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Title: Ultralow Thermal Conductivity in Diamond-Like Semiconductors: Selective Scattering of Phonons from Antisite Defects

Abstract

In this work, we discover anomalously low lattice thermal conductivity (<0.25 W/mK at 300 degrees C) in the Hg-containing quaternary diamond-like semiconductors within the Cu2IIBIVTe4 (IIB: Zn, Cd, Hg) (IV: Si, Ge, Sn) set of compositions. Using high-temperature X-ray diffraction, resonant ultrasound spectroscopy, and transport properties, we uncover the critical role of the antisite defects HgCu and CuHg on phonon transport within the Hg-containing systems. Despite the differences in chemistry between Hg and Cu, the high concentration of these antisite defects emerges from the energetic proximity of the kesterite and stannite cation motifs. Our phonon calculations reveal that heavier group IIB elements not only introduce low-lying optical modes, but the subsequent antisite defects also possess unusually strong point defect phonon scattering power. The scattering strength stems from the fundamentally different vibrational modes supported by the constituent elements (e.g., Hg and Cu). Despite the significant impact on the thermal properties, antisite defects do not negatively impact the mobility (>50 cm2/(Vs) at 300 degrees C) in Hg-containing systems, leading to predicted zT > 1.5 in Cu2HgGeTe4 and Cu2HgSnTe4 under optimized doping. In addition to introducing a potentially new p-type thermoelectric material, this work provides (1) a strategy to use the proximity ofmore » phase transitions to increase point defect phonon scattering, and (2) a means to quantify the power of a given point defect through inexpensive phonon calculations.« less

Authors:
ORCiD logo [1];  [2];  [3];  [4]; ORCiD logo [5];  [2];  [6];  [4]; ORCiD logo [5]; ORCiD logo [2];  [4]
  1. Colorado School of Mines, Golden, Colorado 80401, United States
  2. Michigan State University, East Lansing, Michigan 48824, United States
  3. University of Illinois at Urbana−Champaign, Urbana, Illinois 61820, United States; National Center for Supercomputing Applications, Urbana, Illinois 61801, United States
  4. Colorado School of Mines, Golden, Colorado 80401, United States; National Renewable Energy Laboratory, Golden, Colorado 80401, United States
  5. University of Illinois at Urbana−Champaign, Urbana, Illinois 61820, United States
  6. Northwestern University, Evanston, Illinois 60208, United States
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1456868
Report Number(s):
NREL/JA-5K00-71791
Journal ID: ISSN 0897-4756
DOE Contract Number:  
AC36-08GO28308
Resource Type:
Journal Article
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 10; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; thermal conductivity; semiconductors; phonons

Citation Formats

Ortiz, Brenden R., Peng, Wanyue, Gomes, Lídia C., Gorai, Prashun, Zhu, Taishan, Smiadak, David M., Snyder, G. Jeffrey, Stevanović, Vladan, Ertekin, Elif, Zevalkink, Alexandra, and Toberer, Eric S. Ultralow Thermal Conductivity in Diamond-Like Semiconductors: Selective Scattering of Phonons from Antisite Defects. United States: N. p., 2018. Web. doi:10.1021/acs.chemmater.8b00890.
Ortiz, Brenden R., Peng, Wanyue, Gomes, Lídia C., Gorai, Prashun, Zhu, Taishan, Smiadak, David M., Snyder, G. Jeffrey, Stevanović, Vladan, Ertekin, Elif, Zevalkink, Alexandra, & Toberer, Eric S. Ultralow Thermal Conductivity in Diamond-Like Semiconductors: Selective Scattering of Phonons from Antisite Defects. United States. doi:10.1021/acs.chemmater.8b00890.
Ortiz, Brenden R., Peng, Wanyue, Gomes, Lídia C., Gorai, Prashun, Zhu, Taishan, Smiadak, David M., Snyder, G. Jeffrey, Stevanović, Vladan, Ertekin, Elif, Zevalkink, Alexandra, and Toberer, Eric S. Wed . "Ultralow Thermal Conductivity in Diamond-Like Semiconductors: Selective Scattering of Phonons from Antisite Defects". United States. doi:10.1021/acs.chemmater.8b00890.
@article{osti_1456868,
title = {Ultralow Thermal Conductivity in Diamond-Like Semiconductors: Selective Scattering of Phonons from Antisite Defects},
author = {Ortiz, Brenden R. and Peng, Wanyue and Gomes, Lídia C. and Gorai, Prashun and Zhu, Taishan and Smiadak, David M. and Snyder, G. Jeffrey and Stevanović, Vladan and Ertekin, Elif and Zevalkink, Alexandra and Toberer, Eric S.},
abstractNote = {In this work, we discover anomalously low lattice thermal conductivity (<0.25 W/mK at 300 degrees C) in the Hg-containing quaternary diamond-like semiconductors within the Cu2IIBIVTe4 (IIB: Zn, Cd, Hg) (IV: Si, Ge, Sn) set of compositions. Using high-temperature X-ray diffraction, resonant ultrasound spectroscopy, and transport properties, we uncover the critical role of the antisite defects HgCu and CuHg on phonon transport within the Hg-containing systems. Despite the differences in chemistry between Hg and Cu, the high concentration of these antisite defects emerges from the energetic proximity of the kesterite and stannite cation motifs. Our phonon calculations reveal that heavier group IIB elements not only introduce low-lying optical modes, but the subsequent antisite defects also possess unusually strong point defect phonon scattering power. The scattering strength stems from the fundamentally different vibrational modes supported by the constituent elements (e.g., Hg and Cu). Despite the significant impact on the thermal properties, antisite defects do not negatively impact the mobility (>50 cm2/(Vs) at 300 degrees C) in Hg-containing systems, leading to predicted zT > 1.5 in Cu2HgGeTe4 and Cu2HgSnTe4 under optimized doping. In addition to introducing a potentially new p-type thermoelectric material, this work provides (1) a strategy to use the proximity of phase transitions to increase point defect phonon scattering, and (2) a means to quantify the power of a given point defect through inexpensive phonon calculations.},
doi = {10.1021/acs.chemmater.8b00890},
journal = {Chemistry of Materials},
issn = {0897-4756},
number = 10,
volume = 30,
place = {United States},
year = {2018},
month = {5}
}