arXiv subjects

Maurits W. Haverkort

Publications and source records attributed to Maurits W. Haverkort.

At least 19 recordsLinked to original sources

arXiv2026

Symmetric estimator for discrete self-energy of discrete many-body systems

We derive a discrete spectral representation of the single-particle self-energy using a discrete evaluation of Kugler's symmetric improved estimator. Our construction can be used on both the real and the complex (Matsubara) frequency axis. It is guaranteed to remain causal at the numerical level, in contrast to standard approaches that may generate unphysical negative spectral weight or require additional broadening. Our representation can be used for any Hamiltonian; here we apply it to quantum impurity models and in dynamical mean-field theory. The latter is formulated with a discrete hybridization function throughout its self-consistency loop. In both cases and across various numerical methods, we obtain significantly improved accuracy for a range of impurity properties.

cond-mat.str-el↗

arXiv2026

Critical behavior and evidence of dimensional crossover in quasi-two-dimensional Li$_2$FeSiO$_4$

We report thermal expansion and heat capacity studies on Li$_2$FeSiO$_4$ single crystals which enable us to investigate the critical behavior in the magnetically quasi-two-dimensional (2D) material. Pronounced $λ$-shaped anomalies at the magnetic ordering temperature $T_{\rm N}$ imply significant magneto-elastic coupling. Our analysis of both the thermal expansion and the specific heat data implies the crossover from 2D Ising-like behavior for $|(T-T_{\rm N})/T_{\rm N}|>0.3$ to 3D Ising behavior \rev{below $\simeq 1.3\times T_{\rm N}$. The 2D-like behavior is further supported by density functional calculations which show minimal dispersion perpendicular to the crystallographic $ac$ planes of the layered structure, thereby indicating the 2D nature of magnetism at higher temperatures.} Our results extend the available model materials of quasi-2D magnetism to a high-spin $S=2$ system with tetrahedrally coordinated Fe$^{2+}$-ions, thereby illustrating how magnetic order evolves in a 2D Ising-like system with orbital degrees of freedom.

cond-mat.str-el↗

arXiv2025

High-resolution valence band RIXS at the actinide M$_{4,5}$-edges

Understanding the electronic structure of actinide materials is crucial for both fundamental research and nuclear applications. The partially filled 5f shells exhibit complex behavior due to strong correlations and ligand hybridization, requiring advanced spectroscopic techniques. Here, we report on the development and application of high-resolution valence-band resonant inelastic x-ray spectroscopy (VB-RIXS) experiments at the uranium M$_{4,5}$ edges (3551 and 3725\,eV). We present data of UO$_2$, a well-established model actinide compound. VB-RIXS is particularly well suited for probing the 5f-shell electronic structure, as it probes, in contrast to core-to-core RIXS, excitations without leaving a high-energy core hole in the final state. In VB-RIXS, we achieve energy resolutions of 50\,meV (M$_5$) and 90\,meV (M$_4$), enabling the resolution of multiplet excitations and crystal-field effects, as well as charge-transfer and fluorescence-like features with unprecedented clarity. As such, high resolution VB-RIXS offers direct insights into both low-energy, near ground-state properties and high-energy hybridization and covalency effects. Our results demonstrate the power of VB-RIXS as a versatile and powerful tool for probing the strongly correlated electronic structure of actinide materials, providing essential input for quantitative modeling and the validation of theoretical concepts.

