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2009 MAGNETIC SYSTEMSNuclear magnetic resonance determination of spin-superlattice structureof magnetization plateaus in SrCu 2 (BO 3 ) 2Quantum spin systems are nowadays in the focus of considerableexperim<strong>en</strong>tal and theoretical efforts, in particularfor the magnetic field induced exotic quantum states. Ofspecial interest are interacting systems of Heis<strong>en</strong>berg, antiferromagnetic,S=1/2 spin dimers in a magnetic field whichcloses the gap betwe<strong>en</strong> the singlet and one of three Zeemansplittriplet levels of each dimer. At low temperature, wh<strong>en</strong>only these two states per dimer are relevant, the systemcan be <strong>des</strong>cribed by the corresponding S=1/2 pseudospins,or the equival<strong>en</strong>t hard-core bosons. Interacting dimers areth<strong>en</strong> equival<strong>en</strong>t to a system of interacting bosons where boson(triplet) d<strong>en</strong>sity can be tuned by the magnetic field. Thissystem g<strong>en</strong>erally undergoes a Bose-Einstein cond<strong>en</strong>sation(BEC) and therefore provi<strong>des</strong> an exceptional access for experim<strong>en</strong>talstudies of this ph<strong>en</strong>om<strong>en</strong>on. In the hard-coreboson repres<strong>en</strong>tation the balance of the kinetic and the interaction(repulsion) <strong>en</strong>ergy is determined by the degree offrustration of interdimer spin coupling, where frustrationstrongly reduces kinetic <strong>en</strong>ergy. In this latter case, insteadof being itinerant and undergo BEC, bosons can be localizeddue to mutual repulsion into a charge ordered state,that is a Wigner crystal. Since this state is gapped, the bosond<strong>en</strong>sity will be magnetic field indep<strong>en</strong>d<strong>en</strong>t and the systemwill pres<strong>en</strong>t a plateau of magnetization.Perfect frustration occurs in the geometry of orthogonaldimers in 2D, giv<strong>en</strong> by the Shastry-Sutherland Hamiltonian,and the SrCu 2 (BO 3 ) 2 compound is its first recognizedrealization. The discovery of the magnetization plateaus at1/8, 1/4 and 1/3 of the saturation magnetization in this compoundwas followed by ext<strong>en</strong>sive experim<strong>en</strong>tal and theoreticalinvestigation. In particular, NMR study performed atLNCMI proved that the 1/8 plateau, as predicted, indeedcorresponds to a comm<strong>en</strong>surate spin superstructure. Subsequ<strong>en</strong>tstudies showed that a superstructure persists at highermagnetic field [Takigawa et al., Phys. Rev. Lett. 101,037202 (2008)], and that there are other, yet undiscoveredplateaus. One of these, adjac<strong>en</strong>t to the 1/8 plateau on thehigh field side, was indeed confirmed by the torque measurem<strong>en</strong>ts[Levy et al., EPL 81, 67004 (2008)]. At the sametime appeared several contradictory predictions for the exist<strong>en</strong>ceof many other magnetization plateaus in this system,calling for experim<strong>en</strong>tal verification. However, theoretical<strong>des</strong>cription of SrCu 2 (BO 3 ) 2 is very difficult, because the interdimerinteraction is too strong to be properly <strong>des</strong>cribedby a perturbation theory, while exact numerical methods arelimited to only very small 2D systems.We have therefore continued our NMR investigation to observeevolution of the spin superstructure through magneticfield dep<strong>en</strong>d<strong>en</strong>ce of 11 B NMR spectra in the 27-34 T range,at 0.43 K. From the observed spectra we clearly id<strong>en</strong>tifyplateau phases where the NMR spectra, and thus the spinsuperstructure, is magnetic field indep<strong>en</strong>d<strong>en</strong>t. In additionto the long known 1/8 and 1/4 plateau and the rec<strong>en</strong>tly discoveredplateau adjac<strong>en</strong>t to the 1/8 plateau, a new plateauwas discovered half way up towards the 1/4 plateau (seefigure 111). Betwe<strong>en</strong> these plateaus NMR spectra evolvecontinuously with magnetic field, and no other plateau wasdetected. The same sequ<strong>en</strong>ce of plateaus was confirmedby the new, “differ<strong>en</strong>tial” torque measurem<strong>en</strong>ts, performedat ∼0.1 K. This method determines the magnetization withconsiderably <strong>en</strong>hanced precision, allowing us to find thatthe magnetization of the first three plateaus scales as 1/8: 2/15 : 1/6, which confirms some of the theoreticallyproposed values and exclu<strong>des</strong> others. Detailed analysis ofthe 11 B NMR spectra allows us to make complete determinationof the spin-polarization superstructures. We findthat previously id<strong>en</strong>tified “ext<strong>en</strong>ded triplets” are always arrangedin stripe structures, specific to each plateau, oft<strong>en</strong>differ<strong>en</strong>t from what is proposed theoretically [Takigawa etal., unpublished].Figure 111: The distribution of the internal field at the 11 B sites,obtained by deconvoluting the NMR spectra from the quadrupolesplitting. Pres<strong>en</strong>ted spectra are repres<strong>en</strong>tative of 4 magnetizationplateaus, attributed to fractions 1/8, 2/15, 1/6 and 1/4 of saturationmagnetization.M. Horvatić, C. Berthier, S. Krämer, I. SheikinM. Takigawa, T. Waki, Y. Ueda (ISSP, University of Tokyo, Japan), H. Kageyama (Kyoto University, Japan), F. Mila(EPFL, Lausanne, Switzerland)83

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