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Simulations of a cold-air pool associated with elevated wintertime ozone in the Uintah Basin, Utah

Numerical simulations are used to investigate the meteorological characteristics of the 31 January–6 February 2013 cold-air pool in the Uintah Basin, Utah, and the resulting high ozone concentrations. Flow features affecting cold-air pools and air quality in the Uintah Basin are studied, including the following: penetration of clean air into the basin from across the surrounding mountains, elevated easterlies within the inversion layer, and thermally driven slope and valley flows. The sensitivity of the boundary layer structure to snow cover variations and cloud microphysics are also examined. Snow cover increases boundary layer stability by enhancing the surface albedo, reducing the absorbed solar insolation at the surface, and lowering near-surface air temperatures. Snow cover also increases ozone levels by enhancing solar radiation available for photochemical reactions. Ice-dominant clouds enhance cold-air pool strength compared to liquid-dominant clouds by increasing nocturnal cooling and decreasing longwave cloud forcing.
Inverse modelling of CH4 emissions for 2010–2011 using different satellite retrieval products from GOSAT and SCIAMACHY

At the beginning of 2009 new space-borne observations of dry-air column-averaged mole fractions of atmospheric methane (XCH4) became available from the Thermal And Near infrared Sensor for carbon Observations–Fourier Transform Spectrometer (TANSO-FTS) instrument on board the Greenhouse Gases Observing SATellite (GOSAT). Until April 2012 concurrent {methane (CH4) retrievals} were provided by the SCanning Imaging Absorption spectroMeter for Atmospheric CartograpHY (SCIAMACHY) instrument on board the ENVironmental SATellite (ENVISAT). The GOSAT and SCIAMACHY XCH4 retrievals can be compared during the period of overlap. We estimate monthly average CH4 emissions between January 2010 and December 2011, using the TM5-4DVAR inverse modelling system. In addition to satellite data, high-accuracy measurements from the Cooperative Air Sampling Network of the National Oceanic and Atmospheric Administration Earth System Research Laboratory (NOAA ESRL) are used, providing strong constraints on the remote surface atmosphere. We discuss five inversion scenarios that make use of different GOSAT and SCIAMACHY XCH4 retrieval products, including two sets of GOSAT proxy retrievals processed independently by the Netherlands Institute for Space Research (SRON)/Karlsruhe Institute of Technology (KIT), and the University of Leicester (UL), and the RemoTeC "Full-Physics" (FP) XCH4 retrievals available from SRON/KIT. The GOSAT-based inversions show significant reductions in the root mean square (rms) difference between retrieved and modelled XCH4, and require much smaller bias corrections compared to the inversion using SCIAMACHY retrievals, reflecting the higher precision and relative accuracy of the GOSAT XCH4. Despite the large differences between the GOSAT and SCIAMACHY retrievals, 2-year average emission maps show overall good agreement among all satellite-based inversions, with consistent flux adjustment patterns, particularly across equatorial Africa and North America. Over North America, the satellite inversions result in a significant redistribution of CH4 emissions from North-East to South-Central United States. This result is consistent with recent independent studies suggesting a systematic underestimation of CH4 emissions from North American fossil fuel sources in bottom-up inventories, likely related to natural gas production facilities. Furthermore, all four satellite inversions yield lower CH4 fluxes across the Congo basin compared to the NOAA-only scenario, but higher emissions across tropical East Africa. The GOSAT and SCIAMACHY inversions show similar performance when validated against independent shipboard and aircraft observations, and XCH4 retrievals available from the Total Carbon Column Observing Network (TCCON).
Air quality and atmospheric deposition in the eastern US: 20 years of change

