Alla Zelenyuk - Academia.edu (original) (raw)
Papers by Alla Zelenyuk
2017 New York Scientific Data Summit (NYSDS), 2017
Clustering has become an unavoidable step in big data analysis. It may be used to arrange data in... more Clustering has become an unavoidable step in big data analysis. It may be used to arrange data into a compact format, making operations on big data manageable. However, clustering of big data requires not only the capability of handling data with large volume and high dimensionality, but also the ability to process streaming data, all of which are less developed in most current algorithms. Furthermore, big data processing is seldom interactive, which stands at conflict with users who seek answers immediately. The best one can do is to process incrementally, such that partial and, hopefully, accurate results can be available relatively quickly and are then progressively refined over time. We propose a clustering framework which uses Multi-Dimensional Scaling for layout and GPU acceleration to accomplish these goals. Our domain application is the clustering of mass spectral data of individual aerosol particles with 8 million data points of 450 dimensions each.
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Bulletin of the American Meteorological Society, 2021
The Cloud, Aerosol, and Complex Terrain Interactions (CACTI) field campaign was designed to impro... more The Cloud, Aerosol, and Complex Terrain Interactions (CACTI) field campaign was designed to improve understanding of orographic cloud life cycles in relation to surrounding atmospheric thermodynamic, flow, and aerosol conditions. The deployment to the Sierras de Córdoba range in north-central Argentina was chosen because of very frequent cumulus congestus, deep convection initiation, and mesoscale convective organization uniquely observable from a fixed site. The C-band Scanning Atmospheric Radiation Measurement (ARM) Precipitation Radar was deployed for the first time with over 50 ARM Mobile Facility atmospheric state, surface, aerosol, radiation, cloud, and precipitation instruments between October 2018 and April 2019. An intensive observing period (IOP) coincident with the RELAMPAGO field campaign was held between 1 November and 15 December during which 22 flights were performed by the ARM Gulfstream-1 aircraft. A multitude of atmospheric processes and cloud conditions were obser...
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Atmospheric Chemistry and Physics Discussions, 2019
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Atmospheric Chemistry and Physics, 2018
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Environmental science & technology, Jan 21, 2018
We developed a parametrizable box model to empirically derive the yields of semivolatile products... more We developed a parametrizable box model to empirically derive the yields of semivolatile products from VOC oxidation using chamber measurements, while explicitly accounting for the multigenerational chemical aging processes (such as the gas-phase fragmentation and functionalization and aerosol-phase oligomerization and photolysis) under different NO levels and the loss of particles and gases to chamber walls. Using the oxidation of isoprene as an example, we showed that the assumptions regarding the NO -sensitive, multigenerational aging processes of VOC oxidation products have large impacts on the parametrized product yields and SOA formation. We derived sets of semivolatile product yields from isoprene oxidation under different NO levels. However, we stress that these product yields must be used in conjunction with the corresponding multigenerational aging schemes in chemical transport models. As more mechanistic insights regarding SOA formation from VOC oxidation emerge, our box ...
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Environmental science & technology, Jan 15, 2017
Low bulk diffusivity inside viscous semisolid atmospheric secondary organic aerosol (SOA) can pro... more Low bulk diffusivity inside viscous semisolid atmospheric secondary organic aerosol (SOA) can prolong equilibration timescale, but its broader impacts on aerosol growth and size distribution dynamics are poorly understood. Here we present quantitative insights into the effects of bulk diffusivity on the growth and evaporation kinetics of SOA formed under dry conditions from photooxidation of isoprene in the presence of a bimodal aerosol consisting of Aitken (ammonium sulfate) and accumulation (isoprene or -pinene SOA) mode particles. Aerosol composition measurements and evaporation kinetics indicate that isoprene SOA is composed of several semivolatile organic compounds (SVOCs), with some reversibly reacting to form oligomers. Model analysis shows that liquid-like bulk diffusivities can be used to fit the observed evaporation kinetics of accumulation mode particles, but fail to explain the growth kinetics of bimodal aerosol by significantly under-predicting the evolution of the Ait...