cond-mat.str-el↗

arXiv2025

Polarization dependency in Resonant Inelastic X-Ray Scattering

Resonant Inelastic X-Ray Scattering (RIXS) is a well-established tool for probing excitations in a wide range of materials. The measured spectra strongly depend on the scattering geometry, via its influence on the polarization of the incoming and outgoing light. By employing a tensor representation of the 4-point response function that governs the RIXS intensity, we disentangle the experimental geometry from the intrinsic material properties. In dipole-dipole RIXS processes and low-symmetry crystals, up to 81 linearly independent fundamental spectra can be measured as a function of light polarization. However, for crystals or molecules with symmetry, the number of independent fundamental spectra that define the RIXS tensor is significantly reduced. This work presents a systematic framework for determining the number of fundamental spectra and expressing the RIXS tensor in terms of these fundamental components. Given a specific experimental geometry, the measured spectrum can be represented as a linear combination of these fundamental spectra. To validate our approach, we performed calculations for different point group symmetries, both with and without an applied magnetic field. Within the same framework, we derived expressions for powder spectra in momentum-independent processes and spectra obtained using Bragg spectrometers. This formalism provides a valuable toolkit for optimizing experiment planning, data interpretation, and RIXS simulation.

cond-mat.str-el↗

arXiv2025

Improved limit on the effective electron neutrino mass with the ECHo-1k experiment

The effective electron neutrino mass can be determined by analyzing the endpoint region of the $^{163}$Ho electron capture spectrum, provided a measurement with high energy resolution and high statistics using calorimetric techniques. Here, the Electron Capture in $^{163}$Ho collaboration, ECHo, presents an analysis of the most precise $^{163}$Ho spectrum currently available, obtained with the ECHo-1k experiment and comprising about 200 million events. A very low background rate of $B=9.1(1.3)\times 10^{-6}$ /eV/pixel/day was achieved allowing for a reliable analysis of the endpoint region. The derived endpoint energy $Q = 2862(4)$ eV is in excellent agreement with the one independently determined via Penning-trap mass spectrometry of $Q=2863.2(6)$ eV [1]. The upper limit of the effective electron neutrino mass is improved by almost a factor 2 compared to the lowest current value [2], reaching $m_{ν_\mathrm{e}} < 15 $ eV/c${^2}$ (90\% credible interval).

hep-ex↗

arXiv2025

Influence of Interlayer Stacking on Optical Behavior in WSe$_{2}$/MoS$_{2}$ van der Waals Heterostructures

We investigate the impact of crystal alignment on excitonic behavior in WSe$_{2}$/MoS$_{2}$ van der Waals heterostructures by comparing eclipsed (AA) and staggered (AB) stacking configurations. Our first-principles and symmetry-based analysis reveal that interlayer stacking symmetry plays a central role in determining the nature of electron-hole pairs. We uncover a rich variety of excitonic states, including spatially confined two-dimensional (2D) excitons, delocalized three-dimensional (3D) excitons, and charge-transfer (CT) excitons with interlayer character. The dimensionality and optical activity of these excitons are governed by the interplay among orbital character, interlayer hybridization, and symmetry-imposed selection rules. Our findings establish general principles for engineering excitonic properties in van der Waals heterostructures through controlled layer orientation and stacking order.

cond-mat.str-el↗

arXiv2025

Crystal field excitations in rattling clathrate CeBa$_7$Au$_6$Si$_{40}$

We investigate the local crystal-field environment of cerium in the clathrate compound CeBa$_7$Au$_6$Si$_{40}$ (Ce-BAS) using resonant inelastic x-ray scattering (RIXS) and magnetic susceptibility measurements. Ce-BAS is a rare example of a system where heavy-fermion physics coexists with low-energy rattling phonon modes, making it a candidate for enhanced thermoelectric performance. Magnetic susceptibility measurements reveal a temperature-dependent local moment that cannot be explained within a static crystal-field model. A fit to the susceptibility data requires strong mixing between the j = 5/2 and j = 7/2 crystal-field states, which implies large internal splittings inconsistent with RIXS spectra. In contrast, RIXS data are well described by a model with negligible j = 5/2 - j = 7/2 mixing and an energy separation of 12 meV between the ground and first excited crystal-field states. The inability to reconcile these two datasets within a static framework points to a dynamical modification of the crystal-field potential. We attribute this to coupling between the Ce 4f electrons and low-energy phonons associated with the Ce rattling motion. This interpretation is consistent with theoretical predictions of phonon-enhanced Kondo effects and dynamical Jahn-Teller distortions. Our results highlight the need for multi-orbital impurity models that include phonon coupling to fully describe the low-energy physics of Ce-BAS.

