George Jino, Chervy Thibault, Shalabney Atef, Devaux Eloïse, Hiura Hidefumi, Genet Cyriaque, Ebbesen Thomas W
ISIS and icFRC, Université de Strasbourg and CNRS, 67000 Strasbourg, France.
Braude College, Snunit Street 51, Karmiel 2161002, Israel.
Phys Rev Lett. 2016 Oct 7;117(15):153601. doi: 10.1103/PhysRevLett.117.153601. Epub 2016 Oct 6.
From the high vibrational dipolar strength offered by molecular liquids, we demonstrate that a molecular vibration can be ultrastrongly coupled to multiple IR cavity modes, with Rabi splittings reaching 24% of the vibration frequencies. As a proof of the ultrastrong coupling regime, our experimental data unambiguously reveal the contributions to the polaritonic dynamics coming from the antiresonant terms in the interaction energy and from the dipolar self-energy of the molecular vibrations themselves. In particular, we measure the opening of a genuine vibrational polaritonic band gap of ca. 60 meV. We also demonstrate that the multimode splitting effect defines a whole vibrational ladder of heavy polaritonic states perfectly resolved. These findings reveal the broad possibilities in the vibrational ultrastrong coupling regime which impact both the optical and the molecular properties of such coupled systems, in particular, in the context of mode-selective chemistry.
从分子液体所提供的高振动偶极强度出发，我们证明分子振动能够与多个红外腔模发生超强耦合，拉比分裂达到振动频率的24%。作为超强耦合 regime的一个证明，我们的实验数据明确揭示了相互作用能中的反共振项以及分子振动本身的偶极自能对极化激元动力学的贡献。特别地，我们测量到一个约60毫电子伏特的真正振动极化激元带隙的开启。我们还证明了多模分裂效应定义了一个完全分辨的重极化激元态的完整振动阶梯。这些发现揭示了振动超强耦合 regime中的广泛可能性，这对这类耦合系统的光学和分子性质都有影响，特别是在模式选择性化学的背景下。
