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Phenotypic plasticity, the ability to produce multiple phenotypes from a single genotype, represents an excellent model with which to examine the relationship between gene expression and phenotypes. Analyses of the molecular foundations of phenotypic plasticity are challenging, however, especially in the case of complex social phenotypes. Here we apply a machine learning approach to tackle this challenge by analyzing individual-level gene expression profiles of Polistes dominula paper wasps following the loss of a queen. We find that caste-associated gene expression profiles respond strongly to queen loss, and that this change is partly explained by attributes such as age but occurs even in individuals that appear phenotypically unaffected. These results demonstrate that large changes in gene expression may occur in the absence of outwardly detectable phenotypic changes, resulting here in a socially mediated de-differentiation of individuals at the transcriptomic level but not at the levels of ovarian development or behavior., Connecting genotypes to complex social behaviour is challenging. Taylor et al. use machine learning to show a strong response of caste-associated gene expression to queen loss, wherein individual wasp’s expression profiles become intermediate between queen and worker states, even in the absence of behavioural changes.

Graphene has an extremely high in-plane strength yet considerable out-of-plane softness. High crystalline order of graphene assemblies is desired to utilize their in-plane properties, however, challenged by the easy formation of chaotic wrinkles for the intrinsic softness. Here, we find an intercalation modulated plasticization phenomenon, present a continuous plasticization stretching method to regulate spontaneous wrinkles of graphene sheets into crystalline orders, and fabricate continuous graphene papers with a high Hermans’ order of 0.93. The crystalline graphene paper exhibits superior mechanical (tensile strength of 1.1 GPa, stiffness of 62.8 GPa) and conductive properties (electrical conductivity of 1.1 × 105 S m−1, thermal conductivity of 109.11 W m−1 K−1). We extend the ultrastrong graphene papers to the realistic laminated composites and achieve high strength combining with attractive conductive and electromagnetic shielding performance. The intercalation modulated plasticity is revealed as a vital state of graphene assemblies, contributing to their industrial processing as metals and plastics., Strong but flexible graphene tends to wrinkle, which compromises some properties. Here the authors report a solid plasticization method to prepare continuous graphene papers with high crystalline order, achieving high strength, stiffness, electrical and thermal conductivities.

The effective implantation of conductive and charge storage materials into flexible frames has been strongly demanded for the development of flexible supercapacitors. Here, we introduce metallic cellulose paper-based supercapacitor electrodes with excellent energy storage performance by minimizing the contact resistance between neighboring metal and/or metal oxide nanoparticles using an assembly approach, called ligand-mediated layer-by-layer assembly. This approach can convert the insulating paper to the highly porous metallic paper with large surface areas that can function as current collectors and nanoparticle reservoirs for supercapacitor electrodes. Moreover, we demonstrate that the alternating structure design of the metal and pseudocapacitive nanoparticles on the metallic papers can remarkably increase the areal capacitance and rate capability with a notable decrease in the internal resistance. The maximum power and energy density of the metallic paper-based supercapacitors are estimated to be 15.1 mW cm−2 and 267.3 μWh cm−2, respectively, substantially outperforming the performance of conventional paper or textile-type supercapacitors., With ligand-mediated layer-by-layer assembly between metal nanoparticles and small organic molecules, the authors prepare metallic paper electrodes for supercapacitors with high power and energy densities. This approach could be extended to various electrodes for portable/wearable electronics.

The colour of water-jet rewritable paper (WJRP) is difficult to be expanded via single hydrochromic molecule, especially black. Here, inspired by the amazing phenomenon of bound-water in cells enabling various biological transformations via facilitating synergistic inter-/intra-molecular proton transfer, we present a simple strategy toward WJRP based on binary systems containing less-sensitive acidochromic dyes and mild proton donors (or developers). With such a binary system containing commercial black dye as the colouring agent, benzyl 4-hydroxybenzoate as the developer, and biomimetic bound-water as proton-transferring medium, we successfully achieve the long-awaited black WJRP. Printed images on such WJRP have excellent performances and long retaining time (>1 month). In addition, the robustness, durability and reversibility of WJRP could be increased distinctly by using polyethylene terephthalate as substrate. This strategy significantly expands hydrochromic colours to entire visible range in an eco-friendly way, which opens an avenue of smart materials for practical needs and industrialization., Water based inks used for water-jet rewritable paper (WJRP) are an environmental friendly alternative to conventional printing, but black colour in WJRP could not be realized so far. Here the authors demonstrate black as well as other colour WJRP based on binary systems containing less-sensitive acidochromic dyes and mild proton donors.

Rewritable paper has recently become prevalent in both academic research and marketplace due to the potential environmental advantages, including forest conservation, pollution reduction, energy saving and resource sustainability. However, its real-life applications are limited by a lack of effective strategy to realize multicolour and water-jet printing on rewritable paper with long legible image-lasting times. Herein, we report an effective strategy to construct rewritable paper based on colour or luminescence switching induced by dynamic metal–ligand coordination. This type of rewritable paper can be conveniently utilized for multicolour water-jet printing by using aqueous solutions containing different metal salts as ink. In addition, the printed images on the water-jet rewritable paper can be retained for a long time (> 6 months), which shows great progress compared to previous work. We believe that this type of rewritable paper could be considered as a prototype for multicolour water-jet printing to meet the practical needs., Rewritable paper is environmentally favourable, but its practical realization is stifled by limited ink colour versatility and poor image retention times. Here, the authors exploit the relatively stable but reversible nature of metal–organic coordination bonds to produce long-lasting and multicoloured inks for rewritable paper.

Silicon and graphene are promising anode materials for lithium-ion batteries because of their high theoretical capacity; however, low volumetric energy density, poor efficiency and instability in high loading electrodes limit their practical application. Here we report a large area (approximately 15 cm × 2.5 cm) self-standing anode material consisting of molecular precursor-derived silicon oxycarbide glass particles embedded in a chemically-modified reduced graphene oxide matrix. The porous reduced graphene oxide matrix serves as an effective electron conductor and current collector with a stable mechanical structure, and the amorphous silicon oxycarbide particles cycle lithium-ions with high Coulombic efficiency. The paper electrode (mass loading of 2 mg cm−2) delivers a charge capacity of ∼588 mAh g−1electrode (∼393 mAh cm−3electrode) at 1,020th cycle and shows no evidence of mechanical failure. Elimination of inactive ingredients such as metal current collector and polymeric binder reduces the total electrode weight and may provide the means to produce efficient lightweight batteries., Most high-loading silicon-based anodes for lithium-ion batteries suffer from low efficiency and volumetric capacity. Here, the authors show that a paper-like electrode of silicon oxycarbide glass and graphene at mass loading of >2 mg cm−2 can efficiently deliver high energy density for over 1,000 cycles.

