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Finding methods for the most efficient and fastest detection and control of magnetic domains in antiferromagnets is presently among the main challenges of magnetic research at large. We analyse the problem of optical read-out and control of the antiferromagnetic Neel vector using symmetry analysis and the principles of equilibrium thermodynamics. Following the pioneering approach of Dzyaloshinksii, we divide all antiferromagnets in three classes. It is shown that, using the magneto-optical Faraday effect or other effects which scale linearly with the antiferromagnetic Neel vector, it is possible to distinguish antiferromagnetic domains with mutually opposite N\'eel vectors in two of the three classes. Symmetry properties of one of these two classes are similar to those of altermagnets. The analysis also reveals multiple mechanisms to directly excite spins with light for practically every type of antiferromagnet.

A pair of circularly polarized laser pulses of opposite helicities are shown to control the route of spin reorientation phase transition in rare-earth antiferromagnetic orthoferrite (Sm$_{0.55}$Tb$_{0.45}$)FeO$_3$. The route can be efficiently controlled by the delay between the pulses and the sample temperature. Simulations employing previously published models of \mbox{laser-induced} spin dynamics in orthoferrites failed to reproduce the experimental results. We suggest that the failure is due to neglected temperature dependence of the antiferromagnetic resonance damping in the material. Taking into account the experimentally deduced temperature dependence of the damping, we obtained good agreement between the simulations and the experiment., Comment: 5 pages, 6 figures

It is found that subtle changes in the external magnetic field and temperature result in dramatic changes in the ultrafast response of spins to a femtosecond laser excitation in a ferrimagnetic Gd/FeCo multilayer. A total of six distinct types of spin dynamics were observed and explained by considering the spin-flop transition to the noncollinear phase and the concept of a tricritical point in the $H$-$T$ phase diagram. A particularly interesting type of dynamics is the exchange-driven reversal. These exchange-driven dynamics provide new insights into the tricritical point, which is shown to separate two thermodynamically distinct noncollinear phases with the transition-metal magnetization pointing on adjacent sides of the anisotropy plane., Comment: 21 pages, 11 figures

While in accordance with Curie's principle, one would intuitively expect that symmetry of the cause has to be found in the symmetry of the effect, ultrafast excitation of matter is able to violate this principle. For instance, it is believed that heating alone, obviously not having the symmetry of a magnetic field, cannot result in a deterministic reversal of magnetization. However, if the heating is induced by a femtosecond laser pulse and thus ultrafast, it does facilitate toggle switching of magnetization between stable bit-states without any magnetic field at all. Here we show that the regime of ultrafast toggle switching can be also realized via a mechanism without relying on any heat. The obvious mismatch between symmetries of the cause and the response can thus be seen as a violation of Curie's principle. In particular, ultrafast laser excitation of iron-garnet with linearly polarized light modifies magnetic anisotropy and thus causes toggling magnetization between two stable bit states. In contrast to the laser-heat-induced magnetization reversal, this new regime of 'cold' toggle switching can be observed in ferrimagnets without the compensation point and in an exceptionally broad temperature range. The control of magnetic anisotropy required for the toggle switching is accompanied by lower dissipations, than in the mechanism of laser-induced-heating, but the dissipations and the switching-time are shown to be competing parameters., Comment: 11 pages, 6 figures

Understanding spin-lattice interactions in antiferromagnets is one of the most fundamental issues at the core of the recently emerging and booming fields of antiferromagnetic spintronics and magnonics. Recently, coherent nonlinear spin-lattice coupling was discovered in an antiferromagnet which opened the possibility to control the nonlinear coupling strength and thus showing a novel pathway to coherently control magnon-phonon dynamics. Here, utilizing intense narrow band terahertz (THz) pulses and tunable magnetic fields up to 7 T, we experimentally realize the conditions of the Fermi magnon-phonon resonance in antiferromagnetic $CoF_{2}$. These conditions imply that both the spin and the lattice anharmonicities harvest energy transfer between the subsystems, if the magnon eigenfrequency $f_{m}$ is twice lower than the frequency of the phonon $2f_{m}=f_{ph}$. Performing THz pump-infrared probe spectroscopy in conjunction with simulations, we explore the coupled magnon-phonon dynamics in the vicinity of the Fermi-resonance and reveal the corresponding fingerprints of an impulsive THz-induced response. This study focuses on the role of nonlinearity in spin-lattice interactions, providing insights into the control of coherent magnon-phonon energy exchange.

