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We developed a generalized model that considers light as energy contributedthrough the thermalization of excited carriers to generateexcitation-intensity- and temperature-dependent phase diagrams. We find thatthe model replicates the light-induced phase segregation behavior of theMAPb(I,Br)3 system. From there, we sought to study how best to design new,stable, mixed-halide alloys. The resultant first-principles predictions showthat the pseudo halide anion BF4- suppresses phase segregation inFA0.83Cs0.17Pb(I0.6Br0.4)3, resulting in enhanced operating stability. Thefindings reveal that photostability is linked with the structure and electronicproperties of materials and may be overcome using informed alloying strategies.

Coupling photogeneration with thermodynamic modeling of light-induced alloy segregation enables the discovery of stabilizing dopants