ALBERT

Description: We present a new product with explicit aerosol corrections, POMINO-TROPOMI, for tropospheric nitrogen dioxide (NO2) vertical column densities (VCDs) over East Asia, based on the newly launched TROPOspheric Monitoring Instrument with an unprecedented high horizontal resolution. Compared to the official TM5-MP-DOMINO (OFFLINE) product, POMINO-TROPOMI shows stronger concentration gradients near emission source locations and better agrees with MAX-DOAS measurements (R2=0.75; NMB=0.8 % versus R2=0.68, NMB=-41.9 %). Sensitivity tests suggest that implicit aerosol corrections, as in TM5-MP-DOMINO, lead to underestimations of NO2 columns by about 25 % over the polluted northern East China region. Reducing the horizontal resolution of a priori NO2 profiles would underestimate the retrieved NO2 columns over isolated city clusters in western China by 35 % but with overestimates of more than 50 % over many offshore coastal areas. The effect of a priori NO2 profiles is more important under calm conditions.

Description: China is facing a severe ozone problem, but the origin of its ozone remains unclear. Here we use a GEOS-Chem based global–regional two-way coupled model system to quantify the individual contributions of eight emission source regions worldwide to springtime ozone in 2008 over China. The model reproduces the observed ozone from 31 ground sites and various aircraft and ozonesonde measurements in China and nearby countries, with a mean bias of 10 %–15 % both near the surface and in the troposphere. We then combine zero-out simulations, tagged ozone simulations, and a linear weighting approach to account for the effect of nonlinear chemistry on ozone source attribution. We find considerable contributions of total foreign anthropogenic emissions to surface ozone over China (2–11 ppb). For ozone of anthropogenic origin averaged over China, foreign regions together contribute 40 %–60 % below the height of 2 km and 85 % in the upper troposphere. For total ozone contributed by foreign anthropogenic emissions over China at various heights, the portion of transboundary ozone produced within foreign emission source regions is less than 50 %, with the rest produced by precursors transported out of those source regions. Japan and Korea contribute 0.6–2.1 ppb of surface ozone over the east coastal regions. Southeast Asia contributes 1–5 ppb over much of southern China and South Asia contributes up to 5–10 ppb of surface ozone over the border of southwestern China; and their contributions increase with height due to strong upwelling over the source regions. The European contribution reaches 2.1–3.0 ppb for surface ozone over the northern border of China and 1.5 ppb in the lower troposphere averaged over China. North America contributes 0.9–2.7 ppb of surface ozone over most of China (1.5–2.1 ppb over the North China Plain), with a China average at 1.5–2.5 ppb at different heights below 8 km, due to its large anthropogenic emissions and the transport-favorable midlatitude westerly wind. In addition to domestic emission control, global emission reduction is critical for China's ozone mitigation.

Description: Surface-based measurements from the EMEP and Airbase networks are used to estimate the changes in surface ozone levels during the 1995–2014 period over Europe. We find significant ozone enhancements (0.20–0.59 µg m−3 yr−1 for the annual means; P-value  

Description: Recent studies have shown that surface ozone (O3) concentrations over central eastern China (CEC) have increased significantly during the past decade. We quantified the effects of changes in meteorological conditions and O3 precursor emissions on surface O3 levels over CEC between July 2003 and July 2015 using the GEOS-Chem model. The simulated monthly mean maximum daily 8 h average O3 concentration (MDA8 O3) in July increased by approximately 13.6 %, from 65.5±7.9 ppbv (2003) to 74.4±8.7 ppbv (2015), comparable to the observed results. The change in meteorology led to an increase in MDA8 O3 of 5.8±3.9 ppbv over the central part of CEC, in contrast to a decrease of about -0.8±3.5 ppbv over the eastern part of the region. In comparison, the MDA8 O3 over the central and eastern parts of CEC increased by 3.5±1.4 and 5.6±1.8 ppbv due to the increased emissions. The increase in averaged O3 in the CEC region resulting from the emission increase (4.0±1.9 ppbv) was higher than that caused by meteorological changes (3.1±4.9 ppbv) relative to the 2003 standard simulation, while the regions with larger O3 increases showed a higher sensitivity to meteorological conditions than to emission changes. Sensitivity tests indicate that increased levels of anthropogenic non-methane volatile organic compounds (NMVOCs) dominate the O3 increase over the eastern part of CEC, and anthropogenic nitrogen oxides (NOx) mainly increase MDA8 O3 over the central and western parts and decrease O3 in a few urban areas in the eastern part. Budget analysis showed that net photochemical production and meteorological conditions (transport in particular) are two important factors that influence O3 levels over the CEC. The results of this study suggest a need to further assess the effectiveness of control strategies for O3 pollution in the context of regional meteorology and anthropogenic emission changes.

