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Zintl phase Mg 3 Sb 2 , which has ultra-low thermal conductivity, is a promising anisotropic thermoelectric material. It is worth noting that the prediction and experiment value of lattice thermal conductivity ( κ ) maintain a remarkable difference, troubling the development and application. Thus, we firstly included the four-phonon scattering processes effect and performed the Peierls–Boltzmann transport equation (PBTE) combined with the first-principles lattice dynamics to study the lattice thermal transport in Mg 3 Sb 2 . The results showed that our theoretically predicted κ is consistent with the experimentally measured, breaking through the limitations of the traditional calculation methods. The prominent four-phonon scatterings decreased phonon lifetime, leading to the κ of Mg 3 Sb 2 at 300 K from 2.45 (2.58) W m −1 K −1 to 1.94 (2.19) W m −1 K −1 along the in (cross)-plane directions, respectively, and calculation accuracy increased by 20%. This study successfully explains the lattice thermal transport behind mechanism in Mg 3 Sb 2 and implies guidance to advance the prediction accuracy of thermoelectric materials.
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Electric field tuned anisotropic to isotropic thermal transport transition in monolayer borophene without altering its atomic structure
Thermal anisotropy/isotropy is one of the fundamental thermal transport properties of materials and plays a critical role in a wide range of practical applications. Manipulation of anisotropic to isotropic thermal transport or vice versa is in increasing demand. However, almost all the existing approaches for tuning anisotropy or isotropy focus on structure engineering or materials processing, which is time and cost consuming and irreversible, while little progress has been made with an intact, robust, and reversible method. Motivated by the inherent relationship between interatomic interaction mediated phonon transport and electronic charges, we comprehensively investigate the effect of external electric field on thermal transport in two-dimensional (2D) borophene by performing first-principles calculations along with the phonon Boltzmann transport equation. Under external electric field, the lattice thermal conductivity of borophene in both in-plane directions first increases significantly to peak values with the maximum augmentation factor of 2.82, and the intrinsic anisotropy (the ratio of thermal conductivity along two in-plane directions) is boosted to the highest value of 2.13. After that, thermal conductivities drop down steeply and anisotropy exhibits oscillating decay. With the electric field increasing to 0.4 V Å −1 , the thermal conductivity is dramatically suppressed to 1/40 of the original value at no electric field. More interestingly, the anisotropy of the thermal conductivity decreases to the minimum value of 1.25, showing almost isotropic thermal transport. Such abnormal anisotropic to isotropic thermal transport transition stems from the large enhancement and suppression of phonon lifetime at moderate and high strength of electric field, respectively, and acts as an amplifying or reducing factor to the thermal conductivity. We further explain the tunability of phonon lifetime of the dominant acoustic mode by an electron localization function. By comparing the electric field-modulated thermal conductivity of borophene with the dielectric constant, it is found that the screened potential resulting from the redistributed charge density leads to phonon renormalization and the modulation of phonon anharmonicity and anisotropy through electric field. Our study paves the way for robust tuning of anisotropy of phonon transport in materials by applying intact, robust, and reversible external electric field without altering their atomic structure and would have a significant impact on emerging applications, such as thermal management of nanoelectronics and thermoelectric energy conversion.
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- PAR ID:
- 10230377
- Date Published:
- Journal Name:
- Nanoscale
- Volume:
- 12
- Issue:
- 37
- ISSN:
- 2040-3364
- Page Range / eLocation ID:
- 19178 to 19190
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
-
Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1039/d0nr03273e
