Weihao Zheng

Vapor Growth and Tunable Lasing of Band Gap Engineered Cesium Lead Halide Perovskite Micro/Nanorods with Triangular Cross Section

Although great efforts have been devoted to the synthesis of halide perovskites nanostructures, vapor growth of high-quality one-dimensional cesium lead halide nanostructures for tunable nanoscale lasers is still a challenge. Here, we report the growth of high-quality all-inorganic cesium lead halide alloy perovskite micro/nanorods with complete composition tuning by vapor-phase deposition. The as-grown micro/nanorods are single-crystalline with a triangular cross section and show strong photoluminescence which can be tuned from 415 to 673 nm by varying the halide composition. Furthermore, these single-crystalline perovskite micro/nanorods themselves function as effective Fabry-Perot cavities for nanoscale lasers. We have realized room-temperature tunable lasing of cesium lead halide perovskite with low lasing thresholds (∼14.1 μJ cm-2) and high Q factors (∼3500).

Directional Growth of Ultralong CsPbBr3 Perovskite Nanowires for High-Performance Photodetectors

Directional growth of ultralong nanowires (NWs) is significant for practical application of large-scale optoelectronic integration. Here, we demonstrate the controlled growth of in-plane directional perovskite CsPbBr3 NWs, induced by graphoepitaxial effect on annealed M-plane sapphire substrates. The wires have a diameter of several hundred nanometers, with lengths up to several millimeters. Microstructure characterization shows that CsPbBr3 NWs are high-quality single crystals, with smooth surfaces and well-defined cross section. The NWs have very strong band-edge photoluminescence (PL) with a long PL lifetime of ∼25 ns and can realize high-quality optical waveguides. Photodetectors constructed on these individual NWs exhibit excellent photoresponse with an ultrahigh responsivity of 4400 A/W and a very fast response speed of 252 μs. This work presents an important step toward scalable growth of high-quality perovskite NWs, which will provide promising opportunities in constructing integrated nanophotonic and optoelectronic systems.

Direct Vapor Growth of Perovskite CsPbBr3 Nanoplate Electroluminescence Devices

Metal halide perovskite nanostructures hold great promises as nanoscale light sources for integrated photonics due to their excellent optoelectronic properties. However, it remains a great challenge to fabricate halide perovskite nanodevices using traditional lithographic methods because the halide perovskites can be dissolved in polar solvents that are required in the traditional device fabrication process. Herein, we report single CsPbBr3 nanoplate electroluminescence (EL) devices fabricated by directly growing CsPbBr3 nanoplates on prepatterned indium tin oxide (ITO) electrodes via a vapor-phase deposition. Bright EL occurs in the region near the negatively biased contact, with a turn-on voltage of ∼3 V, a narrow full width at half-maximum of 22 nm, and an external quantum efficiency of ∼0.2%. Moreover, through scanning photocurrent microscopy and surface electrostatic potential measurements, we found that the formation of ITO/p-type CsPbBr3 Schottky barriers with highly efficient carrier injection is essential in realizing the EL. The formation of the ITO/p-type CsPbBr3 Schottky diode is also confirmed by the corresponding transistor characteristics. The achievement of EL nanodevices enabled by directly grown perovskite nanostructures could find applications in on-chip integrated photonics circuits and systems.

Cesium lead halide perovskite triangular nanorods as high-gain medium and effective cavities for multiphoton-pumped lasing

High-performance multiphoton-pumped lasers based on cesium lead halide perovskite nanostructures are promising for nonlinear optics and practical frequency upconversion devices in integrated photonics. However, the performance of such lasers is highly dependent on the quality of the material and cavity, which makes their fabrication challenging. Herein, we demonstrate that cesium lead halide perovskite triangular nanorods fabricated via vapor methods can serve as gain media and effective cavities for multiphoton-pumped lasers. We observed blue-shifts of the lasing modes in the excitation fluence-dependent lasing spectra at increased excitation powers, which fits well with the dynamics of Burstein–Moss shifts caused by the band filling effect. Moreover, efficient multiphoton lasing in CsPbBr3 nanorods can be realized in a wide excitation wavelength range (700–1,400 nm). The dynamics of multiphoton lasing were investigated by time-resolved photoluminescence spectroscopy, which indicated that an electron–hole plasma is responsible for the multiphoton-pumped lasing. This work could lead to new opportunities and applications for cesium lead halide perovskite nanostructures in frequency upconversion lasing devices and optical interconnect systems.

Single-Crystal Thin Films of Cesium Lead Bromide Perovskite Epitaxially Grown on Metal Oxide Perovskite (SrTiO3)

High-quality metal halide perovskite single crystals have low defect densities and excellent photophysical properties, yet thin films are the most sought after material geometry for optoelectronic devices. Perovskite single-crystal thin films (SCTFs) would be highly desirable for high-performance devices, but their growth remains challenging, particularly for inorganic metal halide perovskites. Herein, we report the facile vapor-phase epitaxial growth of cesium lead bromide perovskite (CsPbBr3) continuous SCTFs with controllable micrometer thickness, as well as nanoplate arrays, on traditional oxide perovskite SrTiO3(100) substrates. Heteroepitaxial single-crystal growth is enabled by the serendipitous incommensurate lattice match between these two perovskites, and overcoming the limitation of island-forming Volmer-Weber crystal growth is critical for growing large-area continuous thin films. Time-resolved photoluminescence, transient reflection spectroscopy, and electrical transport measurements show that the CsPbBr3 epitaxial thin film has a slow charge carrier recombination rate, low surface recombination velocity (104 cm s-1), and low defect density of 1012 cm-3, which are comparable to those of CsPbBr3 single crystals. This work suggests a general approach using oxide perovskites as substrates for heteroepitaxial growth of halide perovskites. The high-quality halide perovskite SCTFs epitaxially integrated with multifunctional oxide perovskites could open up opportunities for a variety of high-performance optoelectronics devices.

