Publications

Stratospheric aerosol injection (SAI) might alleviate some climate risks associated with accumulating greenhouse gases. Reduction of specific process uncertainties relevant to the distribution of aerosol in a turbulent stratospheric wake is necessary to support informed decisions about aircraft deployment of this technology. To predict aerosol size distributions we apply microphysical parameterizations of nucleation, condensation and coagulation to simulate an aerosol plume generated via injection of calcite powder or sulphate into a stratospheric wake with velocity and turbulence simulated by a three‐dimensional (3D) fluid dynamic calculation. We apply the model to predict the aerosol distribution that would be generated by a propeller wake in the Stratospheric Controlled Perturbation Experiment (SCoPEx). We find that injecting 0.1 g s^‐1 calcite aerosol produces a nearly monodisperse plume and that at the same injection rate, condensable sulphate aerosol forms particles with average radii of 0.1 µm at 3 km downstream. We test the sensitivity of plume aerosol composition, size, and optical depth to the mass injection rate and injection location. Aerosol size distribution depends more strongly on injection rate than injection configuration. Comparing plume properties with specifications of a typical photometer, we find that plumes could be detected optically as the payload flies under the plume. These findings test the relevance of in situ sampling of aerosol properties by the SCoPEx outdoor experiment to enable quantitative tests of microphysics in a stratospheric plume. Our findings provide a basis for developing predictive models of SAI using aerosols formed in stratospheric aircraft wakes.

Injection of sulfate aerosols into the stratosphere, a form of solar geoengineering, has been proposed as a means to reduce some climatic changes by decreasing net anthropogenic radiative forcing. The cost and technical feasibility of forming aerosols with the appropriate size distribution are uncertain. We examine the possibility of producing the relevant sulfur species, SO₂ or SO₃, by in situ conversion fromelemental sulfur onboard an aircraft. We provide afirst-order engineering analysis of an open cycle chemicalplant for in situ sulfur to sulfate conversion using a Brayton cycle combustor and a catalytic converter. We find that such a plant could have sufficiently low mass that the overall requirement for mass transport to the lower stratosphere may be reduced by roughly a factor of 2. All else equal, this suggests that—for a given radiative forcing—the cost of delivering sulfate aerosols may be nearly halved. Beyond reducing cost, the use of elemental sulfur reduces operational health and safety risks and should therefore reduce environmental side effects associated with delivery. Reduction in cost is not necessarily beneficial as it reduces practical barriers to deployment, increasing the urgency of questions concerningthe efficacy, risks, and governance of solar geoengineering.

Injecting sulfate aerosol into the stratosphere, the most frequently analyzed proposal for solar geoengineering, may reduce some climate risks, but it would also entail new risks, including ozone loss and heating of the lower tropical stratosphere, which, in turn, would increase water vapor concentration causing additional ozone loss and surface warming. We propose a method for stratospheric aerosol climate modification that uses a solid aerosol composed of alkaline metal salts that will convert hydrogen halides and nitric and sulfuric acids into stable salts to enable stratospheric geoengineering while reducing or reversing ozone depletion. Rather than minimizing reactive effects by reducing surface area using high refractive index materials, this method tailors the chemical reactivity. Specifically, we calculate that injection of calcite (CaCO₃) aerosol particles might reduce net radiative forcing while simultaneously increasing column ozone toward its preanthropogenic baseline. A radiative forcing of −1 W⋅m⁻², for example, might be achieved with a simultaneous 3.8% increase in column ozone using 2.1 Tg⋅y⁻¹ of 275-nm radius calcite aerosol. Moreover, the radiative heating of the lower stratosphere would be roughly 10-fold less than if that same radiative forcing had been produced using sulfate aerosol. Although solar geoengineering cannot substitute for emissions cuts, it may supplement them by reducing some of the risks of climate change. Further research on this and similar methods could lead to reductions in risks and improved efficacy of solar geoengineering methods.

Side effects resulting from the deliberate injection of sulfate aerosols intended to partially offset climate change have motivated the investigation of alternatives, including solid aerosol materials. Sulfate aerosols warm the tropical tropopause layer, increasing the flux of water vapor into the stratosphere, accelerating ozone loss, and increasing radiative forcing. The high refractive index of some solid materials may lead to reduction in these risks. We present a new analysis of the scattering efficiency and absorption of a range of candidate solid aerosols. We utilize a comprehensive radiative transfer model driven by updated, physically consistent estimates of optical properties. We compute the potential increase in stratospheric water vapor and associated longwave radiative forcing. We find that the stratospheric heating calculated in this analysis indicates some materials to be substantially riskier than previous work. We also find that there are Earth-abundant materials that may reduce some principal known risks relative to sulfate aerosols.