Optically Pumped Lasing Based on Vibrationally Dressed Exciton Polaritons in a Single-Crystal Molecular Cavity at Room Temperature
Optically Pumped Lasing Based on Vibrationally Dressed Exciton Polaritons in a Single-Crystal Molecular Cavity at Room Temperature
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DOI：
10.1021/acsphotonics.2c00123
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发表时间：
2022-05
期刊：
影响因子：
7
通讯作者：
Takumi Matsuo;Yu. Ueda;H. Mizuno;F. Sasaki;K. Yamashita;H. Yanagi
中科院分区：
文献类型：
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作者：
Takumi Matsuo;Yu. Ueda;H. Mizuno;F. Sasaki;K. Yamashita;H. Yanagi
极化子光子学是未来量子信息与通信的关键技术之一。在这里，我们证明了在室温下，在5，5 ″-双（联苯基）-2，2 ′：5′，2 ″-三噻吩（BP 3 T）的单晶平面腔中形成的振动修饰激子极化激元的强有力的证据.在光泵浦下，BP 3 T晶体基于平面腔侧腔面之间的法布里-珀罗（F-P）谐振在初级和次级电子振动级数带处呈现纵向多模激射。每个增益变窄的电子振动带在激光阈值附近的激发能量密度处异常地分裂成多个峰，并伴随着高达几十皮秒的时间延迟，这是常规光子激光无法解释的。虽然这些激光特性主要被解释为激子极化激元（EP）的制度，分裂光谱的能量与波数图很好地解释了耦合有序BP 3 T分子的合作振动。
Polaritonic photonics is one of the key technologies for future quantum-based information and communication. Here, we demonstrate strong evidence of vibrationally dressed exciton polaritons formed in a single-crystal planar cavity of 5,5″-bis(biphenylyl)-2,2′:5′,2″-terthiophene (BP3T) at room temperature. Under optical pumping, the BP3T crystals exhibit longitudinal multimode lasing at the primary and secondary vibronic progression bands based on Fabry–Pérot (F-P) resonation between side facets of the planar cavity. Each gain-narrowed vibronic band extraordinarily split into multiple peaks at excitation fluence around the lasing threshold, accompanied with time delay up to several tens of picoseconds, which is unexplainable for conventional photon lasing. Although those lasing characteristics are primarily interpreted as a regime of exciton-polaritons (EPs), the energy versus wavenumber plots of splitting spectra are well-explained by coupling with cooperative vibrations of the ordered BP3T molecules.