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Title: Remarkable thermoelectric performance in BaPdS 2 via pudding-mold band structure, band convergence, and ultralow lattice thermal conductivity

Abstract

Efficient thermoelectric materials require a rare and contraindicated combination of materials properties: large electrical conductivity, large Seebeck coefficient, and low thermal conductivity. One strategy to achieve the first two properties is via low-energy electronic bands containing both flat and dispersive parts in different regions of crystal momentum space, known as a pudding-mold band structure. Here, we illustrate that BaPdS 2 successfully achieves the pudding-mold band structure for the valence band, contributing to a large p-type thermoelectric power factor, due to its anisotropic crystal structure containing zigzag chains of edge-sharing square planar PdS 4 units; large power factor is achieved for n-type doping as well due to band convergence. In addition, BaPdS 2 exhibits ultralow lattice thermal conductivity, and thus also achieves the third property, due to extremely soft and anharmonic interactions in its transverse acoustic phonon branch. We predict a remarkably large thermoelectric figure of merit, with peak values between 2 and 3 for two of the three crystallographic directions, suggesting BaPdS 2 warrants experimental investigation.

Authors:
 [1];  [1]
  1. Northwestern Univ., Evanston, IL (United States)
Publication Date:
Research Org.:
Northwestern Univ., Evanston, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1492453
Alternate Identifier(s):
OSTI ID: 1492476
Grant/Contract Number:  
SC0014520; AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 3; Journal Issue: 1; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Isaacs, Eric B., and Wolverton, Chris. Remarkable thermoelectric performance in BaPdS2 via pudding-mold band structure, band convergence, and ultralow lattice thermal conductivity. United States: N. p., 2019. Web. doi:10.1103/PhysRevMaterials.3.015403.
Isaacs, Eric B., & Wolverton, Chris. Remarkable thermoelectric performance in BaPdS2 via pudding-mold band structure, band convergence, and ultralow lattice thermal conductivity. United States. doi:10.1103/PhysRevMaterials.3.015403.
Isaacs, Eric B., and Wolverton, Chris. Mon . "Remarkable thermoelectric performance in BaPdS2 via pudding-mold band structure, band convergence, and ultralow lattice thermal conductivity". United States. doi:10.1103/PhysRevMaterials.3.015403.
@article{osti_1492453,
title = {Remarkable thermoelectric performance in BaPdS2 via pudding-mold band structure, band convergence, and ultralow lattice thermal conductivity},
author = {Isaacs, Eric B. and Wolverton, Chris},
abstractNote = {Efficient thermoelectric materials require a rare and contraindicated combination of materials properties: large electrical conductivity, large Seebeck coefficient, and low thermal conductivity. One strategy to achieve the first two properties is via low-energy electronic bands containing both flat and dispersive parts in different regions of crystal momentum space, known as a pudding-mold band structure. Here, we illustrate that BaPdS2 successfully achieves the pudding-mold band structure for the valence band, contributing to a large p-type thermoelectric power factor, due to its anisotropic crystal structure containing zigzag chains of edge-sharing square planar PdS4 units; large power factor is achieved for n-type doping as well due to band convergence. In addition, BaPdS2 exhibits ultralow lattice thermal conductivity, and thus also achieves the third property, due to extremely soft and anharmonic interactions in its transverse acoustic phonon branch. We predict a remarkably large thermoelectric figure of merit, with peak values between 2 and 3 for two of the three crystallographic directions, suggesting BaPdS2 warrants experimental investigation.},
doi = {10.1103/PhysRevMaterials.3.015403},
journal = {Physical Review Materials},
issn = {2475-9953},
number = 1,
volume = 3,
place = {United States},
year = {2019},
month = {1}
}

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