Materials Science (cond-mat.mtrl-sci)

Abstract: In a stack of atomically-thin Van der Waals layers, introducing interlayer twist creates a moir\'e superlattice whose period is a function of twist angle. Changes in that twist angle of even hundredths of a degree can dramatically transform the system's electronic properties. Setting a precise and uniform twist angle for a stack remains difficult, hence determining that twist angle and mapping its spatial variation is very important. Techniques have emerged to do this by imaging the moir\'e, but most of these require sophisticated infrastructure, time-consuming sample preparation beyond stack synthesis, or both. In this work, we show that Torsional Force Microscopy (TFM), a scanning probe technique sensitive to dynamic friction, can reveal surface and shallow subsurface structure of Van der Waals stacks on multiple length scales: the moir\'es formed between bilayers of graphene and between graphene and hexagonal boron nitride (hBN), and also the atomic crystal lattices of graphene and hBN. In TFM, torsional motion of an AFM cantilever is monitored as the it is actively driven at a torsional resonance while a feedback loop maintains contact at a set force with the surface of a sample. TFM works at room temperature in air, with no need for an electrical bias between the tip and the sample, making it applicable to a wide array of samples. It should enable determination of precise structural information including twist angles and strain in moir\'e superlattices and crystallographic orientation of VdW flakes to support predictable moir\'e heterostructure fabrication.

Abstract: Calculating the electronic structure of materials at finite temperatures is important for rationalizing their physical properties and assessing their technological capabilities. However, finite-temperature calculations typically require large system sizes or long simulation times. This is challenging for non-empirical theoretical methods because the involved bottleneck of performing many first-principles calculations can pose a steep computational barrier for larger systems. While machine-learning molecular dynamics enables large-scale/long-time simulations of the structural properties, the difficulty of computing in particular the electronic structure of large and disordered materials still remains. In this work, we suggest an adaptation of the tight-binding formalism which allows for computationally efficient calculations of temperature-dependent properties of semiconductors. Our dynamic tight-binding approach utilizes hybrid-orbital basis functions and a modeling of the distance dependence of matrix elements via numerical integration of atomic orbitals. We show that these design choices lead to a dynamic tight-binding model with a minimal amount of parameters which are straightforwardly optimized using density functional theory. Combining dynamic tight-binding with machine learning molecular dynamics and hybrid density functional theory, we find that it accurately describes finite-temperature electronic properties in comparison to experiment for the prototypical semiconductor gallium-arsenide.

Abstract: One of the main material properties altered by rare earth additions in magnesium alloys is texture, which can be specifically adjusted to enhance ductility and formability. The current study aims at illuminating the texture selection process in a Mg-0.073at%Gd-0.165at%Zn alloy by investigating recrystallization nucleation and early nucleus growth during static recrystallization. An as-cast sample of the investigated alloy was deformed in uniaxial compression at 200{\deg}C till 40% strain and was then cut into two halves for subsequent microstructure characterization via ex-situ and quasi in-situ EBSD investigations. In order to gain insights into the evolution of texture during recrystallization, the contributions from dynamic and static recrystallization were initially separated and the origin of the non-basal orientation of recrystallization nuclei was traced back to several potential nucleation sites within the deformed matrix. Considering the significant role of double-twin band recrystallization in determining the recrystallization texture, this type of recrystallization nucleation was further investigated via quasi-in-situ EBSD on a deformed sample, annealed at 400{\deg} for different annealing times. With progressive annealing a noticeable trend was observed, in which the basal nuclei gradually diminished and eventually vanished from the annealed microstructure. In contrast, the off-basal nuclei exhibited continuous growth, ultimately becoming the dominant contributors to the recrystallization texture. The study therefore emphasizes the importance of particular nucleation sites that generate favorably oriented off-basal nuclei, which over the course of recrystallization outcompete the neighboring basal-oriented nuclei in terms of growth, and thereby dominate the recrystallization texture.

Abstract: We unveil a new non-basal slip mechanism in the {\mu}-phase at room temperature using nanomechanical testing, transmission electron microscopy and atomistic simulations. The (1-105) planar faults with a displacement vector of 0.07[-5502] can be formed by dislocation glide. They do not disrupt the Frank-Kasper packing and therefore enable the accommodation of plastic strain at low temperatures without requiring atomic diffusion. The intersections between the (1-105) planar faults and basal slip result in stress concentration and crack nucleation during loading.

