Ultrafast Magnetization Dynamics Research Articles

Coupled atomistic spin-lattice simulations of ultrafast demagnetization in 3d ferromagnets.

Despite decades of research, the role of the lattice and its coupling to the magnetisation during ultrafast demagnetisation processes is still not fully understood. Here we report on studies of both explicit and implicit lattice effects on laser induced ultrafast demagnetisation of bcc Fe and fcc Co. We do this using atomistic spin- and lattice dynamics simulations following a heat-conserving three-temperature model. We show that this type of Langevin-based simulation is able to reproduce observed trends of the ultrafast magnetization dynamics of fcc Co and bcc Fe. The parameters used in our models are all obtained from electronic structure theory, with the exception of the lattice dynamics damping term, where a range of parameters were investigated. It was found that while the explicit spin-lattice coupling in the studied systems does not impact the demagnetisation process notably, the lattice damping has a large influence on the details of the magnetization dynamics. The dynamics of Fe and Co following the absorption of a femtosecond laser pulse are compared with previous results for Ni and similarities and differences in the materials' behavior are analysed. 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. Moreover, we demonstrate that the demagnetization amplitude is largest for Ni and smallest for Co. This holds over a wide range of the reported electron-phonon couplings, and this demagnetization trend is in agreement with recent experiments.

Direct versus indirect excitation of ultrafast magnetization dynamics in FeNi alloys

Direct versus indirect excitation of ultrafast magnetization dynamics in FeNi alloys

Terahertz Laser Pulse Boosts Interlayer Spin Transfer in Two-Dimensional van der Waals Magnetic Heterostructures.

Light-induced ultrafast dynamics in two-dimensional (2D) magnetic systems demonstrate substantial advancements in spintronics. Here, using the real-time time-dependent density functional theory (rt-TDDFT), we applied laser pulses with various frequencies, from terahertz (THz) to optical pulse, to systematically study the interlayer spin transfer dynamics in 2D van der Waals nonmagnetic-ferromagnetic heterostructures, including graphene-Fe3GeTe2 (Gr/FGT) and silicene-Fe3GeTe2 (Si/FGT). Our results demonstrate that low-frequency THz pulses are particularly effective in facilitating interlayer spin injection from the ferromagnetic FGT layers to the Si or Gr layers. On the contrary, high-frequency optical pulses exhibit a minimal influence on this process. Such an effect is attributed to the low-frequency THz pulses inducing in-phase oscillations of the electron charge density around atomic centers, leading to a highly efficient interlayer spin transfer. Our results provide a new insight into ultrafast THz radiation control intralayer spin transfer and magnetic proximity dynamics in the 2D limit.

Tunable Tesla-Scale Magnetic Attosecond Pulses through Ring-Current Gating.

Coherent control over electron dynamics in atoms and molecules using high-intensity circularly polarized laser pulses gives rise to current loops, resulting in the emission of magnetic fields. We propose, and demonstrate with ab initio calculations, "current-gating" schemes to generate direct or alternating-current magnetic pulses in the infrared spectral region, with highly tunable waveform and frequency, and showing femtosecond-to-attosecond pulse duration. In optimal conditions, the magnetic pulse can be highly isolated from the driving laser and exhibits a high flux density (∼1 T at a few hundred nanometers from the source, with a pulse duration of 787 attoseconds) for application in forefront experiments of ultrafast spectroscopy. Our work paves the way toward the generation of attosecond magnetic fields to probe ultrafast magnetization, chiral responses, and spin dynamics.

