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We propose a strategy for enabling photodissociation of a normallyphotostable molecule through coupling to a nanoparticle plasmon. The largepossible coupling on the single-molecule level combined with the highly lossynature of plasmonic modes, with lifetimes on the order of femtoseconds, opensan ultrafast decay channel for the molecule. For plasmon mode frequencies belowthe vertical photoexcitation energy of the molecule, the difference betweenexcitation and emission energy is converted into vibrational energy on themolecular ground state in a Raman-like process. Under the correct conditions,this energy can be high enough to enable efficient photodissociation on theelectronic ground state. We demonstrate the concept using numerical simulationsof the Lindblad master equation for the hydrogen molecule in the vicinity of analuminum nanoparticle, and explore the photodissociation efficiency as afunction of various system parameters.

Molecular photodissociation enabled by ultrafast plasmon decay