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Extent of charge separation and exciton delocalization for electronically excited states in a triphenylamine-C60 donor–acceptor conjugate: a combined molecular dynamics and TD-DFT study

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Abstract

Triphenylamine-pyrrolidine-C60 is a potential material to construct high-efficient dye-sensitized solar cells. A combined molecular dynamics and time-dependent density functional theory study has been carried out to analyze charge separation and exciton delocalization in excited states of two constitutional isomers of this compound. Insight into the intrinsic structure of the excited states is provided. The presence of states with a hybrid excitonic and charge-transfer character is suggested to promote the direct charge separation process by excitation, which could have a significant impact on the efficiency of the light-harvesting species. A greater amount of such hybrid states is found at short distances between the triphenylamine fragment and the C60 cage.

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Acknowledgments

This work has been supported by the Ministerio de Economía y Competitividad (MINECO) of Spain (Projects CTQ2011-26573, CTQ2011-23156/BQU, and CTQ2011-25086) and the Generalitat de Catalunya (Project Number 2014SGR931, Xarxa de Referència en Química Teòrica i Computacional, and ICREA Academia 2009 prize for MS). JPM acknowledges CONACYT for his PhD fellowship (Register/Application Number 217067/312543) and SO the Spanish MINECO for Juan de la Cierva contract and European community for FP7-PEOPLE-2013-CIG-630978 project.

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Authors and Affiliations

  1. Institut de Química Computacional i Catàlisi, Departament de Química, Universitat de Girona, Campus de Montilivi, 17071, Girona, Catalonia, Spain

    Juan Pablo Martínez, Sílvia Osuna, Miquel Solà & Alexander Voityuk

  2. Institució Catalana de Recerca i Estudis Avançats (ICREA), 08010, Barcelona, Spain

    Alexander Voityuk

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  1. Juan Pablo Martínez
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  2. Sílvia Osuna
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  3. Miquel Solà
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  4. Alexander Voityuk
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Correspondence to Miquel Solà.

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Published as part of the special collection of articles derived from the XI Girona Seminar and focused on Carbon, Metal, and Carbon–Metal Clusters.

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Martínez, J.P., Osuna, S., Solà, M. et al. Extent of charge separation and exciton delocalization for electronically excited states in a triphenylamine-C60 donor–acceptor conjugate: a combined molecular dynamics and TD-DFT study. Theor Chem Acc 134, 12 (2015). https://doi.org/10.1007/s00214-015-1614-x

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  • DOI: https://doi.org/10.1007/s00214-015-1614-x

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