arXiv subjects

T. M. McQueen

Publications and source records attributed to T. M. McQueen.

At least 37 records · Page 2Linked to original sources

arXiv2018

Single crystal growth of Cu4(OH)6BrF and universal behavior in quantum spin liquid candidates synthetic barlowite and herbertsmithite

Synthetic barlowite, Cu4(OH)6BrF, has emerged as a new quantum spin liquid (QSL) host, containing kagome layers of S=1/2 Cu2+ ions separated by interlayer Cu2+ ions. Similar to synthetic herbertsmithite, ZnCu3(OH)6Cl2, it has been reported that Zn2+ substitution for the interlayer Cu2+ induces a QSL ground state. Here we report a scalable synthesis of single crystals of Cu4(OH)6BrF. Through x-ray, neutron, and electron diffraction measurements coupled with magic angle spinning 19F and 1H NMR spectroscopy, we resolve the previously reported positional disorder of the interlayer Cu2+ ions and find that the structure is best described in the orthorhombic space group, Cmcm, with lattice parameters a = 6.665(13) A, b = 11.521(2) A, c = 9.256(18) A and an ordered arrangement of interlayer Cu2+ ions. Infrared spectroscopy measurements of the O-H and F-H stretching frequencies demonstrate that the orthorhombic symmetry persists upon substitution of Zn2+ for Cu2+. Specific heat and magnetic susceptibility measurements of Zn-substituted barlowite, ZnxCu4-x(OH)6BrF, reveal striking similarities with the behavior of ZnxCu4-x(OH)6Cl2. These parallels imply universal behavior of copper kagome lattices even in the presence of small symmetry breaking distortions. Thus synthetic barlowite demonstrates universality of the physics of synthetic Cu2+ kagome minerals and furthers the development of real QSL states.

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arXiv2017

Impurities or a neutral Fermi surface? A further examination of the low-energy ac optical conductivity of SmB$_6$

Recent experiments have uncovered evidence of low energy excitations in the bulk of SmB$_6$ that are perhaps associated with unconventional quasiparticles, bringing into question whether this Kondo "insulator" is truly insulating in the bulk. Recently, we demonstrated that SmB$_6$ possesses significant in-gap bulk ac conduction far in excess of typical disordered semiconductors. Whether such conduction is an intrinsic feature of SmB$_6$, suggesting the formation of an exotic state, or residual conduction from impurities continues to be a topic of debate. Here, we further examine the origin of the ac optical conductivity of SmB$_6$ in light of recent experimental and theoretical developments. The optical conductivity of SmB$_6$ is shown to possess distinct regimes of either dominant free carrier or $localized$ response contributions. The free carrier response is found to be in good qualitative agreement with previous literature, although quantitative differences are revealed and discussed. The localized response, which dominates at the lowest temperatures, is analyzed in the context of models of either in-gap impurity states or an exotic neutral Fermi surface. The charge density or effective mass of this low temperature in-gap conductivity is extracted through a conductivity sum rule analysis and found to be in general alignment with both models in the appropriate limits. Our results shed further light on the nature of the in-gap states of this remarkable material.

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arXiv2017

Ballistic magnon heat conduction and possible Poiseuille flow in the helimagnetic insulator Cu$_2$OSeO$_3$

We report on the observation of magnon thermal conductivity $κ_m\sim$ 70 W/mK near 5 K in the helimagnetic insulator Cu$_2$OSeO$_3$, exceeding that measured in any other ferromagnet by almost two orders of magnitude. Ballistic, boundary-limited transport for both magnons and phonons is established below 1 K, and Poiseuille flow of magnons is proposed to explain a magnon mean-free path substantially exceeding the specimen width for the least defective specimens in the range 2 K $<T<$ 10 K. These observations establish Cu$_2$OSeO$_3$ as a model system for studying long-wavelength magnon dynamics.

