arXiv subjects

Collin L. Broholm

Publications and source records attributed to Collin L. Broholm.

11 recordsLinked to original sources

arXiv2026

Stacking-dependent anisotropic altermagnetism in V$_{1/3}$NbS$_2$

We report profound impacts of the stacking sequence of triangular lattices of magnetic transition metal ions intercalated between the layers of the van der Waals material NbS$_2$. Using single crystal x-ray and neutron diffraction, and transport and magnetization measurements, we show there are two distinct polytypes of $\rm V_{1/3}NbS_2$ with disparate easy axes of magnetization and different anomalous Hall responses. Self-consistent analysis of inelastic neutron scattering data provides evidence for oscillatory RKKY interactions that extend to 1 nm and stabilize quasi-collinear A-type altermagnetic orders in both polytypes though with perpendicular easy axes. The detailed stacking sequence of a bulk polytype crystal dramatically impact its macroscopic anomalous Hall response and magnetism, which suggests a new path to engineer the bulk properties of a layered three dimensional solid.

cond-mat.str-el↗

arXiv2024

Magnetic excitations and interactions in the Weyl ferrimagnet NdAlSi

Weyl fermions can arise from time-reversal symmetry-breaking magnetism, but their impact on magnetic order is a source of ongoing research. Using high-precision neutron diffraction and spectroscopy, we present a comprehensive exploration of the magnetic structure and excitation spectrum of Weyl semimetal and helical magnet NdAlSi. We use Luttinger-Tisza, classical mean-field, and random-phase approximation techniques to model the dispersive crystal field excitons. We find extended-ranged and sign-changing interactions, suggesting a coupling between conduction electrons and the local moments. We demonstrate that low-symmetry anisotropic Dzyaloshinskii-Moriya interactions, in contrast with higher-symmetry interactions enabled by Weyl fermions, play an important role in stabilizing the complex spin spiral ground state of NdAlSi. Our work provides a first detailed view of microscopic interactions in a Weyl magnet, and constrains the role of Weyl electrons and their chirality on the spiral magnetism.

cond-mat.str-el↗

arXiv2023

Non-collinear 2k antiferromagnetism in the Zintl semiconductor Eu$_5$In$_2$Sb$_6$

Eu$_5$In$_2$Sb$_6$ is an orthorhombic non-symmorphic small band gap semiconductor with three distinct Eu$^{2+}$ sites and two low-temperature magnetic phase transitions. The material displays one of the greatest (negative) magnetoresistances of known stoichiometric antiferromagnets and belongs to a family of Zintl materials that may host an axion insulator. Using single crystal neutron diffraction, we show that the $T_{\mathrm{N1}}=14\mathrm{~K}$ second-order phase transition is associated with long-range antiferromagnetic order within the chemical unit cell $\left( k_1 = (000) \right)$. Upon cooling below $T_{\mathrm{N1}}$, the relative sublattice magnetizations of this structure vary until a second-order phase transition at $T_{\mathrm{N2}}=7\mathrm{~K}$ that doubles the unit cell along the $\hat{c}$ axis $\left( k_2 = \left(00\frac{1}{2}\right) \right)$. We show the anisotropic susceptibility and our magnetic neutron diffraction data are consistent with magnetic structures described by the $Γ_3$ irreducible representation with the staggered magnetization of the $k_1$ and $k_2$ components polarized along the $\hat{b}$ and $\hat{a}$ axis, respectively. As the $k_2$ component develops, the amplitude of the $k_1$ component is reduced, which indicates a 2k non-collinear magnetic structure. Density functional theory is used to calculate the energies of these magnetic structures and to show the $k_1$ phase is a metal so $T_{\mathrm{N1}}$ is a rare example of a unit-cell-preserving second-order phase transition from a paramagnetic semiconductor to an antiferromagnetic metal. DFT indicates the transition at $T_{\mathrm{N2}}$ to a doubled unit cell reduces the carrier density of the metal, which is consistent with resistivity data.

cond-mat.str-el↗

arXiv2023

Fragile superconductivity in a Dirac metal

Studying superconductivity in Dirac semimetals is an important step in understanding quantum matter with topologically non-trivial order parameters. We report on the properties of the superconducting phase in single crystals of the Dirac material LaCuSb2 prepared by the self-flux method. We find that chemical and hydrostatic pressure drastically suppress the superconducting transition. Furthermore, due to large Fermi surface anisotropy, magnetization and muon spin relaxation measurements reveal Type-II superconductivity for applied magnetic fields along the $a$-axis, and Type-I superconductivity for fields along the $c$-axis. Specific heat confirms the bulk nature of the transition, and its deviation from single-gap $s$-wave BCS theory suggests multigap superconductivity. Our tight-binding model points to an anisotropic gap function arising from the spin-orbital texture near the Dirac nodes, providing an explanation for the appearance of an anomaly in specific heat well below $T_c$. Given the existence of superconductivity in a material harboring Dirac fermions, LaCuSb2 proves an interesting material candidate in the search for topological superconductivity.

