National Laboratory for Superconductivity

We show that inversion symmetry breaking together with spin-orbit coupling leads to coupled spin and valley physics in monolayers of MoS2 and other group-VI dichalcogenides, making possible controls of spin and valley in these 2D materials. The spin-valley coupling at the valence-band edges suppresses spin and valley relaxation, as flip of each index alone is forbidden by the valley-contrasting spin splitting. Valley Hall and spin Hall effects coexist in both electron-doped and hole-doped systems. Optical interband transitions have frequency-dependent polarization selection rules which allow selective photoexcitation of carriers with various combination of valley and spin indices. Photoinduced spin Hall and valley Hall effects can generate long lived spin and valley accumulations on sample boundaries. The physics discussed here provides a route towards the integration of valleytronics and spintronics in multivalley materials with strong spin-orbit coupling and inversion symmetry breaking.

Quantized and Anomalous The Hall effect, an electromagnetic phenomenon with a straightforward explanation, has many exotic counterparts, including a quantized version occurring independently of the presence of external magnetic fields. Inspired by a theoretical prediction of the quantum anomalous Hall (QAH) effect in magnetically doped topological insulator thin films, Chang et al. (p. 167 , published online 14 March; see the Perspective by Oh ) prepared thin films of the compound Cr0.15(Bi0.1Sb0.9)1.85Te3, with Cr as the magnetic dopant. They observed a plateau in the Hall resistance as a function of the gating voltage without any applied magnetic fields, signifying the achievement of the QAH state.

We investigate the spin-orbit opened energy gap and the band topology in recently synthesized silicene as well as two-dimensional low-buckled honeycomb structures of germanium using first-principles calculations. We demonstrate that silicene with topologically nontrivial electronic structures can realize the quantum spin Hall effect (QSHE) by exploiting adiabatic continuity and the direct calculation of the Z(2) topological invariant. We predict that the QSHE can be observed in an experimentally accessible low temperature regime in silicene with the spin-orbit band gap of 1.55 meV, much higher than that of graphene. Furthermore, we find that the gap will increase to 2.9 meV under certain pressure strain. Finally, we also study germanium with a similar low-buckled stable structure, and predict that spin-orbit coupling opens a band gap of 23.9 meV, much higher than the liquid nitrogen temperature.

Significant enhancement in mechanical stiffness (10-200%) and fracture strength (approximately 50%) of graphene oxide paper, a novel paperlike material made from individual graphene oxide sheets, can be achieved upon modification with a small amount (less than 1 wt %) of Mg(2+) and Ca(2+). These results can be readily rationalized in terms of the chemical interactions between the functional groups of the graphene oxide sheets and the divalent metals ions. While oxygen functional groups on the basal planes of the sheets and the carboxylate groups on the edges can both bond to Mg(2+) and Ca(2+), the main contribution to mechanical enhancement of the paper comes from the latter.

We report the superconductivity in iron-based oxyarsenide Sm[O1-xFx]FeAs, with the onset resistivity transition temperature at 55.0K and Meissner transition at 54.6 K. This compound has the same crystal structure as LaOFeAs with shrunk crystal lattices, and becomes the superconductor with the highest critical temperature among all materials besides copper oxides up to now.

Doping single-atom metals into MoS₂ matrix can efficiently trigger the electrocatalytic hydrogen evolution activity of inert S atoms on 2D MoS₂ surface and meanwhile enhance catalytic stability and anti-poison ability.

This critical review presents the state of the art research progress, proposes strategies to improve the conductivity of solid electrolytes, discusses the chemical and electrochemical stabilities, and uncovers future perspectives for solid state batteries.

We report the superconductivity at above 30 K in a FeSe-layer compound ${\text{K}}_{0.8}{\text{Fe}}_{2}{\text{Se}}_{2}$ (nominal composition) achieved by metal K intercalating in between FeSe layers. It is isostructural to ${\text{BaFe}}_{2}{\text{As}}_{2}$ and possesses the highest ${T}_{c}$ for FeSe-layer materials so far under ambient pressure. Hall effect indicates the carriers are dominated by electron in this superconductor. We confirm that the observed superconductivity at above 30 K is due to this FeSe-based 122 phase. Our results demonstrate that FeSe-layer materials are really remarkable superconductors via structure and carrier modulation.

Ultrahigh energy density dielectric film Dielectrics help hold charge as capacitors and are fundamental energy storage components. Improving energy density and other properties may help these materials be more competitive with batteries for energy storage applications. Pan et al. introduced a specific type of nanodomain structure in a BiFeO 3 -BaTiO 3 -SrTiO 3 solid solution that dramatically increased the energy density. The nanodomains were organized so as to minimize energy loss during polarization switching. The enhancement in the dielectric properties suggests that the strategy may be useful for designing high-performance dielectrics. Science , this issue p. 578

Abstract Zinc‐based electrochemistry is attracting significant attention for practical energy storage owing to its uniqueness in terms of low cost and high safety. However, the grid‐scale application is plagued by limited output voltage and inadequate energy density when compared with more conventional Li‐ion batteries. Herein, we propose a latent high‐voltage MnO 2 electrolysis process in a conventional Zn‐ion battery, and report a new electrolytic Zn–MnO 2 system, via enabled proton and electron dynamics, that maximizes the electrolysis process. Compared with other Zn‐based electrochemical devices, this new electrolytic Zn–MnO 2 battery has a record‐high output voltage of 1.95 V and an imposing gravimetric capacity of about 570 mAh g −1 , together with a record energy density of approximately 409 Wh kg −1 when both anode and cathode active materials are taken into consideration. The cost was conservatively estimated at <US$ 10 per kWh. This result opens a new opportunity for the development of Zn‐based batteries, and should be of immediate benefit for low‐cost practical energy storage and grid‐scale applications.

