Vibrational modes and lattice distortion of a nitrogen-vacancy center in diamond from first-principles calculations

We investigate vibrational properties and lattice distortion of negatively charged nitrogen-vacancy (NV) center in diamond. Using the first-principles electronic structure calculations, we show that the presence of NV center leads to appearance of a large number of quasilocalized vibrational modes (qLVMs) with different degree of localization. The vibration patterns and the symmetries of the qLVMs are presented and analyzed in detail for both ground and excited orbital states of the NV center. We find that in the high-symmetry ($C_{3v}$) excited orbital state a pair of degenerate qLVMs becomes unstable, and the stable excited state has lower ($C_{1h}$) symmetry. This is a direct indication of the Jahn-Teller effect, and our studies suggest that dynamical Jahn-Teller effect in the weak coupling regime takes place. We have also performed a detailed comparison of our results with the available experimental data on the vibrations involved in optical emission/absorption of the NV centers. We have directly demonstrated that, among other modes, the qLVMs crucially impact the optical properties of the NV centers in diamond, and identified the most important groups of qLVMs. Our results are important for deeper understanding of the optical properties and the orbital relaxation associated with lattice vibrations of the NV centers.Comment: 10 RevTeX pages, 10 EPS figure

First-principles study, fabrication and characterization of (Zr0.25Nb0.25Ti0.25V0.25)C high-entropy ceramic

The formation possibility of a new (Zr0.25Nb0.25Ti0.25V0.25)C high-entropy ceramic (ZHC-1) was first analyzed by the first-principles calculations and thermodynamical analysis and then it was successfully fabricated by hot pressing sintering technique. The first-principles calculation results showed that the mixing enthalpy of ZHC-1 was 5.526 kJ/mol and the mixing entropy of ZHC-1 was in the range of 0.693R-1.040R. The thermodynamical analysis results showed that ZHC-1 was thermodynamically stable above 959 K owing to its negative mixing Gibbs free energy. The experimental results showed that the as-prepared ZHC-1 (95.1% relative density) possessed a single rock-salt crystal structure, some interesting nanoplate-like structures and high compositional uniformity from nanoscale to microscale. By taking advantage of these unique features, compared with the initial metal carbides (ZrC, NbC, TiC and VC), it showed a relatively low thermal conductivity of 15.3 + - 0.3 W/(m.K) at room temperature, which was due to the presence of solid solution effects, nanoplates and porosity. Meanwhile, it exhibited the relatively high nanohardness of 30.3 + - 0.7 GPa and elastic modulus of 460.4 + - 19.2 GPa and the higher fracture toughness of 4.7 + - 0.5 MPa.m1/2, which were attributed to the solid solution strengthening mechanism and nanoplate pullout and microcrack deflection toughening mechanism.Comment: 49 pages,6 figures, 4 table

Calculation of Critical Nucleation Rates by the Persistent Embryo Method: Application to Quasi Hard Sphere Models

We study crystal nucleation of the Weeks-Chandler-Andersen (WCA) model, using the recently introduced Persistent Embryo Method (PEM). The method provides detailed characterization of pre-critical, critical and post-critical nuclei, as well as nucleation rates that compare favorably with those obtained using other methods (umbrella sampling, forward flux sampling or seeding). We further map our results to a hard sphere model allowing to compare with other existing predictions. Implications for experiments are also discussed.Comment: 27 pages, 11 figure

Structural and Chemical Orders in Ni64.5Zr35.5 Metallic Glass by Molecular Dynamics Simulation

The atomic structure of Ni64.5Zr35.5 metallic glass has been investigated by molecular dynamics (MD) simulations. The calculated structure factors from the MD glassy sample at room temperature agree well with the X-ray diffraction (XRD) and neutron diffraction (ND) experimental data. Using the pairwise cluster alignment and clique analysis methods, we show that there are three types dominant short-range order (SRO) motifs around Ni atoms in the glass sample of Ni64.5Zr35.5, i.e., Mixed-Icosahedron(ICO)-Cube, Twined-Cube and icosahedron-like clusters. Furthermore, chemical order and medium-range order (MRO) analysis show that the Mixed-ICO-Cube and Twined-Cube clusters exhibit the characteristics of the crystalline B2 phase. Our simulation results suggest that the weak glass-forming ability (GFA) of Ni64.5Zr35.5 can be attributed to the competition between the glass forming ICO SRO and the crystalline Mixed-ICO-Cube and Twined-Cube motifs

Coexistence of type-II Dirac point and weak topological phase in Pt 3 Sn

Intriguing topological phases may appear in both insulating and semimetallic states. Topological insulators exhibit topologically nontrivial band inversion, while topological Dirac/Weyl semimetals show “relativistic” linear band crossings. Here, we report an unusual topological state of Pt3Sn, where the two topological features appear simultaneously. Based on first-principles calculations, we show that Pt3Sn is a three-dimensional weak topological semimetal with topologically nontrivial band inversion between the valence and conduction bands, where the band structure also possesses type-II Dirac points at the boundary of two electron pockets. The formation of the Dirac points can be understood in terms of the representations of relevant symmetry groups and the compatibility relations. The topological surface states appear in accordance with the nontrivial bulk band topology. The unique coexistence of the two distinct topological features in Pt3Sn enlarges the material scope in topological physics, and is potentially useful for spintronics

Ternary Bismuthide SrPtBi2: Computation and Experiment in Synergism to Explore Solid-State Materials

A combination of theoretical calculation and the experimental synthesis to explore the new ternary compound is demonstrated in the Sr-Pt-Bi system. Since Pt-Bi is considered as a new critical charge-transfer pair for superconductivity, it inspired us to investigate the Sr-Pt-Bi system. With a thorough calculation of all the known stable/metastable compounds in the Sr-Pt-Bi system and crystal structure predictions, the thermodynamic stability of hypothetical stoichiometry, SrPtBi2, is determined. Followed by the high-temperature synthesis and crystallographic analysis, the first ternary bismuthide in Sr-Pt-Bi, SrPtBi2 was prepared and the stoichiometry was confirmed experimentally. SrPtBi2 crystallizes in the space group Pnma (S.G. 62, Pearson Symbol oP48), which matches well with theoretical prediction using an adaptive genetic algorithm (AGA). Using first-principles calculations, we demonstrate that the orthorhombic structure has lower formation energies than other 112 structure types, such as tetragonal BaMnBi2 (CuSmP2) and LaAuBi2 (CuHfSi2) structure types. The bonding analysis indicates the Pt-Bi interactions play a critical role in structural stability. The physical properties measurements show the metallic properties with low electron-phonon interactions at the low temperature, which agrees with the electronic structure assessment.Comment: 12 pages, 7 figure