RPA, an Accurate and Fast Method for the Computation of Static Nonlinear Optical Properties

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Title: RPA, an Accurate and Fast Method for the Computation of Static Nonlinear Optical Properties
Authors: Besalú-Sala, Pau | Bruneval, Fabien | Pérez-Jiménez, Ángel J. | Sancho-Garcia, Juan-Carlos | Rodríguez-Mayorga, Mauricio
Research Group/s: Química Cuántica
Center, Department or Service: Universidad de Alicante. Departamento de Química Física
Keywords: Random Phase Approximation (RPA) | Static Nonlinear Optical Properties | Computation
Issue Date: 11-Sep-2023
Publisher: American Chemical Society
Citation: Journal of Chemical Theory and Computation. 2023, 19(18): 6062-6069. https://doi.org/10.1021/acs.jctc.3c00674
Abstract: The accurate computation of static nonlinear optical properties (SNLOPs) in large polymers requires accounting for electronic correlation effects with a reasonable computational cost. The Random Phase Approximation (RPA) used in the adiabatic connection fluctuation theorem is known to be a reliable and cost-effective method to render electronic correlation effects when combined with density-fitting techniques and integration over imaginary frequencies. We explore the ability of the RPA energy expression to predict SNLOPs by evaluating RPA electronic energies in the presence of finite electric fields to obtain (using the finite difference method) static polarizabilities and hyperpolarizabilities. We show that the RPA based on hybrid functional self-consistent field calculations yields accurate SNLOPs as the best-tuned double-hybrid functionals developed today, with the additional advantage that the RPA avoids any system-specific adjustment.
Sponsor: A.J.P.-J., J.C.S.-G., and M.R.-M. acknowledge the Ministerio de Ciencia e Innovación de España for Grant No. PID2019-106114GB-I00. P.B.-S. acknowledges the financial support received from the Vrije Universiteit Amsterdam. F.B. and M.R.-M. acknowledge the financial support provided by the Cross-Disciplinary Program on Numerical Simulation of the French Alternative Energies and Atomic Energy Commission (CEA) (ABIDM project).
URI: http://hdl.handle.net/10045/137181
ISSN: 1549-9618 (Print) | 1549-9626 (Online)
DOI: 10.1021/acs.jctc.3c00674
Language: eng
Type: info:eu-repo/semantics/article
Rights: © 2023 American Chemical Society
Peer Review: si
Publisher version: https://doi.org/10.1021/acs.jctc.3c00674
Appears in Collections:INV - QC - Artículos de Revistas

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