P. K. Quinn

National Oceanic and Atmospheric Administration, Silver Spring, Maryland, United States

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Publications (208)690.83 Total impact

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    ABSTRACT: The sources and composition of atmospheric marine aerosol particles (aMA) have been investigated with a range of physical and chemical measurements from open-ocean research cruises. This study uses the characteristic functional group composition (from Fourier transform infrared, or FTIR, spectroscopy) of aMA from five ocean regions to show that: (i) The organic functional group composition of aMA that can be identified as mainly atmospheric primary marine (ocean-derived) aerosol particles (aPMA) is 65 ± 12% hydroxyl, 21 ± 9% alkane, 6 ± 6% amine, and 7 ± 8% carboxylic acid functional groups. Contributions from photochemical reactions add carboxylic acid groups (15%-25%), shipping effluent in seawater and ship emissions add additional alkane groups (up to 70%), and coastal or continental emissions mix in alkane and carboxylic acid groups. (ii) The organic composition of aPMA is nearly identical to model generated primary marine aerosol particles from bubbled seawater (gPMA, which has 55 ± 14% hydroxyl, 32 ± 14% alkane, and 13 ± 3% amine functional groups), indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. (iii) While the seawater organic functional group composition was nearly invariant across all three ocean regions studied and the ratio of organic carbon to sodium (OC/Na+) in the gPMA remained nearly constant over a broad range of chlorophyll-a concentrations, the gPMA alkane group fraction appeared to increase with chlorophyll-a concentrations (r =0.66). gPMA from productive seawater had a larger fraction of alkane functional groups (42 ± 9%) compared to gPMA from non-productive seawater (22 ± 10%), perhaps due to the presence of surfactants in productive seawater that stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components. gPMA has a hydroxyl group absorption peak location characteristic of monosaccharides and disaccharides, where the seawater OM hydroxyl group peak location is closer to that of polysaccharides. This may result from the larger saccharides preferentially remaining in the seawater during gPMA and aPMA production.
    Journal of Geophysical Research: Atmospheres. 10/2014;
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    ABSTRACT: We present a sensitive, compact detector that measures total reactive nitrogen (NOy), as well as NO2, NO, and O3. In all channels, NO2 is directly detected by laser diode based cavity ring-down spectroscopy (CRDS) at 405 nm. Ambient O3 is converted to NO2 in excess NO for the O3 measurement channel. Likewise, ambient NO is converted to NO2 in excess O3. Ambient NOy is thermally dissociated at ∼700° to form NO2 or NO in a heated quartz inlet. Any NO present in ambient air or formed from thermal dissociation of other reactive nitrogen compounds is converted to NO2 in excess O3 after the thermal converter. We measured thermal dissociation profiles for six of the major NOy components, and compared ambient measurements with other instruments during field campaigns in Utah and Alabama. Alabama measurements were made in a rural location with high biogenic emissions, and Utah measurements were made in the wintertime in unusual conditions that form high ozone from emissions related to oil and gas production. The NOy comparison in Alabama, to an accepted standard measurement method (a molybdenum catalytic converter/chemiluminescence instrument), agreed to within 12%, which we define as an upper limit to the accuracy of the NOy channel. The 1σ precision is <30 pptv at 1 second and <4 pptv at 1 minute time resolution for all measurement channels. The accuracy is 3% for the NO2 and O3 channels, and 5% for the NO channel. The precision and accuracy of this instrument make it a versatile alternative to standard chemiluminescence-based NOy instruments.
    Environmental Science and Technology 07/2014; · 5.48 Impact Factor
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    ABSTRACT: Quinn, P.K., A. Stohl, A. Baklanov, M.G. Flanner, A. Herber, K.Kupiainen, K.S. Law, J. Schmale, S. Sharma, V. Vestreng, and K. von Salzen, The Arctic, Radiative forcing by black carbon in the Arctic in “State of the Climate in 2013”, Bull. Amer. Meteor, Soc., 95 (7) S124 – 125, 2014.