Data collected in the eastern US between 1990 and 2009 at 34 paired dry and wet monitoring sites are examined. A goal is to evaluate the air quality impacts occurring between 1990 and 2009 that are associated with concurrent legislatively mandated changes in emissions. Four 5-year periods, 1990–1994 (P1), 1995–1999 (P2), 2000–2004 (P3), and 2005–2009 (P4) are considered, with a primary focus on P1-to-P4 changes. Results suggest that legislatively mandated air pollution mitigation strategies have been successful in improving air quality and reducing atmospheric deposition in the eastern US. Respective P1-to-P4 reductions of estimated sulfur dioxide (SO2) and nitrogen oxides (NOx) emissions in the eastern US are 50 and 42%. Corresponding behavior of the following metrics associated with these emissions reductions is examined: monitored atmospheric concentrations of SO2, aerosol sulfate (SO4), and oxidized sulfur (S); dry, wet, and total deposition of S; monitored atmospheric concentrations of nitric acid (HNO3), aerosol nitrate (NO3), and their sum, oxidized nitrogen (OxN); dry, wet, and total deposition of OxN; monitored atmospheric concentration of aerosol ammonium (NH4); dry, wet, and total deposition of NH4; summed monitored atmospheric concentration of oxidized and reduced nitrogen (N); dry, wet, and total deposition of N; wet deposition of hydrogen ion (H+); monitored atmospheric concentration of ozone (O3); dry deposition of O3; and the summed monitored atmospheric concentration of aerosol NO3, SO4, and NH4 (Clean Air Status and Trends Network particulate matter – CASTNET PM). Other metrics (e.g., ratios of dry to total deposition) are also considered. Selected period-to-period changes of air quality and deposition metrics at site, regional, and seasonal scales are discussed. As an example, despite P1-to-P3 reductions in estimated emissions of both SO2 and NOx, aerosol NO3 concentration increased in the east, with widespread wintertime numerical increases in both aerosol NO3 concentration and CASTNET PM. However, a reversal of this behavior is associated with continuing P3-to-P4 reductions of SO2 and NOx emissions. Thus, additional P3-to-P4 reductions of these emissions, especially NOx, appear to have made progress in altering the chemical regime of the wintertime eastern US atmosphere so that future emissions reductions and their resulting reductions in aerosol concentrations may no longer be accompanied by sub-linear changes (or actual increases) in CASTNET PM.
The impact of dust storms on the Arabian Peninsula and the Red Sea

Located in the dust belt, the Arabian Peninsula is a major source of atmospheric dust. Frequent dust outbreaks and some 15 to 20 dust storms per year have profound effects on all aspects of human activity and natural processes in this region. To quantify the effect of severe dust events on radiation fluxes and regional climate characteristics, we simulated the storm that occurred from 18 to 20 March 2012 using a regional weather research forecast model fully coupled with the chemistry/aerosol module (WRF–Chem). This storm swept over a remarkably large area affecting the entire Middle East, northeastern Africa, Afghanistan, and Pakistan. It was caused by a southward propagating cold front, and the associated winds activated the dust production in river valleys of the lower Tigris and Euphrates in Iraq; the coastal areas in Kuwait, Iran, and the United Arab Emirates; the Rub al Khali, An Nafud, and Ad Dahna deserts; and along the Red Sea coast on the west side of the Arabian Peninsula. Our simulation results compare well with available ground-based and satellite observations. We estimate the total amount of dust generated by the storm to have reached 94 Mt. Approximately 78% of this dust was deposited within the calculation domain. The Arabian Sea and Persian Gulf received 5.3 Mt and the Red Sea 1.2 Mt of dust. Dust particles bring nutrients to marine ecosystems, which is especially important for the oligotrophic Northern Red Sea. However, their contribution to the nutrient balance in the Red Sea remains largely unknown. By scaling the effect of one storm to the number of dust storms observed annually over the Red Sea, we estimate the annual dust deposition to the Red Sea, associated with major dust storms, to be 6 Mt.
Elemental ratio measurements of organic compounds using aerosol mass spectrometry: characterization, improved calibration, and implications

