meet their water requirements. In this review, we look at the need for and provision of water for liquid-fed pigs in terms of their production performance, behaviour, health and welfare. We highlight factors which may lead to water ingestion above or below requirements. Increases in the need for water may be caused by numerous factors such as morbidity, ambient temperature or competition within the social group, emphasising the necessity of permanent access to water as also prescribed in EU legislation. The drinkers can be the target of redirected behaviour in response to feed restriction or in the absence of rooting materials, thereby generating water losses. The method of water provision and drinker design is critical to ensure easy access to water regardless of the pig's physiological state, and to limit the amount of water used, which does not benefit the pig.

  6. Flow-Tube Investigations of Hypergolic Reactions of a Dicyanamide Ionic Liquid Via Tunable Vacuum Ultraviolet Aerosol Mass Spectrometry.

    PubMed

    Chambreau, Steven D; Koh, Christine J; Popolan-Vaida, Denisia M; Gallegos, Christopher J; Hooper, Justin B; Bedrov, Dmitry; Vaghjiani, Ghanshyam L; Leone, Stephen R

    2016-10-07

    The unusually high heats of vaporization of room-temperature ionic liquids (RTILs) complicate the utilization of thermal evaporation to study ionic liquid reactivity. Although effusion of RTILs into a reaction flow-tube or mass spectrometer is possible, competition between vaporization and thermal decomposition of the RTIL can greatly increase the complexity of the observed reaction products. In order to investigate the reaction kinetics of a hypergolic RTIL, 1-butyl-3-methylimidazolium dicyanamide (BMIM(+)DCA(-)) was aerosolized and reacted with gaseous nitric acid, and the products were monitored via tunable vacuum ultraviolet photoionization time-of-flight mass spectrometry at the Chemical Dynamics Beamline 9.0.2 at the Advanced Light Source. Reaction product formation at m/z 42, 43, 44, 67, 85, 126, and higher masses was observed as a function of HNO3 exposure. The identities of the product species were assigned to the masses on the basis of their ionization energies. The observed exposure profile of the m/z 67 signal suggests that the excess gaseous HNO3 initiates rapid reactions near the surface of the RTIL aerosol. Nonreactive molecular dynamics simulations support this observation, suggesting that diffusion within the particle may be a limiting step. The mechanism is consistent with previous reports that nitric acid forms protonated dicyanamide species in the first step of the reaction.

  7. Joint retrieval of aerosol and water-leaving radiance from multispectral, multiangular and polarimetric measurements over ocean

    NASA Astrophysics Data System (ADS)

    Xu, Feng; Dubovik, Oleg; Zhai, Peng-Wang; Diner, David J.; Kalashnikova, Olga V.; Seidel, Felix C.; Litvinov, Pavel; Bovchaliuk, Andrii; Garay, Michael J.; van Harten, Gerard; Davis, Anthony B.

    2016-07-01

    An optimization approach has been developed for simultaneous retrieval of aerosol properties and normalized water-leaving radiance (nLw) from multispectral, multiangular, and polarimetric observations over ocean. The main features of the method are (1) use of a simplified bio-optical model to estimate nLw, followed by an empirical refinement within a specified range to improve its accuracy; (2) improved algorithm convergence and stability by applying constraints on the spatial smoothness of aerosol loading and Chlorophyll a (Chl a) concentration across neighboring image patches and spectral constraints on aerosol optical properties and nLw across relevant bands; and (3) enhanced Jacobian calculation by modeling and storing the radiative transfer (RT) in aerosol/Rayleigh mixed layer, pure Rayleigh-scattering layers, and ocean medium separately, then coupling them to calculate the field at the sensor. This approach avoids unnecessary and time-consuming recalculations of RT in unperturbed layers in Jacobian evaluations. The Markov chain method is used to model RT in the aerosol/Rayleigh mixed layer and the doubling method is used for the uniform layers of the atmosphere-ocean system. Our optimization approach has been tested using radiance and polarization measurements acquired by the Airborne Multiangle SpectroPolarimetric Imager (AirMSPI) over the AERONET USC_SeaPRISM ocean site (6 February 2013) and near the AERONET La Jolla site (14 January 2013), which, respectively, reported relatively high and low aerosol loadings. Validation of the results is achieved through comparisons to AERONET aerosol and ocean color products. For comparison, the USC_SeaPRISM retrieval is also performed by use of the Generalized Retrieval of Aerosol and Surface Properties algorithm (Dubovik et al., 2011). Uncertainties of aerosol and nLw retrievals due to random and systematic instrument errors are analyzed by truth-in/truth-out tests with three Chl a concentrations, five aerosol loadings

  8. Is It Possible to Distinguish Between Dust and Salt Aerosol Over Waters with Unknown Chlorophyll Concentrations Using Spectral Remote Sensing?

    NASA Technical Reports Server (NTRS)

    Levy, R. C.; Kaufman, Y. J.

    1999-01-01

    Atmospheric aerosol has uncertain impacts on the global climate system, as well as on atmospheric and bio-geo-chemical processes of regional and local scales. EOS-MODIS is one example of a satellite sensor designed to improve understanding of the aerosols' type, size and distribution at all temporal and spatial scales. Ocean scientists also plan to use data from EOS-MODIS to assess the temporal and spatial coverage of in-water chlorophyll. MODIS is the first sensor planned to observe the combined ocean-atmosphere system with a wide spectral range (from 410 to 2200 nm). Dust aerosol and salt aerosol have similar spectral signals for wavelengths longer than 550 nm, but because dust selectively absorbs blue light, they have divergent signals in the blue wavelength regions (412 to 490 nm). Chlorophyll also selectively absorbs blue radiation, so that varying chlorophyll concentrations produces a highly varying signal in the blue regions, but less variability in the green, and almost no signal in the red to mid-infrared regions. Thus, theoretically, it may be difficult to differentiate dust and salt in the presence of unknown chlorophyll in the ocean. This study attempts to address the cases in which aerosol and chlorophyll signals can and cannot be separated. For the aerosol spectra, we use the aerosol lookup table from the operational MODIS aerosol-over-ocean algorithm, and for chlorophyll spectra, we use the SeaBAM data set (created for SeaWiFS). We compare the signals using Principal Component Analysis and attempt to retrieve both chlorophyll and aerosol properties using a variant of the operational MODIS aerosol-over-ocean algorithm. Results show that for small optical depths, less than 0.5, it is not possible to differentiate between dust and salt and to determine the chlorophyll concentration at the same time. For larger aerosol optical depths, the chlorophyll signals are comparatively insignificant, and we can hope to distinguish between dust and salt.

  9. LASE Measurements of Water Vapor, Aerosol, and Cloud Distributions in Saharan Air Layers and Tropical Disturbances

    NASA Technical Reports Server (NTRS)

    Ismail, Syed; Ferrare, Richard; Browell, Edward; Kooi, Susan; Notari, Anthony; Butler, Carolyn; Burton, Sharon; Fenn, Marta; Krishnamurti, T. N.; Dunion, Jason; Heymsfield, Gerry; Anderson, Bruce

    2008-01-01

    LASE (Lidar Atmospheric Sensing Experiment) onboard the NASA DC-8 was used to measure high resolution profiles of water vapor and aerosols, and cloud distributions in 14 flights over the eastern Atlantic region during the NAMMA (NASA African Monsoon Multidisciplinary Analyses) field experiment, which was conducted from August 15 to September 12, 2006. These measurements were made in conjunction with flights designed to study African Easterly Waves (AEW), Tropical Disturbances (TD), and Saharan Aerosol Layers (SALs) as well as flights performed in clear air and convective regions. As a consequence of their unique radiative properties and dynamics, SAL layers have a significant influence in the development of organized convection associated with TD. Interactions of the SAL with tropical air during early stages of the development of TD were observed. These LASE measurements represent the first simultaneous water vapor and aerosol lidar measurements to study the SAL and its impact on TDs and hurricanes. Seven AEWs were studied and four of these evolved into tropical storms and three did not. Three out of the four tropical storms evolved into hurricanes.

  10. Concentrations and composition of aerosols and particulate matter in surface waters along the transatlantic section

    NASA Astrophysics Data System (ADS)

    Nemirovskaya, I. A.; Lisitzin, A. P.; Novigatsky, A. N.; Redzhepova, Z. U.; Dara, O. M.

    2016-07-01

    Along the transatlantic section from Ushuaia to Gdańsk (March 26-May 7, 2015; cruise 47 of R/V Akademik Ioffe), data were obtained on the concentrations of aerosols in the near-water layer of the atmosphere and of particulate matter in surface waters, as well as of organic compounds within the considered matter (Corg, chlorophyll a, lipids, and hydrocarbons). The concentrations of aerosols amounted to 1237-111 739 particles/L for the fraction of 0.3-1 μm and to 0.02-34.4 μg/m2/day for the matter collected by means of the network procedure. The distribution of aerosols is affected by circumcontinental zoning and by the fluxes from arid areas of African deserts. The maximum concentration of the treated compounds were found in the river-sea frontal area (the runoff of the Colorado River, Argentina), as well as when nearing the coasts, especially in the English Channel.

  11. A mobile remote sensing laboratory for water vapor, trace gas, aerosol, and wind speed measurements

    SciTech Connect

    Slaughter, D.; White, W.; Tulloch, W.; DeSlover, D.

    1993-03-19

    The Lawrence Livermore National Laboratory has developed a mobile field laboratory for remote measurement of atmospheric processes and observables that are important in global climate change, dispersal of hazardous materials, and atmospheric pollution. Specific observables of interest are water vapor, trace gases, aerosol size and density, wind, and temperature. The goal is to study atmospheric processes continuously for extended periods in remote field locations. This laboratory has just reached field ready status with sensors for aerosol and trace gas measurement based on established techniques. A development program is underway to enhance the sensor suite with several new techniques and instruments that are expected to significantly extend the state of the art in remote trace gas analysis. The new sensors will be incorporated into the lab during the next two years.

  12. Effect of particle water on ozone and secondary organic aerosol formation from benzene-NO2-NaCl irradiations

    NASA Astrophysics Data System (ADS)

    Wang, Yujie; Luo, Hao; Jia, Long; Ge, Shuangshuang

    2016-09-01

    Ozone (O3) and secondary organic aerosol (SOA) are important pollutants in the urban atmosphere. Benzene is one of the most important aromatic species in urban air, which could produce O3 and SOA in the presence of NOx (x = 1, 2) and UV light. A series of experiments was carried out to study the effect of particle water on O3 and SOA formation from benzene under various humid conditions in an indoor smog chamber. The results show that the peak O3 concentrations decreased with the increase of RH or the mass concentration of liquid NaCl particles. The peak O3 concentration reduced by 30% as RH increased from 9% to 87% with the similar initial concentrations of NaCl (about 46 μg m-3), and decreased by 10% as the initial NaCl concentrations increased from 36.0 μg m-3 to 152.1 μg m-3 at about 73% RH. The relationships between liquid water content (LWC) and O3 or SOA were investigated. The results show that LWC is the key factor that leads to an opposite effect on O3 and SOA formation from benzene. The peak O3 concentration exponentially decreased 37% as LWC0 increased from zero to 349.8 μg m-3. Heterogeneous reaction of dinitrogen pentoxide (N2O5) with particle water is the major reason for the decrease of O3. The yields of SOA increased from 5.2 to 10.5% as LWC0 increased from zero to 349.8 μg m-3. The relative intensities of bands Osbnd H, Cdbnd O, Csbnd OH and NO3- increased by 22.9, 6.8, 6.7 and 13.1 times respectively as compared with dry condition. Alcohols or hydrates are confirmed to be the major contributors to SOA with increasing LWC.

  13. The putative liquid-liquid transition is a liquid-solid transition in atomistic models of water. II

    SciTech Connect

    Limmer, David T.; Chandler, David

    2013-06-07

    This paper extends our earlier studies of free energy functions of density and crystalline order parameters for models of supercooled water, which allows us to examine the possibility of two distinct metastable liquid phases [D. T. Limmer and D. Chandler, J. Chem. Phys.135, 134503 (2011) and preprint http://arxiv.org/abs/arXiv:1107.0337 (2011)]. Low-temperature reversible free energy surfaces of several different atomistic models are computed: mW water, TIP4P/2005 water, Stillinger-Weber silicon, and ST2 water, the last of these comparing three different treatments of long-ranged forces. In each case, we show that there is one stable or metastable liquid phase, and there is an ice-like crystal phase. The time scales for crystallization in these systems far exceed those of structural relaxation in the supercooled metastable liquid. We show how this wide separation in time scales produces an illusion of a low-temperature liquid-liquid transition. The phenomenon suggesting metastability of two distinct liquid phases is actually coarsening of the ordered ice-like phase, which we elucidate using both analytical theory and computer simulation. For the latter, we describe robust methods for computing reversible free energy surfaces, and we consider effects of electrostatic boundary conditions. We show that sensible alterations of models and boundary conditions produce no qualitative changes in low-temperature phase behaviors of these systems, only marginal changes in equations of state. On the other hand, we show that altering sampling time scales can produce large and qualitative non-equilibrium effects. Recent reports of evidence of a liquid-liquid critical point in computer simulations of supercooled water are considered in this light.

  14. Charge-on-spring polarizable water models revisited: From water clusters to liquid water to ice

    NASA Astrophysics Data System (ADS)

    Yu, Haibo; van Gunsteren, Wilfred F.

    2004-11-01

    The properties of two improved versions of charge-on-spring (COS) polarizable water models (COS/G2 and COS/G3) that explicitly include nonadditive polarization effects are reported. In COS models, the polarization is represented via a self-consistently induced dipole moment consisting of a pair of separated charges. A previous polarizable water model (COS/B2), upon which the improved versions are based, was developed by Yu, Hansson, and van Gunsteren [J. Chem. Phys. 118, 221 (2003)]. To improve the COS/B2 model, which overestimated the dielectric permittivity, one additional virtual atomic site was used to reproduce the water monomer quadrupole moments besides the water monomer dipole moment in the gas phase. The molecular polarizability, residing on the virtual atomic site, and Lennard-Jones parameters for oxygen-oxygen interactions were varied to reproduce the experimental values for the heat of vaporization and the density of liquid water at room temperature and pressure. The improved models were used to study the properties of liquid water at various thermodynamic states as well as gaseous water clusters and ice. Overall, good agreement is obtained between simulated properties and those derived from experiments and ab initio calculations. The COS/G2 and COS/G3 models may serve as simple, classical, rigid, polarizable water models for the study of organic solutes and biopolymers. Due to its simplicity, COS type of polarization can straightforwardly be used to introduce explicit polarization into (bio)molecular force fields.

  15. Inorganic, organic and macromolecular components of fine aerosol in different areas of Europe in relation to their water solubility

    NASA Astrophysics Data System (ADS)

    Zappoli, S.; Andracchio, A.; Fuzzi, S.; Facchini, M. C.; Gelencsér, A.; Kiss, G.; Krivácsy, Z.; Molnár, Á.; Mészáros, E.; Hansson, H.-C.; Rosman, K.; Zebühr, Y.

    A chemical mass balance of fine aerosol (<1.5 μm AED) collected at three European sites was performed with reference to the water solubility of the different aerosol classes of components. The sampling sites are characterised by different pollution conditions and aerosol loading in the air. Aspvreten is a background site in central Sweden, K-puszta is a rural site in the Great Hungarian Plain and San Pietro Capofiume is located in the polluted Po Valley, northern Italy. The average fine aerosol mass concentration was 5.9 μg m -3 at the background site Aspvreten, 24 μg m -3 at the rural K-puszta and 38 μg m -3 at the polluted site San Pietro Capofiume. However, a similarly high soluble fraction of the aerosol (65-75%) was measured at the three sites, while the percentage of water soluble organic species with respect to the total soluble mass was much higher at the background site (ca. 50%) than at the other two sites (ca. 25%). A very high fraction (over 70%) of organic compounds in the aerosol consisted of polar species. The presence of water soluble macromolecular compounds was revealed in the samples from K-puszta and San Pietro Capofiume. At both sites these species accounted for between ca. 20-50% of the water soluble organic fraction. The origin of the compounds was tentatively attributed to biomass combustion.

  16. Behavior of supercooled aqueous solutions stemming from hidden liquid-liquid transition in water

    NASA Astrophysics Data System (ADS)

    Biddle, John W.; Holten, Vincent; Anisimov, Mikhail A.

    2014-08-01

    A popular hypothesis that explains the anomalies of supercooled water is the existence of a metastable liquid-liquid transition hidden below the line of homogeneous nucleation. If this transition exists and if it is terminated by a critical point, the addition of a solute should generate a line of liquid-liquid critical points emanating from the critical point of pure metastable water. We have analyzed thermodynamic consequences of this scenario. In particular, we consider the behavior of two systems, H2O-NaCl and H2O-glycerol. We find the behavior of the heat capacity in supercooled aqueous solutions of NaCl, as reported by Archer and Carter [J. Phys. Chem. B 104, 8563 (2000)], to be consistent with the presence of the metastable liquid-liquid transition. We elucidate the non-conserved nature of the order parameter (extent of "reaction" between two alternative structures of water) and the consequences of its coupling with conserved properties (density and concentration). We also show how the shape of the critical line in a solution controls the difference in concentration of the coexisting liquid phases.

  17. Behavior of supercooled aqueous solutions stemming from hidden liquid-liquid transition in water.

    PubMed

    Biddle, John W; Holten, Vincent; Anisimov, Mikhail A

    2014-08-21

    A popular hypothesis that explains the anomalies of supercooled water is the existence of a metastable liquid-liquid transition hidden below the line of homogeneous nucleation. If this transition exists and if it is terminated by a critical point, the addition of a solute should generate a line of liquid-liquid critical points emanating from the critical point of pure metastable water. We have analyzed thermodynamic consequences of this scenario. In particular, we consider the behavior of two systems, H2O-NaCl and H2O-glycerol. We find the behavior of the heat capacity in supercooled aqueous solutions of NaCl, as reported by Archer and Carter [J. Phys. Chem. B 104, 8563 (2000)], to be consistent with the presence of the metastable liquid-liquid transition. We elucidate the non-conserved nature of the order parameter (extent of "reaction" between two alternative structures of water) and the consequences of its coupling with conserved properties (density and concentration). We also show how the shape of the critical line in a solution controls the difference in concentration of the coexisting liquid phases.

  18. Dependence of marine stratocumulus reflectivities on liquid water paths

    NASA Technical Reports Server (NTRS)

    Coakley, James A., Jr.; Snider, Jack B.

    1990-01-01

    Simple parameterizations that relate cloud liquid water content to cloud reflectivity are often used in general circulation climate models to calculate the effect of clouds in the earth's energy budget. Such parameterizations have been developed by Stephens (1978) and by Slingo and Schrecker (1982) and others. Here researchers seek to verify the parametric relationship through the use of simultaneous observations of cloud liquid water content and cloud reflectivity. The column amount of cloud liquid was measured using a microwave radiometer on San Nicolas Island following techniques described by Hogg et al., (1983). Cloud reflectivity was obtained through spatial coherence analysis of Advanced Very High Resolution Radiometer (AVHRR) imagery data (Coakley and Beckner, 1988). They present the dependence of the observed reflectivity on the observed liquid water path. They also compare this empirical relationship with that proposed by Stephens (1978). Researchers found that by taking clouds to be isotropic reflectors, the observed reflectivities and observed column amounts of cloud liquid water are related in a manner that is consistent with simple parameterizations often used in general circulation climate models to determine the effect of clouds on the earth's radiation budget. Attempts to use the results of radiative transfer calculations to correct for the anisotropy of the AVHRR derived reflectivities resulted in a greater scatter of the points about the relationship expected between liquid water path and reflectivity. The anisotropy of the observed reflectivities proved to be small, much smaller than indicated by theory. To critically assess parameterizations, more simultaneous observations of cloud liquid water and cloud reflectivities and better calibration of the AVHRR sensors are needed.

  19. Characterization of cumulus cloud fields using trajectories in the center of gravity versus water mass phase space: 2. Aerosol effects on warm convective clouds: Center of Gravity Versus Water Mass 2

    SciTech Connect

    Heiblum, Reuven H.; Altaratz, Orit; Koren, Ilan; Feingold, Graham; Kostinski, Alexander B.; Khain, Alexander P.; Ovchinnikov, Mikhail; Fredj, Erick; Dagan, Guy; Pinto, Lital; Yaish, Ricki; Chen, Qian

    2016-06-07

    In Part I of this work a 3D cloud tracking algorithm and phase-space of center of gravity altitude versus cloud liquid water mass (CvM space) were introduced and described in detail. We showed how new physical insight can be gained by following cloud trajectories in the CvM space. Here, this approach is used to investigate aerosol effects on cloud fields of warm cumuli. We show a clear effect of the aerosol loading on the shape and size of CvM clusters. We also find fundamental differences in the CvM space between simulations using bin versus bulk microphysical schemes, with the bin scheme precipitation expressing much higher sensitivity to changes in aerosol concentrations. Using the bin microphysical scheme, we find that the increase in cloud center of gravity altitude with increase in aerosol concentrations occurs for a wide range of cloud sizes. This is attributed to reduced sedimentation, increased buoyancy and vertical velocities, and increased environmental instability, all of which are tightly coupled to inhibition of precipitation processes and subsequent feedbacks of clouds on their environment. Many of the physical processes shown here are consistent with processes typically associated with cloud invigoration.

  20. New Examination of the Traditional Raman Lidar Technique II: Evaluating the Ratios for Water Vapor and Aerosols

    NASA Technical Reports Server (NTRS)

    Whiteman, David N.

    2003-01-01

    In a companion paper, the temperature dependence of Raman scattering and its influence on the Raman and Rayleigh-Mie lidar equations was examined. New forms of the lidar equation were developed to account for this temperature sensitivity. Here those results are used to derive the temperature dependent forms of the equations for the water vapor mixing ratio, aerosol scattering ratio, aerosol backscatter coefficient, and extinction to backscatter ratio (Sa). The error equations are developed, the influence of differential transmission is studied and different laser sources are considered in the analysis. The results indicate that the temperature functions become significant when using narrowband detection. Errors of 5% and more can be introduced in the water vapor mixing ratio calculation at high altitudes and errors larger than 10% are possible for calculations of aerosol scattering ratio and thus aerosol backscatter coefficient and extinction to backscatter ratio.

  1. Mass-based hygroscopicity parameter interaction model and measurement of atmospheric aerosol water uptake

    NASA Astrophysics Data System (ADS)

    Mikhailov, E.; Merkulov, V.; Vlasenko, S.; Rose, D.; Pöschl, U.

    2011-11-01

    In this study we derive and apply a mass-based hygroscopicity parameter interaction model for efficient description of concentration-dependent water uptake by atmospheric aerosol particles. The model approach builds on the single hygroscopicity parameter model of Petters and Kreidenweis (2007). We introduce an observable mass-based hygroscopicity parameter κm, which can be deconvoluted into a dilute intrinsic hygroscopicity parameter (κm,∞) and additional self- and cross-interaction parameters describing non-ideal solution behavior and concentration dependencies of single- and multi-component systems. For sodium chloride, the κm-interaction model (KIM) captures the observed concentration and humidity dependence of the hygroscopicity parameter and is in good agreement with an accurate reference model based on the Pitzer ion-interaction approach (Aerosol Inorganic Model, AIM). For atmospheric aerosol samples collected from boreal rural air and from pristine tropical rainforest air (secondary organic aerosol) we present first mass-based measurements of water uptake over a wide range of relative humidity (1-99%) obtained with a new filter-based differential hygroscopicity analyzer (FDHA) technique. By application of KIM to the measurement data we can distinguish three different regimes of hygroscopicity in the investigated aerosol samples: (I) A quasi-eutonic regime at low relative humidity (~60% RH) where the solutes co-exist in an aqueous and non-aqueous phase; (II) a gradually deliquescent regime at intermediate humidity (~60%-90% RH) where different solutes undergo gradual dissolution in the aqueous phase; and (III) a dilute regime at high humidity (≳90% RH) where the solutes are fully dissolved approaching their dilute intrinsic hygroscopicity. The characteristic features of the three hygroscopicity regimes are similar for both samples, while the RH threshold values vary as expected for samples of different chemical composition. In each regime, the

  2. Experimental Evidence for a Liquid-Liquid Crossover in Deeply Cooled Confined Water

    NASA Astrophysics Data System (ADS)

    Cupane, Antonio; Fomina, Margarita; Piazza, Irina; Peters, Judith; Schirò, Giorgio

    2014-11-01

    In this work we investigate, by means of elastic neutron scattering, the pressure dependence of mean square displacements (MSD) of hydrogen atoms of deeply cooled water confined in the pores of a three-dimensional disordered SiO2 xerogel; experiments have been performed at 250 and 210 K from atmospheric pressure to 1200 bar. The "pressure anomaly" of supercooled water (i.e., a mean square displacement increase with increasing pressure) is observed in our sample at both temperatures; however, contrary to previous simulation results and to the experimental trend observed in bulk water, the pressure effect is smaller at lower (210 K) than at higher (250 K) temperature. Elastic neutron scattering results are complemented by differential scanning calorimetry data that put in evidence, besides the glass transition at about 170 K, a first-order-like endothermic transition occurring at about 230 K that, in view of the neutron scattering results, can be attributed to a liquid-liquid crossover. Our results give experimental evidence for the presence, in deeply cooled confined water, of a crossover occurring at about 230 K (at ambient pressure) from a liquid phase predominant at 210 K to another liquid phase predominant at 250 K; therefore, they are fully consistent with the liquid-liquid transition hypothesis.

  3. A Mechanism for Recent Production of Liquid Water on Mars

    NASA Technical Reports Server (NTRS)

    Hecht, M. H.; Bridges, N. T.

    2003-01-01

    Though Mars is a cold, dry planet, with respect to the thermal stability of liquid water at low altitudes it is not terribly different from comparably cold places on Earth. In dry air such water would evaporate faster on Mars, at a rate comparable to a 60 C hot spring on Earth, but the heat loss associated with that evaporation would be mitigated by the poor thermal convection in the thin Martian air. Even at higher altitudes where the atmospheric pressure does not reach the triple point of water, liquid water might theoretically exist in a low-vapor pressure form such as wet soil, in a briny solution, or simply under a layer of dust or snow. The theoretical stability of liquid water does not suggest its occurrence, either on Mars or in Antarctica. In fact, global models have suggested that locations capable of providing sufficient heat for melting are, precisely for that reason, too dry for water to be present. However, the temperature of irregular local structures such as trenches or craters can be markedly warmer than those of the uniform surfaces of global models. The work described here suggests a plausible scenario in which seasonal liquid water might be produced locally, in sheltered locations, through a process of condensation, cold-trapping, buffering, and melting. While the amounts produced in the present climate would be small, copious amounts of meltwater may have been produced at other phases of the orbital cycle, as recently as 20,000 years ago.

  4. The puzzling unsolved mysteries of liquid water: Some recent progress

    NASA Astrophysics Data System (ADS)

    Stanley, H. E.; Kumar, P.; Xu, L.; Yan, Z.; Mazza, M. G.; Buldyrev, S. V.; Chen, S.-H.; Mallamace, F.

    2007-12-01

    Water is perhaps the most ubiquitous, and the most essential, of any molecule on earth. Indeed, it defies the imagination of even the most creative science fiction writer to picture what life would be like without water. Despite decades of research, however, water's puzzling properties are not understood and 63 anomalies that distinguish water from other liquids remain unsolved. We introduce some of these unsolved mysteries, and demonstrate recent progress in solving them. We present evidence from experiments and computer simulations supporting the hypothesis that water displays a special transition point (which is not unlike the “tipping point” immortalized by Malcolm Gladwell). The general idea is that when the liquid is near this “tipping point,” it suddenly separates into two distinct liquid phases. This concept of a new critical point is finding application to other liquids as well as water, such as silicon and silica. We also discuss related puzzles, such as the mysterious behavior of water near a protein.

  5. Evaluation of CALIOP 532-nm Aerosol Optical Depth Over Opaque Water Clouds

    NASA Technical Reports Server (NTRS)

    Liu, Z.; Winker, D.; Omar, A.; Vaughan, M.; Kar, J.; Trepte, C.; Hu, Y.; Schuster, G.

    2015-01-01

    With its height-resolved measurements and near global coverage, the CALIOP lidar onboard the CALIPSO satellite offers a new capability for aerosol retrievals in cloudy skies. Validation of these retrievals is difficult, however, as independent, collocated and co-temporal data sets are generally not available. In this paper, we evaluate CALIOP aerosol products above opaque water clouds by applying multiple retrieval techniques to CALIOP Level 1 profile data and comparing the results. This approach allows us to both characterize the accuracy of the CALIOP above-cloud aerosol optical depth (AOD) and develop an error budget that quantifies the relative contributions of different error sources. We focus on two spatial domains: the African dust transport pathway over the tropical North Atlantic and the African smoke transport pathway over the southeastern Atlantic. Six years of CALIOP observations (2007-2012) from the northern hemisphere summer and early fall are analyzed. The analysis is limited to cases where aerosol layers are located above opaque water clouds so that a constrained retrieval technique can be used to directly retrieve 532 nm aerosol optical depth and lidar ratio. For the moderately dense Sahara dust layers detected in the CALIOP data used in this study, the mean/median values of the lidar ratios derived from a constrained opaque water cloud (OWC) technique are 45.1/44.4 +/- 8.8 sr, which are somewhat larger than the value of 40 +/- 20 sr used in the CALIOP Level 2 (L2) data products. Comparisons of CALIOP L2 AOD with the OWC-retrieved AOD reveal that for nighttime conditions the L2 AOD in the dust region is underestimated on average by approx. 26% (0.183 vs. 0.247). Examination of the error sources indicates that errors in the L2 dust AOD are primarily due to using a lidar ratio that is somewhat too small. The mean/median lidar ratio retrieved for smoke is 70.8/70.4 +/- 16.2 sr, which is consistent with the modeled value of 70 +/- 28 sr used in the

  6. PD-FiTE - an efficient method for calculating gas / liquid equilibria in atmospheric aerosol particles

    NASA Astrophysics Data System (ADS)

    Topping, D.; Lowe, D.; McFiggans, G.; Barley, M.

    2009-04-01

    Assessing the impact of atmospheric aerosol particles on the environment requires adequate representation of appropriate key processes within large scale models. In the absence of primary particulate material, interactions between the atmospheric gaseous components and particles means that the chemical nature of the particles is largely determined by the availability of condensable gaseous material, such as sulphuric and nitric acids, and by the ambient environmental conditions. Gas to particle mass transfer of semi-volatile components,driven by a difference in equilibrium and actual partial pressures above an aerosol particle, is an important factor in determining the evolving chemical composition of the particle and is necessary for predicting aerosol loading and composition. The design of an appropriate framework required for parameterizations of key variables is challenging. These thermodynamic frameworks are often numerically very complex, resulting in significant computational expense. Three dimensional chemical and aerosol transport models demand that computational expense be kept at a minimum,resulting in a trade-off between accuracy and efficiency. To calculate the equilibrium vapour pressure above a solution requires treatment of solution nonideality. This is manifest through activity coefficients of components pertinent to each condensing specie. However, activity coefficients are complex functions of the solution composition. Parameterisation of activity coefficients provides the main focus of this work largely because reducing the numerical complexity whilst retaining a good level of accuracy is very challenging. The approach presented here, the hybrid Partial Derivative Fitted Taylor Expansion (PDFiTE) (Topping et al 2008), builds on previously reported work, with an aim to derive parameters for an accurate and computationally efficient framework through coupling with a complex thermodynamic model. Such a reduction in complexity is important as it is

  7. A new water-based liquid scintillator and potential applications

    NASA Astrophysics Data System (ADS)

    Yeh, M.; Hans, S.; Beriguete, W.; Rosero, R.; Hu, L.; Hahn, R. L.; Diwan, M. V.; Jaffe, D. E.; Kettell, S. H.; Littenberg, L.

    2011-12-01

    In this paper we describe a new type of scintillating liquid based on water. We describe the concept, preparation, and properties of this liquid, and how it could be used for a very large, but economical detector. The applications of such a detector range from fundamental physics such as nucleon decay and neutrino physics to physics with broader application such as neutron detection. We briefly describe the scientific requirements of these applications, and how they can be satisfied by the new material.

  8. Amorphous and crystalline aerosol particles interacting with water vapor: conceptual framework and experimental evidence for restructuring, phase transitions and kinetic limitations

    NASA Astrophysics Data System (ADS)

    Mikhailov, E.; Vlasenko, S.; Martin, S. T.; Koop, T.; Pöschl, U.

