Material composition engineering and device fabrication of perovskite nanocrystals (PNCs) in solution can introduce organic contamination and entail several synthetic, processing, and stabilization steps. We report three-dimensional (3D) direct lithography of PNCs with tunable composition and bandgap in glass. The halide ion distribution was controlled at the nanoscale with ultrafast laser–induced liquid nanophase separation. The PNCs exhibit notable stability against ultraviolet irradiation, organic solution, and high temperatures (up to 250°C). Printed 3D structures in glass were used for optical storage, micro–light emitting diodes, and holographic displays. The proposed mechanisms of both PNC formation and composition tunability were verified.
Two-dimensional (2D) layered materials, transition-metal dichalcogenides, and black phosphorus have attracted considerable interest from the viewpoints of fundamental physics and device applications. The establishment of new functionalities in anisotropic layered 2D materials is a challenging but rewarding frontier, owing to the remarkable optical properties of these materials and their prospects for new devices. Herein, we report the anisotropic and thickness-dependent optical properties of a 2D layered monochalcogenide of germanium sulfide (GeS). Three Raman-scattering peaks corresponding to the B3g, A g1 , and A g2 modes with a strong polarization dependence are demonstrated in the GeS flakes, which validates polarized Raman spectroscopy as an effective method for identifying the crystal orientation of anisotropic layered GeS. Photoluminescence (PL) is observed with a peak at ~1.66 eV that originates from the direct optical transition in GeS at room temperature. The polarization-dependent characteristics of the PL, which are revealed for the first time, along with the demonstration of anisotropic absorption, indicate an obvious anisotropic optical transition near the band edge of GeS, which is supported by density functional theory calculations. The significantly thickness-dependent PL is observed and discussed. This anisotropic layered GeS presents opportunities for the discovery of new physical phenomena and will find applications that exploit its anisotropic properties, such as polarization-sensitive photodetectors.
Layered materials, such as graphene, transition metal dichalcogenides and black phosphorene, have been established rapidly as intriguing building blocks for optoelectronic devices. Here, we introduce highly polarization sensitive, broadband, and high-temperature-operation photodetectors based on multilayer germanium sulfide (GeS). The GeS photodetector shows a high photoresponsivity of about 6.8 × 103 A W−1, an extremely high specific detectivity of 5.6 × 1014 Jones, and broad spectral response in the wavelength range of 300–800 nm. More importantly, the GeS photodetector has high polarization sensitivity to incident linearly polarized light, which provides another degree of freedom for photodetectors. Tremendously enhanced photoresponsivity is observed with a temperature increase, and high responsivity is achievable at least up to 423 K. The establishment of larger photoinduced reduction of the Schottky barrier height will be significant for the investigation of the photoresponse mechanism of 2D layered material-based photodetectors. These attributes of high photocurrent generation in a wide temperature range, broad spectral response, and polarization sensitivity coupled with environmental stability indicate that the proposed GeS photodetector is very suitable for optoelectronic applications.
Three-dimensional (3D) glass chips are promising waveguide platforms for building hybrid 3D photonic circuits due to their 3D topological capabilities, large transparent windows, and low coupling dispersion. At present, the key challenge in scaling down a benchtop optical system to a glass chip is the lack of precise methods for controlling the mode field and optical coupling of 3D waveguide circuits. Here, we propose an overlap-controlled multi-scan (OCMS) method based on laser-direct lithography that allows customizing the refractive index profile of 3D waveguides with high spatial precision in a variety of glasses. On the basis of this method, we achieve variable mode-field distribution, robust and broadband coupling, and thereby demonstrate dispersionless LP21-mode conversion of supercontinuum pulses with the largest deviation of <0.1 dB in coupling ratios on 210 nm broadband. This approach provides a route to achieve ultra-broadband and low-dispersion coupling in 3D photonic circuits, with overwhelming advantages over conventional planar waveguide-optic platforms for on-chip transmission and manipulation of ultrashort laser pulses and broadband supercontinuum.
All-optical nonlinear activation functions (NAFs) are crucial for enabling rapid optical neural networks (ONNs). As linear matrix computation advances in integrated ONNs, on-chip all-optical NAFs face challenges such as limited integration, high latency, substantial power consumption, and a high activation threshold. In this work, we develop an integrated nonlinear optical activator based on the butt-coupling integration of two-dimensional (2D) MoTe2 and optical waveguides (OWGs). The activator exhibits an ultra-broadband response from visible to near-infrared wavelength, a low activation threshold of 0.94 μW, a small device size (~50 µm2), an ultra-fast response rate (2.08 THz), and high-density integration. The excellent nonlinear effects and broadband response of 2D materials have been utilized to create all-optical NAFs. These activators were applied to simulate MNIST handwritten digit recognition, achieving an accuracy of 97.6%. The results underscore the potential application of this approach in ONNs. Moreover, the classification of more intricate CIFAR-10 images demonstrated a generalizable accuracy of 94.6%. The present nonlinear activator promises a general platform for three-dimensional (3D) ultra-broadband ONNs with dense integration and low activation thresholds by integrating a variety of strong nonlinear optical (NLO) materials (e.g., 2D materials) and OWGs in glass.