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G. M. Luke

Publications and source records attributed to G. M. Luke.

At least 19 recordsLinked to original sources

Conventional superconductivity in single-crystalline BiPt

Binary Bi-Pd/Pt systems have attracted a lot of interest because of their topologically non-trivial nature along with superconductivity. We report the structural and superconducting properties of high-quality single-crystalline BiPt using a comprehensive range of experimental techniques, including X-ray diffraction, electron microscopy, muon spin rotation/relaxation ({\mu}SR), magnetization, resistivity, and heat capacity. Our findings establish that BiPt is a weak type-II superconductor with a transition temperature (Tc) of 1.2 K which exhibits pronounced anisotropic superconducting characteristics attributed to its hexagonal crystal structure. Magnetization and electronic transport studies reveal that BiPt lies within the dirty limit, while {\mu}SR and heat capacity data indicate conventional s-wave superconductivity that maintains time-reversal symmetry. This work provides valuable insights into the pairing symmetry and superconducting mechanism of topologically trivial BiPt, a sound comparison system for other Bi-based topologically nontrivial superconductors.

cond-mat.supr-con

Structure and magnetism of MnGe thin films grown with a nonmagnetic CrSi template

We report a method to grow B20 MnGe thin films using molecular-beam epitaxy, which employs an ultrathin CrSi template layer on Si(111). This layer is expected to be nonmagnetic, in contrast to MnSi and FeGe buffer layers that have been used previously. This template layer permits an investigation of the intrinsic properties of MnGe in the ultrathin-film limit without the influence of a neighboring magnetic layer. Single-phase MnGe(111) films were grown with thicknesses between 2 and 40 nm, which exhibited low interfacial roughnesses on the order of 0.6 nm. The films crystallized in a B20 structure with a small rhombohedral distortion. Magnetometry measurements in out-of-plane fields are consistent with a cone phase derived from helimagnetic order propagating along the film normal. However, an unexpected remanent moment develops below 35K, concomitant with features in the field dependence of the transport data. This provides indirect evidence for the presence of a low-temperature phase which has been identified by others as either a triple-Q topological spin-hedgehog lattice, or a multidomain single-Q helical state.

cond-mat.mtrl-sci

Two-Peak Heat Capacity Accounts for $R\ln(2)$ Entropy and Ground State Access in the Dipole-Octupole Pyrochlore Ce$_2$Hf$_2$O$_7$

Magnetic heat capacity measurements of a high-quality single crystal of the dipole-octupole pyrochlore Ce$_2$Hf$_2$O$_7$ down to a temperature of $T = 0.02$ K are reported. These show a two-peaked structure, with a Schottky-like peak at $T_1 \sim 0.065$ K, similar to what is observed in its sister Ce-pyrochlores Ce$_2$Zr$_2$O$_7$ and Ce$_2$Sn$_2$O$_7$. However, a second sharper peak is observed at $T_2 \sim 0.025$ K, signifying the entrance to the ground state. The ground state appears to have gapped excitations, as even the most abrupt extrapolation to $C_P=0$ at $T = 0$ K fully accounts for the $R\ln(2)$ entropy associated with the pseudospin-1/2 doublet for Ce$^{3+}$ in this environment. The ground state could be conventionally ordered, although theory predicts a much larger anomaly in $C_P$ at much higher temperatures than the measured $T_2$ for expectations from an all-in all-out ground state of the XYZ Hamiltonian for Ce$_2$Hf$_2$O$_7$. The sharp low-temperature peak could also signify a cross-over from a classical spin liquid to a quantum spin liquid (QSL). For both scenarios, comparison of the measured $C_P$ with NLC calculations suggests that weak interactions beyond the nearest-neighbor XYZ Hamiltonian become relevant below $T \sim 0.25$ K. The diffuse magnetic neutron scattering observed from Ce$_2$Hf$_2$O$_7$ at low temperatures between $T_2$ and $T_1$ resembles that observed from Ce$_2$Zr$_2$O$_7$, which is well established as a $π$-flux quantum spin ice (QSI). Together with the peak in the heat capacity at $T_2$, this diffuse scattering from Ce$_2$Hf$_2$O$_7$ is suggestive of a classical spin liquid regime above $T_2$ that is distinct from the zero-entropy quantum ground state below $T_2$.