    Bulletin of the American Meteorological Society 07/2014; 95(7):S124-125. · 11.57 Impact Factor
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    ABSTRACT: We investigate hygroscopic growth of marine aerosols from three research cruises: TexAQS-GoMACCS 2006, ICEALOT 2008 and CalNex 2010. Particle hygroscopic growth was characterized by measuring the effect of water uptake under sub-saturated conditions on the aerosol light extinction at 532 nm. Mie theory calculations were utilized to convert the observed optical growth factors (fext(RH)) into physical growth factors (GF) at 85% RH. GF is found to be a more robust measure of aerosol hygroscopic growth than fext(RH), which can be biased by changes in aerosol dry size. Consistent with previous observations, the overall GF(85%) for submicron aerosol depended on the fraction of organics. The submicron GFOM(85%) specifically was found to range from 1.0-1.3 for all three campaigns. A robust positive linear dependence of the overall supermicron GF(85%) on the mass fraction of sea salt was observed. During TexAQS, two types of dust particles with distinct hygroscopic properties were identified in the supermicron mode; one that originated from the Sahara desert was moderately hygroscopic (GFdust(85%) = ~1.4) and the other from continental sources was nearly hydrophobic. The GF(85%) of supermicron organics was estimated through hygroscopicity closure calculations. Supermicron organics that originated from marine sources were found to be substantially more hygroscopic than those from continental sources, with the latter having a GF(85%) similar to that of the submicron organics. This study demonstrates the potential of using aerosol optical measurements to retrieve hygroscopic growth factor and underlines the importance and need for future investigations on the hygroscopic properties of marine supermicron aerosols.
    Journal of Geophysical Research: Atmospheres. 06/2014;
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    ABSTRACT: Aerosol variations and trends over different land and ocean regions from 1980 to 2009 are analyzed with the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model and observations from multiple satellite sensors and available ground-based networks. Excluding time periods with large volcanic influence, aerosol optical depth (AOD) and surface concentration over polluted land regions generally vary with anthropogenic emissions, but the magnitude of this association can be dampened by the presence of natural aerosols, especially dust. Over the 30-year period in this study, the largest reduction in aerosol levels occurs over Europe, where AOD has decreased by 40–60% on average and surface sulfate concentrations have declined by a factor of up to 3–4. In contrast, East Asia and South Asia show AOD increases, but the relatively high level of dust aerosols in Asia reduces the correlation between AOD and pollutant emission trends. Over major dust source regions, model analysis indicates that the change of dust emissions over the Sahara and Sahel has been predominantly driven by the change of near-surface wind speed, but over Central Asia it has been largely influenced by the change of the surface wetness. The decreasing dust trend in the North African dust outflow region of the tropical North Atlantic and the receptor sites of Barbados and Miami is closely associated with an increase of the sea surface temperature in the North Atlantic. This temperature increase may drive the decrease of the wind velocity over North Africa, which reduces the dust emission, and the increase of precipitation over the tropical North Atlantic, which enhances dust removal during transport. Despite significant trends over some major continental source regions, the model-calculated global annual average AOD shows little change over land and ocean in the past three decades, because opposite trends in different land regions cancel each other out in the global average, and changes over large open oceans are negligible. This highlights the necessity for regional-scale assessment of aerosols and their climate impacts, as global-scale average values can obscure important regional changes.
    ATMOSPHERIC CHEMISTRY AND PHYSICS 05/2014; · 5.30 Impact Factor
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    ABSTRACT: Ship-based measurements of gas-phase hydrochloric acid (HCl), particulate chloride (pCl-), and reactive nitrogen oxides (NOy) were made in the polluted marine boundary layer along the California coastline during spring 2010. These observations are used to assess both the rate of Cl atom production from HCl and the role of direct HCl emissions and subsequent partitioning as a source for pCl-. Observations of HCl made in coastal Southern California are broadly correlated with NOz (NOz ≡ NOy – NOx), peaking at 11 AM. The observed median HCl mixing ratio in Southern California is 1.3 ppb (interquartile range: 0.53 − 2.7 ppb), as compared to 0.19 ppb (interquartile range: 0.10 − 0.38 ppb) measured along the Sacramento River between San Francisco and Sacramento. Concurrent measurements of aerosol ion chemistry indicate that aerosol particles sampled in Northern California are heavily depleted in Cl-, corresponding to a mean pCl- deficit of 0.05 ± 0.03 (1σ) ppb for sub-10 μm aerosol particles. In comparison, aerosols measured in Southern California indicate that over 25% of particles showed an addition of Cl- to the particle population. Observations presented here suggest that primary sources of HCl, or gas-phase chlorine precursors to HCl, are likely underestimated in the California ARB emissions inventory. These results highlight the need for future field observations designed to better constrain direct reactive halogen emissions.
