Spin-Triplet Excitons in the S=1/2S=1/2 Gapped Antiferromagnet BaCuSi2_2O6_6: Electron Paramagnetic Resonance Studies

BaCuSi$_2$O$_6$, a $S=1/2$ quantum antiferromagnet with a double-layer structure of Cu$^{2+}$ ions in a distorted planar-rectangular coordination and with a dimerized spin singlet ground state, is studied by means of the electron paramagnetic resonance technique. It is argued that multiple absorptions observed at low temperatures are intimately related to a thermally-activated spin-triplet exciton superstructure. Analysis of the angular dependence of exciton modes in BaCuSi$_2$O$_6$ allows us to accurately estimate anisotropy parameters. In addition, the temperature dependence of EPR intensity and linewidth is discussed.Comment: Submitted to Phys. Rev.

Electron Spin Resonance in sine-Gordon spin chains in the perturbative spinon regime

We report the low-temperature multi-frequency ESR studies of copper pyrimidine dinitrate, a spin-1/2 antiferromagnetic chain with alternating $g$-tensor and the Dzyaloshinskii-Moriya interaction, allowing us to test a new theoretical concept proposed recently by Oshikawa and Affleck [Phys. Rev. Lett. 82, 5136 (1999)]. Their theory, based on bosonization and the self-energy formalism, can be applied for precise calculation of ESR parameters of $S=1/2$ antiferromagnetic chains in the perturbative spinon regime. Excellent quantitative agreement between the theoretical predictions and experiment is obtained.Comment: 4 pages, 4 figure

Excitation hierarchy of the quantum sine-Gordon spin chain in strong magnetic field

The magnetic excitation spectrum of copper pyrimidine dinitrate, a material containing S=1/2 antiferromagnetic chains with alternating g-tensor and the Dzyaloshinskii-Moriya interaction, and exhibiting a field-induced spin gap, is probed using submillimeter wave electron spin resonance spectroscopy. Ten excitation modes are resolved in the low-temperature spectrum, and their frequency-field diagram is systematically studied in magnetic fields up to 25 T. The experimental data are sufficiently detailed to make a very accurate comparison with predictions based on the quantum sine-Gordon field theory. Signatures of three breather branches and a soliton, as well as those of several multi-particle excitation modes are identified.Comment: 4 RevTeX pages, 3 figure

Magnetic excitations in the spin-1 anisotropic antiferromagnet NiCl2−4SC(NH2)2NiCl_2-4SC(NH_2)_2

The spin-1 anisotropic antiferromagnet NiCl_2-4SC(NH2)_2 exhibits a field-induced quantum phase transition that is formally analogous to Bose-Einstein condensation. Here we present results of systematic high-field electron spin resonance (ESR) experimental and theoretical studies of this compound with a special emphasis on single-ion two-magnon bound states. In order to clarify some remaining discrepancies between theory and experiment, the frequency-field dependence of magnetic excitations in this material is reanalyzed. In particular, a more comprehensive interpretation of the experimental signature of single-ion two-magnon bound states is shown to be fully consistent with theoretical results. We also clarify the structure of the ESR spectrum in the so-called intermediate phase.Comment: 9 pages, 10 figure

Magnetic excitations in the spin-1/2 triangular-lattice antiferromagnet Cs2_2CuBr4_4

We report on high-field electron spin resonance (ESR) studies of magnetic excitations in the spin-1/2 triangular-lattice antiferromagnet Cs$_2$CuBr$_4$. Frequency-field diagrams of ESR excitations are measured for different orientations of magnetic fields up to 25 T. We show that the substantial zero-field energy gap, $\Delta\approx9.5$ K, observed in the low-temperature excitation spectrum of Cs$_2$CuBr$_4$ [Zvyagin $et~al.$, Phys. Rev. Lett. 112, 077206 (2014)], is present well above $T_N$. Noticeably, the transition into the long-range magnetically ordered phase does not significantly affect the size of the gap, suggesting that even below $T_N$ the high-energy spin dynamics in Cs$_2$CuBr$_4$ is determined by short-range-order spin correlations. The experimental data are compared with results of model spin-wave-theory calculations for spin-1/2 triangle-lattice antiferromagnet.Comment: 6 pages, 9 figure

Magnetic Excitations in the Spin-1 Anisotropic Heisenberg Antiferromagnetic Chain System NiCl2_2-4SC(NH2_2)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)], 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

Long-range ferromagnetic dipolar ordering of high-spin molecular clusters

We report the first example of a transition to long-range magnetic order in a purely dipolarly interacting molecular magnet. For the magnetic cluster compound Mn6O4Br4(Et2dbm)6, the anisotropy experienced by the total spin S=12 of each cluster is so small that spin-lattice relaxation remains fast down to the lowest temperatures, thus enabling dipolar order to occur within experimental times at Tc = 0.16 K. In high magnetic fields, the relaxation rate becomes drastically reduced and the interplay between nuclear- and electron-spin lattice relaxation is revealed.Comment: 4 pages, 4 .eps figures; accepted for publication in Phys. Rev. Let