Showing 1–50 of 145 results for author: Luke, G

Unconventional Superconductivity in the Chiral Topological Semimetal Ag2Pd3S

Authors: Roshan Kumar Kushwaha, Dibyendu Samanta, Sudarshan Sharma, Mathew Pula, Shashank Srivastava, Poulami Manna, Arushi, Sajilesh K. P., Suhani Sharma, Priya Mishra, Prabin Kumar Naik, James Beare, Yipeng Cai, Kenji M. Kojima, Amit Kanigel, Graeme M. Luke, Sudeep Kumar Ghosh, Ravi Prakash Singh

Abstract: Chiral crystals provide a unique setting where broken inversion symmetry, strong spin-orbit coupling, and electronic topology intertwine, yet superconductivity in intrinsically chiral materials remains rare. Here, we report unconventional superconductivity in the chiral topological semimetal Ag$_2$Pd$_3$S, an enantiomorphic analog of natural mineral coldwellite, crystallizing in the right-handed s… ▽ More Chiral crystals provide a unique setting where broken inversion symmetry, strong spin-orbit coupling, and electronic topology intertwine, yet superconductivity in intrinsically chiral materials remains rare. Here, we report unconventional superconductivity in the chiral topological semimetal Ag$_2$Pd$_3$S, an enantiomorphic analog of natural mineral coldwellite, crystallizing in the right-handed space group $P4_132$. Bulk superconductivity with a transition temperature $T_C = 1.1(2)$ K is confirmed by electrical resistivity, magnetization, and specific-heat measurements. Muon spin rotation and relaxation ($μ$SR) experiments reveal a fully gapped superconducting state that spontaneously time-reversal symmetry (TRS) breaking establishing Ag$_2$Pd$_3$S as the first chiral topological semimetal superconductor exhibiting intrinsic TRS breaking. First-principles calculations uncover multiple multifold band crossings near the Fermi level, hosting Kramers-Weyl, double spin-1, and spin-3/2 quasiparticles with large topological charges. These unconventional fermions generate symmetry-protected topological surface states and underscore the nontrivial topology of the normal state. Symmetry analysis based on the Ginzburg-Landau theory suggests a loop-supercurrent-ordered superconducting state, yielding a full gap alongside spontaneous TRS breaking. The coexistence of TRS-breaking superconductivity and chiral multifold fermions identifies Ag$_2$Pd$_3$S as a platform for realizing intrinsic superconducting diode effects and chirality-induced spin selectivity, offering a transformative pathway toward dissipationless topological quantum technologies. △ Less

Submitted 29 June, 2026; originally announced June 2026.

Comments: 11 pages, 4 figures,

Conventional superconductivity in single-crystalline BiPt

Authors: S. Sharma, M. Pula, Sajilesh K. P., J. Gautreau, B. S. Agboola, J. P. Clancy, J. E. Sonier, A. Ghara, S. R. Dunsiger, M. Greven, M. J. Lagos, A. Kanigel, G. M. Luke

Abstract: 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 (μSR), magnetization, resistivi… ▽ More 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 (μSR), 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 μSR 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. △ Less

Submitted 24 March, 2026; v1 submitted 19 November, 2025; originally announced November 2025.

Comments: 9 Pages, 5 figures

Journal ref: Phys. Rev. B 113, 094522 (2026)

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

Authors: B. D. MacNeil, J. S. R. McCoombs, D. Kalliecharan, J. Myra, M. Pula, J. F. Britten, G. B. G. Stenning, K. Gupta, G. M. Luke, T. L. Monchesky

Abstract: 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… ▽ More 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. △ Less

Submitted 4 March, 2026; v1 submitted 15 October, 2025; originally announced October 2025.

Comments: Main paper: 14 pages, 11 figures. Supplemental: 10 pages, 6 figures

Journal ref: Phys. Rev. Materials 10, 034405 (2026)

Magnetism of kagome metals $\left(\text{Fe}_{1-x} \text{Co}_{x}\right) \text{Sn}$ studied by $μ$SR

Authors: Yipeng Cai, Sungwon Yoon, Qi Sheng, Guoqiang Zhao, Eric Francis Seewald, Sanat Ghosh, Julian Ingham, Abhay Narayan Pasupathy, Raquel Queiroz, Hechang Lei, Yaofeng Xie, Pengcheng Dai, Takashi Ito, Ruyi Ke, Robert J. Cava, Sudarshan Sharma, Mathew Pula, Graeme M. Luke, Kenji M. Kojima, Yasutomo J. Uemura

Abstract: We study the magnetic properties of the metallic kagome system $\left(\mathrm{Fe}_{1-x} \mathrm{Co}_{x}\right) \mathrm{Sn}$ by a combination of Muon Spin Relaxation ($μ\mathrm{SR}$), magnetic susceptibility and Scanning Tunneling Microscopy (STM) measurements, in single crystal specimens with Co concentrations $\mathrm{x}=0,0.11,0.8$. In the undoped antiferromagnetic compound FeSn, we find possibl… ▽ More We study the magnetic properties of the metallic kagome system $\left(\mathrm{Fe}_{1-x} \mathrm{Co}_{x}\right) \mathrm{Sn}$ by a combination of Muon Spin Relaxation ($μ\mathrm{SR}$), magnetic susceptibility and Scanning Tunneling Microscopy (STM) measurements, in single crystal specimens with Co concentrations $\mathrm{x}=0,0.11,0.8$. In the undoped antiferromagnetic compound FeSn, we find possible signatures for a previously unidentified phase that sets in at $T^*\sim 50$ K, well beneath the Neel temperature $T_N \sim 376$ K, as indicated by a peak in the relaxation rate $1/T_1$ observed in zero field (ZF) and longitudinal field (LF) $μ\mathrm{SR}$ measurements, with a corresponding anomaly in the ac and dc-susceptibility, and an increase in the static width $1/T_2$ in ZF measurements. No signatures of spatial symmetry breaking are found in STM down to $7$ K. In $\mathrm{Fe}_{0.2} \mathrm{Co}_{0.8} \mathrm{Sn}$, we find canonical spin glass behavior with freezing temperature $T_{g} \sim 3.5 \mathrm{~K}$; the ZF and LF time spectra exhibit results similar to those observed in dilute alloy spin glasses CuMn and AuFe, with a critical behavior of $1 / T_{1}$ at $T_{g}$ and $1 / \mathrm{T}_{1}\rightarrow 0$ as $T \rightarrow 0$. The absence of spin dynamics at low temperatures makes a clear contrast to the spin dynamics observed by $μ\mathrm{SR}$ in many geometrically frustrated spin systems on insulating kagome, pyrochlore, and triangular lattices. The spin glass behavior of CoSn doped with dilute Fe moments is shown to originate primarily from the randomness of doped Fe moments rather than due to geometrical frustration of the underlying lattice. △ Less

Submitted 29 July, 2025; originally announced July 2025.

Journal ref: Phys. Rev. B 111, 214412 (2025)

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

Authors: M. Pula, S. Sharma, J. Gautreau, Sajilesh K. P., A. Kanigel, G. M. Luke

Abstract: 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… ▽ More 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. △ Less

Submitted 7 May, 2025; originally announced May 2025.

Comments: 11 pages, 7 figures, 1 table

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

Authors: E. M. Smith, A. Fitterman, R. Schäfer, B. Placke, A. Woods, S. Lee, S. H. -Y. Huang, J. Beare, S. Sharma, D. Chatterjee, C. Balz, M. B. Stone, A. I. Kolesnikov, A. R. Wildes, E. Kermarrec, G. M. Luke, O. Benton, R. Moessner, R. Movshovich, A. D. Bianchi, B. D. Gaulin

Abstract: 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… ▽ More 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 $T_2$. △ Less

Submitted 30 July, 2025; v1 submitted 14 January, 2025; originally announced January 2025.

Comments: Main Text (6 pages, 4 figures), Supplemental Material (14 pages, 17 figures)

Journal ref: Physical Review Letters 135, 086702 (2025)

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

Authors: M. Roppongi, Y. Cai, K. Ogawa, S. Liu, G. Q. Zhao, M. Oudah, T. Fujii, K. Imamura, S. Fang, K. Ishihara, K. Hashimoto, K. Matsuura, Y. Mizukami, M. Pula, C. Young, I. Markovic, D. A. Bonn, T. Watanabe, A. Yamashita, Y. Mizuguchi, G. M. Luke, K. M. Kojima, Y. J. Uemura, T. Shibauchi

Abstract: 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 prob… ▽ More 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. △ Less

Submitted 6 January, 2025; originally announced January 2025.

Comments: 20 pages, 4 figures

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

Authors: M. Pula, S. Sharma, J. Gautreau, Sajilesh K. P., A. Kanigel, C. R. dela Cruz, T. N. Dolling, L. Clark, G. M. Luke

Abstract: 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.… ▽ More 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. △ Less

Submitted 5 December, 2024; originally announced December 2024.

