金属微腔中经聚集工程设计的耐损耗强耦合
Aggregation-engineered loss-tolerant strong coupling in metallic microcavities
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中文总结 AI 辅助
该研究提出将分子聚集作为设计参数，在低品质因子银微腔中实现了耐损耗强耦合，明确了聚集态对耦合强度与发射特性的调控作用，为有机微腔的可扩展加工提供了新途径。
中文摘要 AI 辅助
室温下有机微腔中的强耦合通常需结合高品质光学谐振腔与高度有序的激子介质，这一要求限制了其可扩展性与加工灵活性。本文表明，可通过将分子聚集作为设计参数而非视为寄生效应来放宽该约束。我们制备了旋涂法加工的罗丹明6G-聚乙烯醇薄膜，将其嵌入低品质因子的银法布里-珀罗微腔中，尽管金属镜存在较大光学损耗，仍观测到清晰的角分辨反交叉现象，耦合能量高达324 meV。双激子耦合振子模型显示，这类物种的相对权重控制着集体耦合强度，且可通过染料负载量与旋涂条件进行调控。相比之下，角分辨光致发光由宽化且红移的下极化激元发射主导，这与密集分子域中形成的激基缔合物类态的弛豫过程一致。这些结果表明，分子聚集是湿加工金属微腔中耐损耗强耦合的实用设计手段，且基态聚集体与激发态激基缔合物类物种在极化激元形成与发射中发挥着不同作用。
英文摘要
Room-temperature strong coupling in organic microcavities is usually achieved by combining high-quality optical resonators with highly ordered excitonic media, a requirement that limits scalability and processing flexibility. Here we show that this constraint can be relaxed by using molecular aggregation as a design parameter rather than treating it as a parasitic effect. We realize solution-processed Rhodamine 6G-poly(vinyl alcohol) films embedded in low-quality-factor silver Fabry-Perot microcavities and demonstrate clear angle-resolved anticrossing with coupling energies up to 324 meV despite the large optical losses of the metallic mirrors. A two-exciton coupled-oscillator model shows that the relative weight of these species controls the collective coupling strength and can be tuned through dye loading and spin-coating conditions. In contrast, angle-resolved photoluminescence is dominated by a broad, red-shifted lower-polariton emission, consistent with relaxation through excimer-like states formed in densely packed molecular domains. These results identify molecular aggregation as a practical design lever for loss-tolerant strong coupling in wet-processed metallic cavities and suggest that ground-state aggregates and excited-state excimer-like species play distinct roles in polariton formation and emission.
