Reversible Transition of Semiconducting PtSe2 and Metallic PtTe2 for Scalable All-2D Edge-Contacted FETs.

Two-dimensional (2D) transition metal dichalcogenide (TMD) layers are highly promising as field-effect transistor (FET) channels in the atomic-scale limit. However, accomplishing this superiority in scaled-up FETs remains challenging due to their van der Waals (vdW) bonding nature with respect to conventional metal electrodes. Herein, we report a scalable approach to fabricate centimeter-scale all-2D FET arrays of platinum diselenide (PtSe2) with in-plane platinum ditelluride (PtTe2) edge contacts, mitigating the aforementioned challenges. We realized a reversible transition between semiconducting PtSe2 and metallic PtTe2 via a low-temperature anion exchange reaction compatible with the back-end-of-line (BEOL) processes. All-2D PtSe2 FETs seamlessly edge-contacted with transited metallic PtTe2 exhibited significant performance improvements compared to those with surface-contacted gold electrodes, e.g., an increase of carrier mobility and on/off ratio by over an order of magnitude, achieving a maximum hole mobility of ∼50.30 cm2 V-1 s-1 at room temperature. This study opens up new opportunities toward atomically thin 2D-TMD-based circuitries with extraordinary functionalities.

Large-area vertically aligned 2D MoS2layers on TEMPO-cellulose nanofibers for biodegradable transient gas sensors.

Crystallographically anisotropic two-dimensional (2D) molybdenum disulfide (MoS2) with vertically aligned (VA) layers is attractive for electrochemical sensing owing to its surface-enriched dangling bonds coupled with extremely large mechanical deformability. In this study, we explored VA-2D MoS2layers integrated on cellulose nanofibers (CNFs) for detecting various volatile organic compound gases. Sensor devices employing VA-2D MoS2/CNFs exhibited excellent sensitivities for the tested gases of ethanol, methanol, ammonia, and acetone; e.g. a high response rate up to 83.39% for 100 ppm ethanol, significantly outperforming previously reported sensors employing horizontally aligned 2D MoS2layers. Furthermore, VA-2D MoS2/CNFs were identified to be completely dissolvable in buffer solutions such as phosphate-buffered saline solution and baking soda buffer solution without releasing toxic chemicals. This unusual combination of high sensitivity and excellent biodegradability inherent to VA-2D MoS2/CNFs offers unprecedented opportunities for exploring mechanically reconfigurable sensor technologies with bio-compatible transient characteristics.

Efficient and additive-free synthesis of morphology variant iron oxyhydroxide nanostructures for phosphate adsorption application.

Iron oxyhydroxide (FeOOH) nanostructures of different shapes were successfully synthesized on flexible textile cloth of polyester using a novel and simple technique based on hydrolysis method. The technique used herein is newly designed specifically to improve the efficiency in terms of energy, simplicity and cost involved in large scale synthesis of nanostructured thin films. Additionally, the morphology of nano-sized iron oxyhydroxide could be tuned into different shapes through variation in the type of precursors used for synthesis. The uniformity and adhesion of the depositions were also found to be excellent as examined by qualitative techniques. The as-deposited samples exhibited monoclinic and orthorhombic structures of FeOOH. A significant variation in the shape of as-deposited FeOOH nanostructures with change in precursor was observed through morphological studies, which displayed lance-shaped, rounded clusters and rod-like growth features in different cases. The nanocrystalline FeOOH can be directly applied to attract and trap phosphate from water reservoirs, thus contributing to environmental solutions. The proposed technique can also be utilized to deposit larger areas, which could be suitable for practical applications.

Automated Assembly of Wafer-Scale 2D TMD Heterostructures of Arbitrary Layer Orientation and Stacking Sequence Using Water Dissoluble Salt Substrates.

