Materials Science (cond-mat.mtrl-sci)

Abstract: Disordered rocksalt Li-excess (DRX) compounds are attractive new cathode materials for Li-ion batteries as they contain resource-abundant metals and do not require the use of cobalt or nickel. Understanding the delithiation process and cation short-range ordering (SRO) in DRX compounds is essential to improving these promising cathode materials. Herein, we use first-principles calculations along with the cluster-expansion approach to model the disorder in DRX Li2-xVO3, 0 < x < 1. We discuss the SRO of Li in tetrahedral and octahedral sites, and the order in which Li delithiates and V oxidizes with respect to local environments. We reveal that the number of nearest-neighbor V dictates the order of delithiation from octahedral sites and that V are oxidized in a manner that minimizes the electrostatic interactions among V. Our results provide valuable insight for tailoring the performance of V-based DRX cathode materials in general by controlling the SRO features that reduce energy density.

Abstract: High harmonic emissions from crystalline solids contain rich information on the dynamics of electrons driven by intense infrared laser fields and have been intensively studied owing to their potential use as a probe of microscopic electronic structures. Especially, the ability to measure the temporal response of high harmonics may allow us to investigate electron dynamics directly in quantum materials. However, this most essential aspect of high harmonic emissions has been challenging to measure. Here, we propose a simple solution for this problem: a high harmonic interferometer, where high harmonics are generated in each of the path of a Mach-Zehnder interferometer and an interferogram of them is captured. The high harmonic interferometer allows us to achieve a relative time resolution between the target and reference high harmonics of less than 150 attoseconds, which is fine enough to track sub-cycle dynamics of electrons in solids. By using high harmonic interferometrer, we succeeded in capturing the real time dynamics of Floquet states in WSe2, whose indirect signature had so far been caught only by time-averaged measurement. Our simple technique will open a door to attosecond electron dynamics in solids.

Abstract: The family of Van der Waals dichalcogenides (VdWDs) includes a large number of compositions and phases, exhibiting varied properties and functionalities. They have opened up a novel electronics of two-dimensional materials, characterized by higher integration and interfaces which are atomically sharper and cleaner than conventional electronics. Among these functionalities, some VdWDs possess remarkable thermoelectric properties. SnSe2 has been identified as a promising thermoelectric material on the basis of its estimated electronic and transport properties. In this work we carry out experimental meas-urements of the electric and thermoelectric properties of SnSe2 flakes. For a 30 micron thick SnSe2 flake at room temperature, we measure electron mobility of 40 cm^2 V^-1 s^-1, a carrier density of 4 x 10^18 cm^-3, a Seebeck coefficient S around -400 microV/K and thermoelectric power factor around 0.35 mW m^-1 K^-2. The comparison of experimental results with theoretical calculations shows fair agreement and indicates that the dominant carrier scattering mechanisms are polar optical phonons at room temperature and ionized im-purities below 50 K. In order to explore possible improvement of the thermoelectric properties, we carry out reversible electrostatic doping on a thinner flake, in a field effect setup. On this 75 nm thick SnSe2 flake, we measure a field effect variation of the Seebeck coefficient of up to 290 % at low temperature, and a corresponding variation of the thermoelectric power factor of up to 1050 %. We find that the power factor increases with the depletion of n-type charge carriers. Field effect control of thermoelectric transport opens perspectives for boosting energy harvesting and novel switching technologies based on two-dimensional materials.

Abstract: This work reports the thermal conductivity of RbV3Sb5 and CsV3Sb5 with three-dimensional charge density wave phase transitions from 80 K to 400 K measured by pump-probe thermoreflectance techniques. The in-plane (basal plane) thermal conductivities are found moderate, i.e., 12 W/mK of RbV3Sb5 and 8.8 W/mK of CsV3Sb5 at 300 K. Low cross-plane (stacking direction) thermal conductivities are observed, with 0.72 W/mK of RbV3Sb5 and 0.49 W/mK of CsV3Sb5 at 300 K. A unique glass-like temperature dependence in the cross-plane thermal conductivity is observed, which decreases monotonically even lower than the Cahill-Pohl limit as the temperature decreases below the phase transition point TCDW. This temperature dependence is found to obey the hopping transport picture. In addition, a peak in cross-plane thermal conductivity is observed at TCDW as a fingerprint of the modulated structural distortion along the stacking direction.

