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We present a new approach to femtosecond direct laser writing lithography to pattern nanocavities in ferromagnetic thin films. To demonstrate the concept we irradiated 300~nm thin nickel films by single intense femtosecond laser pulses through the glass substrate and created complex surface landscapes at the nickel-air interface. Using a fluence above the ablation threshold the process is destructive and irradiation leads to the formation of 200~nm thin flakes of nickel around the ablation crater as seen by electron microscopy. By progressively lowering the peak laser fluence, slightly below the ablation threshold the formation of closed spallation cavities is demonstrated by interferometric microscopy. Systematic studies by electron and optical interferometric microscopies enabled us to gain an understanding of the thermo-mechanical mechanism leading to spallation at the solid-molten interface, a conclusion supported by molecular dynamics simulations. We achieved a control of the spallation process that enabled the fabrication of closed spallation nanocavities and their periodic arrangements. Due to their topology closed magnetic nanocavities can support unique couplings of multiple excitations (magnetic, optical, acoustic, spintronic). Thereby, they offer a unique physics playground, before unavailable, for magnetism, magneto-photonic and magneto-acoustic applications., 4 figures

International audience; We perform a theoretical investigation of the magnetization switching in polycrystalline Ni nanoparticles induced by ultrashort pulses of surface acoustic waves via magnetoelastic interactions. In our numerical simulations, a Ni nanoparticle is modeled as an ellipsoidal disk deposited on a dielectric substrate. The in-plane external magnetic field breaks the symmetry and allows us to adjust the height of the energy barrier between two metastable magnetization states of the free-energy density and dramatically lower the amplitude of elastic strain pulses required for magnetization switching. The switching threshold is shown to depend on the duration of an acoustic pulse, the magnetic shape anisotropy of an elliptical nanoparticle, the amplitude of the external magnetic field, and the magnetostriction coefficient. We introduce the magnetoelastic switching diagram, allowing for the simultaneous visualization of the switching threshold and its characteristic timescale as a function of various physical parameters.

Engineering the magnetic properties (Gilbert damping, saturation magnetization, exchange stiffness, and magnetic anisotropy) of multicomponent magnetic compounds plays a key role in fundamental magnetism and its applications. Here, we perform a systematic study of ${({\mathrm{Ni}}_{81}{\mathrm{Fe}}_{19})}_{100\ensuremath{-}x}{\mathrm{Gd}}_{x}$ films with $x=0%$, 5%, 9%, and $13%$ using ferromagnetic resonance (FMR), element-specific time-resolved x-ray magnetic resonance, and femtosecond time-resolved magneto-optical pump-probe techniques. The comparative analysis of field and time domain FMR methods, with complimentary information extracted from the dynamics of high-frequency exchange magnons in ferromagnetic thin films, is used to investigate the dependence of Gilbert damping on the Gd concentration.

We demonstrate a novel method for the excitation of sizable magneto-optical effects in Au by means of the laser-induced injection of hot spin-polarized electrons in Au/Fe/MgO(0 0 1) heterostructures. It is based on the energy- and spin-dependent electron transmittance of Fe/Au interface which acts as a spin filter for non-thermalized electrons optically excited in Fe. We show that after crossing the interface, majority electrons propagate through the Au layer with the velocity on the order of 1 nm fs−1 (close to the Fermi velocity) and the decay length on the order of 100 nm. Featuring ultrafast functionality and requiring no strong external magnetic fields, spin injection results in a distinct magneto-optical response of Au. We develop a formalism based on the phase of the transient complex MOKE response and demonstrate its robustness in a plethora of experimental and theoretical MOKE studies on Au, including our ab initio calculations. Our work introduces a flexible tool to manipulate magneto-optical properties of metals on the femtosecond timescale that holds high potential for active magneto-photonics, plasmonics, and spintronics.

International audience; We investigate generation of exchange magnons by ultrashort, picosecond acoustic pulses propagating through ferromagnetic thin films. Using the Landau-Lifshitz-Gilbert equations we derive the dispersion relation for exchange magnons for an external magnetic field tilted with respect to the film normal. Decomposing the solution in a series of standing spin wave modes, we derive a system of ordinary differential equations and driven harmonic oscillator equations describing the dynamics of individual magnon mode. The external magnetoe-lastic driving force is given by the time-dependent spatial Fourier components of acoustic strain pulses inside the layer. Dependencies of the magnon excita-tion efficiencies on the duration of the acoustic pulses and the external magnetic field highlight the role of acoustic bandwidth and phonon-magnon phase matching. Our simulations for ferromagnetic nickel evidence the possibility of ultrafast magneto-acoustic excitation of exchange magnons within the band-width of acoustic pulses in thin samples under conditions readily obtained in femtosecond pump-probe experiments. $ Fully documented templates are available in the elsarticle package on CTAN.

Representing the future of spintronics, femtosecond spin current (SC) pulses constitute a versatile tool to transfer spin and control magnetization on the ultrafast timescale. It is therefore of paramount importance to understand the kinetics of these pulses and the fundamentals of their interaction with magnetized media. In our work, we demonstrate the key role of interfaces for the SC dynamics in Fe/Au/Fe multilayers. In particular, we argue that both (i) demagnetization caused by a pulse of hot electrons and (ii) spin transfer torque exerted by the orthogonal to the Fe magnetization projection of magnetic moment delivered by SC pulse are localized in the vicinity of the Fe/Au interface. We analyze both processes in details, showing that the SC-driven excitation of the sub-THz spin wave dynamics in Fe film is enabled by the spatial confinement of the exerted spin transfer torque. Moreover, a pulse of hot electrons leads to the efficient demagnetization of the Fe film. By disentangling the magneto-optical Kerr effect (MOKE) transients we demonstrate the strong spatial non-uniformity of this demagnetization. We argue that simultaneous recording of transient MOKE rotation and ellipticity is crucial for drawing such conclusions. Our findings have a twofold impact: firstly, they illustrate rich opportunities of utilizing SC pulses for manipulation of magnetization in ferromagnets and, secondly, they highlight the importance of spatial localization for understanding the ultrafast spin dynamics in multilayers.

