Unexpected increase of intensity-dependent excitonic second- and third-harmonic generation induced by static electric fields

TL;DR

This paper investigates how static electric fields influence intensity-dependent excitonic second- and third-harmonic generation in MoS2, revealing superlinear increases and complex dependencies due to multiple nonlinear effects.

Contribution

It provides a detailed microscopic analysis of the nonlinear optical response of excitons under static electric fields, highlighting new control mechanisms for excitonic nonlinearities.

Findings

THG increases with static field at high excitation intensities

SHG shows superlinear growth with static field

Complex dependencies due to Stark shifts and exciton ionization

Abstract

We compute and analyze the dependence of excitonic second- and third-harmonic generation (SHG/THG) as a function of the optical excitation intensity in the presence of static electric fields by solving the semiconductor Bloch equations. Our simulations are performed for excitation of the strongly bound intralayer exciton of an inversion-symmetric homobilayer of MoS2 with in-plane electric fields. We demonstrate that for resonant excitation at the 1s K-exciton the SHG and the THG show complex dependencies on both the strength of the static field and the peak amplitude of the optical pulse. For sufficiently intense optical excitation, the THG increases and the SHG increases superlinearly with the amplitude of the static field as long as exciton ionization is not yet dominating. Microscopic simulations demonstrate that these dependencies arise from an interplay between several effects including static and transient Stark shifts, exciton ionization, Wannier-Stark localization, off-resonant Rabi oscillations, and a modified interference between optical nonlinearities induced by the intraband acceleration. Our findings offer several new possibilities for controlling the strong-field dynamics of systems with strongly bound excitons.