We report a novel strategy to assemble wafer-scale two-dimensional (2D) transition metal dichalcogenide (TMD) layers of well-defined components and orientations. We directly grew a variety of 2D TMD layers on "water-dissoluble" single-crystalline salt wafers and precisely delaminated them inside water in a chemically benign manner. This manufacturing strategy enables the automated integration of vertically aligned 2D TMD layers as well as 2D/2D heterolayers of arbitrary stacking orders on exotic substrates insensitive to their kind and shape. Furthermore, the original salt wafers can be recycled for additional growths, confirming high process sustainability and scalability. The generality and versatility of this approach have been demonstrated by developing proof-of-concept "all 2D" devices for diverse yet unconventional applications. This study is believed to shed a light on leveraging opportunities of 2D TMD layers toward achieving large-area mechanically reconfigurable devices of various form factors at the industrially demanded scale.

High-performance flexible asymmetric supercapacitor based on rGO anode and WO3/WS2 core/shell nanowire cathode.

Flexible smart electronics require their energy storage device to be flexible in nature. Developing high-performance flexible energy storage devices require direct integration of electrode active materials on current collectors to satisfy the high electronic/ionic conductivity and long-term durability requirements. Herein, we develop a flexible all-solid-state asymmetric supercapacitor comprised of reduced graphene oxide (rGO) and core/shell tungsten trioxide/tungsten disulfide (WO3/WS2) nanowire based electrodes. The electrodes synthesized via electrochemical deposition and chemical vapor deposition avoided the necessity to use non-conductive binders and offered excellent cyclic stability. The structural integrity provided by the rGO and WO3/WS2 electrodes facilitated excellent electrochemical stability with capacitance retention of 90% and 100% after 10 000 charge-discharge cycles, respectively. An all-solid-state device provides a voltage window of 1.5 V and more than 70% capacitance retention after 10 000 charge-discharge cycles. Providing 97% capacitance retention upon mechanical bending reveals its potential to be used as an energy storage devices in flexible electronics.

Simultaneous and synergistic effect of heavy metal adsorption on the enhanced photocatalytic performance of a visible-light-driven RS-TONR/TNT composite.

A hydrothermally synthesized rhodium/antimony co-doped TiO2 nanorod and titanate nanotube (RS-TONR/TNT) composite was prepared for removal of heavy metals and organic pollutants from water under visible light irradiation. The composite provides the dual function of simultaneous adsorption of heavy metal ions and enhanced degradation of dissolved organic compounds. Acid treatment transformed titanate nanotubes to irregular tubular structures distributed homogeneously over untransformed RS/TONRs. Synergistic removal and degradation was studied with various heavy metals, Orange (II) dye, and Bisphenol A. The adsorption capacity of the composite for heavy metal ions was Pb(II) > Cd(II) > Cu(II) > Zn(II). The adsorbed metals enhanced photocatalytic degradation of the organic pollutants, but Cu was most effective, with degradation exceeding 70% for the dye and 80% for Bisphenol A after 5 h of treatment. Photocatalytic activity was enhanced more by adsorption than photodeposition of Cu ions. A decrease in XRD rutile peak intensity with adsorbed metal indicates a change in crystallinity which may enhance photocatalytic activity. Thick and bulging nanostructures in FE-SEM images signify ion adsorption within titanate pores. BET analysis indicated titanate nanotubes with adsorbed metal are mesoporous but their tubular structure persists. XPS showed more active Cu 2p3/2 states under light, supporting an active role of Cu+ in photocatalytic ROS generation. Detection of ROS and Cu species using methanol, EDTA, pCBA, and benzoic acid probes provided strong evidence for degradation via a charge transfer mechanism. Findings demonstrate the potential of the RS-TONR/TNT composite for simultaneous removal of heavy metals and degradation of organic pollutants.

Experimental Realization of Few Layer Two-Dimensional MoS2 Membranes of Near Atomic Thickness for High Efficiency Water Desalination.

