Controlling compositional homogeneity and crystalline orientation in Bi 0.8 Sb 0.2 thermoelectric thin films [Control of composition and crystallinity in Bi0.8Sb0.2 thermoelectric thin films].

Rochford, C.; Medlin, D. L.; Erickson, K. J.; Siegal, M. P.

doi:10.1063/1.4937894

Title: Controlling compositional homogeneity and crystalline orientation in Bi _0.8 Sb _0.2 thermoelectric thin films [Control of composition and crystallinity in Bi_0.8Sb_0.2 thermoelectric thin films].

Abstract

Controlling alloy composition, crystalline quality, and crystal orientation is necessary to achieve high thermoelectric performance in Bi_1-xSb_x thin films. These microstructural attributes are demonstrated in this letter via co-sputter deposition of Bi and Sb metals on Si/SiO₂ substrates followed by ex-situ post anneals ranging from 200 – 300 °C in forming gas with rapid cooling to achieve orientation along the trigonal axis. We show with cross-sectional transmission electron microscopy and energy-dispersive X-ray spectrometry that 50 – 95% of the Sb segregates at the surface upon exposure to air during transfer. This then forms a nanocrystalline Sb₂O₃ layer upon annealing, leaving the bulk of the film primarily Bi metal which is a poor thermoelectric material. We demonstrate a SiN capping technique to eliminate Sb segregation and preserve a uniform composition throughout the thickness of the film. Given that the Bi_1-xSb_x solid solution melting point depends on the Sb content, the SiN cap allows one to carefully approach but not exceed the melting point during annealing. This leads to the strong orientation along the trigonal axis and high crystalline quality desired for thermoelectric applications.

Authors:

^[1]; Medlin, D. L. ^[2]; Erickson, K. J. ^[2]; Siegal, M. P. ^[1]

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sandia National Lab. (SNL-CA), Livermore, CA (United States)

Publication Date:: Tue Dec 01 00:00:00 EST 2015

Research Org.:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Sandia National Lab. (SNL-CA), Livermore, CA (United States)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:: 1339268

Report Number(s):: SAND-2015-5236J
Journal ID: ISSN 2166-532X; 594458

Grant/Contract Number:: AC04-94AL85000

Resource Type:: Accepted Manuscript

Journal Name:: APL Materials

Additional Journal Information:: Journal Volume: 3; Journal Issue: 12; Journal ID: ISSN 2166-532X

Publisher:: American Institute of Physics (AIP)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Rochford, C., Medlin, D. L., Erickson, K. J., and Siegal, M. P. Controlling compositional homogeneity and crystalline orientation in Bi 0.8 Sb 0.2 thermoelectric thin films [Control of composition and crystallinity in Bi0.8Sb0.2 thermoelectric thin films]..  United States: N. p., 2015. 
Web.  doi:10.1063/1.4937894.

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                    Rochford, C., Medlin, D. L., Erickson, K. J., & Siegal, M. P. Controlling compositional homogeneity and crystalline orientation in Bi 0.8 Sb 0.2 thermoelectric thin films [Control of composition and crystallinity in Bi0.8Sb0.2 thermoelectric thin films]..  United States.  https://doi.org/10.1063/1.4937894

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                    Rochford, C., Medlin, D. L., Erickson, K. J., and Siegal, M. P. Tue .  
"Controlling compositional homogeneity and crystalline orientation in Bi 0.8 Sb 0.2 thermoelectric thin films [Control of composition and crystallinity in Bi0.8Sb0.2 thermoelectric thin films].".  United States.  https://doi.org/10.1063/1.4937894.  https://www.osti.gov/servlets/purl/1339268.

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@article{osti_1339268,

  title        = {Controlling compositional homogeneity and crystalline orientation in Bi 0.8 Sb 0.2 thermoelectric thin films [Control of composition and crystallinity in Bi0.8Sb0.2 thermoelectric thin films].},

  author       = {Rochford, C. and Medlin, D. L. and Erickson, K. J. and Siegal, M. P.},

  abstractNote = {Controlling alloy composition, crystalline quality, and crystal orientation is necessary to achieve high thermoelectric performance in Bi1-xSbx thin films. These microstructural attributes are demonstrated in this letter via co-sputter deposition of Bi and Sb metals on Si/SiO2 substrates followed by ex-situ post anneals ranging from 200 – 300 °C in forming gas with rapid cooling to achieve orientation along the trigonal axis. We show with cross-sectional transmission electron microscopy and energy-dispersive X-ray spectrometry that 50 – 95% of the Sb segregates at the surface upon exposure to air during transfer. This then forms a nanocrystalline Sb2O3 layer upon annealing, leaving the bulk of the film primarily Bi metal which is a poor thermoelectric material. We demonstrate a SiN capping technique to eliminate Sb segregation and preserve a uniform composition throughout the thickness of the film. Given that the Bi1-xSbx solid solution melting point depends on the Sb content, the SiN cap allows one to carefully approach but not exceed the melting point during annealing. This leads to the strong orientation along the trigonal axis and high crystalline quality desired for thermoelectric applications.},

  doi          = {10.1063/1.4937894},

  journal      = {APL Materials},

  number       = 12,

  volume       = 3,

  place        = {United States},

  year         = {Tue Dec 01 00:00:00 EST 2015},

  month        = {Tue Dec 01 00:00:00 EST 2015}

}

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Works referencing / citing this record:

Correlating thermoelectric properties with microstructure in Bi _0.8 Sb _0.2 thin films
journal, April 2017

Siegal, M. P.; Lima-Sharma, A. L.; Sharma, P. A.
Applied Physics Letters, Vol. 110, Issue 14
DOI: 10.1063/1.4979785

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Similar Records

Title: Controlling compositional homogeneity and crystalline orientation in Bi 0.8 Sb 0.2 thermoelectric thin films [Control of composition and crystallinity in Bi0.8Sb0.2 thermoelectric thin films].

