arXiv subjects

Christian David

Publications and source records attributed to Christian David.

34 records · Page 2Linked to original sources

arXiv2022

Hard X-ray helical dichroism of disordered molecular media

Chirality is a structural property of molecules lacking mirror symmetry that has strong implications in diverse fields, ranging from life to materials sciences. Established spectroscopic methods that are sensitive to chirality, such as circular dichroism (CD), exhibit weak signal contributions on an achiral background. Helical dichroism (HD), which is based on the orbital angular momentum (OAM) of light, offers a new approach to probe molecular chirality, but it has never been demonstrated on disordered samples. Furthermore, in the optical domain the challenge lies in the need to transfer the OAM of the photon to an electron that is localized on an Å-size orbital. Here, we overcome this challenge using hard X-rays with spiral Fresnel zone, which can induce an OAM. We present the first HD spectra of a disordered powder sample of enantiopure molecular complexes of [Fe(4,4'-diMebpy)3]2+ at the iron K-edge (7.1 keV) with OAM-carrying beams. The HD spectra exhibit the expected inversions of signs switching from a left to a right helical wave front or from an enantiomer to the other. The asymmetry ratios for the HD spectra are within one to five percent for OAM beams with topological charges of one and three. These results open a new window into the studies of molecular chirality and its interaction with the orbital angular momentum of light.

physics.chem-ph↗

arXiv2022

Generation of highly mutually coherent hard x-ray pulse pairs with an amplitude-splitting delay line

Beam splitters and delay lines are among the key building blocks of modern-day optical laser technologies. Progress in x-ray free electron laser source development and applications over the past decade is calling for their counter part operating in the Angstrom wavelength regime. Recent efforts in x-ray optics development have demonstrated relatively stable delay lines that most often adopted the division of wavefront approach for the beam splitting and recombination configuration. However, the two recombined beams have yet to achieve sufficient mutual coherence to enable applications such as interferometry, correlation spectroscopy, and nonlinear spectroscopy. We present the first experimental realization of the generation of highly mutually coherent pulse pairs using an amplitude-split delay line design based on transmission grating beam splitters and channel-cut crystal optic delay lines. The performance of the prototype system was analyzed in the context of x-ray coherent scattering and correlation spectroscopy, where we obtained nearly identical high-contrast speckle patterns from both branches. We show in addition the high level of dynamical stability during continuous delay scans, a capability essential for high sensitivity ultra-fast measurements.

physics.optics↗

arXiv2021

Hard X-ray Transient Grating Spectroscopy on Bismuth Germanate

Optical-domain Transient Grating (TG) spectroscopy is a versatile background-free four-wave-mixing technique used to probe vibrational, magnetic and electronic degrees of freedom in the time domain. The newly developed coherent X-ray Free Electron Laser sources allow its extension to the X-ray regime. Xrays offer multiple advantages for TG: their large penetration depth allows probing the bulk properties of materials, their element-specificity can address core-excited states, and their short wavelengths create excitation gratings with unprecedented momentum transfer and spatial resolution. We demonstrate for the first time TG excitation in the hard X-ray range at 7.1 keV. In Bismuth Germanate (BGO), the nonresonant TG excitation generates coherent optical phonons detected as a function of time by diffraction of an optical probe pulse. This experiment demonstrates the ability to probe bulk properties of materials and paves the way for ultrafast coherent four-wave-mixing techniques using X-ray probes and involving nanoscale TG spatial periods.

physics.optics↗

arXiv2021

Observation of magnetic helicoidal dichroism with extreme ultraviolet light vortices

We report on the experimental evidence of magnetic helicoidal dichroism, observed in the interaction of an extreme ultraviolet vortex beam carrying orbital angular momentum with a magnetic vortex. Numerical simulations based on classical electromagnetic theory show that this dichroism is based on the interference of light modes with different orbital angular momenta, which are populated after the interaction between the light phase chirality and the magnetic topology. This observation gives insight into the interplay between orbital angular momentum and magnetism, and sets the framework for the development of new analytical tools to investigate ultrafast magnetization dynamics.

physics.optics↗

arXiv2020

Time-Resolved XUV absorption spectroscopy and magnetic circular dichroism at the Ni $M_{2,3}$-edges

Ultrashort optical pulses can trigger a variety of non-equilibrium processes in magnetic thin films affecting electrons and spins on femtosecond timescales. In order to probe the charge and magnetic degrees of freedom simultaneously, we developed an x-ray streaking technique that has the advantage of providing a jitter-free picture of absorption cross section changes. In this paper, we present an experiment based on this approach which we performed using five photon probing energies at the Ni $M_{2,3}$-edges. This allowed us to retrieve the absorption and magnetic circular dichroism time traces, yielding detailed information on transient modifications of electron and spin populations close to the Fermi level. Our findings suggest that the observed charge and magnetic dynamics both depend on the XUV probing wavelength, and can be described, at least qualitatively, by assuming ultrafast energy shifts of the electronic and magnetic elemental absorption resonances, as reported in recent work. However, our analysis also hints at more complex changes, highlighting the need for further experimental and theoretical analysis in order to gain a thorough understanding of the interplay of electronic and spin degrees of freedom in optically excited magnetic thin films.

