Charge carrier effective mass and concentration derived from combination of Seebeck coefficient and Te125 NMR measurements in complex tellurides

Levin, E. M.

doi:10.1103/PhysRevB.93.245202

Title: Charge carrier effective mass and concentration derived from combination of Seebeck coefficient and ${}^{125}{Te}$ NMR measurements in complex tellurides

Abstract

Thermoelectric materials utilize the Seebeck effect to convert heat to electrical energy. The Seebeck coefficient (thermopower), S, depends on the free (mobile) carrier concentration, n, and effective mass, m*, as S ~ m*/n^2/3. The carrier concentration in tellurides can be derived from ¹²⁵Te nuclear magnetic resonance (NMR) spin-lattice relaxation measurements. The NMR spin-lattice relaxation rate, 1/T₁, depends on both n and m* as 1/T₁~(m*)^3/2n (within classical Maxwell-Boltzmann statistics) or as 1/T1~(m*)²n^2/3 (within quantum Fermi-Dirac statistics), which challenges the correct determination of the carrier concentration in some materials by NMR. Here it is shown that the combination of the Seebeck coefficient and ¹²⁵Te NMR spin-lattice relaxation measurements in complex tellurides provides a unique opportunity to derive the carrier effective mass and then to calculate the carrier concentration. This approach was used to study Ag_xSb_xGe_50–2xTe₅₀, well-known GeTe-based high-efficiency tellurium-antimony-germanium-silver thermoelectric materials, where the replacement of Ge by [Ag+Sb] results in significant enhancement of the Seebeck coefficient. Thus, values of both m* and n derived using this combination show that the enhancement of thermopower can be attributed primarily to an increase of the carrier effective mass and partially to a decrease of the carrier concentration when the [Ag+Sb] content increases.

Authors:

Levin, E. M. ^[1]

Ames Lab. and Iowa State Univ., Ames, IA (United States)

Publication Date:: Mon Jun 27 00:00:00 EDT 2016

Research Org.:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1278781

Alternate Identifier(s):: OSTI ID: 1259584

Report Number(s):: IS-J-9009
Journal ID: ISSN 2469-9950; PRBMDO

Grant/Contract Number:: AC02-07CH11358

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review B

Additional Journal Information:: Journal Volume: 93; Journal Issue: 24; Journal ID: ISSN 2469-9950

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Ag_xSb_xGe_50–2xTe₅₀ (TAGS); Seebeck coefficient; ¹²⁵Te NMR spin-lattice relaxation time; charge carrier effective mass and concentration

Citation Formats


                    Levin, E. M. Charge carrier effective mass and concentration derived from combination of Seebeck coefficient and Te125 NMR measurements in complex tellurides.  United States: N. p., 2016. 
Web.  doi:10.1103/PhysRevB.93.245202.

Copy to clipboard


                    Levin, E. M. Charge carrier effective mass and concentration derived from combination of Seebeck coefficient and Te125 NMR measurements in complex tellurides.  United States.  https://doi.org/10.1103/PhysRevB.93.245202

Copy to clipboard


                    Levin, E. M. Mon .  
"Charge carrier effective mass and concentration derived from combination of Seebeck coefficient and Te125 NMR measurements in complex tellurides".  United States.  https://doi.org/10.1103/PhysRevB.93.245202.  https://www.osti.gov/servlets/purl/1278781.

Copy to clipboard


                    
@article{osti_1278781,

  title        = {Charge carrier effective mass and concentration derived from combination of Seebeck coefficient and Te125 NMR measurements in complex tellurides},

  author       = {Levin, E. M.},

  abstractNote = {Thermoelectric materials utilize the Seebeck effect to convert heat to electrical energy. The Seebeck coefficient (thermopower), S, depends on the free (mobile) carrier concentration, n, and effective mass, m*, as S ~ m*/n2/3. The carrier concentration in tellurides can be derived from 125Te nuclear magnetic resonance (NMR) spin-lattice relaxation measurements. The NMR spin-lattice relaxation rate, 1/T1, depends on both n and m* as 1/T1~(m*)3/2n (within classical Maxwell-Boltzmann statistics) or as 1/T1~(m*)2n2/3 (within quantum Fermi-Dirac statistics), which challenges the correct determination of the carrier concentration in some materials by NMR. Here it is shown that the combination of the Seebeck coefficient and 125Te NMR spin-lattice relaxation measurements in complex tellurides provides a unique opportunity to derive the carrier effective mass and then to calculate the carrier concentration. This approach was used to study AgxSbxGe50–2xTe50, well-known GeTe-based high-efficiency tellurium-antimony-germanium-silver thermoelectric materials, where the replacement of Ge by [Ag+Sb] results in significant enhancement of the Seebeck coefficient. Thus, values of both m* and n derived using this combination show that the enhancement of thermopower can be attributed primarily to an increase of the carrier effective mass and partially to a decrease of the carrier concentration when the [Ag+Sb] content increases.},

