The magnetization response of bulk ferromagnets after excitation by an ultrashort optical pulse is calculated using a dynamical model of the Elliott-Yafet type that includes the effects of the spin-orbit interaction in the ab-initio ferromagnetic band structure, the electron-phonon interaction at the level of Boltzmann scattering integrals, and dynamical changes in the temperature of the phonon bath. Using realistic parameters for the ultrashort optical pulse, the computed maximum magnetization quenching achievable with electron-phonon scattering in a fixed band structure is much smaller than the quenching observed in experiments. Heating of the phonon bath is found to not appreciably change the magnetization dynamics on ultrashort timescales.
Despite intense experimental effort, theoretical proposals and modeling approaches, a lack of consensus exists about the intrinsic mechanisms driving ultrafast magnetization dynamics in 3$d$ ferromagnets. In this work, we find evidence of electron-phonon mediated spin-flip as the driving mechanism for the ultrafast magnetization dynamics in all three 3$d$ ferromagnets; nickel, iron and cobalt. We use a microscopic three temperature model with parameters calculated from first-principles, which has been validated by direct comparison to the electron and lattice dynamics extracted from previous e…
We investigate ultrafast demagnetization due to electron-phonon interaction in a model band-ferromagnet. We show that the microscopic mechanism behind the spin dynamics due to electron-phonon interaction is the interplay of scattering and the precession around momentum-dependent effective internal spin-orbit magnetic fields. The resulting magnetization dynamics can only be mimicked by spin-flip transitions if the spin precession around the internal fields is sufficiently fast (compared to the scattering time) so that it averages out the transverse spin components.
A hierarchical multiscale approach to model the magnetization dynamics of ferromagnetic ran- dom alloys is presented. First-principles calculations of the Heisenberg exchange integrals are linked to atomistic spin models based upon the stochastic Landau-Lifshitz-Gilbert (LLG) equation to calculate temperature-dependent parameters (e.g., effective exchange interactions, damping param- eters). These parameters are subsequently used in the Landau-Lifshitz-Bloch (LLB) model for multi-sublattice magnets to calculate numerically and analytically the ultrafast demagnetization times. The developed mul…
We demonstrate that light resonant with the bandgap forces the antiferromagnetic semiconducor EuSe to enter ferromagnetic alignment in the picosecond time scale. A photon generates an electron-hole pair, whose electron forms a supergiant spin polaron of magnetic moment of nearly 6,000 Bohr magnetons. By increasing the light intensity, the whole of the sample can be fully magnetized. The key to the novel large photoinduced magnetization mechanism is the huge enhancement of the magnetic susceptibility when both antiferromagnetic and ferromagnetic interactions are present in the material, and are…
Ultrafast optical excitation of gold-cobalt bilayers triggers the nontrivial interplay between the electronic, acoustic, and magnetic degrees of freedom. Laser-heated electrons generated at the gold-air interface diffuse through the layer of gold and strongly overheat the lattice in cobalt resulting in the emission of ultrashort acoustic pulses and generation of exchange-coupled magnons. Time-resolved optical measurements allow for extracting the thermal boundary (Kapitza) resistances at metal/metal interfaces and the hot electron diffusion length in ferromagnetic materials. Both the experimen…
Ultrafast two-color pump-probe measurements, involving coherent acoustic phonon (CAP) waves, have provided information simultaneously on the mechanical properties and on the electronic structure of ferromagnetic GaMnAs. The elastic constant C11 of Ga1-xMnxAs (0.03<x<0.07) are observed to be systematically smaller than those of GaAs. Both C11 and Vs of GaMnAs are found to increase with temperature (78 K<T<295 K), again in contrast to the opposite behavior in GaAs. In addition, the fundamental bandgap (at E0 critical point) of Ga1-xMnxAs is found to shift slightly to higher energies with Mn conc…
We theoretically investigate spin-dependent carrier dynamics due to the electron-phonon interaction after ultrafast optical excitation in ferromagnetic metals. We calculate the electron-phonon matrix elements including the spin-orbit interaction in the electronic wave functions and the interaction potential. Using the matrix elements in Boltzmann scattering integrals, the momentum-resolved carrier distributions are obtained by solving their equation of motion numerically. We find that the optical excitation with realistic laser intensities alone leads to a negligible magnetization change, and …
A dependence of a relaxation rate on the shape of the demagnetized region for a longitudinal evolution of total magnetization to its equilibrium value following the ultrafast demagnetization is demonstrated. This shape-dependence is caused by a motion of the wave front inside the demagnetized region. The contribution of the wave front for spherically symmetric shape of the demagnetized region is up to 3 times and for cylindrically symmetric shape up to 2 times stronger than for one dimensional demagnetized region. This effect can be observed after the demagnetization by a tightly focused femto…
We theoretically demonstrate that the ultrafast magnetic order dynamics in antiferromagnets is exchange-enhanced in comparison to their ferromagnetic counterparts. We provide an equation of motion for the magnetic order dynamics validated by computer simulations using atomistic spin dynamics methods. The exchange of angular momentum between sublattices speeds up the dynamics in antiferromagnets, a process absent in ferromagnets.
