Time-resolved Magneto-optical Kerr Effect Research Articles

Speed limits of the laser-induced phase transition in FeRh

We use ultrafast x-ray diffraction and the polar time-resolved magneto-optical Kerr effect to study the laser-induced metamagnetic phase transition in two FeRh films with thicknesses below and above the optical penetration depth. In the thin film, we identify an intrinsic timescale for the light-induced nucleation of ferromagnetic (FM) domains in the antiferromagnetic material of 8ps, which is substantially longer than the time it takes for strain waves to traverse the film. For the inhomogeneously excited thicker film, only the optically excited near-surface part transforms within 8ps. For strong excitations, we observe an additional slow rise of the FM phase, which we experimentally relate to a growth of the FM phase into the depth of the layer by comparing the transient magnetization in frontside and backside excitation geometry. In the lower lying parts of the film, which are only excited via near-equilibrium heat transport, the FM phase emerges significantly slower than 8ps after heating above the transition temperature.

Evidence of Ferromagnetism and Ultrafast Dynamics of Demagnetization in an Epitaxial FeCl2 Monolayer.

The development of two-dimensional (2D) magnetism is driven not only by the interest of low-dimensional physics but also by potential applications in high-density miniaturized spintronic devices. However, 2D materials possessing a ferromagnetic order with a relatively high Curie temperature (Tc) are rare. In this paper, the evidence of ferromagnetism in monolayer FeCl2 on Au(111) surfaces, as well as the interlayer antiferromagnetic coupling of bilayer FeCl2, is characterized by using spin-polarized scanning tunneling microscopy. A Curie temperature (Tc) of ∼147 K is revealed for monolayer FeCl2, based on our static magneto-optical Kerr effect measurements. Furthermore, temperature-dependent magnetization dynamics is investigated by the time-resolved magneto-optical Kerr effect. A transition from one- to two-step demagnetization occurs as the lattice temperature approaches Tc, which supports the Elliott-Yafet spin relaxation mechanism. The findings contribute to a deeper understanding of the underlying mechanisms governing ultrafast magnetization in 2D ferromagnetic materials.

Terahertz electric-field-driven dynamical multiferroicity in SrTiO3

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 attention1–6. The theoretical concept of dynamical multiferroicity has been introduced to describe the emergence of magnetization due to time-dependent electric polarization in non-ferromagnetic materials7,8. 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 SrTiO3 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 temperature9, 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.

Spatial control of hybridization-induced spin-wave transmission stop band

Spin-wave (SW) propagation close to the hybridization-induced transmission stop band is investigated within a trapezoid-shaped 200 nm thick yttrium iron garnet film using time-resolved magneto-optic Kerr effect microscopy and broadband spin-wave spectroscopy, supported by micromagnetic simulations. The gradual reduction of the effective field within the structure leads to local variations of the SW dispersion relation and results in a SW hybridization at a fixed position in the trapezoid where the propagation vanishes, since the SW group velocity approaches zero. By tuning external field or frequency, spatial control of the spatial stop band position and spin-wave propagation is demonstrated and utilized to gain transmission control over several microstrip lines.

Ultrafast magnetization enhancement via the dynamic spin-filter effect of type-II Weyl nodes in a kagome ferromagnet.

The magnetic type-II Weyl semimetal (MWSM) Co3Sn2S2 has recently been found to host a variety of remarkable phenomena including surface Fermi-arcs, giant anomalous Hall effect, and negative flat band magnetism. However, the dynamic magnetic properties remain relatively unexplored. Here, we investigate the ultrafast spin dynamics of Co3Sn2S2 crystal using time-resolved magneto-optical Kerr effect and reflectivity spectroscopies. We observe a transient magnetization behavior, consisting of spin-flipping dominated fast demagnetization, slow demagnetization due to overall half-metallic electronic structures, and an unexpected ultrafast magnetization enhancement lasting hundreds of picoseconds upon femtosecond laser excitation. By combining temperature-, pump fluence-, and pump polarization-dependent measurements, we unambiguously demonstrate the correlation between the ultrafast magnetization enhancement and the Weyl nodes. Our theoretical modelling suggests that the excited electrons are spin-polarized when relaxing, leading to the enhanced spin-up density of states near the Fermi level and the consequently unusual magnetization enhancement. Our results reveal the unique role of the Weyl properties of Co3Sn2S2 in femtosecond laser-induced spin dynamics.

