Single and multi-pulse based X-ray photon correlation spectroscopy
Wonhyuk Jo, Stephan Stern, Fabian Westermeier, Rustam Rysov, Matthias Riepp, Julian Schmehr, Jörn Lange, Julian Becker, Michael Sprung, Torsten Laurus, Heinz Graafsma, Irina Lokteva, Gerhard Grübel, and Wojciech Roseker
The ability of pulsed nature of synchrotron radiation opens up the possibility of studying microsecond dynamics in complex materials via speckle-based techniques. Here, we present the study of measuring the dynamics of a colloidal system by combining single and multiple X-ray pulses of a storage ring. In addition, we apply speckle correlation techniques at various pulse patterns to collect correlation functions from nanoseconds to milliseconds. The obtained sample dynamics from all correlation techniques at different pulse patterns are in very good agreement with the expected dynamics of Brownian motions of silica nanoparticles in water. Our study will pave the way for future pulsed X-ray investigations at various synchrotron X-ray sources using individual X-ray pulse patterns.
Megahertz-rate ultrafast X-ray scattering and holographic imaging at the European XFEL
Nanna Zhou Hagström et. al.
The advent of X-ray free-electron lasers (XFELs) has revolutionized fundamental science, from atomic to condensed matter physics, from chemistry to biology, giving researchers access to X-rays with unprecedented brightness, coherence and pulse duration. All XFEL facilities built until recently provided X-ray pulses at a relatively low repetition rate, with limited data statistics. Here, results from the first megahertz-repetition-rate X-ray scattering experiments at the Spectroscopy and Coherent Scattering (SCS) instrument of the European XFEL are presented. The experimental capabilities that the SCS instrument offers, resulting from the operation at megahertz repetition rates and the availability of the novel DSSC 2D imaging detector, are illustrated. Time-resolved magnetic X-ray scattering and holographic imaging experiments in solid state samples were chosen as representative, providing an ideal test-bed for operation at megahertz rates. Our results are relevant and applicable to any other non-destructive XFEL experiments in the soft X-ray range.
In-vacuum Helmholtz coils for pulsed magnetic fields studying ultrafast demagnetization
M. Riepp et al.
The availability of sub 100 fs short and highly intense free-electron laser (FEL) pulses allows for new insights in laser-induced ultrafast demagnetization (LID) of ferromagnetic thin films on nanometer length scales. We designed a pair of in-vacuum Helmholtz coils, providing pulsed magnetic fields up to µ0Hz = ±45 mT, for time-resolved experiments at FEL sources in transmission geometry. We report on the implementation of the Helmholtz coils in an optical-pump–resonant-magnetic-scattering (tr-XRMS) experiment at the FEL FERMI (Elettra, Trieste) to study LID in different magnetic domain networks. We discuss the limitations for multi-shot measurements, that rely on the full reversibility of the demagnetization process in-between two pump–probe events, and emphasize the importance of reference–pump–probe schemes, especially in tr-XRMS experiments that employ external Hz fields.
Hard X-ray USAXS Fourier Transform Holography
W. Roseker et al.
We report on a Fourier transform holography study, employing hard X-ray energies at a 3rd generation storage ring. Nano-structures of various sizes and shapes have been measured in ultra small angle x-ray scattering configuration reaching a resolution in the holographic reconstructions of about 50 nm. Reliable holograms have been obtained with 6.9×106 incident photons. Our results provide an important step forward towards routine split-pulse Fourier transform holography measurements at FEL sources and 4th generation ultralow-emittance sources.
The beam stop as an intensity monitor
L. Müller et al.
Free-electron lasers (FELs) provide unique possibilities in investigating matter down to femtosecond time and nanometer length scales, as well as in the regime of non-linear light-matter interaction. Due to the nature of FEL sources, the produced beam is significantly more unstable than beams produced by 3rd generation synchrotrons. As a result, pulse-resolved normalization of measurement data becomes essential and can be challenging. The intensity monitors permanently installed at a facility might indeed accurately measure the pulse intensities at a certain point of the beamline, but cannot precisely normalize experimental data. For example the impact of pointing instabilities and hence different clipping of the beam downstream on the way to the actual experiment is not reflected in the intensity measurement. Here, we show how the integral intensity of the FEL beam transmitted through the sample can be measured by photodiodes providing a proper normalization of measurement data.
