Abstract

Barium copper sulfur fluoride (BaCuSF) is a p-type transparent conductor (p-TC) that, when doped with potassium, exhibits exceptionally high conductivity. The results of a detailed optical and electronic characterization of BaCuSF thin films deposited at a substrate temperature of 100 °C are presented. X-ray diffractometry shows the presence of a cubic BaCuSF phase. Spectroscopic measurements demonstrate that the films transmit from the visible through the mid-infrared with a band gap of 1.8 eV. Hall measurements indicate that the material is a degenerate semiconductor. As deposited, the films exhibit conductivity at room temperature of approximately 260 S/cm – among the highest reported room temperature conductivities for p-TCs. After post-deposition treatment in water, their conductivity increases to as high as 800 S/cm, and their band gap is reduced to 1.5 eV. The potential for low temperature deposition of p-type films with high conductivity and optical transmittance makes BaCuSF promising for several applications including flexible electronics and photovoltaics.

© 2013 Optical Society of America

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  1. H. Kawazoe, M. Yasukawa, H. Hyodo, M. Kurita, H. Yanagi, and H. Hosono, “P-type electrical conduction in transparent thin films of CuAlO2,” Nature389(6654), 939–942 (1997).
    [CrossRef]
  2. R. R. Owings, G. J. Exarhos, C. F. Windisch, P. H. Holloway, and J. G. Wen, “Process enhanced polaron conductivity of infrared transparent nickel–cobalt oxide,” Thin Solid Films483(1–2), 175–184 (2005).
    [CrossRef]
  3. H. Hiramatsu, K. Ueda, H. Ohta, M. Hirano, M. Kikuchi, H. Yanagi, T. Kamiya, and H. Hosono, “Heavy hole doping of epitaxial thin films of a wide gap p-type semiconductor, LaCuOSe, and analysis of the effective mass,” Appl. Phys. Lett.91(1), 012104 (2007).
    [CrossRef]
  4. A. Klein, “Transparent conducting oxides: Electronic structure-property relationship from photoelectron spectroscopy with in situ sample preparation,” J. Am. Ceram. Soc.96, 331–345 (2013).
  5. E. Fortunato, R. Barros, P. Barquinha, V. Figueiredo, S.-H. K. Park, C.-S. Hwang, and R. Martins, “Transparent p-type SnOx thin film transistors produced by reactive rf magnetron sputtering followed by low temperature annealing,” Appl. Phys. Lett.97(5), 052105 (2010).
    [CrossRef]
  6. G. Hautier, A. Miglio, G. Ceder, G.-M. Rignanese, and X. Gonze, “Identification and design principles of low hole effective mass p-type transparent conducting oxides,” Nat Commun.4, 2292 (2013).
    [CrossRef] [PubMed]
  7. S. Inoue, K. Ueda, H. Hosono, and N. Hamada, “Electronic structure of the transparent p-type semiconductor (LaO)CuS,” Phys. Rev. B64(24), 245211 (2001).
    [CrossRef]
  8. J. Tate, P. F. Newhouse, R. Kykyneshi, P. A. Hersh, J. Kinney, D. H. McIntyre, and D. A. Keszler, “Chalcogen-based transparent conductors,” Thin Solid Films516(17), 5795–5799 (2008).
    [CrossRef]
  9. W. Zhu, Y. Huang, F. Wu, C. Dong, H. Chen, and Z. Zhao, “Synthesis and crystal structure of barium copper fluorochalcogenides: [BaCuFQ (Q=S,Se)],” Mater. Res. Bull.29(5), 505–508 (1994).
    [CrossRef]
  10. H. Yanagi, S. Park, A. D. Draeske, D. Keszler, and J. Tate, “P-type conductivity in transparent oxides and sulfide fluorides,” J. Solid State Chem.175(1), 34–38 (2003).
    [CrossRef]
  11. H. Yanagi, J. Tate, S. Park, C.-H. Park, D. A. Keszler, M. Hirano, and H. Hosono, “Valence band structure of BaCuSF and BaCuSeF,” J. Appl. Phys.100(8), 083705 (2006).
    [CrossRef]
  12. A. Zakutayev, D. H. McIntyre, G. Schneider, R. Kykyneshi, D. A. Keszler, C.-H. Park, and J. Tate, “Tunable properties of wide-band gap p-type BaCu(Ch1−xCh’x)F (Ch = S, Se, Te) thin-film solid solutions,” Thin Solid Films518(19), 5494–5500 (2010).
    [CrossRef]
  13. J. A. Frantz, J. S. Sanghera, V. Q. Nguyen, S. S. Bayya, S. B. Qadri, and I. D. Aggarwal, “Formation of a new phase of barium copper sulfur fluoride via sputtering,” Mater. Lett.62(10-11), 1582–1584 (2008).
    [CrossRef]
  14. J. A. Frantz, J. S. Sanghera, S. B. Qadri, and I. D. Aggarwal, “Record conductivity for p-type transparent conductors in polycrystalline thin films of a sulfide-fluoride,” in Materials Research Society Symposium Proceedings (Materials Research Society, 2008) pp. 108–113.
    [CrossRef]
  15. J. A. Frantz, L. B. Shaw, J. S. Sanghera, and I. D. Aggarwal, “Waveguide amplifiers in sputtered films of Er3+-doped gallium lanthanum sulfide glass,” Opt. Express14(5), 1797–1803 (2006).
    [CrossRef] [PubMed]
  16. ASTM Standard F76–86, “Standard test methods for measuring resistivity and Hall coefficient and determining Hall mobility in single crystal semiconductors” (ASTM International, 2002).
  17. T. Hirschfeld and A. W. Mantz, “Elimination of thin film infrared channel spectra in Fourier transform infrared spectroscopy,” Infrared Spectrosc.30(5), 552–553 (1976).
    [CrossRef]
  18. J. Tauc, R. Grigorovici, and A. Vancu, “Optical properties and electronic structure of amorphous germanium,” Phys. Status Solidi15(2), 627–637 (1966).
    [CrossRef]
  19. A. J. Mäkinen, M. Uchida, and Z. H. Kafafi, “Electronic structure of a silole derivative-magnesium thin film interface,” J. Appl. Phys.95(5), 2832–2838 (2004).
    [CrossRef]
  20. M. Qvarford, J. F. van Acker, J. N. Anderson, R. Nyholm, I. Lindau, G. Chiaia, E. Lundgren, S. Söderholm, U. O. Karlsson, S. A. Flodström, and L. Leonyuk, “Resonant valence-band and Cu 3p photoemission at the Cu L3 threshold of Bi2Sr2CuO6 and Bi2Sr2CaCu2O8,” Phys. Rev. B51(1), 410–416 (1995).

