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Manish Shrivastava

Bio: Manish Shrivastava is an academic researcher from Pacific Northwest National Laboratory. The author has contributed to research in topics: Aerosol & Isoprene. The author has an hindex of 22, co-authored 52 publications receiving 5048 citations. Previous affiliations of Manish Shrivastava include University of California, Riverside & Carnegie Mellon University.


Papers
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Journal ArticleDOI
02 Mar 2007-Science
TL;DR: Accounting for partitioning and photochemical processing of primary emissions creates a more regionally distributed aerosol and brings model predictions into better agreement with observations, attribute this unexplained secondary organic-aerosol production to the oxidation of low-volatility gas-phase species.
Abstract: Most primary organic-particulate emissions are semivolatile; thus, they partially evaporate with atmospheric dilution, creating substantial amounts of low-volatility gas-phase material. Laboratory experiments show that photo-oxidation of diesel emissions rapidly generates organic aerosol, greatly exceeding the contribution from known secondary organic-aerosol precursors. We attribute this unexplained secondary organic-aerosol production to the oxidation of low-volatility gas-phase species. Accounting for partitioning and photochemical processing of primary emissions creates a more regionally distributed aerosol and brings model predictions into better agreement with observations. Controlling organic particulate-matter concentrations will require substantial changes in the approaches that are currently used to measure and regulate emissions.

1,563 citations

01 Jan 2007
TL;DR: The amount of primary organic aerosol (POA) depends on the gas-particle partitioning of 1000s of individual organic compounds, expressed in terms of the volatility distribution of the emissions as discussed by the authors.
Abstract: The amount of primary organic aerosol (POA) depends on the gas-particle partitioning of 1000s of individual organic compounds. This partitioning can be expressed in terms of the volatility distribution of the emissions. A volatility distribution can be constructed from speciated emissions data by lumping species with similar saturation vapor pressures. In practice, this is not possible because less than 10% of the condensed and semivolatile mass has been identified on a compound-by-compound basis (

1,344 citations

Journal ArticleDOI
TL;DR: In this paper, a review summarizes some of the important developments during the past decade in understanding secondary organic aerosol (SOA) formation, including formation of extremely low volatility organics in the gas phase, acid-catalyzed multiphase chemistry of isoprene epoxydiols, particle-phase oligomerization, and physical properties such as volatility and viscosity.
Abstract: Anthropogenic emissions and land use changes have modified atmospheric aerosol concentrations and size distributions over time. Understanding preindustrial conditions and changes in organic aerosol due to anthropogenic activities is important because these features (1) influence estimates of aerosol radiative forcing and (2) can confound estimates of the historical response of climate to increases in greenhouse gases. Secondary organic aerosol (SOA), formed in the atmosphere by oxidation of organic gases, represents a major fraction of global submicron-sized atmospheric organic aerosol. Over the past decade, significant advances in understanding SOA properties and formation mechanisms have occurred through measurements, yet current climate models typically do not comprehensively include all important processes. This review summarizes some of the important developments during the past decade in understanding SOA formation. We highlight the importance of some processes that influence the growth of SOA particles to sizes relevant for clouds and radiative forcing, including formation of extremely low volatility organics in the gas phase, acid-catalyzed multiphase chemistry of isoprene epoxydiols, particle-phase oligomerization, and physical properties such as volatility and viscosity. Several SOA processes highlighted in this review are complex and interdependent and have nonlinear effects on the properties, formation, and evolution of SOA. Current global models neglect this complexity and nonlinearity and thus are less likely to accurately predict the climate forcing of SOA and project future climate sensitivity to greenhouse gases. Efforts are also needed to rank the most influential processes and nonlinear process-related interactions, so that these processes can be accurately represented in atmospheric chemistry-climate models.