The ultrafast dynamics of magnetic order in a ferromagnet are governed by the interplay between electronic, magnetic and lattice degrees of freedom. In order to obtain a microscopic understanding of ultrafast demagnetization, information on the response of all three subsystems is required. A consistent description of demagnetization and microscopic energy flow, however, is still missing. Here, we combine a femtosecond electron diffraction study of the ultrafast lattice response of nickel to laser excitation with ab initio calculations of the electron-phonon interaction and energy-conserving at…
To verify the exact underlying mechanism of ultrafast vortex-core reversal as well as the vortex state stability we conducted numerical calculations of the dynamic evolution of magnetic vortices in Permalloy cylindrical nanodots under an oscillating in-plane magnetic field over a wide range of the frequency and amplitude. The calculated results reveal different kinds of the non-trivial dynamic responses of vortices to the driving external field. In particular, the results offer insight into the 10 ps scale underlying physics of the ulrafast vortex-core reversals driven by small amplitude (~10 …
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 …
We report on the observation of ultrafast photo-enhanced ferromagnetism in GaMnAs. It is manifested as a transient magnetization increase on a 100-ps time scale, after an initial sub-ps demagnetization. The dynamic magnetization enhancement exhibits a maximum below the Curie temperature Tc and dominates the demagnetization component when approaching Tc. We attribute the observed ultrafast collective ordering to the p-d exchange interaction between photoexcited holes and Mn spins, leading to a correlation-induced peak around 20K and a transient increase in Tc.
Measuring local magnetization dynamics and its spatial variation is essential for advancements in spintronics and relevant applications. Here we demonstrate a phase-sensitive imaging technique for studying patterned magnetic structures based on picosecond laser heating. With the time-resolved anomalous Nernst effect (TRANE) and extensions, we simultaneously image the dynamic magnetization and RF driving current density. The stroboscopic detection implemented in TRANE microscopy provides access to both amplitude and phase information of ferromagnetic resonance (FMR) and RF current. Using this a…
By correlating time- and angle-resolved photoemission and time-resolved transverse- magneto- optical Kerr effect measurements, both at extreme ultraviolet wavelengths, we uncover the universal nature of the ultrafast photoinduced magnetic phase transition in Ni. This allows us to explain the ultrafast magnetic response of Ni at all laser fluences - from a small reduction of the magnetization at low laser fluences, to complete quenching at high laser fluences. Both probe methods exhibit the same demagnetization and recovery timescales. We further show that the ultrafast demagnetization in Ni is…
Ultrafast strengthening or quenching of the ferromagnetic order of semiconducting Eu1-xGdxO was achieved by resonant photoexcitation. The modification of the magnetic order is established within 3 ps as revealed by optical second harmonic generation. A theoretical analysis shows that the response is determined by the interplay of chemically and optically generated carriers in a nonequilibrium scenario beyond the three-temperature model. General criteria for the design of spintronics materials with tunable ultrafast spin dynamics are given.
The transition frequency between nonthermal coherent magnetic precessions and ultrafast demagnetization is arguably the most sought after answer in magnetism science and technology nowadays. So far, it is believed to be in the terahertz (THz) range. Here, using an ultra-intense low frequency THz bullet, and thin magnetic layers, we report on experimental evidences that fully coherent nonthermal THz magnetic switching may never be reachable in conventional ferromagnetic thin films. At high excitation intensities, while the spins still coherently precess with the THz magnetic field, the deposite…
Through time-resolved two-color magneto-optical Kerr spectroscopy we have demonstrated that photogenerated transient carriers decrease the coercivity of ferromagnetic InMnAs at low temperatures. This transient ``softening'' persists only during the carrier lifetime ($\sim$ 2 ps) and returns to its original value as soon as the carriers recombine to disappear. We discuss the origin of this unusual phenomenon in terms of carrier-enhanced ferromagnetic exchange interactions between Mn ions and propose an entirely nonthermal scheme for magnetization reversal.
