B. D. Gaulin - Department of Physics and Astronomy, McMaster University, Hamilton, Ontario, Canada

B. D. Gaulin
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B. D. Gaulin
Department of Physics and Astronomy, McMaster University, Hamilton, Ontario, Canada

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Physics - Strongly Correlated Electrons (46)
Physics - Superconductivity (7)
Physics - Materials Science (6)
Physics - Disordered Systems and Neural Networks (3)
Physics - Other (2)
Physics - Instrumentation and Detectors (1)

Publications Authored By B. D. Gaulin

We report neutron scattering measurements on Er$_2$Pt$_2$O$_7$, a new addition to the XY family of frustrated pyrochlore magnets. Symmetry analysis of our elastic scattering data shows that Er$_2$Pt$_2$O$_7$ is the first XY pyrochlore to order into the $k=0$, $\Gamma_7$ magnetic structure (the Palmer-Chalker state), at $T_N = 0.38$ K. Read More

A quantum spin liquid is a novel state of matter characterized by quantum entanglement and the absence of any broken symmetry. In condensed matter, the frustrated rare-earth pyrochlore magnets Ho$_2$Ti$_2$O$_7$ and Dy$_2$Ti$_2$O$_7$, so-called spin ices, exhibit a classical spin liquid state with fractionalized thermal excitations (magnetic monopoles). Evidence for a quantum spin ice, in which the magnetic monopoles become long range entangled and an emergent quantum electrodynamics arises, seems within reach. Read More

The XY pyrochlore antiferromagnet Er$_2$Ti$_2$O$_7$ exhibits a rare case of $Z_6$ discrete symmetry breaking in its $\psi_2$ magnetic ground state. Despite being well-studied theoretically, systems with high discrete symmetry breakings are uncommon in nature and, thus, Er$_2$Ti$_2$O$_7$ provides an experimental playground for the study of broken $Z_n$ symmetry, for $n>2$. A recent theoretical work examined the effect of a magnetic field on a pyrochlore lattice with broken $Z_6$ symmetry and applied it to Er$_2$Ti$_2$O$_7$. Read More

Below $T_N = 1.1$K, the XY pyrochlore Er$_2$Ti$_2$O$_7$ orders into a $k=0$ non-collinear, antiferromagnetic structure referred to as the $\psi_2$ state. The magnetic order in Er$_2$Ti$_2$O$_7$ is known to obey conventional three dimensional (3D) percolation in the presence of magnetic dilution, and in that sense is robust to disorder. Read More

The ytterbium pyrochlore magnets, Yb2B2O7 (B = Sn, Ti, Ge) are well described by S_eff = 1/2 quantum spins decorating a network of corner-sharing tetrahedra and interacting via anisotropic exchange. Structurally, only the non-magnetic B-site cation, and hence, primarily the lattice parameter, is changing across the series. Nonetheless, a range of magnetic behaviors are observed: the low temperature magnetism in Yb2Ti2O7 and Yb2Sn2O7 has ferromagnetic character, while Yb2Ge2O7 displays an antiferromagnetically ordered Neel state at low temperatures. Read More

We report neutron scattering and muon spin relaxation measurements (muSR) on the pyrochlore antiferromagnet Yb2Ge2O7. Inelastic neutron scattering was used to probe the transitions between crystal electric field levels, allowing us to determine the eigenvalues and eigenvectors appropriate to the J=7/2 Yb3+ ion in this environment. The crystal electric field ground state doublet in Yb2Ge2O7 corresponds primarily to m_J = +/- 1/2 with local XY anisotropy, consistent with an S_eff = 1/2 description for the Yb moments. Read More

The ground state of the quantum spin ice candidate magnet Yb2Ti2O7 is known to be sensitive to weak disorder at the 1 percent level which occurs in single crystals grown from the melt. Powders produced by solid state synthesis tend to be stoichiometric and display large and sharp heat capacity anomalies at relatively high temperatures, with Tc about 0.26 K. Read More

