Photostrictive Effect and Structure Phase Transition via Nonlinear Photocurrent

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.Comment: 17 pages with 3 figure

Ferroelectricity and Phase Transitions in Monolayer Group-IV Monochalcogenides

Ferroelectricity usually fades away as materials are thinned down below a critical value. We reveal that the unique ionic-potential anharmonicity can induce spontaneous in-plane electrical polarization and ferroelectricity in monolayer group-IV monochalcogenides MX (M=Ge, Sn; X=S, Se). An effective Hamiltonian has been successfully extracted from the parametrized energy space, making it possible to study the ferroelectric phase transitions in a single-atom layer. The ferroelectricity in these materials is found to be robust and the corresponding Curie temperatures are higher than room temperature, making them promising for realizing ultrathin ferroelectric devices of broad interest. We further provide the phase diagram and predict other potentially two-dimensional ferroelectric materials