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Aerosol Science and Technology, 2016
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Proceedings of the National Academy of Sciences of the United States of America, Feb 7, 2017
Polycyclic aromatic hydrocarbons (PAHs) have toxic impacts on humans and ecosystems. One of the m... more Polycyclic aromatic hydrocarbons (PAHs) have toxic impacts on humans and ecosystems. One of the most carcinogenic PAHs, benzo(a)pyrene (BaP), is efficiently bound to and transported with atmospheric particles. Laboratory measurements show that particle-bound BaP degrades in a few hours by heterogeneous reaction with ozone, yet field observations indicate BaP persists much longer in the atmosphere, and some previous chemical transport modeling studies have ignored heterogeneous oxidation of BaP to bring model predictions into better agreement with field observations. We attribute this unexplained discrepancy to the shielding of BaP from oxidation by coatings of viscous organic aerosol (OA). Accounting for this OA viscosity-dependent shielding, which varies with temperature and humidity, in a global climate/chemistry model brings model predictions into much better agreement with BaP measurements, and demonstrates stronger long-range transport, greater deposition fluxes, and substantia...
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Environmental science & technology, Jun 13, 2016
Multiphase chemistry of isomeric isoprene epoxydiols (IEPOX) has been shown to be the dominant so... more Multiphase chemistry of isomeric isoprene epoxydiols (IEPOX) has been shown to be the dominant source of isoprene-derived secondary organic aerosol (SOA). Recent studies have reported particles composed of ammonium bisulfate (ABS) mixed with model organics exhibit slower rates of IEPOX uptake. In the present study, we investigate the effect of atmospherically-relevant organic coatings of α-pinene (AP) SOA on the reactive uptake of trans-β-IEPOX onto ABS particles under different conditions and coating thicknesses. Single particle mass spectrometry was used to characterize in real-time particle size, shape, density, and quantitative composition before and after reaction with IEPOX. We find that IEPOX uptake by pure sulfate particles is a volume-controlled process, which results in particles with uniform concentration of IEPOX-derived SOA across a wide range of sizes. Aerosol acidity was shown to enhance IEPOX-derived SOA formation, consistent with recent studies. The presence of wate...
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Atmospheric Chemistry and Physics Discussions, 2016
Measurements of the optical properties (absorption, scattering and extinction) of…
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New gasoline engine technologies such as Spark Ignition Direct Injection (SIDI), Gasoline Direct ... more New gasoline engine technologies such as Spark Ignition Direct Injection (SIDI), Gasoline Direct Injection Compression Ignition (GDICI), and Reaction Controlled Compression Ignition (RCCI) offer the possibility of dramatically increasing the fuel efficiency of future vehicles. One drawback to these advanced engines is that they have the potential to produce higher levels of exhaust particulates than current Port Fuel Injection (PFI) engines. Regulation of engine particulate emissions in Europe is moving from mass-based standards toward number-based standards. Due to growing health concerns surrounding nano-aerosols, it is likely that similar standards will eventually be applied in the United States. This would place more emphasis on the reliable removal of smaller particles, which make up the vast majority of the particulates generated on a number basis. While Diesel Particulate Filters (DPF) have become standard, different filter systems would likely be required for advanced gasoline vehicles, due to factors such as differing particulate properties and higher exhaust temperatures. High exhaust temperatures can limit the accumulation of a soot cake, which performs most of the actual filtration in a typical DPF system.
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ABSTRACT
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Atmospheric Chemistry and Physics, 2014
We have developed the novel Aerosol Dynamics, gas- and particle-phase chemistry model for laborat... more We have developed the novel Aerosol Dynamics, gas- and particle-phase chemistry model for laboratory CHAMber studies (ADCHAM). The model combines the detailed gas-phase Master Chemical Mechanism version 3.2 (MCMv3.2), an aerosol dynamics and particle-phase chemistry module (which considers acid-catalysed oligomerization, heterogeneous oxidation reactions in the particle phase and non-ideal interactions between organic compounds, water and inorganic ions) and a kinetic multilayer module for diffusion-limited transport of compounds between the gas phase, particle surface and particle bulk phase. In this article we describe and use ADCHAM to study (1) the evaporation of liquid dioctyl phthalate (DOP) particles, (2) the slow and almost particle-size-independent evaporation of α-pinene ozonolysis secondary organic aerosol (SOA) particles, (3) the mass-transfer-limited uptake of ammonia (NH<sub>3</sub>) and formation of organic salts between ammonium (NH<sub>4</sub>...
