Plasmon-Enhanced Light Harvesting of Chlorophylls on Near-Percolating Silver Films via One-Photon Anti-Stokes Upconversion
Abstract
There exists a wealth of means of efficient utilization of solar energy in nature, with photosynthesis of chlorophylls as a prime example. Separately, artificially structured plasmonic materials are versatile in light harvesting and energy conversion. Using a simple and scalable design of near-percolating silver nanostructures, we demonstrate that the light-harvesting efficiency of chlorophylls can be drastically enhanced by tuning the plasmon frequency of the constituent silver nanoparticles to coincide with the maximal photon flux of sunlight. In particular, we show that the photon upconversion efficiency can be readily enhanced by over 20 folds, with the room-temperature fluorescence quantum yield increased by a factor of 2.63. The underlying mechanism for the upconversion enhancement is attributed to a one-electron-per-photon anti-Stokes process, involving absorption of a characteristic phonon mode of the chlorophylls. These findings suggest that chlorophylls can serve as molecular building blocks for high-efficiency light harvesting and solar energy conversion.
- Authors:
-
- Wuhan Univ. (China). Dept. of Physics
- Wuhan Univ. (China). College of Life Sciences
- Inst. of Applied Physics and Computational Mathematics, Beijing (China)
- Univ. of Science and Technology of China, Hefei (China); Univ. of Texas, Austin, TX (United States). Dept. of Physics
- Publication Date:
- Research Org.:
- Univ. of Texas, Austin, TX (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
- OSTI Identifier:
- 1624619
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Scientific Reports
- Additional Journal Information:
- Journal Volume: 3; Journal Issue: 1; Journal ID: ISSN 2045-2322
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 14 SOLAR ENERGY; Applied physics; Nanoparticles; Nanoscale biophysics; Solar energy and photovoltaic technology
Citation Formats
Wang, Ya-Lan, Nan, Fan, Liu, Xiao-Li, Zhou, Li, Peng, Xiao-Niu, Zhou, Zhang-Kai, Yu, Ying, Hao, Zhong-Hua, Wu, Yan, Zhang, Wei, Wang, Qu-Quan, and Zhang, Zhenyu. Plasmon-Enhanced Light Harvesting of Chlorophylls on Near-Percolating Silver Films via One-Photon Anti-Stokes Upconversion. United States: N. p., 2013.
Web. doi:10.1038/srep01861.
Wang, Ya-Lan, Nan, Fan, Liu, Xiao-Li, Zhou, Li, Peng, Xiao-Niu, Zhou, Zhang-Kai, Yu, Ying, Hao, Zhong-Hua, Wu, Yan, Zhang, Wei, Wang, Qu-Quan, & Zhang, Zhenyu. Plasmon-Enhanced Light Harvesting of Chlorophylls on Near-Percolating Silver Films via One-Photon Anti-Stokes Upconversion. United States. https://doi.org/10.1038/srep01861
Wang, Ya-Lan, Nan, Fan, Liu, Xiao-Li, Zhou, Li, Peng, Xiao-Niu, Zhou, Zhang-Kai, Yu, Ying, Hao, Zhong-Hua, Wu, Yan, Zhang, Wei, Wang, Qu-Quan, and Zhang, Zhenyu. Tue .
"Plasmon-Enhanced Light Harvesting of Chlorophylls on Near-Percolating Silver Films via One-Photon Anti-Stokes Upconversion". United States. https://doi.org/10.1038/srep01861. https://www.osti.gov/servlets/purl/1624619.
@article{osti_1624619,
title = {Plasmon-Enhanced Light Harvesting of Chlorophylls on Near-Percolating Silver Films via One-Photon Anti-Stokes Upconversion},
author = {Wang, Ya-Lan and Nan, Fan and Liu, Xiao-Li and Zhou, Li and Peng, Xiao-Niu and Zhou, Zhang-Kai and Yu, Ying and Hao, Zhong-Hua and Wu, Yan and Zhang, Wei and Wang, Qu-Quan and Zhang, Zhenyu},
abstractNote = {There exists a wealth of means of efficient utilization of solar energy in nature, with photosynthesis of chlorophylls as a prime example. Separately, artificially structured plasmonic materials are versatile in light harvesting and energy conversion. Using a simple and scalable design of near-percolating silver nanostructures, we demonstrate that the light-harvesting efficiency of chlorophylls can be drastically enhanced by tuning the plasmon frequency of the constituent silver nanoparticles to coincide with the maximal photon flux of sunlight. In particular, we show that the photon upconversion efficiency can be readily enhanced by over 20 folds, with the room-temperature fluorescence quantum yield increased by a factor of 2.63. The underlying mechanism for the upconversion enhancement is attributed to a one-electron-per-photon anti-Stokes process, involving absorption of a characteristic phonon mode of the chlorophylls. These findings suggest that chlorophylls can serve as molecular building blocks for high-efficiency light harvesting and solar energy conversion.},
doi = {10.1038/srep01861},
journal = {Scientific Reports},
number = 1,
volume = 3,
place = {United States},
year = {Tue May 21 00:00:00 EDT 2013},
month = {Tue May 21 00:00:00 EDT 2013}
}
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