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B. Grenier

Publications and source records attributed to B. Grenier.

At least 19 recordsLinked to original sources

Quantum spin liquid on a 3D bipartite lattice of spin trimers stabilized by enhanced effective anisotropy

Quantum spin liquids (QSLs) represent highly entangled states of matter in which frustration-induced quantum fluctuations suppress any symmetry-breaking phase transition down to absolute zero, giving rise to fractionalized excitations and emergent gauge fields. Theoretically, bond anisotropy can stabilize QSLs even on bipartite lattices, as exemplified by the Kitaev honeycomb model; however, no material has so far been established to realize such a state as its true ground state. Here we identify the three-dimensional spin-trimer magnet KBa$_3$Ca$_4$Cu$_3$V$_7$O$_{28}$ as a promising candidate for a bipartite quantum spin liquid persisting to the lowest temperatures. Strongly coupled Cu$^{2+}$ trimers form effective pseudospin-1/2 degrees of freedom upon cooling, which in turn constitute a three-dimensional bipartite network. Bulk thermodynamic measurements, neutron scattering, $\mu$SR, and NMR detect no spin freezing or symmetry-breaking phase transition down to 20 mK, but instead reveal a gapless dynamical ground state with algebraic spin autocorrelations. Complementary Monte Carlo and exact-diagonalization calculations show that this state is stabilized by a strong enhancement of effective anisotropy: a weak microscopic Cu-Cu exchange anisotropy of approximately 15 percent is generically amplified at the trimer level, producing effective pseudospin-pseudospin interaction anisotropies of 60 to 100 percent. Our results establish trimer-based networks as a promising platform for realizing anisotropy-stabilized quantum entangled states, even in three-dimensional bipartite systems with only weak microscopic anisotropy.

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Topological quantum phase transition in the Ising-like antiferromagnetic spin chain BaCo$_2$V$_2$O$_8$

Since the seminal ideas of Berezinskii, Kosterlitz and Thouless, topological excitations are at the heart of our understanding of a whole novel class of phase transitions. In most of the cases, those transitions are controlled by a single type of topological objects. There are however some situations, still poorly understood, where two dual topological excitations fight to control the phase diagram and the transition. Finding experimental realization of such cases is thus of considerable interest. We show here that this situation occurs in BaCo$_2$V$_2$O$_8$, a spin-1/2 Ising-like quasi-one dimensional antiferromagnet when subjected to a uniform magnetic field transverse to the Ising axis. Using neutron scattering experiments, we measure a drastic modification of the quantum excitations beyond a critical value of the magnetic field. This quantum phase transition is identified, through a comparison with theoretical calculations, to be a transition between two different types of solitonic topological objects, which are captured by different components of the dynamical structure factor.

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Mesoscopic correlations in Tb2Ti2O7 spin liquid

We have studied the spin correlations with $\bf{k}$= ($\frac12$, $\frac12$, $\frac12$) propagation vector which appear below 0.4\, K in \tbti\ spin liquid by combining powder neutron diffraction and specific heat on Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ samples with $x$=0, 0.01, -0.01. The $\bf{k}$= ($\frac12$, $\frac12$, $\frac12$) order clearly appears on all neutron patterns by subtracting a pattern at 1.2(1)\,K. Refining the subtracted patterns at 0.07\,K yields two possible spin structures, with spin-ice-like and monopole-like correlations respectively. Mesoscopic correlations involve Tb moments of 1 to 2 \mub\ ordered on a length scale of about 20 Å. In addition, long range order involving a small spin component of 0.1 to 0.2 \mub\ is detected for the $x$= 0 and 0.01 samples showing a peak in the specific heat. Comparison with previous single crystals data suggests that the ($\frac12$, $\frac12$, $\frac12$) order settles in through nanometric spin textures with dominant spin ice character and correlated orientations, analogous to nanomagnetic twins.

