Factors dominating 3-dimensional ozone distribution during high tropospheric ozone period

Data from an in situ monitoring network and five ozone sondes are analysed during August of 2012, and a high tropospheric ozone episode is observed around the 8th of AUG. The Community Multi-scale Air Quality (CMAQ) model and its process analysis tool were used to study factors and mechanisms for high ozone mixing ratio at different levels of ozone vertical profiles. A sensitive scenario without chemical initial and boundary conditions (ICBCs) from MOZART4-GEOS5 was applied to study the impact of stratosphere-troposphere exchange (STE) on vertical ozone. The simulation results indicated that the first high ozone peak near the tropopause was dominated by STE. Results from process analysis showed that: in the urban area, the second peak at approximately 2 km above ground height was mainly caused by local photochemical production. The third peak (near surface) was mainly caused by the upwind transportation from the suburban/rural areas; in the suburban/rural areas, local photochemical production of ozone dominated the high ozone mixing ratio from the surface to approximately 3 km height. Furthermore, the capability of indicators to distinguish O₃-precursor sensitivity along the vertical O₃ profiles was investigated. Two sensitive scenarios, which had cut 30% anthropogenic NO_X or VOC emissions, showed that O₃-precursor indicators, specifically the ratios of O₃/NOy, H₂O₂/HNO₃ or H₂O₂/NO_Z, could partly distinguish the O₃-precursor sensitivity between VOCs-sensitive and NOx-sensitive along the vertical profiles. In urban area, the O₃-precursor relationship transferred from VOCs-sensitive within the boundary layer to NOx-sensitive at approximately 1–3 km above ground height, further confirming the dominant roles of transportation and photochemical production in high O₃ peaks at the near-ground layer and 2 km above ground height, respectively. - Highlights: • Three-dimensional ozone was analyzed during a high tropospheric ozone period. • Contribution of chemical reactions to O₃ differs from urban to non-urban areas. • Stratosphere-troposphere exchange induces the high ozone peak near tropopause. • Adaptability of O₃-precursor sensitivity in vertical direction are demonstrated. • A transition zone of O₃-precursor sensitivity is found at 1–3 km above urban area. - Distribution and formation mechanism of 3-dimensional ozone in urban/suburban/rural areas. Applications of O₃-precursor sensitivity and its indicators in the vertical direction.