Spin Dynamics across Metallic Layers on the Few-Femtosecond Timescale.

We measure the light-driven response of a magnetic multilayer structure made of thin alternating layers of cobalt and platinum at the few-femtosecond timescale. Using attosecond magnetic circular dichroism, we observe how light rearranges the magnetic moment during and after excitation. The results reveal a sub-5 fs spike of magnetization in the platinum layer, which follows the shape of the driving pulse. With the help of time-dependent density functional theory, we interpret the observations as light-driven spin injection across the metallic layers of the structure. The light-triggered spin current is strikingly short, largely outpacing decoherence and dephasing. The findings suggest that the ability of shaping light fields in refined ways could be translated into shaping new forms of spin currents in materials.

Single-shot experiments at the soft X-FEL FERMI using a back-side-illuminated scientific CMOS detector.

The latest Complementary Metal Oxide Semiconductor (CMOS) 2D sensors now rival the performance of state-of-the-art photon detectors for optical application, combining a high-frame-rate speed with a wide dynamic range. While the advent of high-repetition-rate hard X-ray free-electron lasers (FELs) has boosted the development of complex large-area fast CCD detectors in the extreme ultraviolet (EUV) and soft X-ray domains, scientists lacked such high-performance 2D detectors, principally due to the very poor efficiency limited by the sensor processing. Recently, a new generation of large back-side-illuminated scientific CMOS sensors (CMOS-BSI) has been developed and commercialized. One of these cost-efficient and competitive sensors, the GSENSE400BSI, has been implemented and characterized, and the proof of concept has been carried out at a synchrotron or laser-based X-ray source. In this article, we explore the feasibility of single-shot ultra-fast experiments at FEL sources operating in the EUV/soft X-ray regime with an AXIS-SXR camera equipped with the GSENSE400BSI-TVISB sensor. We illustrate the detector capabilities by performing a soft X-ray magnetic scattering experiment at the DiProi end-station of the FERMI FEL. These measurements show the possibility of integrating this camera for collecting single-shot images at the 50 Hz operation mode of FERMI with a cropped image size of 700 × 700 pixels. The efficiency of the sensor at a working photon energy of 58 eV and the linearity over the large FEL intensity have been verified. Moreover, on-the-fly time-resolved single-shot X-ray resonant magnetic scattering imaging from prototype Co/Pt multilayer films has been carried out with a time collection gain of 30 compared to the classical start-and-stop acquisition method performed with the conventional CCD-BSI detector available at the end-station.

Single-shot experiments at the soft X-FEL FERMI using a back-side-illuminated scientific CMOS detector. Corrigendum.

The name of one of the authors in the article by Léveillé et al. [(2022), J. Synchrotron Rad. 29, 103-110] is corrected.

Sub-15-fs X-ray pump and X-ray probe experiment for the study of ultrafast magnetization dynamics in ferromagnetic alloys.

In this paper, we present a new setup for the measurement of element-specific ultrafast magnetization dynamics in ferromagnetic thin films with a sub-15-fs time resolution. Our experiment relies on a split and delay approach which allows us to fully exploit the shortest X-rays pulses delivered by X-ray Free Electrons Lasers (close to the attosecond range), in an X-ray pump - X-ray probe geometry. The setup performance is demonstrated by measuring the ultrafast elemental response of Ni and Fe during demagnetization of ferromagnetic Ni and Ni80Fe20 (Permalloy) samples upon resonant excitation at the corresponding absorption edges. The transient demagnetization process is measured in both reflection and transmission geometry using, respectively, the transverse magneto-optical Kerr effect (T-MOKE) and the Faraday effect as probing mechanisms.

Pump-probe experiments at the TEMPO beamline using the low-α operation mode of Synchrotron SOLEIL.

The SOLEIL synchrotron radiation source is regularly operated in special filling modes dedicated to pump-probe experiments. Among others, the low-α mode operation is characterized by shorter pulse duration and represents the natural bridge between 50 ps synchrotron pulses and femtosecond experiments. Here, the capabilities in low-α mode of the experimental set-ups developed at the TEMPO beamline to perform pump-probe experiments with soft X-rays based on photoelectron or photon detection are presented. A 282 kHz repetition-rate femtosecond laser is synchronized with the synchrotron radiation time structure to induce fast electronic and/or magnetic excitations. Detection is performed using a two-dimensional space resolution plus time resolution detector based on microchannel plates equipped with a delay line. Results of time-resolved photoelectron spectroscopy, circular dichroism and magnetic scattering experiments are reported, and their respective advantages and limitations in the framework of high-time-resolution pump-probe experiments compared and discussed.

