The Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2), is NASA’s latest reanalysis for the satellite era (1980 onward) using the Goddard Earth Observing System, ...version 5 (GEOS-5), Earth system model. MERRA-2 provides several improvements over its predecessor (MERRA-1), including aerosol assimilation for the entire period. MERRA-2 assimilates bias-corrected aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectroradiometer and the Advanced Very High Resolution Radiometer instruments. Additionally, MERRA-2 assimilates (non bias corrected) AOD from the Multiangle Imaging SpectroRadiometer over bright surfaces and AOD from Aerosol Robotic Network sunphotometer stations. This paper, the second of a pair, summarizes the efforts to assess the quality of the MERRA-2 aerosol products. First, MERRA-2 aerosols are evaluated using independent observations. It is shown that the MERRA-2 absorption aerosol optical depth (AAOD) and ultraviolet aerosol index (AI) compare well with Ozone Monitoring Instrument observations. Next, aerosol vertical structure and surface fine particulate matter (PM2.5) are evaluated using available satellite, aircraft, and ground-based observations. While MERRA-2 generally compares well to these observations, the assimilation cannot correct for all deficiencies in the model (e.g., missing emissions). Such deficiencies can explain many of the biases with observations. Finally, a focus is placed on several major aerosol events to illustrate successes and weaknesses of the AOD assimilation: the Mount Pinatubo eruption, a Saharan dust transport episode, the California Rim Fire, and an extreme pollution event over China. The article concludes with a summary that points to best practices for using the MERRA-2 aerosol reanalysis in future studies.
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BFBNIB, DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
Nitrogen oxides (NOx) have fallen steadily across the US over the last 15 years. At the same time, NOx concentrations decrease on weekends relative to weekdays, largely without co-occurring changes ...in other gas-phase emissions, due to patterns of diesel truck activities. These trends taken together provide two independent constraints on the role of NOx in the nonlinear chemistry of atmospheric oxidation. In this context, we interpret interannual trends in wintertime ammonium nitrate (NH4NO3) in the San Joaquin Valley of California, a location with the worst aerosol pollution in the US and where a large portion of aerosol mass is NH4NO3. Here, we show that NOx reductions have simultaneously decreased nighttime and increased daytime NH4NO3 production over the last decade. We find a substantial decrease in NH4NO3 since 2000 and conclude that this decrease is due to reduced nitrate radical-initiated production at night in residual layers that are decoupled from fresh emissions at the surface. Further reductions in NOx are imminent in California, and nationwide, and we make a quantitative prediction of the response of NH4NO3. We show that the combination of rapid chemical production and efficient NH4NO3 loss via deposition of gas-phase nitric acid implies that high aerosol days in cities in the San Joaquin Valley air basin are responsive to local changes in NOx within those individual cities. Our calculations indicate that large decreases in NOx in the future will not only lower wintertime NH4NO3 concentrations but also cause a transition in the dominant NH4NO3 source from nighttime to daytime chemistry.
The NASA DC-8 aircraft characterized the aerosol properties, chemical composition, and cloud condensation nuclei (CCN) concentrations of the summertime Arctic during the 2008 NASA Arctic Research of ...the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. Air masses characteristic of fresh and aged biomass burning, boreal forest, Arctic background, and anthropogenic industrial pollution were sampled. Observations were spatially extensive (50–85° N and 40–130° W) and exhibit significant variability in aerosol and CCN concentrations. The chemical composition was dominated by highly oxidized organics (66–94% by volume), with a water-soluble mass fraction of more than 50%. The aerosol hygroscopicity parameter, κ, ranged between κ = 0.08–0.32 for all air mass types. Industrial pollution had the lowest κ of 0.08 ± 0.01, while the Arctic background had the highest and most variable κ of 0.32 ± 0.21, resulting from a lower and more variable organic fraction. Both fresh and aged (long-range transported) biomass burning air masses exhibited remarkably similar κ (0.18 ± 0.13), consistent with observed rapid chemical and physical aging of smoke emissions in the atmosphere, even in the vicinity of fresh fires. The organic hygroscopicity (κorg) was parameterized by the volume fraction of water-soluble organic matter (εWSOM), with a κ = 0.12, such that κorg = 0.12εWSOM. Assuming bulk (size-independent) composition and including the κorg parameterization enabled CCN predictions to within 30% accuracy for nearly all environments sampled. The only exception was for industrial pollution from Canadian oil sands exploration, where an external mixture and size-dependent composition was required. Aerosol mixing state assumptions (internal vs. external) in all other environments did not significantly affect CCN predictions; however, the external mixing assumption provided the best results, even though the available observations could not determine the true degree of external mixing and therefore may not always be representative of the environments sampled. No correlation was observed between κorg and O : C. A novel correction of the CCN instrument supersaturation for water vapor depletion, resulting from high concentrations of CCN, was also employed. This correction was especially important for fresh biomass burning plumes where concentrations exceeded 1.5×104 cm−3 and introduced supersaturation depletions of 25%. Not accounting for supersaturation depletion in these high concentration environments would therefore bias CCN closure up to 25% and inferred κ by up to 50%.
