Publications

WRF-Chem configurations and input data sets for sensitivity tests of emission inventories

WRF-Chem and WPS v4.4 source codes and their configurations with namelist files. Emission inventory data sets (EDGAR-HTAP v2 and v3) for 'anthro_emis' input are included. The KORUS v5 emission data are provided with 'wrfchemi' format. The 'namelist.input' contains physics and chemistry options that are used for WRF-Chem model. The model grid information is available in 'namelist.wps'. Kim, K.-M., Kim, S.-W., Seo, S., Blake, D. R., Cho, S., Crawford, J. H., Emmons, L., Fried, A., Herman, J. R., Hong, J., Jung, J., Pfister, G., Weinheimer, A. J., Woo, J.-H., and Zhang, Q.: Sensitivity of the WRF-Chem v4.4 ozone, formaldehyde, and precursor simulations to multiple bottom-up emission inventories over East Asia during the KORUS-AQ 2016 field campaign, Geosci. Model Dev. Discuss. [preprint], https://doi.org/10.5194/gmd-2023-132, in review, 2023.

The characteristics and sources of roadside VOCs in Hong Kong: Effect of the LPG catalytic converter replacement programme

World-wide increase in tropospheric methane, 1978?1983

Ambient mixing ratios of nonmethane hydrocarbons (NMHCs) in two major urban centers of the Pearl River Delta (PRD) region: Guangzhou and Dongguan

Transport of Asian air pollution to North America

Using observations from the Cheeka Peak Observatory in northwestern Washington State during March‐April, 1997, we show that Asian anthropogenic emissions significantly impact the concentrations of a large number of atmospheric species in the air arriving to North America during spring. Isentropic back‐trajectories can be used to identify possible times when this impact will be felt, however trajectories alone are not sufficient to indicate the presence of Asian pollutants. Detailed chemical and meteorological data from one of these periods (March 29th, 1997) indicates that the surface emissions were lifted into the free troposphere over Asia and then transported to North America in ∼6 days.

Effectiveness of replacing catalytic converters in LPG-fueled vehicles in Hong Kong

Abstract. Many taxis and public buses are powered by liquefied petroleum gas (LPG) in Hong Kong. With more vehicles using LPG, they have become the major contributor to ambient volatile organic compounds (VOCs) in Hong Kong. An intervention program aimed to reduce the emissions of VOCs and nitrogen oxides (NOx) from LPG-fueled vehicles was implemented by the Hong Kong Government in September 2013. Long-term real-time measurements indicated that the program was remarkably effective in reducing LPG-related VOCs, NOx and nitric oxide (NO) in the atmosphere. Receptor modeling results further revealed that propane, propene, i-butane, n-butane and NO in LPG-fueled vehicle exhaust emissions decreased by 37.3 ± 0.4, 50.2 ± 0.3, 32.9 ± 0.4, 41.1 ± 0.4 and 75.9 ± 0.3 %, respectively, during the implementation of the program. In contrast, despite the reduction of VOCs and NOx, the O3 production following the program increased by 0.25 ± 0.04 ppbv h−1 (4.8 %). Moreover, the production rate of HOx decreased due to the reduction of VOCs, whereas NO reduction resulted in a more significant decrease of the HOx in destruction compared to the decrease in production, and an increase of hydroxyl (OH) and hydroperoxyl (HO2). Analysis of O3-VOCs-NOx sensitivity in ambient air indicated VOC-limited regimes in the O3 formation before and during the program. Moreover, a maximum reduction percentage of NOx (i.e., 29.4 %) and the lowest reduction ratio of VOCs / NOx (i.e., ~ 3 : 1) in LPG-fueled vehicle emissions were determined to give a zero O3 increment. The findings are of great help to future formulation and implementation of control strategies on vehicle emissions in Hong Kong.

Stratospheric feedback from continued increases in tropospheric methane

Tropospheric concentrations of methane have increased steadily over the past ten years at an average rate of 16.5 ppbv per year, to a value in January 1988 of 1.69 ppmv. Measurements of CH sub 4 concentrations in air bubbles trapped in ice cores have shown concentrations of about 0.7 ppmv 200 years ago, with little further change for thousands of years before that. Interpolation earlier into this century suggests a concentration of about 1.1 to 1.2 ppmv in the 1940's. The only important pathway believed to be important for transfer of air from the troposphere to the stratosphere in through the tropical tropopause which is cold enough to reduce the mixing ratio of H sub 2 O in that air to about 3 ppmv. The only other major pathway for the delivery of H to the stratosphere is through the simultaneous injection of gaseous CH sub 4 in the same rising air. The formation of clouds in the stratosphere is dependent upon very low temperatures, and generally upon the amount of water vapor available. The possibility of a positive feedback exists, especially in well-oxidized methane air, that clouds are easier to form than earlier. This could mean enhancement of PSCs in both Antarctic and Arctic locations. Additional H sub 2 O in the stratosphere can also add to some of the greenhouse calculations.

