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Sample records for aerosol activation parameterization

  1. Parameterization of the influence of organic surfactants on aerosol activation

    NASA Astrophysics Data System (ADS)

    Abdul-Razzak, Hayder; Ghan, Steven J.

    2004-02-01

    Surface-active organic compounds, or surfactants, can affect aerosol activation by two mechanisms: lowering surface tension and altering the bulk hygroscopicity of the particles. A numerical model has been developed to predict the activation of aerosol particles consisting of an internally uniform chemical mixture of organic surfactants and inorganic salts in a parcel of air rising adiabatically at constant speed. Equations reflecting water balance of the air parcel were used together with a modified form of Köhler theory to model droplet nucleation while considering surface effects. We also extend a parametric representation of aerosol activation to the case of a mixture of inorganic salts and organic surfactants by modifying the Raoult term in Köhler theory (assuming additive behavior) and using a simplified relationship between surface tension and surfactant molar concentration to account for surface effects at the critical radius for activation. The close agreement (to within 10% for most and 20% for almost all conditions) between numerical and parametric results validates our modifications. Moreover, the form of the relationship is identical to an empirical relationship between surface tension and organic carbon concentration. Thus the modified form of the parameterization provides a framework that can account for the influence of observed organics on the activation of other salts. The modified form of the parameterization is tested successfully with the Po Valley model both for single aerosol size distribution and three-mode size distributions for marine, rural, and urban aerosols. Further measurements are required to extend the parameterization to other organic surfactants.

  2. Incorporating an advanced aerosol activation parameterization into WRF-CAM5: Model evaluation and parameterization intercomparison

    SciTech Connect

    Zhang, Yang; Zhang, Xin; Wang, Kai; He, Jian; Leung, Lai-Yung R.; Fan, Jiwen; Nenes, Athanasios

    2015-07-22

    Aerosol activation into cloud droplets is an important process that governs aerosol indirect effects. The advanced treatment of aerosol activation by Fountoukis and Nenes (2005) and its recent updates, collectively called the FN series, have been incorporated into a newly developed regional coupled climate-air quality model based on the Weather Research and Forecasting model with the physics package of the Community Atmosphere Model version 5 (WRF-CAM5) to simulate aerosol-cloud interactions in both resolved and convective clouds. The model is applied to East Asia for two full years of 2005 and 2010. A comprehensive model evaluation is performed for model predictions of meteorological, radiative, and cloud variables, chemical concentrations, and column mass abundances against satellite data and surface observations from air quality monitoring sites across East Asia. The model performs overall well for major meteorological variables including near-surface temperature, specific humidity, wind speed, precipitation, cloud fraction, precipitable water, downward shortwave and longwave radiation, and column mass abundances of CO, SO2, NO2, HCHO, and O3 in terms of both magnitudes and spatial distributions. Larger biases exist in the predictions of surface concentrations of CO and NOx at all sites and SO2, O3, PM2.5, and PM10 concentrations at some sites, aerosol optical depth, cloud condensation nuclei over ocean, cloud droplet number concentration (CDNC), cloud liquid and ice water path, and cloud optical thickness. Compared with the default Abdul-Razzack Ghan (2000) parameterization, simulations with the FN series produce ~107–113% higher CDNC, with half of the difference attributable to the higher aerosol activation fraction by the FN series and the remaining half due to feedbacks in subsequent cloud microphysical processes. With the higher CDNC, the FN series are more skillful in simulating cloud water path, cloud optical thickness, downward shortwave radiation

  3. Regional Biases in Droplet Activation Parameterizations: Strong Influence on Aerosol Second Indirect Effect in the Community Atmosphere Model v5.

    NASA Astrophysics Data System (ADS)

    Morales, R.; Nenes, A.

    2014-12-01

    Aerosol-cloud interactions constitute one of the most uncertain aspects of anthropogenic climate change estimates. The magnitude of these interactions as represented in climate models strongly depends on the process of aerosol activation. This process is the most direct physical link between aerosols and cloud microphysical properties. Calculation of droplet number in GCMs requires the computation of new droplet formation (i.e., droplet activation), through physically based activation parameterizations. Considerable effort has been placed in ensuring that droplet activation parameterizations have a physically consistent response to changes in aerosol number concentration. However, recent analyses using an adjoint sensitivity approach showed that parameterizations can exhibit considerable biases in their response to other aerosol properties, such as aerosol modal diameter or to the aerosol chemical composition. This is a potentially important factor in estimating aerosol indirect effects since changes in aerosol properties from pre-industrial times to present day exhibit a very strong regional signature. In this work we use the Community Atmosphere Model (CAM5) to show that the regional imprint of the changes in aerosol properties during the last century interacts with the droplet activation parameterization in a way that these biases are amplified over climatically relevant regions. Two commonly used activation routines, the CAM5 default, Abdul-Razzak and Ghan parameterization, as well as the Fountoukis and Nenes parameterization are used in this study. We further explored the impacts of Nd parameterization biases in the first and second aerosol indirect effects separately, by performing simulations were droplet number was not allowed to intervene in the precipitation initiation process. The simulations performed show that an unphysical response to changes in the diameter of accumulation mode aerosol translates into extremely high Nd concentrations over South

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

    NASA Astrophysics Data System (ADS)

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

    2006-12-01

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

  5. Aerosol hygroscopicity and CCN activity during the AC3Exp campaign: Implications for CCN parameterization

    NASA Astrophysics Data System (ADS)

    Zhang, Fang; Li, Yanan; Li, Zhanqing

    2015-04-01

    Atmospheric aerosol particles acting as CCN are pivotal elements of the hydrological cycle and climate change. In this study, we measured and characterized NCCN in relatively clean and polluted air during the AC3Exp campaign conducted at Xianghe, China during summer 2013. The aim was to examine CCN activation properties under high aerosol loading conditions in a polluted region and to assess the impacts of particle size and chemical composition on the CCN AR which acts as a proxy of the total number of aerosol particles in the atmosphere. A gradual increase in size-resolved AR with particle diameter suggests that aerosol particles have different hygroscopicities. For particles in the accumulation mode, values of κapa range from 0.31-0.38 under background conditions, which is about 20% higher than that derived under polluted conditions. For particles in the nucleation or Aitken mode, κ range from 0.20-0.34 under both background and polluted conditions. Larger particles were on average more hygroscopic than smaller particles. However, the case is more complex for particles originating from heavy pollution due to the diversity in particle composition and mixing state. The low R2 for the NPO CCN closure test suggests a 30%-40% uncertainty in total NCCN estimation. Using bulk chemical composition data from ACSM measurements, the relationship between bulk AR and the physical and chemical properties of atmospheric aerosols is investigated. Based on a case study, it has been concluded that one cannot use a parameterized formula using only total NCN to estimate total NCCN. Our results showed a possibility of using bulk κchem and f44 in combination with bulk NCN > 100 nm to parameterize CCN number concentrations.

  6. Hygroscopic growth and activation of HULIS particles: experimental data and a new iterative parameterization scheme for complex aerosol particles

    NASA Astrophysics Data System (ADS)

    Ziese, M.; Wex, H.; Nilsson, E.; Salma, I.; Ocskay, R.; Hennig, T.; Massling, A.; Stratmann, F.

    2008-03-01

    The hygroscopic growth and activation of two HULIS (HUmic LIke Substance) and one Aerosol-Water-Extract sample, prepared from urban-type aerosol, were investigated. All samples were extracted from filters, redissolved in water and atomized for the investigations presented here. The hygroscopic growth measurements were done using LACIS (Leipzig Aerosol Cloud Interaction Simulator) together with a HH-TDMA (High Humidity Tandem Differential Mobility Analyzer). Hygroscopic growth was determined for relative humidities (RHs) up to 99.75%. The critical diameters for activation were measured for supersaturations between 0.2 and 1%. All three samples showed a similar hygroscopic growth behavior, and the two HULIS samples also were similar in their activation behavior, while the Aerosol-Water-Extract turned out to be more CCN active than the HULIS samples. The experimental data was used to derive parameterizations for the hygroscopic growth and activation of HULIS particles. The concept of ρion (Wex et al., 2007a) and the Szyszkowski-equation (Szyszkowski, 1908; Facchini, 1999) were used for parameterizing the Raoult and the Kelvin (surface tension) terms of the Köhler equation, respectively. This concept proved to be very successful for the HULIS samples in the saturation range from RHs larger than 98% up to activation. It was also shown to work well with data on HULIS taken from literature. Here, different atmospheric life-times and/or different sources for the different samples showed up in different coefficients for the parameterization. However, the parameterization did not work out well for the Aerosol-Water-Extract.

  7. Hygroscopic growth and activation of HULIS particles: experimental data and a new iterative parameterization scheme for complex aerosol particles

    NASA Astrophysics Data System (ADS)

    Ziese, M.; Wex, H.; Nilsson, E.; Salma, I.; Ocskay, R.; Hennig, T.; Massling, A.; Stratmann, F.

    2007-09-01

    The hygroscopic growth and activation of two HULIS and one Aerosol-Water-Extract sample, prepared from urban-type aerosol, were investigated. All samples were extracted from filters, redissolved in water and atomized for the investigations presented here. The hygroscopic growth measurements were done using LACIS (Leipzig Aerosol Cloud Interaction Simulator) together with a HH-TDMA (High Humidity Tandem Differential Mobility Analyzer). Hygroscopic growth was determined for relative humidities up to 99.75%. The critical diameters for activation were measured using LACIS for supersaturations between 2 and 10 per mill. All three samples showed a similar hygroscopic growth behaviour, and the two HULIS samples also were similar in their activation behavior, while the Aerosol-Water-Extract turned out to be more CCN active than the HULIS samples. The experimental data was used to derive parameterizations for the hygroscopic growth and activation of HULIS particles. The concept of ρion (Wex et al., 2007a) and the Szyszkowski-equation (Szyszkowski, 1908; Facchini et al., 1999) were used for parameterizing the Raoult and the Kelvin (surface tension) terms of the Köhler equation, respectively. This concept proved to be very successful for the HULIS samples in the saturation range from relative humidities larger than 98% up to activation. However it failed for the Aerosol-Water extract.

  8. Assessment of aerosol-cloud interactions during southern African biomass burning activity, employing cloud parameterizations

    NASA Astrophysics Data System (ADS)

    Wiston, Modise; McFiggans, Gordon; Schultz, David

    2015-04-01

    In this study, we perform a simulation of the spatial distributions of particle and gas concentrations from a significantly large source of pollution event during a dry season in southern Africa and their interactions with cloud processes. Specific focus is on the extent to which cloud-aerosol interactions are affected by various inputs (i.e. emissions) and parameterizations and feedback mechanisms in a coupled mesoscale chemistry-meteorology model -herein Weather Research and Forecasting model with chemistry (WRF-Chem). The southern African dry season (May-Sep) is characterised by biomass burning (BB) type of pollution. During this period, BB particles are frequently observed over the subcontinent, at the same time a persistent deck of stratocumulus covers the south West African coast, favouring long-range transport over the Atlantic Ocean of aerosols above clouds. While anthropogenic pollutants tend to spread more over the entire domain, biomass pollutants are concentrated around the burning areas, especially the savannah and tropical rainforest of the Congo Basin. BB is linked to agricultural practice at latitudes south of 10° N. During an intense burning event, there is a clear signal of strong interactions of aerosols and cloud microphysics. These species interfere with the radiative budget, and directly affect the amount of solar radiation reflected and scattered back to space and partly absorbed by the atmosphere. Aerosols also affect cloud microphysics by acting as cloud condensation nuclei (CCN), modifying precipitation pattern and the cloud albedo. Key area is to understand the role of pollution on convective cloud processes and its impacts on cloud dynamics. The hypothesis is that an environment of potentially high pollution enables the probability of interactions between co-located aerosols and cloud layers. To investigate this hypothesis, we outline an approach to integrate three elements: i) focusing on regime(s) where there are strong indications of

  9. Characterization and parameterization of aerosol cloud condensation nuclei activation under different pollution conditions.

    PubMed

    Che, H C; Zhang, X Y; Wang, Y Q; Zhang, L; Shen, X J; Zhang, Y M; Ma, Q L; Sun, J Y; Zhang, Y W; Wang, T T

    2016-01-01

    To better understand the cloud condensation nuclei (CCN) activation capacity of aerosol particles in different pollution conditions, a long-term field experiment was carried out at a regional GAW (Global Atmosphere Watch) station in the Yangtze River Delta area of China. The homogeneity of aerosol particles was the highest in clean weather, with the highest active fraction of all the weather types. For pollution with the same visibility, the residual aerosol particles in higher relative humidity weather conditions were more externally mixed and heterogeneous, with a lower hygroscopic capacity. The hygroscopic capacity (κ) of organic aerosols can be classified into 0.1 and 0.2 in different weather types. The particles at ~150 nm were easily activated in haze weather conditions. For CCN predictions, the bulk chemical composition method was closer to observations at low supersaturations (≤0.1%), whereas when the supersaturation was ≥0.2%, the size-resolved chemical composition method was more accurate. As for the mixing state of the aerosol particles, in haze, heavy haze, and severe haze weather conditions CCN predictions based on the internal mixing assumption were robust, whereas for other weather conditions, predictions based on the external mixing assumption were more accurate. PMID:27075947

  10. Characterization and parameterization of aerosol cloud condensation nuclei activation under different pollution conditions

    NASA Astrophysics Data System (ADS)

    Che, H. C.; Zhang, X. Y.; Wang, Y. Q.; Zhang, L.; Shen, X. J.; Zhang, Y. M.; Ma, Q. L.; Sun, J. Y.; Zhang, Y. W.; Wang, T. T.

    2016-04-01

    To better understand the cloud condensation nuclei (CCN) activation capacity of aerosol particles in different pollution conditions, a long-term field experiment was carried out at a regional GAW (Global Atmosphere Watch) station in the Yangtze River Delta area of China. The homogeneity of aerosol particles was the highest in clean weather, with the highest active fraction of all the weather types. For pollution with the same visibility, the residual aerosol particles in higher relative humidity weather conditions were more externally mixed and heterogeneous, with a lower hygroscopic capacity. The hygroscopic capacity (κ) of organic aerosols can be classified into 0.1 and 0.2 in different weather types. The particles at ~150 nm were easily activated in haze weather conditions. For CCN predictions, the bulk chemical composition method was closer to observations at low supersaturations (≤0.1%), whereas when the supersaturation was ≥0.2%, the size-resolved chemical composition method was more accurate. As for the mixing state of the aerosol particles, in haze, heavy haze, and severe haze weather conditions CCN predictions based on the internal mixing assumption were robust, whereas for other weather conditions, predictions based on the external mixing assumption were more accurate.

  11. Characterization and parameterization of aerosol cloud condensation nuclei activation under different pollution conditions

    PubMed Central

    Che, H. C.; Zhang, X. Y.; Wang, Y. Q.; Zhang, L.; Shen, X. J.; Zhang, Y. M.; Ma, Q. L.; Sun, J. Y.; Zhang, Y. W.; Wang, T. T.

    2016-01-01

    To better understand the cloud condensation nuclei (CCN) activation capacity of aerosol particles in different pollution conditions, a long-term field experiment was carried out at a regional GAW (Global Atmosphere Watch) station in the Yangtze River Delta area of China. The homogeneity of aerosol particles was the highest in clean weather, with the highest active fraction of all the weather types. For pollution with the same visibility, the residual aerosol particles in higher relative humidity weather conditions were more externally mixed and heterogeneous, with a lower hygroscopic capacity. The hygroscopic capacity (κ) of organic aerosols can be classified into 0.1 and 0.2 in different weather types. The particles at ~150 nm were easily activated in haze weather conditions. For CCN predictions, the bulk chemical composition method was closer to observations at low supersaturations (≤0.1%), whereas when the supersaturation was ≥0.2%, the size-resolved chemical composition method was more accurate. As for the mixing state of the aerosol particles, in haze, heavy haze, and severe haze weather conditions CCN predictions based on the internal mixing assumption were robust, whereas for other weather conditions, predictions based on the external mixing assumption were more accurate. PMID:27075947

  12. Observational Study and Parameterization of Aerosol-fog Interactions

    NASA Astrophysics Data System (ADS)

    Duan, J.; Guo, X.; Liu, Y.; Fang, C.; Su, Z.; Chen, Y.

    2014-12-01

    Studies have shown that human activities such as increased aerosols affect fog occurrence and properties significantly, and accurate numerical fog forecasting depends on, to a large extent, parameterization of fog microphysics and aerosol-fog interactions. Furthermore, fogs can be considered as clouds near the ground, and enjoy an advantage of permitting comprehensive long-term in-situ measurements that clouds do not. Knowledge learned from studying aerosol-fog interactions will provide useful insights into aerosol-cloud interactions. To serve the twofold objectives of understanding and improving parameterizations of aerosol-fog interactions and aerosol-cloud interactions, this study examines the data collected from fogs, with a focus but not limited to the data collected in Beijing, China. Data examined include aerosol particle size distributions measured by a Passive Cavity Aerosol Spectrometer Probe (PCASP-100X), fog droplet size distributions measured by a Fog Monitor (FM-120), Cloud Condensation Nuclei (CCN), liquid water path measured by radiometers and visibility sensors, along with meteorological variables measured by a Tethered Balloon Sounding System (XLS-Ⅱ) and Automatic Weather Station (AWS). The results will be compared with low-level clouds for similarities and differences between fogs and clouds.

  13. 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.

  14. Optimal Aerosol Parameterization for Remote Sensing Retrievals

    NASA Technical Reports Server (NTRS)

    Newchurch, Michael J.

    2004-01-01

    We have developed a new algorithm for the retrieval of aerosol and gases from SAGE It1 solar transmission measurements. This algorithm improves upon the NASA operational algorithm in several key aspects, including solving the problem non-linearly and incorporating a new methodology for separating the contribution of aerosols and gases. In order to extract aerosol information we have built a huge database of aerosol models for both stratospheric and tropospheric aerosols, and polar stratospheric cloud particles. This set of models allows us to calculate a vast range of possible extinction spectra for aerosols. and from these, derive a set of eigenvectors which then provide the basis set used in our inversion algorithm. Our aerosol algorithm and retrievals are described in several articles (listed in References Section) published under this grant. In particular they allow us to analyze the spectral properties of aerosols and PSCs and ultimately derive their microphysical properties. We have found some considerable differences between our spectra and the ones derived from the SAGE III operational algorithm. These are interesting as they provide an independent check on the validity of published aerosol data and, in particular, on their associated uncertainties. In order to understand these differences, we are assembling independent aerosol data from other sources with which to make comparisons. We have carried out extensive comparisons of our ozone retrievals with both SAGE III and independent lidar, ozonesonde, and satellite measurements (Polyakov et al., 2004). These show very good agreement throughout the stratosphere and help to quantify differences which can be attributed to natural variation in ozone versus that produced by algorithmic differences. In the mid - upper stratosphere, agreement with independent data was generally within 5 - 20%. but in the lower stratosphere the differences were considerably larger. We believe that a large proportion of this

  15. Parameterization of Aerosol Sinks in Chemical Transport Models

    NASA Technical Reports Server (NTRS)

    Colarco, Peter

    2012-01-01

    The modelers point of view is that the aerosol problem is one of sources, evolution, and sinks. Relative to evolution and sink processes, enormous attention is given to the problem of aerosols sources, whether inventory based (e.g., fossil fuel emissions) or dynamic (e.g., dust, sea salt, biomass burning). On the other hand, aerosol losses in models are a major factor in controlling the aerosol distribution and lifetime. Here we shine some light on how aerosol sinks are treated in modern chemical transport models. We discuss the mechanisms of dry and wet loss processes and the parameterizations for those processes in a single model (GEOS-5). We survey the literature of other modeling studies. We additionally compare the budgets of aerosol losses in several of the ICAP models.

  16. Aerosol effects on stratocumulus water paths in a PDF-based parameterization

    NASA Astrophysics Data System (ADS)

    Guo, H.; Golaz, J.-C.; Donner, L. J.

    2011-09-01

    Successful simulation of aerosol indirect effects in climate models requires parameterizations that capture the full range of cloud-aerosol interactions, including positive and negative liquid water path (LWP) responses to increasing aerosol concentrations, as suggested by large eddy simulations (LESs). A parameterization based on multi-variate probability density functions with dynamics (MVD PDFs) has been incorporated into the single-column version of GFDL AM3, extended to treat aerosol activation, and coupled with a two-moment microphysics scheme. We use it to explore cloud-aerosol interactions. In agreement with LESs, our single-column simulations produce both positive and negative LWP responses to increasing aerosol concentrations, depending on precipitation and free atmosphere relative humidity. We have conducted sensitivity tests to vertical resolution and droplet sedimentation parameterization. The dependence of sedimentation on cloud droplet size is essential to capture the full LWP responses to aerosols. Further analyses reveal that the MVD PDFs are able to represent changes in buoyancy profiles induced by sedimentation as well as enhanced entrainment efficiency with aerosols comparable to LESs.

  17. Research on aerosol profiles and parameterization scheme in Southeast China

    NASA Astrophysics Data System (ADS)

    Wang, Gang; Deng, Tao; Tan, Haobo; Liu, Xiantong; Yang, Honglong

    2016-09-01

    The vertical distribution of the aerosol extinction coefficient serves as a basis for evaluating aerosol radiative forcing and air quality modeling. In this study, MODIS AOD data and ground-based lidar extinction coefficients were employed to verify 6 years (2009-2014) aerosol extinction data obtained via CALIOP for Southeast China. The objective was mainly to provide the parameterization scheme of annual and seasonal aerosol extinction profiles. The results showed that the horizontal and vertical distributions of CALIOP extinction data were highly accurate in Southeast China. The annual average AOD below 2 km accounted for 64% of the total layer, with larger proportions observed in winter (80%) and autumn (80%) and lower proportions observed in summer (70%) and spring (59%). The AOD was maximum in the spring (0.58), followed by the autumn and winter (0.44), and reached a minimum in the summer (0.40). The near-surface extinction coefficient increased from summer, spring, autumn and winter, in that order. The Elterman profile is obviously lower than the profiles observed by CALIOP in Southeast China. The annual average and seasonal aerosol profiles showed an exponential distribution, and could be divided into two sections. Two sections exponential fitting was used in the parameterization scheme. In the first section, the aerosol scale height reached 2200 m with a maximum (3,500 m) in summer and a minimum (1,230 m) in winter, which meant that the aerosol extinction decrease with height slower in summer, but more rapidly in winter. In second section, the aerosol scale height was maximum in spring, which meant that the higher aerosol diffused in spring.

  18. A numerical model of aerosol scavenging: Part 1, Microphysics parameterization

    SciTech Connect

    Molenkamp, C.R.; Bradley, M.M.

    1991-09-01

    We have developed a three-dimensional numerical model (OCTET) to simulate the dynamics and microphysics of clouds and the transport, diffusion and precipitation scavenging of aerosol particles. In this paper we describe the cloud microphysics and scavenging parameterizations. The representation of cloud microphysics is a bulk- water parameterization which includes water vapor and five types of hydrometeors (cloud droplets, rain drops, ice crystals, snow, and graupel). A parallel parameterization represents the scavenging interactions between pollutant particles and hydrometeors including collection of particles because of condensation nucleation, Brownian and phoretic attachment, and inertial capture, resuspension because of evaporation and sublimation; and transfer interactions where particles collected by one type of hydrometeor are transferred to another type of freezing, melting, accretion, riming and autoconversion.

  19. A simple parameterization of aerosol emissions in RAMS

    NASA Astrophysics Data System (ADS)

    Letcher, Theodore

    Throughout the past decade, a high degree of attention has been focused on determining the microphysical impact of anthropogenically enhanced concentrations of Cloud Condensation Nuclei (CCN) on orographic snowfall in the mountains of the western United States. This area has garnered a lot of attention due to the implications this effect may have on local water resource distribution within the Region. Recent advances in computing power and the development of highly advanced microphysical schemes within numerical models have provided an estimation of the sensitivity that orographic snowfall has to changes in atmospheric CCN concentrations. However, what is still lacking is a coupling between these advanced microphysical schemes and a real-world representation of CCN sources. Previously, an attempt to representation the heterogeneous evolution of aerosol was made by coupling three-dimensional aerosol output from the WRF Chemistry model to the Colorado State University (CSU) Regional Atmospheric Modeling System (RAMS) (Ward et al. 2011). The biggest problem associated with this scheme was the computational expense. In fact, the computational expense associated with this scheme was so high, that it was prohibitive for simulations with fine enough resolution to accurately represent microphysical processes. To improve upon this method, a new parameterization for aerosol emission was developed in such a way that it was fully contained within RAMS. Several assumptions went into generating a computationally efficient aerosol emissions parameterization in RAMS. The most notable assumption was the decision to neglect the chemical processes in formed in the formation of Secondary Aerosol (SA), and instead treat SA as primary aerosol via short-term WRF-CHEM simulations. While, SA makes up a substantial portion of the total aerosol burden (much of which is made up of organic material), the representation of this process is highly complex and highly expensive within a numerical

  20. Improving bulk microphysics parameterizations in simulations of aerosol effects

    NASA Astrophysics Data System (ADS)

    Wang, Yuan; Fan, Jiwen; Zhang, Renyi; Leung, L. Ruby; Franklin, Charmaine

    2013-06-01

    To improve the microphysical parameterizations for simulations of the aerosol effects in regional and global climate models, the Morrison double-moment bulk microphysical scheme presently implemented in the Weather Research and Forecasting model is modified by replacing the prescribed aerosols in the original bulk scheme (Bulk-OR) with a prognostic double-moment aerosol representation to predict both aerosol number concentration and mass mixing ratio (Bulk-2M). Sensitivity modeling experiments are performed for two distinct cloud regimes: maritime warm stratocumulus clouds (Sc) over southeast Pacific Ocean from the VOCALS project and continental deep convective clouds in the southeast of China. The results from Bulk-OR and Bulk-2M are compared against atmospheric observations and simulations produced by a spectral bin microphysical scheme (SBM). The prescribed aerosol approach (Bulk-OR) produces unreliable aerosol and cloud properties throughout the simulation period, when compared to the results from those using Bulk-2M and SBM, although all of the model simulations are initiated by the same initial aerosol concentration on the basis of the field observations. The impacts of the parameterizations of diffusional growth and autoconversion of cloud droplets and the selection of the embryonic raindrop radius on the performance of the bulk microphysical scheme are also evaluated by comparing the results from the modified Bulk-2M with those from SBM simulations. Sensitivity experiments using four different types of autoconversion schemes reveal that the autoconversion parameterization is crucial in determining the raindrop number, mass concentration, and drizzle formation for warm stratocumulus clouds. An embryonic raindrop size of 40 µm is determined as a more realistic setting in the autoconversion parameterization. The saturation adjustment employed in calculating condensation/evaporation in the bulk scheme is identified as the main factor responsible for the large

  1. Improving Bulk Microphysics Parameterizations in Simulations of Aerosol Effects

    SciTech Connect

    Wang, Yuan; Fan, Jiwen; Zhang, Renyi; Leung, Lai-Yung R.; Franklin, Charmaine N.

    2013-06-05

    To improve the microphysical parameterizations for simulations of the aerosol indirect effect (AIE) in regional and global climate models, a double-moment bulk microphysical scheme presently implemented in the Weather Research and Forecasting (WRF) model is modified and the results are compared against atmospheric observations and simulations produced by a spectral bin microphysical scheme (SBM). Rather than using prescribed aerosols as in the original bulk scheme (Bulk-OR), a prognostic doublemoment aerosol representation is introduced to predict both the aerosol number concentration and mass mixing ratio (Bulk-2M). The impacts of the parameterizations of diffusional growth and autoconversion and the selection of the embryonic raindrop radius on the performance of the bulk microphysical scheme are also evaluated. Sensitivity modeling experiments are performed for two distinct cloud regimes, maritime warm stratocumulus clouds (SC) over southeast Pacific Ocean from the VOCALS project and continental deep convective clouds (DCC) in the southeast of China from the Department of Energy/ARM Mobile Facility (DOE/AMF) - China field campaign. The results from Bulk-2M exhibit a much better agreement in the cloud number concentration and effective droplet radius in both the SC and DCC cases with those from SBM and field measurements than those from Bulk-OR. In the SC case particularly, Bulk-2M reproduces the observed drizzle precipitation, which is largely inhibited in Bulk-OR. Bulk-2M predicts enhanced precipitation and invigorated convection with increased aerosol loading in the DCC case, consistent with the SBM simulation, while Bulk-OR predicts the opposite behaviors. Sensitivity experiments using four different types of autoconversion schemes reveal that the autoconversion parameterization is crucial in determining the raindrop number, mass concentration, and drizzle formation for warm 2 stratocumulus clouds. An embryonic raindrop size of 40 μm is determined as a more

  2. A sea spray aerosol flux parameterization encapsulating wave state

    NASA Astrophysics Data System (ADS)

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

    2014-02-01

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

  3. Development and testing of an aerosol-stratus cloud parameterization scheme for middle and high latitudes

    SciTech Connect

    Olsson, P.Q.; Meyers, M.P.; Kreidenweis, S.; Cotton, W.R.

    1996-04-01

    The aim of this new project is to develop an aerosol/cloud microphysics parameterization of mixed-phase stratus and boundary layer clouds. Our approach is to create, test, and implement a bulk-microphysics/aerosol model using data from Atmospheric Radiation Measurement (ARM) Cloud and Radiation Testbed (CART) sites and large-eddy simulation (LES) explicit bin-resolving aerosol/microphysics models. The primary objectives of this work are twofold. First, we need the prediction of number concentrations of activated aerosol which are transferred to the droplet spectrum, so that the aerosol population directly affects the cloud formation and microphysics. Second, we plan to couple the aerosol model to the gas and aqueous-chemistry module that will drive the aerosol formation and growth. We begin by exploring the feasibility of performing cloud-resolving simulations of Arctic stratus clouds over the North Slope CART site. These simulations using Colorado State University`s regional atmospheric modeling system (RAMS) will be useful in designing the structure of the cloud-resolving model and in interpreting data acquired at the North Slope site.

  4. GCM Simulations of the Aerosol Indirect Effect: Sensitivity to Cloud Parameterization and Aerosol Burden

    NASA Technical Reports Server (NTRS)

    Menon, Surabi; DelGenio, Anthony D.; Koch, Dorothy; Tselioudis, George; Hansen, James E. (Technical Monitor)

    2001-01-01

    We describe the coupling of the Goddard Institute for Space Studies (GISS) general circulation model (GCM) to an online sulfur chemistry model and source models for organic matter and sea-salt that is used to estimate the aerosol indirect effect. The cloud droplet number concentration is diagnosed empirically from field experiment datasets over land and ocean that observe droplet number and all three aerosol types simultaneously; corrections are made for implied variations in cloud turbulence levels. The resulting cloud droplet number is used to calculate variations in droplet effective radius, which in turn allows us to predict aerosol effects on cloud optical thickness and microphysical process rates. We calculate the aerosol indirect effect by differencing the top-of-the-atmosphere net cloud radiative forcing for simulations with present-day vs. pre-industrial emissions. Both the first (radiative) and second (microphysical) indirect effects are explored. We test the sensitivity of our results to cloud parameterization assumptions that control the vertical distribution of cloud occurrence, the autoconversion rate, and the aerosol scavenging rate, each of which feeds back significantly on the model aerosol burden. The global mean aerosol indirect effect for all three aerosol types ranges from -1.55 to -4.36 W m(exp -2) in our simulations. The results are quite sensitive to the pre-industrial background aerosol burden, with low pre-industrial burdens giving strong indirect effects, and to a lesser extent to the anthropogenic aerosol burden, with large burdens giving somewhat larger indirect effects. Because of this dependence on the background aerosol, model diagnostics such as albedo-particle size correlations and column cloud susceptibility, for which satellite validation products are available, are not good predictors of the resulting indirect effect.

  5. GCM Simulations of the Aerosol Indirect Effect: Sensitivity to Cloud Parameterization and Aerosol Burden

    NASA Technical Reports Server (NTRS)

    Menon, Surabi; DelGenio, Anthony D.; Koch, Dorothy; Tselioudis, George; Hansen, James E. (Technical Monitor)

    2001-01-01

    We describe the coupling of the Goddard Institute for Space Studies (GISS) general circulation model (GCM) to an online sulfur chemistry model and source models for organic matter and sea-salt that is used to estimate the aerosol indirect effect. The cloud droplet number concentration is diagnosed empirically from field experiment datasets over land and ocean that observe droplet number and all three aerosol types simultaneously; corrections are made for implied variations in cloud turbulence levels. The resulting cloud droplet number is used to calculate variations in droplet effective radius, which in turn allows us to predict aerosol effects on cloud optical thickness and microphysical process rates. We calculate the aerosol indirect effect by differencing the top-of-the-atmosphere net cloud radiative forcing for simulations with present-day vs. pre-industrial emissions. Both the first (radiative) and second (microphysical) indirect effects are explored. We test the sensitivity of our results to cloud parameterization assumptions that control the vertical distribution of cloud occurrence, the autoconversion rate, and the aerosol scavenging rate, each of which feeds back significantly on the model aerosol burden. The global mean aerosol indirect effect for all three aerosol types ranges from -1.55 to -4.36 W/sq m in our simulations. The results are quite sensitive to the pre-industrial background aerosol burden, with low pre-industrial burdens giving strong indirect effects, and to a lesser extent to the anthropogenic aerosol burden, with large burdens giving somewhat larger indirect effects. Because of this dependence on the background aerosol, model diagnostics such as albedo-particle size correlations and column cloud susceptibility, for which satellite validation products are available, are not good predictors of the resulting indirect effect.

  6. A New WRF-Chem Treatment for Studying Regional Scale Impacts of Cloud-Aerosol Interactions in Parameterized Cumuli

    SciTech Connect

    Berg, Larry K.; Shrivastava, ManishKumar B.; Easter, Richard C.; Fast, Jerome D.; Chapman, Elaine G.; Liu, Ying

    2015-01-01

    A new treatment of cloud-aerosol interactions within parameterized shallow and deep convection has been implemented in WRF-Chem that can be used to better understand the aerosol lifecycle over regional to synoptic scales. The modifications to the model to represent cloud-aerosol interactions include treatment of the cloud dropletnumber mixing ratio; key cloud microphysical and macrophysical parameters (including the updraft fractional area, updraft and downdraft mass fluxes, and entrainment) averaged over the population of shallow clouds, or a single deep convective cloud; and vertical transport, activation/resuspension, aqueous chemistry, and wet removal of aerosol and trace gases in warm clouds. Thesechanges have been implemented in both the WRF-Chem chemistry packages as well as the Kain-Fritsch cumulus parameterization that has been modified to better represent shallow convective clouds. Preliminary testing of the modified WRF-Chem has been completed using observations from the Cumulus Humilis Aerosol Processing Study (CHAPS) as well as a high-resolution simulation that does not include parameterized convection. The simulation results are used to investigate the impact of cloud-aerosol interactions on the regional scale transport of black carbon (BC), organic aerosol (OA), and sulfate aerosol. Based on the simulations presented here, changes in the column integrated BC can be as large as -50% when cloud-aerosol interactions are considered (due largely to wet removal), or as large as +35% for sulfate in non-precipitating conditions due to the sulfate production in the parameterized clouds. The modifications to WRF-Chem version 3.2.1 are found to account for changes in the cloud drop number concentration (CDNC) and changes in the chemical composition of cloud-drop residuals in a way that is consistent with observations collected during CHAPS. Efforts are currently underway to port the changes described here to WRF-Chem version 3.5, and it is anticipated that they

  7. Organic aerosol volatility parameterizations and their impact on atmospheric composition and climate

    NASA Astrophysics Data System (ADS)

    Tsigaridis, K.; Bauer, S.

    2015-12-01

    Despite their importance and ubiquity in the atmosphere, organic aerosols are still very poorly parameterized in global models. This can be explained by two reasons: first, a very large number of unconstrained parameters are involved in accurate parameterizations, and second, a detailed description of semi-volatile organics is computationally very expensive. Even organic aerosol properties that are known to play a major role in the atmosphere, namely volatility and aging, are poorly resolved in global models, if at all. Studies with different models and different parameterizations have not been conclusive on whether the additional complexity improves model simulations, but the added diversity of the different host models used adds an unnecessary degree of variability in the evaluation of results that obscures solid conclusions. Here we will present a thorough study of the most popular organic aerosol parameterizations with regard to volatility in global models, studied within the same host global model, the GISS ModelE2: primary and secondary organic aerosols both being non-volatile, secondary organic aerosols semi-volatile (2-product model), and all organic aerosols semi-volatile (volatility-basis set). We will also present results on the role aerosol microphysical calculations play on organic aerosol concentrations. The changes in aerosol distribution as a result of the different parameterizations, together with their role on gas-phase chemistry and climate, will be presented.

  8. What role do type I polar stratospheric cloud and aerosol parameterizations play in modelled lower stratospheric chlorine activation and ozone loss?

    NASA Astrophysics Data System (ADS)

    Sessler, J.; Good, P.; MacKenzie, A. R.; Pyle, J. A.

    1996-12-01

    The chlorine activation and subsequent ozone loss of the northern winter lower stratosphere have been modelled using different schemes for type I polar stratospheric clouds (PSCs) and sulphate aerosols. Type I PSCs were assumed to consist of either nitric acid trihydrate (NAT) at equilibrium, supercooled ternary solutions (STS) at equilibrium, or to follow a hysteresis cycle between frozen and liquid particles depending on the temperature history. The sulphate aerosol was assumed to be present as either liquid binary H2SO4/H2O aerosol (LBA) or as solid sulphuric acid tetrahydrate (SAT). Our box model integrations show that NAT and STS, representing the upper and lower limits of lower stratospheric chlorine activation, respectively, appear to destroy ozone equally efficiently after a cold PSC event (Tmin ≤ 190K at 50 mbar). For higher minimum temperatures, up to the equilibrium NAT point, there is significantly more ozone loss in the NAT scheme than in the STS scheme. On NAT, chlorine is activated directly by ClONO2 + HCl → 2Cl + HNO3, whereas on STS, indirect activation by ClONO2 + H2O → HOCl + HNO3 followed by HOCl + HCl → 2Cl + H2O, dominates. During the processing period, the indirect activation on STS will produce a temporary peak in HOCl. Box model integrations also show that direct chlorine activation is faster on SAT than on LBA, yielding significantly more ozone loss in air parcels which remain below the SAT melting point (215-220 K). Our single-layer chemical transport model simulations (θ = 465K) of the lower stratospheric chlorine activation during Arctic winter 1994/1995 show that chlorine is activated more quickly on NAT than on STS. However, in mid December 1994, when temperatures are low enough for substantial STS particle growth, maximum active chlorine becomes similar in both schemes and remains similar until the end of January 1995. A model integration which includes SAT produces up to 200 parts per trillion by volume more ClOx, inside

  9. A sea spray aerosol flux parameterization encapsulating wave state

    NASA Astrophysics Data System (ADS)

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

    2013-09-01

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

  10. Sensitivity of aerosol-cloud-precipitation interactions to autoconversion parameterization in WRF model

    NASA Astrophysics Data System (ADS)

    Xie, Xiaoning; Liu, Xiaodong

    2013-04-01

    Autoconversion process is an important bridge between aerosols, clouds, and precipitation, in that the change of the cloud microphysical properties by aerosols could influence the spatial and temporal changes of the surface precipitation, as well as the total precipitation amount. Three types of autoconversion parameterization are considered in our study including the Kessler scheme (Kessler, 1969), the KK scheme (Khairoutdinov and Kogan, 2000), and the Dispersion scheme (Liu et al., 2005). The Kessler scheme doesn't consider aerosol indirect effect and the KK scheme can study the aerosol indirect effect; while the Dispersion scheme can both consider the aerosol indirect effect and the influence of cloud droplet spectral dispersion. In this study, the aerosol effects on clouds and precipitation in mesoscale convective systems are investigated using the Weather Research and Forecast model (WRF) with the Morrison two-moment bulk microphysics scheme. Considering the different types of the autoconversion parameterization schemes including the Kessler scheme, the KK scheme, and the Dispersion scheme, a suite of sensitivity experiments are performed using an initial sounding data of the deep convective cloud system on 31 March 2005 in Beijing under different aerosol concentrations (varying from 50 cm-3 to 10000 cm-3). Numerical experiments in this study show that the aerosol induced precipitation change is strongly dependent on the autoconversion parameterization. For the Kessler scheme, the average cumulative precipitation is enhanced slightly with increasing aerosols. In the meantime, precipitation is reduced significantly with increasing aerosols for the KK scheme. The surface precipitation varies nonmonotonically for the Dispersion scheme, increasing with aerosols at lower concentration, while decreasing at higher concentration. These distinct trends in aerosol-induced precipitation are mainly due to the rain water content change under the different autoconversion

  11. Organic Aerosol Volatility Parameterizations and Their Impact on Atmospheric Composition and Climate

    NASA Technical Reports Server (NTRS)

    Tsigaridis, Kostas; Bauer, Susanne E.

    2015-01-01

    Despite their importance and ubiquity in the atmosphere, organic aerosols are still very poorly parameterized in global models. This can be explained by two reasons: first, a very large number of unconstrained parameters are involved in accurate parameterizations, and second, a detailed description of semi-volatile organics is computationally very expensive. Even organic aerosol properties that are known to play a major role in the atmosphere, namely volatility and aging, are poorly resolved in global models, if at all. Studies with different models and different parameterizations have not been conclusive on whether the additional complexity improves model simulations, but the added diversity of the different host models used adds an unnecessary degree of variability in the evaluation of results that obscures solid conclusions. Aerosol microphysics do not significantly alter the mean OA vertical profile or comparison with surface measurements. This might not be the case for semi-volatile OA with microphysics.

  12. A general circulation model (GCM) parameterization of Pinatubo aerosols

    SciTech Connect

    Lacis, A.A.; Carlson, B.E.; Mishchenko, M.I.

    1996-04-01

    The June 1991 volcanic eruption of Mt. Pinatubo is the largest and best documented global climate forcing experiment in recorded history. The time development and geographical dispersion of the aerosol has been closely monitored and sampled. Based on preliminary estimates of the Pinatubo aerosol loading, general circulation model predictions of the impact on global climate have been made.

  13. Size-resolved parameterization of primary organic carbon in fresh marine aerosols

    SciTech Connect

    Long, Michael S; Keene, William C; Erickson III, David J

    2009-12-01

    Marine aerosols produced by the bursting of artificially generated bubbles in natural seawater are highly enriched (2 to 3 orders of magnitude based on bulk composition) in marine-derived organic carbon (OC). Production of size-resolved particulate OC was parameterized based on a Langmuir kinetics-type association of OC to bubble plumes in seawater and resulting aerosol as constrained by measurements of aerosol produced from highly productive and oligotrophic seawater. This novel approach is the first to account for the influence of adsorption on the size-resolved association between marine aerosols and OC. Production fluxes were simulated globally with an eight aerosol-size-bin version of the NCAR Community Atmosphere Model (CAM v3.5.07). Simulated number and inorganic sea-salt mass production fell within the range of published estimates based on observationally constrained parameterizations. Because the parameterization does not consider contributions from spume drops, the simulated global mass flux (1.5 x 10{sup 3} Tg y{sup -1}) is near the lower limit of published estimates. The simulated production of aerosol number (2.1 x 10{sup 6} cm{sup -2} s{sup -1}) and OC (49 Tg C y{sup -1}) fall near the upper limits of published estimates and suggest that primary marine aerosols may have greater influences on the physiochemical evolution of the troposphere, radiative transfer and climate, and associated feedbacks on the surface ocean than suggested by previous model studies.

  14. The role of aerosols in cloud drop parameterizations and its applications in global climate models

    SciTech Connect

    Chuang, C.C.; Penner, J.E.

    1996-04-01

    The characteristics of the cloud drop size distribution near cloud base are initially determined by aerosols that serve as cloud condensation nuclei and the updraft velocity. We have developed parameterizations relating cloud drop number concentration to aerosol number and sulfate mass concentrations and used them in a coupled global aerosol/general circulation model (GCM) to estimate the indirect aerosol forcing. The global aerosol model made use of our detailed emissions inventories for the amount of particulate matter from biomass burning sources and from fossil fuel sources as well as emissions inventories of the gas-phase anthropogenic SO{sub 2}. This work is aimed at validating the coupled model with the Atmospheric Radiation Measurement (ARM) Program measurements and assessing the possible magnitude of the aerosol-induced cloud effects on climate.

  15. Parameterizations of Cloud Microphysics and Indirect Aerosol Effects

    SciTech Connect

    Tao, Wei-Kuo

    2014-05-19

    1. OVERVIEW Aerosols and especially their effect on clouds are one of the key components of the climate system and the hydrological cycle [Ramanathan et al., 2001]. Yet, the aerosol effect on clouds remains largely unknown and the processes involved not well understood. A recent report published by the National Academy of Science states "The greatest uncertainty about the aerosol climate forcing - indeed, the largest of all the uncertainties about global climate forcing - is probably the indirect effect of aerosols on clouds [NRC, 2001]." The aerosol effect on clouds is often categorized into the traditional "first indirect (i.e., Twomey)" effect on the cloud droplet sizes for a constant liquid water path [Twomey, 1977] and the "semi-direct" effect on cloud coverage [e.g., Ackerman et al., 2000]. Enhanced aerosol concentrations can also suppress warm rain processes by producing a narrow droplet spectrum that inhibits collision and coalescence processes [e.g., Squires and Twomey, 1961; Warner and Twomey, 1967; Warner, 1968; Rosenfeld, 1999]. The aerosol effect on precipitation processes, also known as the second type of aerosol indirect effect [Albrecht, 1989], is even more complex, especially for mixed-phase convective clouds. Table 1 summarizes the key observational studies identifying the microphysical properties, cloud characteristics, thermodynamics and dynamics associated with cloud systems from high-aerosol continental environments. For example, atmospheric aerosol concentrations can influence cloud droplet size distributions, warm-rain process, cold-rain process, cloud-top height, the depth of the mixed phase region, and occurrence of lightning. In addition, high aerosol concentrations in urban environments could affect precipitation variability by providing an enhanced source of cloud condensation nuclei (CCN). Hypotheses have been developed to explain the effect of urban regions on convection and precipitation [van den Heever and Cotton, 2007 and Shepherd

  16. Organic Aerosol Volatility Parameterizations and Their Impact on Atmospheric Composition and Climate

    NASA Technical Reports Server (NTRS)

    Tsigaridis, Konsta; Bauer, Susanne E.

    2015-01-01

    Despite their importance and ubiquity in the atmosphere, organic aerosols are still very poorly parameterized in global models. This can be explained by two reasons: first, a very large number of unconstrained parameters are involved in accurate parameterizations, and second, a detailed description of semi-volatile organics is computationally very expensive. Even organic aerosol properties that are known to play a major role in the atmosphere, namely volatility and aging, are poorly resolved in global models, if at all. Studies with different models and different parameterizations have not been conclusive on whether the additional complexity improves model simulations, but the added diversity of the different host models used adds an unnecessary degree of variability in the evaluation of results that obscures solid conclusions.

  17. A Comparison of Aerosol Parameterizations in the ACOS XCO2 Retrieval Algorithm

    NASA Astrophysics Data System (ADS)

    Nelson, R. R.; O'Dell, C.; Crisp, D.; Eldering, A.; Frankenberg, C.; Gunson, M. R.; Natraj, V.; Fu, D.

    2014-12-01

    An effective parameterization of clouds and aerosols in retrieval algorithms is essential for reducing measurement errors and biases in estimates of the column-averaged dry-air mole fraction of carbon dioxide (XCO2) from space-based measurements of near-infrared reflected sunlight. The NASA Atmospheric CO2 Observations from Space (ACOS) XCO2 retrieval algorithm has evolved significantly over the past several years in an effort to more accurately represent the impact of clouds and aerosols on XCO2. Recent ACOS algorithm versions up to build 3.4 used a water cloud type, ice cloud type, and two generic aerosol types for each sounding. ACOS build 3.5 uses the same cloud parameterization, but was modified to replace the "one-size-fits-all" aerosol scheme. Build 3.5 uses a monthly aerosol climatology based on the Modern-Era Retrospective Analysis for Research and Applications (MERRA) reanalysis to choose the two most likely aerosol types for a given measurement location, along with typical optical depths. The five MERRA types available for selection are sulfate, dust, sea salt, organic carbon, and black carbon. The algorithm then uses a pre-assigned Gaussian width and height and fits for the aerosol amount and peak height based on information from the 760 nm O2 A-band and the CO2 bands centered near 1610 and 2060 nm. Here we compare ACOS builds 3.4 and build 3.5 to quantify the impact of the aerosol scheme update. Two types of tests were performed. Simulated Orbiting Carbon Observatory 2 (OCO-2) retrievals and their associated aerosol and cloud profiles were compared to the "true" aerosol and cloud profiles used to create the simulated environment for a given measurement. The retrieval algorithms were also run on Greenhouse gases Observing SATellite (GOSAT) observations and compared to AErosol RObotic NETwork (AERONET) aerosol optical depth measurements in order to quantify the ability of the algorithms to retrieve information about aerosol optical depths. XCO2 errors

  18. Influences of in-cloud aerosol scavenging parameterizations on aerosol concentrations and wet deposition in ECHAM5-HAM

    NASA Astrophysics Data System (ADS)

    Croft, B.; Lohmann, U.; Martin, R. V.; Stier, P.; Wurzler, S.; Feichter, J.; Hoose, C.; Heikkilä, U.; van Donkelaar, A.; Ferrachat, S.

    2009-10-01

    A diagnostic nucleation scavenging scheme, which determines stratiform cloud scavenging ratios for both aerosol mass and number distributions, based on cloud droplet, and ice crystal number concentrations, is introduced into the ECHAM5-HAM global climate model. This is coupled with a size-dependent in-cloud impaction scavenging parameterization for both cloud droplet-aerosol, and ice crystal-aerosol collisions. Sensitivity studies are presented, which compare aerosol concentrations, and deposition between a variety of in-cloud scavenging approaches, including prescribed fractions, several diagnostic schemes, and a prognostic aerosol cloud processing treatment that passes aerosol in-droplet and in-ice crystal concentrations between model time steps. For one sensitivity study, assuming 100% of the in-cloud aerosol is scavenged into the cloud droplets and ice crystals, the annual global mean accumulation mode number burden is decreased by 65%, relative to a simulation with prognostic aerosol cloud processing. Diagnosing separate nucleation scavenging ratios for aerosol number and mass distributions, as opposed to equating the aerosol mass scavenging to the number scavenging ratios, reduces the annual global mean sulfate burden by near to 10%. The annual global mean sea salt burden is 30% lower for the diagnostic approach, which does not carry aerosol in-droplet and in-crystal concentrations between model time-steps as compared to the prognostic scheme. Implementation of in-cloud impaction scavenging reduced the annual, global mean black carbon burden by 30% for the prognostic aerosol cloud processing scheme. Better agreement with observations of black carbon profiles from aircraft (changes near to one order of magnitude for mixed phase clouds), 210Pb surface layer concentrations and wet deposition, and the geographic distribution of aerosol optical depth are found for the new diagnostic scavenging as compared to prescribed ratio scavenging scheme of the standard ECHAM

  19. Influences of in-cloud aerosol scavenging parameterizations on aerosol concentrations and wet deposition in ECHAM5-HAM

    NASA Astrophysics Data System (ADS)

    Croft, B.; Lohmann, U.; Martin, R. V.; Stier, P.; Wurzler, S.; Feichter, J.; Hoose, C.; Heikkilä, U.; van Donkelaar, A.; Ferrachat, S.

    2010-02-01

    A diagnostic cloud nucleation scavenging scheme, which determines stratiform cloud scavenging ratios for both aerosol mass and number distributions, based on cloud droplet, and ice crystal number concentrations, is introduced into the ECHAM5-HAM global climate model. This scheme is coupled with a size-dependent in-cloud impaction scavenging parameterization for both cloud droplet-aerosol, and ice crystal-aerosol collisions. The aerosol mass scavenged in stratiform clouds is found to be primarily (>90%) scavenged by cloud nucleation processes for all aerosol species, except for dust (50%). The aerosol number scavenged is primarily (>90%) attributed to impaction. 99% of this impaction scavenging occurs in clouds with temperatures less than 273 K. Sensitivity studies are presented, which compare aerosol concentrations, burdens, and deposition for a variety of in-cloud scavenging approaches: prescribed fractions, a more computationally expensive prognostic aerosol cloud processing treatment, and the new diagnostic scheme, also with modified assumptions about in-cloud impaction and nucleation scavenging. Our results show that while uncertainties in the representation of in-cloud scavenging processes can lead to differences in the range of 20-30% for the predicted annual, global mean aerosol mass burdens, and near to 50% for accumulation mode aerosol number burden, the differences in predicted aerosol mass concentrations can be up to one order of magnitude, particularly for regions of the middle troposphere with temperatures below 273 K where mixed and ice phase clouds exist. Different parameterizations for impaction scavenging changed the predicted global, annual mean number removal attributed to ice clouds by seven-fold, and the global, annual dust mass removal attributed to impaction by two orders of magnitude. Closer agreement with observations of black carbon profiles from aircraft (increases near to one order of magnitude for mixed phase clouds), mid

  20. Investigation of Aerosol Indirect Effects using a Cumulus Microphysics Parameterization in a Regional Climate Model

    SciTech Connect

    Lim, Kyo-Sun; Fan, Jiwen; Leung, Lai-Yung R.; Ma, Po-Lun; Singh, Balwinder; Zhao, Chun; Zhang, Yang; Zhang, Guang; Song, Xiaoliang

    2014-01-29

    A new Zhang and McFarlane (ZM) cumulus scheme includes a two-moment cloud microphysics parameterization for convective clouds. This allows aerosol effects to be investigated more comprehensively by linking aerosols with microphysical processes in both stratiform clouds that are explicitly resolved and convective clouds that are parameterized in climate models. This new scheme is implemented in the Weather Research and Forecasting (WRF) model, which is coupled with the physics and aerosol packages from the Community Atmospheric Model version 5 (CAM5). A test case of July 2008 during the East Asian summer monsoon is selected to evaluate the performance of the new ZM scheme and to investigate aerosol effects on monsoon precipitation. The precipitation and radiative fluxes simulated by the new ZM scheme show a better agreement with observations compared to simulations with the original ZM scheme that does not include convective cloud microphysics and aerosol convective cloud interactions. Detailed analysis suggests that an increase in detrained cloud water and ice mass by the new ZM scheme is responsible for this improvement. To investigate precipitation response to increased anthropogenic aerosols, a sensitivity experiment is performed that mimics a clean environment by reducing the primary aerosols and anthropogenic emissions to 30% of that used in the control simulation of a polluted environment. The simulated surface precipitation is reduced by 9.8% from clean to polluted environment and the reduction is less significant when microphysics processes are excluded from the cumulus clouds. Ensemble experiments with ten members under each condition (i.e., clean and polluted) indicate similar response of the monsoon precipitation to increasing aerosols.

  1. Evaluating model parameterizations of submicron aerosol scattering and absorption with in situ data from ARCTAS 2008

    NASA Astrophysics Data System (ADS)

    Alvarado, Matthew J.; Lonsdale, Chantelle R.; Macintyre, Helen L.; Bian, Huisheng; Chin, Mian; Ridley, David A.; Heald, Colette L.; Thornhill, Kenneth L.; Anderson, Bruce E.; Cubison, Michael J.; Jimenez, Jose L.; Kondo, Yutaka; Sahu, Lokesh K.; Dibb, Jack E.; Wang, Chien

    2016-07-01

    Accurate modeling of the scattering and absorption of ultraviolet and visible radiation by aerosols is essential for accurate simulations of atmospheric chemistry and climate. Closure studies using in situ measurements of aerosol scattering and absorption can be used to evaluate and improve models of aerosol optical properties without interference from model errors in aerosol emissions, transport, chemistry, or deposition rates. Here we evaluate the ability of four externally mixed, fixed size distribution parameterizations used in global models to simulate submicron aerosol scattering and absorption at three wavelengths using in situ data gathered during the 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. The four models are the NASA Global Modeling Initiative (GMI) Combo model, GEOS-Chem v9-02, the baseline configuration of a version of GEOS-Chem with online radiative transfer calculations (called GC-RT), and the Optical Properties of Aerosol and Clouds (OPAC v3.1) package. We also use the ARCTAS data to perform the first evaluation of the ability of the Aerosol Simulation Program (ASP v2.1) to simulate submicron aerosol scattering and absorption when in situ data on the aerosol size distribution are used, and examine the impact of different mixing rules for black carbon (BC) on the results. We find that the GMI model tends to overestimate submicron scattering and absorption at shorter wavelengths by 10-23 %, and that GMI has smaller absolute mean biases for submicron absorption than OPAC v3.1, GEOS-Chem v9-02, or GC-RT. However, the changes to the density and refractive index of BC in GC-RT improve the simulation of submicron aerosol absorption at all wavelengths relative to GEOS-Chem v9-02. Adding a variable size distribution, as in ASP v2.1, improves model performance for scattering but not for absorption, likely due to the assumption in ASP v2.1 that BC is present at a constant mass fraction

  2. An explicit study of aerosol mass conversion and its parameterization in warm rain formation of cumulus clouds

    NASA Astrophysics Data System (ADS)

    Sun, J.; Fen, J.; Ungar, R. K.

    2013-10-01

    The life time of atmospheric aerosols is highly affected by in-cloud scavenging processes. Aerosol mass conversion from aerosols embedded in cloud droplets into aerosols embedded in raindrops is a pivotal pathway for wet removal of aerosols in clouds. The aerosol mass conversion rate in the bulk microphysics parameterizations is always assumed to be linearly related to the precipitation production rate, which includes the cloud water autoconversion rate and the cloud water accretion rate. The ratio of the aerosol mass concentration conversion rate to the cloud aerosol mass concentration has typically been considered to be the same as the ratio of the precipitation production rate to the cloud droplet mass concentration. However, the mass of an aerosol embedded in a cloud droplet is not linearly proportional to the mass of the cloud droplet. A simple linear relationship cannot be drawn between the precipitation production rate and the aerosol mass concentration conversion rate. In this paper, we studied the evolution of aerosol mass concentration conversion rates in a warm rain formation process with a 1.5-dimensional non-hydrostatic convective cloud and aerosol interaction model in the bin microphysics. We found that the ratio of the aerosol mass conversion rate to the cloud aerosol mass concentration can be statistically expressed by the ratio of the precipitation production rate to the cloud droplet mass concentration with an exponential function. We further gave some regression equations to determine aerosol conversions in the warm rain formation under different threshold radii of raindrops and different aerosol size distributions.

  3. Global direct radiative forcing by process-parameterized aerosol optical properties

    NASA Astrophysics Data System (ADS)

    KirkevâG, Alf; Iversen, Trond

    2002-10-01

    A parameterization of aerosol optical parameters is developed and implemented in an extended version of the community climate model version 3.2 (CCM3) of the U.S. National Center for Atmospheric Research. Direct radiative forcing (DRF) by monthly averaged calculated concentrations of non-sea-salt sulfate and black carbon (BC) is estimated. Inputs are production-specific BC and sulfate from [2002] and background aerosol size distribution and composition. The scheme interpolates between tabulated values to obtain the aerosol single scattering albedo, asymmetry factor, extinction coefficient, and specific extinction coefficient. The tables are constructed by full calculations of optical properties for an array of aerosol input values, for which size-distributed aerosol properties are estimated from theory for condensation and Brownian coagulation, assumed distribution of cloud-droplet residuals from aqueous phase oxidation, and prescribed properties of the background aerosols. Humidity swelling is estimated from the Köhler equation, and Mie calculations finally yield spectrally resolved aerosol optical parameters for 13 solar bands. The scheme is shown to give excellent agreement with nonparameterized DRF calculations for a wide range of situations. Using IPCC emission scenarios for the years 2000 and 2100, calculations with an atmospheric global cliamte model (AFCM) yield a global net anthropogenic DRF of -0.11 and 0.11 W m-2, respectively, when 90% of BC from biomass burning is assumed anthropogenic. In the 2000 scenario, the individual DRF due to sulfate and BC has separately been estimated to -0.29 and 0.19 W m-2, respectively. Our estimates of DRF by BC per BC mass burden are lower than earlier published estimates. Some sensitivity tests are included to investigate to what extent uncertain assumptions may influence these results.

  4. Ground-based remote sensing of aerosol climatology in China: Aerosol optical properties, direct radiative effect and its parameterization

    NASA Astrophysics Data System (ADS)

    Xia, X.; Che, H.; Zhu, J.; Chen, H.; Cong, Z.; Deng, X.; Fan, X.; Fu, Y.; Goloub, P.; Jiang, H.; Liu, Q.; Mai, B.; Wang, P.; Wu, Y.; Zhang, J.; Zhang, R.; Zhang, X.

    2016-01-01

    Spatio-temporal variation of aerosol optical properties and aerosol direct radiative effects (ADRE) are studied based on high quality aerosol data at 21 sunphotometer stations with at least 4-months worth of measurements in China mainland and Hong Kong. A parameterization is proposed to describe the relationship of ADREs to aerosol optical depth at 550 nm (AOD) and single scattering albedo at 550 nm (SSA). In the middle-east and south China, the maximum AOD is always observed in the burning season, indicating a significant contribution of biomass burning to AOD. Dust aerosols contribute to AOD significantly in spring and their influence decreases from the source regions to the downwind regions. The occurrence frequencies of background level AOD (AOD < 0.10) in the middle-east, south and northwest China are very limited (0.4%, 1.3% and 2.8%, respectively). However, it is 15.7% in north China. Atmosphere is pristine in the Tibetan Plateau where 92.0% of AODs are <0.10. Regional mean SSAs at 550 nm are 0.89-0.90, although SSAs show substantial site and season dependence. ADREs at the top and bottom of the atmosphere for solar zenith angle of 60 ± 5° are -16--37 W m-2 and -66--111 W m-2, respectively. ADRE efficiency shows slight regional dependence. AOD and SSA together account for more than 94 and 87% of ADRE variability at the bottom and top of the atmosphere. The overall picture of ADRE in China is that aerosols cool the climate system, reduce surface solar radiation and heat the atmosphere.

  5. Quantifying the Relationship between Organic Aerosol Composition and Hygroscopicity/CCN Activity

    SciTech Connect

    Ziemann, Paul J.; Kreidenweis, Sonia M.; Petters, Markus D.

    2013-06-30

    The overall objective for this project was to provide the data and underlying process level understanding necessary to facilitate the dynamic treatment of organic aerosol CCN activity in future climate models. The specific objectives were as follows: (1) employ novel approaches to link organic aerosol composition and CCN activity, (2) evaluate the effects of temperature and relative humidity on organic aerosol CCN activity, and (3) develop parameterizations to link organic aerosol composition and CCN activity.

  6. Cloud Dynamical Controls on Climate Forcing by Aerosol-Cloud Interactions: New Insights from Observations, High-Resolution Models, and Parameterizations

    NASA Astrophysics Data System (ADS)

    Donner, Leo

    2016-04-01

    At frequently observed, low updraft speeds, cloud droplet and ice crystal number concentrations are controlled mostly by cloud-scale vertical velocities and not aerosol number concentrations. Reducing uncertainty in estimates of climate forcing by aerosol-cloud interactions will require taking account of these thermodynamically limited cloud regimes in global climate models. The scales of the relevant cloud dynamics are often well-below resolved scales in climate and numerical weather prediction models, ranging to tens of meters at large-eddy scale for stratocumulus clouds. Observations of vertical velocities from cloud radars in field programs and at fixed observational sites are providing a basis for evaluating new classes of parameterizations for convective and non-convective clouds that include probability distribution functions (PDFs) for vertical velocity, which can be used to drive physically based representations of droplet and crystal activation. High-resolution cloud models with detailed treatments of aerosol and microphysical processes can also be evaluated using these observations. Vertical velocities in both high-resolution models and parameterizations currently show discrepancies from observations while capturing qualitative features. Improved treatments of microphysical and turbulence processes in high-resolution cloud models hold promise for improving agreement with observations, while a wide range of advances in parameterization are possible paths to improvement for simulating sub-grid vertical velocities and aerosol-cloud interactions.

  7. Modelling of primary aerosols in the chemical transport model MOCAGE: development and evaluation of aerosol physical parameterizations

    NASA Astrophysics Data System (ADS)

    Sič, B.; El Amraoui, L.; Marécal, V.; Josse, B.; Arteta, J.; Guth, J.; Joly, M.; Hamer, P. D.

    2015-02-01

    This paper deals with recent improvements to the global chemical transport model of Météo-France MOCAGE (Modèle de Chimie Atmosphérique à Grande Echelle) that consists of updates to different aerosol parameterizations. MOCAGE only contains primary aerosol species: desert dust, sea salt, black carbon, organic carbon, and also volcanic ash in the case of large volcanic eruptions. We introduced important changes to the aerosol parameterization concerning emissions, wet deposition and sedimentation. For the emissions, size distribution and wind calculations are modified for desert dust aerosols, and a surface sea temperature dependant source function is introduced for sea salt aerosols. Wet deposition is modified toward a more physically realistic representation by introducing re-evaporation of falling rain and snowfall scavenging and by changing the in-cloud scavenging scheme along with calculations of precipitation cloud cover and rain properties. The sedimentation scheme update includes changes regarding the stability and viscosity calculations. Independent data from satellites (MODIS, SEVIRI), the ground (AERONET, EMEP), and a model inter-comparison project (AeroCom) are compared with MOCAGE simulations and show that the introduced changes brought a significant improvement on aerosol representation, properties and global distribution. Emitted quantities of desert dust and sea salt, as well their lifetimes, moved closer towards values of AeroCom estimates and the multi-model average. When comparing the model simulations with MODIS aerosol optical depth (AOD) observations over the oceans, the updated model configuration shows a decrease in the modified normalized mean bias (MNMB; from 0.42 to 0.10) and a better correlation (from 0.06 to 0.32) in terms of the geographical distribution and the temporal variability. The updates corrected a strong positive MNMB in the sea salt representation at high latitudes (from 0.65 to 0.16), and a negative MNMB in the desert

  8. Molecular corridors and parameterizations of volatility in the evolution of organic aerosols

    NASA Astrophysics Data System (ADS)

    Li, Y.; Pöschl, U.; Shiraiwa, M.

    2015-10-01

    The formation and aging of organic aerosols (OA) proceed through multiple steps of chemical reaction and mass transport in the gas and particle phases, which is challenging for the interpretation of field measurements and laboratory experiments as well as accurate representation of OA evolution in atmospheric aerosol models. Based on data from over 30 000 compounds, we show that organic compounds with a wide variety of functional groups fall into molecular corridors, characterized by a tight inverse correlation between molar mass and volatility. We developed parameterizations to predict the volatility of organic compounds containing oxygen, nitrogen and sulfur from the elemental composition that can be measured by soft-ionization high-resolution mass spectrometry. Field measurement data from new particle formation events, biomass burning, cloud/fog processing, and indoor environments were mapped into molecular corridors to characterize the chemical nature of the observed OA components. We found that less oxidized indoor OA are constrained to a corridor of low molar mass and high volatility, whereas highly oxygenated compounds in atmospheric water extend to high molar mass and low volatility. Among the nitrogen- and sulfur-containing compounds identified in atmospheric aerosols, amines tend to exhibit low molar mass and high volatility, whereas organonitrates and organosulfates follow high O : C corridors extending to high molar mass and low volatility. We suggest that the consideration of molar mass and molecular corridors can help to constrain volatility and particle phase state in the modeling of OA particularly for nitrogen- and sulfur-containing compounds.

  9. A Comparison of Parameterizations of Secondary Organic Aerosol Production: Global Budget and Spatiotemporal Variability

    NASA Astrophysics Data System (ADS)

    Liu, J.; Chen, Z.; Horowitz, L. W.; Carlton, A. M. G.; Fan, S.; Cheng, Y.; Ervens, B.; Fu, T. M.; He, C.; Tao, S.

    2014-12-01

    Secondary organic aerosols (SOA) have a profound influence on air quality and climate, but large uncertainties exist in modeling SOA on the global scale. In this study, five SOA parameterization schemes, including a two-product model (TPM), volatility basis-set (VBS) and three cloud SOA schemes (Ervens et al. (2008, 2014), Fu et al. (2008) , and He et al. (2013)), are implemented into the global chemical transport model (MOZART-4). For each scheme, model simulations are conducted with identical boundary and initial conditions. The VBS scheme produces the highest global annual SOA production (close to 35 Tg·y-1), followed by three cloud schemes (26-30 Tg·y-1) and TPM (23 Tg·y-1). Though sharing a similar partitioning theory to the TPM scheme, the VBS approach simulates the chemical aging of multiple generations of VOCs oxidation products, resulting in a much larger SOA source, particularly from aromatic species, over Europe, the Middle East and Eastern America. The formation of SOA in VBS, which represents the net partitioning of semi-volatile organic compounds from vapor to condensed phase, is highly sensitivity to the aging and wet removal processes of vapor-phase organic compounds. The production of SOA from cloud processes (SOAcld) is constrained by the coincidence of liquid cloud water and water-soluble organic compounds. Therefore, all cloud schemes resolve a fairly similar spatial pattern over the tropical and the mid-latitude continents. The spatiotemporal diversity among SOA parameterizations is largely driven by differences in precursor inputs. Therefore, a deeper understanding of the evolution, wet removal, and phase partitioning of semi-volatile organic compounds, particularly above remote land and oceanic areas, is critical to better constrain the global-scale distribution and related climate forcing of secondary organic aerosols.

  10. Modeling aerosol effects on shallow cumulus convection under various meteorological conditions observed over the Indian Ocean and implications for development of mass-flux parameterizations for climate models

    NASA Astrophysics Data System (ADS)

    Wang, Hailong; McFarquhar, Greg M.

    2008-10-01

    To determine conditions over the Indian Ocean, under which cloud fields are most susceptible to modification from aerosols, and to study how turbulent activities and shallow cumuli vary for different meteorological scenarios, a three-dimensional large-eddy simulation model was initialized using data collected during the Indian Ocean Experiment (INDOEX). Radiosonde data were used to construct six soundings encompassing the range of temperature and humidity observed. A total of 18 meteorological scenarios were then obtained by adding either an average transition layer (TL), a strong inversion layer (IL), or no stable layer to each sounding. Separate simulations were conducted for each scenario assuming pristine or polluted conditions as observed during INDOEX. For aerosol profiles measured during INDOEX, aerosol semidirect effects always dominated indirect effects, with the positive daytime net indirect forcing (semidirect plus indirect forcings) varying between 0.2 and 4.5 W m-2. Anthropogenic aerosols had a larger net indirect forcing when the environmental relative humidity (RH) was higher and in the absence of the IL and TL. Changes in meteorological factors had larger impacts on the cloud properties than did anthropogenic aerosols, indicating large uncertainties can be introduced when solely using observations to quantify aerosol effects without examining their meteorological context. Because mean lateral detrainment and entrainment rates depended on RH, aerosols, and the presence of stable layers, mass-flux parameterizations in climate models should not use single values for such rates that may not represent the range of conditions observed where trade cumuli form.