    Journal of Geophysical Research: Atmospheres. 05/2014;
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    ABSTRACT: Physical and biogeochemical processes in seawater controlling primary marine aerosol (PMA) production and composition are poorly understood and associated with large uncertainties in estimated fluxes into the atmosphere. PMA production was investigated in the biologically-productive NE Pacific Ocean and in biologically-productive and oligotrophic regions of the NW Atlantic Ocean. Physicochemical properties of model PMA, produced by aeration of fresh seawater under controlled conditions, were quantified. Diel variability in model PMA mass and number fluxes was observed in biologically productive waters, increasing following sunrise and decreasing to pre-dawn levels overnight. Such variability was not seen in oligotrophic waters. Surfactant scavenging by aeration in the aerosol generator without replenishing the seawater in the reservoir during daytime reduced model PMA production in productive waters to nighttime levels but had no influence on production from oligotrophic waters. Results suggest bubble-plume interactions with sunlight-mediated biogenic surfactants in productive seawater significantly enhanced model PMA production.
    Geophysical Research Letters. 03/2014; 41(7).
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    ABSTRACT: The Spectral Deconvolution Algorithm (SDA) and SDA+ (extended SDA) methodologies can be employed to separate the fine and coarse mode extinction coefficients from measured total aerosol extinction coefficients, but their common use is currently limited to AERONET Aerosol Optical Depth (AOD). Here we provide the verification of the SDA+ methodology on a non-AERONET aerosol product, by applying it to fine and coarse mode nephelometer and Particle Soot Absorption Photometer (PSAP) data sets collected in the marine boundary layer. Using datasets collected on research vessels by NOAA PMEL, we demonstrate that with accurate input, SDA+ is able to predict the fine and coarse mode scattering and extinction coefficient partition in global data sets representing a range of aerosol regimes. However, in low-extinction regimes commonly found in the clean marine boundary layer, SDA+ output accuracy is sensitive to instrumental calibration errors. This work was extended to the calculation of coarse and fine mode scattering coefficients with similar success. This effort not only verifies the application of the SDA+ method to in situ data, but by inference verifies the method as a whole for a host of applications, including AERONET. Study results open the door to much more extensive use of nephelometers and PSAPs, with the ability to calculate fine and coarse mode scattering and extinction coefficients in field campaigns that do not have the resources to explicitly measure these values.
    Atmospheric Measurement Techniques 03/2014; 7:2545-2584. · 3.21 Impact Factor
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    ABSTRACT: Breaking waves on the ocean surface generate air bubbles that scavenge organic matter from the surrounding sea water. When injected into the atmosphere, these bubbles burst, yielding sea spray aerosols enriched in organic matter, relative to the sea water. Downwind of plankton blooms, the organic carbon content of sea spray aerosol is weakly correlated with satellite-derived measurements of chlorophyll a levels, a measure of phytoplankton biomass. This correlation has been used in large-scale models to calculate the organic enrichment in sea spray aerosol. Here, we assess the relationship between the organic carbon content of sea water and freshly emitted sea spray aerosol in the presence and absence of plankton blooms in the North Atlantic Ocean and the coastal waters of California. The organic carbon content of freshly emitted sea spray aerosol was similar in all regions sampled, despite significant differences in seawater chlorophyll a levels. The proportion of freshly emitted aerosols that served as cloud condensation nuclei at a given supersaturation was also similar across sampling sites. The large reservoir of organic carbon in surface sea water remained relatively constant across the regions sampled, and independent of variations in chlorophyll a concentrations. We suggest that this reservoir is responsible for the organic carbon enrichment of freshly emitted sea spray aerosol, overwhelming any influence of local biological activity as measured by chlorophyll a levels.
