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Ultrafast Transmission Modulation and Recovery via Vibrational Strong Coupling
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2018-01-02 00:00:00 , DOI: 10.1021/acs.jpca.7b10299 Adam D. Dunkelberger 1 , Roderick B. Davidson 1 , Wonmi Ahn 1 , Blake S. Simpkins 1 , Jeffrey C. Owrutsky 1
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2018-01-02 00:00:00 , DOI: 10.1021/acs.jpca.7b10299 Adam D. Dunkelberger 1 , Roderick B. Davidson 1 , Wonmi Ahn 1 , Blake S. Simpkins 1 , Jeffrey C. Owrutsky 1
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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.
中文翻译：
通过振动强耦合实现超快的传输调制和恢复
振动模和腔光学模之间的强耦合导致振动-腔极化子的形成，通过真空拉比分裂将其分开。分裂取决于腔内吸收剂浓度的平方根，这对超快红外激发后耦合系统的响应具有重要意义。在这项工作中，我们报告了W（CO）6在己烷中的溶液，其浓度经选择可进入弱耦合边界。在这些条件下，大部分的W（CO）6振荡器可以被激发，并且分子的非谐性导致拉比分裂的相应减少。我们报告激发分数> 0.4，这取决于激发脉冲强度，并显示传输的急剧增加，可以在皮秒的时间尺度上进行调制。与以前的实验相比，我们观察到的瞬态光谱要简单得多，因为激发态跃迁位于腔体的透射光谱之外，从而对光谱的贡献很小。我们发现Rabi分裂随着未耦合W（CO）6的特征振动弛豫寿命和各向异性衰减而恢复，这表明极化子并不直接参与我们在最初几ps后观察到的弛豫。结果有助于证实我们提出的用于描述较高浓度结果的模型，并表明空腔耦合分子的基态漂白剂具有宽泛的多符号光谱响应。
更新日期：2018-01-02
中文翻译：
通过振动强耦合实现超快的传输调制和恢复
振动模和腔光学模之间的强耦合导致振动-腔极化子的形成，通过真空拉比分裂将其分开。分裂取决于腔内吸收剂浓度的平方根，这对超快红外激发后耦合系统的响应具有重要意义。在这项工作中，我们报告了W（CO）6在己烷中的溶液，其浓度经选择可进入弱耦合边界。在这些条件下，大部分的W（CO）6振荡器可以被激发，并且分子的非谐性导致拉比分裂的相应减少。我们报告激发分数> 0.4，这取决于激发脉冲强度，并显示传输的急剧增加，可以在皮秒的时间尺度上进行调制。与以前的实验相比，我们观察到的瞬态光谱要简单得多，因为激发态跃迁位于腔体的透射光谱之外，从而对光谱的贡献很小。我们发现Rabi分裂随着未耦合W（CO）6的特征振动弛豫寿命和各向异性衰减而恢复，这表明极化子并不直接参与我们在最初几ps后观察到的弛豫。结果有助于证实我们提出的用于描述较高浓度结果的模型，并表明空腔耦合分子的基态漂白剂具有宽泛的多符号光谱响应。
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