Efficient energy transfer in light-harvesting systems, I: optimal temperature, reorganization energy and spatial–temporal correlations
Understanding the mechanisms of efficient and robust energy transfer in light-harvesting systems provides new insights for the optimal design of artificial systems. In this paper, we use the Fenna–Matthews–Olson (FMO) protein complex and phycocyanin 645 (PC 645) to explore the general dependence on...
| Main Authors: | , , , , |
|---|---|
| Other Authors: | |
| Format: | Article |
| Language: | en_US |
| Published: |
Institute of Physics Publishing
2012
|
| Online Access: | http://hdl.handle.net/1721.1/70851 https://orcid.org/0000-0001-7616-7809 |
| _version_ | 1826189709757382656 |
|---|---|
| author | Wu, Jianlan Liu, Fan Shen, Young Cao, Jianshu Silbey, Robert J. |
| author2 | Massachusetts Institute of Technology. Department of Chemistry |
| author_facet | Massachusetts Institute of Technology. Department of Chemistry Wu, Jianlan Liu, Fan Shen, Young Cao, Jianshu Silbey, Robert J. |
| author_sort | Wu, Jianlan |
| collection | MIT |
| description | Understanding the mechanisms of efficient and robust energy transfer in light-harvesting systems provides new insights for the optimal design of artificial systems. In this paper, we use the Fenna–Matthews–Olson (FMO) protein complex and phycocyanin 645 (PC 645) to explore the general dependence on physical parameters that help maximize the efficiency and maintain its stability. With the Haken–Strobl model, the maximal energy transfer efficiency (ETE) is achieved under an intermediate optimal value of dephasing rate. To avoid the infinite temperature assumption in the Haken–Strobl model and the failure of the Redfield equation in predicting the Forster rate behavior, we use the generalized Bloch–Redfield (GBR) equation approach to correctly describe dissipative exciton dynamics, and we find that maximal ETE can be achieved under various physical conditions, including temperature, reorganization energy and spatial–temporal correlations in noise. We also identify regimes of reorganization energy where the ETE changes monotonically with temperature or spatial correlation and therefore cannot be optimized with respect to these two variables. |
| first_indexed | 2024-09-23T08:19:49Z |
| format | Article |
| id | mit-1721.1/70851 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T08:19:49Z |
| publishDate | 2012 |
| publisher | Institute of Physics Publishing |
| record_format | dspace |
| spelling | mit-1721.1/708512022-09-30T09:02:33Z Efficient energy transfer in light-harvesting systems, I: optimal temperature, reorganization energy and spatial–temporal correlations Wu, Jianlan Liu, Fan Shen, Young Cao, Jianshu Silbey, Robert J. Massachusetts Institute of Technology. Department of Chemistry Silbey, Robert J. Wu, Jianlan Liu, Fan Cao, Jianshu Shen, Young Silbey, Robert J. Understanding the mechanisms of efficient and robust energy transfer in light-harvesting systems provides new insights for the optimal design of artificial systems. In this paper, we use the Fenna–Matthews–Olson (FMO) protein complex and phycocyanin 645 (PC 645) to explore the general dependence on physical parameters that help maximize the efficiency and maintain its stability. With the Haken–Strobl model, the maximal energy transfer efficiency (ETE) is achieved under an intermediate optimal value of dephasing rate. To avoid the infinite temperature assumption in the Haken–Strobl model and the failure of the Redfield equation in predicting the Forster rate behavior, we use the generalized Bloch–Redfield (GBR) equation approach to correctly describe dissipative exciton dynamics, and we find that maximal ETE can be achieved under various physical conditions, including temperature, reorganization energy and spatial–temporal correlations in noise. We also identify regimes of reorganization energy where the ETE changes monotonically with temperature or spatial correlation and therefore cannot be optimized with respect to these two variables. National Science Foundation (U.S.) (NSF 0806266) National Institutes of Health (U.S.) (Grant 0556268) Massachusetts Institute of Technology. Energy Initiative (Seed grant) United States. Dept. of Energy (DOE grant number DE-SC0001088) 2012-05-16T19:27:15Z 2012-05-16T19:27:15Z 2010-10 2010-02 Article http://purl.org/eprint/type/JournalArticle 1367-2630 http://hdl.handle.net/1721.1/70851 Wu, Jianlan et al. “Efficient Energy Transfer in Light-harvesting Systems, I: Optimal Temperature, Reorganization Energy and Spatial–temporal Correlations.” New Journal of Physics 12.10 (2010): 105012. Web. https://orcid.org/0000-0001-7616-7809 en_US http://dx.doi.org/10.1088/1367-2630/12/10/105012 New Journal of Physics Creative Commons Attribution 3.0 http://creativecommons.org/licenses/by/3.0/ application/pdf Institute of Physics Publishing New Journal of Physics |
| spellingShingle | Wu, Jianlan Liu, Fan Shen, Young Cao, Jianshu Silbey, Robert J. Efficient energy transfer in light-harvesting systems, I: optimal temperature, reorganization energy and spatial–temporal correlations |
| title | Efficient energy transfer in light-harvesting systems, I: optimal temperature, reorganization energy and spatial–temporal correlations |
| title_full | Efficient energy transfer in light-harvesting systems, I: optimal temperature, reorganization energy and spatial–temporal correlations |
| title_fullStr | Efficient energy transfer in light-harvesting systems, I: optimal temperature, reorganization energy and spatial–temporal correlations |
| title_full_unstemmed | Efficient energy transfer in light-harvesting systems, I: optimal temperature, reorganization energy and spatial–temporal correlations |
| title_short | Efficient energy transfer in light-harvesting systems, I: optimal temperature, reorganization energy and spatial–temporal correlations |
| title_sort | efficient energy transfer in light harvesting systems i optimal temperature reorganization energy and spatial temporal correlations |
| url | http://hdl.handle.net/1721.1/70851 https://orcid.org/0000-0001-7616-7809 |
| work_keys_str_mv | AT wujianlan efficientenergytransferinlightharvestingsystemsioptimaltemperaturereorganizationenergyandspatialtemporalcorrelations AT liufan efficientenergytransferinlightharvestingsystemsioptimaltemperaturereorganizationenergyandspatialtemporalcorrelations AT shenyoung efficientenergytransferinlightharvestingsystemsioptimaltemperaturereorganizationenergyandspatialtemporalcorrelations AT caojianshu efficientenergytransferinlightharvestingsystemsioptimaltemperaturereorganizationenergyandspatialtemporalcorrelations AT silbeyrobertj efficientenergytransferinlightharvestingsystemsioptimaltemperaturereorganizationenergyandspatialtemporalcorrelations |