arXiv subjects

Ralf Röhlsberger

Publications and source records attributed to Ralf Röhlsberger.

At least 19 recordsLinked to original sources

arXiv2026

Probing the Linewidth of the 12.4-keV $^{45}$Sc Isomeric Resonance in Solids by Nuclear Forward Scattering

The $^{45}$Sc transition from the nuclear ground state to the 12.389-keV isomer (lifetime 0.46~s) has an ultranarrow natural linewidth $Γ_{\ind{0}}\simeq 1.4$~feV, corresponding to a quality factor $\simeq 10^{19}$. This makes $^{45}$Sc a compelling candidate for nuclear-clock metrology, provided that coherence in solids can be maintained close to the natural limit. Here we investigate the linewidth and coherence properties of the $^{45}$Sc resonance in solids following resonant x-ray pumping. Using the European XFEL, we confirm persistence of the long-lived isomer excitation in a solid-state environment via time-delayed incoherent $K_{α,β}$ emission and observe a weak delayed elastic channel at 12.4~keV, from which we extract a partial internal-conversion coefficient $α_{K}=390(60)$. Time-domain nuclear forward scattering measurements in crystals of Sc, Sc$_2$O$_3$, ScN and ScAlMgO$_4$ at 20~K show no statistically significant coherent forward-scattering signal beyond $2$~ms; within the adopted linewidth-broadening model, we infer an effective broadening $ΔΓ\gtrsim 500\,Γ_{\ind{0}}$. These results provide the quantitative constraints on linewidth broadening in solid-state $^{45}$Sc with an intrinsic natural linewidth in the femto-electronvolt range thereby laying the groundwork for precision metrology in the X-ray regime and future nuclear-clock frequency references using $^{45}$Sc nuclear isomer.

quant-ph↗

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↗

arXiv2026

Nuclear Heterodyne Interferometry for Gravitational Spectroscopy

Gravitational spectroscopy tests the coupling of gravity to matter by measuring gravitationally induced frequency shifts of quantum transitions. While modern optical clocks probe the gravitational response of electronic transitions with extraordinary precision, tests in the nuclear sector have not progressed since the Mössbauer measurements of the gravitational redshift by Pound and Rebka. Here we introduce a new approach to nuclear gravitational spectroscopy based on phase-sensitive heterodyne interferometry of time-resolved nuclear resonant scattering of synchrotron radiation. In this scheme the gravitational redshift appears as a slowly accumulating phase drift of a delayed heterodyne beat signal, converting nuclear gravitational spectroscopy from energy-domain detection to time-domain interferometry. A Fisher-information analysis supported by Monte Carlo simulations and experimentally confirmed photon count rates shows that the nuclear gravitational redshift of $^{57}$Fe can be detected within hours on a few-meter-scale vertical baseline, with percent-level precision on deviations from general relativity becoming accessible on day-scale timescales. The method thus establishes an experimentally realistic and scalable platform for precision tests of gravitational coupling to nuclear structure.

physics.ins-det↗

arXiv2026

Single-shot sorting of Mössbauer time-domain data at X-ray free-electron lasers

Mössbauer 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 Mössbauer 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 Mössbauer science, enabling the study of out-of-equilibrium transient dynamics of the nuclei or their environment.

quant-ph↗

arXiv2025

Single-particle incoherent diffractive imaging and amplified spontaneous emission in copper nanocubes

We demonstrate element-specific incoherent diffractive imaging (IDI) of single copper nanocubes using intensity correlations of K$α$ fluorescence at a hard X-ray free-electron laser. Combining single particle diffraction classification with IDI, we retrieve the form factor of 88 nm cubes with 20 nm resolution, extending IDI to the destructive single-particle regime with a large gain in resolution. IDI visibility drops sharply above a fluence of $10^2$ J/cm$^2$, consistent with the assumption of amplified spontaneous emission. Our results reveal fundamental limits for high-fluence nanoimaging towards future single-particle X-ray imaging.

physics.optics↗

arXiv2025

Nonlinear phenomena in X-ray fluorescence from single nanoparticles under extreme conditions

Materials exposed to intense femtosecond X-ray pulses with energies above their K-shell absorption edge can enter an extremely ionized state, which could give rise to nonlinear phenomena, such as saturable absorption and reverse saturable absorption. In this work, we investigate these effects on single copper nanoparticles irradiated by an X-ray free-electron laser pulse. We study the properties of the K$α$ fluorescence for two different short pulse durations and three X-ray incident energies below and above the K-shell absorption edge, and correlate these with incident fluence estimates based on coherent diffraction. We observe that the incident fluence of the pulse and not its duration, is the main factor that modulates the nonlinear response, which leads to an effective shortening of the fluorescence emission. Our findings have implications for fluorescence-based methods for imaging single particles using transiently coherent fluorescence, or diffractive imaging through transient resonances.

physics.optics↗

arXiv2025

Dark-fringe interferometer with dynamic phase control for Mössbauer science

Interference is a powerful tool for measuring and control. In Mössbauer science, interference effects are essential to most applications, due to the coherent scattering nature. However, Mössbauer 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 Mössbauer 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 $\sim 10\,μs$. 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

