Search

We report the manifestation of field-induced Berezinskii-Kosterlitz-Thouless (BKT) correlations in the weakly coupled spin-1/2 Heisenberg layers of the molecular-based bulk material [Cu(pz)$_2$(2-HOpy)$_2$](PF$_6$)$_2$. Due to the moderate intralayer exchange coupling of $J/k_\mathrm{B} = 6.8$ K, the application of laboratory magnetic fields induces a substantial $XY$ anisotropy of the spin correlations. Crucially, this provides a significant BKT regime, as the tiny interlayer exchange $J^\prime / k_\mathrm{B} \approx 1$ mK only induces 3D correlations upon close approach to the BKT transition with its exponential growth in the spin-correlation length. We employ nuclear magnetic resonance and $\mu^{+}$SR measurements to probe the spin correlations that determine the critical temperatures of the BKT transition as well as that of the onset of long-range order. Further, we perform stochastic series expansion quantum Monte Carlo simulations based on the experimentally determined model parameters. Finite-size scaling of the in-plane spin stiffness yields excellent agreement of critical temperatures between theory and experiment, providing clear evidence that the nonmonotonic magnetic phase diagram of [Cu(pz)$_2$(2-HOpy)$_2$](PF$_6$)$_2$ is determined by the field-tuned $XY$ anisotropy and the concomitant BKT physics., Comment: 10 pages, 7 figures

We present a detailed $^{31}$P nuclear magnetic resonance (NMR) study of the molecular rotation in the compound [Cu(pz)$_{2}$(2-HOpy)$_{2}$](PF$_{6}$)$_{2}$, where pz = C$_4$H$_4$N$_2$ and 2-HOpy = C$_5$H$_4$NHO. Here, a freezing of the PF$_6$ rotation modes is revealed by several steplike increases of the temperature-dependent second spectral moment, with accompanying broad peaks of the longitudinal and transverse nuclear spin-relaxation rates. An analysis based on the Bloembergen-Purcell-Pound (BPP) theory quantifies the related activation energies as $E_{a}/k_{B}$ = 250 and 1400 K. Further, the anisotropy of the second spectral moment of the $^{31}$P absorption line was calculated for the rigid lattice, as well as in the presence of several sets of PF$_6$ reorientation modes, and is in excellent agreement with the experimental data. Whereas the anisotropy of the frequency shift and enhancement of nuclear spin-relaxation rates is driven by the molecular rotation with respect to the dipole fields stemming from the Cu ions, the second spectral moment is determined by the intramolecular interaction of nuclear $^{19}$F and $^{31}$P moments in the presence of the distinct rotation modes., Comment: 9 pages, 5 figures; additionally 2 pages with 3 figures of supplemental material; typos corrected, references added, supplemental material added

We report on a comprehensive characterization of the newly synthesized Cu$^{2+}$-based molecular magnet [Cu(pz)$_2$(2-HOpy)$_2$](PF$_6$)$_2$ (CuPOF), where pz = C$_4$H$_4$N$_2$ and 2-HOpy = C$_5$H$_4$NHO. From a comparison of theoretical modeling to results of bulk magnetometry, specific heat, $\mu^+$SR, ESR, and NMR spectroscopy, this material is determined as an excellent realization of the 2D square-lattice $S=1/2$ antiferromagnetic Heisenberg model with a moderate intraplane nearest-neighbor exchange coupling of $J/k_\mathrm{B} = 6.80(5)$ K, and an extremely small interlayer interaction of about 1 mK. At zero field, the bulk magnetometry reveals a temperature-driven crossover of spin correlations from isotropic to $XY$ type, caused by the presence of a weak intrinsic easy-plane anisotropy. A transition to long-range order, driven by the low-temperature $XY$ anisotropy under the influence of the interlayer coupling, occurs at $T_\mathrm{N} = 1.38(2)$ K, as revealed by $\mu^+$SR. In applied magnetic fields, our $^1$H-NMR data reveal a strong increase of the magnetic anisotropy, manifested by a pronounced enhancement of the transition temperature to commensurate long-range order at $T_\mathrm{N} =2.8$ K and 7 T., Comment: 14 pages, 8 figures, as well as 10 pages and 18 figures of supplemental material

