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At least 847 records · Page 47

Accelerating magnonic simulations with the pseudospectral Landau-Lifshitz equation

The pseudospectral Landau-Lifshitz (PS-LL) model can describe atomic-scale magnetic exchange interactions within a continuum framework. This is achieved by employing a convolution kernel that models the nonlocal interaction in a grid-independent manner. Even though the PS-LL was originally introduced to address atomic exchange, any nonlocal kernel can be modeled. In the field of magnonics, the dipole field is fundamental to describe the dispersion relation of magnons, the quasiparticle representation of angular momentum. Because dipole-dipole interactions are long-range, numerical approaches typically rely on convolutions. Here, we demonstrate that the PS-LL model can be used to perform magnonic simulations with a single convolution kernel derived from analytical solutions. We demonstrate a twofold increase in computational speed compared with the full dipole calculation. This approach is valid insofar as the excitations are linear, which is typically the case for magnons. Our results have the potential to accelerate magnonic research, particularly for the inverse design method, where several simulations must be performed to achieve the desired outcome.

Mathematics and computing↗

Full-dimensional quantum stereodynamics of the non-adiabatic quenching of OH(A2Σ+) by H2

Abstract The Born–Oppenheimer approximation, assuming separable nuclear and electronic motion, is widely adopted for characterizing chemical reactions in a single electronic state. However, the breakdown of the Born–Oppenheimer approximation is omnipresent in chemistry, and a detailed understanding of the non-adiabatic dynamics is still incomplete. Here we investigate the non-adiabatic quenching of electronically excited OH(A 2 Σ + ) molecules by H 2 molecules using full-dimensional quantum dynamics calculations for zero total nuclear angular momentum using a high-quality diabatic-potential-energy matrix. Good agreement with experimental observations is found for the OH(X 2 Π) ro-vibrational distribution, and the non-adiabatic dynamics are shown to be controlled by stereodynamics, namely the relative orientation of the two reactants. The uncovering of a major (in)elastic channel, neglected in a previous analysis but confirmed by a recent experiment, resolves a long-standing experiment–theory disagreement concerning the branching ratio of the two electronic quenching channels.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Manipulating chiral spin transport with ferroelectric polarization

A magnon is a collective excitation of the spin structure in a magnetic insulator and can transmit spin angular momentum with negligible dissipation. This quantum of a spin wave has always been manipulated through magnetic dipoles (that is, by breaking time-reversal symmetry). Here we report the experimental observation of chiral spin transport in multiferroic BiFeO 3 and its control by reversing the ferroelectric polarization (that is, by breaking spatial inversion symmetry). The ferroelectrically controlled magnons show up to 18% modulation at room temperature. The spin torque that the magnons in BiFeO 3 carry can be used to efficiently switch the magnetization of adjacent magnets, with a spin-torque efficiency comparable to the spin Hall effect in heavy metals. Utilizing such controllable magnon generation and transmission in BiFeO 3 , an all-oxide, energy-scalable logic is demonstrated composed of spin-orbit injection, detection and magnetoelectric control. In conclusion, our observations open a new chapter of multiferroic magnons and pave another path towards low-dissipation nanoelectronics.

36 MATERIALS SCIENCE↗

Extreme-ultraviolet spatiotemporal vortices via high harmonic generation

Spatiotemporal optical vortices (STOVs) are space–time structured light pulses with a unique topology that couples spatial and temporal domains and carry transverse orbital angular momentum (OAM). Up to now, their generation has been limited to the visible and infrared regions of the spectrum. During the last decade, it was shown that through the process of high-order harmonic generation, it is possible to upconvert spatial optical vortices that carry longitudinal OAM from the near-infrared into the extreme-ultraviolet (EUV), thereby producing vortices with distinct femtosecond and attosecond structure. In this work, we demonstrate theoretically and experimentally the generation of EUV spatiotemporal and spatiospectral vortices using near-infrared STOV driving laser pulses. Here, we use analytical expressions for focused STOVs to perform macroscopic calculations of high-order harmonic generation that are directly compared to the experimental results. As STOV beams are not eigenmodes of propagation, we characterize the highly charged EUV STOVs in both the near and far fields to show that they represent conjugated spatiotemporal and spatiospectral vortex pairs. Our work provides high-frequency light beams topologically coupled at the nanometre/attosecond scales domains with transverse OAM that could be suitable to explore electronic dynamics in magnetic materials, chiral media and nanostructures.

