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Abstract A computational search for stable structures among both α and β phases of ternary ATB4 borides (A = Mg, Ca, Sr, Ba, Al, Ga, and Zn, T is 3d or 4d transition elements) has been performed. We found that α-ATB4 compounds with A = Mg, Ca, Al, and T = V, Cr, Mn, Fe, Ni, and Co form a family of structurally stable or almost stable materials. These systems are metallic in non-magnetic states and characterized by the formation of the localized molecular-like state of 3d transition metal atom dimers, which leads to the appearance of numerous Van Hove singularities in the electronic spectrum. The closeness of such singularities to the Fermi level can be easily tuned by electron doping. For the atoms in the middle of the 3d row (Cr, Mn, and Fe), these singularities led to magnetic instabilities and magnetic ground states with a weakly metallic or semiconducting nature. Such states appear as non-trivial coexistence of the different spin ladders formed by magnetic dimers of 3d elements. These magnetic states can be characterized as an analog of the spin glass state. Experimental attempts to produce MgFeB4 and associated challenges are discussed, and promising directions for further synthetic studies are formulated.

Abstract Laser-driven coherent phonons can act as modulated strain fields and modify the adiabatic ground state topology of quantum materials. Here we use time-dependent first-principles and effective model calculations to simulate the effect of the coherent phonon induced by strong terahertz electric field on electronic carriers in the topological insulator ZrTe5. We show that a coherent A 1g Raman mode modulation can effectively pump carriers across the band gap, even though the phonon energy is about an order of magnitude smaller than the equilibrium band gap. We reveal the microscopic mechanism of this effect which occurs via Landau–Zener-Stückelberg tunneling of Bloch electrons in a narrow region in the Brillouin zone center where the transient energy gap closes when the system switches from strong to weak topological insulator. The quantum dynamics simulation results are in excellent agreement with recent pump-probe experiments in ZrTe5 at low temperature.

Abstract Ternary compounds with an immiscible pair of elements are relatively unexplored but promising for novel quantum materials discovery. Exploring what third element and its ratio that can be added to make stable ternary compounds out of an immiscible pair of elements remains a great challenge. In this work, we combine a machine learning (ML) method with ab initio calculations to efficiently search for the energetically favorable ternary La-Co-Pb compounds containing immiscible elements Co and Pb. Three previously reported structures are correctly captured by our approach. Moreover, we predict a ground state La3CoPb compound and 57 low-energy La-Co-Pb ternary compounds. Attempts to synthesize La3CoPb via multiple techniques produce mixed or multi-phases samples with, at best, ambiguous signals of the predicted lowest-energy La3CoPb and the second lowest-energy La18Co28Pb3 phases. The calculated results of Gibbs free energy are consistent with experiments, and will provide very useful guidance for further experimental synthesis.

Abstract There has been a long debate on the stable phase of iron under the Earth’s inner core conditions. Because of the solid‐liquid coexistence at the inner core boundary, the thermodynamic stability of solid phases directly relates to their melting temperatures, which remains considerable uncertainty. In the present study, we utilized a semi‐empirical potential fitted to high‐temperature ab initio data to perform a thermodynamic integration from classical systems described by this potential to ab initio systems. This method provides a smooth path for thermodynamic integration and significantly reduces the uncertainty caused by the finite‐size effect. Our results suggest the hcp phase is the stable phase of pure iron under the inner core conditions, while the free energy difference between the hcp and bcc phases is tiny, on the order of 10 s meV/atom near the melting temperature.

Abstract We report a new graphene allotrope named HOT graphene containing carbon hexagons, octagons, and tetragons. A corresponding series of nanotubes are also constructed by rolling up the HOT graphene sheet. Ab initio calculations are performed on geometric and electronic structures of the HOT graphene and the HOT graphene nanotubes. Dirac cone and high Fermi velocity are achieved in a non-hexagonal structure of HOT graphene, implying that the honeycomb structure is not an indispensable condition for Dirac fermions to exist. HOT graphene nanotubes show distinctive electronic structures depending on their topology. The (0,1) n (n ≥ 3) HOT graphene nanotubes reveal the characteristics of semimetals, while the other set of nanotubes (1,0) n shows continuously adjustable band gaps (0~ 0.51 eV) with tube size. A competition between the curvature effect and the zone-folding approximation determines the band gaps of the (1,0) n nanotubes. Novel conversion between semimetallicity and semiconductivity arises in ultra-small tubes (radius

