Grain Boundary Engineering for Achieving High Thermoelectric Performance in n-Type Skutterudites

Meng, Xianfu; Liu, Zihang; Cui, Bo; Qin, Dandan; Geng, Huiyuan; Cai, Wei; Fu, Liangwei; He, Jiaqing; Ren, Zhifeng; Sui, Jiehe

doi:10.1002/aenm.201602582

Title: Grain Boundary Engineering for Achieving High Thermoelectric Performance in n-Type Skutterudites

Abstract

Grain or phase boundaries play a critical role in the carrier and phonon transport in bulk thermoelectric materials. Previous investigations about controlling boundaries primarily focused on the reducing grain size or forming nanoinclusions. Herein, liquid phase compaction method is first used to fabricate the Yb‐filled CoSb ₃ with excess Sb content, which shows the typical feature of low‐angle grain boundaries with dense dislocation arrays. Seebeck coefficients show a dramatic increase via energy filtering effect through dislocation arrays with little deterioration on the carrier mobility, which significantly enhances the power factor over a broad temperature range with a high room‐temperature value around 47 μW cm ⁻² K ⁻¹ . Simultaneously, the lattice thermal conductivity could be further suppressed via scattering phonons via dense dislocation scattering. As a result, the highest average figure of merit ZT of ≈1.08 from 300 to 850 K could be realized, comparable to the best reported result of single or triple‐filled Skutterudites. This work clearly points out that low‐angle grain boundaries fabricated by liquid phase compaction method could concurrently optimize the electrical and thermal transport properties leading to an obvious enhancement of both power factor and ZT .

Authors:

Meng, Xianfu ^[1]; Liu, Zihang ^[1]; Cui, Bo ^[1]; Qin, Dandan ^[1]; Geng, Huiyuan ^[1]; Cai, Wei ^[1]; Fu, Liangwei ^[2]; He, Jiaqing ^[2]; Ren, Zhifeng ^[3]; Sui, Jiehe ^[1]

Harbin Inst. of Technology, Harbin (China)
South Univ. of Science and Technology of China, Shenzhen (China)
Univ. of Houston, Houston, TX (United States)

Publication Date:: Fri Feb 17 00:00:00 EST 2017

Research Org.:: Energy Frontier Research Centers (EFRC) (United States). Solid-State Solar-Thermal Energy Conversion Center (S3TEC)

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

OSTI Identifier:: 1388361

Alternate Identifier(s):: OSTI ID: 1398281

Grant/Contract Number:: SC0001299; FG02-09ER46577; DE‐SC0001299

Resource Type:: Accepted Manuscript

Journal Name:: Advanced Energy Materials

Additional Journal Information:: Journal Volume: 7; Journal Issue: 13; Related Information: S3TEC partners with Massachusetts Institute of Technology (lead); Boston College; Oak Ridge National Laboratory; Rensselaer Polytechnic Institute; Journal ID: ISSN 1614-6832

Publisher:: Wiley

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; solar (photovoltaic); solar (thermal); solid state lighting; phonons; thermal conductivity; thermoelectric; defects; mechanical behavior; charge transport; spin dynamics; materials and chemistry by design; optics; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing); energy filtering effect; filled Skutterudites; liquid phase compaction; low‐angle grain boundaries; phonon‐dislocation scattering

Citation Formats


                    Meng, Xianfu, Liu, Zihang, Cui, Bo, Qin, Dandan, Geng, Huiyuan, Cai, Wei, Fu, Liangwei, He, Jiaqing, Ren, Zhifeng, and Sui, Jiehe. Grain Boundary Engineering for Achieving High Thermoelectric Performance in n-Type Skutterudites.  United States: N. p., 2017. 
Web.  doi:10.1002/aenm.201602582.