cond-mat.supr-con↗

arXiv2023

Quantum paramagnetism in a non-Kramers rare-earth oxide: Monoclinic $\rm Pr_2Ti_2O_7$

Little is so far known about the magnetism of the $\rm A_2B_2O_7$ monoclinic layered perovskites that replace the spin-ice supporting pyrochlore structure for $r_A/r_B>1.78$. We show that high quality monoclinic Pr$_2$Ti$_2$O$_7$ single crystals with a three-dimensional network of non-Kramers Pr$^{3+}$ ions that interact through edge-sharing super-exchange interactions, form a singlet ground state quantum paramagnet that does not undergo any magnetic phase transitions down to at least 1.8 K. The chemical phase stability, structure, and magnetic properties of the layered perovskite Pr$_2$Ti$_2$O$_7$ were investigated using x-ray diffraction, transmission electron microscopy, and magnetization measurements. Synthesis of polycrystalline samples with the nominal compositions of Pr$_2$Ti$_{2+x}$O$_7$ ($-0.16 \leq x \leq 0.16$) showed that deviations from the Pr$_2$Ti$_2$O$_7$ stoichiometry lead to secondary phases of related, structures including the perovskite phase Pr$_{2/3}$TiO$_3$ and the orthorhombic phases Pr$_4$Ti$_9$O$_{24}$ and Pr$_2$TiO$_5$. No indications of site disordering (stuffing and anti-stuffing) or vacancy defects were observed in the Pr$_2$Ti$_2$O$_7$ majority phase. A procedure for growth of high-structural-quality, stoichiometric single crystals of Pr$_2$Ti$_2$O$_7$ by the traveling solvent floating zone (TSFZ) method is reported. Thermo-magnetic measurements of single-crystalline Pr$_2$Ti$_2$O$_7$ reveal an isolated singlet ground state that we associate with the low symmetry crystal electric field environments that split the $2J+1=9$-fold degenerate spin-orbital multiplets of the four differently coordinated Pr$^{3+}$ ions into 36 isolated singlets resulting in an anisotropic temperature independent van-Vleck susceptibility at low $T$. A small isotropic Curie term is associated with 0.96(2)\% non-interacting Pr$^{4+}$ impurities.

cond-mat.mtrl-sci↗

arXiv2021

A new noncollinear ferromagnetic Weyl semimetal with anisotropic anomalous Hall effect

A developing frontier in condensed matter physics is the emergence of novel electromagnetic responses, such as topological and anomalous Hall effect (AHE), in ferromagnetic Weyl semimetals (FM-WSMs). Candidates of FM-WSM are limited to materials that preserve inversion symmetry and generate Weyl crossings by breaking time-reversal symmetry. These materials share three common features: a centrosymmetric lattice, a collinear FM ordering, and a large AHE observed when the field is parallel to the magnetic easy-axis. Here, we present CeAlSi as a new type of FM-WSM, where the Weyl nodes are stabilized by breaking inversion symmetry, but their positions are tuned by breaking time-reversal symmetry. Unlike the other FM-WSMs, CeAlSi has a noncentrosymmetric lattice, a noncollinear FM ordering, and a novel AHE that is anisotropic between the easy- and hard-axes. It also exhibits large FM domains that are promising for both device applications and an interplay between the Weyl nodes and FM domain walls.

cond-mat.mtrl-sci↗

arXiv2020

Incommensurate magnetism mediated by Weyl fermions in NdAlSi

Emergent relativistic quasiparticles in Weyl semimetals are the source of exotic electronic properties such as surface Fermi arcs, the anomalous Hall effect, and negative magnetoresistance, all observed in real materials. Whereas these phenomena highlight the effect of Weyl fermions on the electronic transport properties, less is known about what collective phenomena they may support. Here, we report a new Weyl semimetal, NdAlSi that offers an example. Using neutron diffraction, we report a long-wavelength magnetic order in NdAlSi whose periodicity is linked to the nesting vector between two topologically non-trivial Fermi pockets, which we characterize using density functional theory and quantum oscillation measurements. Our work provides a rare example of Weyl fermions driving collective magnetism.

