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The discovery of superconductivity in CaC6 with a critical temperature (Tc) of 11.5 K reignites much interest in exploring high-temperature superconductivity in graphite intercalation compounds (GICs). Here we identify a GIC NaC4, discovered by ab initio evolutionary structure search, as a superconductor with a computed Tc of 41.2 K at 5 GPa. This value is eight times higher than that of the synthesized GIC NaC2 and possesses the highest Tc among available GICs. The remarkable superconductivity of GIC NaC4 mainly arises from the coupling of {\pi} electrons in graphene with the low-frequency vibrations involving both Na and C atoms. These findings suggest that Na-GICs may hold great promise as high-Tc superconductors., Comment: 4 figures

Large-area single-crystal surface structures were successfully prepared on Cu(111) substrate with boron deposition, which is critical for prospective applications. However, the proposed borophene structures do not match the scanning tunneling microscopy (STM) results very well, while the proposed copper boride is at odds with the traditional knowledge that ordered copper-rich borides normally do not exist due to small difference in electronegativity and large difference in atomic size. To clarify the controversy and elucidate the formation mechanism of the unexpected copper boride, we conducted systematic STM, X-ray photoelectron spectroscopy and angle-resolved photoemission spectroscopy investigations, confirming the synthesis of two-dimensional copper boride rather than borophene on Cu(111) after boron deposition under ultrahigh vacuum. First-principles calculations with defective surface models further indicate that boron atoms tend to react with Cu atoms near terrace edges or defects, which in turn shapes the intermediate structures of copper boride and leads to the formation of stable Cu-B monolayer via large-scale surface reconstruction eventually., Comment: 15 pages, 4 figures

Controlling the magnetic anisotropy of ferromagnetic materials plays a key role in magnetic switching devices and spintronic applications. Examples of spin-orbit torque devices with different magnetic anisotropy geometries (in-plane or out-of-plane directions) have been demonstrated with novel magnetization switching mechanisms for extended device functionalities. Normally, the intrinsic magnetic anisotropy in ferromagnetic materials is unchanged within a fixed direction, and thus, it is difficult to realize multifunctionality devices. Therefore, continuous modulation of magnetic anisotropy in ferromagnetic materials is highly desired but remains challenging. Here, we demonstrate a gate-tunable magnetic anisotropy transition from out-of-plane to canted and finally to in-plane in layered Fe$_5$GeTe$_2$ by combining the measurements of the angle-dependent anomalous Hall effect and magneto-optical Kerr effect with quantitative Stoner-Wohlfarth analysis. The magnetic easy axis continuously rotates in a spin-flop pathway by gating or temperature modulation. Such observations offer a new avenue for exploring magnetization switching mechanisms and realizing new spintronic functionalities., Comment: 4 figures

Helium (He) is the most inert noble gas at ambient conditions. It adopts a hexagonal close packed structure (P63/mmc) and remains in the insulating phase up to 32 TPa. In contrast, lithium (Li) is one of the most reactive metals at zero pressure, while its cubic high-pressure phase (Fd-3m) is a weak metallic electride above 475 GPa. Strikingly, a stable compound of Li5He2 (R-3m) was formed by mixing Fd-3m Li with P63/mmc He above 700 GPa. The presence of helium promotes the lattice transformation from Fd-3m Li to Pm-3m Li, and tuns the three-dimensional distributed interstitial electrons into the mixture of zero- and two-dimensional anionic electrons. This significantly increases the degree of metallization at the Fermi level, consequently, the coupling of conductive anionic electrons with the Li-dominated vibrations is the key factor to the formation of superconducting electride Li5He2 with a transition temperature up to 26 K, dynamically stable to pressures down to 210 GPa., Comment: 5 pages, 3 figures

Both boron nitride (BN) and carbon (C) have sp, sp2 and sp3 hybridization modes, and thus resulting in a variety of BN and C polymorphs with similar structures, such as hexagonal BN (hBN) and graphite, cubic BN (cBN) and diamond. Here, five types of BN polymorph structures were proposed theoretically, inspired by the graphite-diamond hybrid structures discovered in recent experiment. These BN polymorphs with graphite-diamond hybrid structures possessed excellent mechanical properties with combined high hardness and high ductility, and also exhibited various electronic properties such as semi-conductivity, semi-metallicity, and even one- and two-dimensional conductivity, differing from known insulators hBN and cBN. The simulated diffraction patterns of these BN hybrid structures could account for the unsolved diffraction patterns of intermediate products composed of "compressed hBN" and diamond-like BN, caused by phase transitions in previous experiments. Thus, this work provides a theoretical basis for the presence of these types of hybrid materials during phase transitions between graphite-like and diamond-like BN polymorphs.