    2009-12-01

    Interactions with water are crucial for the properties, transformation and climate effects of atmospheric aerosols. Here we present a conceptual framework for the interaction of amorphous aerosol particles with water vapor, outlining characteristic features and differences in comparison to crystalline particles. We used a hygroscopicity tandem differential mobility analyzer (H-TDMA) to characterize the hydration and dehydration of crystalline ammonium sulfate, amorphous oxalic acid and amorphous levoglucosan particles (diameter ~100 nm, relative humidity 5-95% at 298 K). The experimental data and accompanying Köhler model calculations provide new insights into particle microstructure, surface adsorption, bulk absorption, phase transitions and hygroscopic growth. The results of these and related investigations lead to the following conclusions: (1) Many organic substances, including carboxylic acids, carbohydrates and proteins, tend to form amorphous rather than crystalline phases upon drying of aqueous solution droplets. Depending on viscosity and microstructure, the amorphous phases can be classified as glasses, rubbers, gels or viscous liquids. (2) Amorphous organic substances tend to absorb water vapor and undergo gradual deliquescence and hygroscopic growth at lower relative humidity than their crystalline counterparts. (3) In the course of hydration and dehydration, certain organic substances can form rubber- or gel-like structures (supramolecular networks) and undergo transitions between swollen and collapsed network structures. (4) Organic gels or (semi-)solid amorphous shells (glassy, rubbery, ultra-viscous) with low molecular diffusivity can kinetically limit the uptake and release of water and may influence the hygroscopic growth and activation of aerosol particles as cloud condensation nuclei (CCN) and ice nuclei (IN). Moreover, (semi-)solid amorphous phases may influence the uptake of gaseous photo-oxidants and the chemical transformation and aging of

  9. Comparison of Aerosol Optical Properties and Water Vapor Among Ground and Airborne Lidars and Sun Photometers During TARFOX

    NASA Technical Reports Server (NTRS)

    Ferrare, R.; Ismail, S.; Browell, E.; Brackett, V.; Clayton, M.; Kooi, S.; Melfi, S. H.; Whiteman, D.; Schwemmer, G.; Evans, K.

    2000-01-01

    We compare aerosol optical thickness (AOT) and precipitable water vapor (PWV) measurements derived from ground and airborne lidars and sun photometers during the Tropospheric Aerosol Radiative Forcing Observational Experiment. Such comparisons are important to verify the consistency between various remote sensing measurements before employing them in any assessment of the impact of aerosols on the global radiation balance. Total scattering ratio and extinction profiles measured by the ground-based NASA Goddard Space Flight Center scanning Raman lidar system, which operated from Wallops Island, Virginia (37.86 deg N, 75.51 deg W); are compared with those measured by the Lidar Atmospheric Sensing Experiment (LASE) airborne lidar system aboard the NASA ER-2 aircraft. Bias and root-mean-square differences indicate that these measurements generally agreed within about 10%. Aerosol extinction profiles and estimates of AOT are derived from both lidar measurements using a value for the aerosol extinction/backscattering ratio S(sub a) = 60 sr for the aerosol extinction/backscattering ratio, which was determined from the Raman lidar measurements. The lidar measurements of AOT are found to be generally within 25% of the AOT measured by the NASA Ames Airborne Tracking Sun Photometer (AATS-6). However, during certain periods the lidar and Sun photometer measurements of AOT differed significantly, possibly because of variations in the aerosol physical characteristics (e.g., size, composition) which affect S(sub a). Estimates of PWV, derived from water vapor mixing ratio profiles measured by LASE, are within 5-10% of PWV derived from the airborne Sun photometer. Aerosol extinction profiles measured by both lidars show that aerosols were generally concentrated in the lowest 2-3 km.

  10. CalWater 2 - Precipitation, Aerosols, and Pacific Atmospheric Rivers Experiment

    NASA Astrophysics Data System (ADS)

    Spackman, Ryan; Ralph, Marty; Prather, Kim; Cayan, Dan; DeMott, Paul; Dettinger, Mike; Fairall, Chris; Leung, Ruby; Rosenfeld, Daniel; Rutledge, Steven; Waliser, Duane; White, Allen

    2014-05-01

    Emerging research has identified two phenomena that play key roles in the variability of the water supply and the incidence of extreme precipitation events along the West Coast of the United States. These phenomena include the role of (1) atmospheric rivers (ARs) in delivering much of the precipitation associated with major storms along the U.S. West Coast, and (2) aerosols—from local sources as well as those transported from remote continents—and their modulating effects on western U.S. precipitation. A better understanding of these processes is needed to reduce uncertainties in weather predictions and climate projections of extreme precipitation and its effects, including the provision of beneficial water supply. This presentation summarizes science gaps associated with (1) the evolution and structure of ARs including cloud and precipitation processes and air-sea interaction, and (2) aerosol interaction with ARs and the impact on precipitation, including locally-generated aerosol effects on orographic precipitation along the U.S. West Coast. Observations are proposed for multiple winter seasons as part of a 5-year broad interagency vision referred to as CalWater 2 to address these science gaps (http://esrl.noaa.gov/psd/calwater). In the near term, a science investigation is being planned including a targeted set of aircraft and ship-based measurements and associated evaluation of data in near-shore regions of California and in the eastern Pacific for an intensive observing period between January 2015 and March 2015. DOE's Atmospheric Radiation Measurement (ARM) program and NOAA are coordinating on deployment of airborne and ship-borne facilities for this period in a DOE-sponsored study called ACAPEX (ARM Cloud Aerosol and Precipitation Experiment) to complement CalWater 2. The motivation for this major study is based on findings that have emerged in the last few years from airborne and ground-based studies including CalWater and NOAA's HydroMeterology Testbed

  11. Measurements of mass and heat transfer at a liquid water surface during condensation or evaporation of a subnanometer thickness layer of water.

    PubMed

    Miles, Rachael E H; Knox, Kerry J; Reid, Jonathan P; Laurain, Adèle M C; Mitchem, Laura

    2010-09-10

    A novel approach for exploring the molecular dynamics during condensation or evaporation at a liquid water surface is reported at pressures between 2 and 100 kPa. By introducing or removing a heating laser illuminating an optically tweezed aqueous aerosol droplet, the temperature of the droplet can be controlled with sub-mK accuracy and the change in size to reequilibrate with the surroundings monitored with subnanometer accuracy. The time constant for equilibration is shown to provide important insight into the coupling of heat and mass transfer during condensation or evaporation.

  12. Hygroscopic behavior of water-soluble matter in marine aerosols over the East China Sea.

    PubMed

    Yan, Yu; Fu, Pingqing; Jing, Bo; Peng, Chao; Boreddy, S K R; Yang, Fan; Wei, Lianfang; Sun, Yele; Wang, Zifa; Ge, Maofa

    2017-02-01

    In this study, we investigated hygroscopic properties of water-soluble matter (WSM) in marine aerosols over the East China Sea, which were collected during a Natural Science Foundation of China (NSFC) sharing cruise in 2014. Hygroscopic growth factors (g) of WSM were measured by a hygroscopicity tandem differential mobility analyzer (H-TDMA) with an initial dry particle mobility diameter of 100nm. The observed g at 90% relative humidity (RH), g(90%)WSM, defined as the ratio of the particle diameter at 90% RH to that at RH<5% (initial dry diameter), ranged from 1.67 to 2.41 (mean±std: 1.99±0.23). The g values were lower than that of seawater (2.1) but comparable with those reported for marine aerosols (1.79-2.08). The H-TDMA retrieved hygroscopicity parameter of WSM, κWSM, ranged from 0.46 to 1.56 (0.88±0.35). The observed g(90%)WSM during the daytime ranged from 1.67 to 2.40 (1.95±0.21) versus 1.71 to 2.41 (2.03±0.26) during the nighttime. κWSM was 0.81±0.32 in the daytime and 0.95±0.40 in the nighttime. The day/night differences of g(90%)WSM and κWSM indicated that nighttime marine aerosols were more hygroscopic than those in daytime, which was likely related to enhanced heterogeneous reaction of ammonium nitrate in nighttime and the higher Cl(-)/Na(+) molar ratios obtained (0.80) in nighttime than those (0.47) in daytime. Inorganic ions accounted for 72-99% of WSM with SO4(2-) being the dominant species, contributing to 47% of the total inorganic ion mass. The declined g(90%) comparing with sea water was likely due to the transport of anthropogenic aerosols, chemical aging of dust particles, the contribution of biomass burning products, and the aerosol hygroscopic growth inhibition of organics.

  13. Global Analysis of Aerosol Properties Above Clouds

    NASA Technical Reports Server (NTRS)

    Waquet, F.; Peers, F.; Ducos, F.; Goloub, P.; Platnick, S. E.; Riedi, J.; Tanre, D.; Thieuleux, F.

    2013-01-01

    The seasonal and spatial varability of Aerosol Above Cloud (AAC) properties are derived from passive satellite data for the year 2008. A significant amount of aerosols are transported above liquid water clouds on the global scale. For particles in the fine mode (i.e., radius smaller than 0.3 m), including both clear sky and AAC retrievals increases the global mean aerosol optical thickness by 25(+/- 6%). The two main regions with man-made AAC are the tropical Southeast Atlantic, for biomass burning aerosols, and the North Pacific, mainly for pollutants. Man-made AAC are also detected over the Arctic during the spring. Mineral dust particles are detected above clouds within the so-called dust belt region (5-40 N). AAC may cause a warming effect and bias the retrieval of the cloud properties. This study will then help to better quantify the impacts of aerosols on clouds and climate.

  14. Aerosolized ZnO nanoparticles induce toxicity in alveolar type II epithelial cells at the air-liquid interface

    SciTech Connect

    Xie, Yumei; Williams, Nolann G.; Tolic, Ana; Chrisler, William B.; Teeguarden, Justin G.; Maddux, Bettye L.; Pounds, Joel G.; Laskin, Alexander; Orr, Galya

    2012-01-20

    The majority of in vitro studies characterizing the impact of engineered nanoparticles (NPs) on cells that line the respiratory tract were conducted in cells exposed to NPs in suspension. This approach introduces processes that are unlikely to occur during inhaled NP exposures in vivo, such as the shedding of toxic doses of dissolved ions. ZnO NPs are used extensively and pose significant sources for human exposure. Exposures to airborne ZnO NPs can induce adverse effects, but the relevance of the dissolved Zn2+ to the observed effects in vivo is still unclear. Our goal was to mimic in vivo exposures to airborne NPs and decipher the contribution of the intact NP from the contribution of the dissolved ions to airborne ZnO NP toxicity. We established the exposure of alveolar type II epithelial cells to aerosolized NPs at the air-liquid interface (ALI), and compared the impact of aerosolized ZnO NPs and NPs in suspension at the same cellular doses, measured as the number of particles per cell. By evaluating membrane integrity and cell viability 6 and 24 hours post exposure we found that aerosolized NPs induced toxicity at the ALI at doses that were in the same order of magnitude as doses required to induce toxicity in submersed cultures. In addition, distinct patterns of oxidative stress were observed in the two exposure systems. These observations unravel the ability of airborne ZnO NPs to induce toxicity without the contribution of dissolved Zn2+ and suggest distinct mechanisms at the ALI and in submersed cultures.

  15. Solid−liquid critical behavior of water in nanopores

    PubMed Central

    Mochizuki, Kenji; Koga, Kenichiro

    2015-01-01

    Nanoconfined liquid water can transform into low-dimensional ices whose crystalline structures are dissimilar to any bulk ices and whose melting point may significantly rise with reducing the pore size, as revealed by computer simulation and confirmed by experiment. One of the intriguing, and as yet unresolved, questions concerns the observation that the liquid water may transform into a low-dimensional ice either via a first-order phase change or without any discontinuity in thermodynamic and dynamic properties, which suggests the existence of solid−liquid critical points in this class of nanoconfined systems. Here we explore the phase behavior of a model of water in carbon nanotubes in the temperature−pressure−diameter space by molecular dynamics simulation and provide unambiguous evidence to support solid−liquid critical phenomena of nanoconfined water. Solid−liquid first-order phase boundaries are determined by tracing spontaneous phase separation at various temperatures. All of the boundaries eventually cease to exist at the critical points and there appear loci of response function maxima, or the Widom lines, extending to the supercritical region. The finite-size scaling analysis of the density distribution supports the presence of both first-order and continuous phase changes between solid and liquid. At around the Widom line, there are microscopic domains of two phases, and continuous solid−liquid phase changes occur in such a way that the domains of one phase grow and those of the other evanesce as the thermodynamic state departs from the Widom line. PMID:26100904

  16. Water soluble organic aerosols in the Colorado Rocky Mountains, USA: composition, sources and optical properties

    PubMed Central

    Xie, Mingjie; Mladenov, Natalie; Williams, Mark W.; Neff, Jason C.; Wasswa, Joseph; Hannigan, Michael P.

    2016-01-01

    Atmospheric aerosols have been shown to be an important input of organic carbon and nutrients to alpine watersheds and influence biogeochemical processes in these remote settings. For many remote, high elevation watersheds, direct evidence of the sources of water soluble organic aerosols and their chemical and optical characteristics is lacking. Here, we show that the concentration of water soluble organic carbon (WSOC) in the total suspended particulate (TSP) load at a high elevation site in the Colorado Rocky Mountains was strongly correlated with UV absorbance at 254 nm (Abs254, r = 0.88 p < 0.01) and organic carbon (OC, r = 0.95 p < 0.01), accounting for >90% of OC on average. According to source apportionment analysis, biomass burning had the highest contribution (50.3%) to average WSOC concentration; SOA formation and motor vehicle emissions dominated the contribution to WSOC in the summer. The source apportionment and backward trajectory analysis results supported the notion that both wildfire and Colorado Front Range pollution sources contribute to the summertime OC peaks observed in wet deposition at high elevation sites in the Colorado Rocky Mountains. These findings have important implications for water quality in remote, high-elevation, mountain catchments considered to be our pristine reference sites. PMID:27991554

  17. Water soluble organic aerosols in the Colorado Rocky Mountains, USA: composition, sources and optical properties

    NASA Astrophysics Data System (ADS)

    Xie, Mingjie; Mladenov, Natalie; Williams, Mark W.; Neff, Jason C.; Wasswa, Joseph; Hannigan, Michael P.

    2016-12-01

    Atmospheric aerosols have been shown to be an important input of organic carbon and nutrients to alpine watersheds and influence biogeochemical processes in these remote settings. For many remote, high elevation watersheds, direct evidence of the sources of water soluble organic aerosols and their chemical and optical characteristics is lacking. Here, we show that the concentration of water soluble organic carbon (WSOC) in the total suspended particulate (TSP) load at a high elevation site in the Colorado Rocky Mountains was strongly correlated with UV absorbance at 254 nm (Abs254, r = 0.88 p < 0.01) and organic carbon (OC, r = 0.95 p < 0.01), accounting for >90% of OC on average. According to source apportionment analysis, biomass burning had the highest contribution (50.3%) to average WSOC concentration; SOA formation and motor vehicle emissions dominated the contribution to WSOC in the summer. The source apportionment and backward trajectory analysis results supported the notion that both wildfire and Colorado Front Range pollution sources contribute to the summertime OC peaks observed in wet deposition at high elevation sites in the Colorado Rocky Mountains. These findings have important implications for water quality in remote, high-elevation, mountain catchments considered to be our pristine reference sites.

  18. Impacts of Sulfate Seed Acidity and Water Content on Isoprene Secondary Organic Aerosol Formation.

    PubMed

    Wong, Jenny P S; Lee, Alex K Y; Abbatt, Jonathan P D

    2015-11-17

    The effects of particle-phase water and the acidity of pre-existing sulfate seed particles on the formation of isoprene secondary organic aerosol (SOA) was investigated. SOA was generated from the photo-oxidation of isoprene in a flow tube reactor at 70% relative humidity (RH) and room temperature in the presence of three different sulfate seeds (effloresced and deliquesced ammonium sulfate and ammonium bisulfate) under low NOx conditions. High OH exposure conditions lead to little isoprene epoxydiol (IEPOX) SOA being generated. The primary result is that particle-phase water had the largest effect on the amount of SOA formed, with 60% more SOA formation occurring with deliquesced ammonium sulfate seeds as compared to that on effloresced ones. The additional organic material was highly oxidized. Although the amount of SOA formed did not exhibit a dependence on the range of seed particle acidity examined, perhaps because of the low amount of IEPOX SOA, the levels of high-molecular-weight material increased with acidity. While the uptake of organics was partially reversible under drying, the results nevertheless indicate that particle-phase water enhanced the amount of organic aerosol material formed and that the RH cycling of sulfate particles may mediate the extent of isoprene SOA formation in the atmosphere.

  19. LASE measurements of water vapor, aerosol, and cloud distribution in hurricane environments and their role in hurricane development

    NASA Technical Reports Server (NTRS)

    Mahoney, M. J.; Ismail, S.; Browell, E. V.; Ferrare, R. A.; Kooi, S. A.; Brasseur, L.; Notari, A.; Petway, L.; Brackett, V.; Clayton, M.; Halverson, J.; Rizvi, S.; Krishn, T. N.

    2002-01-01

    LASE measures high resolution moisture, aerosol, and cloud distributions not available from conventional observations. LASE water vapor measurements were compared with dropsondes to evaluate their accuracy. LASE water vapor measurements were used to assess the capability of hurricane models to improve their track accuracy by 100 km on 3 day forecasts using Florida State University models.

  20. On the Stability of Liquid Water on Present Day Mars

    NASA Technical Reports Server (NTRS)

    Haberle, Robert M.; DeVincenzi, Donald L. (Technical Monitor)

    2000-01-01

    The mean annual surface pressure and temperature on present day Mars do not allow for the long term stability of liquid water on the surface. However, theoretical arguments have been advanced that suggest liquid water could form in transient events even though it would not be in equilibrium with the environment. Using a Mars General Circulation Model, we calculate where and for how long the surface pressure and surface temperature meet the minimum requirements for this metastability of liquid water. These requirements are that the pressure and temperature must be above the triple point of water, but below its boiling point. We find that there are five regions on Mars where these requirements are periodically satisfied: in the near equatorial regions of Amazonis, Arabia, and Elysium, and in the Hellas and Argyre impact basins. Whether liquid water ever forms in these regions depends on the availability of ice and heat, and on the evaporation rate. The latter is poorly understood for low pressure CO2 environments, but is likely to be so high that melting occurs rarely, if at all. However, in the relatively recent past, surface pressures may have been higher than they are today perhaps by as much as a factor of 2 or 3. Under these circumstances melting would have been easier to achieve. We plan to undertake laboratory experiments to better understand the potential for melting in low pressure environments.

  1. A new liquid chromatography method with charge aerosol detector (CAD) for the determination of phospholipid classes. Application to milk phospholipids.

    PubMed

    Kiełbowicz, Grzegorz; Micek, Piotr; Wawrzeńczyk, Czesław

    2013-02-15

    A new rapid method for the quantitative analysis of five classes of phospholipids (PLs) (phosphatidylcholine--PC, lysophosphatidylcholine--LPC, phosphatidylethanolamine--PE and phosphatidylserine--PS and phosphatidylinositol--PI) using liquid chromatography with charge aerosol detector (CAD) is described. The separation of the compounds of interest was achieved on a diol stationary phase with a mobile phase consisting of 13% HCOOH, hexane and 2-propanol in 19 min elution program, including 10 min equilibration of the column. The method was applied to characterize the phospholipid fractions of cow milk. PLs present in cow milk were separated by solid-phase extraction (SPE) procedure with Si cartridges before LC analysis with recovery ranging from 95.3% to 104.4%. The use of CAD detection of the eluted compounds was precise, linear and sensitive.

  2. On the Fluctuations that Order and Frustrate Liquid Water

    NASA Astrophysics Data System (ADS)

    Limmer, David Tyler

    At ambient conditions, water sits close to phase coexistence with its crystal. More so than in many other materials, this fact is manifested in the fluctuations that maintain a large degree of local order in the liquid. These fluctuations and how they result in long-ranged order, or its absence, are emergent features of many interacting molecules. Their study therefore requires using the tools of statistical mechanics for their their systematic understanding. In this dissertation we develop such an understanding. In particular, we focus on collective behavior that emerges in liquid and solid water. At room temperatures, the thermophysical properties of water are quantified and rationalized with simple molecular models. A key feature of these models is the correct characterization of the competition between entropic forces of packing and the energetic preference for tetrahedral order. At cold temperatures, the properties of ice surfaces are studied with statistical field theory. The theory we develop for the long wavelength features of ice interfaces allows us to explain the existence of a premelting layer on the surface of ice and the stability of ice in confinement. In between these extremes, the dynamics of supercooled water are considered. A detailed theory for the early stages of coarsening is developed and used to explain the peculiar observation of a transient second liquid state of water. When coarsening dynamics are arrested, the result is the formation of a glassy states of water. We show that out-of-equilibrium the phase diagram for supercooled water exhibits a rich amount of structure, including a triple point between two glass phases of water and the liquid. At the end, we explore possible technological implications for the interplay between ordering and frustration in studies of water at metal interfaces.

  3. Development of a dispersive liquid-liquid microextraction method using a lighter-than-water ionic liquid for the analysis of polycyclic aromatic hydrocarbons in water.

    PubMed

    Medina, Giselle S; Reta, Mario

    2016-11-01

    A dispersive liquid-liquid microextraction method using a lighter-than-water phosphonium-based ionic liquid for the extraction of 16 polycyclic aromatic hydrocarbons from water samples has been developed. The extracted compounds were analyzed by liquid chromatography coupled to fluorescence/diode array detectors. The effects of several experimental parameters on the extraction efficiency, such as type and volume of ionic liquid and disperser solvent, type and concentration of salt in the aqueous phase and extraction time, were investigated and optimized. Three phosphonium-based ionic liquids were assayed, obtaining larger extraction efficiencies when trihexyl-(tetradecyl)phosphonium bromide was used. The optimized methodology requires a few microliters of a lighter-than-water phosphonium-based ionic liquid, which allows an easy separation of the extraction solvent phase. The obtained limits of detection were between 0.02 and 0.56 μg/L, enrichment factors between 109 and 228, recoveries between 60 and 108%, trueness between 0.4 and 9.9% and reproducibility values between 3 and 12% were obtained. These figures of merit combined with the simplicity, rapidity and low cost of the analytical methodology indicate that this is a viable and convenient alternative to the methods reported in the literature. The developed method was used to analyze polycyclic aromatic hydrocarbons in river water samples.

  4. Detection and quantification of water-based aerosols using active open-path FTIR

    PubMed Central

    Kira, Oz; Linker, Raphael; Dubowski, Yael

    2016-01-01

    Aerosols have a leading role in many eco-systems and knowledge of their properties is critical for many applications. This study suggests using active Open-Path Fourier Transform Infra-Red (OP-FTIR) spectroscopy for quantifying water droplets and solutes load in the atmosphere. The OP-FTIR was used to measure water droplets, with and without solutes, in a 20 m spray tunnel. Three sets of spraying experiments generated different hydrosols clouds: (1) tap water only, (2) aqueous ammonium sulfate (0.25–3.6%wt) and (3) aqueous ethylene glycol (0.47–2.38%wt). Experiment (1) yielded a linear relationship between the shift of the extinction spectrum baseline and the water load in the line-of-sight (LOS) (R2 = 0.984). Experiment (2) also yielded a linear relationship between the integrated extinction in the range of 880–1150 cm−1 and the ammonium sulfate load in the LOS (R2 = 0.972). For the semi-volatile ethylene glycol (experiment 3), present in the gas and condense phases, quantification was much more complex and two spectral approaches were developed: (1) according to the linear relationship from the first experiment (determination error of 8%), and (2) inverse modeling (determination error of 57%). This work demonstrates the potential of the OP-FTIR for detecting clouds of water-based aerosols and for quantifying water droplets and solutes at relatively low concentrations. PMID:27121498

  5. Characteristics of Water-Soluble Inorganic Ions in Aerosol Particles in Jingjinji-Mega Typical Cities

    NASA Astrophysics Data System (ADS)

    Wang, Li

    2013-06-01

    Aerosol has important effects on climate, environment and human health and water-soluble ions are important chemical composition in aerosol. It is important to study concentration levels, sources and size distributions of water-soluble ions in aerosol. In recent years, with the increasing of energy consumption and the amount of automobile, regional pollution has become more serious in Beijing-Tianjin-Hebei Region. Especially since the haze happened frequently in Beijing-Tianjin-Hebei Region, it is an imminent study about water-soluble ions in aerosol.To investigate the concentration levels, sources and size distributions of water soluble inorganic ions (WSI), size-segregated aerosol samples were collected using Andersen cascade sampler from Aug2010to Aug2011in Beijing, Tianjin, Tangshan and Baoding. The WSI were analyzed by ion chromatography(IC).The results indicated that the order of total WSI (TWSI) concentration of TSP in the region was Tianjin-Baoding-Beijing-Tangshan. The order of TWSI of the fine particles in the region was Baoding-Tianjin-Beijing-Tangshan. The annual mean concentrations of TWSI in the coarse mode were 41.36±15.76,48.04±15.79,39.40±11.03,40.49±13.32μg m-3in Beijing, Tianjin, Tangshan and Baoding, respectively. The annual mean concentrations of TWSI in the fine mode were 66.54±47.95,69.12±34.85, 61.80±44.63,71.73±45.12μg m-3in Beijing, Tianjin, Tangshan and Baoding, respectively. All the annual mean concentrations of TWSIin the fine mode in the four sites had exceeded averaged concentration of PM2.5in the environmental quality standards (35μg m-3), which indicated that the pollution of TWSI was serious. Secondary water-soluble ions (SWSI)(SO42-, NO3-and NH4+) and Cl-were the main components, and were mainly found in the fine particles in the four sites of Beijing-Tianjin-Hebei Region. In the coarse particles, NO3-Ca2+ and SO42-were the dominant contributions to WSI. Almost all water-soluble ions in fine particles are similar

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

    NASA Technical Reports Server (NTRS)

    Schmid, B.; Redemann, J.; Livingston, J.; Russell, P.; Hegg, D.; Wang, J.; Kahn, R.; Hsu, C.; Masonis, S.; Murayama, T.; Hipskind, R. Stephen (Technical Monitor)

    2002-01-01

    In the Spring 2001 phase of the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia), the 6-channel NASA Ames Airborne Tracking Sunphotometer (AATS-6) operated on 15 of the 19 research flights of the NCAR C-130, while its 14-channel counterpart (AATS-14) flew successfully on all 19 research flights of the CIRPAS Twin Otter. ACE-Asia studied aerosol outflow from the Asian continent to the Pacific basin. It was designed to integrate suborbital and satellite measurements and models to reduce the uncertainty in calculations of the climate forcing due to aerosols. AATS-6 and AATS-14 measured solar beam transmission at six and 14 wavelengths (380-1021 and 354-1558 nm, respectively), yielding aerosol optical depth (AOD) spectra and columnar water vapor (CWV). Vertical differentiation in profiles yielded aerosol extinction spectra and water vapor concentration. In this paper, we plan to present examples of the following, preliminary findings that are based in part on our airborne sunphotometer measurements: (1) The wavelength dependence of sunphotometer-derived AOD and extinction indicates that supermicron dust was often a major component of the aerosol, frequently extending to high altitudes. The percentage of full-column AOD (525 nm) that Jay above 3 km was typically 34+/-13%. In contrast, the analogous percentage of columnar water vapor was only 10+/-4%; (2) Initial comparison studies between AOD data obtained by AATS-6 and AATS-14 during coordinated low-level flight legs show agreement well within the instruments' error bars; (3) Aerosol extinction has been derived from airborne in situ measurements of scattering (nephelometers) and absorption (particle soot/ absorption photometer, PSAP) or calculated from particle size distribution measurements (mobility analyzers and aerodynamic particle sizers). Comparison with corresponding extinction values derived from the Ames airborne sunphotometer measurements shows good agreement for the vertical distribution

  7. Volume and surface area size distribution, water mass and model fitting of GCE/CASE/WATOX marine aerosols

    NASA Astrophysics Data System (ADS)

    Kim, Y.; Sievering, H.; Boatman, J.

    1990-06-01

    As a part of the Global Change Expedition/Coordinated Air-Sea Experiment/Western Atlantic Ocean Experiment (GCE/CASE/WATOX), size distributions of marine aerosols were measured at two altitudes of about 2750 and 150 m above sea level (asl) over the size range 0.1 ˜ 32 μm. Lognormal fitting was applied to the corrected aerosol size spectra to determine the volume and surface area size distributions of the CASE-WATOX marine aerosols. Each aerosol size distribution was fitted with three lognormal distributions representing fine-, large-, and giant-particle modes. Water volume fraction and dry particle size of each aerosol size distribution were also calculated using empirical formulas for particle size as a function of relative humidity and particle type. Because of the increased influence from anthropogenic sources in the continental United States, higher aerosol volume concentrations were observed in the fine-particle mode near-shore off the east coast; 2.11 and 3.63 μm3 cm-3 for free troposphere (FT) and marine boundary layer (MBL), compared with the open-sea Bermuda area values; 0.13 and 0.74 μm3 cm-3 for FT and MBL. The large-particle mode exhibits the least variations in volume distributions between the east coast and open-sea Bermuda area, having a volume geometric median diameter (VGMD) between 1.4 and 1.6 μm and a geometric standard deviation between 1.57 and 1.68. For the giant-particle mode, larger VGMD and volume concentrations were observed for marine aerosols nearshore off the east coast than in the open-sea Bermuda area because of higher relative humidity and higher surface wind speed conditions. Wet VGMD and aerosol water volume concentrations at 15 m asl ship level were determined by extrapolating from those obtained by analysis of the CASE-WATOX aircraft aerosol data. Abundance of aerosol water in the MBL serves as an important pathway for heterogeneous conversion of SO2 in sea salt aerosol particles.

  8. 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.

  9. Determination of the sources and impacts of aerosols on clouds and orographic precipitation during CalWater

    NASA Astrophysics Data System (ADS)

    Prather, K. A.; Suski, K.; Cazorla, A.; Cahill, J. F.; Creamean, J.; Collins, D. B.; Ralph, F. M.; Cayan, D. R.; Rosenfeld, D.; DeMott, P. J.; Sullivan, R. C.; Comstock, J. M.; Leung, L.; Tomlinson, J. M.; Roberts, G. C.; Nenes, A.; Lin, J. J.

    2011-12-01

    Climate projections for the remainder of this century for the U.S. Southwest, including parts of California, suggest a drying trend (reductions ~ 10 -15 %). Thus, understanding factors which could potentially influence the amount and type of precipitation is critical to future water resources in California. Previous studies suggest aerosols transported from the Central Valley into the mountains may be reducing the amount of orographic precipitation in the Sierra Nevada mountain range, the key region for water storage in the snowpack. CalWater, which commenced in the Winter of 2009, is an ongoing multi-year, multi-agency field campaign to investigate the primary sources of aerosols influencing clouds and precipitation in this region. Single particle measurements, used in both ground as well as PNNL G1 aircraft measurements, in the recent campaign provide insight into the sources of aerosols impacting the clouds and precipitation. Biomass burning, Central Valley pollution, long range transported Asian dust and pollution, locally generated newly formed particles, and marine aerosols all show strong impacts on the cloud microphysical properties. This presentation will provide a brief overview of the objective and key findings from CalWater measurements of aerosols, precipitation, clouds, and meteorology conducted from 2009-2011 in this region.

  10. Economics of liquid hydrogen from water electrolysis

    NASA Technical Reports Server (NTRS)

    Lin, F. N.; Moore, W. I.; Walker, S. W.

    1985-01-01

    An economical model for preliminary analysis of LH2 cost from water electrolysis is presented. The model is based on data from vendors and open literature, and is suitable for computer analysis of different scenarios for 'directional' purposes. Cost data associated with a production rate of 10,886 kg/day are presented. With minimum modification, the model can also be used to predict LH2 cost from any electrolyzer once the electrolyzer's cost data are available.

  11. Strong enhancement in light absorption by black carbon due to aerosol water uptake

    NASA Astrophysics Data System (ADS)

    Fierce, Laura; Mena, Francisco; Riemer, Nicole; Bond, Tami C.; Bauer, Susanne E.

