Canted spin order as a platform for ultrafast conversion of magnons.

Traditionally, magnetic solids are divided into two main classes-ferromagnets and antiferromagnets with parallel and antiparallel spin orders, respectively. Although normally the antiferromagnets have zero magnetization, in some of them an additional antisymmetric spin-spin interaction arises owing to a strong spin-orbit coupling and results in canting of the spins, thereby producing net magnetization. The canted antiferromagnets combine antiferromagnetic order with phenomena typical of ferromagnets and hold great potential for spintronics and magnonics1-5. In this way, they can be identified as closely related to the recently proposed new class of magnetic materials called altermagnets6-9. Altermagnets are predicted to have strong magneto-optical effects, terahertz-frequency spin dynamics and degeneracy lifting for chiral spin waves10 (that is, all of the effects present in the canted antiferromagnets11,12). Here, by utilizing these unique phenomena, we demonstrate a new functionality of canted spin order for magnonics and show that it facilitates mechanisms converting a magnon at the centre of the Brillouin zone into propagating magnons using nonlinear magnon-magnon interactions activated by an ultrafast laser pulse. Our experimental findings supported by theoretical analysis show that the mechanism is enabled by the spin canting.

Ultrafast all-optical toggle writing of magnetic bits without relying on heat.

Ultrafast excitation of matter can violate Curie's principle that the symmetry of the cause must be found in the symmetry of the effect. For instance, heating alone cannot result in a deterministic reversal of magnetization. However, if the heating is ultrafast, it facilitates toggle switching of magnetization between stable bit-states without any magnetic field. Here we show that the regime of ultrafast toggle switching can be also realized via a mechanism without relying on heat. Ultrafast laser excitation of iron-garnet with linearly polarized light modifies magnetic anisotropy and thus causes toggling magnetization between two stable bit states. This new regime of 'cold' toggle switching can be observed in ferrimagnets without a compensation point and over an exceptionally broad temperature range. The control of magnetic anisotropy required for the toggle switching exhibits reduced dissipation compared to laser-induced-heating mechanism, however the dissipation and the switching-time are shown to be competing parameters.

Phononic switching of magnetization by the ultrafast Barnett effect.

The historic Barnett effect describes how an inertial body with otherwise zero net magnetic moment acquires spontaneous magnetization when mechanically spinning1,2. Breakthrough experiments have recently shown that an ultrashort laser pulse destroys the magnetization of an ordered ferromagnet within hundreds of femtoseconds3, with the spins losing angular momentum to circularly polarized optical phonons as part of the ultrafast Einstein-de Haas effect4,5. 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 gained temporarily by means of the ultrafast Barnett effect, through the resonant excitation of circularly polarized optical phonons in a paramagnetic substrate, can be used to permanently reverse the magnetic state of a heterostructure mounted atop the said substrate. 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.

Magneto-optical diffraction of visible light as a probe of nanoscale displacement of domain walls at femtosecond timescales.

Using diffraction of femtosecond laser pulses of visible light by a magnetic domain pattern in an iron garnet, we demonstrate a proof of concept of time-resolved measurements of domain pattern movements with nanometer spatial and femtosecond temporal resolution. In this method, a femtosecond laser (pump) pulse initiates magnetization dynamics in a sample that is initially in a labyrinth domain state, while an equally short linearly polarized laser pulse (probe) is diffracted by the domain pattern. The components of the diffracted light that are polarized orthogonally to the incident light generate several concentric diffraction rings. Nanometer small changes in the relative sizes of domains with opposite magnetization result in observable changes in the intensities of the rings. We demonstrate that the signal-to-noise ratio is high enough to detect a 6 nm domain wall displacement with 100 fs temporal resolution using visible light. We also discuss possible artifacts, such as pump-induced changes of optical properties, that can affect the measurements.

Empowering Control of Antiferromagnets by THz-Induced Spin Coherence.

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.

Two-dimensional terahertz spectroscopy as a tool for revealing nonlinear interactions in media.

Usually, the presence of multiple eigenstates (magnons and phonons) in a system makes it difficult to analyze the coupled excitation mechanism using conventional single-pulse terahertz (THz) spectroscopy. On the contrary, 2D THz spectroscopy reveals energy flows between these states, which facilitates the identification of the coupled dynamics. In this article, we provide a theoretical description of this advanced technique and an experimental demonstration of its performance in antiferromagnet CoF2. Here, 2D THz spectroscopy shows that the THz pulse induces energy transfer from the magnon mode to the Raman-active phonon mode via a nonlinear excitation pathway.

Two-Dimensional Terahertz Spectroscopy of Nonlinear Phononics in the Topological Insulator MnBi_{2}Te_{4}.