Magnetic imaging by Fourier transform holography using linearly polarized x-rays.

We present a method for imaging magnetic domains via x-ray Fourier transform holography at linearly polarized sources. Our approach is based on the separation of holographic mask and sample and on the Faraday rotation induced on the reference wave. We compare images of perpendicular magnetic domains obtained with either linearly or circularly polarized x-rays and discuss the relevance of this method to future experiments at free-electron laser and high-harmonic-generation sources.

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.

Analytic description and optimization of magneto-optical Kerr setups with photoelastic modulation.

Instruments based on the magneto-optical Kerr effect are routinely used to probe surface magnetic properties. These tools rely on the characterization of the polarization state of reflected light from the sample to collect information on its magnetization. Here, we present a theoretical optimization of common setups based on the magneto-optical Kerr effect. A detection scheme based on a simple analyzer and photodetector and one made from a polarizing beam splitter and balanced photodetectors are considered. The effect of including a photoelastic modulator (PEM) and a lock-in amplifier to detect the signal at harmonics of the modulating frequency is studied. Jones formalism is used to derive general expressions that link the intensity of the measured signal to the magneto-optical Fresnel reflection coefficients for any orientation of the polarizing optical components. Optimal configurations are then defined as those that allow measuring the Kerr rotation and ellipticity while minimizing nonmagnetic contributions from the diagonal Fresnel coefficients in order to improve the signal-to-noise ratio (SNR). The expressions show that with the PEM, setups based on polarizing beam splitters inherently offer a twofold higher signal than commonly used analyzers, and the experimental results confirm that the SNR is improved by more than 150%. Furthermore, we find that while all proposed detection schemes measure Kerr effects, only those with polarizing beam splitters allow measuring the Kerr rotation directly when no modulator is included. This accommodates, for instance, time-resolved measurements at relatively low laser pulse repetition rates. Ultrafast demagnetization measurements are presented as an example of such applications.

Toward ultrafast magnetic depth profiling using time-resolved x-ray resonant magnetic reflectivity.

During the last two decades, a variety of models have been developed to explain the ultrafast quenching of magnetization following femtosecond optical excitation. These models can be classified into two broad categories, relying either on a local or a non-local transfer of angular momentum. The acquisition of the magnetic depth profiles with femtosecond resolution, using time-resolved x-ray resonant magnetic reflectivity, can distinguish local and non-local effects. Here, we demonstrate the feasibility of this technique in a pump-probe geometry using a custom-built reflectometer at the FLASH2 free-electron laser (FEL). Although FLASH2 is limited to the production of photons with a fundamental wavelength of 4 nm ( ≃ 310 eV ), we were able to probe close to the Fe L 3 edge ( 706.8 eV ) of a magnetic thin film employing the third harmonic of the FEL. Our approach allows us to extract structural and magnetic asymmetry signals revealing two dynamics on different time scales which underpin a non-homogeneous loss of magnetization and a significant dilation of 2 Å of the layer thickness followed by oscillations. Future analysis of the data will pave the way to a full quantitative description of the transient magnetic depth profile combining femtosecond with nanometer resolution, which will provide further insight into the microscopic mechanisms underlying ultrafast demagnetization.

Experimental setup for lensless imaging via soft x-ray resonant scattering.

We have developed a setup for measuring holographically formed interference patterns using an integrated sample-mask design. The direct space image of the sample is obtained via a two-dimensional Fourier transform of the X-ray diffraction pattern. We present the details of our setup, commenting on the influence of geometrical parameters on the imaging capabilities. As an example, we present and discuss the results of test experiments on a patterned Co film.

Indirect excitation of ultrafast demagnetization.

Does the excitation of ultrafast magnetization require direct interaction between the photons of the optical pump pulse and the magnetic layer? Here, we demonstrate unambiguously that this is not the case. For this we have studied the magnetization dynamics of a ferromagnetic cobalt/palladium multilayer capped by an IR-opaque aluminum layer. Upon excitation with an intense femtosecond-short IR laser pulse, the film exhibits the classical ultrafast demagnetization phenomenon although only a negligible number of IR photons penetrate the aluminum layer. In comparison with an uncapped cobalt/palladium reference film, the initial demagnetization of the capped film occurs with a delayed onset and at a slower rate. Both observations are qualitatively in line with energy transport from the aluminum layer into the underlying magnetic film by the excited, hot electrons of the aluminum film. Our data thus confirm recent theoretical predictions.

Widely tunable two-colour seeded free-electron laser source for resonant-pump resonant-probe magnetic scattering.