The Barnett effect, discovered more than a century ago, describes how an inertial body with otherwise zero net magnetic moment acquires spontaneous magnetization when mechanically spinning. Breakthrough experiments have recently shown that an ultrashort laser pulse destroys the magnetization of an ordered ferromagnet within hundreds of femtoseconds, with the spins losing angular momentum to circularly-polarized optical phonons as part of the ultrafast Einstein-de Haas effect. However, the prospect of using such high-frequency vibrations of the lattice to reciprocally switch magnetization in a nearby magnetic medium has not yet been experimentally explored. Here we show that the spontaneous magnetization temporarily gained via the ultrafast Barnett effect, through the resonant excitation of circularly-polarized optical phonons in paramagnetic substrates, can be used to permanently reverse the magnetic state of the substrate-mounted heterostructure. With the handedness of the phonons steering the direction of magnetic switching, the ultrafast Barnett effect offers a selective and potentially universal method for exercising ultrafast non-local control over magnetic order., Comment: Total of 31 pages and 17 figures (main text and supplementary information)

It is found that single-cycle THz electromagnetic fields efficiently excite a GHz spin resonance mode in ferrimagnetic Tm$_3$Fe$_5$O$_{12}$, despite the near absence of GHz spectral components in the exciting THz pulse. By analyzing how the efficiency of excitation depends on the orientation and strength of the THz electric field, we show that it can be explained in terms of the nonlinear THz inverse Cotton-Mouton effect. Here, the THz electric field gets effectively rectified and acts on the ferrimagnetic spins as a uni-polar effective magnetic field pulse. This interpretation is confirmed by a theoretical model based on the phenomenological analysis of the effective magnetic field, combined with the equations of motion derived from the effective Lagrangian for a ferrimagnet. Moreover, by using the outcome of two-dimensional THz spectroscopy, we conjecture a quantum-mechanical interpretation of the observed effect in terms of stimulated Raman scattering of THz photons by the crystal-field split f-f electronic transitions of Tm$^{3+}$., Comment: 15 pages, 9 figures

Controlled generation of coherent spin waves with highest possible frequencies and the shortest possible wavelengths is a cornerstone of spintronics and magnonics. Here, using the Heisenberg antiferromagnet RbMF$_3$, we demonstrate that laser-induced THz spin dynamics corresponding to pairs of mutually coherent counter propagating spin waves with the wavevectors up to the edge of the Brillouin zone cannot be understood in terms of magnetization and antiferromagnetic (N\'eel) vectors, conventionally used to describe spin waves. Instead, we propose to model such spin dynamics using the spin correlation function. We derive a quantum-mechanical equation of motion for the latter and emphasize that, unlike the magnetization and antiferromagnetic vectors the spin correlations in antiferromagnets do not exhibit inertia., Comment: Main article contains 7 pages, 3 figures. With Supplementary material

CoPS3 stands out in the family of the van der Waals antiferromagnets XPS3 (X=Mn, Ni, Fe, Co) due to the unquenched orbital momentum of the magnetic Co2+ ions which is known to facilitate the coupling of spins to both electromagnetic waves and lattice vibrations. Here, using a time-resolved magneto-optical pump-probe technique we experimentally study the ultrafast laser-induced dynamics of mutually correlated spins and lattice. It is shown that a femtosecond laser pulse acts as an ultrafast heater and thus results in the melting of the antiferromagnetic order. At the same time, the resonant pumping of the 4T1g - 4T2g electronic transition in Co2+ ions effectively changes their orbital momentum, giving rise to a mechanical force that moves the ions in the direction parallel to the orientation of their spins, thus generating a coherent Bg phonon mode at the frequency of about 4.7 THz., Comment: The following article has been submitted to APL Materials as a contribution to a special issue "Emerging Materials in Antiferromagnetic Spintronics"