The application of a magnetic field transverse to the easy axis, Ising direction in the quasi-two-dimensional Kagome staircase magnet, Co3V2O8, induces three quantum phase transitions at low temperatures, ultimately producing a novel high field polarized state, with two distinct sublattices. New time-of-flight neutron scattering techniques, accompanied by large angular access, high magnetic field infrastructure allow the mapping of a sequence of ferromagnetic and incommensurate phases and their accompanying spin excitations. At least one of the transitions to incommensurate phases at \mu 0Hc1~6. Read More

Recent low temperature heat capacity (C$_P$) measurements on polycrystalline samples of the pyrochlore antiferromagnet Tb$_{2+x}$Ti$_{2-x}$O$_{7+\delta}$ have shown a strong sensitivity to the precise Tb concentration $x$, with a large anomaly exhibited for $x \sim 0.005$ at $T_C \sim 0.5$ K and no such anomaly and corresponding phase transition for $x \le 0$. Read More

Time-of-flight neutron spectroscopy has been used to determine the crystalline electric field (CEF) Hamiltonian, eigenvalues and eigenvectors appropriate to the $J$ = 7/2 Yb$^{3+}$ ion in the candidate quantum spin ice pyrochlore magnet $\rm Yb_2Ti_2O_7$. The precise ground state (GS) of this exotic, geometrically-frustrated magnet is known to be sensitive to weak disorder associated with the growth of single crystals from the melt. Such materials display weak "stuffing" wherein a small proportion, $\approx$ 2\%, of the non-magnetic Ti$^{4+}$ sites are occupied by excess Yb$^{3+}$. Read More

Solid-solutions of the "soft" quantum spin ice pyrochlore magnets Tb2B2O7 with B=Ti and Sn display a novel magnetic ground state in the presence of strong B-site disorder, characterized by a low susceptibility and strong spin fluctuations to temperatures below 0.1 K. These materials have been studied using ac-susceptibility and muSR techniques to very low temperatures, and time-of-flight inelastic neutron scattering techniques to 1. Read More

The Ho2Ti2O7, Er2Ti2O7 and Yb2Ti2O7 pyrochlores were studied by synchrotron X-ray diffraction to determine whether the (002) peak, forbidden in the pyrochlore space group Fd-3m but observed in single crystal neutron scattering measurements, is present due to a deviation of their pyrochlore structure from Fd-3m symmetry. Synchrotron diffraction measurements on precisely synthesized stoichiometric and non-stoichiometric powders and a crushed floating zone crystal of Ho2Ti2O7 revealed that the (002) reflection is absent in all cases to a sensitivity of approximately one part in 30,000 of the strongest X-ray diffraction peak. This indicates to high sensitivity that the structural space group of these rare earth titanate pyrochlores is Fd-3m, and that thus the (002) peak observed in the neutron scattering experiments has a non-structural origin. Read More

An important and continuing theme of modern solid state physics is the realization of exotic excitations in materials (e.g. quasiparticles) that have no analogy (or have not yet been observed) in the actual physical vacuum of free space. Read More

We present time-of-flight inelastic neutron scattering measurements of $La_{1.965}Ba_{0.035}CuO_{4}$ (LBCO), a lightly doped member of the high temperature superconducting La-based cuprate family. Read More

We report the crystal structure, magnetization and neutron scattering measurements on the double perovskite Ba$_2$YOsO$_6$. The $Fm\overline{3}m$ space group is found both at 290~K and 3.5~K with cell constants $a_0 = 8. Read More

In condensed matter systems, the formation of long range order (LRO) with broken symmetry is often accompanied by new types of excitations. However, in many magnetic pyrochlore oxides, geometrical frustration suppresses conventional LRO while at the same time non-trivial spin correlations are observed. For such materials, a natural question to ask then is what is the nature of the excitations in this highly correlated state without broken symmetry? Frequently the application of a symmetry breaking field can stabilize excitations whose properties still reflect certain aspects of the anomalous state without long-range order. Read More

