Photostrictive Effect and Structure Phase Transition via Nonlinear Photocurrent

Abstract: The phenomena of crystal size changes and structural phase transitions induced by light irradiation have garnered significant interest due to their potential for tuning and controlling a wide range of material properties through highly cooperative interactions. However, a microscopic theory that can comprehensively explain these phenomena in correlation with photon frequency and polarization has remained highly desirable. In this work, we propose that nonlinear photocurrent may correspond to driving these effects, which arise from a competition between light-injected energy and structural variations. By conducting first-principles simulations and comparing them with two established experiments, we show that shift current, a second-order photocurrent, can induce photostriction and nonreciprocal structure phase transitions. The quantitative comparisons across key parameters such as light frequency, irradiation time, polarization, and intensity provide further support for the nonlinear photocurrent mechanism. Beyond shift current, this microscopic understanding proposes to utilize more types of nonlinear photocurrent to enhance light-structure interactions and control material properties.