Modeling of ultrafast X-ray induced magnetization dynamics in magnetic multilayer systems
Kapcia, K.J., Tkachenko, V., Capotondi, F. et al.
In this work, we report on modeling results obtained with our recently developed simulation tool enabling nanoscopic description of electronic processes in X-ray irradiated ferromagnetic materials. With this tool, we have studied the response of Co/Pt multilayer system irradiated by an ultrafast extreme ultraviolet pulse at the M-edge of Co (photon energy ~60 eV). It was previously investigated experimentally at the FERMI free-electron-laser facility, using the magnetic small-angle X-ray scattering technique. Our simulations show that the magnetic scattering signal from cobalt decreases on femtosecond timescales due to electronic excitation, relaxation, and transport processes both in the cobalt and in the platinum layers, following the trend observed in the experimental data. The confirmation of the predominant role of electronic processes for X-ray induced demagnetization in the regime below the structural damage threshold is a step toward quantitative control and manipulation of X-ray induced magnetic processes on femtosecond timescales.
Nanoscale inhomogeneity of charge density waves dynamics in La2−xSrxNiO4
Gaetano Campi, Antonio Bianconi, Boby Joseph, Shrawan Kr Mishra, Leonard Müller, Alexey Zozulya, Agustinus Agung Nugroho, Sujoy Roy, Michael Sprung & Alessandro Ricci
While stripe phases with broken rotational symmetry of charge density are known to emerge in doped strongly correlated perovskites, the dynamics and heterogeneity of spatial ordering remain elusive. Here we shed light on the temperature dependent lattice motion and the spatial nanoscale phase separation of charge density wave order in the archetypal striped phase in La2−xSrxNiO4+y (LSNO) perovskite using X-ray photon correlation spectroscopy (XPCS) joint with scanning micro X-ray diffraction (SµXRD). While it is known that the CDW in 1/8 doped cuprates shows a remarkable stability we report the CDW motion dynamics by XPCS in nickelates with an anomalous quantum glass regime at low temperature, T < 65 K, and the expected thermal melting at higher temperature 65 < T < 120 K. The nanoscale CDW puddles with a shorter correlation length are more mobile than CDW puddles with a longer correlation length. The direct imaging of nanoscale spatial inhomogeneity of CDW by scanning micro X-ray diffraction (SµXRD) shows a nanoscale landscape of percolating short range dynamic CDW puddles competing with large quasi-static CDW puddles giving rise to a novel form of nanoscale phase separation of the incommensurate stripes order landscape.
Demonstration of 3D photon correlation spectroscopy in the hard X-ray regime
Wonhyuk Jo, Rustam Rysov, Fabian Westermeier, Michael Walther, Leonard Müller, André Philippi-Kobs, Matthias Riepp, Simon Marotzke, Irina Lokteva, Michael Sprung, Gerhard Grübel, and Wojciech Roseker
Three-dimensional photon correlation spectroscopy (3D PCS) is a well-known technique developed to suppress multiple scattering contributions in correlation functions, which are inevitably involved when an optical laser is employed to investigate dynamics in a turbid system. Here, we demonstrate a proof-of-principle study of 3D PCS in the hard X-ray regime. We employ an X-ray optical cross-correlator to measure the dynamics of silica colloidal nanoparticles dispersed in polypropylene glycol. The obtained cross correlation functions show very good agreement with auto-correlation measurements. This demonstration provides the foundation for X-ray speckle-based studies of very densely packed soft matter systems.
