arXiv subjects

Lars Bocklage

Publications and source records attributed to Lars Bocklage.

17 recordsLinked to original sources

arXiv2026

Customized spin spirals in ferromagnetic thin films

The advancement of spintronic nanoscale devices hinges on the ability to flexibly engineer magnetic spin structures in thin-film stacks with precision and control. Meeting this demand remains a challenge for stable non-collinear spin configurations and, more specifically, vertical spin spirals in thin films. Innovative methods are required for their fabrication, stabilization and control. Here, we use oblique-incidence deposition to design and stabilize vertical spin spirals at room temperature and without an external field in magnetic thin films. We induce two crossed uniaxial magnetic anisotropies at the thin film boundaries. These anisotropies are tunable in direction and strength, thus providing control over the angular range and depth profile of the resulting spin spiral. The combination of polarized neutron reflectometry and nuclear resonant scattering enables precise and direct determination of the depth-dependent spin configurations. Our results establish a single-film design approach, in which the surface anisotropies independently serve as controllable design parameters for tailoring the vertical spin-spiral profile. Potential applications include nanoscale energy-storage devices, magnetic sensors, and ferromagnetic-resonance filters, advancing all-spin-based device engineering in general.

cond-mat.mtrl-sci↗

arXiv2025

Dark-fringe interferometer with dynamic phase control for M\"ossbauer science

Interference is a powerful tool for measuring and control. In M\"ossbauer science, interference effects are essential to most applications, due to the coherent scattering nature. However, M\"ossbauer interferometry remains challenging, due to stability requirements imposed by the short x-ray wavelength. Here, we put forward a ``dark fringe'' interferometer with vanishing transmission in the empty state, thereby facilitating sensitive measurements. The relative interferometer phase can dynamically be tuned by displacing a M\"ossbauer target. We experimentally demonstrate the tuning capabilities of this interferometer by controlling the transmitted x-ray intensity on nanosecond time scales. Then, we demonstrate sensitive measurements by observing the propagation of impulsively launched sound waves in the target over $\sim 10\,\mu s$. The interferometer concept opens avenues towards polarization-sensitive phase measurements, the generation of coherent multi-pulse sequences for controlling nuclear dynamics, and the implementation of feedback loops to adaptively optimize the interferometer, thereby fueling the further development of nuclear quantum optics.

quant-ph↗

arXiv2025

Single-shot sorting of M\"ossbauer time-domain data at X-ray free-electron lasers

M\"ossbauer spectroscopy is widely used to study structure and dynamics of matter with remarkably high energy resolution, provided by the narrow nuclear resonance line widths. However, the narrow width implies low count rates, such that experiments commonly average over extended measurement times or many x-ray pulses (``shots''). This averaging impedes the study of non-equilibrium phenomena. It has been suggested that X-ray free-electron lasers (XFELs) could enable M\"ossbauer single-shot measurements without averaging, and a proof-of-principle demonstration has been reported. However, so far, only a tiny fraction of all shots resulted in signal-photon numbers which are sufficiently high for a single-shot analysis. Here, we demonstrate coherent nuclear-forward-scattering of self-seeded XFEL radiation, with up to 900 signal-photons per shot. We develop a sorting approach which allows us to include all data on a single-shot level, independent of the signal content of the individual shots. It utilizes the presence of different dynamics classes, i.e. different nuclear evolutions after each excitation. Each shot is assigned to one of the classes, which can then be analyzed separately. Our approach determines the classes from the data without requiring theory modeling nor prior knowledge on the dynamics, making it also applicable to unknown phenomena. We envision that our approach opens up new grounds for M\"ossbauer science, enabling the study of out-of-equilibrium transient dynamics of the nuclei or their environment.

