Real-Time Quantum Dynamics of Long-Range Electronic Excitation Transfer in Plasmonic Nanoantennas

Abstract

Using large-scale, real-time quantum dynamics calculations, we present a detailed analysis of electronic excitation transfer (EET) mechanisms in a multi-particle plasmonic nanoantenna system. Specifically, we utilize real-time, time-dependent, density functional tight binding (RT-TDDFTB) to provide a quantum-mechanical description (at an electronic/atomistic level of detail) for characterizing and analyzing these systems, without recourse to classical approximations. We also demonstrate highly long-range electronic couplings in these complex systems and find that the range of these couplings is more than twice the conventional cutoff limit considered by FRET based approaches. Furthermore, we attribute these unusually long-ranged electronic couplings to the coherent oscillations of conduction electrons in plasmonic nanoparticles. This long-range nature of plasmonic interactions has important ramifications for EET - in particular, we show that the commonly used "nearest-neighbor" FRET model is inadequate for accurately characterizing EET even in simple plasmonic antenna systems. These findings provide a real-time, quantum-mechanical perspective for understanding EET mechanisms and provide guidance in enhancing plasmonic properties in artificial light-harvesting systems.

arXiv commentAccepted by the Journal of Chemical Theory and Computation

References in corpus (4)

• Time-Dependent Density Functional Theory for Open Quantum Systems with Unitary Propagation
• Plasmonic excitations in quantum-sized sodium nanoparticles studied by time-dependent density functional calculations
• Buffering plasmons in nanoparticle waveguides at the virtual-localized transition
• Full quantum dynamics of the electronic coupling between photosynthetic pigments

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