Comments: 9 pages, 8 figures

Discovery of Dynamical Heterogeneity in a Supercooled Magnetic Monopole Fluid

Authors: Jahnatta Dasini, Chaia Carroll, Hiroto Takahashi, Jack Murphy, Chun-Chih Hsu, Sudarshan Sharma, Catherine Dawson, Fabian Jerzembeck, Stephen J. Blundell, Graeme Luke, J. C. Séamus Davis, Jonathan Ward

Abstract: Dynamical heterogeneity, in which transitory local fluctuations occur in the conformation and dynamics of constituent particles, is widely hypothesized to be essential to evolution of supercooled liquids into the structural glass state. Yet its microscopic spatiotemporal phenomenology is challenging to detect directly in molecular glass forming liquids. Because recent theoretical advances predict… ▽ More Dynamical heterogeneity, in which transitory local fluctuations occur in the conformation and dynamics of constituent particles, is widely hypothesized to be essential to evolution of supercooled liquids into the structural glass state. Yet its microscopic spatiotemporal phenomenology is challenging to detect directly in molecular glass forming liquids. Because recent theoretical advances predict that corresponding dynamical heterogeneity could occur in supercooled magnetic monopole fluids (Proc. Nat. Acad. Sci. 112, 8549 (2015)), we searched for such phenomena in Dy2Ti2O7. By measuring its microsecond-resolved spontaneous magnetization fluctuations $M(t,T)$ we discovered a sharp bifurcation in monopole noise characteristics below $T \approx 1500$ mK, with the appearance of powerful spontaneous monopole current bursts. This intense dynamics emerges upon entering the supercooled monopole fluid regime, reaches maximum strength near $T \approx 750$ mK and then collapses along with coincident loss of ergodicity approaching $T_g \approx 750$ mK. Moreover, when the four-point dynamical susceptibility $χ_4(τ, T)$ is determined directly from temperature dependence of correlations in $M(t,T)$, it evolves as predicted when dynamical heterogeneity is present, revealing its simultaneously and rapidly escalating length and time scales, $ξ(T)$. and $τ_4(T)$. This overall phenomenology 2 greatly expands our empirical knowledge of supercooled monopole fluids and, more generally, demonstrates direct detection of the time sequence, magnitude, statistics and correlations of dynamical heterogeneity, access to which may greatly accelerate fundamental vitrification studies. △ Less

Submitted 6 March, 2026; v1 submitted 1 August, 2024; originally announced August 2024.

Comments: 30 pages, 4 figures, 31 page of Supplementary Information

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

Authors: M. Pula, S. Sharma, J. Gautreau, Sajilesh K. P., A. Kanigel, M. D. Frontzek, T. N. Dolling, L. Clark, S. Dunsiger, A. Ghara, G. M. Luke

Abstract: 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 p… ▽ More 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. △ Less

Submitted 21 June, 2024; originally announced June 2024.

Comments: 11 pages, 7 figures, 4 tables

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

Authors: Bo Yuan, Beom Hyun Kim, Qiang Chen, Daniel Dobrowolski, Monika Azmanska, G. M. Luke, Shiyu Fan, Valentina Bisogni, Jonathan Pelliciari, J. P. Clancy

Abstract: 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… ▽ More 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. △ Less

Submitted 15 May, 2024; originally announced May 2024.

Comments: 7 pages, 3 figures, Supplemental Materials available upon request

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

Authors: S. Sharma, A. D. S. Richards, Sajilesh K. P., A. Kataria, B. S. Agboola, M. Pula, J. Gautreau, A. Ghara, D. Singh, S. Marik, S. R. Dunsiger, M. J. Lagos, A. Kanigel, E. S. Sørensen, R. P. Singh, G. M. Luke

Abstract: 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 g… ▽ More 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 $x>0.75$. △ Less

Submitted 27 March, 2024; originally announced March 2024.

Comments: 10 pages, 7 figures

Dichotomous Dynamics of Magnetic Monopole Fluids

Authors: Chun-Chih Hsu, Hiroto Takahashi, Fabian Jerzembeck, Jahnatta Dasini, Chaia Carroll, Ritika Dusad, Jonathan Ward, Catherine Dawson, Sudarshan Sharma, Graeme Luke, Stephen J. Blundell, Claudio Castelnovo, Jonathan N. Hallén, Roderich Moessner, J. C. Séamus Davis

Abstract: A recent advance in the study of emergent magnetic monopoles was the discovery that monopole motion is restricted to dynamical fractal trajectories (J. Hallén et al, Science 378, 1218 (2022)) thus explaining the characteristics of magnetic monopole noise spectra (Dusad, R. et al. Nature 571, 234 (2019); Samarakoon, A. M. et al. Proc. Natl. Acad. Sci. 119, e2117453119 (2022)). Here we apply this ne… ▽ More A recent advance in the study of emergent magnetic monopoles was the discovery that monopole motion is restricted to dynamical fractal trajectories (J. Hallén et al, Science 378, 1218 (2022)) thus explaining the characteristics of magnetic monopole noise spectra (Dusad, R. et al. Nature 571, 234 (2019); Samarakoon, A. M. et al. Proc. Natl. Acad. Sci. 119, e2117453119 (2022)). Here we apply this new theory to explore the dynamics of field-driven monopole currents, finding them comprised of two quite distinct transport processes: initially swift fractal rearrangements of local monopole configurations followed by conventional monopole diffusion. This theory also predicts a characteristic frequency dependence of the dissipative loss-angle for AC-field-driven currents. To explore these novel perspectives on monopole transport, we introduce simultaneous monopole current control and measurement techniques using SQUID-based monopole current sensors. For the canonical material Dy2Ti2O7, we measure $Φ(t)$, the time-dependence of magnetic flux threading the sample when a net monopole current $J(t) = \dotΦ(t)/μ_0$ is generated by applying an external magnetic field $B_0(t)$. These experiments find a sharp dichotomy of monopole currents, separated by their distinct relaxation time-constants before and after $t \approx 600 μs$ from monopole current initiation. Application of sinusoidal magnetic fields $B_0(t) = Bcos(ωt)$ generates oscillating monopole currents whose loss angle $θ(f)$ exhibits a characteristic transition at frequency $f \approx 1.8$ kHz over the same temperature range. Finally, the magnetic noise power is also dichotomic, diminishing sharply after $t \approx 600 μs$. This complex phenomenology represents a new form of heterogeneous dynamics generated by the interplay of fractionalization and local spin configurational symmetry. △ Less

Submitted 9 April, 2024; v1 submitted 1 March, 2024; originally announced March 2024.

Journal ref: Proceedings of the National Academy of Sciences 121 (21) e2320384121 (2024)

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

Authors: R. K. Kushwaha, Arushi, S. Sharma, S. Srivastava, P. K. Meena, M. Pula, J. Beare, J. Gautreau, A. D. Hillier, G. M. Luke, R. P. Singh

Abstract: 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… ▽ More 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. △ Less

Submitted 15 January, 2024; originally announced January 2024.

Comments: 9 pages, 7 figures

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

Authors: J. S. R. McCoombs, B. D. MacNeil, V. Askarpour, J. Myra, H. Herdin, M. Pula, M. D. Robertson, G. M. Luke, K. L. Kavanagh, J. Maassen, T. L. Monchesky

Abstract: 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$Ge. The Hall conductivity is the larg… ▽ More We report on the first example of epitaxial Mn$_{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. △ Less

Submitted 17 July, 2024; v1 submitted 1 November, 2023; originally announced November 2023.

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

Authors: J. Beare, E. M. Smith, J. Dudemaine, R. Schäfer, M. R. Rutherford, S. Sharma, A. Fitterman, C. A. Marjerrison, T. J. Williams, A. A. Aczel, S. R. Dunsiger, A. D. Bianchi, B. D. Gaulin, G. M. Luke

Abstract: 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… ▽ More 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$_7$. △ Less

Submitted 7 November, 2023; v1 submitted 5 August, 2023; originally announced August 2023.

Journal ref: Physical Review B 108, 174411 (2023)

Fragile superconductivity in a Dirac metal

Authors: Chris J. Lygouras, Junyi Zhang, Jonah Gautreau, Mathew Pula, Sudarshan Sharma, Shiyuan Gao, Tanya Berry, Thomas Halloran, Peter Orban, Gael Grissonnanche, Juan R. Chamorro, Kagetora Mikuri, Dilip K. Bhoi, Maxime A. Siegler, Kenneth K. Livi, Yoshiya Uwatoko, Satoru Nakatsuji, B. J. Ramshaw, Yi Li, Graeme M. Luke, Collin L. Broholm, Tyrel M. McQueen

Abstract: 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… ▽ More 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. △ Less

Submitted 4 July, 2023; originally announced July 2023.

Comments: 58 pages, 5 main figures, supplemental information attached

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

Authors: E. M. Smith, J. Dudemaine, B. Placke, R. Schäfer, D. R. Yahne, T. DeLazzer, A. Fitterman, J. Beare, J. Gaudet, C. R. C. Buhariwalla, A. Podlesnyak, Guangyong Xu, J. P. Clancy, R. Movshovich, G. M. Luke, K. A. Ross, R. Moessner, O. Benton, A. D. Bianchi, B. D. Gaulin

Abstract: 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… ▽ More 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. △ Less

Submitted 29 August, 2023; v1 submitted 22 June, 2023; originally announced June 2023.

Journal ref: Physical Review B 108, 054438 (2023)

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

Authors: K. Matsuura, M. Roppongi, M. Qiu, Q. Sheng, Y. Cai, K. Yamakawa, Z. Guguchia, R. P. Day, K. M. Kojima, A. Damascelli, Y. Sugimura, M. Saito, T. Takenaka, K. Ishihara, Y. Mizukami, K. Hashimoto, Y. Gu, S. Guo, L. Fu, Z. Zhang, F. Ning, G. Zhao, G. Dai, C. Jin, J. W. Beare , et al. (3 additional authors not shown)

Abstract: 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 s… ▽ More 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. △ Less

Submitted 12 April, 2023; v1 submitted 6 April, 2023; originally announced April 2023.