The use of alternative fuels for aviation is likely to increase due to concerns over fuel security, price stability, and the sustainability of fuel sources. Concurrent reductions in particulate ...emissions from these alternative fuels are expected because of changes in fuel composition including reduced sulfur and aromatic content. The NASA Alternative Aviation Fuel Experiment (AAFEX) was conducted in January-February 2009 to investigate the effects of synthetic fuels on gas-phase and particulate emissions. Standard petroleum JP-8 fuel, pure synthetic fuels produced from natural gas and coal feedstocks using the Fischer-Tropsch (FT) process, and 50% blends of both fuels were tested in the CFM-56 engines on a DC-8 aircraft. To examine plume chemistry and particle evolution with time, samples were drawn from inlet probes positioned 1, 30, and 145 m downstream of the aircraft engines. No significant alteration to engine performance was measured when burning the alternative fuels. However, leaks in the aircraft fuel system were detected when operated with the pure FT fuels as a result of the absence of aromatic compounds in the fuel. Dramatic reductions in soot emissions were measured for both the pure FT fuels (reductions in mass of 86% averaged over all powers) and blended fuels (66%) relative to the JP-8 baseline with the largest reductions at idle conditions. At 7% power, this corresponds to a reduction from 7.6 mg kg-1 for JP-8 to 1.2 mg kg-1 for the natural gas FT fuel. At full power, soot emissions were reduced from 103 to 24 mg kg-1 (JP-8 and natural gas FT, respectively). The alternative fuels also produced smaller soot (e.g., at 85% power, volume mean diameters were reduced from 78 nm for JP-8 to 51 nm for the natural gas FT fuel), which may reduce their ability to act as cloud condensation nuclei (CCN). The reductions in particulate emissions are expected for all alternative fuels with similar reductions in fuel sulfur and aromatic content regardless of the feedstock. As the plume cools downwind of the engine, nucleation-mode aerosols form. For the pure FT fuels, reductions (94% averaged over all powers) in downwind particle number emissions were similar to those measured at the exhaust plane (84%). However, the blended fuels had less of a reduction (reductions of 30-44%) than initially measured (64%). The likely explanation is that the reduced soot emissions in the blended fuel exhaust plume results in promotion of new particle formation microphysics, rather than coating on pre-existing soot particles, which is dominant in the JP-8 exhaust plume. Downwind particle volume emissions were reduced for both the pure (79 and 86% reductions) and blended FT fuels (36 and 46%) due to the large reductions in soot emissions. In addition, the alternative fuels had reduced particulate sulfate production (near zero for FT fuels) due to decreased fuel sulfur content. To study the formation of volatile aerosols (defined as any aerosol formed as the plume ages) in more detail, tests were performed at varying ambient temperatures (-4 to 20 degree C). At idle, particle number and volume emissions were reduced linearly with increasing ambient temperature, with best fit slopes corresponding to -8 1014 particles (kg fuel)-1 degree C-1 for particle number emissions and -10 mm3 (kg fuel)-1 degree C-1 for particle volume emissions. The temperature dependency of aerosol formation can have large effects on local air quality surrounding airports in cold regions. Aircraft-produced aerosols in these regions will be much larger than levels expected based solely on measurements made directly at the engine exit plane. The majority (90% at idle) of the volatile aerosol mass formed as nucleation-mode aerosols, with a smaller fraction as a soot coating. Conversion efficiencies of up to 2.8% were measured for the partitioning of gas-phase precursors (unburned hydrocarbons and SO2) to form volatile aerosols. Highest conversion efficiencies were measured at 45% power.