A globally imminent shortage of freshwater has been demanding viable strategies for improving desalination efficiencies with the adoption of cost- and energy-efficient membrane materials. The recently explored 2D transition metal dichalcogenides (2D TMDs) of near atomic thickness have been envisioned to offer notable advantages as high-efficiency membranes owing to their structural uniqueness; that is, extremely small thickness and intrinsic atomic porosity. Despite theoretically projected advantages, experimental realization of near atom-thickness 2D TMD-based membranes and their desalination efficiency assessments have remained largely unexplored mainly due to the technical difficulty associated with their seamless large-scale integration. Herein, we report the experimental demonstration of high-efficiency water desalination membranes based on few-layer 2D molybdenum disulfide (MoS2) of only ∼7 nm thickness. Chemical vapor deposition (CVD)-grown centimeter-scale 2D MoS2 layers were integrated onto porous polymeric supports with well-preserved structural integrity enabled by a water-assisted 2D layer transfer method. These 2D MoS2 membranes of near atomic thickness exhibit an excellent combination of high water permeability (>322 L m-2 h-1 bar-1) and high ionic sieving capability (>99%) for various seawater salts including Na+, K+, Ca2+, and Mg2+ with a range of concentrations. Moreover, they present near 100% salt ion rejection rates for actual seawater obtained from the Atlantic coast, significantly outperforming the previously developed 2D MoS2 layer membranes of micrometer thickness as well as conventional reverse osmosis (RO) membranes. Underlying principles behind such remarkably excellent desalination performances are attributed to the intrinsic atomic vacancies inherent to the CVD-grown 2D MoS2 layers as verified by aberration-corrected electron microscopy characterization.

Multifunctional Two-Dimensional PtSe2-Layer Kirigami Conductors with 2000% Stretchability and Metallic-to-Semiconducting Tunability.

Two-dimensional transition-metal dichalcogenide (2D TMD) layers are highly attractive for emerging stretchable and foldable electronics owing to their extremely small thickness coupled with extraordinary electrical and optical properties. Although intrinsically large strain limits are projected in them (i.e., several times greater than silicon), integrating 2D TMDs in their pristine forms does not realize superior mechanical tolerance greatly demanded in high-end stretchable and foldable devices of unconventional form factors. In this article, we report a versatile and rational strategy to convert 2D TMDs of limited mechanical tolerance to tailored 3D structures with extremely large mechanical stretchability accompanying well-preserved electrical integrity and modulated transport properties. We employed a concept of strain engineering inspired by an ancient paper-cutting art, known as kirigami patterning, and developed 2D TMD-based kirigami electrical conductors. Specifically, we directly integrated 2D platinum diselenide (2D PtSe2) layers of controlled carrier transport characteristics on mechanically flexible polyimide (PI) substrates by taking advantage of their low synthesis temperature. The metallic 2D PtSe2/PI kirigami patterns of optimized dimensions exhibit an extremely large stretchability of ∼2000% without compromising their intrinsic electrical conductance. They also present strain-tunable and reversible photoresponsiveness when interfaced with semiconducting carbon nanotubes (CNTs), benefiting from the formation of 2D PtSe2/CNT Schottky junctions. Moreover, kirigami field-effect transistors (FETs) employing semiconducting 2D PtSe2 layers exhibit tunable gate responses coupled with mechanical stretching upon electrolyte gating. The exclusive role of the kirigami pattern parameters in the resulting mechanoelectrical responses was also verified by a finite-element modeling (FEM) simulation. These multifunctional 2D materials in unconventional yet tailored 3D forms are believed to offer vast opportunities for emerging electronics and optoelectronics.

Improving Electrochemical Pb2+ Detection Using a Vertically Aligned 2D MoS2 Nanofilm.

