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  • 1
    Publication Date: 2019-07-13
    Description: Halogens in the troposphere are increasingly recognized as playing an important role for atmospheric chemistry, and possibly climate. Bromine and iodine react catalytically to destroy ozone (O3), oxidize mercury, and modify oxidative capacity that is relevant for the lifetime of greenhouse gases. Most of the tropospheric O3 and methane (CH4) loss occurs at tropical latitudes. Here we report simultaneous measurements of vertical profiles of bromine oxide (BrO) and iodine oxide (IO) in the tropical and subtropical free troposphere (10degN to 40degS), and show that these halogens are responsible for 34% of the column-integrated loss of tropospheric O3. The observed BrO concentrations increase strongly with altitude (approx.3.4 pptv at 13.5 km), and are 2-4 times higher than predicted in the tropical free troposphere. BrO resembles model predictions more closely in stratospheric air. The largest model low bias is observed in the lower tropical transition layer (TTL) over the tropical eastern Pacific Ocean, and may reflect a missing inorganic bromine source supplying an additional 2.5-6.4 pptv total inorganic bromine (Bry), or model overestimated Bry wet scavenging. Our results highlight the importance of heterogeneous chemistry on ice clouds, and imply an additional Bry source from the debromination of sea salt residue in the lower TTL. The observed levels of bromine oxidize mercury up to 3.5 times faster than models predict, possibly increasing mercury deposition to the ocean. The halogen-catalyzed loss of tropospheric O3 needs to be considered when estimating past and future ozone radiative effects.
    Keywords: Meteorology and Climatology
    Type: NF1676L-20964 , Proceedings of the National Academy of Sciences (e-ISSN 1091-6490); 112; 30; 9281-9286
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  • 2
    Publication Date: 2019-07-13
    Description: Airborne Multi-AXis Differential Optical Absorption Spectroscopy (AMAX-DOAS) measurements of NO2 tropospheric vertical columns were performed over California for two months in summer 2010. The observations are compared to the NASA Ozone Monitoring Instrument (OMI) tropospheric vertical columns (data product v2.1) in two ways: (1) Median data were compared for the whole time period for selected boxes, and the agreement was found to be fair (R = 0.97, slope = 1.4 +/- 0.1, N= 10). (2) A comparison was performed on the mean of coincident AMAX-DOAS measurements within the area of the corresponding OMI pixels with the tropospheric NASA OMI NO2 assigned to that pixel. The effects of different data filters were assessed. Excellent agreement and a strong correlation (R = 0.85, slope = 1.05 +/- 0.09, N= 56) was found for (2) when the data were filtered to eliminate large pixels near the edge of the OMI orbit, the cloud radiance fraction was〈50%, the OMI overpass occurred within 2 h of the AMAX-DOAS measurements, the flight altitude was〉2 km, and a representative sample of the footprint was taken by the AMAX-DOAS instrument. The AMAX-DOAS and OMI data sets both show a reduction of NO2 tropospheric columns on weekends by 38 +/- 24% and 33 +/- 11%, respectively. The assumptions in the tropospheric satellite air mass factor simulations were tested using independent measurements of surface albedo, aerosol extinction, and NO2 profiles for Los Angeles for July 2010 indicating an uncertainty of 12%.
