Single-pulse switching has been experimentally demonstrated in ferrimagnetic GdFeCo and Mn$_2$Ru$_x$Ga alloys. Complete understanding of single-pulse switching is missing due to the lack of an established theory accurately describing the transition to the non-equilibrium reversal path induced by femtosecond laser photo-excitation. In this work we present general macroscopic theory for the magnetization dynamics of ferrimagnetic materials upon femtosecond laser excitation. Our theory reproduces quantitatively all stages of the switching process observed in experiments. We directly compare our theory to computer simulations using atomistic spin dynamics methods for both GdFeCo and Mn$_2$Ru$_x$Ga alloys. We provide explicit expressions for the magnetization relaxation rates in terms of microscopic parameters which allows us to propose universal criteria for switching in ferrimagnets.
Ultrafast laser-induced magnetic switching in rare earth, transition metal ferrimagnetic alloys has recently been reported to occur by ultrafast heating alone. Using atomistic simulations and a ferrimagnetic Landau-Lifshitz-Bloch formalism, we demonstrate that for switching to occur it is necessary that angular momentum is transferred from the longitudinal to transverse magnetization components. This dynamical path leads to magnetization switching and subsequent ultrafast precession caused by the inter-sublattice exchange field on the nanoscale.
Synthetic ferrimagnets are composite magnetic structures formed from two or more anti- ferromagnetically coupled magnetic sublattices with different magnetic moments. Here we report on atomistic spin simulations of the laser-induced magnetization dynamics on such synthetic ferrimag- nets, and demonstrate that the application of ultrashort laser pulses leads to sub-picoscond magnetization dynamics and all-optical switching in a similar manner as in ferrimagnetic alloys. Moreover, we present the essential material properties for successful laser-induced switching, demonstrating the feasibility o…
We report on an element- and time-resolved investigation of femtosecond laser induced ultrafast dynamics of 3d and 4f spins in a ferrimagnetic Co80Dy20 alloy as a function of temperature. We observe an increase of the Co3d characteristic demagnetization time and a decrease of the Dy4f demagnetization time when the temperature is approaching the Curie temperature. It suggests that the critical slowing down regime, which affects the laser induced ultrafast dynamics in pure 3d transition metals and 4f rare-earth ferromagnetic layers, vanishes for the Dy sublattice in the CoDy alloy, in line with …
Magneto-optical spectroscopy in fields up to 30 Tesla reveals anomalies in the equilibrium and ultrafast magnetic properties of the ferrimagnetic rare-earth-transition metal alloy TbFeCo. In particular, in the vicinity of the magnetization compensation temperature, each of the magnetizations of the antiferromagnetically coupled Tb and FeCo sublattices show triple hysteresis loops. Contrary to state-of-the-art theory, which explains such loops by sample inhomogeneities, here we show that they are an intrinsic property of the rare-earth ferrimagnets. Assuming that the rare-earth ions are paramag…
We study the heat-induced magnetization dynamics in a toy model of a ferrimagnetic alloy, which includes localized spins antiferromagnetically coupled to an itinerant carrier system with a Stoner gap. We determine the one-particle spin-density matrix including exchange scattering between localized and itinerant bands as well as scattering with phonons. While a transient ferromagnetic-like state can always be achieved by a sufficiently strong excitation, this transient ferromagnetic-like state only leads to magnetization switching for model parameters that also yield a compensation point in the…
We derive an effective Lagrangian in the quasi-antiferromagnetic approximation that allows to describe the magnetization dynamics for uniaxial f-d (rare-earth - transition metal) ferrimagnet near the magnetization compensation point in the presence of external magnetic field. We perform calculations for the parameters of GdFeCo, a metallic ferrimagnet with compensation point that is one of the most promising materials in ultrafast magnetism. Using the developed approach, we find the torque that acts on the magnetization due to ultrafast demagnetization pulse that can be caused either by ultras…
This review discusses the ultrafast magnetization dynamics within the gigahertz to terahertz frequency range in ferrimagnetic rare-earth iron garnets with different substitutions. In these garnets, the roles of spin-orbit and exchange interactions have been detected using femtosecond laser pulses via the inverse Faraday effect. The all-optical control of spin-wave and Kaplan-Kittel exchange resonance modes in different frequency ranges is shown. Generation and localization of the electric field distribution inside the garnet through the metal-bound surface plasmon-polariton strongly enhance th…
We bridge an essential knowledge gap on the understanding of all-optical ultrafast switching in ferrimagnets; namely, the connection between atomistic spin dynamics methods and macroscopic phenomenological models. All-optical switching of the magnetization occurs after the application of a single femtosecond laser pulse to specific ferrimagnetic compounds. This strong excitation puts the involved degrees of freedom, electrons, lattice and spins out-of-equilibrium between each other. Atomistic spin models have quantitatively described all-optical switching in a wide range of experimental condit…
Femtosecond laser induced ultrafast magnetization dynamics have been studied in multisublattice CoxDy1-x alloys. By performing element and time-resolved X-ray spectroscopy, we distinguish the ultrafast quenching of Co3d and Dy4f magnetic order when the initial temperatures are below (T=150K) or above (T=270K) the temperature of magnetic compensation (Tcomp). In accordance with former element-resolved investigations and theoretical calculations, we observe different dynamics for Co3d and Dy4f spins. In addition we observe that, for a given laser fluence, the demagnetization amplitudes and demag…
We follow for the first time the evolution of the spin and orbital angular momentum of a thin Ni film during ultrafast demagnetization, by means of x-ray magnetic circular dichroism. Both components decrease with a 130 +/- 40 fs time constant upon excitation with a femtosecond laser pulse. Additional x-ray absorption measurements reveal an increase in the spin-orbit interaction by 6 +/- 2 % during this process. This is the experimental demonstration quantifying the importance of spin-orbit mediated processes during the demagnetization.
