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Title: Unravelling the Correlation of Electronic Structure and Carrier Dynamics in CuInS 2 Nanoparticles

Here, we report the direct correlation of photoinduced carrier dynamics and electronic structure of CuInS 2 (CIS) nanoparticles (NPs) using the combination of multiple spectroscopic techniques including steady-state X-ray absorption spectroscopy (XAS), optical transient absorption (OTA), and X-ray transient (XTA) absorption spectroscopy. XAS results show that CIS NPs contain a large amount of surface Cu atoms with << four-coordination, which is more severe in CIS NPs with shorter nucleation times, indicating the presence of more Cu defect states in CIS NPs with smaller size particles. Using the combination of OTA and XTA spectroscopy, we show that electrons are trapped at states with mainly In or S nature while holes are trapped in sites characteristic of Cu. While there is no direct correlation of ultrafast trapping dynamics with NP nucleation time, charge recombination is significantly inhibited in CIS NPs with larger particles. These results suggest the key roles that Cu defect sites play in carrier dynamics and imply the possibility to control the carrier dynamics by controlling the surface structure at the Cu site in CIS NPs.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [2] ; ORCiD logo [2] ; ORCiD logo [1]
  1. Marquette Univ., Milwaukee, WI (United States). Dept. of Chemistry
  2. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
Publication Date:
Grant/Contract Number:
AC02-06CH11357; DMR-1654140; 57503-DNI6
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 122; Journal Issue: 1; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF); American Chemical Society Petroleum Research Fund (ACS-PRF)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1461303

Hu, Wenhui, Ludwig, John, Pattengale, Brian, Yang, Sizhuo, Liu, Cunming, Zuo, Xiaobing, Zhang, Xiaoyi, and Huang, Jier. Unravelling the Correlation of Electronic Structure and Carrier Dynamics in CuInS2 Nanoparticles. United States: N. p., Web. doi:10.1021/acs.jpcc.7b11369.
Hu, Wenhui, Ludwig, John, Pattengale, Brian, Yang, Sizhuo, Liu, Cunming, Zuo, Xiaobing, Zhang, Xiaoyi, & Huang, Jier. Unravelling the Correlation of Electronic Structure and Carrier Dynamics in CuInS2 Nanoparticles. United States. doi:10.1021/acs.jpcc.7b11369.
Hu, Wenhui, Ludwig, John, Pattengale, Brian, Yang, Sizhuo, Liu, Cunming, Zuo, Xiaobing, Zhang, Xiaoyi, and Huang, Jier. 2017. "Unravelling the Correlation of Electronic Structure and Carrier Dynamics in CuInS2 Nanoparticles". United States. doi:10.1021/acs.jpcc.7b11369. https://www.osti.gov/servlets/purl/1461303.
@article{osti_1461303,
title = {Unravelling the Correlation of Electronic Structure and Carrier Dynamics in CuInS2 Nanoparticles},
author = {Hu, Wenhui and Ludwig, John and Pattengale, Brian and Yang, Sizhuo and Liu, Cunming and Zuo, Xiaobing and Zhang, Xiaoyi and Huang, Jier},
abstractNote = {Here, we report the direct correlation of photoinduced carrier dynamics and electronic structure of CuInS2 (CIS) nanoparticles (NPs) using the combination of multiple spectroscopic techniques including steady-state X-ray absorption spectroscopy (XAS), optical transient absorption (OTA), and X-ray transient (XTA) absorption spectroscopy. XAS results show that CIS NPs contain a large amount of surface Cu atoms with << four-coordination, which is more severe in CIS NPs with shorter nucleation times, indicating the presence of more Cu defect states in CIS NPs with smaller size particles. Using the combination of OTA and XTA spectroscopy, we show that electrons are trapped at states with mainly In or S nature while holes are trapped in sites characteristic of Cu. While there is no direct correlation of ultrafast trapping dynamics with NP nucleation time, charge recombination is significantly inhibited in CIS NPs with larger particles. These results suggest the key roles that Cu defect sites play in carrier dynamics and imply the possibility to control the carrier dynamics by controlling the surface structure at the Cu site in CIS NPs.},
doi = {10.1021/acs.jpcc.7b11369},
journal = {Journal of Physical Chemistry. C},
number = 1,
volume = 122,
place = {United States},
year = {2017},
month = {12}
}