arXiv subjects

Matthias D. Frontzek

Publications and source records attributed to Matthias D. Frontzek.

11 recordsLinked to original sources

arXiv2026

Frustration induced dimensional reduction and coexistence of long and short-range magnetic order in NdCl$_{3}$

The phenomenon of frustration greatly enriches the accessible physics of quantum magnets. With this in mind we study the magnetism of NdCl$_{3}$ using a combination of bulk properties measurements and neutron scattering techniques. The low-temperature heat capacity reveals two magnetic transitions at $T_{N1}$ = 270 mK and $T_{N2}$ = 180 mK. However, much of the magnetic entropy is released above $T_{N1}$, manifesting as a broad peak centered at $T^{*} \approx$ 450 mK. Single crystal elastic neutron scattering reveals highly anisotropic magnetic diffuse scattering above $T_{N2}$, confirming that quasi-one-dimensional, short-range, antiferromagnetic order is the origin of the broad peak in the heat capacity. Magnetic Bragg peaks characterized by a $\vec{k}$ = ($0$ $0$ $\frac{1}{2}$) propagation vector emerge below $T_{N1}$. Interestingly, the magnetic diffuse scattering persists for $T_{N2} < T < T_{N1}$, indicating a regime of coexisting short and long-range order. The magnetic Bragg peaks exhibit an additional increase in intensity below $T_{N2}$ with no change in $\vec{k}$. Concomitantly, the diffuse scattering disappears indicating the attainment of full long-range order. While the precise nature of the ordered magnetic ground state remains unresolved, the observed magnetic scattering indicates predominate $c$-axis moments with a small $ab$-plane component. We propose that the quasi-one-dimensional behavior and the coexistence of short and long-range order are driven by frustration of anisotropic exchange interactions.

cond-mat.str-el↗

arXiv2026

Magnetism of single crystalline breathing pyrochlore spinel AgInCr4S8

Single crystals of \ce{AgInCr4S8} were grown by chemical vapor transport and crystallographic ordering of Ag/In that results in a breathing pyrochlore motif of Cr$^{3+}$ was verified by x-ray and neutron diffraction. Long-range antiferromagnetic order is observed below a Néel temperature of $T_{\mathrm N}$ $\approx$ 9.6 K. The magnetic properties are characterized using ac and dc magnetization, specific heat capacity, and single crystal neutron diffraction measurements. The specific heat data are characterized by a small lambda anomaly near 9.5 K and the estimated magnetic entropy reaches $\approx$ $\frac{1}{3}$ of the expected value by 3$T_{\mathrm N}$, suggesting significant short-range order in the paramagnetic phase. Single crystal neutron diffraction evidences an incommensurate spin structure with propagation vector $\textbf{\textit{k}}$ = (0,0,$δ$) and $δ$ = 0.343 at 5 K. The minimal model that accounts for the data consists of ferromagnetic layers of Cr atoms, with magnetic moments lying in the plane of the layers and modulating in the perpendicular direction to form a helical structure propagating along $\textbf{\textit{k}}$. This study represents a rare investigation of single crystals within the family of breathing pyrochlore materials.

cond-mat.str-el↗

arXiv2025

Skyrmion and Meron Crystals in Intermetallic Gd$_3$Ru$_4$Al$_{12}$: Microscopic Model Insights into Chiral Phases

Topological spin textures in frustrated intermetallics hold great promise for spintronics applications. However, understanding their origin and properties remains a significant challenge due to competing and often long-range interactions mediated by conduction electrons. Here, by combining neutron scattering experiments with theoretical modeling via unprecedented multi-target fits that further incorporate the ferromagnentic resonance data and magnetization curve, we construct a realistic microscopic model for the prototypical intermetallic skyrmion host \text{Gd}$_3$\text{Ru}$_4$\text{Al}$_{12}$. Beyond magnetic frustration, we identify the competition between dipolar interactions and easy-plane single-ion anisotropy as a key ingredient for stabilizing the rich chiral magnetic phases observed in this compound -- including a hexagonal skyrmion crystal and two distinct meron crystals. Remarkably, the meron crystal in lower field is revealed to be commensurate with the underlying lattice, and its unique three-meron-one-antimeron spin texture is verified by the polarized x-ray diffraction data. At elevated temperatures, the short-range spin correlations in \text{Gd}$_3$\text{Ru}$_4$\text{Al}$_{12}$ are well described by a codimension-two spiral spin-liquid. Perturbations from staggered Dzyaloshinskii-Moriya interactions give rise to chiral fluctuations that account for the temperature and field dependence of the anomalous Hall response. Our results highlight the unique power of neutron scattering, especially when combined with complementary experimental techniques, to unravel complex magnetic phase transitions and provide new insights into the rich variety of topological spin textures in frustrated systems.

