Pump-probe photoelectron spectroscopy is used to study excited states in pr
istine and photopolymerized C-60. For the first time in a molecular solid,
vibrationally broadened singlet (SI) and triplet (TI) exciton photoemission
spectra are temporally isolated and unambiguously assigned. Complex transi
ent behaviors of S, and T, populations, including non-Markovian decays and
a strongly enhanced production of T, states at high excitation, provide evi
dence for interactions among excitons and free carriers. A new rate-equatio
n model reproduces a wide range of both laser- and synchrotron-based data f
rom polymerized films. (C) 2001 Published by Elsevier Science B.V.