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A. M. Strydom

Publications and source records attributed to A. M. Strydom.

At least 19 recordsLinked to original sources

Magnetism and spin dynamics of Na$_5$Yb(MoO$_4$)$_4$: A weakly interacting rare-earth stretched diamond lattice

We report a comprehensive investigation of the structural and magnetic properties of Na$_5$Yb(MoO$_4$)$_4$, a member of the stretched diamond magnetic lattice family. Neutron powder diffraction at 3.3~K confirms that the compound crystallizes in the tetragonal \textit{I4$_1$/a} space group, with a large interatomic separation of 6.33~Å between magnetic Yb ions forming a three-dimensional stretched diamond framework. Magnetic susceptibility and specific heat measurements reveal no evidence of long-range magnetic order down to 60~mK. The low-temperature magnetic behavior is governed by an effective $J_{\mathrm{eff}} = 1/2$ Kramers doublet ground state, well separated from excited crystal-field levels, arising from the distorted dodecahedral oxygen coordination of Yb$^{3+}$. Density functional theory calculations within the DFT+$U$ framework indicate that exchange interactions between Yb ions are negligibly small, consistent with the long O--Mo--O super-superexchange pathways. The temperature dependence of the specific heat exhibits signatures of gapped spin excitations, most likely originating from long-range dipolar correlations and further shaped by weak exchange interactions together with the strong single-ion anisotropy of the Yb moments. Muon spin relaxation measurements reveal persistent low-energy spin dynamics, indicating that dipolar correlations remain dynamic and are insufficient to stabilize static magnetic order down to 50~mK. These results identify Na$_5$Yb(MoO$_4$)$_4$ as a rare example of a dipolar quantum paramagnet in which single-ion physics and long-range dipolar interactions dominate, while exchange interactions are suppressed to the millikelvin energy scale.

cond-mat.str-el

Microscopic origin of hard-plane antiferromagnetism in the Kondo lattice Ce2Rh3Ge5

Hard plane antiferromagnetic order where ordered moments lie perpendicular to the single-ion crystal electric field easy axis is rare in Ce-based Kondo lattices and is a subject of active interest. Here we show that Ce$_2$Rh$_3$Ge$_5$ realizes a hard-plane antiferromagnetic state in which partial delocalization of the local moment gives rise to an RKKY exchange that overturns the single-ion easy-axis preference. Neutron diffraction reveals moments in the $ab$ plane, while inelastic neutron scattering and susceptibility establish a magnetic easy axis along $c$ in the paramagnetic regime, highlighting a clear inversion between single-ion and ordered-state anisotropies. In this work, we establish a unified microscopic framework to consistently account for partial $4f$-moment delocalization, enhanced in-plane RKKY exchange, and the resulting hard-plane antiferromagnetic order. Ce$_2$Rh$_3$Ge$_5$ thus provides a benchmark system in which single-ion anisotropy, Kondo screening, and RKKY exchange compete on comparable energy scales, revealing a cooperative route to hard-axis ordering in strongly hybridized Kondo lattices.

cond-mat.str-el

Emergent Topological Semimetal

A material's electronic topology, which is generally described via its Bloch states and the associated bandstructure, will be enriched by the presence of interactions. In metallic settings, the interactions are usually treated through the concept of quasiparticles. Using the genuinely quantum critical heavy fermion compound CeRu$_4$Sn$_6$, we investigate what happens if no well-defined quasiparticles are present. Surprisingly, we discover a topological semimetal phase that emerges from the material's quantum critical state and exhibits a dome structure as a function of magnetic field and pressure. To understand these results, we study a Weyl-Kondo semimetal model at a Kondo destruction quantum critical point. Indeed, it exhibits features in the spectral function that can define topological crossings beyond the quasiparticle picture. We expect our work to stimulate the search for other emergent topological phases.

cond-mat.str-el

Magnetic properties and spin dynamics in a spin-orbit driven Jeff= 1/2 triangular lattice antiferromagnet

