Ultrafast kinetics of the antiferromagnetic-ferromagnetic phase transition in FeRh.

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 temporal detection window of THz emission probes of transient states without sacrificing any loss of resolution or sensitivity. It allows us to study the kinetics of emergent ferromagnetism from the femtosecond up to the nanosecond timescales in FeRh/Pt bilayers. Our results strongly suggest a latency period between the initial pump-excitation and the emission of THz radiation by ferromagnetic nuclei.

All-optical spin switching probability in [Tb/Co] multilayers.

Since the first experimental observation of all-optical switching phenomena, intensive research has been focused on finding suitable magnetic systems that can be integrated as storage elements within spintronic devices and whose magnetization can be controlled through ultra-short single laser pulses. We report here atomistic spin simulations of all-optical switching in multilayered structures alternating n monolayers of Tb and m monolayers of Co. By using a two temperature model, we numerically calculate the thermal variation of the magnetization of each sublattice as well as the magnetization dynamics of [[Formula: see text]/[Formula: see text]] multilayers upon incidence of a single laser pulse. In particular, the condition to observe thermally-induced magnetization switching is investigated upon varying systematically both the composition of the sample (n,m) and the laser fluence. The samples with one monolayer of Tb as [[Formula: see text]/[Formula: see text]] and [[Formula: see text]/[Formula: see text]] are showing thermally induced magnetization switching above a fluence threshold. The reversal mechanism is mediated by the residual magnetization of the Tb lattice while the Co is fully demagnetized in agreement with the models developed for ferrimagnetic alloys. The switching is however not fully deterministic but the error rate can be tuned by the damping parameter. Increasing the number of monolayers the switching becomes completely stochastic. The intermixing at the Tb/Co interfaces appears to be a promising way to reduce the stochasticity. These results predict for the first time the possibility of TIMS in [Tb/Co] multilayers and suggest the occurrence of sub-picosecond magnetization reversal using single laser pulses.

Sub-picosecond exchange-relaxation in the compensated ferrimagnet Mn2Ru x Ga.

We study the demagnetization dynamics of the fully compensated half-metallic ferrimagnet Mn2Ru x Ga. While the two antiferromagnetically coupled sublattices are both composed of manganese, they exhibit different temperature dependencies due to their differing local environments. The sublattice magnetization dynamics triggered by femtosecond laser pulses are studied to reveal the roles played by the spin and intersublattice exchange. We find a two-step demagnetization process, similar to the well-established case of Gd(FeCo)3, where on a 5 ps timescale the two Mn-sublattices seem to have different demagnetization rates. The behaviour is analysed using a four-temperature model, assigning different temperatures to the two manganese spin baths. Even in this strongly exchange-coupled system, the two spin reservoirs have considerably different behaviour. The half-metallic nature and strong exchange coupling of Mn2Ru x Ga lead to spin angular momentum conservation at much shorter time scales than found for Gd(FeCo)3 which suggests that low-power, sub-picosecond switching of the net moment of Mn2Ru x Ga is possible.

Controlling magnetic domain wall velocity by femtosecond laser pulses.

Using the technique of double high-speed photography, we find that a femtosecond laser pulse is able to change the velocity of a moving domain wall in an yttrium iron garnet. The change depends on the light intensity and the domain wall velocity itself. To explain the results we propose a model in which the domain wall velocity is controlled by photo-induced generation of vertical Bloch lines.

Resonant Pumping of d-d Crystal Field Electronic Transitions as a Mechanism of Ultrafast Optical Control of the Exchange Interactions in Iron Oxides.

The microscopic origin of ultrafast modification of the ratio between the symmetric (J) and antisymmetric (D) exchange interaction in antiferromagnetic iron oxides is revealed, using femtosecond laser excitation as a pump and terahertz emission spectroscopy as a probe. By tuning the photon energy of the laser pump pulse we show that the effect of light on the D/J ratio in two archetypical iron oxides FeBO_{3} and ErFeO_{3} is maximized when the photon energy is in resonance with a spin and parity forbidden d-d transition between the crystal-field split states of Fe^{3+} ions. The experimental findings are supported by a multielectron model, which accounts for the resonant absorption of photons by Fe^{3+} ions. Our results reveal the importance of the parity and spin-change forbidden, and therefore often underestimated, d-d transitions in ultrafast optical control of magnetism.

