Resonance-Enhanced Excitation of Interlayer Vibrations in Atomically Thin Black Phosphorus.

The strength of interlayer coupling critically affects the physical properties of 2D materials such as black phosphorus (BP), where the electronic structure depends sensitively on layer thickness. Rigid-layer vibrations reflect directly the interlayer coupling strength in 2D van der Waals solids, but measurement of these characteristic frequencies is made difficult by sample instability and small Raman scattering cross sections in atomically thin elemental crystals. Here, we overcome these challenges in BP by performing resonance-enhanced low-frequency Raman scattering under an argon-protective environment. Interlayer breathing modes for atomically thin BP were previously unobservable under conventional (nonresonant) excitation but became strongly enhanced when the excitation energy matched the sub-band electronic transitions of few-layer BP, down to bilayer thicknesses. The measured out-of-plane interlayer force constant was found to be 10.1 × 1019 N/m3 in BP, which is comparable to graphene. Accurate characterization of the interlayer coupling strength lays the foundation for future exploration of BP twisted structures and heterostructures.

Anapole enhanced on-chip routing of spin-valley photons in 2D materials for silicon integrated optical communication.

Controlling the propagation direction of polarized light is crucial for optical communications and functional optical components. However, all-dielectric on-chip technology exploiting valley photon emission in transition metal dichalcogenides with enhanced emission has yet to be fully explored. Here, we report a design for enhancing valley emission and manipulating valley photon propagation based on degenerate non-radiating anapole states. By placing circularly polarized dipoles on top of a C4 symmetric cross-slotted silicon disk, the rotating anapole state is excited with a Purcell factor up to two orders. In addition, the photon coupled to the preferred direction of the waveguide are about 2 times larger than that to the opposite direction. Our design could pave the way for realizing on-chip valley-dependent optical communication.

Dynamical Slowing-Down in an Ultrafast Photoinduced Phase Transition.

Complex systems, which consist of a large number of interacting constituents, often exhibit universal behavior near a phase transition. A slowdown of certain dynamical observables is one such recurring feature found in a vast array of contexts. This phenomenon, known as critical slowing-down, is well studied mostly in thermodynamic phase transitions. However, it is less understood in highly nonequilibrium settings, where the time it takes to traverse the phase boundary becomes comparable to the timescale of dynamical fluctuations. Using transient optical spectroscopy and femtosecond electron diffraction, we studied a photoinduced transition of a model charge-density-wave (CDW) compound LaTe_{3}. We observed that it takes the longest time to suppress the order parameter at the threshold photoexcitation density, where the CDW transiently vanishes. This finding can be captured by generalizing the time-dependent Landau theory to a system far from equilibrium. The experimental observation and theoretical understanding of dynamical slowing-down may offer insight into other general principles behind nonequilibrium phase transitions in many-body systems.

Sensitive Phonon-Based Probe for Structure Identification of 1T' MoTe2.

In this work, by combining transmission electron microscopy and polarized Raman spectroscopy for the 1T' MoTe2 flakes with different thicknesses, we found that the polarization dependence of Raman intensity is given as a function of excitation laser wavelength, phonon symmetry, and phonon frequency, but has weak dependence on the flake thickness from few-layer to multilayer. In addition, the frequency of Raman peaks and the relative Raman intensity are sensitive to flake thickness, which manifests Raman spectroscopy as an effective probe for thickness of 1T' MoTe2. Our work demonstrates that polarized Raman spectroscopy is a powerful and nondestructive method to quickly identify the crystal structure and thickness of 1T' MoTe2 simultaneously, which opens up opportunities for the in situ probe of anisotropic properties and broad applications of this novel material.

Vertically architectured stack of multiple graphene field-effect transistors for flexible electronics.

Vertically architectured stack of multiple graphene field-effect transistors (GFETs) on a flexible substrate show great mechanical flexibility and robustness. The four GFETs are integrated in the vertical direction, and dually gated GFETs with graphene channel, PMMA dielectrics, and graphene gate electrodes are realized.

Ultraviolet irradiation-controlled memory effect in graphene field-effect transistors.

Control of graphene memory devices using photons, via control of the charge-transfer process, is demonstrated by employing gate-voltage pulses to program/erase the memory elements. The hysteresis in the conductance-gate voltage-dependence of graphene field-effect transistors on a SiO2 substrate can be greatly enlarged by ultraviolet irradiation in both air and vacuum. An enhanced charge transfer between graphene and its surroundings, induced by ultraviolet illumination, is proposed.