Frustration-induced strong quantum fluctuations accompanied by spin-orbit coupling and crystal electric field can give rise to rich and diverse magnetic phenomena associated with unconventional low-energy excitations in rare-earth based quantum magnets. Herein, we present crystal structure, magnetic susceptibility, specific heat, muon spin relaxation(muSR), and electron spin resonance (ESR) studies on the polycrystalline samples of Ba6Yb2Ti4O17 in which Yb3+ ions constitute a perfect triangular lattice in ab-plane without detectable anti-site disorder between atomic sites. The Curie-Weiss fit of low-temperature magnetic susceptibility data suggest the spin-orbit entangled Jeff = 1/2 degrees of freedom of Yb3+ spin with weak antiferromagnetic exchange interactions in the Kramers doublet ground state. The zero-field specific heat data reveal the presence of long-range magnetic order at TN = 77 mK which is suppressed in a magnetic field 1 T. The broad maximum in specific heat is attributed to the Schottky anomaly implying the Zeeman splitting of the Kramers doublet ground state. The ESR measurements suggest the presence of anisotropic exchange interaction between the moments of Yb3+ spins and the well separated Kramers doublet state. muSR experiments reveal a fluctuating state of Yb3+ spins in the temperature range 0.1 K-100 K owing to depopulation of crystal electric field levels, which suggests that the Kramers doublets are well separated consistent with thermodynamic and ESR results. In addition to the intraplane nearest-neighbor superexchange interaction, the interplane exchange interaction and anisotropy are expected to stabilize the long-range ordered state in this triangular lattice antiferromagnet.

cond-mat.str-el

Quantum Griffiths singularity in the stoichiometric heavy-fermion system CeRh$_4$Al$_{15}$

We present a detailed investigation of the stoichiometric CeRh$_4$Al$_{15}$ single crystal compound using the temperature dependence of the heat capacity [$C_{\text{P}}$($T$)], electrical resistivity [$ρ$($T$)], magnetic susceptibility [$χ$($T$)], and magnetization [$M$($H$)] measurements for a magnetic field ($H$) applied in the basal plane and along the $c$-axis. The low temperature power-law behavior of $C$/$T$ $\propto$ $χ$ $\propto$ $T^{-1+α}$, the isotherm magnetization, $M \sim H^α$ with the exponent $α$ = 0.45 - 0.55, and the $T$-linear resistivity $Δρ$ $\sim$ $T^ε$ with $ε\sim$ 1 are found to be consistent with the formation of quantum Griffiths singularities in the non-Fermi-liquid (NFL) regime. We further investigated the spin dynamics of a polycrystalline sample of CeRh$_4$Al$_{15}$, using zero-field (ZF) and longitudinal-field (LF) muon spin relaxation ($μ$SR) measurements. ZF-$μ$SR measurements do not reveal any sign of long-range magnetic ordering down to 70~mK. The electronic relaxation rate ($λ$) below 0.5~K increases rapidly and shows a thermal activation-like characteristic [$T$log($λ$)$\sim$ $T$] over the entire measured temperature range between 70~mK to 4~K, indicating the presence of low energy spin fluctuations in CeRh$_4$Al$_{15}$. LF-$μ$SR measurements show a time-field ($t/H^η$) scaling of the $μ$SR asymmetry indicating a quantum critical behavior of this compound. Furthermore, inelastic neutron scattering study on the polycrystalline sample reveals two crystal field excitations near 19 and 33~meV. These features collectively provide strong evidence of NFL behavior in CeRh$_4$Al$_{15}$ due to the formation of Griffiths phase close to a $T$ $\rightarrow$ 0~K quantum critical point.

cond-mat.str-el

Quantum critical spin-liquid-like behavior in S = 1/2 quasikagome lattice CeRh1-xPdxSn investigated using muon spin relaxation and neutron scattering