Finding efficient and ultrafast ways to control antiferromagnets is believed to be instrumental in unlocking their potential for magnetic devices operating at THz frequencies. Still, it is challenged by the absence of net magnetization in the ground state. Here, we show that the magnetization emerging from a state of coherent spin precession in antiferromagnetic iron borate FeBO$_3$ can be used to enable the nonlinear coupling of light to another, otherwise weakly susceptible, mode of spin precession. This nonlinear mechanism can facilitate conceptually new ways of controlling antiferromagnetism., Comment: 19 pages, 9 figures

The interaction of a single-cycle THz electric field with the topological insulator $\mathrm{MnBi}_2\mathrm{Te}_4$ triggers strongly anharmonic lattice dynamics, promoting fully coherent energy transfer between the otherwise non-interacting Raman-active $E_g$ and infrared (IR)-active $E_u$ phononic modes. Two-dimensional (2D) THz spectroscopy combined with modeling based on the classical equations of motion and symmetry analysis reveals the multi-stage process underlying the excitation of the Raman-active $E_g$ phonon. In this process, the THz electric field first prepares a coherent IR-active $E_u$ phononic state and subsequently interacts with this state to efficiently excite the $E_g$ phonon., Comment: 27 pages, 20 figures

We review and discuss the process of single-shot helicity-independent all-optical switching of magnetization by which a single suitably-ultrafast excitation, under the right conditions, toggles magnetization from one stable state to another. For almost a decade, this phenomenon was only consistently observed in specific rare-earth-transition-metal ferrimagnetic alloys of GdFeCo, but breakthrough experiments in recent years have revealed that the same behavior can be achieved in a wide range of multi-sublattice magnets including TbCo alloys doped with minute amounts of Gd, Gd/Co and Tb/Co synthetic ferrimagnets, and the rare-earth-free Heusler alloy Mn$_2$Ru$_x$Ga. Aiming to resolve the conditions that allow switching, a series of experiments have shown that the process in the ferrimagnetic alloys GdFeCo and Mn$_2$Ru$_x$Ga is highly sensitive to the pulse duration, starting temperature and the alloy composition. We argue here that the switching displayed by these two very different ferrimagnetic alloys can be generally understood within a single phenomenological framework describing the flow of angular momentum between the constituent sublattices and from the sublattices to the environment. The conditions that facilitate switching stem from the properties of these channels of angular momentum flow in combination with the size of the angular momentum reservoirs. We conclude with providing an outlook in this vibrant research field, with emphasis on the outstanding open questions pertaining to the underlying physics along with noting the advances in exploiting this switching process in technological applications., Comment: 18 pages, 7 figures. Submitted to the special issue on "Advances in magnetic switching technologies" to be published in Journal of Magnetism and Magnetic Materials

Ultrafast heating of FeRh by a femtosecond laser pulse launches a magneto-structural phase transition from an antiferromagnetic to a ferromagnetic state. Aiming to reveal the ultrafast kinetics of this transition, we studied magnetization dynamics with the help of the magneto-optical Kerr effect in a broad range of temperatures (from 4 K to 400 K) and magnetic fields (up to 25 T). Three different types of ultrafast magnetization dynamics were observed and, using a numerically calculated H-T phase diagram, the differences were explained by different initial states of FeRh corresponding to a (i) collinear antiferromagnetic, (ii) canted antiferromagnetic and (iii) ferromagnetic alignment of spins. We argue that ultrafast heating of FeRh in the canted antiferromagnetic phase launches practically the fastest possible emergence of magnetization in this material. The magnetization emerges on a time scale of 2 ps, which corresponds to the earlier reported time-scale of the structural changes during the phase transition.

