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Efficient implementation of isotropic cubic response functions for two-photon absorption cross sections within the self-consistent field approximation
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Theoretical Chemistry and Biology.ORCID iD: 0000-0002-8707-3733
Ruprecht Karls Univ Heidelberg, Interdisciplinary Ctr Sci Comp, Neuenheimer Feld 205, D-69120 Heidelberg, Germany..
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Theoretical Chemistry and Biology.ORCID iD: 0000-0003-3992-043X
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Theoretical Chemistry and Biology.ORCID iD: 0000-0002-9123-8174
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2021 (English)In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 154, no 2, article id 024111Article in journal (Refereed) Published
Abstract [en]

Within the self-consistent field approximation, computationally tractable expressions for the isotropic second-order hyperpolarizability have been derived and implemented for the calculation of two-photon absorption cross sections. The novel tensor average formulation presented in this work allows for the evaluation of isotropic damped cubic response functions using only similar to 3.3% (one-photon off-resonance regions) and similar to 10% (one-photon resonance regions) of the number of auxiliary Fock matrices required when explicitly calculating all the needed individual tensor components. Numerical examples of the two-photon absorption cross section in the one-photon off-resonance and resonance regions are provided for alanine-tryptophan and 2,5-dibromo-1,4-bis(2-(4-diphenylaminophenyl)vinyl)-benzene. Furthermore, a benchmark set of 22 additional small- and medium-sized organic molecules is considered. In all these calculations, a quantitative assessment is made of the reduced and approximate forms of the cubic response function in the one-photon off-resonance regions and results demonstrate a relative error of less than similar to 5% when using the reduced expression as compared to the full form of the isotropic cubic response function.

Place, publisher, year, edition, pages
AIP Publishing , 2021. Vol. 154, no 2, article id 024111
National Category
Theoretical Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-289893DOI: 10.1063/5.0031851ISI: 000609824200001PubMedID: 33445884Scopus ID: 2-s2.0-85099407136OAI: oai:DiVA.org:kth-289893DiVA, id: diva2:1528475
Note

QC 20210215

Available from: 2021-02-15 Created: 2021-02-15 Last updated: 2023-10-03Bibliographically approved
In thesis
1. Efficient Calculation of Nonlinear Spectroscopic Properties within the Time-Dependent Density Functional Theory Approximation
Open this publication in new window or tab >>Efficient Calculation of Nonlinear Spectroscopic Properties within the Time-Dependent Density Functional Theory Approximation
2023 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This thesis introduces a novel computational scheme tailored for efficient calculations of nonlinear spectroscopic observables. First, a derivation and implementation of an algorithm designed to harness the linearity of the Fock matrix construction in calculating two-photon absorption cross-sections within the self-consistent field approximation is presented. Subsequently, this computational scheme is extended to the density functional theory approximation for functionals belonging to the generalized gradient approximation. Lastly the derivation and implementation of the nonlinear exchange-correlation kernel for functionals belonging to the meta generalized gradient approximation are presented for the first time.

Collectively, the advancements presented in this thesis contribute new methodologies and insights to the computational realm of nonlinear spectroscopic calculations, offering the potential for large-scale theoretical spectroscopy calculations at the level of density functional theory.

Abstract [sv]

Denna avhandling introducerar en ny beräkningsmetod skräddarsydd för effektiva beräkningar av icke-linjära spektroskopiska observabler. Först presenteras en härledning och implementering av en algoritm utformad för att utnyttja lineariteten i Fock-matrixkonstruktionen vid beräkning av två-fotons absorptions tvärsnitt inom ramen för "the self-consistent field approximation". Därefter utvidgas denna beräkningsmethod till nivån av "density functional theory" för funktionaler som tillhör den generaliserade gradientapproximationen. Slutligen presenteras härledningen och implementeringen av den icke-linjära "exchange-correlation kernelen" för funktionaler som tillhör meta-generaliserade gradientapproximationen för första gången.

Sammantaget bidrar de framsteg som presenteras i denna avhandling med nya metoder och insikter för beräkningen av för icke-linjära spektroskopiska beräkningar, vilket erbjuder potentialen för storskaliga teoretiska spektroskopiberäkningar.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2023. p. 67
Series
TRITA-CBH-FOU ; 2023:46
Keywords
Cubic response, DFT, Response theory
National Category
Theoretical Chemistry
Research subject
Theoretical Chemistry and Biology
Identifiers
urn:nbn:se:kth:diva-337435 (URN)978-91-8040-721-2 (ISBN)
Public defence
2023-10-31, Kollegiesalen, Brinellvägen 6, https://kth-se.zoom.us/j/66109968018, Stockholm, 09:00 (English)
Opponent
Supervisors
Note

QC 20231005

Available from: 2023-10-05 Created: 2023-10-03 Last updated: 2023-10-30Bibliographically approved

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Ahmadzadeh, KaranBrand, ManuelVahtras, OlavLi, XinRinkevicius, ZilvinasNorman, Patrick

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