Laser irradiation induced structural transformation in layered transition metal trichalcogenide nanoflakes.

Laser irradiation is a powerful tool in inducing changes in lattice structures and properties of two-dimensional (2D) materials through processes such as heating, bleaching, catalysis, etc. However, the underlying mechanisms of such transformations vary dramatically in different 2D materials. Here, we report the structural transformation of layered titanium trisulfide (TiS3) to titanium disulfide (TiS2) after irradiation. We systematically characterized the dependence of the transformation on laser power, flake thickness, irradiation time, and vacuum conditions using microscopic and spectroscopic methods. The underlying mechanism is confirmed as the heat-induced materials decomposition, a process that also occurs in many other transition metal trichalcogenide materials. Furthermore, we demonstrate that this spatial-resolved method also enables the creation of in-plane TiS3-TiS2 heterostructures. Our study identifies a new family of 2D materials that undergo a structural transformation after laser irradiation and enriches the methods available for developing new prototypes of low-dimensional devices in the future.

Intrinsic 1[Formula: see text] phase induced in atomically thin 2H-MoTe2 by a single terahertz pulse.

The polymorphic transition from 2H to 1[Formula: see text]-MoTe2, which was thought to be induced by high-energy photon irradiation among many other means, has been intensely studied for its technological relevance in nanoscale transistors due to the remarkable improvement in electrical performance. However, it remains controversial whether a crystalline 1[Formula: see text] phase is produced because optical signatures of this putative transition are found to be associated with the formation of tellurium clusters instead. Here we demonstrate the creation of an intrinsic 1[Formula: see text] lattice after irradiating a mono- or few-layer 2H-MoTe2 with a single field-enhanced terahertz pulse. Unlike optical pulses, the low terahertz photon energy limits possible structural damages. We further develop a single-shot terahertz-pump-second-harmonic-probe technique and reveal a transition out of the 2H-phase within 10 ns after photoexcitation. Our results not only provide important insights to resolve the long-standing debate over the light-induced polymorphic transition in MoTe2 but also highlight the unique capability of strong-field terahertz pulses in manipulating quantum materials.

A multimode photodetector with polarization-dependent near-infrared responsivity using the tunable split-dual gates control.

As the limited carrier densities in atomic thin materials can be well controlled by electrostatic gates, p-n junctions based on two-dimensional materials in the coplanar split-gate configuration can work as photodetectors or light-emitting diodes. These coplanar gates can be fabricated in a simple one-step lithography process and are frequently used in hybrid integration with on-chip optical structures. However, the polarization-dependent responsivity of such a configuration is less explored in the near-infrared band, and a clear understanding is still missing. Here we fabricate near-infrared tunable multiple modes twisted bilayer graphene photodetector enabled by the coplanar split-gate control and confirm that the photothermoelectric effect governs the photovoltage mechanism of the p-n junction mode. Our study also elucidates that the discrepancy of the responsivities under different linear polarizations is owing to the different cavity modes and provides a valuable example for designing chip-integrated optoelectronic devices.

Improved performance of ZnO nanowire field-effect transistors via focused ion beam treatment.

A seven orders of magnitude increase in the current on/off ratio of ZnO nanowire field-effect transistors (FETs) after Ga( + ) irradiation was observed. Transmission electron microscopy characterization revealed that the surface crystal quality of the ZnO nanowire was improved via the Ga( + ) treatment. The Ga( + ) irradiation efficiently reduces chemisorption effects and decreases oxygen vacancies in the surface layer. The enhanced performance of the nanowire FET was attributed to the decrease of surface trapped electrons and the decrease in carrier concentration.

A versatile sample fabrication method for ultrafast electron diffraction.

Integral to the exploration of nonequilibrium phenomena in solid-state systems is the study of lattice motion after photoexcitation by a femtosecond laser pulse. For the past two decades, ultrafast electron diffraction (UED) has played a critical role in this regard. Despite remarkable progress in instrumental development, this technique is still bottlenecked by a demanding sample preparation process, where ultrathin single crystals of large lateral size are typically required. In this work, we describe an efficient, versatile method that yields high-quality, laterally extended (≥ 100 µm), and thin (≤ 50 nm) single crystals on amorphous films of Si3N4 windows. It applies to most exfoliable materials, including those reactive in ambient conditions, and promises clean, flat surfaces. Besides the natural extension to fabricating van der Waals heterostructures, our method can also be applied to future-generation UED that enables additional control of sample parameters, such as electrostatic gating and excitation by a locally enhanced terahertz field. Our work significantly expands the type of samples for UED studies and also finds application in other time-resolved techniques such as attosecond extreme-ultraviolet absorption spectroscopy. This method hence provides further opportunities to explore photoinduced transitions and to discover novel states of matter out of equilibrium.