The state-of-the-art phase-change memory is usually composed of ovonic threshold switching (OTS) material and ovonic memory switching (OMS) material for selective and data storage, respectively. OMS materials have been intensely studied, while the knowledge of the OTS mechanism is still inadequate. In this article, we have explored the local structure and electronic property of a simple OTS material, the amorphous (a-) SiTe, by first-principles calculations. The results reveal that most of the atoms in a-SiTe obey the “8-N” rule in contrast to a-GeTe, a well-studied OMS material. 76.5% of Si-centered configurations are in the form of randomly distributed tetrahedral clusters, while Te-centered configurations are relatively disordered without notable conformation. Furthermore, a large number of fivefold rings are found in a-SiTe. All of these structural characteristics lead to the high stability of a-SiTe, prohibiting its crystallization. In addition, the p state of Te also contributes much to the mid-gap states, which may be relevant for OTS behavior. Our findings provide an in-depth understanding of the structural signature and electronic properties of a-SiTe, having important implications for the design and applications of OTS materials.

Abstract In this paper, the structural, electronic, and optical properties of MoS2 multilayers are investigated by employing the first-principles method. Up to six-layers of MoS2 have been comparatively studied. The covalency and ionicity in the MoS2 monolayer are shown to be stronger than those in the bulk. As the layer number is increased to two or above two, band splitting is significant due to the interlayer coupling. We found that long plateaus emerged in the imaginary parts of the dielectric function ε2xxω $$ {\varepsilon}_2^{xx}\left(\omega \right) $$ and the joint density of states (JDOS) of MoS2 multilayers, due to the Van Hove singularities in a two-dimensional material. One, two and three small steps appear at the thresholds of both the long plateau of ε2xxω $$ {\varepsilon}_2^{xx}\left(\omega \right) $$ and JDOS, for monolayer, bilayer, and trilayer, respectively. As the number of layers further increased, the number of small steps increases and the width of the small steps decreases accordingly. Due to interlayer coupling, the longest plateau and shortest plateau of JDOS are from the monolayer and bulk, respectively.

We use cryogenic spatial–temporal photoluminescence (PL) imaging measurements down to 10 K and with short-wavelength, 405 nm laser excitation to study surface charge generation, trapping, and recombination at single bright and dark grains as well as their boundaries in model methylammonium lead iodide (MAPbI3) polycrystalline thin films. These salient conditions are shown to be critical for identifying both the detrimental and cooperative roles of grain microstructures where the dark grains serve as the PL quenching center, while the grain boundaries are largely benign and may promote electron–hole separation.

The model of a graphene (Gr) sheet putting on a silicon (Si) substrate is used to simulate the structures of Si microparticles wrapped up in a graphene cage, which may be the anode of lithium-ion batteries (LIBS) to improve the high-volume expansion of Si anode materials. The common low-energy defective graphene (d–Gr) structures of DV5–8–5, DV555–777 and SV are studied and compared with perfect graphene (p–Gr). First-principles calculations are performed to confirm the stable structures before and after Li penetrating through the Gr sheet or graphene/Si-substrate (Gr/Si) slab. The climbing image nudged elastic band (CI-NEB) method is performed to evaluate the diffusion barrier and seek the saddle point. The calculation results reveal that the d–Gr greatly reduces the energy barriers for Li diffusion in Gr or Gr/Si. The energy stability, structural configuration, bond length between the atoms and layer distances of these structures are also discussed in detail.

We propose a general-purpose, self-adaptive approach to construct a variational wave-function ansatz for highly accurate quantum dynamics simulations based on McLachlan’s variational principle. The key idea is to dynamically expand the variational ansatz along the time-evolution path such that the “McLachlan distance”, which is a measure of the simulation accuracy, remains below a set threshold. We apply this adaptive variational quantum dynamics simulation (AVQDS) approach to the integrable Lieb-Schultz-Mattis spin chain and the nonintegrable mixed-field Ising model, where it captures both finite-rate and sudden post-quench dynamics with high fidelity. The AVQDS quantum circuits that prepare the time-evolved state are much shallower than those obtained from first-order Trotterization and contain up to 2 orders of magnitude fewer cnot gate operations. We envision that a wide range of dynamical simulations of quantum many-body systems on near-term quantum-computing devices will be made possible through the AVQDS framework.

The generation of bound electron and hole pairs—excitons—is a key process in photovoltaic technologies, yet it is challenging to follow their initial dynamics. Here, Luoet al. probe the Rydberg eigenstates that characterize the excitonic transport and coherent conversion in a perovskite material.