Measurement of Spin Dynamics in a Layered Nickelate Using X-Ray Photon Correlation Spectroscopy: Evidence for Intrinsic Destabilization of Incommensurate Stripes at Low Temperatures
Alessandro Ricci, Nicola Poccia, Gaetano Campi, Shrawan Mishra, Leonard Müller, Boby Joseph, Bo Shi, Alexey Zozulya, Marcel Buchholz, Christoph Trabant, James C. T. Lee, Jens Viefhaus, Jeroen B. Goedkoop, Agustinus Agung Nugroho, Markus Braden, Sujoy Roy, Michael Sprung, and Christian Schüßler-Langeheine
We study the temporal stability of stripe-type spin order in a layered nickelate with x-ray photon correlation spectroscopy and observe fluctuations on timescales of tens of minutes over a wide temperature range. These fluctuations show an anomalous temperature dependence: they slow down at intermediate temperatures and speed up on both heating and cooling. This behavior appears to be directly connected with spatial correlations: stripes fluctuate slowly when stripe correlation lengths are large and become faster when spatial correlations decrease. A low-temperature decay of nickelate stripe correlations, reminiscent of what occurs in cuprates as a result of a competition between stripes and superconductivity, hence occurs via loss of both spatial and temporal correlations.
Nanosecond X-ray photon correlation spectroscopy using pulse time structure of a storage-ring source
Wonhyuk Jo, Fabian Westermeier, Rustam Rysov, Olaf Leupold, Florian Schulz, Steffen Tober, Verena Markmann, Michael Sprung, Allesandro Ricci, Torsten Laurus, Allahgholi Aschkan, Alexander Klyuev, Ulrich Trunk, Heinz Graafsma, Gerhard Grübel, and Wojciech Roseker
X-ray photon correlation spectroscopy (XPCS) is a routine technique to study slow dynamics in complex systems at storage-ring sources. Achieving nanosecond time resolution with the conventional XPCS technique is, however, still an experimentally challenging task requiring fast detectors and sufficient photon flux. Here, the result of a nanosecond XPCS study of fast colloidal dynamics is shown by employing an adaptive gain integrating pixel detector (AGIPD) operated at frame rates of the intrinsic pulse structure of the storage ring. Correlation functions from single-pulse speckle patterns with the shortest correlation time of 192 ns have been calculated. These studies provide an important step towards routine fast XPCS studies at storage rings.
Enabling time-resolved 2D spatial-coherence measurements using the Fourier-analysis method with an integrated curved-grating beam monitor
Kai Bagschik, Michael Schneider, Jochen Wagner, Ralph Buss, Matthias Riepp, Andre Philippi-Kobs, Leonard Müller, Wojciech Roseker, Florian Trinter, Moritz Hoesch, Jens Viefhaus, Stefan Eisebitt, Gerhard Grübel, Hans Peter Oepen, and Robert Frömter
Direct 2D spatial-coherence measurements are increasingly gaining importance at synchrotron beamlines, especially due to present and future upgrades of synchrotron facilities to diffraction-limited storage rings. We present a method to determine the 2D spatial coherence of synchrotron radiation in a direct and particularly simple way by using the Fourier-analysis method in conjunction with curved gratings. Direct photon-beam monitoring provided by a curved grating circumvents the otherwise necessary separate determination of the illuminating intensity distribution required for the Fourier-analysis method. Hence, combining these two methods allows for time-resolved spatial-coherence measurements. As a consequence, spatial-coherence degradation effects caused by beamline optics vibrations, which is one of the key issues of state-of-the-art X-ray imaging and scattering beamlines, can be identified and analyzed.
