We report the observation of magnetic superstructure in a magnetization plateau state of SrCu2(BO3)(2), a frustrated quasi two-dimensional quantum spin system. The Cu and B nuclear magnetic resonance (NMR) spectra at 35 millikelvin indicate an apparently discontinuous phase transition from uniform magnetization to a modulated superstructure near 27 tesla, above which a magnetization plateau at 1/8 of the full saturation has been observed. Comparison of the Cu NMR spectrum and the theoretical analysis of a Heisenberg spin model demonstrates the crystallization of itinerant triplets in the plateau phase within a large rhomboid unit cell (16 spins per layer) showing oscillations of the spin polarization. Thus, we are now in possession of an interesting model system to study a localization transition of strongly interacting quantum particles.
