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

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].

Journal Article · Tue Dec 01 00:00:00 EST 2015 · APL Materials

DOI:https://doi.org/10.1063/1.4937894· OSTI ID:1339268

^[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)

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.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States); Sandia National Laboratories, Livermore, CA

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC04-94AL85000

OSTI ID:: 1339268

Report Number(s):: SAND--2015-5236J; 594458

Journal Information:: APL Materials, Journal Name: APL Materials Journal Issue: 12 Vol. 3; ISSN 2166-532X

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

References (18)

The Semiconductor–Semimetal Transition in Bi1−xSbx Alloys withx ≧ 0.22 Kraak, W.; Oelgart, G.; Schneider, G. Physica Status Solidi (b), Vol. 88, Issue 1 https://doi.org/10.1002/pssb.2220880111	journal	July 1978
Transport properties of Bi-RICH Bi-Sb alloys Lenoir, B.; Cassart, M.; Michenaud, J. -P. Journal of Physics and Chemistry of Solids, Vol. 57, Issue 1 https://doi.org/10.1016/0022-3697(95)00148-4	journal	January 1996
Thermodynamic evaluation of the system bismuth-antimony Feutelais, Y.; Morgant, G.; Didry, J. R. Calphad, Vol. 16, Issue 2 https://doi.org/10.1016/0364-5916(92)90001-E	journal	April 1992
Lattice- vs. grain-boundary-controlled interdiffusion in BiSb bilayer films Missana, T.; Afonso, C. N.; Petford-Long, A. K. Thin Solid Films, Vol. 288, Issue 1-2 https://doi.org/10.1016/S0040-6090(96)08810-4	journal	November 1996
Structure and electrical transport properties of bismuth thin films prepared by RF magnetron sputtering Kim, Dong-Ho; Lee, Sung-Hun; Kim, Jong-Kuk Applied Surface Science, Vol. 252, Issue 10 https://doi.org/10.1016/j.apsusc.2005.05.046	journal	March 2006
Growth of Bi–Sb alloy thin films and their characterization by TEM, PIXE and RBS Mallik, Ramesh Chandra; Damodara Das, V. Solid State Communications, Vol. 134, Issue 3 https://doi.org/10.1016/j.ssc.2004.11.049	journal	April 2005
Size- and temperature-dependent thermoelectric and electrical properties of Bi88Sb12 alloy thin films Mallik, Ramesh Chandra; Das, V. Damodara Vacuum, Vol. 77, Issue 3 https://doi.org/10.1016/j.vacuum.2004.10.004	journal	February 2005
Recrystallized Arrays of Bismuth Nanowires with Trigonal Orientation Limmer, Steven J.; Yelton, W. Graham; Erickson, Kristopher J. Nano Letters, Vol. 14, Issue 4 https://doi.org/10.1021/nl404752p	journal	March 2014
Anomalously high thermoelectric figure of merit in Bi1−xSbx nanowires by carrier pocket alignment Rabina, Oded; Lin, Yu-Ming; Dresselhaus, Mildred S. Applied Physics Letters, Vol. 79, Issue 1 https://doi.org/10.1063/1.1379365	journal	July 2001
Thermoelectric Properties of Bismuth‐Antimony Alloys Smith, G. E.; Wolfe, R. Journal of Applied Physics, Vol. 33, Issue 3 https://doi.org/10.1063/1.1777178	journal	March 1962
Study of structural-, compositional-, and thickness-dependent thermoelectric and electrical properties of Bi93Sb7 alloy thin films Mallik, Ramesh Chandra; Das, V. Damodara Journal of Applied Physics, Vol. 98, Issue 2 https://doi.org/10.1063/1.1957126	journal	July 2005
Thermoelectric transport properties of n -doped and p -doped Bi0.91Sb0.09 alloy thin films Cho, Sunglae; DiVenere, Antonio; Wong, George K. Journal of Applied Physics, Vol. 85, Issue 7 https://doi.org/10.1063/1.369729	journal	April 1999
Anisotropic Seebeck and magneto-Seebeck coefficients of Bi and Bi0.92Sb0.08 alloy thin films Cho, Sunglae; Kim, Yunki; DiVenere, Antonio Journal of Applied Physics, Vol. 88, Issue 2 https://doi.org/10.1063/1.373740	journal	July 2000
Temperature Dependence of the Electrical Properties of Bismuth-Antimony Alloys Jain, A. L. Physical Review, Vol. 114, Issue 6 https://doi.org/10.1103/PhysRev.114.1518	journal	June 1959
Transport properties of Bi 1 − x Sb x alloy thin films grown on CdTe ( 111 ) B Cho, Sunglae; DiVenere, Antonio; Wong, George K. Physical Review B, Vol. 59, Issue 16 https://doi.org/10.1103/PhysRevB.59.10691	journal	April 1999
Refinement of the crystal structure of cubic antimony trioxide, Sb ₂ O ₃ Svensson, C. Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 31, Issue 8 https://doi.org/10.1107/S0567740875006759	journal	August 1975
Molecular beam epitaxial growth and structural properties of Bi1−xSbx alloy thin films on CdTe(111) substrates Cho, Sunglae; DiVenere, Antonio; Wong, George K. Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 17, Issue 1 https://doi.org/10.1116/1.581546	journal	January 1999
Using galvanostatic electroforming of Bi _{1– x} Sb _x nanowires to control composition, crystallinity, and orientation Limmer, Steven J.; Medlin, Douglas L.; Siegal, Michael P. Journal of Materials Research, Vol. 30, Issue 2 https://doi.org/10.1557/jmr.2014.354	journal	December 2014

Cited By (1)

Correlating thermoelectric properties with microstructure in Bi _0.8 Sb _0.2 thin films Siegal, M. P.; Lima-Sharma, A. L.; Sharma, P. A. Applied Physics Letters, Vol. 110, Issue 14 https://doi.org/10.1063/1.4979785	journal	April 2017

Similar Records

Correlating thermoelectric properties with microstructure in Bi _0.8 Sb _0.2 thin films

Journal Article · Sun Apr 02 20:00:00 EDT 2017 · Applied Physics Letters · OSTI ID:1357018

Using galvanostatic electroforming of Bi_1–xSb_xnanowires to control composition, crystallinity, and orientation

Journal Article · Tue Dec 02 19:00:00 EST 2014 · Journal of Materials Research · OSTI ID:1146606

Thermoelectric power of Bi{sub 92}Sb{sub 8} and Bi{sub 85}Sb{sub 15} thin films

Journal Article · Sat Jul 15 00:00:00 EDT 2017 · Semiconductors · OSTI ID:22756463

Related Subjects

36 MATERIALS SCIENCE