All-optical observation of giant spin transparency at the topological insulator BiSbTe1.5Se1.5/Co20Fe60B20 interface

The rise of three-dimensional topological insulators as an attractive playground for the observation and control of various spin-orbit effects has ushered in the field of topological spintronics. To fully exploit their potential as efficient spin-orbit torque generators, it is crucial to investigate the efficiency of spin injection and transport at various topological insulator/ferromagnet interfaces, as characterized by their spin-mixing conductances and interfacial spin transparencies. Here, we use all-optical time-resolved magneto-optical Kerr effect magnetometry to demonstrate efficient room-temperature spin pumping in Sub/BiSbTe1.5Se1.5(BSTS)/Co20Fe60B20(CoFeB)/SiO2 thin films. From the modulation of Gilbert damping with BSTS and CoFeB thicknesses, the spin-mixing conductances of the BSTS/CoFeB interface and the spin diffusion length in BSTS are determined. For BSTS thicknesses far exceeding the spin diffusion length, in the so-called “perfect spin sink” regime, we obtain an interfacial spin transparency as high as 0.9, promoting such systems as scintillating candidates for spin-orbitronic devices.

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.

Ultrafast laser-induced precession dynamics in perpendicular artificial ferrimagnetic [D022-Mn3Ga/Co2MnSi]5 superlattices

Artificial ferrimagnetic [D022-Mn3Ga/Co2MnSi]N superlattices ([Mn3Ga/CMS]N SLs) combining perpendicular magnetic anisotropy as well as exceptional thermal and magnetic stability hold promises in functional spintronic devices. However, the relevant precession dynamics are still lacking. Here, we report on the magnetic dynamic properties in [Mn3Ga/CMS]5 SLs investigated by the time-resolved magneto-optical Kerr effect (TRMOKE) measurements. The magnetization precession process and magnetic damping constant (α0) of [Mn3Ga/CMS]5 SLs rely heavily on the thickness of Mn3Ga layer (tMn3Ga). In addition, α0 is found to be higher with increasing tMn3Ga, but is not simply scaled by the uniaxial magnetic anisotropy (Ku), which can be ascribed to the contribution of spin–orbit interaction combined with the additional contributions, like spin-pumping. Furthermore, a large Ku value of 1.33 Merg/cm3 and a low α0 of 0.022 have been simultaneously obtained in [Mn3Ga/CMS]5 SL with tMn3Ga = 1.5 nm. This study contributes to the design of high-performance spintronic devices based on [Mn3Ga/CMS]N SLs.

Ultrafast single-pulse all-optical switching in synthetic ferrimagnetic Tb/Co/Gd multilayers

In this work, we investigate single-shot all-optical switching (AOS) in Tb/Co/Gd/Co/Tb multilayers in an attempt to establish AOS in synthetic ferrimagnets with high perpendicular magnetic anisotropy. In particular, we study the effect of varying Tb thicknesses to disentangle the role of the two rare-earth elements. Even though the role of magnetic compensation has been considered to be crucial, we find that the threshold fluence for switching is largely independent of the Tb content. Moreover, we identify the timescale for the magnetization to cross zero to be approximately within the first ps after laser excitation using time-resolved magneto–optic Kerr effect. We conclude that the switching is governed mostly by interactions between Co and Gd.

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.

Photoinduced Nonthermal Reduction of the Coercive Field in FePt and FePt0.84Rh0.16 Epitaxial Thin Films in the L10 Phase

The time-resolved magneto-optical Kerr effect in epitaxial thin films of the FePt compound and the FePt0.84Rh0.16 solid solution with the perpendicular magnetic anisotropy on MgO (001) substrates has been studied. The evolution of hysteresis loops at short (100 fs–1 ns) and long (1–20 ms) time scales after the excitation by a femtosecond light pulse has been studied. Long-lived nonthermal reduction of the coercive field has been detected. The coercive field is recovered in several milliseconds. It has been proposed to explain the observed phenomenon by the excitation of high-Q-factor acoustic resonances in the substrate/film system and to the strong magnetoelastic interaction in FePt and FePt0.84Rh0.16 films.