The 8-Pmmn borophene, a boron analogue of graphene, hosts tilted and anisotropic massless Dirac fermion quasiparticles owing to the presence of the distorted graphene-like sublattice. First-principles calculations show that the stacked 8-Pmmn borophene is transformed into the fused three-dimensional borophene under pressure, being accompanied by the partially bond-breaking and bond-reforming. Strikingly, the fused 8-Pmmn borophene inherits the Dirac band dispersion resulting in an unusual semimetal-semimetal transition. A simple tight-binding model derived from graphene qualitatively reveals the underlying physics due to the maximum preservation of graphene-like substructure after the phase transition, which contrasts greatly to the transformation of graphite into diamond associated with the semimetal-insulator transition., Comment: 6 pages, 4 figures

Search for new high-temperature superconductors and insight into their superconducting mechanism are of fundamental importance in condensed matter physics. The discovery of near-room temperature superconductivity at more than a million atmospheres ushers in a new era for superconductors. However, the critical task of identifying materials with comparable superconductivity at near or ambient pressure remains. Carbon materials can always lead to intriguing surprises due to their structural diversity and electronic adjustability. Insulating diamond upon doping or external stimuli has achieved superconducting state. Thus, it still has a great opportunity to find superconducting ones with higher transition temperature (Tc). Here, we report an intrinsic superconducting graphite-diamond hybrid through first-principles calculations, whose atomic-resolution structural characteristics have been experimentally determined recently. The predicted Tc is approximated at 39 K at ambient pressure, and strain energizing can further boost Tc to 42 K. The strong electron-phonon coupling associated with the out-of-plane vibration of carbon atoms at the junction plays a dominant role in the superconducting transition. Our work demonstrates the great potential of such carbon materials as high-Tc superconductors, which will definitely attract extensive research., Comment: 11 pages, 3 figures

The study of superconductivity in compressed hydrides is of great interest due to measurements of high critical temperatures (Tc) in the vicinity of room temperature, beginning with the observations of LaH10 at 170-190 GPa. However, the pressures required for synthesis of these high Tc superconducting hydrides currently remain extremely high. Here we show the investigation of crystal structures and superconductivity in the La-B-H system under pressure with particle-swarm intelligence structure searches methods in combination with first-principles calculations. Structures with six stoichiometries, LaBH, LaBH3, LaBH4, LaBH6, LaBH7 and LaBH8, were predicted to become stable under pressure. Remarkably, the hydrogen atoms in LaBH8 were found to bond with B atoms in a manner that is similar to that in H3S. Lattice dynamics calculations indicate that LaBH7 and LaBH8 become dynamically stable at pressures as low as 109.2 and 48.3 GPa, respectively. Moreover, the two phases were predicted to be superconducting with a critical temperature (Tc) of 93 K and 156 K at 110 GPa and 55 GPa, respectively. Our results provide guidance for future experiments targeting new hydride superconductors with both low synthesis pressures and high Tc., Comment: 16 pages, 5 figures

New carbon forms exhibiting extraordinary physico-chemical properties can be generated from nanostructured precursors under extreme pressure. Nevertheless, synthesis of such fascinating materials is often not well understood that results, as is the case of C60 precursor, in irreproducibility of the results and impeding further progress in the materials design. Here the semiconducting amorphous carbon having bandgaps of 0.1-0.3 eV and the advantages of isotropic superhardness and superior toughness over single-crystal diamond and inorganic glasses are produced from transformation of fullerene at high pressure and moderate temperatures. A systematic investigation of the structure and bonding evolution was carried out by using rich arsenal of complimentary characterization methods, which helps to build a model of the transformation that can be used in further high p,T synthesis of novel nanocarbon systems for advanced applications. The produced amorphous carbon materials have the potential of demanding optoelectronic applications that diamond and graphene cannot achieve

First-principles calculations reveal that sodium boride (NaB3) undergoes a phase transition from a tetragonal P4/mbm phase to an orthorhombic Pbam phase at about 16 GPa, accompanied by counterintuitive lattice expansion along the crystallographic a-axis. This unusual compression behavior is identified as negative linear compressibility (NLC), which is dominantly attributed to the symmetry-breaking of boron framework. Meanwhile, the P4/mbm and Pbam phases form superionic conductors after undergoing a peculiar swap state at high temperature. Specifically, under warm conditions the Na cation pairs exhibit a rare local exchange (or rotation) behavior, which may be originated from the asymmetric energy barriers of different diffusion paths. The study of NaB3 compound sheds new light on a material with the combination of NLC and ion transportation at extreme conditions., Comment: 5 figures

