Probing Anharmonic Lattice Dynamics and Thermal Transport in Layered Perovskite LiYTiO4 Anode
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| Format: | Preprint |
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2025
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| _version_ | 1866917132009209856 |
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| author | Zhang, Lin Liu, Wen He, Mingquan Huang, Jun |
| author_facet | Zhang, Lin Liu, Wen He, Mingquan Huang, Jun |
| contents | Layered perovskite lithium yttrium titanate ($\rm LiYTiO_4$) has recently emerged as a promising low-potential, ultrahigh-rate intercalation-type anode material for lithium-ion batteries; however, its lattice dynamics and thermal transport properties remain poorly understood, limiting a complete evaluation of its practical potential. Here, we combine experimental measurements with theoretical modeling to systematically investigate the anharmonic lattice dynamics and heat transport in $\rm LiYTiO_4$. We employ a neural evolution potential (NEP)-based framework that integrates the temperature-dependent effective potential method with the Wigner thermal transport (WTT) formalism, explicitly including both diagonal and off-diagonal terms of the heat-flux operator. Zero-temperature phonon calculations reveal dynamical instabilities associated with $\rm TiO_6$ octahedral rotation, which are stabilized at finite temperatures through anharmonic renormalization. Using the WTT approach with contributions from phonon propagation and coherence contributions, we predict a room-temperature lattice thermal conductivity ($κ_{\rm L}$) of 3.8 $\rm Wm^{-1}K^{-1}$ averaged over all crystal orientations, in close agreement with the measured value of 3.2 \pm 0.08 $\rm Wm^{-1}K^{-1}$ for polycrystalline samples. To further examine the possible influence of ionic motion on high-temperature thermal transport, we compute $κ_{\rm L}$ using a Green-Kubo equilibrium molecular dynamics approach based on the same NEP, which yields consistent results with both experiment and WTT predictions, confirming the negligible role of Li-ion mobility in heat conduction. Our study not only identifies the ultralow thermal conductivity of $\rm LiYTiO_4$ as a key limitation for its practical application but also establishes a reliable computational framework for studying thermal properties in battery materials. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2512_06954 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Probing Anharmonic Lattice Dynamics and Thermal Transport in Layered Perovskite LiYTiO4 Anode Zhang, Lin Liu, Wen He, Mingquan Huang, Jun Materials Science Mesoscale and Nanoscale Physics Computational Physics Layered perovskite lithium yttrium titanate ($\rm LiYTiO_4$) has recently emerged as a promising low-potential, ultrahigh-rate intercalation-type anode material for lithium-ion batteries; however, its lattice dynamics and thermal transport properties remain poorly understood, limiting a complete evaluation of its practical potential. Here, we combine experimental measurements with theoretical modeling to systematically investigate the anharmonic lattice dynamics and heat transport in $\rm LiYTiO_4$. We employ a neural evolution potential (NEP)-based framework that integrates the temperature-dependent effective potential method with the Wigner thermal transport (WTT) formalism, explicitly including both diagonal and off-diagonal terms of the heat-flux operator. Zero-temperature phonon calculations reveal dynamical instabilities associated with $\rm TiO_6$ octahedral rotation, which are stabilized at finite temperatures through anharmonic renormalization. Using the WTT approach with contributions from phonon propagation and coherence contributions, we predict a room-temperature lattice thermal conductivity ($κ_{\rm L}$) of 3.8 $\rm Wm^{-1}K^{-1}$ averaged over all crystal orientations, in close agreement with the measured value of 3.2 \pm 0.08 $\rm Wm^{-1}K^{-1}$ for polycrystalline samples. To further examine the possible influence of ionic motion on high-temperature thermal transport, we compute $κ_{\rm L}$ using a Green-Kubo equilibrium molecular dynamics approach based on the same NEP, which yields consistent results with both experiment and WTT predictions, confirming the negligible role of Li-ion mobility in heat conduction. Our study not only identifies the ultralow thermal conductivity of $\rm LiYTiO_4$ as a key limitation for its practical application but also establishes a reliable computational framework for studying thermal properties in battery materials. |
| title | Probing Anharmonic Lattice Dynamics and Thermal Transport in Layered Perovskite LiYTiO4 Anode |
| topic | Materials Science Mesoscale and Nanoscale Physics Computational Physics |
| url | https://arxiv.org/abs/2512.06954 |