Manipulation of the intersublattice interaction strengh (JRE-TM) in rare earth (RE)-transition metal (TM) alloys is a key issue to understand how efficiently the laser-induced angular momentum transfers from 3d to 4f spins and to have a better control of the ultrafast spin dynamics. In this work, the relationships between laser-induced demagnetization process and the intersublattice 3d-4f interaction for the GdCoFe alloys were systematically studied. The ultrafast two-stage demagnetization process could change into a one-stage mode as the angular momentum transferring channel between 3d and 4f…
We predict ultrafast modulation of the pure molten metal surface stress fields under the irradiation of the single femtosecond laser pulse through the two-temperature model molecular-dynamics simulations. High-resolution and precision calculations are used to resolve the ultrafast laser-induced anisotropic relaxations of the pressure components on the time-scale comparable to the intrinsic liquid density relaxation time. The magnitudes of the dynamic surface tensions are found being modulated sharply within picoseconds after the irradiation, due to the development of the nanometer scale non-hy…
Femtosecond, 8.04 KeV x-ray pulses are used to probe the lattice dynamics of 150 nm Cu (111) single crystal on mica substrate irradiated with 400 nm, 100 fs laser pulses. For pump fluencies below the damage and melting threshold, we observed lattice contraction due to the formation of a blast force, and coherent acoustic phonons with a period of ~69 ps. At larger pump fluence, solid to liquid phase transition, annealing, and recrystallization were measured in real time by monitoring the intensity evolution of the probing fs x-ray rocking curves and agreed with theoretical simulation results. T…
Ferrimagnets containing several partially compensated magnetic sublattices are considered the most promising materials for all-optical data storage and for ultrafast communications based on spin waves. There are two magnetic phases of the ferrimagnets: collinear and non-collinear ones. Up to now spin dynamics in ferrimagnets has been studied mostly in the collinear state without paying much attention to the kind of the magnetic phase. Here we investigate laser induced ultrafast spin dynamics in a rare-earth iron garnet film in the noncollinear phase as well. We identify a crucial influence of …
Based on numerical simulations, we demonstrate thermally induced magnetic switching in synthetic ferrimagnets composed of multilayers of rare-earth and transition metals. Our findings show that deterministic magnetization reversal occurs above a certain threshold temperature if the ratio of transition metal atoms to rare-earth atoms is sufficiently large. Surprisingly, the total thickness of the multilayer system has little effect on the occurence of switching. We further provide a simple argument to explain the temperature dependence of the reversal process.
