We report single-crystal 51 V NMR studies on volborthite Cu3V2O7(OH)2·2H2O, which is regarded as a quasi-two-dimensional frustrated magnet with competing ferromagnetic and antiferromagnetic interactions. In the 1/3 magnetization plateau above 28 T, the nuclear spin-lattice relaxation rate 1/T1 indicates an excitation gap with a large effective g factor in the range of 4.6-5.9, pointing to magnon bound states. Below 26 T where the gap has closed, the NMR spectra indicate small internal fields with a Gaussian-like distribution, whereas 1/T1 shows a power-law-like temperature dependence in the paramagnetic state, which resembles a slowing down of spin fluctuations associated with magnetic order. We discuss the possibility of an exotic spin state caused by the condensation of magnon bound states below the magnetization plateau.PACS numbers: 75.30. Kz, 75.40.Gb, The possibilities of exotic states in quantum spin systems with frustrated interactions have attracted strong attention [1,2]. For example, the ground state of the spin-1/2 kagome antiferromagnet is believed to show no long-range magnetic order. Theories have proposed various ground states such as spin liquids [3][4][5] or valencebond-crystal states [6]. Other interesting states such as spin nematic states [7][8][9][10][11] and magnetization plateaus [12][13][14][15][16] are also expected in frustrated spin systems. Theories have predicted that a spin nematic state is realized near a fully polarized state of a frustrated spin system with competing ferromagnetic (FM) interactions J 1 and antiferromagnetic (AFM) interactions J 2 , [7][8][9][10][11]. In such systems, a spin nematic state is characterized by the condensation of two-magnon bound states. The search for a spin nematic phase has been performed by using high-field NMR near the fully polarized state of a quasione-dimensional J 1 -J 2 chain magnet LiCuVO 4 , although definitive results are not obtained yet [17,18].Volborthite Cu 3 V 2 O 7 (OH) 2 ·2H 2 O is a unique antiferromagnet with frustrated interactions [19], which contains layers of distorted kagome nets formed by Cu 2+ ions as shown in Fig. 1(a). Early high-field magnetization and NMR measurements in polycrystalline samples revealed three distinct magnetic phases I (B < 4.5 T), II (4.5 < B < 26 T), and III (26 T < B ) [20][21][22][23][24][25]. The magnetic properties were examined on the basis of the distorted kagome model [25][26][27][28], while the density func- * Present address: Max Plank Institute for Solid State Research, Heisenbergstrasse 1, 70569 Stuttgart, Germany tional theory (DFT) study of the C2/m structure proposed that frustration should be attributed to the competition between a FM J 1 and an AFM J 2 between second neighbors along the b axis [ Fig. 1(b)] [29]. Recently, single crystals were prepared and they have provided a further opportunity to study the unique magnetism of volborthite [30,31]. In the single crystals, the high-field NMR and magnetization measurements revealed two features remarkably different from those previou...