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

Understanding the electronic structure of doped semiconductors is essential to realize advancements in electronics and in the rational design of nanoscale devices. Here, we report 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. Additionally, the transient photoluminescence and the kinetics of dopant oxidation reveal the presence of two types of surface-bound ions that create mid-gap states.
Authors:
 [1] ;  [2] ;  [1] ;  [3] ;  [1] ;  [2] ;  [4] ;  [1] ;  [2] ;  [4] ; ORCiD logo [5] ; ORCiD logo [1]
  1. Univ. of Illinois, Chicago, IL (United States). Department of Chemistry
  2. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
  3. Northwestern Univ., Evanston, IL (United States). Department of Chemistry
  4. Univ. of Illinois, Chicago, IL (United States). Department of Physics
  5. Northwestern Univ., Evanston, IL (United States). Department of Chemistry; Argonne National Lab. (ANL), Argonne, IL (United States). Center of Nanoscale Materials
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 11; Journal Issue: 10; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; cadmium sulfide; doping; nanoparticle; quantum dot; semiconductor; x-ray absorption
OSTI Identifier:
1417192

Hassan, Asra, Zhang, Xiaoyi, Liu, Xiaohan, Rowland, Clare E., Jawaid, Ali M., Chattopadhyay, Soma, Gulec, Ahmet, Shamirian, Armen, Zuo, Xiaobing, Klie, Robert F., Schaller, Richard D., and Snee, Preston T.. Charge Carriers Modulate the Bonding of Semiconductor Nanoparticle Dopants As Revealed by Time-Resolved X-ray Spectroscopy. United States: N. p., Web. doi:10.1021/acsnano.7b04414.
Hassan, Asra, Zhang, Xiaoyi, Liu, Xiaohan, Rowland, Clare E., Jawaid, Ali M., Chattopadhyay, Soma, Gulec, Ahmet, Shamirian, Armen, Zuo, Xiaobing, Klie, Robert F., Schaller, Richard D., & Snee, Preston T.. Charge Carriers Modulate the Bonding of Semiconductor Nanoparticle Dopants As Revealed by Time-Resolved X-ray Spectroscopy. United States. doi:10.1021/acsnano.7b04414.
Hassan, Asra, Zhang, Xiaoyi, Liu, Xiaohan, Rowland, Clare E., Jawaid, Ali M., Chattopadhyay, Soma, Gulec, Ahmet, Shamirian, Armen, Zuo, Xiaobing, Klie, Robert F., Schaller, Richard D., and Snee, Preston T.. 2017. "Charge Carriers Modulate the Bonding of Semiconductor Nanoparticle Dopants As Revealed by Time-Resolved X-ray Spectroscopy". United States. doi:10.1021/acsnano.7b04414. https://www.osti.gov/servlets/purl/1417192.
@article{osti_1417192,
title = {Charge Carriers Modulate the Bonding of Semiconductor Nanoparticle Dopants As Revealed by Time-Resolved X-ray Spectroscopy},
author = {Hassan, Asra and Zhang, Xiaoyi and Liu, Xiaohan and Rowland, Clare E. and Jawaid, Ali M. and Chattopadhyay, Soma and Gulec, Ahmet and Shamirian, Armen and Zuo, Xiaobing and Klie, Robert F. and Schaller, Richard D. and Snee, Preston T.},
abstractNote = {Understanding the electronic structure of doped semiconductors is essential to realize advancements in electronics and in the rational design of nanoscale devices. Here, we report 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. Additionally, the transient photoluminescence and the kinetics of dopant oxidation reveal the presence of two types of surface-bound ions that create mid-gap states.},
doi = {10.1021/acsnano.7b04414},
journal = {ACS Nano},
number = 10,
volume = 11,
place = {United States},
year = {2017},
month = {8}
}