Single-shot all-optical switching of magnetization in Tb/Co multilayer-based electrodes.

Ever since the first observation of all-optical switching of magnetization in the ferrimagnetic alloy GdFeCo using femtosecond laser pulses, there has been significant interest in exploiting this process for data-recording applications. In particular, the ultrafast speed of the magnetic reversal can enable the writing speeds associated with magnetic memory devices to be potentially pushed towards THz frequencies. This work reports the development of perpendicular magnetic tunnel junctions incorporating a stack of Tb/Co nanolayers whose magnetization can be all-optically controlled via helicity-independent single-shot switching. Toggling of the magnetization of the Tb/Co electrode was achieved using either 60 femtosecond-long or 5 picosecond-long laser pulses, with incident fluences down to 3.5 mJ/cm2, for Co-rich compositions of the stack either in isolation or coupled to a CoFeB-electrode/MgO-barrier tunnel-junction stack. Successful switching of the CoFeB-[Tb/Co] electrodes was obtained even after annealing at 250 °C. After integration of the [Tb/Co]-based electrodes within perpendicular magnetic tunnel junctions yielded a maximum tunneling magnetoresistance signal of 41% and RxA value of 150 Ωµm2 with current-in-plane measurements and ratios between 28% and 38% in nanopatterned pillars. These results represent a breakthrough for the development of perpendicular magnetic tunnel junctions controllable using single laser pulses, and offer a technologically-viable path towards the realization of hybrid spintronic-photonic systems featuring THz switching speeds.

Terahertz Optomagnetism: Nonlinear THz Excitation of GHz Spin Waves in Antiferromagnetic FeBO_{3}.

A nearly single cycle intense terahertz (THz) pulse with peak electric and magnetic fields of 0.5 MV/cm and 0.16 T, respectively, excites both modes of spin resonances in the weak antiferromagnet FeBO_{3}. The high frequency quasiantiferromagnetic mode is excited resonantly and its amplitude scales linearly with the strength of the THz magnetic field, whereas the low frequency quasiferromagnetic mode is excited via a nonlinear mechanism that scales quadratically with the strength of the THz electric field and can be regarded as a THz inverse Cotton-Mouton effect. THz optomagnetism is shown to be more energy efficient than similar effects reported previously for the near-infrared spectral range.

Spin-current-mediated rapid magnon localisation and coalescence after ultrafast optical pumping of ferrimagnetic alloys.

Sub-picosecond magnetisation manipulation via femtosecond optical pumping has attracted wide attention ever since its original discovery in 1996. However, the spatial evolution of the magnetisation is not yet well understood, in part due to the difficulty in experimentally probing such rapid dynamics. Here, we find evidence of a universal rapid magnetic order recovery in ferrimagnets with perpendicular magnetic anisotropy via nonlinear magnon processes. We identify magnon localisation and coalescence processes, whereby localised magnetic textures nucleate and subsequently interact and grow in accordance with a power law formalism. A hydrodynamic representation of the numerical simulations indicates that the appearance of noncollinear magnetisation via optical pumping establishes exchange-mediated spin currents with an equivalent 100% spin polarised charge current density of 107 A cm-2. Such large spin currents precipitate rapid recovery of magnetic order after optical pumping. The magnon processes discussed here provide new insights for the stabilization of desired meta-stable states.

Anomalously Damped Heat-Assisted Route for Precessional Magnetization Reversal in an Iron Garnet.

A heat-assisted route for subnanosecond magnetic recording is discovered for the dielectric bismuth-substituted yttrium iron garnet, known for possessing small magnetic damping. The experiments and simulations reveal that the route involves nonlinear magnetization precession, triggered by a transient thermal modification of the growth-induced crystalline anisotropy in the presence of a fixed perpendicular magnetic field. The pathway is rendered robust by the damping becoming anomalously large during the switching process. Subnanosecond deterministic magnetization reversal was achieved within just one-half of a precessional period, and this mechanism should be possible to implement in any material with suitably engineered dissimilar thermal derivatives of magnetization and anisotropy.

