DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Correlating thermoelectric (Bi,Sb)2Te3 film electric transport properties with microstructure

Abstract

The room temperature electronic transport properties of 1 μm thick Bi0.4Sb1.6Te3 (BST) films correlate with overall microstructural quality. Films with homogeneous composition are deposited onto fused silica substrates, capped with SiN to stop both oxidation and Te loss, and postannealed to temperatures ranging from 200 to 450 °C. BST grain sizes and (00l) orientations improve dramatically with annealing to 375 °C, with smaller increases to 450 °C. Tiny few-nanometer-sized voids in the as-deposited film grain boundaries coalesce into larger void sizes up to 300 nm with annealing to 350 °C; the smallest voids continue coalescing with annealing to 450 °C. These voids are decorated with few-nanometer-sized Sb clusters that increase in number with increasing annealing temperatures, reducing the Sb content of the remaining BST film matrix. Resistivity decreases linearly with increasing temperature over the entire range studied, consistent with improving crystalline quality. The Seebeck coefficient also improves with crystalline quality to 350 °C, above which void coalescence and reduced Sb content from the BST matrix correlate with a decrease in the Seebeck coefficient. Yet, a plateau exists for an optimal power factor between 350 and 450 °C, implying thermal stability to higher temperatures than previously reported.

Authors:
 [1];  [2];  [1];  [1];  [3]
  1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); 3M Corporate Research Lab., St. Paul, MN (United States)
  3. Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Publication Date:
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:
1575278
Alternate Identifier(s):
OSTI ID: 1510360
Report Number(s):
SAND-2019-0942J
Journal ID: ISSN 0021-8979; 671922; TRN: US2001231
Grant/Contract Number:  
AC04-94AL85000; NA0003525AC04-94AL85000
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Applied Physics
Additional Journal Information:
Journal Volume: 125; Journal Issue: 17; Journal ID: ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; bismuth antimony telluride; films; thermoelectric

Citation Formats

Siegal, M. P., Podkaminer, J., Lima-Sharma, A. L., Sharma, P. A., and Medlin, D. L. Correlating thermoelectric (Bi,Sb)2Te3 film electric transport properties with microstructure. United States: N. p., 2019. Web. doi:10.1063/1.5089647.
Siegal, M. P., Podkaminer, J., Lima-Sharma, A. L., Sharma, P. A., & Medlin, D. L. Correlating thermoelectric (Bi,Sb)2Te3 film electric transport properties with microstructure. United States. https://doi.org/10.1063/1.5089647
Siegal, M. P., Podkaminer, J., Lima-Sharma, A. L., Sharma, P. A., and Medlin, D. L. Thu . "Correlating thermoelectric (Bi,Sb)2Te3 film electric transport properties with microstructure". United States. https://doi.org/10.1063/1.5089647. https://www.osti.gov/servlets/purl/1575278.
@article{osti_1575278,
title = {Correlating thermoelectric (Bi,Sb)2Te3 film electric transport properties with microstructure},
author = {Siegal, M. P. and Podkaminer, J. and Lima-Sharma, A. L. and Sharma, P. A. and Medlin, D. L.},
abstractNote = {The room temperature electronic transport properties of 1 μm thick Bi0.4Sb1.6Te3 (BST) films correlate with overall microstructural quality. Films with homogeneous composition are deposited onto fused silica substrates, capped with SiN to stop both oxidation and Te loss, and postannealed to temperatures ranging from 200 to 450 °C. BST grain sizes and (00l) orientations improve dramatically with annealing to 375 °C, with smaller increases to 450 °C. Tiny few-nanometer-sized voids in the as-deposited film grain boundaries coalesce into larger void sizes up to 300 nm with annealing to 350 °C; the smallest voids continue coalescing with annealing to 450 °C. These voids are decorated with few-nanometer-sized Sb clusters that increase in number with increasing annealing temperatures, reducing the Sb content of the remaining BST film matrix. Resistivity decreases linearly with increasing temperature over the entire range studied, consistent with improving crystalline quality. The Seebeck coefficient also improves with crystalline quality to 350 °C, above which void coalescence and reduced Sb content from the BST matrix correlate with a decrease in the Seebeck coefficient. Yet, a plateau exists for an optimal power factor between 350 and 450 °C, implying thermal stability to higher temperatures than previously reported.},
doi = {10.1063/1.5089647},
journal = {Journal of Applied Physics},
number = 17,
volume = 125,
place = {United States},
year = {Thu May 02 00:00:00 EDT 2019},
month = {Thu May 02 00:00:00 EDT 2019}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 2 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Microstructural evolution during film growth
journal, September 2003