Recent advancements in MoS2 nanofilms have aided in the development for important water-related environmental applications. However, a MoS2 nanofilm-coated sensor has yet to have been applied for heavy metal detection in water-related environmental samples. In this study, a novel vertically aligned two-dimensional (2D) MoS2 (edge exposed) nanofilm was applied for in situ lead ion (Pb2+) detection. The developed sensor showed an excellent linear relationship toward Pb2+ between 0 and 20 ppb at -0.45 V vs Ag/AgCl using square wave anodic stripping voltammetry (SWASV) with the improved limit of detection (LOD) of 0.3 ppb in a tap water environment. The vertically aligned 2D MoS2 sensor exhibited improved detection sensitivity (2.8 folds greater than a previous metallic [Bi] composite electrode) with lower relative standard deviation for repetitive measurements (n = 11), indicating enhanced reproducibility for Pb2+ detection. The vertically aligned 2D MoS2 layers exhibited 2.6 times higher sensitivity than horizontally aligned 2D MoS2 (basal plane exposed). Density functional theory calculations demonstrated that adsorption energy of Pb on the MoS2 side edge was much higher (4.11 eV) than those on the basal plane (0.36 and 0.07 eV). In addition, the band gap center of vertical MoS2 was found to be higher than the Pb2+ → Pb reduction potential level and capable of reducing Pb2+. Overall, the newly developed vertically aligned 2D MoS2 sensor showed excellent performance for detecting Pb2+ in a real drinking water environment with good reliability.

Centimeter-Scale 2D van der Waals Vertical Heterostructures Integrated on Deformable Substrates Enabled by Gold Sacrificial Layer-Assisted Growth.

Two-dimensional (2D) transition metal dichalcogenides (TMDs) such as molybdenum or tungsten disulfides (MoS2 or WS2) exhibit extremely large in-plane strain limits and unusual optical/electrical properties, offering unprecedented opportunities for flexible electronics/optoelectronics in new form factors. In order for them to be technologically viable building-blocks for such emerging technologies, it is critically demanded to grow/integrate them onto flexible or arbitrary-shaped substrates on a large wafer-scale compatible with the prevailing microelectronics processes. However, conventional approaches to assemble them on such unconventional substrates via mechanical exfoliations or coevaporation chemical growths have been limited to small-area transfers of 2D TMD layers with uncontrolled spatial homogeneity. Moreover, additional processes involving a prolonged exposure to strong chemical etchants have been required for the separation of as-grown 2D layers, which is detrimental to their material properties. Herein, we report a viable strategy to universally combine the centimeter-scale growth of various 2D TMD layers and their direct assemblies on mechanically deformable substrates. By exploring the water-assisted debonding of gold (Au) interfaced with silicon dioxide (SiO2), we demonstrate the direct growth, transfer, and integration of 2D TMD layers and heterostructures such as 2D MoS2 and 2D MoS2/WS2 vertical stacks on centimeter-scale plastic and metal foil substrates. We identify the dual function of the Au layer as a growth substrate as well as a sacrificial layer which facilitates 2D layer transfer. Furthermore, we demonstrate the versatility of this integration approach by fabricating centimeter-scale 2D MoS2/single walled carbon nanotube (SWNT) vertical heterojunctions which exhibit current rectification and photoresponse. This study opens a pathway to explore large-scale 2D TMD van der Waals layers as device building blocks for emerging mechanically deformable electronics/optoelectronics.

Alloyed 2D Metal-Semiconductor Atomic Layer Junctions.

Heterostructures of compositionally and electronically variant two-dimensional (2D) atomic layers are viable building blocks for ultrathin optoelectronic devices. We show that the composition of interfacial transition region between semiconducting WSe2 atomic layer channels and metallic NbSe2 contact layers can be engineered through interfacial doping with Nb atoms. WxNb1-xSe2 interfacial regions considerably lower the potential barrier height of the junction, significantly improving the performance of the corresponding WSe2-based field-effect transistor devices. The creation of such alloyed 2D junctions between dissimilar atomic layer domains could be the most important factor in controlling the electronic properties of 2D junctions and the design and fabrication of 2D atomic layer devices.

High Mobility Transistors and Flexible Optical Synapses Enabled by Wafer-Scale Chemical Transformation of Pt-Based 2D Layers.

