Understanding the evolution of anomalous anharmonicity in Bi2Te3-xSex

Tian, Yao; Jia, Shuang; Cava, R. J.; Zhong, Ruidan; Schneeloch, John; Gu, Genda; Burch, Kenneth S.

doi:10.1103/PhysRevB.95.094104

Title: Understanding the evolution of anomalous anharmonicity in ${Bi}_{2} {Te}_{3 - x} {Se}_{x}$

Abstract

The anharmonic effect in thermoelectrics has been a central topic for decades in both condensed matter physics and material science. However, despite the long-believed strong and complex anharmonicity in the Bi₂Te_3-xSe_x series, experimental verification of anharmonicity and its evolution with doping remains elusive. We fill this important gap with high-resolution, temperature-dependent Raman spectroscopy in high-quality single crystals of Bi₂Te, Bi₂Te₂Se , and Bi₂Se₃ over the temperature range from 4 to 293 K. Klemens's model was employed to explain the renormalization of their phonon linewidths. The phonon energies of Bi₂Se₃ and Bi₂Te₃ are analyzed in detail from three aspects: lattice expansion, cubic anharmonicity, and quartic anharmonicity. For the first time, we explain the evolution of anharmonicity in various phonon modes and across the series. Lastly, in particular, we find that the interplay between cubic and quartic anharmonicity is governed by their distinct dependence on the phonon density of states, providing insights into anomalous anharmonicity designing of new thermoelectrics.

Authors:

Tian, Yao ^[1]; Jia, Shuang ^[2]; Cava, R. J. ^[2]; Zhong, Ruidan ^[3]; Schneeloch, John ^[3]; Gu, Genda ^[3]; Burch, Kenneth S. ^[4]

Univ. of Toronto, ON (Canada). Dept. of Physics & Inst. of Optical Sciences
Princeton Univ., NJ (United States). Dept. of Chemistry
Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter Physics and Materials Science Dept.
Boston College, Chestnut Hill, MA (United States). Dept. of Physics

Publication Date:: Wed Mar 08 00:00:00 EST 2017

Research Org.:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

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

OSTI Identifier:: 1372431

Report Number(s):: BNL-113904-2017-JA
Journal ID: ISSN 2469-9950; PRBMDO; R&D Project: PO010; KC0201060; TRN: US1702667

Grant/Contract Number:: SC0012704; DMR-1420541; DMR-1410846

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review. B

Additional Journal Information:: Journal Volume: 95; Journal Issue: 9; 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; 36 MATERIALS SCIENCE; Lattice dynamics; Phonons; Optical phonons

Citation Formats


                    Tian, Yao, Jia, Shuang, Cava, R. J., Zhong, Ruidan, Schneeloch, John, Gu, Genda, and Burch, Kenneth S. Understanding the evolution of anomalous anharmonicity in Bi2Te3-xSex.  United States: N. p., 2017. 
Web.  doi:10.1103/PhysRevB.95.094104.

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                    Tian, Yao, Jia, Shuang, Cava, R. J., Zhong, Ruidan, Schneeloch, John, Gu, Genda, & Burch, Kenneth S. Understanding the evolution of anomalous anharmonicity in Bi2Te3-xSex.  United States.  https://doi.org/10.1103/PhysRevB.95.094104

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                    Tian, Yao, Jia, Shuang, Cava, R. J., Zhong, Ruidan, Schneeloch, John, Gu, Genda, and Burch, Kenneth S. Wed .  
"Understanding the evolution of anomalous anharmonicity in Bi2Te3-xSex".  United States.  https://doi.org/10.1103/PhysRevB.95.094104.  https://www.osti.gov/servlets/purl/1372431.

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@article{osti_1372431,

  title        = {Understanding the evolution of anomalous anharmonicity in Bi2Te3-xSex},

  author       = {Tian, Yao and Jia, Shuang and Cava, R. J. and Zhong, Ruidan and Schneeloch, John and Gu, Genda and Burch, Kenneth S.},

  abstractNote = {The anharmonic effect in thermoelectrics has been a central topic for decades in both condensed matter physics and material science. However, despite the long-believed strong and complex anharmonicity in the Bi2Te3-xSex series, experimental verification of anharmonicity and its evolution with doping remains elusive. We fill this important gap with high-resolution, temperature-dependent Raman spectroscopy in high-quality single crystals of Bi2Te, Bi2Te2Se , and Bi2Se3 over the temperature range from 4 to 293 K. Klemens's model was employed to explain the renormalization of their phonon linewidths. The phonon energies of Bi2Se3 and Bi2Te3 are analyzed in detail from three aspects: lattice expansion, cubic anharmonicity, and quartic anharmonicity. For the first time, we explain the evolution of anharmonicity in various phonon modes and across the series. Lastly, in particular, we find that the interplay between cubic and quartic anharmonicity is governed by their distinct dependence on the phonon density of states, providing insights into anomalous anharmonicity designing of new thermoelectrics.},

  doi          = {10.1103/PhysRevB.95.094104},

  journal      = {Physical Review. B},

  number       = 9,

  volume       = 95,

  place        = {United States},

  year         = {Wed Mar 08 00:00:00 EST 2017},

  month        = {Wed Mar 08 00:00:00 EST 2017}

}

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Works referencing / citing this record:

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Mode Grüneisen parameters of an efficient thermoelectric half-Heusler
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Coherent phonons in a ${Bi}_{2} {Se}_{3}$ film generated by an intense single-cycle THz pulse
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