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| Main Authors: | , , , , , , , , , , |
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| Format: | Preprint |
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2025
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| Subjects: | |
| Online Access: | https://arxiv.org/abs/2510.07097 |
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| _version_ | 1866911198518181888 |
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| author | Liu, F. Yang, Z. Luo, Y. Guo, S. Zhang, C. Choo, S. Xu, X. Wang, X. Mkhoyan, K. A. Bernardi, M. Jalan, B. |
| author_facet | Liu, F. Yang, Z. Luo, Y. Guo, S. Zhang, C. Choo, S. Xu, X. Wang, X. Mkhoyan, K. A. Bernardi, M. Jalan, B. |
| contents | In complex oxides, charge carriers often couple strongly with lattice vibrations to form polarons-entangled electron-phonon quasiparticles whose transport properties remain difficult to characterize. Experimental access to intrinsic polaronic transport requires ultraclean samples, while theoretical descriptions demand methods beyond low-order perturbation theory. Here, we combine the growth of high-quality oxygen-vacancy-doped anatase TiO2 films by hybrid molecular beam epitaxy (MBE) with a first-principles electron-phonon diagrammatic Monte Carlo (FEP-DMC) framework recently developed for accurate polaron predictions. Our films exhibit record-high electron mobility for anatase TiO2, in excellent agreement with FEP-DMC calculations conducted prior to experiment, which predict a room-temperature mobility of 45 +/- 15 cm2V-1s-1 and a mobility-temperature scaling of mobility proportional to T^(-1.9 +/- 0.077). Microscopic analysis using scanning transmission electron microscopy and X-ray photoelectron spectroscopy reveals the role of oxygen vacancies in modulating transport at lower temperatures. FEP-DMC further provides quantitative insight into polaron formation energy, phonon cloud distribution, lattice distortion around the polaron, and the polaronic contribution to mobility. Together, these results establish a predictive theory-experiment workflow to characterize polarons and provide a microscopic understanding of large-polaron transport in anatase TiO2, with broader implications for complex oxides and other polaronic materials. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2510_07097 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Understanding Polaronic Transport in Anatase TiO2 Films by Combining Precise Synthesis and First-Principles Many-Body Theory Liu, F. Yang, Z. Luo, Y. Guo, S. Zhang, C. Choo, S. Xu, X. Wang, X. Mkhoyan, K. A. Bernardi, M. Jalan, B. Materials Science In complex oxides, charge carriers often couple strongly with lattice vibrations to form polarons-entangled electron-phonon quasiparticles whose transport properties remain difficult to characterize. Experimental access to intrinsic polaronic transport requires ultraclean samples, while theoretical descriptions demand methods beyond low-order perturbation theory. Here, we combine the growth of high-quality oxygen-vacancy-doped anatase TiO2 films by hybrid molecular beam epitaxy (MBE) with a first-principles electron-phonon diagrammatic Monte Carlo (FEP-DMC) framework recently developed for accurate polaron predictions. Our films exhibit record-high electron mobility for anatase TiO2, in excellent agreement with FEP-DMC calculations conducted prior to experiment, which predict a room-temperature mobility of 45 +/- 15 cm2V-1s-1 and a mobility-temperature scaling of mobility proportional to T^(-1.9 +/- 0.077). Microscopic analysis using scanning transmission electron microscopy and X-ray photoelectron spectroscopy reveals the role of oxygen vacancies in modulating transport at lower temperatures. FEP-DMC further provides quantitative insight into polaron formation energy, phonon cloud distribution, lattice distortion around the polaron, and the polaronic contribution to mobility. Together, these results establish a predictive theory-experiment workflow to characterize polarons and provide a microscopic understanding of large-polaron transport in anatase TiO2, with broader implications for complex oxides and other polaronic materials. |
| title | Understanding Polaronic Transport in Anatase TiO2 Films by Combining Precise Synthesis and First-Principles Many-Body Theory |
| topic | Materials Science |
| url | https://arxiv.org/abs/2510.07097 |