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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Ultrafast Transmission Modulation and Recovery via Vibrational Strong Coupling
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Ultrafast Transmission Modulation and Recovery via Vibrational Strong Coupling

机译：超快传输调制和恢复通过振动强耦合

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摘要

Strong coupling between vibrational modes and cavity optical modes leads to the formation of vibration–cavity polaritons, separated by the vacuum Rabi splitting. The splitting depends on the square root of the concentration of absorbers confined in the cavity, which has important implications on the response of the coupled system after ultrafast infrared excitation. In this work, we report on solutions of W(CO)_(6) in hexane with a concentration chosen to access a regime that borders on weak coupling. Under these conditions, large fractions of the W(CO)_(6) oscillators can be excited, and the anharmonicity of the molecules leads to a commensurate reduction in the Rabi splitting. We report excitation fractions > 0.4, depending on excitation pulse intensity, and show drastic increases in transmission that can be modulated on the picosecond time scale. In comparison to previous experiments, the transient spectra that we observe are much simpler because excited-state transitions lie outside of the transmission spectrum of the cavity, thereby contributing only weakly to the spectra. We find that the Rabi splitting recovers with the characteristic vibrational relaxation lifetime and anisotropy decay of uncoupled W(CO)_(6), implying that polaritons are not directly involved in the relaxation we observe after the first few ps. The results help corroborate the model that we proposed to describe the results at higher concentrations and show that the ground-state bleach of cavity-coupled molecules has a broad, multisigned spectral response.
机译：振动模式和腔光学模式之间的强耦合导致形成振动腔极化子，由真空兔分裂分开。分裂取决于腔内限制的吸收剂浓度的平方根，这对超超速红外激发后耦合系统的响应具有重要意义。在这项工作中，我们向己烷中的W（CO）_（6）解报告，浓度选择用于进入弱耦合上边界的制度。在这些条件下，可以激发大的W（CO）_（6）振荡器的大部分，并且分子的anharconicity导致Rabi分裂的相应降低。根据激发脉冲强度，我们报告励磁分数> 0.4，并显示在皮秒上的传输中的急剧增加。与先前的实验相比，我们观察到的瞬态光谱更加简单，因为激励状态转换位于腔的透射光谱之外，从而仅弱到光谱。我们发现Rabi分裂恢复具有特征振动松弛寿命和解耦W（CO）_（6）的各向异性衰减，这意味着Pargitons不直接参与我们在前几PS后观察到的放松。结果有助于证实我们提出以更高浓度描述结果的模型，并表明腔偶联分子的地面漂白剂具有广泛的多重光谱响应。

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