Materials Science (cond-mat.mtrl-sci)

Abstract: In this work, the effect on crystallite orientation, surface morphology, fractal geometry, structural coordination and electronic environment of DC magnetron sputtered AlN films were investigated. X-ray diffraction results disclosed that the c-axis orientation of AlN films increased with the preferred wurtzite hexagonal structure above 17% N2 flow. X-ray reflectivity data confirmed AlN film density increased with increasing N2 flow and was found to be 3.18g/cm3 for 40% N2. The transition of electrons from N 1s to 2p states hybridized with Al 3p states because of {\pi}* resonance was obtained from X-ray absorption spectroscopy of the N K-edge. The semi-empirical coordination geometry of nitrogen atoms has been studied by deconvolution of N K-edge. The surface composition of AlN films at 40% N2 consists of 32.08, 51.94 and 15.97at.% Al, N and O respectively. Blue-shifting of A1(LO) and E1(LO) modes in the Raman spectra at phonon energies 800 and 1051cm-1 respectively was most likely due to the presence of oxygen bonds in the AlN films.

Abstract: Dirac semi-metal with magnetic atoms as constituents delivers an interesting platform to investigate the interplay of Fermi surface (FS) topology, electron correlation, and magnetism. One such family of semi-metal is YbMn$Pn_2$ ($Pn$ = Sb, Bi), which is being actively studied due to the intertwined spin and charge degrees of freedom. In this Letter, we investigate the relationship between the magnetic/crystal structures and FS topology of YbMnSb$_2$ using single crystal x-ray diffraction, neutron scattering, magnetic susceptibility, magnetotransport measurement and complimentary DFT calculation. Contrary to previous reports, the x-ray and neutron diffraction reveal that YbMnSb$_2$ crystallizes in an orthorhombic $Pnma$ structure with notable anti-phase displacement of the magnetic Mn ions that increases in magnitude upon cooling. First principles DFT calculation reveals a reduced Brillouin zone and more anisotropic FS of YbMnSb$_2$ compared to YbMnBi$_2$ as a result of the orthorhombicity. Moreover, the hole type carrier density drops by two orders of magnitude as YbMnSb$_2$ orders antiferromagnetically indicating band folding in magnetic ordered state. In addition, the Landau level fan diagram yields a non-trivial nature of the SdH quantum oscillation frequency arising from the Dirac-like Fermi pocket. These results imply that YbMnSb$_2$ is an ideal platform to explore the interplay of subtle lattice distortion, magnetic order, and topological transport arising from relativistic quasiparticles.

Abstract: Understanding the microscopic spatio-temporal dynamics of nonequilibrium charge carriers in heterosystems promises optimization of process and device design towards desired energy transfer. Hot electron transport is governed by scattering with other electrons, defects, and bosonic excitations. Analysis of the energy dependence of scattering pathways and identification of diffusive, super-diffusive, and ballistic transport regimes are current challenges. We determine in femtosecond time-resolved two-photon photoelectron emission spectroscopy the energy-dependent change of the electron propagation time through epitaxial Au/Fe(001) heteostructures as a function of Au layer thickness for energies of 0.5 to \unit[2.0]{eV} above the Fermi energy. We describe the laser-induced nonequilibrium electron excitation and injection across the Fe/Au interface using real-time time-dependent density functional theory and analyze the electron propagation through the Au layer by microscopic electron transport simulations. We identify ballistic transport of minority electrons at energies with a nascent, optically excited electron population which is determined by the combination of photon energy and the specific electronic structure of the material. At lower energy, super-diffusive transport with 1 to 4 scattering events dominates. The effective electron velocity accelerates from 0.3 to \unit[1]{nm/fs} with an increase in the Au layer thickness from 10 to 100~nm. This phenomenon is explained by electron transport that becomes preferentially aligned with the interface normal for thicker Au layers, which facilitates electron momentum / energy selection by choice of the propagation layer thickness.

Abstract: Using molecular beam epitaxy, we demonstrate the growth of (In,Ga)N shells emitting in the green spectral range around very thin (35 nm diameter) GaN core nanowires. These GaN nanowires are obtained by self-assembled growth on TiN. We present a qualitative shell growth model accounting for both the three-dimensional nature of the nanostructures as well as the directionality of the atomic fluxes. This model allows us, on the one hand, to optimise the conditions for high and homogeneous In incorporation and, on the other hand, to explain the influence of changes in the growth conditions on the sample morphology and In content. Specifically, the impact of the V/III and In/Ga flux ratios, the rotation speed and the rotation direction are investigated. Notably, with In acting as surfactant, the ternary (In,Ga)N shells are much more homogeneous in thickness along the NW length than their binary GaN counterparts.

