We present studies of the ultrafast dynamics of photoexcited carriers in th
in-film nanocrystalline silicon materials in which the degree of crystallin
ity has been systematically varied by controlling the deposition conditions
. Femtosecond pump-probe measurements reveal a multicomponent response that
can be understood in terms of the separate phases of the heterogeneous mat
erial. We observe a 240-fs exponential relaxation process associated with i
ntraband carrier relaxation in the silicon crystallites a response characte
ristic of bimolecular recombination in the amorphous silicon matrix, and a
long-lived component assigned to grain-boundary states.