cond-mat.str-el

Ground-states of the Shastry-Sutherland Lattice Materials Gd$_2$Be$_2$GeO$_7$ and Dy$_2$Be$_2$GeO$_7$

The recent realization that the rare-earth melilites RE$_2$Be$_2$GeO$_7$ host the Shastry-Sutherland lattice within planes of RE$^{3+}$ ions has sparked a number of studies. This family of materials lacks appreciable site mixing and conductivity, making them promising candidates for the Shastry-Sutherland model. Herein, we present the magnetic ground states of two of these rare-earth melilites: RE = Gd and Dy. We find, through measurements of magnetic susceptibility, magnetization, and specific heat capacity (RE = Dy only), that these two melilites are antiferromagnets (T$_N$ $\sim$~1~K). Gd$_2$Be$_2$GeO$_7$, in accordance with its electronic configuration, has isotropic single-ion anisotropy but shows a quadratic contribution to its magnetization. Dy$_2$Be$_2$GeO$_7$ has Ising-like single-ion ansiotropy and is likely an effective spin-$1/2$ system. Both materials exhibit metamagnetic transitions. We identify this transition in Dy$_2$Be$_2$GeO$_7$, occurring at 86(1)~mT for T=500~mK, to likely be a spin-flip transition.

cond-mat.str-el

Topology meets time-reversal symmetry breaking in FeSe$_{1-x}$Te$_{x}$ superconductor

Time-reversal symmetry breaking (TRSB) in magnetic topological insulators induces a Dirac gap in the topological surface state (TSS), leading to exotic phenomena such as the quantum anomalous Hall effect. Yet, the interplay between TRSB and topology in superconductors remains underexplored due to limited suitable materials. Here we employ zero-field muon spin relaxation ($μ$SR) as a sensitive probe of TRSB to map out the electronic phase diagrams of iron-chalcogenide superconductors FeSe$_{1-x}$Te$_{x}$. For the Te composition $x=0.64$ with the highest superconducting transition temperature $T_{\rm c}=14.5$ K, which is known to host a TSS and Majorana zero modes within vortices, we detect spontaneous magnetic fields below $T_{\rm c}$ distinct from a magnetic order. This signifies a TRSB superconducting state in the bulk, revealing the convergence of unconventional TRSB superconductivity with topologically nontrivial electronic structures in FeSe$_{1-x}$Te$_{x}$. Given the relatively high $T_{\rm c}$ and the tunability of the Fermi level through chemical substitution, iron-chalcogenide superconductors offer an intriguing platform for investigating the synergy between topological superconductivity and TRSB.

cond-mat.supr-con

Fractionalized Magnetization Plateaus in the Shastry-Sutherland Lattice Material Er$_2$Be$_2$GeO$_7$

The experimental study of magnetism on the Shastry-Sutherland lattice has been ongoing for more than two decades, following the discovery of the first Shastry-Sutherland lattice materials SrCu$_2$(BO$_3$)$_2$. However, the study of Shastry-Sutherland systems is often complicated by the requirements of high magnetic fields ($>$~20~T SrCu$_2$(BO$_3$)$_2$) or the presence of itinerate electrons (e.g. REB$_4$). In this paper, we present the magnetic properties of the Shastry-Sutherland lattice material Er$_2$Be$_2$GeO$_7$. Like SrCu$_2$(BO$_3$)$_2$, Er$_2$Be$_2$GeO$_7$ exhibits fractionalized magnetization plateaus. Unlike SrCu$_2$(BO$_3$)$_2$, Er$_2$Be$_2$GeO$_7$ exhibits long-range order below $\sim1~$K, and the plateaus are accessible using commercial laboratory equipment, occurring for fields <~1~T. The fractions of magnetization present are closest to $\frac{1}{4}$ and $\frac{1}{2}$ of the full powder moment; we show that the $\frac{1}{4}$ magnetization plateau in Er$_2$Be$_2$GeO$_7$ has a classical analog, well represented by the magnetic structure (canted antiferromagnetic) observed in powder neutron diffraction. The lack of itinerate electrons, chemical disorder, and the low fields required to access the fractionalized magnetization plateaus promises Er$_2$Be$_2$GeO$_7$ to be a prime candidate for the study of frustrated magnetism on the Shastry-Sutherland lattice.