Femtosecond single-shot imaging and control of a laser-induced first-order phase transition in HoFeO3.

Excitation of antiferromagnetic HoFeO3 with a single 80 fs laser pulse triggers a first-order spin-reorientation phase transition. In the ultrafast kinetics of the transition one can distinguish the processes of impulsive excitation of spin precession, nucleation of the new domain and growth of the nuclei. The orientation of the spins in the nuclei is defined by the phase of the laser-induced coherent spin precession. The growth of the nuclei is further promoted by heating induced by the laser excitation. Hereby we demonstrate that in HoFeO3 coherent control of the spin precession allows an effective control of the route of the heat-induced first-order magnetic phase transition. The theoretical description of the excitation of the spin precession by linearly-polarized ultrashort laser pulses is developed with the sigma model. The analysis showed high sensitivity of the excited dynamics to the initial spin orientations with respect to the crystallographic axes of the material.

Ultrafast Magnetism of a Ferrimagnet across the Spin-Flop Transition in High Magnetic Fields.

We show that applying magnetic fields up to 30 T has a dramatic effect on the ultrafast spin dynamics in ferrimagnetic GdFeCo. Upon increasing the field beyond a critical value, the dynamics induced by a femtosecond laser excitation strongly increases in amplitude and slows down significantly. Such a change in spin response is explained by different dynamics of the Gd and FeCo magnetic sublattices following a spin-flop phase transition from a collinear to a noncollinear spin state.

Effect of laser pulse propagation on ultrafast magnetization dynamics in a birefringent medium.

Light propagation effects can strongly influence the excitation and the detection of laser-induced magnetization dynamics. We investigated experimentally and analytically the effects of crystallographic linear birefringence on the excitation and detection of ultrafast magnetization dynamics in the rare-earth orthoferrites (Sm0.5Pr0.5)FeO3 and (Sm0.55Tb0.45)FeO3, which possess weak and strong linear birefringence, respectively. Our finding is that the effect of linear birefringence on the result of a magneto-optical pump-probe experiment strongly depends on the mechanism of excitation. When magnetization dynamics, probed by means of the Faraday effect, is excited via a rapid, heat-induced phase transition, the measured rotation of the probe pulse polarization is strongly suppressed due to the birefringence. This contrasts with the situation for magnetization dynamics induced by the ultrafast inverse Faraday effect, where the corresponding probe polarization rotation values were larger in the orthoferrite with strong linear birefringence. We show that this striking difference results from an interplay between the polarization transformations experienced by pump and probe pulses in the birefringent medium.

Selective Excitation of Terahertz Magnetic and Electric Dipoles in Er

We show that femtosecond laser pulse excitation of the orthoferrite ErFeO_{3} triggers pico- and subpicosecond dynamics of magnetic and electric dipoles associated with the low energy electronic states of the Er^{3+} ions. These dynamics are readily revealed by using polarization sensitive terahertz emission spectroscopy. It is shown that by changing the polarization of the femtosecond laser pulse one can excite either electric dipole-active or magnetic dipole-active transitions between the Kramers doublets of the ^{4}I_{15/2} ground state of the Er^{3+} (4f^{11}) ions. These observations serve as a proof of principle of polarization-selective control of both electric and magnetic degrees of freedom at terahertz frequencies, opening up new vistas for optical manipulation of magnetoelectric materials.

Control of the Ultrafast Photoinduced Magnetization across the Morin Transition in DyFeO_{3}.

Excitation of the collinear compensated antiferromagnet DyFeO_{3} with a single 60 fs laser pulse triggers a phase transition across the Morin point into a noncollinear spin state with a net magnetization. Time-resolved imaging of the magnetization dynamics of this process reveals that the pulse first excites the spin oscillations upon damping of which the noncollinear spin state emerges. The sign of the photoinduced magnetization is defined by the relative orientation of the pump polarization and the direction of the antiferromagnetic vector in the initial collinear spin state.

Femtosecond control of electric currents in metallic ferromagnetic heterostructures.

