Optoelectronic properties of candidate photovoltaic Cu2PbSiS4, Ag2PbGeS4 and KAg2SbS4 semiconductors

Nhalil, Hariharan; Han, Dan; Du, Mao-Hua; Chen, Shiyou; Antonio, Daniel; Gofryk, Krzysztof; Saparov, Bayrammurad

doi:10.1016/j.jallcom.2018.02.331

Title: Optoelectronic properties of candidate photovoltaic Cu₂PbSiS₄, Ag₂PbGeS₄ and KAg₂SbS₄ semiconductors

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Abstract

High temperature synthesis and optical band gaps are reported for three candidate photovoltaic earth-abundant Cu2PbSiS4, Ag2PbGeS4 and KAg2SbS4 semiconductors. The reported synthesis method is found to be more advantageous for KAg2SbS4 compared to the literature reported synthesis utilizing supercritical ammonia as a reaction medium, which produces a mixture of chalcogenide products. Based on optical diffuse reflectance data, Cu2PbSiS4, Ag2PbGeS4 and KAg2SbS4 have band gaps in the 1.6-1.8 eV range, and are shown to be stable in ambient air for a period of 6 weeks, making them attractive candidates for solar cell applications. Density functional theory (DFT) calculations indicate indirect band gaps for Cu2PbSiS4 and KAg2SbS4, and a nearly direct band gap for Ag2PbGeS4 with the calculated difference between indirect and direct gaps of only 30 meV. The p-type semiconducting behavior of Cu2PbSiS4, Ag2PbGeS4 is also verified by the transport measurements. The 3D connectivity of the polyanionic networks in these compounds results in dispersive valence and conduction bands, which is especially noticeable for KAg2SbS4. This fact is in part attributed to the presence of formally pentavalent SbV in this compound leading to empty Sb 5s orbitals in the conduction band. We discuss the potential of Cu2PbSiS4, Ag2PbGeS4 and KAg2SbS4 for photovoltaicmore »« less

Authors:

^[1]; Han, Dan ^[2];

^[3];

^[4]; Antonio, Daniel ^[5];

^[5];

^[1]

Univ. of Oklahoma, Norman, OK (United States). Dept. of Chemistry and Biochemistry
East China Normal Univ. (ECNU), Shanghai (China). Key Lab. of Polar Materials and Devices, Ministry of Education; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
East China Normal Univ. (ECNU), Shanghai (China). Key Lab. of Polar Materials and Devices, Ministry of Education
Idaho National Lab. (INL), Idaho Falls, ID (United States)

Publication Date:: Thu Mar 01 00:00:00 EST 2018

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Idaho National Lab. (INL), Idaho Falls, ID (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); DOE's Early Career Research Program

OSTI Identifier:: 1435252

Alternate Identifier(s):: OSTI ID: 1558455

Report Number(s):: INL/JOU-18-44806-Rev000
Journal ID: ISSN 0925-8388

Grant/Contract Number:: AC05-00OR22725; AC07-05ID14517

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Alloys and Compounds

Additional Journal Information:: Journal Volume: 746; Journal Issue: C; Journal ID: ISSN 0925-8388

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 14 SOLAR ENERGY; Chalcogenides; Semiconductor; Photovoltaic; Band gap; 75 - CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; semiconductors; Optoelectronic properties

Citation Formats


                    Nhalil, Hariharan, Han, Dan, Du, Mao-Hua, Chen, Shiyou, Antonio, Daniel, Gofryk, Krzysztof, and Saparov, Bayrammurad. Optoelectronic properties of candidate photovoltaic Cu2PbSiS4, Ag2PbGeS4 and KAg2SbS4 semiconductors.  United States: N. p., 2018. 
Web.  doi:10.1016/j.jallcom.2018.02.331.

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                    Nhalil, Hariharan, Han, Dan, Du, Mao-Hua, Chen, Shiyou, Antonio, Daniel, Gofryk, Krzysztof, & Saparov, Bayrammurad. Optoelectronic properties of candidate photovoltaic Cu2PbSiS4, Ag2PbGeS4 and KAg2SbS4 semiconductors.  United States.  https://doi.org/10.1016/j.jallcom.2018.02.331

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                    Nhalil, Hariharan, Han, Dan, Du, Mao-Hua, Chen, Shiyou, Antonio, Daniel, Gofryk, Krzysztof, and Saparov, Bayrammurad. Thu .  
"Optoelectronic properties of candidate photovoltaic Cu2PbSiS4, Ag2PbGeS4 and KAg2SbS4 semiconductors".  United States.  https://doi.org/10.1016/j.jallcom.2018.02.331.  https://www.osti.gov/servlets/purl/1435252.

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@article{osti_1435252,

  title        = {Optoelectronic properties of candidate photovoltaic Cu2PbSiS4, Ag2PbGeS4 and KAg2SbS4 semiconductors},

  author       = {Nhalil, Hariharan and Han, Dan and Du, Mao-Hua and Chen, Shiyou and Antonio, Daniel and Gofryk, Krzysztof and Saparov, Bayrammurad},

  abstractNote = {High temperature synthesis and optical band gaps are reported for three candidate photovoltaic earth-abundant Cu2PbSiS4, Ag2PbGeS4 and KAg2SbS4 semiconductors. The reported synthesis method is found to be more advantageous for KAg2SbS4 compared to the literature reported synthesis utilizing supercritical ammonia as a reaction medium, which produces a mixture of chalcogenide products. Based on optical diffuse reflectance data, Cu2PbSiS4, Ag2PbGeS4 and KAg2SbS4 have band gaps in the 1.6-1.8 eV range, and are shown to be stable in ambient air for a period of 6 weeks, making them attractive candidates for solar cell applications. Density functional theory (DFT) calculations indicate indirect band gaps for Cu2PbSiS4 and KAg2SbS4, and a nearly direct band gap for Ag2PbGeS4 with the calculated difference between indirect and direct gaps of only 30 meV. The p-type semiconducting behavior of Cu2PbSiS4, Ag2PbGeS4 is also verified by the transport measurements. The 3D connectivity of the polyanionic networks in these compounds results in dispersive valence and conduction bands, which is especially noticeable for KAg2SbS4. This fact is in part attributed to the presence of formally pentavalent SbV in this compound leading to empty Sb 5s orbitals in the conduction band. We discuss the potential of Cu2PbSiS4, Ag2PbGeS4 and KAg2SbS4 for photovoltaic applications based on synthesis, stability, band gap and electronic structure considerations.},

  doi          = {10.1016/j.jallcom.2018.02.331},

  journal      = {Journal of Alloys and Compounds},

  number       = C,

  volume       = 746,

  place        = {United States},

  year         = {Thu Mar 01 00:00:00 EST 2018},

  month        = {Thu Mar 01 00:00:00 EST 2018}

}

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Title: Optoelectronic properties of candidate photovoltaic Cu2PbSiS4, Ag2PbGeS4 and KAg2SbS4 semiconductors

Abstract

Citation Formats

Title: Optoelectronic properties of candidate photovoltaic Cu₂PbSiS₄, Ag₂PbGeS₄ and KAg₂SbS₄ semiconductors