Structural phase transitions in Pr$_{1-x}$La$_x$AlO$_3$ (0 $\leq x\leq$ 1) single crystals have been studied through heat capacity and high-resolution x-ray scattering measurements. For PrAlO$_3$, the heat capacity shows a sharp first-order peak at the rhombohedral to orthorhombic transition, while a classical mean-field anomaly is observed at the orthorhombic to monoclinic transition at lower temperatures. The transition temperature and the heat capacity anomaly of the two transitions diminish with increasing $x$, and only a single rhombohedral to monoclinic transition is observed for $x = 0. Read More

We present new magnetic heat capacity and neutron scattering results for two magnetically frustrated molybdate pyrochlores: $S=1$ oxide Lu$_2$Mo$_2$O$_7$ and $S={\frac{1}{2}}$ oxynitride Lu$_2$Mo$_2$O$_5$N$_2$. Lu$_2$Mo$_2$O$_7$ undergoes a transition to an unconventional spin glass ground state at $T_f {\sim} 16$ K. However, the preparation of the corresponding oxynitride tunes the nature of the ground state from spin glass to quantum spin liquid. Read More

The superconducting and magnetic properties of HoNi2B2C single crystals are investigated through transport, magnetometry and small-angle neutron scattering measurements. In the magnetic phases that enter below the superconducting critical temperature, the small-angle neutron scattering data uncover networks of magnetic surfaces. These likely originate from uncompensated moments e. Read More

We take advantage of the site-selective nature of the $^{75}$As and $^{63}$Cu NMR techniques to probe the Cu substitution effects on the local magnetic properties of the FeAs planes in Ba(Fe$_{1-x}$Cu$_x$)$_2$As$_2$. We show that the suppression of antiferromagnetic Fe spin fluctuations induced by Cu substitution is weaker than a naive expectation based on a simple rigid band picture, in which each Cu atom would donate 3 electrons to the FeAs planes. Comparison between $^{63}$Cu and $^{75}$As NMR data indicates that spin fluctuations are suppressed at the Cu and their neighboring Fe sites in the tetragonal phase, suggesting the strongly local nature of the Cu substitution effects. Read More

The interplay between magnetism and crystal structures in three CaFe$_{2}$As$_{2}$ samples is studied. For the nonmagnetic quenched crystals, different crystalline domains with varying lattice parameters are found, and three phases (orthorhombic, tetragonal, and collapsed tetragonal) coexist between T$_{S}$ = 95 K and 45 K. Annealing of the quenched crystals at 350{\deg}C leads to a strain relief through a large (~1. Read More

The recent determination of a robust spin Hamiltonian for the anti-ferromagnetic XY pyrochlore Er2Ti2O7 reveals a most convincing case of the "order by quantum disorder" (ObQD) mechanism for ground state selection. This mechanism relies on quantum fluctuations to remove an accidental symmetry of the magnetic ground state, and selects a particular ordered spin structure below T_N=1.2K. Read More

We present a parametric study of the diffuse magnetic scattering at (1/2,1/2,1/2) positions in reciprocal space, ascribed to a frozen antiferromagnetic spin ice state in single crystalline Tb2Ti2O7. Our high-resolution neutron scattering measurements show that the elastic (-0.02 meV < E < 0. Read More

We present time-of-flight inelastic neutron scattering measurements at low temperature on powder samples of the magnetic pyrochlore oxides Tb2Ti2O7 and Tb2Sn2O7. These two materials possess related, but different ground states, with Tb2Sn2O7 displaying "soft" spin ice order below Tn~0.87 K, while Tb2Ti2O7 enters a hybrid, glassy spin ice state below Tg~0. Read More

