Hongjun Liu

Composition-Modulated Two-Dimensional Semiconductor Lateral Heterostructures via Layer-Selected Atomic Substitution

Composition-controlled growth of two-dimensional layered semiconductor heterostructures is crucially important for their applications in multifunctional integrated photonics and optoelectronics devices. Here, we report the realization of composition completely modulated layered semiconductor MoS2-MoS2(1-x)Se2x (0 < x < 1) lateral heterostructures via the controlled layer-selected atomic substitution of pregrown stacking MoS2, with a bilayer located at the center of a monolayer. Through controlling the reaction time, S at the monolayer MoS2 at the peripheral area can be selectively substituted by Se atoms at different levels, while the bilayer region at the center retains the original composition. Microstructure characterizations demonstrated the formation of lateral heterostructures with a sharp interface, with the composition at the monolayer area gradually modulated from MoS2 to MoSe2 and having high-quality crystallization at both the monolayer and the bilayer areas. Photoluminescence and Raman mapping studies exhibit the tunable optical properties only at the monolayer region of the as-grown heterostructures, which further demonstrates the realization of high-quality composition/bandgap modulated lateral heterostructures. This work offers an interesting and easy route for the development of high-quality layered semiconductor heterostructures for potential broad applications in integrated nanoelectronic and optoelectronic devices.

Perovskite–Erbium Silicate Nanosheet Hybrid Waveguide Photodetectors at the Near‐Infrared Telecommunication Band

Methylammonium lead halide perovskites have attracted enormous attentions due to their superior optical and electronic properties. However, the photodetection at near-infrared telecommunication wavelengths is hardly achievable because of their wide bandgaps. Here, this study demonstrates, for the first time, novel perovskite-erbium silicate nanosheet hybrid photodetectors with remarkable spectral response at ≈1.54 µm. Under the near-infrared light illumination, the erbium silicate nanosheets can give strong upconversion luminescence, which will be well confined in their cavities and then be efficiently coupled into and simultaneously excite the adjacent perovskite to realize photodetection. These devices own prominent responsivity and external quantum efficiency as high as previously reported microscale silicon-based subbandgap photodetectors. More importantly, the photoresponse speed (≈900 µs) is faster by five orders than the ever reported hot electron silicon-based photodetectors at telecommunication wavelengths. The realization of perovskite-based telecommunication band photodetectors will open new chances for applications in advanced integrated photonics devices and systems.

High‐Performance Flexible Photodetectors based on High‐Quality Perovskite Thin Films by a Vapor–Solution Method

Organometal halide perovskites are new light-harvesting materials for lightweight and flexible optoelectronic devices due to their excellent optoelectronic properties and low-temperature process capability. However, the preparation of high-quality perovskite films on flexible substrates has still been a great challenge to date. Here, a novel vapor-solution method is developed to achieve uniform and pinhole-free organometal halide perovskite films on flexible indium tin oxide/poly(ethylene terephthalate) substrates. Based on the as-prepared high-quality perovskite thin films, high-performance flexible photodetectors (PDs) are constructed, which display a nR value of 81 A W-1 at a low working voltage of 1 V, three orders higher than that of previously reported flexible perovskite thin-film PDs. In addition, these flexible PDs exhibit excellent flexural stability and durability under various bending situations with their optoelectronic performance well retained. This breakthrough on the growth of high-quality perovskite thin films opens up a new avenue to develop high-performance flexible optoelectronic devices.

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.

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.

Strain-Tuning Atomic Substitution in Two-Dimensional Atomic Crystals

Atomic substitution offers an important route to achieve compositionally engineered two-dimensional nanostructures and their heterostructures. Despite the recent research progress, the fundamental understanding of the reaction mechanism has still remained unclear. Here, we reveal the atomic substitution mechanism of two-dimensional atomic layered materials. We found that the atomic substitution process depends on the varying lattice constant (strain) in monolayer crystals, dominated by two strain-tuning (self-promoted and self-limited) mechanisms using density functional theory calculations. These mechanisms were experimentally confirmed by the controllable realization of a graded substitution ratio in the monolayers by controlling the substitution temperature and time and further theoretically verified by kinetic Monte Carlo simulations. The strain-tuning atomic substitution processes are of general importance to other two-dimensional layered materials, which offers an interesting route for tailoring electronic and optical properties of these materials.

Inversion Domain Boundary Induced Stacking and Bandstructure Diversity in Bilayer MoSe2

Interlayer rotation and stacking were recently demonstrated as effective strategies for tuning physical properties of various two-dimensional materials. The latter strategy was mostly realized in heterostructures with continuously varied stacking orders, which obscure the revelation of the intrinsic role of a certain stacking order in its physical properties. Here, we introduce inversion-domain-boundaries into molecular-beam-epitaxy grown MoSe2 homobilayers, which induce uncommon fractional lattice translations to their surrounding domains, accounting for the observed diversity of large-area and uniform stacking sequences. Low-symmetry stacking orders were observed using scanning transmission electron microscopy and detailed geometries were identified by density functional theory. A linear relation was also revealed between interlayer distance and stacking energy. These stacking sequences yield various energy alignments between the valence states at the Γ and K points of the Brillouin zone, showing stacking-dependent bandgaps and valence band tail states in the measured scanning tunneling spectroscopy. These results may benefit the design of two-dimensional multilayers with manipulable stacking orders.