We present the results of muon spin relaxation ($μ$SR) and neutron scattering on the Ce-based quasikagome lattice CeRh$_{1-x}$Pd$_{x}$Sn ($x=0.1$ to 0.75). Our ZF-$μ$SR results reveal the absence of static long-range magnetic order down to 0.05~K in $x = 0.1$ single crystals. The weak temperature-dependent plateaus of the dynamic spin fluctuations below 0.2~K in ZF-$μ$SR together with its longitudinal-field (LF) dependence between 0 and 3~kG indicate the presence of dynamic spin fluctuations persisting even at $T$ = 0.05~K without static magnetic order. On the other hand, $C_{\text{4f}}$/$T$ increases as --log $T$ on cooling below 0.9~K, passes through a broad maximum at 0.13~K and slightly decreases on further cooling. The ac-susceptibility also exhibits a frequency independent broad peak at 0.16~K, which is prominent with an applied field $H$ along $c$-direction. We, therefore, argue that such a behavior for $x=0.1$ (namely, a plateau in spin relaxation rate ($λ$) below 0.2~K and a linear $T$ dependence in $C_{\text{4f}}$ below 0.13~K) can be attributed to a metallic spin-liquid (SL) ground state near the quantum critical point in the frustrated Kondo lattice. The LF-$μ$SR study suggests that the out of kagome plane spin fluctuations are responsible for the SL behavior. Low energy inelastic neutron scattering (INS) of $x$ = 0.1 reveals gapless magnetic excitations, which are also supported by the behavior of $C_{\text{4f}}$ proportional to $T^{1.1}$ down to 0.06~K.

cond-mat.str-el

Structural 130-K Phase Transition and Emergence of a Two-Ion Kondo State in HT-Ce$_2$Rh$_2$Ga Explored by $^{69,71}$Ga Nuclear Quadrupole Resonance

We have studied the microscopic magnetic properties, the nature of the 130-K phase transition, and the ground state in the recently synthesized compound Ce$_2$Rh$_2$Ga by use of $^{69,71}$Ga nuclear quadrupole resonance (NQR). The NQR spectra clearly show an unusual phase transition at $T_t$ $\sim$ 130 K yielding a splitting of the high-temperature single NQR line into two clearly resolved NQR lines, providing evidence for two crystallographically inequivalent Ga sites. The NQR frequencies are in good agreement with fully-relativistic calculations of the band structure. Our NQR results indicate the absence of magnetic or charge order down to 0.3 K. The temperature dependence of the spin-lattice relaxation rate, 1/$T_1$, shows three distinct regimes, with onset temperatures at $T_t$ and 2 K. The temperature-independent 1/$T_1$, observed between $T_t$ and 2 K, crosses over to a Korringa process, 1/$T_1$ $\propto$ $T$, below $\sim$ 2 K, which evidences a rare two-ion Kondo scenario: the system goes into a dense Kondo coherent state at 2.0 and 0.8 K for the two different Ga sites.

cond-mat.str-el

Spin liquid state in a rare-earth hyperkagome lattice

Quantum fluctuations enhanced by frustration and subtle interplay between competing degrees of freedom offer an ideal ground to realize novel states with fractional quantum numbers in quantum materials that defy standard theoretical paradigms. Quantum spin liquid (QSL) is a highly entangled state wherein frustration induced strong quantum fluctuations preclude symmetry breaking phase transitions down to zero temperature without any order parameter. Experimental realizations of QSL in quantum materials with spin dimensionality greater than one is very rare. Here, we present our thermodynamic, nuclear magnetic resonance, muon spin relaxation and inelastic neutron scattering studies of a new rare-earth hyperkagome compound Li3Yb3Te2O12 in which Yb3+ ions constitute a three dimensional spin-lattice without any detectable disorder. Our comprehensive experiments evince neither signature of magnetic ordering nor spin freezing down to 38 mK that suggest the realization of dynamic liquid-like ground state in this antiferromagnet. The ground state of this material is interpreted by a low energy Jeff = 1/2 degrees of freedom with short range spin correlations. The present results demonstrate a viable basis to explore spin-orbit driven enigmatic correlated quantum states in a new class of rare-earth based three dimensional frustrated magnets that may open new avenues in theoretical and experimental search for spin liquids.

cond-mat.str-el

Signature of a randomness-driven spin-liquid state in a frustrated magnet

Collective behaviour of electrons, frustration induced quantum fluctuations and entanglement in quantum materials underlie some of the emergent quantum phenomena with exotic quasi-particle excitations that are highly relevant for technological applications. Herein, we present our thermodynamic and muon spin relaxation measurements, complemented by ab initio density functional theory and exact diagonalization results, on the recently synthesized frustrated antiferromagnet Li4CuTeO6, in which Cu2+ ions (S = 1/2) constitute disordered spin chains and ladders along the crystallographic [101] direction with weak random inter-chain couplings. Our thermodynamic experiments detect neither long-range magnetic ordering nor spin freezing down to 45 mK despite the presence of strong antiferromagnetic interaction between Cu2+ moments leading to a large effective Curie-Weiss temperature of -154 K. Muon spin relaxation results are consistent with thermodynamic results. The temperature and magnetic field scaling of magnetization and specific heat reveal a data collapse pointing towards the presence of random-singlets within a disorder-driven correlated and dynamic ground-state in this frustrated antiferromagnet.