Comments: 8 pages, 4 figures, typos corrected. Accepted for publication in PNAS

Journal ref: Proc. Natl. Acad. Sci. USA 120, e2208276120 (2023)

Visualizing the atomic-scale origin of metallic behavior in Kondo insulators

Authors: Harris Pirie, Eric Mascot, Christian E. Matt, Yu Liu, Pengcheng Chen, M. H. Hamidian, Shanta Saha, Xiangfeng Wang, Johnpierre Paglione, Graeme Luke, David Goldhaber-Gordon, Cyrus F. Hirjibehedin, J. C. Séamus Davis, Dirk K. Morr, Jennifer E. Hoffman

Abstract: A Kondo lattice is often electrically insulating at low temperatures. However, several recent experiments have detected signatures of bulk metallicity within this Kondo insulating phase. Here we visualize the real-space charge landscape within a Kondo lattice with atomic resolution using a scanning tunneling microscope. We discover nanometer-scale puddles of metallic conduction electrons centered… ▽ More A Kondo lattice is often electrically insulating at low temperatures. However, several recent experiments have detected signatures of bulk metallicity within this Kondo insulating phase. Here we visualize the real-space charge landscape within a Kondo lattice with atomic resolution using a scanning tunneling microscope. We discover nanometer-scale puddles of metallic conduction electrons centered around uranium-site substitutions in the heavy-fermion compound URu$_2$Si$_2$, and around samarium-site defects in the topological Kondo insulator SmB$_6$. These defects disturb the Kondo screening cloud, leaving behind a fingerprint of the metallic parent state. Our results suggest that the mysterious 3D quantum oscillations measured in SmB$_6$ could arise from these Kondo-lattice defects, although we cannot rule out other explanations. Our imaging technique could enable the development of atomic-scale charge sensors using heavy-fermion probes. △ Less

Submitted 27 March, 2023; originally announced March 2023.

Journal ref: Science 379, 1214 (2023)

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

Authors: A. Kataria, Arushi, S. Sharma, T. Agarwal, M. Pula, J. Beare, S. Yoon, Y. Cai, K. M. Kojima, G. M. Luke, R. P. Singh

Abstract: 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 spe… ▽ More 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$_2$. △ Less

Submitted 15 February, 2023; originally announced February 2023.

Comments: 8 pages, 6 figures

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

Authors: E. M. Smith, O. Benton, D. R. Yahne, B. Placke, R. Schäfer, J. Gaudet, J. Dudemaine, A. Fitterman, J. Beare, A. R. Wildes, S. Bhattacharya, T. DeLazzer, C. R. C. Buhariwalla, N. P. Butch, R. Movshovich, J. D. Garrett, C. A. Marjerrison, J. P. Clancy, E. Kermarrec, G. M. Luke, A. D. Bianchi, K. A. Ross, B. D. Gaulin

Abstract: 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 m… ▽ More 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. △ Less

Submitted 30 September, 2022; v1 submitted 29 September, 2022; originally announced September 2022.

Comments: 6 pages, 1 figure

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

Authors: S. Sharma, Sajilesh K. P., A. D. S. Richards, J. Gautreau, M. Pula, J. Beare, K. M. Kojima, S. Yoon, Y. Cai, R. K. Kushwaha, T. Agrawal, E. S. Sørensen, R. P. Singh, G. M. Luke

Abstract: 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, hig… ▽ More 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. △ Less

Submitted 4 October, 2023; v1 submitted 20 September, 2022; originally announced September 2022.

Comments: 11 Pages, 5 Figures: Accepted for publication as a Regular Article in Physical Review B

Three-Dimensional Neutron Far-Field Tomography of a Bulk Skyrmion Lattice

Authors: M. E. Henderson, B. Heacock, M. Bleuel, D. G. Cory, C. Heikes, M. G. Huber, J. Krzywon, O. Nahman-Levesqué, G. M. Luke, M. Pula, D. Sarenac, K. Zhernenkov, D. A. Pushin

Abstract: Skyrmions are topologically-protected spin textures thought to nucleate and annihilate on points of vanishing magnetization, called Bloch points. However, owing to a lack of bulk techniques, experimental visualizations of skyrmion lattices and their stabilization through defects in three-dimensions remain elusive. Here, we present a tomographic algorithm applied to a Co$_8$Zn$_8$Mn$_4$ skyrmion la… ▽ More Skyrmions are topologically-protected spin textures thought to nucleate and annihilate on points of vanishing magnetization, called Bloch points. However, owing to a lack of bulk techniques, experimental visualizations of skyrmion lattices and their stabilization through defects in three-dimensions remain elusive. Here, we present a tomographic algorithm applied to a Co$_8$Zn$_8$Mn$_4$ skyrmion lattice host, processing multi-projection small angle neutron scattering measurements to generate mean scattering feature reconstructions (MSFR) of the bulk spin textures. Digital phantoms validated the algorithm; reconstructions of the sample show a disordered skyrmion lattice with a topological saturation of 63~\%, exhibiting three-dimensional topological transitions through two different emergent (anti)monopole defect pathways with densities of 147~$μ$m$^{-3}$ and 21~$μ\mathrm{m}^{-3}$ for branching and segmentation events, respectively. Our techniques produce experimentally-informed visualizations of bulk skyrmion lattice structures and defects, enabling future bulk studies over a wide variety of sample shapes and chemistries, magnetic phases, and external parameters. △ Less

Submitted 29 July, 2022; originally announced August 2022.

Comments: 10 pages, 2 figures, 1 table

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

Authors: A. A. Aczel, Q. Chen, J. P. Clancy, C. dela Cruz, D. Reig-i-Plessis, G. J. MacDougall, C. J. Pollock, M. H. Upton, T. J. Williams, N. LaManna, J. P. Carlo, J. Beare, G. M. Luke, H. D. Zhou

Abstract: 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… ▽ More 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. △ Less

Submitted 16 September, 2022; v1 submitted 11 April, 2022; originally announced April 2022.

Comments: 13 pages, 7 figures, accepted for publication by PRM

Synthesis, physical and magnetic properties of CuAlCr$_4$S$_8$: a new Cr-based breathing pyrochlore

Authors: S. Sharma, M. Pocrnic, B. N. Richtik, C. R. Wiebe, J. Beare, J. Gautreau, J. P. Clancy, J. P. C. Ruff, M. Pula, Q. Chen, Y. Cai, S. Yoon, G. M. Luke

Abstract: We present the synthesis and physical properties of a new breathing pyrochlore magnet CuAlCr$_4$S$_8$ with the help of synchrotron x-ray diffraction (XRD), magnetization under ambient and applied hydrostatic pressure, heat capacity, and muon spin relaxation/rotation ($μ$SR) measurements. CuAlCr$_4$S$_8$ exhibits positive thermal expansion with concave upward temperature dependence. We observed a s… ▽ More We present the synthesis and physical properties of a new breathing pyrochlore magnet CuAlCr$_4$S$_8$ with the help of synchrotron x-ray diffraction (XRD), magnetization under ambient and applied hydrostatic pressure, heat capacity, and muon spin relaxation/rotation ($μ$SR) measurements. CuAlCr$_4$S$_8$ exhibits positive thermal expansion with concave upward temperature dependence. We observed a sharp antiferromagnetic ordering transition of a purely magnetic nature at 20 K, which shifts by as much as 3.2 K on the application of 600 MPa pressure. The breathing factor (B$_f$ = $J'/J$) in breathing pyrochlores can be an important parameter to tune the magnetic ground states of the pyrochlore lattice. The breathing factor can be modulated through breathing ratio, the ratio of sizes of the two tetrahedra, by using different elements at A and A' sites in the breathing pyrochlore structure. We find that CuAlCr$_4$S$_8$ has a breathing ratio of 1.0663(8), which is comparable to other sulfur breathing pyrochlores. △ Less

Submitted 9 January, 2022; originally announced January 2022.

Comments: 7 pages, 7 figures

Report number: Phys. Rev. B 106, 024407 (2022)

Journal ref: Physical Review B, July 2022

Skyrmion Alignment and Pinning Effects in a Disordered Multi-Phase Skyrmion Material Co8Zn8Mn4

Authors: M. E. Henderson, M. Bleuel, J. Beare, D. G. Cory, B. Heacock, M. G. Huber, G. M. Luke, M. Pula, D. Sarenac, S. Sharma, E. M. Smith, K. Zhernenkov, D. A. Pushin

Abstract: Underlying disorder in skyrmion materials may both inhibit and facilitate skyrmion reorientations and changes in topology. The identification of these disorder-induced topologically active regimes is critical to realizing robust skyrmion spintronic implementations, yet few studies exist for disordered bulk samples. Here, we employ small-angle neutron scattering (SANS) and micromagnetic simulations… ▽ More Underlying disorder in skyrmion materials may both inhibit and facilitate skyrmion reorientations and changes in topology. The identification of these disorder-induced topologically active regimes is critical to realizing robust skyrmion spintronic implementations, yet few studies exist for disordered bulk samples. Here, we employ small-angle neutron scattering (SANS) and micromagnetic simulations to examine the influence of skyrmion order on skyrmion lattice formation, transition, and reorientation dynamics across the phase space of a disordered polycrystalline Co$_{8}$Zn$_{8}$Mn$_{4}$ bulk sample. Our measurements reveal a new disordered-to-ordered skyrmion square lattice transition pathway characterized by the novel promotion of four-fold order in SANS and accompanied by a change in topology of the system, reinforced through micromagnetic simulations. Pinning responses are observed to dominate skyrmion dynamics in the metastable triangular lattice phase, enhancing skyrmion stabilization through a remarkable and previously undetected skyrmion memory effect which reproduces previous ordering processes and persists in zero field. These results uncover the cooperative interplay of anisotropy and disorder in skyrmion formation and restructuring dynamics, establishing new tunable pathways for skyrmion manipulation. △ Less

Submitted 17 August, 2022; v1 submitted 16 December, 2021; originally announced December 2021.