The practical difficulty in distinguishing the impact of magnetic circular dichroism and the inverse Faraday effect fuels intense debates over which mechanism predominantly drives the process of helicity dependent all-optical switching of magnetization in ferromagnets. Here, we quantitatively measure the efficiency of the switching process in a Pt/Co/Pt multilayered stack using visible- to near-infrared optical pulses. We find that the switching efficiency increases by a factor of 8.6 upon increasing the pumping wavelength from 0.5 $ \mu $m to 1.1 $ \mu $m, becoming 100 % efficient at even longer wavelengths up to 2.0 $ \mu $m. Our experimental results can be successfully explained by the phenomenon of magnetic circular dichroism, making a significant step towards resolving the long-standing controversy over the origin of the all-optical process of magnetization reversal in ferromagnets., Comment: 29 pages, 7 figures, 2 tables

Understanding spin-lattice coupling represents a key challenge in modern condensed matter physics, with crucial importance and implications for ultrafast and 2D-magnetism. The efficiency of angular momentum and energy transfer between spins and the lattice imposes fundamental speed limits on the ability to control spins in spintronics, magnonics and magnetic data storage. We report on an efficient nonlinear mechanism of spin-lattice coupling driven by THz light pulses. A nearly single-cycle THz pulse resonantly interacts with a coherent magnonic state in the antiferromagnet CoF2 and excites the Raman-active THz phonon. The results reveal the unique functionality of antiferromagnets allowing ultrafast spin-lattice coupling using light.

Magnonics is a research field complementary to spintronics, in which the quanta of spin waves (magnons) replace electrons as information carriers, promising less energy dissipation. The development of ultrafast nanoscale magnonic logic circuits calls for new tools and materials to generate coherent spin waves with frequencies as high, and wavelengths as short, as possible. Antiferromagnets can host spin waves at THz frequencies and are therefore seen as a future platform for the fastest and the least dissipative transfer of information. However, the generation of short-wavelength coherent propagating magnons in antiferromagnets has so far remained elusive. Here we report the efficient emission and detection of a nanometer-scale wavepacket of coherent propagating magnons in antiferromagnetic DyFeO3 using ultrashort pulses of light. The subwavelength nanoscale confinement of the laser field due to large absorption creates a strongly non-uniform spin excitation profile, thereby enabling the propagation of a broadband continuum of coherent THz spin waves. The wavepacket features magnons with detected wavelengths down to 125 nm and supersonic velocities up to 13 km/s that propagate over macroscopic distances. The long-sought source of coherent short-wavelength spin carriers demonstrated here opens up new prospects for THz antiferromagnetic magnonics and coherence mediated logic devices at THz frequencies., Comment: 33 pages, 13 figures

Neuromorphic computing aims to mimic the architecture of the human brain to carry out computational tasks that are challenging and much more energy consuming for standard hardware. Despite progress in several fields of physics and engineering, the realization of artificial neural networks which combine high operating speeds with fast and low-energy adaptability remains a challenge. Here we demonstrate an opto-magnetic neural network capable of learning and classification of digitized 3x3 characters exploiting local storage in the magnetic material. Using picosecond laser pulses, we find that micrometer sized synapses absorb well below 100 picojoule per synapse per laser pulse, with favorable scaling to smaller spatial dimensions. We thus succeeded in combining the speed and low-dissipation of optical networks with the low-energy adaptability and non-volatility of magnetism, providing a promising approach to fast and energy-efficient neuromorphic computing., Comment: 9 pages, 4 figures

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 [Tbn/Com] 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 [Tb1/Co2] and [Tb1/Co3] 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., Comment: 9 pages, 4 figures

The efficiency of ultrafast excitation of spins in antiferromagnetic $\mathrm{\alpha-Fe_{2}O_{3}}$ using nearly single-cycle THz pulse is studied as a function of the polarization of the THz pulse and the sample temperature. Above the Morin point the most efficient excitation is achieved when the magnetic field of the THz pulse is perpendicular to the antiferromagnetically coupled spins. Using the experimental results and equations of motion for spins, we show that the mechanism of the spin excitation above and below the Morin point relies on magnetic-dipole interaction of the THz magnetic field with spins and the efficiency of the coupling is proportional to the time derivative of the magnetic field.

