Dynamical Response of Nonlinear Optical Anisotropy in a Tin Sulfide Crystal under Ultrafast Photoexcitation.

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Analogous to black phosphorus, SnS processes folded structure that shows a strongly anisotropic optical absorption. Herein, by using ultrafast two-color pump and probe spectroscopy, the azimuthal angle dependence of nonlinear optical anisotropy in SnS is investigated. After 390 nm photoexcitation, the reflectivity of the 780 nm probe beam is first reduced significantly, followed by a complex alternation with the rotation of the sample along the c-axis. The relaxation of reflectivity consisted of two components: a 1-3 ps fast process that shows azimuthal angle and pump fluence dependence, which arises from electron-phonon coupling. The slow process shows strongly azimuthal angle dependence, which arises from the recovery of a photoinduced structural change, i.e., from the photoinduced metastable state with Cmcm-like symmetry to the initial state with Pnma symmetry. In addition, a coherent acoustic phonon with a frequency of 40 GHz is also identified, which originates from the temperature gradient-induced strain wave in the SnS crystal.