Author, as appears in the article.: Aguilar Suarez, Luis Enrique; de Graaf, Coen; Faraji, Shirin;
Department: Química Física i Inorgànica
URV's Author/s: De Graaf, Cornelis
Keywords: Thin-film Tetracene State analysis State Singlet fission Pentacene Nonorthogonal configuration-interaction Multiexciton generation Molecules Model Mechanism Gases Excitons Exciton fission Excited states Electronic coupling Electron-hole correlation Dimers Dimer model Descriptors Crystal structure Crystal packings Charge-transfer
Abstract: Singlet fission (SF), a multiexciton generation process, has been proposed as an alternative to enhance the performance of solar cells. The gas phase dimer model has shown its utility to study this process, but it does not always cover all the physics and the effect of the surrounding atoms has to be included in such cases. In this contribution, we explore the influence of crystal packing on the electronic couplings, and on the so-called exciton descriptors and electron-hole correlation plots. We have studied three tetracene dimers extracted from the crystal structure, as well as several dimers and trimers of the alpha and beta polymorphs of 1,3-diphenylisobenzofuran (DPBF). These polymorphs show different SF yields. Our results highlight that the character of the excited states of tetracene depends on both the mutual disposition of molecules and inclusion of the environment. The latter does however not change significantly the interpretation of the SF mechanism in the studied systems. For DPBF, we establish how the excited state analysis is able to pinpoint differences between the polymorphs. We observe strongly bound correlated excitons in the beta polymorph which might hinder the formation of the (TT)-T-1 state and, consequently, explain its low SF yield.
Thematic Areas: Química Physics, atomic, molecular & chemical Physics and astronomy (miscellaneous) Physics and astronomy (all) Physical and theoretical chemistry Odontología Medicina ii Medicina i Materiais Matemática / probabilidade e estatística Interdisciplinar Geociências General physics and astronomy General medicine Farmacia Ensino Engenharias iv Engenharias iii Engenharias ii Ciências biológicas ii Ciências biológicas i Ciências ambientais Ciências agrárias i Ciência de alimentos Ciência da computação Chemistry, physical Biotecnología Biodiversidade Astronomia / física
licence for use: https://creativecommons.org/licenses/by/3.0/es/
Author's mail: coen.degraaf@urv.cat
Author identifier: 0000-0001-8114-6658
Last page: 14177
Record's date: 2024-07-27
Journal volume: 23
Papper version: info:eu-repo/semantics/publishedVersion
Link to the original source: https://pubs.rsc.org/en/content/articlelanding/2021/CP/D1CP00298H#!divAbstract
Licence document URL: https://repositori.urv.cat/ca/proteccio-de-dades/
Papper original source: Physical Chemistry Chemical Physics. 23 (26): 14164-14177
APA: Aguilar Suarez, Luis Enrique; de Graaf, Coen; Faraji, Shirin; (2021). Influence of the crystal packing in singlet fission: one step beyond the gas phase approximation. Physical Chemistry Chemical Physics, 23(26), 14164-14177. DOI: 10.1039/d1cp00298h
Article's DOI: 10.1039/d1cp00298h
Entity: Universitat Rovira i Virgili
Journal publication year: 2021
First page: 14164
Publication Type: Journal Publications
Repositori URV