Journal of Atmospheric Chemistry

Current research reports and chronological list of recent articles.


The international scientific Journal of Atmospheric Chemistry is devoted to the study of the chemistry of the atmosphere, with particular emphasis on the region below about 100 km. The strongly interdisciplinary nature of atmospheric chemistry means that it embraces a great variety of sciences.

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Journal of Atmospheric Chemistry - Abstracts



Mass spectrometric study of aged benzene secondary organic aerosol in the presence of dry ammonium sulfate

Abstract

Inorganic seed particles have relatively large surface area, and play an important role in the formation and aging of secondary organic aerosol (SOA). The effects of dry (NH4)2SO4 which is the most commonly found in urban atmosphere on the aged benzene SOA were qualitatively studied utilizing aerosol laser time-of-flight mass spectrometer (ALTOFMS) coupled with Fuzzy C-Means (FCM) clustering algorithm in this study. Experimental results indicated that nitrophenol, oxocarboxylic acid, epoxide products are the predominant components in the aged benzene SOA in the presence of low concentration (about 10 μg m−3) of dry (NH4)2SO4. These aged products are the same as the previously obtained aged benzene SOA without (NH4)2SO4 seed aerosol, indicating that low concentration of dry (NH4)2SO4 acts just as the nucleation or condensation center of the SOA, and do not affect the chemical composition of SOA. However, 1 H-imidazole, 1 H-imidazole-2-carbaldehyde, hydrated 1 H-imidazole-2-carbaldehyde, 2,2′-biimidazole, hydrated N-glyoxal substituted 1 H-imidazole, N-glyoxal substituted hydrated 1 H-imidazole-2- carbaldehyde, hydrated mono glyoxal substituted hydrated 1 H-imidazole-2-carboxaldehyde, mono glyoxal substituted 2,2-biimidazole and hydrated glyoxal dimer substituted imidazole which are formed from ammonium ion reaction with glyoxal are the major particulate products in the aged benzene SOA in the presence of high concentration (about 100 μg m−3) of dry (NH4)2SO4. The retention of water on the dry (NH4)2SO4 particles creates ammonium ion, which can promote the formation of high-molecular-weight (HMW) products through multiphase reactions such as hydration and polymerization of aldehydes form from OH-initiated oxidation of benzene.


Datum: 02.02.2016


Dimethyl sulfide and other biogenic volatile organic compound emissions from branching coral and reef seawater: potential sources of secondary aerosol over the Great Barrier Reef

Abstract

Volatile organic compounds (VOCs) in the headspace of bubble chambers containing branches of live coral in filtered reef seawater were analysed using gas chromatography with mass spectrometry (GC-MS). When the coral released mucus it was a source of dimethyl sulfide (DMS) and isoprene; however, these VOCs were not emitted to the chamber headspace from mucus-free coral. This finding, which suggests that coral is an intermittent source of DMS and isoprene, was supported by the observation of occasional large pulses of atmospheric DMS (DMSa) over Heron Island reef on the southern Great Barrier Reef (GBR), Australia, in the austral winter. The highest DMSa pulse (320 ppt) was three orders of magnitude less than the DMS mixing ratio (460 ppb) measured in the headspace of a dynamically purged bubble chamber containing a mucus-coated branch of Acropora aspera indicating that coral reefs can be strong point sources of DMSa. Static headspace GC-MS analysis of coral fragments identified mainly DMS and seven other minor reduced sulfur compounds including dimethyl disulfide, methyl mercaptan, and carbon disulfide, while coral reef seawater was an indicated source of methylene chloride, acetone, and methyl ethyl ketone. The VOCs emitted by coral and reef seawater are capable of producing new atmospheric particles < 15 nm diameter as observed at Heron Island reef. DMS and isoprene are known to play a role in low-level cloud formation, so aerosol precursors such as these could influence regional climate through a sea surface temperature regulation mechanism hypothesized to operate over the GBR.


