ALBERT

Description: With the improved spatial resolution of the Ozone Monitoring Instrument (OMI) over earlier instruments and more than 10 years of service, tropospheric NO2 retrievals from OMI have led to many influential studies on the relationships between socioeconomic activities and NOx emissions. Previous studies have shown that the OMI NO2 data show different relative trends compared to in situ measurements. However, the sources of the discrepancies need further investigations. This study focuses on how to appropriately compare relative trends derived from OMI and in situ measurements. We retrieve OMI tropospheric NO2 vertical column densities (VCDs) and obtain the NO2 seasonal trends over the United States, which are compared with coincident in situ surface NO2 measurements from the Air Quality System (AQS) network. The Mann–Kendall method with Sen's slope estimator is applied to derive the NO2 seasonal and annual trends for four regions at coincident sites during 2005–2014. The OMI-based NO2 seasonal relative decreasing trends are generally biased low compared to the in situ trends by up to 3.7 % yr−1, except for the underestimation in the US Midwest and Northeast during December, January, and February (DJF). We improve the OMI retrievals for trend analysis by removing the ocean trend, using the Moderate Resolution Imaging Spectroradiometer (MODIS) albedo data in air mass factor (AMF) calculation. We apply a lightning flash filter to exclude lightning-affected data to make proper comparisons. These data processing procedures result in close agreement (within 0.3 % yr−1) between in situ and OMI-based NO2 regional annual relative trends. The remaining discrepancies may result from inherent difference between trends of NO2 tropospheric VCDs and surface concentrations, different spatial sampling of the measurements, chemical nonlinearity, and tropospheric NO2 profile changes. We recommend that future studies apply these procedures (ocean trend removal and MODIS albedo update) to ensure the quality of satellite-based NO2 trend analysis and apply the lightning filter in studying surface NOx emission changes using satellite observations and in comparison with the trends derived from in situ NO2 measurements. With these data processing procedures, we derive OMI-based NO2 regional annual relative trends using all available data for the US West (−2.0 % ± 0.3 yr−1), Midwest (−1.8 % ± 0.4 yr−1), Northeast (−3.1 % ± 0.5 yr−1), and South (−0.9 % ± 0.3 yr−1). The OMI-based annual mean trend over the contiguous United States is −1.5 % ± 0.2 yr−1. It is a factor of 2 lower than that of the AQS in situ data (−3.9 % ± 0.4 yr−1); the difference is mainly due to the fact that the locations of AQS sites are concentrated in urban and suburban regions.

Description: Long-range transport followed by deposition of black carbon on glaciers of Tibet is one of the key issues of climate research as it induces changes on radiative forcing and subsequently impacting the melting of glaciers. The transport mechanism, however, is not well understood. In this study, we use short-lived reactive aromatics as proxies to diagnose transport of pollutants to Tibet. In situ observations of short-lived reactive aromatics across the Tibetan Plateau are analyzed using a regional chemistry and transport model. The model performance using the current emission inventories over the region is poor due to problems in the inventories and model transport. Top-down emissions constrained by satellite observations of glyoxal are a factor of 2–6 higher than the a priori emissions over the industrialized Indo-Gangetic Plain. Using the top-down emissions, agreement between model simulations and surface observations of aromatics improves. We find enhancements of reactive aromatics over Tibet by a factor of 6 on average due to rapid transport from India and nearby regions during the presence of a high-altitude cut-off low system. Our results suggest that the cut-off low system is a major pathway for long-range transport of pollutants such as black carbon. The modeling analysis reveals that even the state-of-the-science high-resolution reanalysis cannot simulate this cut-off low system accurately, which probably explains in part the underestimation of black carbon deposition over Tibet in previous modeling studies. Another model deficiency of underestimating pollution transport from the south is due to the complexity of terrain, leading to enhanced transport. It is therefore challenging for coarse-resolution global climate models to properly represent the effects of long-range transport of pollutants on the Tibetan environment and the subsequent consequence for regional climate forcing.