THz magnetization dynamics is excited in ferrimagnetic thulium iron garnet with a picosecond, single-cycle magnetic field pulse and seen as a high-frequency modulation of the magneto-optical Faraday effect. Data analysis combined with numerical modelling and evaluation of the effective Lagrangian allow us to conclude that the dynamics corresponds to the exchange mode excited by Zeeman interaction of the THz field with the antiferromagnetically coupled spins. We argue that THz-pump IR-probe experiments on ferrimagnets offer a unique tool for quantitative studies of dynamics and mechanisms to control antiferromagnetically coupled spins., Comment: 17 pages, 16 figures

Excitation, detection and control of coherent THz magnetic excitation in antiferromagnets are challenging problems that can be addressed using ever shorter laser pulses. We study experimentally excitation of magnetic dynamics at THz frequencies in an antiferromagnetic insulator CoF$_2$ by sub-10 fs laser pulses. Time-resolved pump-probe polarimetric measurements at different temperatures and probe polarizations reveal laser-induced transient circular birefringence oscillating at the frequency of 7.45 THz and present below the N\'eel temperature. The THz oscillations of circular birefringence are ascribed to oscillations of the magnetic moments of Co$^{2+}$ ions induced by the laser-driven coherent E$_g$ phonon mode via the THz analogue of the transverse piezomagnetic effect. It is also shown that the same pulse launches coherent oscillations of the magnetic linear birefringence at the frequency of 3.4 THz corresponding to the two-magnon mode. Analysis of the probe polarization dependence of the transient magnetic linear birefringence at the frequency of the two-magnon mode enables identifying its symmetry., Comment: Main text: 23 pages, 4 figures Supplementary Materials: 8 pages, 1 figure

We report on spin Hall magnetoresistance (SMR) and spin Seebeck effect (SSE) in single crystal of the rare-earth antiferromagnet DyFeO$_{3}$ with a thin Pt film contact. The angular shape and symmetry of the SMR at elevated temperatures reflect the antiferromagnetic order of the Fe$^{3+}$ moments as governed by the Zeeman energy, the magnetocrystalline anisotropy and the Dzyaloshinskii-Moriya interaction. We interpret the observed linear dependence of the signal on the magnetic field strength as evidence for field-induced order of the Dy$^{3+}$ moments up to room temperature. At and below the Morin temperature of 50$\,$K, the SMR monitors the spin-reorientation phase transition of Fe$^{3+}$ spins. Below 23$\,$K, additional features emerge that persist below 4$\,$K, the ordering temperature of the Dy$^{3+}$ magnetic sublattice. We conclude that the combination of SMR and SSE is a simple and efficient tool to study spin reorientation phase transitions and sublattice magnetizations.

Identifying an efficient pathway to change the order parameter via a subtle excitation of the coupled high-frequency mode is the ultimate goal of the field of ultrafast phase transitions. This is an especially interesting research direction in magnetism, where the coupling between spin and lattice excitations is required for magnetization reversal. Despite several attempts however, the switching between magnetic states via resonant pumping of phonon modes has not yet been demonstrated. Here we show how an ultrafast resonant excitation of the longitudinal optical phonon modes in magnetic garnet films switches magnetization into a peculiar quadrupolar magnetic domain pattern, unambiguously revealing the magneto-elastic mechanism of the switching. In contrast, the excitation of strongly absorbing transverse phonon modes results in thermal demagnetization effect only., Comment: 16 pages, 12 figures

Femtosecond laser excitation of FeRh/Pt bilayers launches an ultrafast pulse of electric photocurrent in the Pt-layer and thus results in emission of electromagnetic radiation in the THz spectral range. Analysis of the THz emission as a function of polarization of the femtosecond laser pulse, external magnetic field, sample temperature and sample orientation shows that photocurrent can emerge due to vertical spin pumping and photo-induced inverse spin-orbit torque at the FeRh/Pt interface. The vertical spin pumping from FeRh to Pt does not depend on the polarization of light and originates from ultrafast laser-induced demagnetization of the ferromagnetic phase of FeRh. The photo-induced inverse spin-orbit torque at the FeRh/Pt interface can be described in terms of a helicity-dependent effect of circularly polarized light on the magnetization of the ferromagnetic FeRh and subsequent generation of a photocurrent., Comment: 11 pages

Second-order nonlinear optical response allows to detect different properties of the system associated with the inversion symmetry breaking. Here, we use a second harmonic generation effect to investigate the alignment of a graphene/hexagonal Boron Nitride heterostructure. To achieve that, we activate a commensurate-incommensurate phase transition by a thermal annealing of the sample. We find that this structural change in the system can be directly observed through a strong modification of a nonlinear optical signal. This result reveals the potential of a second harmonic generation technique for probing structural properties of layered systems.

