Aerosol liquid water driven by anthropogenic nitrate: implications for lifetimes of water-soluble organic gases and potential for secondary organic aerosol formation.

Aerosol liquid water (ALW) influences aerosol radiative properties and the partitioning of gas-phase water-soluble organic compounds (WSOCg) to the condensed phase. A recent modeling study drew attention to the anthropogenic nature of ALW in the southeastern United States, where predicted ALW is driven by regional sulfate. Herein, we demonstrate that ALW in the Po Valley, Italy, is also anthropogenic but is driven by locally formed nitrate, illustrating regional differences in the aerosol components responsible for ALW. We present field evidence for the influence of controllable ALW on the lifetimes and atmospheric budgets of reactive organic gases and note the role of ALW in the formation of secondary organic aerosol (SOA). Nitrate is expected to increase in importance due to increased emissions of nitrate precursors, as well as policies aimed at reducing sulfur emissions. We argue that the impacts of increased particulate nitrate in future climate and air quality scenarios may be under predicted because they do not account for the increased potential for SOA formation in nitrate-derived ALW, nor do they account for the impacts of this ALW on reactive gas budgets and gas-phase photochemistry.

[1]  B. Turpin,et al.  Key parameters controlling OH‐initiated formation of secondary organic aerosol in the aqueous phase (aqSOA) , 2014 .

[2]  B. Turpin,et al.  Ammonium addition (and aerosol pH) has a dramatic impact on the volatility and yield of glyoxal secondary organic aerosol. , 2014, Environmental science & technology.

[3]  J. Seinfeld,et al.  Organic aerosol formation from the reactive uptake of isoprene epoxydiols (IEPOX) onto non-acidified inorganic seeds , 2013 .

[4]  B. Turpin,et al.  Particle partitioning potential of organic compounds is highest in the Eastern US and driven by anthropogenic water , 2013 .

[5]  B. Turpin,et al.  Chemical insights, explicit chemistry, and yields of secondary organic aerosol from OH radical oxidation of methylglyoxal and glyoxal in the aqueous phase , 2013 .

[6]  A. Sorooshian,et al.  Evidence of aqueous secondary organic aerosol formation from biogenic emissions in the North American Sonoran Desert , 2013, Geophysical research letters.

[7]  J. Seinfeld,et al.  Reactive uptake and photo-Fenton oxidation of glycolaldehyde in aerosol liquid water. , 2013, Environmental science & technology.

[8]  R. Volkamer,et al.  Effective Henry's law partitioning and the salting constant of glyoxal in aerosols containing sulfate. , 2013, Environmental science & technology.

[9]  S. Madronich,et al.  Secondary organic aerosol formation from semi‐ and intermediate‐volatility organic compounds and glyoxal: Relevance of O/C as a tracer for aqueous multiphase chemistry , 2013 .

[10]  P. Herckes,et al.  Dissolved organic carbon (DOC) and select aldehydes in cloud and fog water: the role of the aqueous phase in impacting trace gas budgets , 2012 .

[11]  R. Cohen,et al.  On the observed response of ozone to NO x and VOC reactivity reductions in San Joaquin Valley California 1995–present , 2012 .

[12]  D. Shindell,et al.  Spatially refined aerosol direct radiative forcing efficiencies. , 2012, Environmental science & technology.

[13]  M. Kleeman,et al.  Quantifying population exposure to airborne particulate matter during extreme events in California due to climate change , 2012 .

[14]  P. DeCarlo,et al.  Aqueous phase processing of secondary organic aerosol from isoprene photooxidation , 2012 .

[15]  P. Renard,et al.  Oligomer and SOA formation through aqueous phase photooxidation of methacrolein and methyl vinyl ketone , 2012 .

[16]  B. Turpin,et al.  Secondary organic aerosol formation in cloud droplets and aqueous particles (aqSOA): a review of laboratory, field and model studies , 2011 .

[17]  O. Boucher,et al.  Aerosol forcing in the Climate Model Intercomparison Project (CMIP5) simulations by HadGEM2‐ES and the role of ammonium nitrate , 2011 .

[18]  Y. Rudich,et al.  The optical, physical and chemical properties of the products of glyoxal uptake on ammonium sulfate seed aerosols , 2011 .

[19]  A. M. Booth,et al.  New and extended parameterization of the thermodynamic model AIOMFAC: calculation of activity coeffi , 2011 .

[20]  F. Keutsch,et al.  Photochemical modeling of glyoxal at a rural site: observations and analysis from BEARPEX 2007 , 2011 .

[21]  J. Seinfeld,et al.  Analysis of photochemical and dark glyoxal uptake: Implications for SOA formation , 2011 .