Observation of compact ferrimagnetic skyrmions in DyCo3 film
K. Chen, D. Lott, A. Philippi-Kobs, M. Weigand, C. Luo, F. Radu
Owing to the experimental discovery of magnetic skyrmions stabilized by the Dzyaloshinskii–Moriya and/or dipolar interactions in thin films, there is a recent upsurge of interest in magnetic skyrmions with antiferromagnetic spins in order to overcome the fundamental limitations inherent with skyrmions in ferromagnetic materials. Here, we report on the observation of compact ferrimagnetic skyrmions for the class of amorphous alloys consisting of 4f rare-earth and 3d transition-metal elements with perpendicular magnetic anisotropy, using a DyCo3 film, that are identified by combining X-ray magnetic scattering, scanning transmission X-ray microscopy, and Hall transport technique. These skyrmions, with antiparallel aligned Dy and Co magnetic moments and a characteristic core radius of about 40 nm, are formed during the nucleation and annihilation of the magnetic maze-like domain pattern exhibiting a topological Hall effect contribution. Our findings provide a promising route for fundamental research in the field of ferrimagnetic/antiferromagnetic spintronics towards practical applications.
Double-pulse speckle contrast correlations with near Fourier transform limited free-electron laser light using hard X-ray split-and-delay
Wojciech Roseker, Sooheyong Lee, Michael Walther, Felix Lehmkühler, Birgit Hankiewicz, Rustam Rysov, Stephan O. Hruszkewycz, G. Brian Stephenson, Mark Sutton, Paul H. Fuoss, Marcin Sikorski, Aymeric Robert, Sanghoon Song & Gerhard Grübel
The ability to deliver two coherent X-ray pulses with precise time-delays ranging from a few femtoseconds to nanoseconds enables critical capabilities of probing ultra-fast phenomena in condensed matter systems at X-ray free electron laser (FEL) sources. Recent progress made in the hard X-ray split-and-delay optics developments now brings a very promising prospect for resolving atomic-scale motions that were not accessible by previous time-resolved techniques. Here, we report on characterizing the spatial and temporal coherence properties of the hard X-ray FEL beam after propagating through split-and-delay optics. Speckle contrast analysis of small-angle scattering measurements from nanoparticles reveals well-preserved transverse coherence of the beam. Measuring intensity fluctuations from successive X-ray pulses also reveals that only single or double temporal modes remain in the transmitted beam, corresponding to nearly Fourier transform limited pulses.
Direct 2D spatial-coherence determination using the Fourier-analysis method: multi-parameter characterization of the P04 beamline at PETRA III
Kai Bagschik, Jochen Wagner, Ralph Buß, Matthias Riepp, André Philippi-Kobs, Leonard Müller, Jens Buck, Florian Trinter, Frank Scholz, Jörn Seltmann, Moritz Hoesch, Jens Viefhaus, Gerhard Grübel, Hans Peter Oepen, and Robert Frömter
We present a systematic 2D spatial-coherence analysis of the soft-X-ray beamline P04 at PETRA III for various beamline configurations. The influence of two different beam-defining apertures on the spatial coherence properties of the beam is discussed and optimal conditions for coherence-based experiments are found. A significant degradation of the spatial coherence in the vertical direction has been measured and sources of this degradation are identified and discussed. The Fourier-analysis method, which gives fast and simple access to the 2D spatial coherence function of the X-ray beam, is used for the experiment. Here, we exploit the charge scattering of a disordered nanodot sample allowing the use of arbitrary X-ray photon energies with this method.
Observation of a Chirality-Induced Exchange-Bias Effect
K. Chen, A. Philippi-Kobs, V. Lauter, A. Vorobiev, E. Dyadkina, V. Yu. Yakovchuk, S. Stolyar, D. Lott
Chiral magnetism that manifests in the existence of skyrmions or chiral domain walls offers an alternative way for creating anisotropies in magnetic materials that might have large potential for application in future spintronic devices. Here we show experimental evidence for an alternative type of in-plane exchange-bias effect present at room temperature that is created from a chiral 90∘ domain wall at the interface of a ferrimagnetic-ferromagnetic Dy-Co/Ni-Fe bilayer system. The chiral interfacial domain wall forms due to the exchange coupling of Ni-Fe and Dy-Co at the interface and the presence of Dzyaloshinskii-Moriya interaction in the Dy-Co layer. As a consequence of the preferred chirality of the interfacial domain wall, the sign of the exchange-bias effect can be reversed by changing the perpendicular orientation of the Dy-Co magnetization. The chirality-created tunable exchange bias in Dy-Co/Ni-Fe is very robust against high in-plane magnetic fields (μ0H≤6T) and does not show any aging effects. Therefore, it overcomes the limitations of conventional exchange-bias systems.