Cu(pz)$_2$(ClO$_4$)$_2$ (with pz denoting pyrazine C$_4$H$_4$N$_2$) is a two-dimensional spin-1/2 square-lattice antiferromagnet with $T_{\mathrm{N}}$ = 4.24 K. Due to a persisting focus on the low-temperature magnetic properties, its room-temperature structural and physical properties caught no attention up to now. Here we report a study of the structural features of Cu(pz)$_2$(ClO$_4$)$_2$ in the paramagnetic phase, up to 330 K. By employing magnetization, specific heat, $^{35}$Cl nuclear magnetic resonance, and neutron diffraction measurements, we provide evidence of a second-order phase transition at $T^{\star}$ = 294 K, not reported before. The absence of a magnetic ordering across $T^{\star}$ in the magnetization data, yet the presence of a sizable anomaly in the specific heat, suggest a structural order-to-disorder type transition. NMR and neutron-diffraction data corroborate our conjecture, by revealing subtle angular distortions of the pyrazine rings and of ClO$^-_4$ counteranion tetrahedra, shown to adopt a configuration of higher symmetry above the transition temperature., Comment: 10 pages, 12 figures

We demonstrate that quantum-critical spin dynamics can be probed in high magnetic fields using muon-spin relaxation ($\mu^{+}$SR). Our model system is the strong-leg spin ladder bis(2,3-dimethylpyridinium) tetrabromocuprate (DIMPY). In the gapless Tomonaga-Luttinger liquid phase we observe finite-temperature scaling of the $\mu^{+}$SR $1/T_1$ relaxation rate which allows us to determine the Luttinger parameter $K$. We discuss the benefits and limitations of local probes compared with inelastic neutron scattering., Comment: 7 pages, 7 figures

Cu(pz)2(ClO4)2 (with pz denoting pyrazine, C4H4N2) is among the best realizations of a two-dimensional spin-1/2 square-lattice antiferromagnet. Below T_N = 4.21 K, its weak interlayer couplings induce a 3D magnetic order, strongly influenced by external magnetic fields and/or hydrostatic pressure. Previous work, focusing on the [H, T] phase diagram, identified a spin-flop transition, resulting in a field-tunable bicritical point. However, the influence of external pressure has not been investigated yet. Here we explore the extended [p, H, T] phase diagram of Cu(pz)2(ClO4)2 under pressures up to 12 kbar and magnetic fields up to 7.1 T, via magnetometry and 35Cl nuclear magnetic resonance (NMR) measurements. The application of magnetic fields enhances T_XY , the crossover temperature from the Heisenberg to the XY model, thus pointing to an enhancement of the effective anisotropy. The applied pressure has an opposite effect [dT_N/dp = 0.050(8) K/kbar], as it modifies marginally the interlayer couplings, but likely changes more significantly the orbital reorientation and the square-lattice deformation. This results in a remodeling of the effective Hamiltonian, whereby the field and pressure effects compensate each other. Finally, by comparing the experimental data with numerical simulations we estimate T_BKT, the temperature of the Berezinskii-Kosterlitz-Thouless topological transition and argue why it is inaccessible in our case., Comment: 7 pages, 9 figures

Raman spectroscopy is used to study magnetic excitations in the quasi one dimensional $S=1/2$ quantum spin systems Cu(Qnx)(Cl$_{1-x}$Br$_x$)$_2$. The low energy spectrum is found to be dominated by a two-magnon continuum as expected from the numerical calculations for the Heisenberg spin ladder model. The continuum shifts to higher energies as more Br is introduced. The cutoff of the scattering increases faster than the onset indicating that the increase of exchange constant along the leg is the main effect on the magnetic properties. The upper and lower continuum thresholds are measured as a function of Br content across the entire range and compared to estimates based on previous bulk studies. We observe small systematic deviations that are discussed.