Electronic devices employing two-dimensional (2D) van der Waals (vdW) transition-metal dichalcogenide (TMD) layers as semiconducting channels often exhibit limited performance (e.g., low carrier mobility), in part, due to their high contact resistances caused by interfacing non-vdW three-dimensional (3D) metal electrodes. Herein, we report that this intrinsic contact issue can be efficiently mitigated by forming the 2D/2D in-plane junctions of 2D semiconductor channels seamlessly interfaced with 2D metal electrodes. For this, we demonstrated the selectively patterned conversion of semiconducting 2D PtSe2 (channels) to metallic 2D PtTe2 (electrodes) layers by employing a wafer-scale low-temperature chemical vapor deposition (CVD) process. We investigated a variety of field-effect transistors (FETs) employing wafer-scale CVD-2D PtSe2/2D PtTe2 heterolayers and identified that silicon dioxide (SiO2) top-gated FETs exhibited an extremely high hole mobility of ∼120 cm2 V-1 s-1 at room temperature, significantly surpassing performances with previous wafer-scale 2D PtSe2-based FETs. The low-temperature nature of the CVD method further allowed for the direct fabrication of wafer-scale arrays of 2D PtSe2/2D PtTe2 heterolayers on polyamide (PI) substrates, which intrinsically displayed optical pulse-induced artificial synaptic behaviors. This study is believed to vastly broaden the applicability of 2D TMD layers for next-generation, high-performance electronic devices with unconventional functionalities.

Defect Passivation of 2D Semiconductors by Fixating Chemisorbed Oxygen Molecules via h-BN Encapsulations.

Hexagonal boron nitride (h-BN) is a key ingredient for various 2D van der Waals heterostructure devices, but the exact role of h-BN encapsulation in relation to the internal defects of 2D semiconductors remains unclear. Here, it is reported that h-BN encapsulation greatly removes the defect-related gap states by stabilizing the chemisorbed oxygen molecules onto the defects of monolayer WS2 crystals. Electron energy loss spectroscopy (EELS) combined with theoretical analysis clearly confirms that the oxygen molecules are chemisorbed onto the defects of WS2 crystals and are fixated by h-BN encapsulation, with excluding a possibility of oxygen molecules trapped in bubbles or wrinkles formed at the interface between WS2 and h-BN. Optical spectroscopic studies show that h-BN encapsulation prevents the desorption of oxygen molecules over various excitation and ambient conditions, resulting in a greatly lowered and stabilized free electron density in monolayer WS2 crystals. This suppresses the exciton annihilation processes by two orders of magnitude compared to that of bare WS2. Furthermore, the valley polarization becomes robust against the various excitation and ambient conditions in the h-BN encapsulated WS2 crystals.

Microwave-assisted thermochemical conversion of Zr-FeOOH nanorods to Zr-ZnFe2O4 nanorods for bacterial disinfection and photo-Fenton catalytic degradation of organic pollutants.

Herein, we report a CoOx-loaded Zr-doped ZnFe2O4 (CoOx/Zr-ZFO) NR photocatalyst synthesized by successive microwave and wet impregnation methods for bacterial inactivation and degradation of organic pollutants. For the first time, microwave treatment was used for Zn attachment on hydrothermally synthesized self-assembled Zr-FeOOH NRs to produce Zr-doped ZnFe2O4 (Zr-ZFO) NRs. The lowest bandgap energy (1.96 eV) enables for significant absorption in the visible light region, which helps to improve bacteria degradation inactivation efficiency. Further, various metal oxides (Cu, Ag and Co) were loaded onto the surface of photocatalysts (Zr-ZFO NRs) by a wet impregnation method. As-synthesized CoOx/Zr-ZFO-3 NRs were systematically characterized and used as photocatalysts for inactivation of E. coli and S. aureus and degradation of organic pollutants. The CoOx/Zr-ZFO-3 NR photocatalyst exhibited better inactivation efficiency (99.4 %) than other metal oxide-loaded Zr-ZFO NRs (Ag2Ox-loaded Zr-ZFO NRs (33.6 %), CuOx-loaded Zr-ZFO NRs (77.6 %)). Additionally, the optimum CoOx/Zr-ZFO-3 NR photocatalyst showed 98.3 % and 98.1 % degradation efficiencies for BPA and orange II dye, respectively, under visible light irradiation (λ ≥ 420 nm). Therefore, this work affords a novel, simple and rapid approach for the development of photocatalysts which active in visible light for bacterial disinfection and organic degradation.