Spin current driven by ultrafast magnetization of FeRh

Laser-induced ultrafast demagnetization is an important phenomenon that probes arguably the ultimate limits of the angular momentum dynamics in solid. Unfortunately, many aspects of the dynamics remain unclear except that the demagnetization transfers the angular momentum eventually to the lattice. In particular, the role and origin of electron-carried spin currents in the demagnetization process are debated. Here we experimentally probe the spin current in the opposite phenomenon, i.e., laser-induced ultrafast magnetization of FeRh, where the laser pump pulse initiates the angular momentum build-up rather than its dissipation. Using the time-resolved magneto-optical Kerr effect, we directly measure the ultrafast-magnetization-driven spin current in a FeRh/Cu heterostructure. A strong correlation between the spin current and the magnetization dynamics of FeRh is found even though the spin filter effect is negligible in this opposite process. This result implies that the angular momentum build-up is achieved by an angular momentum transfer from the electron bath (supplier) to the magnon bath (receiver) and followed by the spatial transport of angular momentum (spin current) and dissipation of angular momentum to the phonon bath (spin relaxation).

Enhancing spin-transfer torque in magnetic tunnel junction devices: Exploring the influence of capping layer materials and thickness on device characteristics

We have developed and optimized two categories of spin-ransfer torque magnetic tunnel junctions (STT-MTJs) that exhibit a high tunnel magnetoresistance ratio, low critical current, high outputpower in the micro-watt range, and auto-oscillation behavior. These characteristics demonstrate the potential of STT-MTJs for low-power, high-speed, and reliable spintronic applications, including magnetic memory, logic, and signal processing. The only distinguishing factor between the two categories, denoted as A-MTJs and B-MTJs, is the composition of their free layers, two CoFeB/0.21 Ta/6 CoFeSiB for A-MTJs and two CoFeB/0.21 Ta/7 NiFe for B-MTJs. Our study reveals that B-MTJs exhibit lower critical currents for auto-oscillation than A-MTJs. We found that both stacks have comparable saturation magnetization and anisotropy field, suggesting that the difference in auto-oscillation behavior is due to the higher damping of A-MTJs compared to B-MTJs. To verify this hypothesis, we employed the all-optical time-resolved magneto-optical Kerr effect technique, which confirmed that STT-MTJs with lower damping exhibited auto-oscillation at lower critical current values. Additionally, our study aimed to optimize the STT-MTJ performance by investigating the impact of the capping layer on the device’s response to electronic and optical stimuli.

Magnetic field modulated ultrafast spin dynamics at Ni80Fe20/Neodymium interface.

Ultrafast spin dynamics is crucial for the next-generation spintronic devices towards high-speed data processing. Here, we investigate the ultrafast spin dynamics of Neodymium/Ni80Fe20 (Nd/Py) bilayers by the time-resolved magneto-optical Kerr effect. The effective modulation of spin dynamics at Nd/Py interfaces is realized by an external magnetic field. The effective magnetic damping of Py increases with increasing Nd thickness, and a large spin mixing conductance (∼19.35×1015 cm-2) at Nd/Py interface is obtained, representing the robust spin pumping effect by Nd/Py interface. The tuning effects are suppressed at a high magnetic field due to the reduced antiparallel magnetic moments at Nd/Py interface. Our results contribute to understanding ultrafast spin dynamics and spin transport behavior in high-speed spintronic devices.

Determining the spin wave exchange constant of ferromagnets using canted high-order exchange magnons

We propose an alternative method for obtaining the spin wave exchange constant of a ferromagnetic material. This involves generating and detecting canted high-order magnons in Co films using a time-resolved magneto-optical Kerr effect instrument, which enables the extraction of the spin wave exchange constant in a single film thickness in a reliable manner. To enhance the sensitivity of high-order magnon detection, we perform simultaneous measurements of differential Kerr rotation and ellipticity on both sides of the film. This method will be particularly useful in practical situations where the magnetic properties of a material vary with thickness or where it is not feasible to produce films of the same quality.