Abstract: Magnetic nano-objects possess great potential for more efficient data processing, storage and neuromorphic type of applications. Using high perpendicular magnetic anisotropy synthetic antiferromagnets in the form of multilayer-based metamaterials we purposely reduce the antiferromagnetic (AF) interlayer exchange energy below the out-of-plane demagnetization energy, which controls the magnetic domain formation. As we show via macroscopic magnetometry as well as microscopic Lorentz transmission electron microscopy, in this unusual magnetic energy regime, it becomes possible to stabilize nanometer scale stripe and bubble textures consisting of ferromagnetic (FM) out-of-plane domain cores separated by AF in-plane Bloch-type domain walls. This unique coexistence of mixed FM/AF order on the nanometer scale opens so far unexplored perspectives in the architecture of magnetic domain landscapes as well as the design and functionality of individual magnetic textures, such as bubble domains with alternating chirality.

Abstract: Oxide-based two-dimensional electron gases (2DEGs) have generated significant interest due to their potential for discovering novel physical properties. Among these, 2DEGs formed in KTaO3 stand out due to the recently discovered crystal face-dependent superconductivity and large Rashba splitting, both of which hold potential for future oxide electronics devices. In this work, angle-resolved photoemission spectroscopy is used to study the electronic structure of the 2DEG formed at the (110) surface of KTaO3 after deposition of a thin Al layer. Our experiments revealed a remarkable anisotropy in the orbital character of the electron-like dispersive bands, which form a Fermi surface consisting of two elliptical contours with their major axes perpendicular to each other. The measured electronic structure is used to constrain the modeling parameters of self-consistent tight-binding slab calculations of the band structure. In these calculations, an anisotropic Rashba splitting is found with a value as large as 4 meV at the Fermi level along the [-110] crystallographic direction. This large unconventional and anisotropic Rashba splitting is rationalized based on the orbital angular momentum formulation. These findings provide insights into the interpretation of spin-orbitronics experiments and help to constrain models for superconductivity in the KTO(110)-2DEG system.

Abstract: Inspired by the neuro-synaptic frameworks in the human brain, neuromorphic computing is expected to overcome the bottleneck of traditional von-Neumann architecture and be used in artificial intelligence. Here, we predict a class of potential candidate materials, MCu$_3$X$_4$ (M = V, Nb, Ta; X = S, Se, Te), for neuromorphic computing applications through first-principles calculations based on density functional theory. We find that when MCu$_3$X$_4$ are inserted with Li atom, the systems would transform from semiconductors to metals due to the considerable electron filling [~0.8 electrons per formula unit (f.u.)] and still maintain well structural stability. Meanwhile, the inserted Li atom also has a low diffusion barrier (~0.6 eV/f.u.), which ensures the feasibility to control the insertion/extraction of Li by gate voltage. These results establish that the system can achieve the reversible switching between two stable memory states, i.e., high/low resistance state, indicating that it could potentially be used to design synaptic transistor to enable neuromorphic computing. Our work provides inspiration for advancing the search of candidate materials related to neuromorphic computing from the perspective of theoretical calculations.

Abstract: Optically driven intersite and interlayer spin transfer are individually known as the fastest processes for manipulating the spin order of magnetic materials on the sub 100 fs time scale. However, their competing influence on the ultrafast magnetization dynamics remains unexplored. In our work, we show that optically induced intersite spin transfer (also known as OISTR) dominates the ultrafast magnetization dynamics of ferromagnetic alloys such as Permalloy (Ni80Fe20) only in the absence of interlayer spin transfer into a substrate. Once interlayer spin transfer is possible, the influence of OISTR is significantly reduced and interlayer spin transfer dominates the ultrafast magnetization dynamics. This provides a new approach to control the magnetization dynamics of alloys on extremely short time scales by fine-tuning the interlayer spin transfer.

