Theory of second harmonic generation in few-layered MoS2

Recent experimental results have demonstrated the ability of monolayer MoS$_2$ to efficiently generate second harmonic fields with susceptibilities between 0.1 and 100 nm/V. However, no theoretical calculations exist with which to interpret these findings. In particular, it is of interest to theoretically estimate the modulus of the second harmonic response, since experimental reports on this differ by almost three orders of magnitude. Here, we present single-particle calculations of the second harmonic response based on a tight-binding band structure. We compare directly with recent experimental findings and include in the discussion also spectral features and the effects of multiple layers.

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