Quantum Griffiths Singularity in Ordered Artificial Superconducting-Islands-Array on Graphene.

Quantum Griffiths phase (QGP) is a novel quantum phenomenon of quantum phase transition in two-dimensional (2D) superconductors, and the emergence of inhomogeneous superconducting rare regions immersed in a metallic matrix is theoretically related to the quantum Griffiths singularity (QGS). However, the theoretical proposal of superconducting rare regions still lacks intuitive experimental verification. Here, we construct an artificial ordered superconducting-islands-array on monolayer graphene with the aid of an anodic aluminum oxide (AAO) membrane. The QGS under both in-plane and out-of-plane magnetic fields is evidenced by the divergent dynamical critical exponent and is in compliance with the direct activated scaling behavior. The phase diagram clearly shows that the QGP is indeed bred in the rare superconducting regions within isolated superconducting islands with a vanished quantum coherence. Our results reveal the universal features of QGP in artificial heterostructured systems and provide a visualized platform for the theoretical proposal of QGS.

Self-rolling of vanadium dioxide nanomembranes for enhanced multi-level solar modulation.

Thermochromic window develops as a competitive solution for carbon emissions due to comprehensive advantages of its passivity and effective utilization of energy. How to further enhance the solar modulation ([Formula: see text]) of thermochromic windows while ensuring high luminous transmittance ([Formula: see text]) becomes the latest challenge to touch the limit of energy efficiency. Here, we show a smart window combining mechanochromism with thermochromism by self-rolling of vanadium dioxide (VO2) nanomembranes to enhance multi-level solar modulation. The mechanochromism is introduced by the temperature-controlled regulation of curvature of rolled-up smart window, which benefits from effective strain adjustment in VO2 nanomembranes upon the phase transition. Under geometry design and optimization, the rolled-up smart window with high [Formula: see text] and [Formula: see text] is achieved for the modulation of indoor temperature self-adapted to seasons and climate. Furthermore, such rolled-up smart window enables high infrared reflectance after triggered phase transition and acts as a smart lens protective cover for strong radiation. This work supports the feasibility of self-rolling technology in smart windows and lens protection, which promises broad interest and practical applications of self-adapting devices and systems for smart building, intelligent sensors and actuators with the perspective of energy efficiency.

Submillimeter-scale multimaterial terrestrial robots.

Robots with submillimeter dimensions are of interest for applications that range from tools for minimally invasive surgical procedures in clinical medicine to vehicles for manipulating cells/tissues in biology research. The limited classes of structures and materials that can be used in such robots, however, create challenges in achieving desired performance parameters and modes of operation. Here, we introduce approaches in manufacturing and actuation that address these constraints to enable untethered, terrestrial robots with complex, three-dimensional (3D) geometries and heterogeneous material construction. The manufacturing procedure exploits controlled mechanical buckling to create 3D multimaterial structures in layouts that range from arrays of filaments and origami constructs to biomimetic configurations and others. A balance of forces associated with a one-way shape memory alloy and the elastic resilience of an encapsulating shell provides the basis for reversible deformations of these structures. Modes of locomotion and manipulation span from bending, twisting, and expansion upon global heating to linear/curvilinear crawling, walking, turning, and jumping upon laser-induced local thermal actuation. Photonic structures such as retroreflectors and colorimetric sensing materials support simple forms of wireless monitoring and localization. These collective advances in materials, manufacturing, actuation, and sensing add to a growing body of capabilities in this emerging field of technology.

2D Transition Metal Dichalcogenide with Increased Entropy for Piezoelectric Electronics.

Piezoelectricity in 2D transition metal dichalcogenides (TMDs) has attracted considerable interest because of their excellent flexibility and high piezoelectric coefficient compared to conventional piezoelectric bulk materials. However, the ability to regulate the piezoelectric properties is limited because the entropy is constant for certain binary TMDs other than multielement ones. Herein, in order to increase the entropy, a ternary TMDs alloy, Mo1- x Wx S2 , with different W concentrations, is synthesized. The W concentration in the Mo1- x Wx S2 alloy can be controlled precisely in the low-supersaturation synthesis and the entropy can be tuned accordingly. The Mo0.46 W0.54 S2 alloy (x = 0.54) has the highest configurational entropy and best piezoelectric properties, such as a piezoelectric coefficient of 4.22 pm V-1 and a piezoelectric output current of 150 pA at 0.24% strain. More importantly, it can be combined into a larger package to increase the output current to 600 pA to cater to self-powered applications. Combining with excellent mechanical durability, a mechanical sensor based on the Mo0.46 W0.54 S2 alloy is demonstrated for real-time health monitoring.

