The origin and potential implications of a molecular phase in coherent
two-pathway excitation are analyzed by means of a time-independent, q
uantum mechanical theory. A unified model is developed describing unim
olecular decay into several continua of general nature, where each bre
akup reaction takes place both directly and via a manifold of resonanc
es. It is found that the molecular phase, observable in two pathway ex
citation experiments, correlates with the single-pathway fragmentation
line shape, in agreement with recent measurements. We propose the mea
surement of molecular phases as a route to molecular properties which
are silent in conventional observables. (C) 1998 American Institute of
Physics.