Comments: 15 pages, 11 figures, Version 2 showing micromagnetic simulations that reinforce a new disordered-to-ordered square lattice skyrmion transition pathway which entails a change in topological charge. SANS simulations are included which estimate the change in the skyrmion lattice and ferromagnetic volume fractions from the metastable triangular lattice skyrmion phase to the skyrmion memory phase

The case for a U(1)$_π$ Quantum Spin Liquid Ground State in the Dipole-Octupole Pyrochlore Ce$_2$Zr$_2$O$_7$

Authors: E. M. Smith, O. Benton, D. R. Yahne, B. Placke, R. Schäfer, J. Gaudet, J. Dudemaine, A. Fitterman, J. Beare, A. R. Wildes, S. Bhattacharya, T. DeLazzer, C. R. C. Buhariwalla, N. P. Butch, R. Movshovich, J. D. Garrett, C. A. Marjerrison, J. P. Clancy, E. Kermarrec, G. M. Luke, A. D. Bianchi, K. A. Ross, B. D. Gaulin

Abstract: The Ce$^{3+}$ pseudospin-$\frac{1}{2}$ degrees of freedom in the pyrochlore magnet Ce$_2$Zr$_2$O$_7$ are known to possess dipole-octupole (DO) character, making it a candidate for novel quantum spin liquid (QSL) ground states at low temperatures. We report new polarized neutron diffraction at low temperatures, as well as heat capacity ($C_p$) measurements on single crystal Ce$_2$Zr$_2$O$_7$. The f… ▽ More The Ce$^{3+}$ pseudospin-$\frac{1}{2}$ degrees of freedom in the pyrochlore magnet Ce$_2$Zr$_2$O$_7$ are known to possess dipole-octupole (DO) character, making it a candidate for novel quantum spin liquid (QSL) ground states at low temperatures. We report new polarized neutron diffraction at low temperatures, as well as heat capacity ($C_p$) measurements on single crystal Ce$_2$Zr$_2$O$_7$. The former bears both similarities and differences from that measured in the canonical dipolar spin ice compound Ho$_2$Ti$_2$O$_7$, while the latter rises sharply at low temperatures, initially plateauing near 0.08 K, before falling off towards a high temperature zero beyond 3 K. Above $\sim$0.5 K, the $C_p$ data set can be fit to the results of a quantum numerical linked cluster (NLC) calculation, carried out to 4$^{\mathrm{th}}$ order, that allows estimates for the terms in the near-neighbour XYZ Hamiltonian expected for such DO pyrochlore systems. Fits of the same theory to the temperature dependence of the magnetic susceptibility and unpolarized neutron scattering complement this analysis. A comparison between the resulting best fit NLC calculation and the polarized neutron diffraction shows both agreement and discrepancies, mostly in the form of zone-boundary diffuse scattering in the non-spin flip channel, which are attributed to interactions beyond near-neighbours. The lack of an observed thermodynamic anomaly and the constraints on the near-neighbour XYZ Hamiltonian suggest that Ce$_2$Zr$_2$O$_7$ realizes a U(1)$_π$ QSL state at low temperatures, and one that likely resides near the boundary between dipolar and octupolar character. △ Less

Submitted 8 December, 2021; v1 submitted 2 August, 2021; originally announced August 2021.

Comments: 11 pages, 11 figures

Journal ref: Physical Review X 12, 021015 (2022)

Microscopics of Quantum Annealing in the Disordered Dipolar Ising Ferromagnet LiHo$_{x}$Y$_{1-x}$F$_4$

Authors: S. Säubert, C. L. Sarkis, F. Ye, G. Luke, K. A. Ross

Abstract: Quantum annealing (QA) refers to an optimization process that uses quantum fluctuations to find the global minimum of a rugged energy landscape with many local minima. Conceptually, QA is often framed in the context of the disordered transverse field Ising model, in which a magnetic field applied perpendicular to the Ising axis tunes the quantum fluctuations and enables the system to tunnel throug… ▽ More Quantum annealing (QA) refers to an optimization process that uses quantum fluctuations to find the global minimum of a rugged energy landscape with many local minima. Conceptually, QA is often framed in the context of the disordered transverse field Ising model, in which a magnetic field applied perpendicular to the Ising axis tunes the quantum fluctuations and enables the system to tunnel through energy barriers, and hence reach the ground state more quickly. A solid state material closely related to this model, LiHo$_{0.45}$Y$_{0.55}$F$_4$, was shown to exhibit faster dynamics after a QA protocol, compared to thermal annealing (TA), but little is known about the actual process of optimization involved or the nature of the spin correlations in the state that is reached. Here, we report on the microscopics of QA in this material using diffuse magnetic neutron scattering. Comparing a QA to a TA protocol that reach the same end-point, we find very similar final diffuse scattering which consists of pinch-point scattering, largely consistent with critical scattering near a phase boundary in the dipolar Ising ferromagnetic model. However, comparing the time evolution at the end of the protocols, we find that the spin correlations evolve more significantly after TA, suggesting that QA produces a state closer to equilibrium. We also observe experimental evidence that the transverse field produces random fields, which had been previously predicted for this material and studied in other contexts. Thus, while the material does exhibit a quantum speedup under quantum annealing conditions, it is not a simple annealing problem; the energy landscape being optimized is changing as the optimization proceeds. △ Less

Submitted 25 May, 2021; v1 submitted 7 May, 2021; originally announced May 2021.

An investigation of type-I superconductivity in single crystal of Pb2Pd

Authors: Arushi, K. Motla, A. Kataria, S. Sharma, J. Beare, M. Pula, M. Nugent, G. M. Luke, R. P. Singh

Abstract: We have investigated the superconducting properties in a single crystal of a new superconductor Pb$_{2}$Pd via various techniques including magnetization, AC transport, transverse field muon spin rotation and relaxation (TF-$μ$SR), and heat capacity. Pb$_{2}$Pd crystallizes in a body-centred tetragonal structure with space group I4/$mcm$. All measurements confirm the superconducting transition tem… ▽ More We have investigated the superconducting properties in a single crystal of a new superconductor Pb$_{2}$Pd via various techniques including magnetization, AC transport, transverse field muon spin rotation and relaxation (TF-$μ$SR), and heat capacity. Pb$_{2}$Pd crystallizes in a body-centred tetragonal structure with space group I4/$mcm$. All measurements confirm the superconducting transition temperature, T$_{C}$ = 3.0 $\pm$ 0.1 K. Electronic specific heat data are well described by the BCS fitting, suggesting that Pb$_{2}$Pd opens an isotropic gap on entering the superconducting state. The specific heat jump and $λ_{e-ph}$ value categorize Pb$_{2}$Pd as a moderately coupled superconductor. Magnetization and transverse field muon spin rotation measurements along with Ginzburg-Landau parameter, $κ$ < 1/$\sqrt{2}$ strongly infers that Pb$_{2}$Pd is a type I superconductor. △ Less

Submitted 11 March, 2021; originally announced March 2021.

Comments: 7 pages, 8 figures

Journal ref: Phys. Rev. B 103, 184506 (2021)

Fully gapped superconductivity in centrosymmetric and non-centrosymmetric Re-B compounds probed with $μ$SR

Authors: S. Sharma, Arushi, K. Motla, J. Beare, M. Nugent, M. Pula, T. J. Munsie, A. D. Hillier, R. P. Singh, G. M. Luke

Abstract: We present a comprehensive study on superconducting properties of Re$_7$B$_3$ and Re$_3$B through specific heat, magnetic susceptibility, resistivity, and transverse and zero-field muon spin rotation/relaxation ($μ$SR) experiments on polycrystalline samples. Re$_7$B$_3$ (T$_C$ = 3.2~K) is a non-centrosymmetric type-II ($κ$ $\approx$ 9.27) superconductor in the weak coupling ($λ_{e-ph}$ = 0.54) reg… ▽ More We present a comprehensive study on superconducting properties of Re$_7$B$_3$ and Re$_3$B through specific heat, magnetic susceptibility, resistivity, and transverse and zero-field muon spin rotation/relaxation ($μ$SR) experiments on polycrystalline samples. Re$_7$B$_3$ (T$_C$ = 3.2~K) is a non-centrosymmetric type-II ($κ$ $\approx$ 9.27) superconductor in the weak coupling ($λ_{e-ph}$ = 0.54) regime. On the other hand, Re$_3$B (T$_C$ = 5.19~K) is a centrosymmetric type-II ($κ$ $\approx$ 34.55) superconductor in the moderate coupling ($λ_{e-ph}$ = 0.64) regime. Our transverse-field $μ$SR measurements show evidence for isotropically gapped BCS type superconductivity with normalized gap ($Δ_0/k_BT_C$) values of 1.69 (Re$_7$B$_3$) and 1.75 (Re$_3$B). △ Less

Submitted 26 February, 2021; v1 submitted 26 November, 2020; originally announced November 2020.