Atomistic Observation of the Local Phase Transition in MoTe2 for Application in Homojunction Photodetectors.

Direct atomic-scale observation of the local phase transition in transition metal dichalcogenides (TMDCs) is critically required to carry out in-depth studies of their atomic structures and electronic features. However, the structural aspects including crystal symmetries tend to be unclear and unintuitive in real-time monitoring of the phase transition process. Herein, by using in situ transmission electron microscopy, information about the phase transition mechanism of MoTe2 from hexagonal structure (2H phase) to monoclinic structure (1T' phase) driven by sublimation of Te atoms after a spike annealing is obtained directly. Furthermore, with the control of Te atom sublimation by modulating the hexagonal boron nitride (h-BN) coverage in the desired area, the lateral 1T'-enriched MoTe2 /2H MoTe2 homojunction can be one-step constructed via an annealing treatment. Owing to the gradient bandgap provided by 1T'-enriched MoTe2 and 2H MoTe2 , the photodetector composed of the 1T'-enriched MoTe2 /2H MoTe2 homojunction shows fast photoresponse and ten times larger photocurrents than that consisting of a pure 2H MoTe2 channel. The study reveals a route to improve the performance of optoelectronic and electronic devices based on TMDCs with both semiconducting and semimetallic phases.

Self-Rolling of Monolayer Graphene for Ultrasensitive Molecular Sensing.

The controllable manipulation of graphene to create three-dimensional (3D) structures is an intriguing approach for favorably tuning its properties and creating new types of 3D devices. However, due to extremely low bending stiffnesses, it is rather challenging to construct monolayer graphene into stable 3D structures. Here, we demonstrate the stable formation of monolayer graphene microtubes with accompanying pre-patterned strain layers. The diameter of graphene microtubes can be effectively tuned by changing the thickness of the strain layers. Benefiting from a high surface-to-volume ratio of the tubular geometry, the 3D geometry leads to a prominent Raman enhancement, which was further applied to molecular sensing. The R6G molecules on graphene microtubes can be detected even for a concentration as low as 10-11 M. We believe that this method can be a generalized way to realize the 3D tubular structure of other 2D materials.

Graphene-mediated ferromagnetic coupling in the nickel nano-islands/graphene hybrid.

Nanoscale magnetic structures are fundamental to the design and fabrication of spintronic devices and have exhibited tremendous potential superior to the conventional semiconductor devices. However, most of the magnetic moments in nanostructures are unstable due to size effect, and the possible solution based on exchange coupling between nanomagnetism is still not clear. Here, graphene-mediated exchange coupling between nanomagnets is demonstrated by depositing discrete superparamagnetic Ni nano-islands on single-crystal graphene. The heterostructure exhibits ideal two-dimensional (2D) ferromagnetism with clear hysteresis loops and Curie temperature up to 80 K. The intrinsic ferromagnetism in graphene and antiferromagnetic exchange coupling between graphene and Ni nano-islands are revealed by x-ray magnetic circular dichroism and density functional theory calculations. The artificial 2D ferromagnets constitute a platform to study the coupling mechanism between complex correlated electronic systems and magnetism on the nanoscale, and the results and concept provide insights into the realization of spin manipulation in quantum computing.

Gaussian-preserved, non-volatile shape morphing in three-dimensional microstructures for dual-functional electronic devices.