cond-mat.str-el

Giant anomalous Hall effect in epitaxial Mn$_{3.2}$Ge films with a cubic kagome structure

We report on the first example of epitaxial Mn$_{3 + δ}$Ge thin films with a cubic $L1_2$ structure. The films are found to exhibit frustrated ferromagnetism with an average magnetization corresponding to 0.98$~\pm~$0.06$~μ_B$/Mn, far larger than the parasitic ferromagnetism in hexagonal Mn$_3$Ge and the partially compensated ferrimagnetism in tetragonal Mn$_3$Ge. The Hall conductivity is the largest reported for the kagome magnets with a low temperature value of $σ_{xy} = 1587~$S/cm. Density functional calculations predict that a chiral antiferromagnetic structure is lower in energy than a ferromagnetic configuration in an ordered stoichiometric crystal. However, chemical disorder driven by the excess Mn in our films explains why a frustrated 120$^\circ$ spin structure is not observed. Comparisons between the magnetization and the Hall resistivity indicate that a non-coplanar spin structure contributes the Hall signal. Anisotropic magnetoresistance and planar Hall effect with hysteresis up to 14 T provides further insights into this material.

cond-mat.mtrl-sci

A Candidate for the Quantum Spin Liquid Ground-State in the Shastry-Sutherland Lattice Material Yb$_2$Be$_2$GeO$_7$

The quasi-2D Shastry-Sutherland model has remained topical in the field of condensed matter physics for the last two decades, following the experimental realization of the model in the material SrCu$_2$(BO$_3$)$_2$. Since then, research into the Shastry-Sutherland system has revealed more nuanced physics than initially predicted; recent theoretical works have even predicted a quantum spin liquid phase may exist. Herein, we report on a new Shastry-Sutherland lattice material, Yb$_2$Be$_2$GeO$_7$, of the rare-earth melilite family RE$_2$Be$_2$GeO$_7$. We find, through SQUID magnetometry, powder neutron diffraction, specific heat capacity, and muon spin relaxation, that Yb$_2$Be$_2$GeO$_7$ lacks magnetic order and exhibits persistent spin dynamics to at least 17 mK. We propose the Shastry-Sutherland lattice material Yb$_2$Be$_2$GeO$_7$ as a candidate to host a quantum spin liquid ground-state.

cond-mat.str-el

Highly Tunable Ru-dimer Molecular Orbital State in 6H-perovskite Ba$_3$MRu$_2$O$_9$

Molecular orbital (MO) systems with clusters of heavy transition metal (TM) ions are one of the most important classes of model materials for studying the interplay between local physics and effects of itinerancy. Despite a large number of candidates identified in the family of 4d TM materials, an understanding of their physics from competing \textit{microscopic} energy scales is still missing. We bridge this gap by reporting the first resonant inelastic X-ray scattering (RIXS) measurement on a well-known series of Ru dimer systems with a 6H-perovskite structure, Ba$_3$MRu$_2$O$_9$ (M$^{3+}$=In$^{3+}$, Y$^{3+}$, La$^{3+}$). Our RIXS measurements reveal an extremely fragile MO state in these Ru dimer compounds, evidenced by an abrupt change in the RIXS spectrum accompanying a tiny change in the local structure tuned by the M-site ion. By modelling the RIXS spectra, we attribute the enhanced electronic instability in Ba$_3$MRu$_2$O$_9$ to the combined effect of a large hopping and a small spin-orbit coupling in the Ru dimers. The unique combination of energy scales uncovered in the present study make Ru MO systems ideal model systems for studying quantum phase transitions with molecular orbitals.

cond-mat.str-el

Evidence for conventional superconductivity in Bi$_2$PdPt and prediction of topological superconductivity in disorder-free $γ$-BiPd

