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The discovery of the 1144-phase, e.g. CaKFe$_4$As$_4$, creates opportunities to build novel intermetallics with alternative stacking of two parent compounds. Here we formalize the idea by defining a class of bulk crystalline solids with $A$-$B$ stacking (including 1144-phases and beyond), which is a generalization of hetero-structures from few-layer or thin-film semi-conductors to bulk intermetallics. Theoretically, four families of phosphides \textit{AB}(TM)$_4$P$_4$ (TM=Fe, Ru, Co, Ni) are investigated by first-principles calculations, wherein configurational, vibrational and electronic degrees of freedom are considered. It predicts a variety of stable 1144-phases (especially Ru- and Fe-phosphides). Stability rules are found and structural/electronic properties are discussed. Experimentally, we synthesize high-purity CaKRu$_4$P$_4$ as a proof of principle example. The synthetic method is simple and easily applied. Moreover, it alludes to a strategy to explore complex multi-component compounds, facilitated by a phase diagram coordinated by collective descriptors., Comment: 15 pages, 9 figures

Molecular dynamics simulations using an interatomic potential developed by artificial neural network deep machine learning are performed to study the local structural order in Al90Tb10 metallic glass. We show that more than 80% of the Tb-centered clusters in Al90Tb10 glass have short-range order (SRO) with their 17 first coordination shell atoms stacked in a '3661' or '15551' sequence. Medium-range order (MRO) in Bergman-type packing extended out to the second and third coordination shells is also clearly observed. Analysis of the network formed by the '3661' and '15551' clusters show that ~82% of such SRO units share their faces or vertexes, while only ~6% of neighboring SRO pairs are interpenetrating. Such a network topology is consistent with the Bergman-type MRO around the Tb-centers. Moreover, crystal structure searches using genetic algorithm and the neural network interatomic potential reveal several low-energy metastable crystalline structures in the composition range close to Al90Tb10. Some of these crystalline structures have the '3661' SRO while others have the '15551' SRO. While the crystalline structures with the '3661' SRO also exhibit the MRO very similar to that observed in the glass, the ones with the '15551' SRO have very different atomic packing in the second and third shells around the Tb centers from that of the Bergman-type MRO observed in the glassy phase.

An interatomic potential for Al-Tb alloy around the composition of Al90Tb10 was developed using the deep neural network (DNN) learning method. The atomic configurations and the corresponding total potential energies and forces on each atom obtained from ab initio molecular dynamics (AIMD) simulations are collected to train a DNN model to construct the interatomic potential for Al-Tb alloy. We show the obtained DNN model can well reproduce the energies and forces calculated by AIMD. Molecular dynamics (MD) simulations using the DNN interatomic potential also accurately describe the structural properties of Al90Tb10 liquid, such as the partial pair correlation functions (PPCFs) and the bond angle distributions, in comparison with the results from AIMD. Furthermore, the developed DNN interatomic potential predicts the formation energies of crystalline phases of Al-Tb system with the accuracy comparable to ab initio calculations. The structure factor of Al90Tb10 metallic glass obtained by MD simulation using the developed DNN interatomic potential is also in good agreement with the experimental X-ray diffraction data.

The development of long-range ferromagnetic (FM) order in dilute magnetic topological insulators can induce dissipationless electronic surface transport via the quantum anomalous Hall effect. We measure the magnetic excitations in a prototypical magnetic topological crystalline insulator, Sn$_{0.95}$Mn$_{0.05}$Te, using inelastic neutron scattering. Neutron diffraction and magnetization data indicate that our Sn$_{0.95}$Mn$_{0.05}$Te sample has no FM long-range order above a temperature of 2 K. However, we observe slow, collective FM fluctuations ($<$~70 $\mu$eV), indicating proximity to FM order. We also find a series of sharp peaks originating from local excitations of antiferromagnetically (AF) coupled and isolated Mn-Mn dimers with $J_{\rm AF}=460$~$\mu$eV\@. The simultaneous presence of collective and localized components in the magnetic spectra highlight different roles for substituted Mn ions, with competition between FM order and the formation of AF-coupled Mn-Mn dimers.