MoS2 Synapses with Ultra-low Variability and Their Implementation in Boolean Logic.

Brain-inspired computing enabled by memristors has gained prominence over the years due to the nanoscale footprint and reduced complexity for implementing synapses and neurons. The demonstration of complex neuromorphic circuits using conventional materials systems has been limited by high cycle-to-cycle and device-to-device variability. Two-dimensional (2D) materials have been used to realize transparent, flexible, ultra-thin memristive synapses for neuromorphic computing, but with limited knowledge on the statistical variation of devices. In this work, we demonstrate ultra-low-variability synapses using chemical vapor deposited 2D MoS2 as the switching medium with Ti/Au electrodes. These devices, fabricated using a transfer-free process, exhibit ultra-low variability in SET voltage, RESET power distribution, and synaptic weight update characteristics. This ultra-low variability is enabled by the interface rendered by a Ti/Au top contact on Si-rich MoS2 layers of mixed orientation, corroborated by transmission electron microscopy (TEM), electron energy loss spectroscopy (EELS), and X-ray photoelectron spectroscopy (XPS). TEM images further confirm the stability of the device stack even after subjecting the device to 100 SET-RESET cycles. Additionally, we implement logic gates by monolithic integration of MoS2 synapses with MoS2 leaky integrate-and-fire neurons to show the viability of these devices for non-von Neumann computing.

In situ synthesis of hierarchically-assembled three-dimensional ZnS nanostructures and 3D printed visualization.

Nanomaterials have gained enormous interest in improving the performance of energy harvest systems, biomedical devices, and high-strength composites. Many studies were performed fabricating more elaborate and heterogeneous nanostructures then the structures were characterized using TEM tomographic images, upgrading the fabrication technique. Despite the effort, intricate fabrication process, agglomeration characteristic, and non-uniform output were still limited to presenting the 3D panoramic views straightforwardly. Here we suggested in situ synthesis method to prepare complex and hierarchically-assembled nanostructures that consisted of ZnS nanowire core and nanoparticles under Ag2S catalyst. We demonstrated that the vaporized Zn and S were solidified in different shapes of nanostructures with the temperatures solely. To our knowledge, this is the first demonstration of synthesizing heterogeneous nanostructures, consisting of a nanowire from the vapor-liquid-solid and then nanoparticles from the vapor-solid grown mechanism by in situ temperature control. The obtained hierarchically-assembled ZnS nanostructures were characterized by various TEM technologies, verifying the crystal growth mechanism. Lastly, electron tomography and 3D printing enabled the nanoscale structures to visualize with centimeter scales. The 3D printing from randomly fabricated nanomaterials is rarely performed to date. The collaborating work could offer a better opportunity to fabricate advanced and sophisticated nanostructures.

Multiwavelength Optoelectronic Synapse with 2D Materials for Mixed-Color Pattern Recognition.

Neuromorphic visual systems emulating biological retina functionalities have enormous potential for in-sensor computing, with prospects of making artificial intelligence ubiquitous. Conventionally, visual information is captured by an image sensor, stored by memory units, and eventually processed by the machine learning algorithm. Here, we present an optoelectronic synapse device with multifunctional integration of all the processes required for real time object identification. Ultraviolet-visible wavelength-sensitive MoS2 FET channel with infrared sensitive PtTe2/Si gate electrode enables the device to sense, store, and process optical data for a wide range of the electromagnetic spectrum, while maintaining a low dark current. The device exhibits optical stimulation-controlled short-term and long-term potentiation, electrically driven long-term depression, synaptic weight update for multiple wavelengths of light ranging from 300 nm in ultraviolet to 2 µm in infrared. An artificial neural network developed using the extracted weight update parameters of the device can be trained to identify both single wavelength and mixed wavelength patterns. This work demonstrates a device that could potentially be used for realizing a multiwavelength neuromorphic visual system for pattern recognition and object identification.

Peel-and-Stick Integration of Atomically Thin Nonlayered PtS Semiconductors for Multidimensionally Stretchable Electronic Devices.

