FLUXestimator: a webserver for predicting metabolic flux and variations using transcriptomics data.

Quantitative assessment of single cell fluxome is critical for understanding the metabolic heterogeneity in diseases. Unfortunately, laboratory-based single cell fluxomics is currently impractical, and the current computational tools for flux estimation are not designed for single cell-level prediction. Given the well-established link between transcriptomic and metabolomic profiles, leveraging single cell transcriptomics data to predict single cell fluxome is not only feasible but also an urgent task. In this study, we present FLUXestimator, an online platform for predicting metabolic fluxome and variations using single cell or general transcriptomics data of large sample-size. The FLUXestimator webserver implements a recently developed unsupervised approach called single cell flux estimation analysis (scFEA), which uses a new neural network architecture to estimate reaction rates from transcriptomics data. To the best of our knowledge, FLUXestimator is the first web-based tool dedicated to predicting cell-/sample-wise metabolic flux and metabolite variations using transcriptomics data of human, mouse and 15 other common experimental organisms. The FLUXestimator webserver is available at http://scFLUX.org/, and stand-alone tools for local use are available at https://github.com/changwn/scFEA. Our tool provides a new avenue for studying metabolic heterogeneity in diseases and has the potential to facilitate the development of new therapeutic strategies.

CO2 Stress-Driven Room Temperature Ferromagnetism of Ultrathin 2D Gallium Oxide.

Spintronic devices work by manipulating the spin of electrons other than charge transfer, which is of revolutionary significance and can largely reduce energy consumption in the future. Herein, ultrathin two-dimensional (2D) non-van der Waals (non-vdW) γ-Ga2O3 with room temperature ferromagnetism is successfully obtained by using supercritical CO2 (SC CO2). The stress effect of SC CO2 under different pressures selectively modulates the orientation and strength of covalent bonds, leading to the change of atomic structure including lattice expansion, introduction of O vacancy, and transition of Ga-O coordination (GaO4 and GaO6). Magnetic measurements show that pristine γ-Ga2O3 is nonferromagnetic, whereas the SC CO2 treated γ-Ga2O3 exhibits obvious ferromagnetic behavior with an optimal magnetization of 0.025 emu g-1 and a Curie temperature of 300 K.

Tunable Circular Photogalvanic and Photovoltaic Effect in 2D Tellurium with Different Chirality.

Chirality arises from the asymmetry of materials, where two counterparts are the mirror image of each other. The interaction between circular-polarized light and quantum materials is enhanced in chiral space groups due to the structural chirality. Tellurium (Te) possesses the simplest chiral crystal structure, with Te atoms covalently bonded into a spiral atomic chain (left- or right-handed) with a periodicity of 3. Here, we investigate the tunable circular photoelectric responses in 2D Te field-effect transistors with different chirality, including the longitudinal circular photogalvanic effect induced by the radial spin texture (electron-spin polarization parallel to the electron momentum direction) and the circular photovoltaic effect induced by the chiral crystal structure (helical Te atomic chains). Our work demonstrates the controllable manipulation of the chirality degree of freedom in materials.

Tunable Chirality-Dependent Nonlinear Electrical Responses in 2D Tellurium.

Tellurium (Te) is an elemental semiconductor with a simple chiral crystal structure. Te in a two-dimensional (2D) form synthesized by a solution-based method shows excellent electrical, optical, and thermal properties. In this work, the chirality of hydrothermally grown 2D Te is identified and analyzed by hot sulfuric acid etching and high-angle tilted high-resolution scanning transmission electron microscopy. The gate-tunable nonlinear electrical responses, including the nonreciprocal electrical transport in the longitudinal direction and the nonlinear planar Hall effect in the transverse direction, are observed in 2D Te under a magnetic field. Moreover, the nonlinear electrical responses have opposite signs in left- and right-handed 2D Te due to the opposite spin polarizations ensured by the chiral symmetry. The fundamental relationship between the spin-orbit coupling and the crystal symmetry in two enantiomers provides a viable platform for realizing chirality-based electronic devices by introducing the degree of freedom of chirality into electron transport.

Comparative floral development in male and female plants of Palmer amaranth (Amaranthus palmeri).