An instrumented NASA P-3B aircraft was used for airborne sampling of trace gases in a plume that had emanated from a small forest understory fire in Georgia, USA. The plume was sampled at its origin ...to derive emission factors and followed ∼ 13.6 km downwind to observe chemical changes during the first hour of atmospheric aging. The P-3B payload included a proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS), which measured non-methane organic gases (NMOGs) at unprecedented spatiotemporal resolution (10 m spatial/0.1 s temporal). Quantitative emission data are reported for CO2, CO, NO, NO2, HONO, NH3, and 16 NMOGs (formaldehyde, methanol, acetonitrile, propene, acetaldehyde, formic acid, acetone plus its isomer propanal, acetic acid plus its isomer glycolaldehyde, furan, isoprene plus isomeric pentadienes and cyclopentene, methyl vinyl ketone plus its isomers crotonaldehyde and methacrolein, methylglyoxal, hydroxy acetone plus its isomers methyl acetate and propionic acid, benzene, 2,3-butanedione, and 2-furfural) with molar emission ratios relative to CO larger than 1 ppbV ppmV−1. Formaldehyde, acetaldehyde, 2-furfural, and methanol dominated NMOG emissions. No NMOGs with more than 10 carbon atoms were observed at mixing ratios larger than 50 pptV ppmV−1 CO. Downwind plume chemistry was investigated using the observations and a 0-D photochemical box model simulation. The model was run on a nearly explicit chemical mechanism (MCM v3.3) and initialized with measured emission data. Ozone formation during the first hour of atmospheric aging was well captured by the model, with carbonyls (formaldehyde, acetaldehyde, 2,3-butanedione, methylglyoxal, 2-furfural) in addition to CO and CH4 being the main drivers of peroxy radical chemistry. The model also accurately reproduced the sequestration of NOx into peroxyacetyl nitrate (PAN) and the OH-initiated degradation of furan and 2-furfural at an average OH concentration of 7.45 ± 1.07 × 106 cm−3 in the plume. Formaldehyde, acetone/propanal, acetic acid/glycolaldehyde, and maleic acid/maleic anhydride (tentatively identified) were found to be the main NMOGs to increase during 1 h of atmospheric plume processing, with the model being unable to capture the observed increase. A mass balance analysis suggests that about 50 % of the aerosol mass formed in the downwind plume is organic in nature.
In order to utilize satellite-based aerosol measurements for the determination of air quality, the relationship between aerosol optical properties (wavelength-dependent, column-integrated extinction ...measured by satellites) and mass measurements of aerosol loading (PM2.5 used for air quality monitoring) must be understood. This connection varies with many factors including those specific to the aerosol type – such as composition, size, and hygroscopicity – and to the surrounding atmosphere, such as temperature, relative humidity (RH), and altitude, all of which can vary spatially and temporally. During the DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality) project, extensive in situ atmospheric profiling in the Baltimore, MD–Washington, D.C. region was performed during 14 flights in July 2011. Identical flight plans and profile locations throughout the project provide meaningful statistics for determining the variability in and correlations between aerosol loading, composition, optical properties, and meteorological conditions. Measured water-soluble aerosol mass was composed primarily of ammonium sulfate (campaign average of 32 %) and organics (57 %). A distinct difference in composition was observed, with high-loading days having a proportionally larger percentage of sulfate due to transport from the Ohio River Valley. This composition shift caused a change in the aerosol water-uptake potential (hygroscopicity) such that higher relative contributions of inorganics increased the bulk aerosol hygroscopicity. These days also tended to have higher relative humidity, causing an increase in the water content of the aerosol. Conversely, low-aerosol-loading days had lower sulfate and higher black carbon contributions, causing lower single-scattering albedos (SSAs). The average black carbon concentrations were 240 ng m−3 in the lowest 1 km, decreasing to 35 ng m−3 in the free troposphere (above 3 km). Routine airborne sampling over six locations was used to evaluate the relative contributions of aerosol loading, composition, and relative humidity (the amount of water available for uptake onto aerosols) to variability in mixed-layer aerosol extinction. Aerosol loading (dry extinction) was found to be the predominant source, accounting for 88 % on average of the measured spatial variability in ambient extinction, with lesser contributions from variability in relative humidity (10 %) and aerosol composition (1.3 %). On average, changes in aerosol loading also caused 82 % of the diurnal variability in ambient aerosol extinction. However on days with relative humidity above 60 %, variability in RH was found to cause up to 62 % of the spatial variability and 95 % of the diurnal variability in ambient extinction. This work shows that extinction is driven to first order by aerosol mass loadings; however, humidity-driven hydration effects play an important secondary role. This motivates combined satellite–modeling assimilation products that are able to capture these components of the aerosol optical depth (AOD)–PM2.5 link. Conversely, aerosol hygroscopicity and SSA play a minor role in driving variations both spatially and throughout the day in aerosol extinction and therefore AOD. However, changes in aerosol hygroscopicity from day to day were large and could cause a bias of up to 27 % if not accounted for. Thus it appears that a single daily measurement of aerosol hygroscopicity can be used for AOD-to-PM2.5 conversions over the study region (on the order of 1400 km2). This is complimentary to the results of Chu et al. (2015), who determined that the aerosol vertical distribution from "a single lidar is feasible to cover the range of 100 km" in the same region.