Broken Symmetry Induced Strong Nonlinear Optical Effects in Spiral WS2 Nanosheets

Transition metal dichalcogenides (TMDs) have provided a fundamental stage to study light-matter interactions and optical applications at the atomic scale due to their ultrathin thickness and their appropriate band gap in the visible region. Here, we report the strong nonlinear optical effects, including second-harmonic generation (SHG) and third-harmonic generation (THG) in spiral WS2 structures. SHG intensity quadratically increases with layer numbers, other than diminishing the oscillation of 2H stacking TMDs. The contrary SHG behavior is attributed to the broken symmetry from twisted screw structures, revealed by aberration-corrected transmission electronic microscope observation. Furthermore, the twist angle of the screw structure (5 degrees) was obtained by high-resolution transmission microscope measurements and confirmed by polarization tests of SHG output. Moreover, we roughly estimate the effective second-order nonlinear susceptibility. The discovery and understanding of the accumulation of nonlinear susceptibility of spiral structures with increasing thickness will extend the nonlinear applications of TMDs.

High-Quality In-Plane Aligned CsPbX3 Perovskite Nanowire Lasers with Composition Dependent Strong Exciton-Photon Coupling

Cesium lead halide perovskite nanowires have emerged as promising low-dimensional semiconductor structures for integrated photonic applications. Understanding light-matter interactions in a nanowire cavity is of both fundamental and practical interest in designing low-power-consumption nanoscale light sources. In this work, high-quality in-plane aligned halide perovskite CsPbX3 (X = Cl, Br, I) nanowires are synthesized by a vapor growth method on an annealed M-plane sapphire substrate. Large-area nanowire laser arrays have been achieved based on the as-grown aligned CsPbX3 nanowires at room temperature with quite low pumping thresholds, very high quality factors, and a high degree of linear polarization. More importantly, it is found that exciton-polaritons are formed in the nanowires under the excitation of a pulsed laser, indicating a strong exciton-photon coupling in the optical microcavities made of cesium lead halide perovskites. The coupling strength in these CsPbX3 nanowires is dependent on the atomic composition, where the obtained room-temperature Rabi splitting energy is ∼210 ± 13, 146 ± 9, and 103 ± 5 meV for the CsPbCl3, CsPbBr3, and CsPbI3 nanowires, respectively. This work provides fundamental insights for the practical applications of all-inorganic perovskite CsPbX3 nanowires in designing light-emitting devices and integrated nanophotonic systems.

Visualizing Carrier Transport in Metal Halide Perovskite Nanoplates via Electric Field Modulated Photoluminescence Imaging

Metal halide perovskite nanostructures have recently been the focus of intense research due to their exceptional optoelectronic properties and potential applications in integrated photonics devices. Charge transport in perovskite nanostructure is a crucial process that defines efficiency of optoelectronic devices but still requires a deep understanding. Herein, we report the study of the charge transport, particularly the drift of minority carrier in both all-inorganic CsPbBr3 and organic-inorganic hybrid CH3NH3PbBr3 perovskite nanoplates by electric field modulated photoluminescence (PL) imaging. Bias voltage dependent elongated PL emission patterns were observed due to the carrier drift at external electric fields. By fitting the drift length as a function of electric field, we obtained the carrier mobility of about 28 cm2 V-1 S-1 in the CsPbBr3 perovskite nanoplate. The result is consistent with the spatially resolved PL dynamics measurement, confirming the feasibility of the method. Furthermore, the electric field modulated PL imaging is successfully applied to the study of temperature-dependent carrier mobility in CsPbBr3 nanoplates. This work not only offers insights for the mobile carrier in metal halide perovskite nanostructures, which is essential for optimizing device design and performance prediction, but also provides a novel and simple method to investigate charge transport in many other optoelectronic materials.

Band alignment engineering in two-dimensional lateral heterostructures

Two-dimensional (2D) heterostructures have aroused widespread attentions due to the fascinating properties originating from the interfaces and the derived potential applications in modern electronics and optoelectronics. The interfacial band alignment engineering of 2D heterostructures would open up promising routes toward the flexible design and optimization of the electronic and optoelectronic properties. Herein, we report a one-step chemical vapor deposition method for the growth of band alignment continuously modulated WS2-WS2(1- x)Se2 x (0 < x ≤ 1) monolayer lateral heterostructures, with atomically sharp interfaces at the junction area. Local photoluminescence (PL) and Raman measurements demonstrate the position-dependent composition and band gap information on the as-grown nanosheets. Kelvin probe force microscopy (KPFM) investigations further confirm the tunable band alignments in the heterostructures, where a continuously decreased Fermi level difference between the core and the shell regions is observed with the x value varied from 1 to 0. The direct growth of high-quality atomic-level junctions with controllable band alignment marks an important step toward the potential applications of 2D semiconductors in integrated electronic and optoelectronic devices.