Tunable Nonlinearity and Efficient Harmonic Generation from a Strongly
Coupled Light-Matter System
- URL: http://arxiv.org/abs/2203.00691v1
- Date: Tue, 1 Mar 2022 19:00:00 GMT
- Title: Tunable Nonlinearity and Efficient Harmonic Generation from a Strongly
Coupled Light-Matter System
- Authors: Davis M. Welakuh and Prineha Narang
- Abstract summary: We investigate the origins of the experimentally observed enhancement of resonant SHG and THG under strong light-matter coupling.
We find that the enhancement of the nonlinear conversion efficiency has its origins in a modification of the associated nonlinear optical susceptibilities.
Our results pave the way for predicting and understanding quantum nonlinear optical phenomena in strongly coupled light-matter systems.
- Score: 0.0
- License: http://creativecommons.org/licenses/by/4.0/
- Abstract: Strong light-matter coupling within electromagnetic environments provides a
promising path to modify and control chemical and physical processes. The
origin of the enhancement of nonlinear optical processes such as
second-harmonic and third-harmonic generation (SHG and THG) due to strong
light-matter coupling is attributed to distinct physical effects which
questions the relevance of strong coupling in these processes. In this work, we
leverage a first-principles approach to investigate the origins of the
experimentally observed enhancement of resonant SHG and THG under strong
light-matter coupling. We find that the enhancement of the nonlinear conversion
efficiency has its origins in a modification of the associated nonlinear
optical susceptibilities as polaritonic resonances emerge in the nonlinear
spectrum. Further, we find that the nonlinear conversion efficiency can be
tuned by increasing the light-matter coupling strength. Finally, we provide a
general framework to compute the harmonic generation spectra from the
displacement field as opposed to the standard approach which computes the
harmonic spectrum from the matter-only induced polarization. Our results
address a key debate in the field, and pave the way for predicting and
understanding quantum nonlinear optical phenomena in strongly coupled
light-matter systems.
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