cond-mat.str-el↗

arXiv2025

Disorder-induced proximate quantum spin ice phase in Pr2Sn2O7

Magnetic pyrochlores with non-Kramers rare-earth ions provide a platform for exploring emergent gauge physics and quantum spin-ice behavior, yet the influence of structural disorder on their ground states remains insufficiently understood. Here we combine bulk characterization and single-crystal neutron-scattering measurements to investigate the non-Kramers pyrochlore Pr2Sn2O7. At temperatures below ~1 K, the system exhibits key hallmarks of quantum spin-ice physics, including anisotropic spin-ice correlations and two distinct dynamical timescales. Upon further cooling, however, we observe a complete spin-freezing transition at T_f ~ 0.15 K, accompanied by recovery of the full nuclear Schottky anomaly, the emergence of a gapped magnetic excitation, and the development of incipient (100) magnetic correlations. Comparison with related Pr-based pyrochlores places Pr2Sn2O7 near the spin-frozen boundary of a disorder-perturbed phase diagram. These results establish a disorder-driven framework for the evolution of quantum spin-ice behavior into frozen ground states, revealing how signatures of a proximate quantum spin liquid can persist despite disorder-induced spin freezing in non-Kramers pyrochlores.

cond-mat.str-el↗

arXiv2025

A planning tool for neutron powder diffraction experiments

We introduce a computer program to simulate the results of neutron powder-diffraction experiments at the High Flux Isotope Reactor at Oak Ridge National Laboratory. The program is freely available as a web application at http://addie.ornl.gov/hfirestimate, and is designed to be straightforward to use for researchers who are new to neutron diffraction. The input includes the crystal structure of the proposed sample, the sample mass, and the instrument configuration. The results include a plot of the simulated data -- including realistic estimates of background and the error bars due to counting statistics -- and suggestions of how to resolve potential problems with the experiment. Here, we explain the design and implementation of this program and demonstrate its performance using comparisons of simulated and experimental data. We hope that this program will enable researchers to plan neutron-scattering experiments more effectively, increasing the likelihood of successful experiments and improving the productivity of neutron-diffraction research.

physics.ins-det↗

arXiv2024

Anomalous Hall effect from inter-superlattice scattering in a noncollinear antiferromagnet

Superlattice formation dictates the physical properties of many materials, including the nature of the ground state in magnetic materials. Chemical composition is commonly considered to be the primary determinant of superlattice identity, especially in intercalation compounds. Here, we find that, contrary to this conventional wisdom, kinetic control of superlattice growth leads to the coexistence of disparate domains within a compositionally "perfect" single crystal. We demonstrate that Cr$_{1/4}$TaS$_2$ is a bulk noncollinear antiferromagnet in which scattering between bulk and minority superlattice domains engenders complex magnetotransport below the Néel temperature, including an anomalous Hall effect. We characterize the magnetic phases in different domains, image their nanoscale morphology, and propose a mechanism for nucleation and growth. These results provide a blueprint for the deliberate engineering of macroscopic transport responses via microscopic patterning of magnetic exchange interactions in superlattice domains.

cond-mat.mtrl-sci↗

arXiv2024

Spin waves in Dirac semimetal Ca$_{0.6}$Sr$_{0.4}$MnSb$_2$ investigated with neutrons by the diffraction method

We report neutron diffraction measurements of Ca$_{0.6}$Sr$_{0.4}$MnSb$_2$, a low-carrier-density Dirac semimetal in which the antiferromagnetic Mn layers are interleaved with Sb layers that host Dirac fermions. We have discovered that we can detect a good quality inelastic spin wave signal from a small (m ~ 0.28 g) single crystal sample by the diffraction method, without energy analysis, using a neutron diffractometer with a position-sensitive area detector; the spin-waves appear as diffuse scattering that is shaped by energy-momentum conservation. By fitting this characteristic magnetic scattering to a spin-wave model, we refine all parameters of the model spin Hamiltonian, including the inter-plane interaction, through use of a three-dimensional measurement in reciprocal space. We also measure the temperature dependence of the spin waves, including the softening of the spin gap on approaching the Neel temperature, $T_N$. Not only do our results provide important new insights into an interplay of magnetism and Dirac electrons, they also establish a new, high-throughput approach to characterizing magnetic excitations on a modern diffractometer without direct energy analysis. Our work opens exciting new opportunities for the follow-up parametric and compositional studies on small, ~0.1 g crystals.

