Anthropogenic Fingerprint Detectable in Upper Tropospheric Ozone Trends Retrieved from Satellite.

Tropospheric ozone (O) is a strong greenhouse gas, particularly in the upper troposphere (UT). Limited observations point to a continuous increase in UT O in recent decades, but the attribution of UT O changes is complicated by large internal climate variability. We show that the anthropogenic signal ("fingerprint") in the patterns of UT O increases is distinguishable from the background noise of internal variability. The time-invariant fingerprint of human-caused UT O changes is derived from a 16-member initial-condition ensemble performed with a chemistry-climate model (CESM2-WACCM6). The fingerprint is largest between 30°S and 40°N, especially near 30°N. In contrast, the noise pattern in UT O is mainly associated with the El Niño-Southern Oscillation (ENSO). The UT O fingerprint pattern can be discerned with high confidence within only 13 years of the 2005 start of the OMI/MLS satellite record. Unlike the UT O fingerprint, the lower tropospheric (LT) O fingerprint varies significantly over time and space in response to large-scale changes in anthropogenic precursor emissions, with the highest signal-to-noise ratios near 40°N in Asia and Europe. Our analysis reveals a significant human effect on Earth's atmospheric chemistry in the UT and indicates promise for identifying fingerprints of specific sources of ozone precursors.