arXiv subjects

Stuart S. P. Parkin

Publications and source records attributed to Stuart S. P. Parkin.

At least 55 records · Page 3Linked to original sources

arXiv2022

Generation of out-of-plane polarized spin current by spin swapping

The generation of spin currents and their application to the manipulation of magnetic states is fundamental to spintronics. Of particular interest are chiral antiferromagnets that exhibit properties typical of ferromagnetic materials even though they have negligible magnetization. Here, we report the generation of a robust spin current with both in-plane and out-of-plane spin polarization in epitaxial thin films of the chiral antiferromagnet Mn3Sn in proximity to permalloy thin layers. By employing temperature-dependent spin-torque ferromagnetic resonance, we find that the chiral antiferromagnetic structure of Mn3Sn is responsible for an in-plane polarized spin current that is generated from the interior of the Mn3Sn layer and whose temperature dependence follows that of this layer's antiferromagnetic order. On the other hand, the out-of-plane spin polarized spin current is unrelated to the chiral antiferromagnetic structure and is instead the result of scattering from the Mn3Sn/permalloy interface. We substantiate the later conclusion by performing studies with several other non-magnetic metals all of which are found to exhibit out-of-plane polarized spin currents arising from the spin swapping effect.

cond-mat.mtrl-sci↗

arXiv2022

Parallel spin-momentum locking in a chiral topological semimetal

Spin-momentum locking in solids describes a directional relationship between the electron's spin angular momentum and its linear momentum over the entire Fermi surface. While orthogonal spin-momentum locking, such as Rashba spin-orbit coupling, has been studied for decades and inspired a vast number of applications, its natural counterpart, the purely parallel spin-momentum locking, has remained elusive in experiments. Recently, chiral topological semimetals that host single- and multifold band crossings have been predicted to realize such parallel locking. Here, we use spin- and angle-resolved photoelectron spectroscopy to probe spin-momentum locking of a multifold fermion in the chiral topological semimetal PtGa via the spin-texture of its topological Fermi-arc surface states. We find that the electron spin of the Fermi-arcs points orthogonal to their Fermi surface contour for momenta close to the projection of the bulk multifold fermion, which is consistent with parallel spin-momentum locking of the latter. We anticipate that our discovery of parallel spin-momentum locking of multifold fermions will lead to the integration of chiral topological semimetals in novel spintronic devices, and the search for spin-dependent superconducting and magnetic instabilities in these materials.

cond-mat.mes-hall↗

arXiv2022

Scaling of Berry-curvature monopole dominated large linear positive magnetoresistance

The linear positive magnetoresistance (LPMR) is a widely observed phenomenon in topological materials, which is promising for potential applications on topological spintronics. However, its mechanism remains ambiguous yet and the effect is thus uncontrollable. Here, we report a quantitative scaling model that correlates the LPMR with the Berry curvature, based on a ferromagnetic Weyl semimetal CoS2 that bears the largest LPMR of over 500% at 2 Kelvin and 9 Tesla, among known magnetic topological semimetals. In this system, masses of Weyl nodes existing near the Fermi level, revealed by theoretical calculations, serve as Berry-curvature monopoles and low-effective-mass carriers. Based on the Weyl picture, we propose a relation \[\text{MR}=\frac{e}{\hbar }B{{Ω}_{\text{F}}}\], with B being the applied magnetic field and \[{{Ω}_{\text{F}}}\] the average Berry curvature near the Fermi surface, and further introduce temperature factor to both MR/B slope (MR per unit field) and anomalous Hall conductivity, which establishes the connection between the model and experimental measurements. A clear picture of the linearly slowing down of carriers, i.e., the LPMR effect, is demonstrated under the cooperation of the k-space Berry curvature and real-space magnetic field. Our study not only provides an experimental evidence of Berry curvature induced LPMR for the first time, but also promotes the common understanding and functional designing of the large Berry-curvature MR in topological Dirac/Weyl systems for magnetic sensing or information storage.

