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Impact of data quality and surface-to-column representativeness on the PM2.5 / satellite AOD relationship for the contiguous United States

Satellite-derived aerosol optical depth (AOD) observations have been used to estimate particulate matter smaller than 2.5 μm (PM2.5). However, such a relationship could be affected by the representativeness of satellite-derived AOD to surface aerosol particle mass concentration and satellite AOD data quality. Using purely measurement-based methods, we have explored the impacts of data quality and representativeness on the AOD-inferred PM2.5 / AOD relationship for the contiguous United States (CONUS). This is done through temporally and spatially collocated data sets of PM2.5 and AOD retrievals from Aqua/Terra Moderate Resolution Imaging Spectroradiometer (MODIS), Multi-angle Imaging Spectroradiometer (MISR), and Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP). These analyses show that improving data quality of satellite AOD, such as done with data assimilation-grade retrievals, increases their correlation with PM2.5. However, overall correlation is relatively low across the CONUS. Also, integrated extinction observed within 500 m above ground level (a.g.l.), as measured by CALIOP, is not well representative of the total column AOD. Surface aerosol in the eastern CONUS is better correlated with total column AOD than in the western CONUS. The best correlation values are found for estimated dry mass CALIOP extinction at 200–300 m a.g.l. and PM2.5, but additional work is needed to address the ability of using actively sensed AOD as a proxy for PM2.5 concentrations.
Impact of tropical land convection on the water vapour budget in the tropical tropopause layer

The tropical deep overshooting convection is known to be most intense above continental areas such as South America, Africa, and the maritime continent. However, its impact on the tropical tropopause layer (TTL) at global scale remains debated. In our analysis, we use the 8-year Microwave Limb Sounder (MLS) water vapour (H2O), cloud ice-water content (IWC), and temperature data sets from 2005 to date, to highlight the interplays between these parameters and their role in the water vapour variability in the TTL, and separately in the northern and southern tropics. In the tropical upper troposphere (177 hPa), continents, including the maritime continent, present the night-time (01:30 local time, LT) peak in the water vapour mixing ratio characteristic of the H2O diurnal cycle above tropical land. The western Pacific region, governed by the tropical oceanic diurnal cycle, has a daytime maximum (13:30 LT). In the TTL (100 hPa) and tropical lower stratosphere (56 hPa), South America and Africa differ from the maritime continent and western Pacific displaying a daytime maximum of H2O. In addition, the relative amplitude between day and night is found to be systematically higher by 5–10% in the southern tropical upper troposphere and 1–3% in the TTL than in the northern tropics during their respective summer, indicative of a larger impact of the convection on H2O in the southern tropics. Using a regional-scale approach, we investigate how mechanisms linked to the H2O variability differ in function of the geography. In summary, the MLS water vapour and cloud ice-water observations demonstrate a clear contribution to the TTL moistening by ice crystals overshooting over tropical land regions. The process is found to be much more effective in the southern tropics. Deep convection is responsible for the diurnal temperature variability in the same geographical areas in the lowermost stratosphere, which in turn drives the variability of H2O.
Assimilation of atmospheric methane products into the MACC-II system: from SCIAMACHY to TANSO and IASI

The Monitoring Atmospheric Composition and Climate Interim Implementation (MACC-II) delayed-mode (DM) system has been producing an atmospheric methane (CH4) analysis 6 months behind real time since June 2009. This analysis used to rely on the assimilation of the CH4 product from the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) instrument onboard Envisat. Recently the Laboratoire de Météorologie Dynamique (LMD) CH4 products from the Infrared Atmospheric Sounding Interferometer (IASI) and the SRON Netherlands Institute for Space Research CH4 products from the Thermal And Near-infrared Sensor for carbon Observation (TANSO) were added to the DM system. With the loss of Envisat in April 2012, the DM system now has to rely on the assimilation of methane data from TANSO and IASI. This paper documents the impact of this change in the observing system on the methane tropospheric analysis. It is based on four experiments: one free run and three analyses from respectively the assimilation of SCIAMACHY, TANSO and a combination of TANSO and IASI CH4 products in the MACC-II system. The period between December 2010 and April 2012 is studied. The SCIAMACHY experiment globally underestimates the tropospheric methane by 35 part per billion (ppb) compared to the HIAPER Pole-to-Pole Observations (HIPPO) data and by 28 ppb compared the Total Carbon Column Observing Network (TCCON) data, while the free run presents an underestimation of 5 ppb and 1 ppb against the same HIPPO and TCCON data, respectively. The assimilated TANSO product changed in October 2011 from version v.1 to version v.2.0. The analysis of version v.1 globally underestimates the tropospheric methane by 18 ppb compared to the HIPPO data and by 15 ppb compared to the TCCON data. In contrast, the analysis of version v.2.0 globally overestimates the column by 3 ppb. When the high density IASI data are added in the tropical region between 30° N and 30° S, their impact is mainly positive but more pronounced and effective when combined with version v.2.0 of the TANSO products. The resulting analysis globally underestimates the column-averaged dry-air mole fractions of methane (xCH4) just under 1 ppb on average compared to the TCCON data, whereas in the tropics it overestimates xCH4 by about 3 ppb. The random error is estimated to be less than 7 ppb when compared to TCCON data.
Emissions of organic aerosol mass, black carbon, particle number, and regulated and unregulated gases from scooters and light and heavy duty vehicles with different fuels

