AI 中文总结
该研究通过介观实时模拟揭示，分子非谐性是光子传输的关键决定因素，可通过调谐腔光子频率控制腔耦合水中的模式选择性能量传输，为相关现象提供了微观机制与解析解释。
AI 中文摘要
近期实验表明，可通过腔增强的振动能量传输来调控化学动力学。本文采用直接介观实时模拟，对光子传输与模式选择性能量传输提供微观解释，并给出振动强耦合下腔调控传输的机制原理。研究发现，分子非谐性在决定光子传输中起关键作用，当将腔模式耦合到分子系统的高度非谐模式时，会发生驱动依赖的光子局域化。我们通过将腔光子频率（正入射时）调谐至接近水的简谐（或弱非谐）弯曲模式或非谐伸缩模式，在腔耦合水中验证了这一现象。我们通过简单模型系统重现光子传输及其局域化，确认了对该现象的理解。我们还证明，模式选择性温度的扩散（通过H-O-H键角或O-H键长的方差量化）高度依赖于腔光子频率，腔光子频率可作为实现和控制模式选择性能量传输的调谐旋钮。我们也对该现象给出了简单的解析解释。研究结果凸显了真实原子系统中分子与光子自由度之间丰富的动力学相互作用。
英文摘要
Recent experiments demonstrate the modification of chemical dynamics via cavity-enhanced vibrational energy transport. Here, we provide a microscopic account of both photonic and mode-selective energy transport using direct mesoscale on-the-fly simulations and provide the mechanistic principles of cavity-modified transport under vibrational strong coupling. We find that molecular anharmonicity plays a crucial role in dictating photonic transport, and driving-dependent photonic localization occurs when coupling cavity modes to a highly anharmonic mode of the molecular system. We demonstrate this in cavity-coupled water by tuning the photon frequency (at normal incidence) close to either the harmonic (or weakly anharmonic) bending mode or the anharmonic stretching modes of water. We confirm our understanding using a simple model system by reproducing the photonic transport and its localization. We also demonstrate that the diffusion of mode-selective temperature, quantified via the variance of the H-O-H bond angle or of the O-H bond length, is highly dependent on the cavity photon frequency. We show that the cavity photon frequency can be used as a tuning knob to achieve and control mode-selective energy transport. We also provide a simple analytical understanding of this phenomenon. Our results highlight the rich dynamical interplay of molecular and photonic degrees of freedom that persist in real atomistic systems.