Magnetic excitations in the strong-leg quantum spin ladder compound (C$_7$H$_{10}$N)$_2$CuBr$_4$ (known as DIMPY) in the field-induced Tomonaga-Luttinger spin liquid phase are studied by means of high-field electron spin resonance (ESR) spectroscopy. The presence of a gapped ESR mode with unusual non-linear frequency-field dependence is revealed experimentally. Using a combination of analytic and exact diagonalization methods, we compute the dynamical structure factor and identify this mode with longitudinal excitations in the antisymmetric channel. We argue that these excitations constitute a fingerprint of the spin dynamics in a strong-leg spin-1/2 Heisenberg antiferromagnetic ladder and owe its ESR observability to the uniform Dzyaloshinskii-Moriya interaction.

Cu(C$_8$H$_6$N$_2$)Cl$_2$, a strong-rung spin-1/2 Heisenberg ladder compound, is probed by means of electron spin resonance (ESR) spectroscopy in the field-induced gapless phase above $H_{c1}$. The temperature dependence of the ESR linewidth is analyzed in the quantum field theory framework, suggesting that the anisotropy of magnetic interactions plays a crucial role, determining the peculiar low-temperature ESR linewidth behavior. In particular, it is argued that the uniform Dzyaloshinskii-Moriya interaction (which is allowed on the bonds along the ladder legs) can be the source of this behavior in Cu(C$_8$H$_6$N$_2$)Cl$_2$.

We report magnetic, specific heat and ESR measurements on a series of $S=1/2$ spin ladder compounds Cu(Qnx)(Cl$_{(1-x)}$Br$_{x}$)$_{2}$. Down to $T=2$ K all the observables can be described by the spin ladder model with about 1% of $S=1/2$ impurities in the background, which are present even in a nominally pure Cu(Qnx)Cl$_{2}$ and Cu(Qnx)Br$_{2}$, for the whole range of $0\leq x\leq1$. We extract ladder exchange constants $J_{l}(x)$ and $J_{r}(x)$ as well as the gap value $\Delta(x)$ by comparing the experimental data to quantum Monte-Carlo simulations. As the ESR measurements show the $g$-factor of impurities to be precisely equal to $g$-factor of the ladder spins, we suppose the impurities to be the consequence of structural defects resulting in a broken ladder ends., Comment: 8 pages, 7 figures

Experiments in the antiferromagnetic phase of a quasi 2D $S=1/2$ quasi-square lattice antiferromagnet Cu(pz)2(ClO4)2 reveal a biaxial type of the anisotropy, instead of the easy-plane one, considered before. The weak in-plane anisotropy, found by means of electron spin resonance spectroscopy and magnetization measurements, is about an order of magnitude weaker, than the off-plane anisotropy. The weak in-plane anisotropy results in a spin-flop phase transition for the magnetic field aligned along easy axis, and, thereby, in a bicritical point on the phase diagram. A remarkable feature of the weak in-plane anisotropy is the abrupt change of its sign at the spin-flop point. This anisotropy switching disappears at the tilting of magnetic field to the easy axis by the angle of 10$^\circ$ within the plane. The nature of the abrupt anisotropy reversal remains unclear. The phase diagram is characterized by the increase of the ordering temperature in the magnetic field used, except for a dip near the bicritical point., Comment: 14 pages, 22 figures

By means of electron spin resonance investigations we revealed the crucial role of the interchain coupling in the spin dynamics of the spin-1/2 Heisenberg antiferromagnetic (AF) chain material copper-pyrazine-dinitrate, Cu(C$_4$H$_4$N$_2$)(NO$_3$)$_2$. We found that the dominating interchain interaction is of a zig-zag type. This interaction gives rise to geometrical frustration effects and strongly influences the character of AF ordering. Combining our experimental findings with the results of a quasiclassical approach we argue that at low temperatures the system orders in an incommensurate spiral state., Comment: 5 pages, 5 figures

The influence of bond randomness on long range magnetic ordering in the weakly coupled S = 1/2 antiferromagnetic spin chain materials Cu(py)2(Cl1-xBrx)2 is studied by muon spin rotation and bulk measurements. Disorder is found to have a strong effect on the ordering temperature TN, and an even stronger one on the saturation magnetization m0, but considerably more so in the effectively lower-dimensional Br-rich materials. The observed behavior is attributed to Random Singlet ground states of individual spin chains, but remains in contradiction with chain mean field theory predictions. In this context, we discuss the possibility of a universal distribution of ordered moments in the weakly coupled Random Singlet chains model.