2013

A. Klein, “Transparent conducting oxides: Electronic structure-property relationship from photoelectron spectroscopy with in situ sample preparation,” J. Am. Ceram. Soc.96, 331–345 (2013).

G. Hautier, A. Miglio, G. Ceder, G.-M. Rignanese, and X. Gonze, “Identification and design principles of low hole effective mass p-type transparent conducting oxides,” Nat Commun.4, 2292 (2013).
[CrossRef] [PubMed]

2010

E. Fortunato, R. Barros, P. Barquinha, V. Figueiredo, S.-H. K. Park, C.-S. Hwang, and R. Martins, “Transparent p-type SnOx thin film transistors produced by reactive rf magnetron sputtering followed by low temperature annealing,” Appl. Phys. Lett.97(5), 052105 (2010).
[CrossRef]

A. Zakutayev, D. H. McIntyre, G. Schneider, R. Kykyneshi, D. A. Keszler, C.-H. Park, and J. Tate, “Tunable properties of wide-band gap p-type BaCu(Ch1−xCh’x)F (Ch = S, Se, Te) thin-film solid solutions,” Thin Solid Films518(19), 5494–5500 (2010).
[CrossRef]

2008

J. A. Frantz, J. S. Sanghera, V. Q. Nguyen, S. S. Bayya, S. B. Qadri, and I. D. Aggarwal, “Formation of a new phase of barium copper sulfur fluoride via sputtering,” Mater. Lett.62(10-11), 1582–1584 (2008).
[CrossRef]

J. Tate, P. F. Newhouse, R. Kykyneshi, P. A. Hersh, J. Kinney, D. H. McIntyre, and D. A. Keszler, “Chalcogen-based transparent conductors,” Thin Solid Films516(17), 5795–5799 (2008).
[CrossRef]

2007

H. Hiramatsu, K. Ueda, H. Ohta, M. Hirano, M. Kikuchi, H. Yanagi, T. Kamiya, and H. Hosono, “Heavy hole doping of epitaxial thin films of a wide gap p-type semiconductor, LaCuOSe, and analysis of the effective mass,” Appl. Phys. Lett.91(1), 012104 (2007).
[CrossRef]

2006

H. Yanagi, J. Tate, S. Park, C.-H. Park, D. A. Keszler, M. Hirano, and H. Hosono, “Valence band structure of BaCuSF and BaCuSeF,” J. Appl. Phys.100(8), 083705 (2006).
[CrossRef]

J. A. Frantz, L. B. Shaw, J. S. Sanghera, and I. D. Aggarwal, “Waveguide amplifiers in sputtered films of Er3+-doped gallium lanthanum sulfide glass,” Opt. Express14(5), 1797–1803 (2006).
[CrossRef] [PubMed]

2005

R. R. Owings, G. J. Exarhos, C. F. Windisch, P. H. Holloway, and J. G. Wen, “Process enhanced polaron conductivity of infrared transparent nickel–cobalt oxide,” Thin Solid Films483(1–2), 175–184 (2005).
[CrossRef]

2004

A. J. Mäkinen, M. Uchida, and Z. H. Kafafi, “Electronic structure of a silole derivative-magnesium thin film interface,” J. Appl. Phys.95(5), 2832–2838 (2004).
[CrossRef]

2003

H. Yanagi, S. Park, A. D. Draeske, D. Keszler, and J. Tate, “P-type conductivity in transparent oxides and sulfide fluorides,” J. Solid State Chem.175(1), 34–38 (2003).
[CrossRef]

2001

S. Inoue, K. Ueda, H. Hosono, and N. Hamada, “Electronic structure of the transparent p-type semiconductor (LaO)CuS,” Phys. Rev. B64(24), 245211 (2001).
[CrossRef]

1997

H. Kawazoe, M. Yasukawa, H. Hyodo, M. Kurita, H. Yanagi, and H. Hosono, “P-type electrical conduction in transparent thin films of CuAlO2,” Nature389(6654), 939–942 (1997).
[CrossRef]

1995

M. Qvarford, J. F. van Acker, J. N. Anderson, R. Nyholm, I. Lindau, G. Chiaia, E. Lundgren, S. Söderholm, U. O. Karlsson, S. A. Flodström, and L. Leonyuk, “Resonant valence-band and Cu 3p photoemission at the Cu L3 threshold of Bi2Sr2CuO6 and Bi2Sr2CaCu2O8,” Phys. Rev. B51(1), 410–416 (1995).

1994

W. Zhu, Y. Huang, F. Wu, C. Dong, H. Chen, and Z. Zhao, “Synthesis and crystal structure of barium copper fluorochalcogenides: [BaCuFQ (Q=S,Se)],” Mater. Res. Bull.29(5), 505–508 (1994).
[CrossRef]

1976

T. Hirschfeld and A. W. Mantz, “Elimination of thin film infrared channel spectra in Fourier transform infrared spectroscopy,” Infrared Spectrosc.30(5), 552–553 (1976).
[CrossRef]

1966

J. Tauc, R. Grigorovici, and A. Vancu, “Optical properties and electronic structure of amorphous germanium,” Phys. Status Solidi15(2), 627–637 (1966).
[CrossRef]

Aggarwal, I. D.

J. A. Frantz, J. S. Sanghera, V. Q. Nguyen, S. S. Bayya, S. B. Qadri, and I. D. Aggarwal, “Formation of a new phase of barium copper sulfur fluoride via sputtering,” Mater. Lett.62(10-11), 1582–1584 (2008).
[CrossRef]

J. A. Frantz, L. B. Shaw, J. S. Sanghera, and I. D. Aggarwal, “Waveguide amplifiers in sputtered films of Er3+-doped gallium lanthanum sulfide glass,” Opt. Express14(5), 1797–1803 (2006).
[CrossRef] [PubMed]

Anderson, J. N.

