Rei Ueyama’s research while affiliated with Ames Research Center and other places

Refractory black carbon (rBC) is a primary aerosol species, produced through incomplete combustion, that absorbs sunlight and contributes to positive radiative forcing. The overall climate effect of rBC depends on its spatial distribution and atmospheric lifetime, both of which are impacted by the efficiency with which rBC is transported or removed by convective systems. These processes are poorly constrained by observations. It is especially interesting to investigate rBC transport efficiency through the Asian Summer Monsoon (ASM) since this meteorological pattern delivers vast quantities of boundary layer air from Asia, where rBC emissions are high to the upper troposphere/lower stratosphere (UT/LS) where the lifetime of rBC is expected to be long. Here, we present in situ observations of rBC made during the Asian Summer Monsoon Chemistry and Climate Impact Project of summer, 2022. We use observed relationships between rBC and CO in ASM outflow to show that rBC is removed nearly completely (>98%) from uplifted air and that rBC concentrations in ASM outflow are statistically indistinguishable from the UT/LS background. We compare observed rBC and CO concentrations to those expected based on two chemical transport models and find that the models reproduce CO to within a factor of 2 at all altitudes whereas rBC is overpredicted by a factor of 20–100 at altitudes associated with ASM outflow. We find that the rBC particles in recently convected air have thinner coatings than those found in the UTLS background, suggesting transport of a small number of rBC particles that are negligible for concentration.

The 2022 Hunga volcanic eruption injected a significant amount of water vapor and a moderate amount of sulfur dioxide into the stratosphere causing observable responses in the climate system. We have developed a model-observation comparison project to investigate the evolution of volcanic water and aerosols, and their impacts on atmospheric dynamics, chemistry, and climate, using several state-of-the-art chemistry climate models. The project goals are: 1. Evaluate the current chemistry-climate models to quantify their performance in comparison to observations; and 2. Understand atmospheric responses in the Earth system after this exceptional event and investigate the potential impacts in the projected future. To achieve these goals, we designed specific experiments for direct comparisons to observations, for example from balloons and the Microwave Limb Sounder satellite instrument. Experiment 1 is a free-running ensemble experiment from 2022 to 2031. Experiment 2 is a nudged-run experiment from 2022 to 2023 using observed meteorology. To allow participation of more climate models with varying complexities of aerosol simulation, we include two sets of simulations in Experiment 2: Experiment 2a is designed for models with internally-generated aerosol while Experiment 2b is designed for models using prescribed aerosol surface area density. We take model results from the previously developed Tonga-MIP to fulfill Experiment 3, which focuses on the initial dispersion and microphysical evolution of aerosol and water plumes. Experiment 4 is designed to understand the climate impact on the mesosphere from 2022–2027, for which the experiment design is the same as Experiment 1 but for models that resolve the upper stratosphere and mesosphere.

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.

Hydration of the stratosphere by tropopause‐overshooting convection has received increasing interest due to the extreme concentrations of water vapor that can result and, ultimately, the climate warming potential such hydration provides. Previous work has recognized the importance of numerous dynamic and physical processes that control stratospheric water vapor delivery by convection. This study leverages recent comprehensive observations from the NASA Dynamics and Chemistry of the Summer Stratosphere (DCOTSS) field campaign to determine the frequency at which each process operates during real events. Specifically, a well‐established analysis technique known as tracer‐tracer correlation is applied to DCOTSS observations of ozone, water vapor, and potential temperature to identify the occurrence of known processes. It is found that approximately half of convectively‐driven stratospheric hydration samples show no indication of significant air mass transport and mixing, emphasizing the importance of ice sublimation to stratospheric water vapor delivery. Furthermore, the temperature of the upper troposphere and lower stratosphere environment and/or overshoot appears to be a commonly active constraint, since the approximate maximum possible water vapor concentration that can be reached in an air mass is limited to the saturation mixing ratio when ice is present. Finally, little evidence of relationships between dynamic and physical processes and their spatial distribution was found, implying that stratospheric water vapor delivery by convection is likely facilitated by a complex collection of processes in each overshooting event.

We calculate the climate forcing for the 2 ys after the 15 January 2022, Hunga Tonga‐Hunga Ha'apai (Hunga) eruption. We use satellite observations of stratospheric aerosols, trace gases and temperatures to compute the tropopause radiative flux changes relative to climatology. Overall, the net downward radiative flux decreased compared to climatology. The Hunga stratospheric water vapor anomaly initially increases the downward infrared radiative flux, but this forcing diminishes as the anomaly disperses. The Hunga aerosols cause a solar flux reduction that dominates the net flux change over most of the 2 yrs period. Hunga induced temperature changes produce a decrease in downward long‐wave flux. Hunga induced ozone reduction increases the short‐wave downward flux creating small sub‐tropical increase in total flux from mid‐2022 to 2023. By the end of 2023, most of the Hunga induced radiative forcing changes have disappeared. There is some disagreement in the satellite measured stratospheric aerosol optical depth (SAOD) observations which we view as a measure of the uncertainty; however, the SAOD uncertainty does not alter our conclusion that, overall, aerosols dominate the radiative flux changes.

Tropopause-overshooting convection in the midlatitudes provides a rapid transport pathway for air from the lower troposphere to reach the upper troposphere and lower stratosphere (UTLS) and can result in the formation of above-anvil cirrus plumes (AACPs) that significantly hydrate the stratosphere. Such UTLS composition changes alter the radiation budget and impact climate. Novel in situ observations from the NASA Dynamics and Chemistry of the Summer Stratosphere (DCOTSS) field campaign are used in this study to examine UTLS impacts from AACP-generating overshooting convection. Namely, a research flight on 31 May 2022 sampled active convection over the state of Oklahoma for more than 3 h with the NASA ER-2 high-altitude research aircraft. An AACP was bisected during this flight, providing the first such extensive in situ sampling of this phenomenon. The convective observations reveal pronounced changes in air mass composition and stratospheric hydration up to altitudes of 2.3 km above the tropopause and concentrations more than double background levels. Unique dynamic and trace gas signatures were found within the AACP, including enhanced vertical mixing near the AACP edge and a positive correlation between water vapor and ozone. Moreover, the water vapor enhancement within the AACP was found to be limited to the saturation mixing ratio of the low temperature overshoot and AACP air. Comparison with all remaining DCOTSS flights demonstrates that the 31 May 2022 flight had some of the largest tropospheric tracer and water vapor perturbations in the stratosphere and within the AACP.

Deep convection in the Asian summer monsoon is a significant transport process for lifting pollutants from the planetary boundary layer to the tropopause level. This process enables efficient injection into the stratosphere of reactive species such as chlorinated very-short-lived substances (Cl-VSLSs) that deplete ozone. Past studies of convective transport associated with the Asian summer monsoon have focused mostly on the south Asian summer monsoon. Airborne observations reported in this work identify the East Asian summer monsoon convection as an effective transport pathway that carried record-breaking levels of ozone-depleting Cl-VSLSs (mean organic chlorine from these VSLSs ~500 ppt) to the base of the stratosphere. These unique observations show total organic chlorine from VSLSs in the lower stratosphere over the Asian monsoon tropopause to be more than twice that previously reported over the tropical tropopause. Considering the recently observed increase in Cl-VSLS emissions and the ongoing strengthening of the East Asian summer monsoon under global warming, our results highlight that a reevaluation of the contribution of Cl-VSLS injection via the Asian monsoon to the total stratospheric chlorine budget is warranted.