Abstract: The low crystal symmetry of rhenium disulphide (ReS2) leads to the emergence of dichroic optical and optoelectronic response, absent in other layered transition metal dichalcogenides, which could be exploited for device applications requiring polarization resolution. To date, spectroscopy studies on the optical response of ReS2 have relied almost exclusively in characterization techniques involving optical detection, such as photoluminescence, absorbance, or reflectance spectroscopy. However, to realize the full potential of this material, it is necessary to develop knowledge on its optoelectronic response with spectral resolution. In this work, we study the polarization-dependent photocurrent spectra of few-layer ReS2 photodetectors, both in room conditions and at cryogenic temperature. Our spectral measurements reveal two main exciton lines at energies matching those reported for optical spectroscopy measurements, as well as their excited states. Moreover, we also observe an additional exciton-like spectral feature with a photoresponse intensity comparable to the two main exciton lines. We attribute this feature, not observed in earlier photoluminescence measurements, to a non-radiative exciton transition. The intensities of the three main exciton features, as well as their excited states, modulate with linear polarization of light, each one acquiring maximal strength at a different polarization angle. We have performed first-principles exciton calculations employing the Bethe-Salpeter formalism, which corroborate our experimental findings. Our results bring new perspectives for the development of ReS2-based nanodevices.

Abstract: The orbital angular momenta (OAM) of electrons play an increasingly important role in ultrafast electron and magnetization dynamics. In this theoretical study, we investigate the electron dynamics induced by femtosecond laser pulses in a normal metal, a ferromagnet, and a ferromagnet/normal metal heterostructure. We analyze the spatio-temporal distributions of the laser-induced OAM and their respective currents. Our findings demonstrate that a circularly polarized laser pulse can induce a sizable and long-lasting OAM component in a normal metal. Furthermore, an interface between a ferromagnet and a normal metal facilitates the demagnetization of the magnet by the OAM contribution to the total magnetization. Finally, to transfer OAM from a ferromagnet into a normal metal, it is advantageous to use a laser setup that induces the desired OAM component in the ferromagnet, but not in the normal metal.

Abstract: Momentum-matched type II van der Waals heterostructures (vdWHs) have been designed by assembling layered two-dimensional semiconductors (2DSs) with special band-structure combinations - that is, the valence band edge at the Gamma point (the Brillouin-zone center) for one 2DS and the conduction band edge at the Gamma point for the other [Ubrig et al., Nat. Mater. 19, 299 (2020)]. However, the band offset sizes, band-alignment types, and whether momentum matched or not, all are affected by the interfacial effects between the component 2DSs, such as the quasichemical-bonding (QB) interaction between layers and the electrical dipole moment formed around the vdW interface. Here, based on density-functional theory calculations, first we probe the interfacial effects (including different QBs for valence and conduction bands, interface dipole, and, the synergistic effects of these two aspects) on band-edge evolution in energy and valley (location in the Brillouin zone) and the resulting changes in band alignment and momentum matching for a typical vdWH of monolayer InSe and bilayer WS2, in which the band edges of subsystems satisfy the special band-structure combination for a momentum-matched type II vdWH. Then, based on the conclusions of the studied interfacial effects, we propose a practical screening method for robust momentum-matched type II vdWHs. This practical screening method can also be applied to other band alignment types. Our current study opens a way for practical screening and designing of vdWHs with robust momentum-matching and band alignment type.

Abstract: A general method to obtain a representation of the structural landscape of nanoparticles in terms of a limited number of variables is proposed. The method is applied to a large dataset of parallel tempering molecular dynamics simulations of gold clusters of 90 and 147 atoms, silver clusters of 147 atoms, and copper clusters of 147 atoms, covering a plethora of structures and temperatures. The method leverages convolutional neural networks to learn the radial distribution functions of the nanoclusters and to distill a low-dimensional chart of the structural landscape. This strategy is found to give rise to a physically meaningful and differentiable mapping of the atom positions to a low-dimensional manifold, in which the main structural motifs are clearly discriminated and meaningfully ordered. Furthermore, unsupervised clustering on the low-dimensional data proved effective at further splitting the motifs into structural subfamilies characterized by very fine and physically relevant differences, such as the presence of specific punctual or planar defects or of atoms with particular coordination features. Owing to these peculiarities, the chart also enabled tracking of the complex structural evolution in a reactive trajectory. In addition to visualization and analysis of complex structural landscapes, the presented approach offers a general, low-dimensional set of differentiable variables which has the potential to be used for exploration and enhanced sampling purposes.

