Poonia Ajay K, Mondal Barnali, Beard Matthew C, Nag Angshuman, Adarsh K V
Department of Physics, Indian Institute of Science Education and Research, Bhopal-462066, India.
Department of Chemistry, Indian Institute of Science Education and Research, Pune-411008, India.
Phys Rev Lett. 2024 Feb 9;132(6):063803. doi: 10.1103/PhysRevLett.132.063803.
Superfluorescence, a cooperative coherent spontaneous emission, is of great importance to the understanding of many-body correlation in optical processes. Even though superfluorescence has been demonstrated in many diverse systems, it is hard to observe in electron-hole plasma (EHP) due to its rapid dephasing and hence needs strong magnetic fields or complex microcavities. Herein, we report the first experimental observation of superfluorescence from EHP up to a moderate temperature of 175 K without external stimuli in a coupled metal halide perovskite quantum dots film. The EHP exhibits macroscopic quantum coherence through spontaneous synchronization. The coherence of the excited state decays by superfluorescence, which is redshifted 40 meV from the spontaneous emission with a ∼1700 times faster decay rate and exhibits quadratic fluence dependence. Notably, the excited state population's delayed growth and abrupt decay, which are strongly influenced by the pump fluence and the Burnham-Chiao ringing, are the characteristics of the superfluorescence. Our findings will open up a new frontier for cooperative emission and light beam-based technologies.
超荧光是一种合作相干自发辐射,对于理解光学过程中的多体关联非常重要。尽管超荧光已在许多不同系统中得到证实,但由于电子 - 空穴等离子体(EHP)的快速退相,在其中很难观察到,因此需要强磁场或复杂的微腔。在此,我们报告了在耦合金属卤化物钙钛矿量子点薄膜中,首次在高达175 K的中等温度下,无需外部刺激就从EHP中观察到超荧光。EHP通过自发同步表现出宏观量子相干。激发态的相干性通过超荧光衰减,其相对于自发发射红移了40 meV,衰减速率快约1700倍,并且表现出二次通量依赖性。值得注意的是,激发态粒子数的延迟增长和突然衰减,受到泵浦通量和伯纳姆 - 乔(Burnham - Chiao)振荡的强烈影响,是超荧光的特征。我们的发现将为合作发射和基于光束的技术开辟一个新的前沿领域。