Magnetic materials having competing, i.e., frustrated, interactions can display magnetism prolific in intricate structures, discrete jumps, plateaus, and exotic spin states with increasing applied magnetic fields. When the associated elastic energy cost is not too expensive, this high potential can be enhanced by the existence of an omnipresent magnetoelastic coupling. Here we report experimental and theoretical evidence of a nonnegligible magnetoelastic coupling in one of these fascinating materials, SrCu2(BO3)2 (SCBO). First, using pulsed-field transversal and longitudinal magnetostriction measurements we show that its physical dimensions, indeed, mimic closely its unusually rich field-induced magnetism. Second, using density functional-based calculations we find that the driving force behind the magnetoelastic coupling is the CuOCu superexchange angle that, due to the orthogonal Cu(2+) dimers acting as pantographs, can shrink significantly (0.44%) with minute (0.01%) variations in the lattice parameters. With this original approach we also find a reduction of ∼ 10% in the intradimer exchange integral J, enough to make predictions for the highly magnetized states and the effects of applied pressure on SCBO.
Keywords: Shastry–Sutherland; density functional theory; high magnetic fields; magnetostriction; spin-lattice coupling.