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T. J. Hicken

Publications and source records attributed to T. J. Hicken.

At least 19 recordsLinked to original sources

Local magnetic properties of the rare-earth intermetallics $R$Mn$_2$Ge$_2$ ($R$=Ce, Pr, Nd)

We present an investigation of the rare-earth intermetallic materials, $R$Mn$_2$Ge$_2$ ($R$=Ce, Pr, Nd), reported to host a lattice of skyrmionic bubbles at room temperature. The magnetism of all three materials is characterised by the onset of local fluctuations as the magnetic state changes from a conical magnetic structure to a collinear antiferromagnetic one as temperature $T$ is increased. In this $T$ regime, where skyrmion-bubble textures have been reported, we see dynamics similar to those observed in other skyrmion-hosting materials. The level of disorder above this transition increases across the series from $R$=Ce to Nd. At low temperatures the magnetism is affected by the ordering of the rare-earth ions, resulting in distinct behaviour for the different members of the series.

cond-mat.str-el

Competing Ordering Modes in the Distorted Quantum Kagome Material Clinoatacamite Cu$_2$Cl(OH)$_3$

We have studied the magnetic properties of clinoatacamite Cu$_2$Cl(OH)$_3$, the parent compound of the quantum spin liquid candidate herbertsmithite and a longstanding puzzle among frustrated quantum magnets. As we reveal using density-functional theory, clinoatacamite belongs to the class of distorted kagome antiferromagnets with the kagome plane being embedded into a low-symmetry crystal structure. By means of thermodynamic measurements, muon spin rotation/relaxation as well as neutron diffraction on single crystals, we find in zero magnetic field complex behavior below $T_\mathrm{I}$ = 18.1 K which unfolds in three temperature regions I-III. We propose this complexity in multicritical clinoatacamite to arise from the competition of antiferromagnetic ordering modes from the underconstrained manifold of modes, which can lead to a metamagnetic texture in zero field.

cond-mat.str-el

Correlated charge order intertwined with time-reversal symmetry-breaking nodal superconductivity in the dual flat band kagome superconductor CeRu$_{3}$Si$_{2}$

Kagome materials provide a powerful platform for exploring how flat electronic bands promote symmetry-breaking quantum states, yet studies have so far focused mainly on kagome-derived $d$-electron flat bands. In this paper, we introduce CeRu$_{3}$Si$_{2}$, a kagome superconductor in which our first-principles calculations show the coexistence of Ru $d$-orbital kagome flat bands and heavy-fermion flat bands derived from Ce$^{4+}$ $4f$-states. X-ray diffraction reveals a dominant 1/2 charge order with a much weaker 1/3 component persisting up to room temperature. Theoretical calculations further highlight the correlated nature of these charge-order states. Deep within the charge-ordered state, magnetoresistance emerges below 80 K and strengthens further below 30 K. Zero-field muon spin-rotation measurements show no time-reversal symmetry (TRS) breaking in the normal state, in contrast to LaRu$_{3}$Si$_{2}$ and YRu$_{3}$Si$_{2}$. However, an applied magnetic field induces weak magnetism. Across the $A$Ru$_{3}$Si$_{2}$ family ($A$ = La, Y, and Ce), the superconducting transition temperature $T_{\rm c}$ scales linearly with the onset temperature of normal-state TRS breaking $T_{\rm {TRSB}}$ and the magnitude of the field-induced magnetic response, revealing a direct positive correlation between normal-state symmetry breaking and superconductivity. Furthermore, we identify that CeRu$_{3}$Si$_{2}$ is the first 132-type kagome compound to host nodal superconductivity together with spontaneous internal magnetic fields, providing clear evidence for intrinsic TRS breaking in the superconducting state. These results establish CeRu$_{3}$Si$_{2}$ as a unique platform where intertwined kagome $d$- and heavy fermion $f$-electron flat bands generate a rich hierarchy of electronic orders.

cond-mat.supr-con

Unified pressure and field response across distinct charge-order regimes in Ti-doped CsV$_3$Sb$_5$

