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

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.

10 pages, 5 figures, 3 tables; Supplementary Information: 12 pages, 6 figures, 6 animations

References in corpus (14)

• Photon blockade induced Mott transitions and XY spin models in coupled cavity arrays
• Quantum Computing for Molecular Biology
• Environment-assisted quantum control of a solid-state spin via coherent dark states
• Semiclassical "Divide-and-Conquer" Method for Spectroscopic Calculations of High Dimensional Molecular Systems
• Mapping Electronic Decoherence Pathways in Molecules
• Thermal stability of solitons in protein $\alpha$-helices
• Observation of biradical spin coupling through hydrogen bonds
• Using a modified version of the Tavis-Cummings-Hubbard model to simulate the formation of neutral hydrogen molecule
• Entanglement and quantum discord in the cavity QED models
• Comparing the effects of nuclear and electron spins on the formation of neutral hydrogen molecule
• Investigating entropic dynamics of multiqubit cavity QED system
• Distributed computing quantum unitary evolution
• Supercomputer model of finite-dimensional quantum electrodynamics applications
• Simulating and investigating various dynamic aspects of the ${\mathrm{H}}_2\mathrm{O}$-related hydrogen bond model