Ubiquitous use of electronic devices has led to an unprecedented increase in related waste as well as the worldwide depletion of reserves of key chemical elements required in their manufacturing. The use of biodegradable and abundant organic (carbon-based) electronic materials can contribute to alleviate the environmental impact of the electronic industry. The pigment eumelanin is a bio-sourced candidate for environmentally benign (green) organic electronics. The biodegradation of eumelanin extracted from cuttlefish ink is studied both at 25 °C (mesophilic conditions) and 58 °C (thermophilic conditions) following ASTM D5338 and comparatively evaluated with the biodegradation of two synthetic organic electronic materials, namely copper (II) phthalocyanine (Cu–Pc) and polyphenylene sulfide (PPS). Eumelanin biodegradation reaches 4.1% (25 °C) in 97 days and 37% (58 °C) in 98 days, and residual material is found to be without phytotoxic effects. The two synthetic materials, Cu–Pc and PPS, do not biodegrade; Cu–Pc brings about the inhibition of microbial respiration in the compost. PPS appears to be potentially phytotoxic. Finally, some considerations regarding the biodegradation test as well as the disambiguation of “biodegradability” and “bioresorbability” are highlighted., Waste build-up from organic electronic components is a major environmental issue; biodegradable electronic materials could be a solution to this. Here, the authors report on the biodegradation of bio-sourced and synthetic electronic materials in industrial compost at different temperatures.

Root nodules are agricultural-important symbiotic plant-microbe composites in which microorganisms receive energy from plants and reduce dinitrogen (N2) into fertilizers. Mimicking root nodules using artificial devices can enable renewable energy-driven fertilizer production. This task is challenging due to the necessity of a microscopic dioxygen (O2) concentration gradient, which reconciles anaerobic N2 fixation with O2-rich atmosphere. Here we report our designed electricity-powered biological|inorganic hybrid system that possesses the function of root nodules. We construct silicon-based microwire array electrodes and replicate the O2 gradient of root nodules in the array. The wire array compatibly accommodates N2-fixing symbiotic bacteria, which receive energy and reducing equivalents from inorganic catalysts on microwires, and fix N2 in the air into biomass and free ammonia. A N2 reduction rate up to 6.5 mg N2 per gram dry biomass per hour is observed in the device, about two orders of magnitude higher than the natural counterparts., Root nodules are of key importance in nitrogen fixation. Here, the authors report on an electrically powered artificial root nodule for nitrogen fixation made from silicon-based microwires which can accommodate nitrogen fixing symbiotic bacteria for fixing nitrogen into biomass and free ammonia.

Biological lignin valorization has emerged as a major solution for sustainable and cost-effective biorefineries. However, current biorefineries yield lignin with inadequate fractionation for bioconversion, yet substantial changes of these biorefinery designs to focus on lignin could jeopardize carbohydrate efficiency and increase capital costs. We resolve the dilemma by designing ‘plug-in processes of lignin’ with the integration of leading pretreatment technologies. Substantial improvement of lignin bioconversion and synergistic enhancement of carbohydrate processing are achieved by solubilizing lignin via lowering molecular weight and increasing hydrophilic groups, addressing the dilemma of lignin- or carbohydrate-first scenarios. The plug-in processes of lignin could enable minimum polyhydroxyalkanoate selling price at as low as $6.18/kg. The results highlight the potential to achieve commercial production of polyhydroxyalkanoates as a co-product of cellulosic ethanol. Here, we show that the plug-in processes of lignin could transform biorefinery design toward sustainability by promoting carbon efficiency and optimizing the total capital cost., The current biorefineries yield lignin with inadequate fractionation for bioconversion, yet substantial changes of these biorefinery designs could jeopardize carbohydrate efficiency and increase capital costs. Here the authors resolve the dilemma by designing ‘plug-in processes of lignin’ to enable economic waste valorization.

Organic electronics is emerging for large-area applications such as photovoltaic cells, rollable displays or electronic paper. Its future development and integration will require a simple, low-power organic memory, that can be written, erased and readout electrically. Here we demonstrate a non-volatile memory in which the ferroelectric polarisation state of an organic tunnel barrier encodes the stored information and sets the readout tunnel current. We use high-sensitivity piezoresponse force microscopy to show that films as thin as one or two layers of ferroelectric poly(vinylidene fluoride) remain switchable with low voltages. Submicron junctions based on these films display tunnel electroresistance reaching 1,000% at room temperature that is driven by ferroelectric switching and explained by electrostatic effects in a direct tunnelling regime. Our findings provide a path to develop low-cost, large-scale arrays of organic ferroelectric tunnel junctions on silicon or flexible substrates., Ferroelectric organic materials can be used for tunnel barriers in memory devices as a cheaper and eco-friendly replacement of their inorganic counterparts. Here, Tian et al. use poly(vinylidene fluoride) with 1–2 layer thickness to achieve giant tunnel electroresistance of 1,000% at room temperature.

The degradation of intrinsic properties of graphene during the transfer process constitutes a major challenge in graphene device fabrication, stimulating the need for direct growth of graphene on dielectric substrates. Previous attempts of metal-induced transformation of diamond and silicon carbide into graphene suffers from metal contamination and inability to scale graphene growth over large area. Here, we introduce a direct approach to transform polycrystalline diamond into high-quality graphene layers on wafer scale (4 inch in diameter) using a rapid thermal annealing process facilitated by a nickel, Ni thin film catalyst on top. We show that the process can be tuned to grow single or multilayer graphene with good electronic properties. Molecular dynamics simulations elucidate the mechanism of graphene growth on polycrystalline diamond. In addition, we demonstrate the lateral growth of free-standing graphene over micron-sized pre-fabricated holes, opening exciting opportunities for future graphene/diamond-based electronics., Direct growth of large-area graphene on dielectric substrates is a promising route to wafer scale integration. Here the authors use a rapid thermal annealing process to grow graphene layers on four-inch diameter polycrystalline diamond, eliminating the need for transfer.

Graphene-based membranes demonstrating ultrafast water transport, precise molecular sieving of gas and solvated molecules shows great promise as novel separation platforms; however, scale-up of these membranes to large-areas remains an unresolved problem. Here we demonstrate that the discotic nematic phase of graphene oxide (GO) can be shear aligned to form highly ordered, continuous, thin films of multi-layered GO on a support membrane by an industrially adaptable method to produce large-area membranes (13 × 14 cm2) in 90%) for charged and uncharged organic probe molecules with a hydrated radius above 5 Å as well as modest (30–40%) retention of monovalent and divalent salts. The highly ordered graphene sheets in the plane of the membrane make organized channels and enhance the permeability (71±5 l m−2 hr−1 bar−1 for 150±15 nm thick membranes)., Membranes made from graphene have ultra-fast water transport and precise molecular sieving properties. Here, the authors show how large-area membranes can be manufactured by a rapid and scalable process based on shear alignment of graphene-oxide liquid crystals for unlocking industrial applications.