  doi          = {10.1103/PhysRevB.93.245202},

  journal      = {Physical Review B},

  number       = 24,

  volume       = 93,

  place        = {United States},

  year         = {Mon Jun 27 00:00:00 EDT 2016},

  month        = {Mon Jun 27 00:00:00 EDT 2016}

}

Copy to clipboard

Journal Article:

Free Publicly Available Full Text

Accepted Manuscript (Publisher)

Accepted Manuscript (DOE)

Publisher's Version of Record

https://doi.org/10.1103/PhysRevB.93.245202

Other availability

Search WorldCat to find libraries that may hold this journal

Citation Metrics:

Cited by: 26 works

Citation information provided by
Web of Science

Save / Share:

Export Metadata

Save to My Library

Works referenced in this record:

Complex thermoelectric materials
journal, February 2008

Snyder, G. Jeffrey; Toberer, Eric S.
Nature Materials, Vol. 7, Issue 2, p. 105-114
DOI: 10.1038/nmat2090

Nanostructured Thermoelectrics: Big Efficiency Gains from Small Features
journal, July 2010

Vineis, Christopher J.; Shakouri, Ali; Majumdar, Arun
Advanced Materials, Vol. 22, Issue 36, p. 3970-3980
DOI: 10.1002/adma.201000839

Recent Developments in Semiconductor Thermoelectric Physics and Materials
journal, August 2011

Shakouri, Ali
Annual Review of Materials Research, Vol. 41, Issue 1
DOI: 10.1146/annurev-matsci-062910-100445

Electronic inhomogeneity and Ag:Sb imbalance of ${Ag}_{1 - y} {Pb}_{18} {Sb}_{1 + z} {Te}_{20}$ high-performance thermoelectrics elucidated by ${}^{125}T e$ and ${}^{207}P b$ NMR
journal, September 2009

Levin, E. M.; Cook, B. A.; Ahn, K.
Physical Review B, Vol. 80, Issue 11
DOI: 10.1103/PhysRevB.80.115211

Electronic inhomogeneity in $n$ - and $p$ -type PbTe detected by $^{125}$ Te NMR
journal, September 2013

Levin, E. M.; Heremans, J. P.; Kanatzidis, M. G.
Physical Review B, Vol. 88, Issue 11
DOI: 10.1103/PhysRevB.88.115211

NMR Probe of Metallic States in Nanoscale Topological Insulators
journal, January 2013

Koumoulis, Dimitrios; Chasapis, Thomas C.; Taylor, Robert E.
Physical Review Letters, Vol. 110, Issue 2
DOI: 10.1103/PhysRevLett.110.026602

NMR study of native defects in PbSe
journal, September 2014

Koumoulis, D.; Taylor, R. E.; King, D.
Physical Review B, Vol. 90, Issue 12
DOI: 10.1103/PhysRevB.90.125201

Electronic and thermal transport in GeTe: A versatile base for thermoelectric materials
journal, August 2013

Levin, E. M.; Besser, M. F.; Hanus, R.
Journal of Applied Physics, Vol. 114, Issue 8
DOI: 10.1063/1.4819222

Enhancement of Thermopower of TAGS-85 High-Performance Thermoelectric Material by Doping with the Rare Earth Dy
journal, April 2012

Levin, E. M.; Bud'ko, S. L.; Schmidt-Rohr, K.
Advanced Functional Materials, Vol. 22, Issue 13
DOI: 10.1002/adfm.201103049

NMR investigation of the diffusion and conduction properties of the semiconductor tellurium. I. Electronic properties
journal, May 1979

Selbach, H.; Kanert, O.; Wolf, D.
Physical Review B, Vol. 19, Issue 9
DOI: 10.1103/PhysRevB.19.4435