When a laser pulse excites a ferromagnet, its spin undergoes a dramatic change. The initial demagnetization process is very fast. Experimentally, it is found that the demagnetization time is related to the spin moment in the sample. In this study, we employ the first-principles method to directly simulate such a process. We use the fixed spin moment method to change the spin moment in ferromagnetic nickel, and then we employ the Liouville equation to couple the laser pulse to the system. We find that in general the dependence of demagnetization time on the spin moment is nonlinear: It decrease…
The Elliott-Yafet mechanism is arguably the most promising candidate to explain the ultrafast demagnetization dynamics in ferromagnetic transition metals on timescales on the order of 100 femtoseconds. So far, only electron-phonon scattering has been analyzed as the scattering process needed to account for the demagnetization due to the Elliott-Yafet mechanism. We show for the first time that the electron-electron scattering contribution to the Elliott-Yafet mechanism has the potential to explain time-resolved magneto-optical Kerr effect measurements on thin magnetic cobalt and nickel films, w…
We have performed a two-color time-resolved magneto-optical Kerr effect (MOKE) study of a ferromagnetic InMnAs/GaSb heterostructure. We observed ultrafast photo-induced changes in the MOKE signal induced by a large density of spin-polarized transient carriers created only within the InMnAs layer using intense 140 fs mid-infrared pulses. Our data clearly demonstrates that magnetic properties, e.g., remanence and coercivity, can be strongly modified. The dependence of these changes on the time delay, pump polarization, pump intensity, and sample temperature is discussed.
Epitaxial strain and chemical substitution have been the workhorses of functional materials design. These static techniques have shown immense success in controlling properties in complex oxides through the tuning of subtle structural distortions. Recently, an approach based on the excitation of an infrared active phonon with intense mid-infrared light has created an opportunity for dynamical control of structure through special nonlinear coupling to Raman phonons. We use first-principles techniques to show that this approach can dynamically induce a magnetic phase transition from the ferromag…
We analyze theoretically the demagnetization dynamics in a ferromagnetic model system due to the interplay of spin-orbit coupling and electron-electron Coulomb scattering. We compute the $k$-resolved electronic reduced spin-density matrix including precessional dynamics around internal spin-orbit and exchange fields as well as the electron-electron Coulomb scattering for densities and spin coherences. Based on a comparison with numerical solutions of the full Boltzmann scattering integrals, we establish that the $k$-resolved reduced spin-density matrix dynamics are well described using a simpl…
We use single-cycle THz fields and the femtosecond magneto-optical Kerr effect to respectively excite and probe the magnetization dynamics in two thin-film ferromagnets with different lattice structure: crystalline Fe and amorphous CoFeB. We observe Landau-Lifshitz-torque magnetization dynamics of comparable magnitude in both systems, but only the amorphous sample shows ultrafast demagnetization caused by the spin-lattice depolarization of the THz-induced ultrafast spin current. Quantitative modelling shows that such spin-lattice scattering events occur on similar time scales than the conventi…
Irradiating a ferromagnetic material with an ultrashort laser pulse leads to demagnetization on a femtosecond timescale. We implement Elliott-Yafet type spin-flip scattering, mediated by electron-electron and electron-phonon collisions, into the framework of a spin-resolved Boltzmann equation. Considering three mutually coupled reservoirs, (i) spin-up electrons, (ii) spin-down electrons and (iii) phonons, we trace non-equilibrium electron distributions during and after laser excitation. We identify the driving force for ultrafast magnetization dynamics as the equilibration of temperatures and …
Time-resolved magneto-optical Kerr spectroscopy of ferromagnetic InMnAs reveals two distinct {\em demagnetization} processes -- fast ($<1$ ps) and slow ($\sim$100 ps). Both components diminish with increasing temperature and are absent above the Curie temperature. The fast component rapidly grows with pump power and saturates at high fluences ($>10$ mJ/cm$^2$); the saturation value indicates a {\em complete quenching} of ferromagnetism on a sub-picosecond time scale. We attribute this fast dynamics to spin heating through $p$-$d$ exchange interaction between photo-carriers and Mn ions while th…