  11. Evaluation of a New Cloud Droplet Activation Parameterization wtih in Situ Data from CRYSTAL-FACE and CSTRIPE

    NASA Technical Reports Server (NTRS)

    Meskhidze, Nicholas; Nenes, Athanasios; Conant, William C.; Seinfeld, John H.

    2005-01-01

    The accuracy of the 2003 prognostic, physically based aerosol activation parameterization of A. Nenes and J. H. Seinfeld (NS) with modification introduced by C. Fountoukis and A. Nenes in 2005 (modified NS) is evaluated against extensive microphysical data sets collected on board the Center for Interdisciplinary Remotely Piloted Aircraft Studies (CIRPAS) Twin Otter aircraft for cumuliform and stratiform clouds of marine and continental origin. The cumuliform cloud data were collected during NASA's Cirrus Regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment (CRYSTAL-FACE, Key West, Florida, July 2002), while the stratiform cloud data were gathered during Coastal Stratocumulus Imposed Perturbation Experiment (CSTRIPE, Monterey, California, July 2003). In situ data sets of aerosol size distribution, chemical composition, and updraft velocities are used as input for the NS parameterization, and the evaluation is carried out by comparing predicted cloud droplet number concentrations (CDNC) with observations. This is the first known study in which a prognostic cloud droplet activation parameterization has been evaluated against a wide range of observations. On average, predicted droplet concentration in adiabatic regions is within -20% of observations at the base of cumuliform clouds and -30% of observations at different altitudes throughout the stratiform clouds, all within experimental uncertainty. Furthermore, CDNC is well parameterized using either a single mean updraft velocity w or by weighting droplet nucleation rates with a Gaussian probability density function of w. This study suggests that for nonprecipitating warm clouds of variable microphysics, aerosol composition, and size distribution the modified NS parameterization can accurately predict cloud droplet activation and can be successfully implemented for describing the aerosol activation process in global climate models.

  12. A new WRF-Chem treatment for studying regional-scale impacts of cloud processes on aerosol and trace gases in parameterized cumuli

    DOE PAGESBeta

    Berg, L. K.; Shrivastava, M.; Easter, R. C.; Fast, J. D.; Chapman, E. G.; Liu, Y.; Ferrare, R. A.

    2015-02-24

    A new treatment of cloud effects on aerosol and trace gases within parameterized shallow and deep convection, and aerosol effects on cloud droplet number, has been implemented in the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) version 3.2.1 that can be used to better understand the aerosol life cycle over regional to synoptic scales. The modifications to the model include treatment of the cloud droplet number mixing ratio; key cloud microphysical and macrophysical parameters (including the updraft fractional area, updraft and downdraft mass fluxes, and entrainment) averaged over the population of shallow clouds, or a single deep convectivemore » cloud; and vertical transport, activation/resuspension, aqueous chemistry, and wet removal of aerosol and trace gases in warm clouds. These changes have been implemented in both the WRF-Chem chemistry packages as well as the Kain–Fritsch (KF) cumulus parameterization that has been modified to better represent shallow convective clouds. Testing of the modified WRF-Chem has been completed using observations from the Cumulus Humilis Aerosol Processing Study (CHAPS). The simulation results are used to investigate the impact of cloud–aerosol interactions on regional-scale transport of black carbon (BC), organic aerosol (OA), and sulfate aerosol. Based on the simulations presented here, changes in the column-integrated BC can be as large as –50% when cloud–aerosol interactions are considered (due largely to wet removal), or as large as +40% for sulfate under non-precipitating conditions due to sulfate production in the parameterized clouds. The modifications to WRF-Chem are found to account for changes in the cloud droplet number concentration (CDNC) and changes in the chemical composition of cloud droplet residuals in a way that is consistent with observations collected during CHAPS. Efforts are currently underway to port the changes described here to the latest version of WRF-Chem, and it

  13. A new WRF-Chem treatment for studying regional-scale impacts of cloud processes on aerosol and trace gases in parameterized cumuli

    SciTech Connect

    Berg, L. K.; Shrivastava, M.; Easter, R. C.; Fast, J. D.; Chapman, E. G.; Liu, Y.; Ferrare, R. A.

    2015-02-24

    A new treatment of cloud effects on aerosol and trace gases within parameterized shallow and deep convection, and aerosol effects on cloud droplet number, has been implemented in the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) version 3.2.1 that can be used to better understand the aerosol life cycle over regional to synoptic scales. The modifications to the model include treatment of the cloud droplet number mixing ratio; key cloud microphysical and macrophysical parameters (including the updraft fractional area, updraft and downdraft mass fluxes, and entrainment) averaged over the population of shallow clouds, or a single deep convective cloud; and vertical transport, activation/resuspension, aqueous chemistry, and wet removal of aerosol and trace gases in warm clouds. These changes have been implemented in both the WRF-Chem chemistry packages as well as the Kain–Fritsch (KF) cumulus parameterization that has been modified to better represent shallow convective clouds. Testing of the modified WRF-Chem has been completed using observations from the Cumulus Humilis Aerosol Processing Study (CHAPS). The simulation results are used to investigate the impact of cloud–aerosol interactions on regional-scale transport of black carbon (BC), organic aerosol (OA), and sulfate aerosol. Based on the simulations presented here, changes in the column-integrated BC can be as large as –50% when cloud–aerosol interactions are considered (due largely to wet removal), or as large as +40% for sulfate under non-precipitating conditions due to sulfate production in the parameterized clouds. The modifications to WRF-Chem are found to account for changes in the cloud droplet number concentration (CDNC) and changes in the chemical composition of cloud droplet residuals in a way that is consistent with observations collected during CHAPS. Efforts are currently underway to port the changes described here to the latest version of WRF-Chem, and it is

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

    NASA Astrophysics Data System (ADS)

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

    2015-09-01

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

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

    SciTech Connect

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

    2015-09-28

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

  16. Molecular corridors and parameterizations of volatility in the chemical evolution of organic aerosols

    NASA Astrophysics Data System (ADS)

    Li, Ying; Pöschl, Ulrich; Shiraiwa, Manabu

    2016-03-01

    The formation and aging of organic aerosols (OA) proceed through multiple steps of chemical reaction and mass transport in the gas and particle phases, which is challenging for the interpretation of field measurements and laboratory experiments as well as accurate representation of OA evolution in atmospheric aerosol models. Based on data from over 30 000 compounds, we show that organic compounds with a wide variety of functional groups fall into molecular corridors, characterized by a tight inverse correlation between molar mass and volatility. We developed parameterizations to predict the saturation mass concentration of organic compounds containing oxygen, nitrogen, and sulfur from the elemental composition that can be measured by soft-ionization high-resolution mass spectrometry. Field measurement data from new particle formation events, biomass burning, cloud/fog processing, and indoor environments were mapped into molecular corridors to characterize the chemical nature of the observed OA components. We found that less-oxidized indoor OA are constrained to a corridor of low molar mass and high volatility, whereas highly oxygenated compounds in atmospheric water extend to high molar mass and low volatility. Among the nitrogen- and sulfur-containing compounds identified in atmospheric aerosols, amines tend to exhibit low molar mass and high volatility, whereas organonitrates and organosulfates follow high O : C corridors extending to high molar mass and low volatility. We suggest that the consideration of molar mass and molecular corridors can help to constrain volatility and particle-phase state in the modeling of OA particularly for nitrogen- and sulfur-containing compounds.

  17. Parameterization of clear-sky surface irradiance and its implications for estimation of aerosol direct radiative effect and aerosol optical depth

    PubMed Central

    Xia, Xiangao

    2015-01-01

    Aerosols impact clear-sky surface irradiance () through the effects of scattering and absorption. Linear or nonlinear relationships between aerosol optical depth (τa) and have been established to describe the aerosol direct radiative effect on (ADRE). However, considerable uncertainties remain associated with ADRE due to the incorrect estimation of (τa in the absence of aerosols). Based on data from the Aerosol Robotic Network, the effects of τa, water vapor content (w) and the cosine of the solar zenith angle (μ) on are thoroughly considered, leading to an effective parameterization of as a nonlinear function of these three quantities. The parameterization is proven able to estimate with a mean bias error of 0.32 W m−2, which is one order of magnitude smaller than that derived using earlier linear or nonlinear functions. Applications of this new parameterization to estimate τa from , or vice versa, show that the root-mean-square errors were 0.08 and 10.0 Wm−2, respectively. Therefore, this study establishes a straightforward method to derive from τa or estimate τa from measurements if water vapor measurements are available. PMID:26395310

  18. Parameterization of clear-sky surface irradiance and its implications for estimation of aerosol direct radiative effect and aerosol optical depth

    NASA Astrophysics Data System (ADS)

    Xia, Xiangao

    2015-09-01

    Aerosols impact clear-sky surface irradiance () through the effects of scattering and absorption. Linear or nonlinear relationships between aerosol optical depth (τa) and have been established to describe the aerosol direct radiative effect on (ADRE). However, considerable uncertainties remain associated with ADRE due to the incorrect estimation of (τa in the absence of aerosols). Based on data from the Aerosol Robotic Network, the effects of τa, water vapor content (w) and the cosine of the solar zenith angle (μ) on are thoroughly considered, leading to an effective parameterization of as a nonlinear function of these three quantities. The parameterization is proven able to estimate with a mean bias error of 0.32 W m-2, which is one order of magnitude smaller than that derived using earlier linear or nonlinear functions. Applications of this new parameterization to estimate τa from , or vice versa, show that the root-mean-square errors were 0.08 and 10.0 Wm-2, respectively. Therefore, this study establishes a straightforward method to derive from τa or estimate τa from measurements if water vapor measurements are available.

  19. Regional-scale simulations of fungal spore aerosols using an emission parameterization adapted to local measurements of fluorescent biological aerosol particles

    NASA Astrophysics Data System (ADS)

    Hummel, M.; Hoose, C.; Gallagher, M.; Healy, D. A.; Huffman, J. A.; O'Connor, D.; Pöschl, U.; Pöhlker, C.; Robinson, N. H.; Schnaiter, M.; Sodeau, J. R.; Stengel, M.; Toprak, E.; Vogel, H.

    2015-06-01

    Fungal spores as a prominent type of primary biological aerosol particles (PBAP) have been incorporated into the COSMO-ART (Consortium for Small-scale Modelling-Aerosols and Reactive Trace gases) regional atmospheric model. Two literature-based emission rates for fungal spores derived from fungal spore colony counts and chemical tracer measurements were used as a parameterization baseline for this study. A third, new emission parameterization for fluorescent biological aerosol particles (FBAP) was adapted to field measurements from four locations across Europe. FBAP concentrations can be regarded as a lower estimate of total PBAP concentrations. Size distributions of FBAP often show a distinct mode at approx. 3 μm, corresponding to a diameter range characteristic for many fungal spores. Previous studies for several locations have suggested that FBAP are in many cases dominated by fungal spores. Thus, we suggest that simulated FBAP and fungal spore concentrations obtained from the three different emission parameterizations can be compared to FBAP measurements. The comparison reveals that simulated fungal spore concentrations based on literature emission parameterizations are lower than measured FBAP concentrations. In agreement with the measurements, the model results show a diurnal cycle in simulated fungal spore concentrations, which may develop partially as a consequence of a varying boundary layer height between day and night. Temperature and specific humidity, together with leaf area index (LAI), were chosen to drive the new emission parameterization which is fitted to the FBAP observations. The new parameterization results in similar root mean square errors (RMSEs) and correlation coefficients compared to the FBAP observations as the previously existing fungal spore emission parameterizations, with some improvements in the bias. Using the new emission parameterization on a model domain covering western Europe, FBAP in the lowest model layer comprise a

  20. Reduced efficacy of marine cloud brightening geoengineering due to in-plume aerosol coagulation: parameterization and global implications

    NASA Astrophysics Data System (ADS)

    Stuart, G. S.; Stevens, R. G.; Partanen, A.-I.; Jenkins, A. K. L.; Korhonen, H.; Forster, P. M.; Spracklen, D. V.; Pierce, J. R.

    2013-10-01

    The intentional enhancement of cloud albedo via controlled sea-spray injection from ships (marine cloud brightening) has been proposed as a possible method to control anthropogenic global warming; however, there remains significant uncertainty in the efficacy of this method due to, amongst other factors, uncertainties in aerosol and cloud microphysics. A major assumption used in recent cloud- and climate-modeling studies is that all sea spray was emitted uniformly into some oceanic grid boxes, and thus these studies did not account for subgrid aerosol coagulation within the sea-spray plumes. We explore the evolution of these sea-salt plumes using a multi-shelled Gaussian plume model with size-resolved aerosol coagulation. We determine how the final number of particles depends on meteorological conditions, including wind speed and boundary-layer stability, as well as the emission rate and size distribution of aerosol emitted. Under previously proposed injection rates and typical marine conditions, we find that the number of aerosol particles is reduced by over 50%, but this reduction varies from under 10% to over 90% depending on the conditions. We provide a computationally efficient parameterization for cloud-resolving and global-scale models to account for subgrid-scale coagulation, and we implement this parameterization in a global-scale aerosol-climate model. While designed to address subgrid-scale coagulation of sea-salt particles, the parameterization is generally applicable for coagulation of subgrid-scale aerosol from point sources. We find that accounting for this subgrid-scale coagulation reduces cloud droplet number concentrations by 46% over emission regions, and reduces the global mean radiative flux perturbation from -1.5 W m-2 to -0.8 W m-2.

  1. Role of the ambient aerosol in the atmospheric processing of semivolatile contaminants: A parameterized numerical model (Gas-Particle Partitioning (GASPAR))

    NASA Astrophysics Data System (ADS)

    Pirrone, Nicola; Hedgecock, Ian M.; Forlano, Luigi

    2000-04-01

    A parameterized description of the ambient aerosol is the basis of a model that treats both gas-particle partitioning and aqueous phase chemical transformations of semivolatile contaminants. Dividing the aerosol population into source, size, hygroscopic, and compositional classes, it is possible to assess the importance of contaminant-aerosol interactions under varying meteorological conditions. Using mercury as a test case, the model provides not only the quantity and speciation of mercury associated with particulate matter for use in dry deposition models and in conjunction with dispersion/meteorological models, but shows conclusively that deliquesced aerosol particles are not simply transporters of adsorbed mercury, but play an active and significant role in the transformation of elemental to oxidized mercury. The sensitivity analysis carried out using a version of the Direct Decoupled Method has shown the transfer of Hg(II) to the gas phase from the aqueous phase to be highly dependent on the chloride ion concentration in the initial parameterization array which describes the ambient aerosol. The chloride ion concentration has a notable effect on the oxidized Hg that is associated with the particle when the chemistry model reaches steady state. The reason for this is clarified by the dependencies of the neutral Hg containing species concentrations on the rates of mass transfer and the initial concentrations. The presence of soot in the aerosol particles is shown to be particularly important in the partitioning of Hg(II) between the gas, aqueous and particulate phases. The implications, given the higher solubility of most oxidized mercury species compared to elemental mercury, are fundamental for the understanding of the cycling and fate of mercury in the environment.

  2. The evolution of biomass-burning aerosol size distributions due to coagulation: dependence on fire and meteorological details and parameterization

    NASA Astrophysics Data System (ADS)

    Sakamoto, Kimiko M.; Laing, James R.; Stevens, Robin G.; Jaffe, Daniel A.; Pierce, Jeffrey R.

    2016-06-01

    Biomass-burning aerosols have a significant effect on global and regional aerosol climate forcings. To model the magnitude of these effects accurately requires knowledge of the size distribution of the emitted and evolving aerosol particles. Current biomass-burning inventories do not include size distributions, and global and regional models generally assume a fixed size distribution from all biomass-burning emissions. However, biomass-burning size distributions evolve in the plume due to coagulation and net organic aerosol (OA) evaporation or formation, and the plume processes occur on spacial scales smaller than global/regional-model grid boxes. The extent of this size-distribution evolution is dependent on a variety of factors relating to the emission source and atmospheric conditions. Therefore, accurately accounting for biomass-burning aerosol size in global models requires an effective aerosol size distribution that accounts for this sub-grid evolution and can be derived from available emission-inventory and meteorological parameters. In this paper, we perform a detailed investigation of the effects of coagulation on the aerosol size distribution in biomass-burning plumes. We compare the effect of coagulation to that of OA evaporation and formation. We develop coagulation-only parameterizations for effective biomass-burning size distributions using the SAM-TOMAS large-eddy simulation plume model. For the most-sophisticated parameterization, we use the Gaussian Emulation Machine for Sensitivity Analysis (GEM-SA) to build a parameterization of the aged size distribution based on the SAM-TOMAS output and seven inputs: emission median dry diameter, emission distribution modal width, mass emissions flux, fire area, mean boundary-layer wind speed, plume mixing depth, and time/distance since emission. This parameterization was tested against an independent set of SAM-TOMAS simulations and yields R2 values of 0.83 and 0.89 for Dpm and modal width, respectively. The

  3. Parameterization of aerosol and cirrus cloud effects on reflected sunlight spectra measured from space: application of the equivalence theorem

    NASA Astrophysics Data System (ADS)

    Bril, Andrey; Oshchepkov, Sergey; Yokota, Tatsuya; Inoue, Gen

    2007-05-01

    An original methodology to account for aerosol and cirrus cloud contributions to reflected sunlight is described. This method can be applied to the problem of retrieving greenhouse gases from satellite-observed data and is based on the equivalence theorem with further parameterization of the photon path-length probability density function (PPDF). Monte Carlo simulation was used to validate this parameterization for a vertically nonhomogeneous atmosphere including an aerosol layer and cirrus clouds. Initial approximation suggests that the PPDF depends on four parameters that can be interpreted as the effective cloud height, cloud relative reflectance, and two additional factors to account for photon path-length distribution under the cloud. We demonstrate that these parameters can be efficiently retrieved from the nadir radiance measured in the oxygen A-band and from the H2O-saturated area of the CO2 2.0 μm spectral band.

  4. Parameterization of aerosol and cirrus cloud effects on reflected sunlight spectra measured from space: application of the equivalence theorem.

    PubMed

    Bril, Andrey; Oshchepkov, Sergey; Yokota, Tatsuya; Inoue, Gen

    2007-05-01

    An original methodology to account for aerosol and cirrus cloud contributions to reflected sunlight is described. This method can be applied to the problem of retrieving greenhouse gases from satellite-observed data and is based on the equivalence theorem with further parameterization of the photon path-length probability density function (PPDF). Monte Carlo simulation was used to validate this parameterization for a vertically nonhomogeneous atmosphere including an aerosol layer and cirrus clouds. Initial approximation suggests that the PPDF depends on four parameters that can be interpreted as the effective cloud height, cloud relative reflectance, and two additional factors to account for photon path-length distribution under the cloud. We demonstrate that these parameters can be efficiently retrieved from the nadir radiance measured in the oxygen A-band and from the H(2)O-saturated area of the CO(2) 2.0 microm spectral band. PMID:17429457

  5. Reduced efficacy of marine cloud brightening geoengineering due to in-plume aerosol coagulation: parameterization and global implications

    NASA Astrophysics Data System (ADS)

    Stuart, G. S.; Stevens, R. G.; Partanen, A.-I.; Jenkins, A. K. L.; Korhonen, H.; Forster, P. M.; Spracklen, D. V.; Pierce, J. R.

    2013-07-01

    The intentional enhancement of cloud albedo via controlled sea-spray injection from ships (Marine Cloud Brightening) has been proposed as a possible method to control anthropogenic global warming; however, there remains significant uncertainty in the efficacy of this method due to, amongst other factors, uncertainties in aerosol and cloud microphysics. A major assumption used in recent cloud- and climate-modeling studies is that all sea spray was emitted uniformly into some oceanic grid boxes, and thus these studies did not account for sub-grid aerosol coagulation within the sea-spray plumes. We explore the evolution of these sea-salt plumes using a multi-shelled Gaussian plume model with size-resolved aerosol coagulation. We determine how the final number of particles depends on meteorological conditions, including wind speed and boundary-layer stability, as well as the emission rate and size distribution of aerosol emitted. Under previously proposed injection rates and typical marine conditions, we find that the number of aerosol particles is reduced by over 50%, but this reduction varies from under 10% to over 90% depending on the conditions. We provide a computationally efficient parameterization for cloud-resolving and global-scale models to account for sub-grid scale coagulation, and we implement this parameterization in a global-scale aerosol-climate model. We find that accounting for this sub-grid scale coagulation reduces cloud droplet number concentrations by 46% over emission regions, and reduces the global mean radiative flux perturbation from -1.5 W m-2 to -0.8 W m-2.

  6. The Explicit-Cloud Parameterized-Pollutant Hybrid Approach for Aerosol-Cloud Interactions in Multiscale Modelling Framework Models: Tracer Transport Results

    SciTech Connect

    Gustafson, William I.; Berg, Larry K.; Easter, Richard C.; Ghan, Steven J.

    2008-05-30

    All estimates of aerosol indirect effects on the global energy balance have either completely neglected the influence of aerosol on convective clouds or treated the influence in a highly parameterized manner. Embedding cloud-resolving models (CRMs) within each grid cell of a global model provides a multiscale modelling framework for treating both the influence of aerosols on convective as well as stratiform clouds and the influence of all clouds on the aerosol, but treating the interactions explicitly by simulating all aerosol processes in the CRM would be computationally prohibitive. An alternate approach is to use horizontal statistics (e.g., cloud mass flux, cloud fraction, and precipitation) from the CRM simulation to drive a single-column parameterization of cloud effects on the aerosol and then use the aerosol profile to simulate aerosol effects on clouds within the CRM. Here we test this concept for vertical transport by clouds, using a CRM with tracer transport simulated explicitly to serve as a benchmark. We show that this parameterization, driven by the CRM’s cloud mass fluxes, reproduces the tracer transport by the CRM significantly better than a single column model that uses a conventional convective cloud parameterization.

  7. Global modelling of secondary organic aerosol from α-pinene oxidation using a parameterization based on a detailed chemical mechanism

    NASA Astrophysics Data System (ADS)

    Ceulemans, Karl; Müller, Jean-Francois; Compernolle, Steven; Stavrakou, Jenny

    2010-05-01

    Monoterpenes are oxidized in the atmosphere by ozone and the hydroxyl and nitrate radicals. The condensable products resulting from these reactions contribute to Secondary Organic Aerosol (SOA). We have developed a detailed α-pinene chemical mechanism BOREAM (Capouet et al. 2008), in which the primary gas phase chemistry is based on quantum-chemical results, structure activity relationships and experimental data. The secondary chemistry of the most important products is treated explicitly, while further chemistry is reduced by the aid of generic species classes. The partitioning between gas phase and SOA is modeled using Pankow's partitioning approach (Pankow 1994), with vapor pressures (Capouet and Müller 2006) and activity coefficients (Compernolle et al. 2009) obtained from group contribution methods. We will discuss the performance of BOREAM through comparison of model predictions for SOA formation with experimental SOA yields for a large number (>150) of photo-oxidation and dark ozonolysis experiments (Ceulemans et al. 2009). Although the BOREAM SOA yields are significantly higher than in several previous box modeling studies, a reasonable agreement is found in comparison with most laboratory measurements. For use in a global model, the detailed BOREAM chemistry is replaced by a parameterized scheme based on the two-product approach (Odum et al. 1996) with parameters obtained through regressions of full model simulations. The reduced scheme accounts for the dependence of SOA yield on the oxidant (ozone, OH or NO3) and the NOx regime. For example, the reaction of alpha-pinene with OH generates a peroxy radical which, upon reaction with either NO or HO2 leads to the formation of two condensable products. The branching ratios and partitioning coefficients are temperature dependent. We inserted the obtained parameterized scheme in the global model IMAGES, where it is used to represent the SOA formation due to the monoterpenes. For aromatics, isoprene and

  8. Improved parameterization for the vertical flux of dust aerosols emitted by an eroding soil

    Technology Transfer Automated Retrieval System (TEKTRAN)

    The representation of the dust cycle in atmospheric circulation models hinges on an accurate parameterization of the vertical dust flux at emission. However, existing parameterizations of the vertical dust flux vary substantially in their scaling with wind friction velocity, require input parameters...

  9. Importance of including ammonium sulfate ((NH4)2SO4) aerosols for ice cloud parameterization in GCMs

    SciTech Connect

    Bhattacharjee, P. S.; Sud, Yogesh C.; Liu, Xiaohong; Walker, Greg K.; Yang, R.; Wang, Jun

    2010-02-22

    A common deficiency of many cloud-physics parameterizations including the NASA’s microphysics of clouds with aerosol- cloud interactions (hereafter called McRAS-AC) is that they simulate less (larger) than the observed ice cloud particle number (size). A single column model (SCM) of McRAS-AC and Global Circulation Model (GCM) physics together with an adiabatic parcel model (APM) for ice-cloud nucleation (IN) of aerosols were used to systematically examine the influence of ammonium sulfate ((NH4)2SO4) aerosols, not included in the present formulations of McRAS-AC. Specifically, the influence of (NH4)2SO4 aerosols on the optical properties of both liquid and ice clouds were analyzed. First an (NH4)2SO4 parameterization was included in the APM to assess its effect vis-à-vis that of the other aerosols. Subsequently, several evaluation tests were conducted over the ARM-SGP and thirteen other locations (sorted into pristine and polluted conditions) distributed over marine and continental sites with the SCM. The statistics of the simulated cloud climatology were evaluated against the available ground and satellite data. The results showed that inclusion of (NH4)2SO4 in the SCM made a remarkable improvement in the simulated effective radius of ice clouds. However, the corresponding ice-cloud optical thickness increased more than is observed. This can be caused by lack of cloud advection and evaporation. We argue that this deficiency can be mitigated by adjusting the other tunable parameters of McRAS-AC such as precipitation efficiency. Inclusion of ice cloud particle splintering introduced through well- established empirical equations is found to further improve the results. Preliminary tests show that these changes make a substantial improvement in simulating the cloud optical properties in the GCM, particularly by simulating a far more realistic cloud distribution over the ITCZ.

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

    SciTech Connect

    Anthony Prenni; Kreidenweis, Sonia M.

    2012-09-28

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

  11. Using cloud resolving WRF-Chem simulations to explore the aerosol impact on numerical weather prediction and evaluate the aerosol aware Grell-Freitas convective parameterization

    NASA Astrophysics Data System (ADS)

    Grell, Georg; Marrapu, Pallavi; Freitas, Saulo R.; Psckham, Steven E.

    2015-04-01

    A convective parameterization is applied and evaluated that may be used in high resolution non-hydrostatic mesoscale models for weather and air quality prediction, as well as in modeling system with unstructured varying grid resolutions and for convection aware simulations. This scheme is based on a stochastic approach originally implemented by Grell and Devenyi (2002) and described in more detail in Grell and Freitas (2014, ACP). Interactions with aerosols have been implemented through a CCN dependent autoconversion of cloud water to rain as well as an aerosol dependent evaporation of cloud drops. Initial tests with this newly implemented aerosol approach showed plausible results with a decrease in predicted precipitation in some areas, caused by the changed autoconversion mechanism. Here we compare and evaluate performance over a 10-day period using the SAMBBA test case of the Working Group for Numerical Experimentation (WGNE) on aerosol impacts on numerical weather prediction. A shorter period is also compared to fully cloud-resolving simulations using WRF-Chem.

  12. Cloud/Aerosol Parameterizations: Application and Improvement of General Circulation Models

    SciTech Connect

    Penner, Joyce

    2012-06-30

    One of the biggest uncertainties associated with climate models and climate forcing is the treatment of aerosols and their effects on clouds. The effect of aerosols on clouds can be divided into two components: The first indirect effect is the forcing associated with increases in droplet concentrations; the second indirect effect is the forcing associated with changes in liquid water path, cloud morphology, and cloud lifetime. Both are highly uncertain. This project applied a cloud-resolving model to understand the response of clouds under a variety of conditions to changes in aerosols. These responses are categorized according to the large-scale meteorological conditions that lead to the response. Meteorological conditions were sampled from various fields, which, together with a global aerosol model determination of the change in aerosols from present day to pre-industrial conditions, was used to determine a first order estimate of the response of global cloud fields to changes in aerosols. The response of the clouds in the NCAR CAM3 GCM coupled to our global aerosol model were tested by examining whether the response is similar to that of the cloud resolving model and methods for improving the representation of clouds and cloud/aerosol interactions were examined.

  13. Reconciliation of coarse mode sea-salt aerosol particle size measurements and parameterizations at a subtropical ocean receptor site

    NASA Astrophysics Data System (ADS)

    Reid, Jeffrey S.; Brooks, Barbara; Crahan, Katie K.; Hegg, Dean A.; Eck, Thomas F.; O'Neill, Norm; de Leeuw, Gerrit; Reid, Elizabeth A.; Anderson, Kenneth D.

    2006-01-01

    In August/September of 2001, the R/P FLIP and CIRPAS Twin Otter research aircraft were deployed to the eastern coast of Oahu, Hawaii, as part of the Rough Evaporation Duct (RED) experiment. Goals included the study of the air/sea exchange, turbulence, and sea-salt aerosol particle characteristics at the subtropical marine Pacific site. Here we examine coarse mode particle size distributions. Similar to what has been shown for airborne dust, optical particle counters such as the Forward Scattering Spectrometer Probe (FSSP), Classical Scattering Aerosol Spectrometer Probe (CSASP) and the Cloud Aerosol Spectrometer (CAS) within the Cloud Aerosol and Precipitation Spectrometer (CAPS) instrument systematically overestimate particle size, and consequently volume, for sea salt particles. Ground-based aerodynamic particle sizers (APS) and AERONET inversions yield much more reasonable results. A wing pod mounted APS gave mixed results and may not be appropriate for marine boundary layer studies. Relating our findings to previous studies does much to explain the bulk of the differences in the literature and leads us to conclude that the largest uncertainty facing flux and airborne cloud/aerosol interaction studies is likely due to the instrumentation itself. To our knowledge, there does not exist an in situ aircraft system that adequately measures the ambient volume distribution of coarse mode sea salt particles. Most empirically based sea salt flux parameterizations can trace their heritage to a clearly biased measurement technique. The current "state of the art" in this field prevents any true form of clear sky radiative "closure" for clean marine environments.

  14. Comparing momentum and mass (aerosol source function) fluxes for the North Atlantic and the European Arctic using different parameterizations

    NASA Astrophysics Data System (ADS)

    Wróbel, Iwona; Piskozub, Jacek

    2016-04-01

    Wind speed has a disproportionate role in the forming of the climate as well it is important part in calculate of the air-sea interaction thanks which we can study climate change. It influences on mass, momentum and energy fluxes and the standard way of parametrizing those fluxes is use this variable. However, the very functions used to calculate fluxes from winds have evolved over time and still have large differences (especially in the case of aerosol sources function). As we have shown last year at the EGU conference (PICO presentation EGU2015-11206-1) and in recent public article (OSD 12,C1262-C1264,2015) there is a lot of uncertainties in the case of air-sea CO2 fluxes. In this study we calculated regional and global mass and momentum fluxes based on several wind speed climatologies. To do this we use wind speed from satellite data in FluxEngine software created within OceanFlux GHG Evolution project. Our main area of interest is European Arctic because of the interesting air-sea interaction physics (six-monthly cycle, strong wind and ice cover) but because of better data coverage we have chosen the North Atlantic as a study region to make it possible to compare the calculated fluxes to measured ones. An additional reason was the importance of the area for the North Hemisphere climate, and especially for Europe. The study is related to an ESA funded OceanFlux GHG Evolution project and is meant to be part of a PhD thesis (of I.W) funded by Centre of Polar Studies "POLAR-KNOW" (a project of the Polish Ministry of Science). We have used a modified version FluxEngine, a tool created within an earlier ESA funded project (OceanFlux Greenhouse Gases) for calculating trace gas fluxes to derive two purely wind driven (at least in the simplified form used in their parameterizations) fluxes. The modifications included removing gas transfer velocity formula from the toolset and replacing it with the respective formulas for momentum transfer and mass (aerosol production

  15. Scanning Backscatter Lidar Observations for Characterizing 4-D Cloud and Aerosol Fields to Improve Radiative Transfer Parameterizations

    NASA Technical Reports Server (NTRS)

    Schwemmer, Geary K.; Miller, David O.

    2005-01-01

    Clouds have a powerful influence on atmospheric radiative transfer and hence are crucial to understanding and interpreting the exchange of radiation between the Earth's surface, the atmosphere, and space. Because clouds are highly variable in space, time and physical makeup, it is important to be able to observe them in three dimensions (3-D) with sufficient resolution that the data can be used to generate and validate parameterizations of cloud fields at the resolution scale of global climate models (GCMs). Simulation of photon transport in three dimensionally inhomogeneous cloud fields show that spatial inhomogeneities tend to decrease cloud reflection and absorption and increase direct and diffuse transmission, Therefore it is an important task to characterize cloud spatial structures in three dimensions on the scale of GCM grid elements. In order to validate cloud parameterizations that represent the ensemble, or mean and variance of cloud properties within a GCM grid element, measurements of the parameters must be obtained on a much finer scale so that the statistics on those measurements are truly representative. High spatial sampling resolution is required, on the order of 1 km or less. Since the radiation fields respond almost instantaneously to changes in the cloud field, and clouds changes occur on scales of seconds and less when viewed on scales of approximately 100m, the temporal resolution of cloud properties should be measured and characterized on second time scales. GCM time steps are typically on the order of an hour, but in order to obtain sufficient statistical representations of cloud properties in the parameterizations that are used as model inputs, averaged values of cloud properties should be calculated on time scales on the order of 10-100 s. The Holographic Airborne Rotating Lidar Instrument Experiment (HARLIE) provides exceptional temporal (100 ms) and spatial (30 m) resolution measurements of aerosol and cloud backscatter in three

  16. Parameterization of single-scattering albedo (SSA) and absorption Ångström exponent (AAE) with EC / OC for aerosol emissions from biomass burning

    NASA Astrophysics Data System (ADS)

    Pokhrel, Rudra P.; Wagner, Nick L.; Langridge, Justin M.; Lack, Daniel A.; Jayarathne, Thilina; Stone, Elizabeth A.; Stockwell, Chelsea E.; Yokelson, Robert J.; Murphy, Shane M.

    2016-08-01

    Single-scattering albedo (SSA) and absorption Ångström exponent (AAE) are two critical parameters in determining the impact of absorbing aerosol on the Earth's radiative balance. Aerosol emitted by biomass burning represent a significant fraction of absorbing aerosol globally, but it remains difficult to accurately predict SSA and AAE for biomass burning aerosol. Black carbon (BC), brown carbon (BrC), and non-absorbing coatings all make substantial contributions to the absorption coefficient of biomass burning aerosol. SSA and AAE cannot be directly predicted based on fuel type because they depend strongly on burn conditions. It has been suggested that SSA can be effectively parameterized via the modified combustion efficiency (MCE) of a biomass burning event and that this would be useful because emission factors for CO and CO2, from which MCE can be calculated, are available for a large number of fuels. Here we demonstrate, with data from the FLAME-4 experiment, that for a wide variety of globally relevant biomass fuels, over a range of combustion conditions, parameterizations of SSA and AAE based on the elemental carbon (EC) to organic carbon (OC) mass ratio are quantitatively superior to parameterizations based on MCE. We show that the EC / OC ratio and the ratio of EC / (EC + OC) both have significantly better correlations with SSA than MCE. Furthermore, the relationship of EC / (EC + OC) with SSA is linear. These improved parameterizations are significant because, similar to MCE, emission factors for EC (or black carbon) and OC are available for a wide range of biomass fuels. Fitting SSA with MCE yields correlation coefficients (Pearson's r) of ˜ 0.65 at the visible wavelengths of 405, 532, and 660 nm while fitting SSA with EC / OC or EC / (EC + OC) yields a Pearson's r of 0.94-0.97 at these same wavelengths. The strong correlation coefficient at 405 nm (r = 0.97) suggests that parameterizations based on EC / OC or EC / (EC + OC) have good predictive

  17. A parameterization of cloud droplet nucleation

    SciTech Connect

    Ghan, S.J. ); Chuang, C.; Penner, J.E. )

    1993-01-01

    Droplet nucleation is a fundamental cloud process. The number of aerosols activated to form cloud droplets influences not only the number of aerosols scavenged by clouds but also the size of the cloud droplets. Cloud droplet size influences the cloud albedo and the conversion of cloud water to precipitation. Global aerosol models are presently being developed with the intention of coupling with global atmospheric circulation models to evaluate the influence of aerosols and aerosol-cloud interactions on climate. If these and other coupled models are to address issues of aerosol-cloud interactions, the droplet nucleation process must be adequately represented. Here we introduce a droplet nucleation parametrization that offers certain advantages over the popular Twomey (1959) parameterization.

  18. Comment on "Reduced efficacy of marine cloud brightening geoengineering due to in-plume aerosol coagulation: parameterization and global implications" by Stuart et al. (2013)

    NASA Astrophysics Data System (ADS)

    Anand, S.; Mayya, Y. S.

    2015-01-01

    We examine the parameterized model of Stuart et al. (2013) vis-à-vis a diffusion-based model proposed by us earlier (Anand and Mayya, 2011) to estimate the fraction of aerosol particles surviving coagulation in a dispersing plume. While the Stuart et al. approach is based on the solutions to the coagulation problem in an expanding plume model, the diffusion-based approach solves the diffusion-coagulation equation for a steady-state standing plume to arrive at the survival fraction correlations. We discuss the differences in the functional forms of the survival fraction expressions obtained in the two approaches and compare the results for the case studies presented in Stuart et al. (2013) involving different particle emission rates and atmospheric stability categories. There appears to be a better agreement between the two models at higher survival fractions as compared to lower survival fractions; on the whole, the two models agree with each other within a difference of 10%. The diffusion-based expression involves a single exponent fit to a theoretically generated similarity variable combining the parameters of the problem with inbuilt exponents and hence avoids the multi-exponent parameterization exercise. It also possesses a wider range of applicability in respect of the source and atmospheric parameters as compared to that based on parameterization. However, in the diffusion model, the choice of a representative value for the coagulation coefficient is more prescriptive than rigorous, which has been addressed in a more satisfactory manner by the parameterization method. The present comparative exercise, although limited in scope, confirms the importance of aerosol microphysical processes envisaged by Stuart et al. for cloud brightening applications. In a larger context, it seems to suggest that either of the two forms of expressions might be suitable for incorporation into global-/regional-scale air pollution models for predicting the contribution of localized

  19. Development and testing of an aerosol/stratus cloud parameterization scheme for middle and high latitudes. Final technical progress report, November 1, 1994--October 31, 1998

    SciTech Connect

    Kreidenweis, S.M.; Cotton, W.R.

    1999-05-20

    At the present time, general circulation models (GCMs) poorly represent clouds, to the extent that they cannot be relied upon to simulate the climatic effects of increasing concentrations of greenhouse gases, or of anthropogenic perturbations to concentrations of cloud condensation nuclei (CCN) or ice nuclei (IN). The long-term objective of this research was the development of an aerosol/cloud microphysics parameterization of mixed-phase stratus and boundary-layer clouds which responds to variations in CCN and IN. The work plan was to perform simulations of these cloud systems to gain understanding of their dynamics and microphysics, especially how aerosols affect cloud development and properties, that cold then be used to guide parameterizations. Several versions of the CSU RAMS (Regional Atmospheric Modeling System), modified to treat Arctic clouds, have been used during the course of this work. The authors also developed a new modeling system, the Trajectory Ensemble Model, to perform detailed chemical and microphysical simulations off-line from the host LES model. The increased understanding of the cloud systems investigated in this research can be applied to a single-column cloud model, designed as an adaptive grid model which can interface into a GCM vertical grid through distinct layers of the troposphere where the presence of layer clouds is expected.

  20. Development and testing of an aerosol/stratus cloud parameterization scheme for middle and high latitudes. Year 3 technical progress report, November 1, 1996--August 31, 1997

    SciTech Connect

    Kreidenweis, S.M.; Cotton, W.R.

    1997-09-02

    At the present time, general circulation models (GCMs) poorly represent clouds, to the extent that they cannot be relied upon to simulate the climatic effects of increasing concentrations of greenhouse gases, or of anthropogenic perturbations to concentrations of cloud condensation nuclei (CCN) or ice nuclei (IN). The net radiative forcing of clouds varies strongly with latitude. Poleward of 30 degrees in both hemispheres, low-level clouds create a net cooling effect corresponding to radiative divergences of {minus}50 to {minus}100 W/m{sup 2}. It is likely that a combination of fogs, boundary-layer stratocumulus, and stratus clouds are the main contributors to this forcing. Models of the response of the microphysical and radiative properties of clouds to changes in aerosol abundance, for a variety of large-scale meteorological forcings, are important additions to GCMs used for the study of the role of Arctic systems in global climate. The overall objective of this research is the development of an aerosol/cloud microphysics parameterization of mixed-phase stratus and boundary-layer clouds which responds to variations in CCN and IN. The parameterization is to be designed for ultimate use in GCM simulations as a tool in understanding the role of CCN, IN, and Arctic clouds in radiation budgets. Several versions of the CSU RAMS (Regional Atmospheric Modeling System) will be used during the course of this work. The parameterizations developed in this research are intended for application in a single-column cloud model, designed as an adaptive grid model which can interface into a GCM vertical grid through distinct layers of the troposphere where the presence of layer clouds is expected.

  1. Final Report for “Simulating the Arctic Winter Longwave Indirect Effects. A New Parameterization for Frost Flower Aerosol Salt Emissions” (DESC0006679) for 9/15/2011 through 9/14/2015

    SciTech Connect

    Russell, Lynn M.; Somerville, Richard C.J.; Burrows, Susannah; Rasch, Phil

    2015-12-12

    Description of the Project: This project has improved the aerosol formulation in a global climate model by using innovative new field and laboratory observations to develop and implement a novel wind-driven sea ice aerosol flux parameterization. This work fills a critical gap in the understanding of clouds, aerosol, and radiation in polar regions by addressing one of the largest missing particle sources in aerosol-climate modeling. Recent measurements of Arctic organic and inorganic aerosol indicate that the largest source of natural aerosol during the Arctic winter is emitted from crystal structures, known as frost flowers, formed on a newly frozen sea ice surface [Shaw et al., 2010]. We have implemented the new parameterization in an updated climate model making it the first capable of investigating how polar natural aerosol-cloud indirect effects relate to this important and previously unrecognized sea ice source. The parameterization is constrained by Arctic ARM in situ cloud and radiation data. The modified climate model has been used to quantify the potential pan-Arctic radiative forcing and aerosol indirect effects due to this missing source. This research supported the work of one postdoc (Li Xu) for two years and contributed to the training and research of an undergraduate student. This research allowed us to establish a collaboration between SIO and PNNL in order to contribute the frost flower parameterization to the new ACME model. One peer-reviewed publications has already resulted from this work, and a manuscript for a second publication has been completed. Additional publications from the PNNL collaboration are expected to follow.

  2. Stochastic Convection Parameterizations

    NASA Technical Reports Server (NTRS)

    Teixeira, Joao; Reynolds, Carolyn; Suselj, Kay; Matheou, Georgios

    2012-01-01

    computational fluid dynamics, radiation, clouds, turbulence, convection, gravity waves, surface interaction, radiation interaction, cloud and aerosol microphysics, complexity (vegetation, biogeochemistry, radiation versus turbulence/convection stochastic approach, non-linearities, Monte Carlo, high resolutions, large-Eddy Simulations, cloud structure, plumes, saturation in tropics, forecasting, parameterizations, stochastic, radiation-clod interaction, hurricane forecasts

  3. New and extended parameterization of the thermodynamic model AIOMFAC: calculation of activity coefficients for organic-inorganic mixtures containing carboxyl, hydroxyl, carbonyl, ether, ester, alkenyl, alkyl, and aromatic functional groups

    NASA Astrophysics Data System (ADS)

    Zuend, A.; Marcolli, C.; Booth, A. M.; Lienhard, D. M.; Soonsin, V.; Krieger, U. K.; Topping, D. O.; McFiggans, G.; Peter, T.; Seinfeld, J. H.

    2011-09-01

    We present a new and considerably extended parameterization of the thermodynamic activity coefficient model AIOMFAC (Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients) at room temperature. AIOMFAC combines a Pitzer-like electrolyte solution model with a UNIFAC-based group-contribution approach and explicitly accounts for interactions between organic functional groups and inorganic ions. Such interactions constitute the salt-effect, may cause liquid-liquid phase separation, and affect the gas-particle partitioning of aerosols. The previous AIOMFAC version was parameterized for alkyl and hydroxyl functional groups of alcohols and polyols. With the goal to describe a wide variety of organic compounds found in atmospheric aerosols, we extend here the parameterization of AIOMFAC to include the functional groups carboxyl, hydroxyl, ketone, aldehyde, ether, ester, alkenyl, alkyl, aromatic carbon-alcohol, and aromatic hydrocarbon. Thermodynamic equilibrium data of organic-inorganic systems from the literature are critically assessed and complemented with new measurements to establish a comprehensive database. The database is used to determine simultaneously the AIOMFAC parameters describing interactions of organic functional groups with the ions H+, Li+, Na+, K+, NH4+, Mg2+, Ca2+, Cl-, Br-, NO3-, HSO4-, and SO42-. Detailed descriptions of different types of thermodynamic data, such as vapor-liquid, solid-liquid, and liquid-liquid equilibria, and their use for the model parameterization are provided. Issues regarding deficiencies of the database, types and uncertainties of experimental data, and limitations of the model, are discussed. The challenging parameter optimization problem is solved with a novel combination of powerful global minimization algorithms. A number of exemplary calculations for systems containing atmospherically relevant aerosol components are shown. Amongst others, we discuss aqueous mixtures of ammonium sulfate with

  4. New and extended parameterization of the thermodynamic model AIOMFAC: calculation of activity coefficients for organic-inorganic mixtures containing carboxyl, hydroxyl, carbonyl, ether, ester, alkenyl, alkyl, and aromatic functional groups

    NASA Astrophysics Data System (ADS)

    Zuend, A.; Marcolli, C.; Booth, A. M.; Lienhard, D. M.; Soonsin, V.; Krieger, U. K.; Topping, D. O.; McFiggans, G.; Peter, T.; Seinfeld, J. H.

    2011-05-01

    We present a new and considerably extended parameterization of the thermodynamic activity coefficient model AIOMFAC (Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients) at room temperature. AIOMFAC combines a Pitzer-like electrolyte solution model with a UNIFAC-based group-contribution approach and explicitly accounts for interactions between organic functional groups and inorganic ions. Such interactions constitute the salt-effect, may cause liquid-liquid phase separation, and affect the gas-particle partitioning of aerosols. The previous AIOMFAC version was parameterized for alkyl and hydroxyl functional groups of alcohols and polyols. With the goal to describe a wide variety of organic compounds found in atmospheric aerosols, we extend here the parameterization of AIOMFAC to include the functional groups carboxyl, hydroxyl, ketone, aldehyde, ether, ester, alkenyl, alkyl, aromatic carbon-alcohol, and aromatic hydrocarbon. Thermodynamic equilibrium data of organic-inorganic systems from the literature are critically assessed and complemented with new measurements to establish a comprehensive database. The database is used to determine simultaneously the AIOMFAC parameters describing interactions of organic functional groups with the ions H+, Li+, Na+, K+, NH4+, Mg2+, Ca2+, Cl-, Br-, NO3-, HSO4-, and SO42-. Detailed descriptions of different types of thermodynamic data, such as vapor-liquid, solid-liquid, and liquid-liquid equilibria, and their use for the model parameterization are provided. Issues regarding deficiencies of the database, types and uncertainties of experimental data, and limitations of the model, are discussed. The challenging parameter optimization problem is solved with a novel combination of powerful global minimization algorithms. A number of exemplary calculations for systems containing atmospherically relevant aerosol components are shown. Amongst others, we discuss aqueous mixtures of ammonium sulfate with

  5. Effects of Aerosols on Cloud Albedo: Evaluation of Twomey's Parameterization of Cloud Susceptibility Using Measurements of Ship Tracks.

    NASA Astrophysics Data System (ADS)

    Ackerman, Andrew S.; Toon, Owen B.; Taylor, Jonathan P.; Johnson, Doug W.; Hobbs, Peter V.; Ferek, Ronald J.

    2000-08-01

    Airborne measurements from the Meteorological Research Flight's Hercules C-130 and the University of Washington's Convair C-131A during the Monterey Area Ship Track field project are used to evaluate Twomey's analytic expression for cloud susceptibility, which describes the sensitivity of cloud albedo to changes in droplet concentrations. This expression incorporates assumptions about cloud physics, such as the independence of the cloud liquid water content and the width of the droplet size distribution on droplet concentrations. Averaged over all 69 ship track penetrations, cloud liquid water content decreased slightly and the droplet size distributions broadened from the ambient values. For the 17 cases for which albedos were measured during overflights, Twomey's parameterization represents the trend of albedo changes with droplet concentrations remarkably well, passing through the midpoints of the considerable spread in the data. The fortuitous agreement results from compensating changes in cloud properties. Together with the albedo changes, the changes in cloud liquid water content and droplet size distributions imply that cloud thickness usually increased in the ship tracks. Such an increase was observed on the occasions that changes in cloud thickness were recorded (in the Sanko Peace ship track during very clean ambient conditions). Unfortunately systematic measurements of cloud thickness were not made for most of the ship tracks observed. The greatest outlier in the data corresponds to measurements made under horizontally inhomogeneous ambient conditions; possible explanations for its divergence include an increase in cloud thickness or an error in matching above-cloud albedo measurements with in-cloud microphysics measurements.

  6. Neural network radiative transfer solvers for the generation of high resolution solar irradiance spectra parameterized by cloud and aerosol parameters

    NASA Astrophysics Data System (ADS)

    Taylor, M.; Kosmopoulos, P. G.; Kazadzis, S.; Keramitsoglou, I.; Kiranoudis, C. T.

    2016-01-01

    This paper reports on the development of a neural network (NN) model for instantaneous and accurate estimation of solar radiation spectra and budgets geared toward satellite cloud data using a ≈2.4 M record, high-spectral resolution look up table (LUT) generated with the radiative transfer model libRadtran. Two NN solvers, one for clear sky conditions dominated by aerosol and one for cloudy skies, were trained on a normally-distributed and multiparametric subset of the LUT that spans a very broad class of atmospheric and meteorological conditions as inputs with corresponding high resolution solar irradiance target spectra as outputs. The NN solvers were tested by feeding them with a large (10 K record) "off-grid" random subset of the LUT spanning the training data space, and then comparing simulated outputs with target values provided by the LUT. The NN solvers demonstrated a capability to interpolate accurately over the entire multiparametric space. Once trained, the NN solvers allow for high-speed estimation of solar radiation spectra with high spectral resolution (1 nm) and for a quantification of the effect of aerosol and cloud optical parameters on the solar radiation budget without the need for a massive database. The cloudy sky NN solver was applied to high spatial resolution (54 K pixel) cloud data extracted from the Spinning Enhanced Visible and Infrared Imager (SEVIRI) onboard the geostationary Meteosat Second Generation 3 (MSG3) satellite and demonstrated that coherent maps of spectrally-integrated global horizontal irradiance at this resolution can be produced on the order of 1 min.

  7. Parameterization of thermal properties of aging secondary organic aerosol produced by photo-oxidation of selected terpene mixtures.

    PubMed

    Emanuelsson, Eva U; Mentel, Thomas F; Watne, Agot K; Spindler, Christian; Bohn, Birger; Brauers, Theo; Dorn, Hans-Peter; Hallquist, Asa M; Häseler, Rolf; Kiendler-Scharr, Astrid; Müller, Klaus-Peter; Pleijel, Håkan; Rohrer, Franz; Rubach, Florian; Schlosser, Eric; Tillmann, Ralf; Hallquist, Mattias

    2014-06-01

    Formation and evolution of secondary organic aerosols (SOA) from biogenic VOCs influences the Earth's radiative balance. We have examined the photo-oxidation and aging of boreal terpene mixtures in the SAPHIR simulation chamber. Changes in thermal properties and chemical composition, deduced from mass spectrometric measurements, were providing information on the aging of biogenic SOA produced under ambient solar conditions. Effects of precursor mixture, concentration, and photochemical oxidation levels (OH exposure) were evaluated. OH exposure was found to be the major driver in the long term photochemical transformations, i.e., reaction times of several hours up to days, of SOA and its thermal properties, whereas the initial concentrations and terpenoid mixtures had only minor influence. The volatility distributions were parametrized using a sigmoidal function to determine TVFR0.5 (the temperature yielding a 50% particle volume fraction remaining) and the steepness of the volatility distribution. TVFR0.5 increased by 0.3±0.1% (ca. 1 K), while the steepness increased by 0.9±0.3% per hour of 1×10(6) cm(-3) OH exposure. Thus, aging reduces volatility and increases homogeneity of the vapor pressure distribution, presumably because highly volatile fractions become increasingly susceptible to gas phase oxidation, while less volatile fractions are less reactive with gas phase OH. PMID:24810838

  8. Laboratory Studies of Processing of Carbonaceous Aerosols by Atmospheric Oxidants/Hygroscopicity and CCN Activity of Secondary & Processed Primary Organic Aerosols

    SciTech Connect

    Ziemann, P.J.; Arey, J.; Atkinson, R.; Kreidenweis, S.M.; Petters, M.D.

    2012-06-13

    to carry out reactions of representative anthropogenic and biogenic VOCs and organic particles with ozone (O3), and hydroxyl (OH), nitrate (NO3), and chlorine (Cl) radicals, which are the major atmospheric oxidants, under simulated atmospheric conditions in large-volume environmental chambers. A combination of on-line and off-line analytical techniques were used to monitor the chemical and physical properties of the particles including their hygroscopicity and CCN activity. The results of the studies were used to (1) improve scientific understanding of the relationships between the chemical composition of organic particles and their hygroscopicity and CCN activity, (2) develop an improved molecular level theoretical framework for describing these relationships, and (3) establish a large database that is being used to develop parameterizations relating organic aerosol chemical properties and SOA sources to particle hygroscopicity and CCN activity for use in regional and global atmospheric air quality and climate models.

  9. Redox activity of naphthalene secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    McWhinney, R. D.; Zhou, S.; Abbatt, J. P. D.

    2013-04-01

    Chamber secondary organic aerosol (SOA) from low-NOx photooxidation of naphthalene by hydroxyl radical was examined with respect to its redox cycling behaviour using the dithiothreitol (DTT) assay. Naphthalene SOA was highly redox active, consuming DTT at an average rate of 118 ± 14 pmol per minute per μg of SOA material. Measured particle-phase masses of the major previously identified redox active products, 1,2- and 1,4-naphthoquinone, accounted for only 21 ± 3% of the observed redox cycling activity. The redox-active 5-hydroxy-1,4-naphthoquinone was identified as a new minor product of naphthalene oxidation, and including this species in redox activity predictions increased the predicted DTT reactivity to 30 ± 5% of observations. Similar attempts to predict redox behaviour of oxidised two-stroke engine exhaust particles by measuring 1,2-naphthoquinone, 1,4-naphthoquinone and 9,10-phenanthrenequinone predicted DTT decay rates only 4.9 ± 2.5% of those observed. Together, these results suggest that there are substantial unidentified redox-active SOA constituents beyond the small quinones that may be important toxic components of these particles. A gas-to-SOA particle partitioning coefficient was calculated to be (7.0 ± 2.5) × 10-4 m3 μg-1 for 1,4-naphthoquinone at 25 °C. This value suggests that under typical warm conditions, 1,4-naphthoquinone is unlikely to contribute strongly to redox behaviour of ambient particles, although further work is needed to determine the potential impact under conditions such as low temperatures where partitioning to the particle is more favourable. As well, higher order oxidation products that likely account for a substantial fraction of the redox cycling capability of the naphthalene SOA are likely to partition much more strongly to the particle phase.

  10. A New Method for Multicomponent Activity Coefficients of Electrolytes in Aqueous Atmospheric Aerosols

    SciTech Connect

    Zaveri, Rahul A.; Easter, Richard C.; Wexler, Anthony S.

    2005-01-21

    Three-dimensional models of atmospheric inorganic aerosols need an accurate yet computationally efficient parameterization of activity coefficients of various electrolytes in multicomponent aqueous solutions. This paper describes the development and application of a new mixing rule for calculating activity coefficients of electrolytes typically found in atmospheric aerosol systems containing H+, NH4+, Na+, Ca2+ SO42-, HSO4-, NO3-, and Cl- ions. The new mixing rule, called MTEM (Multicomponent Taylor Expansion Model), estimates the mean activity coefficient of an electrolyte in a multicomponent solution based on its values in binary solutions of all the electrolytes present in the mixture at the solution water activity aw, assuming aw is equal to the ambient relative humidity. The aerosol water content is calculated using the Zdanovskii-Stokes-Robinson method. For self-consistency, most of the MTEM and Zdanovskii-Stokes-Robinson parameters are derived using the comprehensive Pitzer-Simonson-Clegg model at 298.15 K. MTEM is evaluated for several multicomponent systems representing various continental and marine aerosols, and is contrasted against the mixing rule of Kusik and Meissner and the newer approach of Metzger et al. [2002]. Predictions of MTEM are found to be generally within a factor of 0.8 to 1.25 of the comprehensive Pitzer-Simonson-Clegg model, and are shown to be significantly more accurate than predictions of the other two methods. MTEM also yields a non-iterative solution of the bisulfate ion dissociation in sulfate-rich systems – a major computational advantage over other iterative methods. CPU time requirements of MTEM relative to other methods for sulfate-poor and sulfate-rich systems are also discussed.

  11. Models to support active sensing of biological aerosol clouds

    NASA Astrophysics Data System (ADS)

    Brown, Andrea M.; Kalter, Jeffrey M.; Corson, Elizabeth C.; Chaudhry, Zahra; Boggs, Nathan T.; Brown, David M.; Thomas, Michael E.; Carter, Christopher C.

    2013-05-01

    Elastic backscatter LIght Detection And Ranging (LIDAR) is a promising approach for stand-off detection of biological aerosol clouds. Comprehensive models that explain the scattering behavior from the aerosol cloud are needed to understand and predict the scattering signatures of biological aerosols under varying atmospheric conditions and against different aerosol backgrounds. Elastic signatures are dependent on many parameters of the aerosol cloud, with two major components being the size distribution and refractive index of the aerosols. The Johns Hopkins University Applied Physics Laboratory (JHU/APL) has been in a unique position to measure the size distributions of released biological simulant clouds using a wide assortment of aerosol characterization systems that are available on the commercial market. In conjunction with the size distribution measurements, JHU/APL has also been making a dedicated effort to properly measure the refractive indices of the released materials using a thin-film absorption technique and laboratory characterization of the released materials. Intimate knowledge of the size distributions and refractive indices of the biological aerosols provides JHU/APL with powerful tools to build elastic scattering models, with the purpose of understanding, and ultimately, predicting the active signatures of biological clouds.

  12. The ice nucleation activity of biological aerosols

    NASA Astrophysics Data System (ADS)

    Grothe, H.; Pummer, B.; Bauer, H.; Bernardi, J.

    2012-04-01

    Primary Biological Aerosol Particles (PBAPs), including bacteria, spores and pollen may be important for several atmospheric processes. Particularly, the ice nucleation caused by PBAPs is a topic of growing interest, since their impact on ice cloud formation and thus on radiative forcing, an important parameter in global climate is not yet fully understood. In laboratory model studies we investigated the ice nucleation activity of selected PBAPs. We studied the immersion mode freezing using water-oil emulsion, which we observed by optical microscopy. We particularly focused on pollen. We show that pollen of different species strongly differ in their ice nucleation behavior. The average freezing temperatures in laboratory experiments range from 240 K to 255 K. As the most efficient nuclei (silver birch, Scots pine and common juniper pollen) have a distribution area up to the Northern timberline, their ice nucleation activity might be a cryoprotective mechanism. For comparison the ice nucleation activity of Snomax, fungal spores, and mushrooms will be discussed as well. In the past, pollen have been rejected as important atmospheric IN, as they are not as abundant in the atmosphere as bacteria or mineral dust and are too heavy to reach higher altitudes. However, in our experiments (Pummer et al. 2011) it turned out that water, which had been in contact with pollen and then been separated from the bodies, nucleates as good as the pollen grains themselves. So the ice nuclei have to be easily-suspendable macromolecules (100-300 kDa) located on the pollen. Once extracted, they can be distributed further through the atmosphere than the heavy pollen grains and so augment the impact of pollen on ice cloud formation even in the upper troposphere. It is widely known, that material from the pollen, like allergens and sugars, can indeed leave the pollen body and be distributed independently. The most probable mechanism is the pollen grain bursting by rain, which releases

  13. CCN Activity, Hygroscopicity, and Droplet Activation Kinetics of Secondary Organic Aerosol Resulting from the 2010 Gulf Oil Spill

    NASA Astrophysics Data System (ADS)

    Moore, R.; Lathem, T. L.; Cerully, K.; Bahreini, R.; Brock, C. A.; Langridge, J. M.; Middlebrook, A. M.; Nenes, A.; Calnex Science Team

    2010-12-01

    We present an analysis of the hygroscopicity and droplet activation kinetics of cloud condensation nuclei (CCN) sampled onboard the National Oceanic and Atmospheric Administration WP-3D aircraft downwind of the Deepwater Horizon oil spill site on June 8th and 10th, 2010. This set of measurements provides a unique case study for assessing in-situ the impact of fresh, hydrocarbonlike aerosols, which are expected to be formed via gas-to-particle conversion of the semi-volatile vapors released from oil evaporation. Similar hydrocarbon-rich aerosols constitute an important local emissions source in urban areas, but often coexist as an external/partially-internal mixture with more-oxidized, aged organic and sulfate aerosol. The DWH site provides the means to study the hygroscopic properties of these less-oxidized organic aerosols above a cleaner environmental background typical of marine environments in order to better discern their contribution to CCN activity and droplet growth. Measurements were performed with a Droplet Measurement Technologies Streamwise, Thermal-Gradient CCN counter, operating both as a counter (s=0.3%) and as a spectrometer (s=0.2-0.6%) using the newly-developed Scanning Flow CCN Analysis (SFCA) technique [1]. The instrument measures both the number concentration of particles able to nucleate droplets and also their resulting droplet sizes. The measured size information combined with a comprehensive computational fluid dynamics instrument model enables us to determine the rate of water uptake onto the particles and parameterize it in terms of an effective mass transfer coefficient [2], a key parameter needed to predict the number of activated droplets in ambient clouds. Non-refractory aerosol chemical composition was measured with an Aerodyne compact time-of-flight aerosol mass spectrometer. It was observed that the aerosols sampled downwind of the site on both days were composed predominantly of organics with a low degree of oxidation and low

  14. Lightning activity and aerosols in the Mediterranean region

    NASA Astrophysics Data System (ADS)

    Proestakis, E.; Kazadzis, S.; Lagouvardos, K.; Kotroni, V.; Kazantzidis, A.

    2016-03-01

    In the framework of this study, the effect of aerosols on lightning activity has been investigated for the first time over the broader Mediterranean Sea. Atmospheric optical depth data retrieved by MODIS on board Aqua satellite and cloud to ground lightning activity data provided by ZEUS network operated by the National Observatory of Athens were analyzed for a time period spanning from 01/01/2005 up to 31/12/2013. The results indicate the importance of aerosols in lightning modulation. The mean aerosol optical depth (AOD) values of the days with lightning activity were found to be higher than the mean seasonal AOD in 90% of the under study domain. Furthermore, the increasing rate of lightning activity with increasing aerosol loading was found to be more pronounced during summertime and for AOD values up to 0.4. Additionally, the spatial analysis showed that the percentage of days with lightning activity during summertime is increasing with increasing AOD. Finally, time series showed similar temporal behavior between AOD seasonal anomalies and days with lightning activity differences. Both the spatial and temporal analysis showed that lightning activity is correlated to AOD, a characteristic consistent for all seasons.

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

    NASA Astrophysics Data System (ADS)

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

    2014-09-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-04-01

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

  17. Calculating Capstone depleted uranium aerosol concentrations from beta activity measurements.

    PubMed

    Szrom, Frances; Falo, Gerald A; Parkhurst, Mary Ann; Whicker, Jeffrey J; Alberth, David P

    2009-03-01

    Beta activity measurements were used as surrogate measurements of uranium mass in aerosol samples collected during the field testing phase of the Capstone Depleted Uranium (DU) Aerosol Study. These aerosol samples generated by the perforation of armored combat vehicles were used to characterize the DU source term for the subsequent Human Health Risk Assessment (HHRA) of Capstone aerosols. Establishing a calibration curve between beta activity measurements and uranium mass measurements is straightforward if the uranium isotopes are in equilibrium with their immediate short-lived, beta-emitting progeny. For DU samples collected during the Capstone study, it was determined that the equilibrium between the uranium isotopes and their immediate short-lived, beta-emitting progeny had been disrupted when penetrators had perforated target vehicles. Adjustments were made to account for the disrupted equilibrium and for wall losses in the aerosol samplers. Values for the equilibrium fraction ranged from 0.16 to 1, and the wall loss correction factors ranged from 1 to 1.92. This paper describes the process used and adjustments necessary to calculate uranium mass from proportional counting measurements. PMID:19204483

  18. Calculating Capstone Depleted Uranium Aerosol Concentrations from Beta Activity Measurements

    SciTech Connect

    Szrom, Fran; Falo, Gerald A.; Parkhurst, MaryAnn; Whicker, Jeffrey J.; Alberth, David P.

    2009-03-01

    Beta activity measurements were used as surrogate measurements of uranium mass in aerosol samples collected during the field testing phase of the Capstone Depleted Uranium (DU) Aerosol Study. These aerosol samples generated by the perforation of armored combat vehicles were used to characterize the depleted uranium (DU) source term for the subsequent human health risk assessment (HHRA) of Capstone aerosols. Establishing a calibration curve between beta activity measurements and uranium mass measurements is straightforward if the uranium isotopes are in equilibrium with their immediate short-lived, beta-emitting progeny. For DU samples collected during the Capstone study, it was determined that the equilibrium between the uranium isotopes and their immediate short lived, beta-emitting progeny had been disrupted when penetrators had perforated target vehicles. Adjustments were made to account for the disrupted equilibrium and for wall losses in the aerosol samplers. Correction factors for the disrupted equilibrium ranged from 0.16 to 1, and the wall loss correction factors ranged from 1 to 1.92.

  19. Ice Nucleation Activity of Various Agricultural Soil Dust Aerosol Particles

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

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

  20. Biological aerosol detection with combined passive-active infrared measurements

    NASA Astrophysics Data System (ADS)

    Ifarraguerri, Agustin I.; Vanderbeek, Richard G.; Ben-David, Avishai

    2004-12-01

    A data collection experiment was performed in November of 2003 to measure aerosol signatures using multiple sensors, all operating in the long-wave infrared. The purpose of this data collection experiment was to determine whether combining passive hyperspectral and LIDAR measurements can substantially improve biological aerosol detection performance. Controlled releases of dry aerosols, including road dust, egg albumin and two strains of Bacillus Subtilis var. Niger (BG) spores were performed using the ECBC/ARTEMIS open-path aerosol test chamber located in the Edgewood Area of Aberdeen Proving Grounds, MD. The chamber provides a ~ 20' path without optical windows. Ground truth devices included 3 aerodynamic particle sizers, an optical particle size spectrometer, 6 nephelometers and a high-volume particle sampler. Two sensors were used to make measurements during the test: the AIRIS long-wave infrared imaging spectrometer and the FAL CO2 LIDAR. The AIRIS and FAL data sets were analyzed for detection performance relative to the ground truth. In this paper we present experimental results from the individual sensors as well as results from passive-active sensor fusion. The sensor performance is presented in the form of receiver operating characteristic curves.

  1. Ensemble projections of wildfire activity and carbonaceous aerosol concentrations over the western United States in the mid-21st century

    PubMed Central

    Yue, Xu; Mickley, Loretta J.; Logan, Jennifer A.; Kaplan, Jed O.

    2013-01-01

    We estimate future wildfire activity over the western United States during the mid-21st century (2046–2065), based on results from 15 climate models following the A1B scenario. We develop fire prediction models by regressing meteorological variables from the current and previous years together with fire indexes onto observed regional area burned. The regressions explain 0.25–0.60 of the variance in observed annual area burned during 1980–2004, depending on the ecoregion. We also parameterize daily area burned with temperature, precipitation, and relative humidity. This approach explains ~0.5 of the variance in observed area burned over forest ecoregions but shows no predictive capability in the semi-arid regions of Nevada and California. By applying the meteorological fields from 15 climate models to our fire prediction models, we quantify the robustness of our wildfire projections at mid-century. We calculate increases of 24–124% in area burned using regressions and 63–169% with the parameterization. Our projections are most robust in the southwestern desert, where all GCMs predict significant (p<0.05) meteorological changes. For forested ecoregions, more GCMs predict significant increases in future area burned with the parameterization than with the regressions, because the latter approach is sensitive to hydrological variables that show large inter-model variability in the climate projections. The parameterization predicts that the fire season lengthens by 23 days in the warmer and drier climate at mid-century. Using a chemical transport model, we find that wildfire emissions will increase summertime surface organic carbon aerosol over the western United States by 46–70% and black carbon by 20–27% at midcentury, relative to the present day. The pollution is most enhanced during extreme episodes: above the 84th percentile of concentrations, OC increases by ~90% and BC by ~50%, while visibility decreases from 130 km to 100 km in 32 Federal Class 1

  2. Ensemble projections of wildfire activity and carbonaceous aerosol concentrations over the western United States in the mid-21st century

    NASA Astrophysics Data System (ADS)

    Yue, Xu; Mickley, Loretta J.; Logan, Jennifer A.; Kaplan, Jed O.

    2013-10-01

    We estimate future wildfire activity over the western United States during the mid-21st century (2046-2065), based on results from 15 climate models following the A1B scenario. We develop fire prediction models by regressing meteorological variables from the current and previous years together with fire indexes onto observed regional area burned. The regressions explain 0.25-0.60 of the variance in observed annual area burned during 1980-2004, depending on the ecoregion. We also parameterize daily area burned with temperature, precipitation, and relative humidity. This approach explains ˜0.5 of the variance in observed area burned over forest ecoregions but shows no predictive capability in the semi-arid regions of Nevada and California. By applying the meteorological fields from 15 climate models to our fire prediction models, we quantify the robustness of our wildfire projections at midcentury. We calculate increases of 24-124% in area burned using regressions and 63-169% with the parameterization. Our projections are most robust in the southwestern desert, where all GCMs predict significant (p < 0.05) meteorological changes. For forested ecoregions, more GCMs predict significant increases in future area burned with the parameterization than with the regressions, because the latter approach is sensitive to hydrological variables that show large inter-model variability in the climate projections. The parameterization predicts that the fire season lengthens by 23 days in the warmer and drier climate at midcentury. Using a chemical transport model, we find that wildfire emissions will increase summertime surface organic carbon aerosol over the western United States by 46-70% and black carbon by 20-27% at midcentury, relative to the present day. The pollution is most enhanced during extreme episodes: above the 84th percentile of concentrations, OC increases by ˜90% and BC by ˜50%, while visibility decreases from 130 km to 100 km in 32 Federal Class 1 areas in

  3. Ensemble projections of wildfire activity and carbonaceous aerosol concentrations over the western United States in the mid-21st century.

