Charge Carriers Modulate the Bonding of Semiconductor Nanoparticle Dopants As Revealed by Time-Resolved X-ray Spectroscopy

被引:18
|
作者
Hassan, Asra [1 ]
Zhang, Xiaoyi [3 ]
Liu, Xiaohan [1 ]
Rowland, Clare E. [5 ]
Jawaid, Ali M. [1 ]
Chattopadhyay, Soma [3 ]
Gulec, Ahmet [2 ]
Shamirian, Armen [1 ]
Zuo, Xiaobing [3 ]
Klie, Robert F. [2 ]
Schaller, Richard D. [4 ,5 ]
Snee, Preston T. [1 ]
机构
[1] Univ Illinois, Dept Chem, 845 W Taylor St, Chicago, IL 60607 USA
[2] Univ Illinois, Dept Phys, 845 W Taylor St, Chicago, IL 60607 USA
[3] Argonne Natl Lab, Xray Sci Div, 9700 S Cass Ave, Argonne, IL 60439 USA
[4] Argonne Natl Lab, Ctr Nanoscale Mat, 9700 S Cass Ave, Argonne, IL 60439 USA
[5] Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA
关键词
semiconductor; nanoparticle; quantum dot; cadmium sulfide; X-ray absorption; doping; EFFECTIVE CORE POTENTIALS; MOLECULAR CALCULATIONS; STRUCTURAL DYNAMICS; ABSORPTION; NANOCRYSTALS; COPPER; CU; SCATTERING; CLUSTER; SURFACE;
D O I
10.1021/acsnano.7b04414
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Understanding the electronic structure of doped semiconductors is essential to realize advancements in electronics and in the rational design of nanoscale devices. Reported here are the results of time-resolved X-ray absorption studies on copper-doped cadmium sulfide nanoparticles that provide an explicit description of the electronic dynamics of the dopants. The interaction of a dopant ion and an excess charge carrier is unambiguously observed via monitoring the oxidation state. The experimental data combined with DFT calculations demonstrate that dopant bonding to the host matrix is modulated by its interaction with charge carriers. Furthermore, the transient photoluminescence and the kinetics of dopant oxidation reveal the presence of two types of surface-bound ions that create midgap states.
引用
收藏
页码:10070 / 10076
页数:7
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