    Keywords: Geosciences (General)
    Type: GSFC-E-DAA-TN10039 , Journal of Geophysical Reserach: Atmospheres; 118; 13; 7400-7413
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  • 3
    Publication Date: 2019-07-13
    Description: We report measurements of bromine monoxide (BrO) and use an observationally constrained chemical box model to infer total gas-phase inorganic bromine (Br(sub y)) over the tropical western Pacific Ocean (tWPO) during the CONTRAST field campaign (January-February 2014). The observed BrO and inferred Bry profiles peak in the marine boundary layer (MBL), suggesting the need for a bromine source from sea-salt aerosol (SSA), in addition to organic bromine (CBry ). Both profiles are found to be C-shaped with local maxima in the upper free troposphere (FT). The median tropospheric BrO vertical column density (VCD) was measured as 1.6 x 10(exp 13) molec cm(exp -2), compared to model predictions of 0.9 x 10(exp 13) molec cm(exp -2) in GEOS-Chem (CBr(sub y) but no SSA source), 0.4 x 10(exp 13) molec cm(exp -2) in CAM-Chem (CBr(sub y) and SSA), and 2.1 x 10(exp 13) molec cm(exp -2) in GEOS-Chem (CBry and SSA). Neither global model fully captures the Cshape of the Br(sun y) profile. A local Br(sub y) maximum of 3.6 ppt (2.9-4.4 ppt; 95% confidence interval, CI) is inferred between 9.5 and 13.5 km in air masses influenced by recent convective outflow. Unlike BrO, which increases from the convective tropical tropopause layer (TTL) to the aged TTL, gas-phase Br(sub y) decreases from the convective TTL to the aged TTL. Analysis of gas-phase Br(sub y) against multiple tracers (CFC-11, H2O/O3 ratio, and potential temperature) reveals a Br(sub y) minimum of 2.7 ppt (2.3-3.1 ppt; 95% CI) in the aged TTL, which agrees closely with a stratospheric injection of 2.6 +/- 0.6 ppt of inorganic Br(sub y) (estimated from CFC-11 correlations), and is remarkably insensitive to assumptions about heterogeneous chemistry. Bry increases to 6.3 ppt (5.6-7.0 ppt; 95% CI) in the stratospheric "middleworld" and 6.9 ppt (6.5-7.3 ppt; 95% CI) in the stratospheric "overworld". The local Br(sub y) minimum in the aged TTL is qualitatively (but not quantitatively) captured by CAM-Chem, and suggests a more complex partitioning of gas-phase and aerosol Br(sub y) species than previously recognized. Our data provide corroborating evidence that inorganic bromine sources (e.g., SSA-derived gas-phase Br(sub y) ) are needed to explain the gas-phase Br(sub y) budget in the upper free troposphere and TTL. They are also consistent with observations of significant bromide in Upper Troposphere-Lower Stratosphere aerosols. The total Br(sub y) budget in the TTL is currently not closed, because of the lack of concurrent quantitative measurements of gas-phase Br(sub y) species (i.e., BrO, HOBr, HBr, etc.) and aerosol bromide. Such simultaneous measurements are needed to (1) quantify SSA-derived Br(sub y) in the upper FT, (2) test Br(sub y) partitioning, and possibly explain the gas-phase Br(sub y) minimum in the aged TTL, (3) constrain heterogeneous reaction rates of bromine, and (4) account for all of the sources of Br(sub y) to the lower stratosphere.
    Keywords: Geosciences (General)
    Type: GSFC-E-DAA-TN55227 , Atmospheric Chemistry and Physics (ISSN 1680-7316) (e-ISSN 1680-7324); 17; 24; 15245-15270
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  • 4
    Publication Date: 2019-07-13
    Description: We use a 0-D photochemical box model and a 3-D global chemistry-climate model, combined with observations from the NOAA Southeast Nexus (SENEX) aircraft campaign, to understand the sources and sinks of glyoxal over the Southeast United States. Box model simulations suggest a large difference in glyoxal production among three isoprene oxidation mechanisms (AM3ST, AM3B, and Master Chemical Mechanism (MCM) v3.3.1). These mechanisms are then implemented into a 3-D global chemistry-climate model. Comparison with field observations shows that the average vertical profile of glyoxal is best reproduced by AM3ST with an effective reactive uptake coefficient gamma(sub glyx) of 2 x 10(exp -3) and AM3B without heterogeneous loss of glyoxal. The two mechanisms lead to 0-0.8micrograms m(exp -3) secondary organic aerosol (SOA) from glyoxal in the boundary layer of the Southeast U.S. in summer. We consider this to be the lower limit for the contribution of glyoxal to SOA, as other sources of glyoxal other than isoprene are not included in our model. In addition, we find that AM3B shows better agreement on both formaldehyde and the correlation between glyoxal and formaldehyde (RGF[GLYX]/[HCHO]), resulting from the suppression of delta-isoprene peroxy radicals (delta-ISOPO2). We also find that MCM v3.3.1 may underestimate glyoxal production from isoprene oxidation, in part due to an underestimated yield from the reaction of isoprene epoxydiol (IEPOX) peroxy radicals with HO2. Our work highlights that the gas-phase production of glyoxal represents a large uncertainty in quantifying its contribution to SOA.