Understanding the phase diagram of kagome superconductors from a microscopic perspective is crucial for clarifying the interplay between charge order and superconductivity. Ti-doped CsV$_{3}$Sb$_{5}$ exhibits a nonmonotonic temperature-doping phase diagram in which both $T_{\rm c}$ and the charge-order temperature initially decrease with doping, followed by a crossover from long-range to short-range charge order and a subsequent increase in $T_{\rm c}$. Here, we report a muon spin rotation ($μ$SR) study of Ti-doped CsV$_{3}$Sb$_{5}$ at two representative compositions: underdoped (Ti$_{0.05}$-CVS) and optimally doped (Ti$_{0.22}$-CVS). Using zero-field, high-field, and high-pressure $μ$SR, we find spontaneous time-reversal-symmetry (TRS) breaking in the normal state of both compositions, strongly enhanced by an applied magnetic field and associated with long-range and short-range charge-order correlations, respectively. In the superconducting state, both samples exhibit anisotropic nodeless pairing with low superfluid density. Hydrostatic pressure substantially enhances both $T_{\rm c}$ and the superfluid density (by $\sim$2.5), revealing a linear correlation between them and pointing to unconventional pairing. Above $\sim$1 GPa, a crossover from anisotropic to isotropic nodeless pairing is observed. Despite the different nature of charge order in the two doping regimes, the superconducting responses are remarkably similar, suggesting that the competition between superconductivity and charge order occurs on a local scale, largely independent of the long-range coherence of the charge-ordered state.

cond-mat.supr-con

Crystal electric field excitations and spin dynamics in a spin-orbit coupled distorted honeycomb magnet BiErGeO$_5$

The magnetic properties and crystal electric field (CEF) scheme of BiErGeO$_5$ are investigated via magnetization, heat capacity, muon spin relaxation (muSR), and inelastic neutron scattering (INS) experiments on a polycrystalline sample. The Er$^{3+}$ ions form a quasi-two-dimensional distorted honeycomb network with a Kramers doublet ground state. Magnetic susceptibility and heat capacity reveal short-range antiferromagnetic correlations, manifested as a broad maximum around 1.4 K. Heat-capacity data further confirm the onset of a magnetic long-range order at $T_ N = 0.4$ K. The INS spectra exhibit eight CEF excitations and the CEF analysis yields the $g$-factor anisotropy with $g_{xy}/g_{z} = 1.38$ and exchange anisotropy with $J_{xy} = 2.96$ K and $J_{z} = 1.56$ K. The experimental temperature and field dependent magnetization and heat capacity are also reproduced by the simulation using CEF energy scheme. Zero-field muSR measurements down to 30 mK, do not exhibit coherent oscillations or a static 1/3 tail. The spectra are well described by two exponential relaxation components, indicating two magnetically inequivalent muon environments. The relaxation rates display a nearly temperature-independent plateau below $T_{\rm N}$ and follow an Orbach-type activated behavior at higher temperatures involving excited CEF levels, consistent with the INS results. Longitudinal-field $μ$SR measurements reveal only weak decoupling up to 1.5 T, indicating persistent slow spin fluctuations below $T_{\rm N}$.

cond-mat.mtrl-sci

Inhomogeneous dynamic state in the double trillium lattice antiferromagnet KBaFe$_2$(PO$_4$)$_3$

