Magnetic susceptibility, Cu NQR, and high-filed magnetization have been measured in polycrystalline SrCu 2 ͑BO 3 ͒ 2 having a two-dimensional (2D) orthogonal network of Cu dimers. This cuprate provides a new class of 2D spin-gap system ͑D 30 K͒ in which the ground state can be solved "exactly." Furthermore, in the magnetization, two plateaus corresponding to 1 4 and 1 8 of the full Cu moment were first observed for 2D quantum spin systems. [S0031-9007(99)08878-X]

High-field magnetization measurements up to 57 T have been performed at 0.08 K in a single crystal of a two-dimensional spin-gap material SrCu 2 (BO 3 ) 2 . We successfully observed the predicted plateau at 1/3 of the total magnetization around 50 T, in which the magnetic superstructure is characterized by a novel stripe order of triplets. The 1/3 plateau is much wider than the previously observed 1/4 and 1/8 plateaux.

We performed inelastic neutron scattering on the 2D Shastry-Sutherland system SrCu 2 ( 11 BO 3 ) 2 with an exact dimer ground state. Three energy levels at around 3, 5 and 9 meV were observed at 1.7 K. The lowest excitation at 3.0 meV is almost dispersionless with a bandwidth of 0.2 meV at most, showing a significant constraint on a single-triplet hopping owing to the orthogonality of the neighboring dimers. In contrast, the correlated two-triplets excitations at 5 meV exhibit a more dispersive behavior.-1-

Various spin gap excitations have been observed in the two-dimensional dimer system SrCu2(BO3)2 by means of submillimeter wave ESR. The zero-field energy gap of the lowest spin gap excitation shows a splitting into two triplet modes and the energy splitting clearly depends on the magnetic field orientation when a field is rotated in the ac-plane. A zero-field splitting is also found between the Sz=+1 and Sz=-1 branches of each triplet. These behaviors are qualitatively explained by considering the anisotropic exchange coupling of inter-dimer and intra-dimer, respectively. The averaged value of the lowest spin gap energy is determined to be 722±2 GHz(34.7 K). We have also found the second spin gap excitation at 1140 GHz(54.7 K), which indicates that the inter-dimer coupling is significantly strong. Besides these modes, a number of gapped ESR absorption are found and we propose that these multiple magnetic excitations are caused by the localized nature of the excited state in the present system.

Raman light scattering of the two-dimensional quantum spin system SrCu2(BO3)(2) shows a rich structure in the magnetic excitation spectrum, including several well-defined bound state modes at low temperature, and a scattering continuum and quasielastic light scattering contributions at high temperature. The key to the understanding of the unique features of SrCu2(BO3)(2) is the presence of strong interactions between well-localized triplet excitations in the network of orthogonal spin dimers realized in this compound.

A displacive, 2 nd order structural phase transition at T s =395 K from space group I4 2 m below T s to I 4/m c m above T s has been discovered in the two-dimensional spin dimer compound SrCu 2 (BO 3 ) 2 . The temperature evolution of the structure in both phases has been studied by Xray diffraction and Raman scattering, supplemented by differential scanning calorimetry and SQUID magnetometry. The implications of this transition and of the observed phonon anomalies in Raman scattering for spin-phonon and interlayer coupling in this quantum spin system will be discussed.

The magnetic properties of a two-dimensional spin-gap compound SrCu 2 (BO 3) 2 , realizing the Shastry-Sutherland model, were investigated using high-quality single crystals. The analysis of the temperature-dependent magnetic susceptibility revealed a spin gap of 34 K. The magnetization curve at 0.4 K possibly has, in addition to the already established one-quarter and one-eighth plateaux, another quantized plateau at one-tenth of the full Cu moment, which is one of the plateaux predicted by Miyahara and Ueda.

Using far-infrared spectroscopy in magnetic fields up to 12 T we have studied a two-dimensional dimer spin gap system SrCu2(BO3)2. We found several infrared active modes in the dimerized state (below 10 K) in the frequency range from 3 to 100 cm −1 . The measured splitting from the ground state to the excited triplet MS = 0 sublevel is ∆1 = 24.2 cm −1 and the other two triplet state sublevels in zero magnetic field are 1.4 cm −1 below and above the MS = 0 sublevel. Another multiplet is at ∆2 = 37.6 cm −1 from the ground state. A strong electric dipole active transition polarized in the (ab)-plane is activated in the dimer spin system below 15 K at 52 cm −1 .