论文标题

北极星反应在分子振动的布朗耗散存在下

Polariton response in the presence of Brownian dissipation from molecular vibrations

论文作者

Kansanen, Kalle S. U., Toppari, J. Jussi, Heikkilä, Tero T.

论文摘要

我们研究了由于有限的空腔线宽和分子振动而导致的主要耗散通道,研究了一个腔场的站点驱动系统的弹性响应。我们表明,经常使用的耦合振荡器模型未能描述这种响应,尤其是由于分子对其振动的非lorentzian耗散。该故障的签名是极化峰分裂的温度相关最小点,最小拆分处的北极峰高度不均匀,以及极化峰的不对称形状,即使在实验访问的“零数据”点也是如此。使用一个相当通用但代表性的分子振动模型,我们根据温度,分子stokes偏移和振动频率以及狂犬分裂的大小来预测各种条件下的极化响应。我们的结果可以用作对试图“证明”结果的实验​​的理智检查,源自强耦合,例如真空增强化学反应速率。

We study the elastic response of a stationarily driven system of a cavity field strongly coupled with molecular excitons, taking into account the main dissipation channels due to the finite cavity linewidth and molecular vibrations. We show that the frequently used coupled oscillator model fails in describing this response especially due to the non-Lorentzian dissipation of the molecules to their vibrations. Signatures of this failure are the temperature dependent minimum point of the polariton peak splitting, uneven polariton peak height at the minimum splitting, and the asymmetric shape of the polariton peaks even at the experimentally accessed "zero-detuning" point. Using a rather generic yet representative model of molecular vibrations, we predict the polariton response in various conditions, depending on the temperature, molecular Stokes shift and vibration frequencies, and the size of the Rabi splitting. Our results can be used as a sanity check of the experiments trying to "prove" results originating from strong coupling, such as vacuum-enhanced chemical reaction rate.

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