cond-mat.mtrl-sci↗

arXiv2022

Terahertz spin-to-charge current conversion in stacks of ferromagnets and the transition-metal dichalcogenide NbSe$_2$

Transition-metal dichalcogenides (TMDCs) are an aspiring class of materials with unique electronic and optical properties and potential applications in spin-based electronics. Here, we use terahertz emission spectroscopy to study spin-to-charge current conversion (S2C) in the TMDC NbSe$_2$ in ultra-high-vacuum-grown F|NbSe$_2$ thin-film stacks, where F is a layer of ferromagnetic Fe or Ni. Ultrafast laser excitation triggers an ultrafast spin current that is converted into an in-plane charge current and, thus, a measurable THz electromagnetic pulse. The THz signal amplitude as a function of the NbSe$_2$ thickness shows that the measured signals are fully consistent with an ultrafast optically driven injection of an in-plane-polarized spin current into NbSe$_2$. Modeling of the spin-current dynamics reveals that a sizable fraction of the total S2C originates from the bulk of NbSe$_2$ with the same, negative, sign as the spin Hall angle of pure Nb. By quantitative comparison of the emitted THz radiation from F|NbSe$_2$ to F|Pt reference samples and the results of ab-initio calculations, we estimate that the spin Hall angle of NbSe$_2$ for an in-plane polarized spin current lies between -0.2% and -1.1%, while the THz spin-current relaxation length is of the order of a few nanometers.

cond-mat.mes-hall↗

arXiv2022

Catalogue of Flat-Band Stoichiometric Materials

Topological electronic flatten bands near or at the Fermi level are a promising avenue towards unconventional superconductivity and correlated insulating states. However, the related experiments are mostly limited to the engineered materials, such as moire systems. Here we present a catalogue of all the three-dimensional stoichiometric materials with flat bands around the Fermi level that exist in nature. We consider 55,206 materials from the Inorganic Crystal Structure Database catalogued using the Topological Quantum Chemistry website which provides their structural parameters, space group (SG), band structure, density of states and topological characterization. We combine several direct signatures and properties of band flatness to a high-throughput analysis of all crystal structures. In particular, we identify materials hosting line-graph or bipartite sublattices - either in two or three dimensions - likely leading to flat bands. From this trove of information, we create the Materials Flatband Database website, a powerful search engine for future theoretical and experimental studies. We use it to extract a curated list of 2,379 materials, with among them 345 promising candidates, potentially hosting flat bands whose charge centers are not strongly localized on the atomic sites. We showcase five representative materials: KAg[CN]2 in SG 163 $(P\bar{3}1c)$, Pb2Sb2O7 in SG 227 $(Fd\bar{3}m)$, Rb2CaH4 in SG 139 $(I4/mmm)$, Ca2NCl in SG 166 $(R\bar{3}m)$ and WO3 in SG 221 $(Pm\bar{3}m)$. We provide a theoretical explanation for the origin of their flat bands close to the Fermi energy using the $S$-matrix method introduced in a parallel work [Calugaru et al., Nature Physics 18, 185 (2022)].

cond-mat.str-el↗

arXiv2022

All Topological Bands of All Nonmagnetic Stoichiometric Materials

Topological Quantum Chemistry and Symmetry-Based Indicators have facilitated large-scale searches for materials with topological properties at the Fermi energy ($E_{F}$). We report the completion of a publicly accessible catalog of stable and fragile topology in all of the bands both at and away from $E_{F}$ in the 96,196 processable entries in the Inorganic Crystal Structure Database. Our calculations represent the completion of the symmetry-indicated band topology of known nonmagnetic materials, and enable the discovery of repeat-topological and supertopological materials, which include rhombohedral bismuth and Bi$_2$Mg$_3$. We find that 52.65% of all materials are topological at $E_{F}$, roughly $2/3$ of bands across all materials exhibit symmetry-indicated stable topology, and that 87.99% of all materials contain at least one stable or fragile topological band.