High-harmonic generation↗

Flat band separation and robust spin Berry curvature in bilayer kagome metals

Kagome materials have emerged as a setting for emergent electronic phenomena that encompass different aspects of symmetry and topology. It is debated whether the XV 6 Sn 6 kagome family (where X is a rare-earth element), a recently discovered family of bilayer kagome metals, hosts a topologically non-trivial ground state resulting from the opening of spin–orbit coupling gaps. These states would carry a finite spin Berry curvature, and topological surface states. Here we investigate the spin and electronic structure of the XV 6 Sn 6 kagome family. We obtain evidence for a finite spin Berry curvature contribution at the centre of the Brillouin zone, where the nearly flat band detaches from the dispersing Dirac band because of spin–orbit coupling. In addition, the spin Berry curvature is further investigated in the charge density wave regime of ScV 6 Sn 6 and it is found to be robust against the onset of the temperature-driven ordered phase. Utilizing the sensitivity of angle-resolved photoemission spectroscopy to the spin and orbital angular momentum, our work unveils the spin Berry curvature of topological kagome metals and helps to define its spectroscopic fingerprint.

36 MATERIALS SCIENCE↗

Mirror-symmetry violation in bound nuclear ground states

Conservation laws are deeply related to any symmetry present in a physical system. Analogously to electrons in atoms exhibiting spin symmetries, it is possible to consider neutrons and protons in the atomic nucleus as projections of a single fermion with an isobaric spin (isospin) of t = 1/2. Every nuclear state is thus characterized by a total isobaric spin T and a projection T z —two quantities that are largely conserved in nuclear reactions and decays. A mirror symmetry emerges from this isobaric-spin formalism: nuclei with exchanged numbers of neutrons and protons, known as mirror nuclei, should have an identical set of states, including their ground state, labelled by their total angular momentum J and parity π. In this work, we report evidence of mirror-symmetry violation in bound nuclear ground states within the mirror partners strontium-73 and bromine-73. We find that a J π = 5/2 - spin assignment is needed to explain the proton-emission pattern observed from the T = 3/2 isobaric-analogue state in rubidium-73, which is identical to the ground state of strontium-73. Therefore the ground state of strontium-73 must differ from its J π = 1/2 - mirror bromine-73. This observation offers insights into charge-symmetry-breaking forces acting in atomic nuclei.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Spin-mediated shear oscillators in a van der Waals antiferromagnet

Understanding how microscopic spin configuration gives rise to exotic properties at the macroscopic length scale has long been pursued in magnetic materials. One seminal example is the Einstein-de Haas effect in ferromagnets, in which angular momentum of spins can be converted into mechanical rotation of an entire object. However, for antiferromagnets without net magnetic moment, how spin ordering couples to macroscopic movement remains elusive. Here we observed a seesaw-like rotation of reciprocal lattice peaks of an antiferromagnetic nanolayer film, whose gigahertz structural resonance exhibits more than an order-of-magnitude amplification after cooling below the Neel temperature. Using a suite of ultrafast diffraction and microscopy techniques, we directly visualize this spin-driven rotation in reciprocal space at the nanoscale. This motion corresponds to interlayer shear in real space, in which individual micro-patches of the film behave as coherent oscillators that are phase-locked and shear along the same in-plane axis. Using time-resolved optical polarimetry, we further show that the enhanced mechanical response strongly correlates with ultrafast demagnetization, which releases elastic energy stored in local strain gradients to drive the oscillators. Finally, our work not only offers the first microscopic view of spin-mediated mechanical motion of an antiferromagnet but it also identifies a new route towards realizing high-frequency resonators up to the millimetre band, so the capability of controlling magnetic states on the ultrafast timescale can be readily transferred to engineering the mechanical properties of nanodevices.

