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High concentrations of PM2.5 have become a serious environmental issue in South Korea, which ranked 1st or 2nd among OECD countries in terms of population exposure to PM2.5. Quantitative understanding of PM2.5 source attribution is thus crucial for developing efficient air quality mitigation strategies. Here we use a suite of extensive observations of PM2.5 and its precursors concentrations during the international KORea-US cooperative Air Quality field study in Korea (KORUS-AQ) in May–June 2016 to investigate source contributions to PM2.5 in South Korea under various meteorological conditions. For the quantitative analysis, we updated a 3-D chemical transport model, GEOS-Chem, and its adjoint with the latest regional emission inventory and other recent findings. The updated model is evaluated by comparing against observed daily PM2.5 and its component concentrations from six ground sites (Bangnyung, Bulkwang, Olympic park, Gwangju, Ulsan, and Jeju). Overall, simulated concentrations of daily PM2.5 and its components are in a good agreement with observations over the peninsula. We conduct an adjoint sensitivity analysis for simulated surface level PM2.5 concentrations at five ground sites (except for Bangnyung because of its small population) under four different meteorological conditions: dynamic weather, stagnant, extreme pollution, and blocking periods. Source contributions by regions vary greatly depending on synoptic meteorological conditions. Chinese contribution accounts for almost 68% of PM2.5 in surface air in South Korea during the extreme pollution period of the campaign, whereas an enhanced contribution from domestic sources (57%) occurs for the blocking period. Results from our sensitivity analysis suggest that the reduction of domestic anthropogenic NH3 emissions could be most effective in reducing population exposure to PM2.5 in South Korea (effectiveness = 14%) followed by anthropogenic SO2 emissions from Shandong region (effectiveness = 11%), domestic anthropogenic NOx emissions (effectiveness = 10%), anthropogenic NH3 emissions from Shandong region (effectiveness = 8%), anthropogenic NOx emissions from Shandong region (effectiveness = 7%), domestic anthropogenic OC emissions (effectiveness = 7%), and domestic anthropogenic BC emissions (effectiveness = 5%).

To understand the characteristics of air quality in the Seoul Metropolitan Area, intensive measurements were conducted under the Korea-United States Air Quality (KORUS-AQ) campaign. Trace gases such as O3, NOx, NOy, SO2, CO, and volatile organic compounds (VOCs), photochemical byproducts such as H2O2 and HCHO, aerosol species, and meteorological variables including planetary boundary layer height were simultaneously measured at Olympic Park in Seoul. During the measurement period, high O3 episodes that exceeded the 90 ppbv hourly maximum occurred on 14 days under four distinct synoptic meteorological conditions. Furthermore, local circulation such as land–sea breeze and diurnal evolution of the boundary layer were crucial in determining the concentrations of precursor gases, including NOx and VOC as well as O3. During such episodes, the nighttime NOx and VOC and daytime UV levels were higher compared to non-episode days. The overall precursor levels and photochemical activity were represented fairly well by variations in the HCHO, which peaked in the morning during the high O3 episodes. This study revealed that toluene was the most abundant VOC in Seoul, and its concentration increased greatly with NOx due to the large local influence under stagnant conditions. When O3 was highly elevated concurrently with PM2.5 under dominant westerlies, NOx and VOCs were relatively lower and CO was noticeably higher than in other episodes. Additionally, the O3 production efficiency was the highest due to a low NOx with the highest NOz/NOy ratio among the four episodes. When westerlies were dominant in transport-south episode, the nighttime concentration of O3 remained as high as 40~50 ppbv due to the minimum level of NOx titration. Overall, the Seoul Metropolitan Area is at NOx-saturated and VOC-limited conditions, which was diagnosed by indicator species and VOC/NOx ratios.

