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Title: Characterization of Primary Carrier Transport Properties of the Light-Harvesting Chalcopyrite Semiconductors CuIn(S 1–xSe x) 2

Abstract

We report the carrier transport properties of CuIn(S 1-xSe x) 2 (0 ≤ x ≤ 1), a promising chalcopyrite semiconductor series for solar water splitting. A low concentration Mg dopant is used to decrease the carrier resistivity through facilitating bulk p-type transport at ambient temperature. Temperature-dependent resistivity measurements reveal a four-order magnitude decrease in bulk electrical resistivity (from 10 3 to 10 –1 Ohm cm) for 1% Mg-doped CuIn(S 1–xSe x) 2 as x increases from 0 to 1. Hall effect measurements at room temperature reveal p-type majority carrier concentrations that vary from 10 15 to 10 18 cm –3 and mobilities of approximately 1–10 cm 2 V –1 s –1. These results provide insights into the fundamental carrier transport properties of CuIn(S 1–xSe x) 2 and will be of value in optimizing these materials further for photoelectrochemistry applications.

Authors:
 [1];  [1];  [1]; ORCiD logo [1]
  1. Princeton Univ., NJ (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Princeton Univ., NJ (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1418173
Alternate Identifier(s):
OSTI ID: 1374233
Grant/Contract Number:
SC0002133; AC02-05CH11231; F602-98ER45706
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 121; Journal Issue: 32; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 30 DIRECT ENERGY CONVERSION; p-type semiconductors; photoelectrochemistry; chalcopyrites; hydrogen from water

Citation Formats

Frick, Jessica J., Kushwaha, Satya K., Cava, Robert J., and Bocarsly, Andrew B.. Characterization of Primary Carrier Transport Properties of the Light-Harvesting Chalcopyrite Semiconductors CuIn(S1–xSex)2. United States: N. p., 2017. Web. doi:10.1021/acs.jpcc.7b03152.
Frick, Jessica J., Kushwaha, Satya K., Cava, Robert J., & Bocarsly, Andrew B.. Characterization of Primary Carrier Transport Properties of the Light-Harvesting Chalcopyrite Semiconductors CuIn(S1–xSex)2. United States. doi:10.1021/acs.jpcc.7b03152.
Frick, Jessica J., Kushwaha, Satya K., Cava, Robert J., and Bocarsly, Andrew B.. Thu . "Characterization of Primary Carrier Transport Properties of the Light-Harvesting Chalcopyrite Semiconductors CuIn(S1–xSex)2". United States. doi:10.1021/acs.jpcc.7b03152.
@article{osti_1418173,
title = {Characterization of Primary Carrier Transport Properties of the Light-Harvesting Chalcopyrite Semiconductors CuIn(S1–xSex)2},
author = {Frick, Jessica J. and Kushwaha, Satya K. and Cava, Robert J. and Bocarsly, Andrew B.},
abstractNote = {We report the carrier transport properties of CuIn(S1-xSex)2 (0 ≤ x ≤ 1), a promising chalcopyrite semiconductor series for solar water splitting. A low concentration Mg dopant is used to decrease the carrier resistivity through facilitating bulk p-type transport at ambient temperature. Temperature-dependent resistivity measurements reveal a four-order magnitude decrease in bulk electrical resistivity (from 103 to 10–1 Ohm cm) for 1% Mg-doped CuIn(S1–xSex)2 as x increases from 0 to 1. Hall effect measurements at room temperature reveal p-type majority carrier concentrations that vary from 1015 to 1018 cm–3 and mobilities of approximately 1–10 cm2 V–1 s–1. These results provide insights into the fundamental carrier transport properties of CuIn(S1–xSex)2 and will be of value in optimizing these materials further for photoelectrochemistry applications.},
doi = {10.1021/acs.jpcc.7b03152},
journal = {Journal of Physical Chemistry. C},
number = 32,
volume = 121,
place = {United States},
year = {Thu Jul 27 00:00:00 EDT 2017},
month = {Thu Jul 27 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
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  • Graphical abstract: - Highlights: • A facile and rapid one-pot synthesis method is presented. • The effects of various Ga contents are investigated. • Single phase chalcopyrite CuIn{sub 1−x}Ga{sub x}Se{sub 2} nanoparticles can be easily synthesized. • The phase formation sequence is from CuSe to CuGaSe{sub 2}, then to CuIn{sub 1−x}Ga{sub x}Se{sub 2}. • The possible reaction mechanism of CuIn{sub 1−x}Ga{sub x}Se{sub 2} nanoparticles is proposed. - Abstract: Single phase chalcopyrite and near stoichiometric CuIn{sub 1−x}Ga{sub x}Se{sub 2} (0 ≤ x ≤ 1) nanoparticles were successfully synthesized by using a facile and rapid one-pot method. The effects of various Gamore » contents on crystal phase, morphology, element composition and absorption spectrum of the as-synthesized CuIn{sub 1−x}Ga{sub x}Se{sub 2} nanoparticles were investigated in detail. The XRD and Raman patterns indicated that the as-synthesized nanoparticles had a single phase chalcopyrite structure, and the diffraction peaks shifted toward larger diffraction angles or higher frequencies with increasing Ga content. The FE-SEM images showed that the as-synthesized nanoparticles were polydispersed in both size and shape, and the nanoparticles with higher Ga content were more prone to aggregate. The Vis–IR absorption spectra showed strong absorption in the entire visible light region. The estimated band gap increased from 1.00 eV to 1.68 eV as Ga content increasing.« less
  • We report the results of spectroscopic time-resolved photoluminescence (TRPL) analysis for polycrystalline CuIn 1-xGa xSe 2 (CIGS) films. On the <5 ns time scale, we investigated minority carrier spatial redistribution from the initial absorption profile near the surface of the films to the conduction band minimum. Based on these data, the estimated minority carrier mobility is 75–230 cm 2 V -1s -1. Full TRPL decays were analyzed using models for donor-acceptor pair (DAP) recombination. We estimated that the concentration of DAP recombination centers was 5×10 15–10 17cm -3. Data also show that Shockley-Reed-Hall and surface recombination are not significant formore » polycrystalline CIGS absorbers used in high-efficiency photovoltaic solar cells.« less
  • We used time-resolved photoluminescence (TRPL) spectroscopy to analyze time-domain and spectral-domain charge-carrier dynamics in CuIn{sub 1−x}Ga{sub x}Se{sub 2} (CIGS) photovoltaic (PV) devices. This new approach allowed detailed characterization for the CIGS/CdS buffer interface and for the space-charge region. We find that dynamics at the interface is dominated by diffusion, where the diffusion rate is several times greater than the thermionic emission or interface recombination rate. In the space-charge region, the electric field of the pn junction has the largest effect on the carrier dynamics. Based on the minority-carrier (electron) drift-rate dependence on the electric field strength, we estimated drift mobilitymore » in compensated CuIn{sub 1−x}Ga{sub x}Se{sub 2} (with x ≈ 0.3) as 22 ± 2 cm{sup 2}(Vs){sup −1}. Analysis developed in this study could be applied to evaluate interface and junction properties of PV and other electronic devices. For CIGS PV devices, TRPL spectroscopy could contribute to understanding effects due to absorber compositional grading, which is one of the focus areas in developing record-efficiency CIGS solar cells.« less