The structural and energetic properties of layered materials present a challenge to density functional theory with common semilocal approximations to the exchange-correlation energy. By combining the most widely used semilocal generalized gradient approximation (GGA), the Perdew-Burke-Ernzerhof (PBE) one, with the revised Vydrov–van Voorhis nonlocal correlation functional (rVV10), both excellent structural and energetic properties of 28 layered materials have been recovered with a judicious parameter selection. We term the resulting functional PBE+rVV10L, with the “L” indicating that it is for layered materials. Such a combination is not new, and only involves refitting a single global parameter. However, the resulting excellent accuracy suggests such a dispersion-corrected PBE for many aspects of theoretical studies on layered materials. For comparison, we also present the results for PBE+rVV10 where the parameter is determined by 22 interaction energies between molecules.

Ellipse and hyperbola are two well-known curves in mathematics with numerous applications in various fields, but their properties and inherent differences in spin optics are less understood. Here, we investigate the peculiar optical spin properties of the two curves and establish a connection between their foci and the spin states of incident light by introducing a geometric-phase distribution along the conic curve. We show that the optical spin Hall effect is the intrinsic optical spin property of ellipse, where photons with different spin states can be exactly separated to each of its two foci, while a hyperbola exhibits optical spin-selective effect, where only photons with one particular spin state can be accumulated at its foci. These properties are then experimentally demonstrated in near field by arranging nanoslits in conic shapes. Based on the spin properties of the curves, we design spin-based plasmonic devices with various functionalities. Our results reveal the intrinsic optical spin properties behind conic curves and provide a route for designing spin-based plasmonic devices.

${\mathrm{BaSn}}_2$ has been shown to form as layers of buckled stanene intercalated by barium ions. However, despite an apparently straightforward synthesis and significant interest in stanene as a topological material, ${\mathrm{BaSn}}_2$ has been left largely unexplored, and has only recently been recognized as a potential topological insulator. Belonging to neither the lead nor bismuth chalcogenide families, it would represent a unique manifestation of the topological insulating phase. Here we present a detailed investigation of ${\mathrm{BaSn}}_2$, using both ab initio and experimental methods. First-principles calculations demonstrate that this overlooked material is indeed a strong, wide-gap topological insulator with a bulk band gap of 200 meV. We characterize the surface state dependence on termination chemistry, providing guidance for experimental efforts to measure and manipulate its topological properties. Additionally, through ab initio modeling and synthesis experiments, we explore the stability and accessibility of this phase, revealing a complicated phase diagram that indicates a challenging path to obtaining single crystals.

We present an experimental study describing the effects of surface termination on the electronic structure of the natural topological superlattice phase ${\mathrm{Sb}}_2\mathrm{Te}$. Using scanning angle-resolved photoemission microscopy, we consistently find various nonequivalent regions on the same surface after cleaving various ${\mathrm{Sb}}_2\mathrm{Te}$ single crystals. We were able to identify three distinct terminations characterized by different Sb/Te surface stoichiometric ratios and with clear differences in their band structure. For the dominating Te-rich termination, we also provide a direct observation of the excited electronic states and of their relaxation dynamics by means of time-resolved angle-resolved photoemission spectroscopy. Our results clearly indicate that the surface electronic structure is strongly affected by the bulk properties of the superlattice.

We suggest a hybrid plasmonic device made of a bimodal metallic nanoantenna coupled to an incoherently pumped quantum emitter. This device emits light into the two modes entangled in the number of photons. The process is a prime example of losses changing from being a nuisance into something beneficial, since, although it is counterintuitive, the entanglement is enabled by strong incoherent processes, i.e., the dominant scattering and absorption rates of the nanoantenna. This renders the nanoantenna an active source of nonclassicality. Both the high emission rate and the degree of entanglement of the emitted light are insensitive with respect to imperfections in the nanoantenna length, rendering the scheme feasible for an implementation.

We propose an alternative structure of ${\mathrm{TiO}}_2$ anatase that has a higher energy oxygen $p$-like valence band maximum than pristine ${\mathrm{TiO}}_2$ anatase and thus has a much better alignment with the water splitting levels. This alternative structure is unique when considering a large subspace of possible structural distortions of ${\mathrm{TiO}}_2$ anatase. We propose two routes towards this state and argue that one of them might have been realized in the recently discovered so-called black ${\mathrm{TiO}}_2$.

