Dissipative Dynamics of Polarons and Excitons in Open Quantum Systems Using the Multiparticle Holstein Hamiltonian                                                                          

Polarons and excitons are key quasiparticles that govern the electronic and optical properties of organic semiconducting polymers and molecular aggregates. Understanding the dissipative dynamics of polarons (and excitons) is crucial for elucidating charge transport and coherence loss in organic semiconductors and molecular aggregates. In this work, we investigate the time evolution of polarons (and excitons) in one-dimensional molecular chains coupled to a dissipative quantum bath modeled as a collection of harmonic oscillators, following the Holstein-style vibronic Hamiltonians diagonalized using a multiparticle basis set [1,2]. A unitary time-evolution approach captures the interplay between electronic coupling, vibronic correlations, and environmental decoherence [3-5]. The reduced density matrix formalism is employed to quantify coherence loss via subsystem purity, providing insight into how both the sign and magnitude of intersite coupling affect decoherence rates. Our simulations reveal that H-aggregates (positive coupling) exhibit faster purity decay compared to J-aggregates (negative coupling), consistent with experimental trends and theoretical predictions [6,7]. This study provides new insights into the quantum-to-classical transition and coherence control in organic quantum materials and molecular excitonic systems [8,9].

References:

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[6] F. C. Spano, Annu. Rev. Phys. Chem. 57, 217–243 (2006).

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[8] S. Jang, M. D. Newton and R. J. Silbey, J. Chem. Phys. 118, 9312 (2003).

[9] A. W. Chin, J. Prior, R. Rosenbach, F. Caycedo-Soler, S. F. Huelga and M. B. Plenio, Nat. Phys. 9, 113–118 (2013).