Plasmon-Enhanced Light Harvesting of Chlorophylls on Near-Percolating Silver Films via One-Photon Anti-Stokes Upconversion

被引：27

作者：

Wang, Ya-Lan ^{[1
]}

Nan, Fan ^{[1
]}

Liu, Xiao-Li ^{[1
]}

Zhou, Li ^{[1
]}

Peng, Xiao-Niu ^{[1
]}

Zhou, Zhang-Kai ^{[1
]}

Yu, Ying ^{[1
]}

Hao, Zhong-Hua ^{[1
]}

Wu, Yan ^{[2
]}

Zhang, Wei ^{[3
]}

Wang, Qu-Quan ^{[1
]}

Zhang, Zhenyu ^{[4
,5
]}

机构：

[1] Wuhan Univ, Dept Phys, Wuhan 430072, Peoples R China

[2] Wuhan Univ, Coll Life Sci, Wuhan 430072, Peoples R China

[3] Inst Appl Phys & Computat Math, Beijing 100088, Peoples R China

[4] Univ Sci & Technol China, ICQD, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Peoples R China

[5] Univ Texas Austin, Dept Phys, Austin, TX 78712 USA

来源：

SCIENTIFIC REPORTS | 2013年 / 3卷

基金：

美国国家科学基金会;

关键词：

MOLECULAR-BASIS; FLUORESCENCE; NANOPARTICLE; 2-PHOTON; PROTEIN; RAMAN; SEMICONDUCTOR; HYBRIDIZATION; LUMINESCENCE; EXCITATION;

D O I：

10.1038/srep01861

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

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.

引用

页数：7

共 59 条

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