PREMISE: Characterizing the developmental processes in the transition from hermaphroditism to unisexuality is crucial for understanding floral evolution. Amaranthus palmeri, one of the most devastating weeds in the United States, is an emerging model system for studying a dioecious breeding system and understanding the biological traits of this invasive weed. The objectives of this study were to characterize phases of flower development in A. palmeri and compare organogenesis of flower development in female and male plants. METHODS: Flower buds from male and female plants were dissected for light microscopy. Segments of male and female inflorescences at different stages of development were cut longitudinally and visualized using scanning electron microscopy. RESULTS: Pistillate flowers have two to three styles, one ovary with one ovule, and five obtuse tepals. Staminate flowers have five stamens with five acute tepals. Floral development was classified into 10 stages. The distinction between the two flower types became apparent at stage four by the formation of stamen primordia in staminate flowers, which developed female and male reproductive organs initially, as contrasted to pistillate flowers, which produced carpel primordia only. In staminate flowers, the putative carpel primordia changed little in size and remained undeveloped. CONCLUSIONS: Timing of inappropriate organ termination varies across the two sexes in A. palmeri. Our study suggests that the evolution of A. palmeri from a cosexual ancestral state to complete dioecy is still in progress since males exhibited transient hermaphroditism and females produced strictly pistillate flowers.

Emerging beyond-graphene elemental 2D materials for energy and catalysis applications.

Elemental two-dimensional (2D) materials have emerged as promising candidates for energy and catalysis applications due to their unique physical, chemical, and electronic properties. These materials are advantageous in offering massive surface-to-volume ratios, favorable transport properties, intriguing physicochemical properties, and confinement effects resulting from the 2D ultrathin structure. In this review, we focus on the recent advances in emerging energy and catalysis applications based on beyond-graphene elemental 2D materials. First, we briefly introduce the general classification, structure, and properties of elemental 2D materials and the new advances in material preparation. We then discuss various applications in energy harvesting and storage, including solar cells, piezoelectric and triboelectric nanogenerators, thermoelectric devices, batteries, and supercapacitors. We further discuss the explorations of beyond-graphene elemental 2D materials for electrocatalysis, photocatalysis, and heterogeneous catalysis. Finally, the challenges and perspectives for the future development of elemental 2D materials in energy and catalysis are discussed.

Bilayer Quantum Hall States in an n-Type Wide Tellurium Quantum Well.

Tellurium (Te) is a narrow bandgap semiconductor with a unique chiral crystal structure. The topological nature of electrons in the Te conduction band can be studied by realizing n-type doping using atomic layer deposition (ALD) technique on two-dimensional (2D) Te film. In this work, we fabricated and measured the double-gated n-type Te Hall-bar devices, which can operate as two separate or coupled electron layers controlled by the top gate and back gate. Profound Shubnikov-de Haas (SdH) oscillations are observed in both top and bottom electron layers. Landau level hybridization between two layers, compound and charge-transferable bilayer quantum Hall states at filling factor ν = 4, 6, and 8, are analyzed. Our work opens the door for the study of Weyl physics in coupled bilayer systems of 2D materials.

Piezoelectricity of single-atomic-layer MoS2 for energy conversion and piezotronics.

The piezoelectric characteristics of nanowires, thin films and bulk crystals have been closely studied for potential applications in sensors, transducers, energy conversion and electronics. With their high crystallinity and ability to withstand enormous strain, two-dimensional materials are of great interest as high-performance piezoelectric materials. Monolayer MoS2 is predicted to be strongly piezoelectric, an effect that disappears in the bulk owing to the opposite orientations of adjacent atomic layers. Here we report the first experimental study of the piezoelectric properties of two-dimensional MoS2 and show that cyclic stretching and releasing of thin MoS2 flakes with an odd number of atomic layers produces oscillating piezoelectric voltage and current outputs, whereas no output is observed for flakes with an even number of layers. A single monolayer flake strained by 0.53% generates a peak output of 15 mV and 20 pA, corresponding to a power density of 2 mW m(-2) and a 5.08% mechanical-to-electrical energy conversion efficiency. In agreement with theoretical predictions, the output increases with decreasing thickness and reverses sign when the strain direction is rotated by 90°. Transport measurements show a strong piezotronic effect in single-layer MoS2, but not in bilayer and bulk MoS2. The coupling between piezoelectricity and semiconducting properties in two-dimensional nanomaterials may enable the development of applications in powering nanodevices, adaptive bioprobes and tunable/stretchable electronics/optoelectronics.

Thermoelectric Performance of 2D Tellurium with Accumulation Contacts.