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arXiv2017

Low energy magnon dynamics and magneto-optics of the skyrmionic Mott insulator Cu$_2$OSeO$_3$

In this work, we present a comprehensive study of the low energy optical magnetic response of the skyrmionic Mott insulator Cu$_2$OSeO$_3$ via high resolution time-domain THz spectroscopy. In zero field, a new magnetic excitation not predicted by spin-wave theory with frequency $f$ = 2.03 THz is observed and shown, with accompanying time-of-flight neutron scattering experiments, to be a zone folded magnon from the $\mathrm{R}$ to $\mathrmΓ$ points of the Brillouin zone. Highly sensitive polarimetry experiments performed in weak magnetic fields, $μ_0$H $<$ 200 mT, observe Faraday and Kerr rotations which are proportional to the sample magnetization, allowing for optical detection of the skyrmion phase and construction of a magnetic phase diagram. From these measurements, we extract a critical exponent of $β$ = 0.35 $\pm$ 0.04, in good agreement with the expected value for the 3D Heisenberg universality class of $β$ = 0.367. In large magnetic fields, $μ_0$H $>$ 5 T, we observe the magnetically active uniform mode of the ferrimagnetic field polarized phase whose dynamics as a function of field and temperature are studied. In addition to extracting a $g_\text{eff}$ = 2.08 $\pm$ 0.03, we observe the uniform mode to decay through a non-Gilbert damping mechanism and to possesses a finite spontaneous decay rate, $Γ_0$ $\approx$ 25 GHz, in the zero temperature limit. Our observations are attributed to Dzyaloshinkii-Moriya interactions, which have been proposed to be exceptionally strong in Cu$_2$OSeO$_3$ and are expected to impact the low energy magnetic response of such chiral magnets.

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arXiv2017

Disordered Route to the Coulomb Quantum Spin Liquid: Random Transverse Fields on Spin Ice in Pr$_2$Zr$_2$O$_7$

Inelastic neutron scattering reveals a broad continuum of excitations in Pr$_2$Zr$_2$O$_7$, the temperature and magnetic field dependence of which indicate a continuous distribution of quenched transverse fields ($Δ$) acting on the non-Kramers Pr$^{3+}$ crystal field ground state doublets. Spin-ice correlations are apparent within 0.2 meV of the Zeeman energy. A random phase approximation provides an excellent account of the data with a transverse field distribution $ρ(Δ)\propto (Δ^2+Γ^2)^{-1}$ where $ Γ=0.27(1)$ meV. Established during high temperature synthesis due to an underlying structural instability, it appears disorder in Pr$_2$Zr$_2$O$_7$ actually induces a quantum spin liquid.

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arXiv2017

Impact of Stoichiometry of Yb2Ti2O7 on its Physical Properties

A series of Yb2Ti2O7 doped samples demonstrates the effects of off-stoichiometry on Yb2Ti2O7's structure, properties, and magnetic ground state via x-ray diffraction, specific heat, and magnetization measurements. A stoichiometric single crystal of Yb2Ti2O7 grown by the traveling solvent floating zone technique (solvent = 30 wt% rutile TiO2 and 70 wt% Yb2Ti2O7) is characterized and evaluated in light of this series. Our data shows that upon positive x doping, the cubic lattice parameter a increases and the Curie-Weiss temperature decreases. Heat capacity measurements of stoichiometric Yb2Ti2O7 samples exhibit a sharp, first-order peak at T = 268(4) mK that is suppressed in magnitude and temperature in samples doped off ideal stoichiometry. The full entropy recovered per Yb ion is 5.7 J/K ~ Rln2. Our work establishes the effects of doping on Yb2Ti2O7's physical properties, which provides further evidence indicating that previous crystals grown by the traditional floating zone method are doped off ideal stoichiometry. Additionally, we present how to grow high-quality colorless single crystals of Yb2Ti2O7 by the traveling solvent floating zone growth method.

