Wide Band Gap CuGa(S,Se)2 Thin Films on Transparent Conductive Fluorinated Tin Oxide Substrates as Photocathode Candidates for Tandem Water Splitting Devices

DeAngelis, Alexander D.; Horsley, Kimberly; Gaillard, Nicolas

doi:10.1021/acs.jpcc.8b02915

Title: Wide Band Gap CuGa(S,Se)₂ Thin Films on Transparent Conductive Fluorinated Tin Oxide Substrates as Photocathode Candidates for Tandem Water Splitting Devices

Journal Article · Sun Jun 03 00:00:00 EDT 2018 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.8b02915· OSTI ID:1570461

^[1]; Horsley, Kimberly ^[1]; Gaillard, Nicolas ^[1]

Univ. of Hawaii, Honolulu, HI (United States)

Theaim of this report was to explore the potential of CuGa(S,Se)2 thin films as wide-E_G top cell absorbers for photoelectrochemical (PEC) water splitting. A synthesis was developed on fluorinated tin oxide (FTO) photocathodes by converting copper-rich co-evaporated CuGaSe2 into CuGa(S,Se)2 via a post-deposition annealing. We found it necessary to first anneal CuGaSe2 at low-temperature in sulfur then at high-temperature in nitrogen to preserve the transparency and conductivity of the FTO. Using this two-step synthesis, we fabricated a 1.72eV CuGa(S,Se)₂photocathode with a saturation current density and photocurrent onset potential of 10mA/cm² and -0.20V vs. RHE, respectively. Yet we found that the PEC performance and sub-E_G transmittance, worsened with increasing copper content. Using flatband potential measurements and the Gerischer model, we show that divergences in PEC performance of CuGa(S,Se)₂ photocathodes can be explained by differences in conduction band minimums and Fermi levels. We also explain that sub-E_G transmittance is likely hampered by a defect band 100-400 meV below E_C. Additional external quantum efficiency measurements of a high-efficiency 1.1 eV Cu(In,Ga)Se₂ photovoltaic driver, while shaded by the CuGa(S,Se)₂ photocathode, yielded a short-circuit current density of 4.14 mA/cm² revealing that CuGa(S,Se)₂ reflects promise as a top cell for PEC water splitting.

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Research Organization:: Univ. of Hawaii, Honolulu, HI (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Hydrogen Fuel Cell Technologies Office (HFTO)

Grant/Contract Number:: EE0006670

OSTI ID:: 1570461

Journal Information:: Journal of Physical Chemistry. C, Vol. 122, Issue 26; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 22 works

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