arXiv subjects

C. Franz

Publications and source records attributed to C. Franz.

At least 19 recordsLinked to original sources

arXiv2024

Long-range magnetic order in CePdAl$_3$ enabled by orthorhombic deformation

We investigate the effect of structural deformation on the magnetic properties of orthorhombic CePdAl$_3$ in relation to its tetragonal polymorph. Utilizing x-ray and neutron diffraction we establish that the crystal structure has the $Cmcm$ space group symmetry and exhibits pseudo-tetragonal twinning. According to density-functional calculations the tetragonal-orthorhombic deformation mechanism has its grounds in relatively small free enthalpy difference between the polymorphs, allowing either phase to be quenched and fully accounts for the twinned microstructure of the orthorhombic phase. Neutron diffraction measurements show that orthorhombic CePdAl$_3$ establishes long-range magnetic order below $T_\mathrm{N}$=5.29 (5) K characterized by a collinear, antiferromagnetic arrangement of magnetic moments. Magnetic anisotropies of orthorhombic CePdAl$_3$ arise from strong spin-orbit coupling as evidenced by the crystal-field splitting of the $4f$ multiplet, fully characterised with neutron spectroscopy. We discuss the potential mechanism of frustration posed by antiferromagnetic interactions between nearest neighbours in the tetragonal phase, which hinders the formation of long-range magnetic order in tetragonal CePdAl$_3$. We propose that orthorhombic deformation releases the frustration and allows for long-range magnetic order.

cond-mat.str-el↗

arXiv2024

Spin-Energy Entanglement of a Time-Focused Neutron

Intra-particle entanglement of individual particles such as neutrons could enable another class of scattering probes that are sensitive to entanglement in quantum systems and materials. In this work, we present experimental results demonstrating quantum contextuality as a result of entanglement between the spin and energy modes (i.e., degrees of freedom) of single neutrons in a beam using a pair of resonant radio-frequency neutron spin flippers in the MIEZE configuration (Modulated IntEnsity with Zero Effort). We verified the mode-entanglement by measuring a Clauser-Horne-Shimony-Holt (CHSH) contextuality witness $S$ defined in the spin and energy subsystems, observing a clear breach of the classical bound of $|S| \leq 2$, obtaining $S = 2.40 \pm 0.02$. These entangled beams could enable alternative approaches for directly probing dynamics and entanglement in quantum materials whose low-energy excitation scales match those of the incident entangled neutron.

quant-ph↗

arXiv2023

Comparison of time-of-flight with MIEZE spectroscopy of H$_2$O: Necessity to go beyond the spin-echo approximation

Here, we discuss the comparability of data acquisitioned with the Modulation of IntEnsity with Zero Effort data, a neutron spin-echo (NSE) technique to neutron Time-of-Flight (ToF) spectroscopy data. As a NSE technique MIEZE records the intermediate scattering function $\mathcal{I}(Q, \tau)$ making it necessary to perform a Fourier transform to directly compare it to $S(Q, E)$, measured by ToF spectroscopy. Transforming either data set into the complementary parameter space requires detailed knowledge of detector efficiency, instrumental resolution, and background. We discuss these aspects by comparing measurements on pure water performed on the spectrometers RESEDA and TOFTOF under the same experimental conditions. Additionally, we discuss the data evaluation of spin-echo data beyond the SE approximation, which limits these techniques to small energy transfers. Furthermore, computational methods like molecular dynamics simulations are essential for understanding these processes and will become increasingly important as we study more complex systems.

cond-mat.soft↗

arXiv2022

MIASANS at the longitudinal neutron resonant spin-echo spectrometer RESEDA

The RESEDA (Resonant Spin-Echo for Diverse Applications) instrument has been optimized for neutron scattering measurements of quasi-elastic and inelastic processes over a wide parameter range. One spectrometer arm of RESEDA is configured for the MIEZE (Modulation of Intensity with Zero Effort) technique, where the measured signal is an oscillation in neutron intensity over time prepared by two precisely tuned radio-frequency (RF) flippers. With MIEZE, all spin-manipulations are performed before the beam reaches the sample, and thus the signal from sample scattering is not disrupted by any depolarizing conditions there (i.e. magnetic materials and fields). The MIEZE spectrometer is being further optimized for the requirements of small angle neutron scattering (MIASANS), a versatile combination of the spatial and dynamical resolving power of both techniques. We present the current status of (i) the newly installed superconducting solenoids as part of the RF flippers to significantly extend the dynamic range (ii) the development and installation of a new detector on a translation stage within a new larger SANS-type vacuum vessel for flexibility with angular coverage and resolution, and (iii) the efforts to reduce background.

