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Charge transfer (CT) is a fundamental and ubiquitous mechanism in biology,physics and chemistry. Here, we evidence that CT dynamics can be altered bymulti-layered hyperbolic metamaterial (HMM) substrates. Takingtriphenylene:perylene diimide dyad supramolecular self-assemblies as a modelsystem, we reveal longer-lived CT states in presence of HMM structures withboth charge separation and recombination characteristic times increased byfactors of 2.4 and 1.7, i.e. relative variations of 140 and 73 %, respectively.To rationalise these experimental results in terms of driving force, wesuccessfully introduce image dipole interactions in Marcus theory. Thenon-local effect herein demonstrated is directly linked to the number ofmetal-dielectric pairs, can be formalised in the dielectric permittivity, andis presented as a solid analogue to local solvent polarizability effects. Thismodel and extra PH3T:PC60BM results show the generality of this non-localphenomenon and that a wide range of kinetic tailoring opportunities can arisefrom substrate engineering. This work paves the way toward the design ofartificial substrates to control CT dynamics of interest for applications inoptoelectronics and chemistry.

Charge-Transfer Dynamics and Nonlocal Dielectric Permittivities Tuned with Metamaterial Structures as Solvent Analogues