    PubMed

    Yue, Xu; Mickley, Loretta J; Logan, Jennifer A; Kaplan, Jed O

    2013-10-01

    We estimate future wildfire activity over the western United States during the mid-21(st) century (2046-2065), based on results from 15 climate models following the A1B scenario. We develop fire prediction models by regressing meteorological variables from the current and previous years together with fire indexes onto observed regional area burned. The regressions explain 0.25-0.60 of the variance in observed annual area burned during 1980-2004, depending on the ecoregion. We also parameterize daily area burned with temperature, precipitation, and relative humidity. This approach explains ~0.5 of the variance in observed area burned over forest ecoregions but shows no predictive capability in the semi-arid regions of Nevada and California. By applying the meteorological fields from 15 climate models to our fire prediction models, we quantify the robustness of our wildfire projections at mid-century. We calculate increases of 24-124% in area burned using regressions and 63-169% with the parameterization. Our projections are most robust in the southwestern desert, where all GCMs predict significant (p<0.05) meteorological changes. For forested ecoregions, more GCMs predict significant increases in future area burned with the parameterization than with the regressions, because the latter approach is sensitive to hydrological variables that show large inter-model variability in the climate projections. The parameterization predicts that the fire season lengthens by 23 days in the warmer and drier climate at mid-century. Using a chemical transport model, we find that wildfire emissions will increase summertime surface organic carbon aerosol over the western United States by 46-70% and black carbon by 20-27% at midcentury, relative to the present day. The pollution is most enhanced during extreme episodes: above the 84(th) percentile of concentrations, OC increases by ~90% and BC by ~50%, while visibility decreases from 130 km to 100 km in 32 Federal Class 1 areas in

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

    PubMed

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

    2016-04-15

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

  5. Photochemical Activation of Chlorine by Iron and Iron Oxide Aerosol

    NASA Astrophysics Data System (ADS)

    Wittmer, J.; Zetzsch, C.

    2015-12-01

    The photochemical activation of chlorine by dissolved iron in sea-salt aerosol droplets and by highly dispersed Fe2O3 aerosol particles (mainly hematite, specific surface > 100 m2/g), exposed to gaseous HCl, was investigated in humidified air in a Teflon simulation chamber. Employing the radical-clock technique, we quantified the production of gaseous atomic Cl. When the artificial sea salt aerosols contained suspended Fe2O3 alone at pH 6, no significant Cl production could be observed, even if the dissolution of iron was forced by "weathering" (repeatedly freezing and thawing for five times). Adjusting the pH in the stock suspension to 2.6, 2.2, and 1.9 and equilibrating for one week resulted in a quantifiable amount of dissolved iron (0.03, 0.2, and 0.6 mmol/L, respectively) and in gaseous Cl production rates of ~1.6, 6, and 8 × 1021 atoms cm-2 h-1, respectively. Exposing the pure Fe2O3 aerosol in the absence of salt to various gaseous HCl concentrations resulted in rates ranging from 8 × 1020 Cl atoms cm-2 h-1 (at ~4 ppb HCl) to 5 × 1022 Cl atoms cm-2 h-1 (at ~350 ppb HCl) and confirmed the uptake and conversion of HCl to atomic Cl (at HCl to Cl conversion yields of 2-5 % mol/mol, depending on the relative humidity). The relevance for environmental processes in the atmosphere will be discussed.

  6. Observational Evidence of Aerosol Enhancement of Lightning Activity and Convective Invigoration

    NASA Technical Reports Server (NTRS)

    Yuan, Tianle; Remer, Lorraine A.; Pickering, Kenneth E.; Yu, Hongbin

    2011-01-01

    Lightning activity over the West Pacific Ocean east of the Philippines is usually much less frequent than over the nearby maritime continents. However, in 2005 the Lightning Imaging Sensor (LIS) aboard the TRMM satellite observed anomalously high lightning activity in that area. In the same year the Moderate resolution Imaging Spectroradiometer (MODIS) measured anomalously high aerosol loading. The high aerosol loading was traced to volcanic activity, and not to any factor linked to meteorology, disentangling the usual convolution between aerosols and meteorology. We show that in general lightning activity is tightly correlated with aerosol loadings at both inter-annual and biweekly time scales. We estimate that a approximately 60% increase in aerosol loading leads to more than 150% increase in lightning flashes. Aerosols increase lightning activity through modification of cloud microphysics. Cloud ice particle sizes are reduced and cloud glaciation is delayed to colder temperature when aerosol loading is increased. TRMM precipitation radar measurements indicate that anomalously high aerosol loading is associated with enhanced cloud mixed phase activity and invigorated convection over the maritime ocean. These observed associations between aerosols, cloud microphysics, morphology and lightning activity are not related to meteorological variables or ENSO events. The results have important implications for understanding the variability of lightning and resulting aerosol-chemistry interactions.

  7. CCN Activity of Organic Aerosols Observed Downwind of Urban Emissions during CARES

    SciTech Connect

    Mei, Fan; Setyan, Ari; Zhang, Qi; Wang, J. X.

    2013-12-17

    During the Carbonaceous Aerosols and Radiative Effects Study (CARES), activation fraction of size-resolved aerosol particles and aerosol chemical composition were characterized at the T1 site (~60 km downwind of Sacramento, California) from 10 June to 28 June 2010. The hygroscopicity of CCN-active particles (KCCN) with diameter from 100 to 170 nm, derived from the size-resolved activated fraction, varied from 0.10 to 0.21, with an average of 0.15, which was substantially lower than that proposed for continental sites in earlier studies. The low KCCN value was due to the high organic volume fraction, averaged over 80% at the T1 site. The derived KCCN exhibited little diurnal variation, consistent with the relatively constant organic volume fraction observed. At any time, over 90% of the size selected particles with diameter between 100 and 171nm were CCN active, suggesting most particles within this size range were aged background particles. Due to the large organic volume fraction, organic hygroscopicity (Korg) strongly impacted particle hygroscopicity and therefore calculated CCN concentration. For vast majority of the cases, an increase of Korg from 0.03 to 0.18, which are within the typical range, doubled the calculated CCN concentration. Organic hygroscopicity was derived from KCCN and aerosol chemical composition, and its variations with the fraction of total organic mass spectral signal at m/z 44 (f44) and O:C were compared to results from previous studies. Overall, the relationships between Korg and f44 are quite consistent for organic aerosol (OA) observed during field studies and those formed in smog chamber. Compared to the relationship between Korg and f44, the relationship between Korg and O:C exhibits more significant differences among different studies, suggesting korg may be better parameterized using f44. A

  8. 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

  9. Characterization of indoor cooking aerosol using neutron activation analysis

    SciTech Connect

    Wu, D.; Landsberger, S.; Larson, S. )

    1993-01-01

    Suspended particles in air are potentially harmful to human health, depending on their sizes and chemical composition. Residential indoor particles mainly come from (a) outdoor sources that are transported indoors, (b) indoor dust that is resuspended, and (c) indoor combustion sources, which include cigarette smoking, cooking, and heating. Jedrychowski stated that chronic phlegm in elderly women was strongly related to the cooking exposure. Kamens et al. indicated that cooking could generate small particles (<0.1 [mu]m), and cooking one meal could contribute [approximately]5 to 18% of total daytime particle volume exposure. Although cooking is a basic human activity, there are not many data available on the properties of particles generated by this activity. Some cooking methods, such as stir-frying and frying, which are the most favored for Chinese and other Far East people, generate a large quantity of aerosols. This research included the following efforts: 1. investigating particle number concentrations, distributions, and their variations with four different cooking methods and ventilation conditions; 2. measuring the chemical composition of cooking aerosol samples by instrumental neutron activation analysis.

  10. Evaluation of Aerosol-cloud Interaction in the GISS Model E Using ARM Observations

    NASA Technical Reports Server (NTRS)

    DeBoer, G.; Bauer, S. E.; Toto, T.; Menon, Surabi; Vogelmann, A. M.

    2013-01-01

    Observations from the US Department of Energy's Atmospheric Radiation Measurement (ARM) program are used to evaluate the ability of the NASA GISS ModelE global climate model in reproducing observed interactions between aerosols and clouds. Included in the evaluation are comparisons of basic meteorology and aerosol properties, droplet activation, effective radius parameterizations, and surface-based evaluations of aerosol-cloud interactions (ACI). Differences between the simulated and observed ACI are generally large, but these differences may result partially from vertical distribution of aerosol in the model, rather than the representation of physical processes governing the interactions between aerosols and clouds. Compared to the current observations, the ModelE often features elevated droplet concentrations for a given aerosol concentration, indicating that the activation parameterizations used may be too aggressive. Additionally, parameterizations for effective radius commonly used in models were tested using ARM observations, and there was no clear superior parameterization for the cases reviewed here. This lack of consensus is demonstrated to result in potentially large, statistically significant differences to surface radiative budgets, should one parameterization be chosen over another.

  11. The WISE Gamma-Ray Strip Parameterization: The Nature of the Gamma-Ray Active Galactic Nuclei of Uncertain Type

    NASA Astrophysics Data System (ADS)

    Massaro, F.; D'Abrusco, R.; Tosti, G.; Ajello, M.; Gasparrini, D.; Grindlay, J. E.; Smith, Howard A.

    2012-05-01

    Despite the large number of discoveries made recently by Fermi, the origins of the so-called unidentified γ-ray sources remain unknown. The large number of these sources suggests that there could be a population among them that significantly contributes to the isotropic gamma-ray background and it is therefore crucial to understand their nature. The first step toward a complete comprehension of the unidentified γ-ray source population is to identify those that can be associated with blazars, the most numerous class of extragalactic sources in the γ-ray sky. Recently, we discovered that blazars can be recognized and separated from other extragalactic sources using the infrared (IR) WISE satellite colors. The blazar population delineates a remarkable and distinctive region of the IR color-color space, the WISE blazar strip. In particular, the subregion delineated by the γ-ray emitting blazars is even narrower and we named it the WISE Gamma-ray Strip (WGS). In this paper, we parameterize the WGS on the basis of a single parameter s that we then use to determine if γ-ray active galactic nuclei of the uncertain type (AGUs) detected by Fermi are consistent with the WGS and can be considered blazar candidates. We find that 54 AGUs out of a set of 60 analyzed have IR colors consistent with the WGS; only 6 AGUs are outliers. This result implies that a very high percentage (i.e., in this sample about 90%) of the AGUs detected by Fermi are indeed blazar candidates.

  12. Aerosol activation properties and CCN closure during TCAP

    NASA Astrophysics Data System (ADS)

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

    2013-12-01

    The indirect effects of atmospheric aerosols currently remain the most uncertain components in forcing of climate change over the industrial period (IPCC, 2007). This large uncertainty is partially due to our incomplete understanding of the ability of particles to form cloud droplets under atmospherically relevant supersaturation. In addition, there is a large uncertainty in the aerosol optical depth (AOD) simulated by climate models near the North American coast and a wide variety in the types of clouds are observed over this region. The goal of the US Department of Energy Two Column Aerosol Project (TCAP) is to understand the processes responsible for producing and maintaining aerosol distributions and associated radiative and cloud forcing off the coast of North America. During the TCAP study, aerosol total number concentration, cloud condensation nuclei (CCN) spectra and aerosol chemical composition were in-situ measured from the DOE Gulfstream 1 (G-1) research aircraft during two Intensive Operations Periods (IOPs), one conducted in July 2012 and the other in February 2013. An overall aerosol size distribution was achieved by merging the observations from several instruments, including Ultra High Sensitivity Aerosol Spectrometer - Airborne (UHSAS-A, DMT), Passive Cavity Aerosol Spectrometer Probe (PCASP-200, DMT), and Cloud Aerosol Spectrometer (CAS, DMT). Aerosol chemical composition was characterized using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS, Aerodyne Inc.) and single particle mass spectrometer, mini-SPLAT. Based on the aerosol size distribution, CCN number concentration (characterized by a DMT dual column CCN counter with a range from 0.1% to 0.4%), and chemical composition, a CCN closure was obtained. The sensitivity of CCN closure to organic hygroscopicity was investigated. The differences in aerosol/CCN properties between two columns, and between two phases, will be discussed.

  13. Explicit cloud-top entrainment parameterization in the global climate model ECHAM5-HAM

    NASA Astrophysics Data System (ADS)

    Siegenthaler-Le Drian, C.; Spichtinger, P.; Lohmann, U.

    2011-01-01

    New developments in the turbulence parameterization in the general circulation model ECHAM5-HAM are presented. They consist mainly of an explicit entrainment closure at the top of stratocumulus-capped boundary layers and the addition of an explicit contribution of the radiative divergence in the buoyancy production term. The impact of the new implementations on a single column model study and on the global scale is presented here. The parameterization has a "smoothing" effect: the abnormally high values of turbulence kinetic energy are reduced, both in the single column and in the Californian stratocumulus region. A sensitivity study with prescribed droplet concentration shows a reduction in the sensitivity of liquid water path to increasing cloud aerosol optical depth. We also study the effect of the new implementation on a Pacific cross-section. The entrainment parameterization leads to an enhanced triggering of the convective activity.

  14. Ensemble projections of wildfire activity and carbonaceous aerosol concentrations over the western United States in the mid-21st century

    NASA Astrophysics Data System (ADS)

    Yue, X.; Mickley, L. J.; Logan, J. A.

    2010-12-01

    We estimate future wildfire activity over the western United States during the mid-21st century (2046-2065), based on ensemble results from 16 models following the IPCC A1B scenario. Regression models and a parameterization model of area burned (AB) are developed for the projection. The ecoregion-based regression models consider the meteorological impacts from both the current and previous years on the regional AB; the correlation coefficients between the predicted and observed annual AB range from 0.59 to 0.85 during 1981-2000 for six ecoregions. The parameterization model calculates the effects of temperature, precipitation, and relative humidity on daily AB; the predicted monthly total AB over the western US is highly correlated with observations with a normal (logarithmic) correlation coefficient of 0.73 (0.90) for 300 months (1980-2004). The meteorological fields under the A1B scenario from 15 IPCC models and a general circulation model (NASA/GISS GCM 3) are applied to the fire models to estimate AB during 2046-2065. We calculate that the annual AB will increase by 21~124% (regression models) and 40~198% (parameterization) over six ecoregions in the western US at midcentury relative to present day; the length of fire season will extend by 11.1% for the warmer and drier climate. We also examine the impact of the changing climate on the fuel load with a dynamic vegetation model LPJ driven by future meteorology from the GISS GCM 3; it shows that the fuel load over western US experiences small changes because of the short time period from 2000 to 2050. Based on the projected fuel load and the AB calculations, we estimate that the annual total biomass burning over western US will increase by 68% (regression models) or as much as 161% (parameterization). We further investigate the impact of the changing fire emission on the carbonaceous aerosol concentrations over the western United States in the mid-21st century using the chemistry transport model GEOS-Chem driven

  15. [Characteristics and Parameterization for Atmospheric Extinction Coefficient in Beijing].

    PubMed

    Chen, Yi-na; Zhao, Pu-sheng; He, Di; Dong, Fan; Zhao, Xiu-juan; Zhang, Xiao-ling

    2015-10-01

    In order to study the characteristics of atmospheric extinction coefficient in Beijing, systematic measurements had been carried out for atmospheric visibility, PM2.5 concentration, scattering coefficient, black carbon, reactive gases, and meteorological parameters from 2013 to 2014. Based on these data, we compared some published fitting schemes of aerosol light scattering enhancement factor [ f(RH)], and discussed the characteristics and the key influence factors for atmospheric extinction coefficient. Then a set of parameterization models of atmospheric extinction coefficient for different seasons and different polluted levels had been established. The results showed that aerosol scattering accounted for more than 94% of total light extinction. In the summer and autumn, the aerosol hygroscopic growth caused by high relative humidity had increased the aerosol scattering coefficient by 70 to 80 percent. The parameterization models could reflect the influencing mechanism of aerosol and relative humidity upon ambient light extinction, and describe the seasonal variations of aerosol light extinction ability. PMID:26841588

  16. Development and Validation of a Model to Predict Aerosol Breathing Zone Concentrations During Common Outdoor Activities

    EPA Science Inventory

    Research has been conducted on aerosol emission rates during various activities as well as aerosol transport into the breathing zone under idealized conditions. However, there has been little effort to link the two into a model for predicting a person’s breathing zone concentrat...

  17. DEVELOPMENT OF AN RH -DENUDED MIE ACTIVE SAMPLING SYSTEM AND TARGETED AEROSOL CALIBRATION

    EPA Science Inventory

    The MIE pDR 1200 nephelometer provides time resolved aerosol concentrations during personal and fixed-site sampling. Active (pumped) operation allows defining an upper PM2.5 particle size, however, this dramatically increases the aerosol mass passing through the phot...

  18. Cloud condensation nuclei activity of aliphatic amine secondary aerosol

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Aliphatic amines can form secondary aerosol via oxidation with atmospheric radicals (e.g. hydroxyl radical and nitrate radical). The resulting particle composition can contain both secondary organic aerosol (SOA) and inorganic salts. The fraction of organic to inorganic materials in the particulate ...

  19. Cloud — Aerosol interaction during lightning activity over land and ocean: Precipitation pattern assessment

    NASA Astrophysics Data System (ADS)

    Pal, Jayanti; Chaudhuri, Sutapa; Chowdhury, Arumita Roy; Bandyopadhyay, Tanuka

    2016-06-01

    The present study attempts to identify the land - ocean contrast in cloud - aerosol relation during lightning and non-lightning days and its effect on subsequent precipitation pattern. The thermal hypothesis in view of Convective Available Potential Energy (CAPE) behind the land - ocean contrast is observed to be insignificant in the present study region. The result shows that the lightning activities are significantly and positively correlated with aerosols over both land and ocean in case of low aerosol loading whereas for high aerosol loading the correlation is significant but, only over land. The study attempts to comprehend the mechanism through which the aerosol and lightning interact using the concept of aerosol indirect effect that includes the study of cloud effective radius, cloud fraction and precipitation rate. The result shows that the increase in lightning activity over ocean might have been caused due to the first aerosol indirect effect, while over land the aerosol indirect effect might have been suppressed due to lightning. Thus, depending on the region and relation between cloud parameters it is observed that the precipitation rate decreases (increases) over ocean during lightning (non-lightning) days. On the other hand during non-lightning days, the precipitation rate decreases over land.

  20. Global Distribution of Cloud Droplet Number Concentration, Autoconversion Rate, and Aerosol Indirect Effect Under Diabatic Droplet Activation

    NASA Technical Reports Server (NTRS)

    Barahona, Donifan; Sotiropoulou, Rafaella; Nenes, Athanasios

    2011-01-01

    This study presents a global assessment of the sensitivity of droplet number to diabatic activation (i.e., including effects from entrainment of dry air) and its first-order tendency on indirect forcing and autoconversion. Simulations were carried out with the NASA Global Modeling Initiative (GMI) atmospheric and transport model using climatological metereorological fields derived from the former NASA Data Assimilation Office (DAO), the NASA Finite volume GCM (FVGCM) and the Goddard Institute for Space Studies version II (GISS) GCM. Cloud droplet number concentration (CDNC) is calculated using a physically based prognostic parameterization that explicitly includes entrainment effects on droplet formation. Diabatic activation results in lower CDNC, compared to adiabatic treatment of the process. The largest decrease in CDNC (by up to 75 percent) was found in the tropics and in zones of moderate CCN concentration. This leads to a global mean effective radius increase between 0.2-0.5 micrometers (up to 3.5 micrometers over the tropics), a global mean autoconversion rate increase by a factor of 1.1 to 1.7 (up to a factor of 4 in the tropics), and a 0.2-0.4 W m(exp -2) decrease in indirect forcing. The spatial patterns of entrainment effects on droplet activation tend to reduce biases in effective radius (particularly in the tropics) when compared to satellite retrievals. Considering the diabatic nature of ambient clouds, entrainment effects on CDNC need to be considered in GCM studies of the aerosol indirect effect.

  1. Sources and evolution of cloud-active aerosol in California's Sierra Nevada Mountains

    NASA Astrophysics Data System (ADS)

    Roberts, G. C.; Corrigan, C.; Noblitt, S.; Creamean, J.; Collins, D. B.; Cahill, J. F.; Prather, K. A.; Collett, J. L.; Henry, C.

    2011-12-01

    To assess the sources of cloud-active aerosol and their influence on the hydrological cycle in California, the CalWater Experiment took place in winter 2011 in the foothills of the Sierra Nevada Mountains. During this experiment, we coupled the capabilities of demonstrated miniaturized instrumentation - cloud condensation nuclei (CCN), water condensation nuclei (WCN) and microchip capillary electrophoresis (MCE) - to provide direct chemical measurements of cloud active aerosols. Ion concentrations of CCN droplets attribute the anthropogenic, marine and secondary organic contributions to cloud-active aerosols. Detailed spectra from an Aerosol-Time-of-Flight Mass Spectrometer provide additional information on the sources of aerosol. Storm fronts and changes in atmospheric boundary layer brought aerosol and anions associated with Central Valley pollution to the field site with CCN concentrations reaching several thousand cm-3. Hygroscopicity parameters indicate aging of the organic fraction during aerosol transport from the Central Valley to the mountains. Otherwise, CCN concentrations were low when high pressure systems prevented boundary layer development and intrusion of the Central Valley pollution to the site. MCE results show that nitrates and sulfates comprise most of the fraction of the aerosol anion mass (PM1). During the passage of storm fronts, which transported pollution from the Central Valley upslope, nitrate concentrations peaked at several μ g m-3. Low supersaturation CCN concentrations coincide with increases in aerosol nitrate, which suggests that nitrate has a role in cloud formation of giant CCN and, furthermore, in precipitation processes in the Sierra Nevada. CCN spectra show large variations depending on the aerosol sources and sometimes exhibit bi-modal distributions with minima at 0.3% Sc -- similar to the so-called 'Hoppel minima' associated to number size distributions. During these bi-modal events, sulfate also increases supporting the

  2. Apparatus having reduced background for measuring radiation activity in aerosol particles

    DOEpatents

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

    1992-01-01

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

  3. Aerosol measurements at a high-elevation site: composition, size, and cloud condensation nuclei activity

    SciTech Connect

    Friedman, Beth; Zelenyuk, Alla; Beranek, Josef; Kulkarni, Gourihar R.; Pekour, Mikhail S.; Hallar, Anna G.; McCubbin, Ian; Thornton, Joel A.; Cziczo, D. J.

    2013-12-09

    We present measurements of CCN concentrations and associated aerosol composition and size properties at a high-elevation research site in March 2011. CCN closure and aerosol hygroscopicity were assessed using simplified assumptions of bulk aerosol properties as well as a new method utilizing single particle composition and size to assess the importance of particle mixing state in CCN activation. Free troposphere analysis found no significant difference between the CCN activity of free tropospheric aerosol and boundary layer aerosol at this location. Closure results indicate that using only size and number information leads to adequate prediction, in the majority of cases within 50%, of CCN concentrations, while incorporating the hygroscopicity parameters of the individual aerosol components measured by single particle mass spectrometry adds to the agreement, in most cases within 20%, between predicted and measured CCN concentrations. For high-elevation continental sites, with largely aged aerosol and low amounts of local area emissions, a lack of chemical knowledge and hygroscopicity may not hinder models in predicting CCN concentrations. At sites influenced by fresh emissions or more heterogeneous particle types, single particle composition information may be more useful in predicting CCN concentrations and understanding the importance of particle mixing state on CCN activation.

  4. An interfacial mechanism for cloud droplet formation on organic aerosols

    NASA Astrophysics Data System (ADS)

    Ruehl, Christopher R.; Davies, James F.; Wilson, Kevin R.

    2016-03-01

    Accurate predictions of aerosol/cloud interactions require simple, physically accurate parameterizations of the cloud condensation nuclei (CCN) activity of aerosols. Current models assume that organic aerosol species contribute to CCN activity by lowering water activity. We measured droplet diameters at the point of CCN activation for particles composed of dicarboxylic acids or secondary organic aerosol and ammonium sulfate. Droplet activation diameters were 40 to 60% larger than predicted if the organic was assumed to be dissolved within the bulk droplet, suggesting that a new mechanism is needed to explain cloud droplet formation. A compressed film model explains how surface tension depression by interfacial organic molecules can alter the relationship between water vapor supersaturation and droplet size (i.e., the Köhler curve), leading to the larger diameters observed at activation.

  5. An interfacial mechanism for cloud droplet formation on organic aerosols.

    PubMed

    Ruehl, Christopher R; Davies, James F; Wilson, Kevin R

    2016-03-25

    Accurate predictions of aerosol/cloud interactions require simple, physically accurate parameterizations of the cloud condensation nuclei (CCN) activity of aerosols. Current models assume that organic aerosol species contribute to CCN activity by lowering water activity. We measured droplet diameters at the point of CCN activation for particles composed of dicarboxylic acids or secondary organic aerosol and ammonium sulfate. Droplet activation diameters were 40 to 60% larger than predicted if the organic was assumed to be dissolved within the bulk droplet, suggesting that a new mechanism is needed to explain cloud droplet formation. A compressed film model explains how surface tension depression by interfacial organic molecules can alter the relationship between water vapor supersaturation and droplet size (i.e., the Köhler curve), leading to the larger diameters observed at activation. PMID:27013731

  6. Temperature dependence of bromine activation due to reaction with ozone in a proxy for organic aerosols

    NASA Astrophysics Data System (ADS)

    Edebeli, Jacinta; Ammann, Markus; Gilgen, Anina; Eichler, Anja; Schneebeli, Martin; Bartels-Rausch, Thorsten

    2016-04-01

    The discovery of boundary layer ozone depletion events in the Polar Regions [1] and in the mid-latitudes [2], two areas of very different temperature regimes, begs the question of temperature dependence of reactions responsible for these observations [3]. These ODEs have been attributed to ozone reacting with halides leading to reactive halogens (halogen activation) of which bromide is extensively studied, R1 - R3 [4, 5] (R1 is a multiphase reaction). O3 + Br‑→ O2 + OBr‑ (R1) OBr‑ + H+ ↔ HOBr (R2) HOBr + H+ + Br‑→ Br2 + H2O (R3) Despite extensive studies of ozone-bromide interactions, the temperature dependence of bromine activation is not clear [3]. This limits parameterization of the involved reactions and factors in atmospheric models [3, 6]. Viscosity changes in the matrix (such as organic aerosols) due to temperature have been shown to influence heterogeneous reaction rates and products beyond pure temperature effect [7]. With the application of coated wall flow-tubes, the aim of this study is therefore to investigate the temperature dependence of bromine activation by ozone interaction while attempting to characterize the contributions of the bulk and surface reactions to observed ozone uptake. Citric acid is used in this study as a hygroscopically characterized matrix whose viscosity changes with temperature and humidity. Here, we present reactive ozone uptake measured between 258 and 289 K. The data show high reproducibility. Comparison of measured uptake with modelled bulk uptake at different matrix compositions (and viscosities) indicate that bulk reactive uptake dominates, but there are other factors which still need further consideration in the model. References 1. Barrie, L.A., et al., Nature, 1988. 334: p. 138 - 141. 2. Hebestreit, K., et al., Science, 1999. 283: p. 55-57. 3. Simpson, W.R., et al., Atmospheric Chemistry and Physics, 2007. 7: p. 4375 - 4418. 4. Haag, R.W. and J. Hoigné, Environ Sci Technol, 1983. 17: p. 261-267. 5. Oum

  7. Aerosol Composition and Morphology during the 2005 Marine Stratus Radiation Aerosol and Drizzle Study

    SciTech Connect

    Berkowitz, Carl M.; Jobson, B Tom T.; Alexander, M. Lizabeth; Laskin, Alexander; Laulainen, Nels S.

    2005-12-01

    The composition and morphology of aerosols activated within cloud droplets relative to the properties of aerosols not activated is of central importance to studies directed at improved parameterization of the treatment of aerosols in large-scale models. These models have many applications, including evaluations of the impact of anthropogenic aerosols on climate. To further our understanding of these aerosol characteristics, scientists from the U.S. Department of Energy Atmospheric Science Program (ASP), joined forces with other participants of the Atmospheric Radiation Measurement (ARM) "Marine Stratus Radiation Aerosol and Drizzle Study" between July 4 and July 29, 2005, at Pt. Reyes, California. Observations from in situ aerosol instruments and from the ARM Mobile Facility will be combined in a first look at observations from this period. The in situ aerosol measurements included high time resolution data of size-resolved bulk composition (sulfate, nitrate, NH4, organics, etc.) and single particle analysis to determine elemental composition and morphology. A CCN counter was also deployed to measure the fraction of cloud droplet kernels that are CCN active over a range of super-saturations. Our presentation will partition measurements into periods of cloudy and cloud-free periods, and will also be partitioned between periods associated with northerly back trajectories that arrived at Pt. Reyes after passing along the Washington-Oregon coast, westerly oceanic trajectories and a very limited number of periods when the air flow appeared to be associated with urban areas to the south and southeast.

  8. Aerosol identification using a hybrid active/passive system

    NASA Astrophysics Data System (ADS)

    D'Amico, Francis M.; Moon, Raphael P.; Davidson, Charles E.

    2005-08-01

    Recent experimental work has shown that passive systems such as hyperspectral FTIR and frequency-tunable IR cameras have application in detection of biological aerosols. This provided the motivation for a new detection technique, which we call Aerosol Ranging Spectroscopy (ARS), whereby a scattering LIDAR is used to augment passive spectrometer data to determine the location and optical depth of the aerosol plume. When the two systems are co-aligned or boresighted, the hybrid data product provides valuable enhancements for signal exploitation of the passive spectral data. This paper presents the motivation and theoretical basis for the ARS technique. A prototype implementation of an ARS system will also be described, along with preliminary results from recent outdoor field experiments.

  9. Impact of aerosol size representation on modeling aerosol-cloud interactions

    SciTech Connect

    Zhang, Y.; Easter, R. C.; Ghan, S. J.; Abdul-Razzak, H.

    2002-11-07

    In this study, we use a 1-D version of a climate-aerosol-chemistry model with both modal and sectional aerosol size representations to evaluate the impact of aerosol size representation on modeling aerosol-cloud interactions in shallow stratiform clouds observed during the 2nd Aerosol Characterization Experiment. Both the modal (with prognostic aerosol number and mass or prognostic aerosol number, surface area and mass, referred to as the Modal-NM and Modal-NSM) and the sectional approaches (with 12 and 36 sections) predict total number and mass for interstitial and activated particles that are generally within several percent of references from a high resolution 108-section approach. The modal approach with prognostic aerosol mass but diagnostic number (referred to as the Modal-M) cannot accurately predict the total particle number and surface areas, with deviations from the references ranging from 7-161%. The particle size distributions are sensitive to size representations, with normalized absolute differences of up to 12% and 37% for the 36- and 12-section approaches, and 30%, 39%, and 179% for the Modal-NSM, Modal-NM, and Modal-M, respectively. For the Modal-NSM and Modal-NM, differences from the references are primarily due to the inherent assumptions and limitations of the modal approach. In particular, they cannot resolve the abrupt size transition between the interstitial and activated aerosol fractions. For the 12- and 36-section approaches, differences are largely due to limitations of the parameterized activation for non-log-normal size distributions, plus the coarse resolution for the 12-section case. Differences are larger both with higher aerosol (i.e., less complete activation) and higher SO2 concentrations (i.e., greater modification of the initial aerosol distribution).

  10. Impact of aerosol size representation on modeling aerosol-cloud interactions

    DOE PAGESBeta

    Zhang, Y.; Easter, R. C.; Ghan, S. J.; Abdul-Razzak, H.

    2002-11-07

    In this study, we use a 1-D version of a climate-aerosol-chemistry model with both modal and sectional aerosol size representations to evaluate the impact of aerosol size representation on modeling aerosol-cloud interactions in shallow stratiform clouds observed during the 2nd Aerosol Characterization Experiment. Both the modal (with prognostic aerosol number and mass or prognostic aerosol number, surface area and mass, referred to as the Modal-NM and Modal-NSM) and the sectional approaches (with 12 and 36 sections) predict total number and mass for interstitial and activated particles that are generally within several percent of references from a high resolution 108-section approach.more » The modal approach with prognostic aerosol mass but diagnostic number (referred to as the Modal-M) cannot accurately predict the total particle number and surface areas, with deviations from the references ranging from 7-161%. The particle size distributions are sensitive to size representations, with normalized absolute differences of up to 12% and 37% for the 36- and 12-section approaches, and 30%, 39%, and 179% for the Modal-NSM, Modal-NM, and Modal-M, respectively. For the Modal-NSM and Modal-NM, differences from the references are primarily due to the inherent assumptions and limitations of the modal approach. In particular, they cannot resolve the abrupt size transition between the interstitial and activated aerosol fractions. For the 12- and 36-section approaches, differences are largely due to limitations of the parameterized activation for non-log-normal size distributions, plus the coarse resolution for the 12-section case. Differences are larger both with higher aerosol (i.e., less complete activation) and higher SO2 concentrations (i.e., greater modification of the initial aerosol distribution).« less

  11. Reactive uptake coefficients for N2O5 determined from aircraft measurements during the Second Texas Air Quality Study: Comparison to current model parameterizations

    NASA Astrophysics Data System (ADS)

    Brown, Steven S.; Dubé, William P.; Fuchs, Hendrik; Ryerson, Thomas B.; Wollny, Adam G.; Brock, Charles A.; Bahreini, Roya; Middlebrook, Ann M.; Neuman, J. Andrew; Atlas, Elliot; Roberts, James M.; Osthoff, Hans D.; Trainer, Michael; Fehsenfeld, Frederick C.; Ravishankara, A. R.

    2009-04-01

    This paper presents determinations of reactive uptake coefficients for N2O5, γ(N2O5), on aerosols from nighttime aircraft measurements of ozone, nitrogen oxides, and aerosol surface area on the NOAA P-3 during Second Texas Air Quality Study (TexAQS II). Determinations based on both the steady state approximation for NO3 and N2O5 and a plume modeling approach yielded γ(N2O5) substantially smaller than current parameterizations used for atmospheric modeling and generally in the range 0.5-6 × 10-3. Dependence of γ(N2O5) on variables such as relative humidity and aerosol composition was not apparent in the determinations, although there was considerable scatter in the data. Determinations were also inconsistent with current parameterizations of the rate coefficient for homogenous hydrolysis of N2O5 by water vapor, which may be as much as a factor of 10 too large. Nocturnal halogen activation via conversion of N2O5 to ClNO2 on chloride aerosol was not determinable from these data, although limits based on laboratory parameterizations and maximum nonrefractory aerosol chloride content showed that this chemistry could have been comparable to direct production of HNO3 in some cases.

  12. Influence of Surface Seawater and Atmospheric Conditions on the Ccn Activity of Ocean-Derived Aerosol

    NASA Astrophysics Data System (ADS)

    Quinn, P.; Bates, T. S.; Russell, L. M.; Frossard, A. A.; Keene, W. C.; Kieber, D. J.; Hakala, J. P.

    2012-12-01

    Ocean-derived aerosols are produced from direct injection into the atmosphere (primary production) and gas-to-particle conversion in the atmosphere (secondary production). These different production mechanisms result in a broad range of particle sizes that has implications for the impact of ocean-derived aerosol on climate. The chemical composition of ocean-derived aerosols is a result of a complex mixture of inorganic sea salt and organic matter including polysaccharides, proteins, amino acids, microorganisms and their fragments, and secondary oxidation products. Both production mechanisms and biological processes in the surface ocean impact the ability of ocean-derived aerosol to act as cloud condensation nuclei (CCN). In addition, CCN activity can be impacted by atmospheric processing that modifies particle size and composition after the aerosol is emitted from the ocean. To understand relationships between production mechanism, surface ocean biology, and atmospheric processing, measurements were made of surface ocean chlorophyll and dissolved organic matter; nascent sea spray aerosol freshly emitted from the ocean surface; and ambient marine aerosol. These measurements were made along the coast of California and in the North Atlantic between the northeast US and Bermuda. These regions include both eutrophic and oligotraphic waters and, thus, provide for observations over a wide range of ocean conditions.

  13. Analysis of CCN activity of Arctic aerosol and Canadian biomass burning during summer 2008

    NASA Astrophysics Data System (ADS)

    Lathem, T. L.; Beyersdorf, A. J.; Thornhill, K. L.; Winstead, E. L.; Cubison, M. J.; Hecobian, A.; Jimenez, J. L.; Weber, R. J.; Anderson, B. E.; Nenes, A.

    2013-03-01

    The NASA DC-8 aircraft characterized the aerosol properties, chemical composition, and cloud condensation nuclei (CCN) concentrations of the summertime Arctic during the 2008 NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. Air masses characteristic of fresh and aged biomass burning, boreal forest, Arctic background, and anthropogenic industrial pollution were sampled. Observations were spatially extensive (50-85° N and 40-130° W) and exhibit significant variability in aerosol and CCN concentrations. The chemical composition was dominated by highly oxidized organics (66-94% by volume), with a water-soluble mass fraction of more than 50%. The aerosol hygroscopicity parameter, κ, ranged between κ = 0.08-0.32 for all air mass types. Industrial pollution had the lowest κ of 0.08 ± 0.01, while the Arctic background had the highest and most variable κ of 0.32 ± 0.21, resulting from a lower and more variable organic fraction. Both fresh and aged (long-range transported) biomass burning air masses exhibited remarkably similar κ (0.18 ± 0.13), consistent with observed rapid chemical and physical aging of smoke emissions in the atmosphere, even in the vicinity of fresh fires. The organic hygroscopicity (κorg) was parameterized by the volume fraction of water-soluble organic matter (ɛWSOM), with a κ = 0.12, such that κorg = 0.12ɛWSOM. Assuming bulk (size-independent) composition and including the κorg parameterization enabled CCN predictions to within 30% accuracy for nearly all environments sampled. The only exception was for industrial pollution from Canadian oil sands exploration, where an external mixture and size-dependent composition was required. Aerosol mixing state assumptions (internal vs. external) in all other environments did not significantly affect CCN predictions; however, the external mixing assumption provided the best results, even though the available observations could not determine

  14. Reduction of photosynthetically active radiation under extreme stratospheric aerosol loads

    SciTech Connect

    Gerstl, S.A.W.; Zardecki, A.

    1981-08-01

    The recently published hypothesis that the Cretaceous-Tertiary extinctions might be caused by an obstruction of sunlight is tested by model calculations. First we compute the total mass of stratospheric aerosols under normal atmospheric conditions for four different (measured) aerosol size distributions and vertical profiles. For comparison, the stratospheric dust masses after four volcanic eruptions are also evaluated. Detailed solar radiative transfer calculations are then performed for artificially increased aerosol amounts until the postulated darkness scenario is obtained. Thus we find that a total stratospheric aerosol mass between 1 and 4 times 10/sup 1/ g is sufficient to reduce photosynthesis to 10/sup -3/ of normal. We also infer from this result tha the impact of a 0.4- to 3-km-diameter asteroid or a close encounter with a Halley-size comet may deposit that amount of particulates into the stratosphere. The darkness scenario of Alvarez et al. is thus shown to be a possible extinction mechanism, even with smaller size asteroids of comets than previously estimated.

  15. Comparative Antimicrobial Activities of Aerosolized Sodium Hypochlorite, Chlorine Dioxide, and Electrochemically Activated Solutions Evaluated Using a Novel Standardized Assay

    PubMed Central

    Thorn, R. M. S.; Robinson, G. M.

    2013-01-01

    The main aim of this study was to develop a standardized experimental assay to enable differential antimicrobial comparisons of test biocidal aerosols. This study represents the first chlorine-matched comparative assessment of the antimicrobial activities of aerosolized sodium hypochlorite, chlorine dioxide, and electrochemically activated solution (ECAS) to determine their relative abilities to decontaminate various surface-associated health care-relevant microbial challenges. Standard microbiological challenges were developed by surface-associating typed Pseudomonas aeruginosa, Staphylococcus aureus, Bacillus subtilis spores, or a clinical methicillin-resistant S. aureus (MRSA) strain on stainless steel, polypropylene, or fabric. All test coupons were subjected to 20-min biocidal aerosols of chlorine-matched (100 ppm) sodium hypochlorite, chlorine dioxide, or ECAS within a standard aerosolization chamber using a commercial humidifier under defined conditions. Biocidal treatment type and material surface had a significant effect on the number of microorganisms recovered from various material surfaces following treatment exposure. Under the conditions of the assay, the order of antimicrobial efficacy of biocidal aerosol treatment was as follows: ECAS > chlorine dioxide > sodium hypochlorite. For all biocides, greater antimicrobial reductions were seen when treating stainless steel and fabric than when treating plastic-associated microorganisms. The experimental fogging system and assay protocol designed within this study were shown capable of differentiating the comparative efficacies of multiple chlorine-matched biocidal aerosols against a spectrum of target organisms on a range of test surface materials and would be appropriate for testing other biocidal aerosol treatments or material surfaces. PMID:23459480

  16. Advancements in the Representation of Cloud-Aerosol Microphysics in the GEOS-5 AGCM

    NASA Technical Reports Server (NTRS)

    Lee, D.; Oreopoulos, L.; Sud, Y.; Barahona, D.; Nemes, A.; Bhattacharjee, P.

    2011-01-01

    Despite numerous challenges, the physical parameterization of cloud-aerosol interactions in atmospheric GCMs has become a top priority for advancement because of our need to simulate and understand past, current, and future indirect effects of aerosols on clouds. The challenges stem from the involvement of wide range of cloud-scale dynamics and aerosol activation physical processes. Cloud dynamics modulate cloud areal extent and condensate, while aerosol activation depends on aerosol mass load, size distribution, internal mixing state, and nucleating properties, and ultimately determines cloud optical properties via particle sizes. Both macro- and micro-scale processes are obviously important for cloud-radiation interactions. We will present the main features of cloud microphysical properties in the GEOS- 5 Atmospheric GCM (AGCM) as simulated by the McRAS-AC (Microphysics of Clouds with Relaxed Arakawa-Schubert and Aerosol-Cloud interaction) scheme. McRAS-AC uses Fountoukis and Nenes (2005) aerosol activation for liquid clouds, and has an option for either Liu and Penner (2005) or Barahona and Nenes (2008, 2009) aerosol activation for ice clouds. Aerosol loading (on-line or climatological) comes from GOCART, with an assumed log-normal size distribution. Other features of McRAS-AC are level-by-level cloud-scale thermodynamics, and Seifert-Beheng (2001)-type precipitation microphysics, particularly from moist convection. Results from Single-Column Model simulations will be shown to demonstrate how cloud radiative properties, lifetimes, and precipitation are influenced by different parameterization assumptions. Corresponding fields from year-long simulations of the full AGCM will also be presented with geographical distributions of cloud effective particle sizes compared to satellite retrievals. While the primary emphasis will be on current climate, simulation results with perturbed aerosol loadings will also be shown to expose the radiative sensitivity of the

  17. Calibration correction of an active scattering spectrometer probe to account for refractive index of stratospheric aerosols

    NASA Technical Reports Server (NTRS)

    Pueschel, R. F.; Overbeck, V. R.; Snetsinger, K. G.; Russell, P. B.; Ferry, G. V.

    1990-01-01

    The use of the active scattering spectrometer probe (ASAS-X) to measure sulfuric acid aerosols on U-2 and ER-2 research aircraft has yielded results that are at times ambiguous due to the dependence of particles' optical signatures on refractive index as well as physical dimensions. The calibration correction of the ASAS-X optical spectrometer probe for stratospheric aerosol studies is validated through an independent and simultaneous sampling of the particles with impactors; sizing and counting of particles on SEM images yields total particle areas and volumes. Upon correction of calibration in light of these data, spectrometer results averaged over four size distributions are found to agree with similarly averaged impactor results to within a few percent: indicating that the optical properties or chemical composition of the sample aerosol must be known in order to achieve accurate optical aerosol spectrometer size analysis.

  18. Microfluidic Electrochemical Sensor for On-line Monitoring of Aerosol Oxidative Activity

    PubMed Central

    Sameenoi, Yupaporn; Koehler, Kirsten; Shapiro, Jeff; Boonsong, Kanokporn; Sun, Yele; Collett, Jeffrey; Volckens, John; Henry, Charles S.

    2012-01-01

    Particulate matter (PM) air pollution has a significant impact on human morbidity and mortality; however, the mechanisms of PM-induced toxicity are poorly defined. A leading hypothesis states that airborne PM induces harm by generating reactive oxygen species (ROS) in and around human tissues, leading to oxidative stress. We report here, a system employing a microfluidic electrochemical sensor coupled directly to a Particle-into-Liquid-Sampler (PILS) system to measure aerosol oxidative activity in an on-line format. The oxidative activity measurement is based on the dithiothreitol assay (DTT assay) where after oxidized by PM, the remaining reduced DTT was analyzed by the microfluidic sensor. The sensor consists of an array of working, reference, and auxiliary electrodes fabricated in a poly(dimethylsiloxane) (PDMS)-based microfluidic device. Cobalt (II) phthalocyanine (CoPC)-modified carbon paste was used as the working electrode material allowing selective detection of reduced DTT. The electrochemical sensor was validated off-line against the traditional DTT assay using filter samples taken from urban environments and biomass burning events. After off-line characterization, the sensor was coupled to a PILS to enable on-line sampling/analysis of aerosol oxidative activity. Urban dust and industrial incinerator ash samples were aerosolized in an aerosol chamber and analyzed for their oxidative activity. The on-line sensor reported DTT consumption rates (oxidative activity) in good correlation with aerosol concentration (R2 from 0.86–.97) with a time-resolution of approximately 3 minutes. PMID:22651886

  19. Activity size distribution and residence time of 7Be aerosols in the Arctic atmosphere

    NASA Astrophysics Data System (ADS)

    Ioannidou, Alexandra; Paatero, Jussi

    2014-05-01

    The activity size distributions of the natural radionuclide tracer 7Be in different size range fractions (<0.39 μm, 0.39-0.69 μm, 0.69-1.3 μm, 1.3-2.1 μm, 2.1-4.2 μm, 4.2-10.2 μm and >10.2 μm) were determined in the boreal atmosphere in the Arctic Research Centre of the Finnish Meteorological Institute (FMI) at Sodankylä, Finland (67°22‧ N, 26°38‧ E, 180 m asl). The activity median aerodynamic diameter (AMAD) ranged from 0.54 μm to 1.05 μm (average 0.83 μm). A residence time of about 8 days applies to aerosols of 0.83 μm diameter, representing the residence of aerosol particles in arctic environment. The observed positive correlation between AMAD values and RH% can be explained by the fact that condensation during high relative humidity conditions becomes more intense, resulting in increased particle sizes of atmospheric aerosols. However, greater aerosol particle sizes means higher wet scavenging rate of aerosols and as a result lower activity concentration of 7Be in the atmosphere, explaining the anti-correlation between the AMAD values and activity concentrations of 7Be. But this associated with possibly higher scavenging rates of aerosols does not necessarily alone explain the anti-correlation between the AMAD and the 7Be activities. The air mass origin associated with synoptic scale weather phenomena may contribute to that too. The Flextra model was used to assess the transport pattern and to explain the deviation in radionuclide activity concentrations and AMAD values observed in the site of investigation.

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

    NASA Astrophysics Data System (ADS)

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

    2013-05-01

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

  1. Final Report for Cloud-Aerosol Physics in Super-Parameterized Atmospheric Regional Climate Simulations (CAP-SPARCS)(DE-SC0002003) for 8/15/2009 through 8/14/2012

    SciTech Connect

    Russell, Lynn M; Somerville, Richard C.J.

    2012-11-05

    Improving the representation of local and non-local aerosol interactions in state-of-the-science regional climate models is a priority for the coming decade (Zhang, 2008). With this aim in mind, we have combined two new technologies that have a useful synergy: (1) an aerosol-enabled regional climate model (Advanced Weather Research and Forecasting Model with Chemistry WRF-Chem), whose primary weakness is a lack of high quality boundary conditions and (2) an aerosol-enabled multiscale modeling framework (PNNL Multiscale Aerosol Climate Model (MACM)), which is global but captures aerosol-convection-cloud feedbacks, and thus an ideal source of boundary conditions. Combining these two approaches has resulted in an aerosol-enabled modeling framework that not only resolves high resolution details in a particular region, but crucially does so within a global context that is similarly faithful to multi-scale aerosol-climate interactions. We have applied and improved the representation of aerosol interactions by evaluating model performance over multiple domains, with (1) an extensive evaluation of mid-continent precipitation representation by multiscale modeling, (2) two focused comparisons to transport of aerosol plumes to the eastern United States for comparison with observations made as part of the International Consortium for Atmospheric Research on Transport and Transformation (ICARTT), with the first being idealized and the second being linked to an extensive wildfire plume, and (3) the extension of these ideas to the development of a new approach to evaluating aerosol indirect effects with limited-duration model runs by nudging to observations. This research supported the work of one postdoc (Zhan Zhao) for two years and contributed to the training and research of two graduate students. Four peer-reviewed publications have resulted from this work, and ground work for a follow-on project was completed.

  2. A Physically-Based Estimate of Radiative Forcing by Anthropogenic Sulfate Aerosol

    SciTech Connect

    Ghan, Steven J.); Easter, Richard C.); Chapman, Elaine G.); Abdul-Razzak, Hayder; Zhang, Yang ); Leung, Ruby ); Laulainen, Nels S.); Saylor, Rick D.); Zaveri, Rahul A.)

    2001-04-01

    Estimates of direct and indirect radiative forcing by anthropogenic sulfate aerosols from an integrated global aerosol and climate modeling system are presented. A detailed global tropospheric chemistry and aerosol model that predicts concentrations of oxidants as well as aerosols and aerosol precursors, is coupled to a general circulation model that predicts both cloud water mass and cloud droplet number. Both number and mass of several externally-mixed aerosol size modes are predicted, with internal mixing assumed for the different aerosol components within each mode. Predicted aerosol species include sulfate, organic and black carbon, soil dust, and sea salt. The models use physically-based treatments of aerosol radiative properties (including dependence on relative humidity) and aerosol activation as cloud condensation nuclei. Parallel simulations with and without anthropogenic sulfate aerosol are performed for a global domain. The global and annual mean direct and indirect radiative forcing due to anthropogenic sulfate are estimated to be -0.3 to -0.5 and -1.5 to -3.0 W m-2, respectively. The radiative forcing is sensitive to the model's horizontal resolution, the use of predicted vs. analyzed relative humidity, the prediction vs. diagnosis of aerosol number and droplet number, and the parameterization of droplet collision/coalescence. About half of the indirect radiative forcing is due to changes in droplet radius and half to increased cloud liquid water.

  3. Relationship between volatility, hygroscopicity, and CCN activity of winter aerosols: Kanpur, Indo-Gangetic Basin

    NASA Astrophysics Data System (ADS)

    Bhattu, Deepika; Tripathi, Sachchida

    2016-04-01

    Aerosol volatility is one of the key property in deciding their lifetime and fate. The volatile species have the potential to affect SOA estimation, so their characterization and establishment of relationship with mass loading, chemical composition, hygroscopicity and CCN activity is required. A 42 days long winter campaign was conducted in an anthropogenically polluted location (Kanpur, India) where CCN activity of both ambient and thermally treated aerosols was characterized. Enhanced partitioning of semi-volatile molecules into particle phase at higher loading conditions was observed. Unexpectedly, the most oxidized organic factor was observed both least volatile and hygroscopic in nature. Lower

  4. Comparison of the cloud activation potential of open ocean and coastal aerosol in the Pacific Ocean

    NASA Astrophysics Data System (ADS)

    Vidaurre, G.; Brooks, S. D.; Thornton, D. C.

    2010-12-01

    Continuous measurements of aerosol concentration, particle size distribution, and cloud activation potential between 0.15 and 1.2% supersaturation were performed for open ocean and coastal air during the Halocarbon Air Sea Transect - Pacific (HalocAST) campaign. The nearly 7000 mile transect, aboard the R/V Thomas G. Thompson, started in Punta Arenas, Chile and ended in Seattle, Washington. Air mass source regions were identified on the basis of air mass back trajectories. For air masses in the southern hemisphere, aerosols sampled over the open ocean acted as cloud condensation nuclei at supersaturations between 0.5 and 1%, while coastal aerosols required higher supersaturations. In the pristine open ocean, observed aerosol concentrations were very low, typically below 200 cm-3, with an average particle diameter of approximately 0.4 μm. On the other hand, coastal aerosol concentrations were above 1000 cm-3 with an average particle diameter of 0.7 μm. Air masses originating in the northern hemisphere had much higher aerosol loads, between 500 and 2000 cm-3 over the ocean and above 4000 cm-3 at the coast. In both cases, the average particle diameters were approximately 0.5 μm. Measurements suggest that the northern hemisphere, substantially more polluted than the southern hemisphere, is characterized by alternating regions of high and medium aerosol number concentration. In addition, measurements of microorganism and organic matter concentration in the surface layer of the ocean water were conducted along the cruise track, to test the hypothesis that biogenic aerosol containing marine organic matter contribute to cloud activation potential. There was a significant correlation between mean aerosol diameter and prokaryote concentration in surface waters (r = 0.585, p < 0.01, n = 24), and between critical supersaturation and prokaryote concentration in surface waters (r = 0.538, p < 0.01, n = 24). This correlation indicates that larger aerosols occurred over water

  5. Tying Biological Activity to Changes in Sea Spray Aerosol Chemical Composition via Single Particle Analyses

    NASA Astrophysics Data System (ADS)

    Sultana, C. M.; Lee, C.; Collins, D. B.; Axson, J. L.; Laskina, O.; Grandquist, J. R.; Grassian, V. H.; Prather, K. A.

    2014-12-01

    In remote marine environments, sea spray aerosols (SSA) often represent the greatest aerosol burden, thus having significant impacts on direct radiative interactions and cloud processes. Previous studies have shown that SSA is a complex mixture of inorganic salts and an array of dissolved and particulate organic components. Enrichment of SSA organic content is often correlated to seawater chlorophyll concentrations, a measure of oceanic biological activity. As the physical and chemical properties of aerosols control their radiative effects, recent studies conducted by the Center for Aerosol Impacts on Climate and the Environment have endeavored to further elucidate the ties between marine biological activity and primary SSA chemical composition using highly time resolved single particle analyses. A series of experiments performed in the recently developed Marine Aerosol Reference Tank evaluated the effect of changing marine microbial populations on SSA chemical composition, which was monitored via an aerosol time-of-flight mass spectrometer and a variety of offline spectroscopic and microscopic techniques. Each experiment was initiated using unfiltered and untreated seawater, thus maintaining a high level of biogeochemical complexity. This study is the first of its kind to capture daily changes in the primary SSA mixing state over the growth and death of a natural phytoplankton bloom. Increases in organic aerosol types (0.4-3 μm), internally and externally mixed with sea salt, could not be correlated to chlorophyll concentrations. Maximum production of these populations occurred two to four days after the in vivo chlorophyll fluorescence peaked in intensity. This work is in contrast to the current paradigm of correlating SSA organic content to seawater chlorophyll concentration.

  6. Surface-active and Light-absorbing Secondary Organic Aerosol (SOA) Material

    NASA Astrophysics Data System (ADS)

    McNeill, V. F.; Sareen, N.; Schwier, A. N.; Shapiro, E. L.

    2009-12-01

    We have observed the formation of light-absorbing, high-molecular-weight, and surface-active organics from methylgyloxal interacting with ammonium salts in aqueous aerosol mimics. Mixtures of methylglyoxal and glyoxal also form light-absorbing products and exhibit surface tension depression with a Langmuir-like dependence on initial methylglyoxal concentration. We used chemical ionization mass spectrometry with a volatilization flow tube inlet (Aerosol-CIMS) to characterize the product species. The results are consistent with aldol condensation products, carbon-nitrogen species, sulfur-containing compounds, and oligomeric species up to 759 amu. These observations have potentially significant implications for our understanding of the effects of SOA on climate, since a) SOA are typically treated as non-absorbing in climate models, and b) surface tension depression in aqueous aerosols by SOA material may result in increased cloud condensation nucleus (CCN) activity. Furthermore, surface film formation could affect aerosol heterogeneous chemistry. We will also discuss aerosol flow tube O3 oxidation experiments designed to determine the atmospheric lifetimes of the observed product compounds.

  7. The influence of nitrogen oxides on the activation of bromide and chloride in salt aerosol

    NASA Astrophysics Data System (ADS)

    Bleicher, S.; Buxmann, J. C.; Sander, R.; Riedel, T. P.; Thornton, J. A.; Platt, U.; Zetzsch, C.

    2014-04-01

    Experiments on salt aerosol with different salt contents were performed in a Teflon chamber under tropospheric light conditions with various initial contents of nitrogen oxides (NOx = NO + NO2). A strong activation of halogens was found at high NOx mixing ratios, even in samples with lower bromide contents such as road salts. The ozone depletion by reactive halogen species released from the aerosol, was found to be a function of the initial NOx mixing ratio. Besides bromine, large amounts of chlorine have been released in our smog chamber. Time profiles of the halogen species Cl2, Br2, ClNO2, BrNO2 and BrO, ClO, OClO and Cl atoms were simultaneously measured by various techniques (chemical ionization mass spectrometry, differential optical absorption spectrometry coupled with a multi-reflection cell and gas chromatography of hydrocarbon tracers for Cl and OH, employing cryogenic preconcentration and flame ionization detection). Measurements are compared to calculations by the CAABA/MECCA 0-D box model, which was adapted to the chamber conditions and took the aerosol liquid water content and composition into account. The model results agree reasonably with the observations and provide important information about the prerequisites for halogen release, such as the time profiles of the aerosol bromide and chloride contents as well as the aerosol pH.

  8. Reactive Uptake of Dinitrogen Pentoxide on Aqueous Ammonium Nitrate Aerosols: Dependence on the Nitrate Activity

    NASA Astrophysics Data System (ADS)

    Wahner, A.; Folkers, M.; Mentel, T. F.; Sebald, H.; ten Brink, H. M.; Jongejan, P. A.

    2001-12-01

    The heterogeneous conversion of N2O_5 to HNO3 is an important step in the removal of nitrogen oxides from the atmosphere. In the planetary boundary layer this heterogeneous process occurs on the surfaces of aqueous aerosols. The fraction of NH4NO_3 in secondary inorganic aerosols in western Europe and in the United States is increasing, due to decreasing SO2 emissions at nearly constant NOX source strength. This may become of importance, since increasing nitrate concentrations in aerosols can reduce the reaction probability γ N2O5 by up to an order of magnitude ("nitrate effect" [1,2]). We measured γ N2O5 on NH4NO_3, (NH4)_2SO_4 and NH4HSO_4 aerosols in the large aerosol chamber at the FZ-Jülich. The decrease of N2O_5 and the formation of gas-phase HNO3 was monitored by high resolution FTIR spectroscopy. Simultaneously, the aerosol composition was determined on-line by Steam Jet Aerosol Collection/Ion Chromatography. The aerosol surface area was calculated from measured size distributions in the range of 20 nm to 5 μ m. The γ N2O5 of 0.02(+/- 0.003) on (NH4)_2SO_4 and NH4HSO_4 droplets are independent of the relative humidity (RH), like for the corresponding sodium salts at similar conditions. The γ N2O5 on NH4NO_3 aerosol is decreasing from 0.02 at 80% RH to 0.007 at 60% RH with decreasing relative humidity, thus increasing nitrate concentration. The functional dependence of γ N2O5 on the RH or on the ionic strength is different for NH4NO_3 and NaNO3. However it can be unified by supposing direct dependence of γ N2O5 on the mean nitrate activity. [1] A. Wahner, Th. F. Mentel, M. Sohn, J. Stier , J. Geophys. Res., 103 (1999), 31,103 [2] Th. F. Mentel, M. Sohn, A. Wahner , Phys. Chem. Chem. Phys. 1 (1999), 5451

  9. Evolution of the Physicochemical and Activation Properties of Aerosols within Smoke Plumes during the Biomass Burning Observation Project (BBOP)

    NASA Astrophysics Data System (ADS)

    Tomlinson, J. M.; Mei, F.; Wang, J.; Comstock, J. M.; Hubbe, J. M.; Pekour, M. S.; Shilling, J. E.; Fortner, E.; Chand, D.; Sedlacek, A. J., III; Kleinman, L. I.; Senum, G.; Schmid, B.

    2014-12-01

    Biomass burning from wildfires and controlled agricultural burns are known to be a major source of fine particles and organic aerosols at northern temperate latitudes during the summer months. However, the evolution of the physicochemical properties of the aerosol during transport and the potential impact of this evolution on cloud condensation nuclei (CCN) activity has rarely been studied for these events. During the DOE-sponsored Biomass Burning Observation Project (BBOP) conducted in the summer and fall of 2013, over 30 research flights sampled biomass burning plumes from wildfires in the Northwestern United States and agricultural burns in the Mid-South region of the United States. A large suite of instruments aboard the DOE G-1 (Gulfstream-1) measured the chemical, physical, and optical properties of biomass burning aerosol with an emphasis on black carbon. A Fast Integrated Mobility Spectrometer (FIMS), Ultra High Sensitivity Aerosol Spectrometer - Airborne (UHSAS-A), and Passive Cavity Aerosol Spectrometer (PCASP) were used to measure the aerosol size distribution from 15 - 3,000 nm at 1-Hz. A dual column CCN counter measured the CCN number concentration at supersaturations of 0.25% and 0.50% at a time resolution of 1-Hz and the aerosol chemical composition was measured using a soot particle aerosol mass spectrometer (SP-AMS, Aerodyne, Inc). The SP-AMS was operated in two modes: (i) as a traditional high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS, Aerodyne Inc.), which measured chemical composition of non-refractory aerosols and (ii) as the SP-AMS which measured chemical composition of the refractory black carbon-containing (rBC) particle coating and rBC aerosol mass. Utilizing the aforementioned measurements, a CCN closure study is used to investigate the emitted aerosol hygroscopicity, the evolution of the physicochemical properties of the aerosol, and the potential impacts on cloud microphysics from the different fuel sources.

  10. The effect of phase partitioning of semivolatile compounds on the measured CCN activity of aerosol particles

    NASA Astrophysics Data System (ADS)

    Romakkaniemi, S.; Jaatinen, A.; Laaksonen, A.; Nenes, A.; Raatikainen, T.

    2013-09-01

    The effect of inorganic semivolatile aerosol compounds on the CCN activity of aerosol particles was studied by using a computational model for a DMT-CCN counter, a cloud parcel model for condensation kinetics and experiments to quantify the modelled results. Concentrations of water vapour and semivolatiles as well as aerosol trajectories in the CCN column were calculated by a computational fluid dynamics model. These trajectories and vapour concentrations were then used as an input for the cloud parcel model to simulate mass transfer kinetics of water and semivolatiles between aerosol particles and the gas phase. Two different questions were studied: (1) how big fraction of semivolatiles is evaporated from particles before activation in the CCN counter? (2) How much the CCN activity can be increased due to condensation of semivolatiles prior to the maximum water supersaturation in the case of high semivolatile concentration in the gas phase? The results show that, to increase the CCN activity of aerosol particles, a very high gas phase concentration (as compared to typical ambient conditions) is needed. We used nitric acid as a test compound. A concentration of several ppb or higher is needed for measurable effect. In the case of particle evaporation, we used ammonium nitrate as a test compound and found that it partially evaporates before maximum supersaturation is reached in the CCN counter, thus causing an underestimation of CCN activity. The effect of evaporation is clearly visible in all supersaturations, leading to an underestimation of the critical dry diameter by 10 to 15 nanometres in the case of ammonium nitrate particles in different supersaturations. This result was also confirmed by measurements in supersaturations between 0.1 and 0.7%.

  11. Anticandidal activity of pomegranate peel extract aerosol as an applicable sanitizing method.

    PubMed

    Tayel, Ahmed A; El-Tras, Wael F

    2010-03-01

    Pomegranate is a wonderful fruit from the paradise which contains a wide variety of precious phytochemical compounds applicable in the fields of therapeutics and health care. Candida albicans is the most common etiological agent for many clinical mycoses which could lead to human and animal death. Determination of the anticandidal activity of pomegranate peel extracts (PPE), and application of PPE aerosol as sanitizer agent against C. albicans contamination were investigated. Agar diffusion assay and broth microdilution susceptibility test were applied for qualitative and quantitative determining the PPE anticandidal activity, respectively, versus commonly used fungicides. Aerosolization of PPE using an experimentally designed sanitizer room was applied for examining C. albicans sanitation potentiality of extract. PPE exhibited potent anticandidal activity against C. albicans strains comparing with standard fungicides in both used susceptibility techniques. Methanol, ethanol and water extracts were the most effective for inhibiting C. albicans growth. PPE aerosol was an efficient method for complete sanitizing of semi-closed places against C. albicans growth. Application of PPE aerosol is a proper sanitizing method for preventing C. albicans contamination and growth in suspected places. PMID:19207830

  12. Modeling Secondary Organic Aerosols over Europe: Impact of Activity Coefficients and Viscosity

    NASA Astrophysics Data System (ADS)

    Kim, Y.; Sartelet, K.; Couvidat, F.

    2014-12-01

    Semi-volatile organic species (SVOC) can condense on suspended particulate materials (PM) in the atmosphere. The modeling of condensation/evaporation of SVOC often assumes that gas-phase and particle-phase concentrations are at equilibrium. However, recent studies show that secondary organic aerosols (SOA) may not be accurately represented by an equilibrium approach between the gas and particle phases, because organic aerosols in the particle phase may be very viscous. The condensation in the viscous liquid phase is limited by the diffusion from the surface of PM to its core. Using a surrogate approach to represent SVOC, depending on the user's choice, the secondary organic aerosol processor (SOAP) may assume equilibrium or model dynamically the condensation/evaporation between the gas and particle phases to take into account the viscosity of organic aerosols. The model is implemented in the three-dimensional chemistry-transport model of POLYPHEMUS. In SOAP, activity coefficients for organic mixtures can be computed using UNIFAC for short-range interactions between molecules and AIOMFAC to also take into account the effect of inorganic species on activity coefficients. Simulations over Europe are performed and POLYPHEMUS/SOAP is compared to POLYPHEMUS/H2O, which was previously used to model SOA using the equilibrium approach with activity coefficients from UNIFAC. Impacts of the dynamic approach on modeling SOA over Europe are evaluated. The concentrations of SOA using the dynamic approach are compared with those using the equilibrium approach. The increase of computational cost is also evaluated.

  13. FY 2011 Second Quarter: Demonstration of New Aerosol Measurement Verification Testbed for Present-Day Global Aerosol Simulations

    SciTech Connect

    Koch, D

    2011-03-20

    The regional-scale Weather Research and Forecasting (WRF) model is being used by a DOE Earth System Modeling (ESM) project titled “Improving the Characterization of Clouds, Aerosols and the Cryosphere in Climate Models” to evaluate the performance of atmospheric process modules that treat aerosols and aerosol radiative forcing in the Arctic. We are using a regional-scale modeling framework for three reasons: (1) It is easier to produce a useful comparison to observations with a high resolution model; (2) We can compare the behavior of the CAM parameterization suite with some of the more complex and computationally expensive parameterizations used in WRF; (3) we can explore the behavior of this parameterization suite at high resolution. Climate models like the Community Atmosphere Model version 5 (CAM5) being used within the Community Earth System Model (CESM) will not likely be run at mesoscale spatial resolutions (10–20 km) until 5–10 years from now. The performance of the current suite of physics modules in CAM5 at such resolutions is not known, and current computing resources do not permit high-resolution global simulations to be performed routinely. We are taking advantage of two tools recently developed under PNNL Laboratory Directed Research and Development (LDRD) projects for this activity. The first is the Aerosol Modeling Testbed (Fast et al., 2011b), a new computational framework designed to streamline the process of testing and evaluating aerosol process modules over a range of spatial and temporal scales. The second is the CAM5 suite of physics parameterizations that have been ported into WRF so that their performance and scale dependency can be quantified at mesoscale spatial resolutions (Gustafson et al., 2010; with more publications in preparation).

  14. Modeling Aerosol Effects on Shallow Cumuli and Turbulent Activities Under Various Meteorological Conditions

    NASA Astrophysics Data System (ADS)

    Wang, H.; McFarquhar, G. M.

    2007-12-01

    To determine conditions over the Indian Ocean for which cloud fields are most susceptible to modification from aerosols and to study how turbulent activities and shallow cumuli vary for different meteorological scenarios, the National Center for Atmospheric Research Eulerian-semi-Lagrangian (EULAG) three-dimensional large-eddy simulation model was initialized using data collected during the Indian Ocean Experiment (INDOEX). Radiosonde data were used to construct 6 soundings encompassing the range of temperature and humidity observed in the trade-wind boundary layer. By then adding the characteristics (height, depth and strength) of either a typical transition layer (TL), a strong inversion layer (IL) or no stable layer a total of 18 meteorological scenarios were produced. Separate simulations were conducted using EULAG assuming pristine and polluted conditions (i.e., cloud droplet number concentrations, aerosol extinction profiles and single-scattering albedos) using INDOEX observations. For the range of meteorological conditions observed during INDOEX, sensitivity studies showed that the semi- direct effect always dominated indirect effects, producing a positive daytime mean net indirect forcing varying between 0.2 and 4.5 W m-2. The simulations showed that changes in the environmental relative humidity (RH) and the presence of the TL had critical impacts on the cloud properties, turbulence and lateral detrainment rates, and on how aerosols affect these quantities. The net indirect forcing was larger when the RH was higher and in the absence of any dry and stable layers. It was reduced to less than 1.2 W m-2 when the TL was present. The impact of the IL was dependent on convective strength which increases with increasing RH. In fact, changes in meteorological factors had larger impacts on the simulated cloud properties than did the presence of anthropogenic aerosols, indicating large uncertainties can be introduced when solely using observations of aerosols and

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  16. Survival and ice nucleation activity of bacteria as aerosols in a cloud simulation chamber

    NASA Astrophysics Data System (ADS)

    Amato, P.; Joly, M.; Schaupp, C.; Attard, E.; Möhler, O.; Morris, C. E.; Brunet, Y.; Delort, A.-M.