M. Qvarford, J. F. van Acker, J. N. Anderson, R. Nyholm, I. Lindau, G. Chiaia, E. Lundgren, S. Söderholm, U. O. Karlsson, S. A. Flodström, and L. Leonyuk, “Resonant valence-band and Cu 3p photoemission at the Cu L3 threshold of Bi2Sr2CuO6 and Bi2Sr2CaCu2O8,” Phys. Rev. B51(1), 410–416 (1995).

Barquinha, P.

E. Fortunato, R. Barros, P. Barquinha, V. Figueiredo, S.-H. K. Park, C.-S. Hwang, and R. Martins, “Transparent p-type SnOx thin film transistors produced by reactive rf magnetron sputtering followed by low temperature annealing,” Appl. Phys. Lett.97(5), 052105 (2010).
[CrossRef]

Barros, R.

E. Fortunato, R. Barros, P. Barquinha, V. Figueiredo, S.-H. K. Park, C.-S. Hwang, and R. Martins, “Transparent p-type SnOx thin film transistors produced by reactive rf magnetron sputtering followed by low temperature annealing,” Appl. Phys. Lett.97(5), 052105 (2010).
[CrossRef]

Bayya, S. S.

J. A. Frantz, J. S. Sanghera, V. Q. Nguyen, S. S. Bayya, S. B. Qadri, and I. D. Aggarwal, “Formation of a new phase of barium copper sulfur fluoride via sputtering,” Mater. Lett.62(10-11), 1582–1584 (2008).
[CrossRef]

Ceder, G.

G. Hautier, A. Miglio, G. Ceder, G.-M. Rignanese, and X. Gonze, “Identification and design principles of low hole effective mass p-type transparent conducting oxides,” Nat Commun.4, 2292 (2013).
[CrossRef] [PubMed]

Chen, H.

W. Zhu, Y. Huang, F. Wu, C. Dong, H. Chen, and Z. Zhao, “Synthesis and crystal structure of barium copper fluorochalcogenides: [BaCuFQ (Q=S,Se)],” Mater. Res. Bull.29(5), 505–508 (1994).
[CrossRef]

Chiaia, G.

M. Qvarford, J. F. van Acker, J. N. Anderson, R. Nyholm, I. Lindau, G. Chiaia, E. Lundgren, S. Söderholm, U. O. Karlsson, S. A. Flodström, and L. Leonyuk, “Resonant valence-band and Cu 3p photoemission at the Cu L3 threshold of Bi2Sr2CuO6 and Bi2Sr2CaCu2O8,” Phys. Rev. B51(1), 410–416 (1995).

Dong, C.

W. Zhu, Y. Huang, F. Wu, C. Dong, H. Chen, and Z. Zhao, “Synthesis and crystal structure of barium copper fluorochalcogenides: [BaCuFQ (Q=S,Se)],” Mater. Res. Bull.29(5), 505–508 (1994).
[CrossRef]

Draeske, A. D.

H. Yanagi, S. Park, A. D. Draeske, D. Keszler, and J. Tate, “P-type conductivity in transparent oxides and sulfide fluorides,” J. Solid State Chem.175(1), 34–38 (2003).
[CrossRef]

Exarhos, G. J.

R. R. Owings, G. J. Exarhos, C. F. Windisch, P. H. Holloway, and J. G. Wen, “Process enhanced polaron conductivity of infrared transparent nickel–cobalt oxide,” Thin Solid Films483(1–2), 175–184 (2005).
[CrossRef]

Figueiredo, V.

E. Fortunato, R. Barros, P. Barquinha, V. Figueiredo, S.-H. K. Park, C.-S. Hwang, and R. Martins, “Transparent p-type SnOx thin film transistors produced by reactive rf magnetron sputtering followed by low temperature annealing,” Appl. Phys. Lett.97(5), 052105 (2010).
[CrossRef]

Flodström, S. A.

M. Qvarford, J. F. van Acker, J. N. Anderson, R. Nyholm, I. Lindau, G. Chiaia, E. Lundgren, S. Söderholm, U. O. Karlsson, S. A. Flodström, and L. Leonyuk, “Resonant valence-band and Cu 3p photoemission at the Cu L3 threshold of Bi2Sr2CuO6 and Bi2Sr2CaCu2O8,” Phys. Rev. B51(1), 410–416 (1995).

Fortunato, E.

E. Fortunato, R. Barros, P. Barquinha, V. Figueiredo, S.-H. K. Park, C.-S. Hwang, and R. Martins, “Transparent p-type SnOx thin film transistors produced by reactive rf magnetron sputtering followed by low temperature annealing,” Appl. Phys. Lett.97(5), 052105 (2010).
[CrossRef]

Frantz, J. A.

J. A. Frantz, J. S. Sanghera, V. Q. Nguyen, S. S. Bayya, S. B. Qadri, and I. D. Aggarwal, “Formation of a new phase of barium copper sulfur fluoride via sputtering,” Mater. Lett.62(10-11), 1582–1584 (2008).
[CrossRef]

J. A. Frantz, L. B. Shaw, J. S. Sanghera, and I. D. Aggarwal, “Waveguide amplifiers in sputtered films of Er3+-doped gallium lanthanum sulfide glass,” Opt. Express14(5), 1797–1803 (2006).
[CrossRef] [PubMed]

Gonze, X.

G. Hautier, A. Miglio, G. Ceder, G.-M. Rignanese, and X. Gonze, “Identification and design principles of low hole effective mass p-type transparent conducting oxides,” Nat Commun.4, 2292 (2013).
[CrossRef] [PubMed]

Grigorovici, R.

J. Tauc, R. Grigorovici, and A. Vancu, “Optical properties and electronic structure of amorphous germanium,” Phys. Status Solidi15(2), 627–637 (1966).
[CrossRef]

Hamada, N.

S. Inoue, K. Ueda, H. Hosono, and N. Hamada, “Electronic structure of the transparent p-type semiconductor (LaO)CuS,” Phys. Rev. B64(24), 245211 (2001).
[CrossRef]

Hautier, G.

G. Hautier, A. Miglio, G. Ceder, G.-M. Rignanese, and X. Gonze, “Identification and design principles of low hole effective mass p-type transparent conducting oxides,” Nat Commun.4, 2292 (2013).
[CrossRef] [PubMed]

Hersh, P. A.

J. Tate, P. F. Newhouse, R. Kykyneshi, P. A. Hersh, J. Kinney, D. H. McIntyre, and D. A. Keszler, “Chalcogen-based transparent conductors,” Thin Solid Films516(17), 5795–5799 (2008).
[CrossRef]

Hiramatsu, H.