cond-mat.mtrl-sci↗

arXiv2022

Realization of the field-free Josephson Diode

The superconducting analog to the semiconducting diode, the Josephson diode, has long been sought, with multiple avenues to realization proposed by theorists. Exhibiting magnetic-field free, single directional superconductivity with Josephson coupling of the supercurrent across a tunnel barrier, it would serve as the building-block for next-generation superconducting circuit technology. Here we realized the field-free Josephson diode using an inversion symmetry breaking heterostructure of $\mathrm{NbSe_2/Nb_3Br_8/NbSe_2}$. We demonstrate, for the first time without magnetic field, the junction can be superconducting in one direction while normal in the opposite direction. Based on that, half-wave rectification of a square-wave excitation was achieved with low switching current density ($~2.2\times 10^2 \mathrm{A/cm^2}$), high rectification ratio ($~10^4$) and high robustness (at least $10^4$ cycles). We also demonstrate symmetric $ΔI_\mathrm{c}$ (the difference between positive and negative critical currents) behavior with field and the expected Fraunhofer current phase relation of a Josephson junction. This realization raises fundamental questions about the Josephson effect through an insulator when breaking symmetry, and opens the door to ultralow power, high speed, superconducting circuits for logic and signal modulation.

cond-mat.supr-con↗

arXiv2022

Anomalous excitations of atomically crafted quantum magnets

High energy resolution spectroscopic studies of quantum magnets have proven to be extremely valuable in directly accessing magnetodynamics quantities, such as energy barriers, magnetic interactions, lifetime of excited states and fluctuations at the most fundamental level. Here, we explore the existence of a new flavor of low-energy spin-excitations for quantum spins coupled to an electron bath. In sharp contrast to the usual tunneling signature of two steps symmetrically centered around the Fermi level, we find a single step in the conductance. Combining time-dependent and many-body perturbation theories, magnetic field-dependent tunneling spectra are explained to be the result of an interplay between weak magnetic anisotropy energy, magnetic interactions and Stoner-like electron-hole excitations that are strongly dependent on the magnetic states of the studied nanostructures. We additionally map the evolution of the conductance peak in artificial nanostructures crafted atom-by-atom, which show clear evidence of spin-coupled behavior. The results are rationalized in terms of a non-collinear magnetic ground state and the dominance of ferro- and antiferromagnetic interactions. The atomically crafted nanomagnets offer an appealing model for the exploration of electrically pumped spin systems.

cond-mat.mes-hall↗

arXiv2022

Ultrafast manipulation of the NiO antiferromagnetic order via sub-gap optical excitation

Wide-band-gap insulators such as NiO offer the exciting prospect of coherently manipulating electronic correlations with strong optical fields. Contrary to metals where rapid dephasing of optical excitation via electronic processes occurs, the sub-gap excitation in charge-transfer insulators has been shown to couple to low-energy bosonic excitations. However, it is currently unknown if the bosonic dressing field is composed of phonons or magnons. Here we use the prototypical charge-transfer insulator NiO to demonstrate that 1.5 eV sub-gap optical excitation leads to a renormalised NiO band-gap in combination with a significant reduction of the antiferromagnetic order. We employ element-specific X-ray reflectivity at the FLASH free-electron laser to demonstrate the reduction of the upper band-edge at the O 1s-2p core-valence resonance (K-edge) whereas the antiferromagnetic order is probed via X-ray magnetic linear dichroism (XMLD) at the Ni 2p-3d resonance (L2-edge). Comparing the transient XMLD spectral line shape to ground-state measurements allows us to extract a spin temperature rise of 65 +/- 5 K for time delays longer than 400 fs while at earlier times a non-equilibrium spin state is formed. We identify transient mid-gap states being formed during the first 200 fs accompanied by a band-gap reduction lasting at least up to the maximum measured time delay of 2.4 ps. Electronic structure calculations indicate that magnon excitations significantly contribute to the reduction of the NiO band gap.

