Skip to main content
OSTI.GOVU.S. Department of Energy Office of Scientific and Technical Information
U.S. Department of Energy
Office of Scientific and Technical Information
 

Understanding the role and interplay of heavy-hole and light-hole valence bands in the thermoelectric properties of PbSe

Journal Article · · Physical Review. B, Condensed Matter and Materials Physics
 [1];  [1];  [2];  [2];  [3];  [3];  [1]
  1. Northwestern Univ., Evanston, IL (United States)
  2. Aristotle Univ. of Thessaloniki (Greece)
  3. Univ. of Michigan, Ann Arbor, MI (United States)
+ Show Author Affiliations
The thermoelectric properties of PbSe have significantly improved in recent years reaching figures of merit ZT~1.6. The transport properties of the hole-doped high temperature thermoelectric material PbSe are particularly interesting and play a key role in this. Here, they were analyzed over wide temperature and hole concentration ranges. The special features observed in the variation of the experimental Seebeck coefficient and Hall coefficient can be accounted for within the framework of a two-band model. Two valence bands separated by a temperature dependent energy offset are considered. Furthermore, the extremum of the light-hole band has a density of states mass ~0.27mo at room temperature. It is nonparabolic and anisotropic and can be described by the Kane model. The extremum of the heavy-hole band is isotropic and parabolic with a much larger density of states mass ~2.5mo. We find that for heavily doped compositions, the high mass band contributes the Seebeck coefficient, even at room temperature. With rising temperature, holes are transferred from the light-hole to the heavy-hole branch, giving rise to the anomalous temperature dependent Hall coefficient, which is found peaked near ~650K. For Na-doped samples Pb1–xNaxSe for 0.01 ≤ x ≤ 0.03, the high thermopower values of 200–300μV/K at 900 K arise from the heavy-hole band, which are responsible for the excellent thermoelectric performance of PbSe.
Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Revolutionary Materials for Solid State Energy Conversion (RMSSEC)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
SC0001054
OSTI ID:
1370356
Alternate ID(s):
OSTI ID: 1181587
Journal Information:
Physical Review. B, Condensed Matter and Materials Physics, Journal Name: Physical Review. B, Condensed Matter and Materials Physics Journal Issue: 8 Vol. 91; ISSN 1098-0121
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

References (41)