H. Hiramatsu, K. Ueda, H. Ohta, M. Hirano, M. Kikuchi, H. Yanagi, T. Kamiya, and H. Hosono, “Heavy hole doping of epitaxial thin films of a wide gap p-type semiconductor, LaCuOSe, and analysis of the effective mass,” Appl. Phys. Lett.91(1), 012104 (2007).
[CrossRef]

Hirano, M.

H. Hiramatsu, K. Ueda, H. Ohta, M. Hirano, M. Kikuchi, H. Yanagi, T. Kamiya, and H. Hosono, “Heavy hole doping of epitaxial thin films of a wide gap p-type semiconductor, LaCuOSe, and analysis of the effective mass,” Appl. Phys. Lett.91(1), 012104 (2007).
[CrossRef]

H. Yanagi, J. Tate, S. Park, C.-H. Park, D. A. Keszler, M. Hirano, and H. Hosono, “Valence band structure of BaCuSF and BaCuSeF,” J. Appl. Phys.100(8), 083705 (2006).
[CrossRef]

Hirschfeld, T.

T. Hirschfeld and A. W. Mantz, “Elimination of thin film infrared channel spectra in Fourier transform infrared spectroscopy,” Infrared Spectrosc.30(5), 552–553 (1976).
[CrossRef]

Holloway, P. H.

R. R. Owings, G. J. Exarhos, C. F. Windisch, P. H. Holloway, and J. G. Wen, “Process enhanced polaron conductivity of infrared transparent nickel–cobalt oxide,” Thin Solid Films483(1–2), 175–184 (2005).
[CrossRef]

Hosono, H.

H. Hiramatsu, K. Ueda, H. Ohta, M. Hirano, M. Kikuchi, H. Yanagi, T. Kamiya, and H. Hosono, “Heavy hole doping of epitaxial thin films of a wide gap p-type semiconductor, LaCuOSe, and analysis of the effective mass,” Appl. Phys. Lett.91(1), 012104 (2007).
[CrossRef]

H. Yanagi, J. Tate, S. Park, C.-H. Park, D. A. Keszler, M. Hirano, and H. Hosono, “Valence band structure of BaCuSF and BaCuSeF,” J. Appl. Phys.100(8), 083705 (2006).
[CrossRef]

S. Inoue, K. Ueda, H. Hosono, and N. Hamada, “Electronic structure of the transparent p-type semiconductor (LaO)CuS,” Phys. Rev. B64(24), 245211 (2001).
[CrossRef]

H. Kawazoe, M. Yasukawa, H. Hyodo, M. Kurita, H. Yanagi, and H. Hosono, “P-type electrical conduction in transparent thin films of CuAlO2,” Nature389(6654), 939–942 (1997).
[CrossRef]

Huang, Y.

W. Zhu, Y. Huang, F. Wu, C. Dong, H. Chen, and Z. Zhao, “Synthesis and crystal structure of barium copper fluorochalcogenides: [BaCuFQ (Q=S,Se)],” Mater. Res. Bull.29(5), 505–508 (1994).
[CrossRef]

Hwang, C.-S.

E. Fortunato, R. Barros, P. Barquinha, V. Figueiredo, S.-H. K. Park, C.-S. Hwang, and R. Martins, “Transparent p-type SnOx thin film transistors produced by reactive rf magnetron sputtering followed by low temperature annealing,” Appl. Phys. Lett.97(5), 052105 (2010).
[CrossRef]

Hyodo, H.

H. Kawazoe, M. Yasukawa, H. Hyodo, M. Kurita, H. Yanagi, and H. Hosono, “P-type electrical conduction in transparent thin films of CuAlO2,” Nature389(6654), 939–942 (1997).
[CrossRef]

Inoue, S.

S. Inoue, K. Ueda, H. Hosono, and N. Hamada, “Electronic structure of the transparent p-type semiconductor (LaO)CuS,” Phys. Rev. B64(24), 245211 (2001).
[CrossRef]

Kafafi, Z. H.

A. J. Mäkinen, M. Uchida, and Z. H. Kafafi, “Electronic structure of a silole derivative-magnesium thin film interface,” J. Appl. Phys.95(5), 2832–2838 (2004).
[CrossRef]

Kamiya, T.

H. Hiramatsu, K. Ueda, H. Ohta, M. Hirano, M. Kikuchi, H. Yanagi, T. Kamiya, and H. Hosono, “Heavy hole doping of epitaxial thin films of a wide gap p-type semiconductor, LaCuOSe, and analysis of the effective mass,” Appl. Phys. Lett.91(1), 012104 (2007).
[CrossRef]

Karlsson, U. O.

M. Qvarford, J. F. van Acker, J. N. Anderson, R. Nyholm, I. Lindau, G. Chiaia, E. Lundgren, S. Söderholm, U. O. Karlsson, S. A. Flodström, and L. Leonyuk, “Resonant valence-band and Cu 3p photoemission at the Cu L3 threshold of Bi2Sr2CuO6 and Bi2Sr2CaCu2O8,” Phys. Rev. B51(1), 410–416 (1995).

Kawazoe, H.

H. Kawazoe, M. Yasukawa, H. Hyodo, M. Kurita, H. Yanagi, and H. Hosono, “P-type electrical conduction in transparent thin films of CuAlO2,” Nature389(6654), 939–942 (1997).
[CrossRef]

Keszler, D.

H. Yanagi, S. Park, A. D. Draeske, D. Keszler, and J. Tate, “P-type conductivity in transparent oxides and sulfide fluorides,” J. Solid State Chem.175(1), 34–38 (2003).
[CrossRef]

Keszler, D. A.

A. Zakutayev, D. H. McIntyre, G. Schneider, R. Kykyneshi, D. A. Keszler, C.-H. Park, and J. Tate, “Tunable properties of wide-band gap p-type BaCu(Ch1−xCh’x)F (Ch = S, Se, Te) thin-film solid solutions,” Thin Solid Films518(19), 5494–5500 (2010).
[CrossRef]

J. Tate, P. F. Newhouse, R. Kykyneshi, P. A. Hersh, J. Kinney, D. H. McIntyre, and D. A. Keszler, “Chalcogen-based transparent conductors,” Thin Solid Films516(17), 5795–5799 (2008).
[CrossRef]

H. Yanagi, J. Tate, S. Park, C.-H. Park, D. A. Keszler, M. Hirano, and H. Hosono, “Valence band structure of BaCuSF and BaCuSeF,” J. Appl. Phys.100(8), 083705 (2006).
[CrossRef]

Kikuchi, M.

