Detection of a Disorder-Induced Bose-Einstein Condensate in a Quantum Spin Material at High Magnetic Fields.

The coupled spin-1 chains material NiCl_{2}-4SC(NH_{2})_{2} (DTN) doped with Br impurities is expected to be a perfect candidate for observing many-body localization at high magnetic field: the so-called "Bose glass," a zero-temperature bosonic fluid, compressible, gapless, incoherent, and short-range correlated. Using nuclear magnetic resonance, we critically address the stability of the Bose glass in doped DTN, and find that it hosts a novel disorder-induced ordered state of matter, where many-body physics leads to an unexpected resurgence of quantum coherence emerging from localized impurity states. An experimental phase diagram of this new "order-from-disorder" phase, established from nuclear magnetic resonance T_{1}^{-1} relaxation rate data in the 13±1% Br-doped DTN, is found to be in excellent agreement with the theoretical prediction from large-scale quantum Monte Carlo simulations.

Crossover from one- to three-dimensional behavior in the S = 1/2 Heisenberg antiferromagnet Cu(N2H5)2(SO4)2.

From experimental and theoretical analyses of magnetic and specific-heat properties, we present the complete magnetic phase diagram of the quasi-1D antiferromagnet Cu(N2H5)2(SO4)2. On cooling and at zero magnetic field this compound enters a 1D regime with short-range magnetic correlations, marked by a broad maximum in the specific heat and magnetic susceptibility at [Formula: see text] K, followed by a tridimensional antiferromagnetically ordered phase below [Formula: see text] K induced by small interchain couplings. The intermediate-temperature 1D regime can be modeled using exact quantum-transfer-matrix calculations, which offer a compatible description of the nonmonotonic behavior of [Formula: see text] as a function of the magnetic field, giving [Formula: see text] K for the intrachain exchange parameter. The analysis of magnetic specific-heat and susceptibility data at low temperature indicates that the interchain exchange couplings are an order of magnitude smaller than the coupling inside the chains.

Thermal behavior in the magnetic phase diagram of the easy axis antiferromagnet Cs2FeCl5·H2O.

The specific heat at a constant applied field C(H)(T) and at fixed temperatures C(T)(H) of single crystals of the low anisotropy antiferromagnet Cs2FeCl5·H2O was measured across the different boundaries of its magnetic phase diagram, in magnetic fields up to 9 T applied parallel and perpendicular to the easy axis direction and to temperatures down to 0.3 K. The specific heat data indicate that the critical behavior along the antiferromagnetic to paramagnetic phase boundary and the spin-flop to paramagnetic phase boundary, are basically the same. We also measured the specific heat when the first order antiferromagnetic to spin-flop phase boundary is crossed at a fixed temperature. The entropy of the different magnetic phases is discussed.

Neutron study of the magnetism in NiCl2·4SC(NH2)2.

We study the strongly anisotropic quasi-one-dimensional S = 1 quantum magnet NiCl2·4SC(NH2)2 using elastic and inelastic neutron scattering. We demonstrate that a magnetic field splits the excited doublet state and drives the lower doublet state to zero energy at a critical field Hc1. For Hc1 < H < Hc2, where Hc2 indicates the transition to a fully magnetized state, three-dimensional magnetic order is established with the AF moment perpendicular to the magnetic field. We mapped the temperature/magnetic field phase diagram, and we find that the total ordered magnetic moment reaches m(tot) = 2.1 µB at the field µ(0)H = 6 T and is thus close to the saturation value of the fully ordered moment. We study the magnetic spin dynamics in the fully magnetized state for H > Hc2, and we demonstrate the presence of an AF interaction between Ni(2+) on the two interpenetrating sublattices. In the antiferromagnetically ordered phase, the spin-waves that develop from the lower-energy doublet are split into two modes. This is most likely the result of the presence of the AF interaction between the interpenetrating lattices.

Quantum-critical spin dynamics in quasi-one-dimensional antiferromagnets.

By means of nuclear spin-lattice relaxation rate T(1)(-1), we follow the spin dynamics as a function of the applied magnetic field in two gapped quasi-one-dimensional quantum antiferromagnets: the anisotropic spin-chain system NiCl(2)-4SC(NH(2))(2) and the spin-ladder system (C(5)H(12)N)(2)CuBr(4). In both systems, spin excitations are confirmed to evolve from magnons in the gapped state to spinons in the gapless Tomonaga-Luttinger-liquid state. In between, T(1)(-1) exhibits a pronounced, continuous variation, which is shown to scale in accordance with quantum criticality. We extract the critical exponent for T(1)(-1), compare it to the theory, and show that this behavior is identical in both studied systems, thus demonstrating the universality of quantum-critical behavior.

