High‐Order Shift Current Induced Terahertz Emission from Inorganic Cesium Bromine Lead Perovskite Engendered by Two‐Photon Absorption

Abstract

AbstractHigh‐order nonlinear optical phenomena are interesting from a fundamental point of view as they reveal intrinsic symmetries of the materials. Potentially they can also be used for practical optoelectronic applications. High‐order shift current is one of these phenomena, and yet it has never been detected in experiments, primarily due to the difficulty in conventional contact detection. In this work, the shift current due to the two‐photon absorption (TPA) from all‐inorganic perovskite CsPbBr3 is first observed by a contactless and nondestructive terahertz (THz) emission method. The results reveal that the THz emission is dominated by a high‐order shift current (fourth‐order nonlinear optical effect) with the below‐bandgap photon energy of femtosecond laser excitation. The high‐order shift current origins from the broken inversion symmetry induced by the dynamic stereochemical activity of the Pb2+ lone pair. A microscopic TPA‐assisted nonlinear optical model is presented to describe the photophysical process of the THz emission. The model matches well with the quadratic pump fluence and angular dependence of the THz emission. This work can not only open a new venue for the all‐inorganic perovskite‐based nonlinear optoelectronics and THz devices, but also afford a THz technology for the high‐order nonlinear effect analysis.