    2015-04-01

    Black carbon exerts a strong, yet highly uncertain, warming effect on the climate. One source of uncertainty in predicting black carbon's radiative effects is the absorption per black carbon mass. Although models suggest that light absorption is strongly enhanced if black carbon is coated with non-absorbing aerosol material, recent ambient observations find only weak absorption enhancement from aerosol coatings. In this study, we use a particle-resolved aerosol model to evaluate how oversimplified representations of particle composition impact modeled light absorption by black carbon. We show that oversimplifying the representation of particle composition leads to overestimation of modeled absorption enhancement. In order to improve global model representations of BC absorption, we performed a nonparametric regression on particle-reolved model data from a series of simulations. Through this nonparametric analysis we derived a relationship for absorption enhancement as a function of variables that global models already track, the population-averaged composition and the environmental relative humidity. Finally, we show how this nonparametric relationship can be exploited for use in global models to improve predictions of absorption by black carbon. In order to quantify the global-scale impact of water uptake on light absorption by black carbon, we applied the relationship for absorption enhancement to output of the climate model GISS-MATRIX. We find weak absorption enhancement in locations with low relative humidity, but light absorption is strongly enhanced in humid regions. This enhancement in light absorption by particles taking up water strongly impacts black carbon's radiative effects at the global scale, enhancing light absorption by black carbon by 20% relative to dry conditions.

  12. Water soluble ions in aerosols (TSP) : Characteristics, sources and seasonal variation over the central Himalayas, Nepal

    NASA Astrophysics Data System (ADS)

    Tripathee, Lekhendra; Kang, Shichang; Zhang, Qianggong; Rupakheti, Dipesh

    2016-04-01

    Atmspheric pollutants transported from South Asia could have adverse impact on the Himalayan ecosystems. Investigation of aerosol chemistry in the Himalayan region in Nepal has been limited on a temporal and spatial scale to date. Therefore, the water-soluble ionic composition of aerosol using TSP sampler was investigated for a year period from April 2013 to March 2014 at four sites Bode, Dhunche, Lumbini and Jomsom characterized as an urban, rural, semi-urban and remote sites in Nepal. During the study period, the highest concentration of major cation was Ca2+ with an average concentration of 8.91, 2.17, 7.85 and 6.42 μg m-3 and the highest concentration of major anion was SO42- with an average of 10.96, 4.06, 6.85 and 3.30 μg m-3 at Bode, Dhunche, Lumbini and Jomsom respectively. The soluble ions showed the decrease in concentrations from urban to the rural site. Correlations and PCA analysis suggested that that SO42-, NO3- and NH4+ were derived from the anthropogenic sources where as the Ca2+ and Mg2+ were from crustal sources. Our results also suggest that the largest acid neutralizing agent at our sampling sites in the central Himalayas are Ca2+ followed by NH4+. Seasonal variations of soluble ions in aerosols showed higher concentrations during pre-monsoon and winter (dry-periods) due to limited precipitation amount and lower concentrations during the monsoon which can be explained by the dilution effect, higher the precipitation lower the concentration. K+ which is regarded as the tracer of biomss burning had a significant peaks during pre-monsoon season when the forest fires are active around the regions. In general, the results of this study suggests that the atmospheric chemistry is influenced by natural and anthropogenic sources. Thus, soluble ionic concentrations in aerosols from central Himalayas, Nepal can provide a useful database to assess atmospheric environment and its impacts on human health and ecosystem in the southern side of central

  13. Liquid-liquid interfaces of semifluorinated alkane diblock copolymers with water, alkanes, and perfluorinated alkanes.

    SciTech Connect

    Perahia, Dvora, Dr.; Pierce, Flint; Tsige, Mesfin; Grest, Gary Stephen, Dr.

    2008-08-01

    The liquid-liquid interface between semifluorinated alkane diblock copolymers of the form F3C(CF2)n-1-(CH2)m-1CH3 and water, protonated alkanes, and perfluorinated alkanes are studied by fully atomistic molecular dynamics simulations. A modified version of the OPLS-AA (Optimized Parameter for Liquid Simulation All-Atom) force field of Jorgensen et al. has been used to study the interfacial behavior of semifluorinated diblocks. Aqueous interfaces are found to be sharp, with correspondingly large values of the interfacial tension. Due to the reduced hydrophobicity of the protonated block compared to the fluorinated block, hydrogen enhancement is observed at the interface. Water dipoles in the interfacial region are found to be oriented nearly parallel to the liquid-liquid interface. A number of protonated alkanes and perfluorinated alkanes are found to be mutually miscible with the semifluorinated diblocks. For these liquids, interdiffusion follows the expected Fickian behavior, and concentration-dependent diffusivities are determined.

  14. Liquid-liquid interfaces of semifluorinated alkane diblock copolymers with water, alkanes, and perfluorinated alkanes.

    PubMed

    Pierce, Flint; Tsige, Mesfin; Perahia, Dvora; Grest, Gary S

    2008-12-18

    The liquid-liquid interface between semifluorinated alkane diblock copolymers of the form F3C(CF2)n-1-(CH2)m-1CH3 and water, protonated alkanes, and perfluorinated alkanes are studied by fully atomistic molecular dynamics simulations. A modified version of the OPLS-AA (Optimized Parameter for Liquid Simulation All-Atom) force field of Jorgensen et al. has been used to study the interfacial behavior of semifluorinated diblocks. Aqueous interfaces are found to be sharp, with correspondingly large values of the interfacial tension. Due to the reduced hydrophobicity of the protonated block compared to the fluorinated block, hydrogen enhancement is observed at the interface. Water dipoles in the interfacial region are found to be oriented nearly parallel to the liquid-liquid interface. A number of protonated alkanes and perfluorinated alkanes are found to be mutually miscible with the semifluorinated diblocks. For these liquids, interdiffusion follows the expected Fickian behavior, and concentration-dependent diffusivities are determined.

  15. Limiting shear stress and monotonic properties of liquid water

    NASA Astrophysics Data System (ADS)

    Gorshkov, A. I.

    2016-12-01

    Publications in scientific journals in which the authors attempt to experimentally prove that water, the most widespread substance on the Earth, is not a completely classical liquid, have become more frequent recently. This means, first, that water behaves as a solid at very low shear stress, i.e., does not flow, and, second, that the temperature dependences of its different properties are non-monotonic, i.e., possess singularities. We are aware of several such publications [1-5].

  16. Molecular dynamics simulation of liquid water: Hybrid density functionals

    SciTech Connect

    Todorova, T; Seitsonen, A; Hutter, J; Kuo, W; Mundy, C

    2005-09-12

    The structure, dynamical and electronic properties of liquid water utilizing different hybrid density functionals were tested within the plane wave framework of first principles molecular dynamics simulations. The computational approach, which employs modified functionals with short-ranged Hartree-Fock exchange, was first tested in calculations of the structural and bonding properties of the water dimer and cyclic water trimer. Liquid water simulations were performed at the state point of 350 K at the experimental density. Simulations included three different hybrid functionals, a meta functional, four gradient corrected functionals, the local density and Hartree-Fock approximation. It is found that hybrid functionals are superior in reproducing the experimental structure and dynamical properties as measured by the radial distribution function and self diffusion constant when compared to the pure density functionals. The local density and Hartree-Fock approximations show strongly over- and under-structured liquids, respectively. Hydrogen bond analysis shows that the hybrid functionals give slightly smaller averaged numbers of hydrogen bonds and similar hydrogen bond populations as pure density functionals. The average molecular dipole moments in the liquid from the three hybrid functionals are lower than from the corresponding pure density functionals.

  17. Molecular dynamics of the water liquid-vapor interface

    NASA Technical Reports Server (NTRS)

    Wilson, M. A.; Pohorille, A.; Pratt, L. R.; MacElroy, R. D. (Principal Investigator)

    1987-01-01

    The results of molecular dynamics calculations on the equilibrium interface between liquid water and its vapor at 325 K are presented. For the TIP4P model of water intermolecular pair potentials, the average surface dipole density points from the vapor to the liquid. The most common orientations of water molecules have the C2 nu molecular axis roughly parallel to the interface. The distributions are quite broad and therefore compatible with the intermolecular correlations characteristic of bulk liquid water. All near-neighbor pairs in the outermost interfacial layers are hydrogen bonded according to the common definition adopted here. The orientational preferences of water molecules near a free surface differ from those near rigidly planar walls which can be interpreted in terms of patterns found in hexagonal ice 1. The mean electric field in the interfacial region is parallel to the mean polarization which indicates that attention cannot be limited to dipolar charge distributions in macroscopic descriptions of the electrical properties of this interface. The value of the surface tension obtained is 132 +/- 46 dyn/cm, significantly different from the value for experimental water of 68 dyn/cm at 325 K.

  18. Organic aerosols associated with the generation of reactive oxygen species (ROS) by water-soluble PM2.5.

    PubMed

    Verma, Vishal; Fang, Ting; Xu, Lu; Peltier, Richard E; Russell, Armistead G; Ng, Nga Lee; Weber, Rodney J

    2015-04-07

    We compare the relative toxicity of various organic aerosol (OA) components identified by an aerosol mass spectrometer (AMS) based on their ability to generate reactive oxygen species (ROS). Ambient fine aerosols were collected from urban (three in Atlanta, GA and one in Birmingham, AL) and rural (Yorkville, GA and Centerville, AL) sites in the Southeastern United States. The ROS generating capability of the water-soluble fraction of the particles was measured by the dithiothreitol (DTT) assay. Water-soluble PM extracts were further separated into the hydrophobic and hydrophilic fractions using a C-18 column, and both fractions were analyzed for DTT activity and water-soluble metals. Organic aerosol composition was measured at selected sites using a high-resolution time-of-flight AMS. Positive matrix factorization of the AMS spectra resolved the organic aerosol into isoprene-derived OA (Isop_OA), hydrocarbon-like OA (HOA), less-oxidized oxygenated OA, (LO-OOA), more-oxidized OOA (MO-OOA), cooking OA (COA), and biomass burning OA (BBOA). The association of the DTT activity of water-soluble PM2.5 (WS_DTT) with these factors was investigated by linear regression techniques. BBOA and MO-OOA were most consistently linked with WS_DTT, with intrinsic water-soluble activities of 151 ± 20 and 36 ± 22 pmol/min/μg, respectively. Although less toxic, MO-OOA was most widespread, contributing to WS_DTT activity at all sites and during all seasons. WS_DTT activity was least associated with biogenic secondary organic aerosol. The OA components contributing to WS_DTT were humic-like substances (HULIS), which are abundantly emitted in biomass burning (BBOA) and include highly oxidized OA from multiple sources (MO-OOA). Overall, OA contributed approximately 60% to the WS_DTT activity, with the remaining probably from water-soluble metals, which were mostly associated with the hydrophilic WS_DTT fraction.

  19. Uncertainties in the measurements of water-soluble organic nitrogen in the aerosol

    NASA Astrophysics Data System (ADS)

    Matsumoto, Kiyoshi; Yamato, Koki

    2016-11-01

    In order to evaluate the positive and negative artifacts in the measurements of the water-soluble organic nitrogen (WSON) in the aerosols by filter sampling, comparative experiments between the filter sampling and denuder-filter sampling were conducted during both the warm and cold seasons. The results suggest that the traditional filter sampling underestimates the concentrations of the particulate WSON due to its volatilization loss, but this effect on the ratio of the WSON to the water-soluble total nitrogen (WSTN) was small probably because inorganic nitrogen species were also lost during the filter sampling. Approximately 32.5% of the WSON in the PM2.5 was estimated to be lost during the filter sampling. The denuder-filter sampling also demonstrated the existence of the WSON in the gas phase with approximately quarter concentrations of the WSON in the PM2.5. On the other hand, the filter sampling would overestimate the gaseous WSON concentration due to the loss of the WSON from the aerosol collection filter.

  20. Secondary organic aerosol formation from aqueous chemistry of glyoxal, methylglyoxal, and glycolaldehyde in atmospheric waters: Chemical insights and kinetic model studies

    NASA Astrophysics Data System (ADS)

    Lim, Y. B.; Tan, Y.; Altieri, K. E.; Perri, M. J.; Carlton, A. G.; Seitzinger, S.; Turpin, B. J.

    2010-12-01

    Aqueous chemistry in clouds, fog and aerosol water is now considered an important source of secondary organic aerosol (SOA). Modeling studies confirm that the underlying chemistry is kinetically favorable. Laboratory studies have begun to validate and refine the aqueous chemical mechanisms. Field observations, such as the atmospheric abundance of oxalate, ubiquitous presence of high molecular weight or humic-like substances (HULIS), high ambient O/C ratios, and correlations between SOA and aerosol liquid water content provide atmospheric evidence for SOA formation through aqueous chemistry. In the aqueous phase, small and volatile (C2-C3) but water soluble organic compounds undergo radical (photooxidation) and non-radical (acid/base catalysis) reactions, or reactions with inorganic constituents (sulfate, nitrate or ammonia) to form low volatility products including organic acids, organic-inorganic complexes and oligomers. These products are expected to remain at least in part in the particle phase after water evaporation, forming SOA. While not traditionally considered to be SOA precursors, atmospherically abundant and water soluble organic compounds like glyoxal (C2), methylglyoxal (C3) and glycolaldehyde (C2) have great potential to form SOA via aqueous chemistry. This paper presents a unified reaction mechanism and full kinetic model for the aqueous-phase reaction of glyoxal, methylglyoxal, glycolaldehyde, pyruvic acid and acetic acid with OH radical and validates this mechanism, in part, with laboratory experiments. At cloud relevant concentrations (~1E-6 M), the major product is oxalic acid and formation is well predicted by the previous cloud model (Lim et al., 2005). As concentrations increase radical-radical reactions become increasingly important and yield higher molecular weight products. The full kinetic model suggests that SOA formed in aerosol water (where organic concentrations are > 1 M) is comprised of high molecular weight multifunctional compounds

  1. Solid/liquid phase diagram of the ammonium sulfate/glutaric acid/water system.

    PubMed

    Beyer, Keith D; Pearson, Christian S; Henningfield, Drew S

    2013-05-02

    We have studied the low temperature phase diagram and water activities of the ammonium sulfate/glutaric acid/water system using differential scanning calorimetry, infrared spectroscopy of thin films, and a new technique: differential scanning calorimetry-video microscopy. Using these techniques, we have determined that there is a temperature-dependent kinetic effect to the dissolution of glutaric acid in aqueous solution. We have mapped the solid/liquid ternary phase diagram, determined the water activities based on the freezing point depression, and determined the ice/glutaric acid phase boundary as well as the ternary eutectic composition and temperature. We have also modified our glutaric acid/water binary phase diagram previously published based on these new results. We compare our results for the ternary system to the predictions of the Extended AIM Aerosol Thermodynamics Model (E-AIM), and find good agreement for the ice melting points in the ice primary phase field of this system; however, significant differences were found with respect to phase boundaries, concentration and temperature of the ternary eutectic, and glutaric acid dissolution.

  2. 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

  3. Water uptake is independent of the inferred composition of secondary aerosols derived from multiple biogenic VOCs

    NASA Astrophysics Data System (ADS)

    Alfarra, M. R.; Good, N.; Wyche, K. P.; Hamilton, J. F.; Monks, P. S.; Lewis, A. C.; McFiggans, G.

    2013-12-01

    We demonstrate that the water uptake properties derived from sub- and super-saturated measurements of chamber-generated biogenic secondary organic aerosol (SOA) particles are independent of their degree of oxidation, determined using both online and offline methods. SOA particles are formed from the photooxidation of five structurally different biogenic VOCs, representing a broad range of emitted species and their corresponding range of chemical reactivity: α-pinene, β-caryophyllene, limonene, myrcene and linalool. The fractional contribution of mass fragment 44 to the total organic signal (f44) is used to characterise the extent of oxidation of the formed SOA as measured online by an aerosol mass spectrometer. Results illustrate that the values of f44 are dependent on the precursor, the extent of photochemical ageing as well as on the initial experimental conditions. SOA generated from a single biogenic precursor should therefore not be used as a general proxy for biogenic SOA. Similarly, the generated SOA particles exhibit a range of hygroscopic properties, depending on the precursor, its initial mixing ratio and photochemical ageing. The activation behaviour of the formed SOA particles show no temporal trends with photochemical ageing. The average κ values derived from the HTDMA and CCNc are generally found to cover the same range for each precursor under two different initial mixing ratio conditions. A positive correlation is observed between the hygroscopicity of particles of a single size and f44 for α-pinene, β-caryophyllene, linalool and myrcene, but not for limonene SOA. The investigation of the generality of this relationship reveals that α-pinene, limonene, linalool and myrcene are all able to generate particles with similar hygroscopicity (κHTDMA ~0.1) despite f44 exhibiting a relatively wide range of values (~4 to 11%). Similarly, κCCN is found to be independent of f44. The same findings are also true when sub- and super-saturated water uptake

  4. Water uptake is independent of the inferred composition of secondary aerosols derived from multiple biogenic VOCs

    NASA Astrophysics Data System (ADS)

    Alfarra, M. R.; Good, N.; Wyche, K. P.; Hamilton, J. F.; Monks, P. S.; Lewis, A. C.; McFiggans, G. B.

    2013-04-01

    We demonstrate that the water uptake properties derived from sub- and super-saturated measurements of chamber-generated biogenic secondary organic aerosol (SOA) particles are independent of their degree of oxidation determined using both online and offline methods. SOA particles are formed from the photooxidation of five structurally different biogenic VOCs representing a broad range of emitted species and their corresponding range of chemical reactivity: α-pinene, β-caryophyllene, limonene, myrcene and linalool. The fractional contribution of mass fragment 44 to the total organic signal (f44) is used to characterise the extent of oxidation of the formed SOA as measured online by an aerosol mass spectrometer. Results illustrate that the values of f44 are dependent on the precursor, the extent of photochemical ageing as well as on the initial experimental conditions. SOA generated from a single biogenic precursor should therefore not be used as a general proxy for biogenic SOA. Similarly, the generated SOA particles exhibit a range of hygroscopic properties depending on the precursor, its initial mixing ratio and photochemical ageing. The activation behaviour of the formed SOA particles show no temporal trends with photochemical ageing. The average κ values derived from the HTDMA and CCNc are generally found to cover the same range for each precursor under two different initial mixing ratio conditions. A positive correlation is observed between the hygroscopicity of particles of a single size and f44 for α-pinene, β-caryophyllene, linalool and myrcene, but not for limonene SOA. The investigation of the generality of this relationship reveal that α-pinene, limonene, linalool and myrcene are all able to generate particles with similar hygroscopicity (κHTDMA ~0.1) despite f44 exhibiting a relatively wide range of values (~4 to 11%). Similarly, κCCN is found to be independent of f44. The same findings are also true when sub- and super-saturated water uptake

  5. Computer simulation of liquid/liquid interfaces. I. Theory and application to octane/water

    NASA Astrophysics Data System (ADS)

    Zhang, Yuhong; Feller, Scott E.; Brooks, Bernard R.; Pastor, Richard W.

    1995-12-01

    Statistical ensembles for simulating liquid interfaces at constant pressure and/or surface tension are examined, and equations of motion for molecular dynamics are obtained by various extensions of the Andersen extended system approach. Valid ensembles include: constant normal pressure and surface area; constant tangential pressure and length normal to the interface; constant volume and surface tension; and constant normal pressure and surface tension. Simulations at 293 K and 1 atm normal pressure show consistent results with each other and with a simulation carried out at constant volume and energy. Calculated surface tensions for octane/water (61.5 dyn/cm), octane/vacuum (20.4 dyn/cm) and water/vacuum (70.2 dyn/cm) are in very good agreement with experiment (51.6, 21.7, and 72.8 dyn/cm, respectively). The practical consequences of simulating with two other approaches commonly used for isotropic systems are demonstrated on octane/water: applying equal normal and tangential pressures leads to an instability; and applying a constant isotropic pressure of 1 atm leads to a large positive normal pressure. Both results are expected for a system of nonzero surface tension. Mass density and water polarization profiles in the liquid/liquid and liquid/vapor interfaces are also compared.

  6. Boson peak, Ioffe-Regel Crossover, and Liquid-Liquid phase transition in Supercooled Water

    NASA Astrophysics Data System (ADS)

    Kumar, Pradeep

    We have investigated the onset of Boson peak in a model of liquid water which exhibits a clear first-order phase transition between a low-density liquid phase and a high-density liquid phase of water at low temperature and high pressure. We find that the at low pressures, the onset of Boson peak coincides with the Widom-line of the system. At high pressures, the onset occurs at the transition temperature between the two liquids. Furthermore, we show that at both low and high pressure, the frequency of the Boson peak coincides with the Ioffe-Regel crossover of the transverse phonons, suggesting that the breakdown of Debye behavior is a general feature of Ioffe-Regel limit crossover in supercooled water. The frequency of the Boson peak is weakly pressure dependent and decreases with increasing pressure. Our work bridges gap between the experimental results on the Boson peak nanoconfined water and the behavior that one would expect from a bulk system.

  7. Switchable water: microfluidic investigation of liquid-liquid phase separation mediated by carbon dioxide.

    PubMed

    Lestari, Gabriella; Abolhasani, Milad; Bennett, Darla; Chase, Preston; Günther, Axel; Kumacheva, Eugenia

    2014-08-27

    Increase in the ionic strength of water that is mediated by the reaction of carbon dioxide (CO2) with nitrogenous bases is a promising approach toward phase separation in mixtures of water with organic solvents and potentially water purification. Conventional macroscale studies of this complicated process are challenging, due to its occurrence via several consecutive and concurrent steps, mass transfer limitation, and lack of control over gas-liquid interfaces. We report a new microfluidic strategy for fundamental studies of liquid-liquid phase separation mediated by CO2 as well as screening of the efficiency of nitrogenous agents. A single set of microfluidic experiments provided qualitative and quantitative information on the kinetics and completeness of water-tetrahydrofuran phase separation, the minimum amount of CO2 required to complete phase separation, the total CO2 uptake, and the rate of CO2 consumption by the liquid mixture. The efficiency of tertiary diamines with different lengths of alkyl chain was examined in a time- and labor-efficient manner and characterized with the proposed efficiency parameter. A wealth of information obtained using the MF methodology can facilitate the development of new additives for switchable solvents in green chemistry applications.

  8. Ionic liquid-based dispersive liquid-liquid microextraction for sensitive determination of aromatic amines in environmental water.

    PubMed

    Han, Dandan; Yan, Hongyuan; Row, Kyung H

    2011-05-01

    Ionic liquid-based dispersive liquid-liquid microextraction was developed for the extraction and preconcentration of aromatic amine from environmental water. A suitable mixture of extraction solvent (100 μL, 1-butyl-3-methylimidazolium hexafluorophoshate) and dispersive solvent (750 μL, methanol) were injected into the aqueous samples (10.00 mL), forming a cloudy solution. After centrifuging, enriched analytes in the sediment phase were determined by HPLC-UV. The effect of various factors, such as the extraction and dispersive solvent, sample pH, extraction time and salt effect were investigated. Under optimum conditions, enrichment factors for 2-anilinoethanol, o-chloroaniline and 4-bromo-N,N-dimethylaniline were above 50 and the limits of detection (LODs) were 0.023, 0.015 and 0.026 ng/mL, respectively. Their linear ranges were 0.8-400 ng/mL for 2-anilinoethanol, 0.5-200 ng/mL for o-chloroaniline and 0.4-200 ng/mL for 4-bromo-N,N-dimethylaniline, respectively. Relative standard deviations (RSDs) were below 5.0%. The relative recoveries from samples of environmental water were in the range of 82.0-94.0%. Compared with other methods, dispersive liquid-liquid microextraction is simple, rapid, sensitive and economical.

  9. Liquid Water, the ``Most Complex'' Liquid: New Results in Bulk, Nanoconfined, and Biological Environments

    NASA Astrophysics Data System (ADS)

    Stanley, H. Eugene

    2010-03-01

    We will introduce some of the 63 anomalies of the most complex of liquids, water. We will demonstrate some recent progress in understanding these anomalies by combining information provided by recent experiments and simulations on water in bulk, nanoconfined, and biological environments. We will interpret evidence from recent experiments designed to test the hypothesis that liquid water may display ``polymorphism'' in that it can exist in two different phases---and discuss recent work on water's transport anomalies [1] as well as the unusual behavior of water in biological environments [2]. Finally, we will discuss how the general concept of liquid polymorphism [3] is proving useful in understanding anomalies in other liquids, such as silicon, silica, and carbon, as well as metallic glasses, which have in common that they are characterized by two characteristic length scales in their interactions. This work was supported by NSF Chemistry Division, and carried out in collaboration with a number of colleagues, chief among whom are C. A. Angell, M. C. Barbosa, M. C. Bellissent, L. Bosio, F. Bruni, S. V. Buldyrev, M. Canpolat, S. -H. Chen, P. G. Debenedetti, U. Essmann,G. Franzese, A. Geiger, N. Giovambattista, S. Han, P. Kumar, E. La Nave,G. Malescio, F. Mallamace, M. G. Mazza, O. Mishima, P. Netz, P. H. Poole, P. J. Rossky, R. Sadr,S. Sastry, A. Scala, F. Sciortino, A. Skibinsky, F. W. Starr, K. C. Stokely J. Teixeira, L. Xu, and Z. Yan.[4pt] [1] L. Xu, F. Mallamace, Z. Yan, F. W. Starr, S. V. Buldyrev, and H. E. Stanley, ``Appearance of a Fractional Stokes-Einstein Relation in Water and a Structural Interpretation of Its Onset,'' Nature Physics 5, 565--569 (2009). [0pt] [2] P. Kumar, Z. Yan, L. Xu, M. G. Mazza, S. V. Buldyrev, S. -H. Chen. S. Sastry, and H. E. Stanley, ``Glass Transition in Biomolecules and the Liquid-Liquid Critical Point of Water,'' Phys. Rev. Lett. 97, 177802 (2006). [0pt] [3] H. E. Stanley, ed. , Liquid Polymorphism [Advances in Chemical Physics

  10. Mobile Multiwavelength Polarization Raman Lidar for Water Vapor, Cloud and Aerosol Measurement

    NASA Astrophysics Data System (ADS)

    Wu, Songhua; Song, Xiaoquan; Liu, Bingyi; Dai, Guangyao; Zhang, Kailin; Qin, Shengguang; Gao, Fei; Hua, Dengxin

    2016-06-01

    Aiming at the detection of water vapor mixing ratio, particle linear depolarization ratio, extinction coefficient and cloud information, the Water vapor, Cloud and Aerosol Lidar (WVCAL) was developed by the lidar group at Ocean University of China. The Lidar consists of transmitting subsystem, receiving subsystem, data acquisition and controlling subsystem and auxiliary subsystem. These parts were presented and described in this paper. For the measurement of various physical properties, three channels including Raman channel, polarization channel and infrared channel are integrated in this Lidar system. In this paper, the integration and working principle of these channels is introduced in details. Finally, a measurement example which was operated in coastal area-Qingdao, Shandong province, during 2014 is provided.

  11. Comparison of Stratospheric Aerosol and Gas Experiment II and balloon-borne stratospheric water vapor measurements

    NASA Technical Reports Server (NTRS)

    Pruvost, P.; Ovarlez, J.; Lenoble, J.; Chu, W. P.

    1993-01-01

    The Stratospheric Aerosol and Gas Experiment II has one channel at 940 nm related to water vapor. Two inversion procedures were developed independently in order to obtain the water vapor profile: the Chahine method by the Langley Research Center, and the Mill method by the Laboratoire d'Optique Atmospherique. Comparisons were made between these two algorithms and some results are presented at midlatitudes (about 45 deg N) and tropical latitudes (12-25 deg S). They are compared with in situ frost point hygrometer data provided by balloon experiments from the Laboratoire de Meteorologie Dynamique. At +/- 0.5 ppmv, agreement between the inversion results and the experimental results was obtained in the altitude range from 18-19 to 26-27 km. Below 18-19 km and above 26-27 km the error is larger (sometimes 1 ppmv and more).

  12. Complete wetting of Pt(111) by nanoscale liquid water films

    SciTech Connect

    Xu, Yuntao; Dibble, Collin J.; Petrik, Nikolay G.; Smith, R. Scott; Kay, Bruce D.; Kimmel, Gregory A.

    2016-02-04

    The melting and wetting of nanoscale crystalline ice films on Pt(111) that are transiently heated above the melting point using nanosecond laser pulses are studied with infrared refection absorption spectroscopy (IRAS) and Kr temperature programmed desorption (TPD). The as-grown crystalline ice films consist of isolated nanoscale ice crystallites embedded in a hydrophobic water monolayer. Upon heating above the melting point, these ice crystallites rapidly melt to form nanoscale droplets of liquid water. Rapid cooling of the system to cryogenic temperatures after each laser pulse quenches the water films and allows them to be interrogated with IRAS, Kr TPD and other ultrahigh vacuum surface science techniques. With each successive heat pulse, these liquid drops spread across the surface until it is entirely covered with multilayer water films after several pulses. These results, which show that nanoscale water films completely wet Pt(111), are in contrast to molecular dynamics simulations predicting partial wetting of nanoscale water drops on a hydrophobic water monolayer. The results provide valuable new insights into the wetting characteristics of nanoscale water films on a clean, well-characterized single crystal surface.

  13. Three-dimensional picture of dynamical structure in liquid water

    NASA Astrophysics Data System (ADS)

    Svishchev, Igor M.; Zassetsky, Alexander Yu.

    2000-01-01

    This paper presents a methodology with which to study the local density distributions in molecular liquids and their fluctuations in any spatial direction. The distinct part of the van Hove density-density correlation function for liquid water is calculated in molecular dynamics simulations. Because of the pronounced nonspherical intermolecular interactions this pair-density function is direction dependent in the local molecular frame. We explicitly resolve the distinct van Hove function in the local frame of water molecules. The dynamics of the tetrahedrally coordinated (hydrogen bonded) and the interstitial molecules in liquid water are examined. The spectrum of the pair-density fluctuations for the tetrahedrally coordinated molecules in supercooled and ambient water exhibits a well-known translational mode at 200 cm-1 and a collective relaxation mode at lower frequencies, at approximately 10 cm-1 at 263 K. The correlation time of this relaxation process decreases with temperature, from 2.2 ps at 238 K to 1.4 ps at 298 K. The spectrum for the interstitial coordination also features a 10 cm-1 mode. It represents a secondary relaxation process in water different from a much slower Debye process. As temperature increases this relaxation mode tends to disappear from the pair-density fluctuations.

  14. A study of the indirect aerosol effect on subarctic marine liquid low-level clouds using MODIS cloud data and ground-based aerosol measurements

    NASA Astrophysics Data System (ADS)

    Sporre, Moa K.; Glantz, Paul; Tunved, Peter; Swietlicki, Erik; Kulmala, Markku; Lihavainen, Heikki

    2012-10-01

    Cloud microphysics is substantially affected by aerosol loading and the resulting changes in the reflective properties of the clouds can significantly affect the global radiation budget. A study of how marine low-level clouds over Barents Sea and the northern parts of the Norwegian Sea are affected by air mass origin has been performed by combining ground-based aerosol measurements with satellite cloud retrievals. Aerosol number size distributions have been obtained from measurement stations in northern Finland, and a trajectory model has been used to estimate the movement of the air masses. To identify anthropogenic influences on the clouds, the dataset has been divided according to aerosol loading. The clean air masses arrived to the investigation area from the north and the polluted air masses arrived from the south. Satellite derived microphysical and optical cloud parameters from the Moderate Resolution Imaging Spectrometer (MODIS) have then been analyzed for days when the trajectories coincided with marine low-level clouds over the investigated area. The cloud optical thickness (τ), cloud depth (H) and droplet number concentration (Nd) were significantly higher for the polluted days compared to the clean conditions, while the opposite was found for the cloud droplet effective radius (re). The H and Nd were derived from the satellite retrievals of τ and re. Furthermore, calculations of the aerosol cloud interaction relationship (ACI), relating Nd to boundary layer aerosol concentrations, resulted in a value of 0.17, which is in line with previous remote sensing studies. The results demonstrate that ground-based aerosol measurements can be combined with satellite cloud observations to study the indirect aerosol effect, and that the microphysics of marine sub-polar clouds can be considerably affected by continental aerosols.

  15. Comparison of Aerosol Optical Properties and Water Vapor Among Ground and Airborne Lidars and Sun Photometers During TARFOX

    NASA Technical Reports Server (NTRS)

    Ferrare, R.; Ismail, S.; Browell, E.; Brackett, V.; Clayton, M.; Kooi, S.; Melfi, S. H.; Whiteman, D.; Schwemmer, G.; Evans, K.; Russell, P.; Livingston, J.; Schmid, B.; Holben, B.; Remer, L.; Smirnov, A.; Hobbs, P. V.