Heavily Doped p-Type PbSe with High Thermoelectric Performance: An Alternative for PbTe journal February 2011
Band Engineering of Thermoelectric Materials journal October 2012
High Thermoelectric Efficiency of n-type PbS journal November 2012
Scattering of Current Carriers and Transport Phenomena in Lead Chalcogenides journal January 1971
Free electron effective mass in PbSe and PbSnSe mixed crystals journal June 1970
Room temperature transport properties of p-type PbTe journal January 1972
The mobility of free carriers in PbSe crystals journal April 1973
Nanostructured Thermoelectrics: The New Paradigm? † journal February 2010
Heavy Doping and Band Engineering by Potassium to Improve the Thermoelectric Figure of Merit in p-Type PbTe, PbSe, and PbTe 1– y Se y journal June 2012
Study of the Thermoelectric Properties of Lead Selenide Doped with Boron, Gallium, Indium, or Thallium journal October 2012
Role of Sodium Doping in Lead Chalcogenide Thermoelectrics journal March 2013
High-Performance Tellurium-Free Thermoelectrics: All-Scale Hierarchical Structuring of p-Type PbSe–MSe Systems (M = Ca, Sr, Ba) journal March 2013
High Thermoelectric Performance via Hierarchical Compositionally Alloyed Nanostructures journal May 2013
High ZT in p-Type (PbTe) 1–2 x (PbSe) x (PbS) x Thermoelectric Materials journal February 2014
Thermopower enhancement in Pb1−xMnxTe alloys and its effect on thermoelectric efficiency journal September 2012
Convergence of electronic bands for high performance bulk thermoelectrics journal May 2011
High thermoelectric figure of merit in heavy hole dominated PbTe journal January 2011
All-scale hierarchical thermoelectrics: MgTe in PbTe facilitates valence band convergence and suppresses bipolar thermal transport for high performance journal January 2013
The panoscopic approach to high performance thermoelectrics journal January 2014
Tuning bands of PbSe for better thermoelectric efficiency journal January 2014
Rational design of p-type thermoelectric PbTe: temperature dependent sodium solubility journal January 2013
Highly efficient (In 2 Te 3 ) x (GeTe) 3−3x thermoelectric materials: a substitute for TAGS journal January 2014
The band edge Structure of the Iv-Vi Semiconductors journal November 1968
Extension of the Aukerman‐Willardson Two‐Band Hall Coefficient Analysis journal August 1965
Temperature dependent band gap in PbX (X = S, Se, Te) journal December 2013
Band structure engineering through orbital interaction for enhanced thermoelectric power factor journal February 2014
Weak electron-phonon coupling contributing to high thermoelectric performance in n-type PbSe journal May 2012
Electron transport phenomena in small-gap semiconductors journal May 1974
The Thermoelectric Figure of Merit and its Relation to Thermoelectric Generators† journal July 1959
Infrared absorption of laser deposited PbSe films journal March 1987
Galvano- and thermo-magnetic coefficients for a multi-band conductor journal June 1975
The Hall mobility and thermoelectric power of p-type lead telluride journal September 1967
Optical band gap and the Burstein–Moss effect in iodine doped PbTe using diffuse reflectance infrared Fourier transform spectroscopy journal July 2013
Temperature Dependence of the Effective Masses in PbTe journal July 1964
Electronic transport properties of PbTe and AgPb m SbTe 2 + m systems journal September 2006
Energy and temperature dependence of relaxation time and Wiedemann-Franz law on PbTe journal April 2010
Quasiparticle self-consistent GW calculations for PbS, PbSe, and PbTe: Band structure and pressure coefficients journal June 2010
High-temperature thermoelectric performance of heavily doped PbSe journal July 2010
High-temperature charge and thermal transport properties of the n -type thermoelectric material PbSe journal October 2011
Valence-band structure of highly efficient p -type thermoelectric PbTe-PbS alloys journal January 2013
The dominant mechanisms of charge-carrier scattering in lead telluride journal February 1997

Cited By (5)

High Thermoelectric Performance in PbSe–NaSbSe 2 Alloys from Valence Band Convergence and Low Thermal Conductivity journal July 2019
Soft phonon modes from off-center Ge atoms lead to ultralow thermal conductivity and superior thermoelectric performance in n-type PbSe–GeSe journal January 2018
Fundamental and progress of Bi 2 Te 3 -based thermoelectric materials journal April 2018
Limit of z T enhancement in rocksalt structured chalcogenides by band convergence journal October 2016
Dirac parameters and topological phase diagram of P b 1 − x S n x Se from magnetospectroscopy journal December 2018

Figures / Tables (9)

FIG. 1(p. 33)figure FIG. 1
FIG. 2(p. 34)figure FIG. 2
FIG. 3(p. 35)figure FIG. 3
FIG. 4(p. 36)figure FIG. 4
FIG. 5(p. 37)figure FIG. 5
FIG. 6(p. 38)figure FIG. 6
FIG. 7(p. 39)figure FIG. 7
Table I(p. 40)table Table I
Table II(p. 41)table Table II

Similar Records

High-temperature thermoelectric properties of n-type PbSe doped with Ga, In, and Pb.
Journal Article · Tue May 31 00:00:00 EDT 2011 · Phys. Rev. B · OSTI ID:1015966
All-Scale Hierarchically Structured p-Type PbSe Alloys with High Thermoelectric Performance Enabled by Improved Band Degeneracy
Journal Article · Mon Feb 18 19:00:00 EST 2019 · Journal of the American Chemical Society · OSTI ID:1777264
Study of the Thermoelectric Properties of Lead Selenide Doped with Boron, Gallium, Indium, or Thallium
Journal Article · Wed Oct 24 00:00:00 EDT 2012 · Journal of the American Chemical Society · OSTI ID:1080575

Related Subjects

36 MATERIALS SCIENCE