Observation of thickness-tuned universality class in superconducting ß-W thin films.

The interplay between quenched disorder and critical behavior in quantum phase transitions is conceptually fascinating and of fundamental importance for understanding phase transitions. However, it is still unclear whether or not the quenched disorder influences the universality class of quantum phase transitions. More crucially, the absence of superconducting-metal transitions under in-plane magnetic fields in 2D superconductors imposes constraints on the universality of quantum criticality. Here, we observe the thickness-tuned universality class of superconductor-metal transition by changing the disorder strength in ß-W films with varying thickness. The finite-size scaling uncovers the switch of universality class: quantum Griffiths singularity to multiple quantum criticality at a critical thickness of tc⊥1~8nm and then from multiple quantum criticality to single criticality at tc⊥2~16nm. Moreover, the superconducting-metal transition is observed for the first time under in-plane magnetic fields and the universality class is changed at tc‖~8nm. The observation of thickness-tuned universality class under both out-of-plane and in-plane magnetic fields provides broad information for the disorder effect on superconducting-metal transitions and quantum criticality.

Deep-Learning-Enabled Fast Optical Identification and Characterization of 2D Materials.

Advanced microscopy and/or spectroscopy tools play indispensable roles in nanoscience and nanotechnology research, as they provide rich information about material processes and properties. However, the interpretation of imaging data heavily relies on the "intuition" of experienced researchers. As a result, many of the deep graphical features obtained through these tools are often unused because of difficulties in processing the data and finding the correlations. Such challenges can be well addressed by deep learning. In this work, the optical characterization of 2D materials is used as a case study, and a neural-network-based algorithm is demonstrated for the material and thickness identification of 2D materials with high prediction accuracy and real-time processing capability. Further analysis shows that the trained network can extract deep graphical features such as contrast, color, edges, shapes, flake sizes, and their distributions, based on which an ensemble approach is developed to predict the most relevant physical properties of 2D materials. Finally, a transfer learning technique is applied to adapt the pretrained network to other optical identification applications. This artificial-intelligence-based material characterization approach is a powerful tool that would speed up the preparation, initial characterization of 2D materials and other nanomaterials, and potentially accelerate new material discoveries.

A MoTe2-based light-emitting diode and photodetector for silicon photonic integrated circuits.

One of the current challenges in photonics is developing high-speed, power-efficient, chip-integrated optical communications devices to address the interconnects bottleneck in high-speed computing systems. Silicon photonics has emerged as a leading architecture, in part because of the promise that many components, such as waveguides, couplers, interferometers and modulators, could be directly integrated on silicon-based processors. However, light sources and photodetectors present ongoing challenges. Common approaches for light sources include one or few off-chip or wafer-bonded lasers based on III-V materials, but recent system architecture studies show advantages for the use of many directly modulated light sources positioned at the transmitter location. The most advanced photodetectors in the silicon photonic process are based on germanium, but this requires additional germanium growth, which increases the system cost. The emerging two-dimensional transition-metal dichalcogenides (TMDs) offer a path for optical interconnect components that can be integrated with silicon photonics and complementary metal-oxide-semiconductors (CMOS) processing by back-end-of-the-line steps. Here, we demonstrate a silicon waveguide-integrated light source and photodetector based on a p-n junction of bilayer MoTe2, a TMD semiconductor with an infrared bandgap. This state-of-the-art fabrication technology provides new opportunities for integrated optoelectronic systems.

Photovoltaic Effect and Evidence of Carrier Multiplication in Graphene Vertical Homojunctions with Asymmetrical Metal Contacts.

Graphene exhibits exciting potentials for high-speed wideband photodetection and high quantum efficiency solar energy harvest because of its broad spectral absorption, fast photoelectric response, and potential carrier multiplication. Although photocurrent can be generated near a metal-graphene interface in lateral devices, the photoactive area is usually limited to a tiny one-dimensional line-like interface region. Here, we report photoelectric devices based on vertical graphene two-dimensional homojunction, which is fabricated via vertically stacking four graphene monolayers with asymmetric metal contacts. The devices show excellent photovoltaic output with excitation wavelength ranging from visible light to mid-infrared. The wavelength dependence of the internal quantum efficiency gives direct evidence of the carrier multiplication effect in graphene. The simple fabrication process, easy scale-up, large photoresponsive active area, and broadband response of the vertical graphene device are very promising for practical applications in optoelectronics and photovoltaics.

