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基于亚甲基蓝（Methylene Blue，MB）--银纳米腔中的双拉比分裂实验，建立了MB分子团簇和双金属纳米粒子结构模型，在密度矩阵理论框架下，应用偶极近似，计算了MB分子团簇与双金属纳米粒子形成的杂化态的耦合动力学过程，研究了多激子态--等离激元相互作用下的多模耦合效应，得到了与实验定性一致的结果。通过短脉冲激发，在更大的激发频域下研究激子态和等离激元的耦合态。论文探讨了激子退相干速率和分子间距离对耦合过程的影响、分子与等离激元的耦合强度随激子退相干时间缩短而增强的现象，由于团簇内离域激子与等离激元耦合相互作用，复合体系内可以产生更多杂化能级，使得光学响应峰发生相应变化。通过对分子团簇与金属纳米结构的多模耦合的机理研究，为设计高效光捕获和转换材料提供了理论思路。Based on the double Rabi splitting experiment in the methylene blue (MB) - silver nanocavity, a structural model of MB molecular clusters and dual metal nanoparticles was established. Using the density matrix theory framework and dipole approximation, the coupling dynamics of the hybrid state formed by MB molecular clusters and dual metal nanoparticles were calculated. The multi-mode coupling effect under the interaction between multi-exciton states and plasmons was studied, and qualitatively consistent results with the experiment were obtained. By short pulse excitation, the coupling states of exciton states and plasmons are studied in a larger excitation frequency domain. The paper explores the effects of exciton decoherence rate and intermolecular distance on the coupling process, as well as the phenomenon that the coupling strength between molecules and plasmons increases with the shortening of exciton decoherence time. Due to the coupling interaction between delocalized excitons and plasmons within the cluster, more hybrid energy levels can be generated in the composite system, resulting in corresponding changes in the optical response peak. By studying the mechanism of multi-mode coupling between molecular clusters and metal nanostructures, theoretical ideas have been provided for designing efficient light harvesting and conversion materials.
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Keywords:
- Methylene blue molecular clusters /
- Metal nanoparticles /
- Optical response /
- Multimode coupling
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