    2000-01-01

    We compare aerosol optical thickness (AOT) and precipitable water vapor (PWV) measurements derived from ground and airborne lidars and Sun photometers during TARFOX (Tropospheric Aerosol Radiative Forcing Observational Experiment). Such comparisons are important to verify the consistency between various remote sensing measurements before employing them in any assessment of the impact of aerosols on the global radiation balance. Total scattering ratio and extinction profiles measured by the ground-based NASA/GSFC Scanning Raman Lidar (SRL) system, which operated from Wallops Island, Virginia (37.86 deg N, 75.51 deg W), are compared with those measured by the Lidar Atmospheric Sensing Experiment (LASE) airborne lidar system aboard the NASA ER-2 aircraft. Bias and rms differences indicate that these measurements generally agreed within about 10%. Aerosol extinction profiles and estimates of AOT are derived from both lidar measurements using a value for the aerosol extinction/backscattering ratio S(sub a)=60 sr for the aerosol extinction/backscattering ratio, which was determined from the Raman lidar measurements.

  16. Measurement of radiation damage of water-based liquid scintillator and liquid scintillator

    DOE PAGES

    Bignell, L. J.; Diwan, M. V.; Hans, S.; ...

    2015-10-19

    Liquid scintillating phantoms have been proposed as a means to perform real-time 3D dosimetry for proton therapy treatment plan verification. We have studied what effect radiation damage to the scintillator will have upon this application. We have performed measurements of the degradation of the light yield and optical attenuation length of liquid scintillator and water-based liquid scintillator after irradiation by 201 MeV proton beams that deposited doses of approximately 52 Gy, 300 Gy, and 800 Gy in the scintillator. Liquid scintillator and water-based liquid scintillator (composed of 5% scintillating phase) exhibit light yield reductions of 1.74 ± 0.55 % andmore » 1.31 ± 0.59 % after ≈ 800 Gy of proton dose, respectively. Some increased optical attenuation was observed in the irradiated samples, the measured reduction to the light yield is also due to damage to the scintillation light production. Based on our results and conservative estimates of the expected dose in a clinical context, a scintillating phantom used for proton therapy treatment plan verification would exhibit a systematic light yield reduction of approximately 0.1% after a year of operation.« less

  17. Measurement of radiation damage of water-based liquid scintillator and liquid scintillator

    SciTech Connect

    Bignell, L. J.; Diwan, M. V.; Hans, S.; Jaffe, D. E.; Rosero, R.; Vigdor, S.; Viren, B.; Worcester, E.; Yeh, M.; Zhang, C.

    2015-10-19

    Liquid scintillating phantoms have been proposed as a means to perform real-time 3D dosimetry for proton therapy treatment plan verification. We have studied what effect radiation damage to the scintillator will have upon this application. We have performed measurements of the degradation of the light yield and optical attenuation length of liquid scintillator and water-based liquid scintillator after irradiation by 201 MeV proton beams that deposited doses of approximately 52 Gy, 300 Gy, and 800 Gy in the scintillator. Liquid scintillator and water-based liquid scintillator (composed of 5% scintillating phase) exhibit light yield reductions of 1.74 ± 0.55 % and 1.31 ± 0.59 % after ≈ 800 Gy of proton dose, respectively. Some increased optical attenuation was observed in the irradiated samples, the measured reduction to the light yield is also due to damage to the scintillation light production. Based on our results and conservative estimates of the expected dose in a clinical context, a scintillating phantom used for proton therapy treatment plan verification would exhibit a systematic light yield reduction of approximately 0.1% after a year of operation.

  18. Phase transition behaviour of sodium oleate aerosol particles

    NASA Astrophysics Data System (ADS)

    Nájera, Juan J.

    Field measurements have shown that organic surfactants are significant components of atmospheric aerosols. While fatty acids, among other surfactants, are prevalent in the atmosphere, the influence of these species on the chemical and physical properties of atmospheric aerosols remains not fully characterized. In order to assess the phase in which particles may exist, a detailed study of the deliquescence of a model surfactant aerosol has been carried out. Sodium oleate was chosen as a surfactant proxy relevant in atmospheric aerosol. Sodium oleate micelle aerosol particles were generated nebulizing a sodium oleate aqueous solution. In this study, the water uptake and phase transition of sodium oleate aerosol particles have been studied in a room temperature aerosol flow tube system (AFT) using Fourier transform infrared (FTIR) spectroscopy. Aerosol morphology and elemental composition were also analysed using scanning electron microscopy/energy dispersive X-ray analysis (SEM/EDX) techniques. The particles are homogeneously distributed as ellipsoidal-shape aggregates of micelles particles with an average size of ˜1.1 μm. The deliquescence by the sodium oleate aerosol particles was monitored by infrared extinction spectroscopy, where the dried aerosol particles were exposed to increasing relative humidity as they passed through the AFT. Observations of the infrared absorption features of condensed phase liquid water enable to determine the sodium oleate deliquescence phase transition at 88±2%.

  19. Numerical studies on the separation performance of liquid- liquid Hydrocyclone for higher water-cut wells

    NASA Astrophysics Data System (ADS)

    Osei, H.; Al-Kayiem, H. H.; Hashim, F. M.

    2015-12-01

    Liquid-liquid hydrocyclones have nowadays become very useful in the oil industry because of their numerous applications. They can be installed downhole in the case of a well that produces higher water-oil ratios. The design of a liquid-liquid hydrocyclone for such a task is critical and every geometric part of the hydrocyclone has a part to play as far as separation is concerned. This work, through validated numerical technique, investigated the liquid-liquid hydrocyclone performance for the cases of single-inlet and dual-inlets, with different upper cylindrical lengths, specifically, 30mm and 60mm.It was observed that the hydrocyclones with the 30mm upper cylindrical section perform better than the ones with 60 mm upper cylindrical section. It was again noted that, even though higher number of tangential inlets increases the swirl intensity, they have the tendency to break up the oil droplets within the hydrocyclone because of increasing shear and jet flow interaction.

  20. Study of the ST2 model of water close to the liquid-liquid critical point.

    PubMed

    Sciortino, Francesco; Saika-Voivod, Ivan; Poole, Peter H

    2011-11-28

    We perform successive umbrella sampling grand canonical Monte Carlo computer simulations of the original ST2 model of water in the vicinity of the proposed liquid-liquid critical point, at temperatures above and below the critical temperature. Our results support the previous work of Y. Liu, A. Z. Panagiotopoulos and P. G. Debenedetti [J. Chem. Phys., 2009, 131, 104508], who provided evidence for the existence and location of the critical point for ST2 using the Ewald method to evaluate the long-range forces. Our results therefore demonstrate the robustness of the evidence for critical behavior with respect to the treatment of the electrostatic interactions. In addition, we verify that the liquid is equilibrated at all densities on the Monte Carlo time scale of our simulations, and also that there is no indication of crystal formation during our runs. These findings demonstrate that the processes of liquid-state relaxation and crystal nucleation are well separated in time. Therefore, the bimodal shape of the density of states, and hence the critical point itself, is a purely liquid-state phenomenon that is distinct from the crystal-liquid transition.

  1. Probing Hydrophilic Interface of Solid/Liquid-Water by Nanoultrasonics

    PubMed Central

    Mante, Pierre-Adrien; Chen, Chien-Cheng; Wen, Yu-Chieh; Chen, Hui-Yuan; Yang, Szu-Chi; Huang, Yu-Ru; -Ju Chen, I.; Chen, Yun-Wen; Gusev, Vitalyi; Chen, Miin-Jang; Kuo, Jer-Lai; Sheu, Jinn-Kong; Sun, Chi-Kuang

    2014-01-01

    Despite the numerous devoted studies, water at solid interfaces remains puzzling. An ongoing debate concerns the nature of interfacial water at a hydrophilic surface, whether it is more solid-like, ice-like, or liquid-like. To answer this question, a complete picture of the distribution of the water molecule structure and molecular interactions has to be obtained in a non-invasive way and on an ultrafast time scale. We developed a new experimental technique that extends the classical acoustic technique to the molecular level. Using nanoacoustic waves with a femtosecond pulsewidth and an ångström resolution to noninvasively diagnose the hydration structure distribution at ambient solid/water interface, we performed a complete mapping of the viscoelastic properties and of the density in the whole interfacial water region at hydrophilic surfaces. Our results suggest that water in the interfacial region possesses mixed properties and that the different pictures obtained up to now can be unified. Moreover, we discuss the effect of the interfacial water structure on the abnormal thermal transport properties of solid/liquid interfaces. PMID:25176017

  2. Electronic Excitation Dynamics in Liquid Water under Proton Irradiation

    PubMed Central

    Reeves, Kyle G.; Kanai, Yosuke

    2017-01-01

    Molecular behaviour of liquid water under proton irradiation is of great importance to a number of technological and medical applications. The highly energetic proton generates a time-varying field that is highly localized and heterogeneous at the molecular scale, and massive electronic excitations are produced as a result of the field-matter interaction. Using first-principles quantum dynamics simulations, we reveal details of how electrons are dynamically excited through non-equilibrium energy transfer from highly energetic protons in liquid water on the atto/femto-second time scale. Water molecules along the path of the energetic proton undergo ionization at individual molecular level, and the excitation primarily derives from lone pair electrons on the oxygen atom of water molecules. A reduced charge state on the energetic proton in the condensed phase of water results in the strongly suppressed electronic response when compared to water molecules in the gas phase. These molecular-level findings provide important insights into understanding the water radiolysis process under proton irradiation. PMID:28084420

  3. Electronic Excitation Dynamics in Liquid Water under Proton Irradiation

    NASA Astrophysics Data System (ADS)

    Reeves, Kyle G.; Kanai, Yosuke

    2017-01-01

    Molecular behaviour of liquid water under proton irradiation is of great importance to a number of technological and medical applications. The highly energetic proton generates a time-varying field that is highly localized and heterogeneous at the molecular scale, and massive electronic excitations are produced as a result of the field-matter interaction. Using first-principles quantum dynamics simulations, we reveal details of how electrons are dynamically excited through non-equilibrium energy transfer from highly energetic protons in liquid water on the atto/femto-second time scale. Water molecules along the path of the energetic proton undergo ionization at individual molecular level, and the excitation primarily derives from lone pair electrons on the oxygen atom of water molecules. A reduced charge state on the energetic proton in the condensed phase of water results in the strongly suppressed electronic response when compared to water molecules in the gas phase. These molecular-level findings provide important insights into understanding the water radiolysis process under proton irradiation.

  4. Hydrochloric acid aerosol formation by the interaction of hydrogen chloride with humid air

    NASA Technical Reports Server (NTRS)

    Rhein, R. A.

    1973-01-01

    The conditions in which hydrochloric acid aerosol is predicted by the interaction of hydrogen chloride gas with the water vapor in humid air are analyzed. The liquid gas phase equilibrium for the HCL-H2O system is expressed in terms of relative humidity and hydrogen chloride concentration as parts per million, units commonly used in pollution studies. Presented are the concentration (wt %) of HC1 in the aerosol and the concentration of aerosol (ppm) predicted.

  5. Water-Soluble Organic Species in Biomass Burning Aerosols in Southern Africa: Their Chemical Identification and Spatial Distribution

    NASA Astrophysics Data System (ADS)

    Gao, S.; Hegg, D. A.; Hobbs, P. V.; Kirchstetter, T. W.; Magi, B.

    2001-12-01

    During the SAFARI-2000 field campaign, 14 aerosol samples were collected from an aircraft in plumes from biomass fires (under both flaming and smoldering conditions), at various distances from the fire source. Also collected were 36 aerosol samples in haze layers ranging from the surface to 16,000 feet, some of which could be associated with specific fires. The samples were collected on teflon membrane filters (lower size limit of about 30nm in diameter) which were analyzed for total aerosol mass loading and chemical composition using several analytical techniques. Particular effort was made to speciate the water-soluble portion of the aerosol organics. Seven organic acids and seven carbohydrate species (and their possible stereoisomers) were identified and quantified, along with three inorganic anions and five inorganic cations. The identified organic species accounted for up to 32% of the total aerosol mass; compared with concurrent total carbon and organic carbon measurements, the identified organics constituted at least 5% to 30% of the mass of the total aerosol organics. A number of conspicuous spatial distribution patterns were observed for these species. For instance, using K+ to correct for dilution, it was found that gluconate, oxalate, succinate, and glutarate, along with sulfate and nitrate, all increased significantly in mass concentration from the fire source going downwind. This suggests secondary formation of these species during aerosol aging. On the other hand, formate and acetate showed decreasing trends downwind, probably due to the loss of these volatile species to the gas phase. Another striking pattern is that anhydrosugars (e.g. levoglucosan) had the highest aerosol mass fraction near smoldering fires but a very low fraction in the haze layers, whereas, dicarboxylic acids showed an almost opposite trend. This implies possible chemical reaction processes converting intermediate organic products, such as levoglucosan, to smaller products like

  6. Modeling Impacts On and Feedbacks Among Surface Energy and Water Budgets Due to Aerosols-In-Snow Across North America

    NASA Astrophysics Data System (ADS)

    Oaida, C. M.; Xue, Y.; Chin, M.; Flanner, M.; De Sales, F.; Painter, T. H.

    2014-12-01

    Snow albedo is known to have a significant impact on energy and water budgets by modulating land-atmosphere flux exchanges. In recent decades, anthropogenic activities that cause dust and soot emission and deposition on snow-covered areas have lead to the alteration of snow albedo. Our study aims to investigate and quantitatively assess the impact of aerosols-in-snow on surface energy and water budgets at a local and regional scale using a recently enhanced regional climate model that has physically based snow processes, including aerosols in snow. We employ NCAR's WRF-ARW model, which we have previously coupled with a land surface model, Simplified Simple Biosphere version 3 (SSiB-3). We improve the original WRF/SSiB-3 framework to include a snow-radiative transfer model, Snow, Ice, and Aerosol Radiative (SNICAR) model, which considers the effects of snow grain size and aerosols-in-snow on snow albedo evolution. Furthermore, the modified WRF/SSiB-3 can now account for the deposition and tracking of aerosols in snow. The model is run for 10 continuous years (2000-2009) over North America under two scenarios: (1) no aerosol deposition in snow, and (2) with GOCART dust, black carbon, and organic carbon surface deposition in snow. By comparing the two cases, we can investigate the impact of aerosols-in-snow. We examine the changes in surface energy balance, such as albedo, surface net solar radiation (radiative forcing), and surface air and skin temperature, and how these might interact with, and lead to, changes in the hydrologic cycle, including SWE, runoff, evapotranspiration and soil moisture. We investigate the mechanisms and feedbacks that might contribute to the changes seen across select regions of North America, which are potentially a result of both local and remote effects.

  7. Total ozone column, aerosol optical depth and precipitable water effects on solar erythemal ultraviolet radiation recorded in Malta.

    NASA Astrophysics Data System (ADS)

    Bilbao, Julia; Román, Roberto; Yousif, Charles; Mateos, David; Miguel, Argimiro

    2013-04-01

    The Universities of Malta and Valladolid (Spain) developed a measurement campaign, which took place in the Institute for Energy Technology in Marsaxlokk (Southern Malta) between May and October 2012, and it was supported by the Spanish government through the Project titled "Measurement campaign about Solar Radiation, Ozone, and Aerosol in the Mediterranean area" (with reference CGL2010-12140-E). This campaign provided the first ground-based measurements in Malta of erythemal radiation and UV index, which indicate the effectiveness of the sun exposure to produce sunburn on human skin. A wide variety of instruments was involved in the campaign, providing a complete atmospheric characterization. Data of erythemal radiation and UV index (from UVB-1 pyranometer), total shortwave radiaton (global and diffuse components from CM-6B pyranometers), and total ozone column, aerosol optical thickness, and precitable water column (from a Microtops-II sunphotometer) were available in the campaign. Ground-based and satellite instruments were used in the analysis, and several intercomparisons were carried out to validate remote sensing data. OMI, GOME, GOME-2, and MODIS instruments, which provide data of ozone, aerosol load and optical properties, were used to this end. The effects on solar radiation, ultraviolet and total shortwave ranges, of total ozone column, aerosol optical thickness and precipitable water column were obtained using radiation measurements at different fixed solar zenith angles. The empirical results shown a determinant role of the solar position, a negligible effect of ozone on total shortwave radiation, and a stronger attenuation provided by aerosol particles in the erythemal radiation. A variety of aerosol types from different sources (desert dust, biomass burning, continental, and maritime) reach Malta, in this campaign several dust events from the Sahara desert occurred and were analyzed establishing the air mass back-trajectories ending at Malta at

  8. ACE-Asia Aerosol Optical Depth and Water Vapor Measured by Airborne Sunphotometers and Related to Other Measurements and Calculations

    NASA Technical Reports Server (NTRS)

    Livingston, John M.; Russell, P. B.; Schmid, B.; Redemann, J.; Eilers, J. A.; Ramirez, S. A.; Kahn, R.; Hegg, D.; Pilewskie, P.; Anderson, T.; Hipskind, R. Stephen (Technical Monitor)

    2001-01-01

    In the Spring 2001 phase of the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia), the 6-channel NASA Ames Airborne Tracking Sunphotometer (AATS-6) operated on 15 of the 19 research flights of the NCAR C-130, while its 14-channel counterpart (AATS- 14) flew successfully on all 18 research flights of the CIRPAS Twin Otter. ACE-Asia studied aerosol outflow from the Asian continent to the Pacific basin. It was designed to integrate suborbital and satellite measurements and models so as to reduce the uncertainty in calculations of the climate forcing due to aerosols. AATS-6 and AATS-14 measured solar beam transmission at 6 and 14 wavelengths (380-1021 and 354-1558 nm, respectively), yielding aerosol optical depth (AOD) spectra and column water vapor (CWV). Vertical differentiation in profiles yielded aerosol extinction spectra and water vapor concentration. The wavelength dependence of these AOD and extinction spectra indicates that supermicron dust was often a major component of the ACE-Asia aerosol. Frequently this dust-containing aerosol extended to high altitudes. For example, in AATS- 14 profiles analyzed to date, 36% of full-column AOD at 525 nm was above 3 km. In contrast, only 10% of CWV was above 3 km. Analyses and applications of AATS-6 and AATS-14 data to date include comparisons to (i) extinction products derived using in situ measurements, (ii) extinction profiles derived from lidar measurements, and (iii) AOD retrievals from the Multi-angle Imaging Spectro-Radiometer (MISR) aboard the TERRA satellite. Other planned collaborative studies include comparisons to results from size spectrometers, chemical measurements, other satellite sensors, flux radiometers, and chemical transport models. Early results of these studies will be presented.

  9. Water soluble aerosols and gases at a UK background site - Part 1: Controls of PM2.5 and PM10 aerosol composition

    NASA Astrophysics Data System (ADS)

    Twigg, M. M.; Di Marco, C. F.; Leeson, S.; van Dijk, N.; Jones, M. R.; Leith, I. D.; Morrison, E.; Coyle, M.; Proost, R.; Peeters, A. N. M.; Lemon, E.; Frelink, T.; Braban, C. F.; Nemitz, E.; Cape, J. N.

    2015-07-01

    There is limited availability of long-term, high temporal resolution, chemically speciated aerosol measurements which can provide further insight into the health and environmental impacts of particulate matter. The Monitor for AeRosols and Gases (MARGA, Applikon B.V., NL) allows for the characterisation of the inorganic components of PM10 and PM2.5 (NH4+, NO3-, SO42-, Cl-, Na+, K+, Ca2+, Mg2+) and inorganic reactive gases (NH3, SO2, HCl, HONO and HNO3) at hourly resolution. The following study presents 6.5 years (June 2006 to December 2012) of quasi-continuous observations of PM2.5 and PM10 using the MARGA at the UK EMEP supersite, Auchencorth Moss, SE Scotland. Auchencorth Moss was found to be representative of a remote European site with average total water soluble inorganic mass of PM2.5 of 3.82 μg m-3. Anthropogenically derived secondary inorganic aerosols (sum of NH4+, NO3- and nss-SO42-) were the dominating species (63 %) of PM2.5. In terms of equivalent concentrations, NH4+ provided the single largest contribution to PM2.5 fraction in all seasons. Sea salt was the main component (73 %) of the PMcoarse fraction (PM10-PM2.5), though NO3- was also found to make a relatively large contribution to the measured mass (17 %) providing evidence of considerable processing of sea salt in the coarse mode. There was on occasions evidence of aerosol from combustion events being transported to the site in 2012 as high K+ concentrations (deviating from the known ratio in sea salt) coincided with increases in black carbon at the site. Pollution events in PM10 (defined as concentrations > 12 μg m-3) were on average dominated by NH4+ and NO3-, where smaller loadings at the site tended to be dominated by sea salt. As with other western European sites, the charge balance of the inorganic components resolved were biased towards cations, suggesting the aerosol was basic or more likely that organic acids contributed to the charge balance. This study demonstrates the UK

  10. Water soluble aerosols and gases at a UK background site - Part 1: Controls of PM2.5 and PM10 aerosol composition

    NASA Astrophysics Data System (ADS)

    Twigg, M. M.; Di Marco, C. F.; Leeson, S.; van Dijk, N.; Jones, M. R.; Leith, I. D.; Morrison, E.; Coyle, M.; Proost, R.; Peeters, A. N. M.; Lemon, E.; Frelink, T.; Braban, C. F.; Nemitz, E.; Cape, J. N.

    2015-02-01

    There is limited availability of long-term, high temporal resolution, chemically speciated aerosol measurements, which can lead to further insight into the health and environmental impacts of particulate matter. The Monitor for AeRosols and Gases (MARGA, Applikon B.V., NL) allows characterisation of the inorganic components of PM10 and PM2.5 (NH4+, NO3-, SO42-, Cl-, Na+, K+, Ca2+, Mg2+) and inorganic reactive gases (NH3, SO2, HCl, HONO and HNO3) at hourly resolution. The following study presents 6.5 years (June 2006 to December 2012) of quasi-continuous observations of PM2.5 and PM10 using the MARGA at the UK EMEP "Supersite", Auchencorth Moss, SE Scotland. Auchencorth Moss was found to be representative of a remote European site with average total water soluble inorganic mass of PM2.5 of 3.82 μg m-3. Anthropogenically derived secondary inorganic aerosols (sum of NH4+, NO3- and nss-SO42-), were the dominating species (63%) of PM2.5. In terms of equivalent concentrations, NH4+ provided the single largest contribution to PM2.5 fraction in all seasons. Sea salt, was the main component (73%) of the PMcoarse fraction (PM10-PM2.5), though NO3- was also found to make a relatively large contribution to the measured mass (17%) as providing evidence of considerable processing of sea salt in the coarse mode. There was on occasions evidence of aerosol from combustion events being transported to the site in 2012 as high K+ concentrations (deviating from the known ratio in sea salt) coincided with increases in black carbon at the site. Pollution events in PM10 (defined as concentrations > 12 μg m-3) were on average dominated by NH4+ and NO3-, where as smaller loadings at the site tended to be dominated by sea salt. As with other Western European sites, the charge balance of the inorganic components resolved were biased towards cations, suggesting the aerosol was basic or more likely, that organic acids contributed to the charge

  11. Determination of saccharides in atmospheric aerosol using anion-exchange high-performance liquid chromatography and pulsed-amperometric detection.

    PubMed

    Caseiro, Alexandre; Marr, Iain L; Claeys, Magda; Kasper-Giebl, Anne; Puxbaum, Hans; Pio, Casimiro A

    2007-11-09

    An improved method is described for the quantification of primary sugars, sugar alcohols and anhydrosugars in atmospheric aerosols, making use of separation by high-performance anion-exchange chromatography (HPAEC) with pulsed amperometric detection (PAD). Quartz fibre filters from high-volume samplers were extracted with water and the extract injected directly. Repeatability is typically 4% RSD, for e.g. levoglucosan at 50 ng m(-3) in air, better for winter levels around 700 ng m(-3). Limits of detection for individual sugars are in the range 0.02-0.05 microg mL(-1) in solution, corresponding to 2-5 ng m(-3) from a 20 m(3) air sample. The overlap of arabitol and levogluocosan is overcome by using a Dionex PA-1 column, with appropriate control of eluent composition, and peak deconvolution software, allowing quantification of both sugars in difficult summer samples containing low-levels of levoglucosan. Analysis of a set of ambient aerosol samples by both GC-flame ionization detection and HPAEC-PAD shows good agreement. The new method has the advantage of requiring no sample pretreatment or derivatization and is thus well suited to handling large numbers of samples.

  12. Atmospheric Chemistry: Nature's plasticized aerosols

    NASA Astrophysics Data System (ADS)

    Ziemann, Paul J.

    2016-01-01

    The structure of atmospheric aerosol particles affects their reactivity and growth rates. Measurements of aerosol properties over the Amazon rainforest indicate that organic particles above tropical rainforests are simple liquid drops.

  13. Characterization of Light Non-Methane Hydrocarbons, Surface Water DOC, and Aerosols over the Nordic Seas

    NASA Astrophysics Data System (ADS)

    Hudson, E. D.; Ariya, P. A.

    2006-12-01

    Whole air, size-fractionated marine aerosols, and surface ocean water DOC were sampled together during June-July 2004 on the Nordic seas, in order to explore factors leading to the formation of volatile organic compounds (VOCs) at the sea surface and their transfer to the atmosphere. High site-to-site variability in 19 non-methane hydrocarbon concentrations suggests highly variable, local sources for these compounds. Acetone, C5 and C6 hydrocarbons, and dimethylsulfide were identified in the seawater samples using solid-phase microextraction/GC-MS. The aerosols were analysed by SEM-EDX and contained primarily inorganic material (sea salt, marine sulfates, and carbonates) and little organic matter. However, a culturable bacterium was isolated from the large (9.9 - 18 μ m) fraction at one site, and identified as Micrococcus luteus. We will discuss the implication of these results on potential exchange processes at the ocean-atmosphere interface and the impact of bioaerosols in transferring marine organic carbon to atmospheric organic carbon.

  14. Validation of MODIS and VIIRS derived aerosol optical depth over complex coastal waters

    NASA Astrophysics Data System (ADS)

    Bilal, Muhammad; Nazeer, Majid; Nichol, Janet E.

    2017-04-01

    In this study, the Simplified Aerosol Retrieval Algorithm (SARA) was applied to both MODIS and Visible Infrared Imaging Radiometer Suits (VIIRS) images to retrieve aerosol optical depth (AOD) over water for blue, green and red wavelengths at 500 m (MODISSARA) and 750 m (VIIRSSARA) resolutions, respectively. Retrievals were compared with the Terra-MODIS Dark Target (DT) AOD at 3 km resolution (MODIS3K) and the VIIRS Environmental Data Record (VIIRSEDR) AOD at 6 km resolution. Validation was conducted using 86 Microtops II Sun photometer AOD measurements collected over different classes of water quality (low to high sediment levels) for seven days (6, 8, 9, 13, and 15, 16 and 17 October 2014) between 10:00 to 15:00 local time. Thirty-eight to fifty percent and 44-54% of the MODIS3K and the VIIRSEDR AOD retrievals respectively, fall within the expected error (EE) with root mean square error from 0.12 to 0.14 and mean absolute error from 0.10 to 0.11. The MODISSARA and the VIIRSSARA AOD retrievals are well correlated with the ground-based measurements (R: MODISSARA = 0.86-0.89 and VIIRSSARA = 0.85-0.94), with a larger number of retrievals falling within the EE MODISSARA = 73-77% and VIIRSSARA = 71-82%) than MODIS3K and VIIRSEDR. The results indicate that the SARA algorithm is more robust than MODIS3K and VIIRSEDR global AOD products, and can retrieve accurate AOD over low to highly sedimented water surfaces, similar to good AOD retrievals over land.

  15. A single-site multipole model for liquid water

    NASA Astrophysics Data System (ADS)

    Tran, Kelly N.; Tan, Ming-Liang; Ichiye, Toshiko

    2016-07-01

    Accurate and efficient empirical potential energy models that describe the atomistic interactions between water molecules in the liquid phase are essential for computer simulations of many problems in physics, chemistry, and biology, especially when long length or time scales are important. However, while models with non-polarizable partial charges at four or five sites in a water molecule give remarkably good values for certain properties, deficiencies have been noted in other properties and increasing the number of sites decreases computational efficiency. An alternate approach is to utilize a multipole expansion of the electrostatic potential due to the molecular charge distribution, which is exact outside the charge distribution in the limits of infinite distances or infinite orders of multipoles while partial charges are a qualitative representation of electron density as point charges. Here, a single-site multipole model of water is presented, which is as fast computationally as three-site models but is also more accurate than four- and five-site models. The dipole, quadrupole, and octupole moments are from quantum mechanical-molecular mechanical calculations so that they account for the average polarization in the liquid phase, and represent both the in-plane and out-of-plane electrostatic potentials of a water molecule in the liquid phase. This model gives accurate thermodynamic, dynamic, and dielectric properties at 298 K and 1 atm, as well as good temperature and pressure dependence of these properties.

  16. Water Tank with Capillary Air/Liquid Separation

    NASA Technical Reports Server (NTRS)

    Ungar, Eugene K.; Smith, Frederick; Edeen, Gregg; Almlie, Jay C.

    2010-01-01

    A bladderless water tank (see figure) has been developed that contains capillary devices that allow it to be filled and emptied, as needed, in microgravity. When filled with water, the tank shields human occupants of a spacecraft against cosmic radiation. A membrane that is permeable by air but is hydrophobic (neither wettable nor permeable by liquid water) covers one inside surface of the tank. Grooves between the surface and the membrane allow air to flow through vent holes in the surface as the tank is filled or drained. A margin of wettable surface surrounds the edges of the membrane, and all the other inside tank surfaces are also wettable. A fill/drain port is located in one corner of the tank and is covered with a hydrophilic membrane. As filling begins, water runs from the hydrophilic membrane into the corner fillets of the tank walls. Continued filling in the absence of gravity will result in a single contiguous air bubble that will be vented through the hydrophobic membrane. The bubble will be reduced in size until it becomes spherical and smaller than the tank thickness. Draining the tank reverses the process. Air is introduced through the hydrophobic membrane, and liquid continuity is maintained with the fill/drain port through the corner fillets. Even after the tank is emptied, as long as the suction pressure on the hydrophilic membrane does not exceed its bubble point, no air will be drawn into the liquid line.

  17. Deep convective clouds with sustained supercooled liquid water down to -37.5 degrees C

    PubMed

    Rosenfeld; Woodley

    2000-05-25

    In cirrus and orographic wave clouds, highly supercooled water has been observed in small quantities (less than 0.15 g m(-3)). This high degree of supercooling was attributed to the small droplet size and the lack of ice nuclei at the heights of these clouds. For deep convective clouds, which have much larger droplets near their tops and which take in aerosols from near the ground, no such measurements have hitherto been reported. However, satellite data suggest that highly supercooled water (down to -38 degrees C) frequently occurs in vigorous continental convective storms. Here we report in situ measurements in deep convective clouds from an aircraft, showing that most of the condensed water remains liquid down to -37.5 degrees C. The droplets reach a median volume diameter of 17 microm and amount to 1.8 gm(-3), one order of magnitude more than previously reported. At slightly colder temperatures only ice was found, suggesting homogeneous freezing. Because of the poor knowledge of mixed-phase cloud processes, the simulation of clouds using numerical models is difficult at present. Our observations will help to understand these cloud processes, such as rainfall, hail, and cloud electrification, together with their implications for the climate system.

  18. Longwave radiative forcing by aqueous aerosols

    SciTech Connect

    Gaffney, J.S.; Marley, N.A.

    1995-01-01

    Recently, a great deal of interest has been focused on the role of aerosols in climatic change because of their potential cooling impacts due to light scattering. Recent advances in infrared spectroscopy using cylindrical internal reflectance have allowed the longwave absorption of dissolved aerosol species and the associated liquid water to be accurately determined and evaluated. Experimental measurements using these techniques have shown that dissolved sulfate, nitrate, and numerous other aerosol species will act to cause greenhouse effects. Preliminary calculations indicate that the longwave climate forcing (i.e., heating) for sulfate aerosol will be comparable in magnitude to the cooling effect produced by light scattering. However, more detailed modeling will clearly be needed to address the impact of the longwave forcing due to aerosols as a function of atmospheric height and composition. Their work has shown that aerosol composition will be important in determining longwave forcing, while shortwave forcing will be more related to the physical size of the aerosol droplets. On the basis of these studies, it is increasingly apparent that aerosols, fogs, and clouds play a key role in determining the radiative balance of the atmosphere and in controlling regional and global climates.