The Korea – United States Air Quality Study (May – June 2016) deployed instrumented aircraft and ground-based measurements to elucidate causes of poor air quality related to high ozone and aerosol concentrations in South Korea. This work synthesizes data pertaining to aerosols (specifically, particulate matter with aerodynamic diameters

Photolysis of nitrous acid (HONO) has long been recognized as an early morning source of OH radicals in urban air, but the detailed mechanism of its formation is still unclear. During the Korea-US Air Quality (KORUS-AQ) campaign, HONO was measured using Quantum Cascade Tunable Diode Laser Absorption Spectroscopy (QC-TDLAS) at Olympic Park in Seoul from 17 May to 10 June, 2016. HONO concentrations ranged from 0.07 ppbv to 3.46 ppbv with an average of 0.93 ppbv. HONO remained high at night from 1 am to 5 am, during which the mean concentration was higher in high-O3 episodes (1.82 ppbv) than non-episode (1.20 ppbv). In the morning, OH budget due to HONO photolysis were higher by 50 % (0.95 pptv) during high-O3 episodes compared to non-episode. Diurnal variations of HOx and O3 simulated by the F0AM model demonstrated a difference of ~ 20 ppbv in daily maximum O3 between the two periods. The HONO concentration increased with relative humidity (RH) until 80 %, of which the highest HONO was associated with the top 10 % NOx, confirming that NOx is a crucial precursor of HONO and its formation is facilitated by humidity. The conversion ratio of NOx to HONO was estimated to be 0.86 × 10−2 h−1 at night and also increased with RH. As surrogate for the catalyst surface, the mass concentrations of black carbon (eBC) and the surface areas of particles smaller than 120 nm showed a tendency for RH similar to conversion ratio. Using an Artificial Neuron Network (ANN) model, HONO concentrations were successfully simulated with measured variables (r = 0.8 for the best suite), among which NOx, surface area, and RH were found to be main factors affecting ambient HONO concentrations with weigh values of 26.2 %, 11.9 %, and 10.6 %, respectively. This study demonstrates the coupling of HONO with HOx-VOCs-O3 cycle in Seoul Metropolitan Areas (SMA) and provides practical evidence for heterogeneous formation of HONO by employing the ANN model to atmospheric chemistry.

Photolysis of nitrous acid (HONO) is recognized as an early-morning source of OH radicals in the urban air. During the Korea-US air quality (KORUS-AQ) campaign, HONO was measured using quantum cascade - tunable infrared laser differential absorption spectrometer (QC-TILDAS) at Olympic Park in Seoul from 17 May, 2016 to 14 June, 2016. The HONO concentration was in the range of 0.07-3.46 ppbv, with an average of 0.93 ppbv. Moreover, it remained high from 00:00-05:00 LST. During this time, the mean concentration was higher during the high-O3 episodes (1.82 ppbv) than the non-episodes (1.20 ppbv). In the morning, the OH radicals that were produced from HONO photolysis were 50% higher (0.95 pptv) during the high-O3 episodes than the non-episodes. Diurnal variations in HOx and O3 concentrations were simulated by the F0AM model, which revealed a difference of ~20 ppbv in the daily maximum O3 concentrations between the high-O3 episodes and non-episodes. Furthermore, the HONO concentration increased with an increase in relative humidity (RH) up to 80%; the highest HONO was associated with the top 10% NO2 in each RH group, confirming that NO2 is one of the main precursors of HONO. At night, the conversion ratio of NO2 to HONO was estimated to be 0.88×10-2 h-1; this ratio was found to increase with an increase in RH. The Aitken mode particles (30-120 nm), which act as catalyst surfaces, exhibited a similar tendency with a conversion ratio that increased along with RH, indicating the coupling of surfaces with HONO conversion. Using an artificial neural network (ANN) model, HONO concentrations were successfully simulated with measured variables (r2 = 0.66 as an average of five models). Among these variables, NOx, aerosol surface area, and RH were found to be the main factors affecting the ambient HONO concentrations. The results reveal that RH facilitates the conversion of NO2 to HONO by constraining the availability of aerosol surfaces. This study demonstrates the coupling of HONO with the HOx-O3 cycle in the Seoul Metropolitan Area (SMA) and provides practical evidence of the heterogeneous formation of HONO by employing the ANN model.