Femtosecond carrier recombination in PbI2 is measured using tabletop high-harmonic extreme ultraviolet (XUV) transient absorption spectroscopy and ultrafast electron diffraction. XUV absorption from 45 eV to 62 eV measures transitions from the iodine 4d core level to the conduction band density of states. Photoexcitation at 400 nm creates separate and distinct transient absorption signals for holes and electrons, separated in energy by the 2.4 eV band gap of the semiconductor. The shape of the conduction band and therefore the XUV absorption spectrum is temperature dependent, and nonradiative …
We present a theoretical investigation of the yet unexplored dynamics of the produced excited carriers upon irradiation of hexagonal Silicon Carbide (6H-SiC) with femtosecond laser pulses. To describe the ultrafast behaviour of laser induced out-of-equilibrium carriers, a real time simulation based on Density Functional Theory (DFT) methodology is used to compute both the hot carrier dynamics and transient change of the optical properties. A Two-Temperature model (TTM) is also employed to derive the relaxation processes for laser pulses of wavelength 401 nm, duration 50 fs at normal incidence …
Orientation-resolved ultrafast spin reorientation dynamics in ferrimagnetic DyCo$_5$
Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie（马克斯·玻恩非线性光学和超快光谱学研究所）；Leibniz-Institut für Kristallzüchtung（莱布尼茨晶体生长研究所）；European XFEL（欧洲X射线自由电子激光设施）；Technische Universität Berlin, Institut für Optik und Atomare Physik（柏林工业大学光学与原子物理研究所）
To gain control over magnetic order on ultrafast time scales, a fundamental understanding of the way electron spins interact with the surrounding crystal lattice is required. However, measurement and analysis even of basic collective processes such as spin-phonon equilibration have remained challenging. Here, we directly probe the flow of energy and angular momentum in the model insulating ferrimagnet yttrium iron garnet. Following ultrafast resonant lattice excitation, we observe that magnetic order reduces on distinct time scales of 1 ps and 100 ns. Temperature-dependent measurements, a spin…
In this work, we present evidence for the existence of a magnonic current on the sub-picosecond time-scale in a ferrimagnetic bilayer and its effect on ultrafast spin dynamics. The ferrimagnet, GdFeCo, is a material known to undergo ultrafast switching within 1-2ps after excitation with femtosecond laser pulses. Here, we show that the strong thermal gradients induced by applying femtosecond laser pulses and the presence of chemical inhomogeneities lead to local imbalances in the effective temperatures of the spins that produces a rapid transfer of spin angular momentum, which we interpret as a…
Ferromagnetic materials dominate as the magnetically active element in spintronic devices, but come with drawbacks such as large stray fields, and low operational frequencies. Compensated ferrimagnets provide an alternative as they combine the ultrafast magnetization dynamics of antiferromagnets with a ferromagnet-like spin-orbit-torque (SOT) behavior. However to use ferrimagnets in spintronic devices their advantageous properties must be retained also in ultrathin films (t < 10 nm). In this study, ferrimagnetic Gdx(Fe87.5Co12.5)1-x thin films in the thickness range t = 2-20 nm were grown on h…
A theoretical investigation of the ultrafast processes and dynamics of the excited carriers upon irradiation of GaAs with femtosecond (fs) pulsed lasers is performed in conditions that induce material damage and eventually surface modification of the heated solid. A parametric study is followed to correlate the produced transient carrier density with the damage threshold for various pulse duration values τp (it increases as ~ at relatively small values of τp while it drops for pulse durations of the order of some picoseconds) based on the investigation of the fundamental multiscale physical pr…
Ultrafast magnetization dynamics in metallic heterostructures consists of a combination of local demagnetization in the ferromagnetic constituent and spin-dependent transport contributions within and in between the constituents. Separation of these local and non-local contributions is essential to obtain microscopic understanding and for potential applications of the underlying microscopic processes. By comparing the ultrafast changes of the polarization rotation and ellipticity in the magneto-optical Kerr effect (MOKE) we observe a time-dependent magnetization profile M(z,t) in Co/Cu(001) fil…
We have measured the hot-electron induced demagnetization of a [Co/Pt]2 multilayer in M(x nm)/Cu(100 nm)/[Co(0.6 nm)/Pt(1.1 nm)]2 samples depending on the nature of the capping layer M and its thickness x. We found out that a Pt layer is more efficient than [Co/Pt]X, Cu or MgO layers in converting IR photon pulses into hot-electron pulses at a given laser power. We also found out that the maximum relative demagnetization amplitude is reached for M(x) = Pt (7 nm). Our experimental results show qualitative agreement with numerical simulations based on the superdiffusive spin transport model. We …