Ultrafast laser-induced transparency is demonstrated using femtosecond (fs) pump-probe experiments in the organic P3HT:PCBM (donor:acceptor) blend structure. For above band gap pumping, ultrafast transient signals strongly depend on the probe photon energy. Most intriguingly, for below band gap pumping at 0.95 eV, or 1.3 µm at a telecom wavelength, a huge transmission increase up to 30% only during the laser pulse ∼100 fs is observed as a pump-driven, quasi-instantaneous suppression of absorption for the high photon-energy energy probe beam. We attribute the observed laser-driven transparency to dynamic Franz-Keldysh effect, at least one order of magnitude stronger compared to the multiphoton nonlinearities. Our results may be used for development of low-cost, beyond 100 Gbit/s optical switching devices.

Rapid progress in noisy intermediate-scale quantum (NISQ) computing technology has led to the development of novel resource-efficient hybrid quantum-classical algorithms, such as the variational quantum eigensolver (VQE), that can address open challenges in quantum chemistry, physics, and material science. Proof-of-principle quantum chemistry simulations for small molecules have been demonstrated on NISQ devices. While several approaches have been theoretically proposed for correlated materials, NISQ simulations of interacting periodic models on current quantum devices have not yet been demonstrated. Here, we develop a hybrid quantum-classical simulation framework for correlated electron systems based on the Gutzwiller variational embedding approach. We implement this framework on Rigetti quantum processing units (QPUs) and apply it to the periodic Anderson model, which describes a correlated heavy electron band hybridizing with noninteracting conduction electrons. Our simulation results quantitatively reproduce the known ground state quantum phase diagram including metallic, Kondo and Mott insulating phases. This is the first fully self-consistent hybrid quantum-classical simulation of an infinite correlated lattice model executed on QPUs, demonstrating that the Gutzwiller hybrid quantum-classical embedding framework is a powerful approach to simulate correlated materials on NISQ hardware. This benchmark study also puts forth a concrete pathway towards practical quantum advantage on NISQ devices.

Development of resource-friendly quantum algorithms remains highly desirable for noisy intermediate-scale quantum computing. Based on the variational quantum eigensolver (VQE) with unitary coupled-cluster Ansatz, we demonstrate that partitioning of the Hilbert space made possible by the point-group symmetry of the molecular systems greatly reduces the number of variational operators by confining the variational search within a subspace. In addition, we found that instead of including all subterms for each excitation operator, a single-term representation suffices to reach required accuracy for various molecules tested, resulting in an additional shortening of the quantum circuit by a factor of 4–8. With these strategies, VQE calculations on a noise-free quantum simulator achieve energies within a few meVs of those obtained with the full unitary coupled-cluster Ansatz with single and double excitations for the H_{4}-square, H_{4}-chain, and H_{6}-hexagon molecules, while the number of cnot gates, a measure of the quantum-circuit depth, is reduced by a factor of as large as 35. Furthermore, we introduced an efficient “score” parameter to rank the excitation operators, so that the operators causing larger energy reduction can be applied first. Using the H_{4} square and H_{4} chain as examples, We demonstrated on noisy quantum simulators that the first few variational operators can bring the energy within the chemical accuracy, while additional operators do not improve the energy since the accumulative noise outweighs the gain from the expansion of the variational Ansatz.

Fe, Mg, and O are among the most abundant elements in terrestrial planets. While the behavior of the Fe–O, Mg–O, and Fe–Mg binary systems under pressure have been investigated, there are still very few studies of the Fe–Mg–O ternary system at relevant Earth’s core and super-Earth’s mantle pressures. Here, we use the adaptive genetic algorithm (AGA) to study ternary Fe _x Mg _y O _z phases in a wide range of stoichiometries at 200 GPa and 350 GPa. We discovered three dynamically stable phases with stoichiometries FeMg _2 O _4 , Fe _2 MgO _4, and FeMg _3 O _4 with lower enthalpy than any known combination of Fe–Mg–O high-pressure compounds at 350 GPa. With the discovery of these phases, we construct the Fe–Mg–O ternary convex hull. We further clarify the composition- and pressure-dependence of structural motifs with the analysis of the AGA-found stable and metastable structures. Analysis of binary and ternary stable phases suggest that O, Mg, or both could stabilize a BCC iron alloy at inner core pressures.

