High-order harmonic generation (HHG) from atoms is a coherent light source that opens up attosecond physics, but it is the application of HHG to solids that brings much of excitement for the last decade. Here we report a completely new kind of harmonics in a quasi-one-dimensional and hexagonal barium titanium sulfide: Under circularly polarized laser excitation, harmonics are generated only at first, fifth, seventh and eleventh orders. These magic harmonics appear only with circularly polarized light, not with linearly polarized light. Neither cubic nor tetragonal cells have magic harmonics even with circularly polarized light. Through a careful group-theory analysis, we find that two subgroups of symmetry operations unique to the hexagonal symmetry cancel out third and ninth harmonics. This feature presents a rare opportunity to develop HHG into a crystal-structure characterization tool for phase transitions between hexagonal and nonhexagonal structures.
We study the stability and electronic structure of magic-angle twisted bilayer graphene on the hexagonal boron nitride (TBG/BN). Full relaxation has been performed for commensurate supercells of the heterostructures with different twist angles ($θ'$) and stackings between TBG and BN. We find that the slightly misaligned configuration with $θ' = 0.54^\circ$ and the AA/AA stacking has the globally lowest total energy due to the constructive interference of the moiré interlayer potentials and thus the greatly enhanced relaxation in its $1 \times 1$ commensurate supercell. Gaps are opened at the F…
A hexagonal structure of solid molecular hydrogen with $P6_122$ symmetry is calculated to be more stable below about 200 GPa than the monoclinic $C2/c$ structure identified previously as the best candidate for phase III. We find that the effects of nuclear quantum and thermal vibrations play a central role in the stabilization of $P6_122$. The $P6_122$ and $C2/c$ structures are very similar and their Raman and infra-red data are in good agreement with experiment. However, our calculations show that the hexagonal $P6_122$ structure provides better agreement with the available x-ray diffraction …
In this manuscript we study luminescence of hexagonal boron nitride (hBN) by means of non-equilibrium Green's functions plus time-dependent perturbation theory. We derive a formula for light emission in solids in the limit of a weak excitation that includes perturbatively the contribution of electron-phonon coupling at the first order. This formula is applied to study luminescence in bulk hBN. This material has attracted interest due to its strong luminescence in the ultraviolet [Watanabe et al., Nature Mat. 3, 404(2004)]. The origin of this luminescence has been widely discussed, but only rec…
A molecular solid C$_{50}$Cl$_{10}$ with possible crystalline structures, including the hexagonal-close-packed (hcp) phase, the face-centered cubic (fcc) phase, and a hexagonal monolayer, is predicted in terms of first-principles calculation within the density functional theory. The stable structures are determined from the total-energy calculations, where the hcp phase is uncovered more stable than the fcc phase and the hexagonal monolayer in energy per molecule. The energy bands and density of states for hcp and fcc C$_{50}$Cl$_{10}$ are presented. The results show that C$_{50}$Cl% $_{10}$ m…
First principles FLAPW- GGA calculations have been performed to predict the structural, electronic, cohesive and magnetic properties for hexagonal WC doped with all 3d metals. The optimized lattice parameters, density of states, cohesive and formation energies have been obtained and analyzed for ternary solid solutions with nominal compositions W0.875M0.125C (where M = Sc, Ti, ..., Ni, Cu). In addition, the magnetic properties of these solid solutions have been examined, and magnetization has been established for W0.875Co0.125C.
We report on the discovery of a high-entropy alloy with a hexagonal crystal structure. Equiatomic samples in the alloy system Ho-Dy-Y-Gd-Tb were found to solidify as homogeneous single-phase high-entropy alloys. The results of our electron diffraction investigations and high-resolution scanning transmission electron microscopy are consistent with a Mg-type hexagonal structure. The possibility of hexagonal high-entropy alloys in other alloy systems is discussed.
