Exciton Enhanced Nonlinear Optical Responses in Monolayer h-BN and MoS2: Insight from First-Principles Exciton-State Coupling Formalism and Calculations

Ruan, Jiawei; Chan, Yang-Hao; Louie, Steven G.

doi:10.1021/acs.nanolett.4c03434

Title: Exciton Enhanced Nonlinear Optical Responses in Monolayer h-BN and MoS₂: Insight from First-Principles Exciton-State Coupling Formalism and Calculations

Journal Article · 18 November 2024 · Nano Letters

DOI: https://doi.org/10.1021/acs.nanolett.4c03434 · OSTI ID:2480697

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University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
National Center of Theoretical Sciences, Taipei (Taiwan); Academia Sinica, Taipei (Taiwan)

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 for 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 in the NLO responses requires that the resonant excitons are not only optically bright themselves but also 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.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 2480697

Journal Information:: Nano Letters, Journal Name: Nano Letters Journal Issue: 49 Vol. 24; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Exciton Enhanced Nonlinear Optical Responses in Monolayer h-BN and MoS2: Insight from First-Principles Exciton-State Coupling Formalism and Calculations

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Title: Exciton Enhanced Nonlinear Optical Responses in Monolayer h-BN and MoS₂: Insight from First-Principles Exciton-State Coupling Formalism and Calculations