36 MATERIALS SCIENCE↗

Terahertz electric-field-driven dynamical multiferroicity in SrTiO 3

The emergence of collective order in matter is among the most fundamental and intriguing phenomena in physics. In recent years, the dynamical control and creation of novel ordered states of matter not accessible in thermodynamic equilibrium is receiving much attention. The theoretical concept of dynamical multiferroicity has been introduced to describe the emergence of magnetization due to time-dependent electric polarization in non-ferromagnetic materials. In simple terms, the coherent rotating motion of the ions in a crystal induces a magnetic moment along the axis of rotation. Here we provide experimental evidence of room-temperature magnetization in the archetypal paraelectric perovskite SrTiO 3 due to this mechanism. We resonantly drive the infrared-active soft phonon mode with an intense circularly polarized terahertz electric field and detect the time-resolved magneto-optical Kerr effect. A simple model, which includes two coupled nonlinear oscillators whose forces and couplings are derived with ab initio calculations using self-consistent phonon theory at a finite temperature, reproduces qualitatively our experimental observations. A quantitatively correct magnitude was obtained for the effect by also considering the phonon analogue of the reciprocal of the Einstein–de Haas effect, which is also called the Barnett effect, in which the total angular momentum from the phonon order is transferred to the electronic one. Our findings show a new path for the control of magnetism, for example, for ultrafast magnetic switches, by coherently controlling the lattice vibrations with light.

36 MATERIALS SCIENCE↗

Signatures of chiral superconductivity in rhombohedral graphene

Chiral superconductors are unconventional superconducting states that break time-reversal symmetry spontaneously and typically feature Cooper pairing at non-zero angular momentum. Such states may host Majorana fermions and provide an important platform for topological physics research and fault-tolerant quantum computing. Despite intensive search and prolonged studies of several candidate systems, chiral superconductivity has remained elusive so far. Here we report the discovery of robust unconventional superconductivity in rhombohedral tetralayer and pentalayer graphene without moiré superlattice effects. We observed two superconducting states in the gate-induced flat conduction bands with T c up to 300 mK and charge density n e down to 2.4 ×10 11 cm −2 in five devices. Spontaneous time-reversal-symmetry breaking (TRSB) owing to orbital motion of the electron is found and several observations indicate the chiral nature of these superconducting states, including: (1) in the superconducting state, R xx shows magnetic hysteresis in varying out-of-plane magnetic field B ⊥ —absent from all other superconductors; (2) the superconducting states are robust against in-plane magnetic field and are developed within a spin-polarized and valley-polarized quarter-metal (QM) phase; (3) the normal states show anomalous Hall signals at zero magnetic field and magnetic hysteresis. Here, we also observed a critical B ⊥ of 1.4 T, higher than any graphene superconductivity, which indicates a strong-coupling superconductivity close to the Bardeen–Cooper–Schrieffer (BCS)–Bose–Einstein condensate (BEC) crossover. Our observations establish a pure carbon material for the study of topological superconductivity, with the promise to explore Majorana modes and topological quantum computing.

36 MATERIALS SCIENCE↗

Observing differential spin currents by resonant inelastic X-ray scattering

Controlling spin currents, that is, the flow of spin angular momentum, in small magnetic devices, is the principal objective of spin electronics, a main contender for future energy-efficient information technologies. A pure spin current has never been measured directly because the associated electric stray fields and/or shifts in the non-equilibrium spin-dependent distribution functions are too small for conventional experimental detection methods optimized for charge transport. Here we report that resonant inelastic X-ray scattering (RIXS) can bridge this gap by measuring the spin current carried by magnons—the quanta of the spin wave excitations of the magnetic order—in the presence of temperature gradients across a magnetic insulator. This is possible due to the sensitivity of the momentum- and energy-resolved RIXS intensity to minute changes in the magnon distribution under non-equilibrium conditions. Furthermore, we use the Boltzmann equation in the relaxation time approximation to extract transport parameters, such as the magnon lifetime at finite momentum, essential for the realization of magnon spintronics.