  19. Liquid water confined in carbon nanochannels at high temperatures.

    PubMed

    Nagy, G; Gordillo, M C; Guàrdia, E; Martí, J

    2007-11-01

    Structure, hydrogen bonding, electrostatics, dielectric, and dynamical properties of liquid water confined in flat graphene nanochannels are investigated by molecular dynamics simulations. A wide range of temperatures (between 20 and 360 degrees C) have been considered. Molecular structure suffers substantial changes when the system is heated, with a significant loss of structure and hydrogen bonding. In such case, the interface between adsorbed and bulk-like water has a marked tendency to disappear, and the two preferential orientations of water nearby the graphite layers at room temperature are essentially merging above the boiling point. The general trend for the static dielectric constant is its reduction at high temperature states, as compared to ambient conditions. Similarly, residence times of water molecules in adsorbed and bulk-like regions are significantly influenced by temperature, as well. Finally, we observed relevant changes in water diffusion and spectroscopy along the range of temperatures analyzed.

  20. FEASIBILITY OF THE AEROSOL-TO-LIQUID PARTICLE EXTRACTION SYSTEM (ALPES) FOR COLLECTION OF VIABLE FRANCISELLA SP.

    SciTech Connect

    Heitkamp, M

    2006-08-07

    Several Biowatch monitoring sites in the Houston area have tested positive for Francisella tularensis and there is a need to determine whether natural occurring Francisella-related microorganism(s) may be responsible for these observed positive reactions. The collection, culturing and characterization of Francisella-related natural microorganisms will provide the knowledge base to improve the future selectivity of Biowatch monitoring for Francisella. The aerosol-to-liquid particle extraction system (ALPES) is a high-efficiency, dual mechanism collection system that utilizes a liquid collection medium for capture of airborne microorganisms. Since the viability of microorganisms is preserved better in liquid medium than on air filters, this project was undertaken to determine whether Francisella philomiragia and Francisella tularensis LVS maintain acceptable viability in the continuous liquid recirculation, high direct current voltage and residual ozone concentrations which occur during ALPES operation. Throughout a series of preliminary trial runs with representative gram-negative and gram-positive microorganisms, several design modifications and improvements to the ALPES optimized liquid handling, electrical stability, sampling and overall performance for biological sampling. Initial testing with Francisella philomiragia showed viability was preserved better in PBS buffer than HBSS buffer. Trial runs at starting cell concentrations of 1.8 x 10{sup 6} and 2.5 x 10{sup 4} CFU/L showed less than a 1-log decrease in viability for F. philomiragia after 24 h in the ALPES. Francisella tularensis LVS (live vaccine strain) was used as a surrogate for virulent F. tularensis in ALPES trial runs conducted at starting cell concentrations of 10{sup 4}, 10{sup 5} and 10{sup 6} CFU/L. F. tularensis LVS was slow-growing and required highly selective growth media to prevent overgrowth by collected airborne microorganisms. In addition, one ALPES unit intake was HEPA filtered during

  1. Hydrogen bonding definitions and dynamics in liquid water.

    PubMed

    Kumar, R; Schmidt, J R; Skinner, J L

    2007-05-28

    X-ray and neutron diffractions, vibrational spectroscopy, and x-ray Raman scattering and absorption experiments on water are often interpreted in terms of hydrogen bonding. To this end a number of geometric definitions of hydrogen bonding in water have been developed. While all definitions of hydrogen bonding are to some extent arbitrary, those involving one distance and one angle for a given water dimer are unnecessarily so. In this paper the authors develop a systematic procedure based on two-dimensional potentials of mean force for defining cutoffs for a given pair of distance and angular coordinates. They also develop an electronic structure-based definition of hydrogen bonding in liquid water, related to the electronic occupancy of the antibonding OH orbitals. This definition turns out to be reasonably compatible with one of the distance-angle geometric definitions. These two definitions lead to an estimate of the number of hydrogen bonds per molecule in liquid simple point charge/extended (SPC/E) water of between 3.2 and 3.4. They also used these and other hydrogen-bond definitions to examine the dynamics of local hydrogen-bond number fluctuations, finding an approximate long-time decay constant for SPC/E water of between 0.8 and 0.9 ps, which corresponds to the time scale for local structural relaxation.

  2. Molecular simulation study of water mobility in aerosol-OT reverse micelles.

    PubMed

    Chowdhary, Janamejaya; Ladanyi, Branka M

    2011-06-16

    In this work, we present results from molecular dynamics simulations on the single-molecule relaxation of water within reverse micelles (RMs) of different sizes formed by the surfactant aerosol-OT (AOT, sodium bis(2-ethylhexyl)sulfosuccinate) in isooctane. Results are presented for RM water content w(0) = [H(2)O]/[AOT] in the range from 2.0 to 7.5. We show that translational diffusion of water within the RM can, to a good approximation, be decoupled from the translation of the RM through the isooctane solvent. Water translational mobility within the RM is restricted by the water pool dimensions, and thus, the water mean-squared displacements (MSDs) level off in time. Comparison with models of diffusion in confined geometries shows that a version of the Gaussian confinement model with a biexponential decay of correlations provides a good fit to the MSDs, while a model of free diffusion within a sphere agrees less well with simulation results. We find that the local diffusivity is considerably reduced in the interfacial region, especially as w(0) decreases. Molecular orientational relaxation is monitored by examining the behavior of OH and dipole vectors. For both vectors, orientational relaxation slows down close to the interface and as w(0) decreases. For the OH vector, reorientation is strongly affected by the presence of charged species at the RM interface and these effects are especially pronounced for water molecules hydrogen-bonded to surfactant sites that serve as hydrogen-bond acceptors. For the dipole vector, orientational relaxation near the interface slows down more than that for the OH vector due mainly to the influence of ion-dipole interactions with the sodium counterions. We investigate water OH and dipole reorientation mechanisms by studying the w(0) and interfacial shell dependence of orientational time correlations for different Legendre polynomial orders.

  3. Liquid-liquid critical point in a simple analytical model of water

    NASA Astrophysics Data System (ADS)

    Urbic, Tomaz

    2016-10-01

    A statistical model for a simple three-dimensional Mercedes-Benz model of water was used to study phase diagrams. This model on a simple level describes the thermal and volumetric properties of waterlike molecules. A molecule is presented as a soft sphere with four directions in which hydrogen bonds can be formed. Two neighboring waters can interact through a van der Waals interaction or an orientation-dependent hydrogen-bonding interaction. For pure water, we explored properties such as molar volume, density, heat capacity, thermal expansion coefficient, and isothermal compressibility and found that the volumetric and thermal properties follow the same trends with temperature as in real water and are in good general agreement with Monte Carlo simulations. The model exhibits also two critical points for liquid-gas transition and transition between low-density and high-density fluid. Coexistence curves and a Widom line for the maximum and minimum in thermal expansion coefficient divides the phase space of the model into three parts: in one part we have gas region, in the second a high-density liquid, and the third region contains low-density liquid.

  4. Liquid-Liquid Phase Equilibria and Interactions between Droplets in Water-in-Oil Microemulsions.

    PubMed

    Yin, Tianxiang; Wang, Mingjie; Tao, Xiaoyi; Shen, Weiguo

    2016-12-20

    The liquid-liquid phase equilibria of [water/sodium bis(2-ethylhexyl)sulfosuccinate (AOT)/n-decane] with the molar ratio w0 of water to AOT being 37.9 and [water/AOT/ethoxylated-2,5,8,11-tetramethyl-6-dodecyne-5,8-diol(Dynol-604)/n-decane] with w0 = 37.9 and the mole fraction α of Dynol-604 in the total surfactants being 0.158 were measured in this study. From the data collected in the critical region, the critical exponent β corresponding to the width of the coexistence curve was determined, which showed good agreement with the 3D-Ising value. A thermodynamic approach based on the Carnahan-Starling-van der Waals type equation was proposed to describe the coexistence curves and to deduce the interaction properties between droplets in the microemulsions. The interaction enthalpies were found to be positive for the studied systems, which evidenced that the entropy effect dominated the phase separations as the temperature increased. The addition of Dynol-604 into the (water/AOT/n-decane) microemulsion resulted in the decrease in the critical temperature and the interaction enthalpy. Combining the liquid-liquid equilibrium data for (water/AOT/n-decane) microemulsions with various w0 values determined previously, it was shown that the interaction enthalpy decreased with w0 and tended to change its sign at low w0, which coincided with the results from the isothermal titration calorimetry investigation. All of these behaviors were interpreted by the effects of entropy and enthalpy and their competition, which resulted from the release of solvent molecules entrapped in the interface of microemulsion droplets and were dependent on the rigidity of the surfactant layers and the size of the droplet.

  5. Sources and light absorption of water-soluble organic carbon aerosols in the outflow from northern China

    NASA Astrophysics Data System (ADS)

    Kirillova, E. N.; Andersson, A.; Han, J.; Lee, M.; Gustafsson, Ö.

    2014-02-01

    High loadings of anthropogenic carbonaceous aerosols in Chinese air influence the air quality for over one billion people and impact the regional climate. A large fraction (17-80%) of this aerosol carbon is water-soluble, promoting cloud formation and thus climate cooling. Recent findings, however, suggest that water-soluble carbonaceous aerosols also absorb sunlight, bringing additional direct and indirect climate warming effects, yet the extent and nature of light absorption by this water-soluble "brown carbon" and its relation to sources is poorly understood. Here, we combine source estimates constrained by dual carbon isotopes with light-absorption measurements of water-soluble organic carbon (WSOC) for a March 2011 campaign at the Korea Climate Observatory at Gosan (KCOG), a receptor station in SE Yellow Sea for the outflow from northern China. The mass absorption cross section at 365 nm (MAC365) of WSOC for air masses from N. China were in general higher (0.8-1.1 m2 g-1), than from other source regions (0.3-0.8 m2 g-1). However, this effect corresponds to only 2-10% of the radiative forcing caused by light absorption by elemental carbon. Radiocarbon constraints show that the WSOC in Chinese outflow had significantly higher fraction fossil sources (30-50%) compared to previous findings in S. Asia, N. America and Europe. Stable carbon (δ13C) measurements were consistent with aging during long-range air mass transport for this large fraction of carbonaceous aerosols.

  6. Effect of the secondary organic aerosol coatings on black carbon water uptake, cloud condensation nuclei activity, and particle collapse

    EPA Science Inventory

    The ability of black carbon aerosols to absorb water and act as a cloud condensation nuclei (CCN) directly controls their lifetime in the atmosphere as well as their impact on cloud formation, thus impacting the earth’s climate. Black carbon emitted from most combustion pro...

  7. X-Ray Spectroscopy of the Liquid Water Surface

    NASA Astrophysics Data System (ADS)

    Saykally, Richard

    2004-03-01

    We have developed a new experiment for probing molecular details of liquid-vapor interfaces of volatile substances and their solutions under equilibrium conditions. Electronic and geometric structures of interfacial molecules are probed by EXAFS and NEXAFS methods in the soft X-ray region, using the Advanced Light Source, Berkeley, CA. Liquids are introduced into a high vacuum environment through the use of liquid microjets, which have been characterized independently by Raman spectroscopy. Detection of ions and electrons produced by the Auger avalanche probe the bulk and surface regions of the microjet, respectively, as a result of their different escape depths. Our first efforts involved a comparative study of the interfaces of water and methanol, wherein we detailed the first observation of surface relaxation for a liquid. Analysis of EXAFS data yielded a 6distance at the water interface, whereas a 5was found for methanol. NEXAFS measurements, interpreted in terms of density functional theory simulations, indicate a large population of interfacial water molecules having two free OH bonds ("acceptor only molecules"). This complements the "single donor" species identified in sum frequency generation experiments. These results are supported by recent theoretical calculations. For methanol and other simple alcohols, the data indicate that free alkyl groups extend into the vapor part of the interface. Preliminary results for aqueous solutions, as well as for other pure liquids, have been obtained and are presently under analysis. REFERENCES 1. K.R. Wilson, R.D. Schaller, B.S. Rude, T. Catalano, D.T. Co, J.D. Bozek, and R.J. Saykally, "Surface relaxation in liquid water and methanol studied by X-ray absorption spectroscopy," J. Chem. Phys 117,7738(2002). 2. K.R. Wilson, M. Cavalleri, B.S. Rude, R.D. Schaller, A. Nilsson, L.G.M. Pettersson, N. Goldman, T. Catalano, J.D. Bozek, and R.J. Saykally, "Characterization of hydrogen bond acceptor molecules at the water surface

  8. AEROSOL, CLOUDS, AND CLIMATE CHANGE

    SciTech Connect

    SCHWARTZ, S.E.

    2005-09-01

    Earth's climate is thought to be quite sensitive to changes in radiative fluxes that are quite small in absolute magnitude, a few watts per square meter, and in relation to these fluxes in the natural climate. Atmospheric aerosol particles exert influence on climate directly, by scattering and absorbing radiation, and indirectly by modifying the microphysical properties of clouds and in turn their radiative effects and hydrology. The forcing of climate change by these indirect effects is thought to be quite substantial relative to forcing by incremental concentrations of greenhouse gases, but highly uncertain. Quantification of aerosol indirect forcing by satellite- or ground-based remote sensing has proved quite difficult in view of inherent large variation in the pertinent observables such as cloud optical depth, which is controlled mainly by liquid water path and only secondarily by aerosols. Limited work has shown instances of large magnitude of aerosol indirect forcing, with local instantaneous forcing upwards of 50 W m{sup 66}-2. Ultimately it will be necessary to represent aerosol indirect effects in climate models to accurately identify the anthropogenic forcing at present and over secular time and to assess the influence of this forcing in the context of other forcings of climate change. While the elements of aerosol processes that must be represented in models describing the evolution and properties of aerosol particles that serve as cloud condensation particles are known, many important components of these processes remain to be understood and to be represented in models, and the models evaluated against observation, before such model-based representations can confidently be used to represent aerosol indirect effects in climate models.

  9. Ionic-liquid-based dispersive liquid-liquid microextraction combined with high-performance liquid chromatography for the determination of multiclass pesticide residues in water samples.

    PubMed

    Tadesse, Bezuayehu; Teju, Endale; Gure, Abera; Megersa, Negussie

    2015-03-01

    Ionic-liquid-based dispersive liquid-liquid microextraction in combination with high-performance liquid chromatography and diode array detection has been proposed for the simultaneous analysis of four multiclass pesticide residues including carbaryl, methidathion, chlorothalonil, and ametryn from water samples. The major experimental parameters including the type and volume of ionic liquid, sample pH, type, and volume of disperser solvent and cooling time were investigated and optimum conditions were established. Under the optimum experimental conditions, limits of detection and quantification of the method were in the range of 0.1-1.8 and 0.4-5.9 μg/L, respectively, with satisfactory enrichment factors ranging from 10-20. The matrix-matched calibration curves, which were constructed for lake water, as a representative matrix were linear over wide range with coefficients of determination of 0.996 or better. Intra- and interday precisions, expressed as relative standard deviations, were in the range of 1.1-9.7 and 3.1-7.8%, respectively. The relative recoveries of the spiked environmental water samples at one concentration level were in the range of 77-102%. The results of the present study revealed that the proposed method is simple, fast, and uses environmentally friendly extraction solvent for the analysis of the target pesticide residues in environmental water samples.

  10. Dispersive liquid-liquid microextraction of silver nanoparticles in water using ionic liquid 1-octyl-3-methylimidazolium hexafluorophosphate.

    PubMed

    Chen, Sha; Sun, Yuanjing; Chao, Jingbo; Cheng, Liping; Chen, Yun; Liu, Jingfu

    2016-03-01

    Using the ionic liquid (IL) 1-octyl-3-methylimidazolium hexafluorophosphate as the extractant and methanol as the dispersion solvent, a dispersive liquid-liquid microextraction method was developed to extract silver nanoparticles (AgNPs) from environmental water samples. Parameters that influenced the extraction efficiency such as IL concentration, pH and extraction time were optimized. Under the optimized conditions, the highest extraction efficiency for AgNPs was above 90% with an enrichment factor of >90. The extracted AgNPs in the IL phase were identified by transmission electron microscopy and ultraviolet-visible spectroscopy, and quantified by inductively coupled plasma mass spectrometry after microwave digestion, with a detection limit of 0.01μg/L. The spiked recovery of AgNPs was 84.4% with a relative standard deviation (RSD) of 3.8% (n=6) at a spiked level of 5μg/L, and 89.7% with a RSD of 2.2% (n=6) at a spiked level of 300μg/L, respectively. Commonly existed environmental ions had a very limited influence on the extraction efficiency. The developed method was successfully applied to the analysis of AgNPs in river water, lake water, and the influent and effluent of a wastewater treatment plant, with recoveries in the range of 71.0%-90.9% at spiking levels of 0.11-4.7μg/L.

  11. Characterization of water-soluble inorganic ions in size-segregated aerosols in coastal city, Xiamen

    NASA Astrophysics Data System (ADS)

    Zhao, Jinping; Zhang, Fuwang; Xu, Ya; Chen, Jinsheng

    2011-03-01

    The samples of water-soluble inorganic ions (WSIs), including anions (F-, Cl-, SO42-, NO3-) and cations (NH4+, K+, Na+, Ca2+, Mg2+) in 8 size-segregated particle matter (PM), were collected using a sampler (with 8 nominal cut-sizes ranged from 0.43 to 9.0 μm) from October 2008 to September 2009 at five sites in both polluted and background regions of a coastal city, Xiamen. The results showed that particulate matters in the fine mode (PM2.1, Dp < 2.1 μm) comprised large part of mass concentrations of aerosols, which accounted for 45.56-51.27%, 40.04-60.81%, 42.02-60.81%, and 40.46-57.07% of the total particulate mass in spring, summer, autumn, and winter, respectively. The water-soluble ionic species in the fine mode at five sampling sites varied from 15.33 to 33.82 (spring), 14.03 to 28.06 (summer), 33.47 to 72.52 (autumn), and 48.39 to 69.75 μg m- 3 (winter), respectively, which accounted for 57.30 ± 6.51% of the PM2.1 mass concentrations. Secondary pollutants of NH4+, SO42- and NO3- were the dominant contributors of WSIs, which suggested that pollutants from anthropogenic activities, such as SO2, NOx were formed in aerosols by photochemical reactions. The size distributions of Na+, Cl-, SO42- and NO3- were bimodal, peaking at 0.43-0.65 μm and 3.3-5.8 μm. Although some ions, such as NH4+ presented bimodal distributions, the coarse mode was insignificant compared to the fine mode. Ca2+ and Mg2+ exhibited unimodal distributions at all sampling sites, peaking at 2.1-3.3 μm, while K+ having a bimodal distributions with a major peak at 0.43-0.65 μm and a minor one at 3.3-4.7 μm, were used in most of samples. Seasonal and spatial variations in the size-distribution profiles suggested that meteorological conditions (seasonal patterns) and sampling locations (geographical patterns) were the main factors determining the formation of secondary aerosols and characteristics of size distributions for WSIs.

  12. Determination of Maintaining Time of Temperature Traces of Aerosol Droplet Water Flows During Motion in a Flame

    NASA Astrophysics Data System (ADS)

    Antonov, D. V.; Voitkov, I. S.; Strizhak, P. A.

    2016-02-01

    To develop fire fighting technologies, the temperatures of combustible products were measured after passing an aerosol droplet flow of water through the flames (with monitored temperatures). It was applied the aerosol flows with droplets of sizes less than 100 μm, 100-200 μm, and 200-300 μm. Investigations were conducted at a temperature of combustible products from 500 K to 900 K. Temperatures of gases in droplet flow traces and maintaining times of relatively low temperatures in these areas (it can be considered as temperature trace) were defined. It was obtained the satisfactory agreement of experimental results and numerical simulation data.

  13. Optically Thin Liquid Water Clouds: Their Importance and Our Challenge

    NASA Technical Reports Server (NTRS)

    Turner, D. D.; Vogelmann, A. M.; Austin, R. T.; Barnard, J. C.; Cady-Pereira, K.; Chiu, J. C.; Clough, S. A.; Flynn, C.; Khaiyer, M. M.; Liljegren, J.; Johnson, K.; Lin, B.; Long, C.; Marshak, A.; Matrosov, S. Y.; McFarlane, S. A.; Miller, M.; Min, Q.; Minnis, P.; O'Hirok, W.; Wang, Z.; Wiscombe, W.

    2006-01-01

    Many of the clouds important to the Earth's energy balance, from the tropics to the Arctic, are optically thin and contain liquid water. Longwave and shortwave radiative fluxes are very sensitive to small perturbations of the cloud liquid water path (LWP) when the liquid water path is small (i.e., < g/sq m) and, thus, the radiative properties of these clouds must be well understood to capture them correctly in climate models. We review the importance of these thin clouds to the Earth's energy balance, and explain the difficulties in observing them. In particular, because these clouds are optically thin, potentially mixed-phase, and often (i.e., have large 3-D variability), it is challenging to retrieve their microphysical properties accurately. We describe a retrieval algorithm intercomparison that was conducted to evaluate the issues involved. The intercomparison included eighteen different algorithms to evaluate their retrieved LWP, optical depth, and effective radii. Surprisingly, evaluation of the simplest case, a single-layer overcast cloud, revealed that huge discrepancies exist among the various techniques, even among different algorithms that are in the same general classification. This suggests that, despite considerable advances that have occurred in the field, much more work must be done, and we discuss potential avenues for future work.

  14. Thermally driven electrokinetic energy conversion with liquid water microjets

    NASA Astrophysics Data System (ADS)

    Lam, Royce K.; Gamlieli, Zach; Harris, Stephen J.; Saykally, Richard J.

    2015-11-01

    A goal of current energy research is to design systems and devices that can efficiently exploit waste heat and utilize solar or geothermal heat energy for electrical power generation. We demonstrate a novel technique exploiting water's large coefficient of thermal expansion, wherein modest thermal gradients produce the requisite high pressure for driving fast-flowing liquid water microjets, which can effect the direct conversion of the kinetic energy into electricity and gaseous hydrogen. Waste heat in thermoelectric generating plants and combustion engines, as well as solar and geothermal energy could be used to drive these systems.

  15. Measuring Low Concentrations of Liquid Water in Soil

    NASA Technical Reports Server (NTRS)

    Buehler, Martin

    2009-01-01

    An apparatus has been developed for measuring the low concentrations of liquid water and ice in relatively dry soil samples. Designed as a prototype of instruments for measuring the liquidwater and ice contents of Lunar and Martian soils, the apparatus could also be applied similarly to terrestrial desert soils and sands. The apparatus is a special-purpose impedance spectrometer: Its design is based on the fact that the electrical behavior of a typical soil sample is well approximated by a network of resistors and capacitors in which resistances decrease and capacitances increase (and, hence, the magnitude of impedance decreases) with increasing water content.

  16. Rapid screening of water soluble arsenic species in edible oils using dispersive liquid-liquid microextraction.

    PubMed

    López-García, Ignacio; Briceño, Marisol; Vicente-Martínez, Yesica; Hernández-Córdoba, Manuel

    2015-01-15

    A methodology for the non-chromatographic screening of the main arsenic species present in edible oils is discussed. Reverse dispersive liquid-liquid microextraction was used to extract water soluble arsenic compounds (inorganic arsenic, methylarsonate, dimethylarsinate and arsenobetaine) from the edible oils into a slightly acidic aqueous medium. The total arsenic content was measured in the extracts by electrothermal atomic absorption spectrometry using palladium as the chemical modifier. By repeating the measurement using cerium instead of palladium, the sum of inorganic arsenic and methylarsonate was obtained. The detection limit was 0.03 ng As per gram of oil. Data for the total and water-soluble arsenic levels of 29 samples of different origin are presented. Inorganic arsenic was not found in any of the samples marketed as edible oils.

  17. Liquid water can slip on a hydrophilic surface

    PubMed Central

    Ho, Tuan Anh; Papavassiliou, Dimitrios V.; Lee, Lloyd L.; Striolo, Alberto

    2011-01-01

    Understanding and predicting the behavior of water, especially in contact with various surfaces, is a scientific challenge. Molecular-level understanding of hydrophobic effects and their macroscopic consequences, in particular, is critical to many applications. Macroscopically, a surface is classified as hydrophilic or hydrophobic depending on the contact angle formed by a water droplet. Because hydrophobic surfaces tend to cause water slip whereas hydrophilic ones do not, the former surfaces can yield self-cleaning garments and ice-repellent materials whereas the latter cannot. The results presented herein suggest that this dichotomy might be purely coincidental. Our simulation results demonstrate that hydrophilic surfaces can show features typically associated with hydrophobicity, namely liquid water slip. Further analysis provides details on the molecular mechanism responsible for this surprising result. PMID:21911406

  18. Temperature dependence of the structure of protein hydration water and the liquid-liquid transition.

    PubMed

    Accordino, S R; Malaspina, D C; Rodriguez Fris, J A; Alarcón, L M; Appignanesi, G A

    2012-03-01

    We study the temperature dependence of the structure and orientation of the first hydration layers of the protein lysozyme and compare it with the situation for a model homogeneous hydrophobic surface, a graphene sheet. We show that in both cases these layers are significantly better structured than bulk water. The geometrical constraint of the interface makes the water molecules adjacent to the surface lose one water-water hydrogen bond and expel the fourth neighbors away from the surface, lowering local density. We show that a decrease in temperature improves the ordering of the hydration water molecules, preserving such a geometrical effect. For the case of graphene, this favors an ice Ih-like local structuring, similar to the water-air interface but in the opposite way along the c axis of the basal plane (while the vicinal water molecules of the air interface orient a hydrogen atom toward the surface, the oxygens of the water molecules close to the graphene plane orient a lone pair in such a direction). In turn, the case of the first hydration layers of the lysozyme molecule is shown to be more complicated, but still displaying signs of both kinds of behavior, together with a tendency of the proximal water molecules to hydrogen bond to the protein both as donors and as acceptors. Additionally, we make evident the existence of signatures of a liquid-liquid transition (Widom line crossing) in different structural parameters at the temperature corresponding to the dynamic transition incorrectly referred to as "the protein glass transition."

  19. Comparative In Vitro Toxicity Profile of Electronic and Tobacco Cigarettes, Smokeless Tobacco and Nicotine Replacement Therapy Products: E-Liquids, Extracts and Collected Aerosols

    PubMed Central

    Misra, Manoj; Leverette, Robert D.; Cooper, Bethany T.; Bennett, Melanee B.; Brown, Steven E.

    2014-01-01

    The use of electronic cigarettes (e-cigs) continues to increase worldwide in parallel with accumulating information on their potential toxicity and safety. In this study, an in vitro battery of established assays was used to examine the cytotoxicity, mutagenicity, genotoxicity and inflammatory responses of certain commercial e-cigs and compared to tobacco burning cigarettes, smokeless tobacco (SLT) products and a nicotine replacement therapy (NRT) product. The toxicity evaluation was performed on e-liquids and pad-collected aerosols of e-cigs, pad-collected smoke condensates of tobacco cigarettes and extracts of SLT and NRT products. In all assays, exposures with e-cig liquids and collected aerosols, at the doses tested, showed no significant activity when compared to tobacco burning cigarettes. Results for the e-cigs, with and without nicotine in two evaluated flavor variants, were very similar in all assays, indicating that the presence of nicotine and flavors, at the levels tested, did not induce any cytotoxic, genotoxic or inflammatory effects. The present findings indicate that neither the e-cig liquids and collected aerosols, nor the extracts of the SLT and NRT products produce any meaningful toxic effects in four widely-applied in vitro test systems, in which the conventional cigarette smoke preparations, at comparable exposures, are markedly cytotoxic and genotoxic. PMID:25361047

  20. Comparative in vitro toxicity profile of electronic and tobacco cigarettes, smokeless tobacco and nicotine replacement therapy products: e-liquids, extracts and collected aerosols.

    PubMed

    Misra, Manoj; Leverette, Robert D; Cooper, Bethany T; Bennett, Melanee B; Brown, Steven E

    2014-10-30

    The use of electronic cigarettes (e-cigs) continues to increase worldwide in parallel with accumulating information on their potential toxicity and safety. In this study, an in vitro battery of established assays was used to examine the cytotoxicity, mutagenicity, genotoxicity and inflammatory responses of certain commercial e-cigs and compared to tobacco burning cigarettes, smokeless tobacco (SLT) products and a nicotine replacement therapy (NRT) product. The toxicity evaluation was performed on e-liquids and pad-collected aerosols of e-cigs, pad-collected smoke condensates of tobacco cigarettes and extracts of SLT and NRT products. In all assays, exposures with e-cig liquids and collected aerosols, at the doses tested, showed no significant activity when compared to tobacco burning cigarettes. Results for the e-cigs, with and without nicotine in two evaluated flavor variants, were very similar in all assays, indicating that the presence of nicotine and flavors, at the levels tested, did not induce any cytotoxic, genotoxic or inflammatory effects. The present findings indicate that neither the e-cig liquids and collected aerosols, nor the extracts of the SLT and NRT products produce any meaningful toxic effects in four widely-applied in vitro test systems, in which the conventional cigarette smoke preparations, at comparable exposures, are markedly cytotoxic and genotoxic.

  1. 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

  2. Physico-chemical qualification of a universal portable sampler for aerosols and water-soluble gases

    NASA Astrophysics Data System (ADS)

    Roux, Jean-Maxime; Sarda-Estève, Roland

    2015-10-01

    Developing a universal portable air sampler based on electrostatic precipitation. The challenge is to collect micro and nanoparticles, microorganisms as well as toxic molecules with a portable device. Electrostatic precipitation is an efficient and gentle method to collect airborne microorganisms and preserve their cultivability. But the collection of toxic gases required is not possible in such a device. The collection of such gases requires a liquid into which they have to be solubilized. Two concepts are being evaluated. The first one is based on electrospray. The goal is to investigate the collection efficiency of water-soluble gases. The second concept is based on the semi-humid electrostatic precipitator. Their high collection efficiencies for particles were already demonstrated. In the present study they are both tested with water-soluble gases. Concentrations are measured in the liquid solution by Ion Chromatography and in the gas phase by Proton Transfer Reaction Mass Spectrometry.

  3. Extraction of pesticides in water samples using vortex-assisted liquid-liquid microextraction.

    PubMed

    Jia, Chunhong; Zhu, Xiaodan; Wang, Jihua; Zhao, Ercheng; He, Min; Chen, Li; Yu, Pingzhong

    2010-09-10

    A simple solvent microextraction method termed vortex-assisted liquid-liquid microextraction (VALLME) coupled with gas chromatography micro electron-capture detector (GC-microECD) has been developed and used for the pesticide residue analysis in water samples. In the VALLME method, aliquots of 30 microL toluene used as extraction solvent were directly injected into a 25 mL volumetric flask containing the water sample. The extraction solvent was dispersed into the water phase under vigorously shaking with the vortex. The parameters affecting the extraction efficiency of the proposed VALLME such as extraction solvent, vortex time, volumes of extraction solvent and salt addition were investigated. Under the optimum condition, enrichment factors (EFs) in a range of 835-1115 and limits of detection below 0.010 microg L(-1) were obtained for the determination of target pesticides in water. The calculated calibration curves provide high levels of linearity yielding correlation coefficients (r(2)) greater than 0.9958 with the concentration level ranged from 0.05 to 2.5 microg L(-1). Finally, the proposed method has been successfully applied to the determination of pesticides from real water samples and acceptable recoveries over the range of 72-106.3% were obtained.

  4. A Study of Aerosol Effect on Marine Water Clouds with Long-term Satellite Climate Data Records

    NASA Astrophysics Data System (ADS)

    Zhao, X.; Heidinger, A. K.; Walther, A.

    2015-12-01

    Cloud microphysical structures and properties provide a critical link between the energy and hydrological cycles of Earth's climate system. A change of cloud microphysical properties related to anthropogenic activities may result in distressing climate consequence and changes. Since atmospheric aerosol is the major source of cloud condensation nuclei (CNN) that is critical for the formation of cloud microphysical structures and properties, aerosol changes due to anthropogenic emissions will result in the modification of CCN and cloud microphysical properties and eventually cause the changes of Earth's climate. In this study, we will investigate the effect of aerosol on the microphysical properties, including cloud particle effective radius, cloud water path, and cloud optical depth, of marine stratus clouds by using more than 30-years climate data records (CDRs) of aerosols and clouds derived from NOAA operational AVHRR satellite observations. The correlation between satellite derived cloud and aerosol microphysical parameters will be determined and the statistics significance will be examined using the long-term AVHRR satellite CDRs.

  5. High performance liquid chromatography-charged aerosol detection applying an inverse gradient for quantification of rhamnolipid biosurfactants.

