(320d) First Principles Modeling of Surface Plasmon Dynamics and Mechanism for Photo-Catalytic Rate Enhancement

We have recently reported that optically excited plasmonic nano-particles can activate photo-chemical transformations.[1,2] These reactions exhibit a number of unique characteristics fundamentally different than other photo-catalysts and catalytic reactions.  In this contribution we have used quantum chemical approaches to model the plasmon-driven photo-chemical reactions on metals.[3–6] I will discuss the time-dependent evolution of the electronic structure of optically excited plasmonic metals. Furthermore, I will show how this electronic structure interacts with adsorbates, ultimately driving chemical transformations of the adsorbates. A number of conflicting mechanisms will be discussed and analyzed in the context of previously reported experimental results. 

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