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                    Meng, Xianfu, Liu, Zihang, Cui, Bo, Qin, Dandan, Geng, Huiyuan, Cai, Wei, Fu, Liangwei, He, Jiaqing, Ren, Zhifeng, & Sui, Jiehe. Grain Boundary Engineering for Achieving High Thermoelectric Performance in n-Type Skutterudites.  United States.  https://doi.org/10.1002/aenm.201602582

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                    Meng, Xianfu, Liu, Zihang, Cui, Bo, Qin, Dandan, Geng, Huiyuan, Cai, Wei, Fu, Liangwei, He, Jiaqing, Ren, Zhifeng, and Sui, Jiehe. Fri .  
"Grain Boundary Engineering for Achieving High Thermoelectric Performance in n-Type Skutterudites".  United States.  https://doi.org/10.1002/aenm.201602582.  https://www.osti.gov/servlets/purl/1388361.

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@article{osti_1388361,

  title        = {Grain Boundary Engineering for Achieving High Thermoelectric Performance in n-Type Skutterudites},

  author       = {Meng, Xianfu and Liu, Zihang and Cui, Bo and Qin, Dandan and Geng, Huiyuan and Cai, Wei and Fu, Liangwei and He, Jiaqing and Ren, Zhifeng and Sui, Jiehe},

  abstractNote = {Grain or phase boundaries play a critical role in the carrier and phonon transport in bulk thermoelectric materials. Previous investigations about controlling boundaries primarily focused on the reducing grain size or forming nanoinclusions. Herein, liquid phase compaction method is first used to fabricate the Yb‐filled CoSb 3 with excess Sb content, which shows the typical feature of low‐angle grain boundaries with dense dislocation arrays. Seebeck coefficients show a dramatic increase via energy filtering effect through dislocation arrays with little deterioration on the carrier mobility, which significantly enhances the power factor over a broad temperature range with a high room‐temperature value around 47 μW cm −2 K −1 . Simultaneously, the lattice thermal conductivity could be further suppressed via scattering phonons via dense dislocation scattering. As a result, the highest average figure of merit ZT of ≈1.08 from 300 to 850 K could be realized, comparable to the best reported result of single or triple‐filled Skutterudites. This work clearly points out that low‐angle grain boundaries fabricated by liquid phase compaction method could concurrently optimize the electrical and thermal transport properties leading to an obvious enhancement of both power factor and ZT .},

  doi          = {10.1002/aenm.201602582},

  journal      = {Advanced Energy Materials},

  number       = 13,

  volume       = 7,

  place        = {United States},

  year         = {Fri Feb 17 00:00:00 EST 2017},

  month        = {Fri Feb 17 00:00:00 EST 2017}

}

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Farahi, Nader; Stiewe, Christian; Truong, D. Y. Nhi
RSC Advances, Vol. 9, Issue 40
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New insights into the role of dislocation engineering in N-type filled skutterudite CoSb ₃
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Singh, S.; Dutta, P.; Rathi, M.
APL Materials, Vol. 7, Issue 3
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Manipulation of ionized impurity scattering for achieving high thermoelectric performance in n-type Mg ₃ Sb ₂ -based materials
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Phase-transition temperature suppression to achieve cubic GeTe and high thermoelectric performance by Bi and Mn codoping
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Advances in thermoelectrics
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Liu, Zihang; Mao, Jun; Liu, Te-Huan
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High-Efficiency Skutterudite Modules at a Low Temperature Gradient
journal, November 2019

Li, Wenjie; Stokes, David; Poudel, Bed
Energies, Vol. 12, Issue 22
DOI: 10.3390/en12224292

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Title: Grain Boundary Engineering for Achieving High Thermoelectric Performance in n-Type Skutterudites

Abstract

Citation Formats

High figure of merit in partially filled ytterbium skutterudite materials journal, January 2000

Interfaces in bulk thermoelectric materials journal, August 2009

Genomic Effects of the Quenching Process on the Microstructure and Thermoelectric Properties of Yb0.3Co4Sb12 journal, December 2014

Raising the Thermoelectric Performance of p-Type PbS with Endotaxial Nanostructuring and Valence-Band Offset Engineering Using CdS and ZnS journal, September 2012

Effects of antimony content in MgAg0.97Sbx on output power and energy conversion efficiency journal, January 2016

CRC Handbook of Thermoelectrics book, January 2017

The realization of a high thermoelectric figure of merit in Ge-substituted β-Zn4Sb3 through band structure modification journal, January 2012