H. Hiramatsu, K. Ueda, H. Ohta, M. Hirano, M. Kikuchi, H. Yanagi, T. Kamiya, and H. Hosono, “Heavy hole doping of epitaxial thin films of a wide gap p-type semiconductor, LaCuOSe, and analysis of the effective mass,” Appl. Phys. Lett.91(1), 012104 (2007).
[CrossRef]

Kinney, J.

J. Tate, P. F. Newhouse, R. Kykyneshi, P. A. Hersh, J. Kinney, D. H. McIntyre, and D. A. Keszler, “Chalcogen-based transparent conductors,” Thin Solid Films516(17), 5795–5799 (2008).
[CrossRef]

Klein, A.

A. Klein, “Transparent conducting oxides: Electronic structure-property relationship from photoelectron spectroscopy with in situ sample preparation,” J. Am. Ceram. Soc.96, 331–345 (2013).

Kurita, M.

H. Kawazoe, M. Yasukawa, H. Hyodo, M. Kurita, H. Yanagi, and H. Hosono, “P-type electrical conduction in transparent thin films of CuAlO2,” Nature389(6654), 939–942 (1997).
[CrossRef]

Kykyneshi, R.

A. Zakutayev, D. H. McIntyre, G. Schneider, R. Kykyneshi, D. A. Keszler, C.-H. Park, and J. Tate, “Tunable properties of wide-band gap p-type BaCu(Ch1−xCh’x)F (Ch = S, Se, Te) thin-film solid solutions,” Thin Solid Films518(19), 5494–5500 (2010).
[CrossRef]

J. Tate, P. F. Newhouse, R. Kykyneshi, P. A. Hersh, J. Kinney, D. H. McIntyre, and D. A. Keszler, “Chalcogen-based transparent conductors,” Thin Solid Films516(17), 5795–5799 (2008).
[CrossRef]

Leonyuk, L.

M. Qvarford, J. F. van Acker, J. N. Anderson, R. Nyholm, I. Lindau, G. Chiaia, E. Lundgren, S. Söderholm, U. O. Karlsson, S. A. Flodström, and L. Leonyuk, “Resonant valence-band and Cu 3p photoemission at the Cu L3 threshold of Bi2Sr2CuO6 and Bi2Sr2CaCu2O8,” Phys. Rev. B51(1), 410–416 (1995).

Lindau, I.

M. Qvarford, J. F. van Acker, J. N. Anderson, R. Nyholm, I. Lindau, G. Chiaia, E. Lundgren, S. Söderholm, U. O. Karlsson, S. A. Flodström, and L. Leonyuk, “Resonant valence-band and Cu 3p photoemission at the Cu L3 threshold of Bi2Sr2CuO6 and Bi2Sr2CaCu2O8,” Phys. Rev. B51(1), 410–416 (1995).

Lundgren, E.

M. Qvarford, J. F. van Acker, J. N. Anderson, R. Nyholm, I. Lindau, G. Chiaia, E. Lundgren, S. Söderholm, U. O. Karlsson, S. A. Flodström, and L. Leonyuk, “Resonant valence-band and Cu 3p photoemission at the Cu L3 threshold of Bi2Sr2CuO6 and Bi2Sr2CaCu2O8,” Phys. Rev. B51(1), 410–416 (1995).

Mäkinen, A. J.

A. J. Mäkinen, M. Uchida, and Z. H. Kafafi, “Electronic structure of a silole derivative-magnesium thin film interface,” J. Appl. Phys.95(5), 2832–2838 (2004).
[CrossRef]

Mantz, A. W.

T. Hirschfeld and A. W. Mantz, “Elimination of thin film infrared channel spectra in Fourier transform infrared spectroscopy,” Infrared Spectrosc.30(5), 552–553 (1976).
[CrossRef]

Martins, R.

E. Fortunato, R. Barros, P. Barquinha, V. Figueiredo, S.-H. K. Park, C.-S. Hwang, and R. Martins, “Transparent p-type SnOx thin film transistors produced by reactive rf magnetron sputtering followed by low temperature annealing,” Appl. Phys. Lett.97(5), 052105 (2010).
[CrossRef]

McIntyre, D. H.

A. Zakutayev, D. H. McIntyre, G. Schneider, R. Kykyneshi, D. A. Keszler, C.-H. Park, and J. Tate, “Tunable properties of wide-band gap p-type BaCu(Ch1−xCh’x)F (Ch = S, Se, Te) thin-film solid solutions,” Thin Solid Films518(19), 5494–5500 (2010).
[CrossRef]

J. Tate, P. F. Newhouse, R. Kykyneshi, P. A. Hersh, J. Kinney, D. H. McIntyre, and D. A. Keszler, “Chalcogen-based transparent conductors,” Thin Solid Films516(17), 5795–5799 (2008).
[CrossRef]

Miglio, A.

G. Hautier, A. Miglio, G. Ceder, G.-M. Rignanese, and X. Gonze, “Identification and design principles of low hole effective mass p-type transparent conducting oxides,” Nat Commun.4, 2292 (2013).
[CrossRef] [PubMed]

Newhouse, P. F.

J. Tate, P. F. Newhouse, R. Kykyneshi, P. A. Hersh, J. Kinney, D. H. McIntyre, and D. A. Keszler, “Chalcogen-based transparent conductors,” Thin Solid Films516(17), 5795–5799 (2008).
[CrossRef]

Nguyen, V. Q.

J. A. Frantz, J. S. Sanghera, V. Q. Nguyen, S. S. Bayya, S. B. Qadri, and I. D. Aggarwal, “Formation of a new phase of barium copper sulfur fluoride via sputtering,” Mater. Lett.62(10-11), 1582–1584 (2008).
[CrossRef]

Nyholm, R.

M. Qvarford, J. F. van Acker, J. N. Anderson, R. Nyholm, I. Lindau, G. Chiaia, E. Lundgren, S. Söderholm, U. O. Karlsson, S. A. Flodström, and L. Leonyuk, “Resonant valence-band and Cu 3p photoemission at the Cu L3 threshold of Bi2Sr2CuO6 and Bi2Sr2CaCu2O8,” Phys. Rev. B51(1), 410–416 (1995).

