A variational approach to nonlocal exciton–phonon coupling
In this paper we apply variational energy band theory to a form of the Holstein Hamiltonian in which the influence of lattice vibrations (optical phonons) on both local site energies (local coupling) and transfers of electronic excitations between neighboring sites (nonlocal coupling) is taken into...
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| Format: | Journal Article |
| Language: | English |
| Published: |
2011
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| Online Access: | https://hdl.handle.net/10356/92233 http://hdl.handle.net/10220/6730 |
| _version_ | 1811691371407343616 |
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| author | Brown, David W. Zhao, Yang Lindenberg, Katja |
| author2 | School of Materials Science & Engineering |
| author_facet | School of Materials Science & Engineering Brown, David W. Zhao, Yang Lindenberg, Katja |
| author_sort | Brown, David W. |
| collection | NTU |
| description | In this paper we apply variational energy band theory to a form of the Holstein Hamiltonian in which the influence of lattice vibrations (optical phonons) on both local site energies (local coupling) and transfers of electronic excitations between neighboring sites (nonlocal coupling) is taken into account. A flexible spanning set of orthonormal eigenfunctions of the joint exciton– phonon crystal momentum is used to arrive at a variational estimate (bound) of the ground state energy for every value of the joint crystal momentum, yielding a variational estimate of the lowest polaron energy band across the entire Brillouin zone, as well as the complete set of polaron Bloch functions associated with this band. The variation is implemented numerically, avoiding restrictive assumptions that have limited the scope of previous assaults on the same and similar problems. Polaron energy bands and the structure of the associated Bloch states are studied at general points in the three-dimensional parameter space of the model Hamiltonian (electronic tunneling, local coupling, nonlocal coupling), though our principal emphasis lies in the understudied area of nonlocal coupling and its interplay with electronic tunneling; a phase diagram summarizing the latter is presented. The common notion of a "self-trapping transition" is addressed and generalized. |
| first_indexed | 2024-10-01T06:18:50Z |
| format | Journal Article |
| id | ntu-10356/92233 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T06:18:50Z |
| publishDate | 2011 |
| record_format | dspace |
| spelling | ntu-10356/922332023-07-14T15:51:44Z A variational approach to nonlocal exciton–phonon coupling Brown, David W. Zhao, Yang Lindenberg, Katja School of Materials Science & Engineering DRNTU::Science::Physics::Atomic physics::Solid state physics In this paper we apply variational energy band theory to a form of the Holstein Hamiltonian in which the influence of lattice vibrations (optical phonons) on both local site energies (local coupling) and transfers of electronic excitations between neighboring sites (nonlocal coupling) is taken into account. A flexible spanning set of orthonormal eigenfunctions of the joint exciton– phonon crystal momentum is used to arrive at a variational estimate (bound) of the ground state energy for every value of the joint crystal momentum, yielding a variational estimate of the lowest polaron energy band across the entire Brillouin zone, as well as the complete set of polaron Bloch functions associated with this band. The variation is implemented numerically, avoiding restrictive assumptions that have limited the scope of previous assaults on the same and similar problems. Polaron energy bands and the structure of the associated Bloch states are studied at general points in the three-dimensional parameter space of the model Hamiltonian (electronic tunneling, local coupling, nonlocal coupling), though our principal emphasis lies in the understudied area of nonlocal coupling and its interplay with electronic tunneling; a phase diagram summarizing the latter is presented. The common notion of a "self-trapping transition" is addressed and generalized. Published version 2011-03-03T04:48:31Z 2019-12-06T18:19:44Z 2011-03-03T04:48:31Z 2019-12-06T18:19:44Z 1997 1997 Journal Article Zhao, Y., Brown, D. W. & Lindenberg, K. (1997). A Variational Approach to Nonlocal Exciton-Phonon Coupling. Journal of chemical physics, 106(7), 2728-2740. https://hdl.handle.net/10356/92233 http://hdl.handle.net/10220/6730 10.1063/1.473793 en Journal of chemical physics © 1997 AIP. This paper was published in Journal of Chemical Physics and is made available as an electronic reprint (preprint) with permission of American Institute of Physics. The paper can be found at: [Doi: http://dx.doi.org/10.1063/1.473793]. 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. 13 p. application/pdf |
| spellingShingle | DRNTU::Science::Physics::Atomic physics::Solid state physics Brown, David W. Zhao, Yang Lindenberg, Katja A variational approach to nonlocal exciton–phonon coupling |
| title | A variational approach to nonlocal exciton–phonon coupling |
| title_full | A variational approach to nonlocal exciton–phonon coupling |
| title_fullStr | A variational approach to nonlocal exciton–phonon coupling |
| title_full_unstemmed | A variational approach to nonlocal exciton–phonon coupling |
| title_short | A variational approach to nonlocal exciton–phonon coupling |
| title_sort | variational approach to nonlocal exciton phonon coupling |
| topic | DRNTU::Science::Physics::Atomic physics::Solid state physics |
| url | https://hdl.handle.net/10356/92233 http://hdl.handle.net/10220/6730 |
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