An allotrope of graphene named T graphene was reported to reveal Dirac-like fermions and high Fermi velocity in its buckled phase similar to graphene. However, these Dirac fermions were questioned to be artificial, caused by band folding under the unstable buckling in T graphene. Here, we report first-principles studies on the structural and electronic properties of T graphene nanotubes which are systems rolled up from the two-dimensional planar sheet of T graphene. The ‘artificial’ Dirac fermions in T graphene are turned into reality in the T graphene nanotubes. Two sets of T graphene nanotubes with different diameters were studied. One set of T graphene nanotubes reveals a semi-metallic property and shows an increasing of the number of Dirac points with the diameters. Another set of T graphene nanotubes reveals a metallic property. Our study indicates that rolling up the allotrope of graphene can provide a new avenue for developing new semimetal materials with fascinating properties.

Graphene, a single atomic layer of graphite, has been a material of recent intensive studies due to its novel electronic and structural properties and its potential applications in the emerging area of carbon-based electronic devices. Metal on graphene growth is one of the current research interests, aiming at improving and manipulating the electronic and magnetic properties of graphene through metal atom adsorption or doping to meet various requirements in device applications. In this paper, we will give an overview of recent experimental and computational investigation of interaction, growth morphology, and thermal stability of various metals on graphene grown on 6H-SiC(0001) substrate.

We report the fabrication of a set of new rare-earth-free magnetic compounds, which form the Fe3Co3Ti2-type hexagonal structure with P-6m2 symmetry. Neutron powder diffraction shows a significant Fe/Co anti-site mixing in the Fe3Co3Ti2 structure, which has a strong effect on the magnetocrystalline anisotropy as revealed by first-principle calculations. Increasing substitution of Fe atoms for Co in the Fe3Co3Ti2 lattice leads to the formation of Fe4Co2Ti2, Fe5CoTi, and Fe6Ti2 with significantly improved permanent-magnet properties. A high magnetic anisotropy (13.0 Mergs/cm3) and saturation magnetic polarization (11.4 kG) are achieved at 10 K by altering the atomic arrangements and decreasing Fe/Co occupancy disorder.

Rev is an essential regulatory protein in the equine infectious anemia virus (EIAV) and other lentiviruses, including HIV-1. It binds incompletely spliced viral mRNAs and shuttles them from the nucleus to the cytoplasm, a critical prerequisite for the production of viral structural proteins and genomic RNA. Despite its important role in production of infectious virus, the development of antiviral therapies directed against Rev has been hampered by the lack of an experimentally-determined structure of the full length protein. We have used a combined computational and biochemical approach to generate and evaluate a structural model of the Rev protein. The modeled EIAV Rev (ERev) structure includes a total of 6 helices, four of which form an anti-parallel four-helix bundle. The first helix contains the leucine-rich nuclear export signal (NES). An arginine-rich RNA binding motif, RRDRW, is located in a solvent-exposed loop region. An ERLE motif required for Rev activity is predicted to be buried in the core of modeled structure where it plays an essential role in stabilization of the Rev fold. This structural model is supported by existing genetic and functional data as well as by targeted mutagenesis of residues predicted to be essential for overall structural integrity. Our predicted structure should increase understanding of structure-function relationships in Rev and may provide a basis for the design of new therapies for lentiviral diseases.

We develop a new implementation of the Gutzwiller approximation in combination with the local density approximation, which enables us to study complex 4f and 5f systems beyond the reach of previous approaches. We calculate from first principles the zero-temperature phase diagram and electronic structure of Pr and Pu, finding good agreement with the experiments. Our study of Pr indicates that its pressure-induced volume-collapse transition would not occur without change of lattice structure—contrarily to Ce. Our study of Pu shows that the most important effect originating the differentiation between the equilibrium densities of its allotropes is the competition between the Peierls effect and the Madelung interaction and not the dependence of the electron correlations on the lattice structure.

Ni is the second most abundant element in the Earth's core. Yet, its effects on the inner core's structure and formation process are usually disregarded because of its electronic and size similarity with Fe. Using ab initio molecular dynamics simulations, we find that the bcc phase can spontaneously crystallize in liquid Ni at temperatures above Fe's melting point at inner core pressures. The melting temperature of Ni is shown to be 700 to 800 K higher than that of Fe at 323 to 360 GPa. hcp, bcc, and liquid phase relations differ for Fe and Ni. Ni can be a bcc stabilizer for Fe at high temperatures and inner core pressures. A small amount of Ni can accelerate Fe's crystallization at core pressures. These results suggest that Ni may substantially impact the structure and formation process of the solid inner core. [ABSTRACT FROM AUTHOR]