Various near-atom-thickness two-dimensional (2D) van der Waals (vdW) crystals with unparalleled electromechanical properties have been explored for transformative devices. Currently, the availability of 2D vdW crystals is rather limited in nature as they are only obtained from certain mother crystals with intrinsically possessed layered crystallinity and anisotropic molecular bonding. Recent efforts to transform conventionally non-vdW three-dimensional (3D) crystals into ultrathin 2D-like structures have seen rapid developments to explore device building blocks of unique form factors. Herein, we explore a "peel-and-stick" approach, where a nonlayered 3D platinum sulfide (PtS) crystal, traditionally known as a cooperate mineral material, is transformed into a freestanding 2D-like membrane for electromechanical applications. The ultrathin (∼10 nm) 3D PtS films grown on large-area (>cm2) silicon dioxide/silicon (SiO2/Si) wafers are precisely "peeled" inside water retaining desired geometries via a capillary-force-driven surface wettability control. Subsequently, they are "sticked" on strain-engineered patterned substrates presenting prominent semiconducting properties, i.e., p-type transport with an optical band gap of ∼1.24 eV. A variety of mechanically deformable strain-invariant electronic devices have been demonstrated by this peel-and-stick method, including biaxially stretchable photodetectors and respiratory sensing face masks. This study offers new opportunities of 2D-like nonlayered semiconducting crystals for emerging mechanically reconfigurable and stretchable device technologies.

Nanowire transformation by size-dependent cation exchange reactions.

The unique properties of nanostructured materials enable their transformation into complex, kinetically controlled morphologies that cannot be obtained during their growth. Solution-phase cation-exchange reactions can transform sub-10 nm nanocrystals/nanorods into varying compositions and superlattice structures; however, because of their small size, cation-exchange reaction rates are extremely fast, which limits control over the transformed products and possibilities for obtaining new morphologies. Nanowires are routinely synthesized via gas-phase reactions with 5-200 nm diameters, and their large aspect ratios allow them to be electrically addressed individually. To realize their full potential, it is desirable to develop techniques that can transform nanowires into tunable but precisely controlled morphologies, especially in the gas-phase, to be compatible with nanowire growth schemes. We report transformation of single-crystalline cadmium sulfide nanowires into composition-controlled Zn(x)Cd((1-x))S nanowires, core-shell heterostructures, metal-semiconductor superlattices (Zn-Zn(x)Cd((1-x))S), single-crystalline ZnS nanotubes, and eventually metallic Zn nanowires by utilizing size-dependent cation-exchange reaction along with temperature and gas-phase reactant delivery control. This versatile synthetic ability to transform nanowires offers new opportunities to study size-dependent phenomena at the nanoscale and tune their chemical/physical properties to design reconfigurable circuits.

Mechanically rollable photodetectors enabled by centimetre-scale 2D MoS2 layer/TOCN composites.

Two-dimensional (2D) molybdenum disulfide (MoS2) layers are suitable for visible-to-near infrared photodetection owing to their tunable optical bandgaps. Also, their superior mechanical deformability enabled by an extremely small thickness and van der Waals (vdW) assembly allows them to be structured into unconventional physical forms, unattainable with any other materials. Herein, we demonstrate a new type of 2D MoS2 layer-based rollable photodetector that can be mechanically reconfigured while maintaining excellent geometry-invariant photo-responsiveness. Large-area (>a few cm2) 2D MoS2 layers grown by chemical vapor deposition (CVD) were integrated on transparent and flexible substrates composed of 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO)-oxidized cellulose nanofibers (TOCNs) by a direct solution casting method. These composite materials in three-dimensionally rollable forms exhibited a large set of intriguing photo-responsiveness, well preserving intrinsic opto-electrical characteristics of the integrated 2D MoS2 layers; i.e., light intensity-dependent photocurrents insensitive to illumination angles as well as highly tunable photocurrents varying with the rolling number of 2D MoS2 layers, which were impossible to achieve with conventional photodetectors. This study provides a new design principle for converting 2D materials to three-dimensional (3D) objects of tailored functionalities and structures, significantly broadening their potential and versatility in futuristic devices.