Zhang Heng, Debroye Elke, Zheng Wenhao, Fu Shuai, Virgilio Lucia D, Kumar Pushpendra, Bonn Mischa, Wang Hai I
Max Planck Institute for Polymer Research, Ackermannweg 10, 55128 Mainz, Germany.
Department of Chemistry, KU Leuven, Celestijnenlaan 200F, 3001 Leuven, Belgium.
Sci Adv. 2021 Dec 24;7(52):eabj9066. doi: 10.1126/sciadv.abj9066. Epub 2021 Dec 22.
Highly mobile hot charge carriers are a prerequisite for efficient hot carrier optoelectronics requiring long-range hot carrier transport. However, hot carriers are typically much less mobile than cold ones because of carrier-phonon scattering. Here, we report enhanced hot carrier mobility in CsAgBiBr double perovskite. Following photoexcitation, hot carriers generated with excess energy exhibit boosted mobility, reaching an up to fourfold enhancement compared to cold carriers and a long-range hot carrier transport length beyond 200 nm. By optical pump–infrared push-terahertz probe spectroscopy and frequency-resolved photoconductivity measurements, we provide evidence that the conductivity enhancement originates primarily from hot holes with reduced momentum scattering. We rationalize our observation by considering (quasi-)ballistic transport of thermalized hot holes with energies above an energetic threshold in CsAgBiBr. Our findings render CsAgBiBr as a fascinating platform for studying the fundamentals of hot carrier transport and its exploitation toward hot carrier–based optoelectronic devices.
对于需要长程热载流子传输的高效热载流子光电器件而言,高迁移率的热载流子是必不可少的。然而,由于载流子-声子散射,热载流子的迁移率通常比冷载流子低得多。在此,我们报道了CsAgBiBr双钙钛矿中热载流子迁移率的增强。光激发后,具有多余能量产生的热载流子表现出增强的迁移率,与冷载流子相比提高了四倍,热载流子长程传输长度超过200nm。通过光泵浦-红外推-太赫兹探测光谱和频率分辨光电导率测量,我们提供了电导率增强主要源于动量散射减少的热空穴的证据。我们通过考虑CsAgBiBr中能量高于能量阈值的热化热空穴的(准)弹道输运来解释我们的观察结果。我们的发现使CsAgBiBr成为研究热载流子传输基本原理及其在基于热载流子的光电器件中的应用的一个引人入胜的平台。