The high thermal conductivity of graphene and few-layer graphene undergoes severe degradations through contact with the substrate. Here we show experimentally that the thermal management of a micro heater is substantially improved by introducing alternative heat-escaping channels into a graphene-based film bonded to functionalized graphene oxide through amino-silane molecules. Using a resistance temperature probe for in situ monitoring we demonstrate that the hotspot temperature was lowered by ∼28 °C for a chip operating at 1,300 W cm−2. Thermal resistance probed by pulsed photothermal reflectance measurements demonstrated an improved thermal coupling due to functionalization on the graphene–graphene oxide interface. Three functionalization molecules manifest distinct interfacial thermal transport behaviour, corroborating our atomistic calculations in unveiling the role of molecular chain length and functional groups. Molecular dynamics simulations reveal that the functionalization constrains the cross-plane phonon scattering, which in turn enhances in-plane heat conduction of the bonded graphene film by recovering the long flexural phonon lifetime., The high thermal conductivity of graphene is considerably reduced when the two-dimensional material is in contact with a substrate. Here, the authors show that thermal management of a micro heater is improved using graphene-based films covalently bonded by amino-silane molecules to graphene oxide.

The interest in mechanical properties of two-dimensional materials has emerged in light of new device concepts taking advantage of flexing, adhesion and friction. Here we demonstrate an effective method to measure adhesion of graphene atop highly ordered pyrolytic graphite, utilizing atomic-scale ‘blisters' created in the top layer by neon atom intercalates. Detailed analysis of scanning tunnelling microscopy images is used to reconstruct atomic positions and the strain map within the deformed graphene layer, and demonstrate the tip-induced subsurface translation of neon atoms. We invoke an analytical model, originally devised for graphene macroscopic deformations, to determine the graphite adhesion energy of 0.221±0.011 J m−2. This value is in excellent agreement with reported macroscopic values and our atomistic simulations. This implies mechanical properties of graphene scale down to a few-nanometre length. The simplicity of our method provides a unique opportunity to investigate the local variability of nanomechanical properties in layered materials., Analysis of the mechanical properties of two-dimensional materials is important for device development. Here, the authors report a microscopic method for measuring the adhesion of graphene on top of highly ordered pyrolytic graphite, which exploits atomic-scale blisters formed upon neon atom intercalation.

Herein, we report on a significant discovery, namely, the quantitative discharging of reduced graphite forms, such as graphite intercalation compounds, graphenide dispersions and graphenides deposited on surfaces with the simple solvent benzonitrile. Because of its comparatively low reduction potential, benzonitrile is reduced during this process to the radical anion, which exhibits a red colour and serves as a reporter molecule for the quantitative determination of negative charges on the carbon sheets. Moreover, this discovery reveals a very fundamental physical–chemical phenomenon, namely a quantitative solvent reduction induced and electrostatically driven mass transport of K+ ions from the graphite intercalation compounds into the liquid. The simple treatment of dispersed graphenides suspended on silica substrates with benzonitrile leads to the clean conversion to graphene. This unprecedented procedure represents a rather mild, scalable and inexpensive method for graphene production surpassing previous wet-chemical approaches., Graphite intercalation compounds are promising precursors for the reductive exfoliation of graphene. Here, the authors unveil the discharging mechanism of reduced graphitic compounds in a solid/liquid phase reaction, and further demonstrate its practical use for graphene production.

Electrochemical water splitting is one of the most economical and sustainable methods for large-scale hydrogen production. However, the development of low-cost and earth-abundant non-noble-metal catalysts for the hydrogen evolution reaction remains a challenge. Here we report a two-dimensional coupled hybrid of molybdenum carbide and reduced graphene oxide with a ternary polyoxometalate-polypyrrole/reduced graphene oxide nanocomposite as a precursor. The hybrid exhibits outstanding electrocatalytic activity for the hydrogen evolution reaction and excellent stability in acidic media, which is, to the best of our knowledge, the best among these reported non-noble-metal catalysts. Theoretical calculations on the basis of density functional theory reveal that the active sites for hydrogen evolution stem from the pyridinic nitrogens, as well as the carbon atoms, in the graphene. In a proof-of-concept trial, an electrocatalyst for hydrogen evolution is fabricated, which may open new avenues for the design of nanomaterials utilizing POMs/conducting polymer/reduced-graphene oxide nanocomposites., The development of low-cost and earth-abundant non-noble-metal catalysts for the hydrogen evolution reaction remains a challenge. Here, the authors report and evaluate a catalyst based on a two-dimensional coupled hybrid of molybdenum carbide and reduced graphene oxide.

Synthesis and patterning of carbon nanomaterials cost effectively is a challenge in electronic and energy storage devices. Here report a one-step, scalable approach for producing and patterning porous graphene films with 3-dimensional networks from commercial polymer films using a CO2 infrared laser. The sp3-carbon atoms are photothermally converted to sp2-carbon atoms by pulsed laser irradiation. The resulting laser-induced graphene (LIG) exhibits high electrical conductivity. The LIG can be readily patterned to interdigitated electrodes for in-plane microsupercapacitors with specific capacitances of >4 mF·cm−2 and power densities of ~9 mW·cm−2. Theoretical calculations partially suggest that enhanced capacitance may result from LIG’s unusual ultra-polycrystalline lattice of pentagon-heptagon structures. Combined with the advantage of one-step processing of LIG in air from commercial polymer sheets, which would allow the employment of a roll-to-roll manufacturing process, this technique provides a rapid route to polymer-written electronic and energy storage devices.

Large-area synthesis of high-quality graphene by chemical vapour deposition on metallic substrates requires polishing or substrate grain enlargement followed by a lengthy growth period. Here we demonstrate a novel substrate processing method for facile synthesis of mm-sized, single-crystal graphene by coating polycrystalline platinum foils with a silicon-containing film. The film reacts with platinum on heating, resulting in the formation of a liquid platinum silicide layer that screens the platinum lattice and fills topographic defects. This reduces the dependence on the surface properties of the catalytic substrate, improving the crystallinity, uniformity and size of graphene domains. At elevated temperatures growth rates of more than an order of magnitude higher (120 μm min−1) than typically reported are achieved, allowing savings in costs for consumable materials, energy and time. This generic technique paves the way for using a whole new range of eutectic substrates for the large-area synthesis of 2D materials., Innovative substrate engineering is necessary to improve the quality of CVD-synthesized graphene. Here the authors demonstrate in situ fabrication of an eutectic Pt-Si alloy that forms a wetting liquid surface on polycrystalline Pt foils, allowing millimetre-sized graphene crystals to grow in minutes.

Recent years have seen the rapid growth of new approaches to optical imaging, with an emphasis on extracting three-dimensional (3D) information from what is normally a two-dimensional (2D) image capture. Perhaps most importantly, the rise of computational imaging enables both new physical layouts of optical components and new algorithms to be implemented. This paper concerns the convergence of two advances: the development of a transparent focal stack imaging system using graphene photodetector arrays, and the rapid expansion of the capabilities of machine learning including the development of powerful neural networks. This paper demonstrates 3D tracking of point-like objects with multilayer feedforward neural networks and the extension to tracking positions of multi-point objects. Computer simulations further demonstrate how this optical system can track extended objects in 3D, highlighting the promise of combining nanophotonic devices, new optical system designs, and machine learning for new frontiers in 3D imaging., Transparent photodetectors based on graphene stacked vertically along the optical axis have shown promising potential for light field reconstruction. Here, the authors develop transparent photodetector arrays and implement a neural network for real-time 3D optical imaging and object tracking.

