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Title: Electronic Structure and Dynamics of Copper-Doped Indium Phosphide Nanocrystals Studied with Time-Resolved X-ray Absorption and Large-Scale DFT Calculations

Abstract

Here, the recent development of time-resolved X-ray absorption spectroscopy (TR-XAS) has opened avenues for fundamental research on doped semiconductors. Reported herein are results on the successful doping of indium phosphide nanocrystals (NCs) with copper and subsequent charactenzation with time-resolved X-ray studies and largescale density functional theory (DFT) calculations. The synthetic protocol that was based on the cluster seed method afforded control of both the doping level and the quantity of NCs produced in a batch. The stability of the colloidal dispersion allowed us to monitor the photophysical properties of copper guest ions with static and TR-XAS at the copper K-edge. These data reveal that copper captures a hole from the photoexcited InP NC, and relaxation to the ground state occurs via multiple timescales likely due to the presence of interior and surface-bound dopant ions as well as recombination with surfaceand defect-trapped electrons. Large-scale DFT calculations reveal a striking dependence of the electronic structure on the ligand coating and other effects such as self-compensation.

Authors:
 [1]; ORCiD logo [2];  [2]; ORCiD logo [1]
  1. Univ. of Illinois at Chicago, Chicago, IL (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
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; University of Illinois, Chicago
OSTI Identifier:
1473687
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 122; Journal Issue: 20; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; copper; doping; indium phosphide; nanocrystals; semiconductor; x-ray absorption

Citation Formats

Hassan, Asra, Zhang, Xiaoyi, Liu, Cunming, and Snee, Preston T. Electronic Structure and Dynamics of Copper-Doped Indium Phosphide Nanocrystals Studied with Time-Resolved X-ray Absorption and Large-Scale DFT Calculations. United States: N. p., 2018. Web. doi:10.1021/acs.jpcc.8b02124.
Hassan, Asra, Zhang, Xiaoyi, Liu, Cunming, & Snee, Preston T. Electronic Structure and Dynamics of Copper-Doped Indium Phosphide Nanocrystals Studied with Time-Resolved X-ray Absorption and Large-Scale DFT Calculations. United States. doi:10.1021/acs.jpcc.8b02124.
Hassan, Asra, Zhang, Xiaoyi, Liu, Cunming, and Snee, Preston T. Fri . "Electronic Structure and Dynamics of Copper-Doped Indium Phosphide Nanocrystals Studied with Time-Resolved X-ray Absorption and Large-Scale DFT Calculations". United States. doi:10.1021/acs.jpcc.8b02124. https://www.osti.gov/servlets/purl/1473687.
@article{osti_1473687,
title = {Electronic Structure and Dynamics of Copper-Doped Indium Phosphide Nanocrystals Studied with Time-Resolved X-ray Absorption and Large-Scale DFT Calculations},
author = {Hassan, Asra and Zhang, Xiaoyi and Liu, Cunming and Snee, Preston T.},
abstractNote = {Here, the recent development of time-resolved X-ray absorption spectroscopy (TR-XAS) has opened avenues for fundamental research on doped semiconductors. Reported herein are results on the successful doping of indium phosphide nanocrystals (NCs) with copper and subsequent charactenzation with time-resolved X-ray studies and largescale density functional theory (DFT) calculations. The synthetic protocol that was based on the cluster seed method afforded control of both the doping level and the quantity of NCs produced in a batch. The stability of the colloidal dispersion allowed us to monitor the photophysical properties of copper guest ions with static and TR-XAS at the copper K-edge. These data reveal that copper captures a hole from the photoexcited InP NC, and relaxation to the ground state occurs via multiple timescales likely due to the presence of interior and surface-bound dopant ions as well as recombination with surfaceand defect-trapped electrons. Large-scale DFT calculations reveal a striking dependence of the electronic structure on the ligand coating and other effects such as self-compensation.},
doi = {10.1021/acs.jpcc.8b02124},
journal = {Journal of Physical Chemistry. C},
number = 20,
volume = 122,
place = {United States},
year = {2018},
month = {4}
}

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