Nanostructures in high-performance (GeTe) _x (AgSbTe ₂ ) _{100− x} thermoelectric materials
journal, May 2008

Yang, S. H.; Zhu, T. J.; Sun, T.
Nanotechnology, Vol. 19, Issue 24
DOI: 10.1088/0957-4484/19/24/245707

Transport and mechanical property evaluation of (AgSbTe)1−x(GeTe)x (x=0.80, 0.82, 0.85, 0.87, 0.90)
journal, August 2009

Salvador, James R.; Yang, J.; Shi, X.
Journal of Solid State Chemistry, Vol. 182, Issue 8
DOI: 10.1016/j.jssc.2009.05.024

Thermoelectric properties of Ag ₂ Sb ₂ Ge _{46 − x} Dy _x Te ₅₀ alloys with high power factor: Thermoelectric properties of Ag ₂ Sb ₂ Ge _{46 − x} Dy _x Te ₅₀ alloys
journal, September 2013

Levin, E. M.; Hanus, R.; Hanson, M.
physica status solidi (a), Vol. 210, Issue 12
DOI: 10.1002/pssa.201330217

Solid State NMR
book, January 2012

Chan, Jerry C. C.
Topics in Current Chemistry
DOI: 10.1007/978-3-642-24803-0

Highly Efficient Ge-Rich Ge x Pb1−x Te Thermoelectric Alloys
journal, December 2009

Gelbstein, Yaniv; Dado, Boaz; Ben-Yehuda, Ohad
Journal of Electronic Materials, Vol. 39, Issue 9
DOI: 10.1007/s11664-009-1012-z

Carrier Compensation in Germanium Telluride
journal, January 1963

Lubell, M. S.; Mazelsky, R.
Journal of The Electrochemical Society, Vol. 110, Issue 6
DOI: 10.1149/1.2425805

Effects of Ge substitution in GeTe by Ag or Sb on the Seebeck coefficient and carrier concentration derived from ${}^{125}{Te}$ NMR
journal, January 2016

Levin, E. M.
Physical Review B, Vol. 93, Issue 4
DOI: 10.1103/PhysRevB.93.045209

Transport properties and valence band feature of high-performance (GeTe) ₈₅ (AgSbTe ₂ ) ₁₅ thermoelectric materials
journal, January 2014

Chen, Y.; Jaworski, C. M.; Gao, Y. B.
New Journal of Physics, Vol. 16, Issue 1
DOI: 10.1088/1367-2630/16/1/013057

Works referencing / citing this record:

Thermodynamic and thermoelectric properties of CoFeYGe (Y = Ti, Cr) quaternary Heusler alloys: first principle calculations
journal, November 2019

Haleoot, Raad; Hamad, Bothina
Journal of Physics: Condensed Matter, Vol. 32, Issue 7
DOI: 10.1088/1361-648x/ab5321

Similar Records in DOE PAGES and OSTI.GOV collections:

Electronic properties of GeTe and Ag- or Sb-substituted GeTe studied by low-temperature ${}^{125}{Te}$ NMR

Journal Article Cui, J. ; Levin, E. M. ; Lee, Y. ; ... - Physical Review B

We have carried out ¹²⁵Te nuclear magnetic resonance (NMR) in a wide temperature range of 1.5–300 K to investigate the electronic properties of Ge₅₀ Te₅₀, Ag₂ Ge₄₈Te₅₀ , and Sb₂ Ge₄₈ Te₅₀ from a microscopic point of view. From the temperature dependence of the NMR shift (K) and nuclear spin lattice relaxation rate (1/T₁), we found that two bands contribute to the physical properties of the materials. One band overlaps the Fermi level providing the metallic state where no strong electron correlations are revealed by Korringa analysis. The other band is separated from the Fermi level by an energy gapmore »« less
Cited by 4
https://doi.org/10.1103/PhysRevB.94.085203

Full Text Available
Electronic and thermal transport in GeTe: A versatile base for thermoelectric materials

Journal Article Levin, Evgenii ; Besser, Mathew ; Hanus, Riley - Journal of Applied Physics

