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.

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.

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.

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.

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.

Transient ferromagnetic-like state mediating ultrafast reversal of antiferromagnetically coupled spins.

Ferromagnetic or antiferromagnetic spin ordering is governed by the exchange interaction, the strongest force in magnetism. Understanding spin dynamics in magnetic materials is an issue of crucial importance for progress in information processing and recording technology. Usually the dynamics are studied by observing the collective response of exchange-coupled spins, that is, spin resonances, after an external perturbation by a pulse of magnetic field, current or light. The periods of the corresponding resonances range from one nanosecond for ferromagnets down to one picosecond for antiferromagnets. However, virtually nothing is known about the behaviour of spins in a magnetic material after being excited on a timescale faster than that corresponding to the exchange interaction (10-100 fs), that is, in a non-adiabatic way. Here we use the element-specific technique X-ray magnetic circular dichroism to study spin reversal in GdFeCo that is optically excited on a timescale pertinent to the characteristic time of the exchange interaction between Gd and Fe spins. We unexpectedly find that the ultrafast spin reversal in this material, where spins are coupled antiferromagnetically, occurs by way of a transient ferromagnetic-like state. Following the optical excitation, the net magnetizations of the Gd and Fe sublattices rapidly collapse, switch their direction and rebuild their net magnetic moments at substantially different timescales; the net magnetic moment of the Gd sublattice is found to reverse within 1.5 picoseconds, which is substantially slower than the Fe reversal time of 300 femtoseconds. Consequently, a transient state characterized by a temporary parallel alignment of the net Gd and Fe moments emerges, despite their ground-state antiferromagnetic coupling. These surprising observations, supported by atomistic simulations, provide a concept for the possibility of manipulating magnetic order on the timescale of the exchange interaction.

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.

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.

Nanoscale spin reversal by non-local angular momentum transfer following ultrafast laser excitation in ferrimagnetic GdFeCo.

Ultrafast laser techniques have revealed extraordinary spin dynamics in magnetic materials that equilibrium descriptions of magnetism cannot explain. Particularly important for future applications is understanding non-equilibrium spin dynamics following laser excitation on the nanoscale, yet the limited spatial resolution of optical laser techniques has impeded such nanoscale studies. Here we present ultrafast diffraction experiments with an X-ray laser that probes the nanoscale spin dynamics following optical laser excitation in the ferrimagnetic alloy GdFeCo, which exhibits macroscopic all-optical switching. Our study reveals that GdFeCo displays nanoscale chemical and magnetic inhomogeneities that affect the spin dynamics. In particular, we observe Gd spin reversal in Gd-rich nanoregions within the first picosecond driven by the non-local transfer of angular momentum from larger adjacent Fe-rich nanoregions. These results suggest that a magnetic material's microstructure can be engineered to control transient laser-excited spins, potentially allowing faster (~ 1 ps) spin reversal than in present technologies.

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.

Element-specific probing of ultrafast spin dynamics in multisublattice magnets with visible light.

We demonstrate the feasibility of element-specific probing of ultrafast spin dynamics in the multisublattice magnet TbFe in the visible spectral range. In particular, we show that one can selectively study the dynamics of Tb and Fe sublattices choosing the wavelength of light below and above 610 nm, respectively. We observe that, despite their antiferromagnetic coupling in the ground state, the Tb and Fe spins temporarily align ferromagnetically after excitation with an intense 55-fs laser pulse, after which they relax to their initial states due to the strong anisotropy in Tb.

Laser-induced magnetic nanostructures with tunable topological properties.

We report the creation and real-space observation of magnetic structures with well-defined topological properties and a lateral size as low as about 150 nm. They are generated in a thin ferrimagnetic film by ultrashort single optical laser pulses. Thanks to their topological properties, such structures can be classified as Skyrmions of a particular type that does not require an externally applied magnetic field for stabilization. Besides Skyrmions, we are able to generate magnetic features with topological characteristics that can be tuned by changing the laser fluence. The stability of such features is accounted for by an analytical model based on the interplay between the exchange and the magnetic dipole-dipole interactions.

