Materials Science (cond-mat.mtrl-sci)

Abstract: Aluminosilicate (Al-Si-O) thin films containing up to 31 at. % Al and 23 at. % Si were prepared by reactive RF magnetron co-sputtering. Mechanical and structural properties were measured by indentation and specular reflectance infrared spectroscopy at varying Si sputtering target power and substrate temperature in the range 100 to 500 {\deg}C. It was found that an increased substrate temperature and Al/Si ratio give denser structure and consequently higher hardness (7.4 to 9.5 GPa) and reduced elastic modulus (85 to 93 GPa) while at the same time lower crack resistance (2.6 to 0.9 N). The intensity of the infrared Si-O-Si/Al asymmetric stretching vibrations shows a linear dependence with respect to Al concentration. The Al-O-Al vibrational band (at 1050 cm-1) shifts towards higher wavenumbers with increasing Al concentration which indicates a decrease of the bond length, evidencing denser structure and higher residual stress, which is supported by the increased hardness. The same Al-O-Al vibrational band (at 1050 cm-1) shifts towards lower wavenumber with increasing substrate temperature indicating an increase in the of the average coordination number of Al.

Abstract: $\mathrm{Fe_{n=4,5}GeTe_2}$ exhibits quasi-two-dimensional properties as a promising candidate for a near-room-temperature ferromagnet, which has attracted great interest. In this work, we notice that the crystal lattice of $\mathrm{Fe_{n=4,5}GeTe_2}$ can be approximately considered to be stacked by three bipartite crystal lattices. By combining the model Hamiltonians of bipartite crystal lattices and first-principles calculations, we investigate the electronic structure and the magnetism of $\mathrm{Fe_{n=4,5}GeTe_2}$. We conclude that flat bands near the Fermi level originate from the bipartite crystal lattices and that these flat bands are expected to lead to the itinerant ferromagnetism in $\mathrm{Fe_{n=4,5}GeTe_2}$. Interestingly, we also find that the magnetic moment of the Fe5 atom in $\mathrm{Fe_5 Ge Te_2}$ is distinct from the other Fe atoms and is sensitive with the Coulomb interaction $U$ and external pressure. These findings may be helpful to understand the exotic magnetic behavior of $\mathrm{Fe_{n=4,5} Ge Te_2}$.

Abstract: Processes involving ultrafast laser driven electron-phonon dynamics play a fundamental role in the response of quantum systems in a growing number of situations of interest, as evidenced by phenomena such as strongly driven phase transitions and light driven engineering of material properties. To show how these processes can be captured from a computational perspective, we simulate the transient absorption spectra and high harmonic generation signals associated with valley selective excitation and intra-band charge carrier relaxation in monolayer hexagonal boron nitride. We show that the multi-trajectory Ehrenfest dynamics approach, implemented in combination with real-time time-dependent density functional theory and tight-binding models, offers a simple, accurate and efficient method to study ultrafast electron-phonon coupled phenomena in solids under diverse pump-probe regimes which can be easily incorporated into the majority of real-time ab-initio software packages.

Abstract: In this work, a generalized force-field methodology for the relaxation of large moir\'e heterostructures is proposed. The force-field parameters are optimized to accurately reproduce the structural degrees of freedom of some computationally manageable cells relaxed using density functional theory. The parameters can then be used to handle large moir\'e systems. We specialize to the case of 2H-phased twisted transition-metal dichalcogenide homo- and heterobilayers using a combination of the Stillinger-Weber intralayer- and the Kolmogorov-Crespi interlayer-potential. Force-field parameters are developed for all combinations of MX$_2$ for $\text{M}\in\{\text{Mo},\text{W}\}$ and $\text{X}\in\{\text{S},\text{Se},\text{Te}\}$. The results show agreement within 20 meV in terms of band structure between density functional theory and force-field relaxation. Using the relaxed structures, a simplified and systematic scheme for the extraction of the interlayer moir\'e potential is presented for both R- and H-stacked systems. We show that in-plane and out-of-plane relaxation effects on the moir\'e potential, which is made both deeper and wider after relaxation, are essential. An interpolation based methodology for the calculation of the interlayer binding energy is also proposed. Finally, we show that atomic reconstruction, which is captured by the force-field method, becomes especially prominent for angles below 4-5$^\circ$, when there is no mismatch in lattice constant between layers.