cond-mat.str-el↗

arXiv2017

Screened moments in a Kondo insulator

Long known to have thermodynamic properties at odds with its insulating electrical transport, SmB6 has been the subject of great debate as it is unclear whether its unusual properties are related to the bulk or novel metallic surface states. We have observed a bulk moment-screening effect in nominally pure and Gd-doped SmB6 via heat capacity, magnetization, and resistivity measurements, and show this new Kondo-impurity like effect provides an unexpected but intuitive explanation for metal-like phenomena stemming from the strongly interacting host system. This affords a coherent understanding for decades of mysteries in strongly-correlated insulators, reveals the expanded utility of techniques previously only utilized for metals, and presents the novel effect of even highly-dilute impurities in strongly correlated insulators.

cond-mat.str-el↗

arXiv2017

Multi-Q mesoscale magnetism in CeAuSb$_2$

We report the discovery of a field driven transition from a striped to woven Spin Density Wave (SDW) in the tetragonal heavy fermion compound CeAuSb$_2$. Polarized along $\bf c$, the sinusoidal SDW amplitude is 1.8(2) $μ_B$/Ce for $T \ll T_N$=6.25(10) K with wavevector ${\bf q}_{1}=( η, η, \frac{1}{2} )$ ($η=0.136(2)$). For ${\bf H}\parallel{\bf c}$, harmonics appearing at $2{\bf q}_{1}$ evidence a striped magnetic texture below $μ_\circ H_{c1}=2.78(1)$ T. Above $H_{c1}$, these are replaced by woven harmonics at ${\bf q}_{1}+{\bf q}_2=(2η, 0, 0)+{\bf c}^*$ until $μ_\circ H_{c2}=5.42(5)$ T, where satellites vanish and magnetization non-linearly approaches saturation at 1.64(2) $μ_B$/Ce for $μ_\circ H\approx 7$ T.

cond-mat.str-el↗

arXiv2016

Static and dynamic XY-like short-range order in a frustrated magnet with exchange disorder

A single crystal of the Co2+ based pyrochlore NaCaCo2F7 was studied by inelastic neutron scattering. This frustrated magnet with quenched exchange disorder remains in a strongly correlated paramagnetic state down to one 60th of the Curie-Weiss temperature. Below T_f = 2.4 K, diffuse elastic scattering develops and comprises 30 +/- 10% of the total magnetic scattering, as expected for J_{eff} = 1/2 moments frozen on a time scale that exceeds \hbar/δE=3.8 ps. The diffuse scattering is consistent with short range XY antiferromagnetism with a correlation length of 16 Å. The momentum (Q) dependence of the inelastic intensity indicates relaxing XY-like antiferromagnetic clusters at energies below ~ 5.5 meV, and collinear antiferromagnetic fluctuations above this energy. The relevant XY configurations form a continuous manifold of symmetry-related states. Contrary to well-known models that produce this continuous manifold, order-by-disorder does not select an ordered state in NaCaCo2F7 despite evidence for weak (~12 %) exchange disorder. Instead, NaCaCo2F7 freezes into short range ordered clusters that span this manifold.

cond-mat.str-el↗

arXiv2005

Quasiparticle breakdown in a quantum spin liquid

Much of modern condensed matter physics is understood in terms of elementary excitations, or quasiparticles - fundamental quanta of energy and momentum. Various strongly-interacting atomic systems are successfully treated as a collection of quasiparticles with weak or no interactions. However, there are interesting limitations to this description: the very existence of quasiparticles cannot be taken for granted in some systems. Like unstable elementary particles, quasiparticles cannot survive beyond a threshold where certain decay channels become allowed by conservation laws - their spectrum terminates at this threshold. This regime of quasiparticle failure was first predicted for an exotic state of matter, super-fluid helium-4 at temperatures close to absolute zero - a quantum Bose-liquid where zero-point atomic motion precludes crystallization. Using neutron scattering, here we show that it can also occur in a quantum magnet and, by implication, in other systems with Bose-quasiparticles. We have measured spin excitations in a two dimensional (2D) quantum-magnet, piperazinium hexachlorodicuprate (PHCC) in which spin-1/2 copper ions form a non-magnetic quantum spin liquid (QSL), and find remarkable similarities with excitations measured in superfluid 4He. There is a threshold momentum beyond which the quasiparticle peak merges with the two-quasiparticle continuum. It then acquires a finite energy width and becomes indistinguishable from a leading-edge singularity, so that lowest excited states occupy a wide band of energy. Our findings have important ramifications for understanding phenomena involving excitations with gapped spectra in many condensed matter systems, including high-transition-temperature superconductors.

cond-mat.str-el↗