Description: Recent studies have revealed a significant influx of anthropogenic aerosol from South Asia to the Himalayas and Tibetan Plateau (TP) during pre-monsoon period. In order to characterize the chemical composition, sources, and transport processes of aerosol in this area, we carried out a field study during June 2015 by deploying a suite of online instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) and a multi-angle absorption photometer (MAAP) at Nam Co station (90∘57′ E, 30∘46′ N; 4730 m a.s.l.) at the central of the TP. The measurements were made at a period when the transition from pre-monsoon to monsoon occurred. The average ambient mass concentration of submicron particulate matter (PM1) over the whole campaign was ∼ 2.0 µg m−3, with organics accounting for 68 %, followed by sulfate (15 %), black carbon (8 %), ammonium (7 %), and nitrate (2 %). Relatively higher aerosol mass concentration episodes were observed during the pre-monsoon period, whereas persistently low aerosol concentrations were observed during the monsoon period. However, the chemical composition of aerosol during the higher aerosol concentration episodes in the pre-monsoon season was on a case-by-case basis, depending on the prevailing meteorological conditions and air mass transport routes. Most of the chemical species exhibited significant diurnal variations with higher values occurring during afternoon and lower values during early morning, whereas nitrate peaked during early morning in association with higher relative humidity and lower air temperature. Organic aerosol (OA), with an oxygen-to-carbon ratio (O ∕ C) of 0.94, was more oxidized during the pre-monsoon period than during monsoon (average O ∕ C ratio of 0.72), and an average O ∕ C was 0.88 over the entire campaign period, suggesting overall highly oxygenated aerosol in the central TP. Positive matrix factorization of the high-resolution mass spectra of OA identified two oxygenated organic aerosol (OOA) factors: a less oxidized OOA (LO-OOA) and a more oxidized OOA (MO-OOA). The MO-OOA dominated during the pre-monsoon period, whereas LO-OOA dominated during monsoon. The sensitivity of air mass transport during pre-monsoon with synoptic process was also evaluated with a 3-D chemical transport model.

Description: Emission datasets of nitrogen oxides (NOx) at high horizontal resolutions (e.g., 0.05∘×0.05∘) are crucial for understanding human influences at fine scales, air quality studies, and pollution control. Yet high-resolution emission data are often missing or contain large uncertainties especially for the developing regions. Taking advantage of long-term satellite measurements of nitrogen dioxide (NO2), here we develop a computationally efficient method of estimating NOx emissions in major urban areas at the 0.05∘×0.05∘ resolution. The top-down inversion method accounts for the nonlinear effects of horizontal transport, chemical loss, and deposition. We construct a two-dimensional Peking University High-resolution Lifetime-Emission-Transport model (PHLET), its adjoint model (PHLET-A), and a satellite conversion matrix approach to relate emissions, lifetimes, simulated NO2, and satellite NO2 data. The inversion method is applied to the summer months of 2012–2015 in the Yangtze River Delta (YRD; 29–34∘ N, 118–123∘ E) area, a major polluted region of China, using the NO2 vertical column density data from the Peking University Ozone Monitoring Instrument NO2 product (POMINO). A systematic analysis of inversion errors is performed, including using an independent test based on GEOS-Chem simulations. Across the YRD area, the summer average emissions obtained in this work range from 0 to 15.3 kg km−2 h−1, and the lifetimes (due to chemical loss and deposition) range from 0.6 to 3.3 h. Our emission dataset reveals fine-scale spatial information related to nighttime light, population density, road network, maritime shipping, and land use (from a Google Earth photo). We further compare our emissions with multiple inventories. Many of the fine-scale emission structures are not well represented or not included in the widely used Multi-scale Emissions Inventory of China (MEIC).