Abstract: Permanent magnets draw their properties from a complex interplay, across multiple length scales, of the composition and distribution of their constituting phases, that act as building blocks, each with their associated intrinsic properties. Gaining a fundamental understanding of these interactions is hence key to decipher the origins of their magnetic performance and facilitate the engineering of better-performing magnets, through unlocking the design of the "perfect defects" for ultimate pinning of magnetic domains. Here, we deployed advanced multiscale microscopy and microanalysis on a bulk Sm2(CoFeCuZr)17 pinning-type high-performance magnet with outstanding thermal and chemical stability. Making use of regions with different chemical compositions, we showcase how both a change in the composition and distribution of copper, along with the atomic arrangements enforce the pinning of magnetic domains, as imaged by nanoscale magnetic induction mapping. Micromagnetic simulations bridge the scales to provide an understanding of how these peculiarities of micro- and nanostructure change the hard magnetic behaviour of Sm2(CoFeCuZr)17 magnets. Unveiling the origins of the reduced coercivity allows us to propose an atomic-scale defect and chemistry manipulation strategy to define ways toward future hard magnets.

Abstract: Despite recent advances of layered square-net topological material models that possess ideal semimetallic electronic structures and promising potential in material applications, the identification of experimentally accessible two-dimensional square-net materials with related topological properties has proven challenging. Due to the highly tunable physical and topological properties of III-V semiconductors, we revisit the class of III-V materials and observe that the litharge-phase InBi is a layered square-net material and can be exfoliated into the InBi monolayer. We present a comprehensive first-principles study of the energy landscape of the InBi monolayer. We identify a paraelastic phase and three ferroelastic phases and study their topological properties. Specifically, we show that the paraelastic InBi monolayer is a trivial insulator due to the orbital-ordering-induced band inversion occurring between states with the same parity. Substituting one Bi atom per cell with another V-group element (N, P, As) or applying an electric field that breaks the inversion symmetry and changes the orbital onsite energy, the paraelastic InBi monolayer can be driven into the topological insulator phase. Furthermore, one of the ferroelastic phases of pure InBi, which can be obtained by gently straining the paraelastic phase, also possesses such topological insulating properties. These results provide several experimentally accessible routes to tune the nontrivial topology in the InBi monolayer, including creating heterostructures with piezoelectric or ferroelectric substrates and applying mechanical strain, making the InBi monolayer an ideal platform to study the interplay of reduced dimensionality, square-net chemical bonding networks, and band topology.

Abstract: Magnons are one of the carriers of angular momentum that are involved in the ultrafast magnetization dynamics in ferromagnets, but their contribution to the electronic dynamics and their interplay with other scattering process that occur during ultrafast demagnetization has not yet been studied in the framework of a microscopic dynamical model. The present paper presents such an investigation of electronic scattering dynamics in itinerant ferromagnets at the level of Boltzmann scattering integrals for the magnon distributions and spin-dependent electron distributions. In addition to electron-magnon scattering, we include spin-conserving and effective Elliott-Yafet like spin-flip electron-electron scattering processes and the influence of phonons. In our model system, the creation or annihilation of magnons leads to transitions between two spin-split electronic bands with energy and momentum conservation. Due to the presence of spin-orbit coupling, Coulomb scattering transitions between these bands are also possible, and we describe them on an equal footing in terms of Boltzmann scattering integrals. For an instantaneous carrier excitation process we analyze the influence of both interaction processes on the magnon and spin-dependent electron dynamics, and show that their interplay gives rise to an efficient creation of magnons at higher energies and wave vectors accompanied by only a small increase of the electronic spin polarization. These results present a microscopic dynamical scenario that shows how non-equilibrium magnons may dominate the magnetic response of a ferromagnet on ultrafast timescales.