Causes of growing middle-to-upper tropospheric ozone over the northwest Pacific region

Kurzfassung

Long-term ozone (O3) changes in the middle-to-upper troposphere are critical to climate radiative forcing and tropospheric O3 pollution. Yet, these changes remain poorly quantified through observations in East Asia. Concerns also persist regarding the data quality of the ozonesondes available at the World Ozone and Ultraviolet Radiation Data Centre (WOUDC) for this region. This study aims to address these gaps by analyzing O3 soundings at four sites along the northwestern Pacific coastal region over the past 3 decades and by assessing their consistency with an atmospheric chemistry–climate model simulation. Utilizing the European Centre for Medium-Range Weather Forecasts (ECMWF) Hamburg (ECHAM)/Modular Earth Submodel System (MESSy) Atmospheric Chemistry (EMAC) nudged simulations, it is demonstrated that trends between model and ozonesonde measurements are overall consistent, thereby gaining confidence in the model's ability to simulate O3 trends and confirming the utility of potentially imperfect observational data. A notable increase in O3 mixing ratio around 0.29–0.82 ppb a−1 extending from the middle troposphere to the upper troposphere is observed in both observations and model simulations between 1990 and 2020, primarily during spring and summer. The timing of these O3 tongues is delayed when moving from south to north along the measurement sites, transitioning from late spring to summer. Investigation into the drivers of these trends using tagged model tracers reveals that O3 of stratospheric origin (O3S) dominates the absolute O3 mixing ratios over the middle-to-upper troposphere in the subtropics, contributing to the observed O3 increases by up to 96 % (40 %) during winter (summer), whereas O3 of tropospheric origin (O3T) governs the absolute value throughout the tropical troposphere and contributes generally much more than 60 % to the positive O3 changes, especially during summer and autumn. During winter and spring, a decrease in O3S is partly counterbalanced by an increase in O3T in the tropical troposphere. This study highlights that the enhanced downward transport of stratospheric O3 into the troposphere in the subtropics and a surge of tropospheric O3 in the tropics are the two key factors driving the enhancement of O3 in the middle-to-upper troposphere along the northwest Pacific region.