A sampling campaign with seven different types of vehicles was conducted in 2009 at the vehicle test facilities of the Joint Research Centre (JRC) in Ispra (Italy). The vehicles chosen were representative of some categories circulating in Europe and were fueled either with standard gasoline or diesel and some with blends of rapeseed methyl ester biodiesel. The aim of this work was to improve the knowledge about the emission factors of gas phase and particle-associated regulated and unregulated species from vehicle exhaust. Unregulated species such as black carbon (BC), primary organic aerosol (OA) content, particle number (PN), monocyclic and polycyclic aromatic hydrocarbons (PAHs) and a~selection of unregulated gaseous compounds, including nitrous acid (N2O), ammonia (NH3), hydrogen cyanide (HCN), formaldehyde (HCHO), acetaldehyde (CH3CHO), sulfur dioxide (SO2), and methane (CH4), were measured in real time with a suite of instruments including a high-resolution aerosol time-of-flight mass spectrometer, a resonance enhanced multi-photon ionization time-of-flight mass spectrometer, and a high resolution Fourier transform infrared spectrometer. Diesel vehicles, without particle filters, featured the highest values for particle number, followed by gasoline vehicles and scooters. The particles from diesel and gasoline vehicles were mostly made of BC with a low fraction of OA, while the particles from the scooters were mainly composed of OA. Scooters were characterized by super high emissions factors for OA, which were orders of magnitude higher than for the other vehicles. The heavy duty diesel vehicle (HDDV) featured the highest nitrogen oxides (NOx) emissions, while the scooters had the highest emissions for total hydrocarbons and aromatic compounds due to the unburned and partially burned gasoline and lubricant oil mixture. Generally, vehicles fuelled with biodiesel blends showed lower emission factors of OA and total aromatics than those from the standard fuels. The scooters were the main emitters of aromatic compounds, followed by the gasoline vehicle, the diesel vehicles and the HDDV.
Tropospheric aerosol scattering and absorption over central Europe: a closure study for the dry particle state

This work analyses optical properties of the dry tropospheric aerosol measured at the regional Global Atmosphere Watch (GAW) observation site Melpitz in East Germany. For a continuous observation period between 2007 and 2010, we provide representative values of the dry-state scattering coefficient, hemispheric backscattering coefficient, absorption coefficient, single scattering albedo, and scattering Ångström exponent. Besides the direct measurement, the aerosol scattering coefficient was alternatively computed from experimental particle number size distributions using a Mie model. Within pre-defined limits, a closure could be achieved with the direct measurement. The achievement of closure implies that such calculations can be used as a high-level quality control measure for data sets involving multiple instrumentation. All dry-state optical properties show pronounced annual and diurnal variations, which are attributed to the corresponding variations in the regional emission fluxes, the intensity of secondary particle formation, and the mixing layer height. Air mass classification shows that atmospheric stability is a major factor influencing the dry aerosol properties at the GAW station. In the cold season, temperature inversions limit the volume available for atmospheric mixing, so that the dry-state aerosol optical properties near the ground proved quite sensitive to the geographical origin of the air mass. In the warm season, when the atmosphere is usually well-mixed during daytime, considerably less variability was observed for the optical properties between different air masses. This work provides, on the basis of quality-checked in situ measurements, a first step towards a climatological assessment of direct aerosol radiative forcing in the region under study.
10-year spatial and temporal trends of PM2.5 concentrations in the southeastern US estimated using high-resolution satellite data