cond-mat.str-el↗

arXiv2025

Photo-generated charge-transfer excitons in NiO revealed by ultrafast time-resolved resonant inelastic x-ray scattering

Strong electronic correlation can lead to insulating behavior and to the opening of large optical gaps, even in materials with partly filled valence shells. Although the non-equilibrium optical response encodes both local (quasi atomic) and collective (long range) responses, optical spectroscopy is usually more sensitive to the latter. Resonant x-ray techniques are better suited to investigate the quasi-atomic properties of correlated solids. Using time-resolved resonant inelastic x-ray scattering (RIXS), here we study the ultrafast non-equilibrium processes in NiO following photo-excitation by ultraviolet photons with energy exceeding the optical gap. We observe the creation of charge-transfer excitons that decay with a time constant of about 2\,ps, while itinerant photo-doping persists for tens of picoseconds. Following our discovery, which establishes time-resolved high-resolution RIXS as a powerful tool for the study of transient phenomena in condensed matter, the possible presence of charge-transfer excitons will need to be considered when interpreting optical pump-probe experiments on correlated quantum materials.

cond-mat.str-el↗

arXiv2024

A method for the automatic generation of a minimal basis set of structural templates for material phase-space exploration

We present a novel method for predicting binary phase diagrams through the automatic construction of a minimal basis set of representative templates. The core assumption is that any materials space can be divided into a small number of regions with similar chemical tendencies and bonding properties, and that a minimal set of templates can efficiently represent the key chemical trends across the different regions. By combining data-driven techniques with ab-initio crystal structure prediction, we can efficiently partition the materials space and construct templates reflecting variations in chemical behavior. Preliminary results demonstrate that our method predicts binary convex hulls with accuracy comparable to resource-intensive EA searches, while achieving a significant reduction in computational time (by a factor of 25). The method can be extended to ternary and multinary systems, enabling efficient high-throughput exploration and mapping of complex material spaces. By providing a transformative solution for high-throughput materials discovery, our approach paves the way for uncovering advanced quantum materials and accelerating in silico design.

cond-mat.mtrl-sci↗

arXiv2024

Neural-network-supported basis optimizer for the configuration interaction problem in quantum many-body clusters: Feasibility study and numerical proof

A deep-learning approach to optimize the selection of Slater determinants in configuration interaction calculations for condensed-matter quantum many-body systems is developed. We exemplify our algorithm on the discrete version of the single-impurity Anderson model with up to 299 bath sites. Employing a neural network classifier and active learning, our algorithm enhances computational efficiency by iteratively identifying the most relevant Slater determinants for the ground-state wavefunction. We benchmark our results against established methods and investigate the efficiency of our approach as compared to other basis truncation schemes. Our algorithm demonstrates a substantial improvement in the efficiency of determinant selection, yielding a more compact and computationally manageable basis without compromising accuracy. Given the straightforward application of our neural network-supported selection scheme to other model Hamiltonians of quantum many-body clusters, our algorithm can significantly advance selective configuration interaction calculations in the context of correlated condensed matter.

cond-mat.str-el↗

arXiv2024

Penning-trap measurement of the $Q$-value of the electron capture in $^{163}\mathrm{Ho}$ for the determination of the electron neutrino mass

The investigation of the absolute scale of the effective neutrino mass remains challenging due to the exclusively weak interaction of neutrinos with all known particles in the standard model of particle physics. Currently, the most precise and least model-dependent upper limit on the electron antineutrino mass is set by the KATRIN experiment from the analysis of the tritium \b{eta}-decay. Another promising approach is the electron capture in $^{163}\mathrm{Ho}$, which is under investigation using microcalorimetry within the ECHo and HOLMES collab orations. An independently measured Q-value of this process is vital for the assessment of systematic uncertainties in the neutrino mass determination. Here, we report a direct, independent determination of this $Q$-value by measuring the free-space cyclotron frequency ratio of highly charged ions of $^{163}\mathrm{Ho}$ and $^{163}\mathrm{Dy}$ in the Penning trap experiment \textsc{Pentatrap}. Combining this ratio with atomic physics calculations of the electronic binding energies yields a $Q$-value of $2863.2(0.6)\,\mathrm{eV}/c^{2}$ - a more than 50-fold improvement over the state-of-the-art. This will enable the determination of the electron neutrino mass on a sub-eV level from the analysis of the electron capture in $^{163}\mathrm{Ho}$.