Low-cost flexible microwave circuits with compact size and light weight are highly desirable for flexible wireless communication and other miniaturized microwave systems. However, the prevalent studies on flexible microwave electronics have only focused on individual flexible microwave elements such as transistors, inductors, capacitors, and transmission lines. Thinning down supporting substrate of rigid chip-based monolithic microwave integrated circuits has been the only approach toward flexible microwave integrated circuits. Here, we report a flexible microwave integrated circuit strategy integrating membrane AlGaN/GaN high electron mobility transistor with passive impedance matching networks on cellulose nanofibril paper. The strategy enables a heterogeneously integrated and, to our knowledge, the first flexible microwave amplifier that can output 10 mW power beyond 5 GHz and can also be easily disposed of due to the use of cellulose nanofibril paper as the circuit substrate. The demonstration represents a critical step forward in realizing flexible wireless communication devices., Though flexible microwave integrated circuits (MICs) are desirable for the construction of functional microwave amplifier circuits, realizing low cost III-V-based MMICs remains a challenge. Here, the authors report a heterogeneous integration strategy for the fabrication of flexible low-cost MICs.

Herein, we present an innovative approach for transforming commonly available cellulose paper into a flexible and catalytic current collector for overall water splitting. A solution processed soak-and-coat method of electroless plating was used to render a piece of paper conducting by conformably depositing metallic nickel nanoparticles, while still retaining the open macroporous framework. Proof-of-concept paper-electrodes are realized by modifying nickel-paper current collector with model electrocatalysts nickel-iron oxyhydroxide and nickel-molybdenum bimetallic alloy through electrodeposition route. The paper-electrodes demonstrate exceptional activities towards oxygen evolution reaction and hydrogen evolution reaction, requiring overpotentials of 240 and 32 mV at 50 and −10 mA cm−2, respectively, even as they endure extreme mechanical stress. The generality of this approach is demonstrated by fabricating similar electrodes on cotton fabric, which also show high activity. Finally, a two-electrode paper-electrolyzer is constructed which can split water with an efficiency of 98.01%, and exhibits robust stability for more than 200 h., Water electrolysis provides a means to convert water into carbon-neutral fuels, but current devices are typically heavy, inflexible, or require costly substrates. Here, the authors transform paper and cotton fabrics into efficient, durable, and flexible supports for water-splitting electrocatalysts.

A natural operational paradigm for distributed quantum and classical information processing involves local operations coordinated by multiple rounds of public communication. In this paper we consider the minimum number of communication rounds needed to perform the locality-constrained task of entanglement transformation and the analogous classical task of secrecy manipulation. Specifically we address whether bipartite mixed entanglement can always be converted into pure entanglement or whether unsecure classical correlations can always be transformed into secret shared randomness using local operations and a bounded number of communication exchanges. Our main contribution in this paper is an explicit construction of quantum and classical state transformations which, for any given $r$, can be achieved using $r$ rounds of classical communication exchanges but no fewer. Our results reveal that highly complex communication protocols are indeed necessary to fully harness the information-theoretic resources contained in general quantum and classical states. The major technical contribution of this manuscript lies in proving lower bounds for the required number of communication exchanges using the notion of common information and various lemmas built upon it. We propose a classical analog to the Schmidt rank of a bipartite quantum state which we call the secrecy rank, and we show that it is a monotone under stochastic local classical operations., Submitted to QIP 2017. Proof strategies have been streamlined and differ from the submitted version

Initiation of Mariana-type oceanic subduction zones requires rheologically strong oceanic lithosphere, which developed through secular cooling of Earth’s mantle. Here, we report a 518 Ma Mariana-type subduction initiation ophiolite from northern Tibet, which, along with compilation of similar ophiolites through Earth history, argues for the establishment of the modern plate tectonic regime by the early Cambrian. The ophiolite was formed during the subduction initiation of the Proto-Tethys Ocean that coincided with slab roll-back along the southern and western Gondwana margins at ca. 530-520 Ma. This global tectonic re-organization and the establishment of modern plate tectonic regime was likely controlled by secular cooling of the Earth, and facilitated by enhanced lubrication of subduction zones by sediments derived from widespread surface erosion of the extensive mountain ranges formed during Gondwana assembly. This time also corresponds to extreme events recorded in climate and surface proxies that herald formation of the contemporary Earth., This paper placed the identified Mariana type ophiolite within a global tectonic re-organization at ca. 530-520 Ma. Similar ophiolites, together with other geological and chemical proxies, newly constrained the timing of establishment of modern plate tectonics, along with its links to surficial changes that characterize the contemporary Earth.

Although significant progress has been made in the development of light-emitting materials for organic light-emitting diodes along with the elucidation of emission mechanisms, the electron injection/transport mechanism remains unclear, and the materials used for electron injection/transport have been basically unchanged for more than 20 years. Here, we unravelled the electron injection/transport mechanism by tuning the work function near the cathode to about 2.0 eV using a superbase. This extremely low-work function cathode allows direct electron injection into various materials, and it was found that organic materials can transport electrons independently of their molecular structure. On the basis of these findings, we have realised a simply structured blue organic light-emitting diode with an operational lifetime of more than 1,000,000 hours. Unravelling the electron injection/transport mechanism, as reported in this paper, not only greatly increases the choice of materials to be used for devices, but also allows simple device structures. Understanding the role electron injection and transport in organic light-emitting diodes (OLED) is critical for optimizing device performance. Here, the authors elucidate the electron injection/transport mechanism in OLEDs and identify the cathode/emissive layer energy barrier as the key factor.

Active metasurfaces, whose optical properties can be modulated post-fabrication, have emerged as an intensively explored field in recent years. The efforts to date, however, still face major performance limitations in tuning range, optical quality, and efficiency, especially for non-mechanical actuation mechanisms. In this paper, we introduce an active metasurface platform combining phase tuning in the full 2π range and diffraction-limited performance using an all-dielectric, low-loss architecture based on optical phase change materials (O-PCMs). We present a generic design principle enabling binary switching of metasurfaces between arbitrary phase profiles and propose a new figure-of-merit (FOM) tailored for reconfigurable meta-optics. We implement the approach to realize a high-performance varifocal metalens operating at 5.2 μm wavelength. The reconfigurable metalens features a record large switching contrast ratio of 29.5 dB. We further validate aberration-free and multi-depth imaging using the metalens, which represents a key experimental demonstration of a non-mechanical tunable metalens with diffraction-limited performance., Here, the authors report an active all-dielectric metasurface platform based on phase change materials, combining phase tuning in the full 2π range, and demonstrate aberration-free and multi-depth imaging with a non-mechanical tunable metalens.

