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Stephan Fritzsche

Publications and source records attributed to Stephan Fritzsche.

At least 19 recordsLinked to original sources

Bound-state Compton scattering of linearly polarized photons

We present a theoretical study of Compton scattering of X- and $\gamma$-rays by a $K$-shell electron. Special attention is paid to the double-differential cross section and polarization of the scattered photons for linearly polarized incident photons. To investigate these observables, we employ the scattering matrix (S-matrix) approach based on relativistic Green's functions. The S-matrix results are moreover compared with predictions of the free-electron and impulse approximations, allowing us to assess the role of electron binding effects. Detailed calculations are carried out for hydrogen-like Ne$^{9+}$ and Pb$^{81+}$ targets over a wide range of incident photon energies and scattering angles. The calculations reveal kinematic regimes in which the impulse approximation agrees reasonably well with the S-matrix results. We also explore the polarization of scattered photons for slightly depolarized incident radiation, including the highly sensitive case of scattering at $90^\circ$.

physics.atom-ph

Discrete Cavity Dynamics in Free-Space Brillouin Laser

Highly coherent lasers are central to modern photonics. To date, high-coherence operation has been achieved predominantly in microcavity and fiber-based platforms. More recently, free-space Brillouin-laser experiments have revealed unusually strong noise suppression whose physical origin cannot be explained by conventional continuous-medium models developed for those platforms. In conventional continuous-medium models, the optical and acoustic fields are assumed to remain continuously coupled throughout the cavity evolution, whereas in free-space implementations the coupling is confined to the nonlinear medium and interrupted by passive propagation over the rest of the round trip. To describe this interaction-propagation separation, we develop a discrete-cavity model in which the short Brillouin interaction inside the gain medium and the subsequent free-space propagation are treated as two separate stages of the round-trip evolution. This separation introduces a temporal asymmetry between optical storage and acoustic relaxation, which effectively enhances acoustic damping at the cavity level and strongly reduces pump-noise transfer to the Stokes field. If the cavity round-trip time is much longer than the interaction time in the nonlinear medium, the noise-suppression ratio scales with the ratio of the total cavity length to the nonlinear-medium length. Our discrete-cavity model further provides quantitative predictions for the lasing threshold, output power, phase-noise transfer, and fundamental linewidth, in good agreement with experiment. These results identify the discrete interaction-propagation structure as the physical origin of the unusually strong noise suppression in free-space Brillouin lasers systems.

physics.optics

Large differential attosecond delays in solid state photoemission

Time-resolved photoelectron spectroscopy provides access to the electronic structure and non-equilibrium electron dynamics in matter. At solid surfaces photoemission dynamics can be investigated on its natural time scale by measuring attosecond time delays of emitted electrons. Photoelectrons with final state energies of several tens of eV need tens to hundreds of attoseconds to be released into the vacuum. Competing effects determine the emission dynamics and, hence, the full picture of the process is still under debate. The rather large energy differences between the final states probed in commonly reported relative photoemission delays obscure their complex fine structure and hinders the interpretation of the measurements. Here we report differential attosecond delays $\tau_{\mathrm{DAD}}$, i.e., relative photoemission delays for energetically close-lying spin-orbit split states. Differential attosecond delays on the order of 30 to 100 as for Bi 5d, Te 4d, and Se 3d core level photoemission from Bi$_2$Te$_3$ and Bi$_2$Se$_3$ can neither be attributed to intra-atomic delays, nor to ballistic transport and subsequent emission. Instead, calculations based on the one-step photoemission theory reveal that photoemission delays vary strongly on the energy scale of the spin-orbit splitting and quantitatively match experimental observations. This strong variation arises from multiple scattering at the surface leading to final states that involve both evanescent and propagating Bloch waves. Their relative amplitudes vary strongly affecting thereby the timing of the photoemission event since evanescent and propagating components exhibit inherently different dynamics.

