Accurate Polarization-Resolved Absorption Spectra of Organic Semiconductor Thin Films Using First-Principles Quantum-Chemical Methods: Pentacene as a Case Study

Craciunescu, Luca, Wirsing, Sara, Hammer, Sebastian, Broch, Katharina, Dreuw, Andreas, Fantuzzi, Felipe, Sivanesan, Vipilan, Tegeder, Petra, Engels, Bernd (2022) Accurate Polarization-Resolved Absorption Spectra of Organic Semiconductor Thin Films Using First-Principles Quantum-Chemical Methods: Pentacene as a Case Study. The Journal of Physical Chemistry Letters, 13 (16). pp. 3726-3731. ISSN 1948-7185. (doi:10.1021/acs.jpclett.2c00573) (Access to this publication is currently restricted. You may be able to access a copy if URLs are provided) (KAR id:96270)

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Official URL: https://doi.org/10.1021/acs.jpclett.2c00573

Abstract

Theoretical studies using clusters as model systems have been extremely successful in explaining various photophysical phenomena in organic semiconductor (OSC) thin films. But they have not been able to satisfactorily simulate total and polarization-resolved absorption spectra of OSCs so far. In this work, we demonstrate that accurate spectra are predicted by time-dependent density functional theory (TD-DFT) when the employed cluster reflects the symmetry of the crystal structure and all monomers feel the same environment. Additionally, long-range corrected optimal tuned functionals are mandatory. For pentacene thin films, the computed electronic spectra for thin films then reach an impressive accuracy compared with experimental data with a deviation of less than 0.1 eV. This allows for accurate peak assignments and mechanistic studies, which paves the way for a comprehensive understanding of OSCs using an affordable and easy-to-use cluster approach.

Item Type:	Article
DOI/Identification number:	10.1021/acs.jpclett.2c00573
Divisions:	Divisions > Division of Natural Sciences > Chemistry and Forensics
Depositing User:	Felipe Fantuzzi
Date Deposited:	17 Aug 2022 21:31 UTC
Last Modified:	05 Nov 2024 13:00 UTC
Resource URI:	https://kar.kent.ac.uk/id/eprint/96270 (The current URI for this page, for reference purposes)

University of Kent Author Information

Fantuzzi, Felipe.

Creator's ORCID:	https://orcid.org/0000-0002-8200-8262
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