nucl-ex↗

arXiv2024

Stabilization of U 5$f^2$ configuration in UTe$_2$ through U 6d dimers in the presence of Te2 chains

We investigate the topological superconductor candidate UTe$_2$ using high-resolution valence-band resonant inelastic x-ray scattering at the U $M_{4,5}$-edges. We observe atomic-like low-energy excitations that support the correlated nature of this unconventional superconductor. These excitations originate from the U $5f^2$ configuration, which is unexpected since the short Te2-Te2 distances exclude Te2 being 2-. By utilizing the photoionization cross-section dependence of the photoemission spectra in combination with band structure calculations, we infer that the stabilization of the U $5f^2$ configuration is due to the U $6d$ bonding states in the U-dimers acting as a charge reservoir. Our results emphasize that the description of the physical properties should commence with a $5f^2$ $ansatz$.

cond-mat.str-el↗

arXiv2024

Spectroscopic evidence of Kondo-induced quasi-quartet in CeRh$_2$As$_2$

CeRh$_2$As$_2$ is a new multiphase superconductor with strong suggestions for an additional itinerant multipolar ordered phase. The modeling of the low temperature properties of this heavy fermion compound requires a quartet Ce$^{3+}$ crystal-field ground state. Here we provide the evidence for the formation of such a quartet state using x-ray spectroscopy. Core-level photoelectron and x-ray absorption spectroscopy confirm the presence of Kondo hybridization in CeRh$_2$As$_2$. The temperature dependence of the linear dichroism unambiguously reveils the impact of Kondo physics for coupling the Kramer's doublets into an effective quasi-quartet. Non-resonant inelastic x-ray scattering data find that the $|Γ_7^- \rangle$ state with its lobes along the 110 direction of the tetragonal structure ($xy$ orientation) contributes most to the multi-orbital ground state of CeRh$_2$As$_2$.

cond-mat.str-el↗

arXiv2023

Singlet magnetism in intermetallic UGa$_2$ unveiled by inelastic x-ray scattering

Using high resolution tender-x-ray resonant inelastic scattering and hard-x-ray non-resonant inelastic scattering beyond the dipole limit we were able to detect electronic excitations in intermetallic UGa$_2$ that are highly atomic in nature. Analysis of the spectral lineshape reveals that the local $5f^2$ configuration characterizes the correlated nature of this ferromagnet. The orientation and directional dependence of the spectra indicate that the ground state is made of the $Γ_1$ singlet and/or $Γ_6$ doublet symmetry. With the ordered moment in the $ab$ plane, we infer that the magnetism originates from the higher lying $Γ_6$ doublet being mixed with the $Γ_1$ singlet due to inter-site exchange, qualifying UGa$_2$ to be a true quantum magnet. The ability to observe atomic excitations is crucial to resolve the on-going debate about the degree of localization versus itineracy in U intermetallics.

cond-mat.str-el↗

arXiv2023

Non-Lorentzian atomic natural line-shape of core level multiplets: Access high energy x-ray photons in electron capture nuclear decay

We present a method to calculate the natural line width and energy dependent line shape due to fluorescence decay of core excited atoms within a full relativistic multi-reference configuration interaction theory. The atomic absorption lines show a deviation from a Lorentzian line-shape due to energy dependent matrix elements of the localized electronic state coupling to the photon field. This gives rise to spectral lines with small but visible asymmetry. One generally finds an excess of spectral weight at the high energy shoulder of the atomic absorption line. We present the example of nuclear decay of $^{55}$Fe by electron capture of an inner-shell core electron. We show that the amount of ionizing radiation in the energy window between 50 and 200 keV is around one order of magnitude larger due to the energy dependent fluorescence yield lifetime compared to the value one would obtain if one assumes a constant fluorescence decay rate. This yields a total change of energy deposited into ionizing radiation of about 1\textperthousand. Our calculations are in good agreement with previous calculations and experimental observations where data is available. Our results can be further validated by high precision measurements of electron capture nuclear decay spectra using recently developed experimental methods.