Datum: 22.01.2016


Multi-species chemical data assimilation with the Danish Eulerian hemispheric model: system description and verification

Abstract

Satellite retrievals of atmospheric composition provide a wealth of data on a global scale. These complement results from atmospheric chemistry-transport models (CTMs), and can be combined using data assimilation. We present two assimilation schemes coupled to the Danish Eulerian Hemispheric Model (DEHM), a three-dimensional, off-line CTM with full photochemistry: a variant on the ensemble Kalman filter and the three-dimensional variational scheme. The aim of this paper is to describe the two schemes and present an initial assessment of their impacts on model skill. Retrievals of multiple atmospheric trace gases are assimilated, namely: NO2 tropospheric column densities, CH4 total column densities, and partial column concentrations of O3, CO and CH4; these data are retrieved from four satellite sensors. Data for each species are assimilated independently of one another, and other species are only adjusted indirectly via the model’s chemistry and dynamics. Assimilation results are compared with measurements from surface monitoring stations and other satellite retrievals, and preliminary validation results are presented.Reference simulations (without assimilation) grossly underestimate surface CO concentrations, and both assimilation schemes eliminate this large and systematic model bias. The assimilation improves the spatial correlation of modelled CO with surface observations, and improves the spatial correlation between forecasts and retrievals for CO, NO2 and O3. Results for CH4 show a loss of skill due to a mismatch in model bias between two assimilated CH4 data-sets. Finally, we discuss differences in methodology and results between this paper and a recent study on multi-species chemical data assimilation. Joint optimisation of initial conditions and emission rates offers a promising direction for improving modelled boundary-layer concentrations.


Datum: 22.12.2015


A study on the precipitation in Izmir, Turkey: chemical composition and source apportionment by receptor models

Abstract

The chemistry of rainwater was studied in three sites of a metropolitan city of Turkey to determine the spatial variation, sources affecting composition and the extent of their influence. The acidity of rainwater, Ca, Co, Cr, Zn, Ba, V and Ni showed significant spatial variations. The most of measured species were moderately to extremely enriched compared to the local soil, which is likely arisen from the anthropogenic activities. SO4 2−, K and Ca were found to be predominantly non-sea origin. Two receptor models, Positive Matrix Factorization (PMF) and Chemical Mass Balance (CMB), agreed well on the source contribution estimations of Al, K, Zn, V, Pb and Cr. The PMF and CMB resolved very similar source contribution profiles to the elemental concentrations of Ca, Zn, V, Pb, K and Na, which the majority of those resulted from mineral industries, bell casting+steel industries, fossil fuel burning, biomass burning+sea salt and sea salt, respectively. The PMF resolved the source contributions of long-transported emissions, particularly for Ba, Sr and Mn, which could not be estimated by the CMB.


Datum: 28.11.2015


A new continuous measurement method for gaseous ammonia by counter-current flow tube sampling and indophenol reaction

Abstract

Ammonia (NH3) is the most abundant alkaline gas in the atmosphere and plays a key role in atmospheric chemistry. Reliable and high-time-resolution data for gaseous ammonia are necessary to understand the sources and sinks of ammonia gas in ambient air. In the present study, a sensitive and continuous instrument for measuring gaseous ammonia was developed. Ammonia gas in ambient air was collected in an aqueous solution using a counter-current flow tube (CCFT) sampler. Then, ammonium formed in the aqueous solution was detected by the indophenol method. Based on a CCFT length of 50 cm and air flow rate of 1 L/min, the collection efficiency exceeded 98.5 % at an ammonia mixing ratio of up to 120 ppbv. The detection limit of this method was 0.062 ppbv. Interferences from several gases were investigated, and the results showed that the present method was not affected by NOx, O3, SO2, HONO, methylamine, formaldehyde, hydrogen sulfide or a mixture of these gases. The most important result was that only gaseous ammonia was detected in the present method without any interference from the particulate ammonium in ambient air. Comparisons with data based on the dry denuder method indicated that the present method showed good agreement with the denuder method.


