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| Autori principali: | , , , , , , , |
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| Natura: | Preprint |
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2024
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| Accesso online: | https://arxiv.org/abs/2401.16527 |
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| _version_ | 1866916207896035328 |
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| author | Yue, Jincheng Zheng, Jiongzhi Li, Junda Guo, Siqi Ren, Wenling Liu, Han Liu, Yanhui Cui, Tian |
| author_facet | Yue, Jincheng Zheng, Jiongzhi Li, Junda Guo, Siqi Ren, Wenling Liu, Han Liu, Yanhui Cui, Tian |
| contents | We thoroughly investigate the microscopic mechanisms of the thermal transport in orthorhombic \textit{o}-CsCu$_5$S$_3$ by integrating the first-principles-based self-consistent phonon calculations (SCP) with the linearized Wigner transport equation (LWTE). Our methodology takes into account contributions to phonon energy shifts and phonon scattering rates from both three- and four-phonon processes. Additionally, it incorporates the off-diagonal terms of heat flux operators to calculate the total thermal conductivity. The predicted $κ_\mathrm{L}$ with an extremely weak temperature dependence following $\sim T^{-0.33}$, in good agreement with experimental values along with the parallel to the Bridgman growth direction. Such nonstandard temperature dependence of $κ_\mathrm{L}$ can be traced back to the dual particlelike-wavelike behavior exhibited by thermal phonons. Specifically, the coexistence of the stochastic oscillation of Cs atoms and metavalent bonding among interlayer Cu-S atoms limits the particle-like phonon propagation and enhances the wave-like tunneling of phonons. Simultaneously, the electrical transport properties are determined by employing a precise momentum relaxation-time approximation (MRTA) within the framework of the linearized Boltzmann transport equation (LBTE). By properly adjusting the carrier concentration, excellent thermoelectric performance is achieved, with a maximum thermoelectric conversion efficiency of 18.4$\%$ observed at 800 K in \textit{p}-type \textit{o}-CsCu$_5$S$_3$.} Our work not only elucidates the anomalous thermal transport behavior in the copper-based chalcogenide \textit{o}-CsCu$_5$S$_3$ but also provides insights for manipulating its thermal and electronic properties for potential thermoelectric applications. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2401_16527 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Ultra-low glassy thermal conductivity and controllable, promising thermoelectric properties in crystalline o-CsCu5S3 Yue, Jincheng Zheng, Jiongzhi Li, Junda Guo, Siqi Ren, Wenling Liu, Han Liu, Yanhui Cui, Tian Materials Science We thoroughly investigate the microscopic mechanisms of the thermal transport in orthorhombic \textit{o}-CsCu$_5$S$_3$ by integrating the first-principles-based self-consistent phonon calculations (SCP) with the linearized Wigner transport equation (LWTE). Our methodology takes into account contributions to phonon energy shifts and phonon scattering rates from both three- and four-phonon processes. Additionally, it incorporates the off-diagonal terms of heat flux operators to calculate the total thermal conductivity. The predicted $κ_\mathrm{L}$ with an extremely weak temperature dependence following $\sim T^{-0.33}$, in good agreement with experimental values along with the parallel to the Bridgman growth direction. Such nonstandard temperature dependence of $κ_\mathrm{L}$ can be traced back to the dual particlelike-wavelike behavior exhibited by thermal phonons. Specifically, the coexistence of the stochastic oscillation of Cs atoms and metavalent bonding among interlayer Cu-S atoms limits the particle-like phonon propagation and enhances the wave-like tunneling of phonons. Simultaneously, the electrical transport properties are determined by employing a precise momentum relaxation-time approximation (MRTA) within the framework of the linearized Boltzmann transport equation (LBTE). By properly adjusting the carrier concentration, excellent thermoelectric performance is achieved, with a maximum thermoelectric conversion efficiency of 18.4$\%$ observed at 800 K in \textit{p}-type \textit{o}-CsCu$_5$S$_3$.} Our work not only elucidates the anomalous thermal transport behavior in the copper-based chalcogenide \textit{o}-CsCu$_5$S$_3$ but also provides insights for manipulating its thermal and electronic properties for potential thermoelectric applications. |
| title | Ultra-low glassy thermal conductivity and controllable, promising thermoelectric properties in crystalline o-CsCu5S3 |
| topic | Materials Science |
| url | https://arxiv.org/abs/2401.16527 |