    Nature Geoscience 02/2014; 7(3). · 11.67 Impact Factor
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    ABSTRACT: Black carbon (BC) mass emission factors (EFBC; g BC(kg fuel)
    Atmospheric Chemistry and Physics 01/2014; 14(4). · 4.88 Impact Factor
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    ABSTRACT: Emissions factors (EFs) for gas and sub-micron particle-phase species were measured in intercepted plumes as a function of vessel speed from an underway research vessel, the NOAA ship Miller Freeman, operating a medium-speed diesel engine on low-sulfur marine gas oil (fuel sulfur content ~0.1% by weight). The low-sulfur fuel in use conforms to the MARPOL fuel sulfur limit within emission control areas set to take effect in 2015 and to California-specific limits set to take effect in 2014. For many of the particle-phase species, EFs were determined using multiple measurement methodologies, allowing for an assessment of how well EFs from different techniques agree. The total sub-micron PM (PM1) was dominated by particulate black carbon (BC) and particulate organic matter (POM), with an average POM / BC ratio of 1.3. Consideration of the POM / BC ratios observed here with literature studies suggests that laboratory and in-stack measurement methods may overestimate primary POM EFs relative to those observed in emitted plumes. Comparison of four different methods for black carbon measurement indicates that careful attention must be paid to instrument limitations and biases when assessing EFBC. Particulate sulfate (SO42-) EFs were extremely small and the particles emitted by Miller Freeman were inefficient as cloud condensation nuclei (CCN), even at high super saturations, consistent with the use of very low-sulfur fuel and the overall small emitted particle sizes. All measurement methodologies consistently demonstrate that the measured EFs (fuel mass basis) for PM1 mass, BC and POM decreased as the ship slowed. Particle number EFs were approximately constant across the speed change, with a shift towards smaller particles being emitted at slower speeds. Emissions factors for gas-phase CO and formaldehyde (HCHO) both increased as the vessel slowed, while EFs for NOx decreased and SO2 EFs were approximately constant.
    Atmospheric Chemistry and Physics 01/2014; 14(3). · 4.88 Impact Factor
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    ABSTRACT: Copyright 2014 American Association for Aerosol Research
    Aerosol Science and Technology 01/2014; 48(3). · 3.16 Impact Factor
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    ABSTRACT: Sea-spray aerosols (SSA) are an important part of the climate system because of their effects on the global radiative budget – both directly as scatterers and absorbers of solar and terrestrial radiation, and indirectly as cloud condensation nuclei (CCN) influencing cloud formation, lifetime, and precipitation. In terms of their global mass, SSA have the largest uncertainty of all aerosols. In this study we review 21 SSA source functions from the literature, several of which are used in current climate models. In addition, we propose a~new function. Even excluding outliers, the global annual SSA mass produced spans roughly 3–70 Pg yr−1 for the different source functions, for particles with dry diameter Dp < 10 μm, with relatively little interannual variability for a given function. The FLEXPART Lagrangian particle dispersion model was run in backward mode for a large global set of observed SSA concentrations, comprised of several station networks and ship cruise measurement campaigns. FLEXPART backward calculations produce gridded emission sensitivity fields, which can subsequently be multiplied with gridded SSA production fluxes in order to obtain modeled SSA concentrations. This allowed us to efficiently and simultaneously evaluate all 21 source functions against the measurements. Another advantage of this method is that source-region information on wind speed and sea surface temperatures (SSTs) could be stored and used for improving the SSA source function parameterizations. The best source functions reproduced as much as 70% of the observed SSA concentration variability at several stations, which is comparable with "state of the art" aerosol models. The main driver of SSA production is wind, and we found that the best fit to the observation data could be obtained when the SSA production is proportional to U103.5, where U10 is the source region averaged 10 m wind speed. A strong influence of SST on SSA production, with higher temperatures leading to higher production, could be detected as well, although the underlying physical mechanisms of the SST influence remains unclear. Our new source function with wind speed and temperature dependence gives a global SSA production for particles smaller than Dp < 10 μm of 9 Pg yr−1, and is the best fit to the observed concentrations.