We study the demagnetization dynamics of the fully compensated half-metallic ferrimagnet Mn$_2$Ru$_x$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 the two Mn-sublattices 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 Mn$_2$Ru$_x$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 Mn$_2$Ru$_x$Ga is possible., Comment: 5 pages, 3 figures, J. Phys.: Condens. Matter (2021)

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., Comment: 35 pages total, 8 figures in main text, 7 figures in supplementary

Future information technology demands ultimately fast, low-loss quantum control. Intense light fields have facilitated important milestones, such as inducing novel states of matter, accelerating electrons ballistically, or coherently flipping the valley pseudospin. These dynamics leave unique signatures, such as characteristic bandgaps or high-order harmonic radiation. The fastest and least dissipative way of switching the technologically most important quantum attribute - the spin - between two states separated by a potential barrier is to trigger an all-coherent precession. Pioneering experiments and theory with picosecond electric and magnetic fields have suggested this possibility, yet observing the actual dynamics has remained out of reach. Here, we show that terahertz (1 THz = 10$^{12}$ Hz) electromagnetic pulses allow coherent navigation of spins over a potential barrier and we reveal the corresponding temporal and spectral fingerprints. This goal is achieved by coupling spins in antiferromagnetic TmFeO$_{3}$ with the locally enhanced THz electric field of custom-tailored antennas. Within their duration of 1 ps, the intense THz pulses abruptly change the magnetic anisotropy and trigger a large-amplitude ballistic spin motion. A characteristic phase flip, an asymmetric splitting of the magnon resonance, and a long-lived offset of the Faraday signal are hallmarks of coherent spin switching into adjacent potential minima, in agreement with a numerical simulation. The switchable spin states can be selected by an external magnetic bias. The low dissipation and the antenna's sub-wavelength spatial definition could facilitate scalable spin devices operating at THz rates., Comment: This is a post-peer-review, pre-copyedit version of an article published in Nature. The final authenticated version is available online at https://www.nature.com/articles/s41586-019-1174-7. 32 pages, 4 Figures, 9 Extended Data Figures

Exciting atomic oscillations with light is a powerful technique to control the electronic properties of materials, leading to remarkable phenomena such as light-induced superconductivity and ultrafast insulator to metal transitions. Here we show that light-driven lattice vibrations can be utilised to encode efficiently spin information in a magnetic medium. Intense mid-infrared electric field pulses, tuned to resonance with a vibrational normal mode of antiferromagnetic DyFeO3, drive the emergence of long-living weak ferromagnetic order. Light-driven phonon displacements promptly lower the energy barrier separating competing magnetic states, allowing the alignment of spins to occur within a few picoseconds, via non-equilibrium dynamics of the magnetic energy landscape., Comment: 36 pages 25 figures

Here we study both static and time-resolved dynamic magnetic properties of the compensated ferrimagnet from room temperature down to 10K, thus crossing the magnetic compensation temperature $T_{M}$. The behaviour is analysed with a model of a simple collinear ferrimagnet with uniaxial anisotropy and site-specific gyromagnetic ratios. We find a maximum zero-applied-field resonance frequency of $\sim$160GHz and a low intrinsic Gilbert damping $\alpha$$\sim$0.02, making it a very attractive candidate for various spintronic applications., Comment: 6 pages, 6 figures, accepted paper in PRB (https://journals.aps.org/prb/accepted/df07aOb2T7f1e845c21429304f825e825c3a5f190)

Experimental studies of anomalous Hall effect are performed for thin filmed Ta/TbFeCo in a wide range of temperatures and magnetic fields up to 3 T. While far from the compensation temperature (TM=277 K) the field dependence has a conventional shape of a single hysteresis loop, just below the compensation point the dependence is anomalous having the shape of a triple hysteresis. To understand this behavior, we experimentally reveal the magnetic phase diagram and theoretically analyze it in terms of spin-reorientation phase transitions. We show that one should expect anomalous hysteresis loops below the compensation point if in the vicinity of it the magnetic anisotropy is dominated by FeCo sublattice due to interaction with Ta., Comment: 9 pages, 6 figures