Datum: 21.10.2015


Carbon isotopic ( 14 C and 13 C) characterization of fossil-fuel derived dissolved organic carbon in wet precipitation in Shandong Province, China

Abstract

We present results from a 1-year study of radiocarbon and stable carbon isotope measurement of dissolved organic carbon (DOC) of wet precipitation samples collected in the Shandong province of China. A total of 32 rainfall and 4 snow samples were collected from two coastal cities (Qingdao and Yantai) and one inland site (Taian) during 2014. Concentrations of DOC in the rainwater and snow samples varied widely from 28 to 616 μM. In general, rainwater originating from marine sources had relatively low DOC concentrations compared with continentally generated precipitation. Values of δ13C-DOC and Δ14C-DOC in the snow and rainwater ranged from −19.0 to −29.4 ‰ and −23 to −494 ‰, with corresponding radiocarbon ages of 125 to 5410 years before present. The dominant DOC in the wet precipitation had a relatively old 14C age (average 2841 years) and a depleted 13C value (average −24.4 ‰), indicating the mixing of contemporary organic carbon with 14C-depleted fossil fuel-derived soluble organic carbon in the atmosphere. Using a dual isotopic two-endmember model, we calculate that 7 % to 52 % of DOC in the snow and rainfall originated from fossil fuels. It is estimated that the flux of DOC in continental rainfall of China is 23 × 1012 g C yr−1 and of this, 7.1 × 1012 g C yr−1 could be fossil-fuel OC. On a global scale, the DOC flux in rainfall is estimated to be 357 Tg C yr−1, and 110 Tg C yr−1 could be fossil fuel-derived. Our study demonstrates that wet precipitation is an important removal process for old fossil fuel carbon from the atmosphere. This removal mechanism could play an important role in the carbon cycle, especially for the anthropogenically derived fraction, and it should be taken into consideration in global carbon cycle models.


Datum: 12.10.2015


Characterisation of water-soluble organic aerosols at a site on the southwest coast of India

Abstract

Aerosol samples collected over a tropical location, Thumba, southernmost West Coast of India were analyzed for the abundance of homologous dicarboxylic acids (C2 to C12), oxocarboxylic acids (ωC2 to ωC9, pyruvic acid), α-dicarbonyls (glyoxal and methylglyoxal), organic and elemental carbon. Among the measured organics, oxalic acid was found to be the most abundant species followed by succinic and/or malonic acids. As oxoacid and α-carbonyl groups, glyoxylic acid and glyoxal, respectively, were observed to be dominant. On average, dicarboxylic acids accounted almost 2.1 ± 0.7 % of the aerosol total organic carbon. Among the aerosols over Thumba, two types of formation pathways were noticed for oxalic acid. During the post-monsoon and winter periods, the photo-oxidation of biogenic and anthropogenic volatile organic compounds lead to the formation of oxalic acid through a chain reaction involving glyoxal, methylglyoxal, pyruvic and glyoxylic acids. In contrast, during the pre-monsoon, the oxidative degradation of the biogenic unsaturated fatty acids give rise to succinic acid, which can be decomposed to malonic acid and then to oxalic acid. The observed seasonal variations in acid concentrations are consistent with photochemical production and the subsequent accumulation under favourable meteorological conditions prevailing over the region.


Datum: 09.10.2015


Toxic volatile organic air pollutants across Canada: multi-year concentration trends, regional air quality modelling and source apportionment

Abstract

A Unified Regional Air-quality Modelling System, AURAMS, was expanded to predict six toxic volatile organic compounds (VOCs) within a continental domain and two nested domains covering eastern and western Canada. The model predictions were evaluated against Environment Canada’s National Air Pollution Surveillance (NAPS) data set to assess the predictive capability of the model at daily and seasonal time scales. The predictions were also evaluated with satellite-derived column total maps for formaldehyde, carbon monoxide, and nitrogen dioxide. In general, the model showed fair to good predictive skill in terms of both correlation (R) and normalized mean bias (NMB) for benzene (R = 0.53 NMB = 26 %), formaldehyde (R = 0.73, NMB = −15 %) and acetaldehyde (R = 0.55, NMB = 29 %). For the other toxics VOCs, the model showed less predictive skill in the order 1,2,4-trimethylbenzene (R = 0.50, NMB = −41 %), 1,3-butadiene (R = 0.26, NMB = 40 %) and acrolein (R = 0.052, NMB = −51 %). The goal of this study was to apply an air quality model to assess the contribution of mobile sources to ambient levels of toxic VOCs at urban locations across Canada. The mobile source contribution varied in a complex manner for each species for different regions. For benzene and 1,2,4-trimethylbenzene, the mobile source contribution was in the range 40–65 % for major Canadian cities. The model predicted considerably lower mobile source contributions for rural locations in the Canadian Prairies, where other area sources dominate, such as the petrochemical industry. Measured concentration trends in toxics are also presented from 2004 to 2010. The primary emitted toxics declined gradually (13–16 % over 6 yr) whereas the toxic aldehydes showed no trend.