Spin dynamics in the axion insulator candidate EuIn2As2

We report the investigation of spin dynamics in the antiferromagnetic metal ${\mathrm{EuIn}}_{2}{\mathrm{As}}_{2}$ with the Zintl phase by using time-resolved magneto-optical Kerr effect (TR-MOKE) and transient reflectivity spectroscopy. In TR-MOKE measurement, we observe a spin precession mode with a frequency of about 18 GHz below 1.4 T and a new emerging coherent acoustic phonon mode near 35 GHz at a higher field where the latter shows a field-independent behavior. With temperature increasing, the spin precession disappears above N\'eel temperature ${T}_{N}$, whereas the acoustic phonon persists up to 25 K due to existence of magnetic-field-induced polarized paramagnetism. In contrast, the quasiparticle dynamics of ${\mathrm{EuIn}}_{2}{\mathrm{As}}_{2}$ does not show dramatic change in the vicinity of ${T}_{N}$. By comparing the spin and quasiparticle dynamics, we attribute the appearance of an acoustic phonon in TR-MOKE to photoinduced transient perturbation of magneto-optical coefficient. Our paper provides an in-depth investigation on the dynamical magnetic properties and broadens the understanding of the ${\mathrm{EuIn}}_{2}{\mathrm{As}}_{2}$ system.

Concomitant modulation of interlayer exchange coupling and Gilbert damping in Fe/CoO with spin conductor Ag layer at interface

We report on the modulation of interlayer exchange coupling (IEC) between the ferromagnet (FM) Fe and insulating antiferromagnet (AFM) CoO and its impact on the Gilbert damping by a time-resolved magneto-optical Kerr effect technique. By inserting a wedge spin conductor Ag layer at the interface of Fe/CoO, it is revealed that both uniform spin precession frequency and Gilbert damping constant of Fe film decrease with increasing Ag thickness up to ∼2 nm, and above that with eliminated IEC, these two parameters reach the intrinsic values of the Fe film. The precession frequency and damping also show similar variation tendency with temperature for attenuated IEC. These results prove that the exchange coupling at the FM–AFM interface plays an essential role for the spin angular momentum transfer to the insulating AFM layer, and the spin pumping is insignificant even for the very thin spin conductor layer. Our findings may have general insights into the role of the FM/AFM interface in the magnetization dynamics and spin angular momentum transfer for future spintronic applications.

Ultrafast demagnetization dynamics in the epitaxial FeGe(111) film chiral magnet

The exploring of ultrafast demagnetization is a significant subject for understanding the versatility of spin dynamics. However, the laser-induced ultrafast demagnetization process in chiral magnet FeGe has remained elusive. Here, we report the ultrafast demagnetization processes of FeGe film with various magnetic structures using time-resolved magneto-optical Kerr effect (TRMOKE) measurements. Our work reveals a transition from one-step ultrafast demagnetization (type I) to two-step demagnetization (type II) process by changing ambient temperature, laser fluence, and magnetic field. We confirm that the transition from one-step to two-step ultrafast demagnetization mainly results from the weak electron-phonon (e-p) coupling. In the skyrmion phase region, TRMOKE curves demonstrate a two-step ultrafast demagnetization process. The two-step ultrafast demagnetization will further enhance the magnetization loss, and consequently facilitate the magnetization switching and pave a pathway to engineer chiral magnetic devices on picosecond timescales.

Magnetization dynamics in layered systems with coexisting bilinear and biquadratic interlayer exchange coupling