physics.optics

Asynchronous Multi-photon Interference for Quantum Networks

Advanced quantum communication protocols require high-visibility quantum interference between photons generated at distant nodes, which places stringent demands on optical synchronization. Conventionally, synchronization of optical wave packets relies on pulsed sources and precise optical path stabilization. An alternative approach employs continuous-wave (CW) photon-pair sources, where temporal indistinguishability is enforced by post-selecting detection events within a coincidence window $\tau_w$ shorter than the photon coherence time $T_c$. Despite its conceptual simplicity, the quantitative relation between relevant time scales, achievable interference visibility, and usable multi-photon rates has remained unclear. Here, we develop in detail and experimentally validate a theoretical framework that quantitatively describes time-resolved multi-photon interference in the CW regime. We explicitly incorporate detector timing jitter, photon coherence time, and temporal post-selection. The model is verified using four-photon Hong-Ou-Mandel interference measurements. Based on this validated framework, we determine the coincidence window that maximizes usable four-photon rates for a target visibility. Finally, we compare CW and pulsed SPDC sources under equivalent indistinguishability constraints and show that CW operation can achieve comparable rates while relaxing optical synchronization requirements.

quant-ph

Twisting harmonics: Transfer of orbital angular momentum in solid-state high-harmonic generation

Although solid-state platforms underpin modern electronics, little is known about how intense ultrashort light pulses carrying orbital angular momentum (OAM) interact with solids. This gap persists even though, for more conventional light-matter interactions, the complex underlying electron dynamics can often be confined to a single Brillouin zone and described well within the dipole approximation. Previous studies were restricted to nonlinear, perturbative regimes, largely because the generation of intense ultrashort vortex pulses, particularly in the mid-infrared spectral regime, has remained a long-standing challenge. Consequently, the role of structured light in driving nonlinear, non-perturbative processes in solids, and the associated transfer of angular momentum during these interactions, has not been systematically explored. Here, we investigate solid-state high-harmonic generation (HHG) driven by intense ultrashort structured light using a versatile experimental approach applicable to different materials and geometries. We demonstrate that the OAM of the driving field is coherently transferred to the emitted harmonics. In particular, we show that the OAM is conserved independently of the crystal symmetry, the range of electronic interactions, and the presence of strong spin-orbit coupling. These results establish OAM-resolved HHG as a robust framework for characterizing and controlling angular momentum transfer in solid-state HHG and open new avenues for structured-light-driven quantum technologies and topological materials investigations.

physics.optics

Engineering of maximally entangled orbital angular momentum states via path identity

Cutting-edge quantum technologies lean on sources of high-dimensional entangled states (HDES) that reliably prepare high-fidelity target states. The idea to overlap photon paths from distinct but indistinguishable sources was recently introduced for the creation of HDES, known as entanglement by path identity. In this regard, the use of orbital angular momentum (OAM) modes is promising, as they offer a high-dimensional and discrete Hilbert space to encode information. While entanglement by path identity with OAM has been verified experimentally, a detailed investigation of how the OAM distribution of photon pairs can be engineered to maximize the entanglement is lacking. We address this gap and identify an optimal dimensionality for maximally entangled states (MESs) when the spatial engineering of the pump beam and the path identity approach are combined. Our theoretical study reveals notable limitations for the fidelity of high-dimensional target states. We also establish the equivalence of entangled biphoton states pumped by a spatially engineered beam and generated via path identity. These findings constitute a valuable step toward the optimized preparation of MESs in high dimensions.ngineered beam. These findings constitute a valuable step toward the optimized preparation of MESs in high dimensions.

quant-ph

$\textit{Ab initio}$ multiconfigurational calculations of experimentally significant energy levels and transition rates in Lr I $\left( Z=103 \right)$

