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The interaction of terahertz (THz) radiation with high-frequency spin resonances in complex magnetic materials is central for modern ultrafast magnonics. Here we demonstrate strong variations of the excitation efficiency of the sub-THz exchange magnon in a single crystal ferrimagnet (Gd,Bi)$_3$Fe$_5$O$_{12}$. An enhancement of the exchange magnon amplitude is observed when its frequency matches an eigenmode of the cavity created by the sample interfaces. Moreover, this enhancement is accompanied by a 5-fold decrease in effective damping of the exchange mode. The THz-exchange magnon interaction in the cavity is analyzed within the developed Landau-Lifshitz-Gilbert formalism for three coupled magnetization sublattices and cavity-enhanced THz field. This work presents a novel approach for the THz excitation of spin dynamics in ferrimagnets and outlines promising pathways for the controlled optimization of light-spin coupling in single crystals.

Contemporary quantum plasmonics capture subtle corrections to the properties of plasmonic nano-objects in equilibrium. Here, we demonstrate nonequilibrium spill-out redistribution of the electronic density at the ultrafast time scale. As revealed by time-resolved 2D spectroscopy of nanoplasmonic Fe/Au bilayers, an injection of the laser-excited non-thermal electrons induces transient electron spill-out thus changing the plasma frequency. The response of the local electronic density switches the electronic density behavior from spill-in to strong (an order of magnitude larger) spill-out at the femtosecond time scale. The superdiffusive transport of hot electrons and the lack of a direct laser heating indicate significantly non-thermal origin of the underlying physics. Our results demonstrate an ultrafast and non-thermal way to control surface plasmon dispersion through transient variations of the spatial electron distribution at the nanoscale. These findings expand quantum plasmonics into previously unexplored directions by introducing ultrashort time scales in the non-equilibrium electronic systems., Comment: 3 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

We present experimental and computational findings of the laser-induced non-reciprocal motion of magnetization during ultrafast photo-magnetic switching in garnets. We found distinct coherent magnetization precession trajectories and switching times between four magnetization states, depending on both directions of the light linear polarization and initial magnetic state. As a fingerprint of the topological symmetry, the choice of the switching trajectory is governed by an interplay of the photo-magnetic torque and magnetic anisotropy. Our results open a plethora of possibilities for designing energy-efficient magnetization switching routes at arbitrary energy landscapes.

The developing field of strain-induced magnetization dynamics offers a promising path toward efficiently controlling spins and phase transitions. Understanding the underlying mechanisms is crucial in finding the optimal parameters supporting the phononic switching of magnetization. Here, we present an experimental and numerical study of time-resolved magnetization dynamics driven by the resonant excitation of an optical phonon mode in iron garnets. Upon pumping the latter with an infrared pulse obtained from a free-electron laser, we observe spatially-varying magnetization precession, with its phase depending on the direction of an external magnetic field. Our micromagnetic simulations effectively describe the magnetization precession and switching in terms of laser-induced changes in the crystal's magneto-elastic energy.

Resonant absorption of a photon by bound electrons in a solid can promote an electron to another orbital state or transfer it to a neighboring atomic site. Such a transition in a magnetically ordered material could affect the magnetic order. While this process is an obvious road map for optical control of magnetization, experimental demonstration of such a process remains challenging. Exciting a significant fraction of magnetic ions requires a very intense incoming light beam, as orbital resonances are often weak compared to above-band-gap excitations. In the latter case, a sizeable reduction of the magnetization occurs as the absorbed energy increases the spin temperature, masking the non-thermal optical effects. Here, using ultrafast x-ray spectroscopy, we were able to resolve changes in the magnetization state induced by resonant absorption of infrared photons in Co-doped yttrium iron garnet, with negligible thermal effects. We found that the optical excitation of the Co ions affects the two distinct magnetic Fe sublattices differently, resulting in a transient non-collinear magnetic state. The present results indicate that the all-optical magnetization switching most likely occurs due to the creation of a transient, non-collinear magnetic state followed by coherent spin rotations of the Fe moments.

We analyze, both experimentally and numerically, the nonlinear regime of the photo-induced coherent magnetization dynamics in cobalt-doped yttrium iron garnet films. Photo-magnetic excitation with femtosecond laser pulses reveals a strongly nonlinear response of the spin subsystem with a significant increase of the effective Gilbert damping. By varying both laser fluence and the external magnetic field, we show that this nonlinearity originates in the anharmonicity of the magnetic energy landscape. We numerically map the parameter workspace for the nonlinear photo-induced spin dynamics below the photo-magnetic switching threshold. Corroborated by numerical simulations of the Landau-Lifshitz-Gilbert equation, our results highlight the key role of the cubic symmetry of the magnetic subsystem in reaching the nonlinear spin precession regime. These findings expand the fundamental understanding of laser-induced nonlinear spin dynamics as well as facilitate the development of applied photo-magnetism.