Datum: 08.10.2015


Particulate morphology and elemental characteristics: variability at middle Indo-Gangetic Plain

Abstract

Airborne particulates were monitored at an urban location of middle Indo-Gangetic Plain (IGP) and subsequently analyzed for particulate diversity and mixing states. Exceptionally high particulate loadings were found both in case of coarser (PM10: 157.5 ± 102.9 μgm−3, n = 46) and finer particulates (PM2.5: 92.5 ± 49.8 μgm−3). Based on particulate morphology and elemental composition, five different clusters of particulates namely tarball, soot, sulphur-rich, aluminosilicate and mineral species were found to dominate. Soot particles (0.1–5 μm) were found to be partly coated, having voids filled by coating material without being completely engulfed. A specific type of amorphous, carbonaceous spherules was evident in wintertime fine particulates signifying emissions from biomass burning and wild fire. Traces of S, Na and Ca were found associated with carbonaceous agglomerates suggesting its metal scavenging behavior. Particle laden filters were further processed for metallic and water soluble ionic species to constitute aerosol composition. Coarser particulates were characterized with higher metallic species (9.2–17.8 %), mostly of crustal origin (Ca: 5.5 %; Fe: 1.6 %; Zn: 1.3 % and Na: 3.8 %) while PM2.5 also revealed their association with metallic components (6.0–14.9 %) having Ca (4.6 %), Fe (0.9 %) and K (0.8 %) as principle constituents. Ca, Na and NH4 + found to generate chloride and sulphate salts thus affecting particulate hygroscopicity. Elevated fractions of NO3 and K+ in PM2.5 signified contribution of biomass burning while presence of Cl with carbonaceous aerosols having traces of Si and K denoted contribution of farming and burning practices. Black carbon aerosol exhibited significant seasonal variability (6.9−21.9 μgm−3) which support larger association of carbonaceous aerosols in particle micrograph.


Datum: 05.10.2015


A nocturnal atmospheric loss of CH 2 I 2 in the remote marine boundary layer

Abstract

Ocean emissions of inorganic and organic iodine compounds drive the biogeochemical cycle of iodine and produce reactive ozone-destroying iodine radicals that influence the oxidizing capacity of the atmosphere. Di-iodomethane (CH2I2) and chloro-iodomethane (CH2ICl) are the two most important organic iodine precursors in the marine boundary layer. Ship-borne measurements made during the TORERO (Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated VOC) field campaign in the east tropical Pacific Ocean in January/February 2012 revealed strong diurnal cycles of CH2I2 and CH2ICl in air and of CH2I2 in seawater. Both compounds are known to undergo rapid photolysis during the day, but models assume no night-time atmospheric losses. Surprisingly, the diurnal cycle of CH2I2 was lower in amplitude than that of CH2ICl, despite its faster photolysis rate. We speculate that night-time loss of CH2I2 occurs due to reaction with NO3 radicals. Indirect results from a laboratory study under ambient atmospheric boundary layer conditions indicate a k CH2I2+NO3 of ≤4 × 10−13 cm3 molecule−1 s−1; a previous kinetic study carried out at ≤100 Torr found k CH2I2+NO3 of 4 × 10−13 cm3 molecule−1 s−1. Using the 1-dimensional atmospheric THAMO model driven by sea-air fluxes calculated from the seawater and air measurements (averaging 1.8 +/− 0.8 nmol m−2 d−1 for CH2I2 and 3.7 +/− 0.8 nmol m−2 d−1 for CH2ICl), we show that the model overestimates night-time CH2I2 by >60 % but reaches good agreement with the measurements when the CH2I2 + NO3 reaction is included at 2–4 × 10−13 cm3 molecule−1 s−1. We conclude that the reaction has a significant effect on CH2I2 and helps reconcile observed and modeled concentrations. We recommend further direct measurements of this reaction under atmospheric conditions, including of product branching ratios.