The Tafel slope is a key parameter often quoted to characterize the efficacy of an electrochemical catalyst. In this paper, we develop a Bayesian data analysis approach to estimate the Tafel slope from experimentally-measured current-voltage data. Our approach obviates the human intervention required by current literature practice for Tafel estimation, and provides robust, distributional uncertainty estimates. Using synthetic data, we illustrate how data insufficiency can unknowingly influence current fitting approaches, and how our approach allays these concerns. We apply our approach to conduct a comprehensive re-analysis of data from the CO2 reduction literature. This analysis reveals no systematic preference for Tafel slopes to cluster around certain "cardinal values” (e.g. 60 or 120 mV/decade). We hypothesize several plausible physical explanations for this observation, and discuss the implications of our finding for mechanistic analysis in electrochemical kinetic investigations. The Tafel slope in electrochemical catalysis is usually determined from experimental data and remains error-prone. Here, the authors develop a Bayesian approach for Tafel slope quantification, and apply it to study the prevalence of certain "cardinal" Tafel slopes in the electrochemical CO2 reduction literature.

Seawater desalination plays a critical role in addressing the global water shortage challenge. Directional Solvent Extraction (DSE) is an emerging non-membrane desalination technology that features the ability to utilize very low temperature waste heat (as low as 40 °C). This is enabled by the subtly balanced solubility properties of directional solvents, which do not dissolve in water but can dissolve water and reject salt ions. However, the low water yield of the state-of-the-art directional solvent (decanoic acid) significantly limits its throughput and energy efficiency. In this paper, we demonstrate that by using ionic liquid as a new directional solvent, saline water can be desalinated with much higher production rate and thus significantly lower the energy and exergy consumptions. The ionic liquid identified suitable for DSE is [emim][Tf2N], which has a much (~10×) higher water yield than the currently used decanoic acid. Using molecular dynamics simulations with Gibbs free energy calculations, we reveal that water dissolving in [emim][Tf2N] is energetically favorable, but it takes significant energy for [emim][Tf2N] ions to dissolve in water. Our findings may significantly advance the DSE technology as a solution to the challenges in the global water-energy nexus., Directional Solvent Extraction is an emerging non-membrane desalination technology for sea water desalination but is limited by throughput and energy efficiency. Here, the authors demonstrate that the production rate and energy efficiency can be increased by using ionic liquids as directional solvent.

One of the main applications of atomistic computer simulations is the calculation of ligand binding free energies. The accuracy of these calculations depends on the force field quality and on the thoroughness of configuration sampling. Sampling is an obstacle in simulations due to the frequent appearance of kinetic bottlenecks in the free energy landscape. Very often this difficulty is circumvented by enhanced sampling techniques. Typically, these techniques depend on the introduction of appropriate collective variables that are meant to capture the system’s degrees of freedom. In ligand binding, water has long been known to play a key role, but its complex behaviour has proven difficult to fully capture. In this paper we combine machine learning with physical intuition to build a non-local and highly efficient water-describing collective variable. We use it to study a set of host-guest systems from the SAMPL5 challenge. We obtain highly accurate binding free energies and good agreement with experiments. The role of water during the binding process is then analysed in some detail. © 2021, The Author(s)., Nature Communications, 12 (1), ISSN:2041-1723

Recently, we classified the oceans into 30 biogeographic realms based on species’ endemicity. Castro-Insua et al. criticize the choices of dissimilarity coefficients and clustering approaches used in our paper, and reanalyse the data using alternative techniques. Here, we explain how the approaches used in our original paper yield results in line with existing biogeographical knowledge and are robust to alternative methods of analysis. We also repeat the analysis using several similarity coefficients and clustering algorithms, and a neural network theory method. Although each combination of methods produces outputs differing in detail, the overall pattern of realms is similar. The coarse nature of the present boundaries of the realms reflects the limited field data but may be improved with additional data and mapping to environmental variables.

Large amounts of waste heat generated in our fossil-fuel based economy can be converted into useful electric power by using thermoelectric generators. However, the low-efficiency, scarcity, high-cost and poor production scalability of conventional thermoelectric materials are hindering their mass deployment. Nanoengineering has proven to be an excellent approach for enhancing thermoelectric properties of abundant and cheap materials such as silicon. Nevertheless, the implementation of these nanostructures is still a major challenge especially for covering the large areas required for massive waste heat recovery. Here we present a family of nano-enabled materials in the form of large-area paper-like fabrics made of nanotubes as a cost-effective and scalable solution for thermoelectric generation. A case study of a fabric of p-type silicon nanotubes was developed showing a five-fold improvement of the thermoelectric figure of merit. Outstanding power densities above 100 W/m2 at 700 °C are therefore demonstrated opening a market for waste heat recovery., To realize waste heat recovery solutions based on thermoelectricity, high-performance materials with device and manufacturing compatibility are required. Here, the authors demonstrate large-area paper-like nanostructured fabrics consisting of aligned nanotubes with high thermoelectric performance.

Miscanthus is a perennial wild grass that is of global importance for paper production, roofing, horticultural plantings, and an emerging highly productive temperate biomass crop. We report a chromosome-scale assembly of the paleotetraploid M. sinensis genome, providing a resource for Miscanthus that links its chromosomes to the related diploid Sorghum and complex polyploid sugarcanes. The asymmetric distribution of transposons across the two homoeologous subgenomes proves Miscanthus paleo-allotetraploidy and identifies several balanced reciprocal homoeologous exchanges. Analysis of M. sinensis and M. sacchariflorus populations demonstrates extensive interspecific admixture and hybridization, and documents the origin of the highly productive triploid bioenergy crop M. × giganteus. Transcriptional profiling of leaves, stem, and rhizomes over growing seasons provides insight into rhizome development and nutrient recycling, processes critical for sustainable biomass accumulation in a perennial temperate grass. The Miscanthus genome expands the power of comparative genomics to understand traits of importance to Andropogoneae grasses., The perennial grass Miscanthus is a promising biomass crop. Here, via genomics and transcriptomics, the authors reveal its allotetraploid origin, characterize gene expression associated with rhizome development and nutrient recycling, and describe the hybrid origin of the triploid M. x giganteus.

Blue/deep-blue emission is crucial for organic optoelectronics but remains a formidable challenge in organic afterglow due to the difficulties in populating and stabilizing the high-energy triplet excited states. Here, a facile strategy to realize the efficient deep-blue organic afterglow is proposed via host molecules to sensitize the triplet exciton population of guest and water implement to suppress the non-radiative decays by matrices rigidification. A series of highly luminescent deep-blue (405–428 nm) organic afterglow materials with lifetimes up to 1.67 s and quantum yields of 46.1% are developed. With these high-performance water-responsive materials, lifetime-encrypted rewritable paper has been constructed for water-jet printing of high-resolution anti-counterfeiting patterns that can retain for a long time (>1 month) and be erased by dimethyl sulfoxide vapor in 15 min with high reversibility for many write/erase cycles. These results provide a foundation for the design of high-efficient blue/deep-blue organic afterglow and stimuli-responsive materials with remarkable applications., Though realizing organic materials with deep blue emission is attractive for next-generation display technologies, achieving this emission in afterglow molecules remains a challenge. Here, the authors report blue organic afterglow via a strategy involving guest sensitization and matrix rigidification.

