Davydov Ansatz as an efficient tool for the simulation of nonlinear optical response of molecular aggregates
We have developed a variational approach to the description of four-wave-mixing signals of molecular aggregates, in which the third-order response functions are evaluated in terms of the Davydov Ansätze. Our theory treats both singly and doubly excited excitonic states, handling the contributions du...
| Main Authors: | , , , |
|---|---|
| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2015
|
| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/79390 http://hdl.handle.net/10220/25928 |
| _version_ | 1826111079430750208 |
|---|---|
| author | Chernyak, Vladimir Y. Zhao, Yang Gelin, Maxim F. Sun, Ke-Wei |
| author2 | School of Materials Science & Engineering |
| author_facet | School of Materials Science & Engineering Chernyak, Vladimir Y. Zhao, Yang Gelin, Maxim F. Sun, Ke-Wei |
| author_sort | Chernyak, Vladimir Y. |
| collection | NTU |
| description | We have developed a variational approach to the description of four-wave-mixing signals of molecular aggregates, in which the third-order response functions are evaluated in terms of the Davydov Ansätze. Our theory treats both singly and doubly excited excitonic states, handling the contributions due to stimulated emission, ground state bleach, and excited state absorption. As an illustration, we simulate a series of optical two-dimensional spectra of model J-aggregates. Our approach may become suitable for the computation of femtosecond optical four-wave-mixing signals of molecular aggregates with intermediate-to-strong exciton-phonon and exciton-exciton coupling strengths. |
| first_indexed | 2024-10-01T02:44:44Z |
| format | Journal Article |
| id | ntu-10356/79390 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T02:44:44Z |
| publishDate | 2015 |
| record_format | dspace |
| spelling | ntu-10356/793902023-07-14T15:49:58Z Davydov Ansatz as an efficient tool for the simulation of nonlinear optical response of molecular aggregates Chernyak, Vladimir Y. Zhao, Yang Gelin, Maxim F. Sun, Ke-Wei School of Materials Science & Engineering DRNTU::Science::Chemistry::Physical chemistry::Molecular structure and bonding We have developed a variational approach to the description of four-wave-mixing signals of molecular aggregates, in which the third-order response functions are evaluated in terms of the Davydov Ansätze. Our theory treats both singly and doubly excited excitonic states, handling the contributions due to stimulated emission, ground state bleach, and excited state absorption. As an illustration, we simulate a series of optical two-dimensional spectra of model J-aggregates. Our approach may become suitable for the computation of femtosecond optical four-wave-mixing signals of molecular aggregates with intermediate-to-strong exciton-phonon and exciton-exciton coupling strengths. Accepted version 2015-06-17T02:29:41Z 2019-12-06T13:24:10Z 2015-06-17T02:29:41Z 2019-12-06T13:24:10Z 2015 2015 Journal Article Sun, K.-W., Gelin, M. F., Chernyak, V. Y., & Zhao, Y. (2015). Davydov Ansatz as an efficient tool for the simulation of nonlinear optical response of molecular aggregates. Journal of chemical physics, 142, 212448-. 0021-9606 https://hdl.handle.net/10356/79390 http://hdl.handle.net/10220/25928 10.1063/1.4921575 en Journal of chemical physics © 2015 American Institute of Physics. This is the author created version of a work that has been peer reviewed and accepted for publication by Journal of Chemical Physics, American Institute of Physics. It incorporates referee’s comments but changes resulting from the publishing process, such as copyediting, structural formatting, may not be reflected in this document. The published version is available at: [http://dx.doi.org/10.1063/1.4921575]. application/pdf |
| spellingShingle | DRNTU::Science::Chemistry::Physical chemistry::Molecular structure and bonding Chernyak, Vladimir Y. Zhao, Yang Gelin, Maxim F. Sun, Ke-Wei Davydov Ansatz as an efficient tool for the simulation of nonlinear optical response of molecular aggregates |
| title | Davydov Ansatz as an efficient tool for the simulation of nonlinear optical response of molecular aggregates |
| title_full | Davydov Ansatz as an efficient tool for the simulation of nonlinear optical response of molecular aggregates |
| title_fullStr | Davydov Ansatz as an efficient tool for the simulation of nonlinear optical response of molecular aggregates |
| title_full_unstemmed | Davydov Ansatz as an efficient tool for the simulation of nonlinear optical response of molecular aggregates |
| title_short | Davydov Ansatz as an efficient tool for the simulation of nonlinear optical response of molecular aggregates |
| title_sort | davydov ansatz as an efficient tool for the simulation of nonlinear optical response of molecular aggregates |
| topic | DRNTU::Science::Chemistry::Physical chemistry::Molecular structure and bonding |
| url | https://hdl.handle.net/10356/79390 http://hdl.handle.net/10220/25928 |
| work_keys_str_mv | AT chernyakvladimiry davydovansatzasanefficienttoolforthesimulationofnonlinearopticalresponseofmolecularaggregates AT zhaoyang davydovansatzasanefficienttoolforthesimulationofnonlinearopticalresponseofmolecularaggregates AT gelinmaximf davydovansatzasanefficienttoolforthesimulationofnonlinearopticalresponseofmolecularaggregates AT sunkewei davydovansatzasanefficienttoolforthesimulationofnonlinearopticalresponseofmolecularaggregates |