Important aspects of exchange-coupled magnetic layered structures are related to the noncollinear arrangement of sublayer magnetizations which can arise from competition between bilinear (BL) and biquadratic (BQ) interlayer exchange coupling (IEC). In this work, the influence of coexisting BL and BQ IEC of different strengths on magnetization precession in layered systems is investigated both experimentally and theoretically. Laser-induced magnetization precession has been studied in the $\text{Fe/Si}({d}_{\text{Si}}$) multilayers (MLS) as a function of the amplitude ($H$) and orientation angle (${\ensuremath{\theta}}_{H}$) of external magnetic field using time-resolved magneto-optical Kerr (TRMOKE) effect. Strongly changing characters of precession frequency dependencies $\ensuremath{\omega}(H,{\ensuremath{\theta}}_{H})$ for Fe sublayer thickness ${d}_{\text{Fe}}=3$ nm and Si spacer-layer thicknesses (${d}_{\text{Si}}$) varying in the range of 0.9--2.4 nm have been observed. Analytical formulas for acoustic and optic mode dispersion relations with coexisting BL and BQ IEC, scaled by ${J}_{1}$ and ${J}_{2}$ parameters, respectively, for the in-plane effective magnetic anisotropy and arbitrary magnetic field direction were derived, and very good agreement with the experimentally observed frequency dependencies has been obtained. It is shown that BQ coexisting with BL IEC significantly influences on the magnitude and form of dispersion relations. From analytical formula derived, it follows that zero-field optical mode frequency tends to zero as $|{J}_{1}|$ approaches $2{J}_{2}$. The acoustic and optic mode-crossing effect has been observed and it is found that values of crossing fields and frequency gaps strongly increase as ${\ensuremath{\theta}}_{H}$ angles decrease and depend on relative BL and BQ IEC strengths. The BL IEC is of ferromagnetic type with ${J}_{1}\ensuremath{\approx}1.6$ mJ/${\mathrm{m}}^{2}$ for the MLS with ${d}_{\text{Si}}=0.9$ nm, and changes to antiferromagnetic one with ${J}_{1}\ensuremath{\approx}\ensuremath{-}0.9$ mJ/${\mathrm{m}}^{2}$ for the MLS with ${d}_{\text{Si}}=1.4$ nm, while the ${J}_{2}$ parameter of BQ IEC decreases from 1.8 to 1.0 mJ/${\mathrm{m}}^{2}$. The coupling strengths decrease by one to two orders of magnitude for the sample with ${d}_{\text{Si}}=2.4$ nm, but both mode frequencies are still observed and well reproduced by the theory. It is shown that ${J}_{1}$ and ${J}_{2}$ parameters obtained in the TRMOKE experiment coincide within the estimated error bars with the determined from independent measurements of magnetization processes in the static magneto-optical Kerr effect and interpreted with the use of analytical formulas derived. Numerical solutions of coupled Landau-Lifshitz-Gilbert (LLG) equations for acoustic and optic modes, with inclusion of BL IEC, intrinsic Gilbert damping, and spin-pumping damping terms, and extended to include BQ IEC, were performed and fitted to experimental data. It is shown that determined effective damping coefficients on $H$ and ${\ensuremath{\theta}}_{H}$ dependencies for acoustic and optic modes are very well simulated with the use of LLG equation solutions with Gilbert damping, spin-pumping-damping--related effective spin-mixing conductance, and spin-diffusion length parameters included. The dependencies of the parameters on ${d}_{\text{Si}}$ spacer-layer thickness are discussed and compared with available data for other systems.

Magnetic Damping Properties of Single-Crystalline Co55Mn18Ga27 and Co50Mn18Ga32 Films

We investigate the structural, static magnetic and damping properties in two Mn-deficient magnetic Weyl semimetal Co-Mn-Ga (CMG) alloy films, i.e., Co55Mn18Ga27 (CMG1) and Co50Mn18Ga32 (CMG2), which were epitaxially grown on MgO (001) substrates. CMG1 has a mixing phase of B 2 and L21, larger saturation magnetization (M s ∼ 760 emu/cm3), stronger in-plane magnetic anisotropy. CMG2 has an almost pure B2 phase, smaller M s (∼ 330 emu/cm3), negligible in-plane magnetic anisotropy. Time-resolved magneto-optical Kerr effect results unambiguously demonstrate an obvious perpendicular standing spin wave (PSSW) mode in addition to the Kittel mode for both of the CMG films. The intrinsic damping constant is about 0.0055 and 0.015 for CMG1 and CMG2, respectively, which are both significantly larger than that of the stoichiometric CMG (i.e., Co2MnGa) film reported previously. In combination with the first-principles calculations, the intrinsic damping properties of the Mn-deficient CMG films can be well explained by considering the increase of density of states at the Fermi level, reduction of M s, and excitation of the PSSW mode. These findings provide a new clue to tuning the magnetic damping of the magnetic Weyl semimetal film through slight off-stoichiometry.