Ohta, H.

H. Hiramatsu, K. Ueda, H. Ohta, M. Hirano, M. Kikuchi, H. Yanagi, T. Kamiya, and H. Hosono, “Heavy hole doping of epitaxial thin films of a wide gap p-type semiconductor, LaCuOSe, and analysis of the effective mass,” Appl. Phys. Lett.91(1), 012104 (2007).
[CrossRef]

Owings, R. R.

R. R. Owings, G. J. Exarhos, C. F. Windisch, P. H. Holloway, and J. G. Wen, “Process enhanced polaron conductivity of infrared transparent nickel–cobalt oxide,” Thin Solid Films483(1–2), 175–184 (2005).
[CrossRef]

Park, C.-H.

A. Zakutayev, D. H. McIntyre, G. Schneider, R. Kykyneshi, D. A. Keszler, C.-H. Park, and J. Tate, “Tunable properties of wide-band gap p-type BaCu(Ch1−xCh’x)F (Ch = S, Se, Te) thin-film solid solutions,” Thin Solid Films518(19), 5494–5500 (2010).
[CrossRef]

H. Yanagi, J. Tate, S. Park, C.-H. Park, D. A. Keszler, M. Hirano, and H. Hosono, “Valence band structure of BaCuSF and BaCuSeF,” J. Appl. Phys.100(8), 083705 (2006).
[CrossRef]

Park, S.

H. Yanagi, J. Tate, S. Park, C.-H. Park, D. A. Keszler, M. Hirano, and H. Hosono, “Valence band structure of BaCuSF and BaCuSeF,” J. Appl. Phys.100(8), 083705 (2006).
[CrossRef]

H. Yanagi, S. Park, A. D. Draeske, D. Keszler, and J. Tate, “P-type conductivity in transparent oxides and sulfide fluorides,” J. Solid State Chem.175(1), 34–38 (2003).
[CrossRef]

Park, S.-H. K.

E. Fortunato, R. Barros, P. Barquinha, V. Figueiredo, S.-H. K. Park, C.-S. Hwang, and R. Martins, “Transparent p-type SnOx thin film transistors produced by reactive rf magnetron sputtering followed by low temperature annealing,” Appl. Phys. Lett.97(5), 052105 (2010).
[CrossRef]

Qadri, S. B.

J. A. Frantz, J. S. Sanghera, V. Q. Nguyen, S. S. Bayya, S. B. Qadri, and I. D. Aggarwal, “Formation of a new phase of barium copper sulfur fluoride via sputtering,” Mater. Lett.62(10-11), 1582–1584 (2008).
[CrossRef]

Qvarford, M.

M. Qvarford, J. F. van Acker, J. N. Anderson, R. Nyholm, I. Lindau, G. Chiaia, E. Lundgren, S. Söderholm, U. O. Karlsson, S. A. Flodström, and L. Leonyuk, “Resonant valence-band and Cu 3p photoemission at the Cu L3 threshold of Bi2Sr2CuO6 and Bi2Sr2CaCu2O8,” Phys. Rev. B51(1), 410–416 (1995).

Rignanese, G.-M.

G. Hautier, A. Miglio, G. Ceder, G.-M. Rignanese, and X. Gonze, “Identification and design principles of low hole effective mass p-type transparent conducting oxides,” Nat Commun.4, 2292 (2013).
[CrossRef] [PubMed]

Sanghera, J. S.

J. A. Frantz, J. S. Sanghera, V. Q. Nguyen, S. S. Bayya, S. B. Qadri, and I. D. Aggarwal, “Formation of a new phase of barium copper sulfur fluoride via sputtering,” Mater. Lett.62(10-11), 1582–1584 (2008).
[CrossRef]

J. A. Frantz, L. B. Shaw, J. S. Sanghera, and I. D. Aggarwal, “Waveguide amplifiers in sputtered films of Er3+-doped gallium lanthanum sulfide glass,” Opt. Express14(5), 1797–1803 (2006).
[CrossRef] [PubMed]

Schneider, G.

A. Zakutayev, D. H. McIntyre, G. Schneider, R. Kykyneshi, D. A. Keszler, C.-H. Park, and J. Tate, “Tunable properties of wide-band gap p-type BaCu(Ch1−xCh’x)F (Ch = S, Se, Te) thin-film solid solutions,” Thin Solid Films518(19), 5494–5500 (2010).
[CrossRef]

Shaw, L. B.

Söderholm, S.

M. Qvarford, J. F. van Acker, J. N. Anderson, R. Nyholm, I. Lindau, G. Chiaia, E. Lundgren, S. Söderholm, U. O. Karlsson, S. A. Flodström, and L. Leonyuk, “Resonant valence-band and Cu 3p photoemission at the Cu L3 threshold of Bi2Sr2CuO6 and Bi2Sr2CaCu2O8,” Phys. Rev. B51(1), 410–416 (1995).

Tate, J.

A. Zakutayev, D. H. McIntyre, G. Schneider, R. Kykyneshi, D. A. Keszler, C.-H. Park, and J. Tate, “Tunable properties of wide-band gap p-type BaCu(Ch1−xCh’x)F (Ch = S, Se, Te) thin-film solid solutions,” Thin Solid Films518(19), 5494–5500 (2010).
[CrossRef]

J. Tate, P. F. Newhouse, R. Kykyneshi, P. A. Hersh, J. Kinney, D. H. McIntyre, and D. A. Keszler, “Chalcogen-based transparent conductors,” Thin Solid Films516(17), 5795–5799 (2008).
[CrossRef]

H. Yanagi, J. Tate, S. Park, C.-H. Park, D. A. Keszler, M. Hirano, and H. Hosono, “Valence band structure of BaCuSF and BaCuSeF,” J. Appl. Phys.100(8), 083705 (2006).
[CrossRef]

H. Yanagi, S. Park, A. D. Draeske, D. Keszler, and J. Tate, “P-type conductivity in transparent oxides and sulfide fluorides,” J. Solid State Chem.175(1), 34–38 (2003).
[CrossRef]

Tauc, J.

J. Tauc, R. Grigorovici, and A. Vancu, “Optical properties and electronic structure of amorphous germanium,” Phys. Status Solidi15(2), 627–637 (1966).
[CrossRef]

Uchida, M.