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A review of water uptake measurements conducted over the past 25 years using the Humidified Tande... more A review of water uptake measurements conducted over the past 25 years using the Humidified Tandem Differential Mobility Analyzer (HTDMA) technique reveals that ambient Aitken and accumulation mode particles typically grow substantially less at a given relative humidity compared to pure ammonium sulfate. Multiple hygroscopic modes at a single particle size are routinely observed, revealing that ambient particles are externally mixed with respect to their chemical composition. The observed growth of the multiple hygroscopic modes is typically less than that for particles composed of purely soluble salts, indicating that the externally mixed populations are themselves internally mixed with more and less-water soluble species. Therefore, the HTDMA is a powerful tool for quantitative measurements of size-dependent hygroscopic growth factors and for qualitative observations of the complex chemical composition responsible for the observed growth. The strengths and limitations of the HTDMA...
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The Journal of Physical Chemistry C, 2014
Aerosol particles are ubiquitous in the atmosphere and have been shown to impact the Earth’s clim... more Aerosol particles are ubiquitous in the atmosphere and have been shown to impact the Earth’s climate, reduce visibility, and adversely affect human health. Modeling the evolution of aerosol systems requires an understanding of the species and mechanisms involved in particle growth, including the complex interactions between particle- and gas-phase species. Here we report studies of displacement of amines (methylamine, dimethylamine, or trimethylamine) in methanesulfonate salt particles by exposure to a different gas-phase amine, using a single particle mass spectrometer, SPLAT II. The variation of the displacement with the nature of the amine suggests that behavior is dependent on water in or on the particles. Small clusters of methanesulfonic acid with amines are used as a model in quantum chemical calculations to identify key structural elements that are expected to influence water uptake, and hence the efficiency of displacement by gas-phase molecules in the aminium salts. Such molecular-level understa...
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The three major atmospheric oxidants involved in SOA formation from biogenic volatile organic com... more The three major atmospheric oxidants involved in SOA formation from biogenic volatile organic compounds are O3, OH and nitrate radical (NO3). While O3 and OH-initiated oxidation occur during the day, NO3 radical-initiated oxidation is recognized to be a major contributor to the night-time chemistry of volatile organic compounds in the troposphere. Specifically, the reaction of biogenic hydrocarbons with NO3 is
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A unique, high-volume, low-flow, stainless steel aerosol flow system for the study of the formati... more A unique, high-volume, low-flow, stainless steel aerosol flow system for the study of the formation and reactions of aerosols relevant to the troposphere has been constructed, modeled and experimentally tested. The total flow tube length is 7.3 m which includes a 1.2 m section used for mixing. The flow tube is equipped with ultraviolet lamps for photolysis. The diameter of
Bookmarks Related papers MentionsView impact
SAE International Journal of Fuels and Lubricants, 2011
More stringent emissions regulations are continually being proposed to mitigate adverse human hea... more More stringent emissions regulations are continually being proposed to mitigate adverse human health and environmental impacts of internal combustion engines. With that in mind, it has been proposed that vehicular particulate matter (PM) emissions should be regulated based on particle number in addition to particle mass. One aspect of this project is to study different sample handling methods for number based aerosol measurements, specifically, two different methods for removing volatile organic compounds (VOCs). One method is a thermodenuder (TD) and the other is an evaporative chamber/diluter (EvCh). These sample handling methods have been implemented in an engine test cell with a spark ignited direct injection (SIDI) engine. The engine was designed for stoichiometric, homogeneous combustion. SIDI is of particular interest for improved fuel efficiency compared to other SI engines, however, the efficiency benefit comes with greater PM emissions and may therefore be subject to the proposed number based PM regulation. Another aspect of this project is to characterize PM from this engine in terms of particle number and composition.