cond-mat.mtrl-sci↗

arXiv2020

Simultaneous two-color snapshot view on ultrafast charge and spin dynamics in a Fe-Cu-Ni tri-layer

Ultrafast phenomena on a femtosecond timescale are commonly examined by pump-probe experiments. This implies multiple measurements where the sample under investigation is pumped with a short light pulse and then probed with a second pulse at various time delays to follow its dynamics. Recently, the principle of streaking extreme ultraviolet (XUV) pulses in the temporal domain has enabled recording the dynamics of a system within a single pulse. However, separate pump-probe experiments at different absorption edges still lack a unified timing, when comparing the dynamics in complex systems. Here we report on an experiment using a dedicated optical element and the two-color emission of the FERMI XUV free-electron laser to follow the charge and spin dynamics in composite materials at two distinct absorption edges, simultaneously. The sample, consisting of ferromagnetic Fe and Ni layers, separated by a Cu layer, is pumped by an infrared laser and probed by a two-color XUV pulse with photon energies tuned to the M edges of these two transition metals. The experimental geometry intrinsically avoids any timing uncertainty between the two elements and unambiguously reveals an approximately 100 fs delay of the magnetic response with respect to the electronic excitation for both Fe and Ni. This delay shows that the electronic and spin degrees of freedom are decoupled during the demagnetization process. These observations underline the importance of simultaneous investigation of the temporal response of both charge and spin in multi-component materials. In a more general scenario, the experimental approach can be extended to continuous energy ranges, promising the development of jitter-free transient absorption spectroscopy in the XUV and soft X-ray regimes.

cond-mat.mtrl-sci↗

arXiv2018

Ptychographic characterization of polymer compound refractive lenses manufactured by additive technology

The recent success in the development of high precision printing techniques allows one to manufacture free-standing polymer structures of high quality. Two-photon polymerization lithography is a mask-less technique with down to 100 μm resolution that provides full geometric freedom. It has recently been applied to the nanofabrication of X-ray compound refractive lenses (CRLs). In this article we report on the characterization of two sets of CRLs of different design produced by two-photon polymerization induced lithography.

physics.optics↗

arXiv2018

Ghost Imaging at an XUV Free-Electron Laser

Radiation damage is one of the most severe resolution limiting factors in x-ray imaging, especially relevant to biological samples. One way of circumventing this problem is to exploit correlation-based methods developed in quantum imaging. Among these, there is ghost imaging (GI) in which the image is formed by radiation that has never interacted with the sample. Here, we demonstrate GI at an XUV free-electron laser by utilizing correlation techniques. We discuss the experimental challenges, optimal setup, and crucial ingredients to maximize the achievable resolution.

physics.optics↗

arXiv2018

Single shot time-resolved magnetic x-ray absorption at a Free Electron Laser

Ultrafast dynamics are generally investigated using stroboscopic pump-probe measurements, which characterize the sample properties for a single, specific time delay. These measurements are then repeated for a series of discrete time delays to reconstruct the overall time trace of the process. As a consequence, this approach is limited to the investigation of fully reversible phenomena. We recently introduced an off-axis zone plate based X-ray streaking technique, which overcomes this limitation by sampling the relaxation dynamics with a single femtosecond X-ray pulse streaked over a picosecond long time window. In this article we show that the X-ray absorption cross section can be employed as the contrast mechanism in this novel technique. We show that changes of the absorption cross section on the percent level can be resolved with this method. To this end we measure the ultrafast magnetization dynamics in CoDy alloy films. Investigating different chemical compositions and infrared pump fluences, we demonstrate the routine applicability of this technique. Probing in transmission the average magnetization dynamics of the entire film, our experimental findings indicate that the demagnetization time is independent of the specific infrared laser pump fluence. These results pave the way for the investigation of irreversible phenomena in a wide variety of scientific areas.

cond-mat.mtrl-sci↗

arXiv2018

Exploiting atomic layer deposition for fabricating sub-10 nm X-ray lenses

Moving towards significantly smaller nanostructures, direct structuring techniques such as electron beam lithography approach fundamental limitations in feature size and aspect ratios. Application of nanostructures like diffractive X-ray lenses requires feature sizes of below 10 nm to enter a new regime in high resolution X-raymicroscopy. As such dimensions are difficult to obtain using conventional electron beam lithography, we pursue a line-doubling approach. We demonstrate that thismethod yields structure sizes as small as 6.4 nm. X-ray lenses fabricated in this way are tested for their efficiency and microscopic resolution. In addition, the line-doubling technique is successfully extended to a six-fold scheme, where each line in a template structure written by electron beam lithography evolves into six metal lines.

