Strong Coupling Between Plasmons and Molecular Excitons in Metal–Organic Frameworks,Nano Letters

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Strong Coupling Between Plasmons and Molecular Excitons in Metal–Organic Frameworks
Nano Letters ( IF 9.6 ) Pub Date : 2021-09-07 , DOI: 10.1021/acs.nanolett.1c02740
Alexander D Sample , Jun Guan , Jingtian Hu , Thaddeus Reese , Charles R Cherqui , Jeong-Eun Park , Francisco Freire-Fernández , Richard D Schaller ₁ , George C Schatz , Teri W Odom

Affiliation

This Letter describes strong coupling of densely packed molecular emitters in metal–organic frameworks (MOFs) and plasmonic nanoparticle (NP) lattices. Porphyrin-derived ligands with small transition dipole moments in an ordered MOF film were grown on Ag NP arrays. Angle-resolved optical measurements of the MOF-NP lattice system showed the formation of a polariton that is lower in energy and does not cross the uncoupled MOF Q₁ band. Modeling predicted the upper polariton energy and a calculated Rabi splitting of 110 meV. The coupling strength was systematically controlled by detuning the plasmon energy by changing the refractive index of the solvents infiltrating the MOF pores. Through transient absorption spectroscopy, we found that the lower polariton decays quickly at shorter time scales (<500 ps) and slowly at longer times because of energy transfer from the upper polariton. This hybrid system demonstrates how MOFs can function as an accessible excitonic material for polariton chemistry.

中文翻译：

金属-有机框架中等离子体和分子激子之间的强耦合

这封信描述了金属有机框架 (MOF) 和等离子体纳米粒子 (NP) 晶格中密集堆积的分子发射体的强耦合。在有序 MOF 膜中具有小跃迁偶极矩的卟啉衍生配体生长在 Ag NP 阵列上。MOF-NP 晶格系统的角度分辨光学测量表明，形成了能量较低且不与未耦合 MOF Q ₁交叉的极化子乐队。建模预测了上极化子能量和 110 meV 的计算 Rabi 分裂。通过改变渗入 MOF 孔的溶剂的折射率，通过使等离子体能量失谐来系统地控制耦合强度。通过瞬态吸收光谱，我们发现下极化子在较短的时间尺度 (<500 ps) 内衰减迅速，而在较长时间内由于来自上极化子的能量转移而衰减较慢。该混合系统展示了 MOF 如何作为一种可用于极化子化学的激子材料。

更新日期：2021-09-22

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