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arXiv · 2508.17089

Studying the effect of phonon coherence and inflow on hydrogen bond formation in the $[(\mathrm{H}_2\mathrm{O})_2]^m$ cluster

Hui-hui Miao
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Abstract

We propose a simplified open-quantum-system model for hydrogen-bond formation in water clusters, where each subsystem is mapped to a $\lambda$-type three-level system coupled to two effective phonon modes: a micro-vibration mode ($\Omega_{\mathrm{hyd}}$) representing the O--H stretching vibration, and a macro-displacement mode ($\Omega_{\mathrm{dist}}$) representing the intermolecular donor-acceptor motion. The $[(\mathrm{H}_2\mathrm{O})_2]^m$ cluster is studied for $m=2$ to $6$ in the incoherent case (independent phonon modes) and the coherent case (shared phonon modes). We find that phonon coherence significantly alters the dynamics. In the dissipative case, coherence induces a redistribution of steady-state populations: intermediate hydrogen-bond counts are enhanced while edge counts are suppressed -- a ``squeezing'' effect explained by the interplay of subradiant states and dark states. For $m\ge 3$, true dark states emerge, rooted in the permutation symmetry of the system. Inflow of $\Omega_{\mathrm{dist}}$ phonons promotes hydrogen bond formation, while inflow of $\Omega_{\mathrm{hyd}}$ phonons inhibits it. Our results reveal a nontrivial role of quantum coherence and dark states in hydrogen-bond dynamics, providing a foundation for extending the framework to more complex systems.

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Hui-hui Miao. 2025-08-23. Studying the effect of phonon coherence and inflow on hydrogen bond formation in the $[(\mathrm{H}_2\mathrm{O})_2]^m$ cluster. https://doi.org/10.1016/j.cjph.2026.06.034

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