Direct Visualization of Spatial Inhomogeneity of Spin Stripes Order in La1.72Sr0.28NiO4
Gaetano Campi, Nicola Poccia, Boby Joseph, Antonio Bianconi, Shrawan Mishra, James Lee, Sujoy Roy, Agustinus Agung Nugroho, Marcel Buchholz, Markus Braden, Christoph Trabant, Alexey Zozulya, Leonard Müller, Jens Viefhaus, Christian Schüßler-Langeheine 9, Michael Sprung and Alessandro Ricci
In several strongly correlated electron systems, the short range ordering of defects, charge and local lattice distortions are found to show complex inhomogeneous spatial distributions. There is growing evidence that such inhomogeneity plays a fundamental role in unique functionality of quantum complex materials. La1.72Sr0.28NiO4 is a prototypical strongly correlated perovskite showing spin stripes order. In this work we present the spatial distribution of the spin order inhomogeneity by applying micro X-ray diffraction to La1.72Sr0.28NiO4, mapping the spin-density-wave order below the 120 K onset temperature. We find that the spin-density-wave order shows the formation of nanoscale puddles with large spatial fluctuations. The nano-puddle density changes on the microscopic scale forming a multiscale phase separation extending from nanoscale to micron scale with scale-free distribution. Indeed spin-density-wave striped puddles are disconnected by spatial regions with negligible spin-density-wave order. The present work highlights the complex spatial nanoscale phase separation of spin stripes in nickelate perovskites and opens new perspectives of local spin order control by strain.
Spatial and temporal pre-alignment of an X-ray split-and-delay unit by laser light interferometry
Roseker, W. ; Lee, S. ; Walther, M. ; Rysov, R. ; Sprung, M. ; Gruebel, G.
We present a novel experimental setup for performing a precise pre-alignment of a hard X-ray split-and-delay unit based on low coherence light interferometry and high-precision penta-prisms. A split-and-delay unit is a sophisticated perfect crystal-optics device that splits an incoming X-ray pulse into two sub-pulses and generates a controlled time-delay between them. While the availability of a split-and-delay system will make ultrafast time-correlation and X-ray pump-probe experiments possible at free-electron lasers, its alignment process can be very tedious and time-consuming due to its complex construction. By implementing our experimental setup at beamline P10 of PETRA III, we were able to reduce the time of alignment to less than 3 h. We also propose an alternate method for finding the zero-time delay crossing without the use of X-rays or pulsed laser sources. The successful demonstration of this method brings prospect for operating the split-and-delay systems under alignment-time-critical environments such as X-ray free electron laser facilities.
Towards ultrafast dynamics with split-pulse X-ray photon correlation spectroscopy at free electron laser sources
Roseker, W. ; Hruszkewycz, S. O. ; Lehmkühler, F. ; Walther, M. ; Schulte-Schrepping, H. ; LEE, S. ; Osaka, T. ; Strüder, L. ;Hartmann, R. ; Sikorski, M. ; Song, S. ; Robert, A. ; Fuoss, P. H. ; Sutton, M. ; Stephenson, G. B. ; Grübel, G.
One of the important challenges in condensed matter science is to understand ultrafast, atomic-scale fluctuations that dictate dynamic processes in equilibrium and non-equilibrium materials. Here, we report an important step towards reaching that goal by using a state-of-the-art perfect crystal based split-and-delay system, capable of splitting individual X-ray pulses andintroducing femtosecond to nanosecond time delays. We show the results of an ultrafast hard X-ray Photon Correlation Spectroscopy experiment at LCLS where split X-ray pulses were used to measure the dynamics of gold nanoparticles suspended in hexane. We show how reliable speckle contrast values can be extracted even from very low intensity free electron laser(FEL) speckle patterns by applying maximum likelihood fitting, thus demonstrating the potential of a split-and-delay approach for dynamics measurements at FEL sources. This will enable the characterization of equilibrium and, importantly also reversible non-equilibrium processes in atomically disordered materials.
