Suppressed Blinking and Auger Recombination in Near-Infrared Type-II InP/CdS Nanocrystal Quantum Dots

被引:135
作者
Dennis, Allison M. [1 ]
Mangum, Benjamin D. [1 ]
Piryatinski, Andrei [2 ]
Park, Young-Shin [1 ]
Hannah, Daniel C. [4 ]
Casson, Joanna L. [3 ]
Williams, Darrick J. [1 ]
Schaller, Richard D. [4 ,5 ]
Htoon, Han [1 ]
Hollingsworth, Jennifer A. [1 ]
机构
[1] Los Alamos Natl Lab, Mat Phys & Applicat Div, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USA
[2] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA
[3] Los Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA
[4] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA
[5] Argonne Natl Lab, Ctr Nanoscale Mat, Argonne, IL 60439 USA
关键词
Fluorescence blinking suppression; core/shell heterostructure; near-infrared; type-II nanocrystal quantum dot; biexciton lifetime; Auger recombination; SINGLE; FLUORESCENCE; KINETICS;
D O I
10.1021/nl302453x
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Nonblinking excitonic emission from near-infrared and type-II nanocrystal quantum dots (NQDs) is reported for the first time. To realize: this unusual degree of stability at the single-dot level, novel InP/CdS core/shell NQDs were synthesized for a range, of shell thicknesses (similar to 1-11 monolayers of CdS). Ensemble spectroscopy measurements (photoluminescence peak position And radiative lifetimes). and electronic structure calculations established the transition from type-I to type-II band alignment in these heterostructured NQDs. More significantly, single-NQD studies revealed clear evidence for blinking suppression that was not strongly shell-thickness dependent, while photobleaching and biexciton lifetimes trended explicitly with extent of shelling. Specifically, very long biexciton lifetimes-up to >7 ns-were obtained for the thickest-shell structures, indicating dramatic suppression of nonradiative Auger recombination. This new system demonstrates that electronic structure and shell thickness can be employed together to effect control over key single-dot and ensemble NQD photophysical properties.
引用
收藏
页码:5545 / 5551
页数:7
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