    Atmospheric Chemistry and Physics 01/2014; 14:1277 – 1297. · 5.51 Impact Factor
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    ABSTRACT: [1] Frost flowers are clusters of highly saline ice crystals growing on newly formed sea ice or frozen lakes. Based on observations of particles derived from frost flowers in the Arctic, we formulate an observation-based parameterization of salt aerosol source function from frost flowers. The particle flux from frost flowers in winter has the order of 106 m−2 s−1 at the wind speed of 10 m s−1, but the source flux is highly localized to new sea ice regions and strongly dependent on wind speed. We have implemented this parameterization into the regional Weather Research and Forecasting model with Chemistry initialized for two wintertime scenarios. The addition of sea salt aerosol emissions from frost flowers increases averaged sea salt aerosol mass and number concentration and subsequent cloud droplet number. This change of cloud droplet number concentration increases downward longwave cloud radiative forcing through enhanced cloud optical depth and emissivity. The magnitude of this forcing of sea salt aerosols from frost flowers on clouds and radiation, however, contributes negligibly to surface warming in Barrow, Alaska, in the wintertime scenarios studied here.
    Journal of Geophysical Research: Atmospheres. 12/2013; 118(23).
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    ABSTRACT: [1] Here we present measurements of the size-resolved concentration and isotopic composition of atmospheric nitrate (NO3−) collected during a cruise in coastal California. Significant differences in air mass origin and atmospheric chemistry were observed in the two main regions of this cruise (South and Central Coast) with corresponding differences in NO3− concentration and isotope ratios. Measurements of the 17O-excess (Δ17O) of NO3− suggest that nocturnal chemistry played an important role in terms of total NO3− production (~ 50%) in the coastal Los Angeles region (South Coast), where NO3− concentrations were elevated due to the influence of sea breeze / land breeze recirculation and Δ17O(NO3−) averaged (25.3 ± 1.6)‰. Conversely, Δ17O(NO3−) averaged (22.3 ± 1.8)‰ in the Central Coast region, suggesting that the daytime OH + NO2 reaction was responsible for 60–85% of NO3− production in the marine air sampled in this area. A strong diurnal signal was observed for both the Δ17O and δ15N of NO3−. In the case of Δ17O, this trend is interpreted quantitatively in terms of the relative proportions of daytime and nighttime production and the atmospheric lifetime of NO3−. For δ15N, which had an average value of (0.0 ± 3.2)‰, the observed diurnality suggests a combined effect of isotopic exchange between gas-phase precursors and variability in reactive nitrogen sources. These findings represent a significant advance in our understanding of the isotope dynamics of nitrate and its precursor molecules, with potentially important implications for air quality modeling.
    Journal of Geophysical Research: Atmospheres. 09/2013; 118(18).
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    ABSTRACT: [1] The chemical, physical, and optical properties of sub- and supermicrometer aerosols over the equatorial Indian Ocean were measured on board the R/V Revelle during the fall 2011 Dynamics of the Madden-Julian Oscillation field campaign. During this time, both the retreating of the Asian monsoon and two Madden-Julian Oscillation (MJO) events were observed. The R/V Revelle was on station (0.1°N and 80.5°E) to measure atmospheric and oceanic conditions between 4 October and 30 October 2011 (Leg 2) and 11 November and 4 December 2011 (Leg 3). Throughout the campaign, background marine atmospheric conditions were usually observed. As the Asian monsoon season retreated over the boreal fall and the general wind direction changed from southerly to northerly transporting, respectively, clean marine and polluted continental air masses, the average submicrometer aerosol mass nearly doubled from Leg 2 to Leg 3 and the aerosol appeared to be more influenced by continental sources. The effect of MJO-associated convection anomalies on aerosols in the remote marine boundary layer (MBL) was measured during November when a complete MJO convection wave moved over the equatorial Indian Ocean and during October when a partial MJO event was observed. MJO-associated convection strongly affected the local aerosol as increased vertical mixing introduced new particles into the MBL, rainout cleared the atmosphere of submicrometer aerosol particles, and high winds enhanced the concentration of sea salt aerosol particles in the local atmosphere. Four stages of MJO-affected aerosol population changes in the remote Indian Ocean are defined.
    Journal of Geophysical Research: Atmospheres. 06/2013;
  • Journal of Geophysical Research: Atmospheres. 06/2013; 118(11):5380-5552.
