arXiv subjects

Leonie Spitz

Publications and source records attributed to Leonie Spitz.

10 recordsLinked to original sources

arXiv2026

Probing the real-space density of spin-entangled electrons

On the textbook example of an isolated antiferromagnetic Heisenberg dimer, we demonstrate that the magnetic form factor and the magnetic electron density distribution can be extracted from the momentum-dependence of the inelastic neutron scattering (INS) intensity of a magnetic excitation. We measure the three-dimensional (3D) magnetic structure factor of the singlet-to-triplet excitation in Cu(II) acetate monohydrate with INS. Using a minimal parametrization of the magnetic electron density, we deduce the real-space density of the spin-entangled electrons and the transfer of magnetic electron density between metal and ligand atoms from the experimental data. Density functional theory (DFT) calculations reproduce the measured structure factor quantitatively, providing a direct validation of DFT broken-symmetry spin densities against full 3D INS data. The quantitative agreement between experiment, parametrization, and theory establishes a robust framework for determining magnetic form factors and the magnetic electron density in a broad range of magnetic materials and demonstrates INS as a probe of the envelope of spatial electronic wavefunctions.

cond-mat.str-el↗

arXiv2026

All-optical control of second-harmonic generation in $\beta$-BaB$_2$O$_4$ via coherent, terahertz-driven acentric lattice displacement

Dynamical control of the nonlinear optical properties of solids -- with light itself -- will be essential for future ultrafast photonic technologies. Previously, methods to modulate nonlinear processes including second-harmonic generation (SHG) have relied primarily on non-resonant light-matter interaction or photo-generation of hot electrons in nanoscale materials. However, these approaches are typically constrained by limited interaction lengths and the initial frequency conversion is relatively weak under equilibrium conditions. Here, an approximately 30\% modulation of efficient phase-matched SHG in bulk beta-barium borate (beta-BaB2O4) is achieved through transient lattice deformation by intense terahertz (THz) pulses that are tuned to resonance with an infrared-active phonon mode. The effect originates from modification of the index of refraction ellipsiod and the corresponding nonlinear phase-matching conditions, rather than from direct modulation of the nonlinear susceptibility through THz-mediated chi^(3) processes. This mechanism, of resonant selective lattice excitation, points toward novel THz-control schemes to tune the nonlinear optical response in materials.

physics.optics↗

arXiv2025

Terahertz light driven coherent excitation of a zone-folded Raman-active phonon mode in the Spin-Ladder System $\alpha'$-NaV$_2$O$_5$

We investigate the out-of-equilibrium lattice dynamics in the spin-ladder system $\alpha'$-NaV$_2$O$_5$ using intense terahertz (THz) pump and near-infrared (NIR) probe spectroscopy. When quasi-single-cycle THz pulses interact with $\alpha'$-NaV$_2$O$_5$ in its low-temperature, dimerized charge-ordered phase, they induce coherent oscillations in the time domain at the zone-folded Raman-active phonon frequency of 1.85 THz. By combining pump-probe measurements with lattice dynamics modeling based on equation-of-motion approach, we propose that these oscillations arise from a nonlinear coupling between Raman-active and infrared (IR)-active phonon modes, with the latter being resonantly excited by the THz pulses. In contrast, excitation with NIR femtosecond laser pulses does not produce measurable vibrational dynamics, highlighting the unique potential of THz-driven, nonlinear light-matter interactions for the coherent and selective control of structural dynamics in quantum materials.

cond-mat.mtrl-sci↗

arXiv2025

Entropy-assisted, long-period stacking of honeycomb layers in an AlB2-type silicide

Configurational entropy can impact crystallization processes, tipping the scales between structures of nearly equal internal energy. Using alloyed single crystals of Gd2PdSi3 in the AlB2-type structure, we explore the formation of complex layer sequences made from alternating, two-dimensional triangular and honeycomb slabs. A four-period and an eight-period stacking sequence are found to be very close in internal energy, the latter being favored by entropy associated with covering the full configuration space of interlayer bonds. Possible consequences of polytype formation on magnetism in Gd2PdSi3 are discussed.

cond-mat.mtrl-sci↗

arXiv2024

Lattice-commensurate skyrmion texture in a centrosymmetric breathing kagome magnet

Skyrmion lattices (SkL) in centrosymmetric materials typically have a magnetic period on the nanometer-scale, so that the coupling between magnetic superstructures and the underlying crystal lattice cannot be neglected. Here, we reveal the commensurate locking of a SkL to the atomic lattice in Gd$_3$Ru$_4$Al$_{12}$ via high-resolution resonant elastic x-ray scattering (REXS). Weak easy-plane magnetic anisotropy, demonstrated here by a combination of ferromagnetic resonance and REXS, penalizes placing a skyrmion core on a site of the atomic lattice. Under these conditions, a commensurate SkL, locked to the crystal lattice, is stable at finite temperatures -- but gives way to a competing incommensurate ground state upon cooling. We discuss the role of Umklapp-terms in the Hamiltonian for the formation of this lattice-locked state, its magnetic space group, the role of slight discommensurations, or (line) defects in the magnetic texture, and contrast our findings with the case of SkLs in noncentrosymmetric material platforms.