Comments: 9 pages, 7 figures

Journal ref: Phys. Rev. B 103, 104507 (2021)

Field-induced quantum critical point in the new itinerant antiferromagnet Ti$_3$Cu$_4$

Authors: Jaime M. Moya, Alannah M. Hallas, Vaideesh Loganathan, C. -L. Huang, Lazar Kish, Adam A. Aczel, J. Beare, Y. Cai, G. M. Luke, Franziska Weickert, Andriy H. Nevidomskyy, Christos D. Malliakas, Mercouri G. Kanatzidis, Shiming Lei, Kyle Bayliff, E. Morosan

Abstract: New phases of matter emerge at the edge of magnetic instabilities. In local moment systems, such as heavy fermions, the magnetism can be destabilized by pressure, chemical doping, and, rarely, by magnetic field, towards a zero-temperature transition at a quantum critical point (QCP). Even more rare are instances of QCPs induced by pressure or doping in itinerant moment systems, with no known examp… ▽ More New phases of matter emerge at the edge of magnetic instabilities. In local moment systems, such as heavy fermions, the magnetism can be destabilized by pressure, chemical doping, and, rarely, by magnetic field, towards a zero-temperature transition at a quantum critical point (QCP). Even more rare are instances of QCPs induced by pressure or doping in itinerant moment systems, with no known examples of analogous field-induced \textit{T} = 0 transitions. Here we report the discovery of a new itinerant antiferromagnet with no magnetic constituents, in single crystals of Ti$_3$Cu$_4$ with $T_N$ = 11.3 K. Band structure calculations point to an orbital-selective, spin density wave ground state, a consequence of the square net structural motif in Ti$_3$Cu$_4$. A small magnetic field, $H_C$ = 4.87 T, suppresses the long-range order via a continuous second-order transition, resulting in a field-induced QCP. The magnetic Grüneisen ratio diverges as $H \rightarrow H_C$ and $T\rightarrow0$, with a sign change at $H_C$ and $T^{-1}$ scaling at $H~=~H_C$, providing evidence from thermodynamic measurements for quantum criticality for $H \parallel c$. Non-Fermi liquid (NFL) to Fermi liquid (FL) crossover is observed close to the QCP, as revealed by the power law behavior of the electrical resistivity. △ Less

Submitted 21 February, 2022; v1 submitted 26 October, 2020; originally announced October 2020.

Journal ref: Communications Physics volume 5, Article number: 136 (2022)

Characterization of a Disordered Above Room Temperature Skyrmion Material Co8Zn8Mn4

Authors: M. E. Henderson, J. Beare, S. Sharma, M. Bleuel, P. Clancy, D. G. Cory, M. G. Huber, C. A. Marjerrison, M. Pula, D. Sarenac, E. M. Smith, K. Zhernenkov, G. M. Luke, D. A. Pushin

Abstract: Topologically non trivial spin textures host great promise for future spintronic applications. Skyrmions in particular are of burgeoning interest owing to their nanometric size, topological protection, and high mobility via ultra-low current densities. It has been previously reported through magnetic susceptibility, microscopy, and scattering techniques that Co$_{8}$Zn$_{8}$Mn$_{4}$ forms an above… ▽ More Topologically non trivial spin textures host great promise for future spintronic applications. Skyrmions in particular are of burgeoning interest owing to their nanometric size, topological protection, and high mobility via ultra-low current densities. It has been previously reported through magnetic susceptibility, microscopy, and scattering techniques that Co$_{8}$Zn$_{8}$Mn$_{4}$ forms an above room temperature triangular skyrmion lattice. Here we report the synthesis procedure and characterization of a polycrystalline Co$_{8}$Zn$_{8}$Mn$_{4}$ bulk sample. We employ powder x-ray diffraction, backscatter Laue diffraction, and neutron diffraction as characterization tools of the crystallinity of the samples, while magnetic susceptibility and Small Angle Neutron Scattering (SANS) measurements are performed to study the skyrmion phase. Magnetic susceptibility measurements show a dip anomaly in the magnetization curves which persists over a range of approximately 305 K- 315 K. SANS measurements reveal a rotationally disordered polydomain skymrion lattice. Applying a recently developed symmetry-breaking magnetic field sequence, we were able to orient and order the previously jammed state to yield the prototypical hexagonal diffraction patterns, with secondary diffraction rings. △ Less

Submitted 21 October, 2020; originally announced October 2020.

Comments: 7 pages, 8 figures

Intertwined Magnetic Dipolar and Electric Quadrupolar Correlations in the Pyrochlore Tb$_2$Ge$_2$O$_7$

Authors: A. M. Hallas, W. Jin, J. Gaudet, E. M. Tonita, D. Pomaranski, C. R. C. Buhariwalla, M. Tachibana, N. P. Butch, S. Calder, M. B. Stone, G. M. Luke, C. R. Wiebe, J. B. Kycia, M. J. P. Gingras, B. D. Gaulin

Abstract: We present a comprehensive experimental and theoretical study of the pyrochlore Tb$_2$Ge$_2$O$_7$, an exemplary realization of a material whose properties are dominated by competition between magnetic dipolar and electric quadrupolar correlations. The dipolar and quadrupolar correlations evolve over three distinct regimes that we characterize via heat capacity, elastic and inelastic neutron scatte… ▽ More We present a comprehensive experimental and theoretical study of the pyrochlore Tb$_2$Ge$_2$O$_7$, an exemplary realization of a material whose properties are dominated by competition between magnetic dipolar and electric quadrupolar correlations. The dipolar and quadrupolar correlations evolve over three distinct regimes that we characterize via heat capacity, elastic and inelastic neutron scattering. In the first regime, above $T^*=1.1$ K, significant quadrupolar correlations lead to an intense inelastic mode that cannot be accounted for within a scenario with solely magnetic dipole-dipole correlations. The onset of extended dipole correlations occurs in the intermediate regime, between $T^*=1.1$ K and $T_c = 0.25$ K, with the formation of a collective paramagnetic state characterized by extended ferromagnetic canted spin ice domains. Here, long-range order is impeded not only by the usual frustration operating in classical spin ice systems, but also by a competition between dipolar and quadrupolar correlations. Finally, in the lowest temperature regime, below $T_c=0.25$ K, there is an abrupt and significant increase in the dipole ordered moment. The majority of the ordered moment remains tied up in the ferromagnetic spin ice-like state, but an additional $\mathbf{k}=(0,0,1)$ antiferromagnetic order parameter also develops. Simultaneously, the spectral weight of the inelastic mode, which is a proxy for the quadrupolar correlations, is observed to drop, indicating that dipole order ultimately wins out. Tb$_2$Ge$_2$O$_7$ is therefore a remarkable platform to study intertwined dipolar and quadrupolar correlations in a magnetically frustrated system and provides important insights into the physics of the whole family of terbium pyrochlores. △ Less

Submitted 30 September, 2020; v1 submitted 10 September, 2020; originally announced September 2020.

Multipolar magnetism in d-orbital systems: Crystal field levels, octupolar order, and orbital loop currents

Authors: Sreekar Voleti, Dalini D. Maharaj, Bruce D. Gaulin, Graeme Luke, Arun Paramekanti

Abstract: Quantum magnets with spin $J=2$, which arise in spin-orbit coupled Mott insulators, can potentially display multipolar orders. We carry out an exact diagonalization study of a simple octahedral crystal field Hamiltonian for two electrons, incorporating spin-orbit coupling (SOC) and interactions, finding that either explicitly including the $e_g$ orbitals, or going beyond the rotationally invariant… ▽ More Quantum magnets with spin $J=2$, which arise in spin-orbit coupled Mott insulators, can potentially display multipolar orders. We carry out an exact diagonalization study of a simple octahedral crystal field Hamiltonian for two electrons, incorporating spin-orbit coupling (SOC) and interactions, finding that either explicitly including the $e_g$ orbitals, or going beyond the rotationally invariant Coulomb interaction within the $t_{2g}$ sector, causes a degeneracy breaking of the $J\!=\!2$ level degeneracy. This can lead to a low-lying non-Kramers doublet carrying quadrupolar and octupolar moments and an excited triplet which supports magnetic dipole moments, bolstering our previous phenomenological proposal for the stabilization of ferro-octupolar order in heavy transition metal oxides. We show that the spontaneous time-reversal symmetry breaking due to ferro-octupolar ordering within the non-Kramers doublet leads to electronic orbital loop currents. The resulting internal magnetic fields can potentially explain the small fields inferred from muon-spin relaxation ($μ$SR) experiments on cubic $5d^2$ osmate double perovskites Ba$_2$ZnOsO$_6$, Ba$_2$CaOsO$_6$, and Ba$_2$MgOsO$_6$, which were previously attributed to weak dipolar magnetism. We make further predictions for oxygen NMR experiments on these materials. We also study the reversed level scheme, where the $J\!=\!2$ multiplet splits into a low-lying magnetic triplet and excited non-Kramers doublet, presenting single-ion results for the magnetic susceptibility in this case, and pointing out its possible relevance for the rhenate Ba$_2$YReO$_6$. Our work highlights the intimate connection between the physics of heavy transition metal oxides and that of $f$-electron based heavy fermion compounds. △ Less

Submitted 15 April, 2020; v1 submitted 13 February, 2020; originally announced February 2020.

Comments: 9 pages, 8 figures, published version

Journal ref: Phys. Rev. B 101, 155118 (2020)

Quantum critical point in the itinerant ferromagnet Ni$_{1-x}$Rh$_x$

Authors: C. -L. Huang, A. M. Hallas, K. Grube, S. Kuntz, B. Spiess, K. Bayliff, T. Besara, T. Siegrist, Y. Cai, J. Beare, G. M. Luke, E. Morosan

Abstract: We report a chemical substitution-induced ferromagnetic quantum critical point in polycrystalline Ni$_{1-x}$Rh$_x$ alloys. Through magnetization and muon spin relaxation measurements, we show that the ferromagnetic ordering temperature is suppressed continuously to zero at $x_{crit} = 0.375$ while the magnetic volume fraction remains 100% up to $x_{crit}$, pointing to a second order transition. No… ▽ More We report a chemical substitution-induced ferromagnetic quantum critical point in polycrystalline Ni$_{1-x}$Rh$_x$ alloys. Through magnetization and muon spin relaxation measurements, we show that the ferromagnetic ordering temperature is suppressed continuously to zero at $x_{crit} = 0.375$ while the magnetic volume fraction remains 100% up to $x_{crit}$, pointing to a second order transition. Non-Fermi liquid behavior is observed close to $x_{crit}$, where the electronic specific heat $C_{el}/T$ diverges logarithmically, while immediately above $x_{crit}$ the volume thermal expansion coefficient $α_{V}/T$ and the Grüneisen ratio $Γ= α_{V}/C_{el}$ both diverge logarithmically in the low temperature limit, further indication of a ferromagnetic quantum critical point in Ni$_{1-x}$Rh$_x$. △ Less

Submitted 15 January, 2020; originally announced January 2020.

