Ultralow thermal conductivity via weak interactions in PbSe/PbTe monolayer heterostructure for thermoelectric design

Fuente: arXiv
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Main Authors: Tan, Ruihao, Zhang, Kaiwang, Fang, Yue-Wen
Format: Preprint
Published: 2025
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author Tan, Ruihao
Zhang, Kaiwang
Fang, Yue-Wen
author_facet Tan, Ruihao
Zhang, Kaiwang
Fang, Yue-Wen
contents In this study, we systematically investigate the thermal and electronic transport properties of two-dimensional PbSe/PbTe monolayer heterostructure by combining first-principles calculations, Boltzmann transport theory, and machine learning methods. The heterostructure exhibits a unique honeycomb-like corrugated and asymmetric configuration, which significantly enhances phonon scattering. Moreover, the relatively weak interatomic interactions in PbSe/PbTe lead to the formation of anti-bonding states, resulting in strong anharmonicity and ultimately yielding ultralow lattice thermal conductivity (${κ_{\rm L}}$). In the four-phonon scattering model, the ${κ_{\rm L}}$~values along the $x$ and $y$ directions are as low as 0.37 and 0.31 W/mK, respectively. Contrary to the conventional view that long mean free path acoustic phonons dominate heat transport, we find that optical phonons contribute approximately 59\% of the lattice thermal conductivity in this heterostructure. These optical phonons exhibit large Grüneisen parameters, strong anharmonic scattering, and relatively high group velocities, thereby playing a crucial role in the low ${κ_{\rm L}}$ regime. Further analysis of thermoelectric performance shows that at a high temperature of 800 K, the heterostructure achieves an exceptional dimensionless figure of merit ($ZT$) of 5.3 along the $y$ direction, indicating outstanding thermoelectric conversion efficiency. These findings not only provide theoretical insights into the transport mechanisms of PbSe/PbTe monolayer heterostructure but also offer a practical design strategy for developing high-performance two-dimensional layered thermoelectric materials.
format Preprint
id arxiv_https___arxiv_org_abs_2507_21734
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Ultralow thermal conductivity via weak interactions in PbSe/PbTe monolayer heterostructure for thermoelectric design
Tan, Ruihao
Zhang, Kaiwang
Fang, Yue-Wen
Materials Science
Mesoscale and Nanoscale Physics
In this study, we systematically investigate the thermal and electronic transport properties of two-dimensional PbSe/PbTe monolayer heterostructure by combining first-principles calculations, Boltzmann transport theory, and machine learning methods. The heterostructure exhibits a unique honeycomb-like corrugated and asymmetric configuration, which significantly enhances phonon scattering. Moreover, the relatively weak interatomic interactions in PbSe/PbTe lead to the formation of anti-bonding states, resulting in strong anharmonicity and ultimately yielding ultralow lattice thermal conductivity (${κ_{\rm L}}$). In the four-phonon scattering model, the ${κ_{\rm L}}$~values along the $x$ and $y$ directions are as low as 0.37 and 0.31 W/mK, respectively. Contrary to the conventional view that long mean free path acoustic phonons dominate heat transport, we find that optical phonons contribute approximately 59\% of the lattice thermal conductivity in this heterostructure. These optical phonons exhibit large Grüneisen parameters, strong anharmonic scattering, and relatively high group velocities, thereby playing a crucial role in the low ${κ_{\rm L}}$ regime. Further analysis of thermoelectric performance shows that at a high temperature of 800 K, the heterostructure achieves an exceptional dimensionless figure of merit ($ZT$) of 5.3 along the $y$ direction, indicating outstanding thermoelectric conversion efficiency. These findings not only provide theoretical insights into the transport mechanisms of PbSe/PbTe monolayer heterostructure but also offer a practical design strategy for developing high-performance two-dimensional layered thermoelectric materials.
title Ultralow thermal conductivity via weak interactions in PbSe/PbTe monolayer heterostructure for thermoelectric design
topic Materials Science
Mesoscale and Nanoscale Physics
url https://arxiv.org/abs/2507.21734