Real-time observation of magnetization and magnon dynamics in a two-dimensional topological antiferromagnet MnBi2Te4

Atomically thin van der Waals magnetic materials have not only provided a fertile playground to explore basic physics in the two-dimensional (2D) limit but also created vast opportunities for novel ultrafast functional devices. Here we systematically investigate ultrafast magnetization dynamics and spin wave dynamics in few-layer topological antiferromagnetic MnBi2Te4 crystals as a function of layer number, temperature, and magnetic field. We find laser-induced (de)magnetization processes can be used to accurately track the distinct magnetic states in different magnetic field regimes, including showing clear odd–even layer number effects. In addition, strongly field-dependent AFM magnon modes with tens of gigahertz frequencies are optically generated and directly observed in the time domain. Remarkably, we find that magnetization and magnon dynamics can be observed in not only the time-resolved magneto-optical Kerr effect but also the time resolved reflectivity, indicating strong correlation between the magnetic state and electronic structure. These measurements present the first comprehensive overview of ultrafast spin dynamics in this novel 2D antiferromagnet, paving the way for potential applications in 2D antiferromagnetic spintronics and magnonics as well as further studies of ultrafast control of both magnetization and topological quantum states.

Investigation of the Ultrafast Magnetic Dynamics in Co/Pt Multilayer Structures and Examples of Other Studies at the European XFEL Facility

Investigation of the Ultrafast Magnetic Dynamics in Co/Pt Multilayer Structures and Examples of Other Studies at the European XFEL Facility

An integrated ultra-high vacuum cluster for atomic-scale deposition, interface regulation, and characterization of spintronic multilayers

The study of interface spin effects in spintronic multilayer films requires distinguishing the effects generated by different interfaces. However, testing in atmospheric conditions requires a capping layer to protect the films, which introduces new interfaces and limits the study of interface spin-dependent effects. To address this challenge, we have developed an integrated ultra-high vacuum cluster system that includes magnetron sputtering equipment, ion irradiation equipment, and time-resolved magneto-optical Kerr effect (TR-MOKE) equipment. Our sputtering system integrates 12 cathodes in a single chamber, allowing the co-sputtering of four targets. The ultimate vacuum can reach 1 × 10−10 mbar, and the deposition resolution of 0.1 nm can be achieved. Ion irradiation equipment can ionize to produce He+, and by screening and accelerating the implantation of He+ into multilayer films, ion scanning is realized, and up to 30 keV energy can be applied to the films. The TR-MOKE equipment can detect ultra-fast magnetic dynamics processes in vacuum conditions, and its external magnetic field can be rotated 360°. Our vacuum cluster system connects the three subsystems, allowing in situ film deposition, regulation, and characterization. By accurately detecting the effects of different layers, the system can distinguish the interface effects of multilayers. Experimental results demonstrate that the three subsystems can work independently or coordinate to observe the interface effects of multilayers.

Comparative study of femtosecond laser-induced ultrafast magnetization dynamics in soft ferromagnetic ultra-thin alloy

The typical demagnetization mechanism is applicable in magneto-optic recording systems on a nanoseconds timescale. Interest in this area has expanded rapidly since understanding the physics of ultrafast magnetization processes by experiment are an acutely challenging task. As a result, in order to explain the quenching of magnetization by laser heating in ferromagnetic alloys such as permalloy, we executed a new theoretical study on permalloy, as well as Ni and Fe ultra-thin films with thickness varying from 1 nm to 5 nm. In particular, we demonstrate that the magnetization decays in a timescale of about 0.1 picosecond by the microscopic three-temperature model. Our free electron model-based theoretical model represents that electron–phonon coupling coefficient and demagnetization time in the thin-films are strongly sensitive to film thickness, pulse duration and laser fluence, respectively. In particular, we show that the rapid demagnetization (100 fs) is due to electron-magnon excitation. This feature improves data processing speed in communication systems and the recording industry.

A two-color dual-comb system for time-resolved measurements of ultrafast magnetization dynamics using triggerless asynchronous optical sampling.