Tellurium (Te) is an intrinsically p-type-doped narrow-band gap semiconductor with an excellent electrical conductivity and low thermal conductivity. Bulk trigonal Te has been theoretically predicted and experimentally demonstrated to be an outstanding thermoelectric material with a high value of thermoelectric figure-of-merit ZT. In view of the recent progress in developing the synthesis route of 2D tellurium thin films as well as the growing trend of exploiting nanostructures as thermoelectric devices, here for the first time, we report the excellent thermoelectric performance of tellurium nanofilms, with a room-temperature power factor of 31.7 µW/cm K2 and ZT value of 0.63. To further enhance the efficiency of harvesting thermoelectric power in nanofilm devices, thermoelectrical current mapping was performed with a laser as a heating source, and we found that high work function metals such as palladium can form rare accumulation-type metal-to-semiconductor contacts to Te, which allows thermoelectrically generated carriers to be collected more efficiently. High-performance thermoelectric Te devices have broad applications as energy harvesting devices or nanoscale Peltier coolers in microsystems.

Imaging Carrier Inhomogeneities in Ambipolar Tellurene Field Effect Transistors.

The development of van der Waals (vdW) homojunction devices requires materials with narrow bandgaps and simultaneously high hole and electron mobilities for bipolar transport, as well as methods to image and study spatial variations in carrier type and associated conductivity with nanometer spatial resolution. Here, we demonstrate the general capability of near-field scanning microwave microscopy (SMM) to image and study the local carrier type and associated conductivity in operando by studying ambiploar field-effect transistors (FETs) of the 1D vdW material tellurium in 2D form. To quantitatively understand electronic variations across the device, we produce nanometer-resolved maps of the local carrier equivalence backgate voltage. We show that the global device conductivity minimum determined from transport measurements does not arise from uniform carrier neutrality but rather from the continued coexistence of p-type regions at the device edge and n-type regions in the interior of our micrometer-scale devices. This work both underscores and addresses the need to image and understand spatial variations in the electronic properties of nanoscale devices.

Tellurene: its physical properties, scalable nanomanufacturing, and device applications.

Tellurium (Te) has a trigonal crystal lattice with inherent structural anisotropy. Te is multifunctional, e.g., semiconducting, photoconductive, thermoelectric, piezoelectric, etc., for applications in electronics, sensors, optoelectronics, and energy devices. Due to the inherent structural anisotropy, previously reported synthetic methods predominantly yield one-dimensional (1D) Te nanostructures. Much less is known about 2D Te nanostructures, their processing schemes, and their material properties. This review focuses on the synthesis and morphology control of emerging 2D tellurene and summarizes the latest developments in understanding the fundamental properties of monolayer and few-layer tellurene, as well as the recent advances in demonstrating prototypical tellurene devices. Finally, the prospects for future research and application opportunities as well as the accompanying challenges of 2D tellurene are summarized and highlighted.

Quantum Transport and Band Structure Evolution under High Magnetic Field in Few-Layer Tellurene.

Quantum Hall effect (QHE) is a macroscopic manifestation of quantized states that only occurs in confined two-dimensional electron gas (2DEG) systems. Experimentally, QHE is hosted in high-mobility 2DEG with large external magnetic field at low temperature. Two-dimensional van der Waals materials, such as graphene and black phosphorus, are considered interesting material systems to study quantum transport because they could unveil unique host material properties due to the easy accessibility of monolayer or few-layer thin films at the 2D quantum limit. For the first time, we report direct observation of QHE in a novel low-dimensional material system, tellurene. High-quality 2D tellurene thin films were acquired from recently reported hydrothermal method with high hole mobility of nearly 3000 cm2/(V s) at low temperatures, which allows the observation of well-developed Shubnikov-de Haas (SdH) oscillations and QHE. A four-fold degeneracy of Landau levels in SdH oscillations and QHE was revealed. Quantum oscillations were investigated under different gate biases, tilted magnetic fields, and various temperatures, and the results manifest the inherent information on the electronic structure of Te. Anomalies in both temperature-dependent oscillation amplitudes and transport characteristics were observed that are ascribed to the interplay between the Zeeman effect and spin-orbit coupling, as depicted by the density functional theory calculations.

Activation of MoS2 Basal Planes for Hydrogen Evolution by Zinc.