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Longitudinal and Transverse Zeeman Ladders in the Ising-Like Chain Antiferromagnet BaCo2V2O8

We explore the spin dynamics emerging from the Néel phase of the chain compound antiferromagnet BaCo2V2O8. Our inelastic neutron scattering study reveals unconventional discrete spin excitations, so called Zeeman ladders, understood in terms of spinon confinement, due to the interchain attractive linear potential. These excitations consist in two interlaced series of modes, respectively with transverse and longitudinal polarization. The latter have no classical counterpart and are related to the zero-point fluctuations that weaken the ordered moment in weakly coupled quantum chains. Our analysis reveals that BaCo2V2O8, with moderate Ising anisotropy and sizable interchain interactions, remarkably fulfills the conditions necessary for the observation of these longitudinal excitations.

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Neutron diffraction investigation of the H-T phase diagram above the longitudinal incommensurate phase of BaCo2V2O8

The quasi-one-dimensional antiferromagnetic Ising-like compound BaCo2V2O8 has been shown to be describable by the Tomonaga-Luttinger liquid theory in its gapless phase induced by a magnetic field applied along the Ising axis. Above 3.9 T, this leads to an exotic field-induced low-temperature magnetic order, made of a longitudinal incommensurate spin-density wave, stabilized by weak interchain interactions. By single-crystal neutron diffraction we explore the destabilization of this phase at a higher magnetic field. We evidence a transition at around 8.5 T towards a more conventional magnetic structure with antiferromagnetic components in the plane perpendicular to the magnetic field. The phase diagram boundaries and the nature of this second field-induced phase are discussed with respect to previous results obtained by means of nuclear magnetic resonance and electron spin resonance, and in the framework of the simple model based on the Tomonaga-Luttinger liquid theory, which obviously has to be refined in this complex system.

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Giant magnetic-field dependence of the coupling between spin Tomonaga-Luttinger liquids in BaCo2V2O8

We use nuclear magnetic resonance to map the complete low-temperature phase diagram of the antiferromagnetic Ising-like spin-chain system BaCo2V2O8 as a function of the magnetic field applied along the chains. In contrast to the predicted crossover from the longitudinal incommensurate phase to the transverse antiferromagnetic phase, we find a sequence of three magnetically ordered phases between the critical fields 3.8 T and 22.8 T. Their origin is traced to the giant magnetic-field dependence of the total effective coupling between spin chains, extracted to vary by a factor of 24. We explain this novel phenomenon as emerging from the combination of nontrivially coupled spin chains and incommensurate spin fluctuations in the chains treated as Tomonaga-Luttinger liquids.

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Magnetic phase diagrams, domain switching and a quantum phase transition of the quasi-1D Ising-like antiferromagnet BaCo2V2O8

In the effective Ising spin-1/2 antiferromagnetic chain system BaCo$_2$V$_2$O$_8, the magnetic-field influence is highly anisotropic. For magnetic fields along the easy axis $c$, the Néel order is strongly suppressed already for low fields and an incommensurate order is entered above 4 T. We present a detailed study of the magnetic phase diagrams for different magnetic field directions, which are derived from magnetization data, high-resolution thermal expansion and magnetostriction measurements as well as from the thermal conductivity. Zero-field thermal expansion data reveal that the magnetic transition is accompanied by an orthorhombic distortion within the $ab$ plane. Under ambient conditions the crystals are heavily twinned, but the domain orientation can be influenced either by applying uniaxial pressure or a magnetic field along the [100] direction. In addition, our data reveal a pronounced in-plane magnetic anisotropy for fields applied within the $ab$ plane. For $H || [110]$, the magnetic field influence on T$_N$ is weak, whereas for magnetic fields applied along [100], T$_N$ vanishes at about 10 T and the zero-field Néel order is completely suppressed as is confirmed by neutron diffraction data. The second-order phase transition strongly suggests a quantum critical point being present at $H\simeq 10$ T parallel [100], where the Néel order probably changes to a spin-liquid state.

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Field-induced magnetic behavior in quasi-one-dimensional Ising-like antiferromagnet BaCo2V2O8: A single-crystal neutron diffraction study

BaCo2V2O8 is a nice example of a quasi-one-dimensional quantum spin system that can be described in terms of Tomonaga-Luttinger liquid physics. This is explored in the present study where the magnetic field-temperature phase diagram is thoroughly established up to 12 T using single-crystal neutron diffraction. The transition from the Néel phase to the incommensurate longitudinal spin density wave (LSDW) phase through a first-order transition, as well as the critical exponents associated with the paramagnetic to ordered phase transitions, and the magnetic order both in the Néel and in the LSDW phase are determined, thus providing a stringent test for the theory.