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 Mössbauer 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 Mössbauer isotopes.

physics.optics↗

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 Mössbauer 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

Collective nuclear excitation and pulse propagation in single-mode x-ray waveguides

Waveguides offer a means to controllably couple atomic ensembles to the electromagnetic field therein. Here, we demonstrate x-ray propagation in planar thin-film waveguides coupled to Mössbauer nuclei under collective resonant excitation by short pulses of synchrotron radiation. We record x-ray photons that have been emitted into resonant modes of the waveguide. Depending on the geometry and mode of excitation, two fundamentally different signatures of the collective emission are observed, for which we present a unifying theoretical model. Our results form a new platform for waveguide quantum electrodynamics in the hard x-ray regime with the potential to provide a coherent narrowband source of x-rays on the nanometer scale.

quant-ph↗

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↗

arXiv2021

Disentangling X-ray dichroism and birefringence via high-purity polarimetry

High-brilliance synchrotron radiation sources have opened new avenues for X-ray polarization analysis that go far beyond conventional polarimetry in the optical domain. With linear X-ray polarizers in a crossed setting polarization extinction ratios down to 10$^{-10}$ can be achieved. This renders the method sensitive to probe tiniest optical anisotropies that would occur, for example, in strong-field QED due to vacuum birefringence and dichroism. Here we show that high-purity polarimetry can be employed to reveal electronic anisotropies in condensed matter systems with utmost sensitivity and spectral resolution. Taking CuO and La$_2$CuO$_4$ as benchmark systems, we present a full characterization of the polarization changes across the Cu K-absorption edge and their separation into dichroic and birefringent contributions. At diffraction-limited synchrotron radiation sources and X-ray lasers, where polarization extinction ratios of 10$^{-12}$ can be achieved, our method has the potential to assess birefringence and dichroism of the quantum vacuum in extreme electromagnetic fields.

physics.ins-det↗

arXiv2020

Revealing charge anisotropies in metal compounds via high-purity x-ray polarimetry

Linear polarization analysis of hard x-rays is employed to probe electronic anisotropies in metal-containing complexes with very high selectivity. We use the pronounced linear dichroism of nuclear resonant x-ray scattering to determine electric field gradients in an iron(II) containing compound as they evolve during a temperature-dependent high-spin/low-spin phase transition. This method constitutes a novel approach to analyze changes in the electronic structure of metal-containing molecules as function of external parameters or stimuli. The polarization selectivity of the technique allows us to monitor defect concentrations of electronic valence states across phase transitions. This opens new avenues to trace electronic changes and their precursors that are connected to structural and electronic dynamics in the class of metal compounds ranging from simple molecular solids to biological molecules.

cond-mat.mtrl-sci↗

arXiv2019

Scientific Opportunities with an X-ray Free-Electron Laser Oscillator

An X-ray free-electron laser oscillator (XFELO) is a new type of hard X-ray source that would produce fully coherent pulses with meV bandwidth and stable intensity. The XFELO complements existing sources based on self-amplified spontaneous emission (SASE) from high-gain X-ray free-electron lasers (XFEL) that produce ultra-short pulses with broad-band chaotic spectra. This report is based on discussions of scientific opportunities enabled by an XFELO during a workshop held at SLAC on June 29 - July 1, 2016

physics.ins-det↗

arXiv2018

Nuclear resonant scattering from 193Ir as a probe of the electronic and magnetic properties of iridates

The high brilliance of the modern synchrotron radiation sources facilitates experiments with high energy x-rays. In this Letter we report on Nuclear Resonance Scattering at the 73 keV nuclear level in 193Ir. The transitions between the hyperfine split levels show an exceptionally large E2/M1 multi-polarity mixing ratio combined with an increased sensitivity to certain changes in the hyperfine field direction compared to non-mixing transitions. The method opens a new way for probing local magnetic and electronic properties of correlated materials containing iridium and provides novel insights into their anisotropic magnetism. In particular, unexpected out-of-plane components of magnetic hyperfine fields and non-zero electric field gradients in Sr2IrO4 have been detected and attributed to the presence of strong spin-orbit interaction. Due to the high, 62% natural abundance of the 193Ir isotope, no isotopic enrichment of the samples is required, qualifying the method for a broad range of applications.

cond-mat.str-el↗

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

Incoherent Diffractive Imaging via Intensity Correlations of hard X-rays

Established x-ray diffraction methods allow for high-resolution structure determination of crystals, crystallized protein structures or even single molecules. While these techniques rely on coherent scattering, incoherent processes like Compton scattering or fluorescence emission -- often the predominant scattering mechanisms -- are generally considered detrimental for imaging applications. Here we show that intensity correlations of incoherently scattered x-ray radiation can be used to image the full 3D structure of the scattering atoms with significantly higher resolution compared to conventional coherent diffraction imaging and crystallography, including additional three-dimensional information in Fourier space for a single sample orientation. We present a number of properties of incoherent diffractive imaging that are conceptually superior to those of coherent methods.

physics.optics↗