Abstract: The observed open circuit voltages in best performing solar cells are explained outside of the recombination paradigm, based on such factors as electrostatic screening, Meyer-Neldel effect, and lateral nonuniformities. The underlying concept of suppressed recombination presents a long neglected alternative pathway to efficient PV. The criterion of suppressed recombination is consistent with the data for best performing solar cells. Also, consistent with the observations, is the open circuit voltage deficit that exhibits a lower bound of about $0.2-0.3$ V, does not correlate well with the optical gap, and shows a significant dispersion for materials possessing the same gap values.

Abstract: For quantum electronics, the possibility to finely tune the properties of magnetic topological insulators (TIs) is a key issue. We studied solid solutions between two isostructural Z$_2$ TIs, magnetic MnBi$_2$Te$_4$ and nonmagnetic GeBi$_2$Te$_4$, with Z$_2$ invariants of 1;000 and 1;001, respectively. For high-quality, large mixed crystals of Ge$_x$Mn$_{1-x}$Bi$_2$Te$_4$, we observed linear x-dependent magnetic properties, composition-independent pairwise exchange interactions along with an easy magnetization axis. The bulk band gap gradually decreases to zero for $x$ from 0 to 0.4, before reopening for $x>0.6$, evidencing topological phase transitions (TPTs) between topologically nontrivial phases and the semimetal state. The TPTs are driven purely by the variation of orbital contributions. By tracing the x-dependent $6p$ contribution to the states near the fundamental gap, the effective spin-orbit coupling variation is extracted. As $x$ varies, the maximum of this contribution switches from the valence to the conduction band, thereby driving two TPTs. The gapless state observed at $x=0.42$ closely resembles a Dirac semimetal above the Neel temperature and shows a magnetic gap below, which is clearly visible in raw photoemission data. The observed behavior of the Ge$_x$Mn$_{1-x}$Bi$_2$Te$_4$ system thereby demonstrates an ability to precisely control topological and magnetic properties of TIs.

Abstract: Lithium-ion batteries (LIBs) are crucial for the green economy, powering portable electronics, electric vehicles, and renewable energy systems. The solid-electrolyte interphase (SEI) is vital for LIB operation, performance, and safety. SEI forms due to thermal instability at the anode-electrolyte interface, with electrolyte reduction products stabilizing it as an electrochemical buffer. This article aims to enhance the parametrization of the ReaxFF force field for accurate molecular dynamics (MD) simulations of SEI in LIBs. Focus is on Lithium Fluoride (LiF), an inorganic salt with favorable properties in the passivation layer. The protocol heavily relies on Python libraries for atomistic simulations, enabling robust automation of reparameterization steps. The proposed configurations and dataset enable the new ReaxFF to accurately represent the solid nature of LiF and improve mass transport property prediction in MD simulations. Optimized ReaxFF surpasses previous force fields by adjusting lithium diffusivity, resulting in a significant improvement in room temperature prediction by two orders of magnitude. However, our comprehensive investigation reveals ReaxFF's strong sensitivity to the training set, challenging its ability to interpolate the potential energy surface. Consequently, the current ReaxFF formulation is suitable for modeling specific phenomena by utilizing the proposed interactive reparameterization protocol and constructing a dataset. This work is an important step towards refining ReaxFF for precise reactive MD simulations, shedding light on challenges and limitations in force field parametrization. The demonstrated limitations underscore the potential for developing more advanced force fields through our interactive reparameterization protocol, enabling accurate and comprehensive MD simulations in the future.

Abstract: By performing first-principles calculations in conjunction with Monte Carlo simulations, we systematically investigated the frustrated magnetic states induced by in-plane compressive strain in LiCrTe$_{2}$. Our calculations support that the magnetic ground state of LiCrTe$_{2}$ crystal is A-type antiferromagnetic (AFM), with an in-plane ferromagnetic (FM) state and interlayer AFM coupling. Furthermore, it is found that compressive strain can significantly alter the magnetic interactions, giving rise to a transition from an in-plane FM to an AFM state, undergoing a helimagnetic phase. Remarkably, a highly frustrated helimagnetic state with disordered spin spirals under moderate strain arises from the competition between spiral propagation modes along distinct directions. In addition, various topological spin defects emerge in this frustrated helimagnetic phase, which are assembled from various domain wall units. These topological defects can be further tuned with external magnetic fields. Our calculations not only uncover the origin of exotic frustrated magnetism in triangular lattice magnetic systems, but also offer a promising route to engineer the frustrated and topological magnetic state, which is of significance in both fundamental research and technological applications.