Finite-temperature time-dependent variation with multiple Davydov states
The Dirac-Frenkel time-dependent variational approach with Davydov Ansätze is a sophisticated, yet efficient technique to obtain an accurate solution to many-body Schrödinger equations for energy and charge transfer dynamics in molecular aggregates and light-harvesting complexes. We extend this vari...
| Main Authors: | , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
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2017
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| Online Access: | https://hdl.handle.net/10356/83491 http://hdl.handle.net/10220/42591 |
| _version_ | 1826115772433301504 |
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| author | Wang, Lu Fujihashi, Yuta Chen, Lipeng Zhao, Yang |
| author2 | School of Materials Science & Engineering |
| author_facet | School of Materials Science & Engineering Wang, Lu Fujihashi, Yuta Chen, Lipeng Zhao, Yang |
| author_sort | Wang, Lu |
| collection | NTU |
| description | The Dirac-Frenkel time-dependent variational approach with Davydov Ansätze is a sophisticated, yet efficient technique to obtain an accurate solution to many-body Schrödinger equations for energy and charge transfer dynamics in molecular aggregates and light-harvesting complexes. We extend this variational approach to finite temperature dynamics of the spin-boson model by adopting a Monte Carlo importance sampling method. In order to demonstrate the applicability of this approach, we compare calculated real-time quantum dynamics of the spin-boson model with that from numerically exact iterative quasiadiabatic propagator path integral (QUAPI) technique. The comparison shows that our variational approach with the single Davydov Ansätze is in excellent agreement with the QUAPI method at high temperatures, while the two differ at low temperatures. Accuracy in dynamics calculations employing a multitude of Davydov trial states is found to improve substantially over the single Davydov Ansatz, especially at low temperatures. At a moderate computational cost, our variational approach with the multiple Davydov Ansatz is shown to provide accurate spin-boson dynamics over a wide range of temperatures and bath spectral densities. |
| first_indexed | 2024-10-01T04:00:38Z |
| format | Journal Article |
| id | ntu-10356/83491 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T04:00:38Z |
| publishDate | 2017 |
| record_format | dspace |
| spelling | ntu-10356/834912023-07-14T15:49:24Z Finite-temperature time-dependent variation with multiple Davydov states Wang, Lu Fujihashi, Yuta Chen, Lipeng Zhao, Yang School of Materials Science & Engineering Coherent states Wave functions The Dirac-Frenkel time-dependent variational approach with Davydov Ansätze is a sophisticated, yet efficient technique to obtain an accurate solution to many-body Schrödinger equations for energy and charge transfer dynamics in molecular aggregates and light-harvesting complexes. We extend this variational approach to finite temperature dynamics of the spin-boson model by adopting a Monte Carlo importance sampling method. In order to demonstrate the applicability of this approach, we compare calculated real-time quantum dynamics of the spin-boson model with that from numerically exact iterative quasiadiabatic propagator path integral (QUAPI) technique. The comparison shows that our variational approach with the single Davydov Ansätze is in excellent agreement with the QUAPI method at high temperatures, while the two differ at low temperatures. Accuracy in dynamics calculations employing a multitude of Davydov trial states is found to improve substantially over the single Davydov Ansatz, especially at low temperatures. At a moderate computational cost, our variational approach with the multiple Davydov Ansatz is shown to provide accurate spin-boson dynamics over a wide range of temperatures and bath spectral densities. NRF (Natl Research Foundation, S’pore) MOE (Min. of Education, S’pore) Published version 2017-06-06T08:16:20Z 2019-12-06T15:24:09Z 2017-06-06T08:16:20Z 2019-12-06T15:24:09Z 2017 Journal Article Wang, L., Fujihashi, Y., Chen, L., & Zhao, Y. (2017). Finite-temperature time-dependent variation with multiple Davydov states. The Journal of Chemical Physics, 146(12), 124127-. 0021-9606 https://hdl.handle.net/10356/83491 http://hdl.handle.net/10220/42591 10.1063/1.4979017 en The Journal of Chemical Physics © 2017 American Institute of Physics (AIP). This paper was published in The Journal of Chemical Physics and is made available as an electronic reprint (preprint) with permission of American Institute of Physics (AIP). The published version is available at: [http://dx.doi.org/10.1063/1.4979017]. One print or electronic copy may be made for personal use only. Systematic or multiple reproduction, distribution to multiple locations via electronic or other means, duplication of any material in this paper for a fee or for commercial purposes, or modification of the content of the paper is prohibited and is subject to penalties under law. 8 p. application/pdf |
| spellingShingle | Coherent states Wave functions Wang, Lu Fujihashi, Yuta Chen, Lipeng Zhao, Yang Finite-temperature time-dependent variation with multiple Davydov states |
| title | Finite-temperature time-dependent variation with multiple Davydov states |
| title_full | Finite-temperature time-dependent variation with multiple Davydov states |
| title_fullStr | Finite-temperature time-dependent variation with multiple Davydov states |
| title_full_unstemmed | Finite-temperature time-dependent variation with multiple Davydov states |
| title_short | Finite-temperature time-dependent variation with multiple Davydov states |
| title_sort | finite temperature time dependent variation with multiple davydov states |
| topic | Coherent states Wave functions |
| url | https://hdl.handle.net/10356/83491 http://hdl.handle.net/10220/42591 |
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