Direct Observation of the Quantum Phase Transition of SrCu2(BO3)2 by High-Pressure and Terahertz Electron Spin Resonance

Abstract

High-pressure and high-field electron spin resonance (ESR) measurements have been performed on a single crystal of the orthogonal-dimer spin system SrCu$_{2}$(BO$_{3}$)$_{2}$. With frequencies below 1 THz, ESR signals associated with transitions from the singlet ground state to the one-triplet excited states and the two-triplet bound state were observed at pressures up to 2.1 GPa. We obtained directly the pressure dependence of the gap energies, finding a clear first-order phase transition at $P_{c}=1.85\pm0.05$ GPa. By comparing this pressure dependence with the calculated excitation energies obtained from an exact diagonalization, we determined the precise pressure dependence for inter- ($J'$) and intra-dimer ($J$) exchange interactions considering the Dzyaloshinski-Moriya interaction. Thus this system undergoes a first-order quantum phase transition from the dimer singlet phase to a plaquette singlet phase above the ratio $(J'/J)_{c}=0.660\pm0.003$.