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Monte Carlo Wavefunction Approach to Singlet Fission Dynamics of Molecular Aggregates

We have developed a Monte Carlo wavefunction (MCWF) approach to the singlet fission (SF) dynamics of linear aggregate models composed of monomers with weak diradical character. As an example, the SF dynamics for a pentacene dimer model is investigated by considering the intermolecular electronic cou...

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Detalles Bibliográficos
Autores principales: Nakano, Masayoshi, Okada, Kenji, Nagami, Takanori, Tonami, Takayoshi, Kishi, Ryohei, Kitagawa, Yasutaka
Formato: Online Artículo Texto
Lenguaje:English
Publicado: MDPI 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6384917/
https://www.ncbi.nlm.nih.gov/pubmed/30717244
http://dx.doi.org/10.3390/molecules24030541
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author Nakano, Masayoshi
Okada, Kenji
Nagami, Takanori
Tonami, Takayoshi
Kishi, Ryohei
Kitagawa, Yasutaka
author_facet Nakano, Masayoshi
Okada, Kenji
Nagami, Takanori
Tonami, Takayoshi
Kishi, Ryohei
Kitagawa, Yasutaka
author_sort Nakano, Masayoshi
collection PubMed
description We have developed a Monte Carlo wavefunction (MCWF) approach to the singlet fission (SF) dynamics of linear aggregate models composed of monomers with weak diradical character. As an example, the SF dynamics for a pentacene dimer model is investigated by considering the intermolecular electronic coupling and the vibronic coupling. By comparing with the results by the quantum master equation (QME) approach, we clarify the dependences of the MCWF results on the time step (Δt) and the number of MC trajectories (M(C)). The SF dynamics by the MCWF approach is found to quantitatively (within an error of 0.02% for SF rate and of 0.005% for double-triplet (TT) yield) reproduce that by the QME approach when using a sufficiently small Δt (~0.03 fs) and a sufficiently large M(C) (~10(5)). The computational time (t(req)) in the MCWF approach also exhibits dramatic reduction with increasing the size of aggregates (N-mers) as compared to that in the QME approach, e.g., ~34 times faster at the 20-mer, and the size-dependence of t(req) shows significant reduction from N(5.15) (QME) to N(3.09) (MCWF). These results demonstrate the promising high performance of the MCWF approach to the SF dynamics in extended multiradical molecular aggregates including a large number of quantum dissipation, e.g., vibronic coupling, modes.
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spelling pubmed-63849172019-02-23 Monte Carlo Wavefunction Approach to Singlet Fission Dynamics of Molecular Aggregates Nakano, Masayoshi Okada, Kenji Nagami, Takanori Tonami, Takayoshi Kishi, Ryohei Kitagawa, Yasutaka Molecules Article We have developed a Monte Carlo wavefunction (MCWF) approach to the singlet fission (SF) dynamics of linear aggregate models composed of monomers with weak diradical character. As an example, the SF dynamics for a pentacene dimer model is investigated by considering the intermolecular electronic coupling and the vibronic coupling. By comparing with the results by the quantum master equation (QME) approach, we clarify the dependences of the MCWF results on the time step (Δt) and the number of MC trajectories (M(C)). The SF dynamics by the MCWF approach is found to quantitatively (within an error of 0.02% for SF rate and of 0.005% for double-triplet (TT) yield) reproduce that by the QME approach when using a sufficiently small Δt (~0.03 fs) and a sufficiently large M(C) (~10(5)). The computational time (t(req)) in the MCWF approach also exhibits dramatic reduction with increasing the size of aggregates (N-mers) as compared to that in the QME approach, e.g., ~34 times faster at the 20-mer, and the size-dependence of t(req) shows significant reduction from N(5.15) (QME) to N(3.09) (MCWF). These results demonstrate the promising high performance of the MCWF approach to the SF dynamics in extended multiradical molecular aggregates including a large number of quantum dissipation, e.g., vibronic coupling, modes. MDPI 2019-02-01 /pmc/articles/PMC6384917/ /pubmed/30717244 http://dx.doi.org/10.3390/molecules24030541 Text en © 2019 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).
spellingShingle Article
Nakano, Masayoshi
Okada, Kenji
Nagami, Takanori
Tonami, Takayoshi
Kishi, Ryohei
Kitagawa, Yasutaka
Monte Carlo Wavefunction Approach to Singlet Fission Dynamics of Molecular Aggregates
title Monte Carlo Wavefunction Approach to Singlet Fission Dynamics of Molecular Aggregates
title_full Monte Carlo Wavefunction Approach to Singlet Fission Dynamics of Molecular Aggregates
title_fullStr Monte Carlo Wavefunction Approach to Singlet Fission Dynamics of Molecular Aggregates
title_full_unstemmed Monte Carlo Wavefunction Approach to Singlet Fission Dynamics of Molecular Aggregates
title_short Monte Carlo Wavefunction Approach to Singlet Fission Dynamics of Molecular Aggregates
title_sort monte carlo wavefunction approach to singlet fission dynamics of molecular aggregates
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6384917/
https://www.ncbi.nlm.nih.gov/pubmed/30717244
http://dx.doi.org/10.3390/molecules24030541
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