The three-dimensional (3D) magnet KBaFe$_2$(PO$_4$)$_3$ hosts a double-trillium lattice of Fe$^{3+}$ (spin, $S=5/2$) ions offering a prototypical platform to study the frustration induced effects in 3D. Through magnetization, specific heat, $^{31}$P nuclear magnetic resonance (NMR), and muon spin relaxation ($μ$SR) experiments, supported by first principles calculations, we uncover an unconventional ground state. Despite strong antiferromagnetic interactions with a large Curie-Weiss temperature $θ_{\rm CW} = -70(2)$ K, no magnetic long-range order is observed down to 30 mK. Below $T^{\ast}\simeq 3.5$ K, the NMR linewidth becomes nearly field-independent and the spin-spin relaxation rate $1/T_2$ saturates, accompanied by an inhomogeneous distribution of transverse nuclear magnetization $M_{xy}$. The latter indicates the emergence of short-range dynamical correlations, which was further corroborated by a robust and field-insensitive broad maximum in specific heat. In $μ$SR, we detect neither a static internal field nor spin freezing; instead the relaxation remains dynamic and is best described by two coexisting dynamic relaxation channels: a dominant fast (sporadic) channel and a slower Markovian component. Their differing weights and fluctuation rates suggest microscopic inhomogeneity in spin dynamics. Altogether, KBaFe$_2$(PO$_4$)$_3$ exemplifies a rare high-spin stochiometric 3D antiferromagnet that evades ordering and instead fosters a mosaic of spin dynamics driven by strong geometric frustration intrinsic to the trillium lattice.

cond-mat.mtrl-sci

Intrinsic disorder in the candidate quantum spin ice Pr$_2$Zr$_2$O$_7$

Quantum spin liquids with long-range entanglement are of great interest for applications in quantum technology. The quantum spin ice Pr$_2$Zr$_2$O$_7$ is a promising example, where it is believed that structural disorder plays a key role in enhancing quantum mechanical effects by introducing strains that split the ground state doublet akin to the effect of a local disordered transverse field. However, the precise defect structure responsible for this behaviour is unknown. Here we have determined the intrinsic defect structure of Pr$_2$Zr$_2$O$_7$ using neutron and x-ray scattering techniques supported by density functional theory. We find the main defect is the stuffing of Zr$^{4+}$ sites by Pr$^{3+}$ ions, accompanied by charge compensating O$^{2-}$ vacancies, and the relaxation of a neighbouring O$^{2-}$ ion to an interstitial site. Our results explain the single-ion magnetism by considering the non-magnetic singlets that arise on neighbouring sites as a result of the defect structure. These singlets account for additional features in the crystal electric field excitations. The effects caused by this low level of structural disorder are magnified since several neighbouring Pr sites are affected. This makes a significant contribution towards the observed broadening of pinch points in the magnetic diffuse scattering, which was previously attributed purely to quantum effects.

cond-mat.str-el

Single-ion anisotropy driven chiral magnetic order in a spin-1 antiferromagnetic chain

Chirality in magnetic systems gives rise to a wide range of exotic phenomena, yet its influence in $S=1$ chains remains largely unexplored. Here, we present a comprehensive experimental study of a chiral antiferromagnetic (AFM) $S=1$ chain, [Ni(pym)(H$_{2}$O)$_{4}$]SO$_{4} \cdot$ H$_{2}$O (pym = pyrimidine), where the Ni(II) octahedral orientation exhibits a four-fold chiral periodicity. Muon spin rotation measurements indicate the onset of long-range magnetic order below $T_{\rm N} = 1.82(2)\,\mathrm{K}$. Neutron diffraction measurements reveal a chiral AFM order driven by a chiral modulation of the easy-axis anisotropy direction, rather than the typical scenario of Dzyaloshinskii-Moriya interactions, geometrical frustration or higher-order interactions. Inelastic neutron scattering (INS) measurements reveal dispersive spin-wave excitations well described by linear spin-wave theory, with Hamiltonian parameters $J_{0} = 6.81(1)\,\mathrm{K}$ (intrachain exchange), $J'_{1\rm a} = -0.091(1)\,\mathrm{K}$ (interchain exchange), and $D = -3.02(1)\,\mathrm{K}$ (easy-axis single-ion anisotropy). These parameters are further validated by Monte Carlo simulations of the magnetisation. Additionally, the INS data reveal multiple dispersionless bands, suggesting the presence of further excitations beyond the scope of our linear spin-wave theory.

cond-mat.str-el

Magnetism in $M_{1/3}$NbS$_2$ ($M$ = Fe, V, Mn): insight into intercalated transition-metal dichalcogenides using $μ$SR