Datum: 05.10.2015


Analysis of bulk precipitation chemistry in Serbia for the period from 1982 to 2010

Abstract

Bulk precipitation samples collected daily through bulk collectors at eight meteorological stations in Serbia were analyzed for their chemical composition. The data covers time series, from 20 to 28 years, in the period between 1982 and 2010. The most abundant ion in the samples was sulfate. Only 0.17 % of all samples were from strong acid rains (pH < 3.5). The relatively high average pH values (5.94–6.26) of the collected precipitation indicate the neutral or alkaline nature of local rainwater. Trends in both the annual amount and the composition of precipitation were tested by the nonparametric Mann–Kendall test and Sen’s slope estimator. Significant increasing trend of precipitation was identified for almost all stations. Rebuilding activities after the bombing of Serbia in 1999 were identified as a possible anthropogenic cause of the sharp increase of some ions (Ca2+) in the first year following the bombing. The origin of air masses arriving at one particular station was examined using two-dimensional backward trajectories. Western sectors (W, SW and NW) accounted for almost half (44.3 %) of all rainy days, while eastern sectors (SE, E and NE) brought only 10.4 % of all rainy days. The distribution, per sector, of volume-weighted concentrations of sulfate, nitrate, ammonium, calcium, potassium, magnesium, chloride and sodium ions, as well as the amount of precipitation and its pH values for one station, was also analyzed. Rainwater from the SE and S sectors was the most polluted.


Datum: 02.10.2015


Ozone and secondary organic aerosol formation from Ethylene-NO x -NaCl irradiations under different relative humidity conditions

Abstract

The formation of ozone and secondary organic aerosol (SOA) from ethylene-NO x -NaCl(aerosol) irradiations was studied under various relative humidity (RH) conditions in an indoor smog chamber. In the absence of NaCl seed aerosols, SOA was hardly formed and peak O3 concentrations decreased linearly with increasing RH in ethylene irradiations. For the irradiations with NaCl seed aerosols, when RH <48 % (efflorescence relative humidity of NaCl), NaCl existed as solid phase and had little effect on peak O3 concentrations. The infrared spectra from sampled particles showed that SOA was rarely formed on solid NaCl particles. However, when NaCl was in the aqueous phase as RH ≥ 48 %, the peak O3 concentration was sharply reduced by over 20 % as compared to experiments without NaCl aerosol, and the absorption of NaNO3 in aerosols was coincidently increased with RH. Model results indicated that the heterogeneous reaction of N2O5 with aqueous NaCl aerosols was the main cause for the sharp decrease of O3. Besides, the absorptions from C-H, C = O, ONO2 and COO groups all greatly increased with RH. Our results show that SOA from ethylene-NOx irradiations was mainly formed through aqueous reactions. The yields of SOA from ethylene were measured to be 1.5 and 2.3 % at RH of 65 and 84 %, respectively.


Datum: 10.09.2015


Ozone correlations between mid-tropospheric partial columns and the near-surface at two mid-atlantic sites during the DISCOVER-AQ campaign in July 2011