We present comprehensive investigations into the structural, superconducting, and topological properties of Bi$_2$PdPt. Magnetization and heat capacity measurements performed on polycrystalline Bi$_2$PdPt demonstrate a superconducting transition at $\approx$ 0.8 K. Moreover, muon spin relaxation/rotation ($μ$SR) measurements present evidence for a time reversal symmetry preserving, isotropically gapped superconducting state in Bi$_2$PdPt. We have also performed density-functional theory (DFT) calculations on Bi$_2$PdPt alongside the more general isostructural systems, BiPd$_{x}$Pt$_{1-x}$, of which Bi$_2$PdPt and $γ$-BiPd are special cases for $x=0.5$ and $x=1$ respectively. We have calculated the $Z_2$ topological index from our DFT calculations for a range of substitution fractions, $x$, between $x=0$ and $x=1$ characterizing the topology of the band structure. We find a non-trivial topological state when $x>0.75$ and a trivial topological state when $x<0.75$. Therefore our results indicate that BiPd$_{x}$Pt$_{1-x}$ could be a topological superconductor for $x>0.75$.

cond-mat.supr-con

Broken time-reversal symmetry in a new non-centrosymmetric superconductor Re8NbTa

Re-based superconductors provide a rich platform for the study of unconventional superconductivity. We have investigated the superconducting properties of Re$_{8}$NbTa, a new noncentrosymmetric cubic ($α$-Mn structure) rhenium-based ternary superconductor using transport, magnetization, specific heat, and muon spin rotation/relaxation ($μ$SR) measurements. Specific heat and transverse field $μ$SR measurements suggest moderately coupled fully gapped superconductivity, well described by BCS theory. However, our zero-field $μ$SR measurements reveal a small internal field onsetting around the superconducting T$_c$, indicating that the superconducting order parameter breaks the time-reversal symmetry.

cond-mat.supr-con

$μ$SR Study of the Dipole-Octupole Quantum Spin Ice Candidate Ce$_2$Zr$_2$O$_7$

The Ce$^{3+}$ pseudospin-1/2 degrees of freedom in Ce$_2$Zr$_2$O$_7$ possess both dipolar and octupolar character which enables the possibility of novel quantum spin liquid ground states in this material. Here we report new muon spin relaxation and rotation ($μ$SR) measurements on single crystal samples of Ce$_2$Zr$_2$O$_7$ in zero magnetic field and in magnetic fields directed along the $[1,\bar{1},0]$ and $[1,1,1]$ crystallographic directions, and for magnetic fields directed both longitudinal and transverse to the direction of muon polarization. Our zero-field results show no signs of magnetic ordering or spin freezing, consistent with earlier zero-field $μ$SR measurements on a powder sample of Ce$_2$Zr$_2$O$_7$, and also with the expectations for a quantum spin ice. However, we measure a more gentle relaxation rate for Ce$_2$Zr$_2$O$_7$ in zero-field at low temperatures than was previously reported. This difference in relaxation rate is likely due to the low oxidation, and correspondingly, the high stoichiometry of our single crystal samples. Longitudinal field measurements confirm that the magnetic dipole moments in Ce$_2$Zr$_2$O$_7$ remain dynamic at $T = 0.1$ $\mathrm{K}$. For both $[1,\bar{1},0]$ and $[1,1,1]$ magnetic fields, our $μ$SR Knight shift measurements show a field-induced leveling off of the magnetic susceptibility at low temperature which is qualitatively consistent with corresponding calculations using the numerical-linked-cluster method in combination with recent estimates for the nearest-neighbour exchange parameters of Ce$_2$Zr$_2$O$_7$.

cond-mat.str-el

Evidence for non-unitary triplet-pairing superconductivity in noncentrosymmetric TaRuSi and comparison with isostructural TaReSi