The spin glass behavior of Y2Mo2O7 has puzzled physicists for nearly three decades. Free of bulk disorder within the resolution of powder diffraction methods, it is thought that this material is a rare realization of a spin glass resulting from weak disorder such as bond disorder or local lattice distortions. Here, we report on the single crystal growth of Y2Mo2O7. Read More

The geometrically frustrated double perovskite Ba2YRuO6 has magnetic 4d3 Ru5+ ions decorating an undistorted face-centered cubic (FCC) lattice. This material has been previously reported to exhibit commensurate long-range antiferromagnetic order below T_N = 36K, a factor f = 15 times lower than its Curie-Weiss temperature Theta_CW = -522 K, and purported short-range order to T* = 47K. We report new time-of-flight neutron spectroscopy of Ba2YRuO6 which shows the development of a 5 meV spin gap in the vicinity of the [100] magnetic ordering wavevector below T_N = 36K, with the transition to long-range order occurring at T* = 47K. Read More

We present neutron scattering measurements on single crystals of lightly doped $La_{2-x}Ba_{x}CuO_{4}$, with $0 \leq x \leq? 0.035$. These reveal the evolution of the magnetism in this prototypical doped Mott insulator from a three dimensional (3D) commensurate (C) antiferromagnetic ground state, which orders at a relatively high TN, to a two dimensional (2D) incommensurate (IC) ground state with finite ranged static correlations, which appear below a relatively low effective TN. Read More

We report low temperature specific heat and muon spin relaxation/rotation ($\mu$SR) measurements on both polycrystalline and single crystal samples of the pyrochlore magnet Yb$_2$Ti$_2$O$_7$. This system is believed to possess a spin Hamiltonian supporting a Quantum Spin Ice (QSI) ground state and to display sample variation in its low temperature heat capacity. Our two samples exhibit extremes of this sample variation, yet our $\mu$SR measurements indicate a similar disordered low temperature state down to 16 mK in both. Read More

Solid solutions of the magnetic insulators Ba3Cr2O8 and Sr3Cr2O8 (Ba3-xSrxCr2O8) have been prepared in polycrystalline form for the first time. Single crys- talline material was obtained using a mirror image floating zone technique. X-ray diffraction data taken at room temperature indicate that the space group of Ba3-xSrxCr2O8 remains unchanged for all values of x, while the cell parameters depend on the chemical composition, as expected. Read More

We present high-resolution single crystal time-of-flight neutron scattering measurements on the candidate quantum spin liquid pyrochlore Tb2Ti2O7 at low temperature and in a magnetic field. At ~70 mK and in zero field, Tb2Ti2O7 reveals diffuse magnetic elastic scattering at (1/2,1/2,1/2) positions in reciprocal space, consistent with short-range correlated regions based on a two-in, two-out spin ice configuration on a doubled conventional unit cell. This elastic scattering is separated from very low-energy magnetic inelastic scattering by an energy gap of ~0. Read More

Recent neutron scattering and specific heat studies on the pyrochlore Yb2Ti2O7 have revealed variations in its magnetic behavior below 265mK. In the best samples, a sharp anomaly in the specific heat is observed at T=265mK. Other samples, especially single crystals, have broad features in the specific heat which vary in sharpness and temperature depending on the sample, indicating that the magnetic ground state may be qualitatively different in such samples. Read More

Co3V2O8 is an orthorhombic magnet in which S=3/2 magnetic moments reside on two crystallographically inequivalent Co2+ sites, which decorate a stacked, buckled version of the two dimensional kagome lattice, the stacked kagome staircase. The magnetic interactions between the Co2+ moments in this structure lead to a complex magnetic phase diagram at low temperature, wherein it exhibits a series of five transitions below 11 K that ultimately culminate in a simple ferromagnetic ground state below T~6.2 K. Read More