Note: Soft X-ray transmission polarizer based on ferromagnetic thin films
Mueller, L. ; Hartmann, G. ; Schleitzer, S. ; Berntsen, M. H. ; Walther, M. ; Rysov, R. ; Roseker, W. ; Scholz, F. ; Seltmann, J. ;Glaser, L. ; Viefhaus, J. ; Mertens, K. ; Bagschik, K. ; Frömter, R. ; De Fanis, A. ; Shevchuk, I. ; Medjanik, K. ; Öhrwall, G. ;Oepen, H. P. ; Martins, M. ; Meyer, M. ; Grübel, G.
A transmission polarizer for producing elliptically polarized soft X-ray radiation from linearly polarized light is presented. The setup is intended for use at synchrotron and free-electron laser beamlines that do not directly offer circularly polarized light for, e.g., X-ray magnetic circular dichroism (XMCD) measurements or holographic imaging. Here, we investigate the degree of ellipticity upon transmission of linearly polarized radiation through a cobalt thin film. The experiment was performed at a photon energy resonant to the Co L3-edge, i.e., 778 eV, and the polarization of the transmitted radiation was determined using a polarization analyzer that measures the directional dependence of photo electrons emitted from a gas target. Elliptically polarized radiation can be created at any absorption edge showing the XMCD effect by using the respective magnetic element.
Employing soft x-ray resonant magnetic scattering to study domain sizes and anisotropy in Co/Pd multilayers
K. Bagschik, R. Frömter, J. Bach, B. Beyersdorff, L. Müller, S. Schleitzer, M. Hårdensson Berntsen, C. Weier, R. Adam, J. Viefhaus, C. M. Schneider, G. Grübel, H. P. Oepen
It is demonstrated that the magnetic diffraction pattern of the isotropic disordered maze pattern is well described utilizing a gamma distribution of domain sizes in a one-dimensional model. From the analysis, the mean domain size and the shape parameter of the distribution are obtained. The model reveals an average domain size that is significantly different from the value that is determined from the peak position of the structure factor in reciprocal space. As a proof of principle, a wedge-shaped (CotÅ/Pd10Å)8 multilayer film, that covers the thickness range of the spin-reorientation transition, has been used. By means of soft x-ray resonant magnetic scattering (XRMS) and imaging techniques the thickness-driven evolution of the magnetic properties of the cobalt layers is explored. It is shown that minute changes of the domain pattern concerning domain size and geometry can be investigated and analyzed due to the high sensitivity and lateral resolution of the XRMS technique. The latter allows for the determination of the magnetic anisotropies of the cobalt layers within a thickness range of a few angstroms.
Phys. Rev. B 94, 134413 (2016)
Spatial coherence determination from the Fourier analysis of a resonant soft X-ray magnetic speckle pattern
K. Bagschik, R. Frömter, L. Müller, W. Roseker, J. Bach, P. Staeck, C. Thönnißen, S. Schleitzer, M. H. Berntsen, C. Weier, R. Adam, J. Viefhaus, C. M. Schneider, G. Grübel, H. P. Oepen
We present a method to determine the two-dimensional spatial coherence of synchrotron radiation in the soft X-ray regime by analyzing the Fourier transform of the magnetic speckle pattern from a ferromagnetic film in a multidomain state. To corroborate the results, a Young’s double-pinhole experiment has been performed. The transverse coherence lengths in vertical and horizontal direction of both approaches are in a good agreement. The method presented here is simple and gives a direct access to the coherence properties of synchrotron radiation without nanostructured test objects.
Opt. Express 24(20), 23162-23176 (2016)
Indirect excitation of ultrafast demagnetization
B. Vodungbo, et.al.
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.