Long-term PM2.5 exposure has been associated with various adverse health outcomes. However, most ground monitors are located in urban areas, leading to a potentially biased representation of true regional PM2.5 levels. To facilitate epidemiological studies, accurate estimates of the spatiotemporally continuous distribution of PM2.5 concentrations are important. Satellite-retrieved aerosol optical depth (AOD) has been increasingly used for PM2.5 concentration estimation due to its comprehensive spatial coverage. Nevertheless, previous studies indicated that an inherent disadvantage of many AOD products is their coarse spatial resolution. For instance, the available spatial resolutions of the Moderate Resolution Imaging Spectroradiometer (MODIS) and the Multiangle Imaging SpectroRadiometer (MISR) AOD products are 10 and 17.6 km, respectively. In this paper, a new AOD product with 1 km spatial resolution retrieved by the multi-angle implementation of atmospheric correction (MAIAC) algorithm based on MODIS measurements was used. A two-stage model was developed to account for both spatial and temporal variability in the PM2.5–AOD relationship by incorporating the MAIAC AOD, meteorological fields, and land use variables as predictors. Our study area is in the southeastern US centered at the Atlanta metro area, and data from 2001 to 2010 were collected from various sources. The model was fitted annually, and we obtained model fitting R2 ranging from 0.71 to 0.85, mean prediction error (MPE) from 1.73 to 2.50 μg m−3, and root mean squared prediction error (RMSPE) from 2.75 to 4.10 μg m−3. In addition, we found cross-validation R2 ranging from 0.62 to 0.78, MPE from 2.00 to 3.01 μg m−3, and RMSPE from 3.12 to 5.00 μg m−3, indicating a good agreement between the estimated and observed values. Spatial trends showed that high PM2.5 levels occurred in urban areas and along major highways, while low concentrations appeared in rural or mountainous areas. Our time-series analysis showed that, for the 10-year study period, the PM2.5 levels in the southeastern US have decreased by ~20%. The annual decrease has been relatively steady from 2001 to 2007 and from 2008 to 2010 while a significant drop occurred between 2007 and 2008. An observed increase in PM2.5 levels in year 2005 is attributed to elevated sulfate concentrations in the study area in warm months of 2005.
Sensitivity analysis of an updated bidirectional air–surface exchange model for elemental mercury vapor

A box model for estimating bidirectional air–surface exchange of gaseous elemental mercury (Hg0) has been updated based on the latest understanding of the resistance scheme of atmosphere–biosphere interface transfer. Simulations were performed for two seasonal months to evaluate diurnal and seasonal variation. The base-case results show that water and soil surfaces are net sources, while vegetation is a net sink of Hg0. The estimated net exchange in a domain covering the contiguous US and part of Canada and Mexico is 38.4 and 56.0 Mg as evasion in the summer and winter month, respectively. The smaller evasion in summer is due to the stronger Hg0 uptake by vegetation. Modeling experiments using a two-level factorial design were conducted to examine the sensitivity of flux response to the changes in physical and environmental parameters in the model. It is shown that atmospheric shear flows (surface wind over water and friction velocity over terrestrial surfaces), dissolved gaseous mercury (DGM) concentration, soil organic and Hg content, and air temperature are the most influential factors. The positive effect of friction velocity and soil Hg content on the evasion flux from soil and canopy can be effectively offset by the negative effect of soil organic content. Significant synergistic effects are identified between surface wind and DGM level for water surface, and between soil Hg content and friction velocity for soil surface, leading to ~50% enhanced flux compared to the sum of their individual effects. The air–foliage exchange is mainly controlled by surface resistance terms influenced by solar irradiation and air temperature. Research in providing geospatial distribution of Hg in water and soil will greatly improve the flux estimate. Elucidation on the kinetics and mechanism of Hg(II) reduction in soil/water and quantification of the surface resistances specific to Hg species will also help reduce the model uncertainty.
Analysis of transpacific transport of black carbon during HIPPO-3: implications for black carbon aging