cond-mat.str-el↗

arXiv2021

MIEZE Neutron Spin-Echo Spectroscopy of Strongly Correlated Electron Systems

Recent progress in neutron spin-echo spectroscopy by means of longitudinal Modulation of IntEnsity with Zero Effort (MIEZE) is reviewed. Key technical characteristics are summarized which highlight that the parameter range accessible in momentum and energy, as well as its limitations, are extremely well understood and controlled. Typical experimental data comprising quasi-elastic and inelastic scattering are presented, featuring magneto-elastic coupling and crystal field excitations in Ho2Ti2O7, the skyrmion lattice to paramagnetic transition under applied magnetic field in MnSi, ferromagnetic criticality and spin waves in Fe. In addition bench marking studies of the molecular dynamics in H2O are reported. Taken together, the advantages of MIEZE spectroscopy in studies at small and intermediate momentum transfers comprise an exceptionally wide dynamic range of over seven orders of magnitude, the capability to perform straight forward studies on depolarizing samples or under depolarizing sample environments, as well as on incoherently scattering materials.

cond-mat.str-el↗

arXiv2021

Robust noncoplanar magnetism in band filling-tuned (Nd$_{1-x}$Ca$_x$)$_2$Mo$_2$O$_7$

In the metallic pyrochlore Nd$_2$Mo$_2$O$_7$, the conducting Molybdenum sublattice adopts canted, yet nearly collinear ferromagnetic order with nonzero scalar spin chirality. The chemical potential may be controlled by replacing Nd$^{3+}$ with Ca$^{2+}$, while introducing only minimal additional disorder to the conducting states. Here, we demonstrate the stability of the canted ferromagnetic state, including the tilting angle of Molybdenum spins, in (Nd$_{1-x}$Ca$_{x}$)$_2$Mo$_2$O$_7$ (NCMO) with $x\le 0.15$ using magnetic susceptibility measurements. Mo-Mo and Mo-Nd magnetic couplings both change sign above $x=0.22$, where the canted ferromagnetic state gives way to a spin-glass metallic region. Contributions to the Curie-Weiss law from two magnetic sublattices are separated systematically.

cond-mat.mtrl-sci↗

arXiv2021

Geometrical Hall effect and momentum-space Berry curvature from spin-reversed band pairs

When nanometric, noncoplanar spin textures with scalar spin chirality (SSC) are coupled to itinerant electrons, they endow the quasiparticle wavefunctions with a gauge field, termed Berry curvature, in a way that bears analogy to relativistic spin-orbit coupling (SOC). The resulting deflection of moving charge carriers is termed geometrical (or topological) Hall effect. Previous experimental studies modeled this signal as a real-space motion of wavepackets under the influence of a quantum-mechanical phase. In contrast, we here compare the modification of Bloch waves themselves, and of their energy dispersion, due to SOC and SSC. Using the canted pyrochlore ferromagnet Nd$_2$Mo$_2$O$_7$ as a model compound, our transport experiments and first-principle calculations show that SOC impartially mixes electronic bands with equal or opposite spin, while SSC is much more effective for opposite spin band pairs.

cond-mat.str-el↗

arXiv2020

Topological Nernst effect of the two-dimensional skyrmion lattice

The topological Hall effect (THE) and its thermoelectric counterpart, the topological Nernst effect (TNE), are hallmarks of the skyrmion lattice phase (SkL). We observed the giant TNE of the SkL in centrosymmetric Gd$_2$PdSi$_3$, comparable in magnitude to the largest anomalous Nernst signals in ferromagnets. Significant enhancement (suppression) of the THE occurs when doping electrons (holes) to Gd$_2$PdSi$_3$. On the electron-doped side, the topological Hall conductivity approaches the characteristic threshold $\sim 1000\,\left(\mathrm{Ωcm}\right)^{-1}$ for the intrinsic regime. We use the filling-controlled samples to confirm Mott's relation between TNE and THE and discuss the importance of Gd-5d orbitals for transport in this compound.

cond-mat.str-el↗

arXiv2020

High-field depinned phase and planar Hall effect in skyrmion-host Gd$_2$PdSi$_3$

For the skyrmion-hosting intermetallic Gd$_2$PdSi$_3$ with centrosymmetric hexagonal lattice and triangular net of rare earth sites, we report a thorough investigation of the magnetic phase diagram. Our work reveals a new magnetic phase with isotropic value of the critical field for all orientations, where the magnetic ordering vector $\mathbf{q}$ is depinned from its preferred directions in the basal plane. This is in contrast to the highly anisotropic behavior of the low field phases, such as the skyrmion lattice (SkL), which are easily destroyed by in-plane magnetic field. The bulk nature of the SkL and of other magnetic phases was evidenced by specific-heat measurements. Resistivity anisotropy, likely originating from partial gapping of the density of states along $\mathbf{q}$ in this RKKY magnet, is picked up via the planar Hall effect (PHE). The PHE confirms the single-$\mathbf{q}$ nature of the magnetic order when the field is in the hexagonal plane, and allows to detect the preferred directions of $\mathbf{q}$. For field aligned perpendicular to the basal plane, several scenarios for the depinned phase (DP), such as tilted conical order, are discussed on the basis of the data.

cond-mat.str-el↗