Evaluation of the NAQFC driven by the NOAA Global Forecast System (version 16): comparison with the WRF-CMAQ during the summer 2019 FIREX-AQ campaign

Abstract. The latest operational National Air Quality Forecast Capability (NAQFC) has been advanced to use the Community Multiscale Air Quality (CMAQ) model (version 5.3.1) with the CB6r3 (Carbon Bond 6 revision 3) AERO7 (version 7 of the aerosol module) chemical mechanism and is driven by the Finite-Volume Cubed-Sphere (FV3) Global Forecast System, version 16 (GFSv16). This update has been accomplished via the development of the meteorological preprocessor, NOAA-EPA Atmosphere–Chemistry Coupler (NACC), adapted from the existing Meteorology–Chemistry Interface Processor (MCIP). Differing from the typically used Weather Research and Forecasting (WRF) CMAQ system in the air quality research community, the interpolation-based NACC can use various meteorological outputs to drive the CMAQ model (e.g., FV3-GFSv16), even though they are on different grids. In this study, we compare and evaluate GFSv16-CMAQ and WRFv4.0.3-CMAQ using observations over the contiguous United States (CONUS) in summer 2019 that have been verified with surface meteorological and AIRNow observations. During this period, the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) field campaign was performed, and we compare the two models with airborne measurements from the NASA DC-8 aircraft. The GFS-CMAQ and WRF-CMAQ systems show similar performance overall with some differences for certain events, species and regions. The GFSv16 meteorology tends to have a stronger diurnal variability in the planetary boundary layer height (higher during daytime and lower at night) than WRF over the US Pacific coast, and it also predicted lower nighttime 10 m winds. In summer 2019, the GFS-CMAQ system showed better surface ozone (O3) than WRF-CMAQ at night over the CONUS domain; however, the models' fine particulate matter (PM2.5) predictions showed mixed verification results: GFS-CMAQ yielded better mean biases but poorer correlations over the Pacific coast. These results indicate that using global GFSv16 meteorology with NACC to directly drive CMAQ via interpolation is feasible and yields reasonable results compared to the commonly used WRF approach.

Assessing photochemical ozone formation in the Pearl River Delta with a photochemical trajectory model

methane concentrations and source strengths in urban locations

Higher atmospheric concentrations of methane are found in air samples from urban locations than in contemporary samples at the same latitude in remote locations. Higher concentrations of several trace chlorocarbon gases are also found in the same urban samples than in the corresponding remote samples. The “urban excess”, i.e. urban concentration minus remote concentration, is generally 1000 to 2000 times larger on a molar basis for CH 4 than for CCl 3 F. Because almost all CCl 3 F is emitted in urban environments, the urban release of CH 4 is estimated from the observed molar ratios to be 30 to 60 megatons per year world‐wide. The fraction of world‐wide methane release occurring in the urban environment can be estimated from the concentration ratios, urban to remote, for CH 4 vs. CCl 3 F. About 8% to 15% of the atmospheric methane release is observed to occur in urban locations.

Investigating Elevated Concentrations of Hydrogen in the LAX region

Assessment of NMHCs emissions from savanna burning in Northern Australia based on the results of BIBLE-B aircraft observation campaign (Aug. - Sept., 1999)

Field observational constraints on the controllers in glyoxal (CHOCHO) reactive uptake to aerosol

