Single-molecule strong coupling at room temperature in plasmonic nanocavities.
Single-molecule strong coupling at room temperature in plasmonic nanocavities.
复制标题
血浆纳米腔的室温下单分子强耦合。
DOI：
10.1038/nature17974
复制
发表时间：
2016-07-07
期刊：
影响因子：
64.8
通讯作者：
Baumberg JJ
中科院分区：
文献类型：
--
作者：
Chikkaraddy R;de Nijs B;Benz F;Barrow SJ;Scherman OA;Rosta E;Demetriadou A;Fox P;Hess O;Baumberg JJ
放置在光学腔中的发射器经历改变其对光的耦合的环境。在弱耦合制度的光提取增强，但更深刻的影响出现在单分子强耦合制度，混合轻物质状态的形式。这种腔中的单个两级发射器对于单光子来说是非线性的，形成了量子信息系统以及超低功率开关和激光器的关键构建模块。到目前为止，这种腔量子电动力学一直是低温和复杂制造的保留，严重损害了它们的使用。在这里，通过将腔体积缩放到40 nm 3以下并使用主客体化学来排列1-10个保护性隔离的亚甲基蓝分子，我们在室温和环境条件下达到了强耦合制度。来自>50个等离子体纳米腔的色散曲线显示出特征性的反交叉，10个分子的300 meV的拉比频率降低到单个分子的90 meV，与定量模型匹配。振动光谱时间序列和暗场散射光谱的统计分析提供了单分子强耦合的证据。这种用光修饰分子的方法可以改变光化学，开辟了对复杂自然过程的探索，如光合作用和操纵化学键的途径。
Emitters placed in an optical cavity experience an environment that changes their coupling to light. In the weak-coupling regime light extraction is enhanced, but more profound effects emerge in the single-molecule strong-coupling regime where mixed light-matter states form. Individual two-level emitters in such cavities become non-linear for single photons, forming key building blocks for quantum information systems as well as ultra-low power switches and lasers. Such cavity quantum electrodynamics has until now been the preserve of low temperatures and complex fabrication, severely compromising their use. Here, by scaling the cavity volume below 40 nm3 and using host-guest chemistry to align 1-10 protectively-isolated methylene-blue molecules, we reach the strong-coupling regime at room temperature and in ambient conditions. Dispersion curves from >50 plasmonic nanocavities display characteristic anticrossings, with Rabi frequencies of 300 meV for 10 molecules decreasing to 90 meV for single molecules, matching quantitative models. Statistical analysis of vibrational spectroscopy time-series and dark-field scattering spectra provide evidence of single-molecule strong coupling. This dressing of molecules with light can modify photochemistry, opening up the exploration of complex natural processes such as photosynthesis and pathways towards manipulation of chemical bonds.