Zhang Long, Li Shuoxue, Sun Huaiyang, Jiang Qiwen, Wang Yue, Fang Yuanyuan, Shi Ying, Duan Defang, Wang Kai, Jiang Hong, Sui Laizhi, Wu Guorong, Yuan Kaijun, Zou Bo
State Key Laboratory of Superhard Materials, College of Physics, Jilin University, Changchun, 130012, China.
College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China.
Angew Chem Int Ed Engl. 2023 Mar 27;62(14):e202301573. doi: 10.1002/anie.202301573. Epub 2023 Feb 24.
Pressure-induced emission (PIE) associated with self-trapping excitons (STEs) in low-dimensional halide perovskites has attracted great attention for better materials-by-design. Here, using 2D layered double perovskite (C H CH CH NH ) AgBiBr as a model system, we advance a fundamental physicochemical mechanism of the PIE from the perspective of carrier dynamics and excited-state behaviors of local lattice distortion. We observed a pressure-driven STE transformation from dark to bright states, corresponding a strong broadband Stokes-shifted emission. Further theoretical analysis demonstrated that the suppressed lattice distortion and enhanced electronic dimensionality in the excited-state play an important role in the formation of stabilized bright STEs, which could manipulate the self-trapping energy and lattice deformation energy to form an energy barrier between the potential energy curves of ground- and excited-state, and enhance the electron-hole orbital overlap, respectively.
与低维卤化物钙钛矿中的自陷激子(STE)相关的压力诱导发射(PIE)因其在更好的材料设计方面的潜力而备受关注。在此,我们以二维层状双钙钛矿(CHCHCHNH)AgBiBr作为模型体系,从载流子动力学和局部晶格畸变激发态行为的角度,提出了PIE的基本物理化学机制。我们观察到压力驱动的STE从暗态到亮态的转变,伴随着强烈的宽带斯托克斯位移发射。进一步的理论分析表明,激发态中晶格畸变的抑制和电子维度的增强在稳定亮STE的形成中起着重要作用,它们分别可以控制自陷能量和晶格变形能,以在基态和激发态的势能曲线之间形成能垒,并增强电子 - 空穴轨道重叠。