467 citations

Journal ArticleDOI
TL;DR: In this article, the authors estimate open biomass burning representative of 1995-2000 from forests using burned area and biomass density specific for Indian ecosystems and crop waste burning as a balance between generation and known uses as fuel and fodder.
Abstract: [1] Climatological mean estimates of forest burning and crop waste burning based on broad assumptions of the amounts burned have so far been used for India in global inventories. Here we estimate open biomass burning representative of 1995–2000 from forests using burned area and biomass density specific for Indian ecosystems and crop waste burning as a balance between generation and known uses as fuel and fodder. High-resolution satellite data of active fires and land cover classification from MODIS, both on a scale of 1 km × 1 km, were used to capture the seasonal variability of forest and crop waste burning and in conjunction with field reporting. Correspondence in satellite-detected fire cycles with harvest season was used to identify types crop waste burned in different regions. The fire season in forest areas was from February to May, and that in croplands varied with geographical location, with peaks in April and October, corresponding to the two major harvest seasons. Spatial variability in amount of forest biomass burned differed from corresponding forest fire counts with biomass burned being largest in central India but fire frequency being highest in the east-northeast. Unutilized crop waste and MODIS cropland fires were predominant in the western Indo-Gangetic plain. However, the amounts of unutilized crop waste in the four regions were not strictly proportional to the fire counts. Fraction crop waste burned in fields ranged from 18 to 30% on an all-India basis and had a strong regional variation. Open burning contributes importantly (about 25%) to black carbon, organic matter, and carbon monoxide emissions, a smaller amount (9–13%) to PM2.5 (particulate mass in particles smaller than 2.5 micron diameter) and CO2 emissions, and negligibly to SO2 emissions (1%). However, it cannot explain a large “missing source” of BC or CO from India.

281 citations

Journal ArticleDOI
TL;DR: The Comprehensive Air-Quality Model with extensions dealing with particulate matter (PMCAMx) was extended to investigate the effects of partitioning and photochemical aging of primary emissions on OA concentrations in the eastern United States during July 2001 and January 2002 as discussed by the authors.
Abstract: [1] Organic aerosols (OA) are a highly dynamic system dominated by both variable gas particle partitioning and chemical evolution; however, these phenomena are poorly represented in current air quality models. The chemical transport model Comprehensive Air-Quality Model with extensions dealing with particulate matter (PMCAMx) was extended to investigate the effects of partitioning and photochemical aging of primary emissions on OA concentrations in the eastern United States during July 2001 and January 2002. In both the summer and the winter, much of the traditionally defined primary OA (POA) emissions evaporate, creating a large pool of low-volatility organic vapors. During the summertime, photochemical aging of these vapors creates substantial oxygenated OA that is regionally distributed. Little production of oxygenated OA is predicted in the winter because oxidant levels are low. OA formed from the oxidation of low-volatility vapors is most important in and around urban areas located in the northeast and midwest. In rural locations and throughout the southeast, traditional secondary OA (SOA) formed from biogenic precursors is predicted to be the dominant class of oxidized OA. PMCAMx can only reproduce the large fractional contributions of oxidized OA observed in the atmosphere if some of the POA in the model evaporates. Sensitivity analysis illustrates that the volatility distribution of the existing POA emissions and the amount of intermediate volatility compounds not accounted for in current inventories are key uncertainties. At an upper bound, better accounting for emissions of low-volatility organics has the potential to increase summertime OA concentrations in northeastern and midwestern cities by as much as 50%.

226 citations


Cited by
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[...]