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 directly measure the hole spin lifetime in ferromagnetic GaMnAs via time- and polarization-resolved spectroscopy. Below the Curie temperature Tc, an ultrafast photoexcitation with linearly-polarized light is shown to create a non-equilibrium hole spin population via the dynamical polarization of holes through p-d exchange scattering with ferromagnetically-ordered Mn spins, and we characterize their relaxation dynamics. The observed relaxation consists of a distinct three-step recovery : (i) femtosecond (fs) hole spin relaxation ~ $160-200 fs, (ii) picosecond (ps) hole energy relaxation ~ 1-…
Fast spin manipulation in magnetic heterostructures, where magnetic interactions between different materials often define the functionality of devices, is a key issue in the development of ultrafast spintronics. Although recently developed optical approaches such as ultrafast spin-transfer and spin-orbit torques open new pathways to fast spin manipulation, these processes do not fully utilize the unique possibilities offered by interfacial magnetic coupling effects in ferromagnetic multilayer systems. Here, we experimentally demonstrate ultrafast photo-enhanced interfacial exchange interaction…
We measure the transient strain profile in a nanoscale multilayer system composed of Yttrium, Holmium and Niobium after laser excitation using ultrafast X-ray diffraction. The strain propagation through each layer is determined by transient changes of the material-specific Bragg angles. We experimentally derive the exponentially decreasing stress profile driving the strain wave and show that it closely matches the optical penetration depth. Below the Neel temperature of Ho, the optical excitation triggers negative thermal expansion, which is induced by a quasi-instantaneous contractive stress,…
The ultrafast dynamics of the octahedral rotation in Ca:SrTiO3 is studied by time resolved x-ray diffraction after photo excitation over the band gap. By monitoring the diffraction intensity of a superlattice reflection that is directly related to the structural order parameter of the soft-mode driven antiferrodistortive phase in Ca:SrTiO3, we observe a ultrafast relaxation on a 0.2 ps timescale of the rotation of the oxygen octahedron, which is found to be independent of the initial temperaure despite large changes in the corresponding soft-mode frequency. A further, much smaller reduction on…
A decade ago Rhie \et (Phys. Rev. Lett. {\bf 90}, 247201 (2003)) reported that when ferromagnetic nickel is subject to an intense ultrashort laser pulse, its exchange splitting is reduced quickly. But to simulate such reduction remains a big challenge. The popular rigid band approximation (RBA), where both the band structure and the exchange splitting are held fixed before and after laser excitation, is unsuitable for this purpose, while the time-dependent density functional theory could be time-consuming. To overcome these difficulties, we propose a time-dependent Liouville and density functi…
We report the ultrafast optical pump-probe spectroscopy measurements on the recently discovered quantum critical ferromagnet CeRh$_6$Ge$_4$. Our experimental results reveal the two-stage development of the hybridization between localized $f$ moments and conduction electrons with lowering temperature, as evidenced by (1) the presence of hybridization fluctuation for temperatures from $\sim$85 K ($T^*$) to $\sim$140 K ($T^\dagger$), and (2) the emergence of collective hybridization below the coherence temperature, $T^*$, marked by the opening of an indirect gap of 2$Δ$ $\approx$12 meV. We also o…
Room-temperature sub-100 nm Néel-type skyrmions in non-stoichiometric van der Waals ferromagnet $\rm Fe_{3-x}GaTe_{2}$ with ultrafast laser writability
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…
Band bending at semiconductor surfaces induced by chemical doping or electric fields can create metallic surfaces with properties not found in the bulk, such as high electron mobility, magnetism or superconductivity. Optical generation of such metallic surfaces via BB on ultrafast timescales would facilitate a drastic manipulation of the conduction, magnetic and optical properties of semiconductors for high-speed electronics. Here, we demonstrate the ultrafast generation of a metal at the (10-10) surface of ZnO upon photoexcitation. Compared to hitherto known ultrafast photoinduced semiconduct…
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 (TRMOKE). 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-couplin…
Following the demonstration of laser-induced ultrafast demagnetization in ferromagnetic nickel, several theoretical and phenomenological propositions have sought to uncover its underlying physics. In this work we revisit the three temperature model (3TM) and the microscopic three temperature model (M3TM) to perform a comparative analysis of ultrafast demagnetization in 20-nm-thick cobalt, nickel and permalloy thin films measured using an all-optical pump-probe technique. In addition to the ultrafast dynamics at the femtosecond timescales, the nanosecond magnetization precession and damping are…
