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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MDPI AG
2019-02-01
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| Series: | Molecules |
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| Online Access: | https://www.mdpi.com/1420-3049/24/3/541 |
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| author | Masayoshi Nakano Kenji Okada Takanori Nagami Takayoshi Tonami Ryohei Kishi Yasutaka Kitagawa |
| author_facet | Masayoshi Nakano Kenji Okada Takanori Nagami Takayoshi Tonami Ryohei Kishi Yasutaka Kitagawa |
| author_sort | Masayoshi Nakano |
| collection | DOAJ |
| 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 (Δ<i>t</i>) and the number of MC trajectories (<i>M</i><sub>C</sub>). 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 Δ<i>t</i> (~0.03 fs) and a sufficiently large <i>M</i><sub>C</sub> (~10<sup>5</sup>). The computational time (<i>t</i><sub>req</sub>) in the MCWF approach also exhibits dramatic reduction with increasing the size of aggregates (<i>N</i>-mers) as compared to that in the QME approach, e.g., ~34 times faster at the 20-mer, and the size-dependence of <i>t</i><sub>req</sub> shows significant reduction from <i>N</i><sup>5.15</sup> (QME) to <i>N</i><sup>3.09</sup> (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. |
| first_indexed | 2024-12-14T20:57:40Z |
| format | Article |
| id | doaj.art-a4a5179f1ec24f12bf652913502d0516 |
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| issn | 1420-3049 |
| language | English |
| last_indexed | 2024-12-14T20:57:40Z |
| publishDate | 2019-02-01 |
| publisher | MDPI AG |
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| series | Molecules |
| spelling | doaj.art-a4a5179f1ec24f12bf652913502d05162022-12-21T22:47:39ZengMDPI AGMolecules1420-30492019-02-0124354110.3390/molecules24030541molecules24030541Monte Carlo Wavefunction Approach to Singlet Fission Dynamics of Molecular AggregatesMasayoshi Nakano0Kenji Okada1Takanori Nagami2Takayoshi Tonami3Ryohei Kishi4Yasutaka Kitagawa5Department of Materials Engineering Science, Graduate School of Engineering Science, Osaka University, Toyonaka, Osaka 560-8531, JapanDepartment of Materials Engineering Science, Graduate School of Engineering Science, Osaka University, Toyonaka, Osaka 560-8531, JapanDepartment of Materials Engineering Science, Graduate School of Engineering Science, Osaka University, Toyonaka, Osaka 560-8531, JapanDepartment of Materials Engineering Science, Graduate School of Engineering Science, Osaka University, Toyonaka, Osaka 560-8531, JapanDepartment of Materials Engineering Science, Graduate School of Engineering Science, Osaka University, Toyonaka, Osaka 560-8531, JapanDepartment of Materials Engineering Science, Graduate School of Engineering Science, Osaka University, Toyonaka, Osaka 560-8531, JapanWe 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 (Δ<i>t</i>) and the number of MC trajectories (<i>M</i><sub>C</sub>). 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 Δ<i>t</i> (~0.03 fs) and a sufficiently large <i>M</i><sub>C</sub> (~10<sup>5</sup>). The computational time (<i>t</i><sub>req</sub>) in the MCWF approach also exhibits dramatic reduction with increasing the size of aggregates (<i>N</i>-mers) as compared to that in the QME approach, e.g., ~34 times faster at the 20-mer, and the size-dependence of <i>t</i><sub>req</sub> shows significant reduction from <i>N</i><sup>5.15</sup> (QME) to <i>N</i><sup>3.09</sup> (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.https://www.mdpi.com/1420-3049/24/3/541Monte Carlo wavefunctionsinglet fissionquantum master equationmolecular aggregate |
| spellingShingle | Masayoshi Nakano Kenji Okada Takanori Nagami Takayoshi Tonami Ryohei Kishi Yasutaka Kitagawa Monte Carlo Wavefunction Approach to Singlet Fission Dynamics of Molecular Aggregates Molecules Monte Carlo wavefunction singlet fission quantum master equation molecular aggregate |
| 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 | Monte Carlo wavefunction singlet fission quantum master equation molecular aggregate |
| url | https://www.mdpi.com/1420-3049/24/3/541 |
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