08 Dec 2001-BMJ
TL;DR: There is, I think, something ethereal about i —the square root of minus one, which seems an odd beast at that time—an intruder hovering on the edge of reality.
Abstract: There is, I think, something ethereal about i —the square root of minus one. I remember first hearing about it at school. It seemed an odd beast at that time—an intruder hovering on the edge of reality. Usually familiarity dulls this sense of the bizarre, but in the case of i it was the reverse: over the years the sense of its surreal nature intensified. It seemed that it was impossible to write mathematics that described the real world in …

33,785 citations

Journal ArticleDOI
TL;DR: In this paper, the authors provided an assessment of black-carbon climate forcing that is comprehensive in its inclusion of all known and relevant processes and that is quantitative in providing best estimates and uncertainties of the main forcing terms: direct solar absorption; influence on liquid, mixed phase, and ice clouds; and deposition on snow and ice.
Abstract: Black carbon aerosol plays a unique and important role in Earth's climate system. Black carbon is a type of carbonaceous material with a unique combination of physical properties. This assessment provides an evaluation of black-carbon climate forcing that is comprehensive in its inclusion of all known and relevant processes and that is quantitative in providing best estimates and uncertainties of the main forcing terms: direct solar absorption; influence on liquid, mixed phase, and ice clouds; and deposition on snow and ice. These effects are calculated with climate models, but when possible, they are evaluated with both microphysical measurements and field observations. Predominant sources are combustion related, namely, fossil fuels for transportation, solid fuels for industrial and residential uses, and open burning of biomass. Total global emissions of black carbon using bottom-up inventory methods are 7500 Gg yr−1 in the year 2000 with an uncertainty range of 2000 to 29000. However, global atmospheric absorption attributable to black carbon is too low in many models and should be increased by a factor of almost 3. After this scaling, the best estimate for the industrial-era (1750 to 2005) direct radiative forcing of atmospheric black carbon is +0.71 W m−2 with 90% uncertainty bounds of (+0.08, +1.27) W m−2. Total direct forcing by all black carbon sources, without subtracting the preindustrial background, is estimated as +0.88 (+0.17, +1.48) W m−2. Direct radiative forcing alone does not capture important rapid adjustment mechanisms. A framework is described and used for quantifying climate forcings, including rapid adjustments. The best estimate of industrial-era climate forcing of black carbon through all forcing mechanisms, including clouds and cryosphere forcing, is +1.1 W m−2 with 90% uncertainty bounds of +0.17 to +2.1 W m−2. Thus, there is a very high probability that black carbon emissions, independent of co-emitted species, have a positive forcing and warm the climate. We estimate that black carbon, with a total climate forcing of +1.1 W m−2, is the second most important human emission in terms of its climate forcing in the present-day atmosphere; only carbon dioxide is estimated to have a greater forcing. Sources that emit black carbon also emit other short-lived species that may either cool or warm climate. Climate forcings from co-emitted species are estimated and used in the framework described herein. When the principal effects of short-lived co-emissions, including cooling agents such as sulfur dioxide, are included in net forcing, energy-related sources (fossil fuel and biofuel) have an industrial-era climate forcing of +0.22 (−0.50 to +1.08) W m−2 during the first year after emission. For a few of these sources, such as diesel engines and possibly residential biofuels, warming is strong enough that eliminating all short-lived emissions from these sources would reduce net climate forcing (i.e., produce cooling). When open burning emissions, which emit high levels of organic matter, are included in the total, the best estimate of net industrial-era climate forcing by all short-lived species from black-carbon-rich sources becomes slightly negative (−0.06 W m−2 with 90% uncertainty bounds of −1.45 to +1.29 W m−2). The uncertainties in net climate forcing from black-carbon-rich sources are substantial, largely due to lack of knowledge about cloud interactions with both black carbon and co-emitted organic carbon. In prioritizing potential black-carbon mitigation actions, non-science factors, such as technical feasibility, costs, policy design, and implementation feasibility play important roles. The major sources of black carbon are presently in different stages with regard to the feasibility for near-term mitigation. This assessment, by evaluating the large number and complexity of the associated physical and radiative processes in black-carbon climate forcing, sets a baseline from which to improve future climate forcing estimates.