Reversibly intercalating ions into host materials for electrochemical energy storage is the essence of the working principle of rocking-chair type batteries. The most relevant example is the graphite anode for rechargeable Li-ion batteries which has been commercialized in 1991 and still represents the benchmark anode in Li-ion batteries 30 years later. Learning from past lessons on alkali metal intercalation in graphite, recent breakthroughs in sodium and potassium intercalation in graphite have been demonstrated for Na-ion batteries and K-ion batteries. Interestingly, some significant differences proved to exist for the intercalation of Na+ and K+ into graphite compared with the Li+ case. Such different host-guest interactions are unique depending on the host materials and electrolytes, which greatly contribute to a deeper understanding of intercalation-type electrode materials for next generation alkali metal ion batteries. This review summarizes significant advances from both experimental and theoretical calculations with a focus on comparing the intercalation of three alkali metal ions (Li+, Na+, K+) into graphite and aims to clarify the intimate host-guest relationships and the underlying mechanisms. New approaches developed to achieve favorable intercalation coupled with the challenges in this field are also discussed. We also extrapolate alkali metal ion intercalation in graphite to mono-/multi-valent ions in layered electrode materials, which will deepen the understanding of intercalation chemistry and provide guidance to explore new guests and hosts.

We introduce an expression for the ${\mathbb{Z}}_{2}$ topological invariant of band insulators using the non-Abelian Berry connection. Our expression can identify the topological nature of a general band insulator without any of the gauge-fixing problems that plague the concrete implementation of previous invariants. This expression can be derived from the ``partner switching'' of the Wannier function center during time-reversal pumping and is thus equivalent to the ${Z}_{2}$ topological invariant proposed by Kane and Mele. Using our expression, we have recalculated the ${Z}_{2}$ topological index for several topological insulator material systems and obtained consistent results with the previous studies.

Developing bifunctional efficient and durable non-noble electrocatalysts for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is highly desirable and challenging for overall water splitting. Herein, Co–Mn carbonate hydroxide (CoMnCH) nanosheet arrays with controllable morphology and composition were developed on nickel foam (NF) as such a bifunctional electrocatalyst. It is discovered that Mn doping in CoCH can simultaneously modulate the nanosheet morphology to significantly increase the electrochemical active surface area for exposing more accessible active sites and tune the electronic structure of Co center to effectively boost its intrinsic activity. As a result, the optimized Co1Mn1CH/NF electrode exhibits unprecedented OER activity with an ultralow overpotential of 294 mV at 30 mA cm–2, compared with all reported metal carbonate hydroxides. Benefited from 3D open nanosheet array topographic structure with tight contact between nanosheets and NF, it is able to deliver a high and stable current density of 1000 mA cm–2 at only an overpotential of 462 mV with no interference from high-flux oxygen evolution. Despite no reports about effective HER on metal carbonate hydroxides yet, the small overpotential of 180 mV at 10 mA cm–2 for HER can be also achieved on Co1Mn1CH/NF by the dual modulation of Mn doping. This offers a two-electrode electrolyzer using bifunctional Co1Mn1CH/NF as both anode and cathode to perform stable overall water splitting with a cell voltage of only 1.68 V at 10 mA cm–2. These findings may open up opportunities to explore other multimetal carbonate hydroxides as practical bifunctional electrocatalysts for scale-up water electrolysis.

A robust oxygen-evolving electrocatalyst for high-performance seawater splitting was developed using a cost-effective and industrially compatible method.

Hydrogen production through electrochemical process is at the heart of key renewable energy technologies including water splitting and hydrogen fuel cells. Despite tremendous efforts, exploring cheap, efficient and durable electrocatalysts for hydrogen evolution still remains as a great challenge. Here we synthesize a nickel-carbon-based catalyst, from carbonization of metal-organic frameworks, to replace currently best-known platinum-based materials for electrocatalytic hydrogen evolution. This nickel-carbon-based catalyst can be activated to obtain isolated nickel atoms on the graphitic carbon support when applying electrochemical potential, exhibiting highly efficient hydrogen evolution performance with high exchange current density of 1.2 mA cm(-2) and impressive durability. This work may enable new opportunities for designing and tuning properties of electrocatalysts at atomic scale for large-scale water electrolysis.