This paper considers options for a future Indian power economy in which renewables, wind and solar, could meet 80% of anticipated 2040 power demand supplanting the country’s current reliance on coal. Using a cost optimization model, here we show that renewables could provide a source of power cheaper or at least competitive with what could be supplied using fossil-based alternatives. The ancillary advantage would be a significant reduction in India’s future power sector related emissions of CO2. Using a model in which prices for wind turbines and solar PV systems are assumed to continue their current decreasing trend, we conclude that an investment in renewables at a level consistent with meeting 80% of projected 2040 power demand could result in a reduction of 85% in emissions of CO2 relative to what might be expected if the power sector were to continue its current coal dominated trajectory., India currently relies heavily on fossil-based sources for its power needs. Here the authors show that renewable energy in India could be cheaper than fossil-based alternatives and could reduce CO2 emissions by 85% by 2040.

Sudden steam-driven eruptions strike without warning and are a leading cause of fatalities at touristic volcanoes. Recent deaths following the 2019 Whakaari eruption in New Zealand expose a need for accurate, short-term forecasting. However, current volcano alert systems are heuristic and too slowly updated with human input. Here, we show that a structured machine learning approach can detect eruption precursors in real-time seismic data streamed from Whakaari. We identify four-hour energy bursts that occur hours to days before most eruptions and suggest these indicate charging of the vent hydrothermal system by hot magmatic fluids. We developed a model to issue short-term alerts of elevated eruption likelihood and show that, under cross-validation testing, it could provide advanced warning of an unseen eruption in four out of five instances, including at least four hours warning for the 2019 eruption. This makes a strong case to adopt real-time forecasting models at active volcanoes., In this study, the authors investigate the predictability of sudden eruptions, motivated by the 2019 eruption at Whakaari (White Island), New Zealand. The paper proposes a machine learning approach that is able to identify eruption precursors in data streaming from a single seismic station at Whakaari.

Quantum limit is quite easy to achieve once the band crossing exists exactly at the Fermi level ($E_F$) in topological semimetals. In multilayered Dirac fermion system, the density of Dirac fermions on the zeroth Landau levels (LLs) increases in proportion to the magnetic field, resulting in intriguing angle- and field-dependent interlayer tunneling conductivity near the quantum limit. BaGa$_2$ is an example of multilayered Dirac semimetal with anisotropic Dirac cone close to $E_F$, providing a good platform to study its interlayer transport properties. In this paper, we report the negative interlayer magnetoresistance (NIMR, I//c and B//c) induced by the tunneling of Dirac fermions on the zeroth LLs of neighbouring Ga layers in BaGa$_2$. When the field deviates from the c-axis, the interlayer resistivity $\rho_{zz}(\theta)$ increases and finally results in a peak with the field perpendicular to the c-axis. These unusual interlayer transport properties (NIMR and resistivity peak with B$\perp$c) are observed together for the first time in Dirac semimetal under ambient pressure and are well explained by the model of tunneling between Dirac fermions in the quantum limit., Comment: 12 pages, 8 figures, with supplementary materials

The dynamics of the first-order phase transitions involving a large displacement of atoms, for example, a liquid-solid transition, is generally dominated by the nucleation of the ordered phase and the growth of the nuclei, where the interfacial energy between the two phases plays an important role. On the other hand, electronic phase transitions seldom exhibit such a nucleation-growth behavior, probably because two-phase coexistence is not dominated by only the interfacial energy in such phase transitions. In the present paper, we report that the dynamics of a phase transition associated with an ordering of d orbitals in a vanadate exhibits a clear nucleation-growth behavior and that the interfacial energy between the orbital-ordered and -disordered phases dominated by the orbital-spin coupling can be experimentally obtained., The dynamics of many discontinuous phase transitions is determined by the nucleation and growth of regions of the new phase. Katsufuji et al. demonstrate that the orbital ordering transition of doped BaV10O15 presents an electronic example of nucleation-growth behaviour.

Special thanks to our field assistants in Indonesia (Basri, Bayu and Darwis) and to Frank Tiedemann, Edgar Tunsch, Dietmar Fellert and Malte Puhan for technical assistance. We thank PTPN VI and the owner of the plantation at Pompa Air for allowing us to conduct our research at their plantation. We would also like to thank the Spanish national project GEISpain (CGL2014-52838-C2-1-R) and the DAAD (scholarship from the programme ‘Research Stays for University Academics and Scientist 2018, ref. no. 91687130)' for partly financing A. Meijide during the preparation of this paper., The potential of palm-oil biofuels to reduce greenhouse gas (GHG) emissions compared with fossil fuels is increasingly questioned. So far, no measurement-based GHG budgets were available, and plantation age was ignored in Life Cycle Analyses (LCA). Here, we conduct LCA based on measured CO2, CH4 and N2O fluxes in young and mature Indonesian oil palm plantations. CO2 dominates the on-site GHG budgets. The young plantation is a carbon source (1012 ± 51 gC m−2 yr−1), the mature plantation a sink (−754 ± 38 gC m−2 yr−1). LCA considering the measured fluxes shows higher GHG emissions for palm-oil biodiesel than traditional LCA assuming carbon neutrality. Plantation rotation-cycle extension and earlier-yielding varieties potentially decrease GHG emissions. Due to the high emissions associated with forest conversion to oil palm, our results indicate that only biodiesel from second rotation-cycle plantations or plantations established on degraded land has the potential for pronounced GHG emission savings., This study was financed by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation)— Project-ID 192626868—in the framework of the collaborative German-Indonesian research project CRC990 (subprojects A03, A04 and A05)., Spanish national project GEISpain (CGL2014-52838-C2-1-R) and the DAAD (scholarship from the programme ‘Research Stays for University Academics and Scientist 2018, ref. no. 91687130)

Lipid-protein complexes are the basis of pulmonary surfactants covering the respiratory surface and mediating gas exchange in lungs. Cardiolipin is a mitochondrial lipid overexpressed in mammalian lungs infected by bacterial pneumonia. In addition, increased oxygen supply (hyperoxia) is a pathological factor also critical in bacterial pneumonia. In this paper we fabricate a micrometer-size graphene-based sensor to measure oxygen permeation through pulmonary membranes. Combining oxygen sensing, X-ray scattering, and Atomic Force Microscopy, we show that mammalian pulmonary membranes suffer a structural transformation induced by cardiolipin. We observe that cardiolipin promotes the formation of periodic protein–free inter–membrane contacts with rhombohedral symmetry. Membrane contacts, or stalks, promote a significant increase in oxygen gas permeation which may bear significance for alveoli gas exchange imbalance in pneumonia., Changes in the pulmonary membrane, caused by bacterial infection, form part of the pathology of pneumonia. Here, the authors report on a graphene-based oxygen sensor which is used along with X-ray diffraction and AFM to measure the structural changes and changes in oxygen permeability of pulmonary membranes associated with bacterial pneumonia.

