We report results of 11 B NMR and susceptibility measurements on the quasi 2D frustrated dimer spin system SrCu2(BO3)2 under high pressure. At 2.4 GPa and in a magnetic field of 7 T, NMR lines split with decreasing temperature in two steps. A gradual splitting below T =30 K breaking the four-fold symmetry of magnetic response is followed by a further sudden splitting below 3.6 K. The latter indicates a magnetic phase transition, which is also marked by a kink in the susceptibility at 1.44 GPa. From the magnetic hyperfine shift data, we conclude that the low-T phase has a doubled unit cell containing two types of dimers, one in a nearly singlet state and the other with a finite magnetization down to T =0.KEYWORDS: SrCu2(BO3)2, Shastry-Sutherland model, high pressure, NMR, phase transition A variety of exotic phenomena has been discovered in the quasi two dimensional dimer spin system SrCu 2 (BO 3 ) 2 .1, 2 It has an alternating stack of the magnetic CuBO 3 layers (Figs. 1(a) and 1(b)) and the nonmagnetic Sr layers.3, 4 The magnetic layer containing orthogonal arrays of spin-1/2 Cu 2+ dimers is a realization of the 2D Shastry-Sutherland model,where J (J ′ ) is the intradimer (interdimer) Heisenberg exchange interaction. The ground state of this model is obvious in two limiting cases: the dimer singlet phase for J ′ /J << 1 and the Néel ordered phase for J ′ /J >> 1. The dimer singlet phase is known to be stable up to (J ′ /J) c =0.68. [6][7][8] Various experiments have established that SrCu 2 (BO 3 ) 2 has a dimer singlet ground state at ambient pressure and zero magnetic field 1, 9, 10 with the energy gap of 33 K 11-13 and J ′ /J=0.60-0.64.
14, 15Frustration in the Shastry-Sutherland model strongly suppresses the kinetic energy of triplets.6 Indeed SrCu 2 (BO 3 ) 2 has an extremely small width of the triplet dispersion (∼0.2meV 12,13 scattering. It also leads to the magnetization plateaus at 1/8, 1/4, and 1/3 of the saturated magnetization in high magnetic fields, 19 where triplets crystalize in commensurate superlattices due to mutual repulsion.
20-23Since J ′ /J in SrCu 2 (BO 3 ) 2 is close to the critical value, tuning the exchange parameters, e.g. by applying pressure, might enable us to explore the phase diagram of the Shastry-Sutherland model, which is still an open issue. A plaquette singlet phase was proposed to exist between the dimer singlet and the Néel ordered phase.8, 24 Alternatively, instability of two-triplet bound * E-mail address: twac@issp.u-tokyo.ac.jp † Present address: Hitachi Medical Corporation, Kashiwa, Chiba ‡ E-mail address: masashi@issp.u-tokyo.ac.jp states 25 may lead to a spin nematic phase. Further variation may arise from the Dzyaloshinski-Moriya interaction beyond the Shastry-Sutherland model.
26In spite of such interest, only a few experiments under pressure have been reported to date. Magnetic susceptibility data up to P =0.7 GPa indicates reduction of the energy gap extrapolating to zero near P =2.5-3.0 GPa.
27The X-ray study shows a tetragonal to monoclinic structural transit...