Warren P Smith

and 27 more

The Asian Summer Monsoon (ASM) has garnered attention in recent years for its impacts on the composition of the upper troposphere and lower stratosphere (UTLS) via deep convection. A recent observational effort into this mechanism, the Asian summer monsoon Chemical and CLimate Impact Project (ACCLIP), sampled the composition of the ASM UTLS over the northwestern Pacific during boreal summer 2022 using two airborne platforms. In this work, we integrate Lagrangian trajectory modeling with convective cloud top observations to diagnose ASM convective transport which contributed to ACCLIP airborne observations. This diagnostic is applied to explore the properties of convective transport associated with prominent ASM sub-systems, revealing that convective transport along the East Asia Subtropical Front generally contained more pollutants than from South Asia, for species ranging in lifetime from days to months. The convective transport diagnostic is used to isolate three convective transport events over eastern Asia which had distinct chemical tracer relationship slopes, indicating the different economical behaviors of the contributing source regions. One of these transport events is explored in greater detail, where a polluted air mass was sampled from convection over the Northeast China Plain. This event was largely confined to 12-15 km altitude, which may be high enough to impact the composition of the stratosphere. Overall, the presented diagnosis of convective transport contribution to ACCLIP airborne sampling indicates a key scientific success of the campaign and enables process studies of the climate interactions from the two ASM sub-system.

Laurence Y Yeung

and 7 more

Tropospheric 18O18O is an emerging proxy for past tropospheric ozone and free-tropospheric temperatures. The basis of these applications is the idea that isotope-exchange reactions in the atmosphere drive 18O18O abundances toward isotopic equilibrium. However, previous work used an offline box-model framework to explain the 18O18O budget, approximating the interplay of atmospheric chemistry and transport. This approach, while convenient, has poorly characterized uncertainties. To investigate these uncertainties, and to broaden the applicability of the 18O18O proxy, we developed a scheme to simulate atmospheric 18O18O abundances (quantified as ∆36 values) online within the GEOS-Chem chemical transport model. These results are compared to both new and previously published atmospheric observations from the surface to 33 km. Simulations using a simplified O2 isotopic equilibration scheme within GEOS-Chem show quantitative agreement with measurements only in the middle stratosphere; modeled ∆36 values are too high elsewhere. Investigations using a comprehensive model of the O-O2-O3 isotopic photochemical system and proof-of-principle experiments suggest that the simple equilibration scheme omits an important pressure dependence to ∆36 values: the anomalously efficient titration of 18O18O to form ozone. Incorporating these effects into the online ∆36 calculation scheme in GEOS-Chem yields quantitative agreement for all available observations. While this previously unidentified bias affects the atmospheric budget of 18O18O in O2, the modeled change in the mean tropospheric ∆36 value since 1850 C.E. is only slightly altered; it is still quantitatively consistent with the ice-core ∆36 record, implying that the tropospheric ozone burden increased less than ~40% over the twentieth century.