Expeditious computation of nonlinear optical properties of arbitrary order with native electronic interactions in the time domain

2019/07/31 by Emilia Ridolfi, Paolo E. Trevisanutto, Vitor M. Pereira · 12 citations
Engineering · Materials Science · Mathematics · Physics and Astronomy · #2D Materials and Applications #Algorithm #Computation #Computer science #Coulomb #Electron #Flexibility (engineering) #Laser #Mathematics #Nonlinear system #Perovskite Materials and Applications #Perturbation theory (quantum mechanics) #Physics #Quantum mechanics #Spectroscopy and Quantum Chemical Studies #Statistical physics #Ultrashort pulse #cond-mat.mtrl-sci #cond-mat.str-el

paper · pdf · doi:10.1103/physrevb.102.245110

published in Physical review. B./Physical review. B 102(24) (American Physical Society) · This update contains the published version. 20 pages, 9 figures

openalex publication_date 2020/12/07 · arxiv created 2021/03/01 · arxiv updated 2021/03/02 · openalex created_date 2025/10/10 · openalex updated_date 2026/08/05

Abstract

We adapted a recently proposed framework to characterize the optical response of interacting electrons in solids in order to expedite its computation without compromise in accuracy at the microscopic level. Our formulation is based on reliable parametrizations of Hamiltonians and Coulomb interactions, which allows economy and flexibility in obtaining response functions. It is suited to computing the optical response to fields of arbitrary temporal shape and strength, to arbitrary order in the field, and natively accounts for excitonic effects. We demonstrate the approach by computing the frequency-dependent susceptibilities of MoS₂ and hexagonal BN monolayers up to the third harmonic. Grounded on a generic nonequilibrium many-body perturbation theory, this framework allows extensions to handle generic interaction models or to describe electronic processes taking place at ultrafast time scales.

Citations

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