A transient grating of singlet electronic excited states is produced in a pentacene-doped p-terphenyl molecular crystal by optical absorption from two crossed time-coincident picosecond excitation pulses at 532 nm. The diffraction properties of this volume grating are probed by a weak, variably delayed, Bragg-matched picosecond probe pulse, At high excitation intensities, a strong oscillatory behavior in the time-dependent scattering efficiency is observed superimposed on the exponential decay pattern of the excited-state grating. We attribute the oscillatory behavior to a thermal grating which induces coherent microwave acoustic phonons, These in turn modulate, at the sound frequency, the optical absorption properties of the pentacene molecules in the excited state. An acoustically induced amplitude grating effect is thus obtained, in contrast to conventional acousto-optic phase grating effects. © 1979 IEEE