Femtosecond X-ray induced changes of the electronic and magnetic response of solids from electron redistribution.

Resonant X-ray absorption, where an X-ray photon excites a core electron into an unoccupied valence state, is an essential process in many standard X-ray spectroscopies. With increasing X-ray intensity, the X-ray absorption strength is expected to become nonlinear. Here, we report the onset of such a nonlinearity in the resonant X-ray absorption of magnetic Co/Pd multilayers near the Co L[Formula: see text] edge. The nonlinearity is directly observed through the change of the absorption spectrum, which is modified in less than 40 fs within 2 eV of its threshold. This is interpreted as a redistribution of valence electrons near the Fermi level. For our magnetic sample this also involves mixing of majority and minority spins, due to sample demagnetization. Our findings reveal that nonlinear X-ray responses of materials may already occur at relatively low intensities, where the macroscopic sample is not destroyed, providing insight into ultrafast charge and spin dynamics.

Magnetic Switching in Granular FePt Layers Promoted by Near-Field Laser Enhancement.

Light-matter interaction at the nanoscale in magnetic materials is a topic of intense research in view of potential applications in next-generation high-density magnetic recording. Laser-assisted switching provides a pathway for overcoming the material constraints of high-anisotropy and high-packing density media, though much about the dynamics of the switching process remains unexplored. We use ultrafast small-angle X-ray scattering at an X-ray free-electron laser to probe the magnetic switching dynamics of FePt nanoparticles embedded in a carbon matrix following excitation by an optical femtosecond laser pulse. We observe that the combination of laser excitation and applied static magnetic field, 1 order of magnitude smaller than the coercive field, can overcome the magnetic anisotropy barrier between "up" and "down" magnetization, enabling magnetization switching. This magnetic switching is found to be inhomogeneous throughout the material with some individual FePt nanoparticles neither switching nor demagnetizing. The origin of this behavior is identified as the near-field modification of the incident laser radiation around FePt nanoparticles. The fraction of not-switching nanoparticles is influenced by the heat flow between FePt and a heat-sink layer.

Femtosecond X-ray magnetic circular dichroism absorption spectroscopy at an X-ray free electron laser.

X-ray magnetic circular dichroism spectroscopy using an X-ray free electron laser is demonstrated with spectra over the Fe L(3,2)-edges. The high brightness of the X-ray free electron laser combined with high accuracy detection of incident and transmitted X-rays enables ultrafast X-ray magnetic circular dichroism studies of unprecedented sensitivity. This new capability is applied to a study of all-optical magnetic switching dynamics of Fe and Gd magnetic sublattices in a GdFeCo thin film above its magnetization compensation temperature.

Microwave soft x-ray microscopy for nanoscale magnetization dynamics in the 5-10 GHz frequency range.

We present a scanning transmission x-ray microscopy setup combined with a novel microwave synchronization scheme for studying high frequency magnetization dynamics at synchrotron light sources. The sensitivity necessary to detect small changes in the magnetization on short time scales and nanometer spatial dimensions is achieved by combining the excitation mechanism with single photon counting electronics that is locked to the synchrotron operation frequency. Our instrument is capable of creating direct images of dynamical phenomena in the 5-10 GHz range, with high spatial resolution. When used together with circularly polarized x-rays, the above capabilities can be combined to study magnetic phenomena at microwave frequencies, such as ferromagnetic resonance (FMR) and spin waves. We demonstrate the capabilities of our technique by presenting phase resolved images of a ∼6 GHz nanoscale spin wave generated by a spin torque oscillator, as well as the uniform ferromagnetic precession with ∼0.1° amplitude at ∼9 GHz in a micrometer-sized cobalt strip.

Nanoscale Confinement of All-Optical Magnetic Switching in TbFeCo--Competition with Nanoscale Heterogeneity.