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SAE Technical Paper Series, 2011
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2017 New York Scientific Data Summit (NYSDS), 2017
Clustering has become an unavoidable step in big data analysis. It may be used to arrange data in... more Clustering has become an unavoidable step in big data analysis. It may be used to arrange data into a compact format, making operations on big data manageable. However, clustering of big data requires not only the capability of handling data with large volume and high dimensionality, but also the ability to process streaming data, all of which are less developed in most current algorithms. Furthermore, big data processing is seldom interactive, which stands at conflict with users who seek answers immediately. The best one can do is to process incrementally, such that partial and, hopefully, accurate results can be available relatively quickly and are then progressively refined over time. We propose a clustering framework which uses Multi-Dimensional Scaling for layout and GPU acceleration to accomplish these goals. Our domain application is the clustering of mass spectral data of individual aerosol particles with 8 million data points of 450 dimensions each.
Bookmarks Related papers MentionsView impact
Bookmarks Related papers MentionsView impact
Bulletin of the American Meteorological Society, 2021
The Cloud, Aerosol, and Complex Terrain Interactions (CACTI) field campaign was designed to impro... more The Cloud, Aerosol, and Complex Terrain Interactions (CACTI) field campaign was designed to improve understanding of orographic cloud life cycles in relation to surrounding atmospheric thermodynamic, flow, and aerosol conditions. The deployment to the Sierras de Córdoba range in north-central Argentina was chosen because of very frequent cumulus congestus, deep convection initiation, and mesoscale convective organization uniquely observable from a fixed site. The C-band Scanning Atmospheric Radiation Measurement (ARM) Precipitation Radar was deployed for the first time with over 50 ARM Mobile Facility atmospheric state, surface, aerosol, radiation, cloud, and precipitation instruments between October 2018 and April 2019. An intensive observing period (IOP) coincident with the RELAMPAGO field campaign was held between 1 November and 15 December during which 22 flights were performed by the ARM Gulfstream-1 aircraft. A multitude of atmospheric processes and cloud conditions were obser...
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Atmospheric Chemistry and Physics Discussions, 2019
Bookmarks Related papers MentionsView impact
Atmospheric Chemistry and Physics, 2018
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Environmental science & technology, Jan 21, 2018
We developed a parametrizable box model to empirically derive the yields of semivolatile products... more We developed a parametrizable box model to empirically derive the yields of semivolatile products from VOC oxidation using chamber measurements, while explicitly accounting for the multigenerational chemical aging processes (such as the gas-phase fragmentation and functionalization and aerosol-phase oligomerization and photolysis) under different NO levels and the loss of particles and gases to chamber walls. Using the oxidation of isoprene as an example, we showed that the assumptions regarding the NO -sensitive, multigenerational aging processes of VOC oxidation products have large impacts on the parametrized product yields and SOA formation. We derived sets of semivolatile product yields from isoprene oxidation under different NO levels. However, we stress that these product yields must be used in conjunction with the corresponding multigenerational aging schemes in chemical transport models. As more mechanistic insights regarding SOA formation from VOC oxidation emerge, our box ...
Bookmarks Related papers MentionsView impact
Environmental science & technology, Jan 15, 2017
Low bulk diffusivity inside viscous semisolid atmospheric secondary organic aerosol (SOA) can pro... more Low bulk diffusivity inside viscous semisolid atmospheric secondary organic aerosol (SOA) can prolong equilibration timescale, but its broader impacts on aerosol growth and size distribution dynamics are poorly understood. Here we present quantitative insights into the effects of bulk diffusivity on the growth and evaporation kinetics of SOA formed under dry conditions from photooxidation of isoprene in the presence of a bimodal aerosol consisting of Aitken (ammonium sulfate) and accumulation (isoprene or -pinene SOA) mode particles. Aerosol composition measurements and evaporation kinetics indicate that isoprene SOA is composed of several semivolatile organic compounds (SVOCs), with some reversibly reacting to form oligomers. Model analysis shows that liquid-like bulk diffusivities can be used to fit the observed evaporation kinetics of accumulation mode particles, but fail to explain the growth kinetics of bimodal aerosol by significantly under-predicting the evolution of the Ait...
