The extent to which stratospheric intrusions on synoptic scales influence the tropospheric ozone (O 3 ) levels remains poorly understood, because quantitative detection of stratospheric air has been challenging. Cosmogenic 35 S mainly produced in the stratosphere has the potential to identify stratospheric air masses at ground level, but this approach has not yet been unambiguously shown. Here, we report unusually high 35 S concentrations (7,390 atoms m −3; ∼16 times greater than annual average) in fine sulfate aerosols (aerodynamic diameter less than 0.95 μm) collected at a coastal site in southern California on May 3, 2014, when groundlevel O 3 mixing ratios at air quality monitoring stations across southern California (43 of 85) exceeded the recently revised US National Ambient Air Quality Standard (daily maximum 8-h average: 70 parts per billion by volume). The stratospheric origin of the significantly enhanced 35 S level is supported by in situ measurements of air pollutants and meteorological variables, satellite observations, meteorological analysis, and box model calculations. The deep stratospheric intrusion event was driven by the coupling between midlatitude cyclones and Santa Ana winds, and it was responsible for the regional O 3 pollution episode. These results provide direct field-based evidence that 35 S is an additional sensitive and unambiguous tracer in detecting stratospheric air in the boundary layer and offer the potential for resolving the stratospheric influences on the tropospheric O 3 level.stratosphere-troposphere exchange | surface ozone | National Ambient Air Quality Standard | radioactive isotope of sulfur | Santa Ana wind H igh ground-level ozone (O 3 ) mixing ratios exert adverse impacts on human health, vegetation, and materials (1, 2). In the free troposphere, O 3 is an important greenhouse gas contributing to global warming. It also controls the lifetime of other reactive greenhouse gases through oxidation processes (3), serves as the dominant precursor of the hydroxyl radical, and enhances the oxidizing capacity of the troposphere (4). Tropospheric O 3 formation involves a series of photochemical reactions related to anthropogenic emissions of O 3 precursors [e.g., nitrogen oxides (NO x ), carbon monoxide (CO), and volatile organic compounds (VOCs)], biomass burning, and lightning (5). In addition, elevated levels of tropospheric O 3 may be caused by the intrusion of O 3 -rich stratospheric air masses (4, 6-8). Detection of such stratospheric intrusion events by field-based measurements has been a major scientific concern since the 1970s (9). Concurrent measurement of ground-level O 3 , CO, and humidity is the most common method (10, 11), but it is ambiguous and only useful in extreme events and background sites. Ozonesondes, lidar, and aircraft measurements provide high-resolution information on vertical O 3 distributions (12-14), but they are relatively expensive and not widely available. Therefore, it is crucial to find an additional and unambiguous stratospheric tracer at g...