Two-dimensional (2D) multiple-quantum coherence is reported for the hy
perfine ground state of rubidium and cesium atoms by applying multiple
radio-frequency pulses to the optically polarized atoms. Calculations
of 1D and 2D multiple quantum coherences were performed with a genera
l theory for an arbitrary high spin system by using irreducible tensor
operators. The experimental results compare very well with the calcul
ations.