We present the results of muon-spin relaxation ($μ$SR) measurements of the static and dynamic magnetism of $M_{1/3}$NbS$_2$ ($M$ = Fe, V, Mn), three intercalated transition-metal dichalcogenides. Transitions to long-range magnetic order are observed in all three materials and local magnetic fields at muon sites are compared to dipole field calculations. Measurements on Fe$_{1/3}$NbS$_2$ capture the evolution of two coexisting magnetic phases. In V$_{1/3}$NbS$_2$ we observe a peak in the dynamic response at $9$ K, coincident with previous reports of a possible low-temperature phase transition. The observation of high-frequency muon precession in Mn$_{1/3}$NbS$_2$ suggests the existence of an additional muon site that implies a difference in electronic energy landscape compared to the other materials in the series. Taken together, this demonstrates that the change in intercalant species drives significant variations in magnetism, highlighting the $M_{1/3}$NbS$_2$ ($M$ = Fe, V, Mn) series as an ideal group of materials for investigating a wide range of magnetic phenomena.

cond-mat.str-el

Local probe evidence supporting altermagnetism in Co$_{1/4}$NbSe$_2$

Muon spin rotation ($μ$SR), combined with muon stopping site and local field analysis, was used to investigate the magnetic properties of cobalt intercalated 2H-NbSe$_2$ (Co$_{1/4}$NbSe$_2$). Co$_{1/4}$NbSe$_2$ is predicted to be an altermagnet, and whilst neutron diffraction has proposed its magnetic structure, microscopic details such as the magnetic volume fraction remain unclear. Therefore, a local probe investigation of its magnetism is essential. Here, we report the determination of the magnetically ordered volume fraction, ordered moment size, and magnetic structure. Our results reveal a sharp second-order transition to a full-volume-fraction, homogeneous magnetic order below $T_\mathrm{N}~=~168~$K. The moments are aligned antiparallel along the $c$-axis, consistent with neutron diffraction and altermagnetism. $μ$SR reveals that the state remains stable under a $c$-axis magnetic field up to $0.78~$T, with magnetisation measurements suggesting this robust regimes extends to at least $5$~T. Within the time resolution of $μ$SR, no precursor slow altermagnetic fluctuations were detected above $T_\mathrm{N}$, which is important for interpreting the band splitting in the paramagnetic state reported by photoemission studies. These findings support altermagnetism in Co$_{1/4}$NbSe$_2$ and motivate further experiments to explore the tunability of its magnetic and electronic structure.

cond-mat.str-el

Anisotropic skyrmion and multi-$q$ spin dynamics in centrosymmetric Gd$_2$PdSi$_3$

Skyrmions are particle-like vortices of magnetization with non-trivial topology, which are usually stabilized by Dzyaloshinskii-Moriya interactions (DMI) in noncentrosymmetric bulk materials. Exceptions are centrosymmetric Gd- and Eu-based skyrmion-lattice (SkL) hosts with zero DMI, where both the SkL stabilization mechanisms and magnetic ground states remain controversial. We address these here by investigating both the static and dynamical spin properties of the centrosymmetric SkL host Gd$_2$PdSi$_3$ using muon spectroscopy ($μ$SR). We find that spin fluctuations in the non-coplanar SkL phase are highly anisotropic, implying that spin anisotropy plays a prominent role in stabilizing this phase. We also observe strongly-anisotropic spin dynamics in the ground-state (IC-1) incommensurate magnetic phase of the material, indicating that it hosts a meron-like multi-$q$ structure. In contrast, the higher-field, coplanar IC-2 phase is found to be single-$q$ with nearly-isotropic spin dynamics.

