Ultrafast Coherence Delocalization in Real Space Simulated by Polaritons
Ultrafast Coherence Delocalization in Real Space Simulated by Polaritons
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DOI：
10.1002/adom.202102237
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发表时间：
2021-07
影响因子：
9
通讯作者：
Bo Xiang;Zimo Yang;Yi-Zhuang You;Wei Xiong
中科院分区：
文献类型：
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作者：
Bo Xiang;Zimo Yang;Yi-Zhuang You;Wei Xiong
相干离域已经在耦合腔分子极化激元平台上在时间、频率和空间域中进行了研究，通过超快二维红外高光谱成像实现。在频率和真实的空间中观察到了单向相干离域现象（在一个腔中制备的相干转移到另一个腔中）。这种方向性是由散域光子从高能模式到低能模式的耗散实现的，由Lindblad动力学描述。进一步的实验表明，当在来自不同腔的极化激元之间直接制备相干态时，只有能量上邻近的极化激元才能形成在长程环境涨落中幸存的相干态。与Lindblad动力学一起，这一结果意味着相干光通过一步机制离域，其中光子从一个腔转移到另一个腔，从而为自然和人工量子系统中的相干演化提供光。这种基于分子振动极化激元的新光学平台展示了一种结合光子和分子模式来模拟红外区域相干动力学的方法。
Coherence delocalization has been investigated on a coupled‐cavity molecular polariton platform in time, frequency, and spatial domains, enabled by ultrafast two‐dimensional infrared hyperspectral imaging. Unidirectional coherence delocalization (coherence prepared in one cavity transferred to another cavity) has been observed in frequency and real space. This directionality is enabled by the dissipation of delocalized photon from high‐energy to low‐energy modes, described by Lindblad dynamics. Further experiments show that when coherences are directly prepared between polaritons from different cavities, only energetically nearby polaritons can form coherences that survive the long‐range environmental fluctuation. Together with the Lindblad dynamics, this result implies that coherences delocalize through a one‐step mechanism where photons transfer from one cavity to another, shedding light to coherence evolution in natural and artificial quantum systems. This new optical platform based on molecular vibrational polariton thus demonstrates a way of combining photon and molecular modes to simulate coherence dynamics in the infrared regime.