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Charge-transfer dynamics and nonlocal dielectric permittivity tuned with metamaterial structures as solvent analogues

Title
Charge-transfer dynamics and nonlocal dielectric permittivity tuned with metamaterial structures as solvent analogues
Authors
Lee K.J.Xiao Y.Woo J.H.Kim E.Kreher D.Attias A.-J.Mathevet F.Ribierre J.-C.Wu J.W.André P.
Ewha Authors
우정원
SCOPUS Author ID
우정원scopus
Issue Date
2017
Journal Title
Nature Materials
ISSN
1476-1122JCR Link
Citation
vol. 16, no. 7, pp. 722 - 729
Publisher
Nature Publishing Group
Indexed
SCI; SCIE; SCOPUS WOS scopus
Abstract
Charge transfer (CT) is a fundamental and ubiquitous mechanism in biology, physics and chemistry. Here, we evidence that CT dynamics can be altered by multi-layered hyperbolic metamaterial (HMM) substrates. Taking triphenylene:perylene diimide dyad supramolecular self-assemblies as a model system, we reveal longer-lived CT states in the presence of HMM structures, with both charge separation and recombination characteristic times increased by factors of 2.4 and 1.7 - that is, relative variations of 140 and 73%, respectively. To rationalize these experimental results in terms of driving force, we successfully introduce image dipole interactions in Marcus theory. The non-local effect herein demonstrated is directly linked to the number of metal-dielectric pairs, can be formalized in the dielectric permittivity, and is presented as a solid analogue to local solvent polarity effects. This model and extra PH3T:PC60BM results show the generality of this non-local phenomenon and that a wide range of kinetic tailoring opportunities can arise from substrate engineering. This work paves the way toward the design of artificial substrates to control CT dynamics of interest for applications in optoelectronics and chemistry. © 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.
DOI
10.1038/nmat4907
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자연과학대학 > 물리학전공 > Journal papers
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