A. J. Mäkinen, M. Uchida, and Z. H. Kafafi, “Electronic structure of a silole derivative-magnesium thin film interface,” J. Appl. Phys.95(5), 2832–2838 (2004).
[CrossRef]

Ueda, K.

H. Hiramatsu, K. Ueda, H. Ohta, M. Hirano, M. Kikuchi, H. Yanagi, T. Kamiya, and H. Hosono, “Heavy hole doping of epitaxial thin films of a wide gap p-type semiconductor, LaCuOSe, and analysis of the effective mass,” Appl. Phys. Lett.91(1), 012104 (2007).
[CrossRef]

S. Inoue, K. Ueda, H. Hosono, and N. Hamada, “Electronic structure of the transparent p-type semiconductor (LaO)CuS,” Phys. Rev. B64(24), 245211 (2001).
[CrossRef]

van Acker, J. F.

M. Qvarford, J. F. van Acker, J. N. Anderson, R. Nyholm, I. Lindau, G. Chiaia, E. Lundgren, S. Söderholm, U. O. Karlsson, S. A. Flodström, and L. Leonyuk, “Resonant valence-band and Cu 3p photoemission at the Cu L3 threshold of Bi2Sr2CuO6 and Bi2Sr2CaCu2O8,” Phys. Rev. B51(1), 410–416 (1995).

Vancu, A.

J. Tauc, R. Grigorovici, and A. Vancu, “Optical properties and electronic structure of amorphous germanium,” Phys. Status Solidi15(2), 627–637 (1966).
[CrossRef]

Wen, J. G.

R. R. Owings, G. J. Exarhos, C. F. Windisch, P. H. Holloway, and J. G. Wen, “Process enhanced polaron conductivity of infrared transparent nickel–cobalt oxide,” Thin Solid Films483(1–2), 175–184 (2005).
[CrossRef]

Windisch, C. F.

R. R. Owings, G. J. Exarhos, C. F. Windisch, P. H. Holloway, and J. G. Wen, “Process enhanced polaron conductivity of infrared transparent nickel–cobalt oxide,” Thin Solid Films483(1–2), 175–184 (2005).
[CrossRef]

Wu, F.

W. Zhu, Y. Huang, F. Wu, C. Dong, H. Chen, and Z. Zhao, “Synthesis and crystal structure of barium copper fluorochalcogenides: [BaCuFQ (Q=S,Se)],” Mater. Res. Bull.29(5), 505–508 (1994).
[CrossRef]

Yanagi, H.

H. Hiramatsu, K. Ueda, H. Ohta, M. Hirano, M. Kikuchi, H. Yanagi, T. Kamiya, and H. Hosono, “Heavy hole doping of epitaxial thin films of a wide gap p-type semiconductor, LaCuOSe, and analysis of the effective mass,” Appl. Phys. Lett.91(1), 012104 (2007).
[CrossRef]

H. Yanagi, J. Tate, S. Park, C.-H. Park, D. A. Keszler, M. Hirano, and H. Hosono, “Valence band structure of BaCuSF and BaCuSeF,” J. Appl. Phys.100(8), 083705 (2006).
[CrossRef]

H. Yanagi, S. Park, A. D. Draeske, D. Keszler, and J. Tate, “P-type conductivity in transparent oxides and sulfide fluorides,” J. Solid State Chem.175(1), 34–38 (2003).
[CrossRef]

H. Kawazoe, M. Yasukawa, H. Hyodo, M. Kurita, H. Yanagi, and H. Hosono, “P-type electrical conduction in transparent thin films of CuAlO2,” Nature389(6654), 939–942 (1997).
[CrossRef]

Yasukawa, M.

H. Kawazoe, M. Yasukawa, H. Hyodo, M. Kurita, H. Yanagi, and H. Hosono, “P-type electrical conduction in transparent thin films of CuAlO2,” Nature389(6654), 939–942 (1997).
[CrossRef]

Zakutayev, A.

A. Zakutayev, D. H. McIntyre, G. Schneider, R. Kykyneshi, D. A. Keszler, C.-H. Park, and J. Tate, “Tunable properties of wide-band gap p-type BaCu(Ch1−xCh’x)F (Ch = S, Se, Te) thin-film solid solutions,” Thin Solid Films518(19), 5494–5500 (2010).
[CrossRef]

Zhao, Z.

W. Zhu, Y. Huang, F. Wu, C. Dong, H. Chen, and Z. Zhao, “Synthesis and crystal structure of barium copper fluorochalcogenides: [BaCuFQ (Q=S,Se)],” Mater. Res. Bull.29(5), 505–508 (1994).
[CrossRef]

Zhu, W.

W. Zhu, Y. Huang, F. Wu, C. Dong, H. Chen, and Z. Zhao, “Synthesis and crystal structure of barium copper fluorochalcogenides: [BaCuFQ (Q=S,Se)],” Mater. Res. Bull.29(5), 505–508 (1994).
[CrossRef]

Appl. Phys. Lett.

H. Hiramatsu, K. Ueda, H. Ohta, M. Hirano, M. Kikuchi, H. Yanagi, T. Kamiya, and H. Hosono, “Heavy hole doping of epitaxial thin films of a wide gap p-type semiconductor, LaCuOSe, and analysis of the effective mass,” Appl. Phys. Lett.91(1), 012104 (2007).
[CrossRef]

E. Fortunato, R. Barros, P. Barquinha, V. Figueiredo, S.-H. K. Park, C.-S. Hwang, and R. Martins, “Transparent p-type SnOx thin film transistors produced by reactive rf magnetron sputtering followed by low temperature annealing,” Appl. Phys. Lett.97(5), 052105 (2010).
[CrossRef]

Infrared Spectrosc.

T. Hirschfeld and A. W. Mantz, “Elimination of thin film infrared channel spectra in Fourier transform infrared spectroscopy,” Infrared Spectrosc.30(5), 552–553 (1976).
[CrossRef]

J. Am. Ceram. Soc.

A. Klein, “Transparent conducting oxides: Electronic structure-property relationship from photoelectron spectroscopy with in situ sample preparation,” J. Am. Ceram. Soc.96, 331–345 (2013).

