Polariton-assisted excitation energy channeling in organic heterojunctions

Abstract

Exciton-polaritons are hybrid light-matter states resulting from strong exciton-photon coupling. The wave function of the polariton is a mixture of light and matter, enabling long-range energy transfer between spatially separated chromophores. Moreover, their delocalized nature, inherited from the photon component, has been predicted to enhance exciton transport. Here, we strongly couple an organic heterojunction consisting of energy/electron donor and acceptor materials to the same cavity mode. Using time-resolved spectroscopy and optoelectrical characterization, we show that the rate of exciton harvesting is enhanced with one order of magnitude and the rate of energy transfer in the system is increased two- to threefold in the strong coupling regime. Our results exemplify two means of efficiently channeling excitation energy to a heterojunction interface, where charge separation can occur. This study opens a new door to increase the overall efficiency of light harvesting systems using the tool of strong light-matter interactions.

Selective isomer emission via funneling of exciton polaritons

“…The delocalized LP thus effectively acts as a funnel that can exploit the strong absorption of the dominant P-trans isomer but transfers a significant fraction of the excitations to localized molecular excitations in the TICS and consequently makes emission from the TICS the dominant radiative emission channel. As a difference from previous demonstrations of cavity-enhanced energy transfer processes in which the excitation is always carried out by the polaritonic states of the strongly-coupled system (12)(13)(14)(16)(17)(18)(19), here, the mechanism uses the manifold of molecular dark states as the final emissive mode. The delocalized polaritonic state is only used to store first the excitation energy that is then transferred to the dark states.…”

“…During the past 10 years, substantial experimental and theoretical progress has been made to demonstrate the potential use of strong light-matter coupling for both modifying molecular energy landscapes (4)(5)(6)(7)(8)(9)(10)(11) and enhancing energy transfer in donor-acceptor molecular systems (12)(13)(14)(15)(16)(17)(18)(19), among other capabilities (20). In general, strong coupling emerges when a collection of quantum emitters is placed within an optical cavity and the coherent energy exchange between the excitons in the emitters and photons inside the cavity is faster than the loss mechanisms in the combined system (21).…”

Efficient method to simulate non-perturbative dynamics of an open quantum system using a quantum computer

“…for general light-harvesting complexes. Additional applications are Hamiltonian dynamics simulations of general quantum biological systems [40,52] and condensed matter systems [53][54][55] where perturbative approaches fail to provide answers. In the future, it would be interesting to implement optimizations to reduce the harmonic oscillator chain length in the same spirit as the ones reported in reference [56] and to find applications of the Q-TEDOPA to more general quantum computing problems besides quantum simulation.…”

Exciton‐Polaritons and Their Bose–Einstein Condensates in Organic Semiconductor Microcavities

“…In 1D waveguide structures, strong light–matter coupling typically leads to a significantly large refractive index, [ 23 ] and enables polaritons to propagate and be manipulated via excitonic part below the diffraction limit of light; [ 24 ] thus they have drawn much interest, as they are attractive candidates for miniaturized photonic circuits. Meanwhile, in 2D planar cavities, fruitful organic electronically excited‐state processes can be dramatically modified due to the formation of cavity polaritons, [ 6–9 ] allowing observation of extraordinary photochemistry and photophysics of organic molecules, such as altered chemical reactions, [ 10,11,25–27 ] long‐range energy transfer, [ 28–34 ] modulated single/triplet dynamics, [ 35–45 ] and enhanced nonlinear optical effects. [ 46–49 ]…”