    2015-06-01

    The residence time of bacterial cells in the atmosphere is predictable by numerical models. However, estimations of their aerial dispersion as living entities are limited by a lack of information concerning survival rates and behavior in relation to atmospheric water. Here we investigate the viability and ice nucleation (IN) activity of typical atmospheric ice nucleation active bacteria (Pseudomonas syringae and P. fluorescens) when airborne in a cloud simulation chamber (AIDA, Karlsruhe, Germany). Cell suspensions were sprayed into the chamber and aerosol samples were collected by impingement at designated times over a total duration of up to 18 h, and at some occasions after dissipation of a cloud formed by depressurization. Aerosol concentration was monitored simultaneously by online instruments. The cultivability of airborne cells decreased exponentially over time with a half-life time of 250 ± 30 min (about 3.5 to 4.5 h). In contrast, IN activity remained unchanged for several hours after aerosolization, demonstrating that IN activity was maintained after cell death. Interestingly, the relative abundance of IN active cells still airborne in the chamber was strongly decreased after cloud formation and dissipation. This illustrates the preferential precipitation of IN active cells by wet processes. Our results indicate that from 106 cells aerosolized from a surface, one would survive the average duration of its atmospheric journey estimated at 3.4 days. Statistically, this corresponds to the emission of 1 cell that achieves dissemination every ~ 33 min m-2 of cultivated crops fields, a strong source of airborne bacteria. Based on the observed survival rates, depending on wind speed, the trajectory endpoint could be situated several hundreds to thousands of kilometers from the emission source. These results should improve the representation of the aerial dissemination of bacteria in numeric models.

  17. Survival and ice nucleation activity of bacteria as aerosols in a cloud simulation chamber

    NASA Astrophysics Data System (ADS)

    Amato, P.; Joly, M.; Schaupp, C.; Attard, E.; Möhler, O.; Morris, C. E.; Brunet, Y..; Delort, A.-M.

    2015-02-01

    The residence time of bacterial cells in the atmosphere is predictable by numerical models. However, estimations of their aerial dispersion as living entities are limited by lacks of information concerning survival rates and behavior in relation to atmospheric water. Here we investigate the viability and ice nucleation (IN) activity of typical atmospheric ice nucleation active bacteria (Pseudomonas syringae and P. fluorescens) when airborne in a cloud simulation chamber (AIDA, Karlsruhe, Germany). Cell suspensions were sprayed into the chamber and aerosol samples were collected by impingement at designated times over a total duration of up to 18 h, and at some occasions after dissipation of a cloud formed by depressurization. Aerosol concentration was monitored simultaneously by online instruments. The cultivability of airborne cells decreased exponentially over time with a half-life time of 250 ± 30 min (about 3.5 to 4.5 h). In contrast, IN activity remained unchanged for several hours after aerosolization, demonstrating that IN activity was maintained after cell death. Interestingly, the relative abundance of IN active cells still airborne in the chamber was strongly decreased after cloud formation and dissipation. This illustrates the preferential precipitation of IN active cells by wet processes. Our results indicate that from 106 = cells aerosolized from a surface, one would survive the average duration of its atmospheric journey estimated at 3.4 days. Statistically, this corresponds to the emission of 1 cell that achieves dissemination every ~33 min per m2 of cultivated crops fields, a strong source of airborne bacteria. Based on the observed survival rates, depending on wind speed, the trajectory endpoint could be situated several hundreds to thousands of kilometers from the emission source. These results should improve the representation of the aerial dissemination of bacteria in numeric models.

  18. Anti-tumor activity of CpG-ODN aerosol in mouse lung metastases.

    PubMed

    Sfondrini, Lucia; Sommariva, Michele; Tortoreto, Monica; Meini, Alessandra; Piconese, Silvia; Calvaruso, Marco; Van Rooijen, Nick; Bonecchi, Raffaella; Zaffaroni, Nadia; Colombo, Mario P; Tagliabue, Elda; Balsari, Andrea

    2013-07-15

    Studies in preclinical models have demonstrated the superior anti-tumor effect of CpG oligodeoxynucleotides (CpG-ODN) when administered at the tumor site rather than systemically. We evaluated the effect of aerosolized CpG-ODN on lung metastases in mice injected with immunogenic N202.1A mammary carcinoma cells or weakly immunogenic B16 melanoma cells. Upon reaching the bronchoalveolar space, aerosolized CpG-ODN activated a local immune response, as indicated by production of IL-12p40, IFN-γ and IL-1β and by recruitment and maturation of DC cells in bronchoalveolar lavage fluid of mice. Treatment with aerosolized CpG-ODN induced an expansion of CD4+ cells in lung and was more efficacious than systemic i.p. administration against experimental lung metastases of immunogenic N202.1A mammary carcinoma cells, whereas only i.p. delivery of CpG-ODN provided anti-tumor activity, which correlated with NK cell expansion in the lung, against lung metastases of the poorly immunogenic B16 melanoma. The inefficacy of aerosol therapy to induce NK expansion was related to the presence of immunosuppressive macrophages in B16 tumor-bearing lungs, as mice depleted of these cells by clodronate treatment responded to aerosol CpG-ODN through expansion of the NK cell population and significantly reduced numbers of lung metastases. Our results indicate that tumor immunogenicity and the tumor-induced immunosuppressive environment are critical factors to the success of CpG therapy in the lung, and point to the value of routine sampling of the lung immune environment in defining an optimal immunotherapeutic strategy. PMID:23319306

  19. Active and passive smoking - New insights on the molecular composition of different cigarette smoke aerosols by LDI-FTICRMS

    NASA Astrophysics Data System (ADS)

    Schramm, Sébastien; Carré, Vincent; Scheffler, Jean-Luc; Aubriet, Frédéric

    2014-08-01

    The aerosol generated when a cigarette is smoked is a significant indoor contaminant. Both smokers and non-smokers can be exposed to this class of pollutants. Nevertheless, they are not exposed to the same kind of smoke. The active smoker breathes in the mainstream smoke (MSS) during a puff, whereas the passive smoker inhales not only the smoke generated by the lit cigarette between two puffs (SSS) but also the smoke exhaled by active smokers (EXS). The aerosol fraction of EXS has until now been poorly documented; its composition is expected to be different from MSS. This study aims to investigate the complex composition of aerosol from EXS to better understand the difference in exposure between active and passive smokers. To address this, the in-situ laser desorption ionisation Fourier transform ion cyclotron mass spectrometry (LDI-FTICRMS) was used to characterise the aerosol composition of EXS from two different smokers. Results clearly indicated many similarities between EXS samples but also significant differences with MSS and SSS aerosol. The comparison of MSS and EXS aerosol allowed the chemicals retained by the active smoker's lungs to be identified, whereas the convolution of the EXS and SSS aerosol compositions were considered relevant to the exposition of a passive smoker. As a consequence, active smokers are thought to be mainly exposed to polar and poorly unsaturated oxygenated and nitrogenated organics, compared with poorly oxygenated but highly unsaturated compounds in passive smokers.

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

    NASA Astrophysics Data System (ADS)

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

    2012-06-01

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

  1. Aerosol mixingstate, hygroscopic growth and cloud activation efficiency during MIRAGE 2006

    SciTech Connect

    Lance, Sara; Raatikainen, T.; Onasch, Timothy B.; Worsnop, Douglas R.; Yu, Xiao-Ying; Alexander, M. L.; Stolzenberg, Mark; McMurry, Peter; Smith, James N.; Nenes, Athanasios

    2013-05-15

    Observations of aerosol hygroscopic growth and CCN activation spectra for submicron particles are reported for the T1 ground site outside of Mexico City during the MIRAGE 2006 campaign. K¨ohler theory is used to evaluate the characteristic water uptake coefficient, k*, for the CCN active aerosol population using both size-resolved HTMDA and size-resolved CCNc measurements. Organic mass fractions, (forg), are evaluated from size-resolved aerosol mass spectrometer (AMS) measurements, from which kAMS is inferred and compared against k*. Strong diurnal profiles of aerosol water uptake parameters and aerosol composition are observed. We find that new particle formation (NPF) events are correlated with an increased k* and CCN-active fraction during the daytime, with greater impact on smaller particles. During NPF events, the number concentration of 40 nm particles acting as CCN can surpass by more than a factor of two the concentrations of 100 nm particles acting as CCN, at supersaturations of 0.51% +/- 0.06%. We also find that at 0600-0800 in the morning throughout the campaign, fresh traffic emissions result in substantial changes to the chemical distribution of the aerosol, with on average 65% externally-mixed fraction for 40 nm particles and 30% externally-mixed fraction for 100 nm particles, whereas at midday nearly all particles of both sizes can be described as “internally-mixed”. Average activation spectra and growth factor distributions are analyzed for different time periods characterizing the daytime (with and without NPF events), the early morning “rush hour”, and the entire campaign. We show that k* derived from CCNc measurements decreases as a function of size during all time periods, while the CCN-active fraction increases as a function of size. Size-resolved AMS measurements do not predict the observed trend for k* versus particle size, which can be attributed to unresolved mixing-state and the presence of refractory material not measured by the

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

    NASA Astrophysics Data System (ADS)

    Paukert, M.; Hoose, C.

    2014-07-01

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

  3. Improving aerosol distributions below clouds by assimilating satellite-retrieved cloud droplet number

    PubMed Central

    Saide, Pablo E.; Carmichael, Gregory R.; Spak, Scott N.; Minnis, Patrick; Ayers, J. Kirk

    2012-01-01

    Limitations in current capabilities to constrain aerosols adversely impact atmospheric simulations. Typically, aerosol burdens within models are constrained employing satellite aerosol optical properties, which are not available under cloudy conditions. Here we set the first steps to overcome the long-standing limitation that aerosols cannot be constrained using satellite remote sensing under cloudy conditions. We introduce a unique data assimilation method that uses cloud droplet number (Nd) retrievals to improve predicted below-cloud aerosol mass and number concentrations. The assimilation, which uses an adjoint aerosol activation parameterization, improves agreement with independent Nd observations and with in situ aerosol measurements below shallow cumulus clouds. The impacts of a single assimilation on aerosol and cloud forecasts extend beyond 24 h. Unlike previous methods, this technique can directly improve predictions of near-surface fine mode aerosols responsible for human health impacts and low-cloud radiative forcing. Better constrained aerosol distributions will help improve health effects studies, atmospheric emissions estimates, and air-quality, weather, and climate predictions. PMID:22778436

  4. Sensitivity of Arctic mixed-phase clouds simulated with the global climate model ECHAM6-HAM2 to the heterogeneous freezing parameterization

    NASA Astrophysics Data System (ADS)

    Ickes, Luisa; Welti, André; Hoose, Corinna; Lohmann, Ulrike

    2015-04-01

    Different methods can be used to parameterize heterogeneous freezing in mixed-phase clouds either based on field mesurements, laboratory experiments or using theoretical approaches. In this study a parameterization for immersion freezing based on Classical Nucleation Theory (CNT) and laboratory data from Welti et al. [1] is developed for the GCM ECHAM6-HAM2. The scheme is able to incorporate laboratory data to describe microphysical properties of ice nuclei [2]. As CNT is very sensitive to the description of unconstrained kinetic and thermodynamic parameters in case of homogeneous freezing [3] the sensitivity of immersion freezing to these parameters is investigated. Additionally, several approaches to represent ice nuclei properties are tested in terms of their capability to reproduce temperature, time and size dependence of the experimentally observed freezing process. The developed CNT parameterization scheme for kaolinite, illite, montmorillonite, microcline (K-feldspar) and ATD (Arizona test dust) is then introduced into the global climate model ECHAM6-HAM2 with a two-moment cloud microphysics scheme [4] coupled to the aerosol module HAM [5]. The sensitivity of the parameterization is tested in the framework of an Arctic case study. The parameterization will be evaluated against an empirical freezing parameterization to study if the choice of a parameterization scheme can influence the representation of Arctic mixed-phase clouds in ECHAM6-HAM2. [1] A. Welti et al. Time dependence of immersion freezing. Atmos. Chem. Phys.,12:9893-9907, 2012. [2] J.-P. Chen, A. Hazra, and Z. Levin. Parameterizing ice nucleation rates using contact angle and activation energy derived from laboratory data. Atmos. Chem. Phys., 8(24):7431-7449, 2008. [3] L. Ickes, A. Welti, C. Hosse and U. Lohmann. Classical nucleation theory of homogeneous freezing of water: thermodynamic and kinetic parameters. Phys. Chem. Chem. Phys., 2015. [4] U. Lohmann and C. Hoose. Sensitivity studies of

  5. Parameterization of heterogeneous ice nucleation on mineral dust particles: An application in a regional scale model

    NASA Astrophysics Data System (ADS)

    Niemand, M.; Vogel, B.; Vogel, H.; Connolly, P.; Klein, H.; Bingemer, H.; Hoose, C.; Moehler, O.; Leisner, T.

    2010-12-01

    In climate and weather models, the quantitative description of aerosol and cloud processes relies on simplified assumptions. This contributes major uncertainties to the prediction of global and regional climate change. The parameterization of heterogeneous ice nucleation is a step towards improving our current knowledge of the importance of the cloud ice phase in weather and climate models and can aid in the theoretical understanding of such processes. This contribution presents a new parameterization derived from a large number of experiments carried out at the aerosol and cloud chamber facility AIDA [1] of Karlsruhe Institute of Technology. AIDA is especially suitable to study ice nucleation processes at tropospheric and stratospheric cloud conditions covering a wide range of temperature and pressure. During pumping expansion, cooling rates between -0.3 and -5.0 K/min, equating to vertical wind velocities of 0.5 to 8 m/s, and a relative humidity range of up to more than 200% with respect to ice can be reached. The parameterization is valid for the temperature range -35°C to -15°C. In order to derive and test the parameterization a parameter called the ice-active surface site density was calculated for a number of different experiments with mineral dust acting as ice nuclei in the immersion and/or deposition mode. An exponential function was fitted to this data of ice-active surface site density vs. temperature. The curve fit was then used within the bin microphysical model ACPIM [2] to simulate the ice formation rates from the experiments. The major dust outbreak over the Sahara in May 2008 which was followed by a dust transport over the Mediterranean and Western Europe was simulated using the regional scale online coupled model system COSMO-ART (Vogel et al., 2009). Based on the model results the exponential curve fit was used to calculate the ice nuclei number concentration at Kleiner Feldberg (Germany). The results will be compared to measurements from

  6. Temporal variations of 7Be and 210Pb activity in aerosols at Xiamen, China

    NASA Astrophysics Data System (ADS)

    Huang, Dekun

    2016-04-01

    The radionuclides serve as powerful tracers to identify and quantify several atmospheric processes, such as source, transport and mixing of air masses, air masses exchanging between various atmospheric layers, residence times of atmospheric gasses and pollutants. 7Be and 210Pb activities in aerosols were measurement from October, 2013 to September, 2015 at Xiamen (24°26'7.44″N, 118°5'31.30″N) in South China. The activity of 7Be and 210Pb in aerosols from 2013 to 2015 in Xiamen ranged from 0.26 to 9.05 (mean:4.15) mBq m-3 and from 0.14 to 2.64 (mean:1.05) mBq m-3, respectively. The mean activity of 7Be was comparable with the activities of other places in the same latitude, while the mean activity of 210Pb was lower than the activity of the locations at high altitudes. The possible reason is that Xiamen is a coastal city located on southwest Pacific. The activities of 7Be and 210Pb had a commonly low value in summer (July-September) and a high value in autumn (October-December), it may be controlled by the rainfall. There is significant relationship between the monthly 210Pb activities and the concentration of PM 2.5 and PM 10. In contrast, monthly 7Be activities only show significant correlation with the concentration of PM 10, which implies that 7Be and 210Pb can be used to trace the different sources of the aerosols. And the dry 7Be depositional fluxes increased with latitude along the coast of China (R2=0.92, n=8).

  7. Atmospheric Aerosols: Cloud Condensation Nucleus Activity of Selected Organic Molecules

    NASA Astrophysics Data System (ADS)

    Rosenorn, T.; Henning, S.; Hartz, K. H.; Kiss, G.; Pandis, S.; Bilde, M.

    2005-12-01

    Gas/particle partitioning of vapors in the atmosphere plays a major role in both climate through micro meteorology and in the physical and chemical processes of a single particle. This work has focused on the cloud droplet activation of a number of pure and mixed compounds. The means used to investigate these processes have been the University of Copenhagen cloud condensation nucleus counter setup and the Carnegie Mellon University CCNC setup. The importance of correct water activity modeling has been addressed and it has been pointed out that the molecular mass is an important parameter to consider when choosing model compounds for cloud activation models. It was shown that both traditional Kohler theory and Kohler theory modified to account for limited solubility reproduce measurements of soluble compounds well. For less soluble compounds it is necessary to use Kohler theory modified to account for limited solubility. It was also shown that this works for mixtures of compounds containing both inorganic salts and dicarboxylic acids. It has also been shown that particle phase and humidity history is important for activation behavior of particles consisting of two slightly soluble organic substances (succinic and adipic acid) and a soluble salt (NaCl). Model parameters for terpene oxidation product cloud activation have been derived. These are based on two sets of average parameters covering monoterpene oxidation products and sesquiterpene oxidation products. All parameters except the solubility were estimated and an effective solubility was calculated as the fitting parameter. The average solubility of the model compound found for mono terpene oxidation products is similar to those of sodium chloride and ammonium sulfate; however the higher molecular weight leads to a slightly higher activation diameter at fixed supersaturation. On a molar basis the monoterpene oxidation products show a 1.5 times higher effective solubility than the sesquiterpene oxidation products.

  8. Hygroscopicity Behavior, Activation Properties and Chemical Composition of Atmospheric Aerosol at a Background Site in the Megacity Region of Peking

    NASA Astrophysics Data System (ADS)

    Henning, Silvia; Nowak, Andreas; Mildenberger, Katrin; Göbel, Tina; Nekat, Bettina; van Pinxteren, Dominik; Herrmann, Hartmut; Zhao, Chunsheng; Wiedensohler, Alfred; Stratmann, Frank

    2010-05-01

    Large areas of China suffer from heavy air pollution (both gaseous and particulate) caused by strong economic growth in the last two decades. However, knowledge concerning the physical and chemical properties of the resulting aerosol particles populations, and their effects on the optical properties of the atmosphere, is still sparse. In the framework of the investigations presented here, comprehensive measurements concerning aerosol particle hygroscopicity, CCN ability, composition, and optical properties were performed. The investigations are part of the DFG-funded project HaChi (Haze in China) and are conducted in collaboration with the Peking University. A conclusive parameterization of aerosol hygroscopicity and activation data is aimed for, which will then be implemented in a meso-scale model to investigate aerosol-cloud-radiation and precipitation interactions. During two intensive measurements campaigns (March 2009 and July/ August 2009), in-situ aerosol measurements have been performed in an air-conditioned mobile laboratory next to the Wuqing Meteorological Station (39°23'8.53"N, 117°1'25.88"E), which is located between Bejing and Tijanjin and is thereby an ideal background site in a megacity region. The particle number size distribution (TDMPS), the particle optical properties (MAAP and nephelometer) and their hygroscopic properties at high RH (HH-TDMA, LACIS-mobile) were characterized as well as their cloud nucleating properties above supersaturation (DMT-CCNC). 24 h PM1 particle samples were continuously collected over the two campaigns in winter and summer using a DIGITEL high volume sampler (DHA-80). Additionally two 6h size-resolved samples (daytime and night-time) were collected each day applying an 11-stage Berner impactor. The size-selection of HH-TDMA, LACIS and the CCNC was synchronized with the Berner stages. Opening analysis of the winter campaign data showed that the HH-TDMA usually detected a hydrophobic and a hygroscopic mode, i.e., the

  9. The influence of marine microbial activities on aerosol production: A laboratory mesocosm study

    NASA Astrophysics Data System (ADS)

    Alpert, Peter A.; Kilthau, Wendy P.; Bothe, Dylan W.; Radway, JoAnn C.; Aller, Josephine Y.; Knopf, Daniel A.

    2015-09-01

    The oceans cover most of the Earth's surface, contain nearly half the total global primary biomass productivity, and are a major source of atmospheric aerosol particles. Here we experimentally investigate links between biological activity in seawater and sea spray aerosol (SSA) flux, a relationship of potential significance for organic aerosol loading and cloud formation over the oceans and thus for climate globally. Bubbles were generated in laboratory mesocosm experiments either by recirculating impinging water jets or glass frits. Experiments were conducted with Atlantic Ocean seawater collected off the eastern end of Long Island, NY, and with artificial seawater containing cultures of bacteria and phytoplankton Thalassiosira pseudonana, Emiliania huxleyi, and Nannochloris atomus. Changes in SSA size distributions occurred during all phases of bacterial and phytoplankton growth, as characterized by cell concentrations, dissolved organic carbon, total particulate carbon, and transparent exopolymer particles (gel-forming polysaccharides representing a major component of biogenic exudate material). Over a 2 week growth period, SSA particle concentrations increased by a factor of less than 2 when only bacteria were present and by a factor of about 3 when bacteria and phytoplankton were present. Production of jet-generated SSA particles of diameter less than 200 nm increased with time, while production of all particle diameters increased with time when frits were used. The implications of a marine biological activity dependent SSA flux are discussed.

  10. Differences between the activity size distributions of the different natural radionuclide aerosols in outdoor air

    NASA Astrophysics Data System (ADS)

    Gründel, M.; Porstendörfer, J.

    The results of the activity size distribution of the short-lived ( 218Po, 214Bi/ 214Po) and long-lived ( 210Pb, 210Po) radon decay product aerosols, the thoron decay product aerosols ( 212Pb, 212Po) and 7Be of the outdoor atmosphere are presented. The results were obtained from measurements averaged over an extended period (4 weeks) and were carried out with a low-pressure On-Line Alpha Cascade Impactor (OLACI). The size distributions of the radionuclides were obtained from the same measurement run with the OLACI, so that the size classification technique and the atmospheric and weather conditions for all radionuclides were identical. This measurement technique made it possible to measure the correct differences between the size distributions of the different natural radionuclides in the environmental air. The differences between the activity size distributions of the long- and short-lived radionuclides could be explained by coagulation with aerosol particles of the atmosphere as for instance 210Pb was shown.

  11. The dynamic surface tension of atmospheric aerosol surfactants reveals new aspects of cloud activation

    PubMed Central

    Nozière, Barbara; Baduel, Christine; Jaffrezo, Jean-Luc

    2014-01-01

    The activation of aerosol particles into cloud droplets in the Earth’s atmosphere is both a key process for the climate budget and a main source of uncertainty. Its investigation is facing major experimental challenges, as no technique can measure the main driving parameters, the Raoult’s term and surface tension, σ, for sub-micron atmospheric particles. In addition, the surfactant fraction of atmospheric aerosols could not be isolated until recently. Here we present the first dynamic investigation of the total surfactant fraction of atmospheric aerosols, evidencing adsorption barriers that limit their gradient (partitioning) in particles and should enhance their cloud-forming efficiency compared with current models. The results also show that the equilibration time of surfactants in sub-micron atmospheric particles should be beyond the detection of most on-line instruments. Such instrumental and theoretical shortcomings would be consistent with atmospheric and laboratory observations and could have limited the understanding of cloud activation until now. PMID:24566451

  12. The Two-Column Aerosol Project (TCAP) Science Plan

    SciTech Connect

    Berkowitz, CM; Berg, LK; Cziczo, DJ; Flynn, CJ; Kassianov, EI; Fast, JD; Rasch, PJ; Shilling, JE; Zaveri, RA; Zelenyuk, A; Ferrare, RA; Hostetler, CA; Cairns, B; Russell, PB; Ervens, B

    2011-07-27

    The Two-Column Aerosol Project (TCAP) field campaign will provide a detailed set of observations with which to (1) perform radiative and cloud condensation nuclei (CCN) closure studies, (2) evaluate a new retrieval algorithm for aerosol optical depth (AOD) in the presence of clouds using passive remote sensing, (3) extend a previously developed technique to investigate aerosol indirect effects, and (4) evaluate the performance of a detailed regional-scale model and a more parameterized global-scale model in simulating particle activation and AOD associated with the aging of anthropogenic aerosols. To meet these science objectives, the Atmospheric Radiation Measurement (ARM) Climate Research Facility will deploy the ARM Mobile Facility (AMF) and the Mobile Aerosol Observing System (MAOS) on Cape Cod, Massachusetts, for a 12-month period starting in the summer of 2012 in order to quantify aerosol properties, radiation, and cloud characteristics at a location subject to both clear and cloudy conditions, and clean and polluted conditions. These observations will be supplemented by two aircraft intensive observation periods (IOPs), one in the summer and a second in the winter. Each IOP will deploy one, and possibly two, aircraft depending on available resources. The first aircraft will be equipped with a suite of in situ instrumentation to provide measurements of aerosol optical properties, particle composition and direct-beam irradiance. The second aircraft will fly directly over the first and use a multi-wavelength high spectral resolution lidar (HSRL) and scanning polarimeter to provide continuous optical and cloud properties in the column below.

  13. Sun-Sky Radiometer Synthesis of Interplay Between Aerosols and Monsoon Activity Over Pune, India

    NASA Astrophysics Data System (ADS)

    Devara, P. C. S.; Kumar, Sumit; Vijayakumar, K.; Pandithurai, G.

    2014-09-01

    Besides several thematic campaigns, utilizing a variety of platforms including satellites, ground-based networks have been established to improve our understanding of the role of aerosols in the changing monsoon climate. Two such widely known networks over the globe are `SKYNET' and `AERONET' with sun-sky radiometers as the principal equipment that characterizes aerosols and gases over different geographical locations under varied air mass conditions. Pune (18°43'N, 73°51'E, 559 m above mean sea level), a fast growing low-latitude, urban city in India, is one of the sites where Prede (POM-01L, SKYNET) and Cimel (CE-318, AERONET) Sun-sky radiometers have been in operation since 2004. These radiometers have been extensively used in several studies related to stand-alone and coupled aerosol-cloud-climate processes. The Prede instrument at this site is being augmented for the network of the Global Atmospheric Watch program of the World Meteorological Organization to facilitate data coordination through the World Data Center for Aerosols. The present study envisages understanding the response of atmospheric constituents, through simultaneous operation of the radiometers amongst others, for the rainfall activity over Pune during two contrasting monsoon years of 2008 (active, 98 % of long period average (LPA) rainfall over the whole country) and 2009 (weak, 78 % of LPA). The synthesis of data indicates that, apart from excellent agreement between the direct Sun observations, both radiometers capture well the monsoon features within the instrument density and efficacy of data retrieval algorithms involved. The meteorological fields from the ECMWF re-analysis and NOAA-HYSPLIT air-mass back-trajectory analysis during the study period have been utilized to explain the variations observed in the radiometer products.

  14. Droplet activation properties of organic aerosols observed at an urban site during CalNex-LA

    SciTech Connect

    Mei, Fan; Hayes, Patrick L.; Ortega, Amber; Taylor, Jonathan W.; Allan, James D.; Gilman, Jessica; Kuster, William; de Gouw, Joost; Jimenez, Jose L.; Wang, Jian

    2013-04-11

    Size-resolved cloud condensation nuclei (CCN) spectra and aerosol chemical composition were characterized at an urban supersite in Pasadena, California, from 15 May to 4 June 2010, during the CalNex campaign. The derived hygroscopicity (κCCN) of CCN-active particles with diameter between 97 and 165 nm ranged from 0.05 to 0.4. Diurnal variation showed a slight decrease of κCCN from 8:00 to 16:00 (from 0.24 to 0.20), which is attributed to increasing organics volume fraction resulted from secondary organic aerosol (SOA) formation. The derived hygroscopicity distribution and maximum activated fraction of the size selected particles were examined as functions of photochemical age. The result indicates that condensation of secondary species (e.g., SOA and sulfate) quickly converted hydrophobic particles to hydrophilic ones, and during daytime, nearly every particle became a CCN at ~0.4% in just a few hours. Based on κCCN and aerosol chemical composition, the organic hygroscopicity (κorg) was derived, and ranged from 0.05 to 0.23 with an average value of 0.13, consistent with the results from earlier studies. The derived κorg generally increased with the organic oxidation level, and most of the variation in κorg could be explained by the variation of the organic O : C atomic ratio alone. The least squares fit of the data yielded κorg = (0.83 ± 0.06) × (O:C) + (-0.19 ± 0.02). Compared to previous results based on CCN measurements of laboratory generated aerosols, κorg derived from measurements during the CalNex campaign exhibited stronger increase with O : C atomic ratio and therefore substantially higher values for organics with average O : C greater than 0.5.

  15. Hygroscopicity and CCN activity of atmospheric aerosol particles and their relation to organics: Characteristics of urban aerosols in Nagoya, Japan

    NASA Astrophysics Data System (ADS)

    Kawana, Kaori; Nakayama, Tomoki; Mochida, Michihiro

    2016-04-01

    The size-resolved distributions of hygroscopic growth factor g and the ratios of cloud condensation nuclei (CCN) to condensation nuclei of atmospheric aerosols were investigated in Nagoya, Japan. The average of the distributions of g at 85% relative humidity was bimodal. The size-resolved mean κ derived from g showed an increasing trend with diameter: 0.17-0.33 at 24-359 nm. The κ values calculated from CCN activation curves were 37% higher than those derived from g. Only 9% of the 37% difference is explained by the difference in the κ of inorganics under subsaturated and supersaturated conditions, suggesting a contribution of organics to the remaining 28% difference. The size-averaged κ of organics (κorg) was calculated as 0.14 and 0.19 by two different methods. The number fractions of CCN predicted from the hygroscopicity data over the range of 24-359 nm are loosely consistent with those observed if the size- and time-averaged g is applied to all particles (differences: -30% to +10%). This consistency improves if size- and time-resolved g and g distribution are used (differences: -19% to -3%). Whereas the number fractions of CCN predicted from the composition data are greatly underestimated if organics are assumed to be insoluble (differences: -64% to -45%), they are more consistent if κorg of 0.14 or 0.19 is applied (differences: -10% to +14%). The results demonstrate the importance of the dependence of the g of particles on time and particle size and the hygroscopicity of organics for CCN number concentrations in the urban atmosphere.

  16. A Microfluidic Paper-Based Analytical Device (μPAD) for Aerosol Oxidative Activity

    PubMed Central

    Sameenoi, Yupaporn; Panymeesamer, Pantila; Supalakorn, Natcha; Koehler, Kirsten; Chailapakul, Orawon; Henry, Charles S.; Volckens, John

    2013-01-01

    Human exposure to particulate matter (PM) air pollution has been linked with respiratory, cardiovascular, and neurodegenerative diseases, in addition to various cancers. Consistent among all of these associations is the hypothesis that PM induces inflammation and oxidative stress in the affected tissue. Consequently, a variety of assays have been developed to quantify the oxidative activity of PM as a means to characterize its ability to induced oxidative stress. The vast majority of these assays rely on high-volume, fixed-location sampling methods due to limitations in assay sensitivity and detection limit. As a result, our understanding of how personal exposure contributes to the intake of oxidative air pollution is limited. To further this understanding, we present a microfluidic paper-based analytical device (μPAD) for measuring PM oxidative activity on filters collected by personal sampling. The μPAD is inexpensive to fabricate and provides fast and sensitive analysis of aerosol oxidative activity. The oxidative activity measurement is based on the dithiothreitol assay (DTT assay), uses colorimetric detection, and can be completed in the field within 30 min following sample collection. The μPAD assay was validated against the traditional DTT assay using 13 extracted aerosol samples including urban aerosols, biomass burning PM, cigarette smoke and incense smoke. The results showed no significant differences in DTT consumption rate measured by the two methods. To demonstrate the utility of the approach, personal samples were collected to estimate human exposures to PM from indoor air, outdoor air on a clean day, and outdoor air on a wildfire-impacted day in Fort Collins, CO. Filter samples collected on the wildfire day gave the highest oxidative activity on a mass normalized basis, whereas typical ambient background air showed the lowest oxidative activity. PMID:23227907

  17. Parameterization of HONO sources in Mega-Cities

    NASA Astrophysics Data System (ADS)

    Li, G.; Zhang, R.; Tie, X.; Molina, L. T.

    2013-05-01

    Nitrous acid (HONO) plays an important role in the photochemistry of the troposphere because the photolysis of HONO is a primary source of the hydroxyl radical (OH) in the early morning. However, the formation or sources of HONO are still poorly understood in the troposphere and thence the representation of the HONO sources in chemical transport models (CTMs) is lack of comprehensive consideration. In the present study, the observed HONO, NOx, and aerosols at an urban supersite T0 during the MCMA-2006 field campaign in Mexico City are used to interpret the HONO formation in association with the suggested HONO sources from literature. The HONO source parameterizations are proposed and incorporated into the WRF-CHEM model. Homogeneous sources of HONO include the reaction of NO with OH and excited NO2 with H2O. Four HONO heterogeneous sources are considered: NO2 reaction with semivolatile organics, NO2 reaction with freshly emitted soot, NO2 reaction on aerosol and ground surfaces. Four cases are used in the present study to evaluate the proposed HONO parameterizations during four field campaigns in which HONO measurements are available, including MCMA-2003 and MCMA-2006 (Mexico City Metropolitan Area, Mexico), MIRAGE-2009 (Shanghai, China), and SHARP (Houston, USA). The WRF-CHEM model with the proposed HONO parameterizations performs moderately well in reproducing the observed diurnal variation of HONO concentrations, showing that the HONO parameterizations in the study are reasonable and potentially useful in improving the HONO simulation in CTMs.

  18. Parameterization of HONO sources in Mega-Cities

    NASA Astrophysics Data System (ADS)

    Li, Guohui; Zhang, Renyi; Tie, Xuxie; Molina, Luisa

    2013-04-01

    Nitrous acid (HONO) plays an important role in the photochemistry of the troposphere because the photolysis of HONO is a primary source of the hydroxyl radical (OH) in the early morning. However, the formation or sources of HONO are still poorly understood in the troposphere; hence the representation of the HONO sources in chemical transport models (CTMs) has lack comprehensive consideration. In the present study, the observed HONO, NOx, and aerosols at an urban supersite T0 during the MCMA-2006 field campaign in Mexico City are used to interpret the HONO formation in association with the suggested HONO sources from literature. The HONO source parameterizations are proposed and incorporated into the WRF-CHEM model. Homogeneous sources of HONO include the reaction of NO with OH and excited NO2 with H2O. Four HONO heterogeneous sources are considered: NO2 reaction with semivolatile organics, NO2 reaction with freshly emitted soot, NO2 reaction on aerosol and ground surfaces. Four cases are used in the present study to evaluate the proposed HONO parameterizations during four field campaigns in which HONO measurements are available, including MCMA-2003 and MCMA-2006 (Mexico City Metropolitan Area, Mexico), MIRAGE-2009 (Shanghai, China), and SHARP (Houston, USA). The WRF-CHEM model with the proposed HONO parameterizations performs moderately well in reproducing the observed diurnal variation of HONO concentrations, showing that the HONO parameterizations in the study are reasonable and potentially useful in improving the HONO simulation in CTMs.

  19. Parameterization of sub-grid scale convection

    NASA Technical Reports Server (NTRS)

    Frank, William; Molinari, John; Kain, Jack; Moncrieff, Mitch; Karyampudi, Mohan; Grell, Georg

    1993-01-01

    The following topics are discussed: an overview of the cumulus parameterization problem; interactions between explicit and implicit processes in mesoscale models; effects of model grid size on the cumulus parameterization problem; parameterizing convective effects on momentum fields in mesoscale models; differences between slantwise and vertical cumulus parameterization; experiments with different closure hypotheses; and coupling cumulus parameterizations to boundary layer, stable cloud, and radiation schemes.

  20. 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

  1. Parameterization of solar cells

    NASA Astrophysics Data System (ADS)

    Appelbaum, J.; Chait, A.; Thompson, D.

    1992-10-01

    The aggregation (sorting) of the individual solar cells into an array is commonly based on a single operating point on the current-voltage (I-V) characteristic curve. An alternative approach for cell performance prediction and cell screening is provided by modeling the cell using an equivalent electrical circuit, in which the parameters involved are related to the physical phenomena in the device. These analytical models may be represented by a double exponential I-V characteristic with seven parameters, by a double exponential model with five parameters, or by a single exponential equation with four or five parameters. In this article we address issues concerning methodologies for the determination of solar cell parameters based on measured data points of the I-V characteristic, and introduce a procedure for screening of solar cells for arrays. We show that common curve fitting techniques, e.g., least squares, may produce many combinations of parameter values while maintaining a good fit between the fitted and measured I-V characteristics of the cell. Therefore, techniques relying on curve fitting criteria alone cannot be directly used for cell parameterization. We propose a consistent procedure which takes into account the entire set of parameter values for a batch of cells. This procedure is based on a definition of a mean cell representing the batch, and takes into account the relative contribution of each parameter to the overall goodness of fit. The procedure is demonstrated on a batch of 50 silicon cells for Space Station Freedom.

  2. Parameterization of solar cells

    NASA Technical Reports Server (NTRS)

    Appelbaum, J.; Chait, A.; Thompson, D.

    1992-01-01

    The aggregation (sorting) of the individual solar cells into an array is commonly based on a single operating point on the current-voltage (I-V) characteristic curve. An alternative approach for cell performance prediction and cell screening is provided by modeling the cell using an equivalent electrical circuit, in which the parameters involved are related to the physical phenomena in the device. These analytical models may be represented by a double exponential I-V characteristic with seven parameters, by a double exponential model with five parameters, or by a single exponential equation with four or five parameters. In this article we address issues concerning methodologies for the determination of solar cell parameters based on measured data points of the I-V characteristic, and introduce a procedure for screening of solar cells for arrays. We show that common curve fitting techniques, e.g., least squares, may produce many combinations of parameter values while maintaining a good fit between the fitted and measured I-V characteristics of the cell. Therefore, techniques relying on curve fitting criteria alone cannot be directly used for cell parameterization. We propose a consistent procedure which takes into account the entire set of parameter values for a batch of cells. This procedure is based on a definition of a mean cell representing the batch, and takes into account the relative contribution of each parameter to the overall goodness of fit. The procedure is demonstrated on a batch of 50 silicon cells for Space Station Freedom.

  3. Effects of aerosol sources and chemical compositions on cloud drop sizes and glaciation temperatures

    NASA Astrophysics Data System (ADS)

    Zipori, Assaf; Rosenfeld, Daniel; Tirosh, Ofir; Teutsch, Nadya; Erel, Yigal

    2015-09-01

    The effect of aerosols on cloud properties, such as its droplet sizes and its glaciation temperatures, depends on their compositions and concentrations. In order to examine these effects, we collected rain samples in northern Israel during five winters (2008-2011 and 2013) and determined their chemical composition, which was later used to identify the aerosols' sources. By combining the chemical data with satellite-retrieved cloud properties, we linked the aerosol types, sources, and concentrations with the cloud glaciation temperatures (Tg). The presence of dust increased Tg from -26°C to -12°C already at relatively low dust concentrations. This result is in agreement with the conventional wisdom that desert dust serves as good ice nuclei (INs). With higher dust concentrations, Tg saturated at -12°C, even though cloud droplet sizes decreased as a result of the cloud condensation nucleating (CCN) activity of the dust. Marine air masses also encouraged freezing, but in this case, freezing was enhanced by the larger cloud droplet sizes in the air masses (caused by low CCN concentrations) and not by IN concentrations or by aerosol type. An increased fraction of anthropogenic aerosols in marine air masses caused a decrease in Tg, indicating that these aerosols served as poor IN. Anthropogenic aerosols reduced cloud droplet sizes, which further decreased Tg. Our results could be useful in climate models for aerosol-cloud interactions, as we investigated the effects of aerosols of different sources on cloud properties. Such parameterization can simplify these models substantially.

  4. Effects of a polar stratosphere cloud parameterization on ozone depletion due to stratospheric aircraft in a two-dimensional model

    NASA Technical Reports Server (NTRS)

    Considine, David B.; Douglass, Anne R.; Jackman, Charles H.

    1994-01-01

    A parameterization of Type 1 and 2 polar stratospheric cloud (PSC) formation is presented which is appropriate for use in two-dimensional (2-D) photochemical models of the stratosphere. The calculations of PSC frequency of occurrence and surface area density uses climatological temperature probability distributions obtained from National Meteorological Center data to avoid using zonal mean temperatures, which are not good predictors of PSC behavior. The parameterization does not attempt to model the microphysics of PSCs. The parameterization predicts changes in PSC formation and heterogeneous processing due to perturbations of stratospheric trace constituents. It is therefore useful in assessing the potential effects of a fleet of stratospheric aircraft (high speed civil transports, or HSCTs) on stratospheric composition. the model calculated frequency of PSC occurrence agrees well with a climatology based on stratospheric aerosol measurement (SAM) 2 observations. PSCs are predicted to occur in the tropics. Their vertical range is narrow, however, and their impact on model O3 fields is small. When PSC and sulfate aerosol heterogeneous processes are included in the model calculations, the O3 change for 1980 - 1990 is in substantially better agreement with the total ozone mapping spectrometer (TOMS)-derived O3 trend than otherwise. The overall changes in model O3 response to standard HSCT perturbation scenarios produced by the parameterization are small and tend to decrease the model sensitivity to the HSCT perturbation. However, in the southern hemisphere spring a significant increase in O3 sensitivity to HSCT perturbations is found. At this location and time, increased PSC formation leads to increased levels of active chlorine, which produce the O3 decreases.

  5. Effects of a polar stratospheric cloud parameterization on ozone depletion due to stratospheric aircraft in a two-dimensional model

    SciTech Connect

    Considine, D.B.; Douglass, A.R.; Jackman, C.H.

    1994-09-20

    A parameterization of Type 1 and 2 polar stratospheric cloud (PSC) formation is presented which is appropriate for use in two-dimensional (2-D) photochemical models of the stratosphere. The calculation of PSC frequency of occurrence and surface area density uses climatological temperature probability distributions obtained from National Meteorological Center data to avoid using zonal mean temperatures, which are not good predictors of PSC behavior. The parameterization does not attempt to model the microphysics of PSCs. The parameterization predicts changes in PSC formation and heterogeneous processing due to perturbations of stratospheric trace constituents. It is therefore useful in assessing the potential effects of a fleet of stratospheric aircraft (high speed civil transports, or HSCTs) on stratospheric composition. The model calculated frequency of PSC occurrence agrees well with a climatology based on stratospheric aerosol measurement (SAM) II observations. PSCs are predicted to occur in the tropics. Their vertical range is narrow, however, and their impact on model O{sub 3} fields is small. When PSC and sulfate aerosol heterogeneous processes are included in the model calculations, the O{sub 3} change for 1980-1990 is in substantially better agreement with the total ozone mapping spectrometer (TOMS) - derived O{sub 3} trend than otherwise. However, significant discrepancies in the northern midlatitudes remain. The overall changes in model O{sub 3} response to standard HSCT perturbation scenarios produced by the parameterization are small and tend to decrease the model sensitivity to the HSCT perturbation. However, in the southern hemisphere spring a significant increase in O{sub 3} sensitivity to HSCT perturbations is found. At this location and time, increased PSC formation leads to increased levels of active chlorine, which produce the O{sub 3} decrease. 38 refs., 13 figs., 3 tabs.

  6. A highly sensitive technique for detecting catalytically active nanoparticles against a background of general workplace aerosols

    NASA Astrophysics Data System (ADS)

    Neubauer, N.; Weis, F.; Binder, A.; Seipenbusch, M.; Kasper, G.

    2011-07-01

    A new measurement technique was studied using catalysis to specifically detect airborne nanoparticles in presence of background particles in the workplace air. Catalytically active nanoparticles produced by spark discharge were used as aerosol catalysts. According to these particles suitable catalytic test reactions were chosen and investigated by two different approaches: catalysis on airborne nanoparticles and catalysis on deposited nanoparticles. The results indicate that catalysis is applicable for the specific measurement of nanoparticles in the workplace air. Catalysis on airborne particles is suitable for the specific detection of very active nanoparticles, e.g. platinum or nickel, at high concentrations of about 107 #/cm3. The approach of catalysis on deposited particles is better suited for nanoparticle aerosols at low concentrations, for slow catalytic reactions or less active nanoparticles like iron oxide (Fe2O3). On the basis of the experimental results detection limits in the range of μg or even ng were calculated which assure the good potential of catalysis for the specific detection of nanoparticles in the workplace air based on their catalytic activity.

  7. CCN activation and hygroscopic growth measurements of secondary organic aerosols from tree emissions

    NASA Astrophysics Data System (ADS)

    Buchholz, Angela; Mentel, Thomas F.; Kiendler-Scharr, Astrid; Spindler, Christian; Tillmann, Ralf; Kleist, Einhard; Wildt, Juergen

    2010-05-01

    Plant emitted volatile organic compounds (VOCs) are a major precursor of secondary organic aerosols (SOA), an important constituent of atmospheric aerosols. We used the Juelich Plant Atmosphere Chamber (JPAC) at the Research Center Juelich to investigate the microphysical properties of aerosols. SOA particles were produced from the ozonolysis and reaction of OH radicals with the complex VOC mixture emitted from trees typical for the boreal forest. Hygroscopic growth factors (GF) were determined with a humidity tandem differential mobility analyzer (HTDMA) for different particle sizes at RH = 2 - 97%. Cloud condensation nuclei (CCN) activation was measured with a continuous flow CCN counter (DMT). Additionally, the chemical composition, size distribution and number concentration of the particles were measured. The gas phase was monitored with GC-MS and PTR-MS. Changing the emission pattern of the trees changed the measured GF and the diameter of the dry particles that were activated (Dcrit). However, below 80% RH the GF changes are within the range of the measurement error. The GF (RH = 95%) are between 1.11 and 1.19 and the Dcrit(SS = 0.4%) in a range of 93 - 100nm. Koehler theory was applied to achieve closure between CCN activation and GF measurements. The κ parameter according to Petters and Kreidenweis (2007) was calculated for all SS (κ(CCN)) and RH (κ(GF)). The κ(GF) decrease with increasing RH but levels off at RH > 95%. Assuming the surface tension of pure water, κ(GF, RH>95%) would be by a factor of 2 lower than κ(CCN). Closure between the HTDMA and CCN measurement requires the use of either a lower surface tension or a limited solubility of the organic material. Reference: Petters, M. D. and Kreidenweis, S. M. (2007). Atmos. Chem. Phys., 7, 1961-1971.

  8. Circular Polarimetry: Diagnostic of Magnetic Fields, Atmospheric Aerosols and Biologic Activity

    NASA Astrophysics Data System (ADS)

    Yanamandra-Fisher, P. A.

    2013-12-01

    The overarching goals for the remote sensing and robotic exploration of planetary systems are: (1) understanding the formation of planetary systems and their diversity; and (2) search for habitability. Our solar system is a dynamic laboratory with unique linear and circular polarimetric signatures of planets, satellites, comets, asteroids, dust, etc.. The study of both linear and circular polarization of a given system, therefore, provides insight into its origin and physical properties. Specifically, linear and circular polarimetric signatures of the object arise from different physical processes. Additionally, spectral dependence of polarization is important to separate the macroscopic (bulk) properties of the scattering medium from the microscopic (particulate) properties of the scattering medium. Linear polarization of reflected light by various solar system objects provides insight into the scattering characteristics of atmospheric aerosols and hazes; and surficial properties of atmosphereless bodies. Measurements of linear limb polarization characterizes the variation of aerosol properties across the planetary disk. Many optically active materials are anisotropic and so their scattering properties differ with the object's principal axes (such as dichroic or birefringent materials) and are crystalline in structure instead of amorphous, eg., the presence of olivines and silicates in cometary dust and circumstellar disks; Titan, etc.). Ices (water and other species) are abundant in the system indicated in their near-infrared spectra. Gas giants form outside the frost line (where ices condense), and their satellites and ring systems exhibit signature of water ice; clathrates, non-ices (Si, C, Fe) in their NIR spectra and spectral dependence of linear polarization. Circular polarization is diagnostic of magnetic fields, atmospheric aerosols and biologic activity. Aurorae occur in response to changing local magnetic fields (Earth, Jupiter, Ganymede, etc.). Biologic

  9. Marine organic aerosol and oceanic biological activity: what we know and what we need (Invited)

    NASA Astrophysics Data System (ADS)

    Facchini, M.

    2009-12-01

    Observations carried out in the North Atlantic as well as in other marine locations evidenced a seasonal dependence of sub micron particle chemical composition on biological oceanic activity and a potentially important marine aerosol organic component from primary and/or secondary formation processes associated to marine vegetation and its seasonal cycle. Primary organics generated by bubble bursting in high biological activity periods are almost entirely water insoluble (WIOM up to 96 ± 2 % )and are constituted by aggregation of lipopolysaccharides exuded by phytoplankton with dominant surface tension character. In many marine environments the secondary organic fraction is dominated by MSA and by several oxygenated species (mainly carboxylic acids). New measurements also show the potential importance of secondary organic N species (biogenic amine salts ). However a large fraction of the secondary organic fraction (SOA) is still not characterized and the precursors are not identified. For modeling marine organics, besides reducing the uncertainty in the knowledge of the chemical composition and new precursors, it is of crucial importance to link marine aerosol organic composition to satellite products that could be better proxy for marine biological activity and of its decomposition products than chlorophyll-a.

  10. CCN activity and volatility of β-caryophyllene secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Frosch, M.; Bilde, M.; Nenes, A.; Praplan, A. P.; Jurányi, Z.; Dommen, J.; Gysel, M.; Weingartner, E.; Baltensperger, U.

    2012-08-01

    In a series of smog chamber experiments, the Cloud Condensation Nuclei (CCN) activity of Secondary Organic Aerosol (SOA) generated from ozonolysis of β-caryophyllene was characterized by determining the CCN derived hygroscopicity parameter, κCCN, from experimental data. Two types of CCN counters, operating at different temperatures, were used. The effect of semi-volatile organic compounds on the CCN activity of SOA was studied using a thermodenuder. Overall, SOA was only slightly CCN active (with κCCN in the range 0.001-0.16), and in dark experiments with no OH scavenger present, κCCN decreased when particles were sent through the thermodenuder (with a temperature up to 50 °C). SOA was generated under different experimental conditions: in some experiments, an OH scavenger (2-butanol) was added. SOA from these experiments was less CCN active than SOA produced in experiments without an OH scavenger (i.e. where OH was produced during ozonolysis). In other experiments, lights were turned on, either without or with the addition of HONO (OH source). This led to the formation of more CCN active SOA. SOA was aged up to 30 h through exposure to ozone and (in experiments with no OH scavenger present) to OH. In all experiments, the derived κCCN consistently increased with time after initial injection of β-caryophyllene, showing that chemical ageing increases the CCN activity of β-caryophyllene SOA. κCCN was also observed to depend on supersaturation, which was explained either as an evaporation artifact from semi-volatile SOA (only observed in experiments lacking light exposure) or, alternatively, by effects related to chemical composition depending on dry particle size. Using the method of Threshold Droplet Growth Analysis it was also concluded that the activation kinetics of the SOA do not differ significantly from calibration ammonium sulphate aerosol.

  11. CCN activity and volatility of β-caryophyllene secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Frosch, M.; Bilde, M.; Nenes, A.; Praplan, A. P.; Jurányi, Z.; Dommen, J.; Gysel, M.; Weingartner, E.; Baltensperger, U.

    2013-02-01

    In a series of smog chamber experiments, the cloud condensation nuclei (CCN) activity of secondary organic aerosol (SOA) generated from ozonolysis of β-caryophyllene was characterized by determining the CCN derived hygroscopicity parameter, κCCN, from experimental data. Two types of CCN counters, operating at different temperatures, were used. The effect of semi-volatile organic compounds on the CCN activity of SOA was studied using a thermodenuder. Overall, SOA was only slightly CCN active (with κCCN in the range 0.001-0.16), and in dark experiments with no OH scavenger present, κCCN decreased when particles were sent through the thermodenuder (with a temperature up to 50 °C). SOA was generated under different experimental conditions: In some experiments, an OH scavenger (2-butanol) was added. SOA from these experiments was less CCN active than SOA produced in experiments without an OH scavenger (i.e. where OH was produced during ozonolysis). In other experiments, lights were turned on, either without or with the addition of HONO (OH source). This led to the formation of more CCN active SOA. SOA was aged up to 30 h through exposure to ozone and (in experiments with no OH scavenger present) to OH. In all experiments, the derived κCCN consistently increased with time after initial injection of β-caryophyllene, showing that chemical ageing increases the CCN activity of β-caryophyllene SOA. κCCN was also observed to depend on supersaturation, which was explained either as an evaporation artifact from semi-volatile SOA (only observed in experiments lacking light exposure) or, alternatively, by effects related to chemical composition depending on dry particle size. Using the method of Threshold Droplet Growth Analysis it was also concluded that the activation kinetics of the SOA do not differ significantly from calibration ammonium sulphate aerosol for particles aged for several hours.

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

    NASA Astrophysics Data System (ADS)

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

    2008-08-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2008-03-01

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

  14. Soot Aerosol Particles as Cloud Condensation Nuclei: from Ice Nucleation Activity to Ice Crystal Morphology

    NASA Astrophysics Data System (ADS)

    Pirim, Claire; Ikhenazene, Raouf; Ortega, Isamel Kenneth; Carpentier, Yvain; Focsa, Cristian; Chazallon, Bertrand; Ouf, François-Xavier

    2016-04-01

    Emissions of solid-state particles (soot) from engine exhausts due to incomplete fuel combustion is considered to influence ice and liquid water cloud droplet activation [1]. The activity of these aerosols would originate from their ability to be important centers of ice-particle nucleation, as they would promote ice formation above water homogeneous freezing point. Soot particles are reported to be generally worse ice nuclei than mineral dust because they activate nucleation at higher ice-supersaturations for deposition nucleation and at lower temperatures for immersion freezing than ratios usually expected for homogeneous nucleation [2]. In fact, there are still numerous opened questions as to whether and how soot's physico-chemical properties (structure, morphology and chemical composition) can influence their nucleation ability. Therefore, systematic investigations of soot aerosol nucleation activity via one specific nucleation mode, here deposition nucleation, combined with thorough structural and compositional analyzes are needed in order to establish any association between the particles' activity and their physico-chemical properties. In addition, since the morphology of the ice crystals can influence their radiative properties [3], we investigated their morphology as they grow over both soot and pristine substrates at different temperatures and humidity ratios. In the present work, Combustion Aerosol STandart soot samples were produced from propane using various experimental conditions. Their nucleation activity was studied in deposition mode (from water vapor), and monitored using a temperature-controlled reactor in which the sample's relative humidity is precisely measured with a cryo-hygrometer. Formation of water/ice onto the particles is followed both optically and spectroscopically, using a microscope coupled to a Raman spectrometer. Vibrational signatures of hydroxyls (O-H) emerge when the particle becomes hydrated and are used to characterize ice

  15. Discernible signals of aerosol effects on the diurnal, weekly and decadal variations in thunderstorm activities

    NASA Astrophysics Data System (ADS)

    Li, Z.

    2015-12-01

    Aerosol can affect atmospheric convection, cloud and precipitation in a variety of means by altering energy balance at the surface and in the atmospheric column, and by altering cloud micro- and macro-physical properties. The effects are often contingent upon meteorological variables and aerosol properties. By reducing surface energy budget, aerosol tends to suppress convection, but aerosol-induced heating in the lower atmosphere can destabilize the upper atmosphere and strengthen convection. Aerosol-induced altering cloud microphysics may also suppress or invigorate cloud development pending on various factors. In this talk, I will illustrate how aerosols likely contribute to the thunderstorm variability on three distinct time scales from diurnal, weekly to decadal and how different types of aerosols and varying meteorological conditions may affect with the observed trends. I will first demonstrate the opposite effects of conservative scattering and hygroscopic aerosols versus absorbing and hydrophobic aerosol on the long-term trends of thunderstorms. I will then illustrate that aerosol can have a discernible effect on the weekly cycle of thunderstorms and there is the dependence of the phase of the weekly cycle on aerosol types. Last, I will show how aerosol delays the occurrence of thunderstorms. Of course, the plausible connections are subject to various uncertainties that should be tackled with more rigorous modeling and extensive observation studies.

  16. Data-driven aerosol development in the GEOS-5 modeling and data assimilation system

    NASA Astrophysics Data System (ADS)

    Darmenov, A.; da Silva, A.; Liu, X.; Colarco, P. R.

    2013-12-01

    Atmospheric aerosols are important radiatively active agents that also affect clouds, atmospheric chemistry, the water cycle, land and ocean biogeochemistry. Furthermore, exposure to anthropogenic and/or natural fine particulates can have negative health effects. No single instrument or model is capable of quantifying the diverse and dynamic nature of aerosols at the range of spatial and temporal scales at which they interact with the other constituents and components of the Earth system. However, applying model-data integration techniques can minimize limitations of individual data products and remedy model deficiencies. The Goddard Earth Observing System Model, Version 5 (GEOS-5) is the latest version of the NASA Global Modeling and Assimilation Office (GMAO) Earth system model. GEOS-5 is a modeling and data assimilation framework well suited for aerosol research. It is being used to perform aerosol re-analysis and near real-time aerosol forecast on a global scale at resolutions comparable to those of aerosol products from modern spaceborne instruments. The aerosol processes in GEOS-5 derive from the Goddard Chemistry Aerosol Radiation and Transport (GOCART) but it is implemented on-line, within the climate model. GEOS-5 aerosol modeling capabilities have recently been enhanced by inclusion of the Modal Aerosol Microphysics module (MAM-7) originally developed in the Community Earth System Model (CESM) model. This work will present examples of data driven model development that include refining parameterization of sea-salt emissions, tuning of biomass burning emissions from vegetation fires and the effect of the updated emissions on the modeled direct aerosol forcing. We will also present results from GOES-5/MAM-7 model evaluation against AOD and particulate pollution datasets, and outline future directions of aerosol data assimilation in the GEOS-5 system.

  17. A Thermal Infrared Radiation Parameterization for Atmospheric Studies

    NASA Technical Reports Server (NTRS)

    Chou, Ming-Dah; Suarez, Max J.; Liang, Xin-Zhong; Yan, Michael M.-H.; Cote, Charles (Technical Monitor)

    2001-01-01

    This technical memorandum documents the longwave radiation parameterization developed at the Climate and Radiation Branch, NASA Goddard Space Flight Center, for a wide variety of weather and climate applications. Based on the 1996-version of the Air Force Geophysical Laboratory HITRAN data, the parameterization includes the absorption due to major gaseous absorption (water vapor, CO2, O3) and most of the minor trace gases (N2O, CH4, CFCs), as well as clouds and aerosols. The thermal infrared spectrum is divided into nine bands. To achieve a high degree of accuracy and speed, various approaches of computing the transmission function are applied to different spectral bands and gases. The gaseous transmission function is computed either using the k-distribution method or the table look-up method. To include the effect of scattering due to clouds and aerosols, the optical thickness is scaled by the single-scattering albedo and asymmetry factor. The parameterization can accurately compute fluxes to within 1% of the high spectral-resolution line-by-line calculations. The cooling rate can be accurately computed in the region extending from the surface to the 0.01-hPa level.

  18. Global distribution and climate forcing of marine organic aerosol: 1. Model improvements and evaluation

    SciTech Connect

    Meskhidze, N.; Xu, J.; Gantt, Brett; Zhang, Yang; Nenes, Athanasios; Ghan, Steven J.; Liu, Xiaohong; Easter, Richard C.; Zaveri, Rahul A.

    2011-11-23

    Marine organic aerosol emissions have been implemented and evaluated within the National Center of Atmospheric Research (NCAR)'s Community Atmosphere Model (CAM5) with the Pacific Northwest National Laboratory's 7-mode Modal Aerosol Module (MAM-7). Emissions of marine primary organic aerosols (POA), phytoplanktonproduced isoprene- and monoterpenes-derived secondary organic aerosols (SOA) and methane sulfonate (MS{sup -}) are shown to affect surface concentrations of organic aerosols in remote marine regions. Global emissions of submicron marine POA is estimated to be 7.9 and 9.4 Tg yr{sup -1}, for the Gantt et al. (2011) and Vignati et al. (2010) emission parameterizations, respectively. Marine sources of SOA and particulate MS{sup -} (containing both sulfur and carbon atoms) contribute an additional 0.2 and 5.1 Tg yr{sup -1}, respectively. Widespread areas over productive waters of the Northern Atlantic, Northern Pacific, and the Southern Ocean show marine-source submicron organic aerosol surface concentrations of 100 ngm{sup -3}, with values up to 400 ngm{sup -3} over biologically productive areas. Comparison of long-term surface observations of water insoluble organic matter (WIOM) with POA concentrations from the two emission parameterizations shows that despite revealed discrepancies (often more than a factor of 2), both Gantt et al. (2011) and Vignati et al. (2010) formulations are able to capture the magnitude of marine organic aerosol concentrations, with the Gantt et al. (2011) parameterization attaining better seasonality. Model simulations show that the mixing state of the marine POA can impact the surface number concentration of cloud condensation nuclei (CCN). The largest increases (up to 20 %) in CCN (at a supersaturation (S) of 0.2 %) number concentration are obtained over biologically productive ocean waters when marine organic aerosol is assumed to be externally mixed with sea-salt. Assuming marine organics are internally-mixed with sea

  19. Effect of aerosols on solar UV irradiances during the Photochemical Activity and Solar Ultraviolet Radiation Campaign

    NASA Astrophysics Data System (ADS)

    Kylling, A.; Bais, A. F.; Blumthaler, M.; Schreder, J.; Zerefos, C. S.; Kosmidis, E.

    1998-10-01

    Surface UV irradiances were measured at two different sites in Greece during June 1996 under noncloudy conditions. The measured UV irradiances are simulated by a radiative transfer model using measured ozone density and aerosol optical depth profiles. The absolute difference between model and measurements ranges between -5% and +5% with little dependence on wavelength. The temporal and solar zenith angle dependence in the difference between model and measurement suggests that part of this difference may be explained by assumptions made about the aerosol single-scattering albedo and phase function. Simulated spectra including aerosols are compared with calculated spectra excluding aerosols. It is found that for otherwise similar atmospheric conditions the UVB irradiance is reduced with respect to aerosol free conditions by 5% to 35% depending on the aerosol optical depth and single-scattering albedo. For the campaign period, changes in the aerosol loading gave larger variations in the surface UV irradiances than the changes seen in the ozone column.

  20. 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.

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

    PubMed

    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) (R(2) = 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 (R(2) = 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

  2. VEGF neutralizing aerosol therapy in primary pulmonary adenocarcinoma with K-ras activating-mutations.

    PubMed

    Hervé, Virginie; Rabbe, Nathalie; Guilleminault, Laurent; Paul, Flora; Schlick, Laurène; Azzopardi, Nicolas; Duruisseaux, Michael; Fouquenet, Delphine; Montharu, Jérôme; Redini, Françoise; Paintaud, Gilles; Lemarié, Etienne; Cadranel, Jacques; Wislez, Marie; Heuzé-Vourc'h, Nathalie

    2014-01-01

    K-ras mutations promote angiogenesis in lung cancer and contribute to the drug resistance of cancer cells. It is not clear whether K-ras mutated adenocarcinomas are sensitive to anti-angiogenic therapy with monoclonal antibodies (mAbs) that target vascular endothelial growth factor (VEGF). Anti-angiogenic mAbs are usually delivered systemically, but only a small proportion reaches the lung after intravenous injection. We investigated the relevance of a non-invasive pulmonary route for the delivery of anti-VEGF mAbs in the mouse K-ras(LA1) model. We found that pulmonary delivery of these mAbs significantly reduced the number of tumor lesions and inhibited malignant progression. The antitumor effect involves the VEGFR2-dependent inhibition of blood vessel growth, which impairs tumor proliferation. Pharmacokinetic analysis of aerosolized anti-VEGF showed its low rate of passage into the bloodstream, suggesting that this delivery route is associated with reduced systemic side effects. Our findings highlight the value of the aerosol route for administration of anti-angiogenic mAbs in pulmonary adenocarcinoma with K-ras activating-mutations. PMID:25484066

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

    NASA Astrophysics Data System (ADS)

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

    2014-05-01

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

  4. Selectivity Across the Interface: A Test of Surface Activity in the Composition of Organic-Enriched Aerosols from Bubble Bursting.

    PubMed

    Cochran, Richard E; Jayarathne, Thilina; Stone, Elizabeth A; Grassian, Vicki H

    2016-05-01

    Although theories have been developed that describe surface activity of organic molecules at the air-water interface, few studies have tested how surface activity impacts the selective transfer of molecules from solution phase into the aerosol phase during bubble bursting. The selective transfer of a series of organic compounds that differ in their solubility and surface activity from solution into the aerosol phase is quantified experimentally for the first time. Aerosol was produced from solutions containing salts and a series of linear carboxlyates (LCs) and dicarboxylates (LDCs) using a bubble bursting process. Surface activity of these molecules dominated the transport across the interface, with enrichment factors of the more surface-active C4-C8 LCs (55 ± 8) being greater than those of C4-C8 LDCs (5 ± 1). Trends in the estimated surface concentrations of LCs at the liquid-air interface agreed well with their relative concentrations in the aerosol phase. In addition, enrichment of LCs was followed by enrichment of calcium with respect to other inorganic cations and depletion of chloride and sulfate. PMID:27093579

  5. New particle dependant parameterizations of heterogeneous freezing processes.

    NASA Astrophysics Data System (ADS)

    Diehl, Karoline; Mitra, Subir K.

    2014-05-01

    For detailed investigations of cloud microphysical processes an adiabatic air parcel model with entrainment is used. It represents a spectral bin model which explicitly solves the microphysical equations. The initiation of the ice phase is parameterized and describes the effects of different types of ice nuclei (mineral dust, soot, biological particles) in immersion, contact, and deposition modes. As part of the research group INUIT (Ice Nuclei research UnIT), existing parameterizations have been modified for the present studies and new parameterizations have been developed mainly on the basis of the outcome of INUIT experiments. Deposition freezing in the model is dependant on the presence of dry particles and on ice supersaturation. The description of contact freezing combines the collision kernel of dry particles with the fraction of frozen drops as function of temperature and particle size. A new parameterization of immersion freezing has been coupled to the mass of insoluble particles contained in the drops using measured numbers of ice active sites per unit mass. Sensitivity studies have been performed with a convective temperature and dew point profile and with two dry aerosol particle number size distributions. Single and coupled freezing processes are studied with different types of ice nuclei (e.g., bacteria, illite, kaolinite, feldspar). The strength of convection is varied so that the simulated cloud reaches different levels of temperature. As a parameter to evaluate the results the ice water fraction is selected which is defined as the relation of the ice water content to the total water content. Ice water fractions between 0.1 and 0.9 represent mixed-phase clouds, larger than 0.9 ice clouds. The results indicate the sensitive parameters for the formation of mixed-phase and ice clouds are: 1. broad particle number size distribution with high number of small particles, 2. temperatures below -25°C, 3. specific mineral dust particles as ice nuclei such

  6. Use of active and passive ground based remote sensors to explore cloud droplet modifications in aerosol-cloud interactions

    NASA Astrophysics Data System (ADS)

    Han, Zaw Thet

    We explore the potential aerosol impact on cloud optical properties which is a strong modifier of climate forcing. Previous studies have shown that increased aerosol loading can affect the cloud optical properties such as cloud optical depth and cloud droplet effective radius in rural areas, particularly at the Atmospheric Radiation Measurement, Southern Great Plain site. In this study, we attempt to observe and quantify aerosol-cloud interaction over New York City, using a combination of passive and active radiometric sensors. In particular, we look for signatures of the Twomey indirect effect which states that the droplet size of water phase clouds will decrease with increasing aerosols. We find that under certain conditions, a strong signature is found between the cloud drop effective radius and extinction and this effect is in part due to vertical wind uptake. In demonstrating the Aerosol Cloud Interaction, we use multiple approaches. For example, we derive the integrated liquid water path using both a multiband neural network and dual channel approach and show general agreement between two methods while the DC approach seems more robust. We also find that these measurements are difficult and sensitive to the position of the aerosols relative to the cloud base. As a corollary, we explore whether near surface aerosol loading can effecting the cloud by using particulate matter (PM2.5) and find that the effects are too variable to be given any statistical weight. Finally, we explore the potential of modifying our approach to remove the noisy and difficult measurement of Raman LIDAR derived extinction with calibrated LIDAR backscatter. The results seem to show a general improvement in correlation and offer the possibility of increasing the number of cases observed.

  7. CCN activation and efficiency of nucleation and impaction removal process of biomass burning aerosols in Brazil: preliminary results.

    NASA Astrophysics Data System (ADS)

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

    2015-04-01

    The biomass burning activity constitutes an important source of aerosols and trace gases to the atmosphere globally. In South America, during the dry season, aerosols prevenient from biomass burning are typically transported to long distances from its sources before being removed though contributing significantly to the aerosol budget on a continental scale. The uncertainties in the magnitude of the impacts on the hydrological cycle, the radiation budget and the biogeochemical cycles on a continental scale are still noteworthy. The still unknowns on the efficiency of biomass burning aerosol to act as cloud condensation nuclei (CCN) and the effectiveness of the nucleation and impaction scavenging mechanisms in removing them from the atmosphere contribute to such uncertainties. In the present work, the explicit modelling of the early stages of cloud development using a parcel model for the typical conditions of the dry season and dry-to-wet transition periods in Amazonia allowed an estimation of the efficiency of nucleation scavenging process and the ability of South American biomass burning aerosol to act as CCN. Additionally, the impaction scavenging was simulated for the same aerosol population following a method based on the widely used concept of the efficiency of collision between a raindrop and an aerosol particle. DMPS and H-TDMA data available in the literature for biomass burning aerosol population in the region indicated the presence of a nearly hydrophobic fraction (on average, with specific hygroscopic parameter κ=0.04, and relative abundance of 73 %) and nearly hygroscopic fraction (κ=0.13, 27 %), externally mixed. The hygroscopic parameters and relative abundances of each hygroscopic group, as well as the weighted average specific hygroscopic parameter for the entire population κ=0.06, were used in calculations of aerosol activation and population mass and number concentration scavenged by nucleation. Results from both groups of simulations are

  8. GFDL ARM Project Technical Report: Using ARM Observations to Evaluate Cloud and Convection Parameterizations & Cloud-Convection-Radiation Interactions in the GFDL Atmospheric General Circulation Model

    SciTech Connect

    V. Ramaswamy; L. J. Donner; J-C. Golaz; S. A. Klein

    2010-06-17

    This report briefly summarizes the progress made by ARM postdoctoral fellow, Yanluan Lin, at GFDL during the period from October 2008 to present. Several ARM datasets have been used for GFDL model evaluation, understanding, and improvement. This includes a new ice fall speed parameterization with riming impact and its test in GFDL AM3, evaluation of model cloud and radiation diurnal and seasonal variation using ARM CMBE data, model ice water content evaluation using ARM cirrus data, and coordination of the TWPICE global model intercomparison. The work illustrates the potential and importance of ARM data for GCM evaluation, understanding, and ultimately, improvement of GCM cloud and radiation parameterizations. Future work includes evaluation and improvement of the new dynamicsPDF cloud scheme and aerosol activation in the GFDL model.

  9. Summary of Cumulus Parameterization Workshop

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Starr, David OC.; Hou, Arthur; Newman, Paul; Sud, Yogesh

    2002-01-01

    A workshop on cumulus parameterization took place at the NASA Goddard Space Flight Center from December 3-5, 2001. The major objectives of this workshop were (1) to review the problem of representation of moist processes in large-scale models (mesoscale models, Numerical Weather Prediction models and Atmospheric General Circulation Models), (2) to review the state-of-the-art in cumulus parameterization schemes, and (3) to discuss the need for future research and applications. There were a total of 31 presentations and about 100 participants from the United States, Japan, the United Kingdom, France and South Korea. The specific presentations and discussions during the workshop are summarized in this paper.

