Influence of Copper Composition on Cu2BaSn(S,Se)4 Solution-Deposited Films and Photovoltaic Devices with Over 5% Efficiency
Abstract
Cu2BaSn(S,Se)4 is currently in the spotlight for prospective environmentally friendly, stable, thin-film solar cell application, with demonstrated device power conversion efficiency (PCE) exceeding 5% for vacuum-deposited absorbers. As suggested by first-principles calculations, experimental studies involving related Cu2ZnSn(S,Se)4 and Cu(In,Ga)(S,Se)2 absorbers prove that the detailed chemical composition typically plays a sensitive role in altering defects and electronic properties of these complicated compound semiconductors. Herein, the copper composition of Cu2BaSn(S,Se)4 has been systematically modified, employing a solution-based deposition approach, to provide a more complete picture of the phase stability and optoelectronic property sensitivity for this material. X-ray diffraction and scanning electron microscopy show that phase purity is preserved over a film Cu content range of nominally 0.94 ≤ [Cu]/[Ba + Sn] ≤ 1.01. Terahertz spectroscopy and Hall effect measurements reveal that the majority carrier hole density of ~1013 cm–3 and mobility (~5 cm2/V s), as well as the minority carrier lifetime (a bulk lifetime of 180 ps and a surface recombination velocity >106 cm/s), are nominally independent of Cu content. The champion PCEs exceed 4.7% for all copper compositions in the phase-pure region, with a record value of 5.1%, similar to the reported values for record vacuum-deposited devices. Furthermore, these results suggestmore »
- Authors:
-
[2];
[1]
- Duke Univ., Durham, NC (United States)
- Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Berlin (Germany)
- IBM T. J. Watson Research Center, New York, NY (United States)
- Publication Date:
- Research Org.:
- Duke Univ., Durham, NC (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1903140
- Grant/Contract Number:
- SC0020061
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Energy Materials
- Additional Journal Information:
- Journal Volume: 5; Journal Issue: 9; Journal ID: ISSN 2574-0962
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 14 SOLAR ENERGY; copper composition; optoelectronic properties; Cu2BaSn(S,Se)4; (CBTSSe); chalcogenides; solar cells; copper; layers; power conversion efficiency; precursors; thin films
Citation Formats
Teymur, Betul, Choubrac, Leo, Hempel, Hannes, Gunawan, Oki, Unold, Thomas, and Mitzi, David B. Influence of Copper Composition on Cu2BaSn(S,Se)4 Solution-Deposited Films and Photovoltaic Devices with Over 5% Efficiency. United States: N. p., 2022.
Web. doi:10.1021/acsaem.2c01364.
Teymur, Betul, Choubrac, Leo, Hempel, Hannes, Gunawan, Oki, Unold, Thomas, & Mitzi, David B. Influence of Copper Composition on Cu2BaSn(S,Se)4 Solution-Deposited Films and Photovoltaic Devices with Over 5% Efficiency. United States. https://doi.org/10.1021/acsaem.2c01364
Teymur, Betul, Choubrac, Leo, Hempel, Hannes, Gunawan, Oki, Unold, Thomas, and Mitzi, David B. Tue .
"Influence of Copper Composition on Cu2BaSn(S,Se)4 Solution-Deposited Films and Photovoltaic Devices with Over 5% Efficiency". United States. https://doi.org/10.1021/acsaem.2c01364. https://www.osti.gov/servlets/purl/1903140.
@article{osti_1903140,
title = {Influence of Copper Composition on Cu2BaSn(S,Se)4 Solution-Deposited Films and Photovoltaic Devices with Over 5% Efficiency},
author = {Teymur, Betul and Choubrac, Leo and Hempel, Hannes and Gunawan, Oki and Unold, Thomas and Mitzi, David B.},
abstractNote = {Cu2BaSn(S,Se)4 is currently in the spotlight for prospective environmentally friendly, stable, thin-film solar cell application, with demonstrated device power conversion efficiency (PCE) exceeding 5% for vacuum-deposited absorbers. As suggested by first-principles calculations, experimental studies involving related Cu2ZnSn(S,Se)4 and Cu(In,Ga)(S,Se)2 absorbers prove that the detailed chemical composition typically plays a sensitive role in altering defects and electronic properties of these complicated compound semiconductors. Herein, the copper composition of Cu2BaSn(S,Se)4 has been systematically modified, employing a solution-based deposition approach, to provide a more complete picture of the phase stability and optoelectronic property sensitivity for this material. X-ray diffraction and scanning electron microscopy show that phase purity is preserved over a film Cu content range of nominally 0.94 ≤ [Cu]/[Ba + Sn] ≤ 1.01. Terahertz spectroscopy and Hall effect measurements reveal that the majority carrier hole density of ~1013 cm–3 and mobility (~5 cm2/V s), as well as the minority carrier lifetime (a bulk lifetime of 180 ps and a surface recombination velocity >106 cm/s), are nominally independent of Cu content. The champion PCEs exceed 4.7% for all copper compositions in the phase-pure region, with a record value of 5.1%, similar to the reported values for record vacuum-deposited devices. Furthermore, these results suggest that Cu2BaSn(S,Se)4 films and solar cells (at the current performance level) may be less sensitive to Cu stoichiometry compared to kesterite materials and therefore may provide a more stable material platform to prepare thin-film solar cells.},
doi = {10.1021/acsaem.2c01364},
journal = {ACS Applied Energy Materials},
number = 9,
volume = 5,
place = {United States},
year = {Tue Aug 23 00:00:00 EDT 2022},
month = {Tue Aug 23 00:00:00 EDT 2022}
}
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