An ab initio method on large sized molecular aggregate system: Predicting absorption spectra of crystalline organic semiconducting films

Wenlan Liu; Denis Andrienko

doi:10.1063/5.0138748

An ab initio method on large sized molecular aggregate system: Predicting absorption spectra of crystalline organic semiconducting films

Wenlan Liu, Denis Andrienko

Research output: Contribution to journal › Article › peer-review

7 Scopus citations

Abstract

Theoretical description of electronic excited states of molecular aggregates at an {\em ab initio} level is computationally demanding. To reduce the computational cost, we propose a model Hamiltonian (MH) approach that approximates the electronically excited state wavefunction of the molecular aggregate. We benchmark our approach on a thiophene hexamer, as well as calculate the absorption spectra of several crystalline non-fullerene acceptors (NFAs), including Y6 and ITIC, which are known for their high power conversion efficiency in organic solar cells. The method qualitatively predicts the experimentally measured spectral shape, which can be further linked to the molecular arrangement in the unit cell.

Original language	English (US)
Journal	The Journal of chemical physics
DOIs	https://doi.org/10.1063/5.0138748
State	Published - Feb 13 2023
Externally published	Yes

Bibliographical note

KAUST Repository Item: Exported on 2023-02-17
Acknowledged KAUST grant number(s): OSRCRG2018-3746, OSR-2018-CARF/CCF-3079
Acknowledgements: This publication is based on work supported by the KAUST Office of Sponsored Research (OSR) under award nos. OSR-2018-CARF/CCF-3079 and OSRCRG2018-3746. W. L. acknowledges the National Natural Science Foundation of China (Project 21703023) for financial support. D.A. also acknowledges the KAUST PSE Division for hosting his sabbatical in the framework of the Divisions Visiting Faculty program. D.A. acknowledges funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) for financial support through the collaborative research centers TRR 146, SPP 2196, and grant number 460766640. We thank KunHan Lin, Mukunda Mandal, Andriy Zhugayevych, and Naomi Kinaret for fruitful discussions and proof-reading of the manuscript.
This publication acknowledges KAUST support, but has no KAUST affiliated authors.

ASJC Scopus subject areas

General Physics and Astronomy
Physical and Theoretical Chemistry

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title = "An ab initio method on large sized molecular aggregate system: Predicting absorption spectra of crystalline organic semiconducting films",

abstract = "Theoretical description of electronic excited states of molecular aggregates at an {\em ab initio} level is computationally demanding. To reduce the computational cost, we propose a model Hamiltonian (MH) approach that approximates the electronically excited state wavefunction of the molecular aggregate. We benchmark our approach on a thiophene hexamer, as well as calculate the absorption spectra of several crystalline non-fullerene acceptors (NFAs), including Y6 and ITIC, which are known for their high power conversion efficiency in organic solar cells. The method qualitatively predicts the experimentally measured spectral shape, which can be further linked to the molecular arrangement in the unit cell.",

author = "Wenlan Liu and Denis Andrienko",

note = "KAUST Repository Item: Exported on 2023-02-17 Acknowledged KAUST grant number(s): OSRCRG2018-3746, OSR-2018-CARF/CCF-3079 Acknowledgements: This publication is based on work supported by the KAUST Office of Sponsored Research (OSR) under award nos. OSR-2018-CARF/CCF-3079 and OSRCRG2018-3746. W. L. acknowledges the National Natural Science Foundation of China (Project 21703023) for financial support. D.A. also acknowledges the KAUST PSE Division for hosting his sabbatical in the framework of the Divisions Visiting Faculty program. D.A. acknowledges funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) for financial support through the collaborative research centers TRR 146, SPP 2196, and grant number 460766640. We thank KunHan Lin, Mukunda Mandal, Andriy Zhugayevych, and Naomi Kinaret for fruitful discussions and proof-reading of the manuscript. This publication acknowledges KAUST support, but has no KAUST affiliated authors.",

year = "2023",

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doi = "10.1063/5.0138748",

language = "English (US)",

journal = "The Journal of chemical physics",

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AU - Liu, Wenlan

AU - Andrienko, Denis

N1 - KAUST Repository Item: Exported on 2023-02-17 Acknowledged KAUST grant number(s): OSRCRG2018-3746, OSR-2018-CARF/CCF-3079 Acknowledgements: This publication is based on work supported by the KAUST Office of Sponsored Research (OSR) under award nos. OSR-2018-CARF/CCF-3079 and OSRCRG2018-3746. W. L. acknowledges the National Natural Science Foundation of China (Project 21703023) for financial support. D.A. also acknowledges the KAUST PSE Division for hosting his sabbatical in the framework of the Divisions Visiting Faculty program. D.A. acknowledges funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) for financial support through the collaborative research centers TRR 146, SPP 2196, and grant number 460766640. We thank KunHan Lin, Mukunda Mandal, Andriy Zhugayevych, and Naomi Kinaret for fruitful discussions and proof-reading of the manuscript. This publication acknowledges KAUST support, but has no KAUST affiliated authors.

PY - 2023/2/13

Y1 - 2023/2/13

N2 - Theoretical description of electronic excited states of molecular aggregates at an {\em ab initio} level is computationally demanding. To reduce the computational cost, we propose a model Hamiltonian (MH) approach that approximates the electronically excited state wavefunction of the molecular aggregate. We benchmark our approach on a thiophene hexamer, as well as calculate the absorption spectra of several crystalline non-fullerene acceptors (NFAs), including Y6 and ITIC, which are known for their high power conversion efficiency in organic solar cells. The method qualitatively predicts the experimentally measured spectral shape, which can be further linked to the molecular arrangement in the unit cell.

AB - Theoretical description of electronic excited states of molecular aggregates at an {\em ab initio} level is computationally demanding. To reduce the computational cost, we propose a model Hamiltonian (MH) approach that approximates the electronically excited state wavefunction of the molecular aggregate. We benchmark our approach on a thiophene hexamer, as well as calculate the absorption spectra of several crystalline non-fullerene acceptors (NFAs), including Y6 and ITIC, which are known for their high power conversion efficiency in organic solar cells. The method qualitatively predicts the experimentally measured spectral shape, which can be further linked to the molecular arrangement in the unit cell.

UR - http://hdl.handle.net/10754/687825

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DO - 10.1063/5.0138748

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SN - 0021-9606

JO - The Journal of chemical physics

JF - The Journal of chemical physics

ER -

An ab initio method on large sized molecular aggregate system: Predicting absorption spectra of crystalline organic semiconducting films

Abstract

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