On Intensifying Carrier Impurity Scattering to Enhance Thermoelectric Performance in Cr-Doped Ce y Co 4 Sb 12 journal, October 2015

Importance of high power factor in thermoelectric materials for power generation application: A perspective journal, January 2016

Complex thermoelectric materials journal, February 2008

Multiple-Filled Skutterudites: High Thermoelectric Figure of Merit through Separately Optimizing Electrical and Thermal Transports journal, May 2011

Lattice thermal conductivity of filled skutterudites: An anharmonicity perspective journal, October 2014

Current progress and future challenges in thermoelectric power generation: From materials to devices journal, April 2015

Enhanced Seebeck coefficient in silicon nanowires containing dislocations journal, July 2015

Convergence of multi-valley bands as the electronic origin of high thermoelectric performance in CoSb3 skutterudites journal, October 2015

Mechanical Properties of Skutterudites journal, August 2011

Solidification contraction-free synthesis for the Yb0.15Co4Sb12 bulk material journal, July 2007

n-type thermoelectric material Mg 2 Sn 0.75 Ge 0.25 for high power generation journal, March 2015

Enhanced thermoelectric performance of p -type filled skutterudites via the coherency strain fields from spinodal decomposition journal, October 2015

Thermoelectric Materials for Space and Automotive Power Generation journal, March 2006

A TEM study on TiB2–20%MoSi2 composite: Microstructure development and densification mechanism journal, April 2006

Size effect in thermoelectric materials journal, December 2016

Fast phase formation of double-filled p-type skutterudites by ball-milling and hot-pressing journal, January 2013

Alternative energy technologies journal, November 2001

Preparation of sintered degenerate n -type PbTe with a small grain size and its thermoelectric properties journal, September 2002

Low thermal conductivity and high thermoelectric figure of merit in n-type BaxYbyCo4Sb12 double-filled skutterudites journal, May 2008

Co-Sb (Cobalt-Antimony) journal, April 1991

Opportunities and challenges for a sustainable energy future journal, August 2012

Synthesis of YbyCo4Sb12∕Yb2O3 composites and their thermoelectric properties journal, August 2006

Model for Lattice Thermal Conductivity at Low Temperatures journal, February 1959

Filled Skutterudite Antimonides: A New Class of Thermoelectric Materials journal, May 1996

Solubility study of Yb in n -type skutterudites Yb x Co 4 Sb 12 and their enhanced thermoelectric properties journal, September 2009

Model of transport properties of thermoelectric nanocomposite materials journal, May 2009

High-performance n-type YbxCo4Sb12: from partially filled skutterudites towards composite thermoelectrics journal, July 2016

Skutterudites: Thermoelectric Materials for Automotive Applications? journal, November 2009

Sb-Yb (Antimony-Ytterbium) journal, September 2008

Thermopower enhancement in lead telluride nanostructures journal, September 2004

Temperature dependence of microstructure evolution during hot pressing of ZrB2–30 vol.% SiC composites journal, January 2016

Embedded Ag-rich nanodots in PbTe: Enhancement of thermoelectric properties through energy filtering of the carriers journal, September 2010

Enhancement in Thermoelectric Figure-Of-Merit of an N-Type Half-Heusler Compound by the Nanocomposite Approach journal, May 2011

Dense dislocation arrays embedded in grain boundaries for high-performance bulk thermoelectrics journal, April 2015

Recent advances in thermoelectric nanocomposites journal, January 2012

Cubic AgPbmSbTe2+m: Bulk Thermoelectric Materials with High Figure of Merit journal, February 2004

High-pressure synthesis of phonon-glass electron-crystal featured thermoelectric LixCo4Sb12 journal, February 2012

Electrical and thermal transport properties of Y b x Co 4 Sb 12 filled skutterudites with ultrahigh carrier concentrations journal, November 2015

High thermoelectric performance of Yb0.26Co4Sb12/yGaSb nanocomposites originating from scattering electrons of low energy journal, June 2010

Nanowires with dislocations for ultralow lattice thermal conductivity journal, January 2016