We have studied the superconducting properties of the isostructural ternary noncentrosymmetric superconductors TaXSi (X = Re, Ru) with the help of muon spin rotation/relaxation ($μ$SR) and density functional theory calculations. Our transverse-field $μ$SR measurements indicate isotropic s-wave superconductivity in TaReSi and multi-gap superconductivity in TaRuSi. Zero-field $μ$SR measurements, highly sensitive to very small magnetic fields, and no evidence for spontaneous fields in the superconducting state of TaReSi, whereas we observe small spontaneous fields that onset with superconductivity indicating broken time-reversal symmetry (TRS) superconductivity in TaRuSi. Using density functional theory calculations, we find that spin-orbit coupling is relatively weak in TaRuSi and strong in TaReSi. Using symmetry analysis, we attribute the broken time-reversal symmetry (TRS) in TaRuSi to a non-unitary triplet pairing state. Such a state is not allowed in the presence of strong spin-orbit coupling: our finding of no evidence for broken TRS in TaReSi is consistent with this expectation.

cond-mat.supr-con

Quantum Spin Ice Response to a Magnetic Field in the Dipole-Octupole Pyrochlore Ce$_2$Zr$_2$O$_7$

We report new heat capacity measurements on single crystal Ce$_2$Zr$_2$O$_7$ down to $\sim$ 0.1 K in a magnetic field along the $[1,\bar{1}, 0]$ direction. These new measurements show that the broad hump in the zero-field heat capacity moves higher in temperature with increasing field strength and is split into two humps by the $[1,\bar{1}, 0]$ field at $\sim$ 2 T. These separate features are due to the decomposition of the pyrochlore lattice into effectively decoupled chains for fields in this direction: one set of chains ($α$-chains) is polarized by the field while the other ($β$-chains) remains free. Our theoretical modelling suggests that the $β$-chains are close to a critical state, with nearly-gapless excitations. We also report new elastic and inelastic neutron scattering measurements on single crystal Ce$_2$Zr$_2$O$_7$ in $[1, \bar{1}, 0]$ and $[0, 0, 1]$ magnetic fields at temperatures down to 0.03 K. The elastic scattering behaves consistently with the formation of independent chains for a $[1, \bar{1}, 0]$ field, while the $[0, 0, 1]$ field produces a single field-induced magnetic Bragg peak at $(0, 2, 0)$ and equivalent wavevectors, indicating a polarized spin ice for fields above $\sim$ 3 T. For both $[1, \bar{1}, 0]$ and $[0, 0, 1]$ fields, our inelastic neutron scattering results show an approximately-dispersionless continuum of scattering that increases in both energy and intensity with increasing field strength. By modelling the complete set of experimental data using numerical linked cluster and semiclassical molecular dynamics calculations, we demonstrate the dominantly multipolar nature of the exchange interactions in Ce$_2$Zr$_2$O$_7$ and the smallness of the parameter $θ$ which controls the mixing between dipolar and octupolar degrees of freedom. These results support previous estimates of the microscopic exchange parameters.

cond-mat.str-el

Two superconducting states with broken time-reversal symmetry in FeSe1-xSx

Iron-chalcogenide superconductors FeSe$_{1-x}$S$_x$ possess unique electronic properties such as non-magnetic nematic order and its quantum critical point. The nature of superconductivity with such nematicity is important for understanding the mechanism of unconventional superconductivity. A recent theory suggested the possible emergence of a fundamentally new class of superconductivity with the so-called Bogoliubov Fermi surfaces (BFSs) in this system. However, such an {\em ultranodal} pair state requires broken time-reversal symmetry (TRS) in the superconducting state, which has not been observed experimentally. Here we report muon spin relaxation ($μ$SR) measurements in FeSe$_{1-x}$S$_x$ superconductors for $0\le x \le 0.22$ covering both orthorhombic (nematic) and tetragonal phases. We find that the zero-field muon relaxation rate is enhanced below the superconducting transition temperature $T_{\rm c}$ for all compositions, indicating that the superconducting state breaks TRS both in the nematic and tetragonal phases. Moreover, the transverse-field $μ$SR measurements reveal that the superfluid density shows an unexpected and substantial reduction in the tetragonal phase ($x>0.17$). This implies that a significant fraction of electrons remain unpaired in the zero-temperature limit, which cannot be explained by the known unconventional superconducting states with point or line nodes. The time-reversal symmetry breaking and the suppressed superfluid density in the tetragonal phase, together with the reported enhanced zero-energy excitations, are consistent with the ultranodal pair state with BFSs. The present results reveal two different superconducting states with broken TRS separated by the nematic critical point in FeSe$_{1-x}$S$_x$, which calls for the theory of microscopic origins that account for the relation between the nematicity and superconductivity.

