Femtosecond time-resolved photoelectron imaging (TR-PEI) is applied to the (1 + 2') resonance-enhanced multiphoton ionization of pyrazine (1,4-diazabenzene) via the S-1 state. The intersystem crossing (ISC) from the S-1 (npi*) to the T-1 (npi*) state and the ionization dynamics from 3s and 3p(z) Rydberg states are investigated. Rotational revival features, observed in the time-resolved photoelectron intensities from the T-1 state populated by ISC as well as from the optically prepared S-1 state, are analyzed in detail. The alignment at the rotational revival time in the T-1 state is found to be much smaller than that in the S-1 state. Numerical calculations, using the molecular eigenstate basis and taking account of the angular momentum coupling, to model the transfer of coherence between the S-1 and T-1 states are presented. The calculated time dependence of signal strength and the axis alignment are found to be in excellent agreement with the observed profiles. The diminished alignment in T-1 is explained by the angular momentum coupling mechanism in ISC. Comparison is also made with the rotational coherence transfer in intramolecular vibrational redistribution (IVR). Photoelectron angular distributions (PADS) were also measured in the laboratory frame from spatially aligned ensembles in the 3s and 3p(z) Rydberg states. The results are qualitatively explained on the basis of the selection rules upon photoionization.