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 concluded that the maximum relative demagnetization amplitude, which corresponds to the highest photon conversion into hot-electrons, is an interplay between the IR penetration depth and the hot-electron inelastic mean free path within the capping layer.
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.
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.
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…
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 t…
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…
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 …
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…
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…
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
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 …
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…
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…
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…
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…
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 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…
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…
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…
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…
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 lattice deformation of tens to hundreds of nanometer thick metallic crystals, after femtosecond laser excitation, was measured directly using 8.04 keV subpicosecond x-ray and 59 keV femtosecond electron pulses. Coherent phonons were generated in both single crystal and polycrystalline films. Lattice compression was observed within the first few picoseconds after laser irradiation in single crystal aluminum, which was attributed to the generation of a blast force and the propagation of elastic waves. The different time scale of lattice heating for tens and hundreds nanometer thick fil…
We have studied ultrafast photoinduced demagnetization in GaMnAs via two-color time-resolved magneto-optical Kerr spectroscopy. Below-bandgap midinfrared pump pulses strongly excite the valence band, while near-infrared probe pulses reveal sub-picosecond demagnetization that is followed by an ultrafast ($\sim$1 ps) partial recovery of the Kerr signal. Through comparison with InMnAs, we attribute the signal recovery to an ultrafast energy relaxation of holes. We propose that the dynamical polarization of holes through $p$-$d$ scattering is the source of the observed probe signal. These results …
The mechanism underlying femtosecond laser pulse induced ultrafast magnetization dynamics remains elusive despite two decades of intense research on this phenomenon. Most experiments focused so far on characterizing magnetization and charge carrier dynamics, while first direct measurements of structural dynamics during ultrafast demagnetization were reported only very recently. We here present our investigation of the infrared laser pulse induced ultrafast demagnetization process in a thin Ni film, which characterizes simultaneously magnetization and structural dynamics. This is achieved by em…
Ultrafast control of magnetization on the nanometer length scale, in particular all-optical switching, is key to putting ultrafast magnetism on the path towards future technological application in data storage technology. However, magnetization manipulation with light on this length scale is challenging due to the wavelength limitations of optical radiation. Here, we excite transient magnetic gratings in a GdFe alloy with a periodicity of 87 nm by interference of two coherent femtosecond light pulses in the extreme ultraviolet spectral range at the free electron laser facility FERMI. The subse…
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…
The investigation of ultrafast electronic and structural dynamics in low-dimensional systems like nanowires and two-dimensional materials requires femtosecond probes providing high spatial resolution and strong interaction with small volume samples. Low-energy electrons exhibit large scattering cross sections and high sensitivity to electric fields, but their pronounced dispersion during propagation in vacuum so far prevented their use as femtosecond probe pulses in time-resolved experiments. Employing a laser-triggered point-like source of either divergent or collimated electron wave packets,…
Controlling ultrafast magnetization dynamics by a femtosecond laser is attracting interest both in fundamental science and industry because of the potential to achieve magnetic domain switching at ever advanced speed. Here we report experiments illustrating the ultrastrong and fully coherent light-matter coupling of a high-field single-cycle THz transient to the magnetization vector in a ferromagnetic thin film. We could visualize magnetization dynamics which occur on a timescale of the THz laser cycle and two orders of magnitude faster than the natural precession response of electrons to an e…
Irradiation of solids with ultrashort pulses using laser sources in the mid-infrared (mid-IR) spectral region is a yet predominantly unexplored field that opens broad possibilities for efficient and precise surface texturing for a wide range of applications. In the present work, we investigate both experimentally and theoretically the impact of laser sources on the generation of surface modification related effects and on the subsequent surface patterning of metallic and semiconducting materials. Through a parametric study we correlate the mid-IR pulsed laser parameters with the onset of mater…
