TY - JOUR
T1 - Single-Crystal Growth and Characterization of the Chalcopyrite Semiconductor CuInTe 2 for Photoelectrochemical Solar Fuel Production
AU - Frick, Jessica J.
AU - Topp, Andreas
AU - Klemenz, Sebastian
AU - Krivenkov, Maxim
AU - Varykhalov, Andrei
AU - Ast, Christian R.
AU - Bocarsly, Andrew Bruce
AU - Schoop, Leslie Mareike
N1 - Funding Information:
The authors thank Prof. Robert Cava for instrumentation used in material synthesis and transport property characterization. The authors thank Nan Yao, John Schrieber, and Yao-Wen Yeh for invaluable assistance with X-ray photoelectron spectroscopy. We thank HZB for the allocation of synchrotron radiation beamtime. This manuscript is based upon work supported by the National Science Foundation Graduate Research Fellowship via Grant 1656466 awarded to J.J.F. A.T. was supported by the DFG proposal no. SCHO 1730/1-1. The authors gratefully acknowledge the U.S. Department of Energy for financial support. A.B.B. acknowledges Grant DE-SC0002133. L.M.S. acknowledges funding from the Princeton Catalysis Initiative (PCI).
Publisher Copyright:
Copyright © 2018 American Chemical Society.
PY - 2018/12/6
Y1 - 2018/12/6
N2 - Transition-metal chalcogenides are a promising family of materials for applications as photocathodes in photoelectrochemical (PEC) H 2 generation. A long-standing challenge for chalcopyrite semiconductors is characterizing their electronic structure, both experimentally and theoretically, because of their relatively high-energy band gaps and spin-orbit coupling (SOC), respectively. In this work, we present single crystals of CuInTe 2 , whose relatively small optically measured band gap of 0.9 ± 0.03 eV enables electronic structure characterization by angle-resolved photoelectron spectroscopy (ARPES) in conjunction with first-principles calculations incorporating SOC. ARPES measurements reveal bands that are steeply dispersed in energy with a band velocity of 2.5-5.4 × 10 5 m/s, almost 50% of the extremely conductive material graphene. Additionally, CuInTe 2 single crystals are fabricated into electrodes to experimentally determine the valence band edge energy and confirm the thermodynamic suitability of CuInTe 2 for water redox chemistry. The electronic structure characterization and band edge position presented in this work provide kinetic and thermodynamic factors that support CuInTe 2 as a strong candidate for water reduction.
AB - Transition-metal chalcogenides are a promising family of materials for applications as photocathodes in photoelectrochemical (PEC) H 2 generation. A long-standing challenge for chalcopyrite semiconductors is characterizing their electronic structure, both experimentally and theoretically, because of their relatively high-energy band gaps and spin-orbit coupling (SOC), respectively. In this work, we present single crystals of CuInTe 2 , whose relatively small optically measured band gap of 0.9 ± 0.03 eV enables electronic structure characterization by angle-resolved photoelectron spectroscopy (ARPES) in conjunction with first-principles calculations incorporating SOC. ARPES measurements reveal bands that are steeply dispersed in energy with a band velocity of 2.5-5.4 × 10 5 m/s, almost 50% of the extremely conductive material graphene. Additionally, CuInTe 2 single crystals are fabricated into electrodes to experimentally determine the valence band edge energy and confirm the thermodynamic suitability of CuInTe 2 for water redox chemistry. The electronic structure characterization and band edge position presented in this work provide kinetic and thermodynamic factors that support CuInTe 2 as a strong candidate for water reduction.
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U2 - 10.1021/acs.jpclett.8b03100
DO - 10.1021/acs.jpclett.8b03100
M3 - Article
C2 - 30433790
AN - SCOPUS:85058136786
SN - 1948-7185
VL - 9
SP - 6833
EP - 6840
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 23
ER -