Publication

Singlet fission in tetracene: An excited state analysis

Suarez, L. E. A., Menger, M. F. S. J. & Faraji, S., 26-May-2020, In : Molecular Physics. 21-22, 14 p., e1769870.

Research output: Contribution to journalArticleAcademicpeer-review

APA

Suarez, L. E. A., Menger, M. F. S. J., & Faraji, S. (2020). Singlet fission in tetracene: An excited state analysis. Molecular Physics, (21-22), [e1769870]. https://doi.org/10.1080/00268976.2020.1769870

Author

Suarez, Luis Enrique Aguilar ; Menger, Maximilian F. S. J. ; Faraji, Shirin. / Singlet fission in tetracene : An excited state analysis. In: Molecular Physics. 2020 ; No. 21-22.

Harvard

Suarez, LEA, Menger, MFSJ & Faraji, S 2020, 'Singlet fission in tetracene: An excited state analysis', Molecular Physics, no. 21-22, e1769870. https://doi.org/10.1080/00268976.2020.1769870

Standard

Singlet fission in tetracene : An excited state analysis. / Suarez, Luis Enrique Aguilar; Menger, Maximilian F. S. J.; Faraji, Shirin.

In: Molecular Physics, No. 21-22, e1769870, 26.05.2020.

Research output: Contribution to journalArticleAcademicpeer-review

Vancouver

Suarez LEA, Menger MFSJ, Faraji S. Singlet fission in tetracene: An excited state analysis. Molecular Physics. 2020 May 26;(21-22). e1769870. https://doi.org/10.1080/00268976.2020.1769870


BibTeX

@article{7eb968ad89c646f7827ba9e1823624a0,
title = "Singlet fission in tetracene: An excited state analysis",
abstract = "Singlet fission is a potential mechanism to enhance the performance of current solar cells. However, the actual mechanism is still a matter of debate, with charge transfer states believed to play an essential role. The probability of the overall process can be related to the electronic coupling between the electronic states. Here, we explore the excited states of three pairs of tetracene with different relative orientation in the crystal structure showing different electronic couplings and identify the role of charge transfer states. First, a suitable theoretical method for the study of the tetracene pairs is determined by comparing time-dependent density functional theory with wave function-based methods in terms of excitation energies, so-called exciton descriptors, and graphical tools such as electron-hole correlation plots and natural transition orbitals. The results show the presence of low-lying charge transfer states in those tetracene pairs with non-zero electronic coupling, suggesting a superexchange-mediated mechanism, and high-lying charge resonance states for the pair with zero electronic coupling. Finally, the lower electron-hole correlation coefficients for pairs with non-zero coupling speak in favour of the superexchange-mediated mechanism, as a weaker Coulombic attraction due to the mixing with charge transfer states further facilitates the formation of the (Formula presented.) state from the photoexcited molecule.",
keywords = "Singlet fission, tetracene, exciton analysis, exciton descriptors, EXCHANGE, PACKAGE",
author = "Suarez, {Luis Enrique Aguilar} and Menger, {Maximilian F. S. J.} and Shirin Faraji",
year = "2020",
month = may,
day = "26",
doi = "10.1080/00268976.2020.1769870",
language = "English",
journal = "Molecular Physics",
issn = "0026-8976",
publisher = "Taylor & Francis Ltd",
number = "21-22",

}

RIS

TY - JOUR

T1 - Singlet fission in tetracene

T2 - An excited state analysis

AU - Suarez, Luis Enrique Aguilar

AU - Menger, Maximilian F. S. J.

AU - Faraji, Shirin

PY - 2020/5/26

Y1 - 2020/5/26

N2 - Singlet fission is a potential mechanism to enhance the performance of current solar cells. However, the actual mechanism is still a matter of debate, with charge transfer states believed to play an essential role. The probability of the overall process can be related to the electronic coupling between the electronic states. Here, we explore the excited states of three pairs of tetracene with different relative orientation in the crystal structure showing different electronic couplings and identify the role of charge transfer states. First, a suitable theoretical method for the study of the tetracene pairs is determined by comparing time-dependent density functional theory with wave function-based methods in terms of excitation energies, so-called exciton descriptors, and graphical tools such as electron-hole correlation plots and natural transition orbitals. The results show the presence of low-lying charge transfer states in those tetracene pairs with non-zero electronic coupling, suggesting a superexchange-mediated mechanism, and high-lying charge resonance states for the pair with zero electronic coupling. Finally, the lower electron-hole correlation coefficients for pairs with non-zero coupling speak in favour of the superexchange-mediated mechanism, as a weaker Coulombic attraction due to the mixing with charge transfer states further facilitates the formation of the (Formula presented.) state from the photoexcited molecule.

AB - Singlet fission is a potential mechanism to enhance the performance of current solar cells. However, the actual mechanism is still a matter of debate, with charge transfer states believed to play an essential role. The probability of the overall process can be related to the electronic coupling between the electronic states. Here, we explore the excited states of three pairs of tetracene with different relative orientation in the crystal structure showing different electronic couplings and identify the role of charge transfer states. First, a suitable theoretical method for the study of the tetracene pairs is determined by comparing time-dependent density functional theory with wave function-based methods in terms of excitation energies, so-called exciton descriptors, and graphical tools such as electron-hole correlation plots and natural transition orbitals. The results show the presence of low-lying charge transfer states in those tetracene pairs with non-zero electronic coupling, suggesting a superexchange-mediated mechanism, and high-lying charge resonance states for the pair with zero electronic coupling. Finally, the lower electron-hole correlation coefficients for pairs with non-zero coupling speak in favour of the superexchange-mediated mechanism, as a weaker Coulombic attraction due to the mixing with charge transfer states further facilitates the formation of the (Formula presented.) state from the photoexcited molecule.

KW - Singlet fission

KW - tetracene

KW - exciton analysis

KW - exciton descriptors

KW - EXCHANGE

KW - PACKAGE

U2 - 10.1080/00268976.2020.1769870

DO - 10.1080/00268976.2020.1769870

M3 - Article

JO - Molecular Physics

JF - Molecular Physics

SN - 0026-8976

IS - 21-22

M1 - e1769870

ER -

ID: 128250641