Molybdenum disulfide (MoS2 ) has been widely studied as a potential earth-abundant electrocatalyst for the hydrogen-evolution reaction (HER). Defect engineering and heteroelemental doping are effective methods to enhance the catalytic activity in the HER, so exploring an efficient route to simultaneously achieve in-plane vacancy engineering and elemental doping of MoS2 is necessary. In this study, Zinc, a low-cost and moderately active metal, has been used to realize this strategy by generation of sulfur vacancies and zinc doping on MoS2 in one step. Density functional theory calculations reveal that the zinc atoms not only lower the formation energy of S vacancies, but also help to decrease ΔGH of S-vacancy sites near the Zn atoms. At an optimal zinc-reduced MoS2 (Zn@MoS2 ) example, the activated basal planes contribute to the HER activity with an overpotential of -194 mV at 10 mA cm-2 and a low Tafel slope of 78 mV/dec.

Tellurium: Fast Electrical and Atomic Transport along the Weak Interaction Direction.

In anisotropic materials, the electrical and atomic transport along the weak interaction direction is usually much slower than that along the chemical bond direction. However, Te, an important semiconductor composed of helical atomic chains, exhibits nearly isotropic electrical transport between intrachain and interchain directions. Using first-principles calculations to study bulk and few-layer Te, we show that this isotropy is related to similar effective masses and potentials for charge carriers along different transport directions, benefiting from the delocalization of the lone-pair electrons. This delocalization also enhances the interchain binding, and thus facilitates diffusion of vacancies and interstitial atoms across the chains, which together with the fast intrachain diffusion enable rapid self-healing of these defects at low temperature. Interestingly, the interstitial atoms diffuse along the chain via a concerted rotation mechanism. Our work reveals the unconventional properties underlying the superior performance of Te while providing insight into the transport in anisotropic materials.

One-Dimensional van der Waals Material Tellurium: Raman Spectroscopy under Strain and Magneto-Transport.

Experimental demonstrations of one-dimensional (1D) van der Waals material tellurium (Te) have been presented by Raman spectroscopy under strain and magneto-transport. Raman spectroscopy measurements have been performed under strains along different principle axes. Pronounced strain response along the c-axis is observed due to the strong intrachain covalent bonds, while no strain response is obtained along the a-axis due to the weak interchain van der Waals interaction. Magneto-transport results further verify its anisotropic property, which results in dramatically distinct magneto-resistance behaviors in terms of three different magnetic field directions. Specifically, phase coherence length extracted from weak antilocalization effect, Lϕ ≈ T-0.5, claims its two-dimensional (2D) transport characteristics when an applied magnetic field is perpendicular to the thin film. In contrast, Lϕ ≈ T-0.33 is obtained from universal conductance fluctuations once the magnetic field is along the c-axis of Te, which indicates its nature of 1D transport along the helical atomic chains. Our studies, which are obtained on high quality single crystal Te thin film, appear to serve as strong evidence of its 1D van der Waals structure from experimental perspectives. It is the aim of this paper to address this special concept that differs from the previous well-studied 1D nanowires or 2D van der Waals materials.

High-performance piezoelectric nanogenerators for self-powered nanosystems: quantitative standards and figures of merit.

Harvesting energies from the atmosphere cost-effectively is critical for both addressing worldwide long-term energy needs at the macro-scale, and achieving the sustainable maintenance-free operation of nanodevices at the micro-scale (Wang and Wu 2012 Angew. Chem. Int. Ed. 51 11700-21). Piezoelectric nanogenerator (NG) technology has demonstrated its great application potential in harvesting the ubiquitous and abundant mechanical energy. Despite of the progress made in this rapidly-advancing field, a fundamental understanding and common standard for consistently quantifying and evaluating the performance of the various types of piezoelectric NGs is still lacking. In their recent study Crossley and Kar-Narayan (2015 Nanotechnology 26 344001), systematically investigated dynamical properties of piezoelectric NGs by taking into account the effect of driving mechanism and load frequency on NG performance. They further defined the NGs' figures of merit as energy harvested normalized by applied strain or stress for NGs under strain-driven or stress-driven conditions, which are commonly seen in the vibrational energy harvesting. This work provides new insight and a feasible approach for consistently evaluating piezoelectric nanomaterials and NG devices, which is important for designing and optimizing nanoscale piezoelectric energy harvesters, as well as promoting their applications in emerging areas e.g. the internet of things, wearable devices, and self-powered nanosystems.

Solution-derived ZnO homojunction nanowire films on wearable substrates for energy conversion and self-powered gesture recognition.