Comments: 15 pages, 4 figures

Journal ref: Phys. Rev. Lett. 124, 117203 (2020)

Many-body recombination in insulating cuprates

Authors: Derek G. Sahota, Ruixing Liang, M. Dion, Patrick Fournier, Hanna A. Dąbkowska, Graeme M. Luke, J. Steven Dodge

Abstract: We study the pump-probe response of three insulating cuprates and develop a model for its recombination kinetics. The dependence on time, fluence, and both pump and probe photon energies imply many-body recombination on femtosecond timescales, characterized by anomalously large trapping and Auger coefficients. The fluence dependence follows a universal form that includes a characteristic volume sc… ▽ More We study the pump-probe response of three insulating cuprates and develop a model for its recombination kinetics. The dependence on time, fluence, and both pump and probe photon energies imply many-body recombination on femtosecond timescales, characterized by anomalously large trapping and Auger coefficients. The fluence dependence follows a universal form that includes a characteristic volume scale, which we associate with the holon-doublon excitation efficiency. This volume varies strongly with pump photon energy and peaks near twice the charge-transfer energy, suggesting that the variation is caused by carrier multiplication through impact ionization. △ Less

Submitted 3 December, 2019; originally announced December 2019.

Journal ref: Phys. Rev. Research 1, 033214 (2019)

Complex Transport and Magnetism in Inhomogeneous Mixed Valence Ce$_3$Ir$_4$Ge$_{13}$

Authors: A. M. Hallas, C. L. Huang, Binod K. Rai, A. Weiland, G. T. McCandless, Julia Y. Chan, J. Beare, G. M. Luke, E. Morosan

Abstract: We report the discovery of Ce$_3$Ir$_4$Ge$_{13}$, a new Remeika phase compound with a complex array of structural, electronic, and magnetic properties. Our single crystal x-ray diffraction measurements show that Ce$_3$Ir$_4$Ge$_{13}$ forms in the tetragonally distorted $I4_1/amd$ space group. The electrical resistivity is almost temperature independent over three decades in temperature, from 0.4 K… ▽ More We report the discovery of Ce$_3$Ir$_4$Ge$_{13}$, a new Remeika phase compound with a complex array of structural, electronic, and magnetic properties. Our single crystal x-ray diffraction measurements show that Ce$_3$Ir$_4$Ge$_{13}$ forms in the tetragonally distorted $I4_1/amd$ space group. The electrical resistivity is almost temperature independent over three decades in temperature, from 0.4 K to 400 K, while the Hall coefficient measurements are consistent with a low-carrier semimetal. Magnetic susceptibility measurements reveal an effective moment of $μ^{\text{exp}}_{\text{eff}} = 1.87 μ_B$/Ce, suggesting that this material has a mixture of magnetic Ce$^{3+}$ and non-magnetic Ce$^{4+}$. Upon cooling, Ce$_3$Ir$_4$Ge$_{13}$ first enters a short range magnetically ordered state below $T_{\text{SRO}}=10$ K, marked by a deviation from Curie-Weiss behavior in susceptibility and a broad field-independent heat capacity anomaly. At lower temperatures, we observe a second, sharper peak in the heat capacity at $T^* = 1.7$ K, concurrent with a splitting of the field-cooled and zero-field-cooled susceptibilities. A small resistivity drop at $T^*$ suggests a loss of spin disorder scattering consistent with a magnetic ordering or spin freezing transition. Ce$_3$Ir$_4$Ge$_{13}$ is therefore a rare example of an inhomogeneous mixed valence compound with a complex array of thermodynamic and transport properties. △ Less

Submitted 23 October, 2019; originally announced October 2019.

Comments: 8 pages, 6 figures, accepted for publication in Phys. Rev. Materials

Journal ref: Phys. Rev. Materials 3, 114407 (2019)

Intertwined magnetic, structural, and electronic transitions in V$_2$O$_3$

Authors: Benjamin A. Frandsen, Yoav Kalcheim, Ilya Valmianski, Alexander S. McLeod, Z. Guguchia, Sky C. Cheung, Alannah M. Hallas, Murray N. Wilson, Yipeng Cai, Graeme M. Luke, Z. Salman, A. Suter, T. Prokscha, Taito Murakami, Hiroshi Kageyama, D. N. Basov, Ivan K. Schuller, Yasutomo J. Uemura

Abstract: We present a coordinated study of the paramagnetic-to-antiferromagnetic, rhombohedral-to-monoclinic, and metal-to-insulator transitions in thin-film specimens of the classic Mott insulator V$_2$O$_3$ using low-energy muon spin relaxation, x-ray diffraction, and nanoscale-resolved near-field infrared spectroscopic techniques. The measurements provide a detailed characterization of the thermal evolu… ▽ More We present a coordinated study of the paramagnetic-to-antiferromagnetic, rhombohedral-to-monoclinic, and metal-to-insulator transitions in thin-film specimens of the classic Mott insulator V$_2$O$_3$ using low-energy muon spin relaxation, x-ray diffraction, and nanoscale-resolved near-field infrared spectroscopic techniques. The measurements provide a detailed characterization of the thermal evolution of the magnetic, structural, and electronic phase transitions occurring in a wide temperature range, including quantitative measurements of the high- and low-temperature phase fractions for each transition. The results reveal a stable coexistence of the high- and low-temperature phases over a broad temperature range throughout the transition. Careful comparison of temperature dependence of the different measurements, calibrated by the resistance of the sample, demonstrates that the electronic, magnetic, and structural degrees of freedom remain tightly coupled to each other during the transition process. We also find evidence for antiferromagnetic fluctuations in the vicinity of the phase transition, highlighting the important role of the magnetic degree of freedom in the metal-insulator transition. △ Less

Submitted 23 December, 2019; v1 submitted 22 October, 2019; originally announced October 2019.

Journal ref: Phys. Rev. B 100, 235136 (2019)

$μ$SR study of triangular Ising antiferromagnet ErMgGaO$_{4}$

Authors: Y. Cai, C. Lygouras, G. Thomas, M. N. Wilson, J. Beare, D. R. Yahne, K. Ross, Z. Gong, Y. J. Uemura, H. A. Dabkowska, G. M. Luke

Abstract: We present a detailed magnetic study of the triangular antiferromagnet ErMgGaO$_4$. A point charge calculation under the single ion approximation reveals a crystal field ground state doublet with a strong Ising-like behavior of the Er$^{3+}$ moment along the c axis. Magnetic susceptibility and specific heat measurements indicate no presence of magnetic transitions above 0.5~K and no evidence of re… ▽ More We present a detailed magnetic study of the triangular antiferromagnet ErMgGaO$_4$. A point charge calculation under the single ion approximation reveals a crystal field ground state doublet with a strong Ising-like behavior of the Er$^{3+}$ moment along the c axis. Magnetic susceptibility and specific heat measurements indicate no presence of magnetic transitions above 0.5~K and no evidence of residual entropy as temperature approaching zero. Zero field (ZF) $μ$SR measurements shows no sign of static uniform or random field and longitudinal field (LF) $μ$SR measurements exhibit persistent spin fluctuations down to our lowest temperature of 25~mK. Our results provide evidence of a quantum spin liquid state in the triangular antiferromagnet ErMgGaO$_4$. △ Less

Submitted 29 May, 2019; originally announced May 2019.

Journal ref: Phys. Rev. B 101, 094432 (2020)

Crystal fields and magnetic structure of the Ising antiferromagnet Er$_3$Ga$_5$O$_{12}$

Authors: Y. Cai, M. N. Wilson, J. Beare, C. Lygouras, G. Thomas, D. R. Yahne, K. Ross, K. M. Taddei, G. Sala, H. A. Dabkowska, A. A. Aczel, G. M. Luke

Abstract: Rare earth garnets are an exciting playground for studying the exotic magnetic properties of the frustrated hyperkagome lattice. Here we present a comprehensive study of the single ion and collective magnetic properties of the garnet Er$_3$Ga$_5$O$_{12}$. Using inelastic neutron scattering, we find a crystal field ground state doublet for Er$^{3+}$ with strong Ising anisotropy along local [100] ax… ▽ More Rare earth garnets are an exciting playground for studying the exotic magnetic properties of the frustrated hyperkagome lattice. Here we present a comprehensive study of the single ion and collective magnetic properties of the garnet Er$_3$Ga$_5$O$_{12}$. Using inelastic neutron scattering, we find a crystal field ground state doublet for Er$^{3+}$ with strong Ising anisotropy along local [100] axes. Magnetic susceptibility and heat capacity measurements provide evidence for long-range magnetic ordering with $T_N$~$=$~0.8~K, and no evidence for residual entropy is found when cooling through the ordering transition. Neutron powder diffraction reveals that the ground state spin configuration corresponds to the six-sublattice, Ising antiferromagnetic state ($Γ_3$) common to many of the rare earth garnets. However, we also found that $μ$SR appears to be insensitive to the ordering transition in this material, in which a low-temperature relaxation plateau was observed with no evidence of spontaneous muon precession. The combined muon and neutron results may be indicative of a dynamical ground state with a relatively long correlation time. Despite this potential complication, our work indicates that Er$_3$Ga$_5$O$_{12}$ is an excellent model system for studying the complex metamagnetism expected for a multi-axis antiferromagnet. △ Less

Submitted 22 October, 2019; v1 submitted 9 May, 2019; originally announced May 2019.

