a) Γ K M (b) FIG. 1. (Color online) (a) Honeycomb lattice with the different spin exchange interactions considered in this paper; (b) corresponding Brillouin zone with relevant k points. 2 2.5 Velocity [arb. units] J 3 =0 J 3 =0.3

NMR and magnetization measurements in Li2VOSiO4 and Li2VOGeO4 are reported. The analysis of the susceptibility shows that both compounds are two-dimensional S = 1/2 Heisenberg antiferromagnets on a square lattice with a sizable frustration induced by the competition between the superexchange couplings J1 along the sides of the square and J2 along the diagonal. Li2VOSiO4 undergoes a low-temperature phase transition to a collinear order, as theoretically predicted for J2/J1>0.5. Just above the magnetic transition the degeneracy between the two collinear ground states is lifted by the onset of a structural distortion.

11 pages, 17 figuresInternational audienceUsing both exact diagonalizations and diagonalizations in a subset of short-range valence bond singlets, we address the nature of the groundstate of the Heisenberg spin-1/2 antiferromagnet on the square lattice with competing next-nearest and next-next-nearest neighbor antiferromagnetic couplings (J1-J2-J3 model). A detailed comparison of the two approaches reveals a region along the line (J2+J3)/J1=1/2, where the description in terms of nearest-neighbor singlet coverings is excellent, therefore providing evidence for a magnetically disordered region. Furthermore a careful analysis of dimer-dimer correlation functions, dimer structure factors and plaquette-plaquette correlation functions provides striking evidence for the presence of a plaquette valence bond solid order in part of the magnetically disordered region