Scientific Reports 6, Article number: 18970
Characterization of spatial coherence of synchrotron radiation with non-redundant arrays of apertures
P. Skopintsev, A. Singer, J. Bach, L. Müller, B. Beyersdorff, S. Schleitzer, O. Gorobtsov, A. Shabalin, R. P. Kurta, D. Dzhigaev, O. M. Yefanov, L. Glaser, A. Sakdinawat, G. Grübel, R. Frömter, H. P. Oepen, J. Viefhaus, I. A. Vartanyants
A method to characterize the spatial coherence of soft X-ray radiation from a single diffraction pattern is presented. The technique is based on scattering from non-redundant arrays (NRAs) of slits and records the degree of spatial coherence at several relative separations from 1 to 15 µm, simultaneously. Using NRAs the spatial coherence of the X-ray beam at the XUV X-ray beamline P04 of the PETRA III synchrotron storage ring was measured as a function of different beam parameters. To verify the results obtained with the NRAs, additional Young's double-pinhole experiments were conducted and showed good agreement.
J. Synchrotron Rad. 21, 722-728 (2014)
Imaging Ultrafast Demagnetization Dynamics after a Spatially Localized Optical Excitation
C. von Korff Schmising, B. Pfau, M. Schneider, C. M. Günther, M. Giovannella, J. Perron, B. Vodungbo, L. Müller, F. Capotondi, E. Pedersoli, N. Mahne, J. Lüning, S. Eisebitt
Ultrashort, coherent x-ray pulses of a free-electron laser are used to holographically image the magnetization dynamics within a magnetic domain pattern after creation of a localized excitation via an optical standing wave. We observe a spatially confined reduction of the magnetization within a couple of hundred femtoseconds followed by its slower recovery. Additionally, the experimental results show evidence of a spatial evolution of magnetization, which we attribute to ultrafast transport of nonequilibrium spin-polarized electrons for early times and to a fluence-dependent remagnetization rate for later times.
Phys. Rev. Lett. 112, 217203 (2014)
Endstation for ultrafast magnetic scattering experiments at the free-electron laser in Hamburg
L. Müller, C. Gutt, S. Streit-Nierobisch, M. Walther, S. Schaffert, B. Pfau, J. Geilhufe, F. Büttner, S. Flewett, C. M. Günther, S. Eisebitt, A. Kobs, M. Hille, D. Stickler, R. Frömter, H. P. Oepen, J. Lüning, G. Grübel
An endstation for pump–probe small-angle X-ray scattering (SAXS) experiments at the free-electron laser in Hamburg (FLASH) is presented. The endstation houses a solid-state absorber, optical incoupling for pump–probe experiments, time zero measurement, sample chamber, and detection unit. It can be used at all FLASH beamlines in the whole photon energy range offered by FLASH. The capabilities of the setup are demonstrated by showing the results of resonant magnetic SAXS measurements on cobalt-platinum multilayer samples grown on freestanding Si3N4 membranes and pump-laser-induced grid structures in multilayer samples.
Rev. Sci. Instrum. 84, 013906 (2013)
Invited Article: Coherent imaging using seeded free-electron laser pulses with variable polarization: First results and research opportunities
F. Capotondi, E. Pedersoli, N. Mahne, R. H. Menk, G. Passos, L. Raimondi, C. Svetina, G. Sandrin, M. Zangrando, M. Kiskinova, S. Bajt, M. Barthelmess, H. Fleckenstein, H. N. Chapman, J. Schulz, S. Schleitzer, L. Müller, C. Gutt, G. Grübel, et. al
FERMI@Elettra, the first vacuum ultraviolet and soft X-ray free-electron laser (FEL) using by default a “seeded” scheme, became operational in 2011 and has been opened to users since December 2012. The parameters of the seeded FERMI FEL pulses and, in particular, the superior control of emitted radiation in terms of spectral purity and stability meet the stringent requirements for single-shot and resonant coherent diffraction imaging (CDI) experiments. The advantages of the intense seeded FERMI pulses with variable polarization have been demonstrated with the first experiments performed using the multipurpose experimental station operated at the diffraction and projection imaging (DiProI) beamline. The results reported here were obtained with fixed non-periodic targets during the commissioning period in 2012 using 20–32 nm wavelength range. They demonstrate that the performance of the FERMI FEL source and the experimental station meets the requirements of CDI, holography, and resonant magnetic scattering in both multi- and single-shot modes. Moreover, we present the first magnetic scattering experiments employing the fully circularly polarized FERMI pulses. The ongoing developments aim at pushing the lateral resolution by using shorter wavelengths provided by double-stage cascaded FERMI FEL-2 and probing ultrafast dynamic processes using different pump-probe schemes, including jitter-free seed laser pump or FEL-pump/FEL-probe with two color FEL pulses generated by the same electron bunch.
