arXiv subjects

C. Broholm

Publications and source records attributed to C. Broholm.

At least 55 records · Page 3Linked to original sources

arXiv2009

Spin-lattice order in frustrated ZnCr2O4

Using synchrotron X-rays and neutron diffraction we disentangle spin-lattice order in highly frustrated ZnCr$_2$O$_4$ where magnetic chromium ions occupy the vertices of regular tetrahedra. Upon cooling below 12.5 K the quandary of anti-aligning spins surrounding the triangular faces of tetrahedra is resolved by establishing weak interactions on each triangle through an intricate lattice distortion. The resulting spin order is however, not simply a Néel state on strong bonds. A complex co-planar spin structure indicates that antisymmetric and/or further neighbor exchange interactions also play a role as ZnCr$_2$O$_4$ resolves conflicting magnetic interactions.

cond-mat.str-el↗

arXiv2009

Itinerant magnetic excitations in antiferromagnetic CaFe2As2

Neutron scattering measurements of the magnetic excitations in single crystals of antiferromagnetic CaFe2As2 reveal steeply dispersive and well-defined spin waves up to an energy of 100 meV. Magnetic excitations above 100 meV and up to the maximum energy of 200 meV are however broader in energy and momentum than the experimental resolution. While the low energy modes can be fit to a Heisenberg model, the total spectrum cannot be described as arising from excitations of a local moment system. Ab-initio calculations of the dynamic magnetic susceptibility suggest that the high energy behavior is dominated by the damping of spin waves by particle-hole excitations.

cond-mat.supr-con↗

arXiv2008

Suppression of antiferromagnetic spin fluctuations in the collapsed tetragonal phase of CaFe2As2

Inelastic neutron scattering measurements of CaFe2As2 under applied hydrostatic pressure show that the antiferromagnetic spin fluctuations observed in the ambient pressure, paramagnetic, tetragonal (T) phase are strongly suppressed, if not absent, in the collapsed tetragonal (cT) phase. These results are consistent with a quenched Fe moment in the cT phase and the strong decrease in resistivity observed upon crossing the boundary from the T to cT phase. The suppression or absence of static antiferromagnetic order and dynamic spin fluctuations in the non-superconducting cT phase supports the notion of a coupling between spin fluctuations and superconductivity in the iron arsenides.

cond-mat.supr-con↗

arXiv2008

Anisotropic three-dimensional magnetism in CaFe2As2

Inelastic neutron scattering measurements on the low energy spin waves in CaFe2As2 show that the magnetic exchange interactions in the Fe layers are exceptionally large and similar to the cuprates. However, the exchange between layers is ~10% of the coupling in the layers and the magnetism is more appropriately categorized as anisotropic three-dimensional, in contrast to the two-dimensional cuprates. Band structure calculations of the spin dynamics and magnetic exchange interactions are in good agreement with the experimental data.

cond-mat.supr-con↗

arXiv2008

Mesoscopic Phase Coherence in a Quantum Spin Fluid

Mesoscopic quantum phase coherence is important because it improves the prospects for handling quantum degrees of freedom in technology. Here we show that the development of such coherence can be monitored using magnetic neutron scattering from a one-dimensional spin chain Y2BaNiO5, a quantum spin fluid where no classical, static magnetic order is present. In the cleanest samples, the quantum coherence length is 20 nm, almost an order of magnitude larger than the classical antiferromagnetic correlation length of 3 nm. We also demonstrate that the coherence length can be modified by static and thermally activated defects in a quantitatively predictable manner.

cond-mat.str-el↗

arXiv2008

Roton-like mode in solid He-4

Recent theoretical and experimental work on solid He-4 has focused on vacancies, or other lattice defects and whether these can form a Bose-Einstein condensate within the solid. The earliest suggestion that this could happen was based on the conjecture that the ground state of the solid at T = 0 K would include vacancies. Although no direct evidence for zero point vacancies has been presented, a variety of experimental observations have been interpreted as being due to thermally activated vacancies. Here we directly probe the excitation spectrum of hcp solid He-4 using inelastic neutron scattering. We identify a branch of delocalized excitations, with both longitudinal and transverse dispersion that coexist with acoustic phonons. While the energy gap is larger and the characteristic wavevector is shifted to coincide with the position of the (100) Bragg peak, the longitudinal effective mass of this mode is within 15% of that for rotons in superfluid He-4. The dispersion relation intersects the longitudinal acoustic phonon half way to the zone boundary, and this distinguishes the mode from a conventional optic phonon. Our results provide direct evidence for coherent delocalized non-phonon excitations in solid helium, which we identify as delocalized vacancy modes.

cond-mat.stat-mech↗

arXiv2007

Spin resonance in the d-wave superconductor CeCoIn5

Neutron scattering is used to probe antiferromagnetic spin fluctuations in the d-wave heavy fermion superconductor CeCoIn$_{5}$ (T$_{c}$=2.3 K). Superconductivity develops from a state with slow ($\hbarΓ$=0.3 $\pm$ 0.15 meV) commensurate (${\bf{Q_0}}$=(1/2,1/2,1/2)) antiferromagnetic spin fluctuations and nearly isotropic spin correlations. The characteristic wavevector in CeCoIn$_{5}$ is the same as CeIn$_{3}$ but differs from the incommensurate wavevector measured in antiferromagnetically ordered CeRhIn$_{5}$. A sharp spin resonance ($\hbarΓ<0.07$ meV) at $\hbar ω$ = 0.60 $\pm$ 0.03 meV develops in the superconducting state removing spectral weight from low-energy transfers. The presence of a resonance peak is indicative of strong coupling between f-electron magnetism and superconductivity and consistent with a d-wave gap order parameter satisfying $Δ({\bf q+Q_0})=-Δ({\bf q})$.

cond-mat.supr-con↗

arXiv2007

Absence of low temperature anomaly in the Debye-Waller factor of solid He-4

The mean square atomic displacement in hcp-phase solid He-4 has been measured in crystals with a molar volume of 21.3 cm^3. It is temperature independent from 1 K to 140 mK, with no evidence for an anomaly in the vicinity of the proposed supersolid transition. The mean square displacement is different for in-plane motions (0.122 +/- 0.001 A^(2)) and out-of-plane motions (0.150 +/- 0.001 A ^(2)).

cond-mat.other↗

arXiv2007

From Cooperative Paramagnet to Néel Order in Y_2Ru_2O_7

Spin correlations in the pyrochlore antiferromagnet Y_2Ru_2O_7 with Curie-Weiss temperature $Θ_{CW}=-1100$ K and critical temperature T_N=77 K were examined through neutron scattering. For $T_N<T<Θ_{CW}/3$ the data show spin relaxation with a rate $\hbarΓ= 1.17(9)k_BT$. For T<T_N spectral weight moves to higher energies with substantial changes up to $4\times k_BT_N$. For T<<T_N there is a $Δ=11(1)$ meV energy gap and a pronounced spectral maximum at 19.7 meV. Throughout the temperature range examined the wave vector dependence of inelastic scattering exhibits a broad peak for $Qd\approx 3.8$ (d is Ru-Ru spacing) consistent with dipolar spin correlations.

cond-mat.str-el↗

arXiv2007

Evidence for decay of spin-waves above the pseudogap in underdoped YBa2Cu3O6.35

The magnetic spectrum at high-energies in heavily underdoped YBa$_{2}$Cu$_{3}$O$_{6.35}$ (T$_{c}$=18 K) has been determined throughout the Brillouin zone. At low-energy the scattering forms a cone of spin excitations emanating from the antiferromagnetic (0.5, 0.5) wave vector with an acoustic velocity similar to that of insulating cuprates. At high energy transfers, below the maximum energy of 270 meV at (0.5, 0), we observe zone boundary dispersion much larger and spectral weight loss more extensive than in insulating antiferromagnets. Moreover we report phenomena not found in insulators, an overall lowering of the zone-boundary energies and a large damping of $\sim$ 100 meV of the spin excitations at high-energies. The energy above which the damping occurs coincides approximately with the gap determined from transport measurements. We propose that as the energy is raised the spin excitations encounter an extra channel of decay into particle-hole pairs of a continuum that we associate with the pseudogap.

cond-mat.supr-con↗

arXiv2007

Quantum phase transitions in magnetism and superconductivity: emergent spin topology seen with neutrons

Magnetic spins and charges interact strongly in high-temperature superconductors. New physics emerges as layers of copper oxide are tuned towards the boundary of the superconducting phase. As the pseudogap increases the characteristic spin excitation energy decreases. We show that our well-annealed YBa2Cu3O6+x (YBCO6+x) single crystals are orthorhombic and superconducting but not antiferromagnetically ordered. Near the critical concentration for superconductivity for x = 0.35 the spins fluctuate on two energy scales, one a relaxational spin response at ~2 meV and the other a slow central mode that is resolution-limited in energy (<0.08 meV) but broad in momentum. The gradual formation on cooling of a central mode over a range of momenta suggests that the spin ground state from which coherent superconducting pairing emerges may be quantum disordered. We show that YBCO6.35 adopts a homogeneous state that consists of highly-organized frozen sub-critical three-dimensional spin correlations. The continuous spin evolution indicates that a single quantum state occurs in contrast to claims from site-based probes that lightly doped YBCO undergoes a transition to antiferromagnetic Bragg order followed by a sharp transition to a cluster glass phase. For x = 0.35, where Tc = 18 K is reduced to 1/5 of Tcmax, the spin ground state is reached without a sharp transition and consists of short correlations extending over only 8 Angstrom between cells and 42 Angstrom within the planes. Polarized neutrons show the angular spin distribution to be isotropic unlike the AF insulator. Since moment is conserved we interpret this as evidence for hole-induced spin rotations rather than decay.

cond-mat.supr-con↗

arXiv2007

Direct transition from a disordered to a multiferroic phase on a triangular lattice

Competing interactions and geometric frustration provide favourable conditions for exotic states of matter. Such competition often causes multiple phase transitions as a function of temperature and can lead to magnetic structures that break inversion symmetry, thereby inducing ferroelectricity [1-4]. Although this phenomenon is understood phenomenologically [3-4], it is of great interest to have a conceptually simpler system in which ferroelectricity appears coincident with a single magnetic phase transition. Here we report the first such direct transition from a paramagnetic and paraelectric phase to an incommensurate multiferroic in the triangular lattice antiferromagnet RbFe(MoO4)2 (RFMO). A magnetic field extinguishes the electric polarization when the symmetry of the magnetic order changes and ferroelectricity is only observed when the magnetic structure has chirality and breaks inversion symmetry. Multiferroic behaviour in RFMO provides a theoretically tractable example of ferroelectricity from competing spin interactions. A Landau expansion of symmetry-allowed terms in the free energy demonstrates that the chiral magnetic order of the triangular lattice antiferromagnet gives rise to a pseudoelectric field, whose temperature dependence agrees with that observed experimentally.

cond-mat.mtrl-sci↗

arXiv2007

Phase diagram and spin Hamiltonian of weakly-coupled anisotropic S=1/2 chains in CuCl2*2((CD3)2SO)

Field-dependent specific heat and neutron scattering measurements were used to explore the antiferromagnetic S=1/2 chain compound CuCl2 * 2((CD3)2SO). At zero field the system acquires magnetic long-range order below TN=0.93K with an ordered moment of 0.44muB. An external field along the b-axis strengthens the zero-field magnetic order, while fields along the a- and c-axes lead to a collapse of the exchange stabilized order at mu0 Hc=6T and mu0 Hc=3.5T, respectively (for T=0.65K) and the formation of an energy gap in the excitation spectrum. We relate the field-induced gap to the presence of a staggered g-tensor and Dzyaloshinskii-Moriya interactions, which lead to effective staggered fields for magnetic fields applied along the a- and c-axes. Competition between anisotropy, inter-chain interactions and staggered fields leads to a succession of three phases as a function of field applied along the c-axis. For fields greater than mu0 Hc, we find a magnetic structure that reflects the symmetry of the staggered fields. The critical exponent, beta, of the temperature driven phase transitions are indistinguishable from those of the three-dimensional Heisenberg magnet, while measurements for transitions driven by quantum fluctuations produce larger values of beta.

cond-mat.str-el↗

arXiv2006

Field-driven phase transitions in a quasi-two-dimensional quantum antiferromagnet

We report magnetic susceptibility, specific heat, and neutron scattering measurements as a function of applied magnetic field and temperature to characterize the $S=1/2$ quasi-two-dimensional frustrated magnet piperazinium hexachlorodicuprate (PHCC). The experiments reveal four distinct phases. At low temperatures and fields the material forms a quantum paramagnet with a 1 meV singlet triplet gap and a magnon bandwidth of 1.7 meV. The singlet state involves multiple spin pairs some of which have negative ground state bond energies. Increasing the field at low temperatures induces three dimensional long range antiferromagnetic order at 7.5 Tesla through a continuous phase transition that can be described as magnon Bose-Einstein condensation. The phase transition to a fully polarized ferromagnetic state occurs at 37 Tesla. The ordered antiferromagnetic phase is surrounded by a renormalized classical regime. The crossover to this phase from the quantum paramagnet is marked by a distinct anomaly in the magnetic susceptibility which coincides with closure of the finite temperature singlet-triplet pseudo gap. The phase boundary between the quantum paramagnet and the Bose-Einstein condensate features a finite temperature minimum at $T=0.2$ K, which may be associated with coupling to nuclear spin or lattice degrees of freedom close to quantum criticality.

cond-mat.str-el↗

arXiv2006

Neutron scattering from a coordination polymer quantum paramagnet

Inelastic neutron scattering measurements are reported for a powder sample of the spin-1/2 quantum paramagnet $\rm Cu(Quinoxaline)Br_2$. Magnetic neutron scattering is identified above an energy gap of 1.9 meV. Analysis of the sharp spectral maximum at the onset indicates that the material is magnetically quasi-one-dimensional. Consideration of the wave vector dependence of the scattering and polymeric structure further identifies the material as a two-legged spin-1/2 ladder. Detailed comparison of the data to various models of magnetism in this material based on the single mode approximation and the continuous unitary transformation are presented. The latter theory provides an excellent account of the data with leg exchange $J_{\parallel}=2.0$ meV and rung exchange $J_{\perp}=3.3$ meV.

cond-mat.str-el↗

arXiv2006

Central mode and spin confinement near the boundary of the superconducting phase in YBa2Cu3O6.353 (Tc=18 K)

We have mapped the neutron scattering spin spectrum at low-energies in YBa2Cu3O6.353 (Tc=18 K) where the doping ~0.06 is near the critical value (pc=0.055) for superconductivity. No coexistence with long range ordered antiferromagnetism is found. The spins fluctuate on two energy scales, one a damped spin response with a ~2 meV relaxation rate and the other a central mode with a relaxation rate that slows to less than 0.08 meV below Tc. The spectrum mirrors that of a soft mode driving a central mode. Extremely short correlation lengths, 42+-5 Angstrom in-plane and 8+-2 Angstrom along the c direction, and isotropic spin orientations for the central mode indicate that the correlations are subcritical with respect to any second order transition to Neel order. The dynamics follows a model where damped spin fluctuations are coupled to the slow fluctuations of regions with correlations shortened by the hole doping.

cond-mat.supr-con↗

arXiv2006

Quantum Criticality in an Organic Magnet

Exchange interactions between $S=\frac{1}{2}$ sites in piperazinium hexachlorodicuprate produce a frustrated bilayer magnet with a singlet ground state. We have determined the field-temperature phase diagram by high field magnetization and neutron scattering experiments. There are two quantum critical points: $H_{c1}=7.5$ T separates a quantum paramagnet phase from a three dimensional, antiferromagnetically-ordered state while $H_{c2}=37$ T marks the onset of a fully polarized state. The ordered phase, which we describe as a magnon Bose-Einstein condensate (BEC), is embedded in a quantum critical regime with short range correlations. A low temperature anomaly in the BEC phase boundary indicates that additional low energy features of the material become important near $H_{c1}$.

cond-mat.str-el↗

arXiv2005

Field dependence of magnetic ordering in Kagome-staircase compound Ni3V2O8

We present powder and single-crystal neutron diffraction and bulk measurements of the Kagome-staircase compound Ni3V2O8 (NVO) in fields up to 8.5T applied along the c-direction. (The Kagome plane is the a-c plane.) This system contains two types of Ni ions, which we call "spine" and "cross-tie". Our neutron measurements can be described with the paramagnetic space group Cmca for T < 15K and each observed magnetically ordered phase is characterized by the appropriate irreducible representation(s). Our zero-field measurements show that at T_PH=9.1K NVO undergoes a transition to an incommensurate order which is dominated by a longitudinally-modulated structure with the spine spins mainly parallel to the a-axis. Upon further cooling, a transition is induced at T_HL=6.3K to an elliptically polarized incommensurate structure with both spine and cross-tie moments in the a-b plane. At T_LC=4K the system undergoes a first-order phase transition, below which the magnetic structure is a commensurate antiferromagnet with the staggered magnetization primarily along the a-axis and a weak ferromagnetic moment along the c-axis. A specific heat peak at T_CC'=2.3K indicates an additional transition, which we were however not able to relate to a change of the magnetic structure. Neutron, specific heat, and magnetization measurements produce a comprehensive temperature-field phase diagram. The symmetries of the two incommensurate magnetic phases are consistent with the observation that only one phase has a spontaneous ferroelectric polarization. All the observed magnetic structures are explained theoretically using a simplified model Hamiltonian, involving competing nearest- and next-nearest-neighbor exchange interactions, spin anisotropy, Dzyaloshinskii-Moriya and pseudo-dipolar interactions.

cond-mat.str-el↗