physics.ins-det↗

arXiv2022

Magnetic properties of the noncentrosymmetric tetragonal antiferromagnet EuPtSi$_{3}$

We report a comprehensive study of single crystals of the noncentrosymmetric rare-earth compound EuPtSi$_{3}$ grown by the optical floating-zone technique. Measurements of the magnetization, ac susceptibility, and specific heat consistently establish antiferromagnetic order of localized Eu$^{2+}$ moments below the N\'{e}el temperature $T_{\mathrm{N}} = 17~\mathrm{K}$, followed by a second magnetic transition at $T_{\mathrm{N1}} = 16~\mathrm{K}$. For a magnetic field along the easy $[001]$ axis, the magnetic phase diagram is composed of these two phases. For fields applied in the magnetically hard basal plane, two additional phases emerge under magnetic field, where the in-plane anisotropy is weak with $[100]$ being the hardest axis. At the phase transitions, the magnetic properties exhibit hysteresis and discrepancies between differential and ac susceptibility, suggesting slow reorientation processes of mesoscale magnetic textures. Consistently, powder and single-crystal neutron diffraction in zero field identify magnetic textures that are modulated on a length scale of the order of $100~\textrm{\r{A}}$, most likely in the form of N\'{e}el-type antiferromagnetic cycloids.

cond-mat.str-el↗

arXiv2022

Topological magnon band structure of emergent Landau levels in a skyrmion lattice

The motion of a spin excitation across topologically non-trivial magnetic order exhibits a deflection that is analogous to the effect of the Lorentz force on an electrically charged particle in an orbital magnetic field. We used polarized inelastic neutron scattering to investigate the propagation of magnons (i.e., bosonic collective spin excitations) in a lattice of skyrmion tubes in manganese silicide. For wave vectors perpendicular to the skyrmion tubes, the magnon spectra are consistent with the formation of finely spaced emergent Landau levels that are characteristic of the fictitious magnetic field used to account for the nontrivial topological winding of the skyrmion lattice. This provides evidence of a topological magnon band structure in reciprocal space, which is borne out of the nontrivial real-space topology of a magnetic order.

cond-mat.str-el↗

arXiv2021

Incommensurate antiferromagnetic order in CePtAl$_3$

We report a neutron diffraction study of single-crystal CePtAl$_3$ complemented by measurements of the specific heat under applied magnetic field. Below $T_\mathrm{N}$=3 K CePtAl$_3$ develops incommensurate antiferromagnetic order with a single modulation vector $\vec{k}$=$(0.676 \, 0 \, 0)$. Residual magnetic scattering intensity above $T_\mathrm{N}$ and a broadening of the specific heat anomaly at $T_\mathrm{N}$ may be consistently described in terms of a Gaussian distribution of transition temperatures with a standard deviation $\sigma\approx0.5\,{\rm K}$. The distribution of $T_\mathrm{N}$ may be attributed to the observation of occupational and positional disorder between the Pt and Al sites. Measurements under magnetic field reveal unusual changes of the domain populations when the field is applied along the $[0\,1\,0]$ direction consistent with a transition from cycloidal to amplitude modulated magnetic order around 2.5 T.

cond-mat.str-el↗

arXiv2021

Optimized signal deduction procedure for the MIEZE spectroscopy technique

We report a method to determine the phase and amplitude of sinusoidally modulated event rates, binned into four bins per oscillation, based on data generated at the resonant neutron spin-echo spectrometer RESEDA. The presented algorithm relies on a reconstruction of the unknown parameters. It omits a calculation intensive fitting procedure and avoids contrast reduction due to averaging effects. It allows the current data acquisition bottleneck at RESEDA to be relaxed by a factor of four and thus increases the potential time resolution of the detector by the same factor. We explain the approach in detail and compare it to the established fitting procedures of time series having four and 16 time bins per oscillation. In addition we present the empirical estimates of the errors of the three methods and compare them to each other. We show that the reconstruction is unbiased, asymptotic, and efficient for estimating the phase. Reconstructing the contrast increases the error bars by roughly 10% as compared to fitting 16 time binned oscillations. Finally, we give heuristic, analytical equations to estimate the error for phase and contrast as a function of their initial values and counting statistics.