Using micromechanical force magnetometry, we have measured the magnetization of the strong-leg spin-1/2 ladder compound (C$_7$H$_{10}$N)$_2$CuBr$_2$ at temperatures down to 45 mK. Low-temperature magnetic susceptibility as a function of field exhibits a maximum near the critical field H_c at which the magnon gap vanishes, as expected for a gapped one-dimensional antiferromagnet. Above H_c a clear minimum appears in the magnetization as a function of temperature as predicted by theory. In this field region, the susceptibility in conjunction with our specific heat data yields the Wilson ratio R_W. The result supports the relation R_W=4K, where K is the Tomonaga-Luttinger-liquid parameter.

Inelastic neutron scattering was used to study a quantum S=1/2 antiferromagnetic Heisenberg system-Bis(2-amino-5-fluoropyridinium) Tetrachlorocuprate(II). The magnetic excitation spectrum was shown to be dominated by long-lived excitations with an energy gap as 1.07(3) meV. The measured dispersion relation is consistent with a simple two-dimensional square lattice of weakly-coupled spin dimers. Comparing the data to a random phase approximation treatment of this model gives the intra-dimer and inter-dimer exchange constants J=1.45(2) meV and J'=0.31(3) meV, respectively., Comment: 4 pages, 4 figures

We study the magnetic-field-induced quantum phase transition from a gapped quantum phase that has no magnetic long-range order into a gapless phase in the spin-1/2 ladder compound bis(2,3-dimethylpyridinium) tetrabromocuprate (DIMPY). At temperatures below about 1 K, the specific heat in the gapless phase attains an asymptotic linear temperature dependence, characteristic of a Tomonaga-Luttinger liquid. Inelastic neutron scattering and the specific heat measurements in both phases are in good agreement with theoretical calculations, demonstrating that DIMPY is the first model material for an S=1/2 two-leg spin ladder in the strong-leg regime., Comment: 4.1 pages, 4 figures (Fig. 4 updated), to appear in Physical Review Letters

A comprehensive comparison between the magnetic field- and temperature-dependent low frequency spin dynamics in the antiferromagnetic spin-1/2 Heisenberg chain (AFHC) system copper pyrazine dinitrate, probed via the 13C-nuclear magnetic resonance (NMR) relaxation rate 1/T1, and the field theoretical approach in the Luttinger liquid (LL) regime has been performed. We have found a very good agreement between the experiment and theory in the investigated temperature and field range. Our results demonstrate how strongly the quantum critical point affects the spin dynamics of Heisenberg spin chain compounds., Comment: 5 pages, 3 figures

We present an experimental study of the two-dimensional S=1/2 square-lattice antiferromagnet Cu(pz)$_2$(ClO$_4$)$_2$ (pz denotes pyrazine - $C_4H_4N_2$) using specific heat measurements, neutron diffraction and cold-neutron spectroscopy. The magnetic field dependence of the magnetic ordering temperature was determined from specific heat measurements for fields perpendicular and parallel to the square-lattice planes, showing identical field-temperature phase diagrams. This suggest that spin anisotropies in Cu(pz)$_2$(ClO$_4$)$_2$ are small. The ordered antiferromagnetic structure is a collinear arrangement with the magnetic moments along either the crystallographic b- or c-axis. The estimated ordered magnetic moment at zero field is m_0=0.47(5)mu_B and thus much smaller than the available single-ion magnetic moment. This is evidence for strong quantum fluctuations in the ordered magnetic phase of Cu(pz)$_2$(ClO$_4$)$_2$. Magnetic fields applied perpendicular to the square-lattice planes lead to an increase of the antiferromagnetically ordered moment to m_0=0.93(5)mu_B at mu_0H=13.5T - evidence that magnetic fields quench quantum fluctuations. Neutron spectroscopy reveals the presence of a gapped spin excitations at the antiferromagnetic zone center, and it can be explained with a slightly anisotropic nearest neighbor exchange coupling described by J_1^{xy}=1.563(13)meV and J_1^z=0.9979(2)J_1^{xy}.