Here we establish the systematic existence of a U(1) degeneracy of all symmetry-allowed Hamiltonians quadratic in the spins on the pyrochlore lattice, at the mean-field level. By extracting the Hamiltonian of Er2Ti2O7 from inelastic neutron scattering measurements, we then show that the U(1)-degenerate states of Er2Ti2O7 are its classical ground states, and unambiguously show that quantum fluctuations break the degeneracy in a way which is confirmed by experiment. This is the first definitive observation of order-by-disorder in any material. Read More

Strong geometrical frustration in magnets leads to exotic states, such as spin liquids, spin supersolids and complex magnetic textures. SrCu2(BO3)2, a spin-1/2 Heisenberg antiferromagnet in the archetypical Shastry-Sutherland lattice, exhibits a rich spectrum of magnetization plateaus and stripe-like magnetic textures in applied fields. The structure of these plateaus is still highly controversial due to the intrinsic complexity associated with frustration and competing length scales. Read More

The Shastry-Sutherland model, which consists of a set of spin 1/2 dimers on a 2-dimensional square lattice, is simple and soluble, but captures a central theme of condensed matter physics by sitting precariously on the quantum edge between isolated, gapped excitations and collective, ordered ground states. We compress the model Shastry-Sutherland material, SrCu2(BO3)2, in a diamond anvil cell at cryogenic temperatures to continuously tune the coupling energies and induce changes in state. High-resolution x-ray measurements exploit what emerges as a remarkably strong spin-lattice coupling to both monitor the magnetic behavior and the absence or presence of structural discontinuities. Read More

We have developed an application of a one-dimensional micro-strip detector for capturing x-ray diffraction data in pulsed magnetic fields. This detector consists of a large array of 50 \mu m-wide Si strips with a full-frame read out at 20 kHz. Its use substantially improves data-collection efficiency and quality as compared to point detectors, because diffraction signals are recorded along an arc in reciprocal space in a time-resolved manner. Read More

The pyrochlore material Yb2Ti2O7 displays unexpected quasi-two-dimensional (2D) magnetic correlations within a cubic lattice environment at low temperatures, before entering an exotic disordered ground state below T=265mK. We report neutron scattering measurements of the thermal evolution of the 2D spin correlations in space and time. Short range three dimensional (3D) spin correlations develop below 400 mK, accompanied by a suppression in the quasi-elastic (QE) scattering below ~ 0. Read More

Recent work has highlighted remarkable effects of classical thermal fluctuations in the dipolar spin ice compounds, such as "artificial magnetostatics", manifesting as Coulombic power-law spin correlations and particles behaving as diffusive "magnetic monopoles". In this paper, we address quantum spin ice, giving a unifying framework for the study of magnetism of a large class of magnetic compounds with the pyrochlore structure, and in particular discuss Yb2Ti2O7 and extract its full set of Hamiltonian parameters from high field inelastic neutron scattering experiments. We show that fluctuations in Yb2Ti2O7 are strong, and that the Hamiltonian may support a Coulombic "Quantum Spin Liquid" ground state in low field and host an unusual quantum critical point at larger fields. Read More

CuMoO4 is a triclinic quantum magnet based on S = 1/2 moments at the Cu2+ site. It has recently attracted interest due to the remarkable changes in its chromic and volumetric properties at high temperatures, and in its magnetic properties at low temperatures. This material exhibits a first order structural phase transition at T_C ~ 190 K as well as a magnetic phase transition at T_N ~ 1. Read More

We have performed high resolution x-ray scattering measurements on single crystal samples of Ba(Fe(1-x)Cr(x))2As2 (x = 0 to 0.335). These measurements examine the effect of Cr-doping on the high temperature tetragonal (I4/mmm) to low temperature orthorhombic (Fmmm) structural phase transition of the parent compound BaFe2As2. Read More

We present new high resolution inelastic neutron scattering data on the candidate spin liquid Tb2Ti2O7. We find that there is no evidence for a zero field splitting of the ground state doublet within the 0.2 K resolution of the instrument. Read More