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Aerosol Science and Technology, 2016
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Proceedings of the National Academy of Sciences of the United States of America, Feb 7, 2017
Polycyclic aromatic hydrocarbons (PAHs) have toxic impacts on humans and ecosystems. One of the m... more Polycyclic aromatic hydrocarbons (PAHs) have toxic impacts on humans and ecosystems. One of the most carcinogenic PAHs, benzo(a)pyrene (BaP), is efficiently bound to and transported with atmospheric particles. Laboratory measurements show that particle-bound BaP degrades in a few hours by heterogeneous reaction with ozone, yet field observations indicate BaP persists much longer in the atmosphere, and some previous chemical transport modeling studies have ignored heterogeneous oxidation of BaP to bring model predictions into better agreement with field observations. We attribute this unexplained discrepancy to the shielding of BaP from oxidation by coatings of viscous organic aerosol (OA). Accounting for this OA viscosity-dependent shielding, which varies with temperature and humidity, in a global climate/chemistry model brings model predictions into much better agreement with BaP measurements, and demonstrates stronger long-range transport, greater deposition fluxes, and substantia...
Bookmarks Related papers MentionsView impact
Environmental science & technology, Jun 13, 2016
Multiphase chemistry of isomeric isoprene epoxydiols (IEPOX) has been shown to be the dominant so... more Multiphase chemistry of isomeric isoprene epoxydiols (IEPOX) has been shown to be the dominant source of isoprene-derived secondary organic aerosol (SOA). Recent studies have reported particles composed of ammonium bisulfate (ABS) mixed with model organics exhibit slower rates of IEPOX uptake. In the present study, we investigate the effect of atmospherically-relevant organic coatings of α-pinene (AP) SOA on the reactive uptake of trans-β-IEPOX onto ABS particles under different conditions and coating thicknesses. Single particle mass spectrometry was used to characterize in real-time particle size, shape, density, and quantitative composition before and after reaction with IEPOX. We find that IEPOX uptake by pure sulfate particles is a volume-controlled process, which results in particles with uniform concentration of IEPOX-derived SOA across a wide range of sizes. Aerosol acidity was shown to enhance IEPOX-derived SOA formation, consistent with recent studies. The presence of wate...
Bookmarks Related papers MentionsView impact
Atmospheric Chemistry and Physics Discussions, 2016
Measurements of the optical properties (absorption, scattering and extinction) of…
Bookmarks Related papers MentionsView impact
New gasoline engine technologies such as Spark Ignition Direct Injection (SIDI), Gasoline Direct ... more New gasoline engine technologies such as Spark Ignition Direct Injection (SIDI), Gasoline Direct Injection Compression Ignition (GDICI), and Reaction Controlled Compression Ignition (RCCI) offer the possibility of dramatically increasing the fuel efficiency of future vehicles. One drawback to these advanced engines is that they have the potential to produce higher levels of exhaust particulates than current Port Fuel Injection (PFI) engines. Regulation of engine particulate emissions in Europe is moving from mass-based standards toward number-based standards. Due to growing health concerns surrounding nano-aerosols, it is likely that similar standards will eventually be applied in the United States. This would place more emphasis on the reliable removal of smaller particles, which make up the vast majority of the particulates generated on a number basis. While Diesel Particulate Filters (DPF) have become standard, different filter systems would likely be required for advanced gasoline vehicles, due to factors such as differing particulate properties and higher exhaust temperatures. High exhaust temperatures can limit the accumulation of a soot cake, which performs most of the actual filtration in a typical DPF system.
Bookmarks Related papers MentionsView impact
ABSTRACT
Bookmarks Related papers MentionsView impact
Atmospheric Chemistry and Physics, 2014
We have developed the novel Aerosol Dynamics, gas- and particle-phase chemistry model for laborat... more We have developed the novel Aerosol Dynamics, gas- and particle-phase chemistry model for laboratory CHAMber studies (ADCHAM). The model combines the detailed gas-phase Master Chemical Mechanism version 3.2 (MCMv3.2), an aerosol dynamics and particle-phase chemistry module (which considers acid-catalysed oligomerization, heterogeneous oxidation reactions in the particle phase and non-ideal interactions between organic compounds, water and inorganic ions) and a kinetic multilayer module for diffusion-limited transport of compounds between the gas phase, particle surface and particle bulk phase. In this article we describe and use ADCHAM to study (1) the evaporation of liquid dioctyl phthalate (DOP) particles, (2) the slow and almost particle-size-independent evaporation of α-pinene ozonolysis secondary organic aerosol (SOA) particles, (3) the mass-transfer-limited uptake of ammonia (NH<sub>3</sub>) and formation of organic salts between ammonium (NH<sub>4</sub>...