Large-scale multiconfigurational calculations are conducted on experimentally significant transitions in Lr I and its lanthanide homologue Lu I, exhibiting good agreement with recent theoretical and experimental results. A single reference calculation is performed, allowing for substitutions from the core within a sufficiently large active set to effectively capture the influence of the core on the valence shells, improving upon previous multiconfigurational calculations. An additional calculation utilising a multireference set is performed to account for static correlation effects which contribute to the wavefunction. Reported energies for the two selected transitions are 20716$\pm$550 $\text{cm}^{-1}$ and 28587$\pm$650 $\text{cm}^{-1}$ for $7\!s^2 8s~^{2} \! {S}_{1\!/\!2}$ $\rightarrow$ $7\!s^2 7\!p ~^{2} \! {P}^{o}_{1\!/\!2 }$ and $7\!s^2 7\!d ~^{2} \! {D}_{3\!/\!2 }$ $\rightarrow$ $7\!s^2 7\!p ~^{2} \! {P}^{o}_{1\!/\!2 }$, respectively.

physics.atom-ph

Comparison between Jacobi-Anger and saddle point methods to treat Above-threshold ionization

We present a detailed comparison of theoretical approaches for modeling strong-field ionization by few-cycle laser pulses. The dipole approximation is shown to accurately capture interference structures in photoelectron spectra, while non-dipole effects introduce significant momentum shifts along the propagation direction. Two complementary analytical methods are used: the Jacobi-Anger expansion provides complete spectral decomposition of transition amplitudes, whereas the saddle-point method efficiently identifies dominant ionization pathways. Through this comparative study within the strong-field approximation framework, we establish validity conditions and practical advantages for each approach. Our results provide guidelines for selecting theoretical methods for advancing the interpretation of strong-field processes. These findings provide a roadmap for interpreting strong-field ionization spectra and momentum distributions, highlighting where non-dipole effects and method choice critically alter predictions.

physics.atom-ph

Coincidence measurement of two-photon double ionization of argon through an autoionizing resonance

We present coincidence measurements of two-photon double-ionization (TPDI) of argon driven by femtosecond pulses tunable around 26.5 eV photon energy, which are obtained from a high-harmonic generation source. The measured photoelectron spectra are interpreted with regard to three TPDI mechanisms. Theoretical predictions are obtained by an approximate model for direct TPDI and atomic structure calculations, which are implemented into a Monte Carlo simulation. The prevailing mechanism involves the excitation and prompt photoionization of an autoionizing resonance in neutral argon. We provide evidence for pronounced electron-electron interaction in this ultrafast ionization process. Furthermore, we show that the dominant TPDI mechanism can be altered by slight tuning of the photon energy. The present work paves the way for scrutinizing and controlling non-linear photoionization in the extreme ultraviolet using table-top sources.

physics.atom-ph

Chemical Evolution of R-process Elements in Stars (CERES): IV. An observational run-up of the third r-process peak with Hf, Os, Ir, and Pt

The third r-process peak (Os, Ir, Pt) is poorly understood due to observational challenges, with spectral lines located in the blue or near-ultraviolet region of stellar spectra. These challenges need to be overcome for a better understanding of the r-process in a broader context. To understand how the abundances of the third r-process peak are synthesised and evolve in the Universe, a homogeneous chemical analysis of metal-poor stars using high quality data observed in the blue region of the electromagnetic spectrum (< 400 nm) is necessary. We provide a homogeneous set of abundances for the third r-process peak (Os, Ir, Pt) and Hf, increasing by up to one order of magnitude their availability in the literature. A classical 1D, local thermodynamic equilibrium (LTE) analysis of four elements (Hf, Os, Ir, Pt) is performed, using ATLAS model atmospheres to fit synthetic spectra in high resolution (> 40,000), high signal-to-noise ratio, of 52 red giants observed with UVES/VLT. Due to the heavy line blending involved, a careful determination of upper limits and uncertainties is done. The observational results are compared with state-of-the-art nucleosynthesis models. Our sample displays larger abundances of Ir (Z=77) in comparison to Os (Z=76), which have been measured in a few stars in the past. The results also suggest decoupling between abundances of third r-process peak elements with respect to Eu (rare earth element) in Eu-poor stars. This seems to contradict a co-production scenario of Eu and the third r-process peak elements Os, Ir, and Pt in the progenitors of these objects. Our results are challenging to explain from the nucleosynthetic point of view: the observationally derived abundances indicate the need for an additional early, primary formation channel (or a non-robust r-process).