Thanks to the nature of strong programmability, field-programmable gate arrays (FPGAs) have been playing a significant role in signal processing and control. With the explosive growth in digital data, big data analytics becomes an important emerging field, in which FPGAs are a major player. However, the computational speed and power efficiency provided by FPGAs are limited by electronic clock rates and Ohmic losses. To overcome the limitations, photonics is envisioned as an enabling solution, thanks to its ultrafast and low power consumption feature. In this paper, we propose a scalable photonic field-programmable disk array (FPDA) signal processor. Ultra-compact microdisk resonators are leveraged as a fundamental execution units in the core to route, store and process optical signals. By field-programming the processor, diverse circuit topologies can be realized to perform multiple specific signal processing functions including filtering, temporal differentiation, time delay, beamforming, and spectral shaping., FPGAs have long been of interest as reconfigurable circuits, but their electronic nature provides eventual limitations. Here the authors demonstrate a photonic digital signal processor that is field programmable using arrays of microdisk resonators.

In this paper we develop the stability rules for NASICON-structured materials, as an example of compounds with complex bond topology and composition. By first-principles high-throughput computation of 3881 potential NASICON phases, we have developed guiding stability rules of NASICON and validated the ab initio predictive capability through the synthesis of six attempted materials, five of which were successful. A simple two-dimensional descriptor for predicting NASICON stability was extracted with sure independence screening and machine learned ranking, which classifies NASICON phases in terms of their synthetic accessibility. This machine-learned tolerance factor is based on the Na content, elemental radii and electronegativities, and the Madelung energy and can offer reasonable accuracy for separating stable and unstable NASICONs. This work will not only provide tools to understand the synthetic accessibility of NASICON-type materials, but also demonstrates an efficient paradigm for discovering new materials with complicated composition and atomic structure., Sodium super ionic conductors are a class of promising energy storage materials owing to their high ionic conductivity. Here, the authors conducted high throughput calculations to understand the synthetic accessibility of NASICON-type materials and demonstrate an efficient paradigm for discovering new complex materials.

The bonding of copper ions to lattice oxygens dictates the activity and selectivity of copper exchanged zeolites. By 17O isotopic labelling of the zeolite framework, in conjunction with advanced EPR methodologies and DFT modelling, we determine the local structure of single site CuII species, we quantify the covalency of the metal-framework bond and we assess how this scenario is modified by the presence of solvating H216O or H217O molecules. This enables to follow the migration of CuII species as a function of hydration conditions, providing evidence for a reversible transfer pathway within the zeolite cage as a function of the water pressure. The results presented in this paper establish 17O EPR as a versatile tool for characterizing metal-oxide interactions in open-shell systems., The identification of catalytically active sites with atomic-scale precision occupies a central place in the theory and practice of heterogeneous catalysis. Here the authors assess the nature of the copper-oxygen bond in a Cu-CHA zeolite and recover the microscopic structure of single-metal sites.

Development of catalytic amide bond-forming methods is important because they could potentially address the existing limitations of classical methods using superstoichiometric activating reagents. In this paper, we disclose an Umpolung amidation reaction of carboxylic acids with nitroarenes and nitroalkanes enabled by the triplet synergistic catalysis of FeI2, P(V)/P(III) and photoredox catalysis, which avoids the production of byproducts from stoichiometric coupling reagents. A wide range of carboxylic acids, including aliphatic, aromatic and alkenyl acids participate smoothly in such reactions, generating structurally diverse amides in good yields (86 examples, up to 97% yield). This Umpolung amidation strategy opens a method to address challenging regioselectivity issues between nucleophilic functional groups, and complements the functional group compatibility of the classical amidation protocols. The synthetic robustness of the reaction is demonstrated by late-stage modification of complex molecules and gram-scale applications., Catalytic amide bond-forming methods is important because they could potentially address the existing limitations of classical methods using superstoichiometric activating reagents. Here the authors show an Umpolung amidation reaction of carboxylic acids with nitroarenes and nitroalkanes enabled by FeI2, P(V)/P(III) and photoredox catalysis that avoids the production of byproducts.

The dynamic evolutions of fluid-mineral systems driving large-scale geochemical transformations in the Earth’s crust remain poorly understood. We observed experimentally that successive sodic and potassic alterations of feldspar can occur via a single self-evolved, originally Na-only, hydrothermal fluid. At 600 °C, 2 kbar, sanidine ((K,Na)AlSi3O8) reacted rapidly with a NaCl fluid to form albite (NaAlSi3O8); over time, some of this albite was replaced by K-feldspar (KAlSi3O8), in contrast to predictions from equilibrium reaction modelling. Fluorine accelerated the process, resulting in near-complete back-replacement of albite within 1 day. These findings reveal that potassic alteration can be triggered by Na-rich fluids, indicating that pervasive sequential sodic and potassic alterations associated with mineralization in some of the world’s largest ore deposits may not necessarily reflect externally-driven changes in fluid alkali contents. Here, we show that these reactions are promoted at the micro-scale by a self-evolving, kinetically-driven process; such positive feedbacks between equilibrium and kinetic factors may be essential in driving pervasive mineral transformations., This paper reveals that potassic alteration can be triggered by Na-rich fluids, indicating that pervasive sequential sodic and potassic alterations associated with mineralization in some of the world’s largest ore deposits may not necessarily reflect externally-driven changes in fluid alkali contents.

Complex dynamical fluctuations, from intracellular noise, brain dynamics or computer traffic display bursting dynamics consistent with a critical state between order and disorder. Living close to the critical point has adaptive advantages and it has been conjectured that evolution could select these critical states. Is this the case of living cells? A system can poise itself close to the critical point by means of the so-called self-organized criticality (SOC). In this paper we present an engineered gene network displaying SOC behaviour. This is achieved by exploiting the saturation of the proteolytic degradation machinery in E. coli cells by means of a negative feedback loop that reduces congestion. Our critical motif is built from a two-gene circuit, where SOC can be successfully implemented. The potential implications for both cellular dynamics and behaviour are discussed., This work was supported by the Botin Foundation by Banco Santander through its Santander Universities Global Division, the Spanish Ministry of Economy and Competitiveness, grant AEI-PID2019-111680GB-I00/AEI/10.13039/501100011033, an AGAUR FI 2018 grant, and the Santa Fe Institute (where the key idea was conceived). J.S. and A.G. have been partially funded by the CERCA Programme of the Generalitat de Catalunya. J.S. acknowledges support from Agencia Estatal de Investigación grant RTI2018-098322-B-I00 and Ramón y Cajal contract RYC-2017-22243. A.G. has been funded by the AGAUR grant 2017-SGR-1049 and by the MINECO-FEDER-UE grants PGC-2018-098676-B-100 and RTI2018-093860-B-C21.