GeTe is a narrow-band gap semiconductor, where Ge vacancies generate free charge carriers, holes, forming a self-dopant degenerate system with p-type conductivity, and serves as a base for high-performance multicomponent thermoelectric materials. There is a significant discrepancy between the electronic and thermal transport data for GeTe-based materials reported in the literature, which obscures the baseline knowledge and prevents a clear understanding of the effect of alloying GeTe with various elements. A comprehensive study including XRD, SEM, EDS, Seebeck coefficient, electrical resistivity, thermal conductivity, and ¹²⁵Te NMR of several GeTe samples was conducted. Similar Seebeck coefficient and electrical resistivity are observedmore »« less
https://doi.org/10.1063/1.4819222
Electronic and thermal transport in GeTe: A versatile base for thermoelectric materials

Journal Article Levin, E. M. ; Department of Physics and Astronomy, Iowa State University, Ames, Iowa 50011 ; Besser, M. F. ; ... - Journal of Applied Physics

GeTe is a narrow-band gap semiconductor, where Ge vacancies generate free charge carriers, holes, forming a self-dopant degenerate system with p-type conductivity, and serves as a base for high-performance multicomponent thermoelectric materials. There is a significant discrepancy between the electronic and thermal transport data for GeTe-based materials reported in the literature, which obscures the baseline knowledge and prevents a clear understanding of the effect of alloying GeTe with various elements. A comprehensive study including XRD, SEM, EDS, Seebeck coefficient, electrical resistivity, thermal conductivity, and {sup 125}Te NMR of several GeTe samples was conducted. Similar Seebeck coefficient and electrical resistivity aremore »« less
https://doi.org/10.1063/1.4819222
¹²⁵Te NMR and Seebeck Effect in Bi₂Te₃ Synthesized from Stoichiometric and Te-Rich Melts

Journal Article Levin, E. M. ; Iowa State Univ., Ames, IA ; Riedemann, T. M. ; ... - Journal of Physical Chemistry. C

Bi₂Te₃ is a well-known thermoelectric material and, as a new form of quantum matter, a topological insulator. Variation of local chemical composition in Bi2Te3 results in formation of several types of atomic defects, including Bi and Te vacancies and Bi and Te antisite defects; these defects can strongly affect material functionality via generation of free electrons and/or holes. Nonuniform distribution of atomic defects produces electronic inhomogeneity, which can be detected by ¹²⁵Te nuclear magnetic resonance (NMR). Here we report on ¹²⁵Te NMR and Seebeck effect (heat to electrical energy conversion) for two single crystalline samples: (#1) grown from stoichiometric compositionmore »« less
Cited by 8
https://doi.org/10.1021/acs.jpcc.6b06973

Full Text Available
Enhancement of thermopower of TAGS-85 high-performance thermoelectric materials by doping with the rare earth Dy

Journal Article Levin, Evgenii ; Budko, Serfuei ; Schmidt-Rohr, Klaus - Advanced Functional Materials

Enhancement of thermopower is achieved by doping the narrow-band semiconductor Ag{sub 6.52}Sb{sub 6.52}Ge{sub 36.96}Te{sub 50} (acronym TAGS-85), one of the best p-type thermoelectric materials, with 1 or 2% of the rare earth dysprosium (Dy). Evidence for the incorporation of Dy into the lattice is provided by X-ray diffraction and increased orientation-dependent local fields detected by {sup 125}Te NMR spectroscopy. Since Dy has a stable electronic configuration, the enhancement cannot be attributed to 4f-electron states formed near the Fermi level. It is likely that the enhancement is due to a small reduction in the carrier concentration, detected by {sup 125}Te NMRmore »« less
https://doi.org/10.1002/adfm.201103049

Similar Records

Title: Charge carrier effective mass and concentration derived from combination of Seebeck coefficient and Te 125 NMR measurements in complex tellurides

Abstract

Citation Formats

Complex thermoelectric materials journal, February 2008

Nanostructured Thermoelectrics: Big Efficiency Gains from Small Features journal, July 2010

Recent Developments in Semiconductor Thermoelectric Physics and Materials journal, August 2011

Electronic inhomogeneity and Ag:Sb imbalance of Ag 1 − y Pb 18 Sb 1 + z Te 20 high-performance thermoelectrics elucidated by T 125 e and P 207 b NMR journal, September 2009

Electronic inhomogeneity in n - and p -type PbTe detected by 125 Te NMR journal, September 2013

