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Unravelling the Correlation of Electronic Structure and Carrier Dynamics in CuInS2 Nanoparticles C

Author:
Hu, Wenhui, Ludwig, John, Pattengale, Brian, Yang, Sizhuo, Liu, Cunming, Zuo, Xiaobing, Zhang, Xiaoyi, Huang, Jier
Source:
Journal of physical chemistry 2018 v.122 no.1 pp. 974-980
ISSN:
1932-7455
Subject:
X-radiation, X-ray absorption spectroscopy, absorption, copper, electrons, nanoparticles
Abstract:
In this work, 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.
Agid:
6059294