Vibrational spectroscopy at electrolyte/electrode interfaces with graphene gratings.

Microscopic understanding of physical and electrochemical processes at electrolyte/electrode interfaces is critical for applications ranging from batteries, fuel cells to electrocatalysis. However, probing such buried interfacial processes is experimentally challenging. Infrared spectroscopy is sensitive to molecule vibrational signatures, yet to approach the interface three stringent requirements have to be met: interface specificity, sub-monolayer molecular detection sensitivity, and electrochemically stable and infrared transparent electrodes. Here we show that transparent graphene gratings electrode provide an attractive platform for vibrational spectroscopy at the electrolyte/electrode interfaces: infrared diffraction from graphene gratings offers enhanced detection sensitivity and interface specificity. We demonstrate the vibrational spectroscopy of methylene group of adsorbed sub-monolayer cetrimonium bromide molecules and reveal a reversible field-induced electrochemical deposition of cetrimonium bromide on the electrode controlled by the bias voltage. Such vibrational spectroscopy with graphene gratings is promising for real time and in situ monitoring of different chemical species at the electrolyte/electrode interfaces.

Stretch-induced stiffness enhancement of graphene grown by chemical vapor deposition.

The mechanical properties of ultrathin membranes have attracted considerable attention recently. Nanoindentation based on atomic force microscopy is commonly employed to study mechanical properties. We find that the data processing procedures in previous studies are nice approximations, but it is difficult for them to illustrate the mechanical properties precisely. Accordingly, we develop a revised numerical method to describe the force curve properly, by which the intrinsic mechanical properties of these membranes can be acquired. Combining the nanoindentation measurements with the revised numerical method, we demonstrate that loading-unloading cycles under large load can lead to a pronounced improvement in stiffness of graphene grown by chemical vapor deposition (CVD). The Young's moduli of the stretched CVD graphene membranes can be improved to ∼1 TPa, closing to the value of the pristine graphene. Our findings demonstrate a possible way to recover the exceptional elastic properties of CVD graphene from the softened stiffness caused by wrinkles.

Graphene plasmon enhanced photoluminescence in ZnO microwires.

We report the temperature dependent photoluminescence (PL) properties of monolayer graphene-Au-nanoparticle-ZnO (GAZ) microwire hybrid structures. By comparing with the bare ZnO wire without coverage of graphene, a three times enhancement of PL was found in the GAZ hybrid structures. The enhancement is attributed to the coupling between the PL photons from ZnO and the graphene surface plasmons with ~1-2 nm Au as a corrugated surface. Our results may be valuable for designing graphene-ZnO hybrid based optical and photoelectrical devices.

Layer-by-layer assembly of vertically conducting graphene devices.

Graphene has various potential applications owing to its unique electronic, optical, mechanical and chemical properties, which are primarily based on its two-dimensional nature. Graphene-based vertical devices can extend the investigations and potential applications range to three dimensions, while interfacial properties are crucial for the function and performance of such graphene vertical devices. Here we report a general method to construct graphene vertical devices with controllable functions via choosing different interfaces between graphene and other materials. Two types of vertically conducting devices are demonstrated: graphene stacks sandwiched between two Au micro-strips, and between two Co layers. The Au|graphene|Au junctions exhibit large magnetoresistance with ratios up to 400% at room temperature, which have potential applications in magnetic field sensors. The Co|graphene|Co junctions display a robust spin valve effect at room temperature. The layer-by-layer assembly of graphene offers a new route for graphene vertical structures.

Synthesis and quantum transport properties of Bi2Se3 topological insulator nanostructures.

Bi2Se3 nanocrystals with various morphologies, including nanotower, nanoplate, nanoflake, nanobeam and nanowire, have been synthesized. Well-distinguished Shubnikov-de Haas (SdH) oscillations were observed in Bi2Se3 nanoplates and nanobeams. Careful analysis of the SdH oscillations suggests the existence of Berry's phase π, which confirms the quantum transport of the surface Dirac fermions in both Bi2Se3 nanoplates and nanobeams without intended doping. The observation of the singular quantum transport of the topological surface states implies that the high-quality Bi2Se3 nanostructures have superiorities for investigating the novel physical properties and developing the potential applications.