Quantum magnetism and quantum phase transitions

Abstract:

We explore the effects of noncommuting applied fields on the ground-state ordering of the quasi-one-dimensional spin-1/2 XY-like antiferromagnet Cs2CoCl4 using single-crystal neutron diffraction. In zero field interchain couplings cause long-range order below T_N=217(5) mK with chains ordered antiferromagnetically along their length and moments confined to the (b,c) plane. Magnetic fields applied at an angle to the XY planes are found to initially stabilize the order by promoting a spin-flop phase with an increased perpendicular antiferromagnetic moment. In higher fields the antiferromagnetic order becomes unstable and a transition occurs to a phase with no long-range order in the (b,c) plane, proposed to be a spin liquid phase that arises when the quantum fluctuations induced by the noncommuting field become strong enough to overcome ordering tendencies. Magnetization measurements confirm that saturation occurs at much higher fields and that the proposed spin-liquid state exists in the region 2.10 < H_SL < 2.52 T || a. The observed phase diagram is discussed in terms of known results on XY-like chains in coexisting longitudinal and transverse fields.

Abstract:

Low-dimensional magnets with low-spin quatum number are ideal model systems for investigating strongly interacting macroscopic quantum ground states and their non-linear spin excitations. We present single-crystal neutron-diffraction measurements of the ordered phase of the quasi-one-dimensional spin-1/2 XY antiferromagnet Cs2CoCl4 both in zero field and in fields up to 6.5 T. In zero field the system shows long-range order below TN = 217 mK with a commensurate ordering wave-vector (0, 0.5, 0.5). With increasing magnetic field - applied perpendicular to the magnetic chain axis - the magnetic Bragg peak intensities increase monotonically, reaching a maximum at H = 1.4 T; evidence that the magnetic field suppresses quantum fluctuations in the ground state. At Hc = 2.1 T the ordered structure collapses in an apparent first-order phase transition, with no magnetic Bragg peaks being observed in the (0, k, l) scattering plane above this field. This result suggests that the magnetic field induces a phase transition to a spin-liquid ground state. Magnetic Bragg peak intensities at ferromagnetic positions increase quadratically up to about 2.8 T, corresponding to a linear increase of the magnetic moment. At higher magnetic fields, the intensity increases linearly up to 6.5 T.

Abstract:

We have mapped from the quantum to the classical limit the spin excitation spectrum of the antiferromagnetic spin-1 Heisenberg chain system CsNiCl3 in its paramagnetic phase from T=5 to 200K. Neutron scattering shows that the excitations are resonant and dispersive up to at least T=70K, but broaden considerably with increasing temperature. The dispersion flattens out with increasing temperature as the resonance energy Delta at the antiferromagnetic wave-vector increases and the maximum in the dispersion decreases. The correlation length xi between T=12 and 50K is in agreement with quantum Monte Carlo calculations. xi is also consistent with the single mode approximation, suggesting that the excitations are short-lived single particle excitations. Below T=12K where three-dimensional spin correlations are important, xi is shorter than predicted and the experiment is not consistent with the random phase approximation for coupled quantum chains. At T=200K, the structure factor and second energy moment of the excitation spectrum are in excellent agreement with the high-temperature series expansion.

Abstract:

We report inelastic time-of-flight and triple-axis neutron scattering measurements of the excitation spectrum of the coupled antiferromagnetic spin-1 Heisenberg chain system CsNiCl3. Measurements over a wide range of wave-vector transfers along the chain confirm that above T_N CsNiCl3 is in a quantum-disordered phase with an energy gap in the excitation spectrum. The spin correlations fall off exponentially with increasing distance with a correlation length xi=4.0(2) sites at T=6.2K. This is shorter than the correlation length for an antiferromagnetic spin-1 Heisenberg chain at this temperature, suggesting that the correlations perpendicular to the chain direction and associated with the interchain coupling lower the single-chain correlation length. A multi-particle continuum is observed in the quantum-disordered phase in the region in reciprocal space where antiferromagnetic fluctuations are strongest, extending in energy up to twice the maximum of the dispersion of the well-defined triplet excitations. We show that the continuum satisfies the Hohenberg-Brinkman sum rule. The dependence of the multi-particle continuum on the chain wave-vector resembles that of the two-spinon continuum in antiferromagnetic spin-1/2 Heisenberg chains. This suggests the presence of spin-1/2 degrees of freedom in CsNiCl3 for T < 12K, possibly caused by multiply-frustrated interchain interactions.