Abstract

The current network of ground-based monitors for ozone (O3) is limited due to the spatial heterogeneity of O3 at the surface. Satellite measurements can provide a solution to this limitation, but the lack of sensitivity of satellites to O3 within the boundary layer causes large uncertainties in satellite retrievals at the near-surface. The vertical variability of O3 was investigated using ozonesondes collected as part of NASA’s Deriving Information on Surface Conditions from COlumn and VERtically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign during July 2011 in the Baltimore, MD/Washington D.C. metropolitan area. A subset of the ozonesonde measurements was corrected for a known bias from the electrochemical solution strength using new procedures based on laboratory and field tests. A significant correlation of O3 over the two sites with ozonesonde measurements (Edgewood and Beltsville, MD) was observed between the mid-troposphere (7–10 km) and the near-surface (1–3 km). A linear regression model based on the partial column amounts of O3 within these subregions was developed to calculate the near-surface O3 using mid-tropospheric satellite measurements from the Tropospheric Emission Spectrometer (TES) onboard the Aura spacecraft. The uncertainties of the calculated near-surface O3 using TES mid-tropospheric satellite retrievals and a linear regression model were less than 20 %, which is less than that of the observed variability of O3 at the surface in this region. These results utilize a region of the troposphere to which existing satellites are more sensitive compared to the boundary layer and can provide information of O3 at the near-surface using existing satellite infrastructure and algorithms.


Datum: 01.09.2015


Meteorological controls on particle growth events in Beltsville, MD, USA during July 2011

Abstract

During summer 2011, particle growth events were investigated in Beltsville, Maryland, USA where anthropogenic and biogenic hydrocarbon emissions heavily influenced the lower atmosphere. Aerosol sampling was made from a 5-m tower during July 2011. Ultrafine particle growth events occurred on 4 of the 25 days sampled. Regional particle growth events occurred after the passage of synoptic cold fronts. During regional particle growth events temperature and relative humidity were 2° Celsius lower and 3 % less than on non-event days and the local wind direction came from the northeast. With average growth rates of 3.5 nm hr−1, regional particle growth events happened around 15:00 Universal Time Coordinated, shortly after increased mixing within the atmospheric boundary layer. Regional particle growth events were associated with cooler, drier, mostly sunny days that had low sulfur dioxide mixing ratio (~0.6 parts per billion by volume). Regional particle growth events occurred when the atmospheric boundary layer was dominated by free convection and had lower sensible heat fluxes compared to short-lived events or non-particle growth event days.


Datum: 01.09.2015


Bay breeze climatology at two sites along the Chesapeake bay from 1986–2010: Implications for surface ozone

Abstract

Hourly surface meteorological measurements were coupled with surface ozone (O3) mixing ratio measurements at Hampton, Virginia and Baltimore, Maryland, two sites along the Chesapeake Bay in the Mid-Atlantic United States, to examine the behavior of surface O3 during bay breeze events and quantify the impact of the bay breeze on local O3 pollution. Analyses were performed for the months of May through September for the years 1986 to 2010. The years were split into three groups to account for increasingly stringent environmental regulations that reduced regional emissions of nitrogen oxides (NOx): 1986–1994, 1995–2002, and 2003–2010. Each day in the 25-year record was marked either as a bay breeze day, a non-bay breeze day, or a rainy/cloudy day based on the meteorological data. Mean eight hour (8-h) averaged surface O3 values during bay breeze events were 3 to 5 parts per billion by volume (ppbv) higher at Hampton and Baltimore than on non-bay breeze days in all year periods. Anomalies from mean surface O3 were highest in the afternoon at both sites during bay breeze days in the 2003–2010 study period. In conjunction with an overall lowering of baseline O3 after the 1995-2002 period, the percentage of total exceedances of the Environmental Protection Agency (EPA) 75 ppbv 8-h O3 standard that occurred on bay breeze days increased at Hampton for 2003–2010, while remaining steady at Baltimore. These results suggest that bay breeze circulations are becoming more important to causing exceedance events at particular sites in the region, and support the hypothesis of Martins et al. (2012) that highly localized meteorology increasingly drives air quality events at Hampton.