Abstract. Glyoxal (CHOCHO), the simplest dicarbonyl in the troposphere, is a potential precursor for secondary organic aerosol (SOA) and brown carbon (BrC) affecting air quality and climate. The airborne measurement of CHOCHO concentrations during the KORUS-AQ (KORea–US Air Quality study) campaign in 2016 enables detailed quantification of loss mechanisms pertaining to SOA formation in the real atmosphere. The production of this molecule was mainly from oxidation of aromatics (59 %) initiated by hydroxyl radical (OH). CHOCHO loss to aerosol was found to be the most important removal path (69 %) and contributed to roughly ∼ 20 % (3.7 µg sm−3 ppmv−1 h−1, normalized with excess CO) of SOA growth in the first 6 h in Seoul Metropolitan Area. A reactive uptake coefficient (γ) of ∼ 0.008 best represents the loss of CHOCHO by surface uptake during the campaign. To our knowledge, we show the first field observation of aerosol surface-area-dependent (Asurf) CHOCHO uptake, which diverges from the simple surface uptake assumption as Asurf increases in ambient condition. Specifically, under the low (high) aerosol loading, the CHOCHO effective uptake rate coefficient, keff,uptake, linearly increases (levels off) with Asurf; thus, the irreversible surface uptake is a reasonable (unreasonable) approximation for simulating CHOCHO loss to aerosol. Dependence on photochemical impact and changes in the chemical and physical aerosol properties “free water”, as well as aerosol viscosity, are discussed as other possible factors influencing CHOCHO uptake rate. Our inferred Henry's law coefficient of CHOCHO, 7.0×108 M atm−1, is ∼ 2 orders of magnitude higher than those estimated from salting-in effects constrained by inorganic salts only consistent with laboratory findings that show similar high partitioning into water-soluble organics, which urges more understanding on CHOCHO solubility under real atmospheric conditions.

An Inversion of NO _<i>x</i> and NMVOC Emissions using Satellite Observations during the KORUS-AQ Campaign and Implications for Surface Ozone over East Asia

Abstract. The absence of up-to-date emissions has been a major impediment to accurately simulate aspects of atmospheric chemistry, and to precisely quantify the impact of changes of emissions on air pollution. Hence, a non-linear joint analytical inversion (Gauss–Newton method) of both volatile organic compounds (VOC) and nitrogen oxides (NOx) emissions is made by exploiting the Smithsonian Astrophysical Observatory (SAO) Ozone Mapping and Profile Suite Nadir Mapper (OMPS-NM) formaldehyde (HCHO) and the National Aeronautics and Space Administration (NASA) Ozone Monitoring Instrument (OMI) tropospheric nitrogen dioxide (NO2) retrievals during the Korea-United States Air Quality (KORUS-AQ) campaign over East Asia in May–June 2016. Effects of the chemical feedback of NOx and VOCs on both NO2 and HCHO are implicitly included through iteratively optimizing the inversion. Emissions estimates are greatly improved (averaging kernels &gt; 0.8) over medium- to high-emitting areas such as cities and dense vegetation. The amount of total NOx emissions is mainly dictated by values reported in the MIX-Asia 2010 inventory. After the inversion we conclude a decline in the emissions (before, after, change) for China (87.94 ± 44.09 Gg/day, 68.00 ± 15.94 Gg/day, −23 %), North China Plain (NCP) (27.96 ± 13.49 Gg/day, 19.05 ± 2.50 Gg/day, −32 %), Pearl River Delta (PRD) (4.23 ± 1.78 Gg/day, 2.70 ± 0.32 Gg/day, −36 %), Yangtze River Delta (YRD) (9.84 ± 4.68 Gg/day, 5.77 ± 0.51 Gg/day, −41 %), Taiwan (1.26 ± 0.57 Gg/day, 0.97 ± 0.33 Gg/day, −23 %), and Malaysia (2.89 ± 2.77 Gg/day, 2.25 ± 1.34 Gg/day, −22 %), all of which have effectively implemented various stringent regulations. In contrast, South Korea (2.71 ± 1.34 Gg/day, 2.95 ± 0.58 Gg/day, +9 %) and Japan (3.53 ± 1.71 Gg/day, 3.96 ± 1.04 Gg/day, +12 %) experience an increase in NOx emissions potentially due to risen number of diesel vehicles and new thermal power plants. We revisit the well-documented positive bias of the model in terms of biogenic VOC emissions in the tropics. The inversion, however, suggests a larger growth of VOC (mainly anthropogenic) over NCP (25 %) than previously reported (6 %) relative to 2010. The spatial variation in both magnitude and sign of NOx and VOC emissions results in non-linear responses of ozone production/loss. Due to simultaneous decrease/increase of NOx/VOC over NCP and YRD, we observe an ~ 53 % reduction in the ratio of the chemical loss of NOx (LNOx) to the chemical loss of ROx (RO2 + HO2) transitioning toward NOx-sensitive regimes, which in turn, reduces/increases the afternoon chemical loss/production of ozone through NO2 + OH (−0.42 ppbv hr−1)/HO2 (and RO2) + NO (+0.31 ppbv hr−1). Conversely, a combined decrease in NOx and VOC emissions in Taiwan, Malaysia, and the southern China suppresses the formation of ozone. Ultimately, model simulations indicate enhancements of maximum daily 8-hour average (MDA8) surface ozone over China (0.62 ppbv), NCP (4.56 ppbv), and YRD (5.25 ppbv) due to the non-linear ozone chemistry, suggesting that emissions standards should be extended to regulate VOCs to be able to curb ozone production rates. Taiwan, Malaysia, and PRD stand out as the regions undergoing lower MDA8 ozone levels resulting from the NOx reductions occurring predominantly in NOx-sensitive regimes.