Elemental compositions of organic aerosol (OA) particles provide useful constraints on OA sources, chemical evolution, and effects. The Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) is widely used to measure OA elemental composition. This study evaluates AMS measurements of atomic oxygen-to-carbon (O : C), hydrogen-to-carbon (H : C), and organic mass-to-organic carbon (OM : OC) ratios, and of carbon oxidation state (OS C) for a vastly expanded laboratory data set of multifunctional oxidized OA standards. For the expanded standard data set, the method introduced by Aiken et al. (2008), which uses experimentally measured ion intensities at all ions to determine elemental ratios (referred to here as "Aiken-Explicit"), reproduces known O : C and H : C ratio values within 20% (average absolute value of relative errors) and 12%, respectively. The more commonly used method, which uses empirically estimated H2O+ and CO+ ion intensities to avoid gas phase air interferences at these ions (referred to here as "Aiken-Ambient"), reproduces O : C and H : C of multifunctional oxidized species within 28 and 14% of known values. The values from the latter method are systematically biased low, however, with larger biases observed for alcohols and simple diacids. A detailed examination of the H2O+, CO+, and CO2+ fragments in the high-resolution mass spectra of the standard compounds indicates that the Aiken-Ambient method underestimates the CO+ and especially H2O+ produced from many oxidized species. Combined AMS–vacuum ultraviolet (VUV) ionization measurements indicate that these ions are produced by dehydration and decarboxylation on the AMS vaporizer (usually operated at 600 °C). Thermal decomposition is observed to be efficient at vaporizer temperatures down to 200 °C. These results are used together to develop an "Improved-Ambient" elemental analysis method for AMS spectra measured in air. The Improved-Ambient method uses specific ion fragments as markers to correct for molecular functionality-dependent systematic biases and reproduces known O : C (H : C) ratios of individual oxidized standards within 28% (13%) of the known molecular values. The error in Improved-Ambient O : C (H : C) values is smaller for theoretical standard mixtures of the oxidized organic standards, which are more representative of the complex mix of species present in ambient OA. For ambient OA, the Improved-Ambient method produces O : C (H : C) values that are 27% (11%) larger than previously published Aiken-Ambient values; a corresponding increase of 9% is observed for OM : OC values. These results imply that ambient OA has a higher relative oxygen content than previously estimated. The OS C values calculated for ambient OA by the two methods agree well, however (average relative difference of 0.06 OS C units). This indicates that OS C is a more robust metric of oxidation than O : C, likely since OS C is not affected by hydration or dehydration, either in the atmosphere or during analysis.
Seasonal in situ observations of glyoxal and methylglyoxal over the temperate oceans of the Southern Hemisphere