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arXiv2017

Rearrangement of Van-der-Waals Stacking and Formation of a Singlet State at $T = 90$ K in a Cluster Magnet

Insulating Nb$_3$Cl$_8$ is a layered chloride consisting of two-dimensional triangular layers of $S_{eff}$ = 1/2 Nb$_3$Cl$_{13}$ clusters at room temperature. Magnetic susceptibility measurement show a sharp, hysteretic drop to a temperature independent value below $T = 90$ K. Specific heat measurements show that the transition is first order, with $ΔS \approx 5\ \mathrm{J \cdot K^{-1} \cdot mol\ \mathit{f.u.}^{-1}}$, and a low temperature $T$-linear contribution originating from defect spins. Neutron and X-ray diffraction show a lowering of symmetry from trigonal $P\bar{3}m1$ to monoclinic $C2/m$ symmetry, with a change in layer stacking from -AB-AB- to -AB$^\prime$-BC$^\prime$-CA$^\prime$- and no observed magnetic order. This lowering of symmetry and rearrangement of successive layers evades geometric magnetic frustration to form a singlet ground state. It is the lowest temperature at which a change in stacking sequence is known to occur in a Van-der-Waals solid, occurs in the absence of orbital degeneracies, and suggests that designer 2-D heterostructures may be able to undergo similar phase transitions.

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arXiv2016

Electron Doping a Kagome Spin Liquid

Herbertsmithite, ZnCu$_3$(OH)$_6$Cl$_2$, is a two dimensional kagomé lattice realization of a spin liquid, with evidence for fractionalized excitations and a gapped ground state. Such a quantum spin liquid has been proposed to underlie high temperature superconductivity and is predicted to produce a wealth of new states, including a Dirac metal at $1/3$rd electron doping. Here we report the topochemical synthesis of electron-doped ZnLi$_x$Cu$_3$(OH)$_6$Cl$_2$ from $x$ = 0 to $x$ = 1.8 ($3/5$th per Cu$^{2+}$). Contrary to expectations, no metallicity or superconductivity is induced. Instead, we find a systematic suppression of magnetic behavior across the phase diagram. Our results demonstrate that significant theoretical work is needed to understand and predict the role of doping in magnetically frustrated narrow band insulators, particularly the interplay between local structural disorder and tendency toward electron localization, and pave the way for future studies of doped spin liquids.

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arXiv2016

Anomalous 3D bulk AC conduction within the Kondo gap of SmB$_6$ single crystals

The Kondo insulator SmB$_6$ has long been known to display anomalous transport behavior at low temperatures, T$<5$ K. In this temperatures range, a plateau is observed in the dc resistivity, contrary to the exponential divergence expected for a gapped system. Recent theoretical calculations suggest that SmB$_6$ may be the first topological Kondo insulator (TKI) and propose that the residual conductivity is due to topological surface states which reside within the Kondo gap. Since the TKI prediction many experiments have claimed to observe high mobility surface states within a perfectly insulating hybridization gap. Here, we investigate the low energy optical conductivity within the hybridization gap of single crystals of SmB$_6$ via time domain terahertz spectroscopy. Samples grown by both optical floating zone and aluminum flux methods are investigated to probe for differences originating from sample growth techniques. We find that both samples display significant 3D bulk conduction originating within the Kondo gap. Although SmB$_6$ may be a bulk dc insulator, it shows significant bulk ac conduction that is many orders of magnitude larger than any known impurity band conduction. The nature of these in-gap states and their coupling with the low energy spin excitons of SmB$_6$ is discussed. Additionally, the well defined conduction path geometry of our optical experiments allows us to show that any surface states, which lie below our detection threshold if present, must have a sheet resistance of R$/\square \ge$ 1000 $Ω$.

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arXiv2016

Electronic tunability of the frustrated triangular-lattice cluster magnet LiZn$_{2-x}$Mo$_3$O$_8$

LiZn$_2$Mo$_3$O$_8$ is an electrically insulating geometrically frustrated antiferromagnet in which inorganic Mo$_3$O$_{13}$ clusters each behaves as a single $S = 1/2$ unit, with the clusters arranged on a two-dimensional triangular lattice. Prior results have shown that LiZn$_2$Mo$_3$O$_8$ does not exhibit static magnetic order down to at least $T = 0.05\,K$, and instead possesses a valence bond ground state. Here, we show that LiZn$_2$Mo$_3$O$_8$ can be hole doped by oxidation with $\mathrm{I}_2$ and subsequent removal of $\mathrm{Zn}^{2+}$ cations to access the entire range of electron count, from one to zero unpaired electrons per site on the triangular lattice. Contrary to expectations, no metallic state is induced; instead, the primary effect is to suppress the number of sites contributing to the condensed valence-bond state. Further, diffraction and pair-distribution function analysis show no evidence for local Jahn-Teller distortions or other deviations from the parent trigonal symmetry as a function of doping or temperature. Taken together, the data and density functional theory calculations indicate that removal of electrons from the magnetic layers favors Anderson localization of the resulting hole and an increase in the electrical band-gap over the formation of a metallic and superconducting state. These results put strong constraints on the chemical conditions necessary to realize metallic states from parent insulating geometrically frustrated antiferromagnets.