Abstract: Permanent magnets are of great importance due to their vast applications. MnBi has been proposed to be a potential permanent magnet that can be widely used while past efforts have been focused on optimizing the ferromagnetic low-temperature phase of MnBi. Herein, we report a series of new materials, CuxMn1-xBi, crystallizing in a high-temperature-phase (HTP) MnBi-related structure. We synthesized single crystals of CuxMn1-xBi and found that they crystallize in an unreported trigonal structure (P -31c). Magnetic properties measurements imply high-temperature antiferromagnetic (AFM) ordering and low-temperature ferromagnetic or ferrimagnetic (FM/FiM) ordering. By analyzing the doping effect on crystal structure and magnetic properties, we established a magnetic phase diagram for Cu-doped MnBi and attributed the AFM and FM/FiM to two different atomic sites of Mn. The newly found materials can help interpret the structure-magnetism relation in HTP-MnBi and open a new way for investigating future MnBi permanent magnets.

Abstract: Recently, intriguing physical properties have been unraveled in anisotropic semiconductors, in which the in-plane electronic band structure anisotropy often originates from the low crystallographic symmetry. The atomic chain is the ultimate limit in material downscaling for electronics, a frontier for establishing an entirely new field of one-dimensional quantum materials. Electronic and structural properties of chain-like InTe are essential for better understanding of device applications such as thermoelectrics. Here, we use scanning tunneling microscopy/spectroscopy (STM/STS) measurements and density functional theory (DFT) calculations to directly image the in-plane structural anisotropy in tetragonal Indium Telluride (InTe). As results, we report the direct observation of one-dimensional In1+ chains in InTe. We demonstrate that InTe exhibits a band gap of about 0.40 +-0.02 eV located at the M point of the Brillouin zone. Additionally, line defects are observed in our sample, were attributed to In1+ chain vacancy along the c-axis, a general feature in many other TlSe-like compounds. Our STS and DFT results prove that the presence of In1+ induces localized gap state, located near the valence band maximum (VBM). This acceptor state is responsible for the high intrinsic p-type doping of InTe that we also confirm using angle-resolved photoemission spectroscopy.

Abstract: We study the ultrafast magnetization dynamics of bcc Fe and fcc Co using the recently suggested heat-conserving three-temperature model (HC3TM), together with atomistic spin- and lattice dynamics simulations. It is shown that this type of Langevin-based simulation is able to reproduce observed trends of the ultrafast magnetization dynamics of fcc Co and bcc Fe, in agreement with previous findings for fcc Ni. The simulations are performed by using parameters that to as large extent as possible are obtained from electronic structure theory. The one parameter that was not calculated in this way, was the damping term used for the lattice dynamics simulations, and here a range of parameters were investigated. It is found that this term has a large influence on the details of the magnetization dynamics. The dynamics of iron and cobalt is compared with previous results for nickel and similarities and differences in the materials' behavior are analysed following the absorption of a femtosecond laser pulse. Importantly, for all elements investigated so far with this model, we obtain a linear relationship between the value of the maximally demagnetized state and the fluence of the laser pulse, which is in agreement with experiments.

Abstract: Transduction of quantum information between distinct quantum systems is an essential step in various applications, including quantum networks and quantum computing. However, quantum transduction needs to mediate between photons with vastly different frequencies, making it challenging to design high-performance transducers, due to multifaceted and sometimes conflicting requirements. In this work, we first discuss some general principles for quantum transducer design, and then propose solid-state anti-ferromagnetic topological insulators to serve as highly effective transducers. First, topological insulators exhibit band-inversion, which can greatly enhance their optical responses. Coupled with their robust spin-orbit coupling and high spin density, this property leads to strong nonlinear interaction in topological insulators, thereby substantially improving transduction efficiency. Second, the anti-ferromagnetic order can minimize the detrimental influence on other neighboring quantum systems due to magnetic interactions. Using $\rm MnBi_2Te_4$ as an example, we showcase that unit transduction fidelity can be achieved with modest experimental requirements, while the transduction bandwidth can reach the GHz range. The strong nonlinear interaction in magnetic topological insulators can find diverse applications, including the generation of entanglement between photons of distinct frequencies.