We resolve a significant controversy about how to understand and engineer single-shot all-optical switching of magnetization in ferrimagnets using femto- or picosecond-long heat pulses. By realistically modelling a generic ferrimagnet as two coupled macrospins, we comprehensively show that the net magnetization can be reversed via different pathways, using a heat pulse with duration spanning all relevant timescales within the non-adiabatic limit. This conceptual understanding is fully validated by experiments studying the material and optical limits at which the switching process in GdFeCo alloys loses its reliability. Our interpretation and results constitute a blueprint for understanding how deterministic all-optical switching can be achieved in alternative ferrimagnets using short thermal pulses.

Anomalous hysteresis loops of ferrimagnetic amorphous alloys in high magnetic field and in the vicinity of the compensation temperature have so far been explained by sample inhomogeneities. We obtain H-T magnetic phase diagram for ferrimagnetic GdFeCo alloy using a two-sublattice model in the paramagnetic rare-earth ion approximation and taking into account rare-earth (Gd) magnetic anisotropy. It is shown that if the magnetic anisotropy of the $f$-sublattice is larger than that of the $d$-sublattice, the tricritical point can be at higher temperature than the compensation point. The obtained phase diagram explains the observed anomalous hysteresis loops as a result of high-field magnetic phase transition, the order of which changes with temperature. It also implies that in the vicinity of the magnetic compensation point the shape of magnetic hysteresis loop is strongly temperature dependent., Comment: 8 pages, 3 figures

Magneto-optical spectroscopy in fields up to 30 Tesla reveals anomalies in the equilibrium and ultrafast magnetic properties of the ferrimagnetic rare-earth-transition metal alloy TbFeCo. In particular, in the vicinity of the magnetization compensation temperature, each of the magnetizations of the antiferromagnetically coupled Tb and FeCo sublattices show triple hysteresis loops. Contrary to state-of-the-art theory, which explains such loops by sample inhomogeneities, here we show that they are an intrinsic property of the rare-earth ferrimagnets. Assuming that the rare-earth ions are paramagnetic and have a non-zero orbital momentum in the ground state and, therefore, a large magnetic anisotropy, we are able to reproduce the experimentally observed behavior in equilibrium. The same theory is also able to describe the experimentally observed critical slowdown of the spin dynamics in the vicinity of the magnetization compensation temperature, emphasizing the role played by the orbital momentum in static and ultrafast magnetism of ferrimagnets.

Femtosecond laser excitation of a Co/Pt bilayer results in the efficient emission of picosecond THz pulses. Two known mechanisms for generating THz emission are spin-polarized currents through a Co/Pt interface, resulting in helicity-independent electric currents in the Pt layer due to the inverse spin-Hall effect and helicity-dependent electric currents at the Co/Pt interface due to the inverse spin-orbit torque effect. Here we explore how roughness, crystal structure and intermixing at the Co/Pt interface affect the efficiency of the THz emission. In particular, we varied the roughness of the interface, in the range of 0.1-0.4 nm, by tuning the deposition pressure conditions during the fabrication of the Co/Pt bilayers. To control the intermixing at the Co/Pt interface a 1-2 nm thick CoxPt1-x alloy spacer layer was introduced with various compositions of Co and Pt. Finally, the crystal structure of Co was varied from face centered cubic to hexagonal close packed. Our study shows that the roughness of the interface is of crucial importance for the efficiency of helicity-dependent THz emission induced by femtosecond laser pulses. However, it is puzzling that intermixing while strongly enhancing the helicity-independent THz emission had no effect on the helicity-dependent THz emission which is suppressed and similar to the smooth interfaces., Comment: 17 pages, 7 figures, 1 table