J. Appl. Phys.

H. Yanagi, J. Tate, S. Park, C.-H. Park, D. A. Keszler, M. Hirano, and H. Hosono, “Valence band structure of BaCuSF and BaCuSeF,” J. Appl. Phys.100(8), 083705 (2006).
[CrossRef]

A. J. Mäkinen, M. Uchida, and Z. H. Kafafi, “Electronic structure of a silole derivative-magnesium thin film interface,” J. Appl. Phys.95(5), 2832–2838 (2004).
[CrossRef]

J. Solid State Chem.

H. Yanagi, S. Park, A. D. Draeske, D. Keszler, and J. Tate, “P-type conductivity in transparent oxides and sulfide fluorides,” J. Solid State Chem.175(1), 34–38 (2003).
[CrossRef]

Mater. Lett.

J. A. Frantz, J. S. Sanghera, V. Q. Nguyen, S. S. Bayya, S. B. Qadri, and I. D. Aggarwal, “Formation of a new phase of barium copper sulfur fluoride via sputtering,” Mater. Lett.62(10-11), 1582–1584 (2008).
[CrossRef]

Mater. Res. Bull.

W. Zhu, Y. Huang, F. Wu, C. Dong, H. Chen, and Z. Zhao, “Synthesis and crystal structure of barium copper fluorochalcogenides: [BaCuFQ (Q=S,Se)],” Mater. Res. Bull.29(5), 505–508 (1994).
[CrossRef]

Nat Commun.

G. Hautier, A. Miglio, G. Ceder, G.-M. Rignanese, and X. Gonze, “Identification and design principles of low hole effective mass p-type transparent conducting oxides,” Nat Commun.4, 2292 (2013).
[CrossRef] [PubMed]

Nature

H. Kawazoe, M. Yasukawa, H. Hyodo, M. Kurita, H. Yanagi, and H. Hosono, “P-type electrical conduction in transparent thin films of CuAlO2,” Nature389(6654), 939–942 (1997).
[CrossRef]

Opt. Express

Phys. Rev. B

M. Qvarford, J. F. van Acker, J. N. Anderson, R. Nyholm, I. Lindau, G. Chiaia, E. Lundgren, S. Söderholm, U. O. Karlsson, S. A. Flodström, and L. Leonyuk, “Resonant valence-band and Cu 3p photoemission at the Cu L3 threshold of Bi2Sr2CuO6 and Bi2Sr2CaCu2O8,” Phys. Rev. B51(1), 410–416 (1995).

S. Inoue, K. Ueda, H. Hosono, and N. Hamada, “Electronic structure of the transparent p-type semiconductor (LaO)CuS,” Phys. Rev. B64(24), 245211 (2001).
[CrossRef]

Phys. Status Solidi

J. Tauc, R. Grigorovici, and A. Vancu, “Optical properties and electronic structure of amorphous germanium,” Phys. Status Solidi15(2), 627–637 (1966).
[CrossRef]

Thin Solid Films

A. Zakutayev, D. H. McIntyre, G. Schneider, R. Kykyneshi, D. A. Keszler, C.-H. Park, and J. Tate, “Tunable properties of wide-band gap p-type BaCu(Ch1−xCh’x)F (Ch = S, Se, Te) thin-film solid solutions,” Thin Solid Films518(19), 5494–5500 (2010).
[CrossRef]

J. Tate, P. F. Newhouse, R. Kykyneshi, P. A. Hersh, J. Kinney, D. H. McIntyre, and D. A. Keszler, “Chalcogen-based transparent conductors,” Thin Solid Films516(17), 5795–5799 (2008).
[CrossRef]

R. R. Owings, G. J. Exarhos, C. F. Windisch, P. H. Holloway, and J. G. Wen, “Process enhanced polaron conductivity of infrared transparent nickel–cobalt oxide,” Thin Solid Films483(1–2), 175–184 (2005).
[CrossRef]

Other

J. A. Frantz, J. S. Sanghera, S. B. Qadri, and I. D. Aggarwal, “Record conductivity for p-type transparent conductors in polycrystalline thin films of a sulfide-fluoride,” in Materials Research Society Symposium Proceedings (Materials Research Society, 2008) pp. 108–113.
[CrossRef]

ASTM Standard F76–86, “Standard test methods for measuring resistivity and Hall coefficient and determining Hall mobility in single crystal semiconductors” (ASTM International, 2002).

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Figures (8)

Fig. 1
Fig. 1

Images of (a) a 3” diameter BaCuSF sputtering target, (b) Hall bars in which the central bar is 2 mm wide, and (c) films of as-deposited (left) and H2O-treated BaCuSF on 2” diameter fused silica substrates.

Fig. 2
Fig. 2

XRD plot for as-deposited and H2O-treated 150 nm thick BaCuSF films on 250 μm thick fused silica substrates. Peaks are assigned based on an FCC lattice in space group Fm3m.

Fig. 3
Fig. 3

Transmittance of as-deposited and H2O-treated 150 nm thick BaCuSF films on 250 μm thick fused silica substrates. The transmittance of the blank silica substrate is also shown. The data for wavelengths <2 μm, to the left of the dotted line, was obtained with a spectrophotometer, and the data for wavelengths >2 μm was obtained with an FTIR system. The top inset shows the absorption coefficient for each film. The bottom inset shows mid-IR transmittance of a 150 nm thick BaCuSF film on a 1 mm thick ZnS substrate.

Fig. 4
Fig. 4

Plot of [αhν]1/2 vs. photon energy for both as-deposited and H2O-treated films.

Fig. 5
Fig. 5

Measurements of conductivity obtained with Hall bar structures for (a) as-deposited and (b) H2O treated BaCuSF films. The insets show Arrhenius plots of the same data.

Fig. 6
Fig. 6

Measurements of carrier density and hole mobility derived from PPMS measurements of Hall coefficient and conductivity.

Fig. 7
Fig. 7

XPS measurement of the core line spectra for (a) Ba 4d and Cu 3p and (b) S 2p levels. Depending on the line shape, the spectra were each fitted to one or two Gaussian functions after subtracting a Shirley-type background function from the raw data. The line positions were calibrated with respect to the Ag 4F5/2 core line. The dotted gray lines show the individual Gaussian fits, and the solid red lines shows composite fits. A UPS measurement of the valence levels is shown in (c).

Fig. 8
Fig. 8

Atmospheric effects on an as-deposited film. Comparison of normalized peak transmittance for an uncoated sample and one coated with 10 nm of SiOx as a function of time.

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