Role of magnetic circular dichroism in all-optical magnetic recording.

Using magneto-optical microscopy in combination with ellipsometry measurements, we show that all-optical switching with polarized femtosecond laser pulses in ferrimagnetic GdFeCo is subjected to a threshold fluence absorbed in the magnetic layer, independent of either the excitation wavelength or the polarization of the laser pulse. Furthermore, we present a quantitative explanation of the intensity window in which all-optical helicity-dependent switching (AO-HDS) occurs, based on magnetic circular dichroism. This explanation is consistent with all the experimental findings on AO-HDS so far, varying from single- to multiple-shot experiments. The presented results give a solid understanding of the origin of AO-HDS, and give novel insights into the physics of ultrafast, laser controlled magnetism.

Ultrafast spin dynamics in multisublattice magnets.

We propose a general theoretical framework for ultrafast laser-induced spin dynamics in multisublattice magnets. We distinguish relaxation of relativistic and exchange origin and show that when the former dominates, nonequivalent sublattices have distinct dynamics despite their strong exchange coupling. Even more interesting, in the exchange dominated regime sublattices can show highly counterintuitive transitions between parallel and antiparallel alignment. This allows us to explain recent experiments with antiferromagnetically coupled sublattices, and predict that such transitions are possible with ferromagnetic coupling as well. In addition, we predict that exchange relaxation enhances the demagnetization speed of both sublattices only when they are antiferromagnetically coupled.

Coherent control of the route of an ultrafast magnetic phase transition via low-amplitude spin precession.

Time-resolved magneto-optical imaging of laser-excited rare-earth orthoferrite (SmPr)FeO3 demonstrates that a single 60 fs circularly polarized laser pulse is capable of creating a magnetic domain on a picosecond time scale with a magnetization direction determined by the helicity of light. Depending on the light intensity and sample temperature, pulses of the same helicity can create domains with opposite magnetizations. We argue that this phenomenon relies on a twofold effect of light which (i) instantaneously excites coherent low-amplitude spin precession and (ii) triggers a spin reorientation phase transition. The former dynamically breaks the equivalence between two otherwise degenerate states with opposite magnetizations in the high-temperature phase and thus controls the route of the phase transition.

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.

Femtosecond laser excitation of spin resonances in amorphous ferrimagnetic Gd(1-x)Co(x) alloys.

Using 100 fs laser pulses, a high-frequency exchange and a low-frequency ferromagnetic resonance mode have been excited and detected in an amorphous Gd(1-x)Co(x) (78≤x≤85) ferrimagnetic thin film, on both sides of its angular momentum compensation composition. The excitation efficiency of these modes strongly depends on the amount of laser-induced heating. Ways of selectively and efficiently exciting either one or both of these two coexisting magnetic modes by adjusting laser pulse intensity are demonstrated.

Ultrafast non-thermal control of magnetization by instantaneous photomagnetic pulses.

The demand for ever-increasing density of information storage and speed of manipulation has triggered an intense search for ways to control the magnetization of a medium by means other than magnetic fields. Recent experiments on laser-induced demagnetization and spin reorientation use ultrafast lasers as a means to manipulate magnetization, accessing timescales of a picosecond or less. However, in all these cases the observed magnetic excitation is the result of optical absorption followed by a rapid temperature increase. This thermal origin of spin excitation considerably limits potential applications because the repetition frequency is limited by the cooling time. Here we demonstrate that circularly polarized femtosecond laser pulses can be used to non-thermally excite and coherently control the spin dynamics in magnets by way of the inverse Faraday effect. Such a photomagnetic interaction is instantaneous and is limited in time by the pulse width (approximately 200 fs in our experiment). Our finding thus reveals an alternative mechanism of ultrafast coherent spin control, and offers prospects for applications of ultrafast lasers in magnetic devices.

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.

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.