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Optical spectroscopy has been the primary tool to study the electronicstructure of molecules. However the strict spin selection rule has severelylimited its ability to access states of different spin multiplicities. Here wepropose a new strategy to activate spin-forbidden transitions in molecules byintroducing spatially highly inhomogeneous plasmonic field. The giantenhancement of the magnetic field strength resulted from the curl of theinhomogeneous vector potential makes the transition between states of differentspin multiplicities naturally feasible. The dramatic effect of theinhomogeneity of the plasmonic field on the spin and symmetry selection rulesis well illustrated by first principles calculations of C60. Remarkably, theintensity of singlet-triplet transitions can even be stronger than that ofsinglet-singlet transitions when the plasmon spatial distribution is comparablewith the molecular size. This approach offers a powerful means to completelymap out all excited states of molecules and to actively control theirphotochemical processes. The same concept can also be applied to study nano andbiological systems.

Activating spin-forbidden transitions in molecules by the highly localized plasmonic field