Quantum Materials Corp. (fka QTMM)

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Theory of polariton long-range excitation energy transfer

Matthew Du, Luis A. Martínez-Martínez, Raphael F. Ribeiro, Zixuan Hu, Vinod M. Menon, Joel Yuen-Zhou
(Submitted on 30 Nov 2017)

Strong-coupling between light and matter produces hybridized states (polaritons) whose delocalization and electromagnetic character allow for novel modifications in spectroscopy and chemical reactivity of molecular systems. Recent experiments have demonstrated remarkable distance-independent long-range energy transfer between molecules strongly coupled to optical microcavity modes. To shed light on the mechanism of this phenomenon, we present the first comprehensive theory of polariton energy transfer based on strong-coupling of donor and/or acceptor chromophores to surface plasmons. Application of our theory demonstrates that long-range energy transfer up to a micron is indeed possible via strong-coupling. In particular, we report two regimes for polariton energy transfer: in one case, strong-coupling to a single type of chromophore leads to transfer mediated largely by plasmons while in the other case, strong-coupling to both types of chromophores creates energy transfer pathways mediated by vibrational relaxation. Importantly, we highlight conditions under which coherence enhances or deteriorates these processes. For instance, while strong-coupling to donors only can enhance transfer to acceptors, the reverse turns out not to be true. However, strong-coupling to acceptors can shift energy levels in a way that transfer to donors can occur, thus yielding a chromophore role-reversal or "carnival effect." This theoretical study demonstrates the potential for polaritons to control and mediate long-range energy transfer, thus opening doors to the design of remote mesoscale interactions between molecular systems.

https://arxiv.org/abs/1711.11576