All-optical helicity dependent switching (AO-HDS), deterministic control of magnetization by circularly polarized laser pulses, allows to efficiently manipulate spins without the need of a magnetic field. However, AO-HDS in ferromagnetic metals so far requires many laser pulses for fully switching their magnetic states. Using a combination of a short, 90-fs linearly polarized pulse and a subsequent longer, 3-ps circularly polarized pulse, we demonstrate that the number of pulses for full magnetization reversal can be reduced to 4 pulse pairs in a single stack of Pt/Co/Pt. The obtained results suggest that the dual-pulse approach is a potential route towards realizing efficient AO-HDS in ferromagnetic metals., Comment: 11 pages, 3 figures

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 ultrashort laser or electrical current pulse. We show that the torque is non-zero only in the non-collinear magnetic phase that can be acquired by applying external magnetic field to the material. The coherent response of magnetization dynamics amplitude and its timescale exhibits critical behavior near certain values of the magnetic field corresponding to a spin-flop like phase transition. Understanding the underlying mechanisms for these effects opens the way to efficient control of the amplitude and the timescales of the spin dynamics, which is one of the central problems in the field of ultrafast magnetism., Comment: 6 pages, 1 figure

The explosive growth of data and its related energy consumption is pushing the need to develop energy-efficient brain-inspired schemes and materials for data processing and storage. Here, we demonstrate experimentally that Co/Pt films can be used as artificial synapses by manipulating their magnetization state using circularly-polarized ultrashort optical pulses at room temperature. We also show an efficient implementation of supervised perceptron learning on an opto-magnetic neural network, built from such magnetic synapses. Importantly, we demonstrate that the optimization of synaptic weights can be achieved using a global feedback mechanism, such that the learning does not rely on external storage or additional optimization schemes. These results suggest there is high potential for realizing artificial neural networks using optically-controlled magnetization in technologically relevant materials, that can learn not only fast but also energy-efficient., Comment: 9 pages, 4 figures

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 rapid magnetic order recovery in materials with perpendicular magnetic anisotropy via nonlinear magnon processes. We identify both localisation and coalescence regimes, whereby localised magnetic textures nucleate and subsequently evolve in accordance with a power law formalism. Coalescence is observed for optical excitations both above and below the switching threshold. Simulations indicate that the ultrafast generation of noncollinear magnetisation via optical pumping establishes exchange-mediated spin currents with an equivalent 100% spin polarised charge current density of $10^8$ A/cm$^2$. Such large spin currents precipitate rapid recovery of magnetic order after optical pumping. These processes suggest an ultrafast optical route for the stabilization of desired meta-stable states, e.g., isolated skyrmions.

Finding an electronic transition a subtle excitation of which can launch dramatic changes of electric, optical or magnetic properties of media is one of the long-standing dreams in the field of photo-induced phase transitions [1-5]. Therefore the discovery of the magnetization switching only by a femtosecond laser pulse [6-10] triggered intense discussions about mechanisms responsible for these laser-induced changes. Here we report the experimentally revealed selection rules on polarization and wavelengths of ultrafast photo-magnetic recording in Co-doped garnet film and identify the workspace of the parameters (magnetic damping, wavelength and polarization of light) allowing this effect. The all-optical magnetic switching under both single pulse and multiple-pulse sequences can be achieved at room temperature, in narrow spectral ranges with light polarized either along <110> or <100> crystallographic axes of the garnet. The revealed selection rules indicate that the excitations responsible for the coupling of light to spins are d-electron transitions in octahedral and tetrahedral Co-sublattices, respectively.

The ultrashort laser excitation of Co/Pt magnetic heterostructures can effectively generate spin and charge currents at the interfaces between magnetic and nonmagnetic layers. The direction of these photocurrents can be controlled by the helicity of the circularly polarized laser light and an external magnetic field. Here, we employ THz time-domain spectroscopy to investigate further the role of interfaces in these photo-galvanic phenomena. In particular, the effects of either Cu or ZnO interlayers on the photocurrents in Co/X/Pt (X = Cu, ZnO) have been studied by varying the thickness of the interlayers up to 5 nm. The results are discussed in terms of spin-diffusion phenomena and interfacial spin-orbit torque., Comment: 15 pages, 6 figures, 2 tables