Computer-generated holograms with their animated, three-dimensional appearance have long appealed to our imagination as the path towards truly immersive displays with bi-directional natural parallax. Impressive progress in updateable 3-D imagery has been achieved with liquid crystal modulators and high-resolution, but quasi-static holograms are being recorded in photosensitive materials. However, the memory requirements and computational loads of real-time, large-area holography will be hard to tackle for several decades to come with the current paradigm based on a matrix calculations and bit-plane writing. Here, we experimentally demonstrate a conceptually novel, holistic approach to serial computation and repeatable writing of computer-generated dynamic holograms without Fourier transform, using minimal amounts of computer memory. We use the ultrafast opto-magnetic recording of holographic patterns in a ferrimagnetic film with femtosecond laser pulses, driven by on-the-fly hardware computation of a single holographic point. The intensity-threshold nature of the magnetic medium allows sub-diffraction-limited, point-by-point toggling of arbitrarily localized magnetic spots on the sample, according to the proposed circular detour-phase encoding, providing complex modulation and symmetrical suppression of upper diffractive orders and conjugated terms in holographically reconstructed 3-D images.

We present a laboratory system for single-shot magneto-optical (MO) imaging of ultrafast magnetization dynamics with high-sensitivity of MO rotation. We create a stack of MO images repeatedly employing a single pair of a pump and defocused probe pulses to induce and visualize MO changes in the sample. Both laser beams are independently wavelength-tunable allowing for a flexible, resonant adjustable two-color pump and probe scheme. To increase the MO contrast the probe beam is spatially filtered. We performed the all-optical switching experiment in Co-doped yttrium iron garnet films (YIG:Co) to demonstrate the capability of the presented method. We determine the spatial-temporal distribution of the effective field of photo-induced anisotropy driving the all-optical switching of the magnetization in YIG:Co film without an external magnetic field. Moreover, using this imaging method, we tracked the process of the laser-induced magnetization precession., Comment: 11 pages, 7 figures

This review discusses the ultrafast magnetization dynamics within the gigahertz to terahertz frequency range in ferrimagnetic rare-earth iron garnets with different substitutions. In these garnets, the roles of spin-orbit and exchange interactions have been detected using femtosecond laser pulses via the inverse Faraday effect. The all-optical control of spin-wave and Kaplan-Kittel exchange resonance modes in different frequency ranges is shown. Generation and localization of the electric field distribution inside the garnet through the metal-bound surface plasmon-polariton strongly enhance the amplitude of the exchange resonance modes. The exchange resonance mode in yttrium iron garnets was observed using circularly polarized Raman spectroscopy. The results of this study may be utilized in the development of a wide class of optomagnonic devices in the gigahertz to terahertz frequency range.

We report strong amplification of photo-magnetic spin precession in Co-doped YIG employing a surface plasmon excitation in a metal-dielectric magneto-plasmonic crystal. Plasmonic enhancement is accompanied by the localization of the excitation within the 300~nm-thick layer inside the transparent dielectric garnet. Experimental results are nicely reproduced by numerical simulations of the photo-magnetic excitation. Our findings demonstrate the magneto-plasmonic concept of subwavelength localization and amplification of the photo-magnetic excitation in dielectric YIG:Co and open up a path to all-optical magnetization switching below diffraction limit with energy efficiency approaching the fundamental limit for magnetic memories., Comment: 10 pages, 3 figures

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

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.

We analyze ultrafast electron dynamics in the time domain upon optical excitation of propagating surface plasmon-polaritons (SPs) in metal-dielectric heterostructures. Developing a kinetic model where both local and non-local electron relaxation in metals are included, we identify relevant timescales and extend the existing non-equilibrium electron dynamics framework onto the case of collective electronic excitations. The experimental data obtained in two distinct series of pump-probe measurements (with varied pump wavelength and angle of incidence) demonstrate SP-driven, one order of magnitude enhanced efficiency of the hot electron generation and the fourfold (up to 200 fs) slowdown of their non-local relaxation at the SP resonance. We discuss the perspectives of the SP-enabled manipulation of the non-equilibrium electron population lying at the crossover of photonics and ultrafast spintronics., Comment: 4 figures

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.

Ultrafast all-optical control of spins with femtosecond laser pulses is one of the hot topics at the crossroads of photonics and magnetism with a direct impact on future magnetic recording. Unveiling light-assisted recording mechanisms for an increase of the bit density beyond the diffraction limit without excessive heating of the recording medium is an open challenge. Here we show that surface plasmon-polaritons in hybrid metal-dielectric structures can provide spatial confinement of the inverse Faraday effect, mediating the excitation of localized coherent spin precession with 0.41 THz frequency. We demonstrate a two orders of magnitude enhancement of the excitation efficiency at the surface plasmon resonance within the 100 nm layer in dielectric garnet. Our findings broaden the horizons of ultrafast spin-plasmonics and open pathways towards non-thermal opto-magnetic recording at the nano-scale.

Finding a conceptually new way to control the magnetic state of media with the lowest possible production of heat and simultaneously at the fastest possible time-scale is a new challenge in fundamental magnetism [1-4] as well as an increasingly important issue in modern information technology [5]. Recent results demonstrate that exclusively in metals it is possible to switch magnetization between metastable states by femtosecond circularly polarized laser pulses [6-8]. However, despite the record breaking speed of the switching, the mechanisms in these materials are directly related to strong optical absorption and laser-induced heating close to the Curie temperature [9-12]. Here we report about ultrafast all-optical photo-magnetic recording in transparent dielectrics. In ferrimagnetic garnet film a single linearly polarized femtosecond laser pulse breaks the degeneracy between metastable magnetic states and promotes switching of spins between them. Changing the polarization of the laser pulse we deterministically steer the net magnetization in the garnet, write "0" and "1" magnetic bits at will. This mechanism operates at room temperature and allows ever fastest write-read magnetic recording event (< 20 ps) accompanied by unprecedentedly low heat load (< 6 J/cm3).