Low-energy magnetic excitations in the spin-1/2 chain compound (C$_6$H$_9$N$_2$)CuCl$_3$ [known as (6MAP)CuCl$_3$] are probed by means of tunable-frequency electron spin resonance. Two modes with asymmetric (with respect to the $h\nu=g\mu_B B$ line) frequency-field dependences are resolved, illuminating the striking incompatibility with a simple uniform $S=\frac{1}{2}$ Heisenberg chain model. The unusual ESR spectrum is explained in terms of the recently developed theory for spin-1/2 chains, suggesting the important role of next-nearest-neighbor interactions in this compound. Our conclusion is supported by model calculations for the magnetic susceptibility of (6MAP)CuCl$_3$, revealing a good qualitative agreement with experiment.

The S=1/2 antiferromagnetic Heisenberg chain exhibits a magnetic field driven quantum critical point. We study the low frequency spin dynamics in copper pyrazine dinitrate (CuPzN), a realization of this model system of quantum magnetism, by means of $^{13}$C-NMR spectroscopy. Measurements of the nuclear spin-lattice relaxation rate $T_1^{-1}$ in the vicinity of the saturation field are compared with quantum Monte Carlo calculations of the dynamic structure factor. Both show a strong divergence of low energy excitations at temperatures in the quantum regime. The analysis of the anisotropic $T_1^{-1}$-rates and frequency shifts allows one to disentangle the contributions from transverse and longitudinal spin fluctuations for a selective study and to determine the transfer of delocalized spin moments from copper to the neighboring nitrogen atoms., Comment: 5 pages, 6 figures, published in Physica Status Solidi B

We have studied the two-dimensional S=1/2 square-lattice antiferromagnet $Cu(pz)_2(ClO_4)_2$ using inelastic neutron scattering and series expansion calculations. We show that the presence of antiferromagnetic next-nearest neighbor interactions enhances quantum fluctuations associated with resonating valence bonds. Intermediate magnetic fields lead to a selective tuning of resonating valence bonds and a spectacular inversion of the zone-boundary dispersion, providing novel insight into 2D antiferromagnetism in the quantum limit., Comment: 4 pages, 5 figures

The magnetic properties of a new family of molecular-based quasi-two dimension $S=1/2$ Heisenberg antiferromagnets are reported. Three compounds, ($Cu(pz)_2(ClO_4)_2$, $Cu(pz)_2(BF_4)_2$, and $[Cu(pz)_2(NO_3)](PF_6)$) contain similar planes of Cu$^{2+}$ ions linked into magnetically square lattices by bridging pyrazine molecules (pz = $C_4H_4N_2$). The anions provide charge balance as well as isolation between the layers. Single crystal measurements of susceptibility and magnetization, as well as muon spin relaxation studies, reveal low ratios of N\'{e}el temperatures to exchange strengths ($4.25 / 17.5 = 0.243$, $3.80/15.3=0.248$, and $3.05/10.8=0.282$, respectively) while the ratio of the anisotropy fields $H_A$ (kOe) to the saturation field $H_\mathrm{SAT}$ (kOe) are small ($2.6/490 = 5.3\times10^{-3}$, $2.4/430=5.5\times10^{-3}$, and $0.07/300=2.3\times10^{-4}$, respectively), demonstrating close approximations to a 2D Heisenberg model. The susceptibilities of ClO$_4$ and BF$_4$ show evidence of an exchange anisotropy crossover (Heisenberg to $XY$) at low temperatures; their ordering transitions are primarily driven by the $XY$ behavior with the ultimate 3D transition appearing parasitically. The PF$_6$ compound remains Heisenberg-like at all temperatures, with its transition to the N\'{e}el state due to the interlayer interactions. Effects of field-induced anisotropy have been observed., Comment: Accepted for publication in Physical Review B

