ESR study on the excited state energy spectrum of SrCu₂(BO ₃)₂ - A central role of multiple-triplet bound states

The excited state energy spectrum of a two-dimensional dimer system SrCu₂(BO₃)₂ has been investigated by high field ESR. Besides two non-degenerated one-triplet excitations, various types of multiple-triplet bound states are identified: singlet, triplet, and quintet. The intensity of these bound states is extremely strong because one-triplet process is strongly suppressed in the orthogonal dimer system. The bound singlet state is found slightly below the energy gap of the one-triplet state, indicating the proximity to a quantum critical point. A band of the two-triplet bound state splits due to distant neighbor interactions. The bound quintet state is the direct evidence of two-triplet object made up of four S = 1/2 spins. The energy of the lowest quintet becomes lower than that of the one-triplet excitation before the closing of the lowest spin gap, namely, the quintet touches first to the ground singlet state. The present investigation exhibits an essential role of multiple-triplet bound states in the magnetic excitation spectrum.