Long-range transport of black carbon (BC) is a growing concern as a result of the efficiency of BC in warming the climate and its adverse impact on human health. We study transpacific transport of BC during HIPPO-3 using a combination of inverse modeling and sensitivity analysis. We use the GEOS-Chem chemical transport model and its adjoint to constrain Asian BC emissions and estimate the source of BC over the North Pacific. We find that different sources of BC dominate the transport to the North Pacific during the southbound (29 March 2010) and northbound (13 April 2010) measurements in HIPPO-3. While biomass burning in Southeast Asia (SE) contributes about 60% of BC in March, more than 90% of BC comes from fossil fuel and biofuel combustion in East Asia (EA) during the April mission. GEOS-Chem simulations generally resolve the spatial and temporal variation of BC concentrations over the North Pacific, but are unable to reproduce the low and high tails of the observed BC distribution. We find that the optimized BC emissions derived from inverse modeling fail to improve model simulations significantly. This failure indicates that uncertainties in BC removal as well as transport, rather than in emissions, account for the major biases in GEOS-Chem simulations of BC over the North Pacific. The aging process, transforming BC from hydrophobic into hydrophilic form, is one of the key factors controlling wet scavenging and remote concentrations of BC. Sensitivity tests on BC aging (ignoring uncertainties of other factors controlling BC long range transport) suggest that in order to fit HIPPO-3 observations, the aging timescale of anthropogenic BC from EA may be several hours (faster than assumed in most global models), while the aging process of biomass burning BC from SE may occur much slower, with a timescale of a few days. To evaluate the effects of BC aging and wet deposition on transpacific transport of BC, we develop an idealized model of BC transport. We find that the mid-latitude air masses sampled during HIPPO-3 may have experienced a series of precipitation events, particularly near the EA and SE source region. Transpacific transport of BC is sensitive to BC aging when the aging rate is fast; this sensitivity peaks when the aging timescale is in the range of 1–1.5 d. Our findings indicate that BC aging close to the source must be simulated accurately at a process level in order to simulate better the global abundance and climate forcing of BC.
Monitoring high-ozone events in the US Intermountain West using TEMPO geostationary satellite observations

High-ozone events, approaching or exceeding the National Ambient Air Quality Standard (NAAQS), are frequently observed in the US Intermountain West in association with subsiding air from the free troposphere. Monitoring and attribution of these events is problematic because of the sparsity of the current network of surface measurements and lack of vertical information. We present an Observing System Simulation Experiment (OSSE) to evaluate the ability of the future geostationary satellite instrument Tropospheric Emissions: Monitoring of Pollution (TEMPO), scheduled for launch in 2018–2019, to monitor and attribute high-ozone events in the Intermountain West through data assimilation. TEMPO will observe ozone in the ultraviolet (UV) and visible (Vis) bands to provide sensitivity in the lower troposphere. Our OSSE uses ozone data from the GFDL AM3 chemistry-climate model (CCM) as the "true" atmosphere and samples it for April–June 2010 with the current surface network (CASTNet –Clean Air Status and Trends Network– sites), a configuration designed to represent TEMPO, and a low Earth orbit (LEO) IR (infrared) satellite instrument. These synthetic data are then assimilated into the GEOS-Chem chemical transport model (CTM) using a Kalman filter. Error correlation length scales (500 km in horizontal, 1.7 km in vertical) extend the range of influence of observations. We show that assimilation of surface data alone does not adequately detect high-ozone events in the Intermountain West. Assimilation of TEMPO data greatly improves the monitoring capability, with little information added from the LEO instrument. The vertical information from TEMPO further enables the attribution of NAAQS exceedances to background ozone. This is illustrated with the case of a stratospheric intrusion.
Environmental influences on the intensity changes of tropical cyclones over the western North Pacific

The influence of environmental conditions on the intensity changes of tropical cyclones (TCs) over the western North Pacific (WNP) is investigated through examination of 37 TCs during 2000–2011 that interacted directly with the western North Pacific subtropical high (WNPSH). Comprehensive composite analysis of the environmental conditions is performed for two stages of storms: one is categorized as intensifying events (maximum wind speed increases by 15 kn over 48 h) and the other is categorized as weakening events (maximum wind speed decreases by 15 kn over 48 h). Comparison of the composite analysis of these two cases show that environmental conditions associated with the WNPSH play important roles in the intensity changes of TCs over the WNP. When a TC moves along the southern periphery of the WNPSH, the relatively weaker easterly environmental vertical wind shear helps bring warm moist air from the south and southeast to its southeast quadrant within 500 km, which is favorable for the TC to intensify. However, when a TC moves along the western edge of the WNPSH, under the combined influences of the WNPSH and an upper-level westerly trough, a strong westerly vertical shear promotes the intrusion of dry environmental air associated with the WNPSH from the north and northwest, which may lead to the inhibition of moisture supply and convection over the western half of the TC and thus its weakening. These composite results are consistent with those with additional geographic restrictions, suggesting that the dry air intrusion and the vertical wind shear (VWS) associated with the WNPSH, indeed affect the intensity changes of TCs over the WNP beyond the difference related solely to variations in geographical locations. The average sea surface temperature (SST) of 27.6 °C for the weakening events is also lower than an average of 28.9 °C for the strengthening events, but remains above the critical value of 27 °C for TC intensification, suggesting that the SST may be regarded as a less positive factor for the weakening events.