We present a 13C-NMR study of the magnetic field driven transition to complete polarization of the S=1/2 antiferromagnetic Heisenberg chain system copper pyrazine dinitrate Cu(C_4H_4N_2)(NO_3)_2 (CuPzN). The static local magnetization as well as the low-frequency spin dynamics, probed via the nuclear spin-lattice relaxation rate 1/T_1, were explored from the low to the high field limit and at temperatures from the quantum regime (k_B T << J) up to the classical regime (k_B T >> J). The experimental data show very good agreement with quantum Monte Carlo calculations over the complete range of parameters investigated. Close to the critical field, as derived from static experiments, a pronounced maximum in 1/T_1 is found which we interpret as the finite-temperature manifestation of a diverging density of zero-energy magnetic excitations at the field-driven quantum critical point., Comment: 5 pages, 4 figures

Results of magnetization and high-field ESR studies of the new spin-1 Haldane-chain material [Ni(C2H8N2)2NO2](BF4) (NENB) are reported. A definite signature of the Haldane state in NENB was obtained. From the analysis of the frequency-field dependence of magnetic excitations in NENB, the spin-Hamiltonian parameters were calculated, yielding Delta = 17.4 K, g_parallel = 2.14, D = 7.5 K, and |E| = 0.7 K for the Haldane gap, g factor and the crystal-field anisotropy constants, respectively. The presence of fractional S = 1/2 chain-end states, revealed by ESR and magnetization measurements, is found to be responsible for spin-glass freezing effects. In addition, extra states in the excitation spectrum of NENB have been observed in the vicinity of the Haldane gap, which origin is discussed., Comment: 5 pages, 6 figures

We present an investigation of magnetic ordering in the two-dimensional S=1/2 quantum magnet Cu(Pz)_2(ClO_4)_2 using specific heat and zero field muon-spin relaxation (\mu^+SR). The magnetic contribution to the specific heat is consistent with an exchange strength of 17.7(3) K. We find unambiguous evidence for a transition to a state of three-dimensional long range order below a critical temperature T_N=4.21(1) K using \mu^+SR even though there is no feature in the specific heat at that temperature. The absence of a specific heat anomaly at T_N is consistent with recent theoretical predictions. The ratio of T_N/J=0.24 corresponds to a ratio of intralayer to interlayer exchange constants of |J'/J|=6.8x10^-4, indicative of excellent two-dimensional isolation. The scaled magnetic specific heat of [Cu(Pz)_2(HF_2)]BF_4, a compound with an analogous structure, is essentially identical to that of Cu(Pz)_2(ClO_4)_2 although both differ slightly from the predicted value for an ideal 2D S=1/2 Heisenberg antiferromagnet., Comment: 7 pages, 4 figures

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., Comment: 10 pages, 11 figures, 1 table

We present the first evidence of magnetic order in the quasi-one-dimensional spin 1/2 molecular chain compound, copper pyrazine dinitrate Cu(C4H4N2)(NO3)2}. Zero field muon-spin relaxation measurements made at dilution refrigerator temperatures show oscillations in the measured asymmetry, characteristic of a quasistatic magnetic field at the muon sites. Our measurements provide convincing evidence for long range magnetic order below a temperature T_N=107(1) mK. This leads to an estimate of the interchain coupling constant of |J'|/k_B=0.046 K and to a ratio |J'/J| = 4.4 x 10^-3., Comment: 4 pages, 3 figures. Submitted to Physical Review Letters