  10. Evaluation of aerosol indirect radiative effects on climate in the EMAC model

    NASA Astrophysics Data System (ADS)

    Chang, Dong Yeong; Tost, Holger; Steil, Benedikt; Lelieveld, Jos

    2013-04-01

    Anthropogenic aerosol particles directly and indirectly influence cloud properties and the Earth's radiative energy budget. Several studies have estimated the effects on climate using global circulation models (GCMs), indicating large differences between different models and large uncertainty ranges. These are mostly attributed to different cloud microphysical process parameterizations and uncertainties in the representation of aerosols. Without detailed cloud microphysical processes, using empirical relations between aerosol number or mass and cloud droplet number potentially even large discrepancies may arise. In the present study, a mechanistic aerosol activation scheme, based on double moment cloud microphysics, is used to compute aerosol indirect radiative and cloud effects in the EMAC model. Aerosol activation is linked to the cloud droplet nucleation processes in warm clouds, accounting for the number, size, and chemical composition of particles under ambient meteorological conditions. This approach uses a combination of empirical and semi-empirical parameters to represent aerosol water uptake and hygroscopic growth into cloud droplets. To evaluate the performance of our approach satellite datasets are used; for example, total cloud fraction from MODIS data and cloud radiative forcing at the top of atmosphere from CERES EBAF data.

  11. The standoff aerosol active signature testbed (SAAST) at MIT Lincoln Laboratory

    NASA Astrophysics Data System (ADS)

    Richardson, Jonathan M.; Aldridge, John C.

    2005-11-01

    Standoff LIDAR detection of BW agents depends on accurate knowledge of the infrared and ultraviolet optical elastic scatter (ES) and ultraviolet fluorescence (UVF) signatures of bio-agents and interferents. MIT Lincoln Laboratory has developed the Standoff Aerosol Active Signature Testbed (SAAST) for measuring ES cross sections from BW simulants and interferents at all angles including 180º (direct backscatter). Measurements of interest include the dependence of the ES and UVF signatures on several spore production parameters including growth medium, sporulation protocol, washing protocol, fluidizing additives, and degree of aggregation. Using SAAST, we have made measurements of the ES signature of Bacillus globigii (atropheaus, Bg) spores grown under different growth methods. We have also investigated one common interferent (Arizona Test Dust). Future samples will include pollen and diesel exhaust. This paper presents the details of the SAAST apparatus along with the results of recent measurements.

  12. EFFECT OF AN ACTIVATED SLUDGE WASTEWATER TREATMENT PLANT ON AMBIENT AIR DENSITIES OF AEROSOLS CONTAINING BACTERIA AND VIRUSES

    EPA Science Inventory

    Bacteria and virus-containing aerosols were studied during late summer and fall in a U.S. midwestern suburb before and during the start up and operation of an unenclosed activated sludge wastewater treatment plant. The air in this suburban area contained low-level densities of in...

  13. Long-term study of cloud condensation nuclei (CCN) activation of the atmospheric aerosol in Vienna

    PubMed Central

    Burkart, J.; Steiner, G.; Reischl, G.; Hitzenberger, R.

    2011-01-01

    During a total of 11 months, cloud condensation nuclei (CCN at super-saturation S 0.5%) and condensation nuclei (CN) concentrations were measured in the urban background aerosol of Vienna, Austria. For several months, number size distributions between 13.22 nm and 929 nm were also measured with a scanning mobility particle spectrometer (SMPS). Activation ratios (i.e. CCN/CN ratios) were calculated and apparent activation diameters obtained by integrating the SMPS size distributions. Variations in all CCN parameters (concentration, activation ratio, apparent activation diameter) are quite large on timescales of days to weeks. Passages of fronts influenced CCN parameters. Concentrations decreased with the passage of a front. No significant differences were found for fronts from different sectors (for Vienna mainly north to west and south to east). CCN concentrations at 0.5% S ranged from 160 cm−3 to 3600 cm−3 with a campaign average of 820 cm−3. Activation ratios were quite low (0.02–0.47, average: 0.13) and comparable to activation ratios found in other polluted regions (e.g. Cubison et al., 2008). Apparent activation diameters were found to be much larger (campaign average: 169 nm, range: (69–370) nm) than activation diameters for single-salt particles (around 50 nm depending on the salt). Contrary to CN concentrations, which are influenced by source patterns, CCN concentrations did not exhibit distinct diurnal patterns. Activation ratios showed diurnal variations counter-current to the variations of CN concentrations. PMID:21977003

  14. Ice nucleation by soil dust compared to desert dust aerosols

    NASA Astrophysics Data System (ADS)

    Moehler, O.; Steinke, I.; Ullrich, R.; Höhler, K.; Schiebel, T.; Hoose, C.; Funk, R.

    2015-12-01

    A minor fraction of atmospheric aerosol particles, so-called ice-nucleating particles (INPs), initiates the formation of the ice phase in tropospheric clouds and thereby markedly influences the Earth's weather and climate systems. Whether an aerosol particle acts as an INP depends on its size, morphology and chemical compositions. The INP fraction of certain aerosol types also strongly depends on the temperature and the relative humidity. Because both desert dust and soil dust aerosols typically comprise a variety of different particles, it is difficult to assess and predict their contribution to the atmospheric INP abundance. This requires both accurate modelling of the sources and atmospheric distribution of atmospheric dust components and detailed investigations of their ice nucleation activities. The latter can be achieved in laboratory experiments and parameterized for use in weather and climate models as a function of temperature and particle surface area, a parameter called ice-nucleation active site (INAS) density. Concerning ice nucleation activity studies, the soil dust is of particular interest because it contains a significant fraction of organics and biological components, both with the potential for contributing to the atmospheric INP abundance at relatively high temperatures compared to mineral components. First laboratory ice nucleation experiments with a few soil dust samples indicated their INP fraction to be comparable or slightly enhanced to that of desert dust. We have used the AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud simulation chamber to study the immersion freezing ability of four different arable soil dusts, sampled in Germany, China and Argentina. For temperatures higher than about -20°C, we found the INP fraction of aerosols generated from these samples by a dry dispersion technique to be significantly higher compared to various desert dust aerosols also investigated in AIDA experiments. In this contribution, we

  15. Assessing aerosol indirect effect through ice clouds in CAM5

    NASA Astrophysics Data System (ADS)

    Zhang, Kai; Liu, Xiaohong; Yoon, Jin-Ho; Wang, Minghuai; Comstock, Jennifer M.; Barahona, Donifan; Kooperman, Gabriel

    2013-05-01

    Ice clouds play an important role in regulating the Earth's radiative budget and influencing the hydrological cycle. Aerosols can act as solution droplets or ice nuclei for ice crystal formation, thus affecting the physical properties of ice clouds. Because the related dynamical and microphysical processes happen at very small spatial and temporal scales, it is a great challenge to accurately represent them in global climate models. Consequently, the aerosol indirect effect through ice clouds (ice AIE) estimated by global climate models is associated with large uncertainties. In order to better understand these processes and improve ice cloud parameterization in the Community Atmospheric Model, version 5 (CAM5), we analyze in-situ measurements from various research campaigns, and use the derived statistical information to evaluate and constrain the model [1]. We also make use of new model capabilities (prescribed aerosols and nudging) to estimate the aerosol indirect effect through ice clouds, and quantify the uncertainties associated with ice nucleation processes. In this study, a new approach is applied to separate the impact of aerosols on warm and cold clouds by using the prescribed-aerosol capability in CAM5 [2]. This capability allows a single simulation to simultaneously include up to three aerosol fields: online calculated, as well as prescribed pre-industrial (PI) and present-day conditions (PD). In a set of sensitivity simulations, we use the same aerosol fields to drive droplet activation in warm clouds, and different (PD and PI) conditions for different components of the ice nucleation parameterization in pure ice clouds, so as to investigate various ice nucleation mechanisms in an isolated manner. We also applied nudging in our simulations, which helps to increase the signal-to-noise ratio in much shorter simulation period [3] and isolate the impact of aerosols on ice clouds from other factors, such as temperature and relative humidity change. The

  16. RACORO aerosol data processing

    SciTech Connect

    Elisabeth Andrews

    2011-10-31

    The RACORO aerosol data (cloud condensation nuclei (CCN), condensation nuclei (CN) and aerosol size distributions) need further processing to be useful for model evaluation (e.g., GCM droplet nucleation parameterizations) and other investigations. These tasks include: (1) Identification and flagging of 'splash' contaminated Twin Otter aerosol data. (2) Calculation of actual supersaturation (SS) values in the two CCN columns flown on the Twin Otter. (3) Interpolation of CCN spectra from SGP and Twin Otter to 0.2% SS. (4) Process data for spatial variability studies. (5) Provide calculated light scattering from measured aerosol size distributions. Below we first briefly describe the measurements and then describe the results of several data processing tasks that which have been completed, paving the way for the scientific analyses for which the campaign was designed. The end result of this research will be several aerosol data sets which can be used to achieve some of the goals of the RACORO mission including the enhanced understanding of cloud-aerosol interactions and improved cloud simulations in climate models.

  17. ARM Data for Cloud Parameterization

    SciTech Connect

    Xu, Kuan-Man

    2006-10-02

    The PI's ARM investigation (DE-IA02-02ER633 18) developed a physically-based subgrid-scale saturation representation that fully considers the direct interactions of the parameterized subgrid-scale motions with subgrid-scale cloud microphysical and radiative processes. Major accomplishments under the support of that interagency agreement are summarized in this paper.

  18. Effects of surface-active organic matter on carbon dioxide nucleation in atmospheric wet aerosols: a molecular dynamics study.

    PubMed

    Daskalakis, Vangelis; Charalambous, Fevronia; Panagiotou, Fostira; Nearchou, Irene

    2014-11-21

    Organic matter (OM) uptake in cloud droplets produces water-soluble secondary organic aerosols (SOA) via aqueous chemistry. These play a significant role in aerosol properties. We report the effects of OM uptake in wet aerosols, in terms of the dissolved-to-gas carbon dioxide nucleation using molecular dynamics (MD) simulations. Carbon dioxide has been implicated in the natural rainwater as well as seawater acidity. Variability of the cloud and raindrop pH is assumed in space and time, as regional emissions, local human activities and geophysical characteristics differ. Rain scavenging of inorganic SOx, NOx and NH3 plays a major role in rain acidity in terms of acid-base activity, however carbon dioxide solubility also remains a key parameter. Based on the MD simulations we propose that the presence of surface-active OM promotes the dissolved-to-gas carbon dioxide nucleation in wet aerosols, even at low temperatures, strongly decreasing carbon dioxide solubility. A discussion is made on the role of OM in controlling the pH of a cloud or raindrop, as a consequence, without involving OM ionization equilibrium. The results are compared with experimental and computational studies in the literature. PMID:25272147

  19. Parameterization of cloud glaciation by atmospheric dust

    NASA Astrophysics Data System (ADS)

    Nickovic, Slobodan; Cvetkovic, Bojan; Madonna, Fabio; Pejanovic, Goran; Petkovic, Slavko

    2016-04-01

    The exponential growth of research interest on ice nucleation (IN) is motivated, inter alias, by needs to improve generally unsatisfactory representation of cold cloud formation in atmospheric models, and therefore to increase the accuracy of weather and climate predictions, including better forecasting of precipitation. Research shows that mineral dust significantly contributes to cloud ice nucleation. Samples of residual particles in cloud ice crystals collected by aircraft measurements performed in the upper tropopause of regions distant from desert sources indicate that dust particles dominate over other known ice nuclei such as soot and biological particles. In the nucleation process, dust chemical aging had minor effects. The observational evidence on IN processes has substantially improved over the last decade and clearly shows that there is a significant correlation between IN concentrations and the concentrations of coarser aerosol at a given temperature and moisture. Most recently, due to recognition of the dominant role of dust as ice nuclei, parameterizations for immersion and deposition icing specifically due to dust have been developed. Based on these achievements, we have developed a real-time forecasting coupled atmosphere-dust modelling system capable to operationally predict occurrence of cold clouds generated by dust. We have been thoroughly validated model simulations against available remote sensing observations. We have used the CNR-IMAA Potenza lidar and cloud radar observations to explore the model capability to represent vertical features of the cloud and aerosol vertical profiles. We also utilized the MSG-SEVIRI and MODIS satellite data to examine the accuracy of the simulated horizontal distribution of cold clouds. Based on the obtained encouraging verification scores, operational experimental prediction of ice clouds nucleated by dust has been introduced in the Serbian Hydrometeorological Service as a public available product.

  20. Tropospheric Aerosols

    NASA Astrophysics Data System (ADS)

    Buseck, P. R.; Schwartz, S. E.

    2003-12-01

    It is widely believed that "On a clear day you can see forever," as proclaimed in the 1965 Broadway musical of the same name. While an admittedly beautiful thought, we all know that this concept is only figurative. Aside from Earth's curvature and Rayleigh scattering by air molecules, aerosols - colloidal suspensions of solid or liquid particles in a gas - limit our vision. Even on the clearest day, there are billions of aerosol particles per cubic meter of air.Atmospheric aerosols are commonly referred to as smoke, dust, haze, and smog, terms that are loosely reflective of their origin and composition. Aerosol particles have arisen naturally for eons from sea spray, volcanic emissions, wind entrainment of mineral dust, wildfires, and gas-to-particle conversion of hydrocarbons from plants and dimethylsulfide from the oceans. However, over the industrial period, the natural background aerosol has been greatly augmented by anthropogenic contributions, i.e., those produced by human activities. One manifestation of this impact is reduced visibility (Figure 1). Thus, perhaps more than in other realms of geochemistry, when considering the composition of the troposphere one must consider the effects of these activities. The atmosphere has become a reservoir for vast quantities of anthropogenic emissions that exert important perturbations on it and on the planetary ecosystem in general. Consequently, much recent research focuses on the effects of human activities on the atmosphere and, through them, on the environment and Earth's climate. For these reasons consideration of the geochemistry of the atmosphere, and of atmospheric aerosols in particular, must include the effects of human activities. (201K)Figure 1. Impairment of visibility by aerosols. Photographs at Yosemite National Park, California, USA. (a) Low aerosol concentration (particulate matter of aerodynamic diameter less than 2.5 μm, PM2.5=0.3 μg m-3; particulate matter of aerodynamic diameter less than 10

  1. Determination of Aerosol Oxidative Activity using Silver Nanoparticle Aggregation on Paper-Based Analytical Devices

    PubMed Central

    Dungchai, Wijitar; Sameenoi, Yupaporn; Chailapakul, Orawon; Volckens, John; Henry, Charles S.

    2013-01-01

    Airborne particulate matter (PM) pollution significantly impacts human health, but the cellular mechanisms of PM-induced toxicity remain poorly understood. A leading hypothesis on the effects of inhaled PM involves the generation of cellular oxidative stress. To investigate PM-induced oxidative stress, analytical methods have been developed to study the chemical oxidation of dithiothreitol (DTT) in the presence of PM. Although DTT readily reacts with several forms of reactive oxygen species, this molecule is not endogenously produced in biological systems. Glutathione (GSH), on the other hand, is an endogenous antioxidant that is produced throughout the body and is directly involved in combating oxidative stress in the lungs and other tissues. We report here a new method for measuring aerosol oxidative activity that uses silver nanoparticle (AgNP) aggregation coupled to glutathione (GSH) oxidation in a paper-based analytical device. In this assay, the residual reduced GSH from the oxidation of reduced GSH to its disulfide induces the aggregation of AgNPs on a paper-based analytical device, which produces a reddish-brown product. Two methods for aerosol oxidative reactivity are presented: one based on change in color intensity using a traditional paper-based techniques and one based on the length of the color product formed using a distance-based device. These methods were validated against traditional spectroscopic assays for DTT and GSH that employ Elman’s reagent. No significant difference was found between the levels measured by all three GSH methods (our two paper-based devices and the traditional method) at the 95% confidence level. PM reactivity towards GSH was less than towards DTT most likely due to the difference in the oxidation potential between the two molecules. PMID:24067623

  2. 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

  3. Impacts of organic aerosols and its oxidation level on CCN activity from measurement at a suburban site in China

    NASA Astrophysics Data System (ADS)

    Zhang, Fang; Li, Zhanqing; Li, Yanan; Sun, Yele; Wang, Zhenzhu; Li, Ping; Sun, Li; Wang, Pucai; Cribb, Maureen; Zhao, Chuanfeng; Fan, Tianyi; Yang, Xin; Wang, Qingqing

    2016-05-01

    This study is concerned with the impacts of organic aerosols on cloud condensation nuclei (CCN) activity based on field measurements made at a suburban site in Northern China. The sensitivity of the estimated CCN number concentration (NCCN) to both volume fraction of organic material (xorg) and aerosol oxidation level (using f44, the fraction of m/z 44 in aerosol organic material) are examined. A strong dependence of CCN number concentration (NCCN) on the xorg and f44 was noted. The sensitivity of NCCN to volume fraction of organics increased with increasing xorg. The impacts of the aerosol particles oxidization or aging level on estimating NCCN were also very significant. When the particles were mostly composed of organics (xorg > 60 %), the NCCN at the supersaturation of 0.075 and 0.13 % was underestimated by 46 and 44 %, respectively, if aerosol particles were freshly emitted with primary organics (f44 < 11 %); the underestimation decreased to 32 and 23 % at the corresponding supersaturations, however, if the particles were with more hygroscopic secondary organics (f44 > 15 %). The NCCN at the supersaturation of 0.76 % was underestimated by 11 and 4 %, respectively, at f44 < 11 and f44 > 15 %. However, for the particles composed of low organics (e.g., xorg < 40 %), the effect caused by the f44 was quite insignificant both at high and low supersaturations. This is because the overall hygroscopicity of the particles is dominated by inorganics such as sulfate and nitrate, which are more hygroscopic than organic compounds. Our results indicated that it would decrease the uncertainties in estimating NCCN and lead to a more accurate estimation of NCCN to increase the proportion of secondary organics, especially when the composition of the aerosols is dominated by organics. The applicability of the CCN activation spectrum obtained at Xinzhou to the Xianghe site, about 400 km to the northeast of Xinzhou, was investigated, with the aim of further examining the

  4. Elastolytic activity in the lungs of rats exposed to cadmium aerosolization

    SciTech Connect

    Padmanabhan, R.V.; Gudapaty, S.R.; Liener, I.E.; Hoidal, J.R.

    1982-10-01

    Rats were exposed for 1 hr per day for up to 35 days to an aerosol of 0.1% cadmium chloride. At periodic intervals, animals were sacrificed and their lungs lavaged. The lung lavage fluid was examined for polymorphonuclear leukocytes (PMN) and alveolar macrophages (AM). A portion of the cells of the lavage fluid was lysed, and the remainder of the cells were cultured. The lavage fluids, cell lysates, and conditioned media were assayed for elastolytic activity in the presence and absence of a peptide chloromethyl ketone and EDTA. Exposure to cadmium evoked a biphasic cellular response characterized by an initial influx (1-3 days) of PMN followed by a gradual increase in AM. This biphasic cellular response was accompanied by a shift in the type of elastolytic activity which was present in the lung lavage and its cellular components. The initial PMN phase was accompanied by the enhanced production of an elastase inhibited only by the peptide chloromethyl ketone, while the subsequent AM phase was associated with an elastase activity which was inhibited only by EDTA. The possible implication of these results with respect to the pathogenesis of emphysema is considered.

  5. Performance of McRAS-AC in the GEOS-5 AGCM: Part 1, Aerosol-Activated Cloud Microphysics, Precipitation, Radiative Effects, and Circulation

    NASA Technical Reports Server (NTRS)

    Sud, Y. C.; Lee, D.; Oreopoulos, L.; Barahona, D.; Nenes, A.; Suarez, M. J.

    2012-01-01

    A revised version of the Microphysics of clouds with Relaxed Arakawa-Schubert and Aerosol-Cloud interaction (McRAS-AC), including, among others, the Barahona and Nenes ice nucleation parameterization, is implemented in the GEOS-5 AGCM. Various fields from a 10-year long integration of the AGCM with McRAS-AC were compared with their counterparts from an integration of the baseline GEOS-5 AGCM, and with satellite data as observations. Generally using McRAS-AC reduced biases in cloud fields and cloud radiative effects are much better over most of the regions of the Earth. Two weaknesses are identified in the McRAS-AC runs, namely, too few cloud particles around 40S-60S, and too high cloud water path during northern hemisphere summer over the Gulf Stream and North Pacific. Sensitivity analyses showed that these biases potentially originated from biases in the aerosol input. The first bias is largely eliminated in a sensitivity test using 50% smaller aerosol particles, while the second bias is much reduced when interactive aerosol chemistry was turned on. The main drawback of McRAS-AC is dearth of low-level marine stratus clouds, probably due to lack of dry-convection, not yet implemented into the cloud scheme. Despite these biases, McRAS-AC does simulate realistic clouds and their optical properties that can improve with better aerosol-input and thereby has the potential to be a valuable tool for climate modeling research because of its aerosol indirect effect simulation capabilities involving prediction of cloud particle number concentration and effective particle size for both convective and stratiform clouds is quite realistic.

  6. Spectroscopic investigations of organic aerosol and its reaction with halogens, released by sea-salt activation

    NASA Astrophysics Data System (ADS)

    Ofner, J.; Zetzsch, C.

    2009-04-01

    The release of reactive halogen species from sea-salt aerosol offers a class of reactants for heterogeneous reactions of utmost importance. These heterogeneous reactions have been overlooked so far, although they may occur with internal and external mixtures of sea-salt aerosol and organic aerosol or organic matter. Such reactions might constitute sources of gaseous organohalogen compounds or halogenated organic aerosol in the atmospheric boundary layer. Infrared and UV/VIS spectroscopy provide an insight into chemical processes at reactive sites of the organic phase on a molecular level. Model studies of heterogeneous reactions of halogens with different kinds of (secondary) organic aerosols and organic matter were performed using a 700L smog chamber with a solar simulator. The model compounds alpha-pinene, catechol and humic acid have been chosen as precursors/material for the condensed, organic phase of the aerosol. After formation of the secondary organic aerosol or preparation of the organic material and the sea-salt solution the reaction was carried out using molecular chlorine and bromine in the presence of simulated sunlight. Chemical transformation of the organic material was studied using attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR) on a ZnSe crystal and diffuse reflectance UV/VIS spectroscopy. An electrostatic precipitator was developed to deposit the aerosol particles on the ATR crystal as a thin film. On the other hand, longpath-FTIR spectroscopy with a 40m White-cell allows us to monitor both the condensed and gas phase of the aerosol in situ in the smog chamber directly. These spectroscopic techniques enable us to characterize different organic aerosol particles and their functional groups at reactive sites on these particles as well as to study aerosol formation and transformation directly. The heterogeneous reaction of reactive halogen species with organic material at atmospheric conditions leads to small reactive

  7. The effects of aerosol on development of thunderstorm electrification: A numerical study

    NASA Astrophysics Data System (ADS)

    Zhao, Pengguo; Yin, Yan; Xiao, Hui

    2015-02-01

    The effects of aerosol on electrification of an idealized supercell storm are investigated using the Weather Research and Forecasting model coupled with electrification and discharge parameterizations and an explicit treatment of aerosol activation. It is found that the microphysical and electric processes of the thunderstorm are distinctly different under different aerosol background. Enhancing aerosol loading increases growth rate of snow and graupel particles, and leads to higher concentration of ice particles. Increasing aerosol concentration also results in enhancement in electrification process, due to more ice particles participating in the electrification process in the polluted case. In the clean case, the charge structure maintained dipolarity throughout the simulation, while in the polluted case the charge structure transformed from dipolarity at the initial stage of charging separation to the structure of a negative charge region above the main positive and the main negative charge centers at the later stage. A detailed analysis of the microphysical processes shows that increasing aerosol loading led to more liquid water content and higher rime accretion rate above the freezing level, which was in favor of graupel charge positively and ice crystal and snow charge negatively in this region. In a word, increasing aerosol loading leads to increased cloud water content, resulting in a new negative charge region developed above the main positive charge center.

  8. Aerosol-Radiation-Cloud Interactions in the South-East Atlantic: Future Suborbital Activities to Address Knowledge Gaps in Satellite and Model Assessments

    NASA Technical Reports Server (NTRS)

    Redemann, Jens; Wood, R.; Zuidema, P.; Haywood, J.; Piketh, S.; Formenti, P.; L'Ecuyer, T.; Kacenelenbogen, M.; Segal-Rosenheimer, M.; Shinozuka, Y.; LeBlanc, S.; Vaughan, M.; Schmidt, S.; Flynn, C.; Schmid, B.; Luna, B.; Abel, S.

    2016-01-01

    Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles. Particles lofted into the mid-troposphere are transported westward over the South-East (SE) Atlantic, home to one of the three permanent subtropical stratocumulus (Sc) cloud decks in the world. The SE Atlantic stratocumulus deck interacts with the dense layers of BB aerosols that initially overlay the cloud deck, but later subside and may mix into the clouds. These interactions include adjustments to aerosol-induced solar heating and microphysical effects, and their global representation in climate models remains one of the largest uncertainties in estimates of future climate. Hence, new observations over the SE Atlantic have significant implications for global climate change scenarios. Our understanding of aerosol-cloud interactions in the SE Atlantic is hindered both by the lack of knowledge on aerosol and cloud properties, as well as the lack of knowledge about detailed physical processes involved. Most notably, we are missing knowledge on the absorptive and cloud nucleating properties of aerosols, including their vertical distribution relative to clouds, on the locations and degree of aerosol mixing into clouds, on the processes that govern cloud property adjustments, and on the importance of aerosol effects on clouds relative to co-varying synoptic scale meteorology. We discuss the current knowledge of aerosol and cloud property distributions based on satellite observations and sparse suborbital sampling. Recent efforts to make full use of A-Train aerosol sensor synergies will be highlighted. We describe planned field campaigns in the region to address the existing knowledge gaps. Specifically, we describe the scientific objectives and implementation of the five synergistic, international research activities aimed at providing some of the key aerosol and cloud properties and a process-level understanding of aerosol-cloud interactions over the SE Atlantic: NASA

  9. Sensitivity Studies on the Influence of Aerosols on Cloud and Precipitation Development Using WRF Mesoscale Model Simulations

    NASA Astrophysics Data System (ADS)

    Thompson, G.; Eidhammer, T.; Rasmussen, R.

    2011-12-01

    Using the WRF model in simulations of shallow and deep precipitating cloud systems, we investigated the sensitivity to aerosols initiating as cloud condensation and ice nuclei. A global climatological dataset of sulfates, sea salts, and dust was used as input for a control experiment. Sensitivity experiments with significantly more polluted conditions were conducted to analyze the resulting impacts to cloud and precipitation formation. Simulations were performed using the WRF model with explicit treatment of aerosols added to the Thompson et al (2008) bulk microphysics scheme. The modified scheme achieves droplet formation using pre-tabulated CCN activation tables provided by a parcel model. The ice nucleation is parameterized as a function of dust aerosols as well as homogeneous freezing of deliquesced aerosols. The basic processes of aerosol activation and removal by wet scavenging are considered, but aerosol characteristic size or hygroscopicity does not change due to evaporating droplets. In other words, aerosol processing was ignored. Unique aspects of this study include the usage of one to four kilometer grid spacings and the direct parameterization of ice nucleation from aerosols rather than typical temperature and/or supersaturation relationships alone. Initial results from simulations of a deep winter cloud system and its interaction with significant orography show contrasting sensitivities in regions of warm rain versus mixed liquid and ice conditions. The classical view of higher precipitation amounts in relatively clean maritime clouds with fewer but larger droplets is confirmed for regions dominated by the warm-rain process. However, due to complex interactions with the ice phase and snow riming, the simulations revealed the reverse situation in high terrain areas dominated by snow reaching the surface. Results of other cloud systems will be summarized at the conference.

  10. Fabrication of a metal membrane on a perforated polymer substrate by palladium aerosol activation and subsequent electroless plating.

    PubMed

    Byeon, Jeong Hoon; Hwang, Jungho

    2009-02-01

    Fabrication of a metal membrane on a perforated flexible poly(tetrafluoroethylene) (PTFE) substrate was developed by employing spark-generated palladium (Pd) aerosol activation and the subsequent electroless plating of Pd. After aerosol activation, Pd agglomerates of spark-generated primary particles (approximately 2.6 nm in diameter) with a face-centered-cubic structure were deposited uniformly on the PTFE substrate. Homogeneous Pd particles with an average size of 188 nm were tightly packed together to form a Pd membrane after Pd plating. The average plating rate of Pd during 30 min of plating at an activation intensity of 25 microg/cm(2) was 14.2 microg/cm(2) x min. PMID:20353212

  11. Parameterized Beyond-Einstein Growth

    SciTech Connect

    Linder, Eric; Linder, Eric V.; Cahn, Robert N.

    2007-09-17

    A single parameter, the gravitational growth index gamma, succeeds in characterizing the growth of density perturbations in the linear regime separately from the effects of the cosmic expansion. The parameter is restricted to a very narrow range for models of dark energy obeying the laws of general relativity but can take on distinctly different values in models of beyond-Einstein gravity. Motivated by the parameterized post-Newtonian (PPN) formalism for testing gravity, we analytically derive and extend the gravitational growth index, or Minimal Modified Gravity, approach to parameterizing beyond-Einstein cosmology. The analytic formalism demonstrates how to apply the growth index parameter to early dark energy, time-varying gravity, DGP braneworld gravity, and some scalar-tensor gravity.

  12. Aerosol typing - key information from aerosol studies

    NASA Astrophysics Data System (ADS)

    Mona, Lucia; Kahn, Ralph; Papagiannopoulos, Nikolaos; Holzer-Popp, Thomas; Pappalardo, Gelsomina

    2016-04-01

    Aerosol typing is a key source of aerosol information from ground-based and satellite-borne instruments. Depending on the specific measurement technique, aerosol typing can be used as input for retrievals or represents an output for other applications. Typically aerosol retrievals require some a priori or external aerosol type information. The accuracy of the derived aerosol products strongly depends on the reliability of these assumptions. Different sensors can make use of different aerosol type inputs. A critical review and harmonization of these procedures could significantly reduce related uncertainties. On the other hand, satellite measurements in recent years are providing valuable information about the global distribution of aerosol types, showing for example the main source regions and typical transport paths. Climatological studies of aerosol load at global and regional scales often rely on inferred aerosol type. There is still a high degree of inhomogeneity among satellite aerosol typing schemes, which makes the use different sensor datasets in a consistent way difficult. Knowledge of the 4d aerosol type distribution at these scales is essential for understanding the impact of different aerosol sources on climate, precipitation and air quality. All this information is needed for planning upcoming aerosol emissions policies. The exchange of expertise and the communication among satellite and ground-based measurement communities is fundamental for improving long-term dataset consistency, and for reducing aerosol type distribution uncertainties. Aerosol typing has been recognized as one of its high-priority activities of the AEROSAT (International Satellite Aerosol Science Network, http://aero-sat.org/) initiative. In the AEROSAT framework, a first critical review of aerosol typing procedures has been carried out. The review underlines the high heterogeneity in many aspects: approach, nomenclature, assumed number of components and parameters used for the

  13. Double-moment cloud microphysics scheme for the deep convection parameterization in the GFDL AM3

    NASA Astrophysics Data System (ADS)

    Belochitski, A.; Donner, L.

    2014-12-01

    A double-moment cloud microphysical scheme originally developed by Morrision and Gettelman (2008) for the stratiform clouds and later adopted for the deep convection by Song and Zhang (2011) has been implemented in to the Geophysical Fluid Dynamics Laboratory's atmospheric general circulation model AM3. The scheme treats cloud drop, cloud ice, rain, and snow number concentrations and mixing ratios as diagnostic variables and incorporates processes of autoconversion, self-collection, collection between hydrometeor species, sedimentation, ice nucleation, drop activation, homogeneous and heterogeneous freezing, and the Bergeron-Findeisen process. Such detailed representation of microphysical processes makes the scheme suitable for studying the interactions between aerosols and convection, as well as aerosols' indirect effects on clouds and their roles in climate change. The scheme is first tested in the single column version of the GFDL AM3 using forcing data obtained at the U.S. Department of Energy Atmospheric Radiation Measurment project's Southern Great Planes site. Scheme's impact on SCM simulations is discussed. As the next step, runs of the full atmospheric GCM incorporating the new parameterization are compared to the unmodified version of GFDL AM3. Global climatological fields and their variability are contrasted with those of the original version of the GCM. Impact on cloud radiative forcing and climate sensitivity is investigated.

  14. The predictive consequences of parameterization

    NASA Astrophysics Data System (ADS)

    White, J.; Hughes, J. D.; Doherty, J. E.

    2013-12-01

    In numerical groundwater modeling, parameterization is the process of selecting the aspects of a computer model that will be allowed to vary during history matching. This selection process is dependent on professional judgment and is, therefore, inherently subjective. Ideally, a robust parameterization should be commensurate with the spatial and temporal resolution of the model and should include all uncertain aspects of the model. Limited computing resources typically require reducing the number of adjustable parameters so that only a subset of the uncertain model aspects are treated as estimable parameters; the remaining aspects are treated as fixed parameters during history matching. We use linear subspace theory to develop expressions for the predictive error incurred by fixing parameters. The predictive error is comprised of two terms. The first term arises directly from the sensitivity of a prediction to fixed parameters. The second term arises from prediction-sensitive adjustable parameters that are forced to compensate for fixed parameters during history matching. The compensation is accompanied by inappropriate adjustment of otherwise uninformed, null-space parameter components. Unwarranted adjustment of null-space components away from prior maximum likelihood values may produce bias if a prediction is sensitive to those components. The potential for subjective parameterization choices to corrupt predictions is examined using a synthetic model. Several strategies are evaluated, including use of piecewise constant zones, use of pilot points with Tikhonov regularization and use of the Karhunen-Loeve transformation. The best choice of parameterization (as defined by minimum error variance) is strongly dependent on the types of predictions to be made by the model.

  15. Recursive Abstractions for Parameterized Systems

    NASA Astrophysics Data System (ADS)

    Jaffar, Joxan; Santosa, Andrew E.

    We consider a language of recursively defined formulas about arrays of variables, suitable for specifying safety properties of parameterized systems. We then present an abstract interpretation framework which translates a paramerized system as a symbolic transition system which propagates such formulas as abstractions of underlying concrete states. The main contribution is a proof method for implications between the formulas, which then provides for an implementation of this abstract interpreter.

  16. The Impact of Atmospheric Aerosols on the Fraction of absorbed Photosynthetically Active Radiation

    NASA Astrophysics Data System (ADS)

    Veroustraete, Frank

    2010-05-01

    Aerosol pollution attracts a growing interest from atmospheric scientists with regard to their impact on health, the global climate and vegetation stress. A hypothesis, less investigated, is whether atmospheric aerosol interactions in the solar radiation field affect the amount of radiation absorbed by vegetation canopies and hence terrestrial vegetation productivity. Typically, aerosols affect vegetation canopy radiation absorption efficiency by altering the physical characteristics of solar radiation incoming on for example a forest canopy. It has been illustrated, that increasing mixing ratio's of atmospheric particulate matter lead to a higher fraction of diffuse sunlight as opposed to direct sunlight. It can be demonstrated, based on the application of atmospheric (MODTRAN) and leaf/canopy radiative transfer (LIBERTY/SPRINT) models, that radiation absorption efficiency in the PAR band of Picea like forests increases with increasing levels of diffuse radiation. It can be documented - on a theoretical basis - as well, that increasing aerosol loads in the atmosphere, induce and increased canopy PAR absorption efficiency. In this paper it is suggested, that atmospheric aerosols have to be taken into account when estimating vegetation gross primary productivity (GPP). The results suggest that Northern hemisphere vegetation CO2 uptake magnitude may increase with increasing atmospheric aerosol loads. Many climate impact scenario's related to vegetation productivity estimates, do not take this phenomenon into account. Boldly speaking, the results suggest a larger sink function for terrestrial vegetation than generally accepted. Keywords: Aerosols, vegetation, fAPAR, CO2 uptake, diffuse radiation.

  17. An inexpensive active optical remote sensing instrument for assessing aerosol distributions.

    PubMed

    Barnes, John E; Sharma, Nimmi C P

    2012-02-01

    Air quality studies on a broad variety of topics from health impacts to source/sink analyses, require information on the distributions of atmospheric aerosols over both altitude and time. An inexpensive, simple to implement, ground-based optical remote sensing technique has been developed to assess aerosol distributions. The technique, called CLidar (Charge Coupled Device Camera Light Detection and Ranging), provides aerosol altitude profiles over time. In the CLidar technique a relatively low-power laser transmits light vertically into the atmosphere. The transmitted laser light scatters off of air molecules, clouds, and aerosols. The entire beam from ground to zenith is imaged using a CCD camera and wide-angle (100 degree) optics which are a few hundred meters from the laser. The CLidar technique is optimized for low altitude (boundary layer and lower troposphere) measurements where most aerosols are found and where many other profiling techniques face difficulties. Currently the technique is limited to nighttime measurements. Using the CLidar technique aerosols may be mapped over both altitude and time. The instrumentation required is portable and can easily be moved to locations of interest (e.g. downwind from factories or power plants, near highways). This paper describes the CLidar technique, implementation and data analysis and offers specifics for users wishing to apply the technique for aerosol profiles. PMID:22442935

  18. Aerosol Gemcitabine: Preclinical Safety and In Vivo Antitumor Activity in Osteosarcoma-Bearing Dogs

    PubMed Central

    Crabbs, Torrie A.; Wilson, Dennis W.; Cannan, Virginia A.; Skorupski, Katherine A.; Gordon, Nancy; Koshkina, Nadya; Kleinerman, Eugenie; Anderson, Peter M.

    2010-01-01

    Abstract Background Osteosarcoma is the most common skeletal malignancy in the dog and in young humans. Although chemotherapy improves survival time, death continues to be attributed to metastases. Aerosol delivery can provide a strategy with which to improve the lung drug delivery while reducing systemic toxicity. The purpose of this study is to assess the safety of a regional aerosol approach to chemotherapy delivery in osteosarcoma-bearing dogs, and second, to evaluate the effect of gemcitabine on Fas expression in the pulmonary metastasis. Methods We examined the systemic and local effects of aerosol gemcitabine on lung and pulmonary metastasis in this relevant large-animal tumor model using serial laboratory and arterial blood gas analysis and histopathology and immunohistochemistry, respectively. Results and Conclusions Six hundred seventy-two 1-h doses of aerosol gemcitabine were delivered. The treatment was well tolerated by these subjects with osteosarcoma (n = 20). Aerosol-treated subjects had metastatic foci that demonstrated extensive, predominately central, intratumoral necrosis. Fas expression was decreased in pulmonary metastases compared to the primary tumor (p = 0.008). After aerosol gemcitabine Fas expression in the metastatic foci was increased compared to lung metastases before treatment (p = 0.0075), and even was higher than the primary tumor (p = 0.025). Increased apoptosis (TUNEL) staining was also detected in aerosol gemcitabine treated metastasis compared to untreated controls (p = 0.028). The results from this pivotal translational study support the concept that aerosol gemcitabine may be useful against pulmonary metastases of osteosarcoma. Additional studies that evaluate the aerosol route of administration of gemcitabine in humans should be safe and are warranted. PMID:19803732

  19. Effect of an activated sludge wastewater treatment plant on ambient air densities of aerosols containing bacteria and viruses.

    PubMed

    Fannin, K F; Vana, S C; Jakubowski, W

    1985-05-01

    Bacteria- and virus-containing aerosols were studied during the late summer and fall seasons in a midwestern suburb of the United States before and during the start-up and operation of an unenclosed activated sludge wastewater treatment plant. The study showed that the air in this suburban area contained low-level densities of indicator microorganisms. After the plant began operating, the densities of total aerobic bacteria-containing particles, standard plate count bacteria, total coliforms, fecal coliforms, fecal streptococci, and coliphages increased significantly in the air within the perimeter of the plant. Before plant operations, bacteria were detected from five genera, Klebsiella, Enterobacter, Serratia, Salmonella, and Aeromonas. During plant operations, the number of genera identified increased to 11. In addition to those genera found before plant operations, Escherichia, Providencia, Citrobacter, Acinetobacter, Pasteurella, and Proteus, were also identified. Enteric viruses were detected in low densities from the air emissions of this plant. Only standard plate count bacteria remained at significantly higher than base-line densities beyond 250 m downwind from the center of the aeration tanks. Fecal streptococci and coliphages appeared to be more stable in aerosols than the other indicator microorganisms studied. In general, the densities of microorganism-containing aerosols were higher at night than during the day. The techniques used in this study may be employed to establish microorganism-containing aerosol exposure during epidemiological investigations. PMID:2988442

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

    NASA Astrophysics Data System (ADS)

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

    2014-05-01

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

  1. Cloud condensation nuclei in polluted air and biomass burning smoke near the mega-city Guangzhou, China - Part 1: Size-resolved measurements and implications for the modeling of aerosol particle hygroscopicity and CCN activity

    NASA Astrophysics Data System (ADS)

    Rose, D.; Nowak, A.; Achtert, P.; Wiedensohler, A.; Hu, M.; Shao, M.; Zhang, Y.; Andreae, M. O.; Pöschl, U.

    2010-04-01

    individual CCN efficiency spectra, the relative deviations were on average less than ~10% and hardly exceeded 20%, confirming the applicability of the κ-Köhler model approach for efficient description of the CCN activity of atmospheric aerosols. Note, however, that different types of κ-parameters must be distinguished for external mixtures of CCN-active and -inactive aerosol particles (κa, κt, κcut). Using a constant average hygroscopicity parameter (κ=0.3) and variable size distributions as measured, the deviations between observed and predicted CCN concentrations were on average less than 20%. In contrast, model calculations using variable hygroscopicity parameters as measured and constant size distributions led to much higher deviations: ~70% for the campaign average size distribution, ~80% for a generic rural size distribution, and ~140% for a generic urban size distribution. These findings confirm earlier studies suggesting that aerosol particle number and size are the major predictors for the variability of the CCN concentration in continental boundary layer air, followed by particle composition and hygroscopicity as relatively minor modulators. Depending on the required and applicable level of detail, the information and parameterizations presented in this study should enable efficient description of the CCN activity of atmospheric aerosols in detailed process models as well as in large-scale atmospheric and climate models.

  2. A Solar Radiation Parameterization for Atmospheric Studies. Volume 15

    NASA Technical Reports Server (NTRS)

    Chou, Ming-Dah; Suarez, Max J. (Editor)

    1999-01-01

    The solar radiation parameterization (CLIRAD-SW) developed at the Goddard Climate and Radiation Branch for application to atmospheric models are described. It includes the absorption by water vapor, O3, O2, CO2, clouds, and aerosols and the scattering by clouds, aerosols, and gases. Depending upon the nature of absorption, different approaches are applied to different absorbers. In the ultraviolet and visible regions, the spectrum is divided into 8 bands, and single O3 absorption coefficient and Rayleigh scattering coefficient are used for each band. In the infrared, the spectrum is divided into 3 bands, and the k-distribution method is applied for water vapor absorption. The flux reduction due to O2 is derived from a simple function, while the flux reduction due to CO2 is derived from precomputed tables. Cloud single-scattering properties are parameterized, separately for liquid drops and ice, as functions of water amount and effective particle size. A maximum-random approximation is adopted for the overlapping of clouds at different heights. Fluxes are computed using the Delta-Eddington approximation.

  3. Surface fractal dimension, water adsorption efficiency, and cloud nucleation activity of insoluble aerosol.

    PubMed

    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

  4. Surface fractal dimension, water adsorption efficiency, and cloud nucleation activity of insoluble aerosol

    NASA Astrophysics Data System (ADS)

    Laaksonen, Ari; Malila, Jussi; Nenes, Athanasios; Hung, Hui-Ming; Chen, Jen-Ping

    2016-05-01

    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.

  5. 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

  6. 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.

  7. An Energetic Perspective on Aerosol Radiative Forcing and Interactions with Atmospheric Wave Activity

    NASA Astrophysics Data System (ADS)

    Hosseinpour, F.; Wilcox, E. M.; Colarco, P. R.

    2014-12-01

    Aerosols have the capability to alter regional-scale atmospheric circulations. A better understanding of the contribution of aerosols to multi-scale atmospheric phenomena and their transient changes is crucial for efforts to evaluate climate predictions using next generation climate models. In this study we address the following questions: (1) Is there a mechanistic relationship between variability of oceanic dust aerosol forcing and transient changes in the African easterly jet- African easterly wave (AEJ-AEW) system? (2) What are the long-term impacts of possible aerosol-wave interactions on climate dynamics of eastern tropical Atlantic Ocean and western African monsoon (WAM) region during boreal summer seasons? Our hypothesis is that aerosol radiative forcing may act as additional energy source to fuel the development of African easterly waves on the northern and southern sides of the AEJ. Evidence in support of this hypothesis is presented based on analysis of an ensemble of NASA satellite data sets, including aerosol optical thickness (AOT) observations from the Moderate Resolution Imaging Spectro-radiometer (MODIS) and the Sea-Viewing Wide Field-of-View Sensor (SeaWiFS), as well as an atmospheric reanalysis from the Modern-Era Retrospective Analysis for Research and Applications (MERRA) and a simulation of global aerosol distributions made with the Goddard Earth Observing System Model version 5 (GEOS-5) Earth system model with meteorology constrained by MERRA and an assimilation of MODIS AOT (MERRAero). We propose that the impacts of Saharan aerosols on the regional climate dynamics occur through contributions to the eddy energy of waves with 2—7-day and 7—11-day variability.

  8. Chemical and physical influences on aerosol activation in liquid clouds: a study based on observations from the Jungfraujoch, Switzerland

    SciTech Connect

    Hoyle, Christopher R.; Webster, Clare S.; Rieder, Harald E.; Nenes, Athanasios; Hammer, Emanuel; Herrmann, Erik; Gysel, Martin; Bukowiecki, Nicolas; Weingartner, Ernest; Steinbacher, Martin; Baltensperger, Urs

    2016-01-01

    A simple statistical model to predict the number of aerosols which activate to form cloud droplets in warm clouds has been established, based on regression analysis of data from four summertime Cloud and Aerosol Characterisation Experiments (CLACE) at the high-altitude site Jungfraujoch (JFJ). It is shown that 79 % of the observed variance in droplet numbers can be represented by a model accounting only for the number of potential cloud condensation nuclei (defined as number of particles larger than 80 nm in diameter), while the mean errors in the model representation may be reduced by the addition of further explanatory variables, such as the mixing ratios of O3, CO, and the height of the measurements above cloud base. The statistical model has a similar ability to represent the observed droplet numbers in each of the individual years, as well as for the two predominant local wind directions at the JFJ (northwest and southeast). Given the central European location of the JFJ, with air masses in summer being representative of the free troposphere with regular boundary layer in-mixing via convection, we expect that this statistical model is generally applicable to warm clouds under conditions where droplet formation is aerosol limited (i.e. at relatively high updraught velocities and/or relatively low aerosol number concentrations). A comparison between the statistical model and an established microphysical parametrization shows good agreement between the two and supports the conclusion that cloud droplet formation at the JFJ is predominantly controlled by the number concentration of aerosol particles.

  9. Chemical and physical influences on aerosol activation in liquid clouds: a study based on observations from the Jungfraujoch, Switzerland

    NASA Astrophysics Data System (ADS)

    Hoyle, Christopher R.; Webster, Clare S.; Rieder, Harald E.; Nenes, Athanasios; Hammer, Emanuel; Herrmann, Erik; Gysel, Martin; Bukowiecki, Nicolas; Weingartner, Ernest; Steinbacher, Martin; Baltensperger, Urs

    2016-03-01

    A simple statistical model to predict the number of aerosols which activate to form cloud droplets in warm clouds has been established, based on regression analysis of data from four summertime Cloud and Aerosol Characterisation Experiments (CLACE) at the high-altitude site Jungfraujoch (JFJ). It is shown that 79 % of the observed variance in droplet numbers can be represented by a model accounting only for the number of potential cloud condensation nuclei (defined as number of particles larger than 80 nm in diameter), while the mean errors in the model representation may be reduced by the addition of further explanatory variables, such as the mixing ratios of O3, CO, and the height of the measurements above cloud base. The statistical model has a similar ability to represent the observed droplet numbers in each of the individual years, as well as for the two predominant local wind directions at the JFJ (northwest and southeast). Given the central European location of the JFJ, with air masses in summer being representative of the free troposphere with regular boundary layer in-mixing via convection, we expect that this statistical model is generally applicable to warm clouds under conditions where droplet formation is aerosol limited (i.e. at relatively high updraught velocities and/or relatively low aerosol number concentrations). A comparison between the statistical model and an established microphysical parametrization shows good agreement between the two and supports the conclusion that cloud droplet formation at the JFJ is predominantly controlled by the number concentration of aerosol particles.

  10. Chemical and physical influences on aerosol activation in liquid clouds: a study based on observations from the Jungfraujoch, Switzerland

    DOE PAGESBeta

    Hoyle, Christopher R.; Webster, Clare S.; Rieder, Harald E.; Nenes, Athanasios; Hammer, Emanuel; Herrmann, Erik; Gysel, Martin; Bukowiecki, Nicolas; Weingartner, Ernest; Steinbacher, Martin; et al

    2016-03-29

    In this study, a simple statistical model to predict the number of aerosols which activate to form cloud droplets in warm clouds has been established, based on regression analysis of data from four summertime Cloud and Aerosol Characterisation Experiments (CLACE) at the high-altitude site Jungfraujoch (JFJ). It is shown that 79 % of the observed variance in droplet numbers can be represented by a model accounting only for the number of potential cloud condensation nuclei (defined as number of particles larger than 80 nm in diameter), while the mean errors in the model representation may be reduced by the additionmore » of further explanatory variables, such as the mixing ratios of O3, CO, and the height of the measurements above cloud base. The statistical model has a similar ability to represent the observed droplet numbers in each of the individual years, as well as for the two predominant local wind directions at the JFJ (northwest and southeast). Given the central European location of the JFJ, with air masses in summer being representative of the free troposphere with regular boundary layer in-mixing via convection, we expect that this statistical model is generally applicable to warm clouds under conditions where droplet formation is aerosol limited (i.e. at relatively high updraught velocities and/or relatively low aerosol number concentrations). Finally, a comparison between the statistical model and an established microphysical parametrization shows good agreement between the two and supports the conclusion that cloud droplet formation at the JFJ is predominantly controlled by the number concentration of aerosol particles.« less

  11. The Measurement and Parameterization of Effective Radius of Droplets in Warm Stratocumulus Clouds.

    NASA Astrophysics Data System (ADS)

    Martin, G. M.; Johnson, D. W.; Spice, A.

    1994-07-01

    Observations from the Meteorological Research Flight's Hercules C-130 aircraft of the microphysical characteristics of warm stratocumulus clouds have been analyzed to investigate the variation of the effective radius of cloud droplets in layer clouds. Results from experiments in the eastern Pacific, South Atlantic, subtropical regions of the North Atlantic, and the sea areas around the British Isles are presented. In situations where entrainment effects are small the (effective radius)3 is found to be a linear function of the (volume-averaged radius)3 in a given cloud and can thus be parameterized with respect to the liquid water content and the droplet number concentration in the cloud. However, the shape of the droplet size spectrum is very dependent on the cloud condensation nuclei (CCN) characteristics below cloud base, and the relationship between effective radius and volume-averaged radius varies between maritime air masses and continental air masses. This study also details comparisons that have been made in stratocumulus between the droplet number concentrations and (a) aerosol concentrations below cloud base in the size range 0.1 to 3.0 m and (b) CCN supersaturation spectra in the boundary layer. A parameterization relating droplet concentration and aerosol concentration is suggested. The effects of nonadiabatic processes on the parameterization of effective radius are discussed. Drizzle is found to have little effect near cloud top, but in precipitating stratocumulus clouds the parameterization breaks down near cloud base. Comparisons are made between this parameterization of effective radius and others used currently or in the past.

  12. The thermodynamic and kinetic impacts of organics on marine aerosols

    NASA Astrophysics Data System (ADS)

    Crahan, Kathleen

    Organics can change the manner in which aerosols scatter radiation directly as hydrated aerosols and indirectly as in-cloud activated aerosols, through changing the solution activity, the surface tension, and the accommodation coefficient of the hydrated aerosol. This work explores the kinetic and thermodynamic impacts of the organic component of marine aerosols through data collected over four field campaigns and through several models used to reproduce observations. The Rough Evaporation Duct (RED) project was conducted in the summer of 2001 off the coast of Oahu using the Twin Otter Aircraft and the Floating Instrument Platform research platform for data collection. The Cloud-Aerosol Research in the Marine Atmosphere (CARMA) campaigns were conducted over three summers (2002, 2004, 2005) off the coast of Monterey, California. During the CARMA campaigns, a thick, moist, stratocumulus deck was present during most days, and the Twin Otter Aircraft was the primary research platform used to collect data. However, the research goals and exact instrumentation onboard the Twin Otter varied from campaign to campaign, and each data set was analyzed individually. Data collected from CARMA I were used to explore the mechanism of oxalic acid production in cloud droplets. Oxalate was observed in the clouds in excess to below cloud concentrations by an average of 0.11 mug m-3, suggesting an in-cloud production. The tentative identification in cloud water of an intermediate species in the aqueous oxalate production mechanism lends further support to an in-cloud oxalate source. The data sets collected during the RED campaign and the CARMA II and CARMA III campaigns were used to investigate the impact of aerosol chemical speciation on aerosol hygroscopic behavior. Several models were used to correlate the observations in the subsaturated regime to theory including an explicit thermodynamic model, simple Kohler theory, and a parameterization of the solution activity. These models

  13. Impacts Of Radiatively-Active Aerosols On Mars’ Current Climate: Simulation Results With The NASA ARC Mars GCM

    NASA Astrophysics Data System (ADS)

    Hollingsworth, Jeffery L.; Kahre, M. A.; Haberle, R. M.; Montmessin, F.; Herin, B.; Laamoumi, F.; Wilson, R. J.; Schaeffer, J.

    2010-10-01

    Recent upgrades to the NASA Ames Research Center (ARC) Mars general circulation model (GCM) include a fundamentally new and modernized radiative transfer package which permits radiative effects and interactions of suspended atmospheric aerosols (e.g., water ice clouds, water vapor, dust, and their mutual interactions) to influence the net diabatic heating rate within the atmosphere. Such aerosols are critically important in determining the nature of atmospheric thermal structure and hence the overall climate of the planet. Our Mars GCM simulations indicate that radiatively-active water ice clouds profoundly affect the seasonal and annual mean climate in a variety of ways. In particular, preliminary results suggest that the bulk thermal structure and resultant (i.e., balanced) circulation patterns are strongly modified near the surface and aloft. Generally speaking, we find a bulk warming of the atmosphere in upper layers, a cooling of the atmosphere in the lower and near-surface regions, and, increases in the mean pole-to-equator temperature contrasts (i.e., stronger mean polar vortices). A variety of results from our baseline and control simulations (i.e., where the radiative/physical effects are examined in isolation and when combined) will be presented. Comparisons with MGS/TES and MRO/MCS measurements indicate better agreement between the model's simulated climate compared to that observed. Using a state-of-the-art Mars GCM, these results highlight important effects radiatively-active aerosols have on physical and dynamical processes active in the current climate of Mars.

  14. Anionic, Cationic, and Nonionic Surfactants in Atmospheric Aerosols from the Baltic Coast at Askö, Sweden: Implications for Cloud Droplet Activation.

    PubMed

    Gérard, Violaine; Nozière, Barbara; Baduel, Christine; Fine, Ludovic; Frossard, Amanda A; Cohen, Ronald C

    2016-03-15

    Recent analyses of atmospheric aerosols from different regions have demonstrated the ubiquitous presence of strong surfactants and evidenced surface tension values, σ, below 40 mN m(-1), suspected to enhance the cloud-forming potential of these aerosols. In this work, this approach was further improved and combined with absolute concentration measurements of aerosol surfactants by colorimetric titration. This analysis was applied to PM2.5 aerosols collected at the Baltic station of Askö, Sweden, from July to October 2010. Strong surfactants were found in all the sampled aerosols, with σ = (32-40) ± 1 mN m(-1) and concentrations of at least 27 ± 6 mM or 104 ± 21 pmol m(-3). The absolute surface tension curves and critical micelle concentrations (CMC) determined for these aerosol surfactants show that (1) surfactants are concentrated enough in atmospheric particles to strongly depress the surface tension until activation, and (2) the surface tension does not follow the Szyszkowski equation during activation but is nearly constant and minimal, which provides new insights on cloud droplet activation. In addition, both the CMCs determined and the correlation (R(2) ∼ 0.7) between aerosol surfactant concentrations and chlorophyll-a seawater concentrations suggest a marine and biological origin for these compounds. PMID:26895279

  15. Aerosol and Trace Gas Processing by Clouds During the Cumulus Humilis Aerosol Processing Study (CHAPS)

    NASA Astrophysics Data System (ADS)

    Yu, X.; Berg, L.; Berkowitz, C.; Alexander, L.; Lee, Y.; Ogren, J.; Andrews, B.

    2008-12-01

    Clouds play an active role in the processing and cycling of atmospheric constituents. Gases and particles can partition to cloud droplets by absorption and condensation as well as activation and pact scavenging. The Cumulus Humilis Aerosol Processing Study (CHAPS) aimed at characterizing freshly emitted aerosols above, within and below fields of cumulus humilis (or fair-weather cumulus) in the vicinity of Oklahoma City. The experiment took place in June 2007. Evolution of aerosol and cloud properties downwind of the Oklahoma City is of particular interest in this project. These observations of a mid-size and mid-latitude city can be used in the development and evaluation of regional-scale and global climate model cumulus parameterizations that describes the transport and transformations of these aerosols by fair-weather cumulus. The Department of Energy (DOE) G-1 aircraft was one of the main platforms used in CHAPS. It carried a suite of instruments to measure properties of interstitial aerosols behind an isokinetic inlet and a set of duplicate instruments to determine properties of activated particles behind a counter-flow virtual impactor (CVI). The sampling line to the Aerodyne Aerosol Mass Spectrometer was switched between the isokinetic inlet and the CVI to allow characterization of interstitial particles out of clouds in contrast to particles activated in clouds. Trace gases including ozone, carbon monoxide, sulfur dioxide, and a series of volatile organic compounds (VOCs) were also measured as were key meteorological state parameters including liquid water content, cloud drop size, and dew point temperature were measured. This presentation will focus on results related to the transformation and transport of aerosols and trace gases observed in fair-weather cumulus and compare these results with concurrent observations made outside these clouds. Our interest will focus on the differences in particle size and composition under varying conditions. The role of

  16. Chemical aging of single and multicomponent biomass burning aerosol surrogate particles by OH: implications for cloud condensation nucleus activity

    DOE PAGESBeta

    Slade, J. H.; Thalman, R.; Wang, J.; Knopf, D. A.

    2015-09-14

    Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low-soluble single-component OA by OH and O3 can increase their water solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate particles exposed tomore » OH and O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH and O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~ 0.1, indicating that chemically aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH-exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions

  17. Chemical aging of single and multicomponent biomass burning aerosol surrogate-particles by OH: implications for cloud condensation nucleus activity

    DOE PAGESBeta

    Slade, J. H.; Thalman, R.; Wang, J.; Knopf, D. A.

    2015-03-06

    Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low soluble single-component OA by OH and O3 can increase their water-solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water-solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate-particles exposed to OH andmore » O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH/O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~0.1, indicating that chemically-aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally-mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical

  18. Chemical aging of single and multicomponent biomass burning aerosol surrogate-particles by OH: implications for cloud condensation nucleus activity

    NASA Astrophysics Data System (ADS)

    Slade, J. H.; Thalman, R.; Wang, J.; Knopf, D. A.

    2015-03-01

    Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low soluble single-component OA by OH and O3 can increase their water-solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water-solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate-particles exposed to OH and O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH/O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~0.1, indicating that chemically-aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally-mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical aging

  19. Chemical aging of single and multicomponent biomass burning aerosol surrogate particles by OH: implications for cloud condensation nucleus activity

    NASA Astrophysics Data System (ADS)

    Slade, J. H.; Thalman, R.; Wang, J.; Knopf, D. A.

    2015-09-01

    Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low-soluble single-component OA by OH and O3 can increase their water solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate particles exposed to OH and O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH and O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~ 0.1, indicating that chemically aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH-exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical

  20. Variability of CCN Activation Behaviour of Aerosol Particles in the Marine Boundary Layer of the Northern and Southern Atlantic Ocean

    NASA Astrophysics Data System (ADS)

    Henning, Silvia; Dieckmann, Katrin; Hartmann, Susan; Schäfer, Michael; Wu, Zhijun; Merkel, Maik; Wiedensohler, Alfred; Stratmann, Frank

    2013-04-01

    The variability of cloud condensation nucleus (CCN) activation behaviour and total CCN number concentrations was investigated during three ship cruises. Measurements were performed in a mobile laboratory on the German research vessel FS Polarstern cruising between Cape Town and Bremerhaven (April / May and October / November 2011) as well as between Punta Arenas and Bremerhaven (April / May 2012). CCN size distributions were measured for supersaturations between 0.1% and 0.4% using a Cloud Condensation Nucleus Counter (DMT, USA). Aerosol particle and CCN total number concentrations as well as the hygroscopicity parameter κ (Petters and Kreidenweis, 2007) were determined. Furthermore, size distribution data were collected. The hygroscopicity parameter κ featured a high variability during the cruises, with a median κ-value of 0.52 ± 0.26. The κ-values are depended on air mass origin; and are as expected mainly dominated by marine influences, but also long range transport of aerosol particles was detected. In the Celtic Sea, κ was found to be lower than that of clean marine aerosol particles (0.72 ± 0.24; Pringle et al., 2010) with κ-values ~0.2, possibly influenced by anthropogenic emissions from Europe. Close to the West African coast particle hygroscopicity was found to be influenced by the Saharan dust plume, resulting in low κ-values ~0.25. Petters, M.D. and S.M. Kreidenweis (2007), A single parameter representation of hygroscopic growth and cloud condensation nucleus activity, Atmos. Chem. and Phys., 7, 1961-1971. Pringle, K.J., H. Tost, A. Pozzer, U. Pöschl, and J. Lelieveld (2010), Global distribution of the effective aerosol hygroscopicity parameter for CCN activation, Atmos. Chem. Phys., 10, 5241-5255.

  1. Quantum Consequences of Parameterizing Geometry

    NASA Astrophysics Data System (ADS)

    Wanas, M. I.

    2002-12-01

    The marriage between geometrization and quantization is not successful, so far. It is well known that quantization of gravity , using known quantization schemes, is not satisfactory. It may be of interest to look for another approach to this problem. Recently, it is shown that geometries with torsion admit quantum paths. Such geometries should be parameterizied in order to preserve the quantum properties appeared in the paths. The present work explores the consequences of parameterizing such geometry. It is shown that quantum properties, appeared in the path equations, are transferred to other geometric entities.

  2. Effects of aerosol organics on cloud condensation nucleus (CCN) concentration and first indirect aerosol effect

    SciTech Connect

    Wang, J. X.; Lee, Y.- N.; Daum, Peter H.; Jayne, John T.; Alexander, M. L.

    2008-11-03

    Abstract. Aerosol microphysics, chemical composition, and CCN properties were measured on the Department of Energy Gulfstream-1 aircraft during the Marine Stratus/ Stratocumulus Experiment (MASE) conducted over the coastal waters between Point Reyes National Seashore and Monterey Bay, California, in July 2005. Aerosols measured during MASE included free tropospheric aerosols, marine boundary layer aerosols, and aerosols with high organic concentration within a thin layer above the cloud. Closure analysis was carried out for all three types of aerosols by comparing the measured CCN concentrations at 0.2% supersaturation to those predicted based on size distribution and chemical composition using K¨ohler theory. The effect of aerosol organic species on predicted CCN concentration was examined using a single hygroscopicity parameterization.

  3. Can we better use existing and emerging computing hardware to embed activity coefficient predictions in complex atmospheric aerosol models?

    NASA Astrophysics Data System (ADS)

    Topping, David; Alibay, Irfan; Ruske, Simon; Hindriksen, Vincent; Noisternig, Michael

    2016-04-01

    To predict the evolving concentration, chemical composition and ability of aerosol particles to act as cloud droplets, we rely on numerical modeling. Mechanistic models attempt to account for the movement of compounds between the gaseous and condensed phases at a molecular level. This 'bottom up' approach is designed to increase our fundamental understanding. However, such models rely on predicting the properties of molecules and subsequent mixtures. For partitioning between the gaseous and condensed phases this includes: saturation vapour pressures; Henrys law coefficients; activity coefficients; diffusion coefficients and reaction rates. Current gas phase chemical mechanisms predict the existence of potentially millions of individual species. Within a dynamic ensemble model, this can often be used as justification for neglecting computationally expensive process descriptions. Indeed, on whether we can quantify the true sensitivity to uncertainties in molecular properties, even at the single aerosol particle level it has been impossible to embed fully coupled representations of process level knowledge with all possible compounds, typically relying on heavily parameterised descriptions. Relying on emerging numerical frameworks, and designed for the changing landscape of high-performance computing (HPC), in this study we show that comprehensive microphysical models from single particle to larger scales can be developed to encompass a complete state-of-the-art knowledge of aerosol chemical and process diversity. We focus specifically on the ability to capture activity coefficients in liquid solutions using the UNIFAC method, profiling traditional coding strategies and those that exploit emerging hardware.

  4. Size-spectra of trace elements in urban aerosol particles by instrumental neutron activation analysis

    SciTech Connect

    Ondov, J.M.; Divita, F. Jr.; Suarez, A.

    1994-12-31

    Knowledge of composition and size of atmospheric aerosol particles is needed to elucidate their sources, atmospheric transformation processes, contributions to visibility reduction, and respiratory and environmental deposition. In a previous communication, we described size spectra and hygroscopic growth of arsenic, selenium, antimony, and zinc in College Park, Maryland, an urban, nonindustrial area located near Washington, D.C., wherein, concentrations of these elements are influenced largely by sulfate-containing aerosol transported from the Ohio River valley region, more than 200 km west of the area, and local coal utility plants and incinerators located 20 to 50 km from the sampling site. At College Park, mass median aerodynamic diameters (mmad) versus relative humidity (RH) data for these elements fell along different curves for samples influenced by local and distant aerosols; i.e., the curve for distant sources lay below the curve for local sources, at larger mmads for the same RH. In this paper we discuss size spectra, distribution parameters, and hygroscopic growth of aerosol particles bearing trace elements in aerosol collected in Camden, New Jersey, a heavily industrial area in which major sources, including an antimony roaster and municipal incinerator, lie in close proximity (i.e., 5 to 15 km) to the site.

  5. Aerosol Modeling for the Global Model Initiative

    NASA Technical Reports Server (NTRS)

    Weisenstein, Debra K.; Ko, Malcolm K. W.

    2001-01-01

    The goal of this project is to develop an aerosol module to be used within the framework of the Global Modeling Initiative (GMI). The model development work will be preformed jointly by the University of Michigan and AER, using existing aerosol models at the two institutions as starting points. The GMI aerosol model will be tested, evaluated against observations, and then applied to assessment of the effects of aircraft sulfur emissions as needed by the NASA Subsonic Assessment in 2001. The work includes the following tasks: 1. Implementation of the sulfur cycle within GMI, including sources, sinks, and aqueous conversion of sulfur. Aerosol modules will be added as they are developed and the GMI schedule permits. 2. Addition of aerosol types other than sulfate particles, including dust, soot, organic carbon, and black carbon. 3. Development of new and more efficient parameterizations for treating sulfate aerosol nucleation, condensation, and coagulation among different particle sizes and types.

  6. COMPUTATIONAL CHEMISTRY METHOD FOR PREDICTING VAPOR PRESSURES AND ACTIVITY COEFFICIENTS OF POLAR ORGANIC OXYGENATES IN PM2.5

    EPA Science Inventory

    Parameterizations of interactions of polar multifunctional organic oxygenates in PM2.5 must be included in aerosol chemistry models for evaluating control strategies for reducing ambient concentrations of PM2.5 compounds. Vapor pressures and activity coefficients of these compo...

  7. Hygroscopicity of aerosol particles and CCN activity of nearly hydrophobic particles in the urban atmosphere over Japan during summer

    NASA Astrophysics Data System (ADS)

    Ogawa, Shuhei; Setoguchi, Yoshitaka; Kawana, Kaori; Nakayama, Tomoki; Ikeda, Yuka; Sawada, Yuuki; Matsumi, Yutaka; Mochida, Michihiro

    2016-06-01

    We investigated the hygroscopicity of 150 nm particles and the number-size distributions and the cloud condensation nuclei (CCN) activity of nearly hydrophobic particles in aerosols over Nagoya, Japan, during summer. We analyzed the correlations between the number concentrations of particles in specific hygroscopic growth factor (g) ranges and the mass concentrations of chemical components. This analysis suggests the association of nearly hydrophobic particles with hydrocarbon-like organic aerosol, elemental carbon and semivolatile oxygenated organic aerosol (SV-OOA), that of less hygroscopic particles with SV-OOA and nitrate and that of more hygroscopic particles with low-volatile oxygenated organic aerosol (LV-OOA) and sulfate. The hygroscopicity parameter (κ) of organics was derived based on the g distributions and chemical composition of 150 nm particles. The κ of the organics correlated positively with the fraction of the total organic mass spectral signal at m/z 44 and the volume fraction of the LV-OOA to the organics, indicating that organics with highly oxygenated structures including carboxylic acid groups contribute to the water uptake. The number-size distributions of the nearly hydrophobic particles with g around 1.0 and 1.1 correlated with the mass concentrations of chemical components. The results show that the chemical composition of the particles with g around 1.0 was different between the Aitken mode and the accumulation mode size ranges. An analysis for a parameter Fmax of the curves fitted to the CCN efficiency spectra of the particles with g around 1.0 suggests that the coating by organics associated with SV-OOA elevated the CCN activity of these particles.

  8. Meteorological and trace gas factors affecting the number concentration of atmospheric Aitken (Dp = 50 nm) particles in the continental boundary layer: parameterization using a multivariate mixed effects model

    NASA Astrophysics Data System (ADS)

    Mikkonen, S.; Korhonen, H.; Romakkaniemi, S.; Smith, J. N.; Joutsensaari, J.; Lehtinen, K. E. J.; Hamed, A.; Breider, T. J.; Birmili, W.; Spindler, G.; Plass-Duelmer, C.; Facchini, M. C.; Laaksonen, A.