Bookmarks Related papers MentionsView impact
A review of water uptake measurements conducted over the past 25 years using the Humidified Tande... more A review of water uptake measurements conducted over the past 25 years using the Humidified Tandem Differential Mobility Analyzer (HTDMA) technique reveals that ambient Aitken and accumulation mode particles typically grow substantially less at a given relative humidity compared to pure ammonium sulfate. Multiple hygroscopic modes at a single particle size are routinely observed, revealing that ambient particles are externally mixed with respect to their chemical composition. The observed growth of the multiple hygroscopic modes is typically less than that for particles composed of purely soluble salts, indicating that the externally mixed populations are themselves internally mixed with more and less-water soluble species. Therefore, the HTDMA is a powerful tool for quantitative measurements of size-dependent hygroscopic growth factors and for qualitative observations of the complex chemical composition responsible for the observed growth. The strengths and limitations of the HTDMA...
Bookmarks Related papers MentionsView impact
The Journal of Physical Chemistry C, 2014
Aerosol particles are ubiquitous in the atmosphere and have been shown to impact the Earth’s clim... more Aerosol particles are ubiquitous in the atmosphere and have been shown to impact the Earth’s climate, reduce visibility, and adversely affect human health. Modeling the evolution of aerosol systems requires an understanding of the species and mechanisms involved in particle growth, including the complex interactions between particle- and gas-phase species. Here we report studies of displacement of amines (methylamine, dimethylamine, or trimethylamine) in methanesulfonate salt particles by exposure to a different gas-phase amine, using a single particle mass spectrometer, SPLAT II. The variation of the displacement with the nature of the amine suggests that behavior is dependent on water in or on the particles. Small clusters of methanesulfonic acid with amines are used as a model in quantum chemical calculations to identify key structural elements that are expected to influence water uptake, and hence the efficiency of displacement by gas-phase molecules in the aminium salts. Such molecular-level understa...
Bookmarks Related papers MentionsView impact
The three major atmospheric oxidants involved in SOA formation from biogenic volatile organic com... more The three major atmospheric oxidants involved in SOA formation from biogenic volatile organic compounds are O3, OH and nitrate radical (NO3). While O3 and OH-initiated oxidation occur during the day, NO3 radical-initiated oxidation is recognized to be a major contributor to the night-time chemistry of volatile organic compounds in the troposphere. Specifically, the reaction of biogenic hydrocarbons with NO3 is
Bookmarks Related papers MentionsView impact
A unique, high-volume, low-flow, stainless steel aerosol flow system for the study of the formati... more A unique, high-volume, low-flow, stainless steel aerosol flow system for the study of the formation and reactions of aerosols relevant to the troposphere has been constructed, modeled and experimentally tested. The total flow tube length is 7.3 m which includes a 1.2 m section used for mixing. The flow tube is equipped with ultraviolet lamps for photolysis. The diameter of
Bookmarks Related papers MentionsView impact
SAE International Journal of Fuels and Lubricants, 2011
More stringent emissions regulations are continually being proposed to mitigate adverse human hea... more More stringent emissions regulations are continually being proposed to mitigate adverse human health and environmental impacts of internal combustion engines. With that in mind, it has been proposed that vehicular particulate matter (PM) emissions should be regulated based on particle number in addition to particle mass. One aspect of this project is to study different sample handling methods for number based aerosol measurements, specifically, two different methods for removing volatile organic compounds (VOCs). One method is a thermodenuder (TD) and the other is an evaporative chamber/diluter (EvCh). These sample handling methods have been implemented in an engine test cell with a spark ignited direct injection (SIDI) engine. The engine was designed for stoichiometric, homogeneous combustion. SIDI is of particular interest for improved fuel efficiency compared to other SI engines, however, the efficiency benefit comes with greater PM emissions and may therefore be subject to the proposed number based PM regulation. Another aspect of this project is to characterize PM from this engine in terms of particle number and composition.
Bookmarks Related papers MentionsView impact
SAE Technical Paper Series, 2011
Bookmarks Related papers MentionsView impact