[22]  F. Keutsch,et al.  Glyoxal in aqueous ammonium sulfate solutions: products, kinetics and hydration effects. , 2011, Environmental science & technology.

[23]  G. Schmidt,et al.  Coupled Aerosol-Chemistry-Climate Twentieth-Century Transient Model Investigation: Trends in Short-Lived Species and Climate Responses , 2011 .

[24]  B. Turpin,et al.  SOA from methylglyoxal in clouds and wet aerosols: Measurement and prediction of key products , 2010 .

[25]  B. Turpin,et al.  Aqueous chemistry and its role in secondary organic aerosol (SOA) formation , 2010 .

[26]  John H. Seinfeld,et al.  Constraining the contribution of organic acids and AMS m/z 44 to the organic aerosol budget: On the importance of meteorology, aerosol hygroscopicity, and region , 2010 .

[27]  A. Ebel,et al.  Temperature Dependent Thermodynamic Model of the System H+-NH4+-Na+-SO42--NO3--Cl--H2O , 2010 .

[28]  R. Volkamer,et al.  Glyoxal processing by aerosol multiphase chemistry: towards a kinetic modeling framework of secondary organic aerosol formation in aqueous particles , 2010 .

[29]  M. Esselborn,et al.  Enhancement of the aerosol direct radiative effect by semi-volatile aerosol components: airborne measurements in North-Western Europe , 2010 .

[30]  B. Turpin,et al.  Organosulfates from glycolaldehyde in aqueous aerosols and clouds: Laboratory studies , 2010 .

[31]  N. Sareen,et al.  Secondary organic material formed by methylglyoxal in aqueous aerosol mimics , 2010 .

[32]  D. R. Worsnop,et al.  Evolution of Organic Aerosols in the Atmosphere , 2009, Science.

[33]  B. Turpin,et al.  Effects of Precursor Concentration and Acidic Sulfate in Aqueous Glyoxal−OH Radical Oxidation and Implications for Secondary Organic Aerosol , 2009, Environmental science & technology.

[34]  Armistead G. Russell,et al.  Gas/particle partitioning of water-soluble organic aerosol in Atlanta , 2009 .

[35]  J. Jimenez,et al.  Atmospheric condensed‐phase reactions of glyoxal with methylamine , 2009 .

[36]  N. Sareen,et al.  Light-absorbing secondary organic material formed by glyoxal in aqueous aerosol mimics , 2009 .

[37]  A. Córdova,et al.  Products and kinetics of the liquid-phase reaction of glyoxal catalyzed by ammonium ions (NH4(+)). , 2009, The journal of physical chemistry. A.

[38]  John H. Seinfeld,et al.  the Creative Commons Attribution 3.0 License. Atmospheric Chemistry , 2008 .

[39]  Rodney J. Weber,et al.  Enhanced secondary organic aerosol formation due to water uptake by fine particles , 2008 .

[40]  Beiping Luo,et al.  A thermodynamic model of mixed organic-inorganic aerosols to predict activity coefficients , 2008 .

[41]  Rainer Volkamer,et al.  Secondary Organic Aerosol Formation from Acetylene (C 2 H 2 ): seed effect on SOA yields due to organic photochemistry in the aerosol aqueous phase , 2008 .

[42]  Louisa Emmons,et al.  © Author(s) 2008. This work is distributed under the Creative Commons Attribution 3.0 License. Atmospheric Chemistry and Physics Fast airborne aerosol size and chemistry measurements above , 2008 .

[43]  F. Keutsch,et al.  Laser-induced phosphorescence for the in situ detection of glyoxal at part per trillion mixing ratios. , 2008, Analytical chemistry.

[44]  M. Petters,et al.  Single-parameter estimates of aerosol water content , 2008 .

[45]  F. Giorgi,et al.  Increased aridity in the Mediterranean region under greenhouse gas forcing estimated from high resolution simulations with a regional climate model , 2008 .

[46]  A. L. Corrigan,et al.  Uptake of glyoxal by organic and Inorganic aerosol. , 2008, Environmental science & technology.

[47]  A. Córdova,et al.  A kinetic and mechanistic study of the amino acid catalyzed aldol condensation of acetaldehyde in aqueous and salt solutions. , 2008, The journal of physical chemistry. A.

[48]  John P. Burrows,et al.  Global budgets of atmospheric glyoxal and methylglyoxal, and implications for formation of secondary organic aerosols , 2007 .

[49]  Annmarie G. Carlton,et al.  Atmospheric oxalic acid and SOA production from glyoxal: Results of aqueous photooxidation experiments , 2007 .