    2011-01-01

    Measurements of aerosol size distribution and different gas and meteorological parameters, made in three polluted sites in Central and Southern Europe: Po Valley, Italy, Melpitz and Hohenpeissenberg in Germany, were analysed for this study to examine which of the meteorological and trace gas variables affect the number concentration of Aitken (Dp= 50 nm) particles. The aim of our study was to predict the number concentration of 50 nm particles by a combination of in-situ meteorological and gas phase parameters. The statistical model needs to describe, amongst others, the factors affecting the growth of newly formed aerosol particles (below 10 nm) to 50 nm size, but also sources of direct particle emissions in that size range. As the analysis method we used multivariate nonlinear mixed effects model. Hourly averages of gas and meteorological parameters measured at the stations were used as predictor variables; the best predictive model was attained with a combination of relative humidity, new particle formation event probability, temperature, condensation sink and concentrations of SO2, NO2 and ozone. The seasonal variation was also taken into account in the mixed model structure. Model simulations with the Global Model of Aerosol Processes (GLOMAP) indicate that the parameterization can be used as a part of a larger atmospheric model to predict the concentration of climatically active particles. As an additional benefit, the introduced model framework is, in theory, applicable for any kind of measured aerosol parameter.

  9. Meteorological and trace gas factors affecting the number concentration of atmospheric Aitken (Dp=50 nm) particles in the continental boundary layer: parameterization using a multivariate mixed effects model

    NASA Astrophysics Data System (ADS)

    Mikkonen, S.; Korhonen, H.; Romakkaniemi, S.; Smith, J. N.; Joutsensaari, J.; Lehtinen, K. E. J.; Hamed, A.; Breider, T. J.; Birmili, W.; Spindler, G.; Plass-Duelmer, C.; Facchini, M. C.; Laaksonen, A.

    2010-08-01

    Measurements of aerosol size-distribution and different gas and meteorological parameters, made in three polluted sites in Central- and Southern Europe: Po Valley, Italy, Melpitz and Hohenpeissenberg in Germany, were analysed for this study to examine which of the meteorological and trace gas variables affect the number concentration of Aitken (Dp=50 nm) particles. The aim of our study was to predict the number concentration of 50 nm particles by a combination of in-situ meteorological and gas phase parameters. The statistical model needs to describe, amongst others, the factors affecting the growth of newly formed aerosol particles (below 10 nm) to 50 nm size, but also sources of direct particle emissions in that size range. As the analysis method we used multivariate nonlinear mixed effects model. Hourly averages of gas and meteorological parameters measured at the stations were used as predictor variables; the best predictive model was attained with a combination of relative humidity, new particle formation event probability, temperature, condensation sink and concentrations of SO2, NO2 and ozone. The seasonal variation was also taken into account in the mixed model structure. Model simulations with the Global Model of Aerosol Processes (GLOMAP) indicate that the parameterization can be used as a part of a larger atmospheric model to predict the concentration of climatically active particles. As an additional benefit, the introduced model framework is, in theory, applicable for any kind of measured aerosol parameter.

  10. Characteristics of aerosolized ice forming marine biogenic particles

    NASA Astrophysics Data System (ADS)

    Alpert, Peter A.

    atomus and Emiliania huxleyi, cells and cell fragments efficiently nucleate ice in the deposition mode, however, only T. pseudonana and N. atomus form ice in the immersion mode, presumably due to different cell wall compositions. This further corroborates the role of phytoplanktonic species for aerosolization of marine biogenic cloud active particles. Experimental data are used to parameterize marine biogenic particle fluxes and heterogeneous ice nucleation as a function of biological activity. The atmospheric implications of the results and their implementation into cloud and climate models are discussed.

  11. Competing effects of viscosity and surface-tension depression on the hygroscopicity and CCN activity of laboratory surrogates for oligomers in atmospheric aerosol

    NASA Astrophysics Data System (ADS)

    Hodas, N.; Zuend, A.; Shiraiwa, M.; Flagan, R. C.; Seinfeld, J.; Schilling, K.; Berkemeier, T.

    2015-12-01

    The presence of oligomers in biomass burning aerosol, as well as secondary organic aerosol derived from other sources, influences particle viscosity and can introduce kinetic limitations to water uptake. This, in turn, impacts aerosol optical properties and the efficiency with which these particles serve as cloud condensation nuclei (CCN). To explore the influence of organic-component viscosity on aerosol hygroscopicity, the water-uptake behavior of aerosol systems comprised of polyethylene glycol (PEG) and mixtures of PEG and ammonium sulfate (AS) was measured under sub- and supersaturated relative humidity (RH) conditions. Experiments were conducted with systems containing PEG with average molecular weights ranging from 200 to 10,000 g/mol, corresponding to a range in viscosity of 0.004 - 4.5 Pa s under dry conditions. While evidence suggests that viscous aerosol components can suppress water uptake at RH < 90%, under supersaturated conditions (with respect to RH), an increase in CCN activity with increasing PEG molecular weight was observed. We attribute this to an increase in the efficiency with which PEG serves as a surfactant with increasing molecular weight. This effect is most pronounced for PEG-AS mixtures and, in fact, a modest increase in CCN activity is observed for the PEG 10,000-AS mixture as compared to pure AS, as evidenced by a 4% reduction in critical activation diameter. Experimental results are compared with calculations of hygroscopic growth at thermodynamic equilibrium using the Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients model and the potential influence of kinetic limitations to observed water uptake is further explored with the Kinetic Multi-Layer Model of Gas-Particle Interactions. Results suggest the competing effects of organic-component viscosity and surface-tension depression may lead to RH-dependent differences in hygroscopicity for oligomers and other surface-active compounds present in atmospheric

  12. Limited Effect of Anthropogenic Nitrogen Oxides on Secondary Organic Aerosol Formation

    NASA Astrophysics Data System (ADS)

    Zheng, Y.; Unger, N.; Hodzic, A.; Knote, C. J.; Tilmes, S.; Emmons, L. K.; Lamarque, J. F.; Yu, P.

    2014-12-01

    Globally secondary organic aerosol (SOA) is mostly formed from biogenic vegetation emissions and as such is regarded as natural aerosol that cannot be reduced by emission control legislation. However, recent research implies that human activities facilitate SOA formation by affecting the amount of precursor emission, the chemical processing and the partitioning into the aerosol phase. Among the multiple human influences, nitrogen oxides (NO + NO2 = NOx) have been assumed to play a critical role in the chemical formation of low volatile compounds. The goal of this study is to improve the SOA scheme in the global NCAR Community Atmospheric Model version 4 with chemistry (CAM4-Chem) by implementing an updated 4-product Volatility Basis Set (VBS) scheme, and apply it to investigate the impact of anthropogenic NOx on SOA. We first compare three different SOA parameterizations: a 2-product model and the updated VBS model both with and without a SOA aging parameterization. Secondly we evaluate predicted organic aerosol amounts against surface measurement from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network and Aerosol Mass Spectrometer (AMS) measurements from 13 aircraft-based field campaigns. We then perform sensitivity experiments to examine how the SOA loading responds to a 50% reduction in anthropogenic NOx in different regions. We find limited SOA reductions of -2.3%, -5.6% and -4.0% for global, southeastern U.S. and Amazon NOx perturbations, respectively. To investigate the chemical processes in more detail, we also use a simplified box model with the same gas-phase chemistry and gas-aerosol partitioning mechanism as in CAM4-Chem to examine the SOA yields dependence on initial precursor emissions and background NOx level. The fact that SOA formation is almost unaffected by changes in NOx can be largely attributed to buffering in chemical pathways (low- versus high-NOx pathways, OH versus NO3-initiated oxidation) and to offsetting

  13. A review of research on human activity induced climate change I. Greenhouse gases and aerosols

    NASA Astrophysics Data System (ADS)

    Wang, Mingxing; Liu, Qiang; Yang, Xin

    2004-06-01

    Extensive research on the sources and sinks of greenhouse gases, carbon cycle modeling, and the characterization of atmospheric aerosols has been carried out in China during the last 10 years or so. This paper presents the major achievements in the fields of emissions of greenhouse gases from agricultural lands, carbon cycle modeling, the characterization of Asian mineral dust, source identification of the precursors of the tropospheric ozone, and observations of the concentrations of atmospheric organic compounds. Special, more detailed information on the emissions of methane from rice fields and the physical and chemical characteristics of mineral aerosols are presented.

  14. Infrared radiation parameterizations in numerical climate models

    NASA Technical Reports Server (NTRS)

    Chou, Ming-Dah; Kratz, David P.; Ridgway, William

    1991-01-01

    This study presents various approaches to parameterizing the broadband transmission functions for utilization in numerical climate models. One-parameter scaling is applied to approximate a nonhomogeneous path with an equivalent homogeneous path, and the diffuse transmittances are either interpolated from precomputed tables or fit by analytical functions. Two-parameter scaling is applied to parameterizing the carbon dioxide and ozone transmission functions in both the lower and middle atmosphere. Parameterizations are given for the nitrous oxide and methane diffuse transmission functions.

  15. Independent component analysis of parameterized ECG signals.

    PubMed

    Tanskanen, Jarno M A; Viik, Jari J; Hyttinen, Jari A K

    2006-01-01

    Independent component analysis (ICA) of measured signals yields the independent sources, given certain fulfilled requirements. Properly parameterized signals provide a better view to the considered system aspects, while reducing the amount of data. It is little acknowledged that appropriately parameterized signals may be subjected to ICA, yielding independent components (ICs) displaying more clearly the investigated properties of the sources. In this paper, we propose ICA of parameterized signals, and demonstrate the concept with ICA of ST and R parameterizations of electrocardiogram (ECG) signals from ECG exercise test measurements from two coronary artery disease (CAD) patients. PMID:17945912

  16. Aerosol disturbances of the stratosphere over Tomsk according to data of lidar observations in volcanic activity period 2006-2011

    NASA Astrophysics Data System (ADS)

    Makeev, Andrey P.; Burlakov, Vladimir D.; Dolgii, Sergey I.; Nevzorov, Aleksey V.; Trifonov, Dimitar A.

    2012-11-01

    We summarize and analyze the lidar measurements (Tomsk: 56.5°N; 85.0°E) of the optical characteristics of the stratospheric aerosol layer (SAL) in the volcanic activity period 2006-2011. The background SAL state with minimal aerosol content, which was observed since 1997 under the conditions of long-term volcanically quiescent period, was interrupted in October 2006 by a series of explosive eruptions of volcanoes of the Pacific Ring of Fire: Rabaul (October 2006, New Guinea); Okmok and Kasatochi (July-August 2008, Aleutian Islands); Redoubt (March-April 2009, Alaska); Sarychev Peak (June 2009, Kuril Islands), and Grimsvötn (May 2011, Iceland). A short-term and minor disturbance of the lower stratosphere was also observed in April 2010 after eruption of the Icelandic volcano Eyjafjallajokull. The developed regional empirical model of the vertical distribution of background SAL optical characteristics was used to identify the periods of elevated stratospheric aerosol content after each of the volcanic eruptions.

  17. Parameterization of precipitating shallow convection

    NASA Astrophysics Data System (ADS)

    Seifert, Axel

    2015-04-01

    Shallow convective clouds play a decisive role in many regimes of the atmosphere. They are abundant in the trade wind regions and essential for the radiation budget in the sub-tropics. They are also an integral part of the diurnal cycle of convection over land leading to the formation of deeper modes of convection later on. Errors in the representation of these small and seemingly unimportant clouds can lead to misforecasts in many situations. Especially for high-resolution NWP models at 1-3 km grid spacing which explicitly simulate deeper modes of convection, the parameterization of the sub-grid shallow convection is an important issue. Large-eddy simulations (LES) can provide the data to study shallow convective clouds and their interaction with the boundary layer in great detail. In contrast to observation, simulations provide a complete and consistent dataset, which may not be perfectly realistic due to the necessary simplifications, but nevertheless enables us to study many aspects of those clouds in a self-consistent way. Today's supercomputing capabilities make it possible to use domain sizes that not only span several NWP grid boxes, but also allow for mesoscale self-organization of the cloud field, which is an essential behavior of precipitating shallow convection. By coarse-graining the LES data to the grid of an NWP model, the sub-grid fluctuations caused by shallow convective clouds can be analyzed explicitly. These fluctuations can then be parameterized in terms of a PDF-based closure. The necessary choices for such schemes like the shape of the PDF, the number of predicted moments, etc., will be discussed. For example, it is shown that a universal three-parameter distribution of total water may exist at scales of O(1 km) but not at O(10 km). In a next step the variance budgets of moisture and temperature in the cloud-topped boundary layer are studied. What is the role and magnitude of the microphysical correlation terms in these equations, which

  18. What's Up in the Atmosphere? Exploring How Aerosols Impact Sky Color Through Hands-on Activities with Elementary GLOBE

    NASA Astrophysics Data System (ADS)

    Damadeo, K.; Taylor, J.

    2015-12-01

    What color is the sky today? The GLOBE Kids - Anita, Simon, and Dennis want to know why the sky isn't always the same shade of blue and sometimes isn't even blue. Through the new Elementary GLOBE Aerosols Storybook and Learning Activities, the GLOBE Kids learn that there's a lot more than air in the atmosphere, which can affect the colors we see in the sky. There are four hands-on activities in this unit: 1) Sky Observers - Students make observations of the sky, record their findings and share their observation reports with their peers. The activity promotes active observation and recording skills to help students observe sky color, and recognize that sky color changes; 2) Why (Not) So Blue? - Students make predictions about how drops of milk will affect color and visibility in cups of water representing the atmosphere to help them understand that aerosols in the atmosphere have an effect on sky conditions, including sky color and visibility. The activity also introduces the classification categories for daytime sky color and visibility; 3) See the Light - Students use prisms and glue sticks to explore the properties of light. The activity demonstrates that white light is made up of seven colors that represent different wavelengths, and illustrates why the sky is blue during the day and red at sunset; 4) Up in the Air - Students work in groups to make an aerosol sampler, a simple adhesive tool that allows students to collect data and estimate the extent of aerosols present at their school, understanding that, in fact, there are particles in the air we breathe. NGSS Alignment includes: Disciplinary Core Ideas- ESS2.D: Weather and Climate, ESS3.C: Human Impacts on Earth Systems, PS4.B: Electromagnetic Radiation, ESS3.A: Natural Resources; Science and Engineering Practices- Asking Questions and Defining Problems, Planning and Carrying Out an Investigation, Analyzing and Interpreting Data, Engaging in Argument from Evidence, Obtaining, Evaluating, and Communicating

  19. Cloud condensation nuclei activity, droplet growth kinetics, and hygroscopicity of biogenic and anthropogenic secondary organic aerosol (SOA)

    NASA Astrophysics Data System (ADS)

    Zhao, D. F.; Buchholz, A.; Kortner, B.; Schlag, P.; Rubach, F.; Fuchs, H.; Kiendler-Scharr, A.; Tillmann, R.; Wahner, A.; Watne, Å. K.; Hallquist, M.; Flores, J. M.; Rudich, Y.; Kristensen, K.; Hansen, A. M. K.; Glasius, M.; Kourtchev, I.; Kalberer, M.; Mentel, Th. F.

    2016-02-01

    Interaction of biogenic volatile organic compounds (VOCs) with Anthropogenic VOC (AVOC) affects the physicochemical properties of secondary organic aerosol (SOA). We investigated cloud droplet activation (CCN activity), droplet growth kinetics, and hygroscopicity of mixed anthropogenic and biogenic SOA (ABSOA) compared to pure biogenic SOA (BSOA) and pure anthropogenic SOA (ASOA). Selected monoterpenes and aromatics were used as representative precursors of BSOA and ASOA, respectively.

    We found that BSOA, ASOA, and ABSOA had similar CCN activity despite the higher oxygen to carbon ratio (O/C) of ASOA compared to BSOA and ABSOA. For individual reaction systems, CCN activity increased with the degree of oxidation. Yet, when considering all different types of SOA together, the hygroscopicity parameter, κCCN, did not correlate with O/C. Droplet growth kinetics of BSOA, ASOA, and ABSOA were comparable to that of (NH4)2SO4, which indicates that there was no delay in the water uptake for these SOA in supersaturated conditions.

    In contrast to CCN activity, the hygroscopicity parameter from a hygroscopic tandem differential mobility analyzer (HTDMA) measurement, κHTDMA, of ASOA was distinctively higher (0.09-0.10) than that of BSOA (0.03-0.06), which was attributed to the higher degree of oxidation of ASOA. The ASOA components in mixed ABSOA enhanced aerosol hygroscopicity. Changing the ASOA fraction by adding biogenic VOC (BVOC) to ASOA or vice versa (AVOC to BSOA) changed the hygroscopicity of aerosol, in line with the change in the degree of oxidation of aerosol. However, the hygroscopicity of ABSOA cannot be described by a simple linear combination of pure BSOA and ASOA systems. This indicates that additional processes, possibly oligomerization, affected the hygroscopicity.

    Closure analysis of CCN and HTDMA data showed κHTDMA was lower than κCCN by 30-70 %. Better closure was achieved for ASOA compared to BSOA. This

  20. New Approaches to Parameterizing Convection

    NASA Technical Reports Server (NTRS)

    Randall, David A.; Lappen, Cara-Lyn

    1999-01-01

    Many general circulation models (GCMs) currently use separate schemes for planetary boundary layer (PBL) processes, shallow and deep cumulus (Cu) convection, and stratiform clouds. The conventional distinctions. among these processes are somewhat arbitrary. For example, in the stratocumulus-to-cumulus transition region, stratocumulus clouds break up into a combination of shallow cumulus and broken stratocumulus. Shallow cumulus clouds may be considered to reside completely within the PBL, or they may be regarded as starting in the PBL but terminating above it. Deeper cumulus clouds often originate within the PBL with also can originate aloft. To the extent that our models separately parameterize physical processes which interact strongly on small space and time scales, the currently fashionable practice of modularization may be doing more harm than good.

  1. Automated Classification and Stellar Parameterization .

    NASA Astrophysics Data System (ADS)

    Giridhar, S.; Muneer, S.; Goswami, A.

    2006-08-01

    Different approaches for automated spectral classification are critically reviewed. We also summarize ANN based methods which would be very efficient in quick handling of the large volumes of data generated by different surveys. We have obtained medium resolution spectra for a large sample of stars using 2.3m telescope at VBO, Kavalur, India. Our sample contains uniform distribution of stars in temperature range 4000 to 8000K, log g range of 2.0 to 5.0 and [Fe/H] range of 0 to -3. We have explored the application of artificial neural network for parameterization of these stars. We have used a set of stars with well determined atmospheric parameters for training the networks for temperature, gravity and metallicity estimations. We use these trained network to estimate metallicities for a sample of metal-poor candidate stars.

  2. Parameterization of solar flare dose

    SciTech Connect

    Lamarche, A.H.; Poston, J.W.

    1996-12-31

    A critical aspect of missions to the moon or Mars will be the safety and health of the crew. Radiation in space is a hazard for astronauts, especially high-energy radiation following certain types of solar flares. A solar flare event can be very dangerous if astronauts are not adequately shielded because flares can deliver a very high dose in a short period of time. The goal of this research was to parameterize solar flare dose as a function of time to see if it was possible to predict solar flare occurrence, thus providing a warning time. This would allow astronauts to take corrective action and avoid receiving a dose greater than the recommended limit set by the National Council on Radiation Protection and Measurements (NCRP).

  3. Evolution of Organic Aerosols in the Atmosphere

    NASA Astrophysics Data System (ADS)

    Jimenez, J. L.; Canagaratna, M. R.; Donahue, N. M.; Prevot, A. S. H.; Zhang, Q.; Kroll, J. H.; DeCarlo, P. F.; Allan, J. D.; Coe, H.; Ng, N. L.; Aiken, A. C.; Docherty, K. S.; Ulbrich, I. M.; Grieshop, A. P.; Robinson, A. L.; Duplissy, J.; Smith, J. D.; Wilson, K. R.; Lanz, V. A.; Hueglin, C.; Sun, Y. L.; Tian, J.; Laaksonen, A.; Raatikainen, T.; Rautiainen, J.; Vaattovaara, P.; Ehn, M.; Kulmala, M.; Tomlinson, J. M.; Collins, D. R.; Cubison, M. J.; Dunlea, J.; Huffman, J. A.; Onasch, T. B.; Alfarra, M. R.; Williams, P. I.; Bower, K.; Kondo, Y.; Schneider, J.; Drewnick, F.; Borrmann, S.; Weimer, S.; Demerjian, K.; Salcedo, D.; Cottrell, L.; Griffin, R.; Takami, A.; Miyoshi, T.; Hatakeyama, S.; Shimono, A.; Sun, J. Y.; Zhang, Y. M.; Dzepina, K.; Kimmel, J. R.; Sueper, D.; Jayne, J. T.; Herndon, S. C.; Trimborn, A. M.; Williams, L. R.; Wood, E. C.; Middlebrook, A. M.; Kolb, C. E.; Baltensperger, U.; Worsnop, D. R.

    2009-12-01

    Organic aerosol (OA) particles affect climate forcing and human health, but their sources and evolution remain poorly characterized. We present a unifying model framework describing the atmospheric evolution of OA that is constrained by high-time-resolution measurements of its composition, volatility, and oxidation state. OA and OA precursor gases evolve by becoming increasingly oxidized, less volatile, and more hygroscopic, leading to the formation of oxygenated organic aerosol (OOA), with concentrations comparable to those of sulfate aerosol throughout the Northern Hemisphere. Our model framework captures the dynamic aging behavior observed in both the atmosphere and laboratory: It can serve as a basis for improving parameterizations in regional and global models.

  4. Aerosol-cloud interactions studied with the chemistry-climate model EMAC

    NASA Astrophysics Data System (ADS)

    Chang, D. Y.; Tost, H.; Steil, B.; Lelieveld, J.

    2014-08-01

    This study uses the EMAC atmospheric chemistry-climate model to simulate cloud properties and estimate cloud radiative effects induced by aerosols. We have tested two prognostic cloud droplet nucleation parameterizations, i.e., the standard STN (osmotic coefficient model) and hybrid (HYB, replacing the osmotic coefficient by the κ hygroscopicity parameter) schemes to calculate aerosol hygroscopicity and critical supersaturation, and consider aerosol-cloud feedbacks with a focus on warm clouds. Both prognostic schemes (STN and HYB) account for aerosol number, size and composition effects on droplet nucleation, and are tested in combination with two different cloud cover parameterizations, i.e., a relative humidity threshold and a statistical cloud cover scheme (RH-CLC and ST-CLC). The use of either STN and HYB leads to very different cloud radiative effects, particularly over the continents. The STN scheme predicts highly effective CCN activation in warm clouds and hazes/fogs near the surface. The enhanced CCN activity increases the cloud albedo effect of aerosols and cools the Earth's surface. The cooler surface enhances the hydrostatic stability of the lower continental troposphere and thereby reduces convection and convective precipitation. In contrast, the HYB simulations calculate lower, more realistic CCN activation and consequent cloud albedo effect, leading to relatively stronger convection and high cloud formation. The enhanced high clouds increase greenhouse warming and moderate the cooling effect of the low clouds. With respect to the cloud radiative effects, the statistical ST-CLC scheme shows much higher sensitivity to aerosol-cloud coupling for all continental regions than the RH-CLC threshold scheme, most pronounced for low clouds but also for high clouds. Simulations of the short wave cloud radiative effect at the top of the atmosphere in ST-CLC are a factor of 2-8 more sensitive to aerosol coupling than the RH-CLC configurations. The long wave

  5. Satellite Lidar Data Assimilation For Improved Global Aerosol Forecasting: Lessons Learned From CALIOP, With an Eye Toward EarthCARE

    NASA Astrophysics Data System (ADS)

    Campbell, J. R.; Reid, J. S.; Tackett, J. L.; Westphal, D. L.; Winker, D. M.; Zhang, J.

    2010-12-01

    Active satellite-based aerosol profiling with lidar instruments represents a critical component of advanced global transport modeling and visibility forecasting applications. Parameterized aerosol source functions alone are limited in representing injection scenarios within a model. Two-dimensional variational (2D-VAR; x, y) assimilation of aerosol optical depth (AOD) from passive satellite radiance observations significantly improves the forecast system. However, this procedure does not compensate for any vertical redistribution of mass necessary. The expense of an inaccurate vertical profile of aerosol structure is corresponding errors downwind, since trajectory paths within successive model time steps typically diverge with height. Recent improvements to the Navy Aerosol Analysis and Prediction System (NAAPS) include a newly-designed 3D-VAR assimilation system based on NASA/CNES satellite-borne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) aerosol backscatter profiles. NAAPS forecast skill improves with the benefit of 3D-VAR. However, it has proven considerably more challenging to implement this step than its 2D-VAR AOD counterpart. In this paper, we describe the process of assimilating satellite lidar measurements for aerosol applications, the development of model-friendly datasets, including a new NASA-disseminated product designed specifically for aerosol modeling applications, the importance of optimizing cross-track correlation in order to broaden the limited nadir-retrieved profile relative to the model grid and the potential for the near real-time/operational processing of ESA/JAXA Earth Clouds, Aerosol and Radiation Explorer (EarthCARE) high spectral resolution lidar datasets planned for late 2013. Lessons learned optimizing CALIOP datasets for modeling applications will not only improve performance in the short term, but ensure that developers are duly prepared for the coming EarthCARE data stream.

  6. Overview of the Cumulus Humilis Aerosol Processing Study.

    SciTech Connect

    Berg, L. K.; Berkowitz, C. M.; Ogren, J. A.; Hostetler, C. A.; Ferrare, R. A.; Dubey, M.; Andrews, E.; Coulter, R. L.; Hair, J. W.; Hubbe, J. M.Lee, Y. N.; Mazzoleni, C; Olfert, J; Springston, SR; Environmental Science Division; PNNL; NOAA Earth System Research Lab.; NASA Langley Research Center; LANL; BNL; Univ.of Alberta; Univ. of Colorado

    2009-11-01

    interest to the ASP: (1) How do the below-cloud and above-cloud aerosol optical and cloud nucleating properties downwind of a typical North American city differ from the optical and nucleating properties of aerosols in air unperturbed by urban emissions? Our interest is in the differences in the radiative properties, chemical composition, hygroscopic properties, and size distributions below and above cloud, and upwind and downwind of such a city. (2) How does the distribution of aerosol extinction vary in relation to the proximity to individual clouds and fields of clouds and why? (3) What are the differences, in terms of both size distributions and chemical composition, between activated aerosols within the urban plume and those outside the urban plume? (4) To what extent can models with state-of-the-art cloud parameterizations capture the statistical features of the below-above-cloud aerosols?

  7. Contribution of harbour activities to atmospheric aerosol in the Brindisi area

    NASA Astrophysics Data System (ADS)

    Donateo, Antonio; Cesari, Daniela; Nocioni, Alessandra; Grasso, Fabio M.; Merico, Eva; Giua, Roberto; Contini, Daniele

    2013-04-01

    The port areas are economic centres and transport hubs, that bring together different transport modes (sea, road, railway transport) and also industrial activities. Ship emissions when docked and during port manoeuvring can have a substantial negative effect on local air quality. The Fagerli and Tarrason (2001) simulation results indicated that ship traffic emissions contribute to 5% and 10% of PM10 concentrations in large parts of Great Britain, Portugal and Italy; similarly to what was obtained by Dalsoren et al. (2009). At the beginning of 2012 it was started the research project CESAPO (Contribution of Emission Sources on the Air quality of the POrt-cities in Greece and Italy), funded within the framework of Interreg Italy-Greece (2007/2013), having as objective the quantification of the contribution to atmospheric particles of emission sources in two important Mediterranean port-cities, namely Patra (Greece) and Brindisi (Italy). In this work the first results of the CESAPO project will be presented giving more emphasis on the analysis of the maritime transport and the activities within the harbour of Brindisi that is characterized by several emission sources operating concurrently. In 2010 and 2011, in the port of Brindisi freight traffic and total goods movement accounted for more than 9.5 million tons, with over 520,000 passengers. To recognize the contribution of harbour activities to PM2.5 and to the total number concentration of particles with respect to other emission sources (urban traffic and industrial pollution) it has been performed an intensive observation period (IOP) of 5 months (June 1 to October 31, 2012). During the IOP the data of 10 fixed monitoring stations (of the regional network managed by ARPA Puglia) and those from two additional stations specifically installed during the project inside the harbour area. A station was used to characterize the chemical composition of PM2.5 and PAHs (in the gaseous and aerosol phases) and the other was

  8. Aerosol palladium activation for electroless copper deposition and heat treatment with NO injection to fabricate Cu oxide/carbon fibre

    NASA Astrophysics Data System (ADS)

    Byeon, Jeong Hoon; Lee, Ryang Hwa; Hwang, Jungho

    2009-03-01

    This paper introduces a novel method for fabricating copper (Cu) oxide/activated carbon fibre (ACF) through the aerosol palladium (Pd) activation for use in electroless Cu deposition and heat treatment of Cu deposited ACF with nitric monoxide (NO) gas injection. Electroless Cu deposition was initiated by catalytically activating the ACF surface with spark generated Pd aerosol nanoparticles. The catalytically activated ACF was placed into a solution used for the electroless Cu deposition. Subjecting the Cu deposited ACF to a heat treatment in a NO/nitrogen (N2) gas injection (1000 ppm NO) resulted in changes to the morphology of the Cu particles. As the temperature increased from 100 to 500 °C, the relative mass fraction of oxygen in the Cu particles increased from 3.6% to 14.2% and the fraction of Cu decreased from 41.2% to 34.1%, which was caused by the formation of Cu oxides (Cu2O and CuO). The corresponding surface area and pore volume of the ACF decreased from 1019 m2 g-1 to 401 m2 g-1 and from 0.40 cm3 g-1 to 0.18 cm3 g-1, respectively. The morphological evolution and decrease in porosity were attributed to volume expansion of Cu particles during oxidation.

  9. Air mass origin and its influence on radionuclide activities ( 7Be and 210Pb) in aerosol particles at a coastal site in the western Mediterranean

    NASA Astrophysics Data System (ADS)

    Dueñas, C.; Orza, J. A. G.; Cabello, M.; Fernández, M. C.; Cañete, S.; Pérez, M.; Gordo, E.

    2011-07-01

    Studies of radionuclide activities in aerosol particles provide a means for evaluating the integrated effects of transport and meteorology on the atmospheric loadings of substances with different sources. Measurements of aerosol mass concentration and specific activities of 7Be and 210Pb in aerosols at Málaga (36° 43' 40″ N; 4° 28' 8″ W) for the period 2000-2006 were used to obtain the relationships between radionuclide activities and airflow patterns by comparing the data grouped by air mass trajectory clusters. The average concentration values of 7Be and 210Pb over the 7 year period have been found to be 4.6 and 0.58 mBq m -3, respectively, with mean aerosol mass concentration of 53.6 μg m -3. The identified air flow types arriving at Málaga reflect the transitional location of the Iberian Peninsula and show significant differences in radionuclide activities. Air concentrations of both nuclides and the aerosol mass concentration are controlled predominantly by the synoptic scenarios leading to the entrance of dust-laden continental flows from northern Africa and the arrival of polar maritime air masses, as implied by the strong correlations found between the monthly frequencies of the different air masses and the specific activities of both radionuclides. Correlations between activity concentrations and precipitation are significant though lower than with air masses.

  10. Visibility Parameterization For Forecasting Model Applications

    NASA Astrophysics Data System (ADS)

    Gultepe, I.; Milbrandt, J.; Binbin, Z.

    2010-07-01

    In this study, the visibility parameterizations developed during Fog Remote Sensing And Modeling (FRAM) projects, conducted in central and eastern Canada, will be summarized and their use for forecasting/nowcasting applications will be discussed. Parameterizations developed for reductions in visibility due to 1) fog, 2) rain, 3) snow, and 4) relative humidity (RH) during FRAM will be given and uncertainties in the parameterizations will be discussed. Comparisons made between Canadian GEM NWP model (with 1 and 2.5 km horizontal grid spacing) and observations collected during the Science of Nowcasting Winter Weather for Vancouver 2010 (SNOW-V10) project and FRAM projects, using the new parameterizations, will be given Observations used in this study were obtained using a fog measuring device (FMD) for fog parameterization, a Vaisala all weather precipitation sensor called FD12P for rain and snow parameterizations and visibility measurements, and a total precipitation sensor (TPS), and distrometers called OTT ParSiVel and Laser Precipitation Measurement (LPM) for rain/snow particle spectra. The results from the three SNOW-V10 sites suggested that visibility values given by the GEM model using the new parameterizations were comparable with observed visibility values when model based input parameters such as liquid water content, RH, and precipitation rate for visibility parameterizations were predicted accurately.

  11. Chemical Aging and Cloud Condensation Nuclei Activity of Biomass Burning Aerosol Proxies in the Presence of OH Radicals

    NASA Astrophysics Data System (ADS)

    Slade, Jonathan H., Jr.

    Biomass burning aerosol (BBA) can adversely impact regional and global air quality and represents a significant source of organic aerosol (OA) to the atmosphere that can affect climate. Aerosol particles can alter the transfer of radiation in earth's atmosphere directly by scattering and absorbing radiation or indirectly via cloud formation. Gas-to-particle, also termed heterogeneous, oxidation reactions can significantly alter the particle's physical and chemical properties. In turn, this can lead to the degradation of biomolecular markers for air quality-related aerosol source apportionment studies, the particles' lifetime, and modify the particles' abilities to serve as cloud condensation nuclei (CCN). However, the rates, mechanisms, and conditions by which these multiphase oxidation reactions occur and influence the CCN activity of OA is not well understood. The work presented here aims to determine the reactivity and products from the interaction of BBA surrogate-particles and trace gas-phase oxidants and to link the effects of OA chemical aging on the particles' ability to nucleate clouds. The reactive uptake of OH by BBA surrogate-substrates and particles, including levoglucosan, nitroguaiacol, abietic acid, and methyl-nitrocatechol, was determined as a function of both OH concentration and relative humidity (RH) using chemical ionization mass spectrometry coupled to various flow reactors. OH reactive uptake decreased with increasing OH concentration, indicative of OH adsorption followed by reaction. OH oxidation led to significant volatilization, i.e. mass loss of the organic material, as determined by application of high resolution proton transfer reaction time-of-flight mass spectrometry. Volatilized reaction products were identified, providing mechanistic insight of the chemical pathways in the heterogeneous OH oxidation of BBA. The reactive uptake of OH by levoglucosan particles increased with RH due to enhanced OH and organic bulk diffusivity. In

  12. Potential indirect effects of aerosol on tropical cyclone intensity: convective fluxes and cold-pool activity

    NASA Astrophysics Data System (ADS)

    Krall, G. M.; Cottom, W. R.

    2012-01-01

    Observational and model evidence suggest that a 2008 Western Pacific typhoon (NURI) ingested elevated concentrations of aerosol as it neared the Chinese coast. This study uses a regional model with two-moment bin-emulating microphysics to simulate the typhoon as it enters the field of elevated aerosol concentrations. A clean maritime field of cloud condensation nuclei (CCN) was prescribed as marine background CCN concentrations and then based on satellite and global aerosol model output, increased to pollution levels and further enhanced in sensitivity tests. The typhoon was simulated for 96 h beginning 17 August 2008. During the final 60 h CCN concentrations were enhanced as it neared the Philippines and coastal China. The model was initialized with both global reanalysis model data and irregularly spaced dropsonde data from the 2008 T-PARC observational campaign using an objective analysis routine. At 36 h, the internal nudging of the model was switched off and allowed to freely evolve on its own. As the typhoon encountered the elevated CCN in the sensitivity tests, a significant perturbation of windspeed, convective fluxes, and hydrometeor species behavior was simulated. Early during the ingestion of enhanced CCN, precipitation was reduced due to suppressed collision and coalescence, and storm winds increased in strength. Subsequently, owing to reduced fall speeds of the smaller drops, greater amounts of condensate were thrust into supercooled levels where the drops froze releasing greater amounts of latent heat of freezing. Convection thereby intensified which resulted in enhanced rainfall and more vigorous convectively-produced downdrafts. As the convection intensified in the outer rainbands the storm drifted over the developing cold-pools. The enhanced cold-pools blocked the inflow of warm, moist air into the core of the typhoon which led to a weakening of the typhoon with significantly reduced low level wind speeds. The very high amounts of pollution

  13. Studies of organic aerosol and aerosol-cloud interactions

    NASA Astrophysics Data System (ADS)

    Duong, Hanh To

    and wet scavenging are also shown to cause biases in the magnitude of aerosol-cloud interaction metrics. Air mass source origin and meteorology are also shown to be important factors that influence aerosol-cloud interactions. The results from this work contribute towards a better understanding of atmospheric aerosols and are meant to improve parameterizations that can be embedded in models that treat aerosol affects on clouds, precipitation, air quality, and public health.

  14. An approach for parameterizing mesoscale precipitating systems

    SciTech Connect

    Weissbluth, M.J.; Cotton, W.R.

    1991-12-31

    A cumulus parameterization laboratory has been described which uses a reference numerical model to fabricate, calibrate and verify a cumulus parameterization scheme suitable for use in mesoscale models. Key features of this scheme include resolution independence and the ability to provide hydrometeor source functions to the host model. Thus far, only convective scale drafts have been parameterized, limiting the use of the scheme to those models which can resolve the mesoscale circulations. As it stands, the scheme could probably be incorporated into models having a grid resolution greater than 50 km with results comparable to the existing schemes for the large-scale models. We propose, however, to quantify the mesoscale circulations through the use of the cumulus parameterization laboratory. The inclusion of these mesoscale drafts in the existing scheme will hopefully allow the correct parameterization of the organized mesoscale precipitating systems.

  15. An approach for parameterizing mesoscale precipitating systems

    SciTech Connect

    Weissbluth, M.J.; Cotton, W.R.

    1991-01-01

    A cumulus parameterization laboratory has been described which uses a reference numerical model to fabricate, calibrate and verify a cumulus parameterization scheme suitable for use in mesoscale models. Key features of this scheme include resolution independence and the ability to provide hydrometeor source functions to the host model. Thus far, only convective scale drafts have been parameterized, limiting the use of the scheme to those models which can resolve the mesoscale circulations. As it stands, the scheme could probably be incorporated into models having a grid resolution greater than 50 km with results comparable to the existing schemes for the large-scale models. We propose, however, to quantify the mesoscale circulations through the use of the cumulus parameterization laboratory. The inclusion of these mesoscale drafts in the existing scheme will hopefully allow the correct parameterization of the organized mesoscale precipitating systems.

  16. Measurements of physical and chemical properties of urban aerosols and their CCN activities in Seoul during the KORUS-AQ pre-campaign

    NASA Astrophysics Data System (ADS)

    Kim, N.; Yum, S. S.; Park, M.; Shin, H. J.; Bae, G. N.; Kwak, K. H.; Park, J. S.; Park, S. M.; Ahn, J.

    2015-12-01

    Interest in cloud condensation nuclei (CCN) has been increasing for the last few decades due to their first order effects on radiative and microphysical properties of clouds. Particularly, scientific understanding of CCN from anthropogenic sources becomes important because it is now considered that large uncertainties in climate change predictions stem from insufficient understanding of CCN. CCN activity is influenced by size and chemical component of aerosols. The KORUS-AQ campaign, jointly organized by National Institute of Environmental Research (NIER) of Korea and National Aeronautics and Space Administration (NASA) aims at understanding various aspects of air quality problem in Korea and will be held in spring, 2016. In preparation for this campaign, pre-campaign was held during May 18-June 13, 2015, in Seoul where numerous local anthropogenic sources exist and influence of Chinese continental outflow directly affects. Here we present some of the important results from the pre-campaign. Chemical properties of aerosols were measured with AMS. Aerosol and CCN number concentrations, aerosol size distribution and aerosol hygroscopic growth factor were measured by CPC, CCN counter, SMPS and H-TDMA, respectively. Average diurnal variation of aerosol number concentration showed three dominant peaks at around 0600_UTC and morning and evening rush hours. Each peak seemed to have different characteristics and therefore detailed analyses of physical and chemical properties of aerosols during the peaks as well as during some special events will be made. The hygroscopicity parameter, kappa, will be estimated by examining CCN activity, H-TDMA measured hygroscopic growth factor and mixing rule of aerosol chemical components, and the result will be compared as well.

  17. Parameterizations for convective transport in various cloud-topped boundary layers

    NASA Astrophysics Data System (ADS)

    Sikma, M.; Ouwersloot, H. G.

    2015-09-01

    We investigate the representation of convective transport of atmospheric compounds by boundary layer clouds. We focus on three key parameterizations that, when combined, express this transport: the area fraction of transporting clouds, the upward velocity in the cloud cores and the chemical concentrations at cloud base. The first two parameterizations combined represent the kinematic mass flux by clouds. To investigate the key parameterizations under a wide range of conditions, we use large-eddy simulation model data for 10 meteorological situations, characterized by either shallow cumulus or stratocumulus clouds. The parameterizations have not been previously tested with such large data sets. In the analysis, we show that the parameterization of the area fraction of clouds currently used in mixed-layer models is affected by boundary layer dynamics. Therefore, we (i) simplify the independent variable used for this parameterization, Q1, by considering the variability in moisture rather than in the saturation deficit and update the parameters in the parameterization to account for this simplification. We (ii) next demonstrate that the independent variable has to be evaluated locally to capture cloud presence. Furthermore, we (iii) show that the area fraction of transporting clouds is not represented by the parameterization for the total cloud area fraction, as is currently assumed in literature. To capture cloud transport, a novel active cloud area fraction parameterization is proposed. Subsequently, the scaling of the upward velocity in cloud cores by the Deardorff convective velocity scale and the parameterization for the concentration of atmospheric reactants at cloud base from literature are verified and improved by analysing six shallow cumulus cases. For the latter, we additionally discuss how the parameterization is affected by wind conditions. This study contributes to a more accurate estimation of convective transport, which occurs at sub-grid scales.

  18. Incorporation of new particle formation and early growth treatments into WRF/Chem: Model improvement, evaluation, and impacts of anthropogenic aerosols over East Asia

    NASA Astrophysics Data System (ADS)

    Cai, Changjie; Zhang, Xin; Wang, Kai; Zhang, Yang; Wang, Litao; Zhang, Qiang; Duan, Fengkui; He, Kebin; Yu, Shao-Cai

    2016-01-01

    New particle formation (NPF) provides an important source of aerosol particles and cloud condensation nuclei, which may result in enhanced cloud droplet number concentration (CDNC) and cloud shortwave albedo. In this work, several nucleation parameterizations and one particle early growth parameterization are implemented into the online-coupled Weather Research and Forecasting model coupled with chemistry (WRF/Chem) to improve the model's capability in simulating NPF and early growth of ultrafine particles over East Asia. The default 8-bin over the size range of 39 nm-10 μm used in the Model for Simulating Aerosol Interactions and Chemistry aerosol module is expanded to the 12-bin over 1 nm-10 μm to explicitly track the formation and evolution of new particles. Although model biases remain in simulating H2SO4, condensation sink, growth rate, and formation rate, the evaluation of July 2008 simulation identifies a combination of three nucleation parameterizations (i.e., COMB) that can best represent the atmospheric nucleation processes in terms of both surface nucleation events and the resulting vertical distribution of ultrafine particle concentrations. COMB consists of a power law of Wang et al. (2011) based on activation theory for urban areas in planetary boundary layer (PBL), a power law of Boy et al. (2008) based on activation theory for non-urban areas in PBL, and the ion-mediated nucleation parameterization of YU10 for above PBL. The application and evaluation of the improved model with 12-bin and the COMB nucleation parameterization in East Asia during January, April, July, and October in 2001 show that the model has an overall reasonably good skill in reproducing most observed meteorological variables and surface and column chemical concentrations. Relatively large biases in simulated precipitation and wind speeds are due to inaccurate surface roughness and limitations in model treatments of cloud formation and aerosol-cloud-precipitation interactions

  19. Aerosol Activity and Hygroscopicity Combined with Lidar Data in the Urban Atmosphere of Athens, Greece in the Frame of the HYGRA_CD Campaign

    NASA Astrophysics Data System (ADS)

    Bougiatioti, Aikaterini; Papayannis, Alexandros; Vratolis, Stergios; Argyrouli, Athina; Mihalopoulos, Nikolaos; Tsagkaraki, Maria; Nenes, Athanasios; Eleftheriadis, Konstantinos

    2016-06-01

    Measurements of cloud condensation nuclei (CCN) concentrations between 0.2-1.0% supersaturation and aerosol size distribution were performed at an urban background site of Athens during HygrA-CD. The site is affected by local and long-range transported emissions as portrayed by the external mixing of the particles, as the larger ones appear to be more hygroscopic and more CCN-active than smaller ones. Activation fractions at all supersaturations exhibit a diurnal variability with minimum values around noon, which are considerably lower than unity. This reinforces the conclusion that the aerosol is mostly externally mixed between "fresher", less hygroscopic components with more aged, CCN active constituents.

  20. MBAS (Methylene Blue Active Substances) and LAS (Linear Alkylbenzene Sulphonates) in Mediterranean coastal aerosols: Sources and transport processes

    NASA Astrophysics Data System (ADS)

    Becagli, S.; Ghedini, C.; Peeters, S.; Rottiers, A.; Traversi, R.; Udisti, R.; Chiari, M.; Jalba, A.; Despiau, S.; Dayan, U.; Temara, A.

    2011-12-01

    Methylene Blue Active Substances (MBAS) and Linear Alkylbenzene Sulphonates (LAS) concentrations, together with organic carbon and ions were measured in atmospheric coastal aerosols in the NW Mediterranean Basin. Previous studies have suggested that the presence of surfactants in coastal aerosols may result in vegetation damage without specifically detecting or quantifying these surfactants. Coastal aerosols were collected at a remote site (Porquerolles Island-Var, France) and at a more anthropised site (San Rossore National Park-Tuscany, Italy). The chemical data were interpreted according to a comprehensive local meteorological analysis aiming to decipher the airborne source and transport processes of these classes of compounds. The LAS concentration (anthropogenic surfactants) was measured in the samples using LC-MS/MS, a specific analytical method. The values were compared with the MBAS concentration, determined by a non-specific analytical method. At Porquerolles, the MBAS concentration (103 ± 93 ng m -3) in the summer samples was significantly higher than in the winter samples. In contrast, LAS concentrations were rarely greater than in the blank filters. At San Rossore, the mean annual MBAS concentration (887 ± 473 ng m -3 in PM10) contributed about 10% to the total atmospheric particulate organic matter. LAS mean concentration in these same aerosol samples was 11.5 ± 10.5 ng m -3. A similar MBAS (529 ± 454 ng m -3) - LAS (7.1 ± 4.1 ng m -3 LAS) ratio of ˜75 was measured in the fine (PM2.5) aerosol fraction. No linear correlation was found between MBAS and LAS concentrations. At San Rossore site the variation of LAS concentrations was studied on a daily basis over a year. The LAS concentrations in the coarse fraction (PM10-2.5) were higher during strong sea storm conditions, characterized by strong air flow coming from the sea sector. These events, occurring with more intensity in winter, promoted the formation of primary marine aerosols containing LAS

  1. Influence of functional groups on organic aerosol cloud condensation nucleus activity.

    PubMed

    Suda, Sarah R; Petters, Markus D; Yeh, Geoffrey K; Strollo, Christen; Matsunaga, Aiko; Faulhaber, Annelise; Ziemann, Paul J; Prenni, Anthony J; Carrico, Christian M; Sullivan, Ryan C; Kreidenweis, Sonia M

    2014-09-01

    Organic aerosols in the atmosphere are composed of a wide variety of species, reflecting the multitude of sources and growth processes of these particles. Especially challenging is predicting how these particles act as cloud condensation nuclei (CCN). Previous studies have characterized the CCN efficiency for organic compounds in terms of a hygroscopicity parameter, κ. Here we extend these studies by systematically testing the influence of the number and location of molecular functional groups on the hygroscopicity of organic aerosols. Organic compounds synthesized via gas-phase and liquid-phase reactions were characterized by high-performance liquid chromatography coupled with scanning flow CCN analysis and thermal desorption particle beam mass spectrometry. These experiments quantified changes in κ with the addition of one or more functional groups to otherwise similar molecules. The increase in κ per group decreased in the following order: hydroxyl ≫ carboxyl > hydroperoxide > nitrate ≫ methylene (where nitrate and methylene produced negative effects, and hydroperoxide and nitrate groups produced the smallest absolute effects). Our results contribute to a mechanistic understanding of chemical aging and will help guide input and parametrization choices in models relying on simplified treatments such as the atomic oxygen:carbon ratio to predict the evolution of organic aerosol hygroscopicity. PMID:25118824

  2. A physically based framework for modeling the organic fractionation of sea spray aerosol from bubble film Langmuir equilibria

    NASA Astrophysics Data System (ADS)

    Burrows, S. M.; Ogunro, O.; Frossard, A. A.; Russell, L. M.; Rasch, P. J.; Elliott, S. M.

    2014-12-01

    The presence of a large fraction of organic matter in primary sea spray aerosol (SSA) can strongly affect its cloud condensation nuclei activity and interactions with marine clouds. Global climate models require new parameterizations of the SSA composition in order to improve the representation of these processes. Existing proposals for such a parameterization use remotely sensed chlorophyll a concentrations as a proxy for the biogenic contribution to the aerosol. However, both observations and theoretical considerations suggest that existing relationships with chlorophyll a, derived from observations at only a few locations, may not be representative for all ocean regions. We introduce a novel framework for parameterizing the fractionation of marine organic matter into SSA based on a competitive Langmuir adsorption equilibrium at bubble surfaces. Marine organic matter is partitioned into classes with differing molecular weights, surface excesses, and Langmuir adsorption parameters. The classes include a lipid-like mixture associated with labile dissolved organic carbon (DOC), a polysaccharide-like mixture associated primarily with semilabile DOC, a protein-like mixture with concentrations intermediate between lipids and polysaccharides, a processed mixture associated with recalcitrant surface DOC, and a deep abyssal humic-like mixture. Box model calculations have been performed for several cases of organic adsorption to illustrate the underlying concepts. We then apply the framework to output from a global marine biogeochemistry model, by partitioning total dissolved organic carbon into several classes of macromolecules. Each class is represented by model compounds with physical and chemical properties based on existing laboratory data. This allows us to globally map the predicted organic mass fraction of the nascent submicron sea spray aerosol. Predicted relationships between chlorophyll a and organic fraction are similar to existing empirical parameterizations

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

    NASA Astrophysics Data System (ADS)

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

    2016-10-01

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

  4. Organic Aerosol Formation in the Humid, Photochemically-Active Southeastern US: SOAS Experiments and Simulations

    NASA Astrophysics Data System (ADS)

    Sareen, N.; Lim, Y. B.; Carlton, A. G.; Turpin, B. J.

    2013-12-01

    Aqueous multiphase chemistry in the atmosphere can lead to rapid transformation of organic compounds, forming highly oxidized low volatility organic aerosol and, in some cases, light absorbing (brown) carbon. Because liquid water is globally abundant, this chemistry could substantially impact climate, air quality, health, and the environment. Gas-phase precursors released from biogenic and anthropogenic sources are oxidized and fragmented forming water-soluble gases that can undergo reactions in the aqueous phase (in clouds, fogs, and wet aerosols) leading to the formation of secondary organic aerosol (SOAAQ). Recent studies have highlighted the role of certain precursors like glyoxal, methylglyoxal, glycolaldehyde, acetic acid, acetone, and epoxides in the formation of SOAAQ. The goal of this work is to identify other precursors that are atmospherically important. In this study, ambient mixtures of water-soluble gases were scrubbed from the atmosphere at Brent, Alabama during the Southern Oxidant and Aerosol Study (SOAS). Four mist chambers in parallel collected ambient gases in a DI water medium at 20-25 LPM with a 4 hr collection time. Total organic carbon (TOC) values in daily composited samples were 64-180 μM. Aqueous OH radical oxidation experiments were conducted with these mixtures in a newly designed cuvette chamber to understand the formation of SOA through gas followed by aqueous chemistry. OH radicals (3.5E-2 μM [OH] s-1) were formed in-situ in the chamber, continuously by H2O2 photolysis. Precursors and products of these aqueous OH experiments were characterized using ion chromatography (IC), electrospray ionization mass spectrometry (ESI-MS), and IC-ESI-MS. ESI-MS results from a June 12th, 2013 sample showed precursors to be primarily odd, positive mode ions, indicative of the presence of non-nitrogen containing alcohols, aldehydes, organic peroxides, or epoxides. Products were seen in the negative mode and included organic acid ions like pyruvate

  5. Parameterized Linear Longitudinal Airship Model

    NASA Technical Reports Server (NTRS)

    Kulczycki, Eric; Elfes, Alberto; Bayard, David; Quadrelli, Marco; Johnson, Joseph

    2010-01-01

    A parameterized linear mathematical model of the longitudinal dynamics of an airship is undergoing development. This model is intended to be used in designing control systems for future airships that would operate in the atmospheres of Earth and remote planets. Heretofore, the development of linearized models of the longitudinal dynamics of airships has been costly in that it has been necessary to perform extensive flight testing and to use system-identification techniques to construct models that fit the flight-test data. The present model is a generic one that can be relatively easily specialized to approximate the dynamics of specific airships at specific operating points, without need for further system identification, and with significantly less flight testing. The approach taken in the present development is to merge the linearized dynamical equations of an airship with techniques for estimation of aircraft stability derivatives, and to thereby make it possible to construct a linearized dynamical model of the longitudinal dynamics of a specific airship from geometric and aerodynamic data pertaining to that airship. (It is also planned to develop a model of the lateral dynamics by use of the same methods.) All of the aerodynamic data needed to construct the model of a specific airship can be obtained from wind-tunnel testing and computational fluid dynamics

  6. Automated classification and stellar parameterization

    NASA Astrophysics Data System (ADS)

    Giridhar, Sunetra; Muneer, S.; Goswami, Aruna

    Different approaches for automated spectral classification are critically reviewed. We describe in detail ANN based methods which are very efficient in quick handling of the large volumes of data generated by different surveys. We summarize the application of ANN in various surveys covering UV, visual and IR spectral regions and the accuracies obtained. We also present the preliminary results obtained with medium resolution spectra (R ˜ 1000) for a modest sample of stars using the 2.3 m Vainu Bappu Telescope at Kavalur observatory, India. Our sample contains uniform distribution of stars in temperature range 4500 to 8000 K, log g range of 1.5 to 5.0 and [Fe/H] range of 0 to -3. We have explored the application of artificial neural network for parameterization of these stars. We have used a set of stars with well determined atmospheric parameters for training the networks for temperature, gravity and metallicity estimations. We could get an accuracy of 200 K in temperature, 0.4 in log g and 0.3 dex in [Fe/H] in our preliminary efforts.

  7. Simulating Feedbacks Between Stratocumulus Cloud Dynamics, Microphysics and Aerosols Over Large Scales.

    NASA Astrophysics Data System (ADS)

    Grosvenor, D. P.; Field, P.; Hill, A. A.; Shipway, B. J.

    2014-12-01

    The response of a stratocumulus cloud deck to aerosols involves a complex interplay between cloud microphysics, precipitation, cold pool dynamical interactions between neighboring cells, cloud top entrainment and the boundary layer structure over larger scales. Such feedbacks are thought to be involved in, for example, the formation of Pockets of Open Cells (POCs), which represent a large albedo change relative to the closed cell regime. However, they are not represented in GCM parameterizations and have also so far have not been simulated adequately in mesoscale models, which is a necessary step in order to develop parameterizations. We will show results from high resolution (<1 km) mesoscale simulations of stratocumulus using a new multi-moment microphysics scheme coupled to the UK Met Office Unified Model. The new scheme represents the processing of aerosol by clouds, allowing examination of the feedbacks between cloud dynamics, microphysics and aerosol. Results will be shown for domains of order 1000km that are driven by meteorological analysis, allowing realistic forcing and large scale interactions, in contrast to idealized LES simulations. Additionally, a representation of sub-grid vertical velocities based on resolved motions has been implemented, which will allow consistent droplet activation across a range of horizontal model resolutions. A cloud scheme to account for sub-grid humidity variability was also added and was found to be necessary in order to simulate realistic clouds.

  8. Effects of Organic-Inorganic Interactions on the Hygroscopicity of Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Zuend, A.; Lienhard, D.; Krieger, U. K.

    2013-12-01

    Aerosol hygroscopicity is an important property affecting size as well as phase transitions and viscosity of soluble or partially soluble particles following changes in ambient relative humidity (RH) and temperature. The effects of hygroscopic particle growth on the water contents and physical states of aerosol phases in turn may significantly affect multiphase chemistry, the direct effect of aerosols on climate, and the ability of specific particles to act as cloud condensation or ice nuclei. The hygroscopic growth of organic-inorganic mixtures in stable or metastable equilibrium with the RH of the surrounding air is governed by chemical thermodynamics and can be described, in principle, by adequate thermodynamic models. Organic-inorganic interactions involving dissolved ionic species in liquid (potentially highly viscous) phases tend to deviate substantially from ideal mixing and can lead to hygroscopicity behaviour deviating from simple linear additivity assumptions at given RH. The latter assumptions are employed in the Zdanovskii-Stokes-Robinson (ZSR) mixing rule, which is typically found to describe hygroscopic mass growth well in the RH range of completely liquid aerosol systems. We present a comparison and discussion of thermodynamic calculations based on the Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model and hygroscopic growth factor data from new measurements with an electrodynamic balance (EDB) as well as data from the literature. We focus on the different hygroscopicity features below the full deliquescence RH of multicomponent organic-inorganic systems. Experiments and model calculations are performed for different multicomponent systems showing varying degrees of organic-inorganic miscibility, including liquid-liquid phase separation, hygroscopicity, and hysteresis effects between metastable and stable gas-aerosol equilibria. It is found that depending on the hygroscopicity of the organic aerosol fraction

  9. Parameterization of biomass burning aerosolsin the BRAZIL-SR radiative transfer model.

    NASA Astrophysics Data System (ADS)

    Martins, F. R.; Pereira, E. B.; Stuhlmann, R.

    2003-04-01

    This work describes the impact of the aerosols that are generated during biomass burning events in the solar irradiation, and presents a parameterization technique to improve the model estimations of the surface incident solar irradiation obtained by the BRASIL-SR radiative transfer model. It was verified that the mean systematic deviation error (MBE) of model estimates grows about 3 times and the value of root mean squared error (RMSE) duplicates in clear sky days for stations close to burned sites in central region of Brazil. The proximity of burned sites produces an increment of the same order of that produced by the presence of clouds in MBE. The parameterization technique of the biomass burning aerosols uses optical properties provided by "Global Aerosol Data Set" (GADS) and it is in accordance with measurements values obtained in two field missions: TRACE-A (1992) and SCAR-B (1995). Three different compositions were used in this study and the difference among them is the ratio of black carbon present in the aerosols: 5%, 7.8% and 10% of black carbon. These values are within the range of measured values observed in the field missions: from 4% to 12%. The aerosol profile and spatial distribution was obtained from a transport model for estimation of tracers spreading from biomass burning areas developed at INPE-CPTEC. The surface incident solar irradiation estimates, obtained with new aerosol parameterization, presented smaller systematic deviations in all the stations used in the validation process. The correlation among estimated and measured values for surface incident solar radiation grew about 2,5 times by adopting a composition with 5% of elementary carbon. The validation procedure showed that the improvements in aerosol parameterization allowed for better estimates by the model. However, the improvements are still masked by limitation imposed by the availability of only tri-hourly image schedules for the GOES-8 satellite in Southern Hemisphere

  10. Ice nucleating particles at a coastal marine boundary layer site: correlations with aerosol type and meteorological conditions

    NASA Astrophysics Data System (ADS)

    Mason, R. H.; Si, M.; Li, J.; Chou, C.; Dickie, R.; Toom-Sauntry, D.; Pöhlker, C.; Yakobi-Hancock, J. D.; Ladino, L. A.; Jones, K.; Leaitch, W. R.; Schiller, C. L.; Abbatt, J. P. D.; Huffman, J. A.; Bertram, A. K.

    2015-11-01

    Information on what aerosol particle types are the major sources of ice nucleating particles (INPs) in the atmosphere is needed for climate predictions. To determine which aerosol particles are the major sources of immersion-mode INPs at a coastal site in Western Canada, we investigated correlations between INP number concentrations and both concentrations of different atmospheric particles and meteorological conditions. We show that INP number concentrations are strongly correlated with the number concentrations of fluorescent bioparticles between -15 and -25 °C, and that the size distribution of INPs is most consistent with the size distribution of fluorescent bioparticles. We conclude that biological particles were likely the major source of ice nuclei at freezing temperatures between -15 and -25 °C at this site for the time period studied. At -30 °C, INP number concentrations are also well correlated with number concentrations of the total aerosol particles ≥ 0.5 μm, suggesting that non-biological particles may have an important contribution to the population of INPs active at this temperature. As we found that black carbon particles were unlikely to be a major source of ice nuclei during this study, these non-biological INPs may include mineral dust. Furthermore, correlations involving chemical tracers of marine aerosols and marine biological activity, sodium and methanesulfonic acid, indicate that the majority of INPs measured at the coastal site likely originated from terrestrial rather than marine sources. Finally, six existing empirical parameterizations of ice nucleation were tested to determine if they accurately predict the measured INP number concentrations. We found that none of the parameterizations selected are capable of predicting INP number concentrations with high accuracy over the entire temperature range investigated. This finding illustrates that additional measurements are needed to improve parameterizations of INPs and their

  11. Organic aerosols

    SciTech Connect

    Penner, J.E.

    1994-01-01

    Organic aerosols scatter solar radiation. They may also either enhance or decrease concentrations of cloud condensation nuclei. This paper summarizes observed concentrations of aerosols in remote continental and marine locations and provides estimates for the sources of organic aerosol matter. The anthropogenic sources of organic aerosols may be as large as the anthropogenic sources of sulfate aerosols, implying a similar magnitude of direct forcing of climate. The source estimates are highly uncertain and subject to revision in the future. A slow secondary source of organic aerosols of unknown origin may contribute to the observed oceanic concentrations. The role of organic aerosols acting as cloud condensation nuclei (CCN) is described and it is concluded that they may either enhance or decrease the ability of anthropogenic sulfate aerosols to act as CCN.

  12. Enhanced High-Temperature Ice Nucleation Ability of Crystallized Aerosol Particles after Pre-Activation at Low Temperature

    NASA Astrophysics Data System (ADS)

    Wagner, R.; Moehler, O.; Saathoff, H.; Schnaiter, M.

    2014-12-01

    The term pre-activation in heterogeneous ice nucleation describes the observation that the ice nucleation ability of solid ice nuclei may improve after they have already been involved in ice crystal formation or have been exposed to a temperature lower than 235 K. This can be explained by the retention of small ice embryos in cavities or crevices at the particle surface or by the capillary condensation and freezing of supercooled water, respectively. In recent cloud chamber experiments with crystallized aqueous ammonium sulfate, oxalic acid, and succinic acid solution droplets, we have unraveled a further pre-activation mechanism under ice subsaturated conditions which does not require the preceding growth of ice on the seed aerosol particles (Wagner, R. et al., J. Geophys. Res. Atmos., 119, doi: 10.1002/2014JD021741). First cloud expansion experiments were performed at a high temperature (267 - 244 K) where the crystallized particles did not promote any heterogeneous ice nucleation. Ice nucleation at this temperature, however, could be triggered by temporarily cooling the crystallized particles to a lower temperature. This is because upon crystallization, residuals of the aqueous solution are trapped within the crystals. These captured liquids can freeze when cooled below their respective homogeneous or heterogeneous freezing temperature, leading to the formation of ice pockets in the crystalline particles. When warmed again to the higher temperature, ice formation by the pre-activated particles occurred via depositional and deliquescence-induced ice growth, with ice active fractions ranging from 1 to 4% and 4 to 20%, respectively. Pre-activation disappeared above the eutectic temperature, which for the organic acids are close to the melting point of ice. This mechanism could therefore contribute to the very small fraction of atmospheric aerosol particles that are still ice active well above 263 K.

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

    NASA Astrophysics Data System (ADS)

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

    2013-08-01

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

  14. Organic aerosol formation from biogenic compounds over the Ponderosa pine forest in Colorado

    NASA Astrophysics Data System (ADS)

    Roux, Alma Hodzic; Lee-Taylor, Julia; Cui, Yuyan; Madronich, Sasha

    2013-05-01

    The secondary organic aerosol (SOA) formation and regional growth from biogenic precursors is of particular interest given their abundance in the atmosphere, and has been investigated during the Rocky Mountain Biogenic Aerosol field Study in 2011 in the pine forest canopy (dominated by terpene emissions) using both WRF/Chem 4km simulations and the GECKO-A explicit chemistry box-model runs. We have quantified the relative contribution of different biogenic precursors to SOA levels that were measured by the aerosol mass spectrometer at the site, and investigated the relative contribution of OH, O3 and NO3 chemistry to the formed SOA mass during day-and nighttime. Although, the local production and mass concentrations of submicron organic aerosols at the site seem relatively modest ˜1-2 ug/m3, we show that the optically active regional mass is increased as the SOA formation continues for several days in the background forest air. We investigate whether the simplified SOA parameterizations used in 3D models can capture this growth. In addition, preliminary comparisons of the number concentrations and the composition of ultrafine particles (8 - 30nm) from WRF/Chem simulations and TD-CIMS measurements are also discussed, and the contribution of organic aerosols to CCN formation is quantified.

  15. Comparative analysis of hygroscopic properties of atmospheric aerosols at ZOTTO Siberian background station during summer and winter campaigns of 2011

    NASA Astrophysics Data System (ADS)

    Ryshkevich, T. I.; Mironov, G. N.; Mironova, S. Yu.; Vlasenko, S. S.; Chi, X.; Andreae, M. O.; Mikhailov, E. F.

    2015-09-01

    The results of measurements of hygroscopic properties and chemical analysis of atmospheric aerosol samples collected from June 10 to 20 and December 15 to 25, 2011, at the ZOTTO background stations (60.8° N, 89.35° E) in Central Siberia are presented. The sorption properties of aerosols are studied with the help of a differential analyzer of absorbed water mass in the relative humidity range of 5 to 99%. It has been found that the hygroscopic growth factor of aerosol particles collected during the winter campaign is on average 45% higher than that of the aerosol collected in the summer campaign, which leads to a 40% decrease in the critical supersaturation threshold of cloud activation of particles. The measurement data are analyzed and parameterized using a new approach that takes into account the concentration effects in the particle—water vapor system at low humidities. Based on the chemical analysis, the content of water-soluble substances in the winter sample is 2.5 times higher than in the summer sample. Here, the amount of sulfates and nitrates increases 20 and 88 times, respectively. A trajectory analysis of air mass motion shows that the increased content of inorganic ions in aerosols for the winter sample is caused by long-range transport of pollutants from industrial areas of Siberia. This difference in the chemical composition is the main source of the observed difference in hygroscopic and condensation properties of the aerosol particles.

  16. A comprehensive parameterization of heterogeneous ice nucleation of dust surrogate: laboratory study with hematite particles and its application to atmospheric models

    NASA Astrophysics Data System (ADS)

    Hiranuma, N.; Paukert, M.; Steinke, I.; Zhang, K.; Kulkarni, G.; Hoose, C.; Schnaiter, M.; Saathoff, H.; Möhler, O.

    2014-12-01

    A new heterogeneous ice nucleation parameterization that covers a wide temperature range (-36 to -78 °C) is presented. Developing and testing such an ice nucleation parameterization, which is constrained through identical experimental conditions, is important to accurately simulate the ice nucleation processes in cirrus clouds. The ice nucleation active surface-site density (ns) of hematite particles, used as a proxy for atmospheric dust particles, were derived from AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud chamber measurements under water subsaturated conditions. These conditions were achieved by continuously changing the temperature (T) and relative humidity with respect to ice (RHice) in the chamber. Our measurements showed several different pathways to nucleate ice depending on T and RHice conditions. For instance, almost T-independent freezing was observed at -60 °C < T < -50 °C, where RHice explicitly controlled ice nucleation efficiency, while both T and RHice played roles in other two T regimes: -78 °C < T < -60 °C and -50 °C < T < -36 °C. More specifically, observations at T lower than -60 °C revealed that higher RHice was necessary to maintain a constant ns, whereas T may have played a significant role in ice nucleation at T higher than -50 °C. We implemented the new hematite-derived ns parameterization, which agrees well with previous AIDA measurements of desert dust, into two conceptual cloud models to investigate their sensitivity to the new parameterization in comparison to existing ice nucleation schemes for simulating cirrus cloud properties. Our results show that the new AIDA-based parameterization leads to an order of magnitude higher ice crystal concentrations and to an inhibition of homogeneous nucleation in lower-temperature regions. Our cloud simulation results suggest that atmospheric dust particles that form ice nuclei at lower temperatures, below -36 °C, can potentially have a stronger influence on cloud

  17. Response Timescales and Multiple Equilibria in Boundary-Layer Cloud-Aerosol Interaction

    NASA Astrophysics Data System (ADS)

    Bretherton, C. S.; Berner, A.; Wood, R.

    2012-12-01

    Large-eddy simulations (LES) of subtropical stratocumulus-topped boundary layers coupled to an interactive aerosol model are run for multiday periods to examine their coupled equilibria and adjustment timescales. The LES includes two-moment Morrison microphysics, interactive radiation, and Razzak-Ghan cloud droplet activation from a single log-normal size distribution of hygroscopic aerosol with prognosed total aerosol mass and number. The aerosol evolves due to surface and entrainment sources, dry coalescence, precipitation sinks coupled to the Morrison microphysics due to autoconversion and accretion of cloud droplets (and a source due to raindrop evaporation), and cloud and rain scavenging of interstitial aerosol. Simulations are initialized with an idealized southeast Pacific stratocumulus sounding based on observations during VOCALS REx and forced with specified SST, mean subsidence, geostrophic wind, and free-tropospheric aerosol concentration. The surface aerosol source is based on the Clarke parameterization for the dependence of sea-salt number concentration on wind speed. Both surface and free-tropospheric aerosol are assumed to quickly grow to a specified size due to a surface DMS source. The goal is to explore the adjustment timescales and long-term equilibria produced by this model, to compare with studies such as Wood et al. (2012) that postulate that remote marine boundary layer aerosol concentrations are controlled as much by the precipitation sink as the surface and entrainment sources. We show that the coupled cloud-aerosol model supports rapid transitions from a solid, high aerosol, stratocumulus-capped state to a cumulus-like state reminisniscent of pockets of open cells as the liquid water path rises above a threshold supporting sufficient precipitation. The system can support multiple long-term equilibria for the same boundary forcing, or slow oscillations between a collapsed POC-like state and a deepening, thickening stratocumulus

  18. Aerosol- and updraft-limited regimes of cloud droplet formation: influence of particle number, size and hygroscopicity on the activation of cloud condensation nuclei (CCN)

    NASA Astrophysics Data System (ADS)

    Reutter, P.; Su, H.; Trentmann, J.; Simmel, M.; Rose, D.; Gunthe, S. S.; Wernli, H.; Andreae, M. O.; Pöschl, U.

