TY - JOUR
T1 - In-Situ Observation of the Continuous Phase Transition in Determining the High Thermoelectric Performance of Polycrystalline Sn0.98Se
AU - Dargusch, Matthew
AU - Shi, Xiao Lei
AU - Tran, Xuan Quy
AU - Feng, Tianli
AU - Somidin, Flora
AU - Tan, Xin
AU - Liu, Weidi
AU - Jack, Kevin
AU - Venezuela, Jeffrey
AU - Maeno, Hiroshi
AU - Toriyama, Takaaki
AU - Matsumura, Syo
AU - Pantelides, Sokrates T.
AU - Chen, Zhi Gang
N1 - Funding Information:
This work was financially supported by the Australian Research Council. Z.G.C. thanks the USQ start-up grant and strategic research grant. This research was conducted as part of the international cooperative research program between the University of Queensland (UQ), Australia, and Kyushu University, Japan. X.L.S. thanks the IPRS for supporting his Ph.D. program. X.Q.T. and M.D. acknowledge the technical support of Ms. Xin Fu Tan, Ms. Flora Somidin, Ms. Shiqian Liu ,and Prof. Kazuhiro Nogita for the TEM experiments. The authors acknowledge the facilities and the scientific and technical assistance at the Centre for Microscopy and Microanalysis (the Queensland node of Microscopy Australia), UQ, Australia, and the Ultramicroscopy Research Centre, Kyushu University, Japan. Theoretical work by T.L.F. and S.T.P. is supported in part by Department of Energy grant DE-FG0209ER46554 and by the McMinn Endowment. Computations at Vanderbilt University and ORNL were performed at the National Energy Research Scientific Computing Centre (NERSC), a Department of Energy, Office of Science User Facility funded through Contract No. DE-AC02-05CH11231. Computations also used the Extreme Science and Engineering Discovery Environment (XSEDE)*%blankline%**%blankline%*
Funding Information:
This work was financially supported by the Australian Research Council. Z.G.C. thanks the USQ start-up grant and strategic research grant. This research was conducted as part of the international cooperative research program between the University of Queensland (UQ), Australia, and Kyushu University, Japan. X.L.S. thanks the IPRS for supporting his Ph.D. program. X.Q.T. and M.D. acknowledge the technical support of Ms. Xin Fu Tan, Ms. Flora Somidin, Ms. Shiqian Liu ,and Prof. Kazuhiro Nogita for the TEM experiments. The authors acknowledge the facilities and the scientific and technical assistance at the Centre for Microscopy and Microanalysis (the Queensland node of Microscopy Australia), UQ, Australia, and the Ultramicroscopy Research Centre, Kyushu University, Japan. Theoretical work by T.L.F. and S.T.P. is supported in part by Department of Energy grant DE-FG0209ER46554 and by the McMinn Endowment. Computations at Vanderbilt University and ORNL were performed at the National Energy Research Scientific Computing Centre (NERSC), a Department of Energy, Office of Science, User Facility funded through Contract No. DE-AC02-05CH11231. Computations also used the Extreme Science and Engineering Discovery Environment (XSEDE).
Publisher Copyright:
Copyright © 2019 American Chemical Society.
PY - 2019/11/7
Y1 - 2019/11/7
N2 - We report a comprehensive in-situ phase-change study on polycrystalline Sn0.98Se via high-temperature X-ray diffraction and in-situ high-voltage transmission electron microscopy from room temperature to 843 K. The results clearly demonstrate a continuous phase transition from Pnma to Cmcm starting from 573 to 843 K, rather than a sudden transition at 800 K. We also find that the thermal-conductivity rise at high temperature after the phase transition, as commonly seen in pristine SnSe, does not occur in Sn0.98Se, leading to a high thermoelectric figure of merit. Density functional theory calculations reveal the origin to be the suppression of bipolar thermal conduction in the Cmcm phase of Sn0.98Se due to the enlarged bandgap. This work fills the gap of in-situ characterization on polycrystalline Sn0.98Se and provides new insights into the outstanding thermoelectric performance of polycrystalline Sn0.98Se.
AB - We report a comprehensive in-situ phase-change study on polycrystalline Sn0.98Se via high-temperature X-ray diffraction and in-situ high-voltage transmission electron microscopy from room temperature to 843 K. The results clearly demonstrate a continuous phase transition from Pnma to Cmcm starting from 573 to 843 K, rather than a sudden transition at 800 K. We also find that the thermal-conductivity rise at high temperature after the phase transition, as commonly seen in pristine SnSe, does not occur in Sn0.98Se, leading to a high thermoelectric figure of merit. Density functional theory calculations reveal the origin to be the suppression of bipolar thermal conduction in the Cmcm phase of Sn0.98Se due to the enlarged bandgap. This work fills the gap of in-situ characterization on polycrystalline Sn0.98Se and provides new insights into the outstanding thermoelectric performance of polycrystalline Sn0.98Se.
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U2 - 10.1021/acs.jpclett.9b02818
DO - 10.1021/acs.jpclett.9b02818
M3 - Article
C2 - 31597419
AN - SCOPUS:85073879556
SN - 1948-7185
VL - 10
SP - 6512
EP - 6517
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 21
ER -