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arXiv2016

NaSrMn2F7, NaCaFe2F7, and NaSrFe2F7: novel single crystal pyrochlore antiferromagnets

The crystal structures and magnetic properties of three previously unreported A2B2F7 pyrochlore materials, NaSrMn2F7, NaCaFe2F7, and NaSrFe2F7 are presented. In these compounds, either S=2 Fe2+ or S=5/2 Mn2+ is on the B site, while nonmagnetic Na and Ca (Na and Sr) are disordered on the A site. The materials, which were grown as crystals via the floating zone method, display high effective magnetic moments and large Curie-Weiss thetas. Despite these characteristics, freezing of the magnetic spins, characterized by peaks in the susceptibility or specific heat, is not observed until low temperatures. The empirical frustration index, f=- θcw/Tf, for the materials are 36 (NaSrMn2F7), 27 (NaSrFe2F7), and 19 (NaCaFe2F7). AC susceptibility, DC susceptibility, and heat capacity measurements are used to characterize the observed spin glass behavior. The results suggest that the compounds are frustrated pyrochlore antiferromagnets with weak bond disorder. The magnetic phenomena that these fluoride pyrochlores exhibit, in addition to their availability as relatively large single crystals, make them promising candidates for the study of geometric magnetic frustration.

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arXiv2016

Antiferromagnetic and Orbital Ordering on a Diamond Lattice Near Quantum Criticality

We present neutron scattering measurements on powder samples of the spinel FeSc2S4 that reveal a previously unobserved magnetic ordering transition occurring at 11.8(2)~K. Magnetic ordering occurs subsequent to a subtle cubic-to-tetragonal structural transition which distorts Fe coordinating sulfur tetrahedra lifting the orbital degeneracy. The application of 1~GPa hydrostatic pressure appears to destabilize this Néel state, reducing the transition temperature to 8.6(8)~K and redistributing magnetic spectral weight to higher energies. The relative magnitudes of ordered $\langle m \rangle^2\!=\!3.1(2)$ and fluctuating moments $\langle δm \rangle^2\!=\!13(1)$ show that the magnetically ordered ground state of FeSc2S4 is drastically renormalized and in proximity to criticality.

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arXiv2015

On the Chemistry and Physical Properties of Flux and Floating Zone Grown SmB6 Single Crystals

Recent theoretical and experimental findings suggest that the long-known but not well understood low temperature resistance plateau of SmB6 may originate from protected surface states arising from a topologically non-trivial bulk band structure having strong Kondo hybridization. Yet other studies have ascribed this feature to impurity phases, sample vacancies, and surface reconstructions. Given the typical methods used to prepare SmB6 single crystals, the flux and floating zone procedures, these ascriptions should not be taken lightly. Here, we demonstrate how compositional variations and observable amounts of impurity phases in SmB6 crystals grown by floating zone and flux affect the physical properties. From neutron diffraction and X-ray computed tomography experiments, we observe that a 154Sm11B6 crystal prepared using aluminum flux contains co-crystallized, epitaxial aluminum. A large, nearly stoichiometric crystal of SmB6 was successfully grown using the float-zone technique; upon continuing the zone melting, samarium vacancies are introduced. These samarium vacancies drastically alter the resistance and plateauing magnitude of the low temperature resistance compared to stoichiometric SmB6. These results highlight that small presences of impurity phases and compositional variations must be considered when collecting and analyzing physical property data of SmB6. Finally, a more accurate samarium-154 coherent neutron scattering length value, 8.9(1) fm, is reported.