  • Petrov, I.; Barna, P. B.; Hultman, L.
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 21, Issue 5
  • DOI: 10.1116/1.1601610

Topotactical reactions with ferrimagnetic oxides having hexagonal crystal structures—I
journal, February 1959


Segregation of sulfur during growth of oxide scales
journal, April 1991


Improving Bi 2 Te 3 -based thermoelectric nanowire microstructure via thermal processing
journal, January 2014

  • Siegal, Michael P.; Limmer, Steven J.; Lensch-Falk, Jessica L.
  • Journal of Materials Research, Vol. 29, Issue 2
  • DOI: 10.1557/jmr.2013.370

Thermoelectric properties of p-type (Bi2Te3)x(Sb2Te3)1−x prepared via bulk mechanical alloying and hot pressing
journal, September 2000


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

  • Limmer, Steven J.; Yelton, W. Graham; Erickson, Kristopher J.
  • Nano Letters, Vol. 14, Issue 4
  • DOI: 10.1021/nl404752p

The microstructure of sputter‐deposited coatings
journal, November 1986

  • Thornton, John A.
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 4, Issue 6
  • DOI: 10.1116/1.573628

Improved thermoelectric performance of highly-oriented nanocrystalline bismuth antimony telluride thin films
journal, November 2010


Elastic stiffness and thermal expansion coefficients of various refractory silicides and silicon nitride films
journal, August 1980


Crystal growth and orientation in sputtered films of bismuth telluride
journal, December 1964


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

Bismuth antimony telluride thin films with unique crystal orientation by two-step method
journal, October 2016


Influence of annealing on the structural and electrical transport properties of Bi0.5Sb1.5Te3.0 thin films deposited by co-sputtering
journal, March 2013


THERMOELECTRIC PROPERTIES OF Bi 2 Te 3 –Sb 2 Te 3 ALLOYS
journal, April 1965

  • Champness, C. H.; Chiang, P. T.; Parekh, P.
  • Canadian Journal of Physics, Vol. 43, Issue 4
  • DOI: 10.1139/p65-060

Thermal Expansion of Fused Quartz
journal, April 1969


Electrical contact uniformity and surface oxidation of ternary chalcogenide alloys
journal, January 2019

  • Sharma, P. A.; Brumbach, M.; Adams, D. P.
  • AIP Advances, Vol. 9, Issue 1
  • DOI: 10.1063/1.5081818

Thermoelectric properties of (BixSb1−x)2Te3 single crystal solid solutions grown by the T.H.M. method
journal, August 1992


Low Temperature Transport Properties of the Group V Semimetals
journal, January 1979

  • Issi, J-P
  • Australian Journal of Physics, Vol. 32, Issue 6
  • DOI: 10.1071/PH790585

Fabrication and characterization of bismuth–telluride-based alloy thin film thermoelectric generators by flash evaporation method
journal, August 2007

  • Takashiri, M.; Shirakawa, T.; Miyazaki, K.
  • Sensors and Actuators A: Physical, Vol. 138, Issue 2
  • DOI: 10.1016/j.sna.2007.05.030

Controlling compositional homogeneity and crystalline orientation in Bi 0.8 Sb 0.2 thermoelectric thin films
journal, December 2015

  • Rochford, C.; Medlin, D. L.; Erickson, K. J.
  • APL Materials, Vol. 3, Issue 12
  • DOI: 10.1063/1.4937894

The Seebeck coefficient and the Fermi surface of antimony single crystals
journal, February 1968


Growth of pinhole‐free epitaxial yttrium silicide on Si(111)
journal, July 1990

  • Siegal, Michael P.; Graham, William R.; Santiago‐Aviles, Jorge J.
  • Journal of Applied Physics, Vol. 68, Issue 2
  • DOI: 10.1063/1.346809

Clustering on surfaces
journal, December 1992


Thickness and temperature effects on thermoelectric power and electrical resistivity of (Bi0.25Sb0.75)2Te3 thin films
journal, November 1998


Thermoelectric properties of Bi0.5Sb1.5Te3 thin films grown by pulsed laser deposition
journal, May 2015


High-Thermoelectric Performance of Nanostructured Bismuth Antimony Telluride Bulk Alloys
journal, May 2008


Thermal Expansion of n-Type Doped Bi2Te2.88Se0.12 and p-Type Doped Bi0.52Sb1.48Te3 Solid Solutions from −60°C to +60°C
journal, July 2010