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We report results of 51V NMR experiments on a high-quality powder sample ofvolborthite Cu3V2O7(OH)2/2H2O, a spin-1/2 Heisenberg antiferromagnet on adistorted kagome lattice. Following the previous experiments in magnetic fields$B$ below 12 T, the NMR measurements have been extended to higher fields up to31 T. In addition to the two already known ordered phases (phases I and II), wefound a new high-field phase (phase III) above 25 T, at which a secondmagnetization step has been observed. The transition from the paramagneticphase to the antiferromagnetic phase III occurs at 26 K, which is much higherthan the transition temperatures from the paramagnetic to the lower fieldphases I (B < 4.5 T) and II (4.5 < B < 25 T). At low temperatures, two types ofthe V sites are observed with different relaxation rates and line shapes inphase III as well as in phase II. Our results indicate that both phases II andIII exhibit a heterogeneous spin state consisting of two spatially alternatingCu spin systems, one of which exhibits anomalous spin fluctuations contrastingwith the other showing a conventional static order. The magnetization of thelatter system exhibits a sudden increase upon entering into phase III,resulting in the second magnetization step at 26 T.We discuss the possible spinstructure in phase III.

High-field Phase Diagram and Spin Structure of Volborthite Cu3V2O7(OH)2/2H2O