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arXiv2015

Block magnetic excitations in the orbitally selective Mott insulator BaFe2Se3

Iron pnictides and selenides display a variety of unusual magnetic phases originating from the interplay between electronic, orbital, and lattice degrees of freedom. Using powder inelastic neutron scattering on the two-leg ladder BaFe2Se3, we fully characterize the static and dynamic spin correlations associated with the Fe4 block state, an exotic magnetic ground state observed in this low-dimensional magnet and in Rb0.89Fe1.58Se2. All the magnetic excitations of the Fe4 block state predicted by an effective Heisenberg model with localized spins are observed below 300 meV and quantitatively reproduced. However, the data only account for 16 mub^2 per Fe2+, approximatively 2/3 of the total spectral weight expected for localized S=2 moments. Our results highlight how orbital degrees of freedom in iron-based magnets can conspire to stabilize an exotic magnetic state.

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arXiv2015

Heat capacity anomaly at the quantum critical point of the Transverse Ising Magnet CoNb_2O_6

The transverse Ising magnet Hamiltonian describing the Ising chain in a transverse magnetic field is the archetypal example of a system that undergoes a transition at a quantum critical point (QCP). The columbite CoNb$_2$O$_6$ is the closest realization of the transverse Ising magnet found to date. At low temperatures, neutron diffraction has observed a set of discrete collective spin modes near the QCP. We ask if there are low-lying spin excitations distinct from these relatively high energy modes. Using the heat capacity, we show that a significant band of gapless spin excitations exists. At the QCP, their spin entropy rises to a prominent peak that accounts for 30$\%$ of the total spin degrees of freedom. In a narrow field interval below the QCP, the gapless excitations display a fermion-like, temperature-linear heat capacity below 1 K. These novel gapless modes are the main spin excitations participating in, and affected, by the quantum transition.

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arXiv2015

Disorder from order among anisotropic next-nearest-neighbor Ising spin chains in SrHo$_2$O$_4$

We describe why Ising spin chains with competing interactions in $\rm SrHo_2O_4$ segregate into ordered and disordered ensembles at low temperatures ($T$). Using elastic neutron scattering, magnetization, and specific heat measurements, the two distinct spin chains are inferred to have Néel ($\uparrow\downarrow\uparrow\downarrow$) and double-Néel ($\uparrow\uparrow\downarrow\downarrow$) ground states respectively. Below $T_\mathrm{N}=0.68(2)$~K, the Néel chains develop three dimensional (3D) long range order (LRO), which arrests further thermal equilibration of the double-Néel chains so they remain in a disordered incommensurate state for $T$ below $T_\mathrm{S}= 0.52(2)$~K. $\rm SrHo_2O_4$ distills an important feature of incommensurate low dimensional magnetism: kinetically trapped topological defects in a quasi$-d-$dimensional spin system can preclude order in $d+1$ dimensions.

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arXiv2015

Superconducting Dome and Crossover to an Insulating State in [Tl4]Tl1-xSnxTe3

The structural, superconducting, and electronic phase diagram of [Tl4]Tl1-xSnxTe3 is reported. Magnetization and specific heat measurements show bulk superconductivity exists for 0 < x < 0.4. Resistivity measurements indicate a crossover from a metallic state for low dopings to a doped insulator at x = 1. Universally, there is a large non-Debye specific heat contribution, characterized by an Einstein temperature of θE ~ 35 K. Density functional theory calculations predict x = 0 to be a topological metal, while x = 1 is a topological crystalline insulator. The disappearance of superconductivity correlates with the transition between these distinct topological states.

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arXiv2015

Interaction Driven Subgap Spin Exciton in the Kondo Insulator SmB6

Using inelastic neutron scattering, we map a 14 meV coherent resonant mode in the topological Kondo insulator SmB6 and describe its relation to the low energy insulating band structure. The resonant intensity is confined to the X and R high symmetry points, repeating outside the first Brillouin zone and dispersing less than 2 meV, with a 5d-like magnetic form factor. We present a slave-boson treatment of the Anderson Hamiltonian with a third neighbor dominated hybridized band structure. This approach produces a spin exciton below the charge gap with features that are consistent with the observed neutron scattering. We find that maxima in the wave vector dependence of the inelastic neutron scattering indicate band inversion.

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