Description: Black carbon (BC), which is formed from the incomplete combustion of fuel sources (mainly fossil fuel, biofuel and open biomass burning), is a chemically inert optical absorber in the atmosphere. It has significant impacts on global climate, regional air quality and human health. During transportation, its physical and chemical characteristics as well as its sources change dramatically. To investigate the properties of BC (i.e., mass concentration, sources and optical properties) during intra-regional transport between the southern edge of the North China Plain (SE-NCP) and central China (CC), simultaneous BC observations were conducted in a megacity (Wuhan – WH) in CC, in three borderline cities (Xiangyang – XY, Suixian – SX and Hong'an – HA; from west to east) between the SE-NCP and CC, and in a city (Luohe – LH) in the SE-NCP during typical winter haze episodes. Using an Aethalometer, the highest equivalent BC (eBC) mass concentrations and the highest aerosol absorption coefficients (σabs) were found in LH in the SE-NCP, followed by the borderline cities (XY, SX and HA) and WH. The levels, sources, optical properties (i.e., σabs and absorption Ångström exponent, AAE) and geographic origins of eBC were different between clean and polluted periods. Compared with clean days, higher eBC levels (26.4 %–163 % higher) and σabs (18.2 %–236 % higher) were found during pollution episodes due to the increased combustion of fossil fuels (increased by 51.1 %–277 %), which was supported by the decreased AAE values (decreased by 7.40 %–12.7 %). The conditional bivariate probability function (CBPF) and concentration-weighted trajectory (CWT) results showed that the geographic origins of biomass burning (BCbb) and fossil fuel (BCff) combustion-derived BC were different. Air parcels from the south dominated for border sites during clean days, with contributions of 46.0 %–58.2 %, whereas trajectories from the northeast showed higher contributions (37.5 %–51.2 %) during pollution episodes. At the SE-NCP site (LH), transboundary influences from the south (CC) exhibited a more frequent impact (with air parcels from this direction comprising 47.8 % of all parcels) on the ambient eBC levels during pollution episodes. At WH, eBC was mainly from the northeast transport route throughout the observation period. Two transportation cases showed that the mass concentrations of eBC, BCff and σabs all increased, from upwind to downwind, whereas AAE decreased. This study highlights that intra-regional prevention and control for dominant sources at each specific site should be considered in order to improve the regional air quality.

Description: Eastern China (27–41∘ N, 110–123∘ E) is heavily polluted by nitrogen dioxide (NO2), particulate matter with aerodynamic diameter below 2.5 µm (PM2.5), and other air pollutants. These pollutants vary on a variety of temporal and spatial scales, with many temporal scales that are nonperiodic and nonstationary, challenging proper quantitative characterization and visualization. This study uses a newly compiled EOF–EEMD analysis visualization package to evaluate the spatiotemporal variability of ground-level NO2, PM2.5, and their associations with meteorological processes over Eastern China in fall–winter 2013. Applying the package to observed hourly pollutant data reveals a primary spatial pattern representing Eastern China synchronous variation in time, which is dominated by diurnal variability with a much weaker day-to-day signal. A secondary spatial mode, representing north–south opposing changes in time with no constant period, is characterized by wind-related dilution or a buildup of pollutants from one day to another. We further evaluate simulations of nested GEOS-Chem v9-02 and WRF/CMAQ v5.0.1 in capturing the spatiotemporal variability of pollutants. GEOS-Chem underestimates NO2 by about 17 µg m−3 and PM2.5 by 35 µg m−3 on average over fall–winter 2013. It reproduces the diurnal variability for both pollutants. For the day-to-day variation, GEOS-Chem reproduces the observed north–south contrasting mode for both pollutants but not the Eastern China synchronous mode (especially for NO2). The model errors are due to a first model layer too thick (about 130 m) to capture the near-surface vertical gradient, deficiencies in the nighttime nitrogen chemistry in the first layer, and missing secondary organic aerosols and anthropogenic dust. CMAQ overestimates the diurnal cycle of pollutants due to too-weak boundary layer mixing, especially in the nighttime, and overestimates NO2 by about 30 µg m−3 and PM2.5 by 60 µg m−3. For the day-to-day variability, CMAQ reproduces the observed Eastern China synchronous mode but not the north–south opposing mode of NO2. Both models capture the day-to-day variability of PM2.5 better than that of NO2. These results shed light on model improvement. The EOF–EEMD package is freely available for noncommercial uses.

