Infrared Open Cavities for Strong Vibrational Coupling
Infrared Open Cavities for Strong Vibrational Coupling
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DOI：
10.1021/acs.jpclett.1c01438
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发表时间：
2021-07-22
影响因子：
5.7
通讯作者：
Chuntonov, Lev
中科院分区：
文献类型：
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作者：
Cohn, Bar;Das, Kamalika;Chuntonov, Lev
表现出窄带晶格共振的亚波长等离子体纳米颗粒的阵列被称为开放腔，因为它们能够与分子发色团中的电子激发强烈耦合。然而，这些想法在中红外光谱区域的实现受到限制。我们证明了在大面积阵列的半波长中红外天线的晶格共振的带宽的显着减少，达到200以上的谐振品质因数。通过调谐的天线晶格共振（ALR）的波长，以匹配的分子振动模式的跃迁频率，我们实现了强耦合的ALR和（聚）甲基丙烯酸甲酯（PMMA）聚合物薄膜上沉积的阵列上的羰基伸缩激发。分裂的极化激子过渡，减少其带宽低于裸分子过渡，和特征色散证实了强耦合制度。我们的结果为振动极化激元的多体相关动力学的令人兴奋的研究铺平了道路。
Arrays of subwavelength plasmonic nanoparticles exhibiting narrowband lattice resonances are referred to as open cavities because of their ability to strongly couple with electronic excitations in molecular chromophores. However, realization of these ideas in the mid-infrared spectral region has been limited. We demonstrated a dramatic reduction in the bandwidth of lattice resonances in large-area arrays of half-wavelength mid-infrared antennas, reaching resonance quality factors above 200. By tuning the wavelength of the antenna-lattice resonances (ALR) to match the transition frequency of the molecular vibrational modes, we achieved a strong coupling between the ALR and the carbonyl stretching excitation in a thin film of (poly)methyl methacrylate (PMMA) polymer deposited on the array. Splitting of the polaritonic transitions, reduction of their bandwidth below that of the bare molecular transition, and characteristic dispersion confirmed the strong coupling regime. Our results pave the way for exciting research on the many-body correlated dynamics of vibrational polaritons.