cond-mat.str-el

Crystal Electic Field and Possible Coupling with Phonon in Kondo lattice CeCuGa3

We investigate the magnetic and crystal electric field (CEF) states of the Kondo lattice system CeCuGa3 by muon spin relaxation (muSR), neutron diffraction, and inelastic neutron scattering (INS) measurements. A noncentrosymmetric BaNiSn3-type tetragonal crystal structure (space group I4mm) is inferred from x-ray as well as from neutron powder diffraction. The low-temperature magnetic susceptibility and heat capacity data show an anomaly near 2.3 - 2.5~K associated with long range magnetic ordering, which is further confirmed by muSR and neutron diffraction data. The neutron powder diffraction collected at 1.7 K shows the presence of magnetic Bragg peaks indexed by an incommensurate magnetic propagation vector k = (0.148, 0.148, 0) and the magnetic structure is best described by a longitudinal spin density wave with ordered moments lying in ab-plane. An analysis of the INS data based on a CEF model reveals the presence of two magnetic excitations near 4.5 meV and 6.9 meV. The magnetic heat capacity data suggest an overall CEF splitting of 20.7 meV, however the excitation between 20 and 30 meV is very broad and weak in our INS data, but could provide an evidence of CEF level in this energy range in agreement with the magnetic entropy. Our analysis of INS data based on the CEF-phonon model indicates that the two excitations at 4.5 meV and 6.9 meV have their origin in CEF-phonon coupling (i.e. splitting of one CEF peak into two peaks, called vibron), with an overall splitting of 28.16 meV, similar to the case of CeCuAl3 and CeAuAl3.

cond-mat.str-el

Antiferromagnetic correlations in strongly valence fluctuating CeIrSn

CeIrSn with a quasikagome Ce lattice in the hexagonal basal plane is a strongly valence fluctuating compound, as we confirm by hard x-ray photoelectron spectroscopy and inelastic neutron scattering, with a high Kondo temperature of $T_{\mathrm{K}}\sim 480$\,K. We report a negative in-plane thermal expansion $α/T$ below 2\,K, which passes through a broad minimum near 0.75\,K. Volume and $a$-axis magnetostriction for $B \parallel a$ are markedly negative at low fields and change sign before a sharp metamagnetic anomaly at 6\,T. These behaviors are unexpected for Ce-based intermediate valence systems, which should feature positive expansivity. Rather they point towards antiferromagnetic correlations at very low temperatures. This is supported by muon spin relaxation measurements down to 0.1\,K, which provide microscopic evidence for a broad distribution of internal magnetic fields. Comparison with isostructural CeRhSn suggests that these antiferromagnetic correlations emerging at $T\ll T_{\mathrm{K}}$ result from geometrical frustration.

cond-mat.str-el

Dynamic Spin Fluctuations in the Frustrated Spin Chain Compound Li$_3$Cu$_2$SbO$_6$

We report the signatures of dynamic spin fluctuations in the layered honeycomb Li$_3$Cu$_2$SbO$_6$ compound, with a 3$d$ S = 1/2 $d^9$ Cu$^{2+}$ configuration, through muon spin rotation and relaxation ($μ$SR) and neutron scattering studies. Our zero-field (ZF) and longitudinal-field (LF)-$μ$SR results demonstrate the slowing down of the Cu$^{2+}$ spin fluctuations below 4.0 K. The saturation of the ZF relaxation rate at low temperature, together with its weak dependence on the longitudinal field between 0 and 3.2 kG, indicates the presence of dynamic spin fluctuations persisting even at 80 mK without static order. Neutron scattering study reveals the gaped magnetic excitations with three modes at 7.7, 13.5 and 33 meV. Our DFT calculations reveal that the next nearest neighbors (NNN) AFM exchange ($J_{AFM}$ = 31 meV) is stronger than the NN FM exchange ($J_{FM}$ = -21 meV) indicating the importance of the orbital degrees of freedom. Our results suggest that the physics of Li$_3$Cu$_2$SbO$_6$ can be explained by an alternating AFM chain rather than the honeycomb lattice.