The injection of spin currents in semiconductors is one of the big challenges of spintronics. Motivated by the ultrafast demagnetisation and spin injection into metals, we propose an alternative femtosecond route based on the laser excitation of superdiffusive spin currents in a ferromagnet such as Ni. Our calculations show that even though only a fraction of the current crosses the Ni-Si interface, the laser-induced creation of strong transient electrical fields at a ferromagnet-semiconductor interface allows for the injection of chargeless spin currents with a record spin polarisations of 80…
We present a theoretical investigation of the yet unexplored ultrafast processes and dynamics of the produced excited carriers upon irradiation of Silicon with femtosecond pulsed lasers in the mid-infrared (mid-IR) spectral region. The evolution of the carrier density and thermal response of the electron-hole and lattice subsystems are analysed for various wavelengths λL in the range between 2.2 μm and 3.3 μm where the influence of two and three-photon absorption mechanisms is explored. The role of induced Kerr effect is highlighted and it manifests a more pronounced influence at smaller wavel…
Carrier scattering processes are studied in CH$_3$NH$_3$PbI$_3$ using temperature-dependent four-wave mixing experiments. Our results indicate that scattering by ionized impurities limits the interband dephasing time (T$_2$) below 30~K, with strong electron-phonon scattering dominating at higher temperatures (with a timescale of 125 fs at 100 K). Our theoretical simulations provide quantitative agreement with the measured carrier scattering rate and show that the rate of acoustic phonon scattering is enhanced by strong spin-orbit coupling, which modifies the band-edge density of states. The Ra…
The spin dynamics in Ni is studied by an exact diagonalization method on the ultrafast time scale. It is shown that the femtosecond relaxation of the magneto-optical response results from exchange interaction and spin-orbit coupling. Each of the two mechanisms affects the relaxation process differently. We find that the intrinsic spin dynamics occurs during about 10 fs while extrinsic effects such as laser-pulse duration and spectral width can slow down the observed dynamics considerably. Thus, our theory indicates that there is still room to accelerate the spin dynamics in experiments.
Although ultrafast laser materials processing has advanced at a breakneck pace over the last two decades, most applications have been developed with laser pulses at near-IR or visible wavelengths. Recent progress in mid-infrared (MIR) femtosecond laser source development may create novel capabilities for material processing. This is because, at high intensities required for such processing, wavelength tuning to longer wavelengths opens the pathway to a special regime of laser-solid interactions. Under these conditions, due to the $λ^2$ scaling, the ponderomotive energy of laser-driven electron…
Irradiation with an ultrashort laser pulse can completely destroy the magnetic order of ferromagnetic thin films on the femtosecond timescale. This phenomenon holds great potential for ultrafast spintronics and information processing and is an active field of research. It is still an open question if the angular momentum of light can support this effect. While it has been shown that the spin of light only has a negligible influence, we experimentally demonstrate the influence of ultrashort laser pulses with orbital angular momentum (OAM) on the magnetization dynamics of a thin nickel film. Our…
Fundamental interactions induced by lattice vibrations on ultrafast time scales become increasingly important for modern nanoscience and technology. Experimental access to the physical properties of acoustic phonons in the THz frequency range and over the entire Brillouin zone is crucial for understanding electric and thermal transport in solids and their compounds. Here, we report on the generation and nonlinear propagation of giant (1 percent) acoustic strain pulses in hybrid gold/cobalt bilayer structures probed with ultrafast surface plasmon interferometry. This new technique allows for un…
The use of femtosecond laser pulses to impulsively excite thermal and mechanical transients in matter has led, in the last years, to the development of picosecond acoustics. Recently, the pump-probe approach has been applied to nano-engineered materials to optically generate and detect acoustic waves in the GHz-THz frequency range. In this paper, we review the latest advances on ultrafast generation and detection of thermal gradients and pseudo-surface acoustic waves in two-dimensional lattices of metallic nanostructures. Comparing the experimental findings to the numeric analysis of the full …
We compare femtosecond pump-probe experiments in Ni and micromagnetic modelling based on the Landau-Lifshitz-Bloch equation coupled to a two-temperature model, revealing a predominant thermal ultrafast demagnetization mechanism. We show that both spin (femtosecond demagnetization) and electron-phonon (magnetization recovery) rates in Ni increase as a function of the laser pump fluence. The slowing down for high fluences arises from the increased longitudinal relaxation time.
Microwave treated water soluble and amide functionalized single walled carbon nanotubes have been investigated using femtosecond degenerate pump-probe and nonlinear transmission experiments. The time resolved differential transmission using 75 femtosecond pulse with the central wavelength of 790 nm shows a bi-exponential ultrafast photo-bleaching with time constants of of 160 fs (130 fs) and 920 fs (300 fs) for water soluble (amide functionalized) nanotubes. Open and closed aperture z-scans show saturation absorption and positive (negative) nonlinear refraction for water soluble (amide functio…