Datum: 01.09.2015


Effects of local meteorology and aerosols on ozone and nitrogen dioxide retrievals from OMI and pandora spectrometers in Maryland, USA during DISCOVER-AQ 2011

Abstract

An analysis is presented for both ground- and satellite-based retrievals of total column ozone and nitrogen dioxide levels from the Washington, D.C., and Baltimore, Maryland, metropolitan area during the NASA-sponsored July 2011 campaign of Deriving Information on Surface COnditions from Column and VERtically Resolved Observations Relevant to Air Quality (DISCOVER-AQ). Satellite retrievals of total column ozone and nitrogen dioxide from the Ozone Monitoring Instrument (OMI) on the Aura satellite are used, while Pandora spectrometers provide total column ozone and nitrogen dioxide amounts from the ground. We found that OMI and Pandora agree well (residuals within ±25 % for nitrogen dioxide, and ±4.5 % for ozone) for a majority of coincident observations during July 2011. Comparisons with surface nitrogen dioxide from a Teledyne API 200 EU NOx Analyzer showed nitrogen dioxide diurnal variability that was consistent with measurements by Pandora. However, the wide OMI field of view, clouds, and aerosols affected retrievals on certain days, resulting in differences between Pandora and OMI of up to ±65 % for total column nitrogen dioxide, and ±23 % for total column ozone. As expected, significant cloud cover (cloud fraction >0.2) was the most important parameter affecting comparisons of ozone retrievals; however, small, passing cumulus clouds that do not coincide with a high (>0.2) cloud fraction, or low aerosol layers which cause significant backscatter near the ground affected the comparisons of total column nitrogen dioxide retrievals. Our results will impact post-processing satellite retrieval algorithms and quality control procedures.


Datum: 01.09.2015


Estimating surface NO 2 and SO 2 mixing ratios from fast-response total column observations and potential application to geostationary missions

Abstract

Total-column nitrogen dioxide (NO2) data collected by a ground-based sun-tracking spectrometer system (Pandora) and an photolytic-converter-based in-situ instrument collocated at NASA’s Langley Research Center in Hampton, Virginia were analyzed to study the relationship between total-column and surface NO2 measurements. The measurements span more than a year and cover all seasons. Surface mixing ratios are estimated via application of a planetary boundary-layer (PBL) height correction factor. This PBL correction factor effectively corrects for boundary-layer variability throughout the day, and accounts for up to ≈75 % of the variability between the NO2 data sets. Previous studies have made monthly and seasonal comparisons of column/surface data, which has shown generally good agreement over these long average times. In the current analysis comparisons of column densities averaged over 90 s and 1 h are made. Applicability of this technique to sulfur dioxide (SO2) is briefly explored. The SO2 correlation is improved by excluding conditions where surface levels are considered background. The analysis is extended to data from the July 2011 DISCOVER-AQ mission over the greater Baltimore, MD area to examine the method’s performance in more-polluted urban conditions where NO2 concentrations are typically much higher.


Datum: 01.09.2015


Ozone profiles in the Baltimore-Washington region (2006–2011): satellite comparisons and DISCOVER-AQ observations

Abstract

Much progress has been made in creating satellite products for tracking the pollutants ozone and NO2 in the troposphere. Yet, in mid-latitude regions where meteorological interactions with pollutants are complex, accuracy can be difficult to achieve, largely due to persistent layering of some constituents. We characterize the layering of ozone soundings and related species measured from aircraft over two ground sites in suburban Washington, DC (Beltsville, MD, 39.05 N; 76.9 W) and Baltimore (Edgewood, MD, 39.4 N; 76.3 W) during the July 2011 DISCOVER-AQ (Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality) experiment. First, we compare column-ozone amounts from the Beltsville and Edgewood sondes with data from overpassing satellites. Second, processes influencing ozone profile structure are analyzed using Laminar Identification and tracers: sonde water vapor, aircraft CO and NOy. Third, Beltsville ozone profiles and meteorological influences in July 2011 are compared to those from the summers of 2006–2010. Sonde-satellite offsets in total ozone during July 2011 at Edgewood and Beltsville, compared to the Ozone Monitoring Instrument (OMI), were 3 % mean absolute error, not statistically significant. The disagreement between an OMI/Microwave Limb Sounder-based tropospheric ozone column and the sonde averaged 10 % at both sites, with the sonde usually greater than the satellite. Laminar Identification (LID), that distinguishes ozone segments influenced by convective and advective transport, reveals that on days when both stations launched ozonesondes, vertical mixing was stronger at Edgewood. Approximately half the lower free troposphere sonde profiles have very dry laminae, with coincident aircraft spirals displaying low CO (80–110 ppbv), suggesting stratospheric influence. Ozone budgets at Beltsville in July 2011, determined with LID, as well as standard meteorological indicators, resemble those of 4 of the previous 5 summers. The penetration of stratospheric air throughout the troposphere appears to be typical for summer conditions in the Baltimore-Washington region.


