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Anisotropic Cation Exchange in PbSe/CdSe Core/Shell Nanocrystals of Different Geometry
被引:145
作者:
Casavola, Marianna
[1
]
van Huis, Marijn A.
[2
,3
]
Bals, Sara
[2
]
Lambert, Karel
[4
]
Hens, Zeger
[4
]
Vanmaekelbergh, Daniel
[1
]
机构:
[1] Univ Utrecht, Debye Inst Nanomat Sci, NL-3508 TA Utrecht, Netherlands
[2] Univ Antwerp, EMAT, B-2020 Antwerp, Belgium
[3] Delft Univ Technol, Kavli Inst Nanosci, NL-2628 CJ Delft, Netherlands
[4] Univ Ghent, B-9000 Ghent, Belgium
关键词:
core/shell nanocrystals;
cation exchange;
near-infrared-active nanocrystals;
HAADF-STEM;
PbSe/CdSe;
COLLOIDAL NANOCRYSTALS;
NANORODS;
CDSE;
D O I:
10.1021/cm202796s
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:
We present a study of Cd2+-for-Pb2+ exchange in PbSe nanocrystals (NCs) with cube, star, and rod shapes. Prolonged temperature-activated cation exchange results in PbSe/CdSe heterostructured nanocrystals (HNCs) that preserve their specific overall shape, whereas the PbSe core is strongly faceted with dominance of {111} facets. Hence, cation exchange proceeds while the Se anion lattice is preserved, and well-defined {111}/{111} PbSe/CdSe interfaces develop. Interestingly, by quenching the reaction at different stages of the cation exchange new structures have been isolated, such as core-shell nanorods, CdSe rods that contain one or two separated PbSe dots and fully zinc blende CdSe nanorods. The crystallographically anisotropic cation exchange has been characterized by a combined HRTEM/HAADF-STEM study of heterointerface evolution over reaction time and temperature. Strikingly, Pb and Cd are only intermixed at the PbSe/CdSe interface. We propose a plausible model for the cation exchange based on a layer-by-layer replacement of Pb2+ by Cd2+ enabled by a vacancy-assisted cation migration mechanism.
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页码:294 / 302
页数:9
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