Abstract Defects can greatly influence the properties of oxide materials; however, facile defect engineering of oxides at room temperature remains challenging. The generation of defects in oxides is difficult to control by conventional chemical reduction methods that usually require high temperatures and are time consuming. Here, we develop a facile room-temperature lithium reduction strategy to implant defects into a series of oxide nanoparticles including titanium dioxide (TiO 2 ), zinc oxide (ZnO), tin dioxide (SnO 2 ), and cerium dioxide (CeO 2 ). Our lithium reduction strategy shows advantages including all-room-temperature processing, controllability, time efficiency, versatility and scalability. As a potential application, the photocatalytic hydrogen evolution performance of defective TiO 2 is examined. The hydrogen evolution rate increases up to 41.8 mmol g −1 h −1 under one solar light irradiation, which is ~3 times higher than that of the pristine nanoparticles. The strategy of tuning defect oxides used in this work may be beneficial for many other related applications.

Here we report a new class of superconductors prepared by high pressure synthesis in the quaternary family ReFeAsO1-delta (Re = Sm, Nd, Pr, Ce, La) without fluorine doping. The onset superconducting critical temperature (Tc) in these compounds increases with the reduction of Re atom size, and the highest Tc obtained so far is 55 K in SmFeAsO1-delta. For the NdFeAsO1-delta system with different oxygen concentration a dome-shaped phase diagram was found.

Abstract The oxygen evolution reaction (OER) is the bottleneck that limits the energy efficiency of water-splitting. The process involves four electrons’ transfer and the generation of triplet state O 2 from singlet state species (OH - or H 2 O). Recently, explicit spin selection was described as a possible way to promote OER in alkaline conditions, but the specific spin-polarized kinetics remains unclear. Here, we report that by using ferromagnetic ordered catalysts as the spin polarizer for spin selection under a constant magnetic field, the OER can be enhanced. However, it does not applicable to non-ferromagnetic catalysts. We found that the spin polarization occurs at the first electron transfer step in OER, where coherent spin exchange happens between the ferromagnetic catalyst and the adsorbed oxygen species with fast kinetics, under the principle of spin angular momentum conservation. In the next three electron transfer steps, as the adsorbed O species adopt fixed spin direction, the OER electrons need to follow the Hund rule and Pauling exclusion principle, thus to carry out spin polarization spontaneously and finally lead to the generation of triplet state O 2 . Here, we showcase spin-polarized kinetics of oxygen evolution reaction, which gives references in the understanding and design of spin-dependent catalysts.

MXenes represent a large family of functionalized two-dimensional (2D) transition-metal carbides and carbonitrides. However, most of the understanding on their unique structures and applications stops at the theoretical suggestion and lack of experimental support. Herein, the surface structure and intercalation chemistry of Ti3C2X are clarified at the atomic scale by aberration-corrected scanning transmission electron microscope (STEM) and density functional theory (DFT) calculations. The STEM studies show that the functional groups (e.g., OH(-), F(-), O(-)) and the intercalated sodium (Na) ions prefer to stay on the top sites of the centro-Ti atoms and the C atoms of the Ti3C2 monolayer, respectively. Double Na-atomic layers are found within the Ti3C2X interlayer upon extensive Na intercalation via two-phase transition and solid-solution reactions. In addition, aluminum (Al)-ion intercalation leads to horizontal sliding of the Ti3C2X monolayer. On the basis of these observations, the previous monolayer surface model of Ti3C2X is modified. DFT calculations using the new modeling help to understand more about their physical and chemical properties. These findings enrich the understanding of the MXenes and shed light on future material design and applications. Moreover, the Ti3C2X exhibits prominent rate performance and long-term cycling stability as an anode material for Na-ion batteries.

The properties of propagating surface plasmon polaritons (SPPs) along one-dimensional metal structures have been investigated for more than 10 years and are now well understood. Because of the high confinement of electromagnetic energy, propagating SPPs have been considered to represent one of the best potential ways to construct next-generation circuits that use light to overcome the speed limit of electronics. Many basic plasmonic components have already been developed. In this review, researches on plasmonic waveguides are reviewed from the perspective of plasmonic circuits. Several circuit components are constructed to demonstrate the basic function of an optical digital circuit. In the end of this review, a prototype for an SPP-based nanochip is proposed, and the problems associated with building such plasmonic circuits are discussed. A plasmonic chip that can be practically applied is expected to become available in the near future. The prospects for creating sophisticated nanophotonic circuits by harnessing the opportunities provided by plasmonics are exciting. Yurui Fang and Mengtao Sun from the Beijing National Laboratory for Condensed Matter Physics review recent progress in the development of various components and devices for generating, manipulating and detecting surface plasmon polaritons — tightly confined waves that can be excited by light at the interface between a metal and a dielectric. Their small size offers opportunities for constructing photonic devices that are smaller than the wavelength of light, a major barrier to the miniaturization of optical integrated circuits. Fang and Sun describe how nanoscale waveguides, multiplexers, lasers, high-speed modulators, logic gates and detectors for surface plasmon polaritons are all coming to fruition. They also consider the future prospects of this technology.