4,591 citations

Journal Article
TL;DR: In this article, the authors present a document, redatto, voted and pubblicato by the Ipcc -Comitato intergovernativo sui cambiamenti climatici - illustra la sintesi delle ricerche svolte su questo tema rilevante.
Abstract: Cause, conseguenze e strategie di mitigazione Proponiamo il primo di una serie di articoli in cui affronteremo l’attuale problema dei mutamenti climatici. Presentiamo il documento redatto, votato e pubblicato dall’Ipcc - Comitato intergovernativo sui cambiamenti climatici - che illustra la sintesi delle ricerche svolte su questo tema rilevante.

4,187 citations

Journal ArticleDOI
09 Oct 2014-Nature
TL;DR: The results suggest that, in addition to mitigating primary particulate emissions, reducing the emissions of secondary aerosol precursors from fossil fuel combustion and biomass burning is likely to be important for controlling China’s PM2.5 levels and for reducing the environmental, economic and health impacts resulting from particulate pollution.
Abstract: Rapid industrialization and urbanization in developing countries has led to an increase in air pollution, along a similar trajectory to that previously experienced by the developed nations. In China, particulate pollution is a serious environmental problem that is influencing air quality, regional and global climates, and human health. In response to the extremely severe and persistent haze pollution experienced by about 800 million people during the first quarter of 2013 (refs 4, 5), the Chinese State Council announced its aim to reduce concentrations of PM2.5 (particulate matter with an aerodynamic diameter less than 2.5 micrometres) by up to 25 per cent relative to 2012 levels by 2017 (ref. 6). Such efforts however require elucidation of the factors governing the abundance and composition of PM2.5, which remain poorly constrained in China. Here we combine a comprehensive set of novel and state-of-the-art offline analytical approaches and statistical techniques to investigate the chemical nature and sources of particulate matter at urban locations in Beijing, Shanghai, Guangzhou and Xi'an during January 2013. We find that the severe haze pollution event was driven to a large extent by secondary aerosol formation, which contributed 30-77 per cent and 44-71 per cent (average for all four cities) of PM2.5 and of organic aerosol, respectively. On average, the contribution of secondary organic aerosol (SOA) and secondary inorganic aerosol (SIA) are found to be of similar importance (SOA/SIA ratios range from 0.6 to 1.4). Our results suggest that, in addition to mitigating primary particulate emissions, reducing the emissions of secondary aerosol precursors from, for example, fossil fuel combustion and biomass burning is likely to be important for controlling China's PM2.5 levels and for reducing the environmental, economic and health impacts resulting from particulate pollution.

3,372 citations

Journal ArticleDOI
TL;DR: In this article, an overview of the atmospheric degradation mechanisms for SOA precursors, gas-particle partitioning theory and analytical techniques used to determine the chemical composition of SOA is presented.
Abstract: Secondary organic aerosol (SOA) accounts for a significant fraction of ambient tropospheric aerosol and a detailed knowledge of the formation, properties and transformation of SOA is therefore required to evaluate its impact on atmospheric processes, climate and human health. The chemical and physical processes associated with SOA formation are complex and varied, and, despite considerable progress in recent years, a quantitative and predictive understanding of SOA formation does not exist and therefore represents a major research challenge in atmospheric science. This review begins with an update on the current state of knowledge on the global SOA budget and is followed by an overview of the atmospheric degradation mechanisms for SOA precursors, gas-particle partitioning theory and the analytical techniques used to determine the chemical composition of SOA. A survey of recent laboratory, field and modeling studies is also presented. The following topical and emerging issues are highlighted and discussed in detail: molecular characterization of biogenic SOA constituents, condensed phase reactions and oligomerization, the interaction of atmospheric organic components with sulfuric acid, the chemical and photochemical processing of organics in the atmospheric aqueous phase, aerosol formation from real plant emissions, interaction of atmospheric organic components with water, thermodynamics and mixtures in atmospheric models. Finally, the major challenges ahead in laboratory, field and modeling studies of SOA are discussed and recommendations for future research directions are proposed.

3,324 citations