Molecular dynamics simulations were performed to study the effects of Si solute on the glass formation and crystallization of Pd liquid. Pure Pd sample prepared by quenching process with cooling rate of $10^{13}$ K/s can be in an amorphous state but the structural analysis indicates there is nearly no glass-forming motif in the sample. However, doping a small amount Si (Si concentration ~ 4%) the sample can be vitrified at a cooling rate of $10^{12}$ K/s. The glass-forming motifs such as Pd-centered Z13, Si-centered Z9-like and Mixed-ICO-Cube clusters with 5-fold local symmetry are found to be the dominant short-range orders in the glassy samples. With the increasing of the Si-doping concentration, these glass-forming motifs tend to aggregate and connect with each other forming a network structure. Our calculated results revealed that Si solutes in liquid Pd can significantly enhance the glass-forming ability.

We report the low-energy electrodynamics of a moderately clean A15 superconductor (SC) following ultrafast excitation to understand and manipulate terahertz (THz) quasi--particle (QP) transport by tuning pump photoexcitation of from competing orders. Using 35-fs optical pulses, we observe a non-thermal enhancement in the low frequency conductivity, opposite to that observed for THz pump, which persists up to an additional critical temperature, above the SC one, from an electronic order in the Martensitic normal state. In the SC state, the fluence dependence of pair breaking kinetics together with an analytic model provides evidence for a `one photon-to-one pair' non-resonant energy transfer during the laser pulse. Such initial transfer of photon energy $\hbar\omega$ to QPs at the {\em quantum} limit, set by $2\Delta_{SC}/\hbar\omega$=0.33$\%$, is more than one order of magnitude smaller than in previously studied BCS SCs, which we attribute to strong electron--phonon coupling and possible influence of phonon condensation in A15 SCs., Comment: 5 pages 4 figures

Using an effective genetic algorithm, we uncover the structure of a metastable Al41Sm5 phase that supplements its family sharing similar short-range orders. The phase evolves upon heating an amorphous Al-9.7at.%Sm ribbon, produced by melt-spinning. The dynamical phase selection is discussed with respect to the structural connections between the short-range packing motifs in the amorphous precursor and those observed in the selected phases. The phase elucidated here is one of several newly discovered large-unit-cell phases found to form during devitrification from the glass in this binary system, further illustrating the power and efficiency of our approach, the important role of structural hierarchy in phase selection, and the richness of the metastable phase landscape accessible from the glassy structure.

While the role of the free energy barrier during nucleation is a text-book subject the importance of the kinetic factor is frequently underestimated. We obtained both quantities from molecular dynamics (MD) simulations for the pure Ni and B2 phases in the Ni50Al50 and Cu50Zr50 alloys. The free-energy barrier was found to be higher in Ni but the nucleation rate is much lower in the Ni50Al50 alloy which was attributed to the ordered nature of the B2 phase. Since the Cu50Zr50 B2 phase can has even smaller fraction of the anti-site defects its nucleation is never observed in the MD simulation.

The 1144 iron arsenide (e.g. CaKFe4As4) has recently been discovered and inspired a tide of search for superconductors. Such far, the discovered compounds are confined to iron arsenides (ABFe4As4), where A and B are either alkali metals or alkaline earth elements. In this work, we propose two directions in searching 1144 structures: (i) using tri-valence cations for A; (ii) substituting the transition metal, e.g. replacing Fe by Co. Following the two directions, we employ density functional theory to study stability and electronic structures of 1144 pnictides of various tri-valence cations (La, Y, In, Tl, Sm and Gd), as well as cobalt arsenides. For LaAFe4As4, the 1144 phase can be stabilized in three systems: LaKFe4As4, LaRbFe4As4 and LaCsFe4As4, which show quasi-two-dimensional semi-metal features similar to the iron pnictide superconductors: hole-type Fermi surface at Gama point and electron-type Fermi surface at M point in B.Z. In addition, LaKFe4As4 feature an extra bubble shaped Fermi surface sheets, distinct from the other two peers. Y does not support any 1144 phase within our search. For In and Tl, substitute Fe by Co and two unknown compounds of the 122 phase are stabilized: InCo2As2 and TlCo2As2. The two cobalt arsenides have Fermi surfaces of similar topology as iron arsenides, but the Fermi surfaces are all electron-type, showing potentials to be undiscovered superconductors. Stable 1144 phases are also found in InKCo4As4 and InRbCo4As4. For Sm and Gd, most 1144 and 122 iron arsenides are found unstable., Comment: 11 pages, 8 figures