physics.app-ph↗

arXiv2018

Generation and Measurement of Sub-Micrometer Relativistic Electron Beams

The generation of low-emittance electron beams has received significant interest in recent years. Driven by the requirements of X-ray free electron lasers, the emittance of photocathode injectors has been reduced significantly, with a corresponding increase in beam brightness. At the same time, this has put increasingly stringent requirements on the instrumentation to measure the beam size. These requirements are even more stringent for novel accelerator developments, such as laser-driven accelerators based on dielectric structures or on a plasma, or for linear colliders at the energy frontier. We present here the generation and measurement of a sub-micrometer electron beam, at a particle energy of 330 MeV, and a bunch charge below 1 pC. An electron beam optics with a beta-function of a few millimeters in the vertical plane had been set up. The beam was characterized through a wire scanner that employs a 1 um wide metallic structure fabricated using the electron beam lithography on a silicon nitride membrane. The smallest (rms) beam size presented here is less than 500 nm.

physics.acc-ph↗

arXiv2017

Tunable kinoform x-ray beam splitter

We demonstrate an x-ray beam splitter with high performances for multi-kilo-electron-volt photons. The device is based on diffraction on kinoform structures, which overcome the limitations of binary diffraction gratings. This beam splitter achieves a dynamical splitting ratio in the range 0-99.1% by tilting the optics and is tunable, here shown in a photon energy range of 7.2-19 keV. High diffraction efficiency of 62.6% together with an extinction ratio of 0.6% is demonstrated at 12.4 keV, with angular separation for the split beam of 0.5 mrad. This device can find applications in beam monitoring at synchrotrons, at x-ray free electron lasers for online diagnostics and beamline multiplexing and, possibly, as key elements for delay lines or ultrashort x-ray pulses manipulation.

physics.app-ph↗

arXiv2017

Systematic efficiency study of line-doubled zone plates

Line-doubled Fresnel zone plates provide nanoscale, high aspect ratio structures required for efficient high resolution imaging in the multi-keV x-ray range. For the fabrication of such optics a high aspect ratio HSQ resist template is produced by electron-beam lithography and then covered with Ir by atomic layer deposition (ALD).

cond-mat.mtrl-sci↗

arXiv2017

Fabrication of diamond diffraction gratings for experiments with intense hard x-rays

The demands on optical components to tolerate high radiation dose and manipulate hard x-ray beams that can fit the experiment requirements, are constantly increasing due to the advancements in the available x-ray sources. Here we have successfully fabricated the transmission type gratings using diamond, with structure sizes ranging from few tens of nanometres up to micrometres, and aspect ratio of up to 20. The efficiencies of the gratings were measured over a wide range of photon energies and their radiation tolerance was confirmed using the most intense x-ray source in the world. The fidelity of these grating structures was confirmed by the quality of the measured experimental results.

cond-mat.mtrl-sci↗

arXiv2016

High-Resolution Hard X-ray Holography by Unconfined Atomic Layer Deposited Phase-Shifting 3D References

We demonstrate high-resolution non-iterative holographic coherent diffraction imaging with hard X-rays using a novel phase-shifting reference, fabricated by atomic layer deposition to produce nanosharp 3D structure. The method surpasses the limitations associated with absorbing substrates predominantly employed in soft X-ray holography using extended, customized and point-source references. The unconfined experimental setup relaxes the technical constraints, allows effective data correction, and enables independent sample translation and rotation for data averaging and tomography. Applicable to single-shot measurements, phase and amplitude reconstructions of samples are retrieved with single-pixel resolution and differential contrast by simple non-iterative computation.

cond-mat.mes-hall↗

arXiv2006

Characterization of a CCD array for Bragg spectroscopy

The average pixel distance as well as the relative orientation of an array of 6 CCD detectors have been measured with accuracies of about 0.5 nm and 50 $μ$rad, respectively. Such a precision satisfies the needs of modern crystal spectroscopy experiments in the field of exotic atoms and highly charged ions. Two different measurements have been performed by illuminating masks in front of the detector array by remote sources of radiation. In one case, an aluminum mask was irradiated with X-rays and in a second attempt, a nanometric quartz wafer was illuminated by a light bulb. Both methods gave consistent results with a smaller error for the optical method. In addition, the thermal expansion of the CCD detectors was characterized between -105 C and -40 C.

physics.atom-ph↗