Motile plant structures such as Mimosa pudica leaves, Impatiens glandulifera seedpods, and Dionaea muscipula leaves exhibit fast nastic movements in a few seconds or less. This motion is stimuli-independent mechanical movement following theorema egregium rules. Artificial analogs of tropistic motion in plants are exemplified by shape-morphing systems, which are characterized by high functional robustness and resilience for creating 3D structures. However, all shape-morphing systems developed so far rely exclusively on continuous external stimuli and result in slow response. Here, we report a Gaussian-preserved shape-morphing system to realize ultrafast shape morphing and non-volatile reconfiguration. Relying on the Gaussian-preserved rules, the transformation can be triggered by mechanical or thermal stimuli within a microsecond. Moreover, as localized energy minima are encountered during shape morphing, non-volatile configuration is preserved by geometrically enhanced rigidity. Using this system, we demonstrate a suite of electronic devices that are reconfigurable, and therefore, expand functional diversification.

Microdroplet-guided intercalation and deterministic delamination towards intelligent rolling origami.

Three-dimensional microstructures fabricated by origami, including folding, rolling and buckling, gain great interests in mechanics, optics and electronics. We propose a general strategy on on-demand and spontaneous rolling origami for artificial microstructures aiming at massive and intelligent production. Deposited nanomembranes are rolled-up in great amount triggered by the intercalation of tiny droplet, taking advantage of a creative design of van der Waals interaction with substrate. The rolling of nanomembranes delaminated by liquid permits a wide choice in materials as well as precise manipulation in rolling direction by controlling the motion of microdroplet, resulting in intelligent construction of rolling microstructures with designable geometries. Moreover, this liquid-triggered delamination phenomenon and constructed microstructures are demonstrated in the applications among vapor sensing, microresonators, micromotors, and microactuators. This investigation offers a simple, massive, low-cost, versatile and designable construction of rolling microstructures for fundamental research and practical applications.

Rolling up MoSe2 Nanomembranes as a Sensitive Tubular Photodetector.

Transition metal dichalcogenides, as a kind of 2D material, are suitable for near-infrared to visible photodetection owing to the bandgaps ranging from 1.0 to 2.0 eV. However, limited light absorption restricts photoresponsivity due to the ultrathin thickness of 2D materials. 3D tubular structures offer a solution to solve the problem because of the light trapping effect which can enhance optical absorption. In this work, thanks to mechanical flexibility of 2D materials, self-rolled-up technology is applied to build up a 3D tubular structure and a tubular photodetector is realized based on the rolled-up molybdenum diselenide microtube. The tubular device is shown to present one order higher photosensitivity compared with planar counterparts. Enhanced optical absorption arising from the multiple reflections inside the tube is the main reason for the increased photocurrent. This tubular device offers a new design for increasing the efficiency of transition metal dichalcogenide-based photodetection and could hold great potential in the field of 3D optoelectronics.

Silicon nanomembrane-based near infrared phototransistor with positive and negative photodetections.

Surface plasmon polariton induces hot carrier injection that enables near infrared photodetection in Si nanomembranes and is of great significance for Si photonics integrated circuits. In this study, near infrared photodiode and phototransistor based on Si nanomembranes are designed and demonstrated, where the channel carrier concentration can be tuned through a gate modulation to implement both positive and negative photodetections. Through patterning a nanogroove array, Si nanomembrane-based photodetector exhibits high performance in near infrared range with an Ion/Ioff ratio of 102, and a responsivity of 7 mA W-1, under 1550 nm laser irradiation. Moreover, the photodetection ability, determined by Ioff/Ion can be further enhanced to ∼6 × 102 when the photodetector is modulated to work at the negative photodetection mode. Our study may provide a practical approach with fundamental guidelines and designs for fabricating high-performance Si-based infrared photodetection, which promotes the development of Si photonics.

Rolled-up single-layered vanadium oxide nanomembranes for microactuators with tunable active temperature.

Multilayer vanadium dioxide (VO2) actuators are a widespread concern as these micro/nano-actuators present a fast and efficient dynamic response when VO2 occurs in metal-insulator transition (MIT) at 68 °C. By tuning the O2 flow rate during oxide deposition and rolled-up nanotechnology, a microactuator based on a single-layered vanadium oxide nanomembrane with vertical component gradient is fabricated. Upward bending of the nanomembrane is driven by the release of the compressive strain gradient which is revealed through the difference in Raman shift of the vibration mode. Combining strain engineering, the initial curvature of microactuators is tuned in a wide range by the thickness of the nanomembranes. The actuation behavior from low curvature to high final curvature across the MIT is observed which depends on the nanomembrane thickness. Initial compressive strain distribution of the rolled-up nanomembrane decreases the MIT temperature simultaneously. Thus, taking advantage of the tunable MIT and reversible shape transformation, micro/nano-actuators with tunable triggering temperature, controllable initial curvature and large-displacement actuation are fabricated for curvature engineering in micromechanical systems.