Description: In the United States, the decline of summertime daytime peak ozone in the last 20 years has been clearly connected to reductions in anthropogenic emissions. However, questions remain about how and through what mechanisms ozone at other times of day have changed over recent decades. Here we analyze the interannual variability and trends of ozone at different hours of day, using observations from about 1000 US sites during 1990–2014. We find a clear diurnal cycle both in the magnitude of ozone trends and in the relative importance of climate variability versus anthropogenic emissions to ozone changes. Interannual climate variability has mainly been associated with the detrended fluctuation in the US annual daytime ozone over 1990–2014, with a much smaller effect on the nighttime ozone. Reductions in anthropogenic emissions of nitrogen oxides have led to substantial growth in the US annual average nighttime ozone due to reduced ozone titration, while the summertime daytime ozone has declined. Environmental policymaking might consider further improvements to reduce ozone levels at night and other non-peak hours.

Description: Satellite retrieval of vertical column densities (VCDs) of tropospheric nitrogen dioxide (NO2) is critical for NOx pollution and impact evaluation. For regions with high aerosol loadings, the retrieval accuracy is greatly affected by whether aerosol optical effects are treated implicitly (as additional “effective” clouds) or explicitly, among other factors. Our previous POMINO algorithm explicitly accounts for aerosol effects to improve the retrieval, especially in polluted situations over China, by using aerosol information from GEOS-Chem simulations with further monthly constraints by MODIS/Aqua aerosol optical depth (AOD) data. Here we present a major algorithm update, POMINO v1.1, by constructing a monthly climatological dataset of aerosol extinction profiles, based on level 2 CALIOP/CALIPSO data over 2007–2015, to better constrain the modeled aerosol vertical profiles. We find that GEOS-Chem captures the month-to-month variation in CALIOP aerosol layer height (ALH) but with a systematic underestimate by about 300–600 m (season and location dependent), due to a too strong negative vertical gradient of extinction above 1 km. Correcting the model aerosol extinction profiles results in small changes in retrieved cloud fraction, increases in cloud-top pressure (within 2 %–6 % in most cases), and increases in tropospheric NO2 VCD by 4 %–16 % over China on a monthly basis in 2012. The improved NO2 VCDs (in POMINO v1.1) are more consistent with independent ground-based MAX-DOAS observations (R2=0.80, NMB = −3.4 %, for 162 pixels in 49 days) than POMINO (R2=0.80, NMB = −9.6 %), DOMINO v2 (R2=0.68, NMB = −2.1 %), and QA4ECV (R2=0.75, NMB = −22.0 %) are. Especially on haze days, R2 reaches 0.76 for POMINO v1.1, much higher than that for POMINO (0.68), DOMINO v2 (0.38), and QA4ECV (0.34). Furthermore, the increase in cloud pressure likely reveals a more realistic vertical relationship between cloud and aerosol layers, with aerosols situated above the clouds in certain months instead of always below the clouds. The POMINO v1.1 algorithm is a core step towards our next public release of the data product (POMINO v2), and it will also be applied to the recently launched S5P-TROPOMI sensor.

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: Surface-based measurements from the EMEP network are used to estimate the changes in surface ozone levels during the 1995–2014 period over Europe. It is shown that a significantly decreasing trend in the 95th percentile ozone concentrations has occurred, especially during noontime (0.9 µg/m3/y), while the 5th percentile ozone concentrations continued to increase with a trend of 0.3 µg/m3/y during the study period. With the help of numerical simulations performed with the global chemistry-climate model EMAC, the importance of anthropogenic emissions changes in determining these changes are investigated. The EMAC model is found to successfully capture the observed temporal variability in mean ozone concentrations, as well as the contrast in the trends of 95th and 5th percentile ozone over Europe. Sensitivity simulations and statistical analysis show that a decrease in European anthropogenic emissions had contrasting effects on surface ozone trends between the 95th and 5th percentile levels, and that background ozone levels have been influenced by hemispheric transport, while climate variability generally regulated the inter-annual variations of surface ozone in Europe.