Stratospheric controlled perturbation experiment: a small-scale experiment to improve understanding of the risks of solar geoengineering

Although solar radiation management (SRM) through stratospheric aerosol methods has the potential to mitigate impacts of climate change, our current knowledge of stratospheric processes suggests that these methods may entail significant risks. In addition to the risks associated with current knowledge, the possibility of ‘unknown unknowns’ exists that could significantly alter the risk assessment relative to our current understanding. While laboratory experimentation can improve the current state of knowledge and atmospheric models can assess large-scale climate response, they cannot capture possible unknown chemistry or represent the full range of interactive atmospheric chemical physics. Small-scale, in situ experimentation under well-regulated circumstances can begin to remove some of these uncertainties. This experiment—provisionally titled the stratospheric controlled perturbation experiment—is under development and will only proceed with transparent and predominantly governmental funding and independent risk assessment. We describe the scientific and technical foundation for performing, under external oversight, small-scale experiments to quantify the risks posed by SRM to activation of halogen species and subsequent erosion of stratospheric ozone. The paper's scope includes selection of the measurement platform, relevant aspects of stratospheric meteorology, operational considerations and instrument design and engineering

A Case Study of Convectively Sourced Water Vapor Observed in the Overworld Stratosphere over the United States

On 27 August 2013, during the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys field mission, NASA's ER2 research aircraft encountered a region of enhanced water vapor, extending over a depth of approximately 2 km and a minimum areal extent of 20,000 km(exp 2) in the stratosphere (375 K to 415 K potential temperature), south of the Great Lakes (42N, 90W). Water vapor mixing ratios in this plume, measured by the Harvard Water Vapor instrument, constitute the highest values recorded in situ at these potential temperatures and latitudes. An analysis of geostationary satellite imagery in combination with trajectory calculations links this water vapor enhancement to its source, a deep tropopausepenetrating convective storm system that developed over Minnesota 20 h prior to the aircraft plume encounter. High resolution, groundbased radar data reveal that this system was composed of multiple individual storms, each with convective turrets that extended to a maximum of ~4 km above the tropopause level for several hours. In situ water vapor data show that this storm system irreversibly delivered between 6.6 kt and 13.5 kt of water to the stratosphere. This constitutes a 2025% increase in water vapor abundance in a column extending from 115 hP to 70 hPa over the plume area. Both in situ and satellite climatologies show a high frequency of localized water vapor enhancements over the central U.S. in summer, suggesting that deep convection can contribute to the stratospheric water budget over this region and season

Chemical Impact of Stratospheric Alumina Particle Injection for Solar Radiation Modification and Related Uncertainties

Compared to stratospheric SO2 injection for climate intervention, alumina particle injection could reduce stratospheric warming and associated adverse impacts. However, heterogeneous chemistry on alumina particles, especially chlorine activation via ${\text{ClONO}}_{2}+\text{HCl}\stackrel{\text{surf}}{\to }{\text{Cl}}_{2}+{\text{HNO}}_{3}$, is poorly constrained under stratospheric conditions, such as low temperature and humidity. This study quantifies the uncertainty in modeling the ozone response to alumina injection. We show that extrapolating the limited experimental data for ClONO2 + HCl to stratospheric conditions leads to uncertainties in heterogeneous reaction rates of almost two orders of magnitude. Implementation of injection of 5 Mt/yr of particles with 240 nm radius in an aerosol-chemistry-climate model shows that resulting global total ozone depletions range between negligible and as large as 9%, that is more than twice the loss caused by chlorofluorocarbons, depending on assumptions on the degree of dissociation and interaction of the acids HCl, HNO3, and H2SO4 on the alumina surface.ISSN:0094-8276ISSN:1944-800

Chemical Impact of Stratospheric Alumina Particle Injection for Solar Radiation Modification and Related Uncertainties

Abstract Compared to stratospheric SO2 injection for climate intervention, alumina particle injection could reduce stratospheric warming and associated adverse impacts. However, heterogeneous chemistry on alumina particles, especially chlorine activation via ClONO2+HCl→surfCl2+HNO3, is poorly constrained under stratospheric conditions, such as low temperature and humidity. This study quantifies the uncertainty in modeling the ozone response to alumina injection. We show that extrapolating the limited experimental data for ClONO2 + HCl to stratospheric conditions leads to uncertainties in heterogeneous reaction rates of almost two orders of magnitude. Implementation of injection of 5 Mt/yr of particles with 240 nm radius in an aerosol‐chemistry‐climate model shows that resulting global total ozone depletions range between negligible and as large as 9%, that is more than twice the loss caused by chlorofluorocarbons, depending on assumptions on the degree of dissociation and interaction of the acids HCl, HNO3, and H2SO4 on the alumina surface

In situ measurements of perturbations to stratospheric aerosol and modeled ozone and radiative impacts following the 2021 La Soufrière eruption

Stratospheric aerosols play important roles in Earth’s radiative budget and in heterogeneous chemistry. Volcanic eruptions modulate the stratospheric aerosol layer by injecting particles and particle precursors like sulfur dioxide (SO2) into the stratosphere. Beginning on 9 April 2021, La Soufrière erupted, injecting SO2 into the tropical upper troposphere and lower stratosphere, yielding a peak SO2 loading of 0.3–0.4 Tg. The resulting volcanic aerosol plumes dispersed predominately over the Northern Hemisphere (NH), as indicated by the CALIOP/CALIPSO satellite observations and model simulations. From June to August 2021 and May to July 2022, the NASA ER-2 high-altitude aircraft extensively sampled the stratospheric aerosol layer over the continental United States during the Dynamics and Chemistry of the Summer Stratosphere (DCOTSS) mission. These in situ aerosol measurements provide detailed insights into the number concentration, size distribution, and spatiotemporal variations of particles within volcanic plumes. Notably, aerosol surface area density and number density in 2021 were enhanced by a factor of 2–4 between 380–500 K potential temperature compared to the 2022 DCOTSS observations, which were minimally influenced by volcanic activity. Within the volcanic plume, the observed aerosol number density exhibited significant meridional and zonal variations, while the mode and shape of aerosol size distributions did not vary. The La Soufrière eruption led to an increase in the number concentration of small particles (<400 nm), resulting in a smaller aerosol effective diameter during the summer of 2021 compared to the baseline conditions in the summer of 2022, as observed in regular ER-2 profiles over Salina, Kansas. A similar reduction in aerosol effective diameter was not observed in ER-2 profiles over Palmdale, California, possibly due to the values that were already smaller in that region during the limited sampling period in 2022. Additionally, we modeled the eruption with the SOCOL-AERv2 aerosol–chemistry–climate model. The modeled aerosol enhancement aligned well with DCOTSS observations, although the direct comparison was complicated by issues related to the model’s background aerosol burden. This study indicates that the La Soufrière eruption contributed approximately 0.6 % to Arctic and Antarctic ozone column depletion in both 2021 and 2022, which is well within the range of natural variability. The modeled top-of-atmosphere 1-year global average radiative forcing was −0.08 W m−2 clear-sky and −0.04 W m−2 all-sky. The radiative effects were concentrated in the tropics and NH midlatitudes and diminished to near-baseline levels after 1 year.ISSN:1680-7375ISSN:1680-736