Size-Dependent Biexciton Quantum Yields and Carrier Dynamics of Quasi-Two-Dimensional Core/Shell Nanoplatelets

被引:67
|
作者
Ma, Xuedan [1 ]
Diroll, Benjamin T. [1 ]
Cho, Wooje [2 ,3 ]
Fedin, Igor [2 ,3 ]
Schaller, Richard D. [1 ,4 ]
Talapin, Dmitri V. [1 ,2 ,3 ]
Gray, Stephen K. [1 ]
Wiederrecht, Gary P. [1 ]
Gosztola, David J. [1 ]
机构
[1] Argonne Natl Lab, Ctr Nanoscale Mat, Argonne, IL 60439 USA
[2] Univ Chicago, Dept Chem, Chicago, IL 60637 USA
[3] Univ Chicago, James Franck Inst, Chicago, IL 60637 USA
[4] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA
关键词
CdSe/CdS nanoplatelets; biexciton; radiative lifetime; second-order photon correlation function; exciton coherent motion area; quasi-2D exciton; COLLOIDAL CDSE NANOPLATELETS; AMPLIFIED SPONTANEOUS EMISSION; CORE-SHELL NANOCRYSTALS; SEMICONDUCTOR NANOPLATELETS; ELECTRONIC-STRUCTURE; AUGER RECOMBINATION; CARBON NANOTUBES; PHOTON-EMISSION; DOTS; FLUORESCENCE;
D O I
10.1021/acsnano.7b03943
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Quasi-two-dimensional nanoplatelets (NPLs) possess fundamentally different excitonic properties from zero-dimensional quantum dots. We study lateral size-dependent photon emission statistics and carrier dynamics of individual NPLs using second-order photon correlation (g((2))(tau)) spectroscopy and photoluminescence (PL) intensity-dependent lifetime analysis. Room-temperature radiative lifetimes of NPLs can be derived from maximum PL intensity periods in PL time traces. It first decreases with NPL lateral size and then stays constant, deviating from the electric dipole approximation. Analysis of the PL time traces further reveals that the single exciton quantum yield in NPLs decreases with NPL lateral size and increases with protecting shell thickness, indicating the importance of surface passivation on NPL emission quality. Second order photon correlation (g((2))(tau)) studies of single NPLs show that the biexciton quantum yield is strongly dependent on the lateral size and single exciton quantum yield of the NPLs. In large NPLs with unity single exciton quantum yield, the corresponding biexciton quantum yield can reach unity. These findings reveal that by careful growth control and core shell material engineering, NPLs can be of great potential for light amplification and integrated quantum photonic applications.
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页码:9119 / 9127
页数:9
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