Emerging applications in wearable technology, pervasive computing, human-machine interfacing, and implantable biomedical devices demand an appropriate power source that can sustainably operate for extended periods of time with minimal intervention (Wang, Z. L.; et al. Angew. Chem., Int. Ed. 2012, 51, 11700). Self-powered nanosystems, which harvest operating energy from its host (i.e., the human body), may be feasible due to their extremely low power consumption (Tian, B. Z.; et al. Nature 2007, 449, 885. Javey, A.; et al. Nature 2003, 424, 654. Cui, Y.; et al. Science 2001, 291, 851). Here we report materials and designs for wearable-on-skin piezoelectric devices based on ultrathin (2 µm) solution-derived ZnO p-n homojunction films for the first time. The depletion region formed at the p-n homojunction effectively reduces internal screening of strain-induced polarization charges by free carriers in both n-ZnO and Sb-doped p-ZnO, resulting in significantly enhanced piezoelectric output compared to a single layer device. The p-n structure can be further grown on polymeric substrates conformable to a human wrist and used to convert movement of the flexor tendons into distinguishable electrical signals for gesture recognition. The ZnO homojunction piezoelectric devices may have applications in powering nanodevices, bioprobes, and self-powered human-machine interfacing.

One-pot glovebox-free synthesis, characterization, and self-assembly of novel amphiphilic poly(sarcosine-b-caprolactone) diblock copolymers.

Novel amphiphilic polypeptoid-polyester diblock copolymers based on poly(sarcosine) (PSar) and poly(ε-caprolactone) (PCL) are synthesized by a one-pot glovebox-free approach. In this method, sarcosine N-carboxy anhydride (Sar-NCA) is firstly polymerized in the presence of benzylamine under N(2) flow, then the resulting poly(sarcosine) is used in situ as the macro-initiator for the ring-opening polymerization (ROP) of ε-caprolactone using tin(II) octanoate as a catalyst. The degree of poly-merization of each block is controlled by various feed ratios of monomer/initiator. The diblock copolymers with controlled molecular weight and narrow molecular weight distributions (D(M) < 1.2) are characterized by (1)H NMR, (13)C NMR, and size-exclusion chromatography. The self-assembly behavior of PSar-b-PCL in water is investigated by dynamic light scattering (DLS) and transmission electron microscopy. DLS results reveal that the diblock copolymers associate into nanoparticles with average hydrodynamic diameters (D(H)) around 100 nm in water, which may be used as drug delivery carriers.

Piezotronic effect in solution-grown p-type ZnO nanowires and films.

Investigating the piezotronic effect in p-type piezoelectric semiconductor is critical for developing a complete piezotronic theory and designing/fabricating novel piezotronic applications with more complex functionality. Using a low temperature solution method, we were able to produce ultralong (up to 60 µm in length) Sb doped p-type ZnO nanowires on both rigid and flexible substrates. For the p-type nanowire field effect transistor, the on/off ratio, threshold voltage, mobility, and carrier concentration of 0.2% Sb-doped sample are found to be 10(5), 2.1 V, 0.82 cm(2)·V(-1)·s(-1), and 2.6 × 10(17) cm(-3), respectively, and the corresponding values for 1% Sb doped samples are 10(4), 2.0 V, 1.24 cm(2)·V(-1)·s(-1), and 3.8 × 10(17) cm(-3). We further investigated the universality of piezotronic effect in the as-synthesized Sb-doped p-type ZnO NWs and reported for the first time strain-gated piezotronic transistors as well as piezopotential-driven mechanical energy harvesting based on solution-grown p-type ZnO NWs. The results presented here broaden the scope of piezotronics and extend the framework for its potential applications in electronics, optoelectronics, smart MEMS/NEMS, and human-machine interfacing.

Superconducting Field-Effect Transistors with PdxTe-Te Intimate Contacts.

Superconducting-based electronic devices have shown great potential for future quantum computing applications. One key building block device is a superconducting field-effect transistor based on a superconductor-semiconductor-superconductor Josephson-junction (JJ) with a gate-tunable semiconducting channel. However, the performance of such devices is highly dependent on the quality of the superconductor to semiconductor interface. In this study, we present an alternative method to obtain a high-quality interface by using intimate contact. We investigate the proximity-induced superconductivity in chiral crystal tellurium (Te) and fabricate a PdxTe-Te-PdxTe JJ with an ambipolar supercurrent that is gate-tunable and exhibits multiple Andreev reflections. The semiconducting two-dimensional Te single crystal is grown hydrothermally and partially converted to superconducting PdxTe by controlled annealing. Our work demonstrates a promising path for realizing controllable superconducting electronic devices with high-quality superconducting interfaces; thus, we can continue to advance the field of quantum computing and other interface-based technologies.