Abstract: Recent experiments and calculations in topological semimetals have observed anomalously strong second-order optical nonlinearity, but yet whether the enhancement also occurs at surfaces of topological semimetals in general remains an open question. In this work, we tackle this problem by measuring polarization-dependent and rotational-anisotropy optical second harmonic generation (SHG) from centrosymmetric type-II Dirac semimetal PdTe$_2$. We found the SHG to follow C$_{3v}$ surface symmetry with a time-varying intensity dictated by the oxidation kinetics of the material after its surface cleavage, indicating the surface origin of SHG. Quantitative characterization of the surface nonlinear susceptibility indicates a large out-of-plane response of PdTe$_2$ with $|\chi_{ccc}^{(2)}|$ up to 25 $\times$ 10$^{-18}$ m$^2$/V. Our results support the topological surfaces/interfaces as a new route toward applications of nonlinear optical effects with released symmetry constraints, and demonstrate SHG as a viable means to in situ study of kinetics of topological surfaces.

Abstract: The inverse Faraday effect is an opto-magnetic phenomenon that describes the ability of circularly polarized light to induce magnetism in solids. The capability of light to control magnetic order in solid state materials and devices is of interest for a variety of applications, such as magnetic recording, quantum computation and spintronic technologies. However, significant gaps in understanding about the effect persist, such as what material properties govern the magnitude of the effect in metals. In this work, we report time-resolved measurements of the specular inverse Faraday effect in non-magnetic metals, i.e., the magneto-optic Kerr effect induced by circularly polarized light. We measure this specular inverse Faraday effect in Cu, Pd, Pt, W, Ta, and Au at a laser wavelength of 783 nm. For Ta and W, we investigate both {\alpha} and \{beta} phases. We observe that excitation of these metals with circularly polarized light induces significant circular dichroism. This nonlinear magneto-optical response to circularly polarized light is an order of magnitude larger in {\alpha}-W than other metals, e.g., Pt, Au, and is greater than nearly all other reported values for IFE in other materials. Our results benchmark the range of IFE that can be observed in non-magnetic metals and provide insight into what material properties govern the inverse Faraday effect in metals.

Abstract: Control of magnetism by an applied electric field is a desirable technique for the functionalization of magnetic materials. Motivated by recent experiments, we study the electric field control of the interfacial magnetism of CaRuO$_3$/CaMnO$_3$ (CRO/CMO) (001), a prototype interface between a non-magnetic metal and an antiferromagnetic insulator. Even without the electric field, the interfacial CMO layer acquires a ferromagnetic moment due to a spin-canted state, caused by the Anderson-Hasegawa double exchange (DEX) between the Mn moments and the leaked electrons from the CRO side. An electric field would alter the carrier density at the interface, leading to the possibility of controlling the magnetism, since DEX is sensitive to the carrier density. We study this effect quantitatively usingdensity-functional calculations in the slab geometry. We find a text-book like dielectric screening of the electric field, which introduces polarization charges at the interfaces and the surfaces. The extra charge at the interface enhances the ferromagnetism via the DEX interaction, while away from the interface the original AFM state of the Mn layers remains unchanged. The effect could have potential application in spintronics devices.

Abstract: We present a comprehensive study of the magnetocaloric effect (MCE) in a family of kagome magnets with formula RMn6Sn6 (R=Tb, Ho, Er, and Lu). These materials have a small rare-earth content and tunable magnetic ordering, hence they provide a venue to study the fundamentals of the MCE. We examine the effect of different types of order (ferromagnetic, ferrimagnetic, and antiferromagnetic) and the presence of a metamagnetic transition on the MCE. We extend the study to a high-entropy rare-earth alloys of the family, and conclude with several guidelines for enhancing the MCE in tunable magnetic materials with a small rare-earth content.

Abstract: Predicting quasicrystal structures is a multifaceted problem that can involve predicting a previously unknown phase, predicting the structure of an experimentally observed phase, or predicting the thermodynamic stability of a given structure. We survey the history and current state of these prediction efforts with a focus on methods that have improved our understanding of the structure and stability of known metallic quasicrystal phases. Advances in the structural modeling of quasicrystals, along with first principles total energy calculation and statistical mechanical methods that enable the calculation of quasicrystal thermodynamic stability, are illustrated by means of cited examples of recent work.