1981–2020 winter ozone trends, Erzgebirge, Central Europe

Abstract Tropospheric ozone (O3) acts as greenhouse gas and air pollutant. Over the last 100 years, tropospheric O3 levels increased above background by factor 2.5 in the northern hemisphere and by factor 3–4 across Europe. The gas poses a potential risk to forest ecosystems in many mountain areas. There, O3 concentrations result from long-range transport and are influenced by removal processes (dry deposition, gas phase and cloud removal, reduction on wet aerosols). Most trend studies analyzed annual-mean concentrations. We focus on winter O3 trends at high altitudes in the German/Czech Erzgebirge (period 1981–2020) to avoid major noise from photochemical reactions and to better explain recent O3 behavior in Central Europe. Hourly air quality and meteorological data from four stations (Carlsfeld, CAR; Fichtelberg, FIB; Schwartenberg, SWB; Zinnwald, ZIW) were used to analyze O3 trends. The data can explain the complex O3 formation and removal behavior. Three distinct periods of O3-concentration trends can be discerned: i) Until the late 1980s, characterized by relatively low O3 concentrations. ii) Dramatic transformation in the 1990s with changing air pollution in Central Europe. Strong O3-concentration increase at FIB is corroborated by data from CAR and ZIW. iii) Stabilization as of 1997/98, when O3 concentrations remained at the same level for all four stations, despite general regional air pollution decrease. Key results are: a) Winter O3 trends mainly depend on O3 concentration of air masses transported to the stations and on the O3-removal potential (ORP) of clouds, not on local formation processes. b) ORP differs between clouds and fog, depending on droplet chemical composition. Fog from the North Bohemian Basin showed the highest ORP due to reaction with liquid phase S(IV). However, O3 reactions with O2- in fog droplets showed high ORP, too, depending on cloud-water pH values and NOx concentrations. c) So-called “Bohemian fog” decreased, and with it related ORP, while that of clouds from westerly and northwesterly air masses remained nearly unchanged since 1997/98. d) Decreasing ORP in clouds and fog (= higher O3 concentration) oppose decreasing O3 concentrations in westerly air masses. Both effects lead to unchanged O3 levels in the Erzgebirge since 1997/98.