Boris Vodungbo

ultrafast optical demagnetization manipulates nanoscale spin structure in domain walls

During ultrafast demagnetization of a magnetically ordered solid, angular momentum has to be transferred between the spins, electrons, and phonons in the system on femto- and picosecond timescales. Although the intrinsic spin-transfer mechanisms are intensely debated, additional extrinsic mechanisms arising due to nanoscale heterogeneity have only recently entered the discussion. Here we use femtosecond X-ray pulses from a free-electron laser to study thin film samples with magnetic domain patterns. We observe an infrared-pump-induced change of the spin structure within the domain walls on the sub-picosecond timescale. This domain-topography-dependent contribution connects the intrinsic demagnetization process in each domain with spin-transport processes across the domain walls, demonstrating the importance of spin-dependent electron transport between differently magnetized regions as an ultrafast demagnetization channel. This pathway exists independent from structural inhomogeneities such as chemical interfaces, and gives rise to an ultrafast spatially varying response to optical pump pulses.

Polarization control of high order harmonics in the EUV photon energy range

We report the generation of circularly polarized high order harmonics in the extreme ultraviolet range (18-27 nm) from a linearly polarized infrared laser (40 fs, 0.25 TW) focused into a neon filled gas cell. To circularly polarize the initially linearly polarized harmonics we have implemented a four-reflector phase-shifter. Fully circularly polarized radiation has been obtained with an efficiency of a few percents, thus being significantly more efficient than currently demonstrated direct generation of elliptically polarized harmonics. This demonstration opens up new experimental capabilities based on high order harmonics, for example, in biology and materials science. The inherent femtosecond time resolution of high order harmonic generating table top laser sources renders these an ideal tool for the investigation of ultrafast magnetization dynamics now that the magnetic circular dichroism at the absorption M-edges of transition metals can be exploited.

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.

Structural dynamics during laser-induced ultrafast demagnetization

Funding from the European Communitys Seventh Framework Programme under Grant Agreement No. 312284 (CALIPSO Project) is gratefully acknowledged, as well as financial support received from the following agencies: (i) The French “Agence National de la Recherche” (ANR) via the projects UMAMI, ANR-11-LABX-0058_NIE and the EQUIPEX UNION (ANR-10-EQPX-52), and (ii) the CNRS-PICS program.

Multi-color imaging of magnetic Co/Pt heterostructures

We present an element specific and spatially resolved view of magnetic domains in Co/Pt heterostructures in the extreme ultraviolet spectral range. Resonant small-angle scattering and coherent imaging with Fourier-transform holography reveal nanoscale magnetic domain networks via magnetic dichroism of Co at the M2,3 edges as well as via strong dichroic signals at the O2,3 and N6,7 edges of Pt. We demonstrate for the first time simultaneous, two-color coherent imaging at a free-electron laser facility paving the way for a direct real space access to ultrafast magnetization dynamics in complex multicomponent material systems.

Polarization measurement of free electron laser pulses in the VUV generated by the variable polarization source FERMI

FERMI, based at Elettra (Trieste, Italy) is the first free electron laser (FEL) facility operated for user experiments in seeded mode. Another unique property of FERMI, among other FEL sources, is to allow control of the polarization state of the radiation. Polarization dependence in the study of the interaction of coherent, high field, short-pulse ionizing radiation with matter, is a new frontier with potential in a wide range of research areas. The first measurement of the polarization-state of VUV light from a single-pass FEL was performed at FERMI FEL-1 operated in the 52 nm-26 nm range. Three different experimental techniques were used. The experiments were carried out at the end-station of two different beamlines to assess the impact of transport optics and provide polarization data for the end user. In this paper we summarize the results obtained from different setups. The results are consistent with each other and allow a general discussion about the viability of permanent diagnostics aimed at monitoring the polarization of FEL pulses.

Ultrafast Dynamics of Magnetic Domain Structures Probed by Coherent Free-Electron Laser Light

The free-electron laser (FEL) sources FLASH in Hamburg, LCLS at Stanford, and FERMI in Trieste provide XUV to soft X-ray radiation (FLASH and FERMI) or soft to hard X-ray radiation (LCLS) with unprecedented parameters in terms of ultrashort pulse length, high photon flux, and coherence. These properties make FELs ideal tools for studying ultrafast dynamics in matter on a previously unaccessible level. This paper first reviews results obtained at FEL sources during the last few years in the field of magnetism research. We start with pioneering experiments at FLASH demonstrating the feasibility of magnetic scattering at FELs [1, 2], then present pump–probe scattering experiments [3, 4] as well as the first FEL magnetic imaging experiments [5], and finally discuss a limitation of the scattering methods due to a quenching of the magnetic scattering signal by high-fluence FEL pulses [6]. All of the presented experiments exploit the X-ray magnetic circular dichroism effect [7, 8] to obtain element-specific magnetic scattering contrast, as known from synchrotron experiments [9–12].

Single-shot Monitoring of Ultrafast Processes via X-ray Streaking at a Free Electron Laser

The advent of x-ray free electron lasers has extended the unique capabilities of resonant x-ray spectroscopy techniques to ultrafast time scales. Here, we report on a novel experimental method that allows retrieving with a single x-ray pulse the time evolution of an ultrafast process, not only at a few discrete time delays, but continuously over an extended time window. We used a single x-ray pulse to resolve the laser-induced ultrafast demagnetisation dynamics in a thin cobalt film over a time window of about 1.6 ps with an excellent signal to noise ratio. From one representative single shot measurement we extract a spin relaxation time of (130 ± 30) fs with an average value, based on 193 single shot events of (113 ± 20) fs. These results are limited by the achieved experimental time resolution of 120 fs, and both values are in excellent agreement with previous results and theoretical modelling. More generally, this new experimental approach to ultrafast x-ray spectroscopy paves the way to the study of non-repetitive processes that cannot be investigated using traditional repetitive pump-probe schemes.

Multi-Color Imaging of Magnetic Co/Pt Multilayers

We demonstrate for the first time the realization of a spatial resolved two color, element-specific imaging experiment at the free-electron laser facility FERMI. Coherent imaging using Fourier transform holography was used to achieve direct real space access to the nanometer length scale of magnetic domains of Co/Pt heterostructures via the element-specific magnetic dichroism in the extreme ultraviolet spectral range. As a first step to implement this technique for studies of ultrafast phenomena we present the spatially resolved response of magnetic domains upon femtosecond laser excitation.

Imaging Non-Local Magnetization Dynamics

Many fundamental processes in magnetism take place on a nanometer length and sub-picosecond time scale. An important example of such phenomena in magnetism is ultrafast, spin-polarized transport of laser-excited hot electrons, which is now being recognized as playing a crucial role for novel spintronic devices and for optically induced magnetic switching. Recent experimental examples include the demonstration of all-optical helicity dependent control of spin-polarized currents at interfaces [1], the design of novel and efficient terahertz emitters [2], and nanoscale spin reversal in chemically heterogeneous GdFeCo driven by non-local transfer of angular momentum [3]. In particular, for advanced information technologies with bit densities already exceeding 1 terabit per square inch with bit cell dimensions of (15 × 38 nm2) [4], it is of fundamental importance to understand and eventually control the mechanisms responsible for optically induced spin dynamics on the nanoscale.