Conductivity of an electron coupled to anharmonic phonons
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arXiv
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| Format: | Preprint |
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2022
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| _version_ | 1866915507041468416 |
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| author | Fetherolf, Jonathan H. Shih, Petra Berkelbach, Timothy C. |
| author_facet | Fetherolf, Jonathan H. Shih, Petra Berkelbach, Timothy C. |
| contents | We study the impact of phonon anharmonicity on the electronic dynamics of soft materials using a nonperturbative quantum-classical approach. The method is applied to a one-dimensional model of doped organic semiconductors with low-frequency intermolecular lattice phonons. We find that anharmonicity that leads to phonon hardening increases the mobility and anharmonicity that leads to phonon softening decreases the mobility. We also test various approximations, including the use of adiabatic phonon disorder, an effective harmonic model with temperature-dependent frequencies, and the Boltzmann transport equation with second-order perturbation theory scattering rates. Overall, we find surprisingly good agreement between all methods but that accounting for phonon anharmonicity is important for accurate prediction of electronic transport including both quantitative mobility values and their qualitative temperature dependence. For the model studied, phonon lifetime effects have relatively little impact on carrier transport, but the effective frequency shift due to anharmonicity is essential. In cases with highly asymmetric, non-Gaussian disorder, an effective harmonic model cannot quantitatively reproduce mobilities or finite-frequency conductivity, and this is especially true for acoustic phonons. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2205_09811 |
| institution | arXiv |
| publishDate | 2022 |
| record_format | arxiv |
| spellingShingle | Conductivity of an electron coupled to anharmonic phonons Fetherolf, Jonathan H. Shih, Petra Berkelbach, Timothy C. Materials Science Chemical Physics We study the impact of phonon anharmonicity on the electronic dynamics of soft materials using a nonperturbative quantum-classical approach. The method is applied to a one-dimensional model of doped organic semiconductors with low-frequency intermolecular lattice phonons. We find that anharmonicity that leads to phonon hardening increases the mobility and anharmonicity that leads to phonon softening decreases the mobility. We also test various approximations, including the use of adiabatic phonon disorder, an effective harmonic model with temperature-dependent frequencies, and the Boltzmann transport equation with second-order perturbation theory scattering rates. Overall, we find surprisingly good agreement between all methods but that accounting for phonon anharmonicity is important for accurate prediction of electronic transport including both quantitative mobility values and their qualitative temperature dependence. For the model studied, phonon lifetime effects have relatively little impact on carrier transport, but the effective frequency shift due to anharmonicity is essential. In cases with highly asymmetric, non-Gaussian disorder, an effective harmonic model cannot quantitatively reproduce mobilities or finite-frequency conductivity, and this is especially true for acoustic phonons. |
| title | Conductivity of an electron coupled to anharmonic phonons |
| topic | Materials Science Chemical Physics |
| url | https://arxiv.org/abs/2205.09811 |