Solid-State Chemistry on the Nanoscale: Ion Transport through Interstitial Sites or Vacancies?

被引:41
作者
Bothe, Cornelia [1 ]
Kornowski, Andreas [1 ]
Tornatzky, Hans [2 ]
Schmidtke, Christian [1 ]
Lange, Holger [1 ,4 ]
Maultzsch, Janina [2 ]
Weller, Horst [1 ,3 ,4 ,5 ]
机构
[1] Univ Hamburg, Inst Phys Chem, Fachbereich Chem, D-20146 Hamburg, Germany
[2] Tech Univ Berlin, Inst Festkorperphys, D-10623 Berlin, Germany
[3] Ctr Angew Nanotechnol, D-20146 Hamburg, Germany
[4] Hamburg Ctr Ultrafast Imaging CUI, D-22761 Hamburg, Germany
[5] King Abdulaziz Univ, Fac Sci, Dept Chem, Jeddah, Saudi Arabia
关键词
cation exchange; nanoparticles; PbSe; reaction kinetics; ZnSe; DOT QUANTUM-WELL; SEMICONDUCTOR NANOCRYSTALS; CATION-EXCHANGE; DIFFUSION; PHOTOPHYSICS; CDS/HGS/CDS; MODEL; LESS; GOLD;
D O I
10.1002/anie.201507263
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
How can ion-exchange process occur in nanocrystals without the size and shape changing and why is the ion transport much faster than in classical interdiffusion processes in macrocrystalline solids? We have investigated these processes at the molecular level by means of high-resolution and analytical electron microscopy in temperature-dependent kinetic experiments for several model reactions. The results clearly show a diffusion process that proceeds exclusively through the interstitial lattice positions with a subsequent "kick out" to remove individual ions from lattice sites without the formation of vacancies. This mechanism has not been observed in nanocrystalline systems before.
引用
收藏
页码:14183 / 14186
页数:4
相关论文
共 28 条
[1]   Homogeneously Alloyed CdSe1-xSx Quantum Dots (0 ≤ x ≤ 1): An Efficient Synthesis for Full Optical Tunability [J].
Aubert, Tangi ;
Cirillo, Marco ;
Flamee, Stijn ;
Van Deun, Rik ;
Lange, Holger ;
Thomsen, Christian ;
Hens, Zeger .
CHEMISTRY OF MATERIALS, 2013, 25 (12) :2388-2390
[2]  
Borg R.J., 1988, An Introduction to Solid State Diffusion
[3]  
Bruff C. M., 1998, CHEM DIFFUSION BULK
[4]   SIZE EFFECT ON MELTING TEMPERATURE OF GOLD PARTICLES [J].
BUFFAT, P ;
BOREL, JP .
PHYSICAL REVIEW A, 1976, 13 (06) :2287-2298
[5]  
Burgel R., 1998, Handbuch Hochtemperatur Werkstofftechnik
[6]   Anisotropic Cation Exchange in PbSe/CdSe Core/Shell Nanocrystals of Different Geometry [J].
Casavola, Marianna ;
van Huis, Marijn A. ;
Bals, Sara ;
Lambert, Karel ;
Hens, Zeger ;
Vanmaekelbergh, Daniel .
CHEMISTRY OF MATERIALS, 2012, 24 (02) :294-302
[7]   Self-purification in semiconductor nanocrystals [J].
Dalpian, Gustavo M. ;
Chelikowsky, James R. .
PHYSICAL REVIEW LETTERS, 2006, 96 (22)
[8]  
DAVID R, 1997, CRC HDB CHEM PHYS
[9]  
Dean J.A., 2001, Lange's Handbook of Chemistry, V15
[10]   Trapped-dopant model of doping in semiconductor nanocrystals [J].
Du, Mao-Hua ;
Erwin, Steven C. ;
Efros, Al. L. .
NANO LETTERS, 2008, 8 (09) :2878-2882