astro-ph.SR

Quadratic Zeeman and Electric Quadrupole Shifts in Highly Charged Ions

Recent advances in high-precision spectroscopy of highly charged ions necessitate an understanding of energy shifts of ionic levels caused by external electric and magnetic fields. Beyond the well-known Stark and linear Zeeman shifts, trapped ions may also exhibit quadratic Zeeman and electric quadrupole shifts. In this contribution, we present a systematic approach for the theoretical analysis of these shifts for arbitrary many-electron ions. Based on the derived expressions and making use of the multiconfigurational Dirac-Fock approach, we performed calculations of quadratic Zeeman shift coefficients and quadrupole moments for various ionic states in Ca$^{14+}$, Ni$^{12+}$ and Xe$^{q+}$ ions. These ions attract particular interest for ongoing and future experiments in optical clocks and tests of fundamental physics.

physics.atom-ph

Hanle effect for lifetime determinations in the soft X-ray regime

By exciting a series of $1\mathrm{s}^{2}\, ^{1}\mathrm{S}_{0} \to 1\mathrm{s}n\mathrm{p}\, ^{1}\mathrm{P}_{1}$ transitions in helium-like nitrogen ions with linearly polarized monochromatic soft X-rays at the Elettra facility, we found a change in the angular distribution of the fluorescence sensitive to the principal quantum number $n$. In particular it is observed that the ratio of emission in directions parallel and perpendicular to the polarization of incident radiation increases with higher $n$. We find this $n$-dependence to be a manifestation of the Hanle effect, which served as a practical tool for lifetime determinations of optical transitions since its discovery in 1924. In contrast to traditional Hanle effect experiments, in which one varies the magnetic field and considers a particular excited state, we demonstrate a 'soft X-ray Hanle effect' which arises in a static magnetic field but for a series of excited states. By comparing experimental data with theoretical predictions, we were able to determine lifetimes ranging from hundreds of femtoseconds to tens of picoseconds of the $1\mathrm{s}n\mathrm{p}\, ^{1}\mathrm{P}_{1}$ levels, which find excellent agreement with atomic-structure calculations. We argue that dedicated soft X-ray measurements could yield lifetime data that is beyond current experimental reach and cannot yet be predicted with sufficient accuracy.

physics.atom-ph

Interaction of vector light beams with atoms exposed to a time-dependent magnetic field

During recent years interest has been rising for applications of vector light beams towards magnetic field sensing. In particular, a series of experiments were performed to extract information about properties of static magnetic fields from absorption profiles of light passing through an atomic gas target. In the present work, we propose an extension to this method for oscillating magnetic fields. To investigate this scenario, we carried out theoretical analysis based on the time-dependent density matrix theory. We found that absorption profiles, even when averaged over typical observation times, are indeed sensitive to both strength and frequency of the time-dependent field, thus opening the prospect for a powerful diagnostic technique. To illustrate this sensitivity, we performed detailed calculations for the $5s \;\, {}^2S_{1/2}$ ($F=1$) $-$ $5p \;\, {}^2 P_{3/2}$ ($F=0$) transition in rubidium atoms, subject to a superposition of an oscillating (test) and a static (reference) magnetic field.

physics.atom-ph

High-dimensional maximally entangled photon pairs in parametric down-conversion

Photon pairs generated from spontaneous parametric down-conversion are a well-established method to realize entangled bipartite photonic systems. Laguerre-Gaussian modes, which carry orbital angular momentum (OAM), are commonly exploited to engineer high-dimensional entangled quantum states. %experimentally. For Hilbert spaces with dimension d>2, maximally entangled states (MESs) help to improve the capacity and security of quantum communication protocols, among several other promising features. However, the direct generation of MES in well-defined high-dimensional subspaces of the infinite OAM basis has remained a challenge. Here, we formalize how the spatial distribution of the pump beam and the nonlinear profile of the crystal can be simultaneously utilized to generate MES without additional spatial filtering of OAM modes within a subspace. We illustrate our approach with maximally entangled qutrits (d=3) and ququints (d=5).