Improvement of the Efficiency of Thermoelectric Energy Conversion by Utilizing Potential Barriers journal, January 1997

Thermopower enhancement in PbTe with Pb precipitates journal, September 2005

Temperature dependent solubility of Yb in Yb–CoSb3 skutterudite and its effect on preparation, optimization and lifetime of thermoelectrics journal, March 2015

High thermoelectric power factor in Cu–Ni alloy originate from potential barrier scattering of twin boundaries journal, October 2015

Enhanced thermoelectric performance of Bi2S3 by synergistical action of bromine substitution and copper nanoparticles journal, April 2015

Enhancement of the thermoelectric performance of β-Zn4Sb3 by in situ nanostructures and minute Cd-doping journal, July 2011

Bulk nanostructured thermoelectric materials: current research and future prospects journal, January 2009

Enhancement of thermoelectric properties by energy filtering: Theoretical potential and experimental reality in nanostructured ZnSb journal, March 2016

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

Effects of edge dislocations on thermal transport in UO2 journal, March 2013

High-performance nanostructured thermoelectric materials journal, October 2010

Review: liquid phase sintering journal, January 2009

Lithium Doping to Enhance Thermoelectric Performance of MgAgSb with Weak Electron-Phonon Coupling journal, January 2016

Multiple-Filled Skutterudites: High Thermoelectric Figure of Merit through Separately Optimizing Electrical and Thermal Transports journal, January 2012

Complex thermoelectric materials book, October 2010

Alternative energy technologies journal, January 2000

Co-Sb (Cobalt-Antimony) book, January 1993

Co-Sb (Cobalt-Antimony) journal, April 2005

Enhancement of thermoelectric properties by energy filtering: Theoretical potential and experimental reality in nanostructured ZnSb text, January 2016

Synergistic Compositional-Mechanical-Thermal Effects Leading to a Record High zT in n-Type V 2 VI 3 Alloys Through Progressive Hot Deformation journal, July 2018

Mg 3+ δ Sb x Bi 2− x Family: A Promising Substitute for the State-of-the-Art n-Type Thermoelectric Materials near Room Temperature journal, December 2018

High‐Performance Solution‐Processable Flexible SnSe Nanosheet Films for Lower Grade Waste Heat Recovery journal, February 2019

Manipulation of Ni Interstitials for Realizing Large Power Factor in TiNiSn‐Based Materials journal, May 2019

Realizing Excellent Thermoelectric Performance of Sb 2 Te 3 Based Segmented Leg with a Wide Temperature Range Using One‐Step Sintering journal, December 2019

High Performance Thermoelectric Materials: Progress and Their Applications journal, November 2017

Effect of Dislocation Arrays at Grain Boundaries on Electronic Transport Properties of Bismuth Antimony Telluride: Unified Strategy for High Thermoelectric Performance journal, April 2018

Enhanced Thermoelectric and Mechanical Properties in Yb 0.3 Co 4 Sb 12 with In Situ Formed CoSi Nanoprecipitates journal, October 2019

Enhancement of Thermoelectric Performance of Sr 0.9-x Nd 0.1 Ti 0.9 Nb 0.1 O 3 Ceramics by Introducing Sr Vacancies journal, August 2018

Thermoelectric SnTe with Band Convergence, Dense Dislocations, and Interstitials through Sn Self-Compensation and Mn Alloying journal, August 2018

Simultaneous Boost of Power Factor and Figure‐of‐Merit in In–Cu Codoped SnTe journal, July 2019

High figure of merit in partially filled ytterbium skutterudite materials
journal, January 2000

Interfaces in bulk thermoelectric materials
journal, August 2009

Genomic Effects of the Quenching Process on the Microstructure and Thermoelectric Properties of Yb0.3Co4Sb12
journal, December 2014

Raising the Thermoelectric Performance of p-Type PbS with Endotaxial Nanostructuring and Valence-Band Offset Engineering Using CdS and ZnS
journal, September 2012

Effects of antimony content in MgAg0.97Sbx on output power and energy conversion efficiency
journal, January 2016