Datum: 01.09.2015


Sensitivity of convection to observed variation in aerosol size distributions and composition at a rural site in the southeastern United States

Abstract

We present a sensitivity analysis to determine the impact of variations in aerosol physical and chemical characteristics, as observed in the field in the southeastern United States, on convective cloud microphysics. Scenarios reflecting changes in aerosol properties, observed over the Piedmont of Virginia and associated with new particle formation and growth events, were evaluated using the two-dimensional version of the Goddard Cumulus Ensemble Model with detailed spectral-bin microphysics. Two aerosol size distributions represented early and late stages of particle growth, and two aerosol chemical compositions (norpinic acid and ammonium sulfate) represented extremes in aerosol hygroscopicity observed at the field site, for a total of four scenarios. The chosen compositions reflect inferred local changes in aerosol composition over short time scales. Variations in the aerosol size distribution and composition resulted in substantial variation in the total number of cloud condensation nuclei (CCN) produced in the four case studies. Cases with high CCN concentrations developed larger, more vigorous clouds with more precipitation generated by both warm and cold rain processes. Greater numbers of drops were propelled aloft and formed an extensive ice anvil that produced a large area of stratiform rain. Convection was enhanced by increasing aerosols despite decreases in precipitation efficiency. In contrast, lower CCN concentrations developed smaller clouds with suppressed cold rain processes and less total precipitation. The relatively small increase in CCN concentration associated with the increase in aerosol hygroscopicity resulted in an increase in accumulated modeled precipitation of 12 % after 180 min of simulation time in both high and low CCN cases. The increase in accumulated precipitation due to the substantial increase in CCN concentration associated with growth of the aerosol size distribution was 93 % for both aerosol compositions. The timing of the onset of precipitation was not affected by aerosol concentration or composition.


Datum: 01.09.2015


Chemical processing within and above a loblolly pine forest in North Carolina, USA

Abstract

Hydrocarbon species and related meteorological and chemical variables were measured within and immediately above a loblolly pine forest in North Carolina, USA during 15–18 July 2003. The degree of photochemical processing within the forest canopy of biogenic hydrocarbons emitted at the foliage level is investigated with the aid of a one-dimensional photochemical model. Such in-canopy photochemical processes remain poorly understood largely due to limited observations of plant-emitted gases, chemical reactions, and yields of photochemical reactions inside plant canopies. These hydrocarbons are vented into the overlying atmospheric boundary layer and participate in regional-scale photochemical processes. At the forested site, isoprene was the dominant sink for hydroxyl radicals and ozone precursor among all the volatile organic compounds. Abundances of many hydrocarbons peaked in the early morning and late afternoon/early evening due to local emissions, while reaching minima at mid-day due to intense turbulent mixing and vigorous photochemistry. Methyl vinyl ketone and methacrolein, which were produced mostly from isoprene oxidation, had elevated mixing ratios during noontime in addition to maximum levels in the early morning and early evening. Abundances of species with dominant biogenic origin (e.g., isoprene, α-pinene, β-pinene, and limonene) were higher within the canopy than above the forest. For the species produced in the atmospheric boundary layer due to photochemical reactions, abundances residing away from the canopy were higher than those just above the canopy in response to photochemical production and/or transport associated with advection. Within the forest canopy photochemical reactions destroyed approximately 10 % of the locally emitted isoprene. Chemically more reactive species such as limonene experienced greater rates of removal in response to in-canopy chemical processing. Model sensitivity studies indicated that nitrogen oxides limited the formation of oxidants at the forested study site.


Datum: 01.09.2015






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