    PubMed

    Behrens, Beate; Baune, Matthias; Jungkeit, Janek; Tiso, Till; Blank, Lars M; Hayen, Heiko

    2016-07-15

    A method using high performance liquid chromatography coupled to charged-aerosol detection (HPLC-CAD) was developed for the quantification of rhamnolipid biosurfactants. Qualitative sample composition was determined by liquid chromatography coupled to tandem mass spectrometry (LC-MS/MS). The relative quantification of different derivatives of rhamnolipids including di-rhamnolipids, mono-rhamnolipids, and their precursors 3-(3-hydroxyalkanoyloxy)alkanoic acids (HAAs) differed for two compared LC-MS instruments and revealed instrument dependent responses. Our here reported HPLC-CAD method provides uniform response. An inverse gradient was applied for the absolute quantification of rhamnolipid congeners to account for the detector's dependency on the solvent composition. The CAD produces a uniform response not only for the analytes but also for structurally different (nonvolatile) compounds. It was demonstrated that n-dodecyl-β-d-maltoside or deoxycholic acid can be used as alternative standards. The method of HPLC-ultra violet (UV) detection after a derivatization of rhamnolipids and HAAs to their corresponding phenacyl esters confirmed the obtained results but required additional, laborious sample preparation steps. Sensitivity determined as limit of detection and limit of quantification for four mono-rhamnolipids was in the range of 0.3-1.0 and 1.2-2.0μg/mL, respectively, for HPLC-CAD and 0.4 and 1.5μg/mL, respectively, for HPLC-UV. Linearity for HPLC-CAD was at least 0.996 (R(2)) in the calibrated range of about 1-200μg/mL. Hence, the here presented HPLC-CAD method allows absolute quantification of rhamnolipids and derivatives.

  6. LASE measurements of water vapor and aerosol profiles during the Plains Elevated Convection at Night (PECAN) field experiment

    NASA Astrophysics Data System (ADS)

    Nehrir, A. R.; Ferrare, R. A.; Kooi, S. A.; Butler, C. F.; Notari, A.; Hair, J. W.; Collins, J. E., Jr.; Ismail, S.

    2015-12-01

    The Lidar Atmospheric Sensing Experiment (LASE) system was deployed on the NASA DC-8 aircraft during the Plains Elevated Convection At Night (PECAN) field experiment, which was conducted during June-July 2015 over the central and southern plains. LASE is an active remote sensor that employs the differential absorption lidar (DIAL) technique to measure range resolved profiles of water vapor and aerosols above and below the aircraft. The DC-8 conducted nine local science flights from June 30- July 14 where LASE sampled water vapor and aerosol fields in support of the PECAN primary science objectives relating to better understanding nocturnal Mesoscale Convective Systems (MCSs), Convective Initiation (CI), the Low Level Jet (LLJ), bores, and to compare different airborne and ground based measurements. LASE observed large spatial and temporal variability in water vapor and aerosol distributions in advance of nocturnal MCSs, across bores resulting from MCS outflow boundaries, and across the LLJ associated with the development of MCSs and CI. An overview of the LASE data collected during the PECAN field experiment will be presented where emphasis will be placed on variability of water vapor profiles in the vicinity of severe storms and intense convection in the central and southern plains. Preliminary comparisons show good agreement between coincident LASE and radiosonde water vapor profiles. In addition, an advanced water vapor DIAL system being developed at NASA Langley will be discussed.

  7. Measuring ice and liquid water content in moderately supercooled clouds with Cloudnet

    NASA Astrophysics Data System (ADS)

    Bühl, Johannes; Seifert, Patric; Myagkov, Alexander; Albert, Ansmann

    2016-04-01

    The interaction between ice nuclei and clouds is an important topic in weather and climate research. Recent laboratory experiments and field in-situ field campaigns present more and more detailed measurements of ice nucleating particles (INP) at temperatures close to 0°C. This brings moderately supercooled mixed-phase clouds into the focus of current cloud research. One current example is the European Union BACCHUS project. A major goal of BACCHUS is the analysis of the anthropogenic impact on ice nucleation. Within this project, we use the Leipzig Aerosol Cloud Remote Observations System (LACROS) and the Cloudnet framework in order to get quantitative insight into the formation of ice in mixed-phase layered clouds with cloud top temperature (CTT) from -40 to 0°C. Depolarization measurements from lidar and radar show a clear dependence between particle shape and the temperature under which the particles have been formed. The special focus of this work is on the CTT range from -10 to 0°C. An algorithm is presented to decide between ice and liquid water precipitation falling from the clouds showing that between 10% and 30% of all layered clouds show ice precipitation with CTT between -5 and 0°C. For these slightly supercooled clouds an average ice-water-content between 10e-7 and 10e-8 [kg per cubic meter] is found.

  8. Surface fractal dimension, water adsorption efficiency, and cloud nucleation activity of insoluble aerosol

    PubMed Central

    Laaksonen, Ari; Malila, Jussi; Nenes, Athanasios; Hung, Hui-Ming; Chen, Jen-Ping

    2016-01-01

    Surface porosity affects the ability of a substance to adsorb gases. The surface fractal dimension D is a measure that indicates the amount that a surface fills a space, and can thereby be used to characterize the surface porosity. Here we propose a new method for determining D, based on measuring both the water vapour adsorption isotherm of a given substance, and its ability to act as a cloud condensation nucleus when introduced to humidified air in aerosol form. We show that our method agrees well with previous methods based on measurement of nitrogen adsorption. Besides proving the usefulness of the new method for general surface characterization of materials, our results show that the surface fractal dimension is an important determinant in cloud drop formation on water insoluble particles. We suggest that a closure can be obtained between experimental critical supersaturation for cloud drop activation and that calculated based on water adsorption data, if the latter is corrected using the surface fractal dimension of the insoluble cloud nucleus. PMID:27138171

  9. Heterogeneous Chemistry of HONO on Liquid Sulfuric Acid: A New Mechanism of Chlorine Activation on Stratospheric Sulfate Aerosols

    NASA Technical Reports Server (NTRS)

    Zhang, Renyi; Leu, Ming-Taun; Keyser, Leon F.

    1996-01-01

    Heterogeneous chemistry of nitrous acid (HONO) on liquid sulfuric acid (H2SO4) Was investigated at conditions that prevail in the stratosphere. The measured uptake coefficient (gamma) of HONO on H2SO4 increased with increasing acid content, ranging from 0.03 for 65 wt % to about 0.1 for 74 wt %. In the aqueous phase, HONO underwent irreversible reaction with H2SO4 to form nitrosylsulfuric acid (NO(+)HSO4(-). At temperatures below 230 K, NO(+)HSO4(-) was observed to be stable and accumulated in concentrated solutions (less than 70 wt % H2SO4) but was unstable and quickly regenerated HONO in dilute solutions (less than 70 wt %). HCl reacted with HONO dissolved in sulfuric acid, releasing gaseous nitrosyl chloride (ClNO). The reaction probability between HCl and HONO varied from 0.01 to 0.02 for 60-72 wt % H2SO4. In the stratosphere, ClNO photodissociates rapidly to yield atomic chlorine, which catalytically destroys ozone. Analysis of the laboratory data reveals that the reaction of HCl with HONO on sulfate aerosols can affect stratospheric ozone balance during elevated sulfuric acid loadings after volcanic eruptions or due to emissions from the projected high-speed civil transport (HSCT). The present results may have important implications on the assessment of environmental acceptability of HSCT.

  10. Prediction of activity coefficients in liquid aerosol particles containing organic compounds, dissolved inorganic salts, and water—Part 2: Consideration of phase separation effects by an X-UNIFAC model

    NASA Astrophysics Data System (ADS)

    Chang, Elsa I.; Pankow, James F.

    A thermodynamic model is presented for predicting the formation of particulate matter (PM) within an aerosol that contains organic compounds, inorganic salts, and water. Neutral components are allowed to partition from the gas phase to the PM, with the latter potentially composed of both a primarily aqueous ( α) liquid phase and a primarily organic ( β) liquid phase. Partitioning is allowed to occur without any artificial restraints: when both α and β PM phases are present, ionic constituents are allowed to partition to both. X-UNIFAC.2, an extended UNIFAC method based on Yan et al. (1999. Prediction of vapor-liquid equilibria in mixed-solvent electrolyte systems using the group contribution concept. Fluid Phase Equilibria 162, 97-113), was developed for activity coefficient estimation. X-UNIFAC.2 utilizes the standard UNIFAC terms, a Debye-Hückel term, and a virial equation term that represents the middle-range (MR) contribution to activity coefficient effects. A large number (234) of MR parameters are already available from Yan et al. (1999). Six additional MR parameters were optimized here to enable X-UNIFAC.2 to account for interactions between the carboxylic acid group and Na +, Cl -, and Ca 2+. Predictions of PM formation were made for a hypothetical sabinene/O 3 system with varying amounts of NaCl in the PM. Predictions were also made for the chamber experiments with α-pinene/O 3 (and CaCl 2 seed) carried out by Cocker et al. (2001. The effect of water on gas-particle partitioning of secondary organic aerosol. Part I. α-pinene/ozone system. Atmospheric Environment 35, 6049-6072); good agreement between the predicted and chamber-measured PM mass concentrations was achieved.

  11. Ab initio liquid water from PBE0 hybrid functional simulations

    NASA Astrophysics Data System (ADS)

    Li, Zhaofeng; Wu, Xifan; Car, Roberto

    2010-03-01

    For reasons of computational efficiency, so far most ab initio molecular dynamics simulations of liquid water have been based on semi-local density functional approximations, such as PBE and BLYP. These approaches yield a liquid structure that, albeit qualitatively correct, is overstructured compared to experiment, even after nuclear quantum effects have been taken into account.footnotetextJ. A. Morrone and R. Car, Phys. Rev. Lett. 101, 017801(2008) A major cause of this inaccuracy is the delocalization error associated to semi-local density functional approximations, which, as a consequence, overestimate slightly the hydrogen bond strength in the liquid. In this work we adopt the PBE0 hybrid functional approximation, which, by mixing a fraction of exact (Hartree-Fock) exchange, reduces significantly the delocalization error of semi-local functionals. Our approach is based on a numerically efficient order-N implementation of exact exchange.footnotetextX. Wu, A. Selloni, and R. Car, Phys. Rev. B 79, 085102(2009) We find that PBE0 systematically improves the agreement of the simulated liquid with experiment. Our conclusion is substantiated by the calculated radial distribution functions, H-bond statistics, and molecular dipole distribution.

  12. IR and Raman spectra of liquid water: theory and interpretation.

    PubMed

    Auer, B M; Skinner, J L

    2008-06-14

    IR and Raman (parallel- and perpendicular-polarized) spectra in the OH stretch region for liquid water were measured some years ago, but their interpretation is still controversial. In part, this is because theoretical calculation of such spectra for a neat liquid presents a formidable challenge due to the coupling between vibrational chromophores and the effects of motional narrowing. Recently we proposed an electronic structure/molecular dynamics method for calculating spectra of dilute HOD in liquid D(2)O, which relied on ab initio calculations on clusters to provide a map from nuclear coordinates of the molecules in the liquid to OH stretch frequencies, transition dipoles, and polarizabilities. Here we extend this approach to the calculation of couplings between chromophores. From the trajectories of the fluctuating local-mode frequencies, transition moments, and couplings, we use our recently developed time-averaging approximation to calculate the line shapes. Our results are in good agreement with experiment for the IR and Raman line shapes, and capture the significant differences among them. Our analysis shows that while the coupling between chromophores is relatively modest, it nevertheless produces delocalization of the vibrational eigenstates over up to 12 chromophores, which has a profound effect on the spectroscopy. In particular, our results demonstrate that the peak in the parallel-polarized Raman spectrum at about 3250 wavenumbers is collective in nature.

  13. Tuning the Liquid-Liquid Transition by Modulating the Hydrogen-Bond Angular Flexibility in a Model for Water

    NASA Astrophysics Data System (ADS)

    Smallenburg, Frank; Sciortino, Francesco

    2015-07-01

    We propose a simple extension of the well known ST2 model for water [F. H. Stillinger and A. Rahman, J. Chem. Phys. 60, 1545 (1974)] that allows for a continuous modification of the hydrogen-bond angular flexibility. We show that the bond flexibility affects the relative thermodynamic stability of the liquid and of the hexagonal (or cubic) ice. On increasing the flexibility, the liquid-liquid critical point, which in the original ST2 model is located in the no-man's land (i.e., the region where ice is the thermodynamically stable phase) progressively moves to a temperature where the liquid is more stable than ice. Our study definitively proves that the liquid-liquid transition in the ST2 model is a genuine phenomenon, of high relevance in all tetrahedral network-forming liquids, including water.

  14. Liquid water simulations with the density fragment interaction approach.

    PubMed

    Hu, Xiangqian; Jin, Yingdi; Zeng, Xiancheng; Hu, Hao; Yang, Weitao

    2012-06-07

    We reformulate the density fragment interaction (DFI) approach [Fujimoto and Yang, J. Chem. Phys., 2008, 129, 054102.] to achieve linear-scaling quantum mechanical calculations for large molecular systems. Two key approximations are developed to improve the efficiency of the DFI approach and thus enable the calculations for large molecules: the electrostatic interactions between fragments are computed efficiently by means of polarizable electrostatic-potential-fitted atomic charges; and frozen fragment pseudopotentials, similar to the effective fragment potentials that can be fitted from interactions between small molecules, are employed to take into account the Pauli repulsion effect among fragments. Our reformulated and parallelized DFI method demonstrates excellent parallel performance based on the benchmarks for the system of 256 water molecules. Molecular dynamics simulations for the structural properties of liquid water also show a qualitatively good agreement with experimental measurements including the heat capacity, binding energy per water molecule, and the radial distribution functions of atomic pairs of O-O, O-H, and H-H. With this approach, large-scale quantum mechanical simulations for water and other liquids become feasible.

  15. Characterization of Chromophoric Water-Soluble Organic Matter in Urban, Forest, and Marine Aerosols by HR-ToF-AMS Analysis and Excitation-Emission Matrix Spectroscopy.

    PubMed

    Chen, Qingcai; Miyazaki, Yuzo; Kawamura, Kimitaka; Matsumoto, Kiyoshi; Coburn, Sean; Volkamer, Rainer; Iwamoto, Yoko; Kagami, Sara; Deng, Yange; Ogawa, Shuhei; Ramasamy, Sathiyamurthi; Kato, Shungo; Ida, Akira; Kajii, Yoshizumi; Mochida, Michihiro

    2016-10-04

    Chromophoric water-soluble organic matter in atmospheric aerosols potentially plays an important role in aqueous reactions and light absorption by organics. The fluorescence and chemical-structural characteristics of the chromophoric water-soluble organic matter in submicron aerosols collected in urban, forest, and marine environments (Nagoya, Kii Peninsula, and the tropical Eastern Pacific) were investigated using excitation-emission matrices (EEMs) and a high-resolution aerosol mass spectrometer. A total of three types of water-soluble chromophores, two with fluorescence characteristics similar to those of humiclike substances (HULIS-1 and HULIS-2) and one with fluorescence characteristics similar to those of protein compounds (PLOM), were identified in atmospheric aerosols by parallel factor analysis (PARAFAC) for EEMs. We found that the chromophore components of HULIS-1 and -2 were associated with highly and less-oxygenated structures, respectively, which may provide a clue to understanding the chemical formation or loss of organic chromophores in atmospheric aerosols. Whereas HULIS-1 was ubiquitous in water-soluble chromophores over different environments, HULIS-2 was abundant only in terrestrial aerosols, and PLOM was abundant in marine aerosols. These findings are useful for further studies regarding the classification and source identification of chromophores in atmospheric aerosols.

  16. Aerosol-cloud interactions in the ECHAM6-HAM2 GCM and Aerosol_cci/Cloud_cci satellite products

    NASA Astrophysics Data System (ADS)

    Neubauer, David; Lohmann, Ulrike

    2015-04-01

    The first indirect aerosol effect or cloud albedo effect can be estimated as a radiative forcing. While the sign of this forcing is agreed to be negative, model-based estimates of its magnitude show a large variability. The responses of cloud liquid water content and cloud cover to aerosol increases also referred to as secondary indirect aerosol effects or fast adjustments are uncertain as well. In studies that use the variability in the present day satellite data to infer aerosol-cloud interactions (ACI), or that constrain model parameterizations to better agree with satellite observations a less negative ACI radiative forcing is found. The projects of the Climate Change Initiative (CCI) programme of ESA aim at producing long time series of satellite data of essential climate variables with specific information on errors and uncertainties. The quantification of uncertainty in satellite retrievals provides an opportunity to get insights in the discrepancy between model based and satellite based estimates of ACI. Within the Aerosol_cci project susceptibilities of cloud properties from Cloud_cci to aerosol properties from Aerosol_cci datasets are to be compared to susceptibilities from the aerosol climate model ECHAM6-HAM2. Particularly interesting relationships for the first indirect aerosol effect and the second aerosol indirect effect will be investigated. Satellite studies show a strong effect of aerosol on cloud amount, which could be a methodological artefact such as aerosol swelling or meteorological covariation. The immediate vicinity of clouds needs to be excluded due to these potential cloud contaminations although it would be the most interesting region for associations between aerosol and clouds. As the resolution of the data can have an impact on statistical correlations between cloud and aerosol properties, the assessment will be done on different scales. First results will be presented at the conference.

  17. One-dimensional model for water and aqueous solutions. I. Pure liquid water

    NASA Astrophysics Data System (ADS)

    Ben-Naim, Arieh

    2008-01-01

    Two simplified one-dimensional models for waterlike particles are studied. One is referred to as the primitive model which is a simplified version of a model introduced by Ben-Naim in 1992 [Statistical Thermodynamics for Chemists and Biochemists (Plenum, New York, 1992)]. The second, referred to as the primitive cluster model, is a simplified version of the model used by Lovett and Ben-Naim in 1969 [J. Chem. Phys. 51, 3108 (1969)]. The two models are shown to be nearly equivalent and both exhibit some of the most characteristic behavior of liquid water. It is argued that a key feature of the molecular interactions—the correlation between the strong binding energy and low local density—is essential for the manifestation of the anomalous behavior of liquid water. It is also essential for the understanding of the outstanding behavior of liquid water.

  18. Selective extraction of emerging contaminants from water samples by dispersive liquid-liquid microextraction using functionalized ionic liquids.

    PubMed

    Yao, Cong; Li, Tianhao; Twu, Pamela; Pitner, William R; Anderson, Jared L

    2011-03-25

    Functionalized ionic liquids containing the tris(pentafluoroethyl)trifluorophosphate (FAP) anion were used as extraction solvents in dispersive liquid-liquid microextraction (DLLME) for the extraction of 14 emerging contaminants from water samples. The extraction efficiencies and selectivities were compared to those of an in situ IL DLLME method which uses an in situ metathesis reaction to exchange 1-butyl-3-methylimidazolium chloride (BMIM-Cl) to 1-butyl-3-methylimidazolium bis[(trifluoromethyl)sulfonyl]imide (BMIM-NTf(2)). Compounds containing tertiary amine functionality were extracted with high selectivity and sensitivity by the 1-(6-amino-hexyl)-1-methylpyrrolidinium tris(pentafluoroethyl)trifluorophosphate (HNH(2)MPL-FAP) IL compared to other FAP-based ILs and the BMIM-NTf(2) IL. On the other hand, polar or acidic compounds without amine groups exhibited higher enrichment factors using the BMIM-NTf(2) IL. The detection limits for the studied analytes varied from 0.1 to 55.1 μg/L using the traditional IL DLLME method with the HNH(2)MPL-FAP IL as extraction solvent, and from 0.1 to 55.8 μg/L using in situ IL DLLME method with BMIM-Cl+LiNTf(2) as extraction solvent. A 93-fold decrease in the detection limit of caffeine was observed when using the HNH(2)MPL-FAP IL compared to that obtained using in situ IL DLLME method. Real water samples including tap water and creek water were analyzed with both IL DLLME methods and yielded recoveries ranging from 91% to 110%.

  19. Evidence for liquid-phase cirrus cloud formation from volcanic aerosols - Climatic implications

    NASA Technical Reports Server (NTRS)

    Sassen, Kenneth

    1992-01-01

    Supercooled droplets in cirrus uncinus cell heads between -40 and -50 C are identified from the First International Satellite Cloud Climatology Project Regional Experiment polarization lidar measurements. Although short-lived, complexes of these small liquid cells seem to have contributed importantly to the formation of the cirrus. Freezing-point depression effects in solution droplets, apparently resulting from relatively large cloud condensation nuclei of volcanic origin, can be used to explain this rare phenomenon. An unrecognized volcano-cirrus cloud climate feedback mechanism is implied by these findings.

  20. Evidence for liquid-phase cirrus cloud formation from volcanic aerosols: climatic implications.

    PubMed

    Sassen, K

    1992-07-24

    Supercooled droplets in cirrus uncinus cell heads between -40 degrees and -50 degrees C are identified from Project FIRE [First ISCCP (International Satellite Cloud Climatology Project) Regional Experiment] polarization lidar measurements. Although short-lived, complexes of these small liquid cells seem to have contributed importantly to the formation of the cirrus. Freezing-point depression effects in solution droplets, apparently resulting from relatively large cloud condensation nuclei of volcanic origin, can be used to explain this rare phenomenon. An unrecognized volcano-cirrus cloud climate feedback mechanism is implied by these findings.

  1. [The spectra of a laser-produced plasma source with CO2, O2 and CF4 liquid aerosol spray target].

    PubMed

    Ni, Qi-Liang; Chen, Bo

    2008-11-01

    A laser-produced plasma (LPP) source with liquid aerosol spray target and nanosecond laser was developed, based on both soft X-ray radiation metrology and extreme ultraviolet projection lithography (EUVL). The LPP source is composed of a stainless steel solenoid valve whose temperature can be continuously controlled, a Nd : YAG laser with pulse width, working wavelength and pulse energy being 7 ns, 1.064 microm and 1J respectively, and a pulse generator which can synchronously control the valve and the laser. A standard General Valve Corporation series 99 stainless steel solenoid valve with copper gasket seals and a Kel-F poppet are used in order to minimize leakage and poppet deformation during high-pressure cryogenic operation. A close fitting copper cooling jacket surrounds the valve body. The jacket clamps a copper coolant carrying tube 3 mm in diameter, which is fed by an automatically pressurized liquid nitrogen-filled dewar. The valve temperature can be controlled between 77 and 473 K. For sufficiently high backing pressure and low temperature, the valve reservoir gas can undergo a gas-to-liquid phase transition. Upon valve pulsing, the liquid is ejected into a vacuum and breaks up into droplets, which is called liquid aerosol spray target. For the above-mentioned LPP source, firstly, by the use of Cowan program on the basis of non-relativistic quantum mechanics, the authors computed the radiative transition wavelengths and probabilities in soft X-ray region for O4+, O5+, O6+, O7+, F5+, F6+ and F7+ ions which were correspondingly produced from the interaction of the 10(11)-10(12) W x cm(-2) power laser with liquid O2, CO2 and CF4 aerosol spray targets. Secondly, the authors measured the spectra of liquid O2, CO2 and CF4 aerosol spray target LPP sources in the 6-20 nm band for the 8 x 10(11) W x cm(-2) laser irradiance. The measured results were compared with the Cowan calculated results ones, and the radiative transition wavelength and probability for the

  2. A "First Principles" Potential Energy Surface for Liquid Water from VRT Spectroscopy of Water Clusters

    SciTech Connect

    Goldman, N; Leforestier, C; Saykally, R J

    2004-05-25

    We present results of gas phase cluster and liquid water simulations from the recently determined VRT(ASP-W)III water dimer potential energy surface. VRT(ASP-W)III is shown to not only be a model of high ''spectroscopic'' accuracy for the water dimer, but also makes accurate predictions of vibrational ground-state properties for clusters up through the hexamer. Results of ambient liquid water simulations from VRT(ASP-W)III are compared to those from ab initio Molecular Dynamics, other potentials of ''spectroscopic'' accuracy, and to experiment. The results herein represent the first time that a ''spectroscopic'' potential surface is able to correctly model condensed phase properties of water.

  3. Changes in snow cover and water cycle over the Tibetan plateau induced by absorbing aerosols

    NASA Astrophysics Data System (ADS)

    Lau, W. K.; Kim, M.; Kim, K.; Lee, W.

    2009-12-01

    The warming of the land surface and retreating glacier and snowpack in Hindu-Kush-Himalayas-Tibet (HKHT) are well known observations often attributed to effect of greenhouse warming. In this study, based on numerical experiments with the NASA fvGCM, we find that the elevated -heat-pump (EHP) effect by absorbing aerosols (dust and black carbon) over the Indo-Gangetic Plain and Himalayas foothills can lead to substantial warming of the atmosphere and land surface, and reduction in snow cover over the HKHT region . Atmosphere and surface energy analyses show that beginning in April, the middle atmosphere, near the high-altitude surface over the Tibetan Plateau, heats up due to absorption of solar radiation by black carbon and dust. The near surface heating increases convection, which spreads the warming to the upper troposphere over the Plateau. As the monsoon season approaches in May, the increased convection draws in warmer and moister monsoon air into the HKHT, which further enhances the convection, cloudiness and precipitation over the region in late May and early June. The moister and warmer atmosphere over the HKHT region suppresses evaporation and sensible heat fluxes from the surface during April-May. The excess heat received by the surface goes into melting of the snowpack, exposing more of the bare land. The exposed land surface leads to further increase in land surface temperature over the HKHT. Results show that most of the snow melt occurs in the western region (west of 90E) in April and May, when black carbon aerosol loading in the atmosphere is highest, and dust loading is on the rise. The equivalent surface albedo change due to snow melt is reduced by about 8-10%, and 4-6% over the western and eastern TP respectively. The proposed mechanism appear to be relevant on interannnual time scales and beyond. The consequence of these changes in HKHT on the water cycle of Asia will be discussed.

  4. Remote Sensing of Cloud, Aerosol, and Water Vapor Properties from MODIS

    NASA Technical Reports Server (NTRS)

    King, Michael D.; Platnick, Steven; Menzel, W. Paul; Kaufman, Yoram J.; Ackerman, Steven A.; Tanre, Didier; Gao, Bo-Cai

    2001-01-01

    MODIS is an earth-viewing cross-track scanning spectroradiometer launched on the Terra satellite in December 1999. MODIS scans a swath width sufficient to provide nearly complete global coverage every two days from a polar orbiting, sun-synchronous, platform at an altitude of 705 kilometers, and provides images in 36 spectral bands between 0.415 and 14.235 micrometers with spatial resolutions of 250 meters (2 bands), 500 meters (5 bands) and 1000 meters (29 bands). These bands have been carefully selected to enable advanced studies of land, ocean, and atmospheric processes. In this presentation we review the comprehensive set of remote sensing algorithms that have been developed for the remote sensing of atmospheric properties using MODIS data, placing primary emphasis on the principal atmospheric applications of (i) developing a cloud mask for distinguishing clear sky from clouds, (ii) retrieving global cloud radiative and microphysical properties, including cloud top pressure and temperature, effective emissivity, cloud optical thickness, thermodynamic phase, and effective radius, (iii) monitoring tropospheric aerosol optical thickness over the land and ocean and aerosol size distribution over the ocean, (iv) determining atmospheric profiles of moisture and temperature, and (v) estimating column water amount. The physical principles behind the determination of each of these atmospheric products will be described, together with an example of their application using MODIS observations. All products are archived into two categories: pixel-level retrievals (referred to as Level-2 products) and global gridded products at a latitude and longitude resolution of 1 degree (Level-3 products). An overview of the MODIS atmosphere algorithms and products, status, validation activities, and early level-2 and -3 results will be presented.

  5. Radiative Importance of Aerosol-Cloud Interaction

    NASA Technical Reports Server (NTRS)

    Tsay, Si-Chee

    1999-01-01

    Aerosol particles are input into the troposphere by biomass burning, among other sources. These aerosol palls cover large expanses of the earth's surface. Aerosols may directly scatter solar radiation back to space, thus increasing the earth's albedo and act to cool the earth's surface and atmosphere. Aerosols also contribute to the earth's energy balance indirectly. Hygroscopic aerosol act as cloud condensation nuclei (CCN) and thus affects cloud properties. In 1977, Twomey theorized that additional available CCN would create smaller but more numerous cloud droplets in a cloud with a given amount of liquid water. This in turn would increase the cloud albedo which would scatter additional radiation back to space and create a similar cooling pattern as the direct aerosol effect. Estimates of the magnitude of the aerosol indirect effect on a global scale range from 0.0 to -4.8 W/sq m. Thus the indirect effect can be of comparable magnitude and opposite in sign to the estimates of global greenhouse gas forcing Aerosol-cloud interaction is not a one-way process. Just as aerosols have an influence on clouds through the cloud microphysics, clouds have an influence on aerosols. Cloud droplets are solutions of liquid water and CCN, now dissolved. When the cloud droplet evaporates it leaves behind an aerosol particle. This new particle does not have to have the same properties as the original CCN. In fact, studies show that aerosol particles that result from cloud processing are larger in size than the original CCN. Optical properties of aerosol particles are dependent on the size of the particles. Larger particles have a smaller backscattering fraction, and thus less incoming solar radiation will be backscattered to space if the aerosol particles are larger. Therefore, we see that aerosols and clouds modify each other to influence the radiative balance of the earth. Understanding and quantifying the spatial and seasonal patterns of the aerosol indirect forcing may have

  6. Liquid-liquid coexistence and crystallization in supercooled ST2 water

    NASA Astrophysics Data System (ADS)

    Martelli, Fausto; Palmer, Jeremy; Debenedetti, Pablo; Car, Roberto

    2014-03-01

    We have computed the free energy landscape of ST2 water in the supercooled regime (228.6 K and 2.4 kbar) using several state-of-the-art computational techniques, including umbrella sampling and metadynamics. Such results conclusively demonstrate coexistence between two liquid phases, a high-density liquid (HDL) and a low-density liquid (HDL), which are metastable with respect to cubic ice. We show that the three phases have distinct structural features characterized by the local structure index and ring statistics. We also find that ice nucleation, should it occur, does so from the low-density liquid. Interestingly, we find that the number of 6-member rings increases monotonically along the path from HDL to LDL, while non-monotonic behavior is observed near the saddle point along the LDL-ice Ic path. This behavior indicates a complex re-arrangement of the H-bond network, followed by progressive crystallization. DOE: DE-SC0008626 (F. M. and R.C.)

  7. Shock wave initiated by an ion passing through liquid water

    NASA Astrophysics Data System (ADS)

    Surdutovich, Eugene; Solov'Yov, Andrey V.

    2010-11-01

    We investigate the shock wave produced by an energetic ion in liquid water. This wave is initiated by a rapid energy loss when the ion moves through the Bragg peak. The energy is transferred from the ion to secondary electrons, which then transfer it to the water molecules. The pressure in the overheated water increases by several orders of magnitude and drives a cylindrical shock wave on a nanometer scale. This wave eventually weakens as the front expands further; but before that, it may contribute to DNA damage due to large pressure gradients developed within a few nanometers from the ion’s trajectory. This mechanism of DNA damage may be a very important contribution to the direct chemical effects of low-energy electrons and holes.

  8. Development of a liquid-fed water resistojet

    NASA Technical Reports Server (NTRS)

    Morren, W. Earl; Stone, James R.

    1988-01-01

    A concept for a forced-flow once-through water vaporizer for application to resistojet thrusters was evaluated as an element of a laboratory model thruster and tested to investigate its operating characteristics. The vaporizer design concept employs flow swirling to attach the liquid flow to the boiler chamber wall, providing for separation of the two liquid phases. This vaporizer was modified with a nozzle and a centrally-located heater to facilitate vaporization, superheating, and expansion of the propellant, allowing it to function as a resistojet. Performance was measured at thrust levels ranging from 170 to 360 mN and at power levels ranging from 443 to 192 W. Maximum measured specific impulse was 192 sec.

  9. Thermodynamic properties of liquid water from a polarizable intermolecular potential.

    PubMed

    Yigzawe, Tesfaye M; Sadus, Richard J

    2013-01-28

    Molecular dynamics simulation results are reported for the pressure, isothermal pressure coefficient, thermal expansion coefficient, isothermal and adiabatic compressibilities, isobaric and isochoric heat capacities, Joule-Thomson coefficient and speed of sound of liquid water using a polarizable potential [Li et al., J. Chem. Phys. 127, 154509 (2007)]. These properties were obtained for a wide range of temperatures and pressures at a common liquid density using the treatment of Lustig [J. Chem. Phys. 100, 3048 (1994)] and Meier and Kabelac [J. Chem. Phys. 124, 064104 (2006)], whereby thermodynamic state variables are expressible in terms of phase-space functions determined directly from molecular dynamics simulations. Comparison with experimental data indicates that the polarizable potential can be used to predict most thermodynamic properties with a very good degree of accuracy.

