Chemo-mechanical coupling stabilizes mixed ${\mathrm{Ag}}_x{\mathrm{Cu}}_{1-x}{\mathrm{GaSe}}_2$ solar-cell absorbers: Insights from Monte-Carlo simulations assisted by ab initio informed machine-learning potentials

Abstract

Alloying Ag into Cu(In,Ga)Se${}_2$ has enabled record solar-cell efficiencies ($\sim 23.6\%$), yet their long-term stability remains in question because initio calculations predict a Ag-Cu miscibility gap near ambient temperature. By off-lattice Monte-Carlo simulations using a newly developed machine learning (ML) interatomic potential we show that the presence of coherency strain is resolving the controversy between experimental observations and the predicted phase stability. Incorporating elastic energy contributions present in a coherent setup results in complete Ag-Cu miscibility, whereas the expected phase separation occurs in the absence of coherency strains with respect to the end boundary phases, which are mimicked by an incoherent interface with misfit dislocations. The developed ML-MC framework provides a novel approach for resolving discrepancies in thermodynamic stability for systems where mechanical and chemical effects compete.

14 pages, 7 figures