cond-mat.str-el↗

arXiv2022

Magnetic Interactions of the Centrosymmetric Skyrmion Material Gd2PdSi3

The experimental realization of magnetic skyrmions in centrosymmetric materials has been driven by theoretical understanding of how a delicate balance of anisotropy and frustration can stabilize topological spin structures in applied magnetic fields. Recently, the centrosymmetric material Gd$_{2}$PdSi$_{3}$ was shown to host a field-induced skyrmion phase, but the skyrmion stabilization mechanism remains unclear. Here, we employ neutron-scattering measurements on an isotopically-enriched polycrystalline Gd$_{2}$PdSi$_{3}$ sample to quantify the interactions that drive skyrmion formation. Our analysis reveals spatially-extended interactions in triangular planes that are consistent with an RKKY mechanism, and large ferromagnetic inter-planar magnetic interactions that are modulated by the Pd/Si superstructure. The skyrmion phase emerges from a zero-field helical magnetic order with magnetic moments perpendicular to the magnetic propagation vector, indicating that the magnetic dipolar interaction plays a significant role. Our experimental results establish an interaction space that can promote skyrmion formation, facilitating identification and design of centrosymmetric skyrmion materials.

cond-mat.str-el↗

arXiv2020

Ferrimagnetic 120$^\circ$ magnetic structure in Cu2OSO4

We report magnetic properties of a 3d$^9$ (Cu$^{2+}$) magnetic insulator Cu2OSO4 measured on both powder and single crystal. The magnetic atoms of this compound form layers, whose geometry can be described either as a system of chains coupled through dimers or as a Kagomé lattice where every 3rd spin is replaced by a dimer. Specific heat and DC-susceptibility show a magnetic transition at 20 K, which is also confirmed by neutron scattering. Magnetic entropy extracted from the specific heat data is consistent with a $S=1/2$ degree of freedom per Cu$^{2+}$, and so is the effective moment extracted from DC-susceptibility. The ground state has been identified by means of neutron diffraction on both powder and single crystal and corresponds to a $\sim120$ degree spin structure in which ferromagnetic intra-dimer alignment results in a net ferrimagnetic moment. No evidence is found for a change in lattice symmetry down to 2 K. Our results suggest that \sample \ represents a new type of model lattice with frustrated interactions where interplay between magnetic order, thermal and quantum fluctuations can be explored.

cond-mat.str-el↗

arXiv2019

An in-plane hexagonal antiferromagnet in the Cu-Mn-As system, Cu$_{0.82}$Mn$_{1.18}$As

We report the single-crystal growth and characterization of a new hexagonal phase, Cu$_{0.82}$Mn$_{1.18}$As, in the Cu-Mn-As system. This compound contains the same square-pyramidal MnAs$_5$ units as the tetragonal and orthorhombic polymorphs of CuMnAs. Calorimetry, magnetometry, and neutron diffraction measurements reveal antiferromagnetic ordering at 270 K. The magnetic structure consists of a triangular arrangement of spins in the $ab$ plane. Hexagonal Cu$_{0.82}$Mn$_{1.18}$As shows resistivity that varies only weakly from 5 K to 300 K, and is many times higher than tetragonal CuMnAs, indicative of a strongly-scattering metal. First-principles calculations confirm the metallic band structure with a small density of states at the Fermi energy. The neutron-refined magnetic ground state is close to the computationally-determined minimum energy configuration. This compound should serve as a clear control when disentangling the effects of current-driven Néel switching of metallic antiferromagnets since it exhibits in-plane spins but the magnetic ordering does not break degeneracy along the $a$ and $b$ directions, unlike tetragonal CuMnAs.

cond-mat.mtrl-sci↗

arXiv2018

Unique Helical Magnetic Order and Field-Induced Phase in Trillium Lattice Antiferromagnet EuPtSi

Magnetic transition phenomena in cubic chiral antiferromagnet EuPtSi with $T_{\rm N}$=4.0~K were investigated by means of single crystal neutron diffraction. At 0.3~K in the ground state, magnetic peaks emerge at positions represented by an ordering vector ${q}_{1}$=$(0.2, 0.3, 0)$ and its cyclic permutation. Upon heating, an additional magnetic peak splitting with hysteresis was uncovered at around $T^*_{\rm N}{\sim}$2.5~K, indicating the presence of a first-order commensurate-incommensurate transition with ${q}^*_{1}$=$(0.2, 0.3, δ)$ ($δ_{\rm max}{\simeq}$0.04) at $T^*_{\rm N}$. A half-polarized neutron scattering experiment for polarization parallel to the scattering vector revealed that polarization antiparallel to the scattering vector has stronger intensity in both magnetic phases. This feature clarifies the single chiral character of the helical structure with moments lying perpendicular to the ordering vector in both ordered states. Under a vertical magnetic field of 1.2~T for ${B}{\parallel}$[1,1,1] at 1.9~K entering into the so-called $A$ phase, magnetic peaks form characteristic hexagonal patterns in the equatorial scattering plane around nuclear peaks. An ordering vector ${q}_{A}{\simeq}({\pm}0.09, {\pm}0.20, {\mp}0.28)$ of the $A$-phase has similar periodic length as $q_{1}$, and could be the hallmark of a formation of skyrmion lattice in EuPtSi.

cond-mat.str-el↗