cond-mat.str-el↗

arXiv2021

Josephson diode effect from Cooper pair momentum in a topological semimetal

In the presence of an external magnetic field Cooper pairs in noncentrosymmetric superconductors can acquire finite momentum. Recent theory predicts that such finite-momentum pairing can lead to an asymmetric critical current, where a dissipationless supercurrent can flow along one direction but not the opposite. However, to date this has not been observed. Here we report the discovery of a giant Josephson diode effect (JDE) in Josephson junctions formed from a type II Dirac semimetal, NiTe2. A distinguishing feature is that the asymmetry in the critical current depends sensitively on the magnitude and direction of an applied magnetic field and achieves its maximum value of ~60% when the magnetic field is perpendicular to the current and is of the order of just 10 mT. Moreover the asymmetry changes sign several times with increasing field. These characteristic features are accounted for in a theoretical model based on finite-momentum Cooper pairing derived from spin-helical topological surface states, in an otherwise centrosymmetric system. The finite pairing momentum is further established, and its value determined, from the evolution of the interference pattern under an in-plane magnetic field. The observed giant magnitude of the asymmetry in critical current and the clear exposition of its underlying mechanism paves the way to building novel superconducting computing devices using the Josephson diode effect.

cond-mat.supr-con↗

arXiv2021

Obstructed surface states as the origin of catalytic activity in inorganic heterogeneous catalysts

The discovery of new catalysts that are efficient, sustainable, and low-cost is a major research endeavor for many industrial chemical processes. This requires an understanding and determination of the catalytic origins for the given catalysts, which still remains a challenge. Here we describe a novel method to identify new catalysts based on searching for crystalline symmetry-protected obstructed atomic insulators (OAIs) that have metallic surface states on otherwise semiconducting or insulating compounds. The Wannier charge centers in OAIs are pinned by symmetries at some empty Wyckoff positions so that surfaces that accommodate these sites are guaranteed to have metallic obstructed surface states (OSSs). Beyond the well-studied 2H-MoS2, we further verified our theory on the catalysts, 2H-MoTe2, and 1T'-MoTe2, whose catalytic active sites are consistent with our calculations of obstructed Wannier charge centers (OWCCs) and OSSs. In addition, we have predicted the location of catalytic active sites and confirmed these predictions by exploring the hydrogen evolution reaction on NiPS3 bulk single crystals, which we find to be one of the most promising new catalysts with high activity and, moreover, of low cost. Most importantly, we successfully identified several high-efficient catalysts just by considering the number of OWCCs and the crystal symmetry of the OAIs. Using the real space invariant theory and high-throughput computational methods applied to a database of 34013 topologically trivial insulators, we have identified 1788 unique OAIs (3383 ICSDs), of which 465 are potential high-quality catalysts for heterogeneous reactions. The Miller indices of the active surfaces are also obtained. Our new methodology will facilitate and accelerate the discovery of new catalysts for a wide range of heterogeneous redox reactions, where sustainability, toxicity, and cost must be considered.

cond-mat.mtrl-sci↗

arXiv2021

Role of two-dimensional Ising superconductivity in the non-equilibrium quasiparticle spin-to-charge conversion efficiency