Abstract

Citation Formats

Transport properties of Bi-RICH Bi-Sb alloys journal, January 1996

The Semiconductor–Semimetal Transition in Bi1−xSbx Alloys withx ≧ 0.22 journal, July 1978

Temperature Dependence of the Electrical Properties of Bismuth-Antimony Alloys journal, June 1959

Thermoelectric Properties of Bismuth‐Antimony Alloys journal, March 1962

Molecular beam epitaxial growth and structural properties of Bi1−xSbx alloy thin films on CdTe(111) substrates journal, January 1999

Thermoelectric transport properties of n -doped and p -doped Bi0.91Sb0.09 alloy thin films journal, April 1999

Transport properties of Bi 1 − x Sb x alloy thin films grown on CdTe ( 111 ) B journal, April 1999

Anisotropic Seebeck and magneto-Seebeck coefficients of Bi and Bi0.92Sb0.08 alloy thin films journal, July 2000

Size- and temperature-dependent thermoelectric and electrical properties of Bi88Sb12 alloy thin films journal, February 2005

Study of structural-, compositional-, and thickness-dependent thermoelectric and electrical properties of Bi93Sb7 alloy thin films journal, July 2005

Anomalously high thermoelectric figure of merit in Bi1−xSbx nanowires by carrier pocket alignment journal, July 2001

Lattice- vs. grain-boundary-controlled interdiffusion in BiSb bilayer films journal, November 1996

Growth of Bi–Sb alloy thin films and their characterization by TEM, PIXE and RBS journal, April 2005

Structure and electrical transport properties of bismuth thin films prepared by RF magnetron sputtering journal, March 2006

Recrystallized Arrays of Bismuth Nanowires with Trigonal Orientation journal, March 2014

Refinement of the crystal structure of cubic antimony trioxide, Sb 2 O 3 journal, August 1975

Using galvanostatic electroforming of Bi 1– x Sb x nanowires to control composition, crystallinity, and orientation journal, December 2014

Thermodynamic evaluation of the system bismuth-antimony journal, April 1992

Correlating thermoelectric properties with microstructure in Bi 0.8 Sb 0.2 thin films journal, April 2017

Title: Controlling compositional homogeneity and crystalline orientation in Bi _0.8 Sb _0.2 thermoelectric thin films [Control of composition and crystallinity in Bi_0.8Sb_0.2 thermoelectric thin films].

Transport properties of Bi-RICH Bi-Sb alloys
journal, January 1996

The Semiconductor–Semimetal Transition in Bi1−xSbx Alloys withx ≧ 0.22
journal, July 1978

Temperature Dependence of the Electrical Properties of Bismuth-Antimony Alloys
journal, June 1959

Thermoelectric Properties of Bismuth‐Antimony Alloys
journal, March 1962

Molecular beam epitaxial growth and structural properties of Bi1−xSbx alloy thin films on CdTe(111) substrates
journal, January 1999

Thermoelectric transport properties of n -doped and p -doped Bi0.91Sb0.09 alloy thin films
journal, April 1999

Transport properties of ${Bi}_{1 - x} {Sb}_{x}$ alloy thin films grown on $CdTe (111) B$
journal, April 1999

Anisotropic Seebeck and magneto-Seebeck coefficients of Bi and Bi0.92Sb0.08 alloy thin films
journal, July 2000

Size- and temperature-dependent thermoelectric and electrical properties of Bi88Sb12 alloy thin films
journal, February 2005

Study of structural-, compositional-, and thickness-dependent thermoelectric and electrical properties of Bi93Sb7 alloy thin films
journal, July 2005

Anomalously high thermoelectric figure of merit in Bi1−xSbx nanowires by carrier pocket alignment
journal, July 2001

Lattice- vs. grain-boundary-controlled interdiffusion in BiSb bilayer films
journal, November 1996

Growth of Bi–Sb alloy thin films and their characterization by TEM, PIXE and RBS
journal, April 2005

Structure and electrical transport properties of bismuth thin films prepared by RF magnetron sputtering
journal, March 2006

Recrystallized Arrays of Bismuth Nanowires with Trigonal Orientation
journal, March 2014

Refinement of the crystal structure of cubic antimony trioxide, Sb ₂ O ₃
journal, August 1975

Using galvanostatic electroforming of Bi _{1– x} Sb _x nanowires to control composition, crystallinity, and orientation
journal, December 2014

Thermodynamic evaluation of the system bismuth-antimony
journal, April 1992

Correlating thermoelectric properties with microstructure in Bi _0.8 Sb _0.2 thin films
journal, April 2017