36 MATERIALS SCIENCE↗

Studying local Berry curvature in 2H-WSe 2 by circular dichroism photoemission utilizing crystal mirror plane

It was recently reported that circular dichroism in angle-resolved photoemission spectroscopy (CD-ARPES) can be used to observe the Berry curvature in 2H-WSe 2 . In that study, the mirror plane of the experiment was intentionally set to be perpendicular to the crystal mirror plane, such that the Berry curvature becomes a symmetric function about the experimental mirror plane. In the present study, we performed CD-ARPES on 2H-WSe 2 with the crystal mirror plane taken as the experimental mirror plane. Within such an experimental constraint, two experimental geometries are possible for CD-ARPES. The Berry curvature distributions for the two geometries are expected to be antisymmetric about the experimental mirror plane and exactly opposite to each other. Our experimental CD intensities taken with the two geometries were found to be almost opposite near the corners of the 2D projected hexagonal Brillouin zone (BZ) and were almost identical near the center of the BZ. This observation is well explained by taking the Berry curvature or the atomic orbital angular momentum (OAM) into account. The Berry curvature (or OAM) contribution to the CD intensities can be successfully extracted through a comparison of the CD-ARPES data for the two experimental geometries. Thus, the CD-ARPES experimental procedure described provides a method for mapping Berry curvature in the momentum space of topological materials, such as Weyl semimetals.

36 MATERIALS SCIENCE↗

Ultrafast optical observation of spin-pumping induced dynamic exchange coupling in ferromagnetic semiconductor/metal bilayer

Abstract Spin angular momentum transfer in magnetic bilayers offers the possibility of ultrafast and low-loss operation for next-generation spintronic devices. We report the field- and temperature- dependent measurements on the magnetization precessions in Co 2 FeAl/(Ga,Mn)As by time-resolved magneto-optical Kerr effect. Analysis of the effective Gilbert damping and phase shift indicates a clear signature of an enhanced dynamic exchange coupling between the two ferromagnetic (FM) layers due to the reinforced spin pumping at resonance. The temperature dependence of the dynamic exchange-coupling reveals a primary contribution from the ferromagnetism in (Ga,Mn)As.

30 DIRECT ENERGY CONVERSION↗

Element-specific visualization of dynamic magnetic coupling in a Co/Py bilayer microstructure

We present the element-specific and time resolved visualization of uniform ferromagnetic resonance excitations of a Permalloy (Py) disk–Cobalt (Co) stripe bilayer microstructure. The transverse high frequency component of the resonantly excited magnetization is sampled in the ps regime by a combination of ferromagnetic resonance (FMR) and scanning transmission X-ray microscopy (STXM-FMR) recording snapshots of the local magnetization precession of Py and Co with nanometer spatial resolution. The approach allows us to individually image the resonant dynamic response of each element, and we find that angular momentum is transferred from the Py disk to the Co stripe and vice versa at their respective resonances. The integral (cavity) FMR spectrum of our sample shows an unexpected additional third resonance. This resonance is observed in the STXM-FMR experiments as well. Our microscopic findings suggest that it is governed by magnetic exchange between Py and Co, showing for the Co stripe a difference in relative phase of the magnetization due to stray field influence.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Anisotropic MagnetoMemristance

Abstract In the last decade, nanoscale resistive devices with memory have been the subject of intense study because of their possible use in brain-inspired computing. However, operational endurance is one of the limiting factors in the adoption of such technology. For this reason, we discuss the emergence of current-induced memristance in magnetic materials, known for their durability. We show analytically and numerically that a single ferromagnetic layer can possess GHz memristance, due to a combination of two factors: a current-induced transfer of angular momentum (Zhang-Li torque) and the anisotropic magnetoresistance (AMR). We term the resulting effect the anisotropic magneto-memristance (AMM). We connect the AMM to the topology of the magnetization state, within a simple model of a one-dimensional annulus-shaped magnetic layer, confirming the analytical results with micromagnetic simulations for permalloy. Our results open a new path towards the realization of single-layer magnetic memristive devices operating at GHz frequencies.

