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We report the observations of unexpected layer-dependent, strong, andanisotropic second harmonic generations (SHGs) in atomically thin ReS2.Appreciable (negligible) SHGs are obtained from even (odd) numbers of ReS2layers, which is opposite to the layer-dependence of SHGs in group VItransition metal dichalcogenides, such as MoS2 and WS2. The results areanalyzed from ReS2's crystal structure, implying second harmonic polarizationsgenerated from the interlayer coupling. Pumped by a telecomband laser, SHG fromthe bilayer ReS2 is almost one order of magnitude larger than that from themonolayer WS2. The estimated second-order nonlinear susceptibility of 900 pm/Vis remarkably high among those reported in two-dimensional materials. The laserpolarization dependence of ReS2's SHG is strongly anisotropic and indicates itsdistorted lattice structure with more unequal and non-zero second-ordersusceptibility elements.

Extraordinary second harmonic generation in ReS2 atomic crystals