NMR Probe of Metallic States in Nanoscale Topological Insulators journal, January 2013

NMR study of native defects in PbSe journal, September 2014

Electronic and thermal transport in GeTe: A versatile base for thermoelectric materials journal, August 2013

Enhancement of Thermopower of TAGS-85 High-Performance Thermoelectric Material by Doping with the Rare Earth Dy journal, April 2012

NMR investigation of the diffusion and conduction properties of the semiconductor tellurium. I. Electronic properties journal, May 1979

Nanostructures in high-performance (GeTe) x (AgSbTe 2 ) 100− x thermoelectric materials journal, May 2008

Transport and mechanical property evaluation of (AgSbTe)1−x(GeTe)x (x=0.80, 0.82, 0.85, 0.87, 0.90) journal, August 2009

Thermoelectric properties of Ag 2 Sb 2 Ge 46 − x Dy x Te 50 alloys with high power factor: Thermoelectric properties of Ag 2 Sb 2 Ge 46 − x Dy x Te 50 alloys journal, September 2013

Solid State NMR book, January 2012

Highly Efficient Ge-Rich Ge x Pb1−x Te Thermoelectric Alloys journal, December 2009

Carrier Compensation in Germanium Telluride journal, January 1963

Effects of Ge substitution in GeTe by Ag or Sb on the Seebeck coefficient and carrier concentration derived from Te 125 NMR journal, January 2016

Transport properties and valence band feature of high-performance (GeTe) 85 (AgSbTe 2 ) 15 thermoelectric materials journal, January 2014

Thermodynamic and thermoelectric properties of CoFeYGe (Y = Ti, Cr) quaternary Heusler alloys: first principle calculations journal, November 2019

Title: Charge carrier effective mass and concentration derived from combination of Seebeck coefficient and ${}^{125}{Te}$ NMR measurements in complex tellurides

Complex thermoelectric materials
journal, February 2008

Nanostructured Thermoelectrics: Big Efficiency Gains from Small Features
journal, July 2010

Recent Developments in Semiconductor Thermoelectric Physics and Materials
journal, August 2011

Electronic inhomogeneity and Ag:Sb imbalance of ${Ag}_{1 - y} {Pb}_{18} {Sb}_{1 + z} {Te}_{20}$ high-performance thermoelectrics elucidated by ${}^{125}T e$ and ${}^{207}P b$ NMR
journal, September 2009

Electronic inhomogeneity in $n$ - and $p$ -type PbTe detected by $^{125}$ Te NMR
journal, September 2013

NMR Probe of Metallic States in Nanoscale Topological Insulators
journal, January 2013

NMR study of native defects in PbSe
journal, September 2014

Electronic and thermal transport in GeTe: A versatile base for thermoelectric materials
journal, August 2013

Enhancement of Thermopower of TAGS-85 High-Performance Thermoelectric Material by Doping with the Rare Earth Dy
journal, April 2012

NMR investigation of the diffusion and conduction properties of the semiconductor tellurium. I. Electronic properties
journal, May 1979

Nanostructures in high-performance (GeTe) _x (AgSbTe ₂ ) _{100− x} thermoelectric materials
journal, May 2008

Transport and mechanical property evaluation of (AgSbTe)1−x(GeTe)x (x=0.80, 0.82, 0.85, 0.87, 0.90)
journal, August 2009

Thermoelectric properties of Ag ₂ Sb ₂ Ge _{46 − x} Dy _x Te ₅₀ alloys with high power factor: Thermoelectric properties of Ag ₂ Sb ₂ Ge _{46 − x} Dy _x Te ₅₀ alloys
journal, September 2013

Solid State NMR
book, January 2012

Highly Efficient Ge-Rich Ge x Pb1−x Te Thermoelectric Alloys
journal, December 2009

Carrier Compensation in Germanium Telluride
journal, January 1963

Effects of Ge substitution in GeTe by Ag or Sb on the Seebeck coefficient and carrier concentration derived from ${}^{125}{Te}$ NMR
journal, January 2016

Transport properties and valence band feature of high-performance (GeTe) ₈₅ (AgSbTe ₂ ) ₁₅ thermoelectric materials
journal, January 2014

Thermodynamic and thermoelectric properties of CoFeYGe (Y = Ti, Cr) quaternary Heusler alloys: first principle calculations
journal, November 2019