Organic-inorganic perovskites have attracted great attentions driven by exceptional progress in photovoltaics, photonics and optoelectronics. Different from the corner sharing framework of three-dimensional (3D) perovskite, two-dimensional (2D) organic-inorganic perovskites possess a layered staking structure composed of alternative organic and inorganic components.Due to the inherent multi-quantum-well-like structure, it is intriguing to explore the optical properties of 2D perovskites enabled by spatial and dielectric confinement. Herein, the twophoton absorption (TPA) properties of 2D perovskite phenylethylamine lead iodide ((PEA)2PbI4) are systematically studied. The 2D perovskite exhibits a giant TPA and saturation effect under excitation of 800 nm femtosecond laser. The TPA coefficient of a (PEA)2PbI4 flake is measured to be about 211.5 cm/MW, which is at least one order of magnitude larger than those of 3D perovskite films and some typical semiconductor Submitted to 2 2 nanostructures. The giant TPA can be attributed to the enhanced quantum and dielectric confinement in the organic-inorganic multi-quantum-well structure. In addition, a highly thickness-dependent TPA is observed for the 2D perovskite flakes. The result advocates a great promise of 2D organic-inorganic perovskites for nonlinear optical absorption related optoelectronic devices.
'Blinking', or 'fluorescence intermittency', refers to a random switching between 'ON' (bright) and 'OFF' (dark) states of an emitter; it has been studied widely in zero-dimensional quantum dots and molecules, and scarcely in one-dimensional systems. A generally accepted mechanism for blinking in quantum dots involves random switching between neutral and charged states (or is accompanied by fluctuations in charge-carrier traps), which substantially alters the dynamics of radiative and non-radiative decay. Here, we uncover a new type of blinking effect in vertically stacked, two-dimensional semiconductor heterostructures, which consist of two distinct monolayers of transition metal dichalcogenides (TMDs) that are weakly coupled by van der Waals forces. Unlike zero-dimensional or one-dimensional systems, two-dimensional TMD heterostructures show a correlated blinking effect, comprising randomly switching bright, neutral and dark states. Fluorescence cross-correlation spectroscopy analyses show that a bright state occurring in one monolayer will simultaneously lead to a dark state in the other monolayer, owing to an intermittent interlayer carrier-transfer process. Our findings suggest that bilayer van der Waals heterostructures provide unique platforms for the study of charge-transfer dynamics and non-equilibrium-state physics, and could see application as correlated light emitters in quantum technology.
Arbitrary control of terahertz (THz) waves remains a significant challenge although it promises many important applications. Here, a method to tailor the reflection and scattering of THz waves in an anomalous manner by using 1‐bit coding metamaterials is presented. Specific coding sequences result in various THz far‐field reflection and scattering patterns, ranging from a single beam to two, three, and numerous beams, which depart obviously from the ordinary Snell's law of reflection. By optimizing the coding sequences, a wideband THz thin film metamaterial with extremely low specular reflection, due to the scattering of the incident wave into various directions, is demonstrated. As a result, the reflection from a flat and flexible metamaterial can be nearly uniformly distributed in the half space with small intensity at each specific direction, manifesting a diffuse reflection from a rough surface. Both simulation and experimental results show that a reflectivity less than −10 dB is achieved over a wide frequency range from 0.8 to 1.4 THz, and it is insensitive to the polarization of the incident wave. This work reveals new opportunities arising from coding metamaterials in effective manipulation of THz wave propagation and may offer widespread applications.
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