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Triplet space(dark state) can play an important role in photochemistry.Recently we developed a newtechnique termed femtosecond time-reversed pump-probe(fs-TRPP for short) that enables real-time mappingof the ultrafast dynamics of triplets in molecular system,as experimentally verified in a proof-of-conceptsystem of malachite green molecule.We found that the involvement of long-lived triplet states can control theultrafast electron dynamics in the endohedral metallofullerenes(EMF) under visible—light excitation and theopening of the singlet-to-triplet pathways highly correlates to the EMF cage symmetry and also to the electroncharacter of the substituent groups(electron donor or acceptor) that are externally encrafted onto the fullerenecage.The ultrafast electron dynamics in photoelectric conversion processes of nanomaterial systems has alsobeen explored by means of fs pump-probe spectroscopy in conjunction with theoretical simulations.