Micromagnetic simulations of alnico show substantial deviations from Stoner-Wohlfarth behavior due to the unique size and spatial distribution of the rod-like Fe-Co phase formed during spinodal decomposition in an external magnetic field. The maximum coercivity is limited by single-rod effects, especially deviations from ellipsoidal shape, and by interactions between the rods. Both the exchange interaction between connected rods and magnetostatic interaction between rods are considered, and the results of our calculations show good agreement with recent experiments. Unlike systems dominated by magnetocrystalline anisotropy, coercivity in alnico is highly dependent on size, shape, and geometric distribution of the Fe-Co phase, all factors that can be tuned with appropriate chemistry and thermal-magnetic annealing.

Sodium orthosilicates Na2MSiO4 (M denotes transition metals) have attracted much attention due to the possibility of exchanging two electrons per formula unit. In this work, we report a group of sodium iron orthosilicates Na2FeSiO4, the crystal structures of which are characterized by a diamond-like Fe-Si network. The Fe-Si network is quite robust against the charge/discharge process, which explains the high structural stability observed in experiment. Using the density functional theory within the GGA+U framework and X-ray diffraction studies, the crystal structures and structural stabilities during the sodium insertion/deinsertion process are systematically investigated. The calculated average deintercalation voltages are in good agreement with the experimental result., Comment: 14 pages, 8 figures

The phonon properties, electronic structures and optical properties of novel carbon allotropes, such as monolayer penta-graphene (PG), double-layer PG and T12-carbon, were explored by means of first-principles calculations. Results of phonon calculations demonstrate that these exotic carbon allotropes are dynamically stable. In addition, the bulk T12 phase is an indirect-gap semiconductor having a bandgap of ~4.89 eV. Whereas the bulk material transforms to a 2D phase, the monolayer and double-layer PG become quasi-direct gap semiconductors with smaller band gaps of ~2.64 eV and ~3.27eV, respectively. Furthermore, the partial charge density analysis indicates that the 2D phases retain part of the electronic characteristics of the T12 phase. The linear photon energy-dependent dielectric functions and related optical properties including refractive index, extinction coefficient, absorption spectrum, reflectivity, and energy loss spectrum were also computed and discussed. The structural estimation obtained as well as other findings are in agreement with existing theoretical data. The calculated results are beneficial to the practical applications of these exotic carbon allotropes in optoelectronics and electronics.

We present an efficient \textit{ab initio} method for calculating the electronic structure and total energy of strongly correlated electron systems. The method extends the traditional Gutzwiller approximation for one-particle operators to the evaluation of the expectation values of two particle operators in a full many-electron Hamiltonian. The method is free of adjustable Coulomb parameters, and has no double counting issues in the calculation of total energy, and has the correct atomic limit. We demonstrate that the method describes well the bonding and dissociation behaviors of the hydrogen and nitrogen clusters. We also show that the method can satisfactorily tackle great challenging problems faced by the density functional theory recently discussed in the literature. The computational workload of our method is similar to the Hartree-Fock approach while the results are comparable to high-level quantum chemistry calculations., Comment: 5 pages, 5 figures

We present a genetic algorithm (GA) for structural search that combines the speed of structure exploration by classical potentials with the accuracy of density functional theory (DFT) calculations in an adaptive and iterative way. This strategy increases the efficiency of the DFT-based GA by several orders of magnitude. This gain allows considerable increase in size and complexity of systems that can be studied by first principles. The method's performance is illustrated by successful structure identifications of complex binary and ternary inter-metallic compounds with 36 and 54 atoms per cell, respectively. The discovery of a multi-TPa Mg-silicate phase with unit cell containing up to 56 atoms is also reported. Such phase is likely to be an essential component of terrestrial exoplanetary mantles., Comment: 14 pages, 4 figures

