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Light-induced mechanical deformations in single-domain (PbTiO)/(SrTiO) superlattices were simulated using first-principle calculations. By varying the chemical fraction PbTiO, we discover that these heterostructures’ photostrictive behavior can be tuned quantitatively and qualitatively. Additionally, we present simple analytical models to explain the calculated deformations and predict a critical PbTiO fraction with no photostriction. In addition to the report in [1], our results present another way for tuning the photostrictive behavior of (PbTiO)/(SrTiO) superlattices, which could be utilized for innovative optomechanical applications.

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