Descriptors for the bulk modulus of amorphous carbon are investigated through the implementation of data mining where data sets are prepared using first-principles calculations. Data mining reveals that the number of bonds in each C atom and the density of amorphous carbon are found to be descriptors representing the bulk modulus. Support vector regression (SVR) within machine learning is implemented and descriptors are trained where trained SVR is able to predict the bulk modulus of amorphous carbon. An inverse problem, starting from the bulk modulus towards structural information of amorphous carbon, is performed and structural information of amorphous carbon is successfully predicted from the desired bulk modulus. Thus, treating several physics factors in multidimensional space allows for the prediction of physical phenomena. In addition, the reported approach proposes that “big data” can be generated from a small data set using machine learning if descriptors are well defined. This would greatly change how amorphous carbon would be treated and help accelerate further development of amorphous carbon materials.

We report an alternative mechanism for the physical origin of the temperature-dependent ferromagnetic relaxation observed in bare permalloy (NiFe) thin films. Through spin-pumping experiments, we demonstrate that the peak in the temperature dependence of NiFe damping can be understood in terms of enhanced absorption of spin angular momentum at the magnetic phase transition in native antiferromagnetic surface-oxidized layers. These results suggest some avenues for the investigation of an incompletely understood phenomenon in physics.

We calculate superconducting gaps and quasiparticle density of states of ${\mathrm{YNi}}_2{\mathrm{B}}_2\mathrm{C}$ in the framework of the density functional theory for superconductors to investigate the origin of highly anisotropic superconducting gaps in this material. Calculated phonon frequencies, the quasiparticle density of states, and the transition temperature show good agreement with experimental results. From our calculation of superconducting gaps and orbital character analysis, we establish that the orbital character variation of the Fermi surface is the key factor of the anisotropic gap. Since the electronic states that consist of mainly Ni $3d$ orbitals couple weakly with phonons, the superconducting gap function is suppressed for the corresponding states, which results in the anisotropy observed in the experiments. These results are hints to increase the transition temperature of materials in the borocarbide family.

The change of the lattice dynamics upon the charge disproportionation (CD) transition has been investigated for the ${\mathrm{CaFeO}}_3$ crystal by measuring its infrared optical spectra. Across the CD transition, ${\mathrm{CaFeO}}_3$ undergoes a metal-insulator transition, and it is found that below $T_{CD}\approx 290$ K the low-frequency optical conductivity gradually decreases to a rather low value and is dominated by a series of infrared-active phonons. Intriguingly, accompanied by the CD transition, two prominent phonon modes at $\sim 243$ and $\sim 559$ ${\mathrm{cm}}^{-1}\text{associated}$ with the vibrations of Fe-O bonds show obvious redshift and asymmetric line shapes characterized by a Fano profile, suggesting a strong electron-phonon coupling. This coupling behavior reveals an intimate relationship between charge and lattice in the CD transition of ${\mathrm{CaFeO}}_3$.

We report hyperpolarization of the electronic spins associated with substitutional nitrogen defects in bulk diamond crystals. Hyperpolarization is achieved by optical pumping of nitrogen vacancy centers followed by rapid cross relaxation at the energy level matching condition in a 51 mT bias field. The maximum observed donor spin polarization is $0.9\%$, corresponding to an enhancement of 25 compared to the thermal Boltzmann polarization. A further accumulation of polarization is impeded by an anomalous optical saturation effect that we attribute to charge state conversion processes. Hyperpolarized nitrogen donors may form a useful resource for increasing the efficiency of diamond-based dynamic nuclear polarization devices.

Surface x-ray diffraction has been used to determine the quantitative structure of the (101) termination of anatase $\mathrm{Ti}{\mathrm{O}}_2$. The atomic displacements from the bulk-terminated structure are significantly different from those previously calculated with density functional theory (DFT) methods with discrepancies for the Ti displacements in the $\left[10\overline{1}\right]$ direction of up to $0.3\AA$. DFT calculations carried out as part of the current paper provide a much better agreement through improved accuracy and thicker slab models.