The geometrically frustrated double perovskite Ba2YMoO6 is characterized by quantum s=1/2 spins at the Mo5+ sites of an undistorted face-centered cubic (FCC) lattice. Previous low-temperature characterization revealed an absence of static long-range magnetic order and suggested a non-magnetic spin-singlet ground state. We report new time-of-flight and triple-axis neutron spectroscopy of Ba2YMoO6 that shows a 28 meV spin excitation with a bandwidth of ~4 meV, which vanishes above ~125 K. Read More

Low temperature measurements of the ac magnetic susceptibility along the [110] direction of a single crystal of the dipolar spin ice material Ho2Ti2O7, in zero static field, are presented. While behavior that is qualitatively consistent with previous work on Ho2Ti2O7 and the related material Dy2Ti2O7 is observed, this work extends measurements to appreciably lower temperatures and frequencies. In the freezing regime, below 1 K, the dynamics are found to be temperature activated, thus well described by an Arrhenius law with an activation energy close to 6J_eff, a result that is not easily explained with the current model of magnetic monopole excitations in dipolar spin ice. Read More

We have performed time-of-flight neutron scattering measurements on powder samples of the unconventional spin-Peierls compound TiOBr using the fine-resolution Fermi chopper spectrometer (SEQUOIA) at the SNS. These measurements reveal two branches of magnetic excitations within the commensurate and incommensurate spin-Peierls phases, which we associate with n = 1 and n = 2 triplet excitations out of the singlet ground state. These measurements represent the first direct measure of the singlet-triplet energy gap in TiOBr, which is determined to be Eg = 21. Read More

We report high resolution single crystal x-ray diffraction measurements of the frustrated pyrochlore magnet Tb2Ti2O7, collected using a novel low temperature pulsed magnet system. This instrument allows characterization of structural degrees of freedom to temperatures as low as 4.4 K, and in applied magnetic fields as large as 30 Tesla. Read More

We report an analysis of neutron diffraction from single crystals of the spin-liquid pyrochlore Tb2Ti2O7 under the application of magnetic fields along the crystallographic $[110]$ direction. Such a perturbation has been shown to destroy the spin liquid ground state and induce long-range order, although the nature of the ordered state was not immediately determined. Recently, it has been proposed that the ordered state is characterized by spin-ice-like correlations, evincing an emergent ferromagnetic tendency in this material despite the large negative Curie-Weiss constant. Read More

We have performed detailed x-ray scattering measurements on single crystals of the spin-Peierls compound TiOBr in order to study the critical properties of the transition between the incommensurate spin-Peierls state and the paramagnetic state at Tc2 ~ 48 K. We have determined a value of the critical exponent beta which is consistent with the conventional 3D universality classes, in contrast with earlier results reported for TiOBr and TiOCl. Using a simple power law fit function we demonstrate that the asymptotic critical regime in TiOBr is quite narrow, and obtain a value of beta_{asy} = 0. Read More

Neutron scattering measurements show the ferromagnetic XY pyrochlore Yb2Ti2O7 to display strong quasi-two dimensional (2D) spin correlations at low temperature, which give way to long range order (LRO) under the application of modest magnetic fields. Rods of scattering along < 111 > directions due to these 2D spin correlations imply a magnetic decomposition of the cubic pyrochlore system into decoupled kagome planes. A magnetic field of ~0. Read More

Elastic and inelastic neutron scattering studies have been carried out on the pyrochlore magnet Ho2Ti2O7. Measurements in zero applied magnetic field show that the disordered spin ice ground state of Ho2Ti2O7 is characterized by a pattern of rectangular diffuse elastic scattering within the [HHL] plane of reciprocal space, which closely resembles the zone boundary scattering seen in its sister compound Dy2Ti2O7. Well-defined peaks in the zone boundary scattering develop only within the spin ice ground state below ~ 2 K. Read More