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Optimizing Lasing Performance of CsPbBr3 Microplates by Regulating Exciton Recombination Dynamics with Pressure
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2024-12-16 , DOI: 10.1021/acs.jpclett.4c02962 Xiuru Yao, Ruiyu Li, Zihan Zhang, Xinmiao Wei, Xinmiao Gai, Jinming Zhu, Hongyu Yu, Xin Wang, Yongjun Bao
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2024-12-16 , DOI: 10.1021/acs.jpclett.4c02962 Xiuru Yao, Ruiyu Li, Zihan Zhang, Xinmiao Wei, Xinmiao Gai, Jinming Zhu, Hongyu Yu, Xin Wang, Yongjun Bao
This study aims to achieve an ultralow lasing threshold in CsPbBr3 microplates (MPs), a crucial step toward developing electrically driven micro/nanolasers for optics integrated chips. We investigate the lasing behavior of CsPbBr3 MPs under varying pressures by using static-state photoluminescence (PL), time-resolved PL (TRPL), and first-principles theory calculations based on density functional theory (DFT). Our results reveal that the lasing threshold initially decreases and then increases, with a critical turning point at 0.44 GPa. Notably, we achieve an optimal lasing threshold of 20.87 μJ/cm2 after releasing pressure from 1.87 GPa, highlighting the potential of pressure modulation to optimize the lasing performance. At low pressure, pressure-induced phonon hardening enhances the barrier, preventing excitons decay from free states to trapping states. Conversely, at higher pressure, the increased density of surface defects, due to pressure-induced anisotropic contraction of lattice constants along the c-axis, leads to excitons decay from free states to trapping states. For CsPbBr3 MPs, it is evident that only free excitons contribute to lasing, while both free and trapped excitons contribute to luminescence. These findings offer a novel strategy to optimize the lasing performance of perovskite micro/nanolasers, significantly advancing their potential for practical applications in optoelectronic devices.
中文翻译:
通过压力调节激子复合动力学来优化 CsPbBr3 微孔板的激光处理性能
本研究旨在在 CsPbBr3 微孔板 (MPs) 中实现超低激光阈值,这是开发用于光学集成芯片的电驱动微/纳米激光器的关键一步。我们使用静态光致发光 (PL)、时间分辨 PL (TRPL) 和基于密度泛函理论 (DFT) 的第一性原理理论计算研究了 CsPbBr3 MPs 在不同压力下的激光行为。我们的结果表明,激光阈值最初降低后增加,临界转折点为 0.44 GPa。值得注意的是,在从 1.87 GPa 释放压力后,我们实现了 20.87 μJ/cm2 的最佳激光阈值,这凸显了压力调制优化激光性能的潜力。在低压下,压力诱导的声子硬化增强了势垒,防止激子从自由态衰变为俘获态。相反,在较高压力下,由于压力诱导的晶格常数沿 c 轴的各向异性收缩,表面缺陷的密度增加,导致激子从自由态衰变为俘获态。对于 CsPbBr3 MP,很明显,只有游离激子有助于激光,而游离激子和俘获激子都有助于发光。这些发现为优化钙钛矿微/纳米激光器的激光性能提供了一种新策略,显着提高了它们在光电器件中的实际应用潜力。
更新日期:2024-12-16
中文翻译:
通过压力调节激子复合动力学来优化 CsPbBr3 微孔板的激光处理性能
本研究旨在在 CsPbBr3 微孔板 (MPs) 中实现超低激光阈值,这是开发用于光学集成芯片的电驱动微/纳米激光器的关键一步。我们使用静态光致发光 (PL)、时间分辨 PL (TRPL) 和基于密度泛函理论 (DFT) 的第一性原理理论计算研究了 CsPbBr3 MPs 在不同压力下的激光行为。我们的结果表明,激光阈值最初降低后增加,临界转折点为 0.44 GPa。值得注意的是,在从 1.87 GPa 释放压力后,我们实现了 20.87 μJ/cm2 的最佳激光阈值,这凸显了压力调制优化激光性能的潜力。在低压下,压力诱导的声子硬化增强了势垒,防止激子从自由态衰变为俘获态。相反,在较高压力下,由于压力诱导的晶格常数沿 c 轴的各向异性收缩,表面缺陷的密度增加,导致激子从自由态衰变为俘获态。对于 CsPbBr3 MP,很明显,只有游离激子有助于激光,而游离激子和俘获激子都有助于发光。这些发现为优化钙钛矿微/纳米激光器的激光性能提供了一种新策略,显着提高了它们在光电器件中的实际应用潜力。