CRC Handbook of Thermoelectrics
book, January 2017

The realization of a high thermoelectric figure of merit in Ge-substituted β-Zn4Sb3 through band structure modification
journal, January 2012

On Intensifying Carrier Impurity Scattering to Enhance Thermoelectric Performance in Cr-Doped Ce _y Co ₄ Sb ₁₂
journal, October 2015

Importance of high power factor in thermoelectric materials for power generation application: A perspective
journal, January 2016

Complex thermoelectric materials
journal, February 2008

Multiple-Filled Skutterudites: High Thermoelectric Figure of Merit through Separately Optimizing Electrical and Thermal Transports
journal, May 2011

Lattice thermal conductivity of filled skutterudites: An anharmonicity perspective
journal, October 2014

Current progress and future challenges in thermoelectric power generation: From materials to devices
journal, April 2015

Enhanced Seebeck coefficient in silicon nanowires containing dislocations
journal, July 2015

Convergence of multi-valley bands as the electronic origin of high thermoelectric performance in CoSb3 skutterudites
journal, October 2015

Mechanical Properties of Skutterudites
journal, August 2011

Solidification contraction-free synthesis for the Yb0.15Co4Sb12 bulk material
journal, July 2007

n-type thermoelectric material Mg ₂ Sn _0.75 Ge _0.25 for high power generation
journal, March 2015

Enhanced thermoelectric performance of p -type filled skutterudites via the coherency strain fields from spinodal decomposition
journal, October 2015

Thermoelectric Materials for Space and Automotive Power Generation
journal, March 2006

A TEM study on TiB2–20%MoSi2 composite: Microstructure development and densification mechanism
journal, April 2006

Size effect in thermoelectric materials
journal, December 2016

Fast phase formation of double-filled p-type skutterudites by ball-milling and hot-pressing
journal, January 2013

Alternative energy technologies
journal, November 2001

Preparation of sintered degenerate n -type PbTe with a small grain size and its thermoelectric properties
journal, September 2002

Low thermal conductivity and high thermoelectric figure of merit in n-type BaxYbyCo4Sb12 double-filled skutterudites
journal, May 2008

Co-Sb (Cobalt-Antimony)
journal, April 1991

Opportunities and challenges for a sustainable energy future
journal, August 2012

Synthesis of YbyCo4Sb12∕Yb2O3 composites and their thermoelectric properties
journal, August 2006

Model for Lattice Thermal Conductivity at Low Temperatures
journal, February 1959

Filled Skutterudite Antimonides: A New Class of Thermoelectric Materials
journal, May 1996

Solubility study of Yb in $n$ -type skutterudites ${Yb}_{x} {Co}_{4} {Sb}_{12}$ and their enhanced thermoelectric properties
journal, September 2009

Model of transport properties of thermoelectric nanocomposite materials
journal, May 2009

High-performance n-type YbxCo4Sb12: from partially filled skutterudites towards composite thermoelectrics
journal, July 2016

Skutterudites: Thermoelectric Materials for Automotive Applications?
journal, November 2009

Sb-Yb (Antimony-Ytterbium)
journal, September 2008

Thermopower enhancement in lead telluride nanostructures
journal, September 2004

Temperature dependence of microstructure evolution during hot pressing of ZrB2–30 vol.% SiC composites
journal, January 2016

Embedded Ag-rich nanodots in PbTe: Enhancement of thermoelectric properties through energy filtering of the carriers
journal, September 2010

Enhancement in Thermoelectric Figure-Of-Merit of an N-Type Half-Heusler Compound by the Nanocomposite Approach
journal, May 2011

Dense dislocation arrays embedded in grain boundaries for high-performance bulk thermoelectrics
journal, April 2015

Recent advances in thermoelectric nanocomposites
journal, January 2012

Cubic AgPb_mSbTe_2+m: Bulk Thermoelectric Materials with High Figure of Merit
journal, February 2004

High-pressure synthesis of phonon-glass electron-crystal featured thermoelectric LixCo4Sb12
journal, February 2012

Electrical and thermal transport properties of Y b _x Co ₄ Sb ₁₂ filled skutterudites with ultrahigh carrier concentrations
journal, November 2015