    2009-09-01

    We have investigated the formation of cloud droplets under pyro-convective conditions using a cloud parcel model with detailed spectral microphysics and with the κ-Köhler model approach for efficient and realistic description of the cloud condensation nucleus (CCN) activity of aerosol particles. Assuming a typical biomass burning aerosol size distribution (accumulation mode centred at 120 nm), we have calculated initial cloud droplet number concentrations (NCD) for a wide range of updraft velocities (w=0.25-20 m s-1) and aerosol particle number concentrations (NCN=200-105 cm-3) at the cloud base. Depending on the ratio between updraft velocity and particle number concentration (w/NCN), we found three distinctly different regimes of CCN activation and cloud droplet formation: (1) An aerosol-limited regime that is characterized by high w/NCN ratios (>≈10-3 m s-1 cm3), high maximum values of water vapour supersaturation (Smax>≈0.5%), and high activated fractions of aerosol particles (NCN/NCN>≈90%). In this regime NCD is directly proportional to NCN and practically independent of w. (2) An updraft-limited regime that is characterized by low w/NCN ratios (<≈10-4 m s-1 cm3), low maximum values of water vapour supersaturation (Smax<≈0.2%), and low activated fractions of aerosol particles (NCD/NCN<≈20%). In this regime NCD is directly proportional to w and practically independent of NCN. (3) An aerosol- and updraft-sensitive regime (transitional regime), which is characterized by parameter values in between the two other regimes and covers most of the conditions relevant for pyro-convection. In this regime NCD depends non-linearly on both NCN and w. In sensitivity studies we have tested the influence of aerosol particle size distribution and hygroscopicity on NCD. Within the range of effective hygroscopicity parameters that is characteristic for continental atmospheric aerosols (κ≈0.05-0.6), we found that NCD depends rather weakly on the actual value of κ

  19. A Comparative Study of Nucleation Parameterizations: 2. Three-Dimensional Model Application and Evaluation

    EPA Science Inventory

    Following the examination and evaluation of 12 nucleation parameterizations presented in part 1, 11 of them representing binary, ternary, kinetic, and cluster‐activated nucleation theories are evaluated in the U.S. Environmental Protection Agency Community Multiscale Air Quality ...

  20. A comparative study of nucleation parameterizations: 1. Examination and evaluation of the formulations

    NASA Astrophysics Data System (ADS)

    Zhang, Yang; McMurry, Peter H.; Yu, Fangqun; Jacobson, Mark Z.

    2010-10-01

    Large uncertainty exists in the nucleation parameterizations that may be propagated into climate change predictions through affecting aerosol direct and indirect effects. These parameterizations are derived either empirically from laboratory/field measurements or from theoretical models for nucleation rates. A total of 12 nucleation parameterizations (7 binary, 3 ternary, and 2 power laws) that are currently used in three-dimensional air quality models are examined comparatively under a variety of atmospheric conditions from polluted surface to very clean mesosphere environments and evaluated using observations from several laboratory experiments and a field campaign conducted in a sulfate-rich urban environment in the southeastern United States (i.e., Atlanta, Georgia). Significant differences (by up to 18 orders of magnitude) are found among the nucleation rates calculated with different parameterizations under the same meteorological and chemical conditions. All parameterizations give nucleation rates that increase with the number concentrations of sulfuric acid but differ in terms of the magnitude of such increases. Differences exist in their dependencies on temperatures, relative humidity, and the mixing ratios of ammonia in terms of both trends and magnitudes. Among the 12 parameterizations tested, the parameterizations of Kuang et al. (2008), Sihto et al. (2006), and Harrington and Kreidenweis (1998) give the best agreement with the observed nucleation rates in most laboratory studies and in Atlanta during a summer season field campaign and either do not exceed or rarely exceed the upper limits of the nucleation rates (i.e., the dimer formation rate) and new particle formation rates (i.e., the formation rate of particles with 2 nm diameter). They are thus the most plausible nucleation parameterizations for applications in the planetary boundary layer of polluted sulfate-rich urban areas. Limitation with the two power laws are that they were derived

  1. Chemical and physical influences on aerosol activation in liquid clouds: an empirical study based on observations from the Jungfraujoch, Switzerland

    NASA Astrophysics Data System (ADS)

    Hoyle, C. R.; Webster, C. S.; Rieder, H. E.; Hammer, E.; Gysel, M.; Bukowiecki, N.; Weingartner, E.; Steinbacher, M.; Baltensperger, U.

    2015-06-01

    A simple empirical model to predict the number of aerosols which activate to form cloud droplets in a warm, free tropospheric cloud has been established, based on data from four summertime Cloud and Aerosol Characterisation Experiments (CLACE) campaigns at the Jungfraujoch (JFJ). It is shown that 76% of the observed variance in droplet numbers can be represented by a model accounting only for the number of potential CCN (defined as number of particles larger than 90 nm in diameter), while the mean errors in the model representation may be reduced by the addition of further explanatory variables, such as the mixing ratios of O3, CO and the height of the measurements above cloud base. The model has similar ability to represent the observed droplet numbers in each of the individual years, as well as for the two predominant local wind directions at the JFJ (north west and south east). Given the central European location of the JFJ, with air masses in summer being representative of the free troposphere with regular boundary layer in-mixing via convection, we expect that this model is applicable to warm, free tropospheric clouds over the European continent.

  2. Methods of testing parameterizations: Vertical ocean mixing

    NASA Technical Reports Server (NTRS)

    Tziperman, Eli

    1992-01-01

    The ocean's velocity field is characterized by an exceptional variety of scales. While the small-scale oceanic turbulence responsible for the vertical mixing in the ocean is of scales a few centimeters and smaller, the oceanic general circulation is characterized by horizontal scales of thousands of kilometers. In oceanic general circulation models that are typically run today, the vertical structure of the ocean is represented by a few tens of discrete grid points. Such models cannot explicitly model the small-scale mixing processes, and must, therefore, find ways to parameterize them in terms of the larger-scale fields. Finding a parameterization that is both reliable and plausible to use in ocean models is not a simple task. Vertical mixing in the ocean is the combined result of many complex processes, and, in fact, mixing is one of the less known and less understood aspects of the oceanic circulation. In present models of the oceanic circulation, the many complex processes responsible for vertical mixing are often parameterized in an oversimplified manner. Yet, finding an adequate parameterization of vertical ocean mixing is crucial to the successful application of ocean models to climate studies. The results of general circulation models for quantities that are of particular interest to climate studies, such as the meridional heat flux carried by the ocean, are quite sensitive to the strength of the vertical mixing. We try to examine the difficulties in choosing an appropriate vertical mixing parameterization, and the methods that are available for validating different parameterizations by comparing model results to oceanographic data. First, some of the physical processes responsible for vertically mixing the ocean are briefly mentioned, and some possible approaches to the parameterization of these processes in oceanographic general circulation models are described in the following section. We then discuss the role of the vertical mixing in the physics of the

  3. Global modelling of direct and indirect effects of sea spray aerosol using a source function encapsulating wave state

    NASA Astrophysics Data System (ADS)

    Partanen, A.-I.; Dunne, E. M.; Bergman, T.; Laakso, A.; Kokkola, H.; Ovadnevaite, J.; Sogacheva, L.; Baisnée, D.; Sciare, J.; Manders, A.; O'Dowd, C.; de Leeuw, G.; Korhonen, H.

    2014-02-01

    Recently developed parameterizations for the sea spray aerosol source flux, encapsulating wave state, and its organic fraction were incorporated into the aerosol-climate model ECHAM-HAMMOZ to investigate the direct and indirect radiative effects of sea spray aerosol particles. Our simulated global sea salt emission of 805 Tg yr-1 (uncertainty range 378-1233 Tg yr-1) was much lower than typically found in previous studies. Modelled sea salt and sodium ion concentrations agreed relatively well with measurements in the smaller size ranges at Mace Head (annual normalized mean model bias -13% for particles with vacuum aerodynamic diameter Dva < 1 μm), Point Reyes (-29% for particles with aerodynamic diameter Da < 2.5 μm) and Amsterdam Island (-52% for particles with Da < 1 μm) but the larger sizes were overestimated (899% for particles with 2.5 μm aerosol at Mace Head (-82%) and Amsterdam Island (-68%). The large overestimation (212%) of organic matter at Point Reyes was due to the contribution of continental sources. At the remote Amsterdam Island site, the organic concentration was underestimated especially in the biologically active months, suggesting a need to improve the parameterization of the organic sea spray fraction. Globally, the satellite-retrieved AOD over the oceans, using PARASOL data, was underestimated by the model (means over ocean 0.16 and 0.10, respectively); however, in the pristine region around Amsterdam Island the measured AOD fell well within the simulated uncertainty range. The simulated sea spray aerosol contribution to the indirect radiative effect was positive (0.3 W m-2), in contrast to previous studies. This positive effect was ascribed to the tendency of sea salt aerosol to

  4. Global modelling of direct and indirect effects of sea spray aerosol using a source function encapsulating wave state

    NASA Astrophysics Data System (ADS)

    Partanen, A.-I.; Dunne, E. M.; Bergman, T.; Laakso, A.; Kokkola, H.; Ovadnevaite, J.; Sogacheva, L.; Baisnée, D.; Sciare, J.; Manders, A.; O'Dowd, C.; de Leeuw, G.; Korhonen, H.

    2014-11-01

    Recently developed parameterizations for the sea spray aerosol source flux, encapsulating wave state, and its organic fraction were incorporated into the aerosol-climate model ECHAM-HAMMOZ to investigate the direct and indirect radiative effects of sea spray aerosol particles. Our simulated global sea salt emission of 805 Tg yr-1 (uncertainty range 378-1233 Tg yr-1) was much lower than typically found in previous studies. Modelled sea salt and sodium ion concentrations agreed relatively well with measurements in the smaller size ranges at Mace Head (annual normalized mean model bias -13% for particles with vacuum aerodynamic diameter Dva < 1 μm), Point Reyes (-29% for particles with aerodynamic diameter Da < 2.5 μm) and Amsterdam Island (-52% for particles with Da < 1 μm) but the larger sizes were overestimated (899% for particles with 2.5 μm < Da < 10 μm) at Amsterdam Island. This suggests that at least the high end of the previous estimates of sea spray mass emissions is unrealistic. On the other hand, the model clearly underestimated the observed concentrations of organic or total carbonaceous aerosol at Mace Head (-82%) and Amsterdam Island (-68%). The large overestimation (212%) of organic matter at Point Reyes was due to the contribution of continental sources. At the remote Amsterdam Island site, the organic concentration was underestimated especially in the biologically active months, suggesting a need to improve the parameterization of the organic sea spray fraction. Globally, the satellite-retrieved AOD over the oceans, using PARASOL data, was underestimated by the model (means over ocean 0.16 and 0.10, respectively); however, in the pristine region around Amsterdam Island the measured AOD fell well within the simulated uncertainty range. The simulated sea spray aerosol contribution to the indirect radiative effect was positive (0.3 W m-2), in contrast to previous studies. This positive effect was ascribed to the tendency of sea salt aerosol to

  5. Contribution to the cloud droplet effective radius parameterization

    SciTech Connect

    Pontikis, C.; Hicks, E. )

    1992-11-01

    An analytic cloud droplet effective radius expression is derived and validated by using field experiment microphysical data. This expression shows that the effective radius depends simultaneously upon the cloud liquid water content, droplet concentration and droplet spectral dispersion. It further suggests that the variability in these parameters present at all scales, due to turbulent mixing and secondary droplet activation, could limit the accuracy of the effective radius parameterizations used in climate models. 12 refs.

  6. Shortwave radiation parameterization scheme for subgrid topography

    NASA Astrophysics Data System (ADS)

    Helbig, N.; LöWe, H.

    2012-02-01

    Topography is well known to alter the shortwave radiation balance at the surface. A detailed radiation balance is therefore required in mountainous terrain. In order to maintain the computational performance of large-scale models while at the same time increasing grid resolutions, subgrid parameterizations are gaining more importance. A complete radiation parameterization scheme for subgrid topography accounting for shading, limited sky view, and terrain reflections is presented. Each radiative flux is parameterized individually as a function of sky view factor, slope and sun elevation angle, and albedo. We validated the parameterization with domain-averaged values computed from a distributed radiation model which includes a detailed shortwave radiation balance. Furthermore, we quantify the individual topographic impacts on the shortwave radiation balance. Rather than using a limited set of real topographies we used a large ensemble of simulated topographies with a wide range of typical terrain characteristics to study all topographic influences on the radiation balance. To this end slopes and partial derivatives of seven real topographies from Switzerland and the United States were analyzed and Gaussian statistics were found to best approximate real topographies. Parameterized direct beam radiation presented previously compared well with modeled values over the entire range of slope angles. The approximation of multiple, anisotropic terrain reflections with single, isotropic terrain reflections was confirmed as long as domain-averaged values are considered. The validation of all parameterized radiative fluxes showed that it is indeed not necessary to compute subgrid fluxes in order to account for all topographic influences in large grid sizes.

  7. Ceilometer for aerosol profiling: comparison with the multiwavelength in the frame of INTERACT (INTERcomparison of Aerosol and Cloud Tracking)

    NASA Astrophysics Data System (ADS)

    Madonna, Fabio; Vande Hey, Joshua; Rosoldi, Marco; Amato, Francesco; Pappalardo, Gelsomina

    2015-04-01

    Observations of cloud base height are important for meteorology, observations of aerosols are important for air quality applications, observations of cloud cover and aerosols address key uncertainties in climate study. To improve parameterization and uncertainties of numerical models, observations provided by high resolution networks of ground-based instruments are needed. In order to achieve broad, high resolution coverage, low-cost instruments are preferable, though it is essential that the sensitivity, stability, biases and uncertainties of these instruments are well-understood. Despite of their differences from more advanced and more powerful lidars, low construction and operation cost of ceilometer, originally designed for cloud base height monitoring, has fostered their use for the quantitative study of aerosol properties. The large number of ceilometers available worldwide represent a strong motivation to investigate to which extent they can be used to fill the geographical gaps between advanced lidar stations and how their continuous data flow can be linked to existing networks of the advanced lidars, like EARLINET (European Aerosol research LIdar NETwork). In order to make the best use of existing and future ceilometer deployments, ceilometer must be better characterized. This is the purpose of the INTERACT campaign carried out in the frame of ACTRIS Transnational Access activities at CNR-IMAA Atmospheric Observatory (CIAO - 760 m a.s.l., 40.60 N, 15.72 E). In this paper, an overview of the results achieved during the campaign is provided. In particular multi-wavelength Raman lidar measurements are used to investigate the capability of ceilometers to provide reliable information about atmospheric aerosol content through the INTERACT (INTERcomparison of Aerosol and Cloud Tracking) campaign carried out at the CNR-IMAA Atmospheric Observatory (760 m a.s.l., 40.60N, 15.72E), in the framework of ACTRIS (Aerosol Clouds Trace gases Research InfraStructure) FP7

  8. Meteorological and aerosol effects on marine cloud microphysical properties

    NASA Astrophysics Data System (ADS)

    Sanchez, K. J.; Russell, L. M.; Modini, R. L.; Frossard, A. A.; Ahlm, L.; Corrigan, C. E.; Roberts, G. C.; Hawkins, L. N.; Schroder, J. C.; Bertram, A. K.; Zhao, R.; Lee, A. K. Y.; Lin, J. J.; Nenes, A.; Wang, Z.; Wonaschütz, A.; Sorooshian, A.; Noone, K. J.; Jonsson, H.; Toom, D.; Macdonald, A. M.; Leaitch, W. R.; Seinfeld, J. H.

    2016-04-01

    Meteorology and microphysics affect cloud formation, cloud droplet distributions, and shortwave reflectance. The Eastern Pacific Emitted Aerosol Cloud Experiment and the Stratocumulus Observations of Los-Angeles Emissions Derived Aerosol-Droplets studies provided measurements in six case studies of cloud thermodynamic properties, initial particle number distribution and composition, and cloud drop distribution. In this study, we use simulations from a chemical and microphysical aerosol-cloud parcel (ACP) model with explicit kinetic drop activation to reproduce observed cloud droplet distributions of the case studies. Four cases had subadiabatic lapse rates, resulting in fewer activated droplets, lower liquid water content, and higher cloud base height than an adiabatic lapse rate. A weighted ensemble of simulations that reflect measured variation in updraft velocity and cloud base height was used to reproduce observed droplet distributions. Simulations show that organic hygroscopicity in internally mixed cases causes small effects on cloud reflectivity (CR) (<0.01), except for cargo ship and smoke plumes, which increased CR by 0.02 and 0.07, respectively, owing to their high organic mass fraction. Organic hygroscopicity had larger effects on droplet concentrations for cases with higher aerosol concentrations near the critical diameter (namely, polluted cases with a modal peak near 0.1 µm). Differences in simulated droplet spectral widths (k) caused larger differences in CR than organic hygroscopicity in cases with organic mass fractions of 60% or less for the cases shown. Finally, simulations from a numerical parameterization of cloud droplet activation suitable for general circulation models compared well with the ACP model, except under high organic mass fraction.

  9. Parameterizing Size Distribution in Ice Clouds

    SciTech Connect

    DeSlover, Daniel; Mitchell, David L.

    2009-09-25

    cloud optical properties formulated in terms of PSD parameters in combination with remote measurements of thermal radiances to characterize the small mode. This is possible since the absorption efficiency (Qabs) of small mode crystals is larger at 12 µm wavelength relative to 11 µm wavelength due to the process of wave resonance or photon tunneling more active at 12 µm. This makes the 12/11 µm absorption optical depth ratio (or equivalently the 12/11 µm Qabs ratio) a means for detecting the relative concentration of small ice particles in cirrus. Using this principle, this project tested and developed PSD schemes that can help characterize cirrus clouds at each of the three ARM sites: SGP, NSA and TWP. This was the main effort of this project. These PSD schemes and ice sedimentation velocities predicted from them have been used to test the new cirrus microphysics parameterization in the GCM known as the Community Climate Systems Model (CCSM) as part of an ongoing collaboration with NCAR. Regarding the second problem, we developed and did preliminary testing on a passive thermal method for retrieving the total water path (TWP) of Arctic mixed phase clouds where TWPs are often in the range of 20 to 130 g m-2 (difficult for microwave radiometers to accurately measure). We also developed a new radar method for retrieving the cloud ice water content (IWC), which can be vertically integrated to yield the ice water path (IWP). These techniques were combined to determine the IWP and liquid water path (LWP) in Arctic clouds, and hence the fraction of ice and liquid water. We have tested this approach using a case study from the ARM field campaign called M-PACE (Mixed-Phase Arctic Cloud Experiment). This research led to a new satellite remote sensing method that appears promising for detecting low levels of liquid water in high clouds typically between -20 and -36 oC. We hope to develop this method in future research.

  10. The dynamical core, physical parameterizations, and basic simulation characteristics of the atmospheric component AM3 of the GFDL global coupled model CM3

    USGS Publications Warehouse

    Donner, L.J.; Wyman, B.L.; Hemler, R.S.; Horowitz, L.W.; Ming, Y.; Zhao, M.; Golaz, J.-C.; Ginoux, P.; Lin, S.-J.; Schwarzkopf, M.D.; Austin, J.; Alaka, G.; Cooke, W.F.; Delworth, T.L.; Freidenreich, S.M.; Gordon, C.T.; Griffies, S.M.; Held, I.M.; Hurlin, W.J.; Klein, S.A.; Knutson, T.R.; Langenhorst, A.R.; Lee, H.-C.; Lin, Y.; Magi, B.I.; Malyshev, S.L.; Milly, P.C.D.; Naik, V.; Nath, M.J.; Pincus, R.; Ploshay, J.J.; Ramaswamy, V.; Seman, C.J.; Shevliakova, E.; Sirutis, J.J.; Stern, W.F.; Stouffer, R.J.; Wilson, R.J.; Winton, M.; Wittenberg, A.T.; Zeng, F.

    2011-01-01

    The Geophysical Fluid Dynamics Laboratory (GFDL) has developed a coupled general circulation model (CM3) for the atmosphere, oceans, land, and sea ice. The goal of CM3 is to address emerging issues in climate change, including aerosol-cloud interactions, chemistry-climate interactions, and coupling between the troposphere and stratosphere. The model is also designed to serve as the physical system component of earth system models and models for decadal prediction in the near-term future-for example, through improved simulations in tropical land precipitation relative to earlier-generation GFDL models. This paper describes the dynamical core, physical parameterizations, and basic simulation characteristics of the atmospheric component (AM3) of this model. Relative to GFDL AM2, AM3 includes new treatments of deep and shallow cumulus convection, cloud droplet activation by aerosols, subgrid variability of stratiform vertical velocities for droplet activation, and atmospheric chemistry driven by emissions with advective, convective, and turbulent transport. AM3 employs a cubed-sphere implementation of a finite-volume dynamical core and is coupled to LM3, a new land model with ecosystem dynamics and hydrology. Its horizontal resolution is approximately 200 km, and its vertical resolution ranges approximately from 70 m near the earth's surface to 1 to 1.5 km near the tropopause and 3 to 4 km in much of the stratosphere. Most basic circulation features in AM3 are simulated as realistically, or more so, as in AM2. In particular, dry biases have been reduced over South America. In coupled mode, the simulation of Arctic sea ice concentration has improved. AM3 aerosol optical depths, scattering properties, and surface clear-sky downward shortwave radiation are more realistic than in AM2. The simulation of marine stratocumulus decks remains problematic, as in AM2. The most intense 0.2% of precipitation rates occur less frequently in AM3 than observed. The last two decades of

  11. Evaluating WRF-Chem aerosol indirect effects in Southeast Pacific marine stratocumulus during VOCALS-REx

    SciTech Connect

    Saide P. E.; Springston S.; Spak, S. N.; Carmichael, G. R.; Mena-Carrasco, M. A.; Yang, Q.; Howell, S.; Leon, D. C.; Snider, J. R.; Bandy, A. R.; Collett, J. L.; Benedict, K. B.; de Szoeke, S. P.; Hawkins, L. N.; Allen, G.; Crawford, I.; Crosier, J.

    2012-03-29

    We evaluate a regional-scale simulation with the WRF-Chem model for the VAMOS (Variability of the American Monsoon Systems) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx), which sampled the Southeast Pacific's persistent stratocumulus deck. Evaluation of VOCALS-REx ship-based and three aircraft observations focuses on analyzing how aerosol loading affects marine boundary layer (MBL) dynamics and cloud microphysics. We compare local time series and campaign-averaged longitudinal gradients, and highlight differences in model simulations with (W) and without (NW) wet deposition processes. The higher aerosol loadings in the NW case produce considerable changes in MBL dynamics and cloud microphysics, in accordance with the established conceptual model of aerosol indirect effects. These include increase in cloud albedo, increase in MBL and cloud heights, drizzle suppression, increase in liquid water content, and increase in cloud lifetime. Moreover, better statistical representation of aerosol mass and number concentration improves model fidelity in reproducing observed spatial and temporal variability in cloud properties, including top and base height, droplet concentration, water content, rain rate, optical depth (COD) and liquid water path (LWP). Together, these help to quantify confidence in WRF-Chem's modeled aerosol-cloud interactions, especially in the activation parameterization, while identifying structural and parametric uncertainties including: irreversibility in rain wet removal; overestimation of marine DMS and sea salt emissions, and accelerated aqueous sulfate conversion. Our findings suggest that WRF-Chem simulates marine cloud-aerosol interactions at a level sufficient for applications in forecasting weather and air quality and studying aerosol climate forcing, and may do so with the reliability required for policy analysis.

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  13. A Physically Based Framework for Modelling the Organic Fractionation of Sea Spray Aerosol from Bubble Film Langmuir Equilibria

    SciTech Connect

    Burrows, Susannah M.; Ogunro, O.; Frossard, Amanda; Russell, Lynn M.; Rasch, Philip J.; Elliott, S.

    2014-12-19

    The presence of a large fraction of organic matter in primary sea spray aerosol (SSA) can strongly affect its cloud condensation nuclei activity and interactions with marine clouds. Global climate models require new parameterizations of the SSA composition in order to improve the representation of these processes. Existing proposals for such a parameterization use remotely-sensed chlorophyll-a concentrations as a proxy for the biogenic contribution to the aerosol. However, both observations and theoretical considerations suggest that existing relationships with chlorophyll-a, derived from observations at only a few locations, may not be representative for all ocean regions. We introduce a novel framework for parameterizing the fractionation of marine organic matter into SSA based on a competitive Langmuir adsorption equilibrium at bubble surfaces. Marine organic matter is partitioned into classes with differing molecular weights, surface excesses, and Langmuir adsorption parameters. The classes include a lipid-like mixture associated with labile dissolved organic carbon (DOC), a polysaccharide-like mixture associated primarily with semi-labile DOC, a protein-like mixture with concentrations intermediate between lipids and polysaccharides, a processed mixture associated with recalcitrant surface DOC, and a deep abyssal humic-like mixture. Box model calculations have been performed for several cases of organic adsorption to illustrate the underlying concepts. We then apply the framework to output from a global marine biogeochemistry model, by partitioning total dissolved organic carbon into several classes of macromolecule. Each class is represented by model compounds with physical and chemical properties based on existing laboratory data. This allows us to globally map the predicted organic mass fraction of the nascent submicron sea spray aerosol. Predicted relationships between chlorophyll-\\textit{a} and organic fraction are similar to existing empirical

  14. Coagulation effect on the activity size distributions of long lived radon progeny aerosols and its application to atmospheric residence time estimation techniques.

    PubMed

    Anand, S; Mayya, Y S

    2015-03-01

    The long lived naturally occurring radon progeny species in the atmosphere, namely (210)Pb, (210)Bi and (210)Po, have been used as important tracers for understanding the atmospheric mixing processes and estimating aerosol residence times. Several observations in the past have shown that the activity size distribution of these species peaks at larger particle sizes as compared to the short lived radon progeny species - an effect that has been attributed to the process of coagulation of the background aerosols to which they are attached. To address this issue, a mathematical equation is derived for the activity-size distribution of tracer species by formulating a generalized distribution function for the number of tracer atoms present in coagulating background particles in the presence of radioactive decay and removal. A set of these equations is numerically solved for the progeny chain using Fuchs coagulation kernel combined with a realistic steady-state aerosol size spectrum that includes nucleation, accumulation and coarse mode components. The important findings are: (i) larger shifts in the modal sizes of (210)Pb and (210)Po at higher aerosol concentrations such as that found in certain Asian urban regions (ii) enrichment of tracer specific activity on particles as compared to that predicted by pure attachment laws (iii) sharp decline of daughter-to-parent activity ratios for decreasing particle sizes. The implication of the results to size-fractionated residence time estimation techniques is highlighted. A coagulation corrected graphical approach is presented for estimating the residence times from the size-segregated activity ratios of (210)Bi and (210)Po with respect to (210)Pb. The discrepancy between the residence times predicted by conventional formula and the coagulation corrected approach for specified activity ratios increases at higher atmospheric aerosol number concentrations (>10(10) #/m(3)) for smaller sizes (<1 μm). The results are further

  15. Type-segregated aerosol effects on regional monsoon activity: A study using ground-based experiments and model simulations

    NASA Astrophysics Data System (ADS)

    Vijayakumar, K.; Devara, P. C. S.; Sonbawne, S. M.

    2014-12-01

    Classification of observed aerosols into key types [e.g., clean-maritime (CM), desert-dust (DD), urban-industrial/biomass-burning (UI/BB), black carbon (BC), organic carbon (OC) and mixed-type aerosols (MA)] would facilitate to infer aerosol sources, effects, and feedback mechanisms, not only to improve the accuracy of satellite retrievals but also to quantify the assessment of aerosol radiative impacts on climate. In this paper, we report the results of a study conducted in this direction, employing a Cimel Sun-sky radiometer at the Indian Institute of Tropical Meteorology (IITM), Pune, India during 2008 and 2009, which represent two successive contrasting monsoon years. The study provided an observational evidence to show that the local sources are subject to heavy loading of absorbing aerosols (dust and black carbon), with strong seasonality closely linked to the monsoon annual rainfall cycle over Pune, a tropical urban station in India. The results revealed the absence of CM aerosols in the pre-monsoon as well as in the monsoon seasons of 2009 as opposed to 2008. Higher loading of dust aerosols is observed in the pre-monsoon and monsoon seasons of 2009; majority may be coated with fine BC aerosols from local emissions, leading to reduction in regional rainfall. Further, significant decrease in coarse-mode AOD and presence of carbonaceous aerosols, affecting the aerosol-cloud interaction and monsoon-rain processes via microphysics and dynamics, is considered responsible for the reduction in rainfall during 2009. Additionally, we discuss how optical depth, contributed by different types of aerosols, influences the distribution of monsoon rainfall over an urban region using the Monitoring Atmospheric Composition and Climate (MACC) aerosol reanalysis. Furthermore, predictions of the Dust REgional Atmospheric Model (DREAM) simulations combined with HYSPLIT (HYbrid Single Particle Lagrangian Integrated Trajectory) cluster model are also discussed in support of the

  16. Parameter sensitivity study of Arctic aerosol vertical distribution in CAM5

    NASA Astrophysics Data System (ADS)

    Jiao, C.; Flanner, M.

    2015-12-01

    Arctic surface temperature response to light-absorbing aerosols (black carbon, brown carbon and dust) depends strongly on their vertical distributions. Improving model simulations of three dimensional aerosol fields in the remote Arctic region will therefore lead to improved projections of the climate change caused by aerosol emissions. In this study, we investigate how different physical parameterizations in the Community Atmosphere Model version 5 (CAM5) influence the simulated vertical distribution of Arctic aerosols. We design experiments to test the sensitivity of the simulated aerosol fields to perturbations of selected aerosol process-related parameters in the Modal Aerosol Module with seven lognormal modes (MAM7), such as those govern aerosol aging, in-cloud and below-cloud scavenging, aerosol hygroscopicity and so on. The simulations are compared with observed aerosol vertical distributions and total optical depth to assess model performance and quantify uncertainties associated with these model parameterizations. Observations applied here include Arctic aircraft measurements of black carbon and sulfate vertical profiles, along with Aerosol Robotic Network (AERONET) optical depth measurements. We also assess the utility of using High Spectral Resolution Lidar (HSRL) measurements from the ARM Barrow site to infer vertical profiles of aerosol extinction. The sensitivity study explored here will provide guidance for optimizing global aerosol simulations.

  17. Predicting/Extrapolating Active Layer Thickness Using Statistical Learning from Remotely-Sensed High-resolution Data in Arctic Permafrost Landscapes: Improved parameterization of Ice-wedge polygons from LiDAR/WorldView-2 derived metrics

    NASA Astrophysics Data System (ADS)

    Gangodagamage, C.; Rowland, J. C.; Hubbard, S. S.; Brumby, S. P.; Liljedahl, A.; Wainwright, H. M.; Sloan, V. L.; Altmann, G.; Skurikhin, A. N.; Shelef, E.; Wilson, C. J.; Dafflon, B.; Peterson, J.; Ulrich, C.; Gibbs, A.; Tweedie, C. E.; Painter, S. L.; Wullschleger, S. D.

    2014-12-01

    Landscape attributes that vary with micro-topography, such as active layer thickness (ALT) in ice-wedge polygon ground, are labor-intensive to document in the field at large spatial extents, necessitating remotely sensed methods. Robust techniques to estimate ALT over large areas would improve understanding of coupled dynamics between permafrost, hydrology and landsurface processes, and improve simulations of the rate and timing of release of soil carbon from permafrost settings. In particular, it would provide critically needed data to parameterize and initialize soil property information in permafrost models and evaluate model predictions for large, complex domains. In this work, we demonstrate a new data fusion approach using high-resolution remotely sensed data for estimating cm scale ALT in a 5 km2 area of ice-wedge polygon terrain in Barrow, Alaska. We used topographic (directed distance, slope, wavelet-curvature) and spectral (NDVI) metrics derived from multisensor data obtained from LiDAR and WorldView-2 platforms to develop a simple data fusion algorithm using statistical machine learning. This algorithm was used to estimate ALT (2 m spatial resolution) across the study area. A comparison of the estimates with ground-based measurements documented the accuracy (±4.4 cm, r2=0.76) of the approach. Our findings suggest that the broad climatic variability associated with warming air temperature will govern the regional averages of ALT, but the smaller-scale variability could be controlled by local eco-hydro-geomorphic variables. This work demonstrates a path forward for mapping subsurface properties over large areas from readily available remote sensing data. Methodology of Mapping and Characterization Polygons:We convolve LiDAR elevations with multiscale wavelets and objectively chose appropriate scales to map interconnected troughs of high- and low-centered polygons. For the ice wedges where LiDAR surface expressions (troughs) are not well developed, we used

  18. Modeling the Absorbing Aerosol Index

    NASA Technical Reports Server (NTRS)

    Penner, Joyce; Zhang, Sophia

    2003-01-01

    We propose a scheme to model the absorbing aerosol index and improve the biomass carbon inventories by optimizing the difference between TOMS aerosol index (AI) and modeled AI with an inverse model. Two absorbing aerosol types are considered, including biomass carbon and mineral dust. A priori biomass carbon source was generated by Liousse et al [1996]. Mineral dust emission is parameterized according to surface wind and soil moisture using the method developed by Ginoux [2000]. In this initial study, the coupled CCM1 and GRANTOUR model was used to determine the aerosol spatial and temporal distribution. With modeled aerosol concentrations and optical properties, we calculate the radiance at the top of the atmosphere at 340 nm and 380 nm with a radiative transfer model. The contrast of radiance at these two wavelengths will be used to calculate AI. Then we compare the modeled AI with TOMS AI. This paper reports our initial modeling for AI and its comparison with TOMS Nimbus 7 AI. For our follow-on project we will model the global AI with aerosol spatial and temporal distribution recomputed from the IMPACT model and DAO GEOS-1 meteorology fields. Then we will build an inverse model, which applies a Bayesian inverse technique to optimize the agreement of between model and observational data. The inverse model will tune the biomass burning source strength to reduce the difference between modelled AI and TOMS AI. Further simulations with a posteriori biomass carbon sources from the inverse model will be carried out. Results will be compared to available observations such as surface concentration and aerosol optical depth.

  19. MIRAGE: Model Description and Evaluation of Aerosols and Trace Gases

    SciTech Connect

    Easter, Richard C.; Ghan, Steven J.; Zhang, Yang; Saylor, Rick D.; Chapman, Elaine G.; Laulainen, Nels S.; Abdul-Razzak, Hayder; Leung, Lai-Yung R.; Bian, Xindi; Zaveri, Rahul A.

    2004-10-27

    The MIRAGE (Model for Integrated Research on Atmospheric Global Exchanges) modeling system, designed to study the impacts of anthropogenic aerosols on the global environment, is described. MIRAGE consists of a chemical transport model coupled on line with a global climate model. The chemical transport model simulates trace gases, aerosol number, and aerosol chemical component mass [sulfate, MSA, organic matter, black carbon (BC), sea salt, mineral dust] for four aerosol modes (Aitken, accumulation, coarse sea salt, coarse mineral dust) using the modal aerosol dynamics approach. Cloud-phase and interstitial aerosol are predicted separately. The climate model, based on the CCM2, has physically-based treatments of aerosol direct and indirect forcing. Stratiform cloud water and droplet number are simulated using a bulk microphysics parameterization that includes aerosol activation. Aerosol and trace gas species simulated by MIRAGE are presented and evaluated using surface and aircraft measurements. Surface-level SO2 in N. American and European source regions is higher than observed. SO2 above the boundary layer is in better agreement with observations, and surface-level SO2 at marine locations is somewhat lower than observed. Comparison with other models suggests insufficient SO2 dry deposition; increasing the deposition velocity improves simulated SO2. Surface-level sulfate in N. American and European source regions is in good agreement with observations, although the seasonal cycle in Europe is stronger than observed. Surface-level sulfate at high-latitude and marine locations, and sulfate above the boundary layer, are higher than observed. This is attributed primarily to insufficient wet removal; increasing the wet removal improves simulated sulfate at remote locations and aloft. Because of the high sulfate bias, radiative forcing estimates for anthropogenic sulfur in Ghan et al. [2001c] are probably too high. Surface-level DMS is {approx}40% higher than observed

  20. Accounting for dust aerosol size distribution in radiative transfer

    NASA Astrophysics Data System (ADS)

    Li, Jiangnan; Min, Qilong; Peng, Yiran; Sun, Zhian; Zhao, Jian-Qi

    2015-07-01

    The impact of size distribution of mineral dust aerosol on radiative transfer was investigated using the Aerosol Robotic Network-retrieved aerosol size distributions. Three methods for determining the aerosol optical properties using size distributions were discussed. The first is referred to as a bin method in which the aerosol optical properties are determined for each bin of the size distribution. The second is named as an assembly mean method in which the aerosol optical properties are determined with an integration of the aerosol optical parameters over the observed size distribution. The third is a normal parameterization method based on an assumed size distribution. The bin method was used to generate the benchmark results in the radiation calculations against the methods of the assembly mean, and parameterizations based on two size distribution functions, namely, lognormal and gamma were examined. It is seen that the assembly mean method can produce aerosol radiative forcing with accuracy of better than 1%. The accuracies of the parameterizations based on lognormal and gamma size distributions are about 25% and 5%, respectively. Both the lognormal and gamma size distributions can be determined by two parameters, the effective radius and effective variance. The better results from the gamma size distribution can be explained by a third parameter of skewness which is found to be useful for judging how close the assumed distribution is to the observation result. The parameterizations based on the two assumed size distributions are also evaluated in a climate model. The results show that the reflected solar fluxes over the desert areas determined by the scheme based on the gamma size distribution are about 1 W m-2 less than those from the scheme based on the lognormal size distribution, bringing the model results closer to the observations.

  1. What We Can Say About the Roles of Natural and Anthropogenic Aerosols in Climate Change

    NASA Astrophysics Data System (ADS)

    Kahn, Ralph

    2016-07-01

    Although particles from natural sources dominate the globally averaged aerosol load, it is widely understood that human activity has added significantly to the atmospheric aerosol inventory in many regions. Anthropogenic contributions include pollution particles from industrial activity, transportation, cook-stoves, and other combustion sources, smoke from agricultural fires and those wildfires that result from land-management practices, soil and mineral dust mobilized in regions where overgrazing, severe tilling, or overuse of surface water resources have occurred, and biogenic particles from vegetation planted and maintained by the populance. The history of human influence is complex - in the 18th and 19th centuries agricultural burning tended to dominate the anthropogenic component in most places, whereas more recently, fossil fuel combustion leads the human contribution is many areas. However, identifying and quantifying the anthropogenic aerosol component on global scales is a challenging endeavor at present. Most estimates of the anthropogenic component come from aerosol transport models that are initialized with aerosol and precursor-gas source locations, emission strengths, and injection heights. The aerosol is then advected based on meteorological modeling, possibly modified chemically or physically, and removed by parameterized wet or dry deposition processes. Aerosol effects on clouds are also represented in some climate models, but with even greater uncertainty than the direct aerosol effects on Earth's radiation balance. Even for present conditions, aerosol source inventories are deduced from whatever constraints can be found, along with much creativity and many assumptions. Aerosol amount (i.e., aerosol optical depth) is routinely measured globally from space, but observational constraints on the anthropogenic component require some knowledge of the aerosol type as well, a much more difficult quantity to derive. As large-swath, multi-spectral, single

  2. Final Report for Research Conducted at The Scripps Institution of Oceanography, University of California San Diego from 2/2002 to 8/2003 for ''Aerosol and Cloud-Field Radiative Effects in the Tropical Western Pacific: Analyses and General Circulation Model Parameterizations''

    SciTech Connect

    Vogelmann, A. M.

    2004-01-27

    OAK-B135 Final report from the University of California San Diego for an ongoing research project that was moved to Brookhaven National Laboratory where proposed work will be completed. The research uses measurements made by the Atmospheric Radiation Measurement (ARM) Program to quantify the effects of aerosols and clouds on the Earth's energy balance in the climatically important Tropical Western Pacific.

  3. Antibodies to Bordetella pertussis in human colostrum and their protective activity against aerosol infection of mice.

    PubMed Central

    Oda, M; Cowell, J L; Burstyn, D G; Thaib, S; Manclark, C R

    1985-01-01

    Colostrum samples from Indonesian mothers were assayed for antibodies which agglutinate Bordetella pertussis and for antibodies to the filamentous hemagglutinin and the lymphocytosis-promoting factor of B. pertussis. Agglutinins were assayed by a microtiter method, and 36 of 58 samples tested (62%) had titers above 1:10 (range, less than 1:10 to 1:160). An enzyme-linked immunosorbent assay detected anti-filamentous hemagglutinin in 39 of 60 samples (65%) and anti-lymphocytosis-promoting factor in 26 of 60 samples assayed (43%). A total of 52 samples (87%) were positive for at least one of these antibodies. Pooled colostrum samples were separated by affinity chromatography into fractions enriched secretory immunoglobulin A (sIgA) or IgG and examined for their ability to passively protect suckling mice from aerosol challenge with B. pertussis. Samples (160 micrograms of protein) were given intraperitoneally 90 min before challenge. Death, rate of gain in body weight, and leukocytosis were used as indicators of illness. Colostrum containing anti-lymphocytosis-promoting factor or agglutinins was protective, whereas colostrum lacking these but containing anti-filamentous hemagglutinin gave little protection. The sIgA-enriched and IgG-enriched fractions appeared to be equal in their ability to protect against respiratory challenge with B. pertussis. PMID:2857154

  4. POET: Parameterized Optimization for Empirical Tuning

    SciTech Connect

    Yi, Q; Seymour, K; You, H; Vuduc, R; Quinlan, D

    2007-01-29

    The excessive complexity of both machine architectures and applications have made it difficult for compilers to statically model and predict application behavior. This observation motivates the recent interest in performance tuning using empirical techniques. We present a new embedded scripting language, POET (Parameterized Optimization for Empirical Tuning), for parameterizing complex code transformations so that they can be empirically tuned. The POET language aims to significantly improve the generality, flexibility, and efficiency of existing empirical tuning systems. We have used the language to parameterize and to empirically tune three loop optimizations-interchange, blocking, and unrolling-for two linear algebra kernels. We show experimentally that the time required to tune these optimizations using POET, which does not require any program analysis, is significantly shorter than that when using a full compiler-based source-code optimizer which performs sophisticated program analysis and optimizations.

  5. Effect of aerosol immunization with RE 595 Salmonella minnesota on lung bactericidal activity against Serratia marcescens, Enterobacter cloacae, and Pseudomonas aeruginosa.

    PubMed

    LaForce, F M

    1977-08-01

    Intrapulmonary bactericidal activity was measured after mice were given 3 weekly aerosol exposures to acid-hydrolyzed Re 595 Salmonella minnesota. Ten days after their last immunization, mice were challenged with aerolized Serratia marcescens, Enterobacter cloacae, or Pseudomonas aeruginosa. Quantitative bacterial counts in ground lung were obtained immediately after exposure and again 4 hours later. Enhanced bactericidal activity against Serratia marcescens and Enterobacter cloacae was seen in immunized animals, whereas no difference with Pseudomonas aeruginosa was noted. In separate studies, immunization with Serratia marcescens yielded a similar enhancement of lung bactericidal activity. Mucociliary transport, as measured by disappearance of aerosolized Serratia marcescens labeled with phosphorus-32, was identical for both immunized and control animals. Using a standardized in vitro mouse alveolar macrophage phagocytic system, lung washes from animals immunized with Re 595 Salmonella minnesota had significant opsonic activity for Serratia marcescens but not for Pseudomonas aeruginosa. PMID:407823

  6. Evaluating Aerosol Process Modules within the Framework of the Aerosol Modeling Testbed

    NASA Astrophysics Data System (ADS)

    Fast, J. D.; Velu, V.; Gustafson, W. I.; Chapman, E.; Easter, R. C.; Shrivastava, M.; Singh, B.

    2012-12-01

    Factors that influence predictions of aerosol direct and indirect forcing, such as aerosol mass, composition, size distribution, hygroscopicity, and optical properties, still contain large uncertainties in both regional and global models. New aerosol treatments are usually implemented into a 3-D atmospheric model and evaluated using a limited number of measurements from a specific case study. Under this modeling paradigm, the performance and computational efficiency of several treatments for a specific aerosol process cannot be adequately quantified because many other processes among various modeling studies (e.g. grid configuration, meteorology, emission rates) are different as well. The scientific community needs to know the advantages and disadvantages of specific aerosol treatments when the meteorology, chemistry, and other aerosol processes are identical in order to reduce the uncertainties associated with aerosols predictions. To address these issues, an Aerosol Modeling Testbed (AMT) has been developed that systematically and objectively evaluates new aerosol treatments for use in regional and global models. The AMT consists of the modular Weather Research and Forecasting (WRF) model, a series testbed cases for which extensive in situ and remote sensing measurements of meteorological, trace gas, and aerosol properties are available, and a suite of tools to evaluate the performance of meteorological, chemical, aerosol process modules. WRF contains various parameterizations of meteorological, chemical, and aerosol processes and includes interactive aerosol-cloud-radiation treatments similar to those employed by climate models. In addition, the physics suite from the Community Atmosphere Model version 5 (CAM5) have also been ported to WRF so that they can be tested at various spatial scales and compared directly with field campaign data and other parameterizations commonly used by the mesoscale modeling community. Data from several campaigns, including the 2006

  7. Impact of Aerosol Processing on Orographic Clouds

    NASA Astrophysics Data System (ADS)

    Pousse-Nottelmann, Sara; Zubler, Elias M.; Lohmann, Ulrike

    2010-05-01

    Aerosol particles undergo significant modifications during their residence time in the atmosphere. Physical processes like coagulation, coating and water uptake, and aqueous surface chemistry alter the aerosol size distribution and composition. At this, clouds play a primary role as physical and chemical processing inside cloud droplets contributes considerably to the changes in aerosol particles. A previous study estimates that on global average atmospheric particles are cycled three times through a cloud before being removed from the atmosphere [1]. An explicit and detailed treatment of cloud-borne particles has been implemented in the regional weather forecast and climate model COSMO-CLM. The employed model version includes a two-moment cloud microphysical scheme [2] that has been coupled to the aerosol microphysical scheme M7 [3] as described by Muhlbauer and Lohmann, 2008 [4]. So far, the formation, transfer and removal of cloud-borne aerosol number and mass were not considered in the model. Following the parameterization for cloud-borne particles developed by Hoose et al., 2008 [5], distinction between in-droplet and in-crystal particles is made to more physically account for processes in mixed-phase clouds, such as the Wegener-Bergeron-Findeisen process and contact and immersion freezing. In our model, this approach has been extended to allow for aerosol particles in five different hydrometeors: cloud droplets, rain drops, ice crystals, snow flakes and graupel. We account for nucleation scavenging, freezing and melting processes, autoconversion, accretion, aggregation, riming and selfcollection, collisions between interstitial aerosol particles and hydrometeors, ice multiplication, sedimentation, evaporation and sublimation. The new scheme allows an evaluation of the cloud cycling of aerosol particles by tracking the particles even when scavenged into hydrometeors. Global simulations of aerosol processing in clouds have recently been conducted by Hoose et al

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

    PubMed

    Herich, Hanna; Tritscher, Torsten; Wiacek, Aldona; Gysel, Martin; Weingartner, Ernest; Lohmann, Ulrike; Baltensperger, Urs; Cziczo, Daniel J

    2009-09-28

    Airborne mineral dust particles serve as cloud condensation nuclei (CCN), thereby influencing the formation and properties of warm clouds. It is therefore of atmospheric interest how dust aerosols with different mineralogy behave when exposed to high relative humidity (RH) or supersaturation (SS) with respect to liquid water. In this study the subsaturated hygroscopic growth and the supersaturated cloud condensation nucleus activity of pure clays and real desert dust aerosols were 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 investigated. Aerosols were generated both with a wet and a dry disperser. The water uptake was parameterized via the hygroscopicity parameter kappa. The hygroscopicity of dry generated dust aerosols was found to be negligible when compared to processed atmospheric aerosols, with CCNC derived kappa values between 0.00 and 0.02 (the latter corresponds to a particle consisting of 96.7% by volume insoluble material and approximately 3.3% ammonium sulfate). Pure clay aerosols were generally found to be less hygroscopic than natural desert dust particles. The illite and montmorillonite samples had kappa approximately 0.003. The kaolinite samples were less hygroscopic and had kappa=0.001. SD (kappa=0.023) was found to be the most hygroscopic dry-generated desert dust followed by CD (kappa=0.007) and ATD (kappa=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. Thus, the generation method is critically important when presenting such data. These results indicate any atmospheric processing of a fresh mineral dust particle which

  9. Delivery of Highly Active Noble-Metal Nanoparticles into Microspherical Supports by an Aerosol-Spray Method.

    PubMed

    Kan, Erjie; Kuai, Long; Wang, Wenhai; Geng, Baoyou

    2015-09-14

    Noble metal nanoparticles (NPs) with 1-5 nm diameter obtained from NaHB4 reduction possess high catalytic activity. However, they are rarely used directly. This work presents a facile, versatile, and efficient aerosol-spray approach to deliver noble-metal NPs into metal oxide supports, while maintaining the size of the NPs and the ability to easily adjust the loading amount. In comparison with the conventional spray approach, the size of the loaded noble-metal nanoparticles can be significantly decreased. An investigation of the 4-nitrophenol hydrogenation reaction catalyzed by these materials suggests that the NPs/oxides catalysts have high activity and good endurance. For 1 % Au/CeO2 and Pd/Al2 O3 catalysts, the rate constants reach 2.03 and 1.46 min(-1) , which is much higher than many other reports with the same noble-metal loading scale. Besides, the thermal stability of catalysts can be significantly enhanced by modifying the supports. Therefore, this work contributes an efficient method as well as some guidance on how to produce highly active and stable supported noble-metal catalysts. PMID:26234910

  10. Modeling of clouds and radiation for developing parameterizations for general circulation models. Annual report, 1995

    SciTech Connect

    Toon, O.B.; Westphal, D.L.

    1996-07-01

    We have used a hierarchy of numerical models for cirrus and stratus clouds and for radiative transfer to improve the reliability of general circulation models. Our detailed cloud microphysical model includes all of the physical processes believed to control the lifecycles of liquid and ice clouds in the troposphere. We have worked on specific GCM parameterizations for the radiative properties of cirrus clouds, making use of a mesocale model as the test-bed for the parameterizations. We have also modeled cirrus cloud properties with a detailed cloud physics model to better understand how the radiatively important properties of cirrus are controlled by their environment. We have used another cloud microphysics model to investigate of the interactions between aerosols and clouds. This work is some of the first to follow the details of interactions between aerosols and cloud droplets and has shown some unexpected relations between clouds and aerosols. We have also used line-by- line radiative transfer results verified with ARM data, to derive a GCMS.

  11. Parameterization of marine stratus microphysics based on in situ observations: Implications for GCMs

    SciTech Connect

    Gultepe, I.; Isaac, G.A.; Leaitch, W.R.; Banic, C.M.

    1996-02-01

    Airborne observations conducted in marine stratus over the east coast of Canada during the North Atlantic Regional Experiment in the summer of 1993 are used to develop cloud microphysical parameterization schemes for general circulation models. Observations of cloud droplet number concentration (N{sub d}), interstitial aerosol number concentration, temperature, verticle air velocity (w), and liquid water content (LWC) are considered, as well as determination of the effective radius (r{sub eff}) and total particle concentration (interstitial aerosol + cloud droplet). Statistical techniques are used to obtain regression equations among the above parameters. For individual clouds, an inverse relationship between the interstitial aerosol concentration and droplet concentration is always observed. In general, variations in r{sub eff} are determined by N{sub d} as much as by LWC. The regression equations are compared with current parameterizations for GCMs. Results showed that multiple relationships are present among N{sub d}, N{sub t}, and w; and r{sub eff}, LWC, and N{sub d}. 37 refs., 12 figs., 3 tabs.

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

    NASA Technical Reports Server (NTRS)

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

    2010-01-01

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

  13. N(2)O(5) reaction on submicron sea salt aerosol: kinetics, products, and the effect of surface active organics.

    PubMed

    Thornton, Joel A; Abbatt, Jonathan P D

    2005-11-10

    The reaction of N(2)O(5) on sea salt aerosol is a sink for atmospheric nitrogen oxides and a source of the Cl radical. We present room-temperature measurements of the N(2)O(5) loss rate on submicron artificial seawater (ASW) aerosol, performed with an entrained aerosol flow tube coupled to a chemical ionization mass spectrometer, as a function of aerosol phase (aqueous or partially crystalline), liquid water content, and size. We also present an analysis of the product growth kinetics showing that ClNO(2) is produced at a rate equal to N(2)O(5) loss, with an estimated lower limit yield of 50% at 50% relative humidity (RH). The reaction probability for N(2)O(5), gamma(N(2)(O)(5)), depends strongly on the particle phase, being 0.005 +/- 0.004 on partially crystalline ASW aerosol at 30% RH and 0.03 +/- 0.008 on aqueous ASW aerosol at 65% RH. At 50% RH, N(2)O(5) loss is relatively insensitive to particle size for radii greater than 100 nm, and gamma(N(2)(O)(5)) displays a statistically insignificant increase from 0.022 to approximately 0.03 for aqueous ASW aerosol over the RH range of 43-70%. We find that the presence of millimolar levels of hexanoic acid in the aerosol bulk decreases the gamma(N(2)(O)(5)) at 70% RH by a factor of 3-4 from approximately 0.025 to 0.008 +/- 0.004. This reduction is likely due to the partitioning of hexanoic acid to the gas-aerosol interface at a surface coverage that we estimate to be equivalent to a monolayer. This result is the first evidence that a monolayer coating of aqueous organic surfactant can slow the reactive uptake of atmospheric trace gases to aerosol. PMID:16838918

  14. An intermediate process-based fire parameterization in Dynamic Global Vegetation Model

    NASA Astrophysics Data System (ADS)

    Li, F.; Zeng, X.

    2011-12-01

    An intermediate process-based fire parameterization has been developed for global fire simulation. It fits the framework of Dynamic Global Vegetation Model (DGVM) which has been a pivot component in Earth System Model (ESM). The fire parameterization comprises three parts: fire occurrence, fire spread, and fire impact. In the first part, the number of fires is determined by ignition counts due to anthropogenic and natural causes and three constraints: fuel load, fuel moisture, and human suppression. Human caused ignition and suppression is explicitly considered as a nonlinear function of population density. The fire counts rather than fire occurrence probability is estimated to avoid underestimating the observed high burned area fraction in tropical savannas where fire occurs frequently. In the second part, post-fire region is assumed to be elliptical in shape with the wind direction along the major axis and the point of ignition at one of the foci. Burned area is determined by fire spread rate,fire duration, and fire counts. Mathematical characteristics of ellipse and some mathematical derivations are used to avoid redundant and unreasonable equations and assumptions in the CTEM-FIRE and make the parameterization equations self-consistently. In the third part, the impact of fire on vegetation component and structure, carbon cycle, trace gases and aerosol emissions are taken into account. The new estimates of trace gas and aerosol emissions due to biomass burning offers an interface with aerosol and atmospheric chemistry model in ESMs. Furthermore, in the new fire parameterization, fire occurrence part and fire spread part can be updated hourly or daily, and fire impact part can be updated daily, monthly, or annually. Its flexibility in selection of time-step length makes it easily applied to various DGVMs. The improved Community Land Model 3.0's Dynamic Global Vegetation Model (CLM-DGVM) is used as the model platform to assess the global performance of the new

  15. Approaches for Subgrid Parameterization: Does Scaling Help?

    NASA Astrophysics Data System (ADS)

    Yano, Jun-Ichi

    2016-04-01

    Arguably the scaling behavior is a well-established fact in many geophysical systems. There are already many theoretical studies elucidating this issue. However, the scaling law is slow to be introduced in "operational" geophysical modelling, notably for weather forecast as well as climate projection models. The main purpose of this presentation is to ask why, and try to answer this question. As a reference point, the presentation reviews the three major approaches for traditional subgrid parameterization: moment, PDF (probability density function), and mode decomposition. The moment expansion is a standard method for describing the subgrid-scale turbulent flows both in the atmosphere and the oceans. The PDF approach is intuitively appealing as it directly deals with a distribution of variables in subgrid scale in a more direct manner. The third category, originally proposed by Aubry et al (1988) in context of the wall boundary-layer turbulence, is specifically designed to represent coherencies in compact manner by a low--dimensional dynamical system. Their original proposal adopts the proper orthogonal decomposition (POD, or empirical orthogonal functions, EOF) as their mode-decomposition basis. However, the methodology can easily be generalized into any decomposition basis. The mass-flux formulation that is currently adopted in majority of atmospheric models for parameterizing convection can also be considered a special case of the mode decomposition, adopting the segmentally-constant modes for the expansion basis. The mode decomposition can, furthermore, be re-interpreted as a type of Galarkin approach for numerically modelling the subgrid-scale processes. Simple extrapolation of this re-interpretation further suggests us that the subgrid parameterization problem may be re-interpreted as a type of mesh-refinement problem in numerical modelling. We furthermore see a link between the subgrid parameterization and downscaling problems along this line. The mode

  16. Direct Quantification of Ice Nucleation Active Bacteria in Aerosols and Precipitation: Their Potential Contribution as Ice Nuclei

    NASA Astrophysics Data System (ADS)

    Hill, T. C.; DeMott, P. J.; Garcia, E.; Moffett, B. F.; Prenni, A. J.; Kreidenweis, S. M.; Franc, G. D.

    2013-12-01

    Ice nucleation active (INA) bacteria are a potentially prodigious source of highly active (≥-12°C) atmospheric ice nuclei, especially from agricultural land. However, we know little about the conditions that promote their release (eg, daily or seasonal cycles, precipitation, harvesting or post-harvest decay of litter) or their typical contribution to the pool of boundary layer ice nucleating particles (INP). To initiate these investigations we developed a quantitative Polymerase Chain Reaction (qPCR) test of the ina gene, the gene that codes for the ice nucleating protein, to directly count INA bacteria in environmental samples. The qPCR test amplifies most forms of the gene and is highly sensitive, able to detect perhaps a single gene copy (ie, a single bacterium) in DNA extracted from precipitation. Direct measurement of the INA bacteria is essential because environmental populations will be a mixture of living, viable-but-not culturable, moribund and dead cells, all of which may retain ice nucleating proteins. Using the qPCR test on leaf washings of plants from three farms in Wyoming, Colorado and Nebraska we found INA bacteria to be abundant on crops, especially on cereals. Mid-summer populations on wheat and barley were ~108/g fresh weigh of foliage. Broadleaf crops, such as corn, alfalfa, sugar beet and potato supported 105-107/g. Unexpectedly, however, in the absence of a significant physical disturbance, such as harvesting, we were unable to detect the ina gene in aerosols sampled above the crops. Likewise, in fresh snow samples taken over two winters, ina genes from a range of INA bacteria were detected in about half the samples but at abundances that equated to INA bacterial numbers that accounted for only a minor proportion of INP active at -10°C. By contrast, in a hail sample from a summer thunderstorm we found 0.3 INA bacteria per INP at -10°C and ~0.5 per hail stone. Although the role of the INA bacteria as warm-temperature INP in these samples

  17. Improving aerosol interaction with clouds and precipitation in a regional chemical weather modeling system

    NASA Astrophysics Data System (ADS)

    Zhou, C.; Zhang, X.; Gong, S.

    2015-12-01

    A comprehensive aerosol-cloud-precipitation interaction (ACI) scheme has been developed under CMA chemical weather modeling system GRAPES/CUACE. Calculated by a sectional aerosol activation scheme based on the information of size and mass from CUACE and the thermal-dynamic and humid states from the weather model GRAPES at each time step, the cloud condensation nuclei (CCN) is fed online interactively into a two-moment cloud scheme (WDM6) and a convective parameterization to drive the cloud physics and precipitation formation processes. The modeling system has been applied to study the ACI for January 2013 when several persistent haze-fog events and eight precipitation events occurred. The results show that interactive aerosols with the WDM6 in GRAPES/CUACE obviously increase the total cloud water, liquid water content and cloud droplet number concentrations while decrease the mean diameter of cloud droplets with varying magnitudes of the changes in each case and region. These interactive micro-physical properties of clouds improve the calculation of their collection growth rates in some regions and hence the precipitation rate and distributions in the model, showing 24% to 48% enhancements of TS scoring for 6-h precipitation in almost all regions. The interactive aerosols with the WDM6 also reduce the regional mean bias of temperature by 3 °C during certain precipitation events, but the monthly means bias is only reduced by about 0.3°C.

  18. The contribution of dust devils and dusty plumes to the aerosol budget in western China

    NASA Astrophysics Data System (ADS)

    Han, Yongxiang; Wang, Kanghong; Liu, Feng; Zhao, Tianliang; Yin, Yan; Duan, Jiapeng; Luan, Zhaopeng

    2016-02-01

    Based on thermodynamic theory and comprehensive analyses of the Total Ozone Mapping Spectrometer Aerosol Index, surface micro-pulse LiDAR, meteorological elements in the atmospheric boundary layer, observations of sporadic dust devil, the diurnal and seasonal changes of dust devil are characterized, the contribution to the aerosol budget from dust devils and dusty plumes is quantitatively analyzed. The results show that: 1) dust devils and dusty plumes show obvious diurnal and seasonal variations with a single-peaked distribution; 2) thermodynamic efficiency can effectively account for the daily variations of dust devils and dusty plumes from morning to early afternoon, seasonal changes of dust devil activity in summer. The future improved thermodynamic efficiency could be applied to their parameterization; 3) dust devils and dusty plumes may contribute more than 53% of annual total dust aerosols over desert regions in western China,but the calculated contributions have uncertainties. It will be helpful to understand the dust devil and dusty plume contributions to global and regional aerosol loading.

  19. Improving aerosol interaction with clouds and precipitation in a regional chemical weather modeling system

    NASA Astrophysics Data System (ADS)

    Zhou, C.; Zhang, X.; Gong, S.; Wang, Y.; Xue, M.

    2015-06-01

    A comprehensive aerosol-cloud-precipitation interaction (ACI) scheme has been developed under CMA chemical weather modeling system GRAPES/CUACE. Calculated by a sectional aerosol activation scheme based on the information of size and mass from CUACE and the thermal-dynamic and humid states from the weather model GRAPES at each time step, the cloud condensation nuclei (CCN) is fed online interactively into a two-moment cloud scheme (WDM6) and a convective parameterization to drive the cloud physics and precipitation formation processes. The modeling system has been applied to study the ACI for January 2013 when several persistent haze-fog events and eight precipitation events occurred. The results show that interactive aerosols with the WDM6 in GRAPES/CUACE obviously increase the total cloud water, liquid water content and cloud droplet number concentrations while decrease the mean diameter of cloud droplets with varying magnitudes of the changes in each case and region. These interactive micro-physical properties of clouds improve the calculation of their collection growth rates in some regions and hence the precipitation rate and distributions in the model, showing 24 to 48% enhancements of TS scoring for 6 h precipitation in almost all regions. The interactive aerosols with the WDM6 also reduce the regional mean bias of temperature by 3 °C during certain precipitation events, but the monthly means bias is only reduced by about 0.3 °C.

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  1. Multicomponent aerosol dynamics model UHMA: model development and validation

    NASA Astrophysics Data System (ADS)

    Korhonen, H.; Lehtinen, K. E. J.; Kulmala, M.

    2004-05-01

    A size-segregated aerosol dynamics model UHMA (University of Helsinki Multicomponent Aerosol model) was developed for studies of multicomponent tropospheric aerosol particles. The model includes major aerosol microphysical processes in the atmosphere with a focus on new particle formation and growth; thus it incorporates particle coagulation and multicomponent condensation, applying a revised treatment of condensation flux onto free molecular regime particles and the activation of nanosized clusters by organic vapours (Nano-Köhler theory), as well as recent parameterizations for binary H2SO4-H2O and ternary H2SO4-NH3-H2O homogeneous nucleation and dry deposition. The representation of particle size distribution can be chosen from three sectional methods: the hybrid method, the moving center method, and the retracking method in which moving sections are retracked to a fixed grid after a certain time interval. All these methods can treat particle emissions and atmospheric transport consistently, and are therefore suitable for use in large scale atmospheric models. In a test simulation against an accurate high resolution solution, all the methods showed reasonable treatment of new particle formation with 20 size sections although the hybrid and the retracking methods suffered from artificial widening of the distribution. The moving center approach, on the other hand, showed extra dents in the particle size distribution and failed to predict the onset of detectable particle formation. In a separate test simulation of an observed nucleation event, the model captured the key qualitative behaviour of the system well. Furthermore, its prediction of the organic volume fraction in newly formed particles, suggesting values as high as 0.5 for 3-4 nm particles and approximately 0.8 for 10 nm particles, agrees with recent indirect composition measurements.

  2. Effect of organic compounds on cloud condensation nuclei (CCN) activity of sea spray aerosol produced by bubble bursting

    NASA Astrophysics Data System (ADS)

    Moore, Meagan J. K.; Furutani, Hiroshi; Roberts, Gregory C.; Moffet, Ryan C.; Gilles, Mary K.; Palenik, Brian; Prather, Kimberly A.

    2011-12-01

    The ocean comprises over 70% of the surface of the earth and thus sea spray aerosols generated by wave processes represent a critical component of our climate system. The manner in which different complex oceanic mixtures of organic species and inorganic salts are distributed between individual particles in sea spray directly determines which particles will effectively form cloud nuclei. Controlled laboratory experiments were undertaken to better understand the full range of particle properties produced by bubbling solutions composed of simplistic model organic species, oleic acid and sodium dodecyl sulfate (SDS), mixed with NaCl to more complex artificial seawater mixed with complex organic mixtures produced by common oceanic microorganisms. Simple mixtures of NaCl and oleic acid or SDS had a significant effect on CCN activity, even in relatively small amounts. However, an artificial seawater (ASW) solution containing microorganisms, the common cyanobacteria ( Synechococcus) and DMS-producing green algae ( Ostreococcus), produced particles containing ˜34 times more carbon than the particles produced from pure ASW, yet no significant change was observed in the overall CCN activity. We hypothesize that these microorganisms produce diverse mixtures of organic species with a wide range of properties that produced offsetting effects, leading to no net change in the overall average measured hygroscopicity of the collection of sea spray particles. Based on these observations, changes in CCN activity due to "bloom" conditions would be predicted to lead to small changes in the average CCN activity, and thus have a negligible impact on cloud formation. However, each sea spray particle will contain a broad spectrum of different species, and thus further studies are needed of the CCN activity of individual sea spray particles and biological processes under a wide range of controllable conditions.

  3. A uniform parameterization of moment tensors

    NASA Astrophysics Data System (ADS)

    Tape, C.; Tape, W.

    2015-12-01

    A moment tensor is a 3 x 3 symmetric matrix that expresses an earthquake source. We construct a parameterization of the five-dimensional space of all moment tensors of unit norm. The coordinates associated with the parameterization are closely related to moment tensor orientations and source types. The parameterization is uniform, in the sense that equal volumes in the coordinate domain of the parameterization correspond to equal volumes of moment tensors. Uniformly distributed points in the coordinate domain therefore give uniformly distributed moment tensors. A cartesian grid in the coordinate domain can be used to search efficiently over moment tensors. We find that uniformly distributed moment tensors have uniformly distributed orientations (eigenframes), but that their source types (eigenvalue triples) are distributed so as to favor double couples. An appropriate choice of a priori moment tensor probability is a prerequisite for parameter estimation. As a seemingly sensible choice, we consider the homogeneous probability, in which equal volumes of moment tensors are equally likely. We believe that it will lead to improved characterization of source processes.

  4. Soil processes parameterization in meteorological model.

    NASA Astrophysics Data System (ADS)

    Mazur, Andrzej; Duniec, Grzegorz

    2014-05-01

    In August 2012 Polish Institute Meteorology and Water Management - National Research Institute (IMWM-NRI) started a collaboration with the Institute of Agrophysics - Polish Academy of Science (IA-PAS) in order to improve soil processes parameterization in COSMO meteorological model of high resolution (horizontal grid size equal to 2,8 km). This cooperation turned into a project named "New approach to parameterization of physical processes in soil in numerical model". The new set of soil processes parameterizations is being developed considering many physical and microphysical processes in soil. Currently, main effort is focused on description of bare soil evaporation, soil water transport and the runoff from soil layers. The preliminary results from new mathematical formulation of bare soil evaporation implemented in COSMO model will be presented. Moreover, during the Conference authors (realizing a constant need for further improvement) would like to show future plans and topics for further studies. It is planned to combine the mentioned new approach with TILE and MOSAIC parameterizations, previously investigated as a part of TERRA-MultiLevel module of COSMO model, and to use measurements data received from IA-PAS and from Satellite Remote Sensing Center in soil-related COSMO model numerical experiments.

  5. Evaluating N2O5 heterogeneous hydrolysis parameterizations for CalNex 2010

    NASA Astrophysics Data System (ADS)

    Chang, Wayne L.; Brown, Steven S.; Stutz, Jochen; Middlebrook, Ann M.; Bahreini, Roya; Wagner, Nicholas L.; Dubé, William P.; Pollack, Ilana B.; Ryerson, Thomas B.; Riemer, Nicole

    2016-05-01

    Nighttime chemistry in the troposphere is closely tied to the dinitrogen pentoxide (N2O5) budget, but high uncertainties remain regarding the model representation of the heterogeneous hydrolysis of N2O5 on aerosol particles. In this study we used the community model WRF-Chem to simulate a 3-day period during the California Nexus (CalNex) Campaign in 2010. We extended WRF-Chem to include the heterogeneous hydrolysis of N2O5 and contrasted the impact of different published parameterizations of N2O5 heterogeneous hydrolysis on the spatial distribution of uptake coefficients and the resulting N2O5 concentrations. For all the cases, modeled N2O5 uptake coefficients showed strong spatial variability, with higher values in the nocturnal boundary layer compared to the residual layer, especially in environments with high relative humidities, such as over the ocean and along the coast. The best agreement of modeled and observed uptake coefficients was obtained using the parameterization by Davis et al. (2008) combined with the treatment of organic coating by Riemer et al. (2009). For this case the temporal evolution of lower boundary layer N2O5 mixing ratios was reproduced well, and the predictions of surface mixing ratios of ozone and NOx were improved. However, the model still overpredicted the uptake coefficients in the residual layer and consequently underpredicted N2O5 concentrations in the residual layer. This study also highlights that environments with low relative humidities pose a challenge for aerosol thermodynamic models in calculating aerosol water uptake, and this impacts N2O5 heterogeneous hydrolysis parameterizations.

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

    NASA Technical Reports Server (NTRS)

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

    2008-01-01

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

  7. Empirical parameterization of setup, swash, and runup

    USGS Publications Warehouse

    Stockdon, H.F.; Holman, R.A.; Howd, P.A.; Sallenger, A.H., Jr.