Single femtosecond optical laser pulses, of sufficient intensity, are demonstrated to reverse magnetization in a process known as all-optical switching. Gold two-wire antennas are placed on the all-optical switching film TbFeCo. These structures are resonant with the optical field, and they create a field enhancement in the near-field which confines the area where optical switching can occur. The magnetic switching that occurs around and below the antenna is imaged using resonant X-ray holography and magnetic circular dichroism. The results not only show the feasibility of controllable switching with antenna assistance but also demonstrate the highly inhomogeneous nature of the switching process, which is attributed to the process depending on the material's heterogeneity.

Femtosecond single-shot imaging of nanoscale ferromagnetic order in Co/Pd multilayers using resonant x-ray holography.

We present the first single-shot images of ferromagnetic, nanoscale spin order taken with femtosecond x-ray pulses. X-ray-induced electron and spin dynamics can be outrun with pulses shorter than 80 fs in the investigated fluence regime, and no permanent aftereffects in the samples are observed below a fluence of 25 mJ/cm(2). Employing resonant spatially muliplexed x-ray holography results in a low imaging threshold of 5 mJ/cm(2). Our results open new ways to combine ultrafast laser spectroscopy with sequential snapshot imaging on a single sample, generating a movie of excited state dynamics.

High-resolution X-ray lensless imaging by differential holographic encoding.

We demonstrate in the soft x-ray regime a novel technique for high-resolution lensless imaging based on differential holographic encoding. We have achieved superior resolution over x-ray Fourier transform holography while maintaining the signal-to-noise ratio and algorithmic simplicity. We obtain a resolution of 16 nm by synthesizing images in the Fourier domain from a single diffraction pattern, which allows resolution improvement beyond the reference fabrication limit. Direct comparisons with iterative phase retrieval and images from state-of-the-art zone-plate microscopes are presented.

Holographic x-ray image reconstruction through the application of differential and integral operators.

We introduce a noniterative image-reconstruction technique for coherent diffractive imaging. Through the application of differential and integral operators, an extended reference can be used to recover the complex-valued transmissivity of an object, in closed form, from a measurement of its far-field (Fraunhofer) diffraction intensity. We demonstrate the feasibility of this approach, using a reference of a pair of crossed wires and slits, through numerical simulations and a soft x-ray coherent diffractive imaging experiment.

Phase retrieval in x-ray lensless holography by reference beam tuning.

We show the ability to determine the relative phase between the object and a reference scatterer by tuning the overall intensity and phase of the reference wave. The proposed reference-guided phase retrieval algorithm uses the relative phase as a constraint to iteratively reconstruct the object and the reference simultaneously, and thus does not require precisely defined reference structures. The algorithm also features rapid and reliable convergence and overcomes the uniqueness problem. The method is demonstrated by a soft-x-ray coherent imaging experiment that utilizes a large micrometer-sized reference structure that can be turned on and off, yielding an object image with resolution close to the reconstruction pixel size of 21 nm.

Extended field of view soft x-ray Fourier transform holography: toward imaging ultrafast evolution in a single shot.

Panoramic full-field imaging is demonstrated by applying spatial multiplexing to Fourier transform holography. Multiple object and reference waves extend the effective field of view for lensless imaging without compromising the spatial resolution. In this way, local regions of interest distributed throughout a sample can be simultaneously imaged with high spatial resolution. A method is proposed for capturing multiple ultrafast images of a sample with a single x-ray pulse.

Parallel versus antiparallel interfacial coupling in exchange biased Co/FeF2.

By using the surface and element specificity of soft x-ray magnetic dichroism we provide direct experimental evidence for two different types of interfacial uncompensated Fe moments in exchange biased Co/FeF2 bilayers. Some moments are pinned and coupled antiparallel to the ferromagnet (FM). They give rise to a positive exchange bias and vanish above T(N) = 78 together with the antiferromagnet (AF) order. Other interfacial Fe moments are unpinned and coupled parallel to the FM. They persist up to 300 K and give rise to magnetic order at the AF surface even above T(N) .