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Magnetic order, magnetic correlations and spin dynamics in the pyrochlore antiferromagnet Er2Ti2O7

Er2Ti2O7 is believed to be a realization of an XY antiferromagnet on a frustrated lattice of corner-sharing regular tetrahedra. It is presented as an example of the order-by-disorder mechanism in which fluctuations lift the degeneracy of the ground state, leading to an ordered state. Here we report detailed measurements of the low temperature magnetic properties of Er2Ti2O7, which displays a second-order phase transition at T_N \simeq 1.2 K with coexisting short- and long-range orders. Magnetic-susceptibility studies show that there is no spin-glass-like irreversible effect. Heat-capacity measurements reveal that the paramagnetic critical exponent is typical of a 3-dimensional XY magnet while the low-temperature specific heat sets an upper limit on the possible spin-gap value and provides an estimate for the spin-wave velocity. Muon spin relaxation measurements show the presence of spin dynamics in the nanosecond time scale down to 21 mK. This time range is intermediate between the shorter time characterizing the spin dynamics in Tb2Sn2O7, which also displays long- and short-range magnetic order, and the time scale typical of conventional magnets. Hence the ground state is characterized by exotic spin dynamics. We determine the parameters of a symmetry-dictated Hamiltonian restricted to the spins in a tetrahedron, by fitting the paramagnetic diffuse neutron scattering intensity for two reciprocal lattice planes. These data are recorded in a temperature region where the assumption that the correlations are limited to nearest neighbors is fair.

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Spin-chain system as a tunable simulator of frustrated planar magnetism

At low temperatures, weakly coupled spin chains develop a magnetic order that reflects the character of gapless spin fluctuations along the chains. Using nuclear magnetic resonance, we identify and characterize two ordered states in the gapless region of the antiferromagnetic, Ising-like spin-chain system BaCo2V2O8, both arising from the incommensurate fluctuations along the chains. They correspond to the columnar and ferromagnetic ordered states of the frustrated J1-J2 spin model on a square lattice, where the spins are encoded in original spin chains. As a result of field-dependent incommensurate fluctuations and frustrated interchain interaction, J1 can be tuned continuously with the magnetic field, and its value with respect to a fixed J2 selects the ordered state. Spin-chain systems can thus be used as tunable simulators of frustrated planar magnetism.

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Field-Induced magnetic structures in Tb2Ti2O7 at low temperatures: From spin-ice to spin-flip structures

We studied the field-induced magnetic structures of the Tb2Ti2O7 pyrochlore by single-crystal neutron diffraction with a magnetic field applied along a [110] axis, focusing on the influence of a small misalignment. Both induced magnetic structures with k=0 and k=(0,0,1) propagation vectors are found to be sensitive to the misalignment, which controls the magnitude and orientation of the Tb moments involved in the beta chains, with local [111] anisotropy axis perpendicular to the field. For k=0, spin-ice-like structures are observed for a misalignment of a few degrees, whereas other structures, where the Tb-beta moments flip by "melting" on the field axis, occur when the field is perfectly aligned. The field evolution of the k=0 structure is well reproduced by a molecular field model with anisotropic exchange. We give a complete symmetry analysis of the k=0 and k=(0,0,1) magnetic structures, both being described by the basis functions of single irreducible representations.

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Dimensional crossover in a spin liquid to helimagnet quantum phase transition

Neutron scattering is used to study magnetic field induced ordering in the quasi-1D quantum spin-tube compound Sul--Cu$_2$Cl$_4$ that in zero field has a non-magnetic spin-liquid ground state. The experiments reveal an incommensurate chiral high-field phase stabilized by a geometric frustration of the magnetic interactions. The measured critical exponents $β\approx0.235$ and $ν\approx0.34$ at $H_c\approx3.7$ T point to an unusual sub-critical scaling regime and may reflect the chiral nature of the quantum critical point.