cond-mat.str-el↗

arXiv2020

Oscillatory magnetic fields for neutron resonance spin-echo spectroscopy

The generation of high frequency oscillatory magnetic fields represents a fundamental component underlying the successful implementation of neutron resonant spin-echo spectrometers, a class of instrumentation critical for the high-resolution extraction of dynamical excitations (structural and magnetic) in materials. In this paper, the setup of the resonant circuits at the longitudinal resonant spin-echo spectrometer RESEDA is described in comprehensive technical detail. We demonstrate that these circuits are capable of functioning at frequencies up to 3.6 MHz and over a broad bandwidth down to 35 kHz using a combination of signal generators, amplifiers, impedance matching transformers, and a carefully designed cascade of tunable capacitors and customized coils.

cond-mat.str-el↗

arXiv2019

Weak crystallization of fluctuating skyrmion textures in MnSi

We report an experimental study of the emergence of non-trivial topological winding and long-range order across the paramagnetic to skyrmion lattice transition in the transition metal helimagnet MnSi. Combining measurements of the susceptibility with small angle neutron scattering, neutron resonance spin echo spectroscopy and all-electrical microwave spectroscopy, we find evidence of skyrmion textures in the paramagnetic state exceeding $10^3$Åwith lifetimes above several 10$^{-9}$s. Our experimental findings establish that the paramagnetic to skyrmion lattice transition in MnSi is well-described by the Landau soft-mode mechanism of weak crystallization, originally proposed in the context of the liquid to crystal transition. As a key aspect of this theoretical model, the modulation-vectors of periodic small amplitude components of the magnetization form triangles that add to zero. In excellent agreement with our experimental findings, these triangles of the modulation-vectors entail the presence of the non-trivial topological winding of skyrmions already in the paramagnetic state of MnSi when approaching the skyrmion lattice transition.

cond-mat.str-el↗

arXiv2019

Time of Flight Modulation of Intensity by Zero Effort on Larmor

A time of flight Modulation of IntEnsity by Zero Effort (MIEZE) spectrometer mode has been developed for the Larmor instrument at the ISIS pulsed neutron source. The instrument utilizes resonant neutron spin flippers which employ electromagnets with pole shoes, allowing the flippers to operate at frequencies of up to 3 MHz. Tests were conducted at modulation frequencies of 103 kHz, 413 kHz, 826 kHz and 1.03 MHz, resulting in a Fourier time range of ~0.1 ns to 30 ns using wavelength band of 4 {\AA}-11 {\AA}.

physics.app-ph↗

arXiv2019

Ultra-High Resolution Neutron Spectroscopy of Low-Energy Spin Dynamics in UGe$_2$

Studying the prototypical ferromagnetic superconductor UGe$_2$ we demonstrate the potential of the Modulated IntEnsity by Zero Effort (MIEZE) technique---a novel neutron spectroscopy method with ultra-high energy resolution of at least 1~$μ$eV---for the study of quantum matter. We reveal purely longitudinal spin fluctuations in UGe$_2$ with a dual nature arising from $5f$ electrons that are hybridized with the conduction electrons. Local spin fluctuations are perfectly described by the Ising universality class in three dimensions, whereas itinerant spin fluctuations occur over length scales comparable to the superconducting coherence length, showing that MIEZE is able to spectroscopically disentangle the complex low-energy behavior characteristic of quantum materials.

cond-mat.str-el↗

arXiv2018

Lattice dynamics and coupled quadrupole-phonon excitations in CeAuAl$_3$

We report first principles calculations of the structural parameters and phonon dispersion of the tetragonal non-centrosymmetric heavy fermion compound CeAuAl$_3$. Taking into account weak magnetoelastic interactions of the rare-earth (RE) ions with the spectrum of phonons, we obtain an analytical expression for the hybridization of quadrupole excitations and phonons from the poles of the one-phonon Green-function. In the paramagnetic phase, we predict the formation of mixed modes that may be observed by inelastic neutron scattering. Our results show that magnetoelastic interactions, albeit being moderate, play an important role in CeAuAl$_3$. This suggests that magnetoelastic interactions may be equally important in a wide range of related compounds.

cond-mat.mtrl-sci↗

arXiv2016

Ultra-high vacuum compatible preparation chain for intermetallic compounds

We report the development of a versatile material preparation chain for intermetallic compounds that focuses on the realization of a high-purity growth environment. The preparation chain comprises of an argon glovebox, an inductively heated horizontal cold boat furnace, an arc melting furnace, an inductively heated rod casting furnace, an optically heated floating-zone furnace, a resistively heated annealing furnace, and an inductively heated annealing furnace. The cold boat furnace and the arc melting furnace may be loaded from the glovebox by means of a load-lock permitting to synthesize compounds starting with air-sensitive elements while handling the constituents exclusively in an inert gas atmosphere. All furnaces are all-metal sealed, bakeable, and may be pumped to ultra-high vacuum. We find that the latter represents an important prerequisite for handling compounds with high vapor pressure under high-purity argon atmosphere. We illustrate operational aspects of the preparation chain in terms of the single-crystal growth of the heavy-fermion compound CeNi2Ge2.