Volatile organic compound (VOC) mixing ratios were measured with two different instruments at the T1 ground site in Mexico City during the Megacity Initiative: Local and Global Research Observations ...(MILAGRO) campaign in March of 2006. A gas chromatograph with flame ionization detector (GC-FID) quantified 18 light alkanes, alkenes and acetylene while a proton-transfer-reaction ion-trap mass spectrometer (PIT-MS) quantified 12 VOC species including oxygenated VOCs (OVOCs) and aromatics. A GC separation system was used in conjunction with the PIT-MS (GC-PIT-MS) to evaluate PIT-MS measurements and to aid in the identification of unknown VOCs. The VOC measurements are also compared to simultaneous canister samples and to two independent proton-transfer-reaction mass spectrometers (PTR-MS) deployed on a mobile and an airborne platform during MILAGRO. VOC diurnal cycles demonstrate the large influence of vehicle traffic and liquid propane gas (LPG) emissions during the night and photochemical processing during the afternoon. Emission ratios for VOCs and OVOCs relative to CO are derived from early-morning measurements. Average emission ratios for non-oxygenated species relative to CO are on average a factor of ~2 higher than measured for US cities. Emission ratios for OVOCs are estimated and compared to literature values the northeastern US and to tunnel studies in California. Positive matrix factorization analysis (PMF) is used to provide insight into VOC sources and processing. Three PMF factors were distinguished by the analysis including the emissions from vehicles, the use of liquid propane gas and the production of secondary VOCs + long-lived species. Emission ratios to CO calculated from the results of PMF analysis are compared to emission ratios calculated directly from measurements. The total PIT-MS signal is summed to estimate the fraction of identified versus unidentified VOC species.
Organic aerosol (OA) is an important fraction of submicron aerosols. However,
it is challenging to predict and attribute the specific organic compounds and
sources that lead to observed OA loadings, ...largely due to contributions from
secondary production. This is especially true for megacities surrounded by
numerous regional sources that create an OA background. Here, we utilize
in situ gas and aerosol observations collected on board the NASA DC-8 during
the NASA–NIER KORUS-AQ (Korea–United States Air Quality) campaign to
investigate the sources and hydrocarbon precursors that led to the secondary
OA (SOA) production observed over Seoul. First, we investigate the
contribution of transported OA to total loadings observed over Seoul by
using observations over the Yellow Sea coupled to FLEXPART Lagrangian
simulations. During KORUS-AQ, the average OA loading advected into Seoul was
∼1–3 µg sm−3. Second, taking this background into
account, the dilution-corrected SOA concentration observed over Seoul was
∼140 µgsm-3ppmv-1 at 0.5 equivalent photochemical
days. This value is at the high end of what has been observed in other
megacities around the world (20–70 µgsm-3ppmv-1 at 0.5
equivalent days). For the average OA concentration observed over Seoul
(13 µg sm−3), it is clear that production of SOA from locally
emitted precursors is the major source in the region. The importance
of local SOA production was supported by the following observations.
(1) FLEXPART source contribution calculations indicate any
hydrocarbons with a lifetime of less than 1 day, which are shown to dominate the
observed SOA production, mainly originate from South Korea. (2) SOA
correlated strongly with other secondary photochemical species, including
short-lived species (formaldehyde, peroxy acetyl nitrate, sum of acyl peroxy
nitrates, dihydroxytoluene, and nitrate aerosol). (3) Results from
an airborne oxidation flow reactor (OFR), flown for the first time, show a
factor of 4.5 increase in potential SOA concentrations over Seoul versus over
the Yellow Sea, a region where background air masses that are advected into
Seoul can be measured. (4) Box model simulations reproduce SOA
observed over Seoul within 11 % on average and suggest that short-lived
hydrocarbons (i.e., xylenes, trimethylbenzenes, and semi-volatile and intermediate-volatility compounds) were the main SOA precursors over Seoul. Toluene
alone contributes 9 % of the modeled SOA over Seoul. Finally, along with
these results, we use the metric ΔOA/ΔCO2 to
examine the amount of OA produced per fuel consumed in a megacity, which
shows less variability across the world than ΔOA∕ΔCO.