cond-mat.str-el

Muon spectroscopy investigation of anomalous dynamic magnetism in NiI$_2$

We present the results of muon-spin relaxation ($μ^{+}$SR) measurements of the van der Waals magnet NiI$_2$, which probe magnetic phase transitions at $T_{\mathrm{N1}}=73$~K and $T_{\mathrm{N2}}=60$~K. Supporting density functional theory (DFT) calculations allow the determination of a single muon stopping site whose magnetic environment is consistent with the proposed ground-state magnetic structure. $μ^{+}$SR measurements of the dynamics reveal behavior consistent with spin-wave excitations below $T_{\mathrm{N2}}$. In the region $T_{\mathrm{N2}}<T<T_{\mathrm{N1}}$ the character of the dynamics changes qualitatively, resulting in an unusual region of temperature-independent fluctuations.

cond-mat.str-el

Field-orientation-dependent magnetic phases in GdRu$_2$Si$_2$ probed with muon-spin spectroscopy

Centrosymmetric GdRu$_2$Si$_2$ exhibits a variety of multi-Q magnetic states as a function of temperature and applied magnetic field, including a square skyrmion-lattice phase. The material's behavior is strongly dependent on the direction of the applied field, with different phase diagrams resulting for fields applied parallel or perpendicular to the crystallographic $c$ axis. Here, we present the results of muon-spin relaxation ($μ^+$SR) measurements on single crystals of GdRu$_2$Si$_2$. Our analysis is based on the computation of muon stopping sites and consideration of zero-point motion effects, allowing direct comparison with the underlying spin textures in the material. The muon site is confirmed experimentally, using angle-dependent measurements of the muon Knight shift. Using transverse-field $μ^+$SR with fields applied along either the [001] or [100] crystallographic directions, we distinguish between the magnetic phases in this system via their distinct muon response, providing additional evidence for the skyrmion and meron-lattice phases, while also suggesting the existence of RKKY-driven muon hyperfine coupling. Zero-field $μ^+$SR provides clear evidence for a transition between two distinct magnetically-ordered phases at 39 K.

cond-mat.str-el

Magnetic properties and field-induced phenomena in the Jeff = 1/2 distorted kagome antiferromagnet

The intertwining between competing degrees of freedom, anisotropy, and frustration-induced quantum fluctuations offers an ideal ground to realize exotic quantum phenomena in the rare-earth-based kagome lattice. The magnetic susceptibility reveals the presence of two energy scales in agreement with the INS results. The higher energy state is dominated by CEF excitations, where the lowest Kramers ground-state doublet is well separated from the excited state suggesting that the compound realizes a low-energy state at low temperatures. The second energy scale is witnessed via thermodynamic results that reveal an anomaly at 0.3 K typical of a phase transition, which is attributed to the presence of complex magnetic ordering phenomena. The broad maximum in the specific heat well above 0.3 K indicates the presence of short-range spin correlations that is corroborated by muon spin relaxation rate results. The isothermal magnetization reveals a field-induced 1/3 magnetization plateau at low temperatures. muSR relaxation rate experiments, on the other hand, neither show the signature of a phase transition nor spin-freezing down to 34 mK. The ZF muSR relaxation is governed by the Orbach process and reveals the presence of a fluctuating state owing to the depopulation of crystal field levels reflected as a constant value of relaxation rate in the temperature range 0.4-10 K. NMR results indicate the presence of fluctuating Nd3+ moments down to 1.8 K consistent with muSR experiments. Our comprehensive results reveal that a field-induced quantum critical phenomenon is at play in this frustrated kagome magnet and enable us to construct a phase diagram exemplifying the proximity effect of competing magnetic states. This sets the stage to investigate the broad RE3BWO9 family of rare-earth kagome magnets promising to host exotic quantum states driven by spin-orbit coupling and geometrical frustration.

cond-mat.str-el

Excitation Spectrum and Spin Hamiltonian of the Frustrated Quantum Ising Magnet Pr$_3$BWO$_9$

