https://egusphere.copernicus.org/preprints/2024/egusphere-2024-444/

*Authors*
Sandro Vattioni, Rahel Weber, Aryehe Feinberg, Andrea Stenke, John A.
Dykema, Beiping Luo, Georgios A. Kelesidis, Christian A. Bruun, Timofei
Sukhodolov, Frank N. Keutsch, Thomas Peter, and Gabriel Chiodo

*How to cite*. Vattioni, S., Weber, R., Feinberg, A., Stenke, A., Dykema,
J. A., Luo, B., Kelesidis, G. A., Bruun, C. A., Sukhodolov, T., Keutsch, F.
N., Peter, T., and Chiodo, G.: A fully coupled solid particle microphysics
scheme for stratospheric aerosol injections within the
aerosol-chemistry-climate-model SOCOL-AERv2, EGUsphere [preprint],
https://doi.org/10.5194/egusphere-2024-444, 2024.

*Received: 27 Feb 2024 – Discussion started: 15 Apr 2024*

*Abstract*
Recent studies have suggested that injection of solid particles such as
alumina and calcite particles for stratospheric aerosol injection (SAI)
instead of sulfur-based injections could reduce some of the adverse side
effects of SAI such as ozone depletion and stratospheric heating. Here, we
present a version of the global aerosol-chemistry-climate model SOCOL-AERv2
and the Earth System Model (ESM) SOCOLv4 which incorporate a solid particle
microphysics scheme for assessment of SAI of solid particles. Microphysical
interactions of the solid particle with the stratospheric sulfur cycle were
interactively coupled to the heterogeneous chemistry scheme and the
radiative transfer code (RTC) for the first time within an ESM. Therefore,
the model allows simulation of heterogeneous chemistry at the particle
surface as well as feedbacks between microphysics, chemistry, radiation and
climate. We show that sulfur-based SAI results in a doubling of the
stratospheric aerosol burden compared to the same injection rate of calcite
and alumina particles with radius of 240 nm, mainly due to the smaller
density and the smaller average particle size of sulfuric acid aerosols and
thus, slower sedimentation. Therefore, to achieve the same radiative
forcing, larger injection rates are needed for calcite and alumina particle
injection than for sulfur-based SAI. The stratospheric sulfur cycle would
be significantly perturbed, with a reduction in stratospheric sulfuric acid
burden by 53 %, when injecting 5 Mt/yr of alumina or calcite particles of
240 nm radius. We show that alumina particles will acquire a sulfuric acid
coating equivalent of about 10 nm thickness, if the sulfuric acid is
equally distributed over the whole available particle surface area in the
lower stratosphere. However, due to a steep contact angle of sulfuric acid
on alumina particles, the sulfuric acid coating would likely not cover the
entire alumina surface, which would result in available surface for
heterogeneous reactions other than the ones on sulfuric acid. When applying
realistic uptake coefficients of 1.0, 10-5 and 10-4 for H2SO4, HCl and
HNO3, respectively, the same scenario with injections of calcite particles
results in 94 % of the particle mass remaining in the form of CaCO3. This
likely keeps the optical properties of the calcite particles intact, but
could significantly alter the heterogeneous reactions occurring on the
particle surfaces. The major process uncertainties of solid particle SAI
are 1) the solid particle microphysics in the injection plume and degree of
agglomeration of solid particles on the sub-ESM grid scale, 2) the
scattering properties of the resulting agglomerates 3) heterogeneous
chemistry on the particle surface and 4) aerosol-cloud interactions. These
uncertainties can only be addressed with extensive, coordinated,
experimental and modelling research efforts. The model presented in this
work offers a useful tool for sensitivity studies and impact analysis of
new experimental results on points 1) to 3) for SAI of solid particles.


*Source: EGUsphere *

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