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Accurate polarization-resolved absorption spectra of organic semiconductor thin films using first-principles quantum-chemical methods: Pentacene as a case study

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 thi...

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Main Authors: Craciunescu, Luca (Author) , Wirsing, Sara (Author) , Hammer, Sebastian (Author) , Broch, Katharina (Author) , Dreuw, Andreas (Author) , Fantuzzi, Felipe (Author) , Sivanesan, Vipilan (Author) , Tegeder, Petra (Author) , Engels, Bernd (Author)
Format: Article (Journal)
Language:English
Published: April 20, 2022
In: The journal of physical chemistry letters
Year: 2022, Volume: 13, Issue: 16, Pages: 3726-3731
ISSN:1948-7185
DOI:10.1021/acs.jpclett.2c00573
Online Access:Verlag, lizenzpflichtig, Volltext: https://doi.org/10.1021/acs.jpclett.2c00573
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Author Notes:Luca Craciunescu, Sara Wirsing, Sebastian Hammer, Katharina Broch, Andreas Dreuw, Felipe Fantuzzi, Vipilan Sivanesan, Petra Tegeder, and Bernd Engels
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Summary: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 Description:Gesehen am 23.06.2022
Physical Description:Online Resource
ISSN:1948-7185
DOI:10.1021/acs.jpclett.2c00573

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