Multi-principle element alloys have enormous potential, but their exploration suffers from the tremendously large range of configurations. In the last decade such alloys have been designed with a focus on random solid solutions. Here we apply an experimentally verified, combined thermodynamic and first-principles design strategy to reverse the traditional approach and to generate a new type of hcp Al-Hf-Sc-Ti-Zr high entropy alloy with a hitherto unique structure. A phase diagram analysis narrows down the large compositional space to a well-defined set of candidates. First-principles calculati…
Friction is one of the main sources of dissipation at liquid water/solid interfaces. Despite recent progress, a detailed understanding of water/solid friction in connection with the structure and energetics of the solid surface is lacking. Here we show for the first time that \textit{ab initio} molecular dynamics can be used to unravel the connection between the structure of nanoscale water and friction for liquid water in contact with graphene and with hexagonal boron nitride. We find that whilst the interface presents a very similar structure between the two sheets, the friction coefficient …
This paper reports on the growth and characterization of hexagonal boron nitride (hBN) and its use for solid-state thermal neutron detection. The hBN epilayers were grown by metalorganic chemical vapor deposition on sapphire substrates at a temperature of 1350 C. X-ray diffraction peak from the (002) hBN plane at a 2theta angle of 26.7 deg exhibited the c-lattice constant of 6.66 Å for these films. A strong peak corresponding to the high frequency Raman active mode of hBN was found for the films at 1370.5/cm. hBN-based solid-state neutron detectors were fabricated and tested with a metal-semic…
High-order harmonic generation (HHG) is a fundamental process which can be simplified as the production of high energetic photons from a material subjected to a strong driving laser field. This highly nonlinear optical process contains rich information concerning the electron structure and dynamics of matter, for instance, gases, solids and liquids. Moreover, the HHG from solids has recently attracted the attention of both attosecond science and condensed matter physicist, since the HHG spectra can carry information of electron-hole dynamics in bands and inter- and intra-band current dynamics.…
Based on ab initio band structure calculations we formulate a general theoretical method for description of the temperature dependence of electric field gradient in solids. The method employs a procedure of averaging multipole electron density component (l \neq 0) inside a sphere vibrating with the nucleus at its center. As a result of averaging each Fourier component (K \neq 0) on the sphere is effectively reduced by the square root of the Debye-Waller factor [exp(-W)]. The electric field gradient related to a sum of K-components most frequently decreases with temperature (T), but under certa…
The hydrostatic pressure is expected to be an effective knob to tune the magnetostructural phase transitions of hexagonal MMX alloy. In this study, magnetization measurements under hydrostatic pressure were performed on a MMX martensitic MnNi0.77Fe0.23Ge alloy. The magnetostructural transition temperature can be efficiently tuned to lower temperatures by applying moderate pressures, with a giant shift rate of -151 K GPa-1. A temperature span of 30 K is obtained under the pressure, within which a large magnetic entropy change of -23 J kg-1 K-1 in a field change of 5 T is induced by the mechanic…
The polarized Raman spectroscopy is capable of giving confirmation regarding the crystalline phase as well as the crystallographic orientation of the sample. In this context, apart from crystallographic x-ray and electron diffraction tools, polarized Raman spectroscopy and corresponding spectral imaging can be a promising crystallographic tool for determining both crystalline phase and orientation. Sub-micron sized hexagonal AlGaN crystallites are grown by a simple atmospheric pressure chemical vapor deposition technique using the self catalytic vapor-solid process under N-rich condition. The …
High-entropy alloys, near-equiatomic solid solutions of five or more elements, represent a new strategy for the design of materials with properties superior to those of conventional alloys. However, their phase space remains constrained, with transition metal high-entropy alloys exhibiting only face- or body-centered cubic structures. Here, we report the high-pressure synthesis of a hexagonal close-packed phase of the prototypical high-entropy alloy CrMnFeCoNi. This martensitic transformation begins at 14 GPa and is attributed to suppression of the local magnetic moments, destabilizing the ini…