The out-of-equilibrium dynamics of electrons and phonons upon laser excitation are often described by the two-temperature model, which assumes that both subsystems are separately in thermal equilibrium. However, recent experiments show that this description is not sufficient to describe the out-of-equilibrium dynamics on ultrashort timescales. Here, we extend and apply a parameter-free microscopic out-of-equilibrium model to describe the ultrafast laser-induced system dynamics of archetypical metallic systems such as gold, aluminum, iron, nickel, and cobalt. We report strong deviations from th…
The quasiparticle spectra of atomically thin semiconducting transition metal dichalcogenides (TMDCs) and their response to an ultrafast optical excitation critically depend on interactions with the underlying substrate. Here, we present a comparative time- and angle-resolved photoemission spectroscopy (TR-ARPES) study of the transient electronic structure and ultrafast carrier dynamics in the single- and bilayer TMDCs MoS$_2$ and WS$_2$ on three different substrates: Au(111), Ag(111) and graphene/SiC. The photoexcited quasiparticle bandgaps are observed to vary over the range of 1.9-2.3 eV bet…
The relaxation dynamics of hot carriers in silicon (100) is studied via a novel holistic approach based on phase-resolved transient absorption spectroscopy with few-cycle optical pulses. After excitation by a sub-5 fs light pulse, strong electron-phonon coupling leads to an ultrafast momentum relaxation with time constant of 10 fs. The thermalization of the hot carriers occurs on a time constant of 150 fs, visible in the temporal evolution of the collision time as extracted from the Drude model. We find an increase of the collision time from 3 fs for the shortest timescales with a saturation a…
Understanding how fast short-range interactions build up long-range order is one of the most intriguing topics in condensed matter physics. FeRh is a test specimen for studying this problem in magnetism, where the microscopic spin-spin exchange interaction is ultimately responsible for either ferro- or antiferromagnetic macroscopic order. Femtosecond laser excitation can induce ferromagnetism in antiferromagnetic FeRh, but the mechanism and dynamics of this transition are topics of intense debates. Employing double-pump THz emission spectroscopy has enabled us to dramatically increase the temp…
All-optical spin reversal presents a new opportunity for spin manipulations, free of a magnetic field. Most of all-optical-spin-reversal ferromagnets are found to have a perpendicular magnetic anisotropy (PMA), but it has been unknown whether PMA is necessary for the spin reversal. Here we theoretically investigate magnetic thin films with either PMA or in-plane magnetic anisotropy (IMA). Our results show that the spin reversal in IMA systems is possible, but only with a longer laser pulse and within a narrow laser parameter region. The spin reversal does not show a strong helicity dependence …
We report a computational theoretical investigation of electron spin-flip scattering induced by the electron-phonon interaction in the transition-metal ferromagnets bcc Fe, fcc Co and fcc Ni. The Elliott-Yafet electron-phonon spin-flip scattering is computed from first-principles, employing a generalized spin-flip Eliashberg function as well as ab initio computed phonon dispersions. Aiming at investigating the amount of electron-phonon mediated demagnetization in femtosecond laser-excited ferromagnets, the formalism is extended to treat laser-created thermalized as well as nonequilibrium, nont…
The mechanism of electron-hole separation in organic solar cells is currently hotly debated. Recent experimental work suggests that these charges can separate on extremely short timescales (<100 fs). This can be understood in terms of delocalised transport within fullerene aggregates, which is thought to emerge on short timescales before vibronic relaxation induces polaron formation. However, in the optimal heterojunction morphology, electrons and holes will often re-encounter each other before reaching the electrodes. If such charges trap and cannot separate, then device efficiency will suffe…
Spin valve ultrafast spin injection devices are described: an amplifier, a frequency multiplier, and a square-law detector. Their operation is based on injection of spin polarized electrons from one ferromagnet to another through a semiconductor layer and spin precession of the electrons in the semiconductor layer in a magnetic field induced by a (base) current in an adjacent nanowire. The base current can control the emitter current between the magnetic layers with frequencies up to several 100 GHz.
Black phosphorus is a quasi-two-dimensional layered semiconductor with a narrow direct band gap of 0.3 eV. A giant surface Stark effect can be produced by the potassium doping of black phosphorus, leading to a semiconductor to semimetal phase transition originating from the creation of a strong surface dipole and associated band bending. By using time- and angle-resolved photoemission spectroscopy, we report the partial photoinduced screening of this band bending by the creation of a compensating surface photovoltage. We further resolve the detailed dynamics of this effect at the pertinent tim…