The advent of free-electron laser (FEL) sources delivering two synchronized pulses of different wavelengths (or colours) has made available a whole range of novel pump-probe experiments. This communication describes a major step forward using a new configuration of the FERMI FEL-seeded source to deliver two pulses with different wavelengths, each tunable independently over a broad spectral range with adjustable time delay. The FEL scheme makes use of two seed laser beams of different wavelengths and of a split radiator section to generate two extreme ultraviolet pulses from distinct portions of the same electron bunch. The tunability range of this new two-colour source meets the requirements of double-resonant FEL pump/FEL probe time-resolved studies. We demonstrate its performance in a proof-of-principle magnetic scattering experiment in Fe-Ni compounds, by tuning the FEL wavelengths to the Fe and Ni 3p resonances.

Thermally induced magnetization switching in Fe/MnAs/GaAs(001): selectable magnetic configurations by temperature and field control.

Spintronic devices currently rely on magnetization control by external magnetic fields or spin-polarized currents. Developing temperature-driven magnetization control has potential for achieving enhanced device functionalities. Recently, there has been much interest in thermally induced magnetisation switching (TIMS), where the temperature control of intrinsic material properties drives a deterministic switching without applying external fields. TIMS, mainly investigated in rare-earth-transition-metal ferrimagnets, has also been observed in epitaxial Fe/MnAs/GaAs(001), where it stems from a completely different physical mechanism. In Fe/MnAs temperature actually modifies the surface dipolar fields associated with the MnAs magnetic microstructure. This in turn determines the effective magnetic field acting on the Fe overlayer. In this way one can reverse the Fe magnetization direction by performing thermal cycles at ambient temperatures. Here we use element selective magnetization measurements to demonstrate that various magnetic configurations of the Fe/MnAs/GaAs(001) system are stabilized predictably by acting on the thermal cycle parameters and on the presence of a bias field. We show in particular that the maximum temperature reached during the cycle affects the final magnetic configuration. Our findings show that applications are possible for fast magnetization switching, where local temperature changes are induced by laser excitations.

Design and performance of AERHA, a high acceptance high resolution soft x-ray spectrometer.

A soft x-ray spectrometer based on the use of an elliptical focusing mirror and a plane varied line spacing grating is described. It achieves both high resolution and high overall efficiency while remaining relatively compact. The instrument is dedicated to resonant inelastic x-ray scattering studies. We set out how this optical arrangement was judged best able to guarantee performance for the 50 - 1000 eV range within achievable fabrication targets. The AERHA (adjustable energy resolution high acceptance) spectrometer operates with an effective angular acceptance between 100 and 250 µsr (energy dependent) and a resolving power well in excess of 5000 according to the Rayleigh criterion. The high angular acceptance is obtained by means of a collecting pre-mirror. Three scattering geometries are available to enable momentum dependent measurements with 135°, 90°, and 50° scattering angles. The instrument operates on the Synchrotron SOLEIL SEXTANTS beamline which serves as a high photon flux 2 × 200 µm(2) focal spot source with full polarization control.

Laser-induced ultrafast demagnetization in the presence of a nanoscale magnetic domain network.

Femtosecond magnetization phenomena have been challenging our understanding for over a decade. Most experiments have relied on infrared femtosecond lasers, limiting the spatial resolution to a few micrometres. With the advent of femtosecond X-ray sources, nanometric resolution can now be reached, which matches key length scales in femtomagnetism such as the travelling length of excited 'hot' electrons on a femtosecond timescale. Here we study laser-induced ultrafast demagnetization in [Co/Pd](30) multilayer films, which, for the first time, achieves a spatial resolution better than 100 nm by using femtosecond soft X-ray pulses. This allows us to follow the femtosecond demagnetization process in a magnetic system consisting of alternating nanometric domains of opposite magnetization. No modification of the magnetic structure is observed, but, in comparison with uniformly magnetized systems of similar composition, we find a significantly faster demagnetization time. We argue that this may be caused by direct transfer of spin angular momentum between neighbouring domains.

Performances of a bent-crystal spectrometer adapted to resonant x-ray emission measurements on gas-phase samples.

We describe a bent-crystal spectrometer adapted to measure x-ray emission resulting from core-level excitation of gas-phase molecules in the 0.8-8 keV energy range. The spectrometer is based on the Johann principle, and uses a microfocused photon beam to provide high-resolution (resolving power of approximately 7500). A gas cell was designed to hold a high-pressure (300 mbar) sample of gas while maintaining a high vacuum (10(-9) mbar) in the chamber. The cell was designed to optimize the counting rate (2000 cts/s at the maximum of the Cl Kalpha emission line), while minimizing self-absorption. Example of the Kalpha emission lines of CH(3)Cl molecules is presented to illustrate the capabilities of this new instrument.