  10. Size-Resolved Photoelectron Anisotropy of Gas Phase Water Clusters and Predictions for Liquid Water

    NASA Astrophysics Data System (ADS)

    Hartweg, Sebastian; Yoder, Bruce L.; Garcia, Gustavo A.; Nahon, Laurent; Signorell, Ruth

    2017-03-01

    We report the first measurements of size-resolved photoelectron angular distributions for the valence orbitals of neutral water clusters with up to 20 molecules. A systematic decrease of the photoelectron anisotropy is found for clusters with up to 5-6 molecules, and most remarkably, convergence of the anisotropy for larger clusters. We suggest the latter to be the result of a local short-range scattering potential that is fully described by a unit of 5-6 molecules. The cluster data and a detailed electron scattering model are used to predict the anisotropy of slow photoelectrons in liquid water. Reasonable agreement with experimental liquid jet data is found.

  11. Analysis of Measurement Requirements for the Aerosol Indirect Effect: A Synthesis of Observations and Modeling

    NASA Astrophysics Data System (ADS)

    Feingold, G.; Previdi, M.; Veron, D. E.

    2003-12-01

    The aerosol indirect effect has been measured for some time now by satellite remote sensors, and more recently by surface-based remote sensors. The indirect effect is often expressed in terms of a relative change in drop size for a relative change in aerosol optical depth or extinction. Here we present some recent results of surface based remote sensing of the indirect effect and assess whether aerosol optical depth or extinction is a suitable proxy for the aerosol affecting drop formation. To do so, we use multiple realizations of a cloud model to investigate the sensitivity of cloud drop effective radius re to aerosol parameters (size distribution and composition) and dynamical parameters (updraft and liquid water content). A breakdown of the individual aerosol terms contributing to drop size change shows that use of aerosol extinction as a proxy for size distribution and composition tends to underestimate the magnitude of the first indirect effect. The use of the aerosol index alleviates this problem somewhat. We show that re is most sensitive to cloud liquid water, a parameter often ignored in indirect effect analyses. The relative importance of the other parameters varies for different conditions but aerosol concentration Na is consistently important. Updraft plays an increasingly important role under high aerosol loadings. Requirements for measuring the indirect effect over polluted continents are shown to be more stringent than those over cleaner, remote oceans. This may influence interpretation of current satellite and surface remote measurements of the indirect effect.

  12. Liquid water and resurfacing of Enceladus' south polar terrain

    NASA Astrophysics Data System (ADS)

    Tobie, G.; Besserer, J.; Cadek, O.; Choblet, G.; Sotin, C.

    2008-09-01

    Enceladus are the only solid objects in the Solar System to be sufficiently geologically active for their internal heat to be detected by remote sensing. Interestingly, the endogenic activity on Enceladus is only located on a specific region at the south pole, from which jets of water vapor and ice particles have been observed ([1], [2]). The current polar location of the thermal anomaly can possibly be explained by diapirinduced reorientation of the satellite [3], but the triggering of the thermal anomaly and the heat power required to sustain it over geologic timescales remain problematic. Using a three-dimensional viscoelastic numerical model simulating the response of Enceladus to tidal forcing, we have demonstrated in a previous recent study [4] that only interior models with a liquid water layer at depth can explain the observed magnitude of dissipation and its particular location at the south pole (Fig. 1). Moreover, as tidally-induced heat must be generated over a relatively broad region in the southern hemisphere to explain the observed thermal emission, we proposed that this heat is then transferred toward the south polar terrain where it could be episodically released during relatively short resurfacing events. In the present study, we investigate the thermal stability of localized liquid water reservoir at the rock-ice interface by performing simulations of thermal convection in three-dimensional spherical geometry with the numerical tool OEDIPUS ([5],[6]) and by computing the corresponding dissipation pattern using the method developped in [4]. Where liquid water is present, a constant temperature equal to the melting temperature of water ice is prescribed at the base of the ice shell. Outside this region, a constant heat flux owing to the radiogenic power coming out of the silicate core is prescribed. Figure 2 illustrates the temperature field obtained for varying size of the liquid reservoir (ranging from 60o to 120o). These preliminary results

  13. Ionic liquid foam floatation coupled with ionic liquid dispersive liquid-liquid microextraction for the separation and determination of estrogens in water samples by high-performance liquid chromatography with fluorescence detection.

    PubMed

    Zhang, Rui; Wang, Chuanliu; Yue, Qiaohong; Zhou, Tiecheng; Li, Na; Zhang, Hanqi; Hao, Xiaoke

    2014-11-01

    An ionic liquid foam floatation coupled with ionic liquid dispersive liquid-liquid microextraction method was proposed for the extraction and concentration of 17-α-estradiol, 17-β-estradiol-benzoate, and quinestrol in environmental water samples by high-performance liquid chromatography with fluorescence detection. 1-Hexyl-3-methylimidazolium tetrafluoroborate was applied as foaming agent in the foam flotation process and dispersive solvent in microextraction. The introduction of the ion-pairing and salting-out agent NH4 PF6 was beneficial to the improvement of recoveries for the hydrophobic ionic liquid phase and analytes. Parameters of the proposed method including concentration of 1-hexyl-3-methylimidazolium tetrafluoroborate, flow rate of carrier gas, floatation time, types and concentration of ionic liquids, salt concentration in samples, extraction time, and centrifugation time were evaluated. The recoveries were between 98 and 105% with relative standard deviations lower than 7% for lake water and well water samples. The isolation of the target compounds from the water was found to be efficient, and the enrichment factors ranged from 4445 to 4632. This developing method is free of volatile organic solvents compared with regular extraction. Based on the unique properties of ionic liquids, the application of foam floatation, and dispersive liquid-liquid microextraction was widened.

  14. Small-scale experimental study of vaporization flux of liquid nitrogen released on water.

    PubMed

    Gopalaswami, Nirupama; Olewski, Tomasz; Véchot, Luc N; Mannan, M Sam

    2015-10-30

    A small-scale experimental study was conducted using liquid nitrogen to investigate the convective heat transfer behavior of cryogenic liquids released on water. The experiment was performed by spilling five different amounts of liquid nitrogen at different release rates and initial water temperatures. The vaporization mass fluxes of liquid nitrogen were determined directly from the mass loss measured during the experiment. A variation of initial vaporization fluxes and a subsequent shift in heat transfer mechanism were observed with changes in initial water temperature. The initial vaporization fluxes were directly dependent on the liquid nitrogen spill rate. The heat flux from water to liquid nitrogen determined from experimental data was validated with two theoretical correlations for convective boiling. It was also observed from validation with correlations that liquid nitrogen was found to be predominantly in the film boiling regime. The substantial results provide a suitable procedure for predicting the heat flux from water to cryogenic liquids that is required for source term modeling.

  15. 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.

  16. Removal of bio-aerosols by water flow on surfaces in health-care settings

    NASA Astrophysics Data System (ADS)

    Yu, Han; Li, Yuguo

    2016-11-01

    Hand hygiene is one of the most important and efficient measures to prevent infections, however the compliance with hand hygiene remains poor especially for health-care workers. To improve this situation, the mechanisms of hand cleansing need to be explored and a detailed study on the adhesion interactions for bio-aerosols on hand surfaces and the process during particles removal by flow is significant for more efficient methods to decrease infections. The first part of presentation will focus on modelling adhesion interactions between particles, like bacteria and virus, and hand surfaces with roughness in water environment. The model presented is based on the DLVO and its extended theories. The removal process comes next, which will put forward a new model to describe the removal of particles by water flow. In this model, molecular dynamics is combined with particle motion and the results by the model will be compared with experiment results and existed models (RnR, Rock & Roll). Finally, possible improvement of the study and future design of experiments will be discussed.

  17. Determination of trace lead in biological and water samples with dispersive liquid-liquid microextraction preconcentration.

    PubMed

    Liang, Pei; Sang, Hongbo

    2008-09-01

    A new method for the determination of trace lead was developed by dispersive liquid-liquid microextraction preconcentration and graphite furnace atomic absorption spectrometry. In the proposed approach, 1-phenyl-3-methyl-4-benzoyl-5-pyrazolone (PMBP) was used as a chelating agent, and carbon tetrachloride and ethanol were selected as extraction and dispersive solvents. Some factors influencing the extraction efficiency of lead and its subsequent determination, including extraction and dispersive solvent type and volume, pH of sample solution, concentration of the chelating agent, and extraction time, were studied and optimized. Under the optimum conditions, the enrichment factor of this method for lead was reached at 78. The detection limit for lead was 39 ng L(-1) (3 sigma), and the relative standard deviation (RSD) was 3.2% (n=7, c=10 ng mL(-1)). The method was successfully applied to the determination of trace amounts of lead in human urine and water samples.

  18. Interfacial thermodynamics of water and six other liquid solvents.

    PubMed

    Pascal, Tod A; Goddard, William A

    2014-06-05

    We examine the thermodynamics of the liquid-vapor interface by direct calculation of the surface entropy, enthalpy, and free energy from extensive molecular dynamics simulations using the two-phase thermodynamics (2PT) method. Results for water, acetonitrile, cyclohexane, dimethyl sulfoxide, hexanol, N-methyl acetamide, and toluene are presented. We validate our approach by predicting the interfacial surface tensions (IFT--excess surface free energy per unit area) in excellent agreement with the mechanical calculations using Kirkwood-Buff theory. Additionally, we evaluate the temperature dependence of the IFT of water as described by the TIP4P/2005, SPC/Ew, TIP3P, and mW classical water models. We find that the TIP4P/2005 and SPC/Ew water models do a reasonable job of describing the interfacial thermodynamics; however, the TIP3P and mW are quite poor. We find that the underprediction of the experimental IFT at 298 K by these water models results from understructured surface molecules whose binding energies are too weak. Finally, we performed depth profiles of the interfacial thermodynamics which revealed long tails that extend far into what would be considered bulk from standard Gibbs theory. In fact, we find a nonmonotonic interfacial free energy profile for water, a unique feature that could have important consequences for the absorption of ions and other small molecules.

  19. Gas hydrate inhibition by perturbation of liquid water structure

    NASA Astrophysics Data System (ADS)

    Sa, Jeong-Hoon; Kwak, Gye-Hoon; Han, Kunwoo; Ahn, Docheon; Lee, Kun-Hong

    2015-06-01

    Natural gas hydrates are icy crystalline materials that contain hydrocarbons, which are the primary energy source for this civilization. The abundance of naturally occurring gas hydrates leads to a growing interest in exploitation. Despite their potential as energy resources and in industrial applications, there is insufficient understanding of hydrate kinetics, which hinders the utilization of these invaluable resources. Perturbation of liquid water structure by solutes has been proposed to be a key process in hydrate inhibition, but this hypothesis remains unproven. Here, we report the direct observation of the perturbation of the liquid water structure induced by amino acids using polarized Raman spectroscopy, and its influence on gas hydrate nucleation and growth kinetics. Amino acids with hydrophilic and/or electrically charged side chains disrupted the water structure and thus provided effective hydrate inhibition. The strong correlation between the extent of perturbation by amino acids and their inhibition performance constitutes convincing evidence for the perturbation inhibition mechanism. The present findings bring the practical applications of gas hydrates significantly closer, and provide a new perspective on the freezing and melting phenomena of naturally occurring gas hydrates.

  20. Gas hydrate inhibition by perturbation of liquid water structure.

    PubMed

    Sa, Jeong-Hoon; Kwak, Gye-Hoon; Han, Kunwoo; Ahn, Docheon; Lee, Kun-Hong

    2015-06-17

    Natural gas hydrates are icy crystalline materials that contain hydrocarbons, which are the primary energy source for this civilization. The abundance of naturally occurring gas hydrates leads to a growing interest in exploitation. Despite their potential as energy resources and in industrial applications, there is insufficient understanding of hydrate kinetics, which hinders the utilization of these invaluable resources. Perturbation of liquid water structure by solutes has been proposed to be a key process in hydrate inhibition, but this hypothesis remains unproven. Here, we report the direct observation of the perturbation of the liquid water structure induced by amino acids using polarized Raman spectroscopy, and its influence on gas hydrate nucleation and growth kinetics. Amino acids with hydrophilic and/or electrically charged side chains disrupted the water structure and thus provided effective hydrate inhibition. The strong correlation between the extent of perturbation by amino acids and their inhibition performance constitutes convincing evidence for the perturbation inhibition mechanism. The present findings bring the practical applications of gas hydrates significantly closer, and provide a new perspective on the freezing and melting phenomena of naturally occurring gas hydrates.

  1. Natural abundance 13C and 14C analysis of water-soluble organic carbon in atmospheric aerosols.

    PubMed

    Kirillova, Elena N; Sheesley, Rebecca J; Andersson, August; Gustafsson, Örjan

    2010-10-01

    Water-soluble organic carbon (WSOC) constitutes a large fraction of climate-forcing organic aerosols in the atmosphere, yet the sources of WSOC are poorly constrained. A method was developed to measure the stable carbon isotope (δ(13)C) and radiocarbon (Δ(14)C) composition of WSOC for apportionment between fossil fuel and different biogenic sources. Synthetic WSOC test substances and ambient aerosols were employed to investigate the effect of both modern and fossil carbon contamination and any method-induced isotope fractionation. The method includes extraction of aerosols collected on quartz filters followed by purification and preparation for off-line δ(13)C and Δ(14)C determination. The preparative freeze-drying step for isotope analysis yielded recoveries of only ∼70% for ambient aerosols and WSOC probes. However, the δ(13)C of the WSOC isolates were in agreement with the δ(13)C of the unprocessed starting material, even for the volatile oxalic acid probe (6.59 ± 0.37‰ vs 6.33 ± 0.31‰; 2 sd). A (14)C-fossil phthalic acid WSOC probe returned a fraction modern biomass of <0.008 whereas a (14)C-modern sucrose standard yielded a fraction modern of >0.999, indicating the Δ(14)C-WSOC method to be free of both fossil and contemporary carbon contamination. Application of the δ(13)C/Δ(14)C-WSOC method to source apportion climate-affecting aerosols was illustrated be constraining that WSOC in ambient Stockholm aerosols were 88% of contemporary biogenic C3 plant origin.

  2. Fluorescent behavior of B-phycoerythrin in microemulsions of aerosol OT/water/isooctane.

    PubMed

    Bermejo, Ruperto; Tobaruela, Diego J; Talavera, Eva M; Orte, Angel; Alvarez-Pez, Jose M

    2003-07-15

    Taking advantage of its unusual fluorescent properties, the incorporation of B-phycoerythrin (B-PE) in aerosol OT (AOT, sodium bis-(2-ethylhexyl) sulphosuccinate)/water/isooctane microemulsions was investigated by following their steady-state and time-resolved fluorescence as a function of the water-to-surfactant molar ratio, w(0). The fluorescent intensity at 575 nm increased continuously with increasing water content, saturating at a w(0) around 35 and staying practically constant at w(0)> or =40. The steady-state anisotropy showed an initial increase with increasing water content until w(0)=23 and then decreased strongly, staying practically constant when w(0)> or =40. The values of the fluorescent parameters, anisotropy and fluorescent intensity, were unchanged when the water content of the system increased in the range between w(0)=40 to 50. This implies the effective incorporation of B-PE in the microemulsion droplets with w(0)> or =40, as well as the equilibrium of the dispersion at these water/surfactant ratios, since higher water content does not affect the main surrounding microenvironment of the protein. The overall incorporation in the microemulsion droplets caused minor spectroscopic changes with respect to biliprotein in aqueous solution of 20 mM sodium phosphate buffer, pH 7.0, such as a blue absorption shift of 3 nm and an emission shift of 1.5 nm, as well as a slight increase in excitation anisotropy spectrum mainly caused by a decrease in protein mobility. Therefore, there are no important interactions between the chromophores and the AOT sulfonate head groups. Emission intensity decays followed complex kinetics in both aqueous and dispersion media. The stability with time and temperature of the biliprotein in the microemulsion was higher than in the aqueous solution. All the results can be explained in terms of B-PE inclusion in the water droplets of AOT microemulsions where the protein has similar configuration and conformation to that in

  3. Chemical characteristics of aerosol and rain water during an El Niño and PDO influenced Indian summer monsoon

    NASA Astrophysics Data System (ADS)

    Rajeev, Pradhi; Rajput, Prashant; Gupta, Tarun

    2016-11-01

    According to the meteorological long-term variability pattern, year 2015 was influenced by El Niño and PDO (Pacific Decadal Oscillation; causes weakening of Indian Summer Monsoon). These conditions facilitate the assessment of chemical characteristics of fine-mode ambient aerosols (PM2.5; n = 48) and individual rain waters (pH: 6.4-7.6; n = 15) during the South-west monsoon (July-September 2015) in the central Indo-Gangetic Plain (IGP; Kanpur). Water-soluble ionic species (WSIS) have been measured to assess the undergoing processes (neutralization, formation and below-cloud scavenging) and estimate their dry and wet deposition fluxes. The ∑WSIS varies from 4 to 32 μg/m3 in PM2.5, whereas it ranges from 32 to 102 mg/L in rain waters. The NH4+ and SO42- are found to be predominant in PM2.5 (16-120 μg/m3), whereas HCO3- and Ca2+ are predominant in rain water samples. The difference in chemical composition of PM2.5 and rain water is largely attributed to additional contribution of coarse-mode mineral dust in rain water. The Ca2+ and Mg2+ in both aerosols and rain water samples are associated with HCO3-. The NO3- and SO42- are neutralized predominantly by NH4+ and ∑-/∑+ ratio is ≈ 1 in both aerosols and rain waters. Furthermore, co-variability of NO3- with nss-Ca2+ in PM2.5 indicates role of fine-mode mineral dust surface in the formation of ammonium nitrate. Characteristic mass ratios (HCO3-/Ca2+ and SO42-/NH4+) in rain water look quite similar to those in aerosols (PM2.5). This suggests that below-cloud scavenging is predominant mechanism of aerosols wash-out. Dry deposition fluxes of Mg2+, NH4+ and SO42- are ∼13% of their wet deposition fluxes, whereas for K+, Ca2+ and NO3- it is <6%.

  4. Storage tank with liquid insulator for storing cryogenic fluids using water displacement

    SciTech Connect

    McCabe, J.S.; Stafford, D.C.; Laverman, R.J.

    1980-06-24

    For storing cryogenic liquids such as LNG at or slightly above atmospheric pressure, this design uses a tank with insulated vertical walls and an insulated top located in and surrounded by a body of water in communication with a layer of water inside the tank; the level of the tank contents can thus be controlled using the water-displacement principle. A layer of insulating liquid having a specific gravity lower than water and higher than LNG (or the cryogenic liquid being stored) separates the water and LNG while remaining liquid at the cryogenic temperature; the insulating liquid - pentanes, particularly isopentane, are suitable - must be essentially immiscible with water, LNG, or both. For preventing turbulent mixing of the water and LNG while the tank is being filled or emptied, a float in the form of a closed or open shell made partially or entirely of insulating material extends over the water layer and contains the insulating liquid.

  5. Cloud and rain liquid water statistics in the CHUVA campaign

    NASA Astrophysics Data System (ADS)

    Calheiros, Alan J. P.; Machado, Luiz A. T.

    2014-07-01

    The purpose of this study is to present statistics related to the integration of cloud and rain liquid water and the profiles for different cloud types and regimes. From 2010 to 2012, the CHUVA project collected information regarding cloud and rain characteristics in different precipitation regimes in Brazil. CHUVA had four field campaigns between 2010 and 2011, located in the North, Northeast and Southeast regions of Brazil, covering the semi-arid, Amazon, coastal and mountain regions. The synergy of several instruments allowed us to classify rain events and describe the cloud processes regionally. Microwave radiometers, LiDAR, radar, and disdrometers were employed in this study. The rain type classification was made using vertical profiles of reflectivity (VPR) and polarimetric variables from dual polarization radar (XPOL). The integrated liquid water (ILWC) for non-precipitating clouds was retrieved with a microwave ground-based radiometer using a neural network. For rainy conditions, the profiles from the rain liquid water content (LWCR) and their integrated (ILWR) properties were estimated by Micro Rain Radar (MRR) and XPOL VPRs. For non-precipitating clouds, the ILWC values were larger for the sites in tropical regions, in particular near the coast, than for Southeast Brazil. For rainy cases, distinct LWCR profiles were observed for different rain classifications and regions. The differences are small for low rain rates and a distinction between different rainfall regimes is more evident for high rain rates. Vale and Belém clouds present the deepest layers and largest convective rain rates. The clouds in the Southeast region of Brazil (Vale do Paraíba) and North region (Belém) showed the largest reflectivity in the mixed and glaciated layers, respectively. In contrast, the Northeast coastal site (e.g. Fortaleza) showed larger values in the warm part of the clouds. Several analyses are presented, describing the cloud processes and the differences among the

  6. A Laboratory Investigation of Aerosol and Extinction Characteristics for SALTY DOG, NWC 29 and NWC 78 Pyrotechnics

    DTIC Science & Technology

    1980-10-01

    Dispersion Extinction Pyrotechnics Salty Dog Smokes Deliquescent Growth i *0. ABSTRACT (Continue on reverse aide Iti nee.,ary and idently by block... deliquescent aerosol. Results from the laboratory investigation of individual particle growth indicate that the aerosol generated by NVC 78 has the...due to liquid water (i.e., the deliquesced aerosol) absorption at those IR wavelengths. To compare the extinction effectiveness of Salty Dog to that of

  7. Identification of dimethoate-containing water using partitioned dispersive liquid-liquid microextraction coupled with near-infrared spectroscopy.

    PubMed

    Zhang, Ming; Geng, Ying; Xiang, Bingren

    2011-01-01

    A simple, rapid and efficient extraction procedure, partitioned dispersive liquid-liquid microextraction, has been developed in combination with near-infrared spectroscopy for the extraction and discrimination of dimethoate from aqueous samples. For this technique, the appropriate mixture of extraction solvent (CCl(4)) and disperser solvent (THF) was utilized. Partial least squares discriminant analysis was applied to build the model with several pre-process methods over the wavenumber regions between 7100 cm(-1) to 7300 cm(-1). The best model gave satisfactory classification accuracy, 98.6% for calibration set (n=74) and 97.6% for prediction set (n=42), using preprocessing of standard normal variate followed by Savitzky-Golay first derivative. The method was successfully applied to bottled water, tap water, lake water and farm water samples. The results demonstrated the possibility of near-infrared spectroscopy after partitioned dispersive liquid-liquid microextraction for the identification of water contaminated by dimethoate.

  8. The Boson peak in confined water: An experimental investigation of the liquid-liquid phase transition hypothesis

    NASA Astrophysics Data System (ADS)

    Mallamace, Francesco; Corsaro, Carmelo; Mallamace, Domenico; Wang, Zhe; Chen, Sow-Hsin

    2015-10-01

    The Boson peak (BP) of deeply cooled confined water is studied by using inelastic neutron scattering (INS) in a large interval of the ( P, T) phase plane. By taking into account the different behavior of such a collective vibrational mode in both strong and fragile glasses as well as in glass-forming materials, we were able to determine the Widom line that characterizes supercooled bulk water within the frame of the liquid-liquid phase transition (LLPT) hypothesis. The peak frequency and width of the BP correlated with the water polymorphism of the LLPT scenario, allowing us to distinguish the "low-density liquid" (LDL) and "high-density liquid" (HDL) phases in deeply cooled bulk water.Moreover, the BP properties afford a further confirmation of theWidom line temperature T W as the ( P, T) locus in which the local structure of water transforms from a predominately LDL form to a predominately HDL form.

  9. Water-based scintillators for large-scale liquid calorimetry

    SciTech Connect

    Winn, D.R.; Raftery, D.

    1985-02-01

    We have investigated primary and secondary solvent intermediates in search of a recipe to create a bulk liquid scintillator with water as the bulk solvent and common fluors as the solutes. As we are not concerned with energy resolution below 1 MeV in large-scale experiments, light-output at the 10% level of high-quality organic solvent based scintillators is acceptable. We have found encouraging performance from industrial surfactants as primary solvents for PPO and POPOP. This technique may allow economical and environmentally safe bulk scintillator for kiloton-sized high energy calorimetry.

  10. The structural origin of anomalous properties of liquid water

    PubMed Central

    Nilsson, Anders; Pettersson, Lars G. M.

    2015-01-01

    Water is unique in its number of unusual, often called anomalous, properties. When hot it is a normal simple liquid; however, close to ambient temperatures properties, such as the compressibility, begin to deviate and do so increasingly on further cooling. Clearly, these emerging properties are connected to its ability to form up to four well-defined hydrogen bonds allowing for different local structural arrangements. A wealth of new data from various experiments and simulations has recently become available. When taken together they point to a heterogeneous picture with fluctuations between two classes of local structural environments developing on temperature-dependent length scales. PMID:26643439

  11. Radar and the Detection of Liquid Water on Mars

    NASA Technical Reports Server (NTRS)

    Roth, L. E.; Saunders, R. S.

    1985-01-01

    Detection of the seasonally variable radar reflectivity in the Goldstone Mars data (the Solis Lacus radar anomaly and the proposed interpretation in terms of the near-surface presence of liquid water created a controversy in the planetary science community. Over the past year, skepticism was voiced about the reality of the phenomenon of a seasonally variable radar reflectivity anywhere on Mars. The necessary background information and the pertinent data are reviewed in a format perhaps more convincing than that employed in the original presentation of the discovery. A summary of the results and recommendations for future work are included.

  12. Analysis of Characteristics of Dust Aerosols in Northwest China based on Satellite Remote-sensing Data

    NASA Astrophysics Data System (ADS)

    Zhang, L.; Liu, L.; Zhao, Y.; Gong, S.; Henze, D. K.

    2014-12-01

    Based on the CloudSat data, effects of dust aerosol on cloud parameters under the circumstance of the monthly average, dusty days and dust-free days were analyzed during April, 2010. By using L2 aerosol profiles satellite data of CALIOP/CALIOPSO the aerosol extinction coefficients were analyzed over northwest China. As an important case, space distribution and transmission route of dust aerosol were investigated during the dust events occurred from April 16th to 18th in 2013 over northwest China, based on L1 data of CALIOP/CALIOPSO, a combination of multiple satellite data and models. The results show that (1) dust aerosols could cause the reduction in effective radius of particle, cloud liquid water content and cloud optical thickness, and the increase of the number concentration of liquid cloud particles as well, (2) The aerosol extinction coefficients were decreased with the increase of height. The value of the aerosol extinction coefficients in desert area was greater than that in the area of Gansu Province due to urbanization. Distribution of the aerosol extinction coefficients in spring was nearly the same as the annual average. (3) Using aerosol products of the vertical characteristics from CALIOP/CALIOPSO, aerosol was classified during dust events, and with NAPPS Global aerosol model, daily distribution of the dust aerosol concentration was given, showing the transport and diffusion of dust aerosol. With HYSPLIT trajectory model dust transportation path of the sand dust source areas was simulated and identified. During the outbreak of dust event dust aerosol was mainly distributed over the surface about 3km, with depolarization ratio at 0.4 and color ratio at 1.2. During the dust events were close to weak and stop, dust aerosol was mainly distributed over the surface under 2 km, with depolarization ratio from 0.2 to 0.3, and color ratio about 1.

  13. Analysis of Characteristics of Dust Aerosols in Northwest China based on Satellite Remote-sensing Data

    NASA Astrophysics Data System (ADS)

    Zhang, W.; Liu, D.; Zhao, Q.

    2015-12-01

    Based on the CloudSat data, effects of dust aerosol on cloud parameters under the circumstance of the monthly average, dusty days and dust-free days were analyzed during April, 2010. By using L2 aerosol profiles satellite data of CALIOP/CALIOPSO the aerosol extinction coefficients were analyzed over northwest China. As an important case, space distribution and transmission route of dust aerosol were investigated during the dust events occurred from April 16th to 18th in 2013 over northwest China, based on L1 data of CALIOP/CALIOPSO, a combination of multiple satellite data and models. The results show that (1) dust aerosols could cause the reduction in effective radius of particle, cloud liquid water content and cloud optical thickness, and the increase of the number concentration of liquid cloud particles as well, (2) The aerosol extinction coefficients were decreased with the increase of height. The value of the aerosol extinction coefficients in desert area was greater than that in the area of Gansu Province due to urbanization. Distribution of the aerosol extinction coefficients in spring was nearly the same as the annual average. (3) Using aerosol products of the vertical characteristics from CALIOP/CALIOPSO, aerosol was classified during dust events, and with NAPPS Global aerosol model, daily distribution of the dust aerosol concentration was given, showing the transport and diffusion of dust aerosol. With HYSPLIT trajectory model dust transportation path of the sand dust source areas was simulated and identified. During the outbreak of dust event dust aerosol was mainly distributed over the surface about 3km, with depolarization ratio at 0.4 and color ratio at 1.2. During the dust events were close to weak and stop, dust aerosol was mainly distributed over the surface under 2 km, with depolarization ratio from 0.2 to 0.3, and color ratio about 1.

  14. Remote Sensing of Cloud, Aerosol, and Water Vapor Properties from MODIS

    NASA Technical Reports Server (NTRS)

    King, Michael D.

    2001-01-01

    MODIS is an earth-viewing cross-track scanning spectroradiometer launched on the Terra satellite in December 1999. MODIS scans a swath width sufficient to provide nearly complete global coverage every two days from a polar-orbiting, sun-synchronous, platform at an altitude of 705 km, and provides images in 36 spectral bands from 0.415 to 14.235 microns with spatial resolutions of 250 m (2 bands), 500 m (5 bands) and 1000 m (29 bands). These bands have been carefully selected to enable advanced studies of land, ocean, and atmospheric processes. In this presentation I will review the comprehensive set of remote sensing algorithms that have been developed for the remote sensing of atmospheric properties using MODIS data, placing primary emphasis on the principal atmospheric applications of: (1) developing a cloud mask for distinguishing clear sky from clouds, (2) retrieving global cloud radiative and microphysical properties, including cloud top pressure and temperature, effective emissivity, cloud optical thickness, thermodynamic phase, and effective radius, (3) monitoring tropospheric aerosol optical thickness over the land and ocean and aerosol size distribution over the ocean, (4) determining atmospheric profiles of moisture and temperature, and (5) estimating column water amount. The physical principles behind the determination of each of these atmospheric products will be described, together with an example of their application using MODIS observations. All products are archived into two categories: pixel-level retrievals (referred to as Level-2 products) and global gridded products at a latitude and longitude resolution of 1 deg (Level-3 products). An overview of the MODIS atmosphere algorithms and products, status, validation activities, and early level-2 and -3 results will be presented. Finally, I will present some highlights from the land and ocean algorithms developed for processing global MODIS observations, including: (1) surface reflectance, (2

  15. Gas and liquid measurements in air-water bubbly flows

    SciTech Connect

    Zhou, X.; Doup, B.; Sun, X.

    2012-07-01

    Local measurements of gas- and liquid-phase flow parameters are conducted in an air-water two-phase flow loop. The test section is a vertical pipe with an inner diameter of 50 mm and a height of 3.2 m. The measurements are performed at z/D = 10. The gas-phase measurements are performed using a four-sensor conductivity probe. The data taken from this probe are processed using a signal processing program to yield radial profiles of the void fraction, bubble velocity, and interfacial area concentration. The velocity measurements of the liquid-phase are performed using a state-of-the-art Particle Image Velocimetry (PIV) system. The raw PIV images are acquired using fluorescent particles and an optical filtration device. Image processing is used to remove noise in the raw PIV images. The statistical cross correlation is introduced to determine the axial velocity field and turbulence intensity of the liquid-phase. Measurements are currently being performed at z/D = 32 to provide a more complete data set. These data can be used for computational fluid dynamic model development and validation. (authors)

  16. Determination of organic compounds in water using dispersive liquid-liquid microextraction.

    PubMed

    Rezaee, Mohammad; Assadi, Yaghoub; Milani Hosseini, Mohammad-Reza; Aghaee, Elham; Ahmadi, Fardin; Berijani, Sana

    2006-05-26

    A new microextraction technique termed dispersive liquid-liquid microextraction (DLLME) was developed. DLLME is a very simple and rapid method for extraction and preconcentration of organic compounds from water samples. In this method, the appropriate mixture of extraction solvent (8.0 microL C2Cl4) and disperser solvent (1.00 mL acetone) are injected into the aqueous sample (5.00 mL) by syringe, rapidly. Therefore, cloudy solution is formed. In fact, it is consisted of fine particles of extraction solvent which is dispersed entirely into aqueous phase. After centrifuging, the fine particles of extraction solvent are sedimented in the bottom of the conical test tube (5.0 +/- 0.2 microL). The performance of DLLME is illustrated with the determination of polycyclic aromatic hydrocarbons (PAHs) in water samples by using gas chromatography-flame ionization detection (GC-FID). Some important parameters, such as kind of extraction and disperser solvent and volume of them, and extraction time were investigated. Under the optimum conditions the enrichment factor ranged from 603 to 1113 and the recovery ranged from 60.3 to 111.3%. The linear range was 0.02-200 microg/L (four orders of magnitude) and limit of detection was 0.007-0.030 microg/L for most of analytes. The relative standard deviations (RSDs) for 2 microg/L of PAHs in water by using internal standard were in the range 1.4-10.2% (n = 5). The recoveries of PAHs from surface water at spiking level of 5.0 microg/L were 82.0-111.0%. The ability of DLLME technique in the extraction of other organic compounds such as organochlorine pesticides, organophosphorus pesticides and substituted benzene compounds (benzene, toluene, ethyl benzene, and xylenes) from water samples were studied. The advantages of DLLME method are simplicity of operation, rapidity, low cost, high recovery, and enrichment factor.

