AI 中文总结
本研究利用稳态吸收等光谱技术，在室温下发现Mo2配合物中存在由极化激元散射驱动的强模式选择性激子-光子耦合，为极化激元化学提供了化学明确的分子量子系统平台。
AI 中文摘要
具有四重键的Mo2配合物是一种独特的分子平台，在室温下，其中多个二能级电子跃迁会与量子化散射模式相互作用。本文表明，在Mo2配合物中，本征光子模式会选择性地与分子激发态耦合，包括特征性的δ-δ*跃迁、配体到金属的电荷转移（LMCT）跃迁以及金属到配体的电荷转移（MLCT）跃迁，从而形成分辨清晰的激子-光子杂化态。结合稳态吸收、共振荧光和超快瞬态光谱技术，我们确定了与这些电子流形相关的不同极化激元分支，其耦合强度涵盖强耦合和超强耦合区域（g/ω0高达0.1）。模式选择性耦合导致单氧化配合物出现显著的光谱重组，包括稳态光谱中出现吸收谷和相关共振的边带、光致发光光谱中出现特征性极化激元发射，以及瞬态光谱中出现长寿命的低能杂化态。这些结果支持了如下观点：Mo2单元可作为集成分子谐振器，其本征量子化场可选择性驱动并重新分布分子激发态。本研究强化了将键合双金属配合物视为室温分子量子系统的新兴观点，并为探索极化激元化学提供了化学明确的平台。
英文摘要
Quadruply bonded Mo2 complexes provide a distinctive molecular platform in which multiple two-level electronic transitions interact with quantized scattering modes under ambient conditions. Here we show that, in the Mo2 complexes, the intrinsic photonic modes selectively couple to molecular excitations, including the characteristic delta-delta(star), ligand to metal charge transfer (LMCT) and metal to ligand charge transfer (MLCT) transitions, to form the well-resolved exciton-photon hybrid states. By combining steady-state absorption, resonance fluorescence, and ultrafast transient spectroscopies, we identify distinct polaritonic branches associated with these electronic manifolds, with coupling strengths spanning the strong and ultrastrong regimes (g/omega0 up to 0.1). Mode-selective coupling accounts for the pronounced spectral reorganization for the singly oxidized complexes, including the emergence of absorption valleys and sidebands of the associated resonances in the steady-state spectra, characteristic polaritonic emissions in the photoluminescence spectra, and long-lived low-energy hybrid states in the transient spectra. These results support the picture that the Mo2 unit functions as an integrated molecular resonator whose intrinsic quantized field selectively drives and redistributes molecular excitations. This work strengthens the emerging view of bonded dimetal complexes as ambient-condition molecular quantum systems and provides a chemically defined platform for exploring polaritonic chemistry.