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Field-Controlled Magnetic Order in the Quantum Spin-Ladder System (Hpip)2CuBr4

Neutron diffraction is used to investigate the field-induced, antiferromagnetically ordered state in the two-leg spin-ladder material (Hpip)2CuBr4. This "classical" phase, a consequence of weak interladder coupling, is nevertheless highly unconventional: its properties are influenced strongly by the spin Luttinger-liquid state of the ladder subunits. We determine directly the order parameter (transverse magnetization), the ordering temperature, the spin structure, and the critical exponents around the transition. We introduce a minimal, microscopic model for the interladder coupling and calculate the quantum fluctuation corrections to the mean-field interaction.

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Dynamics of quantum spin liquid and spin solid phases in IPA-CuCl3 under field

Inelastic and elastic neutron scattering is used to study spin correlations in the quasi-one dimensional quantum antiferromagnet IPA-CuCl3 in strong applied magnetic fields. A condensation of magnons and commensurate transverse long-range ordering is observe at a critical filed $H_c=9.5$ T. The field dependencies of the energies and polarizations of all magnon branches are investigated both below and above the transition point. Their dispersion is measured across the entire 1D Brillouin zone in magnetic fields up to 14 T. The critical wave vector of magnon spectrum truncation [Masuda et al., Phys. Rev. Lett. 96, 047210 (2006)] is found to shift from h_c 0.35 at H>H_c. A drastic reduction of magnon bandwidths in the ordered phase [Garlea et al., Phys. Rev. Lett. 98, 167202 (2007)] is observed and studied in detail. New features of the spectrum, presumably related to this bandwidth collapse, are observed just above the transition field.

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Temperature excitation of the Co3+ triplet spin-state in LaCoO3 determined by polarized neutron diffraction

The magnetic moment induced by an external magnetic field of 5.8 T on the Co3+ ions in LaCoO3 has been measured by polarized neutron diffraction. Measurements were made at 100 K, near to the spin-state transition, at 1.5 K and at 285 K. The data give evidence for a transition from the ground singlet state (S = 0) to the excited triplet intermediate spin state (S = 1). The energy of K estimated for the high-spin (S = 2) state, is too high to contribute significantly even at T = 285 K. There is evidence for a small negative covalent spin density associated with the oxygen ligands amounting to about one fifth of the aligned Co3+ moment at all three temperatures.

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Half-ordered state in the anisotropic Haldane-gap antiferromagnet NDMAP

Neutron diffraction experiments performed on the Haldane gap material NDMAP in high magnetic fields applied at an angle to the principal anisotropy axes reveal two consecutive field-induced phase transitions. The low-field phase is the gapped Haldane state, while at high fields the system exhibits 3-dimensional long-range Neel order. In a peculiar phase found at intermediate fields only half of all the spin chains participate in the long-range ordering, while the other half remains disordered and gapped.

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Cooperative ordering of gapped and gapless spin networks in Cu$_2$Fe$_2$Ge$_4$O$_{13}$

The unusual magnetic properties of a novel low-dimensional quantum ferrimagnet Cu$_2$Fe$_2$Ge$_4$O$_{13}$ are studied using bulk methods, neutron diffraction and inelastic neutron scattering. It is shown that this material can be described in terms of two low-dimensional quantum spin subsystems, one gapped and the other gapless, characterized by two distinct energy scales. Long-range magnetic ordering observed at low temperatures is a cooperative phenomenon caused by weak coupling of these two spin networks.

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Ordering and Excitations in the Field-Induced Magnetic Phase of Cs_3Cr_2Br_9

Field-induced magnetic order has been investigated in detail in the interacting spin 3/2 dimer system Cs_3Cr_2Br_9. Elastic and inelastic neutron scattering measurements were performed up to H = 6 T, well above the critical field H_c1 = 1.5 T. The ordering displays incommensurabilities and a large hysteresis before a commensurate structure is reached. This structure is fully determined. Surprisingly, the lowest excitation branch never closes. Above H_c1, the gap increases slowly with field. An analysis in terms of projected pseudo-spin is given.

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