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<p>Studies of stratospheric solar geoengineering have tended to focus on modification of the sulfuric acid aerosol layer, and almost all climate model experiments that mechanistically increase the sulfuric acid aerosol burden assume injection of SO<span class="inline-formula">₂</span>. A key finding from these model studies is that the radiative forcing would increase sublinearly with increasing SO<span class="inline-formula">₂</span> injection because most of the added sulfur increases the mass of existing particles, resulting in shorter aerosol residence times and aerosols that are above the optimal size for scattering. Injection of SO<span class="inline-formula">₃</span> or H<span class="inline-formula">₂</span>SO<span class="inline-formula">₄</span> from an aircraft in stratospheric flight is expected to produce particles predominantly in the accumulation-mode size range following microphysical processing within an expanding plume, and such injection may result in a smaller average stratospheric particle size, allowing a given injection of sulfur to produce more radiative forcing. We report the first multi-model intercomparison to evaluate this approach, which we label AM-H<span class="inline-formula">₂</span>SO<span class="inline-formula">₄</span> injection. A coordinated multi-model experiment designed to represent this SO<span class="inline-formula">₃</span>- or H<span class="inline-formula">₂</span>SO<span class="inline-formula">₄</span>-driven geoengineering scenario was carried out with three interactive stratospheric aerosol microphysics models: the National Center for Atmospheric Research (NCAR) Community Earth System Model (CESM2) with the Whole Atmosphere Community Climate Model (WACCM) atmospheric configuration, the Max-Planck Institute's middle atmosphere version of ECHAM5 with the HAM microphysical module (MAECHAM5-HAM) and ETH's SOlar Climate Ozone Links with AER microphysics (SOCOL-AER) coordinated as a test-bed experiment within the Geoengineering Model Intercomparison Project (GeoMIP). The intercomparison explores how the injection of new accumulation-mode particles changes the large-scale particle size distribution and thus the overall radiative and dynamical response to stratospheric sulfur injection. Each model used the same injection scenarios testing AM-H<span class="inline-formula">₂</span>SO<span class="inline-formula">₄</span> and SO<span class="inline-formula">₂</span> injections at 5 and 25 Tg(S) yr<span class="inline-formula">⁻¹</span> to test linearity and climate response sensitivity. All three models find that AM-H<span class="inline-formula">₂</span>SO<span class="inline-formula">₄</span> injection increases the radiative efficacy, defined as the radiative forcing per unit of sulfur injected, relative to SO<span class="inline-formula">₂</span> injection. Increased radiative efficacy means that when compared to the use of SO<span class="inline-formula">₂</span> to produce the same radiative forcing, AM-H<span class="inline-formula">₂</span>SO<span class="inline-formula">₄</span> emissions would reduce side effects of sulfuric acid aerosol geoengineering that are proportional to mass burden. The model studies were carried out with two different idealized geographical distributions of injection mass representing deployment scenarios with different objectives, one designed to force mainly the midlatitudes by injecting into two grid points at 30<span class="inline-formula">^∘</span> N and 30<span class="inline-formula">^∘</span> S, and the other designed to maximize aerosol residence time by injecting uniformly in the region between 30<span class="inline-formula">^∘</span> S and 30<span class="inline-formula">^∘</span> N. Analysis of aerosol size distributions in the perturbed stratosphere of the models shows that particle sizes evolve differently in response to concentrated versus dispersed injections depending on the form of the injected sulfur (SO<span class="inline-formula">₂</span> gas or AM-H<span class="inline-formula">₂</span>SO<span class="inline-formula">₄</span> particulate) and suggests that prior model results for concentrated injection of SO<span class="inline-formula">₂</span> may be strongly dependent on model resolution. Differences among models arise from differences in aerosol formulation and differences in model dynamics, factors whose interplay cannot be easily untangled by this intercomparison.</p>