Description: Long-range transport and subsequent deposition of black carbon on glaciers of Tibet is one of the key issues of climate research inducing changes on radiative forcing and subsequently impacting on the melting of glaciers. The transport mechanism, however, is not well understood. In this study, we use short-lived reactive aromatics as proxies to diagnose transport of pollutants to Tibet. In situ observations of short-lived reactive aromatics across the Tibetan Plateau are analyzed using a regional chemistry and transport model. The model performance using the current emission inventories over the region is poor due to problems in the inventories and model transport. Top-down emissions constrained by satellite observations of glyoxal (CHOCHO) are a factor of 2–6 higher than the a priori emissions over the industrialized Indo-Gangetic Plain. Using the top-down emissions, agreement between model simulations and surface observations of aromatics improves. We find enhancements of reactive aromatics over Tibet by a factor of 6 on average due to rapid transport from India and nearby regions during the presence of a high-altitude cut-off low system. Our results suggest that the cut-off low system is a major pathway for long-range transport of pollutants such as black carbon. The modeling analysis reveals that even the state-of-the-science high-resolution reanalysis cannot simulate this cut-off low system accurately, which probably explains in part the underestimation of black carbon deposition over Tibet in previous modeling studies. Furthermore, another model deficiency of underestimating pollution transport from the south is due to the complexity of terrain, leading to enhanced transport. It is therefore challenging for coarse-resolution global climate models to properly represent the effects of long-range transport of pollutants on the Tibetan environment and the subsequent consequence for regional climate forcing.

Description: With the improved spatial resolution than earlier instruments and more than ten years of service, tropospheric NO2 retrievals from the Ozone Monitoring Instrument (OMI) have led to many influential studies on the relationships between socioeconomic activities and NOx emissions. This study focuses on how to improve OMI NO2 retrievals for more reliable trend analysis. We retrieve OMI tropospheric NO2 vertical column densities (VCDs) and obtain the NO2 seasonal trends over the United States, which are compared with coincident in situ surface NO2 measurements from the Air Quality System (AQS) network. The Mann-Kendall method is applied to derive the NO2 seasonal and annual trends for four regions at coincident sites during 2005–2014. The OMI-based NO2 seasonal relative trends are generally biased high compared to the in situ trends by up to 3.7 % yr−1, except for the underestimation in the Midwest and Northeast during Dec–Jan–Feb (DJF). We improve the OMI retrievals for trend analysis by removing the ocean trend, using the MODerate-resolution Imaging Spectroradiometer (MODIS) albedo data in air mass factor (AMF) calculation, and applying a lightning flash filter to exclude lightning affected OMI NO2 retrievals. These improvements result in close agreement (within 0.3 % yr−1) between in situ and OMI-based NO2 regional annual relative trends. Thus, we recommend future studies to apply these procedures to ensure the quality of satellite-based NO2 trend analysis, especially in regions without reliable long-term in situ NO2 measurements. We derive optimized OMI-based NO2 regional annual relative trends using all available data for the West (−2.0 % ± 0.3 yr−1), the Midwest (−1.8 % ± 0.4 yr−1), the Northeast (−3.1 % ± 0.5 yr−1), and the South (−0.9 % ± 0.3 yr−1). The OMI-based annual mean trend over the contiguous United States is −1.5 % ± 0.2 yr−1. It is a factor of 2 lower than that of the AQS in situ data (−3.9 % ± 0.4 yr−1); the difference is mainly due to the fact that the locations of AQS sites are concentrated in urban and suburban regions.