We report on an Er-doped fiber (EDF)-laser-based dual-comb system that allows us to perform triggerless asynchronous optical sampling pump-probe measurements of ultrafast demagnetization and spin precession in magnetic materials. Because the oscillation frequencies of the two frequency-comb light sources are highly stabilized, the pulse-to-pulse timing jitter is sufficiently suppressed, and data accumulation without any trigger signals is possible. To effectively induce spin precession in ferromagnetic thin films, the spectral bandwidth of the output of one of the EDF frequency comb sources is broadened by a highly nonlinear fiber and then amplified at a wavelength of about 1030nm by a Yb-doped fiber amplifier. The output of the other frequency comb source is converted to about 775nm by second harmonic generation. We used this system to observe ultrafast demagnetization and spin precession dynamics on the picosecond and nanosecond time scales in a permalloy thin film. This time-domain spectroscopy system is promising for the rapid characterization of spin-wave generation and propagation dynamics in magnetic materials.

Tailoring the magneto-electronic and optical properties of cobalt doped strontium titanate by first-principles calculations

Ferromagnetic semiconductors or half metals offer strategic advantage in spintronic applications due to their robust stray fields and ultrafast magnetic dynamics. Controlling their magnetization and readout of their magnetic state are essential for these applications but remain challenging. Herein, we present a density functional theory (DFT) based full potential linearized augmented plane wave (FP-LAPW) analysis of the magneto-optical properties of novel and most widely studied diamagnetic SrTiO3 (STO) doped with cobalt. Pure STO is non-magnetic wide band gap (3.25 eV) semiconductor. Our study shows that versatile transport and magnetic properties can be obtained in CoxSr1-xTiO3, ranging from magnetic semiconductor to half metallic ferromagnetic nature depending upon the dopant's concentration. Spin resolved electronic properties and non-zero values of calculated magnetic moments for doped supercells reveal that Co0·125Sr0·875TiO3 and Co0·25Sr0·75TiO3 are good DMSs while Co0·5Sr0·5TiO3 and Co0·75Sr0·25TiO3 are half metallic ferromagnets. The analysis of band structures and density of states reveal that partially filled Co-3d and O-2p states show hybridization. Moreover, calculated optical conductivity lie in the visible region of the order of 103 (Ω cm)−1 while reflectivity in this region is minimum. Our findings demonstrate Co doping as a powerful approach to control the magneto-optoelectronic physics in STO, which will stimulate further experimental research with promise for tailored magnetic and optoelectronic properties in Co doped STO systems.

Ultrafast magnetization reversal in ferromagnetic spin valves: An s−d model perspective

We present an extension to simple s-d models, aiming at simulating ultrafast magnetization dynamics and spin transport in metallic heterostructures. In particular, we consider an alternative spin dissipation channel due to a finite exchange splitting of the s band. From this theory, we show three different mechanisms governing the dynamics of spin accumulation. On top of the already widely discussed "-dM/dt" electron-magnon mechanism, we study the role of a dynamic change of exchange splitting (of conduction electrons) as well as the rotation of spins reflected at an interface with a ferromagnet. Finally, we use the presented theory to explain the recent observation of subpicosecond reversal of a ferromagnet in rare-earth free spin-valves. Our conclusion agrees with the one of reference [1] favoring magnetization reversal due to the rotation of the spin polarization of a reflected spin current.

Magneto-ionic Control of Ferrimagnetic Order by Oxygen Gating.

Ferrimagnets are considered an excellent spintronic material candidate which combines ultrafast magnetic dynamics and straightforward electrical detectability. However, efficient routes toward magneto-ionic control of ferrimagnetic order remain elusive. In this study, a solid-state oxygen gating device was designed to control the magnetic properties of the ferrimagnetic CoTb alloy. Experimental results show that applying a small voltage can irreversibly tune a Tb-dominant device to a stable Co-dominant state and decrease the magnetization compensation temperature by 130 K. In addition, a reversible voltage control of the magnetization axis between out-of-plane and in-plane states is observed, which indicates that the migrated oxygen ions can bond to both Tb and Co sublattices. First-principles calculations indicate that voltage can dynamically control the flow-in and flow-out of oxygen ions that bond to the Co sublattice. Our work provides an effective means to manipulate ferrimagnetic order and contributes to the development of ultra-low-power spintronic devices.