Hexagonal boron nitride (h-BN) has been recently found to host a variety of quantum point defects, which are promising candidates as single-photon sources for solid-state quantum nanophotonics applications. Most recently, optically addressable spin qubits in h-BN have been the focus of intensive research due to their unique potential in quantum computing, communication, and sensing. However, the number of high-symmetry high-spin defects that are desirable for developing spin qubits in h-BN is highly limited. Here, we combine density functional theory (DFT) and quantum embedding theories to sho…
We study the effect of temperature up to 1000K on the structure of dense molecular para-hydrogen and ortho-deuterium, using the path-integral Monte Carlo method. We find a structural phase transition from orientationally disordered hexagonal close packed (hcp) to an orthorhombic structure of Cmca symmetry before melting. The transition is basically induced by thermal fluctuations, but quantum fluctuations of protons (deuterons) are important in determining the transition temperature through effectively hardening the intermolecular interaction. We estimate the phase line between hcp and Cmca ph…
We study the phase equilibrium between liquid water and ice Ih modeled by the TIP4P/Ice interatomic potential using enhanced sampling molecular dynamics simulations. Our approach is based on the calculation of ice Ih-liquid free energy differences from simulations that visit reversibly both phases. The reversible interconversion is achieved by introducing a static bias potential as a function of an order parameter. The order parameter was tailored to crystallize the hexagonal diamond structure of oxygen in ice Ih. We analyze the effect of the system size on the ice Ih-liquid free energy differ…
We use the diffusion quantum Monte Carlo (DMC) method to calculate the ground state phase diagram of solid molecular hydrogen and examine the stability of the most important insulating phases relative to metallic crystalline molecular hydrogen. We develop a new method to account for finite-size errors by combining the use of twist-averaged boundary conditions with corrections obtained using the Kwee-Zhang-Krakauer (KZK) functional in density functional theory. To study band-gap closure and find the metallization pressure, we perform accurate quasi-particle many-body calculations using the $GW$…
Transparent and colorless hexagonal boron nitride (hBN) single crystals were grown from the Mg-B-N system using high-pressure high-temperature cubic anvil technique. By varying the synthesis conditions we could determine the sequence of phase transformations occurring in the Mg-B-N system, construct the pressure-temperature (P-T) phase diagram and discuss the possible growth mechanism. The largest plate-like-shaped hBN crystals with sizes up to 2.5 mm in length and up to 10 (micro)m in thickness were grown at 30 kbar and 1900-2100 °C. The hBN crystals exhibited strong, narrow diffraction peaks…
Generation of high-order harmonics in gases enabled to probe the attosecond electron dynamics in atoms and molecules with unprecedented resolution. Extending the techniques developed originally for atomic and molecular gases to solid state materials requires a fundamental understanding of the physics that has been partially addressed theoretically. Here we employ time-dependent density-functional theory to investigate how the electron dynamics resulting in high-harmonic emission in monolayer hexagonal boron nitride is affected by the presence of vacancies. We show how these realistic spin-pola…
Color centers in solid state crystals have become a frequently used system for single photon generation, advancing the development of integrated photonic devices for quantum optics and quantum communication applications. In particular, defects hosted by two-dimensional (2D) hexagonal boron nitride (hBN) are a promising candidate for next-generation single photon sources, due to its chemical and thermal robustness and high brightness at room temperature. The 2D crystal lattice of hBN allows for a high extraction efficiency and easy integration into photonic circuits. Here we develop plasma etch…
Dielectrics with low loss at microwave frequencies are imperative for high-coherence solid-state quantum computing platforms. We study the dielectric loss of hexagonal boron nitride (hBN) thin films in the microwave regime by measuring the quality factor of parallel-plate capacitors (PPCs) made of NbSe$_{2}$-hBN-NbSe$_{2}$ heterostructures integrated into superconducting circuits. The extracted microwave loss tangent of hBN is bounded to be at most in the mid-10$^{-6}$ range in the low temperature, single-photon regime. We integrate hBN PPCs with aluminum Josephson junctions to realize transmo…
