Abstract
The pulse-width-dependent self-focusing–defocusing transformation of the planar heterothiometallic cluster compound [Et4 N]2 [MoS4 Cu4 (SCN)4 (2-pic)4 ] in DMF solution is observed at a wavelength of 532 nm. We also investigate the nonlinear refraction and absorption behaviours of the cluster compound based on excited state theory. For picosecond pulses the compound possesses a self-focusing property, which is attributed to population transitions between singlet excited states, while for nanosecond pulses it exhibits a self-defocusing property, which is attributed to the population relaxing to triplet states. In addition, we found that the singlet excited state absorption is stronger than triplet excited state absorption.
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