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    ABSTRACT: [1] The Research at the Nexus of Air Quality and Climate Change (CalNex) field campaign was undertaken to obtain a better understanding of the regional impacts of different pollution sources in California. As part of this study, real-time shipboard measurements were made of the size-resolved, single-particle mixing state of submicron and supermicron particles (0.2–3.0 µm aerodynamic diameter) along the California coast where major differences were noted between Southern and Northern California. In Southern California, particles containing soot made up the largest fraction of submicron particles (~38% on average and up to ~89% by number), whereas organic carbon particles comprised the largest fraction of submicron number concentrations (~29% on average and up to ~78% by number) in Northern California including the Sacramento area. The mixing state of these carbonaceous particle types varied during the cruise with sulfate being more prevalent on soot-containing particles in Southern California due to the influence of fresh shipping and port emissions in addition to contributions from marine biogenic emissions. Contributions from secondary organic aerosol species, including amines, and nitrate were more prevalent in Northern California, as well as during time periods impacted by agricultural emissions (e.g., from the inland Riverside and Central Valley regions). These regional differences and changes in the mixing state and sources of particles have implications for heterogeneous reactivity, water uptake, and cloud-nucleating abilities for aerosols in California.
    Journal of Geophysical Research: Atmospheres. 05/2013; 118(10).
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    ABSTRACT: Marine aerosol particles play an important role in the earth's radiative balance, yet the sources and composition of the organic fraction remain largely unconstrained. Recent measurements have been made in order to characterize the sources, composition, and concentration of aerosol particles in the marine boundary layer. The organic composition of submicron particles derived from multiple seawater regions have been measured using Fourier Transform Infrared (FTIR) spectroscopy. Cluster analysis of FTIR organic spectra suggest different spectral signatures based on collection location, seawater composition, and ambient conditions. Measurements including non-refractory aerosol composition from a high-resolution time of flight aerosol mass spectrometer (HR-ToF-AMS), seawater composition, and wind speed were used to interpret the cluster results, depending on the availability from each campaign. FTIR spectra of ambient particles are compared to FTIR spectra of primary marine particles generated from model ocean systems to infer the ambient particle production mechanisms and aging processes. Recent measurements used in the comparison include ambient and generated marine aerosol particles measured off the coast of California during CalNex in May and June 2010. Remote ambient marine aerosol particles were collected 100 miles off the coast of Monterey in the eastern Pacific during the EPEACE experiment in July 2011. Ambient and generated marine particles were measured in two different seawater types during WACS 2012 including colder, more productive water off the coast of the northeastern United States and warmer, oligotrophic water in the Sargasso Sea. These particles are also compared with those measured in the southeastern Pacific during VOCALS and the north Atlantic during ICEALOT.
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    ABSTRACT: Several recent observations of nitryl chloride (ClNO2) have suggested that this compound can accumulate to significant levels (several ppb) in the nocturnal boundary layer at night. Its photolytic loss the next day can be a significant source of chlorine atom radicals. The source of ClNO2 is known to be the heterogeneous reaction of N2O5 with aerosol chloride, not just confined to coastal regions but also observed thousands of kilometers inland in urban areas. During the Uintah Basin Winter Ozone Study (2012), we made measurements of ClNO2 by CIMS on a tower in a remote region of Utah where intensive natural gas extraction operations via hydraulic fracturing were occurring. Levels of ClNO2 were surprisingly high at night (up to 2 ppb) even though coastal aerosols were not present. Soils in the region were alkaline with high chloride content. To address the potential of N2O5 dry deposition as a source of ClNO2, we measured vertical profiles of ClNO2 from 1 to 12 m agl with a movable inlet. We observed negative gradients of ClNO2 and positive gradients of N2O5, which suggest that dry deposition of N2O5 and reaction with soil chloride as a source of ClNO2.

Publication Stats

7k Citations
690.83 Total Impact Points


  • 1997–2014
    • National Oceanic and Atmospheric Administration
      • • Pacific Marine Environmental Laboratory
      • • Chemical Science Division
      Silver Spring, Maryland, United States
  • 2010
    • University of California, San Diego
      • Department of Chemistry and Biochemistry
      San Diego, California, United States
  • 1987–2007
    • University of Washington Seattle
      • • Joint Institute for the Study of the Atmosphere and Ocean
      • • Department of Chemistry
      Seattle, Washington, United States
  • 2004
    • National Institute of Water and Atmospheric Research
      Wellington, Wellington, New Zealand
  • 2003
    • University of Illinois, Urbana-Champaign
      • Department of Civil and Environmental Engineering
      Urbana, Illinois, United States