Nonequilibrium polariton dynamics in organic microcavities
Nonequilibrium polariton dynamics in organic microcavities
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有机微腔中的非平衡极化子动力学
DOI：
10.1103/physrevb.66.081203
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发表时间：
2002
影响因子：
3.7
通讯作者：
R. Mahrt
中科院分区：
文献类型：
--
作者：
P. Schouwink;J. Lupton;H. Berlepsch;L. Dähne;R. Mahrt
在强耦合状态下制备含有 J-聚集体形成有机染料的微腔。改变微腔内整齐的有机薄膜的位置可以调整观察到的巨大拉比分裂。我们将拉比分裂设置为 25 meV，并研究在非共振激发下高能极化子发射的热激活。发现这表现出阿累尼乌斯激活，其能量对应于极化子分支分裂。在低温下观察到上部极化子的恒定偏移。微秒门控光谱表明系统的热化发生在毫秒的时间尺度上，这与皮秒范围内的极化子寿命形成对比。大量样品加热不能完全解释稳态实验中观察到的缓慢极化子热化，这表明长寿命的宏观极化子相干性影响极化子弛豫。
Microcavities containing a J-aggregate forming organic dye were prepared in the strong-coupling regime. Changing the position of the neat organic films within the microcavity allows a tuning of the giant Rabi splitting observed. We set the Rabi splitting to 25 meV and study the thermal activation of the higher-energy polariton emission under excitation off resonance. This is found to exhibit an Arrhenius activation with an energy corresponding to the polariton branch splitting. A constant offset to the upper polariton is observed at low temperature. Microsecond gated spectroscopy reveals that thermalization of the system occurs on the time scale of milliseconds, which contrasts with the polariton lifetime in the range of picoseconds. Bulk sample heating cannot fully account for the slow polariton thermalization observed in steady-state experiments, suggesting that long-lived macroscopic polariton coherence influences the polariton relaxation.