Correlating exciton coherence length, localization, and its optical lineshape. I. a finite temperature solution of the Davydov soliton model

• URL: http://arxiv.org/abs/2203.05611v1
• Date: Thu, 10 Mar 2022 19:51:02 GMT
• Title: Correlating exciton coherence length, localization, and its optical lineshape. I. a finite temperature solution of the Davydov soliton model
• Authors: Eric R. Bittner and Carlos Silva and S. A. Shah and Hao Li
• Abstract summary: We present a novel approach for connecting the lineshape of a molecular exciton to finite-temperature lattice vibrations. We find that both the energy fluctuations and the localization can be described in terms of a parameter-free, reduced description.
• Score: 6.321935605877715
• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• Abstract: The lineshape of spectroscopic transitions offer windows into the local environment of a system. Here, we present a novel approach for connecting the lineshape of a molecular exciton to finite-temperature lattice vibrations within the context of the Davydov soliton model (A. S. Davydov and N. I. Kislukha, Phys. Stat. Sol. {\bf 59},465(1973)). Our results are based upon a numerically exact, self-consistent treatment of the model in which thermal effects are introduced as fluctuations about the zero-temperature localized soliton state. We find that both the energy fluctuations and the localization can be described in terms of a parameter-free, reduced description by introducing a critical temperature below which exciton self-trapping is expected to be stable. Above this temperature, the self-consistent ansatz relating the lattice distortion to the exciton wavefunction breaks down. Our theoretical model coorelates well with both experimental observations on molecular J-aggregate and resolves one of the critical issues concerning the finite temperture stability of soliton states in alpha-helices and protein peptide chains.

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