We propose an analytical model describing Fermi arc surface states observed in the recent investigations of Weyl semimetals. The effective two-valley Hamiltonian is supplemented by the boundary conditions taking into account both the intravalley and intervalley interfacial interactions. We demonstrate that the latter is crucial for the formation of the surface states having the form consistent with the experimental data. Depending on the magnitude and interplay between the intravalley and intervalley interactions, the Fermi arc connects two nearby or distant valleys. Moreover, the emergence of additional Fermi contours (closed curves not intersecting the Weyl points) can be understood in the simplest four-valley approximation. These results open up opportunities for searching new effects in Weyl semimetals under an external field.

We prepared nonlocal spin valves based on single crystals of an organic multilayered zero-gap conductor $\alpha \text{−}{\left(\mathrm{BEDT}\text{−}\mathrm{TTF}\right)}_2{\mathrm{I}}_3$ and succeeded in evaluating the spin-diffusion length (1.1 μm) and relaxation time (3 ns) at 2.5 K under a static pressure of 1.6 GPa using a polyethylene naphthalate as a substrate. Although $\alpha \text{−}{\left(\mathrm{BEDT}\text{−}\mathrm{TTF}\right)}_2{\mathrm{I}}_3$ includes heavy atoms, such as iodine, it exhibited a rather long spin-relaxation time comparable to that of graphene. The spin-orbit interaction (SOI) estimated on the basis of the experimental values of the spin-relaxation time and carrier lifetime (1.2 ps) was 90 mK. The long spin-relaxation time and small SOI evaluated for $\alpha \text{−}{\left(\mathrm{BEDT}\text{−}\mathrm{TTF}\right)}_2{\mathrm{I}}_3$ are considered to originate from its layered structure in which spin scattering induced by surface defects is suppressed. In addition, the inversion asymmetry, which generates an extra term in the equation for the SOI, might be reduced in layered structures. These findings provide guiding principles for materials design in organic spintronics.

We report on the energy spectrum of electrons in twisted bilayer graphene (tBLG) obtained by the band-unfolding method in the tight-binding model. We find the band-gap opening at particular points in the reciprocal space, that elucidates the drastic reduction of the Fermi-level velocity with the tiny twisted angles in tBLGs. We find that moiré pattern caused by the twist of the two graphene layers generates interactions among Dirac cones, otherwise absent, and the resultant cone-cone interactions peculiar to each point in the reciprocal space causes the energy gap and thus reduces the Fermi-level velocity.

We study the relation of crystal-liquid interfacial free energy and medium range order in the quasicrystal-forming $\mathrm{T}{\mathrm{i}}_{37}\mathrm{Z}{\mathrm{r}}_{42}\mathrm{N}{\mathrm{i}}_{21}$ liquid from undercooling experiment and ab initio molecular dynamics (MD) simulation. Adding a small amount of Ag to the liquid significantly reduces the degree of undercooling, which is suggestive of small interfacial free energy, and thus very similar atomic configuration between the liquid and the icosahedral quasicrystal phases. Using ab initio MD study, we find that Ag atoms predominantly form a bond with Zr atoms in the short range and, further, Ag-Zr pairs are extended in the liquid, as a medium range order which is identical to the global structural feature reported recently [Liu et al., Phys. Rev. Lett. 105, 155501 (2010)]. This result may expect extremely small undercooling if the icosahedral medium range order exists in a liquid forming an icosahedral quasicrystal, which implies the ambiguity of clear distinction of heterogeneous and homogeneous nucleation.

Mechanical spectroscopy, i.e., cyclic deformations at varying frequencies, is used theoretically and numerically to compute dissipation in model glasses. From a normal mode analysis, we show that in the high-frequency terahertz regime where dissipation is harmonic, the quality factor (or loss angle) can be expressed analytically. This expression is validated through nonequilibrium molecular dynamics simulations applied to a model of amorphous silica (${\mathrm{SiO}}_2$). Dissipation is shown to arise from nonaffine relaxations triggered by the applied strain through the excitation of vibrational eigenmodes that act as damped harmonic oscillators. We discuss an asymmetry vector field, which encodes the information about the structural origin of dissipation computed by mechanical spectroscopy. In the particular case of silica, we find that the motion of oxygen atoms, which induce a deformation of the Si-O-Si bonds, is the main contributor to harmonic energy dissipation.