A coarse-grained description of anharmonic lattice environments affecting the quantum dynamics of charge carriers

• URL: http://arxiv.org/abs/2404.02459v1
• Date: Wed, 3 Apr 2024 05:02:46 GMT
• Title: A coarse-grained description of anharmonic lattice environments affecting the quantum dynamics of charge carriers
• Authors: Kuniyuki Miwa, Souichi Sakamoto, Ken Funo, Akihito Ishizaki,
• Abstract summary: Lattice softness has a significant impact on charge carrier dynamics in condensed matter systems. Recent studies suggest the contribution of quartic anharmonicity of the lattice vibrations. We present a theory that describes quantum dynamics under the influence of an environment with two stable states.
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• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• Abstract: Lattice softness has a significant impact on charge carrier dynamics in condensed matter systems, contributing to the emergence of various properties and functions. Examples include the remarkable carrier lifetimes and defect tolerances of hybrid organic-inorganic perovskites. Recent studies suggest the contribution of quartic anharmonicity of the lattice vibrations. The quartic anharmonicity can be discussed with a double-well potential, and the transition between the two minima can be coarse-grained as a two-state jump stochastic process. Such a stochastic approach is typically employed to describe dynamic fluctuations introduced into a system by two-state transitions in the surroundings. To investigate charge transport in materials, however, it is crucial to describe not only the fluctuations but also the dynamic lattice distortion associated with charge transport. Therefore, there is a need for a theory to describe the charge carrier dynamics proceeding alongside the lattice distortion dynamics. In this study, we present a theory that describes quantum dynamics under the influence of an environment with two stable states, termed a bistable environment. The theory describes the effects of fluctuations and dissipation induced from the bistable environment in a reasonable manner, and the effects exhibit a different temperature dependence than the widely employed Gaussian environment. The physical implication of this temperature dependence is provided in terms of the environmental dynamics. The results of this study are expected to provide a step forward in describing charge carrier dynamics in materials with lattice softness and pronounced lattice anharmonicity, e.g., hybrid organic-inorganic perovskites. Moreover, these findings represent an advancement in our understanding of and capacity to predict and control the physical properties and functions of these materials.

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