The magnetization of a non-magnetic semiconductor by femtosecond light pulses is crucial to achieve an all-optical control of the spin dynamics in materials and to develop faster memory devices. However, the conditions for its detection are largely unknown. In this work we identify the criteria for the observation of ultrafast magnetization and critically discuss the difficulties hindering its experimental detection. We show that ultrafast magnetization of a non magnetic semiconductor can be observed in compounds with very localized conduction band states and more delocalized valence bands, su…
Precision-controlled ultrafast electron microscope platforms. A case study: Multiple-order coherent phonon dynamics in 1T-TaSe$_2$ probed at 50 femtosecond - 10 femtometer scales
Faster magnetic recording technology is indispensable to massive data storage and big data sciences. {All-optical spin switching offers a possible solution}, but at present it is limited to a handful of expensive and complex rare-earth ferrimagnets. The spin switching in more abundant ferromagnets may significantly expand the scope of all-optical spin switching. Here by studying 40,000 ferromagnetic spins, we show that it is the optical spin-orbit torque that determines the course of spin switching in both ferromagnets and ferrimagnets. Spin switching occurs only if the effective spin angular …
The effect of ultrashort laser-induced morphological changes upon irradiation of silicon with double pulse sequences is investigated under conditions that lead to mass removal. The temporal delay between twelve double and equal-energy pulses (Ep=0.24J/cm2 each, with pulse duration tp=430fs, 800nm laser wavelength) was varied between 0 and 14ps and a decrease of the damaged area, crater depth size and periodicity of the induced subwavelength ripples (by 3-4%) was observed with increasing pulse delay. The proposed underlying mechanism is based on the combination of carrier excitation and energy …
Magnetic phenomena are ubiquitous in our surroundings and indispensable for modern science and technology, but it is notoriously difficult to change the magnetic order of a material in a rapid way. However, if a thin nickel film is subjected to ultrashort laser pulses, it can lose its magnetic order almost completely within merely femtosecond times. This phenomenon, in the meantime also observed in many other materials, has connected magnetism with femtosecond optics in an efficient, ultrafast and complex way, offering opportunities for rapid information processing or ultrafast spintronics at …
Laser induced ultrafast Co 3d and Ho 4f spin dynamics in CoHo ferrimagnetic alloys
Helmholtz-Zentrum Berlin für Materialien und Energie（柏林亥姆霍兹材料与能源中心）；Institut Jean Lamour, Université de Lorraine（洛林大学让·拉缪尔研究所）；Université de Strasbourg, CNRS, Institut de Physique et Chimie des Matériaux de Strasbourg（斯特拉斯堡大学、法国国家科学研究中心、斯特拉斯堡物理与化学材料研究所）
From Ultrafast Demagnetization to Ultrafast Spintronics : a 30 years story
Université de Lorraine（洛林大学）；CNRS, Institut Jean Lamour（法国国家科学研究中心，让·拉穆尔研究所）；Department of Physics, Freie Universität Berlin（柏林自由大学物理系）；Center for Science and Innovation in Spintronics, Tohoku University（东北大学自旋电子学科学与创新中心）
The femtosecond evolution of the electronic temperature of laser-excited gold nanoparticles is measured, by means of ultrafast time-resolved photoemission spectroscopy induced by extreme-ultraviolet radiation pulses. The temperature of the electron gas is deduced by recording and fitting high-resolution photo emission spectra around the Fermi edge of gold nanoparticles providing a direct, unambiguous picture of the ultrafast electron-gas dynamics. These results will be instrumental to the refinement of existing models of femtosecond processes in laterally-confined and bulk condensed-matter sys…
In spintronics applications, ultrafast spin dynamics have to be controlled at femtosecond (fs) timescales via fs-laser radiation. At such ultrafast timescales, the effect of the Gilbert damping factor α on ultrafast demagnetization time should be considered. In previous explorations for the relationship between these two parameters, it was found that the theoretical calculations based on the local spin-flip scattering model do not agree with the experimental results. Here, we find that in Fe81Ga19(FeGa)/Ir20Mn80(IrMn) bilayers, the unconventional IrMn thickness dependence of α results from the…
Excitation and propagation dynamics of spin waves in an iron-based garnet film under out-of-plane magnetic field were investigated by time-resolved magneto-optical imaging. The experimental results and the following data analysis by phase-resolved spin-wave tomography reveal the excitation of spin waves triggered by photo-induced demagnetization (PID) along the sample depth direction. Moreover, the fast relaxation of PID accompanied by the spin transfer due to spin-wave emission was observed. Possible scenarios of PID in the garnet film are discussed. Finally, we develop a model for the spin-w…
The dynamics of the photoinduced commensurate to incommensurate charge density wave (CDW) phase transition in 4Hb-TaSe2 are investigated by femtosecond electron diffraction. In the perturbative regime the CDW reforms on a 150 ps timescale, which is two orders of magnitude slower than in other transition-metal dichalcogenides. We attribute this to a weak coupling between the CDW carrying T-layers and thus demonstrate the importance of three-dimensionality for the existence of CDWs. With increasing optical excitation the phase transition is achieved showing a second order character in contrast t…