    Keywords: Environment Pollution
    Type: GSFC-E-DAA-TN41635 , Journal of Geophysical Research: Atmospheres (ISSN 2169-897X) (e-ISSN 2169-8996); 121; 16; 9849-9861
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  • 5
    Publication Date: 2019-07-13
    Description: The Two-Column Aerosol Project (TCAP), conducted from June 2012 through June 2013, was a unique study designed to provide a comprehensive data set that can be used to investigate a number of important climate science questions, including those related to aerosol mixing state and aerosol radiative forcing. The study was designed to sample the atmosphere be tween and within two atmospheric columns; one fixed near the coast of North America (over Cape Cod, MA) and a second moveable column over the Atlantic Ocean several hundred kilometers from the coast. The U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) was deployed at the base of the Cape Cod column, and the ARM Aerial Facility was utilized for the summer and winter intensive observation periods. One important finding from TCAP is that four of six nearly cloud-free flight days had aerosol layers aloft in both the Cape Cod and maritime columns that were detected using the nadir pointing second-generation NASA high-spectral resolution lidar (HSRL-2).These layer s contributed up to 60 of the total observed aerosol optical depth (AOD). Many of these layers were also intercepted by the aircraft configured for in situ sampling, and the aerosol in the layers was found to have increased amounts of biomass burning material and nitrate compared to aerosol found near the surface. In addition, while there was a great deal of spatial and day-to-day variability in the aerosol chemical composition and optical properties, no systematic differences between the two columns were observed.
    Keywords: Earth Resources and Remote Sensing
    Type: GSFC-E-DAA-TN29469 , Journal of Geophysical Research: Atmospheres (ISSN 2169-897X); 121; 1; 336-361
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  • 6
    Publication Date: 2019-08-01
    Description: We use aircraft observations combined with the reanalysis data to investigate the radiative effects of ice supersaturation (ISS). Our results show that although the excess water vapor over ice saturation itself has relatively small radiative effects, mistaking it as ice crystals in climate models would lead to considerable impacts: on average, +2.49 W/m(exp 2) change in the top of the atmosphere (TOA) radiation, -2.7 W/m(exp 2) change in surface radiation, and 1.47 K/d change in heating rates. The radiative effects of ISS generally increase with the magnitudes of supersaturation. However, there is a strong dependence on the preexisting ice water path, which can even change the sign of the TOA radiative effect. It is therefore important to consider coexistence between ISS and ice clouds and to validate their relationship in the parameterizations of ISS in climate models.
    Keywords: Meteorology and Climatology
    Type: NF1676L-24430 , Geophysical Research Letters (ISSN 0094-8276) (e-ISSN 1944-8007); 43; 20; 11,039-11,047
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  • 7
    Publication Date: 2016-03-14
    Description: Stable carbon isotopic compositions of water-soluble organic carbon (WSOC) and organic molecular markers were measured to investigate the relative contributions of the sea-surface sources to the water-soluble fraction of submicron organic aerosols collected over the eastern equatorial Pacific during the Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated VOCs (TORERO)/KA-12-01 cruise. On average, the water-soluble organic fraction of the total carbon (TC) mass in submicron aerosols was ~ 30–35 % in the open oceans, whereas it was ~ 60 % in the coastal oceans. The average stable carbon isotope ratio of WSOC (δ13CWSOC) was −19.8 ± 2.0 ‰, which was systematically higher than that of TC (δ13CTC) (−21.8 ± 1.4 ‰). We found that in both coastal and open oceans, the δ13CWSOC was close to the typical values of δ13C for dissolved organic carbon (DOC), ranging from −22 ‰ to −20 ‰ in surface seawater of tropical Pacific oceans. This suggests an enrichment of marine biological products in WSOC aerosols in the study region regardless of the oceanic area. In particular, enhanced levels of WSOC and biogenic organic marker compounds together with high values of WSOC/TC (~ 60 %) and δ13CWSOC were observed over upwelling areas and phytoplankton blooms, which was attributed to planktonic tissues being more enriched in δ13C. The δ13C analysis estimated that on average, marine sources contribute ~ 90 ± 25 % of the aerosol carbon, indicating the predominance of marine-derived carbon in the submicron WSOC. This conclusion is supported by Lagrangian trajectory analysis, which suggests that the majority of the sampling points on the ship had been exposed to marine boundary layer air for more than 80 % of the time during the previous 7 days. The combined analysis of the δ13C and monosaccharides, such as glucose and fructose, indicated that DOC concentration was the major factor controlling the concentration levels of the submicron WSOC regardless of the oceanic areas over the study region.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union (EGU).
