论文标题

有机微腔内强耦合的超快热耦合

Ultrafast Thermal Modification of Strong Coupling in an Organic Microcavity

论文作者

Liu, Bin, Menon, Vinod M., Sfeir, Matthew Y.

论文摘要

人们对使用强耦合有机微腔来调整分子动力学的兴趣越来越大,包括分子的电子和振动特性。然而,很少关注腔极化子作为传感器的效用,以弥补现象,包括热激发。在这里,我们证明了有机微腔系统的非共振红外激发在腔polariton共振附近的可见光谱范围内引起瞬态响应。我们展示了如何通过金属腔镜中电子的超快速加热来理解这些光学响应,从而修改了有效的折射率,然后修改了强耦合条件。微腔的时间动力学严格由金属中的载体确定,包括通过电子 - 音波耦合冷却电子以及晶格中传播相干模式的激发。我们排除多光子激发过程,并验证尽管有很强的瞬时特征,但仍不存在真正的极性人群。这些结果表明,腔偏极的希望是非平衡现象的敏感探针。

There is growing interest in using strongly coupled organic microcavities to tune molecular dynamics, including the electronic and vibrational properties of molecules. However, very little attention has been paid to the utility of cavity polaritons as sensors for out-of-equilibrium phenomena, including thermal excitations. Here, we demonstrate that non-resonant infrared excitation of an organic microcavity system induces a transient response in the visible spectral range near the cavity polariton resonances. We show how these optical response can be understood in terms of ultrafast heating of electrons in the metal cavity mirror, which modifies the effective refractive index and subsequently the strong coupling conditions. The temporal dynamics of the microcavity are strictly determined by carriers in the metal, including the cooling of electrons via electron-phonon coupling and excitation of propagating coherent acoustic modes in the lattice. We rule out multiphoton excitation processes and verify that no real polariton population exists despite their strong transient features. These results suggest the promise of cavity polaritons as sensitive probes of non-equilibrium phenomena.

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