[50]  David G. Streets,et al.  Nitrate aerosols today and in 2030: a global simulation including aerosols and tropospheric ozone , 2007 .

[51]  D. Salcedo,et al.  A missing sink for gas‐phase glyoxal in Mexico City: Formation of secondary organic aerosol , 2007 .

[52]  P. Formenti,et al.  Chemical composition of summertime aerosol in the Po Valley (Italy), northern Adriatic and Black Sea , 2007 .

[53]  J. Haywood,et al.  In situ and remote‐sensing measurements of the mean microphysical and optical properties of industrial pollution aerosol during ADRIEX , 2007 .

[54]  John H. Seinfeld,et al.  Secondary aerosol formation from atmospheric reactions of aliphatic amines , 2007 .

[55]  Armin Sorooshian,et al.  Evidence for organosulfates in secondary organic aerosol. , 2007, Environmental science & technology.

[56]  M. Petters,et al.  A single parameter representation of hygroscopic growth and cloud condensation nucleus activity , 2006 .

[57]  John H. Seinfeld,et al.  Modeling and Characterization of a Particle-into-Liquid Sampler (PILS) , 2006 .

[58]  John H. Seinfeld,et al.  Role of Climate Change in Global Predictions of Future Tropospheric Ozone and Aerosols , 2006 .

[59]  M. Guzman,et al.  Photoinduced oligomerization of aqueous pyruvic acid. , 2006, The journal of physical chemistry. A.

[60]  John H. Seinfeld,et al.  Chamber studies of secondary organic aerosol growth by reactive uptake of simple carbonyl compounds , 2005 .

[61]  Earl L. Bailey,et al.  Secondary organic aerosol formation by glyoxal hydration and oligomer formation: humidity effects and equilibrium shifts during analysis. , 2005, Environmental science & technology.

[62]  Robert McLaren,et al.  Reactive uptake of glyoxal by particulate matter , 2005 .

[63]  Annmarie G Carlton,et al.  Isoprene forms secondary organic aerosol through cloud processing: model simulations. , 2005, Environmental science & technology.

[64]  M. Facchini,et al.  Cloud condensation nucleus production from nucleation events at a highly polluted region , 2005 .

[65]  Robert McLaren,et al.  Heterogeneous reactions of glyoxal on particulate matter: identification of acetals and sulfate esters. , 2005, Environmental science & technology.

[66]  John H. Seinfeld,et al.  Global radiative forcing of coupled tropospheric ozone and aerosols in a unified general circulation model , 2004 .

[67]  Sonia M. Kreidenweis,et al.  A modeling study of aqueous production of dicarboxylic acids: 1. Chemical pathways and speciated organic mass production , 2004 .

[68]  Sebnem Andreani-Aksoyoglu,et al.  Modeling of formation and distribution of secondary aerosols in the Milan area (Italy) , 2004 .

[69]  A. Sullivan,et al.  Variability in ammonium nitrate formation and nitric acid depletion with altitude and location over California , 2003 .

[70]  Amy P. Sullivan,et al.  Refinements to the particle-into-liquid sampler (PILS) for ground and airborne measurements of water soluble aerosol composition , 2003 .

[71]  R. Kamens,et al.  Heterogeneous Atmospheric Aerosol Production by Acid-Catalyzed Particle-Phase Reactions , 2002, Science.

[72]  A. Wexler,et al.  Atmospheric aerosol models for systems including the ions H+, NH4+, Na+, SO42−, NO3−, Cl−, Br−, and H2O , 2002 .

[73]  M. Jacobson.  Global direct radiative forcing due to multicomponent anthropogenic and natural aerosols , 2001 .

[74]  J. Seinfeld,et al.  General circulation model assessment of direct radiative forcing by the sulfate-nitrate-ammonium-water inorganic aerosol system , 2001 .

[75]  Rodney J. Weber,et al.  A Particle-into-Liquid Collector for Rapid Measurement of Aerosol Bulk Chemical Composition , 2001 .

[76]  Barbara J. Turpin,et al.  Secondary organic aerosol formation in cloud and fog droplets: a literature evaluation of plausibility , 2000 .

[77]  I. Tang.  Chemical and size effects of hygroscopic aerosols on light scattering coefficients , 1996 .

[78]  T. Vesala,et al.  Changes in cloud properties due to NOx emissions , 1995 .

[79]  M. Mozurkewich,et al.  The dissociation constant of ammonium nitrate and its dependence on temperature, relative humidity and particle size , 1993 .

[80]  John H. Seinfeld,et al.  Relative humidity and temperature dependence of the ammonium nitrate dissociation constant , 1982 .

[81]  F. Tampieri,et al.  Summer daily circulation in the Po Valley, Italy , 1981 .