Thermally populated versus field-induced triplon bound states in the Shastry-Sutherland lattice SrCu2(BO3)2

The Shastry–Sutherland compound SrCu2(BO3)2 constituting orthogonally coupled dimers harbors an S = 0 singlet ground state. The confluence of strong interdimer interaction and frustration engenders a spectrum of low-energy excitations including localized triplons as well as singlet and triplet bound states. Their dynamics are controlled by an external magnetic field and temperature. Here, we employ high-field Raman spectroscopy to map the field and temperature evolution of such bosonic composite quasiparticles on approaching the 1/8 magnetization plateau. Our study unveils that the magnetic field and thermal fluctuations show remarkably similar effects in melting the singlet bound states, but are disparate in their effects on the fine spectral shapes. This, together with the anti-crossing of two singlet bound states in the intermediate field B = 10 − 16 T, is discussed in terms of the correlated dynamics of frustrated, interacting bosons.