Energy Transfer between Spatially Separated Entangled Molecules

Abstract

Light–matter strong coupling allows for the possibility of entangling the wave functions of different molecules through the light field. We hereby present direct evidence of non‐radiative energy transfer well beyond the Förster limit for spatially separated donor and acceptor cyanine dyes strongly coupled to a cavity. The transient dynamics and the static spectra show an energy transfer efficiency approaching 37 % for donor–acceptor distances ≥100 nm. In such systems, the energy transfer process becomes independent of distance as long as the coupling strength is maintained. This is consistent with the entangled and delocalized nature of the polaritonic states.

Strong Light–Matter Coupling as a New Tool for Molecular and Material Engineering: Quantum Approach

“…The vibration lifetimes are also strongly modified in this pump–probe infrared absorption study of the CO group stretching vibration, with additional evidence of coherent energy transfers between the two polaritons provided by the prediction of quantum beats. The observation of energy transfers between donor–acceptor molecules separated by more than 100 nm, much further apart than normal transfer distances, evidences the delocalized and coherent nature of polaritons . Polaritons can thus entangle cyanine dyes at a distance.…”

“…The observation of energy transfers between donor-acceptor molecules separated by more than 100 nm, much further apart than normal transfer distances, evidences the delocalized and coherent nature of polaritons. [93] Polaritons can thus entangle cyanine dyes at a distance. Studies of the transient absorption dynamics of donor-acceptor systems also showed the modification of the non-radiative transfers in the cavity.…”

Molecular polaritons for controlling chemistry with quantum optics

“…There are several widely-used technologies that ultimately base their efficiency on the rates of chemical reactions or electron transfer processes that occur in excited electronic states (e.g., sunscreens, polymers, catalysis, solar cells, OLEDs). Therefore, the ability to manipulate the rates and branching ratios of these fundamental chemical processes in a reversible manner using light-matter interaction with a vacuum field, suggests a promising route for targeted control of excited state reactivity, without exposing fragile molecular species or materials to ESC Cavity-enhanced energy transfer and conductivity in organic media [30,[137][138][139] ESC/VSC Strong coupling with biological light-harvesting systems [44,[140][141][142] ESC Cavity-modified photoisomerization and intersystem crossing [28,104,[143][144][145] ESC Strong coupling with an individual molecule in a plasmonic nanocavity [95,96,98,146] ESC Polariton-enhanced organic light emitting devices [32,35,147,148] EUSC Ultrastrong light-matter interaction with molecular ensembles [29,36,92,147,[149][150][151] VSC/VUSC Vibrational polaritons in solid phase and liquid phase Fabry-Perot cavities [38-40, 45-47, 49-54, 152] VSC Manipulation of chemical reactivity in the ground electronic state [43,55,153] ESC Cavity-controlled intramolecular electron transfer in molecular ensembles. [134,[154][155]…”

Relevance of the Quadratic Diamagnetic and Self-Polarization Terms in Cavity Quantum Electrodynamics

“…Driven by substantial experimental progress in the field of cavity-modified chemistry [1][2][3][4][5][6][7][8][9][10][11], theoretical methods at the border between quantum-chemical ab initio methods and optics have become the focus of many recent investigations . The high complexity of a molecular system, which can undergo, e.g., chemical reactions or quantum phase-transitions, coupled strongly to photons makes the use of some sort of approximation strategy necessary.…”