Exciton enhanced nonlinear optical responses in monolayer h-BN and MoS2: Insight from first-principles exciton-state coupling formalism and calculations

Abstract

Excitons are vital in the photophysics of materials, especially in low-dimensional systems. The conceptual and quantitative understanding of excitonic effects in nonlinear optical (NLO) processes is more challenging compared to linear ones. Here, we present an ab initio approach to second-order NLO responses, incorporating excitonic effects, that employs an exciton-state coupling formalism and allows a detailed analysis of the role of individual excitonic states. Taking monolayer h-BN and MoS2 as two prototype 2D materials, we calculate their second harmonic generation (SHG) susceptibility and shift current conductivity tensor. We find strong excitonic enhancement requires that the resonant excitons are not only optically bright themselves, but also be able to couple strongly to other bright excitons. Our results explain the occurrence of two strong peaks in the SHG of monolayer h-BN and why the A and B excitons of MoS2 unexpectedly exhibit minimal excitonic enhancement in both SHG and shift current generation.

References in corpus (4)

• Non-linear Optical Spectroscopy of Excited Exciton States for Efficient Valley Coherence Generation in WSe2 Monolayers
• Optical imaging of strain in two-dimensional crystals
• Topology and geometry under the nonlinear electromagnetic spotlight
• Exciton-Enhanced Spontaneous Parametric Down-Conversion in Two-Dimensional Crystals

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