Description: Recent studies have revealed a significant influx of air pollution from south Asia to Himalayas and Tibet Plateau (TP) during pre-monsoon period. In order to characterize the chemical composition, sources, and transport mechanism of polluted air mass in this pristine area, we performed a field study during June 2015 by deploying a suite of online instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) and a multi-angle absorption photometer (MAAP) at Nam Co Station (90°57' E, 30°46 ' N 4730 m a.s.l.) at the central of the TP. The measurements were made at a time when the transition from pre-monsoon to monsoon occurred. The average ambient mass concentration of submicron particulate matter (PM1) over the whole campaign period was 2.0 µg m−3, with organics accounting for 64 %, followed by sulfate (16 %), black carbon (9 %), ammonium (8 %), and nitrate (3 %). This mass loading and composition were comparable with most of AMS results in remote sites worldwide. Air pollution episodes were observed during the pre-monsoon period, while consistently low aerosol concentrations were observed during the monsoon period. However, the chemical composition of aerosol during the air pollution episodes in the pre-monsoon season was on a case-by-case basis, depending on the prevailing meteorological conditions and air mass transport routes. Most of the chemical species exhibited significant diurnal variations with higher values occurring during afternoon and lower values during early morning time whereas nitrate peaked during early morning in association with higher relative humidity and lower air temperature. Organic aerosol (OA) was more oxidized with an oxygen-to-carbon ratio (O / C) of 0.94 during the pre-monsoon period than during monsoon (average O / C of 0.48). The average O / C of OA was 0.88 over the entire campaign period. Positive matrix factorization of the high resolution mass spectra of OA identified two oxygenated organic aerosol (OOA) factors: a less oxidized OOA (LO-OOA) and a more oxidized OOA (MO-OOA). The MO-OOA dominated during the pre-monsoon period, while LO-OOA dominated during the monsoon. The sensitivity of air pollution transport with synoptic process was also evaluated with a 3-D chemical transport model.

Description: Emission datasets of nitrogen oxides (NOx) at high horizontal resolutions (e.g., 0.05° × 0.05°) are crucial for understanding human influences at fine scales, air quality studies, and pollution control. Yet high-resolution emission data are often lacking or contain large uncertainties especially for the developing regions. Taking advantage of long-term satellite measurements of nitrogen dioxide (NO2), here we develop a computationally efficient method to inverting NOx emissions in major urban areas at the 0.05° × 0.05° resolution. The inversion accounts for the nonlinear effects of horizontal transport, chemical loss, and deposition. We construct a 2-dimensional Peking University High-resolution Lifetime-Emission-Transport (PHLET) model, its adjoint model (PHLET-A), and a Satellite Conversion Metrix approach to relate emissions, simulated NO2, and satellite NO2 data. The inversion method is applied to summer months of 2012–2016 in the Yangtze River Delta area (YRD, 118 °E–123 °E, 29 °N–34 °N), a major polluted region of China, using the POMINO NO2 vertical column density product retrieved from the Ozone Monitoring Instrument. A systematic analysis of inversion errors is performed, including using an Observing System Simulation Experiment-like test. Across the YRD area, the inverted summer average emission ranges from 0 to 12.0 kg km−2 h−1, and the lifetime (due to chemical loss and deposition) from 1.4 to 3.6 h. Our inverted emission dataset reveals fine-scale spatial information tied to nighttime light, population density, road network, and maritime shipping. Many of the inverted fine-scale emission features are not well represented or not included in the widely used Multi-scale Emissions Inventory of China. Our inversion method can be applied to other regions and other satellite sensors such as the TROPOspheric Monitoring Instrument.

Description: Gas flaring is a commonly used practice in the oil and gas sector that leads to key air pollutant and greenhouse gas emissions. Here we use multipollutant (NO 2 , SO 2 ) satellite observations from 2005 to 2017 to quantify gas flaring activity in Mexico's offshore production cluster, which produces ~50–70% of the country's oil and is among the world's largest oil fields. We estimate annual flared gas volume ranging from 5.5 to 20 × 10 9  m 3 over the Mexican offshore corresponding to 〉40% associated gas production, which is significantly larger than for instance offshore United States where reportedly 〈3% of associated gas is flared. The 13-year record of satellite-derived gas flaring indicates a drastic increase until 2008 and a decline afterward. While the increased flaring is associated with efforts to enhance oil production, the post-2008 decline is linked to an expanding capacity of associated gas utilization, providing a continuing opportunity to reduce flaring for environmental and economic benefits. ©2019. The Authors.