Measurements are reported of the magnetic field dependence of excitations in the quantum critical state of the spin S=1/2 linear chain Heisenberg antiferromagnet copper pyrazine dinitrate (CuPzN). The complete spectrum was measured at k_B T/J <= 0.025 for H=0 and H=8.7 Tesla where the system is ~30% magnetized. At H=0, the results are in quantitative agreement with exact calculations of the dynamic spin correlation function for a two-spinon continuum. At high magnetic field, there are multiple overlapping continua with incommensurate soft modes. The boundaries of these continua confirm long-standing predictions, and the intensities are consistent with exact diagonalization and Bethe Ansatz calculations., Comment: 4 pages, 4 figures

The magnetic susceptibility and magnetization of two new layered S=1/2 Heisenberg antiferromagnets with moderate exchange are reported. The two isostructural compounds, (2-amino-5-chloropyridinium)2CuBr4 ((5CAP)2CuBr4) and (2-amino-5-methylpyridinium)2CuBr4 ((5MAP)2CuBr4), contain S=1/2, Cu(II) ions related by C-centering, yielding four equivalent nearest neighbors. The crystal structure of newly synthesized compound, (5CAP)2CuBr4, shows the existence of layers of distorted copper(II)-bromide tetrahedra parallel to the ab plane, separated by the organic cations along the c axis. Magnetic pathways are available through the bromide-bromide contacts within the layers and provide for moderate antiferromagnetic exchange. Susceptibility measurements indicate interaction strengths to be 8.5(1) K, and 6.5(1) K and ordering temperatures of 5.1(2) K and 3.8(2) K for (5CAP)2CuBr4 and (5MAP)2CuBr4 respectively. High field magnetization experiments on both compounds show upward curvature of M(H,T). Magnetization measurements made at T = 1.3 K show saturation occurs in (5MAP)2CuBr4 at 18.8 T and in (5CAP)2CuBr4 at 24.1 T. The magnetization curves are consistent with recent theoretical predictions. Single crystal magnetization measured at 2.0 K indicate a spin flop transition at 0.38 T and 0.63 T for (5CAP)2CuBr4 and (5MAP)2CuBr4 respectively., Comment: 20 pages, 10 Figures Updated Figures and minor corrections to text

We have synthesized and characterized a new spin-1/2 Heisenberg antiferromagnetic ladder: bis 5-iodo-2-aminopyridinium tetrabromocuprate(II) dihydrate. X-ray diffraction studies show the structure of the compound to consist of well isolated stacked ladders and the interaction between the Cu(2+) atoms to be due to direct Br...Br contacts. Magnetic susceptibility and magnetization studies show the compound to be in the strong-coupling limit, with the interaction along the rungs (J' ~ 13 K) much greater than the interaction along the rails (J ~ 1 K). Magnetic critical fields are observed near 8.3 T and 10.4 T, respectively, establishing the existence of the energy gap., Comment: 10 pages, 4 figures, submitted to Phys. Rev. B Figure 4 did not print. *.eps files replaced with figures.ps file

High field mangetization, field-dependent specific heat measurements, and zero field inelastic magnetic neutron scattering have been used to explore the magnetic properties of copper pyrazine dinitrate (Cu(C4H4N2)(NO3)2). The material is an ideal one-dimensional spin-1/2 Heisenberg antiferromagnet with nearest neighbor exchange constant J=0.90(1) meV and chains extending along the orthorhombic a-direction. As opposed to previosly studied molecular-based spin-1/2 magnetic systems, coppyer pyrazine dinitrate remains gapless and paramagnetic for g mu_B H/J at least up to 1.4 and for k_B T/J at least down to 0.03 this makes the material an excellent model system for exploring the T=0 critical line which is expected in the H - T phase diagram on the one-dimensional spin-1/2 Heisenberg antiferromagnet. As a first example of such a study we present accurate measurements of the Sommerfeld constant of the spinon gas versus g mu_B H/J < 1.4 which reveal a decrease of the averages spinon velocity by 32% in that field range. The results are in excellent agreement with numerical calculations based on the Bethe ansatz with no adjustable parameters., Comment: 9 pages with figures included, 9 figures, Submitted to Phys. Rev. B (8/31/98), email comments to dhr@pha.jhu.edu