97 MATHEMATICS AND COMPUTING↗

Unimolecular dissociation dynamics of electronically excited HCO(Ã 2 A"): rotational control of nonadiabatic decay

The photoinduced unimolecular decay of the electronically excited HCO(Ã 2 A") is investigated in a combined experimental–theoretical study. The molecule is excited to the (1, n 2 , 0) combination bands, which decay via Renner–Teller coupling to the ground electronic state. The rovibrational state distribution of the CO fragment was measured via the high-n Rydberg H-atom time-of-flight method and calculated using a wave packet method on an accurate set of potential energy surfaces. It is shown that the non-adiabatic decay rate is strongly modulated by the HCO rotational angular momentum, which leaves unique signatures in the product state distribution. Finally, the experimentally observed bimodal rotational distribution of the dominant CO(v = 0) fragment is likely due to decay of different vibronic states populated by the excitation and modulated by the excited state lifetime, which is in turn controlled by the parent rotational quantum number.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Predicting third-body collision efficiencies for water and other polyatomic baths

Low-pressure-limit microcanonical (collisional activation) and thermal rate constants are predicted using a combination of automated ab initio potential energy surface construction, classical trajectories, transition state theory, and a detailed energy- and angular-momentum-resolved collision kernel. Several systems are considered, including CH 4 (+M) and HO 2 (+M), with an emphasis on systems where experimental information is available for comparison. The a priori approach involves no adjustable parameters, and we show that the predicted thermal rate constants are in excellent agreement with experiments, with average deviations of less than 25%. Notably, the a priori approach is shown to perform equally well for atomic, diatomic, and polyatomic baths, including M = H 2 O, CO 2 , and “fuel” baths like M = CH 4 and NH 3 . Additionally, the utility of microcanonical rate constants for interpreting trends and inferring mechanistic details in the thermal kinetics is demonstrated.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Spiers Memorial Lecture: Theory of unimolecular reactions

One hundred years ago, at an earlier Faraday Discussion meeting, Lindemann presented a mechanism that provides the foundation for contemplating the pressure dependence of unimolecular reactions. Since that time, our ability to model and predict the kinetics of such reactions has grown in leaps and bounds through the synergy of ever more sophisticated experimental studies with increasingly high level theoretical analyses. Herein, this review begins with a brief historical overview of the progress from the Lindemann mechanism to the master equation, which now provides the cornerstone for most theoretical analyses. The current status of ab initio transition state theory based implementations of the master equation is then reviewed, beginning with a discussion of the energy resolved chemical conversion rates, followed by a review of the pressure dependence of the thermal kinetics. The latter discussion focusses on the collisional energy and angular momentum transfer rates as well as the complexities of non-thermal effects and of multiple-well multiple-channel reactions. The synergy with recent state-of-the-art experiments is used to motivate these discussions. Attempts to automate the calculations are also briefly reviewed. Throughout the discussion, we provide our perspective on current understanding and continuing challenges and opportunities. One key challenge relates to the coupling of sequences of reactions, which frequently leads to deviations from the classic presumption of thermal reactants.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Quantum dynamics of the temporary capture of light atoms by superfluid helium nanodroplets at very low collision energies (≈1–13 meV): the case of the hydrogen atom and its isotopes

The capture dynamics of a H atom and isotopic variants [D, T and Q (hypothetical isotope of mass equal to four times the mass of H)] by a superfluid helium nanodroplet (HeND) has been investigated theoretically. The HeND (T = 0.37 K) is ( 4 He) N=400 and a mean field quantum hybrid approach [TDDFT (helium) + quantum wave packet (H, D, T or Q)] at zero angular momentum, is used to explore a rather wide range of very low initial kinetic energies (E k,0 ≈ 10–150 K). The analysis of the capture mechanism shows the existence of a dynamical barrier and a dynamical minimum that play key roles to understand the time evolution of the capture, especially the former property. In general, the H atom shows a different behavior from the other isotopes, with the behavior of T and Q being very similar to each other and the D atom behaving inbetween H and T. Besides, it is worth noting that, in principle, at the very low initial kinetic energies considered only “short” and “long” lived atom⋯HeND collision complexes are formed, i.e., in the atom-helium nanodroplet collision only the temporary capture of the atom takes place. The different behaviors observed have been interpreted considering the faster motion of the H atom when colliding with ( 4 He) N=400 and the more quantum character of the H behavior both due to its significantly lower mass. As far as we know, this is the first quantum dynamics study carried out on the collision of light atoms with HeNDs at very low energies.

Sternberg, Michael [Argonne National Laboratory (A↗