Interlayer coupling-dependent magnetoelastic response in synthetic antiferromagnets

In recent years, antiferromagnetic materials have been attracting increasing interest for their stability in high magnetic fields and ultrafast magnetization dynamics. Since the energy scale of an interlayer exchange coupling (IEC) in a synthetic antiferromagnet (SAF) consisting of ferromagnetic/nonmagnetic/ferromagnetic multilayers is relatively smaller than that of an exchange coupling in antiferromagnetic materials, magnetic ordering of a SAF can be potentially controlled by an electric field, which is promising for energy-saving spintronic memory devices. However, an electric field-induced magnetoelastic response of SAFs on ferroelectric materials has not been sufficiently understood due to the presence of IEC that complicates magnetization dynamics. In this study, we prepare Co/Ru/Co SAFs with various amplitude of IEC on ferroelectric Pb(Mg1/3Nb2/3)O3-PbTiO3 substrates and systematically investigate their electric field-induced magnetoelastic response. We demonstrate that the magnetoelastic response disappears at the boundary where a switching between the antiferromagnetic and ferromagnetic IEC coupling occurs. The result provides insight into the coupling of the magnetoelastic effect and IEC and is useful in designing spintronic memory devices based on SAFs.

Light-Induced Phonon-Mediated Magnetization in Monolayer MoS2

Light-induced ultrafast spin dynamics in materials is of great importance for developments of spintronics and magnetic storage technology. Recent progresses include ultrafast demagnetization, magnetic switching, and magnetic phase transitions, while the ultrafast generation of magnetism is hardly achieved. Here, a strong light-induced magnetization (up to 0.86μ B per formula unit) is identified in non-magnetic monolayer molybdenum disulfide (MoS2). With the state-of-the-art time-dependent density functional theory simulations, we demonstrate that the out-of-plane magnetization can be induced by circularly polarized laser, where chiral phonons play a vital role. The phonons strongly modulate spin-orbital interactions and promote electronic transitions between the two conduction band states, achieving an effective magnetic field ∼ 380 T. Our study provides important insights into the ultrafast magnetization and spin-phonon coupling dynamics, facilitating effective light-controlled valleytronics and magnetism.

Microscopic insights to spin transport-driven ultrafast magnetization dynamics in a Gd/Fe bilayer.

Laser-induced spin transport is a key ingredient in ultrafast spin dynamics. However, it remains debated to what extent ultrafast magnetization dynamics generates spin currents and vice versa. We use time- and spin-resolved photoemission spectroscopy to study an antiferromagnetically coupled Gd/Fe bilayer, a prototype system for all-optical switching. Spin transport leads to an ultrafast drop of the spin polarization at the Gd surface, demonstrating angular-momentum transfer over several nanometers. Thereby, Fe acts as spin filter, absorbing spin majority but reflecting spin minority electrons. Spin transport from Gd to Fe was corroborated by an ultrafast increase of the Fe spin polarization in a reversed Fe/Gd bilayer. In contrast, for a pure Gd film, spin transport into the tungsten substrate can be neglected, as spin polarization stays constant. Our results suggest that ultrafast spin transport drives the magnetization dynamics in Gd/Fe and reveal microscopic insights into ultrafast spin dynamics.

The Phenomenological Models for Ultrafast Magnetization Dynamics

We study ultrafast magnetization dynamics induced by laser heating using various phenomenological temperature models. The temperature dynamics of the electrons, spins and lattice for thin foils is investigated. Numerical results for the temperature and magnetization dynamics for them are compared with those available in the literature.