The dicarbonyls glyoxal and methylglyoxal have been measured with 2,4-dinitrophenylhydrazine (2,4-DNPH) cartridges and high-performance liquid chromatography (HPLC), optimised for dicarbonyl detection, in clean marine air over the temperate Southern Hemisphere (SH) oceans. Measurements of a range of dicarbonyl precursors (volatile organic compounds, VOCs) were made in parallel. These are the first in situ measurements of glyoxal and methylglyoxal over the remote temperate oceans. Six 24 h samples were collected in summer (February–March) over the Chatham Rise in the south-west Pacific Ocean during the Surface Ocean Aerosol Production (SOAP) voyage in 2012, while 34 24 h samples were collected at Cape Grim Baseline Air Pollution Station in the late winter (August–September) of 2011. Average glyoxal mixing ratios in clean marine air were 7 ppt at Cape Grim and 23 ppt over Chatham Rise. Average methylglyoxal mixing ratios in clean marine air were 28 ppt at Cape Grim and 10 ppt over Chatham Rise. The mixing ratios of glyoxal at Cape Grim are the lowest observed over the remote oceans, while mixing ratios over Chatham Rise are in good agreement with other temperate and tropical observations, including concurrent Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) observations. Methylglyoxal mixing ratios at both sites are comparable to the only other marine methylglyoxal observations available over the tropical Northern Hemisphere (NH) ocean. Ratios of glyoxal : methylglyoxal > 1 over Chatham Rise but < 1 at Cape Grim suggest that a different formation and/or loss processes or rates dominate at each site. Dicarbonyl precursor VOCs, including isoprene and monoterpenes, are used to calculate an upper-estimate yield of glyoxal and methylglyoxal in the remote marine boundary layer and explain at most 1–3 ppt of dicarbonyls observed, corresponding to 10% and 17% of the observed glyoxal and 29 and 10% of the methylglyoxal at Chatham Rise and Cape Grim, respectively, highlighting a significant but as yet unknown production mechanism. Surface-level glyoxal observations from both sites were converted to vertical columns and compared to average vertical column densities (VCDs) from GOME-2 satellite retrievals. Both satellite columns and in situ observations are higher in summer than winter; however, satellite vertical column densities exceeded the surface observations by more than 1.5 × 1014 molecules cm−2 at both sites. This discrepancy may be due to the incorrect assumption that all glyoxal observed by satellite is within the boundary layer, or it may be due to challenges retrieving low VCDs of glyoxal over the oceans due to interferences by liquid water absorption or the use of an inappropriate normalisation reference value in the retrieval algorithm. This study provides much-needed data to verify the presence of these short-lived gases over the remote ocean and provide further evidence of an as yet unidentified source of both glyoxal and also methylglyoxal over the remote oceans.
Estimation of PM10 concentrations over Seoul using multiple empirical models with AERONET and MODIS data collected during the DRAGON-Asia campaign

The performance of various empirical linear models to estimate the concentrations of surface-level particulate matter with a diameter less than 10 μm (PM10) was evaluated using Aerosol Robotic Network (AERONET) sun photometer and Moderate-Resolution Imaging Spectroradiometer (MODIS) data collected in Seoul during the Distributed Regional Aerosol Gridded Observation Network (DRAGON)-Asia campaign from March to May 2012. An observed relationship between the PM10 concentration and the aerosol optical depth (AOD) was accounted for by several parameters in the empirical models, including boundary layer height (BLH), relative humidity (RH), and effective radius of the aerosol size distribution (Reff), which was used here for the first time in empirical modeling. Among various empirical models, the model which incorporates both BLH and Reff showed the highest correlation, which indicates the strong influence of BLH and Reff on the PM10 estimations. Meanwhile, the effect of RH on the relationship between AOD and PM10 appeared to be negligible during the campaign period (spring), when RH is generally low in northeast Asia. A large spatial dependency of the empirical model performance was found by categorizing the locations of the collected data into three different site types, which varied in terms of the distances between instruments and source locations. When both AERONET and MODIS data sets were used in the PM10 estimation, the highest correlations between measured and estimated values (R = 0.76 and 0.76 using AERONET and MODIS data, respectively) were found for the residential area (RA) site type, while the poorest correlations (R = 0.61 and 0.68 using AERONET and MODIS data, respectively) were found for the near-source (NS) site type. Significant seasonal variations of empirical model performances for PM10 estimation were found using the data collected at Yonsei University (one of the DRAGON campaign sites) over a period of 17 months including the DRAGON campaign period. The best correlation between measured and estimated PM10 concentrations (R = 0.81) was found in winter, due to the presence of a stagnant air mass and low BLH conditions, which may have resulted in relatively homogeneous aerosol properties within the BLH. On the other hand, the poorest correlation between measured and estimated PM10 concentrations (R = 0.54) was found in spring, due to the influence of the long-range transport of dust to both within and above the BLH.
A global non-hydrostatic model study of a downward coupling through the tropical tropopause layer during a stratospheric sudden warming