Carbon is likely the most fascinating element of the periodic table because of the diversity of its allotropes stemming from its variable (sp, sp2, and sp3) bonding motifs. Exploration of new forms of carbon has been an eternal theme of contemporary scientific research. Here we report on novel amorphous carbon phases containing high fraction of sp3 bonded atoms recovered after compressing fullerene C60 to previously unexplored high pressure and temperature. The synthesized carbons are the hardest and strongest amorphous materials known to date, capable of scratching diamond crystal and approaching its strength which is evidenced by complimentary mechanical tests. Photoluminescence and absorption spectra of the materials demonstrate they are semiconductors with tunable bandgaps in the range of 1.5-2.2 eV, comparable to that of amorphous silicon. A remarkable combination of the outstanding mechanical and electronic properties makes this class of amorphous carbons an excellent candidate for photovoltaic applications demanding ultrahigh strength and wear resistance., Comment: 40 pages, 17 figures

The energy landscape of helium-nitrogen mixtures is explored by ab initio evolutionary searches, which predicted several stable helium-nitrogen compounds in the pressure range from 25 to 100 GPa. In particular, the monoclinic structure of HeN$_{22}$ consists of neutral He atoms, partially ionic dimers N$_{2}$$^{\delta-}$, and lantern-like cages N$_{20}$$^{\delta+}$. The presence of helium not only greatly enhances structural diversity of nitrogen solids, but also tremendously lowers the formation pressure of nitrogen salt. The unique nitrogen framework of (HeN$_{20}$)$^{\delta+}$N$_{2}$$^{\delta-}$ may be quenchable to ambient pressure even after removing helium. The estimated energy density of N$_{20}$$^{\delta+}$N$_{2}$$^{\delta-}$ (10.44 kJ/g) is $\sim$2.4 times larger than that of trinitrotoluene (TNT), indicating a very promising high-energy-density material., Comment: 6 pages, 4 figures

It is well known that diamond does not deform plastically at room temperature and usually fails in catastrophic brittle fracture. Here we demonstrate room-temperature dislocation plasticity in sub-micrometer sized diamond pillars by in-situ mechanical testing in the transmission electron microscope. We document in unprecedented details of spatio-temporal features of the dislocations introduced by the confinement-free compression, including dislocation generation and propagation. Atom-resolved observations with tomographic reconstructions show unequivocally that mixed-type dislocations with Burgers vectors of 1/2<110> are activated in the non-close-packed {001} planes of diamond under uniaxial compression of <111> and <110> directions, respectively, while being activated in the {111} planes under the <100> directional loading, indicating orientation-dependent dislocation plasticity. These results provide new insights into the mechanical behavior of diamond and stimulate reconsideration of the basic deformation mechanism in diamond as well as in other brittle covalent crystals at low temperatures.

Boron forms compounds with nearly all metals, with notable exception of copper and other group IB and IIB elements. Here, we report an unexpected discovery of ordered copper boride grown epitaxially on Cu(111) under ultrahigh vacuum. Scanning tunneling microscopy experiments combined with ab initio evolutionary structure prediction reveal a remarkably complex structure of 2D-Cu8B14. Strong intra-layer p-d hybridization and a large amount of charge transfer between Cu and B atoms are the key factors for the emergence of copper boride. This makes the discovered material unique and opens up the possibility of synthesizing ordered low-dimensional structures in similar immiscible systems., Comment: 19 pages

Understanding temperature-dependent hardness of covalent materials is not only of fundamental scientific interest, but also of crucial importance for technical applications. In this work, a temperature-dependent hardness formula for diamond-structured covalent materials is constructed on the basis of the dislocation theory. Our results show that, at low temperature, the Vickers hardness is mainly controlled by Poisson's ratio and shear modulus with the latter playing a dominant role. With increasing temperature, the plastic deformation mechanism undergoes a transition from shuffle-set dislocation control to glide-set dislocation control, leading to a steeper drop of hardness at high temperature. In addition, an intrinsic parameter, a3G, is revealed for diamond-structured covalent materials, which measures the resistance to soften at high temperature. Our hardness model shows remarkable agreement with experimental data. Current work not only sheds lights on the physical origin of hardness, but also provides a direct principle for superhard materials design., Comment: Main manuscript (abstract, 147 words; main text, 2012 words; 31 references; 4 figures and 2 tables, etc.), supplementary materials (4 figures)