Using the sensitivity of magneto-induced second harmonic generation to spin currents (SC), we demonstrate in Fe/Au/Fe/MgO(001) pseudo spin valves the generation of 250 fs-long SC pulses. Their temporal profile indicates that superdiffusive hot electron transport across a sub-100~nm Au layer is close to the ballistic limit and the pulse duration is primarily determined by the thermalization time of laser-excited hot carriers in Fe. Considering the calculated spin-dependent Fe/Au interface transmittance we conclude that a non-thermal spin-dependent Seebeck effect is responsible for the generation of ultrashort SC pulses. We also show that hot electron spins rotate upon interaction with non-collinear magnetization at the Au/Fe interface, which holds high potential for future spintronic devices., 5 pages, 4 figures

We discuss fundamental aspects of laser-induced ultrafast demagnetization probed by the time-resolved magneto-optical Kerr effect (MOKE). Studying thin Fe films on MgO substrate in the absence of electronic transport, we demonstrate how to disentangle pump-induced variations of magnetization and magneto-optical coefficients. We provide a mathematical formalism for retrieving genuine laser-induced magnetization dynamics and discuss its applicability in real experimental situations. We further stress the importance of temporal resolution achieved in the experiments and argue that measurements of both time-resolved MOKE rotation and ellipticity are needed for the correct assessment of magnetization dynamics on sub-picosecond timescales. The framework developed here sheds light onto the details of the time-resolved MOKE technique and contributes to the understanding of the interplay between ultrafast laser-induced optical and magnetic effects.

Further development of spintronics requires miniaturization and reduction of characteristic timescales of spin dynamics combining the nanometer spatial and femtosecond temporal ranges. These demands shift the focus of interest towards the fundamental open question of the interaction of femtosecond spin current (SC) pulses with a ferromagnet (FM). The spatio-temporal properties of the spin transfer torque (STT) exerted by ultrashort SC pulses on the FM open the time domain for studying STT fingerprint on spatially non-uniform magnetization dynamics. Using the sensitivity of magneto-induced second harmonic generation to SC, we develop technique for SC monitoring. With 20 fs resolution, we demonstrate the generation of 250 fs-long SC pulses in Fe/Au/Fe/MgO(001) structures. Their temporal profile indicates (i) nearly-ballistic hot electron transport in Au and (ii) that the pulse duration is primarily determined by the thermalization time of laser-excited hot carriers in Fe. Together with strongly spin-dependent Fe/Au interface transmission calculated for these carriers, this suggests the non-thermal spin-dependent Seebeck effect dominating the generation of ultrashort SC pulses. The analysis of SC transmission/reflection at the Au/Fe interface shows that hot electron spins orthogonal to the Fe magnetization rotate gaining huge parallel (anti-parallel) projection in transmitted (reflected) SC. This is accompanied by a STT-induced perturbation of the magnetization localized at the interface, which excites the inhomogeneous high-frequency spin dynamics in the FM. Time-resolved magneto-optical studies reveal the excitation of several standing spin wave modes in the Fe film with their spectrum extending up to 0.6 THz and indicating the STT spatial confinement to 2 nm.

Propagation dynamics of spin-dependent optical excitations is investigated by back-pump front-probe experiments in Au/Fe/MgO(001). We observe a decrease for all pump-probe signals detected at the Au surface, if the Fe thickness in increased. Relaxation processes within Fe limit the emission region of ballistic spins at the Fe/Au interface to ~1 nm.

We make a step towards the understanding of spin dynamics induced by spin-polarized hot carriers in metals. Exciting the Fe layer of Au/Fe/MgO(001) structures with femtosecond laser pulses, we demonstrate the ultrafast spin transport from Fe into Au using time-resolved MOKE and mSHG for depth-sensitive detection of the transient magnetization.

This paper discusses the dynamics of nanoparticle formation during the pulsed picosecond laser ablation of samples of crystalline and porous silicon by means of elastic light scattering. Experimental measurements are presented of how the signal produced by scattering at the ablation products depends on the distance between the probe radiation and the target surface. The differences of these dependences for crystalline and porous silicon wafers are discussed. It was found that the scattering kinetics of the probe radiation on the ablation products has two characteristic peaks at times of about several microseconds and several tens of microseconds, respectively.

Linear and nonlinear magneto-photonic properties of periodic arrays of nickel nanodimers are governed by the interplay of the (local) optical response of individual nanoparticles and (non-local) diffraction phenomena, with a striking example of Wood's anomaly. Angular and magnetic-field dependencies of the second harmonic intensity evidence Wood's anomaly when new diffraction orders emerge. Near-infrared spectroscopic measurements performed at different optical wavelengths and grating constants discriminate between the linear and nonlinear excitation mechanisms of Wood's anomalies. In the nonlinear regime the Wood's anomaly is characterized by an order-of-magnitude larger effect in intensity redistribution between the diffracted beams, as compared to the linear case. The nonlinear Wood's anomaly manifests itself also in the nonlinear magnetic contrast highlighting the prospects of nonlinear magneto-photonics., 8 pages, 6 figures