Decoupling from a Thermal Bath via Molecular Polariton Formation
Decoupling from a Thermal Bath via Molecular Polariton Formation
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通过分子极化子形成与热浴解耦
DOI：
10.1021/acs.jpclett.9b03789
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发表时间：
2020
期刊：
影响因子：
--
通讯作者：
Watanabe Kazuya
中科院分区：
文献类型：
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作者：
Takahashi Shota;Watanabe Kazuya
电子系统和环境浴之间的耦合在人工/天然分子凝聚相的激发态动力学中起着决定性的作用。虽然通常难以控制凝聚态物质中系统与热浴之间的耦合，但强的光-物质耦合可以使用极化子去耦效应来控制系统-浴耦合性质，其中激子和光子之间的相干相互作用降低了重组能量。在这里，我们表明，这种极化子去耦强烈地降低了嵌入在光学微腔中的四苯基二苯并哌喃薄膜中的电子能量的波动。利用二维电子能谱，揭示了低极化激元态的频率涨落相关函数，表明由于微腔内部的浴耦合的动力学不均匀性几乎完全消失。这是由于在腔中超过105个分子的低极化激元态的显著离域，降低了浴模的有效耦合强度。
The coupling between an electronic system and an environmental bath plays a decisive role in the excited state dynamics of artificial/natural molecular condensed phases. Although it is generally difficult to control the coupling between the system and the thermal bath in condensed matter, a strong light–matter coupling can control system–bath coupling properties using the polaron decoupling effect, in which a coherent interaction between excitons and photons reduces the reorganization energy. Here we demonstrate that this polaron decoupling strongly reduces the fluctuations in electronic energy in tetraphenyldibenzoperiflanthene thin films embedded in an optical microcavity. Using two-dimensional electronic spectroscopy, the frequency–fluctuation correlation function of the lower polariton state was revealed, showing that the dynamic inhomogeneity due to bath coupling inside the microcavity almost vanishes completely. This was attributed to a significant delocalization of the lower polariton state over 105molecules in the cavity, reducing the effective coupling strength of the bath modes.