cond-mat.mtrl-sci↗

arXiv2016

Single crystal growth of CeTAl$_3$ (T = Cu, Ag, Au, Pd and Pt)

We report single crystal growth of the series of CeTAl$_3$ compounds with T = Cu, Ag, Au, Pd and Pt by means of optical float zoning. High crystalline quality was confirmed in a thorough characterization process. With the exception of CeAgAl$_3$, all compounds crystallize in the non-centrosymmetric tetragonal BaNiSn$_{3}$ structure (space group: I4mm, No. 107), whereas CeAgAl$_3$ adopts the related orthorhombic PbSbO$_2$Cl structure (Cmcm, No. 63). An attempt to grow CeNiAl$_3$ resulted in the composition CeNi$_2$Al$_5$. Low temperature resistivity measurements down to $\sim$0.1K did not reveal evidence suggestive of magnetic order in CePtAl$_3$ and CePdAl$_3$. In contrast, CeAuAl$_3$, CeCuAl$_3$ and CeAgAl$_3$ display signatures of magnetic transitions at 1.3K, 2.1K and 3.2K, respectively. This is consistent with previous reports of antiferromagnetic order in CeAuAl$_3$, and CeCuAl$_3$ as well as ferromagnetism in CeAgAl$_3$, respectively.

cond-mat.str-el↗

arXiv2015

Coherent ultrafast spin-dynamics probed in three dimensional topological insulators

Topological insulators are candidates to open up a novel route in spin based electronics. Different to traditional ferromagnetic materials, where the carrier spin-polarization and magnetization are based on the exchange interaction, the spin properties in topological insulators are based on the coupling of spin- and orbit interaction connected to its momentum. Specific ways to control the spin-polarization with light have been demonstrated: the energy momentum landscape of the Dirac cone provides spin-momentum locking of the charge current and its spin. The directionality of spin and momentum, as well as control with light has been demonstrated. Here we demonstrate a coherent femtosecond control of spin-polarization for states in the valence band at around the Dirac cone.

cond-mat.mes-hall↗

arXiv2014

Real-Space and Reciprocal-Space Berry Phases in the Hall Effect of Mn$_{\rm 1-x}$Fe$_{\rm x}$Si

We report an experimental and computational study of the Hall effect in Mn$_{\rm 1-x}$Fe$_{\rm x}$Si, as complemented by measurements in Mn$_{\rm 1-x}$Co$_{\rm x}$Si, when helimagnetic order is suppressed under substitutional doping. For small $x$ the anomalous Hall effect (AHE) and the topological Hall effect (THE) change sign. Under larger doping the AHE remains small and consistent with the magnetization, while the THE grows by over a factor of ten. Both the sign and the magnitude of the AHE and the THE are in excellent agreement with calculations based on density functional theory. Our study provides the long-sought material-specific microscopic justification, that while the AHE is due to the reciprocal-space Berry curvature, the THE originates in real-space Berry phases.

cond-mat.str-el↗

arXiv2014

Formation of a topological non-Fermi liquid in MnSi

Fermi liquid theory provides a remarkably powerful framework for the description of the conduction electrons in metals and their ordering phenomena, such as superconductivity, ferromagnetism, and spin- and charge-density-wave order. A different class of ordering phenomena of great interest concerns spin configurations that are topologically protected, that is, their topology can be destroyed only by forcing the average magnetization locally to zero. Examples of such configurations are hedgehogs (points at which all spins are either pointing inwards or outwards) or vortices. A central question concerns the nature of the metallic state in the presence of such topologically distinct spin textures. Here we report a high-pressure study of the metallic state at the border of the skyrmion lattice in MnSi, which represents a new form of magnetic order composed of topologically non-trivial vortices. When long-range magnetic order is suppressed under pressure, the key characteristic of the skyrmion lattice - that is, the topological Hall signal due to the emergent magnetic flux associated with their topological winding - is unaffected in sign or magnitude and becomes an important characteristic of the metallic state. The regime of the topological Hall signal in temperature, pressure and magnetic field coincides thereby with the exceptionally extended regime of a pronounced non-Fermi-liquid resistivity. The observation of this topological Hall signal in the regime of the NFL resistivity suggests empirically that spin correlations with non-trivial topological character may drive a breakdown of Fermi liquid theory in pure metals.

cond-mat.str-el↗