Single-Molecule Interfacial Electron Transfer in Donor-Bridge-Nanoparticle Acceptor Complexes

被引:22
作者
Jin, Shengye [2 ]
Snoeberger, Robert C., III [1 ]
Issac, Abey [2 ]
Stockwell, David [2 ]
Batista, Victor S. [1 ]
Lian, Tianquan [2 ]
机构
[1] Yale Univ, Dept Chem, New Haven, CT 06520 USA
[2] Emory Univ, Dept Chem, Atlanta, GA USA
基金
美国国家科学基金会;
关键词
DENSITY-FUNCTIONAL THEORY; TOTAL-ENERGY CALCULATIONS; RE-BIPYRIDYL COMPLEXES; INJECTION DYNAMICS; POLYPYRIDYL COMPLEXES; NANOCRYSTALLINE SNO2; EXCITATION-ENERGIES; CHARGE SEPARATION; TRANSFER KINETICS; RHODAMINE-B;
D O I
10.1021/jp911662g
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Photoinduced interfacial electron transfer (IET) in sulforhodamine B (SRhB) aminosilane-I in oxide (SnO2) nanoparticle donor-bridge-acceptor complexes has been studied on a single molecule and ensemble average level On both SnO2 and ZrO2, the sum of single molecule fluorescence decays agree with the ensemble average results suggesting complete sampling of molecules under single molecule conditions Shorter fluorescence lifetime on SnO2 than on ZrO2 is observed and attributed to JET from SRhB to SnO2 Single molecule lifetimes fluctuate with time and vary among different molecules, suggesting both static and dynamic IET heterogeneity in this system Computational modeling of the complexes shows a distribution of molecular conformation leading to a distribution of electronic coupling strengths and El rates It is likely that the conversion between these conformations led to the fluctuation of ET rate and fluorescence lifetime on the single molecule level
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页码:14309 / 14319
页数:11
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