cond-mat.str-el

Quantum Fluctuations in the Non-Fermi Liquid System CeCo$_{2}$Ga$_{8}$ Investigated Using $μ$SR

Reduced dimensionality offers a crucial information in deciding the type of the quantum ground state in heavy fermion materials. Here we have examined stoichiometric CeCo$_{2}$Ga$_{8}$ compound, which crystallizes in a quasi-one-dimensional crystal structure with Ga-Ce-Co chains along the $c$-axis. The low-temperature behavior of magnetic susceptibility ($χ\sim-\ln T$), heat capacity ($C_p/T\sim-\ln T$), and resistivity ($ρ\sim T^{n}$) firmly confirm the non-Fermi liquid ground state of CeCo$_{2}$Ga$_{8}$. We studied the low-energy spin dynamics of CeCo$_{2}$Ga$_{8}$ compound utilizing zero field (ZF-) and longitudinal field (LF-) muon spin relaxation ($μ$SR) measurements. ZF-$μ$SR measurement reveals the absence of long-range magnetic ordering down to 70 mK, and interestingly below 1 K, the electronic relaxation rate sharply rises, intimating the appearance of low energy quantum spin fluctuations in CeCo$_{2}$Ga$_{8}$.

cond-mat.str-el

Anisotropic field-induced ordering in the triangular-lattice quantum spin liquid NaYbSe$_2$

High-quality single crystals of NaYbSe$_2$, which resembles a perfect triangular-lattice antiferromagnet without the intrinsic disorder, are investigated by magnetization and specific heat, as well as the local probe techniques nuclear magnetic resonance (NMR) and electron spin resonance (ESR). The low-field measurements confirm the absence of any spin freezing or long-range magnetic order down to 50~mK, which suggests a quantum spin liquid ground (QSL) state with gapless excitations. The instability of the QSL state is observed upon applying magnetic fields. For the $H\bot c$ direction, a field-induced magnetic phase transition is observed above 2~T from the $C_{\rm p}(T)$ data, agreeing with a clear $\frac{M_s}{3}$ plateau of $M(H)$, which is associated with an up-up-down (uud) spin arrangement. For the $H\|c$ direction, a field-induced transition could be evidenced at a much higher field range (9 - 21~T). The $^{23}$Na NMR measurements provide microscopic evidence for field-induced ordering for both directions. A reentrant behavior of $T_{\rm N}$, originating from the thermal and quantum spin fluctuations, is observed for both directions. The anisotropic exchange interactions $J_{\perp}\simeq$ 4.7~K and $J_z\simeq$2.33~K are extracted from the modified bond-dependent XXZ model for the spin-$\frac{1}{2}$ triangular-lattice antiferromagnet. The absence of magnetic long-range order at zero fields is assigned to the effect of strong bond-frustration, arising from the complex spin-orbit entangled $4f$ ground state. Finally, we derive the highly anisotropic magnetic phase diagram, which is discussed in comparison with the existing theoretical models for spin-$\frac{1}{2}$ triangular-lattice antiferromagnets.

cond-mat.str-el

Signatures of low-dimensional magnetism and short-range magnetic order in Co-based trirutiles