  17. Innovative Strategy on Hydrogen Evolution Reaction Utilizing Activated Liquid Water

    PubMed Central

    Hwang, Bing-Joe; Chen, Hsiao-Chien; Mai, Fu-Der; Tsai, Hui-Yen; Yang, Chih-Ping; Rick, John; Liu, Yu-Chuan

    2015-01-01

    Splitting water for hydrogen production using light, or electrical energy, is the most developed ‘green technique’. For increasing efficiency in hydrogen production, currently, the most exciting and thriving strategies are focused on efficient and inexpensive catalysts. Here, we report an innovative idea for efficient hydrogen evolution reaction (HER) utilizing plasmon-activated liquid water with reduced hydrogen-bonded structure by hot electron transfer. This strategy is effective for all HERs in acidic, basic and neutral systems, photocatalytic system with a g-C3N4 (graphite carbon nitride) electrode, as well as in an inert system with an ITO (indium tin oxide) electrode. Compared to deionized water, the efficiency of HER increases by 48% based on activated water ex situ on a Pt electrode. Increase in energy efficiency from activated water is 18% at a specific current yield of −20 mA in situ on a nanoscale-granulated Au electrode. Moreover, the onset potential of −0.023 V vs RHE was very close to the thermodynamic potential of the HER (0 V). The measured current density at the corresponding overpotential for HER in an acidic system was higher than any data previously reported in the literature. This approach establishes a new vista in clean green energy production. PMID:26541371

  18. Innovative Strategy on Hydrogen Evolution Reaction Utilizing Activated Liquid Water

    NASA Astrophysics Data System (ADS)

    Hwang, Bing-Joe; Chen, Hsiao-Chien; Mai, Fu-Der; Tsai, Hui-Yen; Yang, Chih-Ping; Rick, John; Liu, Yu-Chuan

    2015-11-01

    Splitting water for hydrogen production using light, or electrical energy, is the most developed ‘green technique’. For increasing efficiency in hydrogen production, currently, the most exciting and thriving strategies are focused on efficient and inexpensive catalysts. Here, we report an innovative idea for efficient hydrogen evolution reaction (HER) utilizing plasmon-activated liquid water with reduced hydrogen-bonded structure by hot electron transfer. This strategy is effective for all HERs in acidic, basic and neutral systems, photocatalytic system with a g-C3N4 (graphite carbon nitride) electrode, as well as in an inert system with an ITO (indium tin oxide) electrode. Compared to deionized water, the efficiency of HER increases by 48% based on activated water ex situ on a Pt electrode. Increase in energy efficiency from activated water is 18% at a specific current yield of -20 mA in situ on a nanoscale-granulated Au electrode. Moreover, the onset potential of -0.023 V vs RHE was very close to the thermodynamic potential of the HER (0 V). The measured current density at the corresponding overpotential for HER in an acidic system was higher than any data previously reported in the literature. This approach establishes a new vista in clean green energy production.

  19. Distribution of binding energies of a water molecule in the water liquid-vapor interface

    SciTech Connect

    Chempath, Shaji; Pratt, Lawrence R

    2008-01-01

    Distributions of binding energies of a water molecule in the water liquid-vapor interface are obtained on the basis of molecular simulation with the SPC/E model of water. These binding energies together with the observed interfacial density profile are used to test a minimally conditioned Gaussian quasi-chemical statistical thermodynamic theory. Binding energy distributions for water molecules in that interfacial region clearly exhibit a composite structure. A minimally conditioned Gaussian quasi-chemical model that is accurate for the free energy of bulk liquid water breaks down for water molecules in the liquid-vapor interfacial region. This breakdown is associated with the fact that this minimally conditioned Gaussian model would be inaccurate for the statistical thermodynamics of a dilute gas. Aggressive conditioning greatly improves the performance of that Gaussian quasi-chemical model. The analogy between the Gaussian quasi-chemical model and dielectric models of hydration free energies suggests that naive dielectric models without the conditioning features of quasi-chemical theory will be unreliable for these interfacial problems. Multi-Gaussian models that address the composite nature of the binding energy distributions observed in the interfacial region might provide a mechanism for correcting dielectric models for practical applications.

  20. Hot electron dominated rapid transverse ionization growth in liquid water.

    PubMed

    Brown, Michael S; Erickson, Thomas; Frische, Kyle; Roquemore, William M

    2011-06-20

    Pump/probe optical-transmission measurements are used to monitor in space and time the ionization of a liquid column of water following impact of an 800-nm, 45-fs pump pulse. The pump pulse strikes the 53-μm-diameter column normal to its axis with intensities up to 2 × 10(15) W/cm2. After the initial photoinization and for probe delay times < 500 fs, the neutral water surrounding the beam is rapidly ionized in the transverse direction, presumably by hot electrons with initial velocities of 0.55 times the speed of light (relativistic kinetic energy of ~100 keV). Such velocities are unusual for condensed-matter excitation at the stated laser intensities.

  1. ETV REPORT AND VERIFICATION STATEMENT; EVALUATION OF LOBO LIQUIDS RINSE WATER RECOVERY SYSTEM

    EPA Science Inventory

    The Lobo Liquids Rinse Water Recovery System (Lobo Liquids system) was tested, under actual production conditions, processing metal finishing wastewater, at Gull Industries in Houston, Texas. The verification test evaluated the ability of the ion exchange (IX) treatment system t...

  2. A comparison of the Stratospheric Aerosol and Gas Experiment II tropospheric water vapor to radiosonde measurements

    SciTech Connect

    Larsen, J.C.; Chiou, E.W. ); Chu, W.P.; McCormick, M.P.; McMaster, L.R. ); Oltmans, S. ); Rind, D. )

    1993-03-20

    Upper tropospheric Stratospheric Aerosol and Gas Experiment II (SAGE II) water vapor observations are compared to correlative radiosonde observations and radiosonde based climatologies. The SAGE II 1987 monthly zonal mean water vapor climatology is compared to both the Global Atmospheric Circulation Statistics (1963-1973) climatology and to the 1987 radiosonde climatology. The clear sky SAGE II climatology is found to be approximately half the level of both the clear/cloudy sky radiosonde climatologies. To determine whether this is realistic for these two different climatologies or includes additional observational and instrumental biases, the authors took the 1987 radiosonde data set and identified approximately 800 correlative profile pairs. The observational biases inherent to SAGE II and the radiosondes produce a set of profile pairs characteristic of clear sky, land conditions. A critical review of the radiosonde measurement capability was carried out to establish the operating range and accuracy in the upper troposphere. The authors show that even with tight coincidence criterion, the quality of the profile pair comparisons varies considerably because of strong water vapor variability occurring on small time and space scales. Annual zonal means calculated from the set of profile pairs again finds SAGE II significantly drier in many latitude bands. Resolving the radiosonde data base by hygrometer type shows this to be true for all hygrometers except for the thin film capacitive type (Vaisala Humicap). For this hygrometer, between 4.5 and 6.5 km SAGE II is drier by approximately 25.%, and from 8.5 to 11.5 km they are nearly equivalent when global annual means are compared. The good agreement with the Vaisala Humicap, currently the most accurate and responsive hygrometer in operational use, suggests existing radiosonde climatologies contain a significant moist bias in the upper troposphere. 31 refs., 16 figs., 6 tabs.

  3. Estimation of Droplet Size and Liquid Water Content Using Radar and Lidar: Marine Cumulus Clouds

    NASA Astrophysics Data System (ADS)

    Vivekanandan, J. Vivek; Jensen, Jorgen; Ellis, Scott; Morley, Bruce; Tsai, Peisang; Spuler, Scott; Ghate, Virendra; Schwartz, Christian

    2016-04-01

    During the Cloud Systems Evolution in the Trades (CSET) field campaign airborne measurements from the High-Performance Instrumented Airborne Platform for Environmental Research (HIAPER) Cloud Radar (HCR) and the High Spectral Resolution Lidar (HSRL) were made in the North Pacific. In addition, in situ observations of cloud and aerosols size distributions and radiation were also collected. The HCR operated at a frequency of 94 GHz (3 mm wavelength) and collected observations at high temporal (0.5 sec) and range (30 m) resolution. The capability of HCR is enhanced by the coordination with the HSRL that made high temporal and range resolution observations of calibrated backscatter and extinction. The lidar, designed and built by the University of Wisconsin. The radar and lidar are designed to fly on the NCAR Gulfstream V HIAPER aircraft. The remote and in situ measurements collected during CSET offer opportunities for evaluating the engineering performance of the instruments and developing cloud microphysical scientific products. The coincident HCR and HSRL measurements are analyzed for assess their utility to characterize cloud boundaries, estimate liquid water content (LWC) and mean particle size. Retrievals of LWC and mean particle sizes from remote radar and lidar measurements will be compared with those from the in situ instruments.

  4. Submicron aerosol organic functional groups, ions, and water content at the Centreville SEARCH site (Alabama), during SOAS campaign

    NASA Astrophysics Data System (ADS)

    Ruggeri, G.; Ergin, G.; Modini, R. L.; Takahama, S.

    2013-12-01

    The SOAS campaign was conducted from June 1 to July 15 of 2013 in order to understand the relationship between biogenic and anthropogenic emissions in the South East US1,2. In this study, the organic and inorganic composition of submicron aerosol in the Centreville SEARCH site was measured by Fourier Transform Infrared Spectroscopy (FTIR) and the Ambient Ion Monitor (AIM; URG Corporation), whereas the aerosol water content was measured with a Dry Ambient Aerosol Size Spectrometer (DAASS)3. Organic functional group analysis was performed on PM1 aerosol selected by cyclone and collected on teflon filters with a time resolution of 4-12 hours, using one inlet heated to 50 °C and the other operated either at ambient temperature or 70 °C 4. The AIM measured both condensed and gas phase composition with a time resolution of 1 hour, providing partitioning behavior of inorganic species such as NH3/NH4+, HNO3/NO3-. These measurements collectively permit calculation of pure-component vapor pressures of candidate organic compounds and activity coefficients of interacting components in the condensed phase, using models such as SIMPOL.15, E-AIM6, and AIOMFAC7. From these results, the water content of the aerosol is predicted, and a comparison between modeled and measured partitioning of inorganic compounds and water vapor are discussed, in addition to organic aerosol volatility prediction based on functional group analysis. [1]- Goldstein, A.H., et al., Biogenic carbon and anthropogenic pollutants combine to form a cooling haze over the southeastern United States. Proceedings of the National Academy of Sciences of the United States of America, 2009. 106(22), 8835-8840. [2]- Carlton, A.G., Turpin, B.J., 2013. Particle partitioning potential of organic compounds is highest in the Eastern US and driven by anthropogenic water. Atmospheric Chemistry and Physics Discussions 13, 12743-12770. [3]- Khlystov, A., Stanier, C.O., Takahama, S., Pandis, S.N., 2005. Water content of ambient

  5. Water-soluble organic carbon, dicarboxylic acids, ketoacids, and α-dicarbonyls in the tropical Indian aerosols

    NASA Astrophysics Data System (ADS)

    Pavuluri, Chandra Mouli; Kawamura, Kimitaka; Swaminathan, T.

    2010-06-01

    Tropical aerosol (PM10) samples (n = 49) collected from southeast coast of India were studied for water-soluble dicarboxylic acids (C2-C12), ketocarboxylic acids (C2-C9), and α-dicarbonyls (glyoxal and methylglyoxal), together with analyses of total carbon (TC) and water-soluble organic carbon (WSOC). Their distributions were characterized by a predominance of oxalic acid followed by terephthalic (t-Ph), malonic, and succinic acids. Total concentrations of diacids (227-1030 ng m-3), ketoacids (16-105 ng m-3), and dicarbonyls (4-23 ng m-3) are comparative to those from other Asian megacities such as Tokyo and Hong Kong. t-Ph acid was found as the second most abundant diacid in the Chennai aerosols. This feature has not been reported previously in atmospheric aerosols. t-Ph acid is most likely derived from the field burning of plastics. Water-soluble diacids were found to contribute 0.4%-3% of TC and 4%-11% of WSOC. Based on molecular distributions and backward air mass trajectories, we found that diacids and related compounds in coastal South Indian aerosols are influenced by South Asian and Indian Ocean monsoons. Organic aerosols are also suggested to be significantly transported long distances from North India and the Middle East in early winter and from Southeast Asia in late winter, but some originate from photochemical reactions over the Bay of Bengal. In contrast, the Arabian Sea, Indian Ocean, and South Indian continent are suggested as major source regions in summer. We also found daytime maxima of most diacids, except for C9 and t-Ph acids, which showed nighttime maxima in summer. Emissions from marine and terrestrial plants, combined with land/sea breezes and in situ photochemical oxidation, are suggested especially in summer as an important factor that controls the composition of water-soluble organic aerosols over the southeast coast of India. Regional emissions from anthropogenic sources are also important in megacity Chennai, but their influence is

  6. Rapid determination of octanol-water partition coefficient using vortex-assisted liquid-liquid microextraction.

    PubMed

    Román, Iván P; Mastromichali, Anna; Tyrovola, Konstantina; Canals, Antonio; Psillakis, Elefteria

    2014-02-21

    Vortex-assisted liquid-liquid microextraction (VALLME) coupled with high-performance liquid chromatography (HPLC) is proposed here for the rapid determination of octanol-water partitioning coefficients (Kow). VALLME uses vortex agitation, a mild emulsification procedure, to disperse microvolumes of octanol in the aqueous phase thus increasing the interfacial contact area and ensuring faster partitioning rates. With VALLME, 2min were enough to achieve equilibrium conditions between the octanolic and aqueous phases. Upon equilibration, separation was achieved using centrifugation and the octanolic microdrop was collected and analyzed in a HPLC system. Six model compounds with logKow values ranging between ∼0.5 and 3.5 were used during the present investigations. The proposed method produced logKow values that were consistent with previously published values and the recorded uncertainty was well within the acceptable log unit range. Overall, the key features of the proposed Kow determination procedure comprised speed, reliability, simplicity, low cost and minimal solvent consumption.

  7. Response functions near the liquid-liquid critical point of ST2 water

    NASA Astrophysics Data System (ADS)

    Lascaris, Erik; Kesselring, T. A.; Franzese, G.; Buldyrev, S. V.; Herrmann, H. J.; Stanley, H. E.

    2013-02-01

    We simulate the ST2 water model for time periods up to 1000 ns, and for four different system sizes, N = 63, 73, 83, and 93. We locate the liquid-liquid phase transition line and its critical point in the supercooled region. Near the liquidliquid phase transition line, we observe that the system continuously flips between the low-density and high-density liquid phases. We analyze the transition line further by calculating two thermodynamic response functions, the isobaric specific heat capacity CP and the isothermal compressibility KT. We use two different methods: (i) from fluctuations and (ii) with the relevant thermodynamic derivative. We find that, within the accuracy of our simulations, the maxima of two different response functions occur at the same temperatures. The lines of CP and KT maxima below the critical pressure approximate the Widom line which is continuous with the line of first-order transitions in the two-phase region where we observe the phase flipping.

  8. Hygroscopic growth of water soluble organic carbon isolated from atmospheric aerosol collected at US national parks and Storm Peak Laboratory

    NASA Astrophysics Data System (ADS)

    Taylor, Nathan F.; Collins, Don R.; Lowenthal, Douglas H.; McCubbin, Ian B.; Gannet Hallar, A.; Samburova, Vera; Zielinska, Barbara; Kumar, Naresh; Mazzoleni, Lynn R.

    2017-02-01

    Due to the atmospheric abundance and chemical complexity of water soluble organic carbon (WSOC), its contribution to the hydration behavior of atmospheric aerosol is both significant and difficult to assess. For the present study, the hygroscopicity and CCN activity of isolated atmospheric WSOC particulate matter was measured without the compounding effects of common, soluble inorganic aerosol constituents. WSOC was extracted with high purity water from daily high-volume PM2.5 filter samples and separated from water soluble inorganic constituents using solid-phase extraction. The WSOC filter extracts were concentrated and combined to provide sufficient mass for continuous generation of the WSOC-only aerosol over the combined measurement time of the tandem differential mobility analyzer and coupled scanning mobility particle sizer-CCN counter used for the analysis. Aerosol samples were taken at Great Smoky Mountains National Park during the summer of 2006 and fall-winter of 2007-2008; Mount Rainier National Park during the summer of 2009; Storm Peak Laboratory (SPL) near Steamboat Springs, Colorado, during the summer of 2010; and Acadia National Park during the summer of 2011. Across all sampling locations and seasons, the hygroscopic growth of WSOC samples at 90 % RH, expressed in terms of the hygroscopicity parameter, κ, ranged from 0.05 to 0.15. Comparisons between the hygroscopicity of WSOC and that of samples containing all soluble materials extracted from the filters implied a significant modification of the hydration behavior of inorganic components, including decreased hysteresis separating efflorescence and deliquescence and enhanced water uptake between 30 and 70 % RH.

  9. The Effects of Transpacific Transported Aerosol on Clouds in California

    NASA Astrophysics Data System (ADS)

    Suski, K.; Creamean, J.; Rosenfeld, D.; Cazorla, A.; DeMott, P. J.; Sullivan, R. C.; White, A. B.; Ralph, F. M.; Cahill, J.; Tomlinson, J. M.; Chand, D.; Schmid, B.; Prather, K. A.

    2012-12-01

    Atmospheric aerosols are frequently lofted high into the atmosphere and can travel large distances within several days. Long-range transported aerosols can have large impacts on radiative and microphysical cloud properties and can affect precipitation on both regional and global scales. Research flights were conducted out of Sacramento, California onboard the DOE G-1 aircraft during the CalWater 2011 flight campaign, which aimed to understand the effects of aerosols on clouds and precipitation in California. To investigate aerosol effects on clouds, measurements of cloud microphysical properties were coupled with an aircraft aerosol time-of-flight mass spectrometer (A-ATOFMS), which characterized the chemical composition of aerosols and cloud residues. California Central Valley pollution aerosols were hypothesized to have a large impact on orographic clouds in the California Sierra Nevada Mountains; however transpacific transported aerosols were observed in cloud residues on several flights. Our observations indicate that dust from Asia, Africa, and the Middle East initiated ice formation in upper level clouds, while Asian soot from biomass burning served as cloud condensation nuclei in clouds with large concentrations of small liquid droplets. Previous work has linked large concentrations of small droplets to suppression of orographic precipitation, while ice formation has been shown to enhance precipitation. Therefore, the overall impact of these competing effects on precipitation in the Sierra Nevada is highly uncertain. The varying impacts of long-range transported aerosols on clouds and precipitation in California are presented.

  10. Ionic liquid-based ultrasound-assisted dispersive liquid-liquid microextraction followed high-performance liquid chromatography for the determination of ultraviolet filters in environmental water samples.

    PubMed

    Zhang, Yufeng; Lee, Hian Kee

    2012-10-31

    In the present study, a rapid, highly efficient and environmentally friendly sample preparation method named ionic liquid-based ultrasound-assisted dispersive liquid-liquid microextraction (IL-USA-DLLME), followed by high performance liquid chromatography (HPLC) has been developed for the extraction and preconcentration of four benzophenone-type ultraviolet (UV) filters (viz. benzophenone (BP), 2-hydroxy-4-methoxybenzophenone (BP-3), ethylhexyl salicylate (EHS) and homosalate (HMS)) from three different water matrices. The procedure was based on a ternary solvent system containing tiny droplets of ionic liquid (IL) in the sample solution formed by dissolving an appropriate amount of the IL extraction solvent 1-hexyl-3-methylimidazolium tris(pentafluoroethyl)trifluorophosphate ([HMIM][FAP]) in a small amount of water-miscible dispersive solvent (methanol). An ultrasound-assisted process was applied to accelerate the formation of the fine cloudy solution, which markedly increased the extraction efficiency and reduced the equilibrium time. Various parameters that affected the extraction efficiency (such as type and volume of extraction and dispersive solvents, ionic strength, pH and extraction time) were evaluated. Under optimal conditions, the proposed method provided good enrichment factors in the range of 354-464, and good repeatability of the extractions (RSDs below 6.3%, n=5). The limits of detection were in the range of 0.2-5.0 ng mL(-1), depending on the analytes. The linearities were between 1 and 500 ng mL(-1) for BP, 5 and 500 ng mL(-1) for BP-3 and HMS and 10 and 500 ng mL(-1) for EHS. Finally, the proposed method was successfully applied to the determination of UV filters in river, swimming pool and tap water samples and acceptable relative recoveries over the range of 71.0-118.0% were obtained.

  11. IR spectra of water droplets in no man's land and the location of the liquid-liquid critical point.

    PubMed

    Ni, Yicun; Skinner, J L

    2016-09-28

    No man's land is the region in the metastable phase diagram of water where it is very difficult to do experiments on liquid water because of homogeneous nucleation to the crystal. There are a number of estimates of the location in no man's land of the liquid-liquid critical point, if it exists. We suggest that published IR absorption experiments on water droplets in no man's land can provide information about the correct location. To this end, we calculate theoretical IR spectra for liquid water over a wide range of temperatures and pressures, using our E3B3 model, and use the results to argue that the temperature dependence of the experimental spectra is inconsistent with several of the estimated critical point locations, but consistent with others.

  12. Airborne differential absorption lidar system for measurements of atmospheric water vapor and aerosols.

    PubMed

    Higdon, N S; Browell, E V; Ponsardin, P; Grossmann, B E; Butler, C F; Chyba, T H; Mayo, M N; Allen, R J; Heuser, A W; Grant, W B; Ismail, S; Mayor, S D; Carter, A F

    1994-09-20

    An airborne differential absorption lidar (DIAL) system has been developed at the NASA Langley Research Center for remote measurements of atmospheric water vapor (H(2)O) and aerosols. A solid-state alexandrite laser with a 1-pm linewidth and > 99.85% spectral purity was used as the on-line transmitter. Solid-state avalanche photodiode detector technology has replaced photomultiplier tubes in the receiver system, providing an average increase by a factor of 1.5-2.5 in the signal-to-noise ratio of the H(2)O measurement. By incorporating advanced diagnostic and data-acquisition instrumentation into other subsystems, we achieved additional improvements in system operational reliability and measurement accuracy. Laboratory spectroscopic measurements of H(2)O absorption-line parameters were perfo med to reduce the uncertainties in our knowledge of the absorption cross sections. Line-center H(2)O absorption cross sections were determined, with errors of 3-6%, for more than 120 lines in the 720-nm region. Flight tests of the system were conducted during 1989-1991 on the NASA Wallops Flight Facility Electra aircraft, and extensive intercomparison measurements were performed with dew-point hygrometers and H(2)O radiosondes. The H(2)O distributions measured with the DIAL system differed by ≤ 10% from the profiles determined with the in situ probes in a variety of atmospheric conditions.

  13. Airborne differential absorption lidar system for measurements of atmospheric water vapor and aerosols

    NASA Technical Reports Server (NTRS)

    Carter, Arlen F.; Allen, Robert J.; Mayo, M. Neale; Butler, Carolyn F.; Grossman, Benoist E.; Ismail, Syed; Grant, William B.; Browell, Edward V.; Higdon, Noah S.; Mayor, Shane D.; Ponsardin, Patrick; Hueser, Alene W.

    1994-01-01

    An airborne differential absorption lidar (DIAL) system has been developed at the NASA Langley Research Center for remote measurements of atmospheric water vapor (H2O) and aerosols. A solid-state alexandrite laser with a 1-pm linewidth and greater than 99.85% spectral purity was used as the on-line transmitter. Solid-state avalanche photodiode detector technology has replaced photomultiplier tubes in the receiver system, providing an average increase by a factor of 1.5-2.5 in the signal-to-noise ratio of the H2O measurement. By incorporating advanced diagnostic and data-acquisition instrumentation into other subsystems, we achieved additional improvements in system operational reliability and measurement accuracy. Laboratory spectroscopic measurements of H2O absorption-line parameters were performed to reduce the uncertainties in our knowledge of the absorption cross sections. Line-center H2O absorption cross sections were determined, with errors of 3-6%, for more than 120 lines in the 720-nm region. Flight tests of the system were conducted during 1989-1991 on the NASA Wallops Flight Facility Electra aircraft, and extensive intercomparison measurements were performed with dew-point hygrometers and H2O radiosondes. The H2O distributions measured with the DIAL system differed by less than 10% from the profiles determined with the in situ probes in a variety of atmospheric conditions.

  14. Quantitation of antioxidants in water samples using ionic liquid dispersive liquid-liquid microextraction followed by high-performance liquid chromatography-ultraviolet detection.

    PubMed

    Sobhi, Hamid Reza; Kashtiaray, Amir; Farahani, Hadi; Farahani, Mohammad Reza

    2011-01-01

    A simple and efficient method, ionic liquid-based dispersive liquid-liquid microextraction combined with high-performance liquid chromatography-ultraviolet detection (HPLC-UV), has been applied for the extraction and determination of some antioxidants (Irganox 1010, Irganox 1076 and Irgafos 168) in water samples. The microextraction efficiency factors were investigated and optimized: 1-hexyl-3-methylimidazolium hexafluorophosphate [C(6)MIM][PF(6)] (0.06 g) as extracting solvent, methanol (0.5 mL) as disperser solvent without salt addition. Under the selected conditions, enrichment factors up to 48-fold, limits of detection (LODs) of 5.0-10.0 ng/mL and dynamic linear ranges of 25-1500 ng/mL were obtained. A reasonable repeatability (RSD≤11.8%, n=5) with satisfactory linearity (r(2)≥0.9954) of the results illustrated a good performance of the presented method. The accuracy of the method was tested by the relative recovery experiments on spiked samples, with results ranging from 85 to 118%. Finally, the method was successfully applied for determination of the analytes in several real water samples.

  15. Impact of Mars Water Ice Clouds and Thermal Aerosol Enforcement to the Shortscale Climate Dynamics: Evidence from 1-D Model

    NASA Astrophysics Data System (ADS)

    Rodin, A. V.; Clancy, R. T.; Wilson, R. J.; Richardson, M.; Wolff, M.; Woods, S.

    1997-07-01

    Ground-based observations of Mars atmospheric temperatures, water, and aerosols have suggested that water ice clouds may regulate vertical distribution of dust and, hence, the global radiation balance, with strong seasonal forcing (Clancy et al., 1996). Under specific Martian conditions, condensation of atmospheric water occurs on the dust as Aitken cores, without external sources, dust is efficiently confined below the saturation level of water vapor. This in turn forces the thermal regime and the saturation conditions, particularly around the aphelion northern summer (Clancy et al., 1996). This effect is studied with two 1-D models, a time marching simulation (time step is 4 min), and reduced local steady-state model. Both models treat aerosol particle microphysics, turbulent transport and thermal enforcement interactively, including radiation transfer consistent with derived aerosol vertical and size distributions. Simulations show that in the aphelion season, when clouds are formed below or near 10 km, strong nonlinearity of cloud thermal feedback results in nonuniqueness of a steady-state solution with water vapor saturation level varying by as high as 5-7 km. Such model behavior appears related to observations of rapid variations of a global-average, lower atmosphere temperature over the planet in northern summer (Clancy, 1997). The stability of thermal equilibrium state is controlled by water vapor abundance and the strength of the dust source at the surface. Time marching simulations provide access to the dynamics of seasonal global dust storm relaxation that may play an important role in interannual climate variations on Mars. References: Clancy, R.T., A.W. Grossman, M.J. Wolff, P.B. James, Y.N. Billawala, B.J. Sandor, S.W. Lee, and D.J. Rudy. Water vapor saturation at low altitudes around Mars aphelion: A key to Mars climate? Icarus, 122, 36-62, 1996.

  16. Ionic liquid-based dispersive liquid-liquid microextraction followed high-performance liquid chromatography for the determination of organophosphorus pesticides in water sample.

    PubMed

    He, Lijun; Luo, Xianli; Xie, Hongxue; Wang, Chunjian; Jiang, Xiuming; Lu, Kui

    2009-11-23

    Using 1-octyl-3-methylimidazolium hexafluorophosphate ([C(8)MIM][PF(6)]) ionic liquid as extraction solvent, organophosphorus pesticides (OPPs) (parathion, phoxim, phorate and chlorpyifos) in water were determined by dispersive liquid-liquid microextraction (DLLME) combined with high-performance liquid chromatography (HPLC). The extraction procedure was induced by the formation of cloudy solution, which was composed of fine drops of [C(8)MIM][PF(6)] dispersed entirely into sample solution with the help of disperser solvent (methanol). Parameters including extraction solvent and its volume, disperser solvent and its volume, extraction time, centrifugal time, salt addition, extraction temperature and sample pH were investigated and optimized. Under the optimized conditions, up to 200-fold enrichment factor of analytes and acceptable extraction recovery (>70%) were obtained. The calibration curves were linear in the concentration range of 10.5-1045.0 microg L(-1) for parathion, 10.2-1020.0 microg L(-1) for phoxim, 54.5-1089.0 microg L(-1) for phorate and 27.2-1089.0 microg L(-1) for chlorpyifos, respectively. The limits of detection calculated at a signal-to-noise ratio of 3 were in the range of 0.1-5.0 microg L(-1). The relative standard deviations for seven replicate experiments at 200 microg L(-1) concentration level were less than 4.7%. The proposed method was applied to the analysis of four different sources water samples (tap, well, rain and Yellow River water) and the relative recoveries of spiked water samples are 99.9-115.4%, 101.8-113.7% and 87.3-117.6% at three different concentration levels of 75, 200 and 1000 microg L(-1), respectively.

  17. Aerosol-Cloud Interactions in the South-East Atlantic

    NASA Astrophysics Data System (ADS)

    Andersen, Hendrik; Cermak, Jan

    2014-05-01

    In this contribution, a satellite-based study on aerosol-cloud interactions (ACI) in the South-East Atlantic with explicit consideration of meteorological conditions is presented. Aerosol-Cloud Interactions remain difficult to quantify and contribute the largest uncertainty to global radiative forcing. These uncertainties make them one of the most important factors for anthropogenic climate perturbations. Interactions are highly complex as microphysical and macrostructural cloud adjustments to aerosol perturbations do not transpire in a black box but are highly dependent on a variety of factors like cloud regime, meteorology and aerosol properties. To gain understanding of the processes that govern ACI in order to increase accuracy of climate models and predictions of future changes in the climate system is thus of great importance. This process study uses multiple statistical approaches to untangle the various influences on ACI. Stratocumulus clouds in the South-East Atlantic are investigated over a time span of 10 years using daily Terra MODIS L3 data for aerosol and cloud parameters. Together with ERA-Interim reanalysis data of cloud-relevant meteorological parameters, statistical relationships between aerosol and cloud properties are derived for different weather types on the basis of a kmeans cluster analysis, in addition to bivariate relationships. Also, the influence of aerosol loading on aerosol-cloud relationships is investigated. Relationships between aerosol and cloud microphysical properties are established. Macrostructural cloud adjustments are more ambiguous, as the observed positive relationship between aerosol and cloud liquid water path (LWP) is inconsistent with the Albrecht hypothesis (more cloud water due to drizzle suppression). Adjustments of cloud optical thickness (COT) to aerosol perturbations are negligible as COT is highly dependent on LWP. Strong relationships between aerosol and cloud fraction are identified, but might be spurious and

  18. Temporal changes in endmember abundances,