Abstract: Determining the melting curves of materials up to high pressures has long been a challenge experimentally and theoretically. A large class of materials, including most metals, has been shown to exhibit hidden scale invariance, an approximate scale invariance of the potential-energy landscape that is not obvious from the Hamiltonian. For these materials the isomorph theory allows the identification of curves in the phase diagram along which structural and dynamical properties are invariant to a good approximation when expressed in appropriately scaled form. These curves, the isomorphs, can also be used as the basis for constructing accurate melting curves from simulations at a single state point [U. R. Pedersen \textit{et al.}, Nat. Comm. \textbf{7}, 12386 (2016)]. In this work we apply the method to the metals Cu simulated using the effective medium theory and Al simulated using density functional theory (DFT). For Cu the method works very well and is validated using two-phase melting point simulations. For Al there are likewise good isomorphs and the method generates the melting curve accurately as compared to previous experimental and DFT results. In line with a recent suggestion of Hong and van de Walle [Phys. Rev. B \textbf{100}, 140102 (2019)], we finally argue that the tendency for the density-scaling exponent $\gamma$ to decrease with increasing density in metals implies that metals in general will undergo re-entrant melting, i.e., have a maximum of melting temperature as a function of pressure.

Abstract: Spin textures, i.e., the distribution of spin polarization vectors in reciprocal space, exhibit diverse patterns determined by symmetry constraints, resulting in a variety of spintronic phenomena. Here, we propose a universal theory to comprehensively describe the nature of spin textures by incorporating three symmetry flavors of reciprocal wavevector, atomic orbital and atomic site. Such approach enables us to establish a complete classification of spin textures constrained by the little co-group and predict unprecedentedly reported spin texture types, such as Zeeman-type spin splitting in antiferromagnets and quadratic spin texture. To examine the impact of atomic orbitals and sites, we predict orbital-dependent spin texture and anisotropic spin-momentum-site locking effects and corresponding material candidates validated through first-principles calculations. Our theory not only covers all possible spin textures in crystal solids described by magnetic space groups, but also introduces new possibilities for designing innovative spin textures by the coupling of multiple degrees of freedom.

Abstract: Accurate classification of molecular chemical motifs from experimental measurement is an important problem in molecular physics, chemistry and biology. In this work, we present neural network ensemble classifiers for predicting the presence (or lack thereof) of 41 different chemical motifs on small molecules from simulated C, N and O K-edge X-ray absorption near-edge structure (XANES) spectra. Our classifiers not only reach a maximum average class-balanced accuracy of 0.99 but also accurately quantify uncertainty. We also show that including multiple XANES modalities improves predictions notably on average, demonstrating a "multi-modal advantage" over any single modality. In addition to structure refinement, our approach can be generalized for broad applications with molecular design pipelines.

Abstract: The morphological evolution of nanoporous gold is generally believed to be governed by surface diffusion. This work specifically explores the dependence of mass transport by surface diffusion on the curvature of a gold surface. The surface diffusivity is estimated by molecular dynamics simulations for a variety of surfaces of constant mean curvature, eliminating any chemical potential gradients and allowing the possible dependence of the surface diffusivity on mean curvature to be isolated. The apparent surface diffusivity is found to have an activation energy of ~0.74 eV with a weak dependence on curvature, but is consistent with the values reported in the literature. The apparent concentration of mobile surface atoms is found to be highly variable, having an Arrhenius dependence on temperature with an activation energy that also has a weak curvature dependence. These activation energies depend on curvature in such a way that the rate of mass transport by surface diffusion is nearly independent of curvature, but with a higher activation energy of ~1.01 eV. The curvature dependencies of the apparent surface diffusivity and concentration of mobile surface atoms is believed to be related to the expected lifetime of a mobile surface atom, and has the practical consequence that a simulation study that does not account for this finite lifetime could underestimate the activation energy for mass transport via surface diffusion by ~0.27 eV.

Abstract: Re-configurable materials and meta-materials can jump between space symmetry classes during their deformations. Here, we introduce the concept of singular symmetry enhancement, which refers to an abrupt jump to a higher symmetry class accompanied by an un-avoidable reduction in the number of dispersion bands of the excitations of the material. Such phenomenon prompts closings of some of the spectral resonant gaps along singular manifolds in a parameter space. In this work, we demonstrate that these singular manifolds carry topological charges. As a concrete example, we show that a deformation of an acoustic crystal that encircles a $p11g$-symmetric configuration of the cavity resonators results in an adiabatic cycle that carries a Chern number in the bulk and displays Thouless pumping at the edges. The outcome is a very general principle for recognizing or engineering topological adiabatic processes in complex materials and meta-materials.