We present a theoretical study of the ultrafast electron dynamics in transition metals using ultrashort pulsed laser beams. The significant influence of the contribution of the dynamics of produced nonthermal electrons to electron thermalisation and electron-phonon interaction is thoroughly investigated within a range of values of the pulse duration (i.e. from 10fs to 2.3ps). The theoretical model elaborates firstly on possible transient changes of optical parameters during irradiation due to the presence of the non-equilibrium electrons and the modification of the electron distribution functi…
Characterizing and controlling the out-of-equilibrium state of nanostructured Mott insulators hold great promises for emerging quantum technologies while providing an exciting playground for investigating fundamental physics of strongly-correlated systems. Here, we use two-colour near-field ultrafast electron microscopy to photo-induce the insulator-to-metal transition in a single VO2 nanowire and probe the ensuing electronic dynamics with combined nanometer-femtosecond resolution. We take advantage of a femtosecond temporal gating of the electron pulse mediated by an infrared laser pulse, and…
Many linked processes occur concurrently in strongly excited semiconductors, such as interband and intraband absorption, scattering of electrons and holes by the heated lattice, Pauli blocking, bandgap renormalization and the formation of Mahan excitons. In this work, we disentangle their dynamics and contributions to the optical response of a ZnO thin film. Using broadband pump-probe ellipsometry, we can directly and unambiguously obtain the real and imaginary part of the transient dielectric function which we compare with first-principles simulations. We find interband and excitonic absorpti…
The ability to manipulate ferroelectrics at ultrafast speeds has long been an elusive target for materials research. Coherently exciting the ferroelectric mode with ultrashort optical pulses holds the promise to switch the ferroelectric polarization on femtosecond timescale, two orders of magnitude faster compared to what is possible today with pulsed electric fields. Here, we report on the demonstration of ultrafast optical reversal of the ferroelectric polarization in LiNbO3. Rather than driving the ferroelectric mode directly, we couple to it indirectly by resonant excitation of an auxiliar…
We present the development of the first ultrafast transmission electron microscope (UTEM) driven by localized photoemission from a field emitter cathode. We describe the implementation of the instrument, the photoemitter concept and the quantitative electron beam parameters achieved. Establishing a new source for ultrafast TEM, the Göttingen UTEM employs nano-localized linear photoemission from a Schottky emitter, which enables operation with freely tunable temporal structure, from continuous wave to femtosecond pulsed mode. Using this emission mechanism, we achieve record pulse properties in …
We derive the Landau-Lifshitz-Bloch (LLB) equation for a two-component magnetic system valid up to the Curie temperature. As an example, we consider disordered GdFeCo ferrimagnet where the ultrafast optically induced magnetization switching under the action of heat alone has been recently reported. The two-component LLB equation contains the longitudinal relaxation terms responding to the exchange fields from the proper and the neighboring sublattices. We show that the sign of the longitudinal relaxation rate at high temperatures can change depending on the dynamical magnetization value and a …
X-ray scattering is one of the primary tools to determine crystallographic configuration with atomic accuracy. However, the measurement of ultrafast structural dynamics in monolayer crystals remains a long-standing challenge due to a significant reduction of diffraction volume and complexity of data analysis, prohibiting the application of ultrafast x-ray scattering to study nonequilibrium structural properties at the two-dimensional limit. Here, we demonstrate femtosecond surface x-ray diffraction in combination with crystallographic model-refinement calculations to quantify the ultrafast str…
Current induced magnetization manipulation is a key issue for spintronic application. Therefore, deterministic switching of the magnetization at the picoseconds timescale with a single electronic pulse represents a major step towards the future developments of ultrafast spintronic. Here, we have studied the ultrafast magnetization dynamics in engineered Gdx[FeCo]1-x based structure to compare the effect of femtosecond laser and hot-electrons pulses. We demonstrate that a single femtosecond hot-electrons pulse allows a deterministic magnetization reversal in either Gd-rich and FeCo-rich alloys …
Ultrafast imaging is essential in physics and chemistry to investigate the femtosecond dynamics of nonuniform samples or of phenomena with strong spatial variations. It relies on observing the phenomena induced by an ultrashort laser pump pulse using an ultrashort probe pulse at a later time. Recent years have seen the emergence of very successful ultrafast imaging techniques of single non-reproducible events with extremely high frame rate, based on wavelength or spatial frequency encoding. However, further progress in ultrafast imaging towards high spatial resolution is hampered by the lack o…