Characteristic of Atmospheric Fine Structure of Ozone, Carbon Monoxide, and Humidity During PEACE in Winter and Spring 2002

Impact of Mexico City emissions on regional air quality from MOZART-4 simulations

Abstract. An extensive set of measurements was made in and around Mexico City as part of the MILAGRO (Megacity Initiative: Local and Global Research Observations) experiments in March 2006. Simulations with the Model for Ozone and Related Chemical Tracers, version 4 (MOZART-4), a global chemical transport model, have been used to provide a regional context for these observations and assist in their interpretation. These MOZART-4 simulations reproduce the aircraft observations generally well, but some differences in the modeled volatile organic compounds (VOCs) from the observations result from incorrect VOC speciation assumed for the emission inventories. The different types of CO sources represented in the model have been "tagged" to quantify the contributions of regions outside Mexico, as well as the various emissions sectors within Mexico, to the regional air quality of Mexico. This analysis indicates open fires have some, but not a dominant, impact on the atmospheric composition in the region around Mexico City, when averaged over the month. However, considerable variation in the fire contribution (2–15% of total CO) is seen during the month. The transport and photochemical aging of Mexico City emissions were studied using tags of CO emissions for each day, showing that typically the air near Mexico City was a combination of many ages. Ozone production in MOZART-4 is shown to agree well with the net production rates from box model calculations constrained by the MILAGRO aircraft measurements. Ozone production efficiency derived from the ratio of Ox to NOz is higher in MOZART-4 than in the observations for moderately polluted air. OH reactivity determined from the MOZART-4 results shows the same increase in relative importance of oxygenated VOCs downwind of Mexico City as the reactivity inferred from the observations. The amount of ozone produced by emissions from Mexico City and surrounding areas has been quantified in the model by tracking NO emissions, showing little influence beyond Mexico's borders, and also relatively minor influence from fire emissions on the monthly average tropospheric ozone column.

Mechanisms that influence the formation of high‐ozone regions in the boundary layer downwind of the Asian continent in winter and spring

The seasonal variation of ozone (O 3 ) in the boundary layer (BL) over the western Pacific is investigated using a chemistry‐transport model. The model results for January and April–May 2002 were evaluated by comparison with PEACE aircraft observations. In January, strong northwesterlies efficiently transported NO x from the continent, leading to an O 3 increase of approximately 5–10 ppbv over a distance of about 3000 km. In April, southwesterlies dominated due to anticyclone development over the western Pacific. Along this flow, O 3 continued to be produced by NO x emitted from East Asia. This resulted in the formation of a high‐O 3 (&gt; 50 ppbv) region extending along the coastal areas of East Asia. This seasonal change in O 3 was driven in part by a change in the net O 3 production rate due to increases in solar UV and H 2 O. Its exact response depended on the NO x values in the BL. The net O 3 production rate increased between winter and spring over the Asian continent and decreased over the remote western Pacific. Model simulations show that about 25% of the total O 3 (of 10–20 ppbv) increase over the coastal region of Northeast Asia was due to local production from NO x emissions from China, and the rest was due to changes in background levels as well as emissions from Korea, Japan, and east Siberia. Uplift of BL air over Asia, horizontal transport in the free troposphere, and subsidence were the principal mechanisms of transporting Asian O 3 to the central and eastern North Pacific.

Aged Organic Aerosol in the Upper Troposphere: Aging of boundary layer aerosol during and after convective transport and in-situ SOA formation during DC3. (Invited)