Journal ref: Phys. Rev. B 100, 184415 (2019)

Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce$_2$Zr$_2$O$_7$

Authors: J. Gaudet, E. M. Smith, J. Dudemaine, J. Beare, C. R. C. Buhariwalla, N. P. Butch, M. B. Stone, D. R. Yahne, K. A. Ross, C. A. Marjerrison, J. D. Garrett, G. M. Luke, A. D. Bianchi, B. D. Gaulin

Abstract: Neutron scattering measurements on the pyrochlore magnet Ce$_2$Zr$_2$O$_7$ reveal an unusual crystal field splitting of its lowest $J$=5/2 multiplet, such that its ground state doublet is composed of m$_J$=$\pm$3/2, giving these doublets a dipole - octupole (DO) character with local Ising anisotropy. Its magnetic susceptibility shows weak antiferromagnetic correlations with $θ_{CW}$=-0.4(2)K, lead… ▽ More Neutron scattering measurements on the pyrochlore magnet Ce$_2$Zr$_2$O$_7$ reveal an unusual crystal field splitting of its lowest $J$=5/2 multiplet, such that its ground state doublet is composed of m$_J$=$\pm$3/2, giving these doublets a dipole - octupole (DO) character with local Ising anisotropy. Its magnetic susceptibility shows weak antiferromagnetic correlations with $θ_{CW}$=-0.4(2)K, leading to a naive expectation of an All-In, All-Out ordered state at low temperatures. Instead our low energy inelastic neutron scattering measurements show a dynamic quantum spin ice state, with suppressed scattering near |$\textbf{Q}$|=0, and no long range order at low temperatures. This is consistent with recent theory predicting symmetry enriched U(1) quantum spin liquids for such DO doublets decorating the pyrochlore lattice. Finally, we show that disorder, especially oxidation of powder samples, is important in Ce$_2$Zr$_2$O$_7$ and could play an important role in the low temperature behaviour of this material. △ Less

Submitted 21 March, 2019; originally announced March 2019.

Comments: Submitted to APS journal on 11/28/2018

Journal ref: Phys. Rev. Lett. 122, 187201 (2019)

Coexistence of metallic and nonmetallic properties in the pyrochlore Lu$_2$Rh$_2$O$_7$

Authors: Alannah M. Hallas, Arzoo Z. Sharma, Cole Mauws, Qiang Chen, Haidong D. Zhou, Cui Ding, Zizhou Gong, Makoto Tachibana, Paul M. Sarte, J. Paul Attfield, Graeme M. Luke, Christopher R. Wiebe

Abstract: Transition metal oxides of the $4d$ and $5d$ block have recently become the targets of materials discovery, largely due to their strong spin-orbit coupling that can generate exotic magnetic and electronic states. Here we report the high pressure synthesis of Lu$_2$Rh$_2$O$_7$, a new cubic pyrochlore oxide based on $4d^5$ Rh$^{4+}$ and characterizations via thermodynamic, electrical transport, and… ▽ More Transition metal oxides of the $4d$ and $5d$ block have recently become the targets of materials discovery, largely due to their strong spin-orbit coupling that can generate exotic magnetic and electronic states. Here we report the high pressure synthesis of Lu$_2$Rh$_2$O$_7$, a new cubic pyrochlore oxide based on $4d^5$ Rh$^{4+}$ and characterizations via thermodynamic, electrical transport, and muon spin relaxation measurements. Magnetic susceptibility measurements reveal a large temperature-independent Pauli paramagnetic contribution, while heat capacity shows an enhanced Sommerfeld coefficient, $γ$ = 21.8(1) mJ/mol-Rh K$^2$. Muon spin relaxation measurements confirm that Lu$_2$Rh$_2$O$_7$ remains paramagnetic down to 2 K. Taken in combination, these three measurements suggest that Lu$_2$Rh$_2$O$_7$ is a correlated paramagnetic metal with a Wilson ratio of $R_W = 2.5$. However, electric transport measurements present a striking contradiction as the resistivity of Lu$_2$Rh$_2$O$_7$ is observed to monotonically increase with decreasing temperature, indicative of a nonmetallic state. Furthermore, although the magnitude of the resistivity is that of a semiconductor, the temperature dependence does not obey any conventional form. Thus, we propose that Lu$_2$Rh$_2$O$_7$ may belong to the same novel class of non-Fermi liquids as the nonmetallic metal FeCrAs. △ Less

Submitted 1 March, 2019; originally announced March 2019.

Comments: 11 pages, 5 figures

Journal ref: npj Quantum Materials, Volume 4, Article number: 9 (2019)

muSR and Magnetometry Study of the Type-I Superconductor BeAu

Authors: James Beare, Matthew Nugent, Murray Wilson, Yipeng Cai, Timothy Munsie, Alfred Amon, Andreas Leithe-Jasper, Zizhou Gong, Shengli Guo, Zurab Guguchia, Yuri Grin, Yasutomo Uemura, Eteri Svanidze, Graeme Luke

Abstract: We present muon spin rotation and relaxation (muSR) measurements as well as demagnetising field corrected magnetisation measurements on polycrystalline samples of the noncentrosymmetric superconductor BeAu. From muSR measurements in a transverse field, we determine that BeAu is a type-I superconductor with Hc = 256 Oe, amending the previous understanding of the compound as a type-II superconductor… ▽ More We present muon spin rotation and relaxation (muSR) measurements as well as demagnetising field corrected magnetisation measurements on polycrystalline samples of the noncentrosymmetric superconductor BeAu. From muSR measurements in a transverse field, we determine that BeAu is a type-I superconductor with Hc = 256 Oe, amending the previous understanding of the compound as a type-II superconductor. To account for demagnetising effects in magnetisation measurements, we produce an ellipsoidal sample, for which a demagnetisation factor can be calculated. After correcting for demagnetising effects, our magnetisation results are in agreement with our muSR measurements. Using both types of measurements we construct a phase diagram from T = 30 mK to Tc = 3.25 K. We then study the effect of hydrostatic pressure and find that 450 MPa decreases Tc by 34 mK, comparable to the change seen in type-I elemental superconductors Sn, In and Ta, suggesting BeAu is far from a quantum critical point accessible by the application of pressure. △ Less

Submitted 31 January, 2019; originally announced February 2019.

Comments: 10 pages, 8 figures

Journal ref: Phys. Rev. B 99, 134510 (2019)

Magnetic Monopole Noise

Authors: Ritika Dusad, Franziska K. K. Kirschner, Jesse C. Hoke, Benjamin Roberts, Anna Eyal, Felix Flicker, Graeme M. Luke, Stephen J. Blundell, J. C. Seamus Davis

Abstract: Magnetic monopoles are hypothetical elementary particles exhibiting quantized magnetic charge $m_0=\pm(h/μ_0e)$ and quantized magnetic flux $Φ_0=\pm h/e$. A classic proposal for detecting such magnetic charges is to measure the quantized jump in magnetic flux $Φ$ threading the loop of a superconducting quantum interference device (SQUID) when a monopole passes through it. Naturally, with the theor… ▽ More Magnetic monopoles are hypothetical elementary particles exhibiting quantized magnetic charge $m_0=\pm(h/μ_0e)$ and quantized magnetic flux $Φ_0=\pm h/e$. A classic proposal for detecting such magnetic charges is to measure the quantized jump in magnetic flux $Φ$ threading the loop of a superconducting quantum interference device (SQUID) when a monopole passes through it. Naturally, with the theoretical discovery that a plasma of emergent magnetic charges should exist in several lanthanide-pyrochlore magnetic insulators, including Dy$_2$Ti$_2$O$_7$, this SQUID technique was proposed for their direct detection. Experimentally, this has proven extremely challenging because of the high number density, and the generation-recombination (GR) fluctuations, of the monopole plasma. Recently, however, theoretical advances have allowed the spectral density of magnetic-flux noise $S_Φ(ω,T)$ due to GR fluctuations of $\pm m_*$ magnetic charge pairs to be determined. These theories present a sequence of strikingly clear predictions for the magnetic-flux noise signature of emergent magnetic monopoles. Here we report development of a high-sensitivity, SQUID based flux-noise spectrometer, and consequent measurements of the frequency and temperature dependence of $S_Φ(ω,T)$ for Dy$_2$Ti$_2$O$_7$ samples. Virtually all the elements of $S_Φ(ω,T)$ predicted for a magnetic monopole plasma, including the existence of intense magnetization noise and its characteristic frequency and temperature dependence, are detected directly. Moreover, comparisons of simulated and measured correlation functions $C_Φ(t)$ of the magnetic-flux noise $Φ(t)$ imply that the motion of magnetic charges is strongly correlated because traversal of the same trajectory by two magnetic charges of same sign is forbidden. △ Less

Submitted 24 April, 2019; v1 submitted 28 January, 2019; originally announced January 2019.