physics.atom-ph↗

arXiv2023

Orbital selective coupling in CeRh$_3$B$_2$: co-existence of high Curie and high Kondo temperature

We investigated the electronic structure of the enigmatic CeRh$_3$B$_2$ using resonant inelastic scattering and x-ray absorption spectroscopy in combination with $ab$ $initio$ density functional calculations. We find that the Rh 4$d$ states are irrelevant for the high-temperature ferromagnetism and the Kondo effect. We also find that the Ce 4$f$ crystal-field strength is too small to explain the strong reduction of the Ce magnetic moment. The data reveal instead the presence of two different active Ce 4$f$ orbitals, with each coupling selectively to different bands in CeRh$_3$B$_2$. The inter-site hybridization of the |J=5/2,Jz=+/-1/2> crystal-field state and Ce 5$d$ band combined with the intra-site Ce 4$f$-5$d$ exchange creates the strong ferromagnetism, while hybridization between the |J=5/2,Jz=+/-5/2> and the B $sp$ in the $ab$-plane contributes to the Kondo interaction which causes the moment reduction. This orbital selective coupling explains the unique and seemingly contradictory properties of CeRh$_3$B$_2$.

cond-mat.str-el↗

arXiv2023

Intermixing-driven surface and bulk ferromagnetism in the quantum anomalous Hall candidate MnBi$_6$Te$_{10}$

The recent realizations of the quantum anomalous Hall effect (QAHE) in MnBi$_2$Te$_4$ and MnBi$_4$Te$_7$ benchmark the (MnBi$_2$Te$_4$)(Bi$_2$Te$_3$)$_n$ family as a promising hotbed for further QAHE improvements. The family owes its potential to its ferromagnetically (FM) ordered MnBi$_2$Te$_4$ septuple layers (SL). However, the QAHE realization is complicated in MnBi$_2$Te$_4$ and MnBi$_4$Te$_7$ due to the substantial antiferromagnetic (AFM) coupling between the SL. An FM state, advantageous for the QAHE, can be stabilized by interlacing the SL with an increasing number $n$ of Bi$_2$Te$_3$ layers. However, the mechanisms driving the FM state and the number of necessary QLs are not understood, and the surface magnetism remains obscure. Here, we demonstrate robust FM properties in MnBi$_6$Te$_{10}$ ($n = 2$) with $T_C \approx 12$ K and establish their origin in the Mn/Bi intermixing phenomenon by a combined experimental and theoretical study. Our measurements reveal a magnetically intact surface with a large magnetic moment, and with FM properties similar to the bulk. Our investigation thus consolidates the MnBi$_6$Te$_{10}$ system as perspective for the QAHE at elevated temperatures.

cond-mat.mtrl-sci↗

arXiv2022

Novel magnetic excitations beyond the single- and double-magnons

Conventional wisdom suggests that one photon that carries one unit of angular momentum can change the spin angular momentum of a magnetic system with one unit (delta Ms = +-1) at most. This would imply that a two-photon scattering process can manipulate the spin angular momentum of the magnetic system with a maximum of two units. Here we examine the fundamental limit of the photon-driven transport of angular momentum by studying the magnon spectrum of α-Fe2O3 using resonant inelastic x-ray scattering. We discovered a cascade of higher-rank magnons carrying double, triple, quadruple, and quintuple the spin angular momentum of a single-magnon. Guided by theoretical calculations, we reveal how a two-photons scattering process can create exotic higher-rank magnons and the relevance of these quasiparticles for magnon-based applications.

cond-mat.str-el↗