Cluster-Based Approach Utilizing Optimally Tuned TD-DFT to Calculate Absorption Spectra of Organic Semiconductor Thin FilmsClick to copy article linkArticle link copied!
- Luca CraciunescuLuca CraciunescuInstitut für Physikalische und Theoretische Chemie, Julius-Maximilians-Universität Würzburg, Emil-Fischer-Str. 42, 97074 Würzburg, GermanyInstitute of Chemical Sciences, School of Engineering and Physical Sciences, Heriot-Watt University, Edinburgh, EH14 4AS Scotland, U.K.More by Luca Craciunescu
- Maximilian AsbachMaximilian AsbachInstitut für Physikalische und Theoretische Chemie, Julius-Maximilians-Universität Würzburg, Emil-Fischer-Str. 42, 97074 Würzburg, GermanyMore by Maximilian Asbach
- Sara WirsingSara WirsingInstitut für Physikalische und Theoretische Chemie, Julius-Maximilians-Universität Würzburg, Emil-Fischer-Str. 42, 97074 Würzburg, GermanyMore by Sara Wirsing
- Sebastian HammerSebastian HammerExperimentelle Physik VI, Julius-Maximilians-Universität Würzburg, Am Hubland, 97074 Würzburg, GermanyCenter for the Physics of Materials, Department of Physics and Department of Chemistry, McGill University, 801 Sherbrooke St. W, Montreal, H3A 2K6 Québec, CanadaMore by Sebastian Hammer
- Frederik UngerFrederik UngerInstitut für Angewandte Physik, Universität Tübingen, Auf der Morgenstelle 10, 72076 Tübingen, GermanyMore by Frederik Unger
- Katharina BrochKatharina BrochInstitut für Angewandte Physik, Universität Tübingen, Auf der Morgenstelle 10, 72076 Tübingen, GermanyMore by Katharina Broch
- Frank SchreiberFrank SchreiberInstitut für Angewandte Physik, Universität Tübingen, Auf der Morgenstelle 10, 72076 Tübingen, GermanyMore by Frank Schreiber
- Gregor WitteGregor WitteMolekulare Festkörperphysik, Philipps-Universität Marburg, 35032 Marburg, GermanyMore by Gregor Witte
- Andreas DreuwAndreas DreuwInterdisziplinäres Zentrum für Wissenschaftliches Rechnen, Universität Heidelberg, Im Neuenheimer Feld 205, 69120 Heidelberg, GermanyMore by Andreas Dreuw
- Petra TegederPetra TegederPhysikalisch-Chemisches Institut, Universität Heidelberg, Im Neuenheimer Feld 253, 69120 Heidelberg, GermanyMore by Petra Tegeder
- Felipe FantuzziFelipe FantuzziSchool of Chemistry and Forensic Science, University of Kent, Park Wood Rd, CT2 7NH Canterbury, U.K.More by Felipe Fantuzzi
- Bernd Engels*Bernd Engels*Email: [email protected]Institut für Physikalische und Theoretische Chemie, Julius-Maximilians-Universität Würzburg, Emil-Fischer-Str. 42, 97074 Würzburg, GermanyMore by Bernd Engels
Abstract
The photophysics of organic semiconductor (OSC) thin films or crystals has garnered significant attention in recent years since a comprehensive theoretical understanding of the various processes occurring upon photoexcitation is crucial for assessing the efficiency of OSC materials. To date, research in this area has relied on methods using Frenkel–Holstein Hamiltonians, calculations of the GW-Bethe–Salpeter equation with periodic boundaries, or cluster-based approaches using quantum chemical methods, with each of the three approaches having distinct advantages and disadvantages. In this work, we introduce an optimally tuned, range-separated time-dependent density functional theory approach to accurately reproduce the total and polarization-resolved absorption spectra of pentacene, tetracene, and perylene thin films, all representative OSC materials. Our approach achieves excellent agreement with experimental data (mostly ≤0.1 eV) when combined with the utilization of clusters comprising multiple monomers and a standard polarizable continuum model to simulate the thin-film environment. Our protocol therefore addresses a major drawback of cluster-based approaches and makes them attractive tools for OSC investigations. Its key advantages include its independence from external, system-specific fitting parameters and its straightforward application with well-known quantum chemical program codes. It demonstrates how chemical intuition can help to reduce computational cost and still arrive at chemically meaningful and almost quantitative results.
Cited By
This article is cited by 4 publications.
- Frederik Unger, Daniel Lepple, Maximilian Asbach, Luca Craciunescu, Clemens Zeiser, Andreas F. Kandolf, Zbyněk Fišer, Jakub Hagara, Jan Hagenlocher, Stefan Hiller, Sara Haug, Marian Deutsch, Peter Grüninger, Jiří Novák, Holger F. Bettinger, Katharina Broch, Bernd Engels, Frank Schreiber. Optical Absorption Properties in Pentacene/Tetracene Solid Solutions. The Journal of Physical Chemistry A 2024, 128
(4)
, 747-760. https://doi.org/10.1021/acs.jpca.3c06737
- Sebastian Hammer, Tristan L. Britt, Laurenz Kremeyer, Maximilian Rödel, David Cai, Jens Pflaum, Bradley J. Siwick. Excimer formation in zinc-phthalocyanine revealed using ultrafast electron diffraction. Proceedings of the National Academy of Sciences 2024, 121
(51)
https://doi.org/10.1073/pnas.2411975121
- J. T. Kohn, S. Grimme, A. Hansen. A semi-automated quantum-mechanical workflow for the generation of molecular monolayers and aggregates. The Journal of Chemical Physics 2024, 161
(12)
https://doi.org/10.1063/5.0230341
- Jin Zhang, Alejandra Traspas Muiña, Duncan V Mifsud, Zuzana Kaňuchová, Klaudia Cielinska, Péter Herczku, K K Rahul, Sándor T S Kovács, Richárd Rácz, Julia C Santos, Alfred T Hopkinson, Luca Craciunescu, Nykola C Jones, Søren V Hoffmann, Sándor Biri, István Vajda, István Rajta, Anita Dawes, Bhalamurugan Sivaraman, Zoltán Juhász, Béla Sulik, Harold Linnartz, Liv Hornekær, Felipe Fantuzzi, Nigel J Mason, Sergio Ioppolo. A systematic IR and VUV spectroscopic investigation of ion, electron, and thermally processed ethanolamine ice. Monthly Notices of the Royal Astronomical Society 2024, 533
(1)
, 826-840. https://doi.org/10.1093/mnras/stae1860
Article Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.
Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.
The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated.