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.Comment: Submitted to New Journal of Physic

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 ($\hbar\Gamma$=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 ($\hbar\Gamma<0.07$ meV) at $\hbar \omega$ = 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 $\Delta({\bf q+Q_0})=-\Delta({\bf q})$.Comment: (5 pages, 4 figures, to be published in Phys. Rev. Lett.

Magnetic field splitting of the spin-resonance in CeCoIn5

Neutron scattering in strong magnetic fields is used to show the spin-resonance in superconducting CeCoIn5 (Tc=2.3 K) is a doublet. The underdamped resonance (\hbar \Gamma=0.069 \pm 0.019 meV) Zeeman splits into two modes at E_{\pm}=\hbar \Omega_{0}\pm g\mu_{B} \mu_{0}H with g=0.96 \pm 0.05. A linear extrapolation of the lower peak reaches zero energy at 11.2 \pm 0.5 T, near the critical field for the incommensurate "Q-phase" indicating that the Q-phase is a bose condensate of spin excitons.Comment: 5 pages, 4 figure

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 N\'{e}el 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

The S=1/2 chain in a staggered field: High-energy bound-spinon state and the effects of a discrete lattice

We report an experimental and theoretical study of the antiferromagnetic S=1/2 chain subject to uniform and staggered fields. Using inelastic neutron scattering, we observe a novel bound-spinon state at high energies in the linear chain compound CuCl2 * 2((CD3)2SO). The excitation is explained with a mean-field theory of interacting S=1/2 fermions and arises from the opening of a gap at the Fermi surface due to confining spinon interactions. The mean-field model also describes the wave-vector dependence of the bound-spinon states, particularly in regions where effects of the discrete lattice are important. We calculate the dynamic structure factor using exact diagonalization of finite length chains, obtaining excellent agreement with the experiments.Comment: 16 pages, 7 figures, accepted by Phys. Rev.

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.Comment: revtex 12 pages, 11 figure

From incommensurate correlations to mesoscopic spin resonance in YbRh2Si2

Spin fluctuations are reported near the magnetic field driven quantum critical point in YbRh2Si2. On cooling, ferromagnetic fluctuations evolve into incommensurate correlations located at q0=+/- (delta,delta) with delta=0.14 +/- 0.04 r.l.u. At low temperatures, an in plane magnetic field induces a sharp intra doublet resonant excitation at an energy E0=g muB mu0 H with g=3.8 +/- 0.2. The intensity is localized at the zone center indicating precession of spin density extending xi=6 +/- 2 A beyond the 4f site.Comment: (main text - 4 pages, 4 figures; supplementary information - 3 pages, 3 figures; to be published in Physical Review Letters

The Lorenz number in CeCoIn5_5 inferred from the thermal and charge Hall currents

The thermal Hall conductivity $\kappa_{xy}$ and Hall conductivity $\sigma_{xy}$ in CeCoIn$_5$ are used to determine the Lorenz number ${\cal L}_H$ at low temperature $T$. This enables the separation of the observed thermal conductivity into its electronic and non-electronic parts. We uncover evidence for a charge-neutral, field-dependent thermal conductivity, which we identify with spin excitations. At low $T$, these excitations dominate the scattering of charge carriers. We show that suppression of the spin excitations in high fields leads to a steep enhancement of the electron mean-free-path, which leads to an interesting scaling relation between the magnetoresistance, thermal conductivity and $\sigma_{xy}$.Comment: 6 pages, 7 figures Intro para slightly lengthened. Added 2 new re

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 $H_{c1}$.Comment: 4 pages, 4 figures, submitted to Phys. Rev. Lett. Replaced original text with additional conten