quant-ph↗

arXiv2025

Probing the Linewidth of the 12.4-keV Solid-State $^{45}$Sc Isomeric Resonance

The $^{45}$Sc nuclear transition from the ground to the isomeric state at 12.389~keV, with a lifetime of 0.46~s, exhibits an extraordinarily narrow natural width of 1.4~feV and a quality factor $\simeq 10^{19}$ -- surpassing those of the most precise atomic clocks -- making $^{45}$Sc a compelling platform for advanced metrology and nuclear clocks. Here we investigate how closely the spectral width and quality factor of the solid-state $^{45}$Sc resonance can approach these natural limits. Using the European X-ray Free-Electron Laser, we confirm the isomer's lifetime via time-delayed incoherent $K_{\alpha,\beta}$ fluorescence and observe previously unreported elastic fluorescence, yielding a partial internal conversion coefficient of 390(60). The absence of a clear nuclear forward scattering signal beyond a 2-ms delay implies environmental broadening of at least $500~\Gamma_{0}$ under experimental conditions, placing bounds on solid-state decoherence mechanisms. These findings set new experimental benchmarks for solid-state nuclear clock development.

quant-ph↗

arXiv2025

Interferometric measurement of nuclear resonant phase shift with a nanoscale Young double waveguide

The phase shift of an electromagnetic wave, imprinted by its interaction with atomic scatterers, is a central quantity in optics and photonics. In particular, it encodes information about optical resonances and photon-matter interaction. While being a routine task in the optical regime, interferometric measurements of phase shifts in the x-ray frequency regime are notoriously challenging due to the short wavelengths and associated stability requirements. As a result, the methods demonstrated to date are unsuitable for nanoscopic systems. Here, we demonstrate a nanoscale interferometer, inspired by Young's double-slit experiment, to measure the dispersive phase shift due to the 14.4 keV nuclear resonance of the M\"ossbauer isotope $^{57}$Fe coupled to an x-ray waveguide. From the single-photon interference patterns, we precisely extract the phase shifts in the vicinity of the nuclear resonance resolved in photon energy by using Bayesian inference. We find that the combined information from phase shift and absorbance reveals microscopic coupling parameters, which are not accessible from the intensity data alone. The demonstrated principle lays a basis for integrated x-ray interferometric sensors.

physics.optics↗

arXiv2025

Energy Time Ptychography for one-dimensional phase retrieval

Phase retrieval is at the heart of adaptive optics and modern high-resolution imaging. Without phase information, optical systems are limited to intensity-only measurements, hindering full reconstruction of object structures and wavefront dynamics essential for advanced applications. Here, we address a one-dimensional phase problem linking energy and time, which arises in X-ray scattering from ultrasharp nuclear resonances. We leverage the M\"ossbauer effect, where nuclei scatter radiation without energy loss to the lattice, and are sensitive to their magneto-chemical environments. Rather than using traditional spectroscopy with radioactive gamma-ray sources, we measure nuclear forward scattering of synchrotron X-ray pulses in the time domain, providing superior sensitivity and faster data acquisition. Extracting spectral information from a single measurement is challenging due to the missing phase information, typically requiring extensive modeling. Instead, we use multiple energetically overlapping measurements to retrieve both the transmission spectrum and the phase of the scattering response, similar to ptychographic phase retrieval in imaging. Our robust approach can overcome the bandwidth limitations of gamma-ray sources, opening new research directions with modern X-ray sources and M\"ossbauer isotopes.

physics.optics↗

arXiv2025

Constraints on magnetism and correlations in RuO$_2$ from lattice dynamics and M\"ossbauer spectroscopy

We provide experimental evidence for the absence of a magnetic moment in bulk RuO$_2$, a candidate altermagnetic material, by using a combination of M\"ossbauer spectroscopy, nuclear forward scattering, inelastic X-ray and neutron scattering, and density functional theory calculations. Using complementary M\"ossbauer and nuclear forward scattering we determine the $^{99}$Ru magnetic hyperfine splitting to be negligible. Inelastic X-ray and neutron scattering derived lattice dynamics of RuO$_2$ are compared to density functional theory calculations of varying flavors. Comparisons among theory with experiments indicate that electronic correlations, rather than magnetic order, are key in describing the lattice dynamics.

