Vibrational Strong Coupling in Subwavelength Nanogap Patch Antenna at the Single Resonator Level
Vibrational Strong Coupling in Subwavelength Nanogap Patch Antenna at the Single Resonator Level
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DOI：
10.1021/acs.jpclett.1c00081
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发表时间：
2021-03-23
影响因子：
5.7
通讯作者：
Ashihara, Satoshi
中科院分区：
文献类型：
--
作者：
Dayal, Govind;Morichika, Ikki;Ashihara, Satoshi
真空场与腔中分子之间的振动强耦合（VSC）在腔修饰化学反应和超灵敏振动光谱学中提供了有前途的应用。目前，为了实现变结构腔，通常采用体积较大的微腔，这限制了其在纳米尺度上的应用。在这里，我们报告的实验实现分子振动和红外光子之间的强耦合限制在深亚波长纳米间隙贴片天线腔。我们的系统表现出一个特征的反交叉色散，表明拉比分裂的108厘米（-1）在单谐振腔水平具有良好的角度不敏感性。数值模拟和理论分析定量地揭示了耦合强度取决于腔场-分子重叠积分和镜像电荷效应。单纳米间隙贴片天线水平的VSC为分子尺度化学、超灵敏生物传感器和中红外光谱范围内超低功率全光学器件的开发铺平了道路。
Vibrational strong coupling (VSC) between a vacuum field and molecules in a cavity offers promising applications in cavity-modified chemical reactions and ultrasensitive vibrational spectroscopy. At present, in order to realize VSC, bulky microcavities with large mode volume are utilized, which limits their potential applications at the nanoscale. Here, we report on the experimental realization of strong coupling between molecular vibrations and infrared photons confined within a deeply subwavelength nanogap patch antenna cavity. Our system exhibits a characteristic anticrossing dispersion, indicating a Rabi splitting of 108 cm(-1) at the single resonator level with excellent angular insensitivity. The numerical simulations and theoretical analyses quantitatively reveal that the strength of coupling depends on the cavity field-molecule overlap integral and the image charge effect. VSC at the single nanogap patch antenna level paves the way for molecular-scale chemistry, ultrasensitive biosensors, and the development of ultralow-power all-optical devices in the mid-infrared spectral range.