Nonlinear Optical Properties of Transition Metal Dichalcogenide MX${}_2$ (M = Mo, W; X = S, Se) Monolayers and Trilayers from First-principles Calculations

Abstract

Due to the absence of interlayer coupling and inversion symmetry, transition metal dichalcogenide (MX${}_2$) semiconductor monolayers exhibit novel properties that are distinctly different from their bulk crystals such as direct optical band gaps, large band spin splittings, spin-valley coupling, piezoelectric and nonlinear optical responses, and thus have promising applications in, e.g., opto-electronic and spintronic devices. Here we have performed a systematic first-principles study of the second-order nonlinear optical properties of MX${}_2$ (M = Mo, W; X = S, Se) monolayers and trilayers within the density functional theory with the generalized gradient approximation plus scissors correction. We find that all the four MX${}_2$ monolayers possess large second-order optical susceptibility ${\chi }^{(2)}$ in the optical frequency range and significant linear electro-optical coefficients in low frequency limit, thus indicating their potential applications in non-linear optical devices and electric optical switches. The ${\chi }^{(2)}$ spectra of the MX${}_2$ trilayers are overall similar to the corresponding MX${}_2$ monolayers, {\it albeit} with the magnitude reduced by roughly a factor of 3. The prominent features in the ${\chi }^{(2)}$ spectra of the MX${}_2$ multilayers are analyzed in terms of the underlying band structures and optical dielectric function, and also compared with available experiments.

arXiv commentreferences updated, new Figure 2, revised Figure 8 and text improved

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