cond-mat.supr-con

Superconducting ground state study of valence skip compound AgSnSe$_2$

The valence-skipped superconductors are natural candidates for unconventional superconductivity, as they can exhibit a negative effective, attractive interaction for electron-pairing. This work reports comprehensive XRD, magnetization, specific heat and muon spin rotation and relaxation measurements ($μ$SR) on a valence-skipped compound: AgSnSe$_2$. The temperature dependence of the electronic specific heat ($C_{el}(T)$) and of the upper critical field ($H_{c2}(T)$) provide evidence of two-gap superconductivity, which is also confirmed by our transverse-field $μ$SR measurements. Our zero-field $μ$SR measurements suggest preserved time-reversal symmetry in the superconducting ground state of AgSnSe$_2$.

cond-mat.supr-con

Reply to "Comment on: 'Case for a U(1)$_π$ Quantum Spin Liquid Ground State in the Dipole-Octupole Pyrochlore $\mathrm{Ce}_2\mathrm{Zr}_2\mathrm{O}_7$' "

In his comment [arXiv:2209.03235], S. W. Lovesey argues that our analysis of neutron scattering experiments performed on Ce$_2$Zr$_2$O$_7$ is invalid. Lovesey argues that we have not properly accounted for the higher-order multipolar contributions to the magnetic scattering and that our use of pseudospin-$1/2$ operators to describe the scattering is inappropriate. In this reply, we show that the multipolar corrections discussed by Lovesey only become significant at scattering wavevectors exceeding those accessed in our experiments. This in no way contradicts or undermines our work, which never claimed a direct observation of scattering from higher-order multipoles. We further show that Lovesey's objections to our use of pseudospins are unfounded, and that the pseudospin operators are able to describe all magnetic scattering processes at the energy scale of our experiments, far below the crystal field gap. Finally, we comment on certain assumptions in Lovesey's calculations of the scattering amplitude which are inconsistent with experiment.

cond-mat.str-el

Spin-orbit coupling controlled ground states in the double perovskite iridates A2BIrO6 (A = Ba, Sr; B = Lu, Sc)

Iridates with the 5$d^4$ electronic configuration have attracted recent interest due to reports of magnetically-ordered ground states despite longstanding expectations that their strong spin-orbit coupling would generate a $J = 0$ electronic ground state for each Ir$^{5+}$ ion. The major focus of prior research has been on the double perovskite iridates Ba$_2$YIrO$_6$ and Sr$_2$YIrO$_6$, where the nature of the ground states (i.e. ordered vs non-magnetic) is still controversial. Here we present neutron powder diffraction, high energy resolution fluorescence detected x-ray absorption spectroscopy (HERFD-XAS), resonant inelastic x-ray scattering (RIXS), magnetic susceptibility, and muon spin relaxation data on the related double perovskite iridates Ba$_2$LuIrO$_6$, Sr$_2$LuIrO$_6$, Ba$_2$ScIrO$_6$, and Sr$_2$ScIrO$_6$ that enable us to gain a general understanding of the electronic and magnetic properties for this family of materials. Our HERFD-XAS and RIXS measurements establish $J = 0$ electronic ground states for the Ir$^{5+}$ ions in all cases, with similar values for Hund's coupling $J_{\rm H}$ and the spin-orbit coupling constant $λ_{\rm SOC}$. Our bulk susceptibility and muon spin relaxation data find no evidence for long-range magnetic order or spin freezing, but they do reveal weak magnetic signals that are consistent with extrinsic local moments. Our results indicate that the large $λ_{\rm SOC}$ is the key driving force behind the electronic and magnetic ground states realized in the 5$d^4$ double perovskite iridates, which agrees well with conventional wisdom.

cond-mat.str-el