Long-Range Non-Equilibrium Coherent Tunneling Induced by Fractional Vibronic Resonances

Abstract

We study the influence of a linear energy bias on a non-equilibrium excitation on a chain of molecules coupled to local phonons (a tilted Holstein model) using both a random-walk rate kernel theory and a nonperturbative, massively parallelized adaptive-basis algorithm. We uncover structured and discrete vibronic resonance behavior fundamentally different from both linear response theory and homogeneous polaron dynamics. Remarkably, resonance between the phonon energy $\hslash \omega$ and the bias ${\delta }_{\epsilon }$ occurs not only at integer but also fractional ratios ${\delta }_{\epsilon }/(\hslash \omega )=\frac{m}{n}$, which effect long-range $n$-bond $m$-phonon tunneling. These observations are also reproduced in a model calculation of a recently demonstrated Cy3 system. Potential applications range from molecular electronics to optical lattices and artificial light harvesting via vibronic engineering of coherent quantum transport.

Added results on Cy3 model system and streamlined presentation

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Cited by in corpus (6)

• Understanding the Energy Gap Law under Vibrational Strong Coupling
• Spectral and thermodynamic properties of the Holstein polaron: Hierarchical equations of motion approach
• Random Walk in Random Permutation Set Theory
• Disordered ensembles of strongly coupled single-molecule plasmonic picocavities as nonlinear optical metamaterials
• Long-Range Quantum Tunneling via Matter Wave
• paces: Parallelized Application of Co-Evolving Subspaces, a method for computing quantum dynamics on GPUs