Resonantly Pumped Bright-Triplet Exciton Lasing in Cesium Lead Bromide Perovskites.
Resonantly Pumped Bright-Triplet Exciton Lasing in Cesium Lead Bromide Perovskites.
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DOI：
10.1021/acsphotonics.1c00720
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发表时间：
2021-09-15
期刊：
影响因子：
7
通讯作者：
Taylor RA
中科院分区：
文献类型：
--
作者：
Ying G;Farrow T;Jana A;Shao H;Im H;Osokin V;Baek SB;Alanazi M;Karmakar S;Mukherjee M;Park Y;Taylor RA
令人惊讶的是，最近在卤化铅钙钛矿中观察到高度发射的三重态，这说明了与其他半导体相比，它们的数量级更亮的光学信号和高量子效率。这使得它们在未来的光电应用中具有吸引力，特别是在明亮的低阈值纳米激光器中。虽然非共振泵浦激光从所有无机铅卤化物钙钛矿现在是一个有吸引力的途径，可扩展的低功率激光源的纳米光电子学，在这里，我们展示了一个共振光泵浦方案的快速三重态CsPbBr 3纳米晶体。该方案使我们能够实现偏振三重态激光源，大大提高了1个数量级的相干信号，同时抑制非相干的贡献。其结果是具有高度吸引人的技术特性的源，包括明亮的偏振信号和高的受激自发发射信号对比度，可以过滤以提高光谱纯度。发射是通过选择性地泵浦纳米晶体中玻尔半径为10 nm的弱限制激子态产生的。在具有四重对称性的纳米晶体中，激子的精细结构是由能量分裂引起的。我们使用线性偏振器来解决2倍的非简并次能级的三重态激子和使用光致发光激发光谱来确定的状态的能量之前，它共振泵浦。
The surprising recent observation of highly emissive triplet-states in lead halide perovskites accounts for their orders-of-magnitude brighter optical signals and high quantum efficiencies compared to other semiconductors. This makes them attractive for future optoelectronic applications, especially in bright low-threshold nanolasers. While nonresonantly pumped lasing from all-inorganic lead-halide perovskites is now well-established as an attractive pathway to scalable low-power laser sources for nano-optoelectronics, here we showcase a resonant optical pumping scheme on a fast triplet-state in CsPbBr3 nanocrystals. The scheme allows us to realize a polarized triplet-laser source that dramatically enhances the coherent signal by 1 order of magnitude while suppressing noncoherent contributions. The result is a source with highly attractive technological characteristics, including a bright and polarized signal and a high stimulated-to-spontaneous emission signal contrast that can be filtered to enhance spectral purity. The emission is generated by pumping selectively on a weakly confined excitonic state with a Bohr radius ∼10 nm in the nanocrystals. The exciton fine-structure is revealed by the energy-splitting resulting from confinement in nanocrystals with tetragonal symmetry. We use a linear polarizer to resolve 2-fold nondegenerate sublevels in the triplet exciton and use photoluminescence excitation spectroscopy to determine the energy of the state before pumping it resonantly.
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