Picosecond nonlinear absorption dynamics of neutral metal-dithiolenes belonging to the general class @M~R,R8timdt!2# ~M5Ni, Pd, Pt; R,R8 timdt5monoreduced form of disubstituted imidazolidine-2,4,5-trithione! has been investigated at l51064 nm using the pump–probe technique. Both central metal ion M and substituents R,R8 have been found to strongly influence the temporal evolution of the absorption saturation. In particular, it has been observed that the intersystem crossing rate always increases by a factor ;1.5 when changing the central metal from Pd to Pt. The mechanisms leading to the measured dynamics have been explained using a multilevel rate equation analysis, based on the results of relativistic time-dependent density functional calculations.
Picosecond absorption saturation dynamics in neutral [M(R,R’timdt)2] metal-dithiolenes
ARAGONI, MARIA CARLA;ARCA, MASSIMILIANO;ISAIA, FRANCESCO;LIPPOLIS, VITO;
2003-01-01
Abstract
Picosecond nonlinear absorption dynamics of neutral metal-dithiolenes belonging to the general class @M~R,R8timdt!2# ~M5Ni, Pd, Pt; R,R8 timdt5monoreduced form of disubstituted imidazolidine-2,4,5-trithione! has been investigated at l51064 nm using the pump–probe technique. Both central metal ion M and substituents R,R8 have been found to strongly influence the temporal evolution of the absorption saturation. In particular, it has been observed that the intersystem crossing rate always increases by a factor ;1.5 when changing the central metal from Pd to Pt. The mechanisms leading to the measured dynamics have been explained using a multilevel rate equation analysis, based on the results of relativistic time-dependent density functional calculations.
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