High thermoelectric performance of Yb0.26Co4Sb12/yGaSb nanocomposites originating from scattering electrons of low energy
journal, June 2010

Nanowires with dislocations for ultralow lattice thermal conductivity
journal, January 2016

Improvement of the Efficiency of Thermoelectric Energy Conversion by Utilizing Potential Barriers
journal, January 1997

Thermopower enhancement in PbTe with Pb precipitates
journal, September 2005

Temperature dependent solubility of Yb in Yb–CoSb3 skutterudite and its effect on preparation, optimization and lifetime of thermoelectrics
journal, March 2015

High thermoelectric power factor in Cu–Ni alloy originate from potential barrier scattering of twin boundaries
journal, October 2015

Enhanced thermoelectric performance of Bi2S3 by synergistical action of bromine substitution and copper nanoparticles
journal, April 2015

Enhancement of the thermoelectric performance of β-Zn4Sb3 by in situ nanostructures and minute Cd-doping
journal, July 2011

Bulk nanostructured thermoelectric materials: current research and future prospects
journal, January 2009

Enhancement of thermoelectric properties by energy filtering: Theoretical potential and experimental reality in nanostructured ZnSb
journal, March 2016

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

Effects of edge dislocations on thermal transport in UO2
journal, March 2013

High-performance nanostructured thermoelectric materials
journal, October 2010

Review: liquid phase sintering
journal, January 2009

Lithium Doping to Enhance Thermoelectric Performance of MgAgSb with Weak Electron-Phonon Coupling
journal, January 2016

Multiple-Filled Skutterudites: High Thermoelectric Figure of Merit through Separately Optimizing Electrical and Thermal Transports
journal, January 2012

Complex thermoelectric materials
book, October 2010

Alternative energy technologies
journal, January 2000

Co-Sb (Cobalt-Antimony)
book, January 1993

Co-Sb (Cobalt-Antimony)
journal, April 2005

Enhancement of thermoelectric properties by energy filtering: Theoretical potential and experimental reality in nanostructured ZnSb
text, January 2016

Synergistic Compositional-Mechanical-Thermal Effects Leading to a Record High zT in n-Type V ₂ VI ₃ Alloys Through Progressive Hot Deformation
journal, July 2018

Mg ₃₊ _δ Sb _x Bi ₂₋ _x Family: A Promising Substitute for the State-of-the-Art n-Type Thermoelectric Materials near Room Temperature
journal, December 2018

High‐Performance Solution‐Processable Flexible SnSe Nanosheet Films for Lower Grade Waste Heat Recovery
journal, February 2019

Manipulation of Ni Interstitials for Realizing Large Power Factor in TiNiSn‐Based Materials
journal, May 2019

Realizing Excellent Thermoelectric Performance of Sb ₂ Te ₃ Based Segmented Leg with a Wide Temperature Range Using One‐Step Sintering
journal, December 2019

High Performance Thermoelectric Materials: Progress and Their Applications
journal, November 2017

Effect of Dislocation Arrays at Grain Boundaries on Electronic Transport Properties of Bismuth Antimony Telluride: Unified Strategy for High Thermoelectric Performance
journal, April 2018

Enhanced Thermoelectric and Mechanical Properties in Yb _0.3 Co ₄ Sb ₁₂ with In Situ Formed CoSi Nanoprecipitates
journal, October 2019

Enhancement of Thermoelectric Performance of Sr _0.9-x Nd _0.1 Ti _0.9 Nb _0.1 O ₃ Ceramics by Introducing Sr Vacancies
journal, August 2018

Thermoelectric SnTe with Band Convergence, Dense Dislocations, and Interstitials through Sn Self-Compensation and Mn Alloying
journal, August 2018

Simultaneous Boost of Power Factor and Figure‐of‐Merit in In–Cu Codoped SnTe
journal, July 2019

A 2D and 3D nanostructural study of naturally deformed pyrite: assessing the links between trace element mobility and defect structures
journal, August 2019

Small-molecule additives for organic thin film transistors
journal, November 2019

Charge and phonon transport in PbTe-based thermoelectric materials
journal, November 2018