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  • 8
    Publication Date: 2016-02-11
    Description: The multiphase chemistry of glyoxal is a source of secondary organic aerosol (SOA), including its light-absorbing product imidazole-2-carboxaldehyde (IC). IC is a photosensitizer that can contribute to additional aerosol ageing and growth when its excited triplet state oxidizes hydrocarbons (reactive uptake) via H-transfer chemistry. We have conducted a series of photochemical coated-wall flow tube (CWFT) experiments using films of IC and citric acid (CA), an organic proxy and H-donor in the condensed-phase. The formation rate of gas-phase HO2 radicals (PHO2) was measured indirectly by converting gas-phase NO into NO2. We report on experiments that relied on measurements of NO2 formation, NO loss; and HONO formation. PHO2 was found to be a linear function of (1) the [IC]×[CA] concentration product, and (2) the photon actinic flux. Additionally, (3) a more complex function of relative humidity (25 % 〈 RH 〈 63 %), and of (4) the O2/N2 ratio (15 % 〈 O2/N2 〈 56 %) was observed, most likely indicating competing effects of dilution, HO2 mobility and losses in the film. The maximum PHO2 was observed at 25–55 % RH and at ambient O2/N2. The HO2 radicals form in the condensed-phase when excited IC triplet states are reduced by H-transfer from a donor, CA in our system, and subsequently react with O2 to re-generate IC, leading to a catalytic cycle. OH does not appear to be formed as a primary product but is produced from the reaction of NO with HO2 in the gas phase. Further, seed aerosols containing IC and ammonium sulfate were exposed to gas-phase limonene and NOx in aerosol flow tube experiments, confirming significant PHO2 from aerosol surfaces. Atmospheric implications consist in a potentially relevant contribution of triplet state photochemistry for gas-phase HO2 production, aerosol growth and ageing.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union (EGU).
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  • 9
    Publication Date: 2016-06-03
    Description: Ammonia (NH3) has been detected in the upper troposphere by analysis of averaged MIPAS (Michelson Interferomter for Passive Atmospheric Sounding) infrared limb-emission spectra. We have found enhanced amounts of NH3 within the region of the Asian monsoon at 12–15 km altitude. Three-monthly, 10° longitude x 10° latitude average profiles reaching maximum mixing ratios of around 30 pptv in this altitude range have been retrieved with a vertical resolution of 3–8 km and estimated errors of about 5 pptv. These observations show that loss processes during transport from the boundary layer to the upper troposphere within the Asian monsoon do not deplete the air entirely of NH3. Thus, ammonia might contribute to the so-called Asian tropopause aersol layer by formation of ammonium aerosol particles. On a global scale, outside the monsoon area and during different seasons, we could not detect enhanced values of NH3 above the actual detection limit of about 3–5 pptv. This upper bound helps to constrain global model simulations.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union (EGU).
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  • 10
    Publication Date: 2016-11-18
    Description: Ammonia (NH3) has been detected in the upper troposphere by the analysis of averaged MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) infrared limb-emission spectra. We have found enhanced amounts of NH3 within the region of the Asian summer monsoon at 12–15km altitude. Three-monthly, 10° longitude × 10° latitude average profiles reaching maximum mixing ratios of around 30pptv in this altitude range have been retrieved, with a vertical resolution of 3–8km and estimated errors of about 5pptv. These observations show that loss processes during transport from the boundary layer to the upper troposphere within the Asian monsoon do not deplete the air entirely of NH3. Thus, ammonia might contribute to the so-called Asian tropopause aerosol layer by the formation of ammonium aerosol particles. On a global scale, outside the monsoon area and during different seasons, we could not detect enhanced values of NH3 above the actual detection limit of about 3–5pptv. This upper bound helps to constrain global model simulations.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union (EGU).
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