Structural and electronic properties, including deformation, magnetic moment, Mulliken population, bond order as well as electronic transport properties, of zigzag graphene nanoribbon (ZGNR) with Co adatom on hollow site are investigated by quasi-atomic minimal basis orbits (QUAMBOs), a first-principles tight binding (TB) scheme based on density functional theory (DFT), combined with non-equilibrium Green's function. As for electronic transport, below Fermi level the transmission is strongly suppressed and spin-dependent as a result of magnetism by Co adatom adsorption, while above Fermi level the transmission is slightly distorted and spin-independent. Due to local environment dependence of QUAMBOs-TB parameters, we construct QUAMBOs-TB parameters of ZGNR lead and ZGNR with Co adatom on the hollow center site by divide-and-conquer approach, and well reproduce the electronic transmission behavior. Our QUAMBO-NEGF method is a new and promising way for electronic transport in large-scale system., Comment: 13 pages, 5 figures

We introduce a scheme to include many-body screening processes explicitly into a set of self-consistent equations for electronic structure calculations using the Gutzwiller approximation. The method is illustrated by the application to a tight-binding model describing the strongly correlated {\gamma}-Ce system. With the inclusion of the 5d-electrons into the local Gutzwiller projection subspace, the correct input Coulomb repulsion U_{ff} between the 4f-electrons for {\gamma}-Ce in the calculations can be pushed far beyond the usual screened value U_{ff}^{scr} and close to the bare atomic value U_{ff}^{bare}. This indicates that the d-f many-body screening is the dominant contribution to the screening of U_{ff} in this system. The method provides a promising way towards the ab initio Gutzwiller density functional theory.

To elucidate the role played by the transition metal ion in the pnictide materials, we compare the electronic and magnetic properties of BaFe_{2}As_{2} with BaMn_{2}As_{2}. To this end we employ the LDA+Gutzwiller method to analyze the mass renormalizations and the size of the ordered magnetic moment of the two systems. We study a model that contains all five transition metal 3d orbitals together with the Ba-5d and As-4p states (ddp-model) and compare these results with a downfolded model that consists of Fe/Mn d-states only (d-model). Electronic correlations are treated using the multiband Gutzwiller approximation. The paramagnetic phase has also been investigated using LDA+Gutzwiller method with electron density self-consistency. The renormalization factors for the correlated Mn 3d orbitals in the paramagnetic phase of BaMn_{2}As_{2} are shown to be generally smaller than those of BaFe_{2}As_{2}, which indicates that BaMn_{2}As_{2} has stronger electron correlation effect than BaFe_{2}As_{2}. The screening effect of the main As 4p electrons to the correlated Fe/Mn 3d electrons is evident by the systematic shift of the results to larger Hund's rule coupling J side from the ddp-model compared with those from the d-model. A gradual transition from paramagnetic state to the antiferromagnetic ground state with increasing J is obtained for the models of BaFe_{2}As_{2} which has a small experimental magnetic moment; while a rather sharp jump occurs for the models of BaMn_{2}As_{2}, which has a large experimental magnetic moment. The key difference between the two systems is shown to be the d-level occupation. BaMn_{2}As_{2}, with approximately five d-electrons per Mn atom, is for same values of the electron correlations closer to the transition to a Mott insulating state than BaFe_{2}As_{2}. Here an orbitally selective transition, required for a system with close to six electrons only occurs at significantly larger values for the Coulomb interactions.

We report a collection of lowest-energy structures of hydrocarbon molecules C_{m}H_{n} (m=1-18; n=0-2m+2). The structures are examined within a wide hydrogen chemical potential range. The genetic algorithm combined with Brenner's empirical potential is applied for the search. The resultant low-energy structures are further studied by ab initio quantum chemical calculations. The lowest-energy structures are presented with several additional low-energy structures for comparison. The results are expected to provide useful information for some unresolved astronomical spectra and the nucleation of growth of nano-diamond film.