The idea to use not only the charge but also the spin of electrons in the operation of electronic devices has led to the development of spintronics, causing a revolution in how information is stored and processed. A novel advancement would be to develop ultrafast spintronics using femtosecond laser pulses. Employing terahertz (10(12) Hz) emission spectroscopy and exploiting the spin-orbit interaction, we demonstrate the optical generation of electric photocurrents in metallic ferromagnetic heterostructures at the femtosecond timescale. The direction of the photocurrent is controlled by the helicity of the circularly polarized light. These results open up new opportunities for realizing spintronics in the unprecedented terahertz regime and provide new insights in all-optical control of magnetism.

Macrospin dynamics in antiferromagnets triggered by sub-20 femtosecond injection of nanomagnons.

The understanding of how the sub-nanoscale exchange interaction evolves in macroscale correlations and ordered phases of matter, such as magnetism and superconductivity, requires to bridging the quantum and classical worlds. This monumental challenge has so far only been achieved for systems close to their thermodynamical equilibrium. Here we follow in real time the ultrafast dynamics of the macroscale magnetic order parameter in the Heisenberg antiferromagnet KNiF3 triggered by the impulsive optical generation of spin excitations with the shortest possible nanometre wavelength and femtosecond period. Our magneto-optical pump-probe experiments also demonstrate the coherent manipulation of the phase and amplitude of these femtosecond nanomagnons, whose frequencies are defined by the exchange energy. These findings open up opportunities for fundamental research on the role of short-wavelength spin excitations in magnetism and strongly correlated materials; they also suggest that nanospintronics and nanomagnonics can employ coherently controllable spin waves with frequencies in the 20 THz domain.

Ultrafast optical modification of exchange interactions in iron oxides.

Ultrafast non-thermal manipulation of magnetization by light relies on either indirect coupling of the electric field component of the light with spins via spin-orbit interaction or direct coupling between the magnetic field component and spins. Here we propose a scenario for coupling between the electric field of light and spins via optical modification of the exchange interaction, one of the strongest quantum effects with strength of 10(3) Tesla. We demonstrate that this isotropic opto-magnetic effect, which can be called inverse magneto-refraction, is allowed in a material of any symmetry. Its existence is corroborated by the experimental observation of terahertz emission by spin resonances optically excited in a broad class of iron oxides with a canted spin configuration. From its strength we estimate that a sub-picosecond modification of the exchange interaction by laser pulses with fluence of about 1 mJ cm(-2) acts as a pulsed effective magnetic field of 0.01 Tesla.

Strong thermo-induced single and two-photon green luminescence in self-organized peptide microtubes.

Diphenylalanine peptide nano- and microtubes formed by self-assembly demonstrate strongly enhanced and tunable single-photon and two-photon luminescence in the visible range, which appears after heat- or laser treatment of these self-organized peptide microtubes. This process significantly extends the functionality of these microstructures and can trigger a new interest in the optical properties of structures based on short peptides.

Ultrafast time-resolved magneto-optical imaging of all-optical switching in GdFeCo with femtosecond time-resolution and a µm spatial-resolution.

We developed an ultrafast time-resolved magneto-optical (MO) imaging system with several millidegree resolution of light polarization angle, 100 fs time-resolution, and a micrometer spatial resolution. A CCD camera with about 10(6) pixels is used for detection and MO images with an absolute angle of the light polarization are acquired by the rotating analyzer method. By optimizing the analysis procedure with a least square method and the help of graphical processor units, this novel system significantly improves the speed for MO imaging, allowing to obtain a MO map of a sample within 15 s. To demonstrate the strength of the technique, we applied the method in a pump-and-probe experiment of all-optical switching in a GdFeCo sample in which we were able to detect temporal evolution of the MO images with sub-picosecond resolution.

Laser excitation of lattice-driven anharmonic magnetization dynamics in dielectric FeBO3.

Femtosecond laser pulses trigger in dielectric FeBO3 coherent oscillations of the magnetic anisotropy followed by spins. The oscillations are driven by optically excited lattice vibrations strongly coupled to the magnetic system. Unlike the spin resonances, this mode is characterized by a very small damping ratio and can be easily pushed into an anharmonic regime.