Journal ref: Nature (2019)

Probing the quantum phase transition in Mott insulator BaCoS_2 tuned by pressure and Ni-substitution

Authors: Z. Guguchia, B. A. Frandsen, D. Santos-Cottin, S. C. Cheung, Z. Gong, Q. Sheng, K. Yamakawa, A. M. Hallas, M. N. Wilson, Y. Cai, J. Beare, R. Khasanov, R. De Renzi, G. M. Luke, S. Shamoto, A. Gauzzi, Y. Klein, Y. J. Uemura

Abstract: We present a muon spin relaxation study of the Mott transition in BaCoS_2 using two independent control parameters: (i) pressure p to tune the electronic bandwidth and (ii) Ni-substitution x on the Co site to tune the band filling. For both tuning parameters, the antiferromagnetic insulating state first transitions to an antiferromagnetic metal and finally to a paramagnetic metal without undergoin… ▽ More We present a muon spin relaxation study of the Mott transition in BaCoS_2 using two independent control parameters: (i) pressure p to tune the electronic bandwidth and (ii) Ni-substitution x on the Co site to tune the band filling. For both tuning parameters, the antiferromagnetic insulating state first transitions to an antiferromagnetic metal and finally to a paramagnetic metal without undergoing any structural phase transition. BaCoS_2 under pressure displays minimal change in the ordered magnetic moment S_ord until it collapses abruptly upon entering the antiferromagnetic metallic state at p_cr ~ 1.3 GPa. In contrast, S_ord in the Ni-doped system Ba(Co_{1-x}Ni_{x})S_{2} steadily decreases with increasing x until the antiferromagnetic metallic region is reached at x_cr ~ 0.22. In both cases, significant phase separation between magnetic and nonmagnetic regions develops when approaching p_cr or x_cr, and the antiferromagnetic metallic state is characterized by weak, random, static magnetism in a small volume fraction. No dynamical critical behavior is observed near the transition for either tuning parameter. These results demonstrate that the quantum evolution of both the bandwidth- and filling-controlled metal-insulator transition at zero temperature proceeds as a first-order transition. This behavior is common to magnetic Mott transitions in RENiO_3 and V_2O_3, which are accompanied by structural transitions without the formation of an antiferromagnetic metal phase. △ Less

Submitted 23 January, 2019; originally announced January 2019.

Comments: 8 pages, 6 Figures

Journal ref: Phys. Rev. Materials 3, 045001 (2019)

Low-Temperature and Dynamic Magnetism of Highly Frustrated 5d2 Li4MgOsO6 Polymorphs in Comparison with 5d3 Li3Mg2OsO6

Authors: Gia T. Tran, Phuong-Hieu T. Nguyen, Charles J. Bloed, Michael E. Evans, Jamie A. Anczarski, William P. Martin, Jefferson Toro, Demetrios V. Papakostas, James Beare, Murray N. Wilson, John E. Greedan, Graeme M. Luke, Thomas Gredig, Jeremy P. Carlo, Shahab Derakhshan

Abstract: Geometric magnetic frustration (GMF) has attracted substantial interest due to the exotic physics and rich phase diagrams revealed by the cancellation of normally-dominant magnetic interactions, giving impetus for the search for novel frustrated systems, most often based on antiferromagnetic correlations between magnetic ions decorating triangular or tetrahedral lattices. We report here low-temper… ▽ More Geometric magnetic frustration (GMF) has attracted substantial interest due to the exotic physics and rich phase diagrams revealed by the cancellation of normally-dominant magnetic interactions, giving impetus for the search for novel frustrated systems, most often based on antiferromagnetic correlations between magnetic ions decorating triangular or tetrahedral lattices. We report here low-temperature magnetic susceptibility and muon spin relaxation results on Li4MgOsO6 and Li3Mg2OsO6, members of the A5BO6 "rock salt ordered" family of frustrated materials. In Li3Mg2OsO6 we find spin freezing below 12K. In Li4MgOsO6, which can crystallize into either orthorhombic Fddd or monoclinic C2/m crystal symmetries depending on synthesis conditions, we find magnetism consistent with glassy-like behavior dominating below 2K, with partial ordering and evidence for dynamics at somewhat higher temperatures. △ Less

Submitted 1 November, 2018; v1 submitted 12 September, 2018; originally announced September 2018.

Comments: 5 pages, 5 figures

Journal ref: Phys. Rev. B 98, 184401 (2018)

$μ$SR study of spin freezing and persistent spin dynamics in NaCaNi$_2$F$_7$

Authors: Y. Cai, M. N. Wilson, A. M. Hallas, L. Liu, B. A. Frandsen, S. R. Dunsiger, J. W. Krizan, R. J. Cava, Y. J. Uemura, O. Rubel, G. M. Luke

Abstract: A new pyrochlore compound, NaCaNi$_2$F$_7$, was recently synthesized and has a single magnetic site with spin-1 Ni$^{2+}$. We present zero field (ZF) and longitudinal field (LF) muon spin rotation ($μ$SR) measurements on this pyrochlore. Density functional theory (DFT) calculations show that the most likely muon site is located between two fluorine ions, but off-centre. A characteristic F-$μ$-F mu… ▽ More A new pyrochlore compound, NaCaNi$_2$F$_7$, was recently synthesized and has a single magnetic site with spin-1 Ni$^{2+}$. We present zero field (ZF) and longitudinal field (LF) muon spin rotation ($μ$SR) measurements on this pyrochlore. Density functional theory (DFT) calculations show that the most likely muon site is located between two fluorine ions, but off-centre. A characteristic F-$μ$-F muon spin polarization function is observed at high temperatures where Ni spin fluctuations are sufficiently rapid. The Ni$^{2+}$ spins undergo spin freezing into a disordered ground state below 4~K, with a characteristic internal field strength of 140~G. Persistent Ni spin dynamics are present to our lowest temperatures (75~mK), a feature characteristic of many geometrically frustrated magnetic systems. △ Less

Submitted 28 June, 2018; originally announced June 2018.

Dipolar-Octupolar Ising Antiferromagnetism in Sm$_2$Ti$_2$O$_7$: A Moment Fragmentation Candidate

Authors: C. Mauws, A. M. Hallas, G. Sala, A. A. Aczel, P. M. Sarte, J. Gaudet, D. Ziat, J. A. Quilliam, J. A. Lussier, M. Bieringer, H. D. Zhou, A. Wildes, M. B. Stone, D. Abernathy, G. M. Luke, B. D. Gaulin, C. R. Wiebe

Abstract: Over the past two decades, the magnetic ground states of all rare earth titanate pyrochlores have been extensively studied, with the exception of Sm$_2$Ti$_2$O$_7$. This is, in large part, due to the very high absorption cross-section of naturally-occurring samarium, which renders neutron scattering infeasible. To combat this, we have grown a large, isotopically-enriched single crystal of Sm$_2$Ti… ▽ More Over the past two decades, the magnetic ground states of all rare earth titanate pyrochlores have been extensively studied, with the exception of Sm$_2$Ti$_2$O$_7$. This is, in large part, due to the very high absorption cross-section of naturally-occurring samarium, which renders neutron scattering infeasible. To combat this, we have grown a large, isotopically-enriched single crystal of Sm$_2$Ti$_2$O$_7$. Using inelastic neutron scattering, we determine that the crystal field ground state for Sm$^{3+}$ is a dipolar-octupolar doublet with Ising anisotropy. Neutron diffraction experiments reveal that Sm$_2$Ti$_2$O$_7$ orders into the all-in, all-out magnetic structure with an ordered moment of 0.44(7) $μ_B$ below $T_N=0.35$ K, consistent with expectations for antiferromagnetically-coupled Ising spins on the pyrochlore lattice. Zero-field muon spin relaxation measurements reveal an absence of spontaneous oscillations and persistent spin fluctuations down to 0.03 K. The combination of the dipolar-octupolar nature of the Sm$^{3+}$ moment, the all-in, all-out ordered state, and the low-temperature persistent spin dynamics make this material an intriguing candidate for moment fragmentation physics. △ Less

Submitted 23 May, 2018; originally announced May 2018.

Comments: 5 pages, 4 figures. Supplemental Material

Journal ref: Phys. Rev. B 98, 100401 (2018)

Low-carrier density and fragile magnetism in a Kondo lattice system

Authors: Binod K. Rai, Iain W. H. Oswald, Wenjing Ban, C. -L. Huang, V. Loganathan, A. M. Hallas, M. N. Wilson, G. M. Luke, L. Harriger, Q. Huang, Y. Li, Sami Dzsaber, Julia Y. Chan, N. L. Wang, Silke Paschen, J. W. Lynn, Andriy H. Nevidomskyy, P. Dai, Q. Si, E. Morosan

Abstract: Kondo-based semimetals and semiconductors are of extensive current interest as a viable platform for strongly correlated states. It is thus important to understand the routes towards such dilute-carrier correlated states. One established pathway is through Kondo effect in metallic non-magnetic analogues. Here we advance a new mechanism, through which Kondo-based semimetals develop out of conductio… ▽ More Kondo-based semimetals and semiconductors are of extensive current interest as a viable platform for strongly correlated states. It is thus important to understand the routes towards such dilute-carrier correlated states. One established pathway is through Kondo effect in metallic non-magnetic analogues. Here we advance a new mechanism, through which Kondo-based semimetals develop out of conduction electrons with a low carrier-density in the presence of an even number of rare-earth sites. We demonstrate this effect by studying the Kondo material Yb3Ir4Ge13 along with its closed-f-shell counterpart, Lu3Ir4Ge13. Through magnetotransport, optical conductivity and thermodynamic measurements, we establish that the correlated semimetallic state of Yb3Ir4Ge13 below its Kondo temperature originates from the Kondo effect of a low carrier conduction-electron background. In addition, it displays fragile magnetism at very low temperatures, which, in turn, can be tuned to a non Fermi liquid regime through Lu-for-Yb substitution. These findings are connected with recent theoretical studies in simplified models. Our results open an entirely new venue to explore the strong correlation physics in a semimetallic environment. △ Less

Submitted 20 August, 2018; v1 submitted 4 May, 2018; originally announced May 2018.

Journal ref: Phys. Rev. B 99, 085120 (2019)