On-Chip Rolling Design for Controllable Strain Engineering and Enhanced Photon-Phonon Interaction in Graphene.

On-chip strain engineering is highly demanded in 2D materials as an effective route for tuning their extraordinary properties and integrating consistent functionalities toward various applications. Herein, rolling technique is proposed for strain engineering in monolayer graphene grown on a germanium substrate, where compressive or tensile strain could be acquired, depending on the designed layer stressors. Unusual compressive strains up to 0.30% are achieved in the rolled-up graphene tubular structures. The subsequent phonon hardening under compressive loading is observed through strain-induced Raman G band splitting, while distinct blueshifts of characteristic peaks (G+ , G- , or 2D) can be well regulated on an asymmetric tubular structure with a strain variation. In addition, due to the strong confinement of the local electromagnetic field under 3D tubular geometry, the photon-phonon interaction is highly strengthened, and thus, the Raman scattering of graphene in rolled-up tubes is enhanced. Such an on-chip rolling approach leads to a superior strain tuning method in 2D materials and could improve their light-matter interaction in a tubular configuration, which may hold great capability in 2D materials integration for on-chip applications such as in mechanics, electronics, and photonics.

Selected and Enhanced Single Whispering-Gallery Mode Emission from a Mesostructured Nanomembrane Microcavity.

Quantum sciences are revolutionizing computing and communication technologies, in which single-photon emitters are the key components for creating strong quantum entanglement. Color centers in diamonds in coupled-cavity systems are considered great candidates for the efficient generation of quantum carriers over other solid-state emitters. Owing to the multi-mode nature of high quality factor ( Q) diamond cavities, however, it is a grand challenge to the achievement of single photon emission with high rate and indistinguishability. To this end, a single-mode high- Q diamond cavity is highly desired. Here, we report a diamond mesostructured nanomembrane microcavity of a discrete rotational symmetry that selectively produces the desired single-mode emission in a broad spectrum. The strategic rolling up of a flexible diamond nanomembrane with aligned holes effectively defines the designed symmetry while maintaining the high- Q resonance through the whispering-gallery mode supported in the central hollow microcavity. The demonstrated diamond mesostructured microcavity features a distinct and enhanced single-mode emission, a step toward efficient quantum sources with designed positions or bands for quantum information technology.

Infrared tubular microcavity based on rolled-up GeSn/Ge nanomembranes.

Germanium-Tin (GeSn) alloys have attracted great amounts of attention as these group IV semiconductors present direct band-gap behavior with high Sn content and are compatible with current complementary metal oxide semiconductor technology. In this work, three dimensional tubular GeSn/Ge micro-resonators with a diameter of around 7.3 µm were demonstrated by rolling up GeSn nanomembranes (NM) grown on a Ge-on-insulator wafer via molecular beam epitaxy. The microstructural properties of the resonators were carefully investigated and the strain distributions of the rolled-up GeSn/Ge microcavities along the radial direction were studied by utilizing micro-Raman spectroscopy with different excitation laser wavelengths. The values of the strains calculated from Raman shifts agree well with the theoretical prediction. Coupled with fiber tapers, as-fabricated devices present a high quality factor of up to 800 in the transmission spectral measurements. The micro-resonators fabricated via rolled-up nanotechnology and GeSn/Ge NMs in this work may have great potential in photonic micro- and nanodevices.

Multifunctional Nanocracks in Silicon Nanomembranes by Notch-Assisted Transfer Printing.