Rev. Sci. Instrum. 84, 051301 (2013)
Breakdown of the X-Ray Resonant Magnetic Scattering Signal during Intense Pulses of Extreme Ultraviolet Free-Electron-Laser Radiation
We present results of single-shot resonant magnetic scattering experiments of Co/Pt multilayer systems using 100 fs long ultraintense pulses from an extreme ultraviolet (XUV) free-electron laser. An x-ray-induced breakdown of the resonant magnetic scattering channel during the pulse duration is observed at fluences of 5 J/cm2. Simultaneously, the speckle contrast of the high-fluence scattering pattern is significantly reduced. We performed simulations of the nonequilibrium evolution of the Co/Pt multilayer system during the XUV pulse duration. We find that the electronic state of the sample is strongly perturbed during the first few femtoseconds of exposure leading to an ultrafast quenching of the resonant magnetic scattering mechanism.
Phys. Rev. Lett. 110, 234801, (2013)
Nanoscale spin reversal by non-local angular momentum transfer following ultrafast laser excitation in ferrimagnetic GdFeCo
C. E. Graves, A. H. Reid, T. Wang, B. Wu, S. de Jong, K. Vahaplar, I. Radu, D. P. Bernstein, M. Messerschmidt, L. Müller, R. Coffee, M. Bionta, S. W. Epp, R. Hartmann, N. Kimmel, et. al.
Ultrafast laser techniques have revealed extraordinary spin dynamics in magnetic materials that equilibrium descriptions of magnetism cannot explain. Particularly important for future applications is understanding non-equilibrium spin dynamics following laser excitation on the nanoscale, yet the limited spatial resolution of optical laser techniques has impeded such nanoscale studies. Here we present ultrafast diffraction experiments with an X-ray laser that probes the nanoscale spin dynamics following optical laser excitation in the ferrimagnetic alloy GdFeCo, which exhibits macroscopic all-optical switching. Our study reveals that GdFeCo displays nanoscale chemical and magnetic inhomogeneities that affect the spin dynamics. In particular, we observe Gd spin reversal in Gd-rich nanoregions within the first picosecond driven by the non-local transfer of angular momentum from larger adjacent Fe-rich nanoregions. These results suggest that a magnetic material’s microstructure can be engineered to control transient laser-excited spins, potentially allowing faster (~ 1 ps) spin reversal than in present technologies.
Nature Materials 12, 293–298, (2013)
Ultrafast optical demagnetization manipulates nanoscale spin structure in domain walls
B. Pfau, S. Schaffert, L. Müller, C. Gutt, A. Al-Shemmary, F. Büttner, R. Delaunay, S. Düsterer, S. Flewett, R. Frömter, J. Geilhufe, E. Guehrs, C.M. Günther, R. Hawaldar, M. Hille, N. Jaouen, A. Kobs, K. Li, J. Mohanty, H. Redlin et. al
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.
Nature Communications 3, Article number: 1100
Femtosecond Single-Shot Imaging of Nanoscale Ferromagnetic Order in Co/Pd Multilayers Using Resonant X-Ray Holography
Tianhan Wang et al.
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/cm2. Employing resonant spatially muliplexed x-ray holography results in a low imaging threshold of 5 mJ/cm2. 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.
Phys. Rev. Lett. 108, 267403 (2012)