This investigation examines aerosol dynamics during major fine mode aerosol transboundary pollution events in South Korea primarily during the KORUS-AQ campaign from May 1 – June 10, 2016, ...particularly when cloud fraction was high and/or fog was present to quantify the change in aerosol characteristics due to near-cloud or fog interaction. We analyze the new AERONET Version 3 data that have significant changes to cloud screening algorithms, allowing many more fine-mode observations in the near vicinity of clouds or fog. Case studies for detailed investigation include May 25–26, 2016 when cloud fraction was high over much of the peninsula, associated with a weak frontal passage and advection of pollution from China. These cloud-influenced Chinese transport dates also had the highest aerosol optical depth (AOD), surface PM2.5 concentrations and fine mode particle sizes of the entire campaign. Another likewise cloud/high relative humidity (RH) case is June 9 and 10, 2016 when fog was present over the Yellow Sea that appears to have affected aerosol properties well downwind over the Korean peninsula. In comparison we also investigated aerosol properties on air stagnation days with very low cloud cover and relatively low RH (May 17 & 18, 2016), when local Korean emissions dominated. Aerosol volume size distributions show marked differences between the transport days (with high RH and cloud influences) and the local pollution stagnation days, with total column-integrated particle fine mode volume being an order of magnitude greater on the pollution transport dates. The PM2.5 over central Seoul were significantly greater than for coastal sites on the transboundary transport days yet not on stagnation days, suggesting additional particle formation from gaseous urban emissions in cloud/fog droplets and/or in the high RH humidified aerosol environment. Many days had KORUS-AQ research aircraft flights that provided observations of aerosol absorption, particle chemistry and vertical profiles of extinction. AERONET retrievals and aircraft in situ measurements both showed high single scattering albedo (weak absorption) on the cloudy or cloud influenced days, plus aircraft profile in situ measurements showed large AOD enhancements (versus dried aerosol) at ambient relative humidity (RH) on the pollution transport days, consistent with the significantly larger fine mode particle radii and weak absorption.
•Highest AOD and PM2.5 over S. Korea had significant cloud cover and/or sea fog.•Particle volume was at least 10 times larger on high RH pollution transport days.•Particle SSA was high (0.97–0.99 in mid-visible) on pollution transport days.•The PM2.5 was higher over central Seoul than the coast during pollution transport.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
Actinic flux, as well as aerosol chemical and optical properties, were measured aboard the NASA DC-8 aircraft during the ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft ...and Satellites) mission in Spring and Summer 2008. These measurements were used in a radiative transfer code to retrieve spectral (350–550 nm) aerosol single scattering albedo (SSA) for biomass burning plumes encountered on 17 April and 29 June. Retrieved SSA values were subsequently used to calculate the absorption Angstrom exponent (AAE) over the 350–500 nm range. Both plumes exhibited enhanced spectral absorption with AAE values that exceeded 1 (6.78 0.38 for 17 April and 3.34 0.11 for 29 June). This enhanced absorption was primarily due to organic aerosol (OA) which contributed significantly to total absorption at all wavelengths for both 17 April (57.7%) and 29 June (56.2%). OA contributions to absorption were greater at UV wavelengths than at visible wavelengths for both cases. Differences in AAE values between the two cases were attributed to differences in plume age and thus to differences in the ratio of OA and black carbon (BC) concentrations. However, notable differences between AAE values calculated for the OA (AAEOA) for 17 April (11.15 0.59) and 29 June (4.94 0.19) suggested differences in the plume AAE values might also be due to differences in organic aerosol composition. The 17 April OA was much more oxidized than the 29 June OA as denoted by a higher oxidation state value for 17 April (+0.16 vs. −0.32). Differences in the AAEOA, as well as the overall AAE, were thus also possibly due to oxidation of biomass burning primary organic aerosol in the 17 April plume that resulted in the formation of OA with a greater spectral-dependence of absorption.
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