Non-equilibrium studies of two-dimensional (2D) superconductors (SCs) with Ising spin-orbit coupling are prerequisite for their successful application to equilibrium spin-triplet Cooper pairs and, potentially, Majorana fermions. By taking advantage of the recent discoveries of 2D SCs and their compatibility with any other materials, we fabricate here non-local magnon devices to examine how such 2D Ising superconductivity affects the conversion efficiency of magnon spin to quasiparticle charge in superconducting flakes of 2H-NbSe2 transferred onto ferrimagnetic insulating Y3Fe5O12. Comparison with a reference device based on a conventionally paired superconductor shows that the Y3Fe5O12-induced in-plane (IP) exchange spin-splitting in the NbSe2 flake is hindered by its inherent out-of-plane (OOP) spin-orbit-field, which, in turn, limits the transition-state enhancement of the spin-to-charge conversion efficiency. Our out-of-equilibrium study highlights the significance of symmetry matching between underlying Cooper pairs and exchange-induced spin-splitting for the giant transition-state spin-to-charge conversion and may have implications towards proximity-engineered spin-polarized triplet pairing via tuning the relative strength of IP exchange and OOP spin-orbit fields in ferromagnetic insulator/2D Ising SC bilayers.

cond-mat.supr-con↗

arXiv2021

Long range and highly tunable interaction between local spins coupled to a superconducting condensate

Interfacing magnetism with superconducting condensates is rapidly emerging as a viable route for the development of innovative quantum technologies. In this context, the development of rational design strategies to controllably tune the interaction between magnetic moments is crucial. In the metallic regime, the indirect interaction mediated by conduction electrons, the so-called RKKY coupling, has been proven to be remarkably fertile in creating and controlling magnetic phenomena. However, despite its potential, the possibility of using superconductivity to control the sign and the strength of indirect interactions between magnet moments remains largely unexplored. Here we address this problem at its ultimate limit, demonstrating the possibility of maximally tuning the interaction between local spins coupled through a superconducting condensate with atomic scale precision. By using Cr atoms coupled to superconducting Nb as a prototypical system, we use atomic manipulation techniques to precisely control the relative distance between local spins along different crystallographic directions while simultaneously sensing their coupling by scanning tunneling spectroscopy. Our results reveal the existence of highly anisotropic superconductor-mediated indirect couplings between the local spins, lasting up to very long distances, up to 12 times the lattice constant of Nb. Moreover, we demonstrate the possibility of controllably crossing a quantum phase transition by acting on the direction and interatomic distance between spins. The extremely high tunability provides novel opportunities for the realization of exotic phenomena such as topological superconductivity and the rational design of magneto-superconducting interfaces.

cond-mat.supr-con↗

arXiv2021

Atomic scale control of spin current transmission at interfaces

Spin transmission at ferromagnet/heavy metal interfaces is of vital importance for many spintronic devices. Usually the spin current transmission is limited by the spin mixing conductance and loss mechanisms such as spin memory loss. In order to understand these effects, we study the interface transmission when an insulating interlayer is inserted between the ferromagnet and the heavy metal. For this we measure the inverse spin Hall voltage generated from optically injected spin current pulses as well as the magnitude of the spin pumping using ferromagnetic resonance. From our results we conclude that significant spin memory loss only occurs for 5d metals with less than half filled d-shell.

cond-mat.mes-hall↗

arXiv2021

Filling-Enforced Obstructed Atomic Insulators

Topological band theory has achieved great success in the high-throughput search for topological band structures both in paramagnetic and magnetic crystal materials. However, a significant proportion of materials are topologically trivial insulators at the Fermi level. In this paper, we show that, remarkably, for a subset of the topologically trivial insulators, knowing only their electron number and the Wyckoff positions of the atoms we can separate them into two groups: the obstructed atomic insulator (OAI) and the atomic insulator (AI). The interesting group, the OAI, have a center of charge not localized on the atoms. Using the theory of topological quantum chemistry, in this work we first derive the necessary and sufficient conditions for a topologically trivial insulator to be a filling enforced obstructed atomic insulator (feOAI) in the 1651 Shubnikov space groups. Remarkably, the filling enforced criteria enable the identification of obstructed atomic bands without knowing the representations of the band structures. Hence, no ab-initio calculations are needed for the filling enforced criteria, although they are needed to obtain the band gaps. With the help of the Topological Quantum Chemistry website, we have performed a high-throughput search for feOAIs and have found that 957 ICSD entries (638 unique materials) are paramagnetic feOAIs, among which 738 (475) materials have an indirect gap. The metallic obstructed surface states of feOAIs are also showcased by several material examples.