The dynamical coupling process between the stratosphere and troposphere in the tropical tropopause layer (TTL) during a~stratospheric sudden warming (SSW) in boreal winter was investigated using simulation data from a global non-hydrostatic model (NICAM) that does not use cumulus parameterization. The model reproduced well the observed tropical tropospheric changes during the SSW, including the enhancement of convective activity following the amplification of planetary waves. Deep convective activity was enhanced in the latitude zone 20–10° S, in particular over the southwest Pacific and southwest Indian Ocean. Although the upwelling in the TTL was correlated with that in the stratosphere, the temperature tendency in the TTL changed little due to a compensation by diabatic heating originating from cloud formation. This result suggests that the stratospheric meridional circulation affects cloud formation in the TTL.
Development towards a global operational aerosol consensus: basic climatological characteristics of the International Cooperative for Aerosol Prediction Multi-Model Ensemble (ICAP-MME)

Here we present the first steps in developing a global multi-model aerosol forecasting ensemble intended for eventual operational and basic research use. Drawing from members of the International Cooperative for Aerosol Prediction (ICAP) latest generation of quasi-operational aerosol models, 5-day aerosol optical thickness (AOT) forecasts are analyzed for December 2011 through November 2012 from four institutions: European Centre for Medium-Range Weather Forecasts (ECMWF), Japan Meteorological Agency (JMA), NASA Goddard Space Flight Center (GSFC), and Naval Research Lab/Fleet Numerical Meteorology and Oceanography Center (NRL/FNMOC). For dust, we also include the National Oceanic and Atmospheric Administration-National Geospatial Advisory Committee (NOAA NGAC) product in our analysis. The Barcelona Supercomputing Centre and UK Met Office dust products have also recently become members of ICAP, but have insufficient data to be included in this analysis period. A simple consensus ensemble of member and mean AOT fields for modal species (e.g., fine and coarse mode, and a separate dust ensemble) is used to create the ICAP Multi-Model Ensemble (ICAP-MME). The ICAP-MME is run daily at 00:00 UTC for 6-hourly forecasts out to 120 h. Basing metrics on comparisons to 21 regionally representative Aerosol Robotic Network (AERONET) sites, all models generally captured the basic aerosol features of the globe. However, there is an overall AOT low bias among models, particularly for high AOT events. Biomass burning regions have the most diversity in seasonal average AOT. The Southern Ocean, though low in AOT, nevertheless also has high diversity. With regard to root mean square error (RMSE), as expected the ICAP-MME placed first over all models worldwide, and was typically first or second in ranking against all models at individual sites. These results are encouraging; furthermore, as more global operational aerosol models come online, we expect their inclusion in a robust operational multi-model ensemble will provide valuable aerosol forecasting guidance.
Simulations of atmospheric methane for Cape Grim, Tasmania, to constrain southeastern Australian methane emissions

This study uses two climate models and six scenarios of prescribed methane emissions to compare modelled and observed atmospheric methane between 1994 and 2007, for Cape Grim, Australia (40.7° S, 144.7° E). The model simulations follow the TransCom-CH4 protocol and use the Australian Community Climate and Earth System Simulator (ACCESS) and the CSIRO Conformal-Cubic Atmospheric Model (CCAM). Radon is also simulated and used to reduce the impact of transport differences between the models and observations. Comparisons are made for air samples that have traversed the Australian continent. All six emission scenarios give modelled concentrations that are broadly consistent with those observed. There are three notable mismatches, however. Firstly, scenarios that incorporate interannually varying biomass burning emissions produce anomalously high methane concentrations at Cape Grim at times of large fire events in southeastern Australia, most likely due to the fire methane emissions being unrealistically input into the lowest model level. Secondly, scenarios with wetland methane emissions in the austral winter overestimate methane concentrations at Cape Grim during wintertime while scenarios without winter wetland emissions perform better. Finally, all scenarios fail to represent a~methane source in austral spring implied by the observations. It is possible that the timing of wetland emissions in the scenarios is incorrect with recent satellite measurements suggesting an austral spring (September–October–November), rather than winter, maximum for wetland emissions.