quant-ph

Laser Resonance Chromatography of $^{229}$Th$^{3+}$ in He: an ab initio investigation

We propose a laser resonance chromatography (LRC) experiment on $^{229}$Th$^{3+}$, with the goal of detecting the ion's electronic ground $5f$ $^2$F$_{5/2}$ state and metastable $7s$ $^2$S$_{1/2}$ state by means of their ion mobilities. To this end, we first model the ion-neutral interaction potentials for the two electronic states with a relativistic Fock space coupled cluster method and complete basis-set extrapolation scheme. The interaction potentials are used to simulate the state-specific reduced ion mobilities in terms of the operating temperature and the external electric field. The ion mobilities differ by more than 7% at 300 K and moderate field strengths; thus, separation of the $^{229}$Th$^{3+}$ metastable state lies within the reach of LRC experiments targeting optical probing and monitoring of the nuclear clock transition in this isotope.

physics.atom-ph

Coulomb excitation of hydrogen atoms by vortex ion beams

Coulomb excitation of hydrogen atoms by vortex protons is theoretically investigated within the framework of the non--relativistic first--Born approximation and the density matrix approach. Special attention is paid to the magnetic sublevel population of excited atoms and, consequently, to the angular distribution of the fluorescence radiation. We argue that both these properties are sensitive to the projection of the orbital angular momentum (OAM), carried by the projectile ions. In order to illustrate the OAM--effect, detailed calculations have been performed for the $1s \to 2p$ excitation and the subsequent $2p \to 1s$ radiative decay of a hydrogen target, interacting with incident Laguerre--Gaussian vortex protons. The calculation results suggest that Coulomb excitation can be employed for the diagnostics of vortex ion beam at accelerator and storage ring facilities.

physics.atom-ph

Exploring Valence Electron Dynamics of Xenon through Laser-Induced Electron Diffraction

Strong-field ionization can induce electron motion in both the continuum and the valence shell of the parent ion. Here, we explore their interplay by studying laser-induced electron diffraction (LIED) patterns arising from interaction with the potentials of two-hole states of the xenon cation. The quantitative rescattering theory is used to calculate the corresponding photoelectron momentum distributions, providing evidence that the spin-orbit dynamics could be detected by LIED. We identify the contribution of these time-evolving hole states to the angular distribution of the rescattered electrons, particularly noting a distinct change along the backward scattering angles. We benchmark numerical results with experiments using ultrabroad and femtosecond laser pulses centered at \SI{3100}{nm}.

physics.atom-ph

Transport property predictions for laser resonance chromatography on Rf$^+$ (Z = 104)

We propose a theoretically designed laser resonance chromatography (LRC) experiment on Rf$^+$ (Z = 104) drifting in He buffer gas. To this end, we first developed a four-level rate equation model that simulates the optical pumping of Rf$^+$ from its ground state, $^2$D$_{3/2}$ (7s$^2$6d$^1$), to the metastable $^4$F$_{3/2}$ (7s$^1$6d$^2$) state via laser resonant excitation of the intermediate $^4$F$_{3/2}$ (7s$^1$6d$^1$7p$^1$) state prior to electronic state chromatography. This model predicts a 93% pumping efficiency that suffices to enable efficient laser resonance chromatography of this ion. We then performed accurate relativistic Multi-Reference Configuration-Interaction (MRCI) calculations to model the interaction of Rf$^+$ with He in the ground $^2$D$_{3/2}$ (7s$^2$6d$^1$), low-lying $^2$D$_{5/2}$ (7s$^2$6d$^1$), and metastable $^4$F$_{3/2}$ (7s$^1$6d$^2$) states. These ion-atom interaction potentials were used to calculate the state-specific ion mobilities. For gas temperatures above 100 K and small applied electric fields, the reduced ion mobilities of the ground and metastable states differ significantly. In particular, at room temperature the difference between the reduced ion mobilities of these states is larger than 11%, and as such sufficiently large to ensure LRC of this ion.

physics.atom-ph