cond-mat.mtrl-sci↗

arXiv2021

Correlating Josephson supercurrents and Shiba states in quantum spins unconventionally coupled to superconductors

Local spins coupled to superconductors give rise to several emerging phenomena directly linked to the competition between Cooper pair formation and magnetic exchange. These effects are generally scrutinized using a spectroscopic approach which relies on detecting the in-gap bound modes arising from Cooper pair breaking, the so-called Yu-Shiba-Rusinov (YSR) states. However, the impact of local magnetic impurities on the superconducting order parameter remains largely unexplored. Here, we use scanning Josephson spectroscopy to directly visualize the effect of magnetic perturbations on Cooper pair tunneling between superconducting electrodes at the atomic scale. By increasing the magnetic impurity orbital occupation by adding one electron at a time, we reveal the existence of a direct correlation between Josephson supercurrent suppression and YSR states. Moreover, in the metallic regime, we detect zero bias anomalies which break the existing framework based on competing Kondo and Cooper pair singlet formation mechanisms. Based on first-principle calculations, these results are rationalized in terms of unconventional spin-excitations induced by the finite magnetic anisotropy energy. Our findings have far reaching implications for phenomena that rely on the interplay between quantum spins and superconductivity.

cond-mat.supr-con↗

arXiv2020

Fermi surface chirality induced in a TaSe$_{2}$ monosheet formed by a Ta/ Bi$_{2}$Se$_{3}$ interface reaction

Spin-momentum locking in topological insulators and materials with Rashba-type interactions is an extremely attractive feature for novel spintronic devices and is therefore under intense investigation. Significant efforts are underway to identify new material systems with spin-momentum locking, but also to create heterostructures with new spintronic functionalities. In the present study we address both subjects and investigate a van der Waals-type heterostructure consisting of the topological insulator Bi$_{2}$Se$_{3}$ and a single Se-Ta-Se triple-layer (TL) of H-type TaSe$_{2}$ grown by a novel method which exploits an interface reaction between the adsorbed metal and selenium. We then show, using surface x-ray diffraction, that the symmetry of the TaSe2-like TL is reduced from D$_{3h}$ to C$_{3v}$ resulting from a vertical atomic shift of the tantalum atom. Spin- and angle-resolved photoemission indicates that, owing to the symmetry lowering, the states at the Fermi surface acquire an in-plane spin component forming a surface contour with a helical Rashba-like spin texture, which is coupled to the Dirac cone of the substrate. Our approach provides a new route to realize novel chiral two-dimensional electron systems via interface engineering that do not exist in the corresponding bulk materials.

cond-mat.mes-hall↗

arXiv2020

Size scaling, dynamics, and electro-thermal bifurcation of VO2 Mott oscillators

Traditional electronic devices are well-known to improve in speed and energy-efficiency as their dimensions are reduced to the nanoscale. However, this scaling behavior remains unclear for nonlinear dynamical circuit elements, such as Mott neuron-like spiking oscillators, which are of interest for bio-inspired computing. Here we show that shrinking micrometer-sized VO2 oscillators to sub-100 nm effective sizes, achieved using a nanogap cut in a metallic carbon nanotube (CNT) electrode, does not guarantee faster spiking. However, an additional heat source such as Joule heating from the CNT, in combination with small size and heat capacity (defined by the narrow volume of VO2 whose insulator-metal transition is triggered by the CNT), can increase the spiking frequency by ~1000x due to an electro-thermal bifurcation in the nonlinear dynamics. These results demonstrate that nonlinear dynamical switches operate in a complex phase space which can be controlled by careful electro-thermal design, offering new tuning parameters for designing future biomimetic electronics.

cond-mat.mtrl-sci↗