Magnetoelastic coupling and spin excitations in the spin-gap system (VO)₂P₂O₇: A Raman scattering study

Single crystals of the spin-gap system $\rm (VO)_2P_2O_7$ have been investigated by means of Raman scattering. At temperatures below T=75 K~$\approx 2\Delta_{01}({\bf k}=0)$, with $\Delta_{01}$ the singlet-triplet gap, a shoulder appears at 47 cm$^{-1}$. An analysis of the polarization selection rules and the temperature dependence of the scattering intensity leads to its identification as a singlet bound state with very small binding energy. Therefore in contrast to recent theoretical models the importance of frustration for this compound must be rejected. The observation of a strong anharmonicity of three phonons with energies close to $\Delta_{01}$ at the zone boundary and additional quasielastic light scattering, however, both point to a strong spin-phonon coupling in this system. We propose this coupling to be the origin of the second bound triplet state observed in recent neutron scattering experiments.