cond-mat.mtrl-sci↗

arXiv2024

TEMPUS, a Timepix4-based system for event-based X-rays detection

A readout system based on the Timepix4 ASIC, is being developed for photon science. The TEMPUS detector can be operated in two distinct modes: a photon counting mode, which allows for conventional full-frame readout at rates up to 40 kfps; and an event-driven time-stamping mode, which allows excellent time resolution in the nanosecond regime in measurements with moderate X-ray flux. In this paper, we introduce the initial prototype, a single-chip system, and present the first results obtained at PETRA III and ESRF.

physics.ins-det↗

arXiv2022

Strain and electric field control of magnetic and electrical transport properties in a magneto-elastically coupled Fe3O4/BaTiO3(001) heterostructure

We present a study of the control of electric field induced strain on the magnetic and electrical transport properties in a magneto-elastically coupled artificial multiferroic Fe3O4/BaTiO3 heterostructure. In this Fe3O4/BaTiO3 heterostructure, the Fe3O4 thin film is epitaxially grown in the form of bilateral domains, analogous to a-c stripe domains of the underlying BaTiO3(001) substrate. By in-situ electric field dependent magnetization measurements, we demonstrate the extrinsic control of the magnetic anisotropy and the characteristic Verwey metal-insulator transition of the epitaxial Fe3O4 thin film in a wide temperature range between 20-300 K, via strain mediated converse magnetoelectric coupling. In addition, we observe strain induced modulations in the magnetic and electrical transport properties of the Fe3O4 thin film across the thermally driven intrinsic ferroelectric and structural phase transitions of the BaTiO3 substrate. In-situ electric field dependent Raman measurements reveal that the electric field does not significantly modify the anti-phase boundary defects in the Fe3O4 thin film once it is thermodynamically stable after deposition and that the modification of the magnetic properties is mainly caused by strain induced lattice distortions and magnetic anisotropy. These results provide a framework to realize electrical control of the magnetization in a classical highly correlated transition metal oxide.

cond-mat.mtrl-sci↗

arXiv2022

Electronic Quantum Coherence in Glycine Molecules Probed with Ultrashort X-ray Pulses in Real Time

Quantum coherence between electronic states of a photoionized molecule and the resulting process of ultrafast electron-hole migration have been put forward as a possible quantum mechanism of charge-directed reactivity governing the photoionization-induced molecular decomposition. Attosecond experiments based on the indirect (fragment ion-based) characterization of the proposed electronic phenomena suggest that the photoionization-induced electronic coherence can survive for tens of femtoseconds, while some theoretical studies predict much faster decay of the coherence due to the quantum uncertainty in the nuclear positions and the nuclear-motion effects. The open questions are: do long-lived electronic quantum coherences exist in complex molecules and can they be probed directly, i.e. via electronic observables? Here, we use x-rays both to create and to directly probe quantum coherence in the photoionized amino acid glycine. The outgoing photoelectron wave leaves behind a positively charged ion that is in a coherent superposition of quantum mechanical eigenstates lying within the ionizing pulse spectral bandwidth. Delayed x-ray pulses track the induced coherence through resonant x-ray absorption that induces Auger decay and by the photoelectron emission from sequential double photoionization. Sinusoidal temporal modulation of the detected signal at early times (0 - 25 fs) is observed in both measurements. Advanced ab initio many-electron simulations, taking into account the quantum uncertainty in the nuclear positions, allow us to explain the first 25 fs of the detected coherent quantum evolution in terms of the electronic coherence.

physics.chem-ph↗

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↗

arXiv2017

Quantum Imaging with Incoherently Scattered Light from a Free-Electron Laser

The advent of accelerator-driven free-electron lasers (FEL) has opened new avenues for high-resolution structure determination via diffraction methods that go far beyond conventional x-ray crystallography methods. These techniques rely on coherent scattering processes that require the maintenance of first-order coherence of the radiation field throughout the imaging procedure. Here we show that higher-order degrees of coherence, displayed in the intensity correlations of incoherently scattered x-rays from an FEL, can be used to image two-dimensional objects with a spatial resolution close to or even below the Abbe limit. This constitutes a new approach towards structure determination based on incoherent processes, including Compton scattering, fluorescence emission or wavefront distortions, generally considered detrimental for imaging applications. Our method is an extension of the landmark intensity correlation measurements of Hanbury Brown and Twiss to higher than second-order paving the way towards determination of structure and dynamics of matter in regimes where coherent imaging methods have intrinsic limitations.