Thermal transport and strong mass renormalization in NiCl2-4SC(NH2)2.

Several quantum paramagnets exhibit magnetic-field-induced quantum phase transitions to an antiferromagnetic state that exists for H c1 ≤ H ≤ H c2. For some of these compounds, there is a significant asymmetry between the low- and high-field transitions. We present specific heat and thermal conductivity measurements in NiCl2-4SC(NH2)2, together with calculations which show that the asymmetry is caused by a strong mass renormalization due to quantum fluctuations for H ≤ H c1 that are absent for H ≥ H c2. We argue that the enigmatic lack of asymmetry in thermal conductivity is due to a concomitant renormalization of the impurity scattering.

Critical properties at the field-induced Bose-Einstein condensation in NiCl(2)-4SC(NH2)2.

We report new magnetization measurements on the spin-gap compound NiCl(2)-4SC(NH2)2 at the low-field boundary of the magnetic field-induced ordering. The critical density of the magnetization is analyzed in terms of a Bose-Einstein condensation of bosonic quasiparticles. The analysis of the magnetization at the transition leads to the conclusion for the preservation of the U(1) symmetry, as required for Bose-Einstein condensation. The experimental data are well described by quantum Monte Carlo simulations.

Direct measurement of the Bose-Einstein condensation universality class in NiCl2-4SC(NH2)2 at ultralow temperatures.

In this work, we demonstrate field-induced Bose-Einstein condensation (BEC) in the organic compound NiCl2-4SC(NH2)_{2} using ac susceptibility measurements down to 1 mK. The Ni S=1 spins exhibit 3D XY antiferromagnetism between a lower critical field H_{c1} approximately 2 T and a upper critical field H_{c2} approximately 12 T. The results show a power-law temperature dependence of the phase transition line H_{c1}(T)-H_{c1}(0)=aT;{alpha} with alpha=1.47+/-0.10 and H_{c1}(0)=2.053 T, consistent with the 3D BEC universality class. Near H_{c2}, a kink was found in the phase boundary at approximately 150 mK.

Unusual magneto-optical phenomenon reveals low energy spin dispersion in the spin-1 anisotropic Heisenberg antiferromagnetic chain system NiCl2-4SC(NH2)_{2}.

Electron paramagnetic resonance measurements of NiCl2-4SC(NH2)_{2} reveal the low-energy spin dispersion, including a magnetic-field interval in which the two-magnon continuum is within k_{B}T of the ground state, allowing a continuum of excitations over a range of k states, rather than only the k=0 single-magnon excitations. This produces a novel Y shape in the frequency-field EPR spectrum measured at T > or = 1.5 K. Since the interchain coupling J_{ perpendicular}<

Magnetic excitations in the spin-1 anisotropic Heisenberg antiferromagnetic chain system NiCl(2)-4SC(NH(2))(2).

NiCl(2)-4SC(NH(2))(2) (DTN) is a quantum S=1 chain system with strong easy-pane anisotropy and a new candidate for the Bose-Einstein condensation of the spin degrees of freedom. ESR studies of magnetic excitations in DTN in fields up to 25 T are presented. Based on analysis of the single-magnon excitation mode in the high-field spin-polarized phase and previous experimental results [Phys. Rev. Lett. 96, 077204 (2006)10.1103/PhysRevLett.96.077204], a revised set of spin-Hamiltonian parameters is obtained. Our results yield D=8.9 K, J(c) = 2.2 K, and J(a,b) = 0.18 K for the anisotropy, intrachain, and interchain exchange interactions, respectively. These values are used to calculate the antiferromagnetic phase boundary, magnetization, and the frequency-field dependence of two-magnon bound-state excitations predicted by theory and observed in DTN for the first time. Excellent quantitative agreement with experimental data is obtained.

Bose-Einstein condensation of S = 1 nickel spin degrees of freedom in NiCl2-4SC(NH2)2.

It has recently been suggested that the organic compound NiCl2-4SC(NH2)2 (DTN) undergoes field-induced Bose-Einstein condensation (BEC) of the Ni spin degrees of freedom. The Ni S = 1 spins exhibit three-dimensional XY antiferromagnetism above a critical field H(c1) approximately 2 T. The spin fluid can be described as a gas of hard-core bosons where the field-induced antiferromagnetic transition corresponds to Bose-Einstein condensation. We have determined the spin Hamiltonian of DTN using inelastic neutron diffraction measurements, and we have studied the high-field phase diagram by means of specific heat and magnetocaloric effect measurements. Our results show that the field-temperature phase boundary approaches a power-law H - H(c1) proportional variant T(alpha)(c) near the quantum critical point, with an exponent that is consistent with the 3D BEC universal value of alpha = 1.5.