期刊
ACS NANO
卷 7, 期 1, 页码 263-275出版社
AMER CHEMICAL SOC
DOI: 10.1021/nn303964v
关键词
electron transfer; fluorogenic probe; single-molecule fluorescence spectroscopy; surface plasmon resonance; TiO2 nanoparticle
类别
资金
- Ministry of Education, Science and Technology through the National Research Foundation of Korea [R31-2011-000-10035-0]
- Innovative Project for Advanced Instruments, Renovation Center of Instruments for Science Education and Technology, Osaka University
- Ministry of Education, Culture, Sports, Science and Technology (MEXT) of the Japanese Government [22245022]
- Murata Science Foundation
- Grants-in-Aid for Scientific Research [22245022, 23655009] Funding Source: KAKEN
Interfacial charge transfer at the heterogeneous surface of semiconductor nanoparticles is a fundamental process that is relevant to many Important applications, such as photocatalysis, solar cells, and sensors. In this study, we developed new water-soluble fluorogenic probes for interfacial electron transfer reactions on semiconductor nanoparticles. The synthesized boron-dipyrromethene-based fluorescence dyes have one or two sulfonate groups, which confer solubility in aqueous media, and a dinitrophenyl group as a redox reaction site. These probes produce the corresponding fluorescent products via multiple interfacial electron transfer processes, allowing us to investigate the photoinduced redox reactions over individual pristine and Au-nanoparticle-deposited TiO2 nanoparticles at the single-particle, single-molecule levels. The minimum probe concentration to detect single-product molecules on a single TiO2 nanoparticle was found to be In the nanomolar range (<10 nM) in acidic solution. furthermore, super-resolution mapping of the reaction sites revealed that visible-light-induced reduction reactions preferentially occurred on the TiO2 surface within a distance of a few tens of nanometers around the deposited Au nanoparticles. This result was qualitatively interpreted on the basis of plasmon-induced electron and/or energy transfer mechanisms. Overall, this study provides a great deal of valuable information related to solar-energy-conversion processes that is impossible or difficult to obtain from ensemble-averaged experiments.
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