physics.ins-det↗

arXiv2017

Disentangling magnetic order on nanostructured surfaces

We present a synchrotron-based X-ray scattering technique which allows disentangling magnetic properties of heterogeneous systems with nanopatterned surfaces. This technique combines the nmrange spatial resolution of surface morphology features provided by Grazing Incidence Small Angle X-ray Scattering and the high sensitivity of Nuclear Resonant Scattering to magnetic order. A single experiment thus allows attributing magnetic properties to structural features of the sample; chemical and structural properties may be correlated analogously. We demonstrate how this technique shows the correlation between structural growth and evolution of magnetic properties for the case of a remarkable magnetization reversal in a structurally and magnetically nanopatterned sample system.

cond-mat.mes-hall↗

arXiv2017

Nuclear resonant surface diffraction

Nuclear resonant x-ray diffraction in grazing incidence geometry is used to determine the lateral magnetic configuration in a one-dimensional lattice of ferromagnetic nanostripes. During magnetic reversal, strong nuclear superstructure diffraction peaks appear in addition to the electronic ones due to an antiferromagnetic order in the nanostripe lattice. We show that the analysis of the angular distribution of the resonantly diffracted x-rays together with the time-dependence of the coherently diffracted nuclear signal reveals surface spin structures with very high sensitivity. This novel scattering technique provides a unique access to laterally correlated spin configurations in magnetically ordered nanostructures and, in perspective, also to their dynamics.

cond-mat.mtrl-sci↗

arXiv2014

Spin precession mapping at ferromagnetic resonance via nuclear resonant scattering

We probe the spin dynamics in a thin magnetic film at ferromagnetic resonance by nuclear resonant scattering of synchrotron radiation at the 14.4 keV resonance of $^{57}$Fe. The precession of the magnetization leads to an apparent reduction of the magnetic hyperfine field acting at the $^{57}$Fe nuclei. The spin dynamics is described in a stochastic relaxation model adapted to the ferromagnetic resonance theory by Smit and Beljers to model the decay of the excited nuclear state. From the fits of the measured data the shape of the precession cone of the spins is determined. Our results open a new perspective to determine magnetization dynamics in layered structures with very high depth resolution by employing ultrathin isotopic probe layers.

cond-mat.mtrl-sci↗

arXiv2010

Tunable energy transfer between dipolar-coupled magnetic disks by stimulated vortex gyration

A wide variety of coupled harmonic oscillators exist in nature1. Coupling between different oscillators allows for the possibility of mutual energy transfer between them2-4 and the information-signal propagation5,6. Low-energy input signals and their transport with low-energy dissipation are the key technical factors in the design of information processing devices7. Here, utilizing the concept of coupled oscillators, we experimentally demonstrated a robust new mechanism for energy transfer between spatially separated dipolar-coupled magnetic disks - stimulated vortex gyration. Direct experimental evidence was obtained by time-resolved soft X-ray microscopy. The rate of energy transfer from one disk to the other was deduced from the two normal modes' frequency splitting caused by dipolar interaction. This mechanism provides the advantages of tunable energy transfer rate, low-power input signal, and low-energy dissipation for magnetic elements with negligible damping. Coupled vortex-state disks are promising candidates for information-signal processing devices that operate above room temperature.

cond-mat.mtrl-sci↗

arXiv2008

Time-Resolved X-ray Microscopy of Spin-Torque-Induced Magnetic Vortex Gyration

Time-resolved X-ray microscopy is used to image the influence of alternating high-density currents on the magnetization dynamics of ferromagnetic vortices. Spin-torque induced vortex gyration is observed in micrometer-sized permalloy squares. The phases of the gyration in structures with different chirality are compared to an analytical model and micromagnetic simulations, considering both alternating spinpolarized currents and the current's Oersted field. In our case the driving force due to spin-transfer torque is about 70% of the total excitation while the remainder originates from the current's Oersted field. This finding has implications to magnetic storage devices using spin-torque driven magnetization switching and domain-wall motion.

cond-mat.other↗