Features of low dimensional magnetism resulting from a square-net arrangement of Co atoms in trirutile CoTa$_2$O$_6$ is studied in the present work by means of density functional theory and is compared with the experimental results of specific heat and neutron diffraction. The small total energy differences between the ferromagnetic (FM) and antiferromagnetic (AFM) configuration of CoTa$_2$O$_6$ shows that competing magnetic ground states exist, with the possibility of transition from FM to AFM phase at low temperature. Our calculation further suggests the semi-conducting behavior for CoTa$_2$O$_6$ with a band gap of $\sim$0.41 eV. The calculated magnetic anisotropy energy is $\sim$2.5 meV with its easy axis along the [100] (in-plane) direction. Studying the evolution of magnetism in Co$_{1-x}$Mg$_x$Ta$_2$O$_6$ (x = 0, 0.1, 0.3, 0.5, 0.7 and 1). it is found that the sharp AFM transition exhibited by CoTa$_2$O$_6$ at $T_N$ = 6.2 K in its heat capacity vanishes with Mg-dilution, indicating the obvious effect of weakening the superexchange pathways of Co. The current specific heat study reveals the robust nature of $T_N$ for CoTa$_2$O$_6$ in applied magnetic fields. Clear indication of short-range magnetism is obtained from the magnetic entropy, however, diffuse components are absent in neutron diffraction data. At $T_N$, CoTa$_2$O$_6$ enters a long-range ordered magnetic state which can be described using a propagation vector, (1/4, 1/4, 0). Upon Mg-dilution at $x \geq$0.1, the long-range ordered magnetism is destroyed. The present results should motivate an investigation of magnetic excitations in this low-dimensional anisotropic magnet.

cond-mat.str-el

Sequential localization of a complex electron fluid

Complex and correlated quantum systems with promise for new functionality often involve entwined electronic degrees of freedom. In such materials, highly unusual properties emerge and could be the result of electron localization. Here, a cubic heavy fermion metal governed by spins and orbitals is chosen as a model system for this physics. Its properties are found to originate from surprisingly simple low-energy behavior, with two distinct localization transitions driven by a single degree of freedom at a time. This result is unexpected, but we are able to understand it by advancing the notion of sequential destruction of an SU(4) spin-orbital-coupled Kondo entanglement. Our results implicate electron localization as a unified framework for strongly correlated materials and suggest ways to exploit multiple degrees of freedom for quantum engineering.

cond-mat.str-el

Unconventional superconductivity in the cage type compound Sc$_5$Rh$_6$Sn$_{18}$

We have examined the superconducting ground state properties of the caged type compound Sc$_5$Rh$_6$Sn$_{18}$ using magnetization, heat capacity, and muon-spin relaxation or rotation ($μ$SR) measurements. Magnetization measurements indicate type-II superconductivity with an upper critical field $μ_0H_{c2}(0)$ = 7.24 T. The zero-field cooled and field cooled susceptibility measurements unveil an onset of diamagnetic signal below $T_{\bf c}$ = 4.4 K. The interpretation of the heat capacity results below $T_{\bf c}$ using the $α-$BCS model unveils the value of $α$ = 2.65, which gives the dimensionless ratio 2$Δ(0)/k_B T_{\bf c}$ = 5.3, intimating that Sc$_5$Rh$_6$Sn$_{18}$ is a strong-coupling BCS superconductor. The zero-field $μ$SR measurements in the longitudinal geometry exhibit a signature of a spontaneous appearance of the internal magnetic field below the superconducting transition temperature, indicating that the superconducting state is characterized by the broken time-reversal symmetry (TRS). We have compared the results of broken TRS in Sc$_5$Rh$_6$Sn$_{18}$ with that observed in R$_5$Rh$_6$Sn$_{18}$ (R = Lu and Y).

cond-mat.supr-con

In-depth study of the $H -T$ phase diagram of Sr4Ru3O10 by magnetization experiments

We present magnetization measurements on Sr4Ru3O10 as a function of temperature and magnetic field applied perpendicular to the magnetic easy $c$-axis inside the ferromagnetic phase. Peculiar metamagnetism evolves in Sr4Ru3O10 below the ferromagnetic transition $T_{C}$ as a double step in the magnetization at two critical fields $H_{c1}$ and $H_{c2}$. We map the $H-T$ phase diagram with special focus on the temperature range 50\,K $\le T \le T_{C}$. We find that the critical field $H_{c1}(T)$ connects the field and temperature axes of the phase diagram, whereas the $H_{c2}$ boundary starts at 2.8\,T for the lowest temperatures and ends in a critical endpoint at (1\,T; 80\,K). We conclude from the temperature dependence of the ratio $\frac{Hc1}{Hc2}(T)$ that the double metamagnetic transition is an intrinisc effect of the material and it is not caused by sample stacking faults such as twinning or partial in-plane rotation between layers.

cond-mat.str-el