    2006-01-01

    Using shoreline water-level time series collected during 10 dynamically diverse field experiments, an empirical parameterization for extreme runup, defined by the 2% exceedence value, has been developed for use on natural beaches over a wide range of conditions. Runup, the height of discrete water-level maxima, depends on two dynamically different processes; time-averaged wave setup and total swash excursion, each of which is parameterized separately. Setup at the shoreline was best parameterized using a dimensional form of the more common Iribarren-based setup expression that includes foreshore beach slope, offshore wave height, and deep-water wavelength. Significant swash can be decomposed into the incident and infragravity frequency bands. Incident swash is also best parameterized using a dimensional form of the Iribarren-based expression. Infragravity swash is best modeled dimensionally using offshore wave height and wavelength and shows no statistically significant linear dependence on either foreshore or surf-zone slope. On infragravity-dominated dissipative beaches, the magnitudes of both setup and swash, modeling both incident and infragravity frequency components together, are dependent only on offshore wave height and wavelength. Statistics of predicted runup averaged over all sites indicate a - 17 cm bias and an rms error of 38 cm: the mean observed runup elevation for all experiments was 144 cm. On intermediate and reflective beaches with complex foreshore topography, the use of an alongshore-averaged beach slope in practical applications of the runup parameterization may result in a relative runup error equal to 51% of the fractional variability between the measured and the averaged slope.

  8. A stochastic parameterization for deep convection using cellular automata

    NASA Astrophysics Data System (ADS)

    Bengtsson, L.; Steinheimer, M.; Bechtold, P.; Geleyn, J.

    2012-12-01

    Cumulus parameterizations used in most operational weather and climate models today are based on the mass-flux concept which took form in the early 1970's. In such schemes it is assumed that a unique relationship exists between the ensemble-average of the sub-grid convection, and the instantaneous state of the atmosphere in a vertical grid box column. However, such a relationship is unlikely to be described by a simple deterministic function (Palmer, 2011). Thus, because of the statistical nature of the parameterization challenge, it has been recognized by the community that it is important to introduce stochastic elements to the parameterizations (for instance: Plant and Craig, 2008, Khouider et al. 2010, Frenkel et al. 2011, Bentsson et al. 2011, but the list is far from exhaustive). There are undoubtedly many ways in which stochastisity can enter new developments. In this study we use a two-way interacting cellular automata (CA), as its intrinsic nature possesses many qualities interesting for deep convection parameterization. In the one-dimensional entraining plume approach, there is no parameterization of horizontal transport of heat, moisture or momentum due to cumulus convection. In reality, mass transport due to gravity waves that propagate in the horizontal can trigger new convection, important for the organization of deep convection (Huang, 1988). The self-organizational characteristics of the CA allows for lateral communication between adjacent NWP model grid-boxes, and temporal memory. Thus the CA scheme used in this study contain three interesting components for representation of cumulus convection, which are not present in the traditional one-dimensional bulk entraining plume method: horizontal communication, memory and stochastisity. The scheme is implemented in the high resolution regional NWP model ALARO, and simulations show enhanced organization of convective activity along squall-lines. Probabilistic evaluation demonstrate an enhanced spread in

  9. Investigating primary marine aerosol properties: CCN activity of sea salt and mixed particles

    NASA Astrophysics Data System (ADS)

    King, S. M.; Butcher, A. C.; Rosenoern, T.; Coz, E.; Lieke, K. I.; de Leeuw, G.; Nilsson, E. D.; Bilde, M.

    2012-04-01

    Sea salt particles ejected as a result of bubbles bursting from artificial seawater in a closed stainless steel tank were sampled for size distribution, morphology, and cloud condensation nucleus (CCN) activity. The two-component artificial seawater consisted of salt, either NaCl or sea salt, and one organic compound in deionized water. Several organic molecules representative of oceanic organic matter were investigated. Bubbles were generated either by aeration through a porous diffuser or by water jet impingement on the surface of the artificial seawater. The effect of bubble lifetime, which was controlled by varying the depth of the diffuser in the water column, on particle size and CCN activity was investigated and was found to be insignificant for the organic compounds studied. The CCN activities of particles produced from diffuser-generated bubbles were generally governed by the high hygroscopicity of salt, such that activation was indistinguishable from that of salt, except in the case of very low mass ratio of salt to organic matter in the seawater solution. There was, however, a considerable decrease in CCN activity for particles produced from jet impingement on seawater that had a salinity of 10‰ and contained 0.45 mM of sodium laurate, an organic surfactant. The production of a thick foam layer from impingement may explain the difference in activation and supports hypotheses that particle production from the two methods of generating bubbles is not similar. Accurate conclusions from observed CCN activities of particles from artificial seawater containing organic matter require knowledge of the CCN activity of the inorganic component, especially as a small amount of the inorganic can heavily influence activation. Therefore, the CCN activity of both artificial sea salt and NaCl were measured and compared. Part of the discrepancy observed between the CCN activities of the two salts may be due to morphological differences, which were investigated using

  10. Aerosol residence times and changes in radioiodine-131I and radiocaesium-137 Cs activity over Central Poland after the Fukushima-Daiichi Nuclear reactor accident.

    PubMed

    Długosz-Lisiecka, Magdalena; Bem, Henryk

    2012-05-01

    The first detectable activities of radioiodine (131)I, and radiocaesium (134)Cs and (137)Cs in the air over Central Poland were measured in dust samples collected by the ASS-500 station in the period of 21(st) to 24(th) of March, 2011. However, the highest activity of both fission products, (131)I and (137)Cs: 8.3 mBq m(-3) and 0.75 mBq m(-3), respectively, were obtained in the samples collected on 30(th) March, i.e.∼18 days after the beginning of the fission products' discharge from the damaged units of the Fukushima Daiichi Nuclear Power Plant. The simultaneously determined corrected aerosol residence time for the same samples by (210)Pb/(210)Bi and (210)Pb/(210)Po methods was equal to 10 days. Additionally, on the basis of the activity ratio of two other natural cosmogenic radionuclides, (7)Be and (22)Na in these aerosol samples, it was possible to estimate the aerosol residence time at ∼150 days for the solid particles coming from the stratospheric fallout. These data, as well as the differences in the activity size distribution of (7)Be and (131)I in the air particulate matter, show, in contrast to the Chernobyl discharge, a negligible input of stratospheric transport of Fukushima-released fission products. PMID:22481111

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

    NASA Astrophysics Data System (ADS)

    Brock, Charles; Wagner, Nick; Gordon, Timothy

    2016-04-01

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

  12. Model Intercomparison of Indirect Aerosol Effects

    NASA Technical Reports Server (NTRS)

    Penner, J. E.; Quaas, J.; Storelvmo, T.; Takemura, T.; Boucher, O.; Guo, H.; Kirkevag, A.; Kristjansson, J. E.; Seland, O.

    2006-01-01

    Modeled differences in predicted effects are increasingly used to help quantify the uncertainty of these effects. Here, we examine modeled differences in the aerosol indirect effect in a series of experiments that help to quantify how and why model-predicted aerosol indirect forcing varies between models. The experiments start with an experiment in which aerosol concentrations, the parameterization of droplet concentrations and the autoconversion scheme are all specified and end with an experiment that examines the predicted aerosol indirect forcing when only aerosol sources are specified. Although there are large differences in the predicted liquid water path among the models, the predicted aerosol first indirect effect for the first experiment is rather similar, about -0.6 W/sq m to -0.7 W/sq m. Changes to the autoconversion scheme can lead to large changes in the liquid water path of the models and to the response of the liquid water path to changes in aerosols. Adding an autoconversion scheme that depends on the droplet concentration caused a larger (negative) change in net outgoing shortwave radiation compared to the 1st indirect effect, and the increase varied from only 22% to more than a factor of three. The change in net shortwave forcing in the models due to varying the autoconversion scheme depends on the liquid water content of the clouds as well as their predicted droplet concentrations, and both increases and decreases in the net shortwave forcing can occur when autoconversion schemes are changed. The parameterization of cloud fraction within models is not sensitive to the aerosol concentration, and, therefore, the response of the modeled cloud fraction within the present models appears to be smaller than that which would be associated with model "noise". The prediction of aerosol concentrations, given a fixed set of sources, leads to some of the largest differences in the predicted aerosol indirect radiative forcing among the models, with values of

  13. Global Aerosols

    Atmospheric Science Data Center

    2013-04-19

    ... sizes and from multiple sources, including biomass burning, mineral dust, sea salt and regional industrial pollution. A color scale is ... desert source region. Deserts are the main sources of mineral dust, and MISR obtains aerosol optical depth at visible wavelengths ...

  14. Parameterization of contrail radiative properties for climate studies

    NASA Astrophysics Data System (ADS)

    Xie, Yu; Yang, Ping; Liou, Kuo-Nan; Minnis, Patrick; Duda, David P.

    2012-12-01

    The study of contrails and their impact on global climate change requires a cloud model that statistically represents contrail radiative properties. In this study, the microphysical properties of global contrails are statistically analyzed using collocated Moderate Resolution Imaging Spectroradiometer (MODIS) and Cloud Aerosol Lidar with Orthogonal Polarization (CALIOP) observations. The MODIS contrail pixels are detected using an automated contrail detection algorithm and a manual technique using the brightness temperature differences between the MODIS 11 and 12 μm channels. The scattering and absorption properties of typical contrail ice crystals are used to determine an appropriate contrail model to minimize the uncertainties arising from the assumptions in a particular cloud model. The depolarization ratio is simulated with a variety of ice crystal habit fractions and matched to the collocated MODIS and CALIOP observations. The contrail habit fractions are determined and used to compute the bulk-scattering properties of contrails. A parameterization of shortwave and longwave contrail optical properties is developed for the spectral bands of the Rapid Radiative Transfer Model (RRTM). The contrail forcing at the top of the atmosphere is investigated using the RRTM and compared with spherical and hexagonal ice cloud models. Contrail forcing is overestimated when spherical ice crystals are used to represent contrails, but if a hexagonal ice cloud model is used, the forcing is underestimated for small particles and overestimated for large particles in comparison to the contrail model developed in this study.

  15. Fluorescence spectra and biological activity of aerosolized bacillus spores and MS2 bacteriophage exposed to ozone at different relative humidities in a rotating drum

    SciTech Connect

    Ratnesar-Shumate, Shanna; Pan, Yong-Le; Hill, Steven C.; Kinahan, Sean; Corson, Elizabeth; Eshbaugh, Jonathan; Santarpia, Joshua L.

    2015-10-14

    Biological aerosols (bioaerosols) released into the environment may undergo physical and chemical transformations when exposed to atmospheric constituents such as solar irradiation, reactive oxygenated species, ozone, free radicals, water vapor and pollutants. Aging experiments were performed in a rotating drum chamber subjecting bioaerosols, Bacillus thuringiensis Al Hakam (BtAH) spores and MS2 bacteriophages to ozone at 0 and 150 ppb, and relative humidities (RH) at 10%, 50%, and 80+%. Fluorescence spectra and intensities of the aerosols as a function of time in the reaction chamber were measured with a single particle fluorescence spectrometer (SPFS) and an Ultra-Violet Aerodynamic Particle Sizer® Spectrometer (UV-APS). Losses in biological activity were measured by culture and quantitative polymerase chain reaction (q-PCR) assay. For both types of aerosols the largest change in fluorescence emission was between 280 and 400 nm when excited at 263 nm followed by fluorescence emission between 380 and 700 nm when excited at 351 nm. The fluorescence for both BtAH and MS2 were observed to decrease significantly at high ozone concentration and high RH when excited at 263 nm excitation. The decreases in 263 nm excited fluorescence are indicative of hydrolysis and oxidation of tryptophan in the aerosols. Fluorescence measured with the UV-APS (355-nm excitation) increased with time for both BtAH and MS2 aerosols. A two log loss of MS2 bacteriophage infectivity was observed in the presence of ozone at ~50% and 80% RH when measured by culture and normalized for physical losses by q-PCR. Viability of BtAH spores after exposure could not be measured due to the loss of genomic material during experiments, suggesting degradation of extracelluar DNA attributable to oxidation. The results of these studies indicate that the physical and biological properties of bioaerosols change significantly after exposure to ozone and water vapor.

  16. Fluorescence spectra and biological activity of aerosolized bacillus spores and MS2 bacteriophage exposed to ozone at different relative humidities in a rotating drum

    DOE PAGESBeta

    Ratnesar-Shumate, Shanna; Pan, Yong-Le; Hill, Steven C.; Kinahan, Sean; Corson, Elizabeth; Eshbaugh, Jonathan; Santarpia, Joshua L.

    2015-10-14

    Biological aerosols (bioaerosols) released into the environment may undergo physical and chemical transformations when exposed to atmospheric constituents such as solar irradiation, reactive oxygenated species, ozone, free radicals, water vapor and pollutants. Aging experiments were performed in a rotating drum chamber subjecting bioaerosols, Bacillus thuringiensis Al Hakam (BtAH) spores and MS2 bacteriophages to ozone at 0 and 150 ppb, and relative humidities (RH) at 10%, 50%, and 80+%. Fluorescence spectra and intensities of the aerosols as a function of time in the reaction chamber were measured with a single particle fluorescence spectrometer (SPFS) and an Ultra-Violet Aerodynamic Particle Sizer® Spectrometermore » (UV-APS). Losses in biological activity were measured by culture and quantitative polymerase chain reaction (q-PCR) assay. For both types of aerosols the largest change in fluorescence emission was between 280 and 400 nm when excited at 263 nm followed by fluorescence emission between 380 and 700 nm when excited at 351 nm. The fluorescence for both BtAH and MS2 were observed to decrease significantly at high ozone concentration and high RH when excited at 263 nm excitation. The decreases in 263 nm excited fluorescence are indicative of hydrolysis and oxidation of tryptophan in the aerosols. Fluorescence measured with the UV-APS (355-nm excitation) increased with time for both BtAH and MS2 aerosols. A two log loss of MS2 bacteriophage infectivity was observed in the presence of ozone at ~50% and 80% RH when measured by culture and normalized for physical losses by q-PCR. Viability of BtAH spores after exposure could not be measured due to the loss of genomic material during experiments, suggesting degradation of extracelluar DNA attributable to oxidation. The results of these studies indicate that the physical and biological properties of bioaerosols change significantly after exposure to ozone and water vapor.« less

  17. Fluorescence spectra and biological activity of aerosolized bacillus spores and MS2 bacteriophage exposed to ozone at different relative humidities in a rotating drum

    NASA Astrophysics Data System (ADS)

    Ratnesar-Shumate, Shanna; Pan, Yong-Le; Hill, Steven C.; Kinahan, Sean; Corson, Elizabeth; Eshbaugh, Jonathan; Santarpia, Joshua L.

    2015-03-01

    Biological aerosols (bioaerosols) released into the environment may undergo physical and chemical transformations when exposed to atmospheric constituents such as solar irradiation, reactive oxygenated species, ozone, free radicals, water vapor and pollutants. Aging experiments were performed in a rotating drum chamber subjecting bioaerosols, Bacillus thuringiensis Al Hakam (BtAH) spores and MS2 bacteriophages to ozone at 0 and 150 ppb, and relative humidities (RH) at 10%, 50%, and 80+%. Fluorescence spectra and intensities of the aerosols as a function of time in the reaction chamber were measured with a single particle fluorescence spectrometer (SPFS) and an Ultra-Violet Aerodynamic Particle Sizer® Spectrometer (UV-APS). Losses in biological activity were measured by culture and quantitative polymerase chain reaction (q-PCR) assay. For both types of aerosols the largest change in fluorescence emission was between 280 and 400 nm when excited at 263 nm followed by fluorescence emission between 380 and 700 nm when excited at 351 nm. The fluorescence for both BtAH and MS2 were observed to decrease significantly at high ozone concentration and high RH when excited at 263 nm excitation. The decreases in 263 nm excited fluorescence are indicative of hydrolysis and oxidation of tryptophan in the aerosols. Fluorescence measured with the UV-APS (355-nm excitation) increased with time for both BtAH and MS2 aerosols. A two log loss of MS2 bacteriophage infectivity was observed in the presence of ozone at ~50% and 80% RH when measured by culture and normalized for physical losses by q-PCR. Viability of BtAH spores after exposure could not be measured due to the loss of genomic material during experiments, suggesting degradation of extracelluar DNA attributable to oxidation. The results of these studies indicate that the physical and biological properties of bioaerosols change significantly after exposure to ozone and water vapor.

  18. A Simple Parameterization of 3 x 3 Magic Squares

    ERIC Educational Resources Information Center

    Trenkler, Gotz; Schmidt, Karsten; Trenkler, Dietrich

    2012-01-01

    In this article a new parameterization of magic squares of order three is presented. This parameterization permits an easy computation of their inverses, eigenvalues, eigenvectors and adjoints. Some attention is paid to the Luoshu, one of the oldest magic squares.

  19. Exploring Atmospheric Aerosol Chemistry with Advanced High-Resolution Mass Spectrometry and Particle Imaging Methods

    NASA Astrophysics Data System (ADS)

    Nizkorodov, S.

    2014-12-01

    Physical and chemical complexity of atmospheric aerosols presents significant challenges both to experimentalists working on aerosol characterization and to modelers trying to parameterize critical aerosol properties. Multi-modal approaches that combine state-of-the-art experimental, theoretical, and modeling methods are becoming increasingly important in aerosol research. This presentation will discuss recent applications of unique high-resolution mass spectrometry and particle imaging tools developed at two Department of Energy's user facilities, the Environmental Molecular Science Laboratory (EMSL) and Advanced Light Source (ALS), to studies of molecular composition, photochemical aging, and properties of laboratory-generated and field aerosols. Specifically, this presentation will attempt to address the following questions: (a) how do NO2, SO2, and NH3 affect molecular level composition of anthropogenic aerosols?; (b) what factors determine viscosity/surface tension of organic aerosol particles?; (c) how does photolysis affect molecular composition and optical properties of organic aerosols?

  20. Optical modeling of aerosol extinction for remote sensing in the marine environment

    NASA Astrophysics Data System (ADS)

    Kaloshin, G. A.

    2013-05-01

    A microphysical model is presented for the surface layer marine and coastal atmospheric aerosols that is based on long-term observations of size distributions for 0.01-100 μm particles in different geographic sites. The fundamental feature of the model is a parameterization of amplitudes and widths for aerosol modes of the aerosol size distribution function (ASDF) as functions of fetch and wind speed. The shape of the ASDF and its dependence on meteorological parameters, altitudes above sea level (H), fetch (X), wind speed (U) and relative humidity (RH) are investigated. The spectral profiles of the aerosol extinction coefficients calculated by MaexPro (Marine Aerosol Extinction Profiles) are in good agreement with observational data and the numerical results obtained from the Navy Aerosol Model (NAM) and the Advanced Navy Aerosol Model (ANAM). Moreover, MaexPro was found to be an accurate and reliable tool for investigation of the optical properties of atmospheric aerosols.

  1. Ice nucleating particles at a coastal marine boundary layer site: correlations with aerosol type and meteorological conditions

    NASA Astrophysics Data System (ADS)

    Mason, R. H.; Si, M.; Li, J.; Chou, C.; Dickie, R.; Toom-Sauntry, D.; Pöhlker, C.; Yakobi-Hancock, J. D.; Ladino, L. A.; Jones, K.; Leaitch, W. R.; Schiller, C. L.; Abbatt, J. P. D.; Huffman, J. A.; Bertram, A. K.

    2015-06-01

    Information on what aerosol particle types are the major sources of ice nucleating particles (INPs) in the atmosphere is needed for climate predictions. To determine which aerosol particles are the major sources of immersion-mode INPs at a coastal site in Western Canada, we investigated correlations between INP number concentrations and both concentrations of different atmospheric particles and meteorological conditions. We show that INP number concentrations are strongly correlated with the number concentrations of fluorescent bioparticles between -15 and -25 °C, and that the size distribution of INPs is most consistent with the size distribution of fluorescent bioparticles. We conclude that biological particles were likely the major source of ice nuclei at freezing temperatures between -15 and -25 °C at this site for the time period studied. At -30 °C, INP number concentrations are also well correlated with number concentrations of the total aerosol particles ≥ 0.5 μm, suggesting that non-biological particles may have an important contribution to the population of INPs active at this temperature. As we found that black carbon particles were unlikely to be a major source of ice nuclei during this study, these non-biological INPs may include mineral dust. Furthermore, correlations involving tracers of marine aerosols and marine biological activity indicate that the majority of INPs measured at the coastal site likely originated from terrestrial rather than marine sources. Finally, six existing empirical parameterizations of ice nucleation were tested to determine if they accurately predict the measured INP number concentrations. We found that none of the parameterizations selected are capable of predicting INP number concentrations with high accuracy over the entire temperature range investigated.

  2. Tropical anvil characteristics and water vapor of the tropical tropopause layer: Impact of heterogeneous and homogeneous freezing parameterizations

    SciTech Connect

    Fan, Jiwen; Comstock, Jennifer M.; Ovchinnikov, Mikhail; McFarlane, Sally A.; McFarquhar, Greg; Allen, Grant

    2010-06-16

    Abstract Two isolated deep convective clouds (DCCs) that developed in clean-humid and polluted-dry air masses, observed during the TWP-ICE and ACTIVE campaigns, are simulated using a 3-dimensional cloud-resolving model with size-resolved aerosol and cloud microphysics. We examine the impacts of different homogeneous and immersion freezing parameterizations on the anvil characteristics and the water vapor content (WVC) in the Tropical Tropopause Layer (TTL) for the two DCCs that developed in contrasting environments. The modeled cloud properties such as liquid/ice water path and precipitation generally agree with the available radar and satellite retrievals and in situ aircraft measurements. We find that anvil size and anvil microphysical properties such as ice number concentration and ice effective radius (rei) are much more sensitive to the homogeneous freezing parameterization (HomFP) under the polluted-dry condition, while the strength of anvil convection is more sensitive to HomFP under the clean-humid condition. Specifically, the cloud anvil with the Koop et al. (2000) (KOOP) relative humidity dependent scheme has up to 2 and 4 times lower ice number than those with other schemes (temperature dependent) for the clean humid and polluted-dry cases, respectively. Consequently, the rei is increased in both cases, with a larger increase in the polluted-dry case. As a result, extinction coefficient of cloud anvils is reduced by over 25% for the polluted-dry case. Anvil size and evolution are also much affected by HomFPs in the polluted-dry case. Higher immersion-freezing rates leads to a stronger convective cloud, with higher precipitation and ice water path under both humid and dry conditions. As a result, homogeneous freezing rates are enhanced by over 20%. Also, the higher immersion-freezing rate results in stronger convection in cloud anvils, much larger anvil size (up to 3 times) and longer lifetime. The moistening effect of deep convection on the WVC in the

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

    PubMed Central

    2012-01-01

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

  4. The Earth Clouds and Radiation Explorer (EarthCARE) Mission: Cloud and Aerosol Lidar and Imager algorithms.

    NASA Astrophysics Data System (ADS)

    Donovan, David; van Zadelhoff, Gerd-Jan; Wandinger, Ulla; Hünerbein, Anjah; Fischer, Jurgen; von Bismarck, Jonas; Eisinger, Michael; Lajas, Dulce; Wehr, Tobias

    2015-04-01

    The value of multi-sensor remote sensing applied to clouds and aerosol has become clear in recent years. For example, combinations of instruments including passive radiometers, lidars and cloud radars have proved invaluable for their ability to retrieve profiles of cloud macrophysical and microphysical properties. This is amply illustrated by various results from the US-DoE ARM (and similar) surface sites as well as results from data collected by sensors aboard the A-train satellites CloudSat, CALIPSO, and Terra. The Earth Clouds Aerosol and Radiation Explorer (EarthCARE) mission is a combined ESA/JAXA mission to be launched in 2018 which has been designed with sensor-synergy playing a key role. The mission consists of a cloud-profiling radar (CPR), a high-spectral resolution cloud/aerosol lidar (ATLID), a cloud/aerosol multi-spectral imager (MSI), and a three-view broad-band radiometer (BBR). The mission will deliver cloud, aerosol and radiation products focusing on horizontal scales ranging from 1 km to 10 km. EarthCARE data will be used in multiple ways ranging from model evaluation studies, to GCM-orientated cloud microphysical property parameterization development, to data assimilation activities. Recently a number of activities, funded by ESA, have kicked-off which will ultimately deliver operational algorithms for EarthCARE. One of these activities is the "Atmospheric Products from Imager and Lidar" (APRIL) project which focuses on the development of lidar, imager and combined lidar-imager cloud and aerosol algorithms. In this presentation an overview of the APRIL algorithms within the wider context of the planned EarthCARE processing chain will be given.

  5. Mechanistic Parameterization of the Kinomic Signal in Peptide Arrays

    PubMed Central

    Dussaq, Alex; Anderson, Joshua C; Willey, Christopher D; Almeida, Jonas S

    2016-01-01

    Kinases play a role in every cellular process involved in tumorigenesis ranging from proliferation, migration, and protein synthesis to DNA repair. While genetic sequencing has identified most kinases in the human genome, it does not describe the ‘kinome’ at the level of activity of kinases against their substrate targets. An attempt to address that limitation and give researchers a more direct view of cellular kinase activity is found in the PamGene PamChip® system, which records and compares the phosphorylation of 144 tyrosine or serine/threonine peptides as they are phosphorylated by cellular kinases. Accordingly, the kinetics of this time dependent kinomic signal needs to be well understood in order to transduce a parameter set into an accurate and meaningful mathematical model. Here we report the analysis and mathematical modeling of kinomic time series, which achieves a more accurate description of the accumulation of phosphorylated product than the current model, which assumes first order enzyme-substrate kinetics. Reproducibility of the proposed solution was of particular attention. Specifically, the non-linear parameterization procedure is delivered as a public open source web application where kinomic time series can be accurately decomposed into the model’s two parameter values measuring phosphorylation rate and capacity. The ability to deliver model parameterization entirely as a client side web application is an important result on its own given increasing scientific preoccupation with reproducibility. There is also no need for a potentially transitory and opaque server-side component maintained by the authors, nor of exchanging potentially sensitive data as part of the model parameterization process since the code is transferred to the browser client where it can be inspected and executed. PMID:27601856

  6. A Bioluminescence Assay System for Imaging Metal Cationic Activities in Urban Aerosols.

    PubMed

    Kim, Sung-Bae; Naganawa, Ryuichi; Murata, Shingo; Nakayama, Takayoshi; Miller, Simon; Senda, Toshiya

    2016-01-01

    A bioluminescence-based assay system was fabricated for an efficient determination of the activities of air pollutants. The following four components were integrated into this assay system: (1) an 8-channel assay platform uniquely designed for simultaneously sensing multiple optical samples, (2) single-chain probes illuminating toxic chemicals or heavy metal cations from air pollutants, (3) a microfluidic system for circulating medium mimicking the human body, and (4) the software manimulating the above system. In the protocol, we briefly introduce how to integrate the components into the system and the application to the illumination of the metal cationic activities in air pollutants. PMID:27424913

  7. Indian aerosols: present status.

    PubMed

    Mitra, A P; Sharma, C

    2002-12-01

    This article presents the status of aerosols in India based on the research activities undertaken during last few decades in this region. Programs, like International Geophysical Year (IGY), Monsoon Experiment (MONEX), Indian Middle Atmospheric Program (IMAP) and recently conducted Indian Ocean Experiment (INDOEX), have thrown new lights on the role of aerosols in global change. INDOEX has proved that the effects of aerosols are no longer confined to the local levels but extend at regional as well as global scales due to occurrence of long range transportation of aerosols from source regions along with wind trajectories. The loading of aerosols in the atmosphere is on rising due to energy intensive activities for developmental processes and other anthropogenic activities. One of the significant observation of INDOEX is the presence of high concentrations of carbonaceous aerosols in the near persistent winter time haze layer over tropical Indian Ocean which have probably been emitted from the burning of fossil-fuels and biofuels in the source region. These have significant bearing on the radiative forcing in the region and, therefore, have potential to alter monsoon and hydrological cycles. In general, the SPM concentrations have been found to be on higher sides in ambient atmosphere in many Indian cities but the NOx concentrations have been found to be on lower side. Even in the haze layer over Indian Ocean and surrounding areas, the NOx concentrations have been reported to be low which is not conducive of O3 formation in the haze/smog layer. The acid rain problem does not seem to exist at the moment in India because of the presence of neutralizing soil dust in the atmosphere. But the high particulate concentrations in most of the cities' atmosphere in India are of concern as it can cause deteriorated health conditions. PMID:12492171

  8. Cloud parameterization for climate modeling - Status and prospects

    NASA Technical Reports Server (NTRS)

    Randall, David A.

    1989-01-01

    The current status of cloud parameterization research is reviewed. It is emphasized that the upper tropospheric stratiform clouds associated with deep convection are both physically important and poorly parameterized in current models. Emerging parameterizations are described in general terms, with emphasis on prognostic cloud water and fractional cloudiness, and how these relate to the problem just mentioned.

  9. Parameterization of cloud effects on the absorption of solar radiation

    NASA Technical Reports Server (NTRS)

    Davies, R.

    1983-01-01

    A radiation parameterization for the NASA Goddard climate model was developed, tested, and implemented. Interactive and off-hire experiments with the climate model to determine the limitations of the present parameterization scheme are summarized. The parameterization of Cloud absorption in terms of solar zeith angle, column water vapors about the cloud top, and cloud liquid water content is discussed.

  10. Numerical Archetypal Parameterization for Mesoscale Convective Systems

    NASA Astrophysics Data System (ADS)

    Yano, J. I.

    2015-12-01

    Vertical shear tends to organize atmospheric moist convection into multiscale coherent structures. Especially, the counter-gradient vertical transport of horizontal momentum by organized convection can enhance the wind shear and transport kinetic energy upscale. However, this process is not represented by traditional parameterizations. The present paper sets the archetypal dynamical models, originally formulated by the second author, into a parameterization context by utilizing a nonhydrostatic anelastic model with segmentally-constant approximation (NAM-SCA). Using a two-dimensional framework as a starting point, NAM-SCA spontaneously generates propagating tropical squall-lines in a sheared environment. A high numerical efficiency is achieved through a novel compression methodology. The numerically-generated archetypes produce vertical profiles of convective momentum transport that are consistent with the analytic archetype.

  11. Rapid Parameterization Schemes for Aircraft Shape Optimization

    NASA Technical Reports Server (NTRS)

    Li, Wu

    2012-01-01

    A rapid shape parameterization tool called PROTEUS is developed for aircraft shape optimization. This tool can be applied directly to any aircraft geometry that has been defined in PLOT3D format, with the restriction that each aircraft component must be defined by only one data block. PROTEUS has eight types of parameterization schemes: planform, wing surface, twist, body surface, body scaling, body camber line, shifting/scaling, and linear morphing. These parametric schemes can be applied to two types of components: wing-type surfaces (e.g., wing, canard, horizontal tail, vertical tail, and pylon) and body-type surfaces (e.g., fuselage, pod, and nacelle). These schemes permit the easy setup of commonly used shape modification methods, and each customized parametric scheme can be applied to the same type of component for any configuration. This paper explains the mathematics for these parametric schemes and uses two supersonic configurations to demonstrate the application of these schemes.

  12. Stochastic methods for aerosol chemistry: a compact molecular description of functionalization and fragmentation in the heterogeneous oxidation of squalane aerosol by OH radicals.

    PubMed

    Wiegel, A A; Wilson, K R; Hinsberg, W D; Houle, F A

    2015-02-14

    The heterogeneous oxidation of organic aerosol by hydroxyl radicals (OH) can proceed through two general pathways: functionalization, in which oxygen functional groups are added to the carbon skeleton, and fragmentation, in which carbon-carbon bonds are broken, producing higher volatility, lower molecular weight products. An ongoing challenge is to develop a quantitative molecular description of these pathways that connects the oxidative evolution of the average aerosol properties (e.g. size and hygroscopicity) to the transformation of free radical intermediates. In order to investigate the underlying molecular mechanism of aerosol oxidation, a relatively compact kinetics model is developed for the heterogeneous oxidation of squalane particles by OH using free radical intermediates that convert reactive hydrogen sites into oxygen functional groups. Stochastic simulation techniques are used to compare calculated system properties over ten oxidation lifetimes with the same properties measured in experiment. The time-dependent average squalane aerosol mass, volume, density, carbon number distribution of scission products, and the average elemental composition are predicted using known rate coefficients. For functionalization, the calculations reveal that the distribution of alcohol and carbonyl groups is controlled primarily by the initial OH abstraction rate and to lesser extent by the branching ratio between secondary peroxy radical product channels. For fragmentation, the calculations reveal that the formation of activated alkoxy radicals with neighboring functional groups controls the molecular decomposition, particularly at high O/C ratios. This kinetic scheme provides a framework for understanding the oxidation chemistry of a model organic aerosol and informs parameterizations of more complex systems. PMID:25578323

  13. Increased Cloud Activation Potential of Secondary Organic Aerosol for Atmospheric Mass Loadings

    SciTech Connect

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

    2009-05-01

    The effect of organic particle mass loading from 1 to ≥100 μg m-3 on the cloud condensation nuclei (CCN) properties of mixed organic-sulfate particles was investigated in the Harvard Environmental Chamber. Mixed particles were produced by the condensation of organic molecules onto ammonium sulfate particles during the dark ozonolysis of α-pinene. A continuous-flow mode of the chamber provided stable conditions over long time periods, allowing for signal integration and hence increased measurement precision at low organic mass loadings representative of atmospheric conditions. CCN activity was measured at eight mass loadings for 80- and 100-nm particles grown on 50-nm sulfate seeds. A two-component (organic/sulfate) Köhler model, which included the particle heterogeneity arising from DMA size selection and from organic volume fraction for the selected 80- and 100-nm particles, was used to predict CCN activity. For organic mass loadings of 2.9 μg m-3 and greater, the observed activation curves were well predicted using a single set of physicochemical parameters for the organic component. For mass loadings of 1.74 μg m-3 and less, the observed CCN activity increased beyond predicted values using the same parameters, implying changed physicochemical properties of the organic component. Of possible changes in surface tension, effective molecular weight, and effective density, a sensitivity analysis implicated a decrease of up to 10% in surface tension at low mass loadings as the plausible dominant mechanism for the observed increase in CCN activity.

  14. A Survey of Shape Parameterization Techniques

    NASA Technical Reports Server (NTRS)

    Samareh, Jamshid A.

    1999-01-01

    This paper provides a survey of shape parameterization techniques for multidisciplinary optimization and highlights some emerging ideas. The survey focuses on the suitability of available techniques for complex configurations, with suitability criteria based on the efficiency, effectiveness, ease of implementation, and availability of analytical sensitivities for geometry and grids. The paper also contains a section on field grid regeneration, grid deformation, and sensitivity analysis techniques.

  15. Evolution of Organic Aerosols in the Atmosphere.

    SciTech Connect

    Jimenez, J. L.; Canagaratna, M. R.; Donahue, N. M.; Prevot, A. S. H.; Zhang, Qi; Kroll, Jesse H.; DeCarlo, Peter F.; Allan, James D.; Coe, H.; Ng, N. L.; Aiken, Allison; Docherty, Kenneth S.; Ulbrich, Ingrid M.; Grieshop, A. P.; Robinson, A. L.; Duplissy, J.; Smith, J. D.; Wilson, K. R.; Lanz, V. A.; Hueglin, C.; Sun, Y. L.; Tian, J.; Laaksonen, A.; Raatikainen, T.; Rautiainen, J.; Vaattovaara, P.; Ehn, M.; Kulmala, M.; Tomlinson, Jason M.; Collins, Donald R.; Cubison, Michael J.; Dunlea, E. J.; Huffman, John A.; Onasch, Timothy B.; Alfarra, M. R.; Williams, Paul I.; Bower, K.; Kondo, Yutaka; Schneider, J.; Drewnick, F.; Borrmann, S.; Weimer, S.; Demerjian, K.; Salcedo, D.; Cottrell, L.; Griffin, Robert; Takami, A.; Miyoshi, T.; Hatakeyama, S.; Shimono, A.; Sun, J. Y.; Zhang, Y. M.; Dzepina, K.; Kimmel, Joel; Sueper, D.; Jayne, J. T.; Herndon, Scott C.; Trimborn, Achim; Williams, L. R.; Wood, Ezra C.; Middlebrook, A. M.; Kolb, C. E.; Baltensperger, Urs; Worsnop, Douglas R.

    2009-12-11

    Organic aerosol (OA) particles affect climate forcing and human health, but their sources and evolution remain poorly characterized. We present a unifying model framework that describes the atmospheric evolution of OA and is constrained and motivated by new, high time resolution, experimental characterizations of their composition, volatility, and oxidation state. OA and OA-precursor gases evolve by becoming increasingly oxidized, less volatile, and more hygroscopic, leading to the formation of large amounts of oxygenated organic aerosol (OOA) mass that has comparable concentrations to sulfate aerosol over the Northern Hemisphere. Our new model framework captures the dynamic aging behavior observed in the atmosphere and the laboratory and can serve as a basis for improving parameterizations in regional and global models.

  16. Implicit Shape Parameterization for Kansei Design Methodology

    NASA Astrophysics Data System (ADS)

    Nordgren, Andreas Kjell; Aoyama, Hideki

    Implicit shape parameterization for Kansei design is a procedure that use 3D-models, or concepts, to span a shape space for surfaces in the automotive field. A low-dimensional, yet accurate shape descriptor was found by Principal Component Analysis of an ensemble of point-clouds, which were extracted from mesh-based surfaces modeled in a CAD-program. A theoretical background of the procedure is given along with step-by-step instructions for the required data-processing. The results show that complex surfaces can be described very efficiently, and encode design features by an implicit approach that does not rely on error-prone explicit parameterizations. This provides a very intuitive way to explore shapes for a designer, because various design features can simply be introduced by adding new concepts to the ensemble. Complex shapes have been difficult to analyze with Kansei methods due to the large number of parameters involved, but implicit parameterization of design features provides a low-dimensional shape descriptor for efficient data collection, model-building and analysis of emotional content in 3D-surfaces.

  17. Aerosol chemistry in GLOBE

    NASA Technical Reports Server (NTRS)

    Clarke, Antony D.; Rothermel, Jeffry; Jarzembski, Maurice A.

    1993-01-01

    This task addresses the measurement and understanding of the physical and chemical properties of aerosol in remote regions that are responsible for aerosol backscatter at infrared wavelengths. Because it is representative of other clean areas, the remote Pacific is of extreme interest. Emphasis is on the determination size dependent aerosol properties that are required for modeling backscatter at various wavelengths and upon those features that may be used to help understand the nature, origin, cycling and climatology of these aerosols in the remote troposphere. Empirical relationships will be established between lidar measurements and backscatter derived from the aerosol microphysics as required by the NASA Doppler Lidar Program. This will include the analysis of results from the NASA GLOBE Survey Mission Flight Program. Additional instrument development and deployment will be carried out in order to extend and refine this data base. Identified activities include participation in groundbased and airborne experiments. Progress to date includes participation in, analysis of, and publication of results from Mauna Loa Backscatter Intercomparison Experiment (MABIE) and Global Backscatter Experiment (GLOBE).

  18. Contribution of fungi to primary biogenic aerosols in the atmosphere: active discharge of spores, carbohydrates, and inorganic ions by Asco- and Basidiomycota

    NASA Astrophysics Data System (ADS)

    Elbert, W.; Taylor, P. E.; Andreae, M. O.; Pöschl, U.

    2006-11-01

    Spores and related chemical compounds from actively spore-discharging Ascomycota (AAM) and actively spore-discharging Basidiomycota (ABM) are primary biogenic components of air particulate matter (characteristic size range 1-10 μm). Measurement results and budget calculations based on investigations in Amazonia (Balbina, Brazil, July 2001) indicate that the forcible discharge of fungal spores may account for a large proportion of coarse air particulate matter in tropical rainforest regions during the wet season. For the particle diameter range of 1-10 μm, the estimated proportions are ~25% during day-time, ~45% at night, and ~35% on average. For the sugar alcohol, mannitol, the budget calculations indicate that it is suitable for use as a molecular tracer for actively discharged basidiospores (ABS), and that the literature-derived emission ratio of about 5 pg per ABS may be taken as a representative average. ABM emissions may account for most of the atmospheric abundance of mannitol, and can explain the observed diurnal cycle (higher abundance at night). ABM emissions of hexose carbohydrates might also account for a significant proportion of glucose and fructose in air particulate matter, but the literature-derived ratios are not consistent with the observed diurnal cycle (lower abundance at night). AAM emissions appear to account for a large proportion of potassium in air particulate matter over tropical rainforest regions during the wet season, and they can also explain the observed diurnal cycle (higher abundance at night). The results of our investigations and budget calculations for tropical rainforest aerosols are consistent with measurements performed at other locations. Based on the average abundance of mannitol in particulate matter, which is consistent with the above emission ratio and the observed abundance of ABS, we have also calculated a value of ~17 Tg yr-1 as a first estimate for the global average emission rate of ABS over land surfaces

  19. Identifying Aerosol Type/Mixture from Aerosol Absorption Properties Using AERONET

    NASA Technical Reports Server (NTRS)

    Giles, D. M.; Holben, B. N.; Eck, T. F.; Sinyuk, A.; Dickerson, R. R.; Thompson, A. M.; Slutsker, I.; Li, Z.; Tripathi, S. N.; Singh, R. P.; Zibordi, G.

    2010-01-01

    Aerosols are generated in the atmosphere through anthropogenic and natural mechanisms. These sources have signatures in the aerosol optical and microphysical properties that can be used to identify the aerosol type/mixture. Spectral aerosol absorption information (absorption Angstrom exponent; AAE) used in conjunction with the particle size parameterization (extinction Angstrom exponent; EAE) can only identify the dominant absorbing aerosol type in the sample volume (e.g., black carbon vs. iron oxides in dust). This AAE/EAE relationship can be expanded to also identify non-absorbing aerosol types/mixtures by applying an absorption weighting. This new relationship provides improved aerosol type distinction when the magnitude of absorption is not equal (e.g, black carbon vs. sulfates). The Aerosol Robotic Network (AERONET) data provide spectral aerosol optical depth and single scattering albedo - key parameters used to determine EAE and AAE. The proposed aerosol type/mixture relationship is demonstrated using the long-term data archive acquired at AERONET sites within various source regions. The preliminary analysis has found that dust, sulfate, organic carbon, and black carbon aerosol types/mixtures can be determined from this AAE/EAE relationship when applying the absorption weighting for each available wavelength (Le., 440, 675, 870nm). Large, non-spherical dust particles absorb in the shorter wavelengths and the application of 440nm wavelength absorption weighting produced the best particle type definition. Sulfate particles scatter light efficiently and organic carbon particles are small near the source and aggregate over time to form larger less absorbing particles. Both sulfates and organic carbon showed generally better definition using the 870nm wavelength absorption weighting. Black carbon generation results from varying combustion rates from a number of sources including industrial processes and biomass burning. Cases with primarily black carbon showed

  20. Parameterization Impacts on Linear Uncertainty Calculation

    NASA Astrophysics Data System (ADS)

    Fienen, M. N.; Doherty, J.; Reeves, H. W.; Hunt, R. J.

    2009-12-01

    Efficient linear calculation of model prediction uncertainty can be an insightful diagnostic metric for decision-making. Specifically, the contributions of parameter uncertainty or the location and type of data to prediction uncertainty can be used to evaluate which types of information are most valuable. Information that most significantly reduces prediction uncertainty can be considered to have greater worth. Prediction uncertainty is commonly calculated including or excluding specific information and compared to a base scenario. The quantitative difference in uncertainty with or without the information is indicative of that information's worth in the decision-making process. These results can be calculated at many hypothetical locations to guide network design (i.e., where to install new wells/stream gages/etc.) or used to indicate which parameters are the most important to understand thus likely candidates for future characterization work. We examine a hypothetical case in which an inset model is created from a large regional model in order to better represent a surface stream network and make predictions of head near and flux in a stream due to installation and pumping of a large well near a stream headwater. Parameterization and edge boundary conditions are inherited from the regional model, the simple act of refining discretization and stream geometry shows improvement in the representation of the streams. Even visual inspection of the simulated head field highlights the need to recalibrate and potentially re-parametrize the inset model. A network of potential head observations is evaluated and contoured in the shallowest two layers of the six-layer model to assess their worth in both predicting flux at a specific gage, and head at a specific location near the stream. Three hydraulic conductivity parameterization scenarios are evaluated: using a single multiplier on hydraulic conductivity acting on the inherited hydraulic conductivity zonation using; the

  1. Enhanced Bactericidal Activity of Silver Thin Films Deposited via Aerosol-Assisted Chemical Vapor Deposition.

    PubMed

    Ponja, Sapna D; Sehmi, Sandeep K; Allan, Elaine; MacRobert, Alexander J; Parkin, Ivan P; Carmalt, Claire J

    2015-12-30

    Silver thin films were deposited on SiO2-barrier-coated float glass, fluorine-doped tin oxide (FTO) glass, Activ glass, and TiO2-coated float glass via AACVD using silver nitrate at 350 °C. The films were annealed at 600 °C and analyzed by X-ray powder diffraction, X-ray photoelectron spectroscopy, UV/vis/near-IR spectroscopy, and scanning electron microscopy. All the films were crystalline, and the silver was present in its elemental form and of nanometer dimension. The antibacterial activity of these samples was tested against Escherichia coli and Staphylococcus aureus in the dark and under UV light (365 nm). All Ag-deposited films reduced the numbers of E. coli by 99.9% within 6 h and the numbers of S. aureus by 99.9% within only 2 h. FTO/Ag reduced bacterial numbers of E. coli to below the detection limit after 60 min and caused a 99.9% reduction of S. aureus within only 15 min of UV irradiation. Activ/Ag reduced the numbers of S. aureus by 66.6% after 60 min and TiO2/Ag killed 99.9% of S. aureus within 60 min of UV exposure. More remarkably, we observed a 99.9% reduction in the numbers of E. coli within 6 h and the numbers of S. aureus within 4 h in the dark using our novel TiO2/Ag system. PMID:26632854

  2. Numerical simulations of snowfall events: Sensitivity analysis of physical parameterizations

    NASA Astrophysics Data System (ADS)

    Fernández-González, S.; Valero, F.; Sánchez, J. L.; Gascón, E.; López, L.; García-Ortega, E.; Merino, A.

    2015-10-01

    Accurate estimation of snowfall episodes several hours or even days in advance is essential to minimize risks to transport and other human activities. Every year, these episodes cause severe traffic problems on the northwestern Iberian Peninsula. In order to analyze the influence of different parameterization schemes, 15 snowfall days were analyzed with the Weather Research and Forecasting (WRF) model, defining three nested domains with resolutions of 27, 9, and 3 km. We implemented four microphysical parameterizations (WRF Single-Moment 6-class scheme, Goddard, Thompson, and Morrison) and two planetary boundary layer schemes (Yonsei University and Mellor-Yamada-Janjic), yielding eight distinct combinations. To validate model estimates, a network of 97 precipitation gauges was used, together with dichotomous data of snowfall presence/absence from snowplow requests to the emergency service of Spain and observatories of the Spanish Meteorological Agency. The results indicate that the most accurate setting of WRF for the study area was that using the Thompson microphysical parameterization and Mellor-Yamada-Janjic scheme, although the Thompson and Yonsei University combination had greater accuracy in determining the temporal distribution of precipitation over 1 day. Combining the eight deterministic members in an ensemble average improved results considerably. Further, the root mean square difference decreased markedly using a multiple linear regression as postprocessing. In addition, our method was able to provide mean ensemble precipitation and maximum expected precipitation,which can be very useful in the management of water resources. Finally, we developed an application that allows determination of the risk of snowfall above a certain threshold.

  3. Cloud-Driven Changes in Aerosol Optical Properties - Final Technical Report

    SciTech Connect

    Ogren, John A.; Sheridan, Patrick S.; Andrews, Elisabeth

    2007-09-30

    The optical properties of aerosol particles are the controlling factors in determining direct aerosol radiative forcing. These optical properties depend on the chemical composition and size distribution of the aerosol particles, which can change due to various processes during the particles’ lifetime in the atmosphere. Over the course of this project we have studied how cloud processing of atmospheric aerosol changes the aerosol optical properties. A counterflow virtual impactor was used to separate cloud drops from interstitial aerosol and parallel aerosol systems were used to measure the optical properties of the interstitial and cloud-scavenged aerosol. Specifically, aerosol light scattering, back-scattering and absorption were measured and used to derive radiatively significant parameters such as aerosol single scattering albedo and backscatter fraction for cloud-scavenged and interstitial aerosol. This data allows us to demonstrate that the radiative properties of cloud-processed aerosol can be quite different than pre-cloud aerosol. These differences can be used to improve the parameterization of aerosol forcing in climate models.

  4. Cloud Scavenging Effects on Aerosol Radiative and Cloud-nucleating Properties - Final Technical Report

    SciTech Connect

    Ogren, John A.; Sheridan, Patrick S.; Andrews, Elisabeth

    2009-03-05

    The optical properties of aerosol particles are the controlling factors in determining direct aerosol radiative forcing. These optical properties depend on the chemical composition and size distribution of the aerosol particles, which can change due to various processes during the particles’ lifetime in the atmosphere. Over the course of this project we have studied how cloud processing of atmospheric aerosol changes the aerosol optical properties. A counterflow virtual impactor was used to separate cloud drops from interstitial aerosol and parallel aerosol systems were used to measure the optical properties of the interstitial and cloud-scavenged aerosol. Specifically, aerosol light scattering, back-scattering and absorption were measured and used to derive radiatively significant parameters such as aerosol single scattering albedo and backscatter fraction for cloud-scavenged and interstitial aerosol. This data allows us to demonstrate that the radiative properties of cloud-processed aerosol can be quite different than pre-cloud aerosol. These differences can be used to improve the parameterization of aerosol forcing in climate models.

  5. Aerosol in the Pacific troposphere

    NASA Technical Reports Server (NTRS)

    Clarke, Antony D.

    1989-01-01

    The use of near real-time optical techniques is emphasized for the measurement of mid-tropospheric aerosol over the Central Pacific. The primary focus is on measurement of the aerosol size distribution over the range of particle diameters from 0.15 to 5.0 microns that are essential for modeling CO2 backscatter values in support of the laser atmospheric wind sounder (LAWS) program. The measurement system employs a LAS-X (Laser Aerosol Spectrometer-PMS, Boulder, CO) with a custom 256 channel pulse height analyzer and software for detailed measurement and analysis of aerosol size distributions. A thermal preheater system (Thermo Optic Aerosol Descriminator (TOAD) conditions the aerosol in a manner that allows the discrimination of the size distribution of individual aerosol components such as sulfuric acid, sulfates and refractory species. This allows assessment of the relative contribution of each component to the BCO2 signal. This is necessary since the different components have different sources, exhibit independent variability and provide different BCO2 signals for a given mass and particle size. Field activities involve experiments designed to examine both temporal and spatial variability of these aerosol components from ground based and aircraft platforms.

  6. Limitations on Cloud-Resolving Models Posed by Their Sub-Grid Parameterizations (Invited)

    NASA Astrophysics Data System (ADS)

    Donner, L.

    2013-12-01

    Among the important applications of cloud-resolving models (CRMs) are their use in multi-scale model frameworks and as 'ground truth' for developing parameterizations for coarser-resolution models for numerical weather prediction and climate simulation. Both of these applications are limited in critical ways by deficiencies in the CRM's own sub-grid parameterizations for turbulence and smaller-scale clouds. Microphysics, aerosols, and associated cloud-radiation interactions are particularly important problems where these CRM limitations are apparent, and a focus of these problems is the CRM simulation of vertical velocities. Realistic simulation of vertical velocities is essential for many aerosol and microphysical processes. Radar observations of vertical velocities in deep convection are becoming available in the DOE ARM program and can be used to evaluate vertical velocities in CRMs. Early results indicate problems both with the magnitude and vertical profile shape of vertical velocities in deep convection in some CRMs. Possible solutions include higher-resolution CRMs, for example, 'giga-LES,' and the use of higher-order-closure methods in coarser-resolution CRMs.

  7. Ice Nucleation in Mixed-Phase Clouds: Parameterization Evaluation and Climate Impacts

    NASA Astrophysics Data System (ADS)

    Liu, X.; Ghan, S. J.; Xie, S.; Boyle, J. S.; Klein, S. A.; Demott, P. J.; Prenni, A. J.

    2009-12-01

    There are still large uncertainties on ice nucleation mechanisms and ice crystal numbers in mixed-phase clouds, which affects modeled cloud phase, cloud lifetime and radiative properties in the Arctic clouds in global climate models. In this study we evaluate model simulations with three mixed-phase ice nucleation parameterizations (Phillips et al., 2008; DeMott et al., 2009; Meyers et al. 1992) against the Atmospheric Radiation Measurement (ARM) Indirect and Semi-Direct Aerosol Campaign (ISDAC) observations using the NCAR Community Atmospheric Model Version 4 (CAM4) running in the single column mode (SCAM) and in the CCPP-ARM Parameterization Testbed (CAPT) forecasts. It is found that SCAM and CAPT with the new physically-based ice nucleation schemes (Phillips et al., 2008; DeMott et al., 2009) produce a more realistic simulation of the cloud phase structure and the partitioning of condensed water into liquid droplets against observations during the ISDAC than the CAM with an oversimplified Meyers et al. (1992). Both SCAM simulations and CAPT forecasts suggest that the ice number concentration could play an important role in the simulated mixed-phase cloud microphysics, and thereby needs to be realistically represented in global climate models. The global climate implication of different ice nucleation parameterizations are also be studied.

  8. Microphysics Parameterization in Convection and its Effects on Cloud Simulation in the NCAR CAM5

    NASA Astrophysics Data System (ADS)

    Zhang, G. J.; Song, X.

    2010-12-01

    Microphysical processes in convection are important to convection-cloud-climate interactions and atmospheric hydrological cycle. They are also essential to understanding aerosol-cloud interaction. However, their parameterization in GCMs is crude. As part of an effort to improve the convection parameterization scheme for the NCAR CAM using observations, we incorporate a cloud microphysics parameterization into the Zhang-McFarlane convection scheme. The scheme is then evaluated against observations of cloud ice and water from the TWP-ICE experiment and other sources using the NCAR SCAM. It is found that this physically-based treatment of convective microphysics yields more realistic vertical profiles of convective cloud ice and liquid water contents. Cloud water and ice budgets are calculated to estimate the role of cloud water and ice detrainment from convection as water and ice sources for large-scale clouds. The new microphysics treatment is further implemented into CAM5 to test its effect on GCM simulations of clouds. Results will be presented at the meeting, and the implications on the simulation of hydrological cycle will be discussed.

  9. Sensitivity of Homogeneous Freezing to Aerosol Perturbation and Implication for Aerosol Indirect Forcing through Cirrus Clouds

    NASA Astrophysics Data System (ADS)

    Liu, X.; Shi, X.; Zhang, K.

    2014-12-01

    The susceptibility of cloud properties to aerosol perturbation is critical for the aerosol-cloud-climate interactions. Burdens of aerosols such as sulfate have substantially increased from preindustrial time to present-day. However, it is still not clear whether the number of ice crystals (Ni) resulting from homogeneous freezing of sulfate solution droplets is sensitive to the change in sulfate number concentration (Na) in the upper troposphere. Some cloud parcel modeling studies show that Ni is insensitive to Na (Kärcher and Lohmann, 2002; Kay and Wood, 2008), while others show moderate sensitivity of Ni to Na (Liu and Penner, 2005; Barahona and Nenes, 2008). The poorly understood cirrus cloud processes lead to large uncertainties in ice nucleation parameterizations in global climate models, with implications for climate change studies. In this study, we examine the sensitivity of Ni from homogeneous freezing to Na with a cloud parcel model running at different input aerosol and cloud conditions and under different model assumptions. By these sensitivity tests, we are able to reconcile the contrasting results from previous studies on the sensitivity of Ni to Na. Furthermore, the implications of these results on aerosol indirect forcing through ice clouds are quantified by comparing three ice nucleation parameterizations (Liu and Penner, 2005; Barahona and Nenes, 2008; Kärcher and Lohmann, 2002) implemented in the Community Atmospheric Model version 5 (CAM5). The global and annual mean longwave aerosol indirect forcing through cirrus clouds ranges from -0.03 (Kärcher and Lohmann, 2002) to ~0.3 W m-2 (Liu and Penner, 2005; Barahona and Nenes, 2008). Future studies should quantify the occurrence frequency of homogeneous nucleation in the upper troposphere and the relative contribution between homogeneous versus heterogeneous freezing to Ni in cirrus clouds to further narrow down the aerosol indirect forcing through cirrus clouds.

  10. Development of new parameterizations for SOA production from SVOC and IVOC oxidation

    NASA Astrophysics Data System (ADS)

    Lemaire, Vincent; Coll, Isabelle; Camredon, Marie; Aumont, Bernard; Siour, Guillaume

    2014-05-01

    Recent experimental studies have demonstrated the partially volatile pattern of primary organic aerosol (POA) that is actually associated with organic species of so-called intermediate volatility (IVOCs), and by semi-volatile (SVOCs) species. Indeed, 50% to 75% of the total emitted mass of POA may be present in the atmospheric gas phase in accordance with the thermodynamic properties of its components (Shrivastava et al., 2006). During the processing of the emission plume, this gaseous material will then undergo photochemical oxidation, enhancing the production of secondary organic aerosol (SOA) (Robinson et al., 2007; Hodzic et al., 2010; Lee-Taylor et al., 2011). Considering POA as non volatile in Chemistry Transport Models (CTMs) could thus lead to an underestimation of SOA and an overestimation of POA (Aksoyoglu et al., 2011) and bias the temporal formation of the organic aerosol (Kroll et al., 2007; Presto et al., 2012). However, very rare experimental data exist on the fate of these species and their aerosol yield, but all existing studies have shown a significant SOA production (Presto et al., 2009; Miracolo et al., 2010; Lambe et al., 2012). Our works aims at including and testing in the CHIMERE CTM new parameterizations of SOA formation from the oxidation of IVOCs and SVOCs, arising from explicit 0D-model experiments. Our approach is based on the works of Aumont et al., (2013) who used the GECKO-A tool (Generator for Explicit Chemistry and Kinetics of Organics in the Atmosphere) to generate the explicit chemistry and gas-particle partitioning of superior alkanes and their oxidation products. Using this explicit scheme, Aumont et al., (2013) indeed produced 0D simulations of the oxidation of given SVOCs and IVOCs under different initial conditions of organic aerosol mass. We first focused on the chemistry of n-hexadecane. From the 0D-experiments, we tested the influence of the number of first generation surrogate species and the number of generation taken

  11. The global aerosol-climate model ECHAM-HAM, version 2: sensitivity to improvements in process representations

    NASA Astrophysics Data System (ADS)

    Zhang, K.; O'Donnell, D.; Kazil, J.; Stier, P.; Kinne, S.; Lohmann, U.; Ferrachat, S.; Croft, B.; Quaas, J.; Wan, H.; Rast, S.; Feichter, J.

    2012-03-01

    This paper introduces and evaluates the second version of the global aerosol-climate model ECHAM-HAM. Major changes have been brought into the model, including new parameterizations for aerosol nucleation and water uptake, an explicit treatment of secondary organic aerosols, modified emission calculations for sea salt and mineral dust, the coupling of aerosol microphysics to a two-moment stratiform cloud microphysics scheme, and alternative wet scavenging parameterizations. These revisions extend the model's capability to represent details of the aerosol lifecycle and its interaction with climate. Sensitivity experiments are carried out to analyse the effects of these improvements in the process representation on the simulated aerosol properties and global distribution. The new parameterizations that have largest impact on the global mean aerosol optical depth and radiative effects turn out to be the water uptake scheme and cloud microphysics. The former leads to a significant decrease of aerosol water contents in the lower troposphere, and consequently smaller optical depth; the latter results in higher aerosol loading and longer lifetime due to weaker in-cloud scavenging. The combined effects of the new/updated parameterizations are demonstrated by comparing the new model results with those from the earlier version, and against observations. Model simulations are evaluated in terms of aerosol number concentrations against measurements collected from twenty field campaigns as well as from fixed measurement sites, and in terms of optical properties against the AERONET measurements. Results indicate a general improvement with respect to the earlier version. The aerosol size distribution and spatial-temporal variance simulated by HAM2 are in better agreement with the observations. Biases in the earlier model version in aerosol optical depth and in the Ångström parameter have been reduced. The paper also points out the remaining model deficiencies that need to be

  12. FY 2010 Fourth Quarter Report: Evaluation of the Dependency of Drizzle Formation on Aerosol Properties

    SciTech Connect

    Lin, W; McGraw, R; Liu, Y; Wang, J; Vogelmann, A; Daum, PH

    2010-10-01

    Metric for Quarter 4: Report results of implementation of composite parameterization in single-column model (SCM) to explore the dependency of drizzle formation on aerosol properties. To better represent VOCALS conditions during a test flight, the Liu-Duam-McGraw (LDM) drizzle parameterization is implemented in the high-resolution Weather Research and Forecasting (WRF) model, as well as in the single-column Community Atmosphere Model (CAM), to explore this dependency.

  13. International Cooperative for Aerosol Prediction Workshop on Aerosol Forecast Verification

    NASA Technical Reports Server (NTRS)

    Benedetti, Angela; Reid, Jeffrey S.; Colarco, Peter R.

    2011-01-01

    The purpose of this workshop was to reinforce the working partnership between centers who are actively involved in global aerosol forecasting, and to discuss issues related to forecast verification. Participants included representatives from operational centers with global aerosol forecasting requirements, a panel of experts on Numerical Weather Prediction and Air Quality forecast verification, data providers, and several observers from the research community. The presentations centered on a review of current NWP and AQ practices with subsequent discussion focused on the challenges in defining appropriate verification measures for the next generation of aerosol forecast systems.

  14. Evaluating the Impact of Aerosols on Numerical Weather Prediction

    NASA Astrophysics Data System (ADS)

    Freitas, Saulo; Silva, Arlindo; Benedetti, Angela; Grell, Georg; Members, Wgne; Zarzur, Mauricio

    2015-04-01

    The Working Group on Numerical Experimentation (WMO, http://www.wmo.int/pages/about/sec/rescrosscut/resdept_wgne.html) has organized an exercise to evaluate the impact of aerosols on NWP. This exercise will involve regional and global models currently used for weather forecast by the operational centers worldwide and aims at addressing the following questions: a) How important are aerosols for predicting the physical system (NWP, seasonal, climate) as distinct from predicting the aerosols themselves? b) How important is atmospheric model quality for air quality forecasting? c) What are the current capabilities of NWP models to simulate aerosol impacts on weather prediction? Toward this goal we have selected 3 strong or persistent events of aerosol pollution worldwide that could be fairly represented in current NWP models and that allowed for an evaluation of the aerosol impact on weather prediction. The selected events includes a strong dust storm that blew off the coast of Libya and over the Mediterranean, an extremely severe episode of air pollution in Beijing and surrounding areas, and an extreme case of biomass burning smoke in Brazil. The experimental design calls for simulations with and without explicitly accounting for aerosol feedbacks in the cloud and radiation parameterizations. In this presentation we will summarize the results of this study focusing on the evaluation of model performance in terms of its ability to faithfully simulate aerosol optical depth, and the assessment of the aerosol impact on the predictions of near surface wind, temperature, humidity, rainfall and the surface energy budget.

  15. New Parameterization of Neutron Absorption Cross Sections

    NASA Technical Reports Server (NTRS)

    Tripathi, Ram K.; Wilson, John W.; Cucinotta, Francis A.

    1997-01-01

    Recent parameterization of absorption cross sections for any system of charged ion collisions, including proton-nucleus collisions, is extended for neutron-nucleus collisions valid from approx. 1 MeV to a few GeV, thus providing a comprehensive picture of absorption cross sections for any system of collision pairs (charged or uncharged). The parameters are associated with the physics of the problem. At lower energies, optical potential at the surface is important, and the Pauli operator plays an increasingly important role at intermediate energies. The agreement between the calculated and experimental data is better than earlier published results.

  16. Lightning parameterization in a storm electrification model

    NASA Technical Reports Server (NTRS)

    Helsdon, John H., Jr.; Farley, Richard D.; Wu, Gang

    1988-01-01

    The parameterization of an intracloud lightning discharge has been implemented in our Storm Electrification Model. The initiation, propagation direction, termination and charge redistribution of the discharge are approximated assuming overall charge neutrality. Various simulations involving differing amounts of charge transferred have been done. The effects of the lightning-produced ions on the hydrometeor charges, electric field components and electrical energy depend strongly on the charge transferred. A comparison between the measured electric field change of an actual intracloud flash and the field change due to the simulated discharge show favorable agreement.

  17. 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...

  18. Parameterizing correlations between hydrometeor species in mixed-phase Arctic clouds

    SciTech Connect

    Larson, Vincent E.; Nielsen, Brandon J.; Fan, Jiwen; Ovchinnikov, Mikhail

    2011-08-16

    Mixed-phase Arctic clouds, like other clouds, contain small-scale variability in hydrometeor fields, such as cloud water or snow mixing ratio. This variability may be worth parameterizing in coarse-resolution numerical models. In particular, for modeling processes such as accretion and aggregation, it would be useful to parameterize subgrid correlations among hydrometeor species. However, one difficulty is that there exist many hydrometeor species and many microphysical processes, leading to complexity and computational expense.Existing lower and upper bounds (inequalities) on linear correlation coefficients provide useful guidance, but these bounds are too loose to serve directly as a method to predict subgrid correlations. Therefore, this paper proposes an alternative method that is based on a blend of theory and empiricism. The method begins with the spherical parameterization framework of Pinheiro and Bates (1996), which expresses the correlation matrix in terms of its Cholesky factorization. The values of the elements of the Cholesky matrix are parameterized here using a cosine row-wise formula that is inspired by the aforementioned bounds on correlations. The method has three advantages: 1) the computational expense is tolerable; 2) the correlations are, by construction, guaranteed to be consistent with each other; and 3) the methodology is fairly general and hence may be applicable to other problems. The method is tested non-interactively using simulations of three Arctic mixed-phase cloud cases from two different field experiments: the Indirect and Semi-Direct Aerosol Campaign (ISDAC) and the Mixed-Phase Arctic Cloud Experiment (M-PACE). Benchmark simulations are performed using a large-eddy simulation (LES) model that includes a bin microphysical scheme. The correlations estimated by the new method satisfactorily approximate the correlations produced by the LES.

  19. An efficient physically based parameterization to derive surface solar irradiance based on satellite atmospheric products

    NASA Astrophysics Data System (ADS)

    Qin, Jun; Tang, Wenjun; Yang, Kun; Lu, Ning; Niu, Xiaolei; Liang, Shunlin

    2015-05-01

    Surface solar irradiance (SSI) is required in a wide range of scientific researches and practical applications. Many parameterization schemes are developed to estimate it using routinely measured meteorological variables, since SSI is directly measured at a very limited number of stations. Even so, meteorological stations are still sparse, especially in remote areas. Remote sensing can be used to map spatiotemporally continuous SSI. Considering the huge amount of satellite data, coarse-resolution SSI has been estimated for reducing the computational burden when the estimation is based on a complex radiative transfer model. On the other hand, many empirical relationships are used to enhance the retrieval efficiency, but the accuracy cannot be guaranteed out of regions where they are locally calibrated. In this study, an efficient physically based parameterization is proposed to balance computational efficiency and retrieval accuracy for SSI estimation. In this parameterization, the transmittances for gases, aerosols, and clouds are all handled in full band form and the multiple reflections between the atmosphere and surface are explicitly taken into account. The newly proposed parameterization is applied to estimate SSI with both Moderate Resolution Imaging Spectroradiometer (MODIS) atmospheric and land products as inputs. These retrievals are validated against in situ measurements at the Surface Radiation Budget Network and at the North China Plain on an instantaneous basis, and moreover, they are validated and compared with Global Energy and Water Exchanges-Surface Radiation Budget and International Satellite Cloud Climatology Project-flux data SSI estimates at radiation stations of China Meteorological Administration on a daily mean basis. The estimation results indicates that the newly proposed SSI estimation scheme can effectively retrieve SSI based on MODIS products with mean root-mean-square errors of about 100 Wm- 1 and 35 Wm- 1 on an instantaneous and daily

  20. Towards a parameterization of convective wind gusts in Sahel

    NASA Astrophysics Data System (ADS)

    Largeron, Yann; Guichard, Françoise; Bouniol, Dominique; Couvreux, Fleur; Birch, Cathryn; Beucher, Florent

    2014-05-01

    ] who focused on the wet tropical Pacific region, and linked wind gusts to convective precipitation rates alone, here, we also analyse the subgrid wind distribution during convective events, and quantify the statistical moments (variance, skewness and kurtosis) in terms of mean wind speed and convective indexes such as DCAPE. Next step of the work will be to formulate a parameterization of the cold pool convective gust from those probability density functions and analytical formulaes obtained from basic energy budget models. References : [Carslaw et al., 2010] A review of natural aerosol interactions and feedbacks within the earth system. Atmospheric Chemistry and Physics, 10(4):1701{1737. [Engelstaedter et al., 2006] North african dust emissions and transport. Earth-Science Reviews, 79(1):73{100. [Knippertz and Todd, 2012] Mineral dust aerosols over the sahara: Meteorological controls on emission and transport and implications for modeling. Reviews of Geophysics, 50(1). [Marsham et al., 2011] The importance of the representation of deep convection for modeled dust-generating winds over west africa during summer.Geophysical Research Letters, 38(16). [Marticorena and Bergametti, 1995] Modeling the atmospheric dust cycle: 1. design of a soil-derived dust emission scheme. Journal of Geophysical Research, 100(D8):16415{16. [Menut, 2008] Sensitivity of hourly saharan dust emissions to ncep and ecmwf modeled wind speed. Journal of Geophysical Research: Atmospheres (1984{2012), 113(D16). [Pierre et al., 2012] Impact of vegetation and soil moisture seasonal dynamics on dust emissions over the sahel. Journal of Geophysical Research: Atmospheres (1984{2012), 117(D6). [Redelsperger et al., 2000] A parameterization of mesoscale enhancement of surface fluxes for large-scale models. Journal of climate, 13(2):402{421.

  1. Impacts of Ice Nucleation Parameterizations and Dust on Deep Convective C louds and Precipitation

    NASA Astrophysics Data System (ADS)

    Lim, K. S. S.; Fan, J.; Leung, L. Y.; Zhao, C.; Zhang, K.; Ma, P. L.; Phillips, V. T.; Liu, X.; Yang, Q.

    2014-12-01

    Ice nucleation plays a critical role in the formation of ice clouds and converting liquid to ice in mixed-phase clouds. Many past heterogeneous ice nucleation parameterizations (INPs) were developed based on field measurements with the artifacts of shattering, and also not connected with aerosol particles. Recent laboratory and field measurements have led to a few new ice nucleation parameterizations connecting with aerosols, which should be implemented to models and evaluated by observations. In this study, we evaluated three very recently developed heterogeneous INPs linked with dust particles: Niemand et al. (2012), DeMott et al. (2013), and Phillips et al. (2013), using the Weather Research and Forecasting (WRF) model coupled with the physics and aerosol packages from the Community Atmospheric Model version 5 (CAM5). Results from the three new schemes and the default scheme by Meyers et al. (1992) are compared with available observations including aircraft measurements of cloud anvil properties of a storm case from the Deep Convective Clouds and Chemistry (DC3) field campaign. The Meyers scheme simulates higher ice number concentrations (Ni), while the Phillips scheme simulates lower Ni and shows the best agreement with aircraft measurements in the anvil area. Although the total precipitation amount and evolution o