在CH3NH3PbI3/Graphene接口处展开用于热载流子收集的曲折路径
Unravelling a Zigzag Pathway for Hot-Carrier Collection at CH3NH3PbI3/Graphene Interfaces
摘要：
由能量远高于带隙的光子激发的光激发的深带热载流子的捕获对于光伏和光电应用是非常重要的，因为它直接关系到光子到电子转换的量子效率。通过采用时间分辨光致发光和最先进的时域密度泛函理论，我们揭示了有机-无机杂化钙钛矿中的光激发热载流子更喜欢曲折的界面电荷转移路径，即，热载流子在它们达到电荷分离状态之前在CH 3 NH3 PbI 3和石墨烯之间来回转移。在量子相干性和层间振动模式的驱动下，在石墨烯-石墨烯界面处的这一路径需要大约400飞秒，比CH 3 NH3 PbI 3内的弛豫过程（几皮秒）快得多。我们进一步证明，传输速率的途径可以进一步提高界面缺陷。我们的工作提供了一个新的见解的基本理解和精确操纵的热载流子动力学在复杂的超导体-石墨烯界面，铺平了道路，高效的光伏和光电器件优化。
英文摘要：
The capture of photoexcited deep-band hot carriers, excited by photons with energies far above the bandgap, is of significant importance for photovoltaic and photoelectronic applications since it is directly related to the quantum efficiency of photon-to-electron conversion. By employing time-resolved photoluminescence and state-of-the-art time-domain density functional theory, we reveal that photoexcited hot carriers in organic-inorganic hybrid perovskites prefer a zigzag interfacial charge-transfer pathway, i.e., the hot carriers transfer back and forth between CH3NH3PbI3 and graphene, before they reach a charge separated state. Driven by quantum coherence and interlayer vibrational modes, this pathway at the semiconductor-graphene interface takes about 400 femtoseconds, much faster than the relaxation process within CH3NH3PbI3 (in several picoseconds). We further demonstrate that the transfer rate of the pathway can be further enhanced by interfacial defects. Our work provides a new insight for the fundamental understanding and precise manipulation of hot-carrier dynamics at the complex semiconductor-graphene interfaces, paving the way for highly efficient photovoltaic and photoelectric device optimization.
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