Manipulating nanocracks to produce various nanodevices has attracted increasing interest. Here, based on the mature transfer printing technique, a novel notch-assisted transfer printing technique was engaged to produce nanocracks by simply introducing notch structures into the transferred nanomembranes. Both experiments and finite element simulations were used to elucidate the probability of nanocrack formation during the transfer process, and the results demonstrated that the geometry of nanomembranes played a key role in concentrating stress and producing nanocracks. We further demonstrated that the obtained nanocrack can be used as a surface-enhanced Raman scattering substrate because of the significant enhancement of electric fields. In addition, the capillary condensation of water molecules in the nanocrack led to an obvious change of resistance, thus providing an opportunity for the crack-based structure to be used as an ultrasensitive humidity sensor. The current approach can be applied to producing nanocracks from multiple materials and will have important applications in the field of nanodevices.

Anisotropic Rolling and Controlled Chirality of Nanocrystalline Diamond Nanomembranes toward Biomimetic Helical Frameworks.

Future advances in materials will be aided by improved dimensional control in fabrication of 3D hierarchical structures. Self-rolling technology provides additional degrees of freedom in 3D design by enabling an arbitrary rolling direction with controllable curvature. Here, we demonstrate that deterministic helical structures with variable rolling directions can be formed through releasing a strained nanomembrane patterned in a "utility knife" shape. The asymmetry of the membrane shape provides anisotropic driving force generated by the disparity between the etching rates along different sides in this asymmetric shape. A transient finite element method (FEM) model of diagonal rolling is established to analyze the relationships among geometries, elastic properties, and boundary conditions. On the basis of this model, a diamond-based helical framework consisting of two or three helical segments has been fabricated to mimic the shapes of natural plants. Further experiment has been done to extend this approach to other materials and material combinations, such as MoSe2/Cr, Cr/Pt, and VO2. To demonstrate the possible application accessible by our technology to new fields, VO2-based helical microscale actuation has been demonstrated with photocontrollable bending in a selected region, as well as morphable and recognizable helix. This study offers a new way to construct helical mesostructures that combine special properties of the advanced materials, thus possess novel features and potential applications.

Stimuli-responsive and on-chip nanomembrane micro-rolls for enhanced macroscopic visual hydrogen detection.

Nanomembrane rolling offers advanced three-dimensional (3D) mesostructures in electronics, optics, and biomedical applications. We demonstrate a high-density and on-chip array of rolled-up nanomembrane actuators with stimuli-responsive function based on the volume expansion of palladium in hydrogen milieu. The uniform stimuli-responsive behavior of high-density nanomembrane rolls leads to huge macroscopic visual detection with more than 50% transmittance change under optimization of micropattern design. The reversible shape changing between rolled and flat (unrolled) statuses can be well explained on the basis of the elastic mechanical model. The strain change in the palladium layer during hydrogen absorption and desorption produces a marked change in the diameter of nanomembrane rolls. We found that a functional palladium layer established an external compressive strain after hydrogen stimuli and thus also reduced the rolls' diameters. The large area of the nanomembrane roll array performs excellent nonelectrical hydrogen detection, with response and recovery speeds within seconds. Our work suggests a new strategy to integrate high-density 3D mesoscale architectures into functional devices and systems.

Reconfigurable Vanadium Dioxide Nanomembranes and Microtubes with Controllable Phase Transition Temperatures.

Two additional structural forms, free-standing nanomembranes and microtubes, are reported and added to the vanadium dioxide (VO2) material family. Free-standing VO2 nanomembranes were fabricated by precisely thinning as-grown VO2 thin films and etching away the sacrificial layer underneath. VO2 microtubes with a range of controllable diameters were rolled-up from the VO2 nanomembranes. When a VO2 nanomembrane is rolled-up into a microtubular structure, a significant compressive strain is generated and accommodated therein, which decreases the phase transition temperature of the VO2 material. The magnitude of the compressive strain is determined by the curvature of the VO2 microtube, which can be rationally and accurately designed by controlling the tube diameter during the rolling-up fabrication process. The VO2 microtube rolling-up process presents a novel way to controllably tune the phase transition temperature of VO2 materials over a wide range toward practical applications. Furthermore, the rolling-up process is reversible. A VO2 microtube can be transformed back into a nanomembrane by introducing an external strain. Because of its tunable phase transition temperature and reversible shape transformation, the VO2 nanomembrane-microtube structure is promising for device applications. As an example application, a tubular microactuator device with low driving energy but large displacement is demonstrated at various triggering temperatures.