This paper has been withdrawn by the author due to the error in figure 2, we did not optimized c-value of the supercell, so the results can not give the true physics of this material., Comment: This paper has been withdrawn

We develop a new density functional theory (DFT) and formalism for correlated electron systems by taking as reference an interacting electron system that has a ground state wavefunction which obeys exactly the Gutzwiller approximation for all one particle operators. The solution of the many electron problem is mapped onto the self-consistent solution of a set of single particle Schroedinger equations analogous to standard DFT-LDA calculations., Comment: 4 pages

Although unstable, the Si(337) orientation has been known to appear in diverse experimental situations such as the nanoscale faceting of Si(112), or in the case of miscutting a Si(113) surface. Various models for Si(337) have been proposed over time, which motivates a comprehensive study of the structure of this orientation. Such a study is undertaken in this article, where we report the results of a genetic algorithm optimization of the Si(337)-$(2\times 1)$ surface. The algorithm is coupled with a highly optimized empirical potential for silicon, which is used as an efficient way to build a set of possible Si(337) models; these structures are subsequently relaxed at the level of ab initio density functional methods. Using this procedure, we retrieve most of the (337) reconstructions proposed in previous works, as well as a number of novel ones., Comment: 5 figures (low res.); to appear in J. Appl. Phys

In this article we report the results of global structural optimization of the Si(114) surface, which is a stable high-index orientation of silicon. We use two independent procedures recently developed for the determination of surface reconstructions, the parallel-tempering Monte Carlo method and the genetic algorithm. These procedures, coupled with the use of a highly-optimized interatomic potential for silicon, lead to finding a set of possible models for Si(114), whose energies are recalculated with ab-initio density functional methods. The most stable structure obtained here without experimental input coincides with the structure determined from scanning tunneling microscopy experiments and density functional calculations by Erwin, Baski and Whitman [Phys. Rev. Lett. 77, 687 (1996)]., Comment: 19 pages, 5 figures

In this article we show that the reconstructions of semiconductor surfaces can be determined using a genetic procedure. Coupled with highly optimized interatomic potentials, the present approach represents an efficient tool for finding and sorting good structural candidates for further electronic structure calculations and comparison with scanning tunnelling microscope (STM) images. We illustrate the method for the case of Si(105), and build a database of structures that includes the previously found low-energy models, as well as a number of novel configurations., Comment: 4 figures, 1 table

Recent experimental studies have shown that well-annealed, unstrained Si(105) surfaces appear disordered and atomically rough when imaged using scanning tunnelling microscopy (STM). We construct new models for the Si(105) surface that are based on single- and double-height steps separated by Si(001) terraces, and propose that the observed surface disorder of Si(105) originates from the presence of several structural models with different atomic-scale features but similar energies. This degeneracy can be removed by applying compressive strains, a result that is consistent with recent observations of the structure of the Ge/Si(105) surface., Comment: 4 figures, 1 table

Recent experiments have shown that steps on Si(113) surfaces self-organize into bunches due to a competition between long-range repulsive and short-range attractive interactions. Using empirical and tight-binding interatomic potentials, we investigate the physical origin of the short-range attraction, and report the formation and interaction energies of steps. We find that the short-range attraction between steps is due to the annihilation of force monopoles at their edges as they combine to form bunches. Our results for the strengths of the attractive interactions are consistent with the values determined from experimental studies on kinetics of faceting., Comment: 4 pages, 3 figures, to appear in Phys. Rev B, Rapid Communications

Molecular-dynamics simulations of KNbO$_3$ reveal preformed dynamic chain-like structures, present even in the paraelectric phase, that are related to the softening of phonon branches over large regions of the Brillouin zone. The phase sequence of ferroelectric transitions is correctly reproduced, showing that the first-principles effective Hamiltonian used in the simulations captures the essential behavior of the microscopic fluctuations driving the transitions. Real space chains provide a framework for understanding both the displacive and order-disorder characteristics of these phase transitions., Comment: 4 pages, REVTeX, three eps figures

We present molecular-dynamics simulations of the Si(100) surface in the temperature range 1100-1750K. To describe the total energy and forces we use the Effective-Medium Tight-Binding model. The defect-free surface is found to melt at the bulk melting point, which we determine to be 1650 K, but for a surface with dimer vacancies we find a pre-melting of the first two layers 100 K below the melting point. We show that these findings can rationalize recent experimental studies of the high temperature Si(100) surface., Comment: 13 pages, 7 figures; To appear in Surface Science