The interaction of a single-cycle terahertz electric field with the topological insulator MnBi_{2}Te_{4} triggers strongly anharmonic lattice dynamics, promoting fully coherent energy transfer between the otherwise noninteracting Raman-active E_{g} and infrared (IR)-active E_{u} phononic modes. Two-dimensional terahertz spectroscopy combined with modeling based on the classical equations of motion and symmetry analysis reveals the multistage process underlying the excitation of the Raman-active E_{g} phonon. In this nonlinear combined photophononic process, the terahertz 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.

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.

Laser-induced THz magnetism of antiferromagnetic CoF2.

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 CoF2by 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 Néel temperature. The THz oscillations of circular birefringence are ascribed to oscillations of the magnetic moments of Co2+ions induced by the laser-driven coherentEgphonon 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.

Coherent spin-wave transport in an antiferromagnet.

Magnonics is a research field complementary to spintronics, in which quanta of spin waves (magnons) replace electrons as information carriers, promising lower dissipation1-3. 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 possible4,5. Antiferromagnets can host spin waves at terahertz (THz) frequencies and are therefore seen as a future platform for the fastest and the least dissipative transfer of information6-11. 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 confinement of the laser field due to large absorption creates a strongly non-uniform spin excitation profile, enabling the propagation of a broadband continuum of coherent THz spin waves. The wavepacket contains magnons with a shortest detected wavelength of 125 nm that propagate with supersonic velocities of more than 13 km/s into the material. This source of coherent short-wavelength spin carriers opens up new prospects for THz antiferromagnetic magnonics and coherence-mediated logic devices at THz frequencies.

THz-Scale Field-Induced Spin Dynamics in Ferrimagnetic Iron Garnets.

THz magnetization dynamics of antiferromagnetically coupled spins in ferrimagnetic Tm_{3}Fe_{5}O_{12} is excited by a picosecond single-cycle pulse of a magnetic field and probed with the help of the magneto-optical Faraday effect. Data analysis combined with numerical modeling shows that the dynamics corresponds to the exchange mode excited by the Zeeman interaction of the THz magnetic field with the 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.

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.

Ultrafast control of magnetic interactions via light-driven phonons.

Resonant ultrafast excitation of infrared-active phonons is a powerful technique with which to control the electronic properties of materials that leads to remarkable phenomena such as the light-induced enhancement of superconductivity1,2, switching of ferroelectric polarization3,4 and ultrafast insulator-to-metal transitions5. Here, we show that light-driven phonons can be utilized to coherently manipulate macroscopic magnetic states. Intense mid-infrared electric field pulses tuned to resonance with a phonon mode of the archetypical antiferromagnet DyFeO3 induce ultrafast and long-living changes of the fundamental exchange interaction between rare-earth orbitals and transition metal spins. Non-thermal lattice control of the magnetic exchange, which defines the stability of the macroscopic magnetic state, allows us to perform picosecond coherent switching between competing antiferromagnetic and weakly ferromagnetic spin orders. Our discovery emphasizes the potential of resonant phonon excitation for the manipulation of ferroic order on ultrafast timescales6.

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.

Direct Observation of Incommensurate-Commensurate Transition in Graphene-hBN Heterostructures via Optical Second Harmonic Generation.

Commensurability effects play a crucial role in the formation of electronic properties of novel layered heterostructures. The interest in these moiré superstructures has increased tremendously since the recent observation of a superconducting state (Nature 2018, 556, 43-50) and metal-insulator transition (Nature 2018, 556, 80-84) in twisted bilayer graphene. In this regard, a straightforward and efficient experimental technique for detection of the alignment of layered materials is desired. In this work, we use optical second harmonic generation, which is sensitive to the inversion symmetry breaking, to investigate the alignment of graphene/hexagonal boron nitride heterostructures. 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 via a strong modification of a nonlinear optical signal. Unambiguous interpretation of obtained results reveals the potential of a second harmonic generation technique for probing of structural changes in layered systems.

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.

Ultrafast spin dynamics in ferrimagnets with compensation point.

We derive an effective Lagrangian that facilitates the modeling of magnetization dynamics in a ferrimagnet with magnetization compensation point. The model is able to explain the earlier reported magnetization dynamics in the noncollinear magnetic phase triggered by a femtosecond laser pulse in GdFeCo amorphous alloy in the vicinity of spin-flop transition. Moreover, the described approach can be easily extended and applied to other cases of ultrafast magnetism in uniaxial f -d (rare-earth-transition metal) ferrimagnet near the magnetization compensation point in high magnetic fields. We assume that the primary effect of the femtosecond laser pulse is the ultrafast demagnetization of the ferrimagnet. We show that in the noncollinear magnetic phase, which can be prepared by applying external magnetic field above the spin-flop transition, such a demagnetization results in a torque acting on the magnetizations of both sublattices. It is shown that, similarly to the experiment, the amplitude and timescales of the dynamics strongly depend on temperature and applied magnetic field. In particular, in the vicinity of the spin-flop phase transition the amplitude dramatically increases while the dynamics exhibit a critical slowdown. We expect that the developed theoretical framework will boost further research of ultrafast magnetism of noncollinear spin systems.

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.