We present a thorough experimental investigation on single crystals of the rare-earth based frustrated quantum antiferromagnet Pr$_3$BWO$_9$, a purported spin-liquid candidate on the breathing kagome lattice. This material possesses a disordered ground state with an unusual excitation spectrum involving a coexistence of sharp spin-waves and broad continuum excitations. Nevertheless, we show through a combination of thermodynamic, magnetometric and spectroscopic probes with detailed theoretical modeling that it should be understood in a completely different framework. The crystal field splits the lowest quasi-doublet states into two singlets moderately coupled through frustrated superexchange, resulting in a simple effective Hamiltonian of an Ising model in a transverse magnetic field. While our neutron spectroscopy data do point to significant correlations within the kagome planes, the dominant interactions are out-of-plane, forming frustrated triangular spin-tubes through two competing ferro-antiferromagnetic bonds. The resulting ground state is a simple quantum paramagnet, but with significant modifications to both thermodynamic and dynamic properties due to small perturbations to the transverse field Ising model in the form of hyperfine enhanced nuclear moments and weak structural disorder.

cond-mat.str-el

Depth-dependent magnetic crossover in a room-temperature skyrmion-hosting multilayer

Skyrmion-hosting multilayer stacks are promising avenues for applications, although little is known about the depth dependence of the magnetism. We address this by reporting the results of circular dichroic resonant elastic x-ray scattering (CD-REXS), micromagnetic simulations, and low-energy muon-spin rotation (LE-$μ^+$SR) measurements on a stack comprising [Ta/CoFeB/MgO]$_{16}$/Ta on a Si substrate. Energy-dependent CD-REXS shows a continuous, monotonic evolution of the domain-wall helicity angle with incident energy, consistent with a three-dimensional hybrid domain-wall-like structure that changes from Néel-like near the surface to Bloch-like deeper within the sample. LE-$μ^+$SR reveals that the magnetic field distribution in the trilayers near the surface of the stack is distinct from that in trilayers deeper within the sample. Our micromagnetic simulations support a quantitative analysis of the $μ^+$SR results. By increasing the applied magnetic field, we find a reduction in the volume occupied by domain walls at all depths, consistent with a crossover into a region dominated by skyrmions above approximately 180 mT.

cond-mat.str-el

Unusual magnetism of the axion-insulator candidate Eu$_5$In$_2$Sb$_6$

Eu$_5$In$_2$Sb$_6$ is a member of a family of orthorhombic nonsymmorphic rare-earth intermetallics that combines large localized magnetic moments and itinerant exchange with a low carrier density and perpendicular glide planes. This may result in special topological crystalline (wallpaper fermion) or axion insulating phases. Recent studies of Eu$_5$In$_2$Sb$_6$ single crystals have revealed colossal negative magnetoresistance and multiple magnetic phase transitions. Here, we clarify this ordering process using neutron scattering, resonant elastic X-ray scattering, muon spin-rotation, and magnetometry. The nonsymmorphic and multisite character of Eu$_5$In$_2$Sb$_6$ results in coplanar noncollinear magnetic structure with an Ising-like net magnetization along the $a$ axis. A reordering transition, attributable to competing ferro- and antiferromagnetic couplings, manifests as the onset of a second commensurate Fourier component. In the absence of spatially resolved probes, the experimental evidence for this low-temperature state can be interpreted either as an unusual double-$q$ structure or in a phase separation scenario. The net magnetization produces variable anisotropic hysteretic effects which also couple to charge transport. The implied potential for functional domain physics and topological transport suggests that this structural family may be a promising platform to implement concepts of topological antiferromagnetic spintronics.

cond-mat.str-el

Band-filling-controlled magnetism from transition metal intercalation in $N_{1/3}$NbS$_2$ revealed with first-principles calculations

We present a first-principles study of the effect of 3$d$ transition metal intercalation on the magnetic properties of the 2H-NbS$_2$ system, using spin-resolved density functional theory calculations to investigate the electronic structure of $N_{1/3}$NbS$_2$ ($N$ = Ti, V, Cr, Mn, Fe, Co, Ni). We are able to accurately determine the magnetic moments and crystal field splitting, and find that the magnetic properties of the materials are determined by a mechanism based on filling rigid bands with electrons from the intercalant. We predict the dominant magnetic interaction of these materials by considering Fermi surface nesting, finding agreement with experiment where data are available.

cond-mat.mtrl-sci