AI 中文总结
本研究在无腔环境下发现Mo₂分子谐振器中Mo-Mo伸缩模式与局域受限拉曼场强耦合，为金属-金属键内的振动-场耦合和光场限制提供了光谱学证据。
AI 中文摘要
将光场限制在分子尺寸内是纳米光子学和分子量子光学的核心目标。本研究报道了四重键合的二钼配合物中Mo-Mo伸缩振动与局域受限拉曼散射场的强耦合。在无腔的环境条件下，二钼甲脒配合物Mo₂(DAniF)₄和Mo₂(DTolF)₄表现出拉比型分裂、莫洛（Mollow）型边带以及以400 cm⁻¹的Mo-Mo伸缩频率为中心的高阶拉曼特征，表明形成了修饰振动场态。边带相对于共振的位移遵循光子数依赖关系Ωₙ=Ω√νₙ，与杰恩斯-卡明斯（Jaynes Cummings）型耦合一致，而强位移的拉曼特征被归为同一修饰态阶梯内的跳跃跃迁。相比之下，极化率较低的Mo₂(O₂CCH₃)₄配合物仅表现出单一的Mo-Mo伸缩带。对已报道的炔基Mo₂配合物的共振拉曼光谱的重新分析进一步支持了这一耦合框架。这些结果表明，Mo₂单元同时作为拉曼活性振荡器和分子谐振器，支撑、限制并增强局域产生的散射场，为化学键定义的金属-金属键内的振动-场耦合和光场限制提供了光谱学证据。
英文摘要
Confining optical fields to molecular dimensions is a central objective in nanophotonics and molecular quantum optics. Here, we report strong coupling of the Mo Mo stretching vibration to a locally confined Raman scattering field in quadruply bonded dimolybdenum complexes. Under ambient, cavity-free conditions, the dimolybdenum formamidinate complexes Mo2(DAniF)4 and Mo2(DTolF)4 exhibit Rabi-type splitting, Mollow-type sidebands, and higher-order Raman features centered near the Mo Mo stretching frequency of 400 cm-1, indicating formation of dressed vibration field states. The sideband displacements from the resonance follow the photon-number-dependent relation Ωn=Ωνn, consistent with Jaynes Cummings-type coupling, while strongly displaced Raman features are assigned to leapfrog transitions within the same dressed-state ladder. In contrast, the less polarizable Mo2(O2CCH3)4 complex exhibits essentially a single Mo Mo stretching band. Reanalysis of reported resonance Raman spectra of an alkynyl Mo2 complex further supports this coupling framework. These results suggest that the Mo2 unit simultaneously serves as the Raman active oscillator and the molecular resonator that supports, confines, and enhances the locally generated scattering field, providing spectroscopic evidence for vibration field coupling and optical-field confinement within a chemically defined metal metal bond.