Ultrafast heat-assisted magnetization dynamics in a ferrimagnetic insulator

Ultrafast laser-induced heating of ferrimagnetic iron garnet in an external magnetic field triggers magnetization precessional dynamics with a large amplitude. The dynamics is studied as a function of magnetic field, laser fluence, and sample temperature. Exploring the three-dimensional space of these parameters experimentally and computationally, we identify the conditions for which the amplitude of the precession is the largest and even achieves values sufficient for magnetic recording. We found that the range of external magnetic fields and temperatures, which corresponds to the magnetic recording, is rather narrow. Modeling the dynamics, using magnetization as a macroscopic parameter, reveals that this range of parameters is defined by the optimal height of the potential barrier separating two stable states. The barrier needs to be low enough to allow the switching but not so low that the stability of the states is lost.

Evidence of electron-phonon mediated spin flip as driving mechanism for ultrafast magnetization dynamics in 3d ferromagnets

Despite intense experimental effort, theoretical proposals, and modeling approaches, a lack of consensus exists about the intrinsic mechanisms driving ultrafast magnetization dynamics in $3d$ ferromagnets. In this Letter, we find evidence of an electron-phonon mediated spin flip as the driving mechanism for the ultrafast magnetization dynamics in all three $3d$ ferromagnets: nickel, iron, and cobalt. We use a microscopic three-temperature model with parameters calculated from first principles, which has been validated by a direct comparison to the electron and lattice dynamics extracted from previous experiments. By a direct comparison to the experimentally measured magnetization dynamics for different laser fluences, we determine the spin-flip probability of each material. We find robust evidence that relatively small values of the spin-flip probability enable ultrafast demagnetization in all three $3d$ ferromagnets.

Ultrafast magnetization and energy flow in the laser-induced dynamics of transition metal compounds

An electronic theory of the laser-induced ultrafast magnetization dynamics in transition-metal alloys is presented. A many-body model Hamiltonian is considered that incorporates the fundamental electronic hopping, local Coulomb interaction, and spin-orbit coupling (SOC) on the same footing. Exact time propagations are performed on a tetrahedral cluster, from which the time dependencies of the local spin moments, orbital occupations, and single-particle energies of homogeneous systems and binary alloys are obtained. The consequences of inhomogeneities in the laser absorption and in the SOC strengths are investigated giving emphasis to the nature of spin-density transfers between the alloy components. A local perspective on the optically induced spin transfer is proposed in terms of which two main steps emerge: a dominantly local optical excitation followed by hopping-driven spin-density transfers among the different alloy components. The conjoint action of the spin-orbit interactions at the origin of local spin flips and spin-to-orbital angular-momentum transfer and the interatomic hoppings responsible for charge, spin, and energy flows between different sublattices is demonstrated. Transient and steady-state dynamical regimes are identified that result in delays in the onset of the local demagnetizations and in ultrafast redistributions of the spin. The central role of electron delocalization and electronic hopping in the spin-density redistribution and demagnetization of the different alloy components is demonstrated.

Ferrimagnets for spintronic devices: From materials to applications

Spintronic devices use spin instead of charge to process information and are widely considered as promising candidates for next-generation electronic devices. In past decades, the main motivation in spintronics has been to discover new mechanisms and novel material systems to improve both device performance and the application prospects of spintronics. Recently, researchers have found that ferrimagnetic materials—in which sublattices are coupled antiferromagnetically—offer an emerging platform for realizing high-density, high-speed, and low-power-consumption memory and logic functions. Within such a ferrimagnetic class, vanishing magnetization and ultrafast magnetic dynamics can be achieved by adjusting chemical composition and temperature, among other parameters. Meanwhile, unlike for antiferromagnets, conventional electrical read–write methods remain suitable for ferrimagnets, which is beneficial for applications. In this review, an abundant class of ferrimagnets including oxides and alloys is surveyed, and unique magnetic dynamics and effective methods for manipulating the magnetic states of ferrimagnets are discussed. Finally, novel storage and computing devices based on ferrimagnets are considered, as there are some challenges to be addressed in future applications of ferrimagnets.