Donor spins in silicon provide a promising material platform for large scale quantum computing. Excellent electron spin coherence times of \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$${T}_{2}^{* }=268$$\end{document}T2*=268 μs with fidelities of 99.9% have been demonstrated for isolated phosphorus donors in isotopically pure 28Si, where donors are local-area-implanted in a nanoscale MOS device. Despite robust single qubit gates, realising two-qubit exchange gates using this technique is challenging due to the statistical nature of the dopant implant and placement process. In parallel a precision scanning probe lithography route has been developed to place single donors and donor molecules on one atomic plane of silicon with high accuracy aligned to heavily phosphorus doped silicon in-plane gates. Recent results using this technique have demonstrated a fast (0.8 ns) two-qubit gate with two P donor molecules placed 13 nm apart in natSi. In this paper we demonstrate a single qubit gate with coherent oscillations of the electron spin on a P donor molecule in natSi patterned by scanning tunneling microscope (STM) lithography. The electron spin exhibits excellent coherence properties, with a \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$${T}_{2}$$\end{document}T2 decoherence time of 298 ± 30 μs, and \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$${T}_{2}^{* }$$\end{document}T2* dephasing time of 295 ± 23 ns., Multi-donor molecules in Si provide a promising qubit platform, offering advantages over single donor qubits in terms of performance and fabrication. Here, the authors report a single qubit gate and long coherence times in a P donor molecule qubit in natural Si patterned by scanning tunneling microscope hydrogen lithography.

The origins of spin lifetimes in quantum systems is a matter of importance in several areas of quantum information. Spectrally mapping spin relaxation processes provides insight into their origin and motivates methods to mitigate them. In this paper, we map nuclear relaxation in a prototypical system of $${}^{13}{\rm{C}}$$ 13 C nuclei in diamond coupled to Nitrogen Vacancy (NV) centers over a wide field range (1 mT-7 T). Nuclear hyperpolarization through optically pumped NV electrons allows signal measurement savings exceeding million-fold over conventional methods. Through a systematic study with varying substitutional electron (P1 center) and $${}^{13}{\rm{C}}$$ 13 C concentrations, we identify the operational relaxation channels for the nuclei at different fields as well as the dominant role played by $${}^{13}{\rm{C}}$$ 13 C coupling to the interacting P1 electronic spin bath. These results motivate quantum control techniques for dissipation engineering to boost spin lifetimes in diamond, with applications including engineered quantum memories and hyperpolarized $${}^{13}{\rm{C}}$$ 13 C imaging.

Fast switching ‘transparent-to-black’ electrochromic devices are currently under investigation as potential candidates in modern applications like e-papers or with additional functionality as ultracompact iris or switchable neutral filter in camera systems. However, recent electrochromic devices show either a lack of contrast or slow response times. To overcome these deficiencies we focus on a careful material composition of the colouring hybrid electrodes in our device. We have established a nanoporous Sb-doped SnO\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$${}_{2}$$\end{document}2 electrode as supporting electrode for chemisorbed electrochromic tetraphenylbenzidine molecules due to its good conductivity in the redox potential range of the molecule. This hybrid electrode was combined with a modified nanoporous TiO\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$${}_{2}$$\end{document}2 / viologen electrode to realize a high performance, complementary electrochromic device. Fast switching time constants of 0.5 s and concurrently high change in optical density \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$\Delta$$\end{document}ΔOD = 2.04 at 605 nm confirm our successful concept. The achieved colouration efficiency of 440 cm\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$${}^{2}$$\end{document}2 C\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$${}^{-1}$$\end{document}−1 exceeds every high contrast device presented so far., Electrochromic devices have a range of applications as switchable shutters. Here the authors report a hybrid device that uses complementary electrochromic molecules immobilized on nanoporous electrodes to concurrently achieve fast colouration and bleaching with high contrast over a broad spectral range.

The benzylic positions in drugs are sites that readily react with cytochrome P450 oxidases via single-electron oxidation. New synthetic methodologies to incorporate a fluoroalkyl group at the benzylic site are continually being developed, and in this paper, we report a metal-free and site-selective organophotoredox-catalyzed trifluoromethylthiolation of benzylic C-H bonds for a wide variety of alkyl arenes and heteroarenes. The precise and predictive regioselectivity among various C(sp3)-H bonds originates from an inner-sphere benzylic radical initiation mechanism, and avoids the use of external oxidants or hydrogen atom abstractors. Its practicality stems from the trifluoromethylthiolation of a series of drugs and complex organic molecules, which is overwhelmingly selective for benzyl groups. This operationally simple protocol can provide a general and practical access to structurally diverse benzylic trifluoromethyl sulfides produced from ubiquitous benzylic C-H bonds. Large scale trifluoromethylthiolation can be achieved with continuous flow photoredox technology., Fluoroalkylation of C-H bonds is a class of reaction highly sought after in medicinal chemistry. Here, the authors report a regioselective organophotoredox-catalyzed, trifluoromethylthiolation of benzylic C-H bonds for a wide variety of alkyl (hetero)arenes, and demonstrate its utility in continuous flow.

Spin ice systems display a variety of very nontrivial properties, the most striking being the existence in them of magnetic monopoles. Such monopole states can also have nontrivial electric properties: there exist electric dipoles attached to each monopole. A novel situation is encountered in the moment fragmentation (MF) state, in which monopoles and antimonopoles are perfectly ordered, whereas spins themselves remain disordered. We show that such partial ordering strongly modifies the electric activity of such systems: the electric dipoles, which are usually random and dynamic, become paired in the MF state in (d, −d) pairs, thus strongly reducing their electric activity. The electric currents existing in systems with noncoplanar spins are also strongly influenced by MF. We also consider modifications in dipole and current patterns in magnetic textures (domain walls, local defects) and at excitations with nontrivial dynamics in a MF state, which show very rich behaviour and which could in principle allow to control them by electric field., Spin-ices can exhibit a variety of remarkable phenomena, not least the appearance of emergent magnetic monopoles. In this theory paper, Daniel Khomskii shows that in the moment fragmentation state, the electric dipoles associated with magnetic monopoles become ordered, leading to a change in electrical activity.

Microdevice integrating energy storage with wireless charging could create opportunities for electronics design, such as moveable charging. Herein, we report seamlessly integrated wireless charging micro-supercapacitors by taking advantage of a designed highly consistent material system that both wireless coils and electrodes are of the graphite paper. The transferring power efficiency of the wireless charging is 52.8%. Benefitting from unique circuit structure, the intact device displays low resistance and excellent voltage tolerability with a capacitance of 454.1 mF cm−2, superior to state-of-the-art conventional planar micro-supercapacitors. Besides, a record high energy density of 463.1 μWh cm−2 exceeds the existing metal ion hybrid micro-supercapacitors and even commercial thin film battery (350 μWh cm−2). After charging for 6 min, the integrated device reaches up to a power output of 45.9 mW, which can drive an electrical toy car immediately. This work brings an insight for contactless micro-electronics and flexible micro-robotics. Miniaturized energy storage devices integrated with wireless charging bring opportunities for next generation electronics. Here, authors report seamlessly integrated wireless charging micro-supercapacitors with high energy density capable of driving a model electrical car.