Modified relaxation dynamics and coherent energy exchange in coupled vibration-cavity polaritons.
Modified relaxation dynamics and coherent energy exchange in coupled vibration-cavity polaritons.
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DOI：
10.1038/ncomms13504
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发表时间：
2016-11-22
影响因子：
16.6
通讯作者：
Owrutsky, J. C.
中科院分区：
文献类型：
--
作者：
Dunkelberger, A. D.;Spann, B. T.;Fears, K. P.;Simpkins, B. S.;Owrutsky, J. C.
将振动跃迁耦合到共振光学模式产生了从非耦合分子共振偏移的振动极化激元，并提供了一种方便的方式来修改分子振动的能量学。该方法是探索控制化学反应性的可行方法。在这项工作中，我们报告的泵浦-探测红外光谱的腔耦合的C-O伸缩带的W（CO）6和振动腔极化激元的寿命的直接测量。上极化激元的弛豫速度比非耦合振动模式快10倍。调整极化激元能量改变极化激元瞬态谱和弛豫时间。我们还观察到量子拍频，所谓的真空拉比振荡，上下振动腔极化激元之间。除了建立耦合到一个光学腔修改耦合分子的能量传递动力学，这项工作指出了系统的和预测的振动腔极化激元系统的激发态动力学的修改的可能性。振动腔极化激元是由振动模和光学腔之间的强耦合产生的混合态。在这里，作者表明，这些极化激元可以相干地交换能量，并表现出显着改变瞬态光谱和动力学相比，非耦合振动。
Coupling vibrational transitions to resonant optical modes creates vibrational polaritons shifted from the uncoupled molecular resonances and provides a convenient way to modify the energetics of molecular vibrations. This approach is a viable method to explore controlling chemical reactivity. In this work, we report pump–probe infrared spectroscopy of the cavity-coupled C–O stretching band of W(CO)6 and the direct measurement of the lifetime of a vibration-cavity polariton. The upper polariton relaxes 10 times more quickly than the uncoupled vibrational mode. Tuning the polariton energy changes the polariton transient spectra and relaxation times. We also observe quantum beats, so-called vacuum Rabi oscillations, between the upper and lower vibration-cavity polaritons. In addition to establishing that coupling to an optical cavity modifies the energy-transfer dynamics of the coupled molecules, this work points out the possibility of systematic and predictive modification of the excited-state kinetics of vibration-cavity polariton systems. Vibration-cavity polaritons are mixed states produced by strong coupling between a vibrational mode and an optical cavity. Here, the authors show that these polaritons can coherently exchange energy and exhibit drastically altered transient spectra and dynamics compared to uncoupled vibrations.
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影响因子：
8.6
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