Reorganization Energy upon Controlled Intermolecular Charge-Transfer Reactions in Monolithically Integrated Nanodevices

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dc.contributor.authorMerces L.
dc.contributor.authorCandiotto G.
dc.contributor.authorFerro L.M.M.
dc.contributor.authorde Barros A.
dc.contributor.authorBatista C.V.S.
dc.contributor.authorNawaz A.
dc.contributor.authorRiul A.
dc.contributor.authorCapaz R.B.
dc.contributor.authorBufon C.C.B.
dc.date.accessioned2024-03-12T19:18:43Z
dc.date.available2024-03-12T19:18:43Z
dc.date.issued2021
dc.description.abstract© 2021 Wiley-VCH GmbHIntermolecular electron-transfer reactions are key processes in physics, chemistry, and biology. The electron-transfer rates depend primarily on the system reorganization energy, that is, the energetic cost to rearrange each reactant and its surrounding environment when a charge is transferred. Despite the evident impact of electron-transfer reactions on charge-carrier hopping, well-controlled electronic transport measurements using monolithically integrated electrochemical devices have not successfully measured the reorganization energies to this date. Here, it is shown that self-rolling nanomembrane devices with strain-engineered mechanical properties, on-a-chip monolithic integration, and multi-environment operation features can overcome this challenge. The ongoing advances in nanomembrane-origami technology allow to manufacture the nCap, a nanocapacitor platform, to perform molecular-level charge transport characterization. Thereby, employing nCap, the copper-phthalocyanine (CuPc) reorganization energy is probed, ≈0.93 eV, from temperature-dependent measurements of CuPc nanometer-thick films. Supporting the experimental findings, density functional theory calculations provide the atomistic picture of the measured CuPc charge-transfer reaction. The experimental strategy demonstrated here is a consistent route towards determining the reorganization energy of a system formed by molecules monolithically integrated into electrochemical nanodevices.
dc.description.issuenumber45
dc.description.volume17
dc.identifier.doi10.1002/smll.202103897
dc.identifier.issn1613-6829
dc.identifier.urihttps://dspace.mackenzie.br/handle/10899/34565
dc.relation.ispartofSmall
dc.rightsAcesso Restrito
dc.subject.otherlanguagedensity functional
dc.subject.otherlanguageelectrochemical
dc.subject.otherlanguageelectron transfer
dc.subject.otherlanguagehopping
dc.subject.otherlanguageMarcus
dc.subject.otherlanguagenanogap
dc.subject.otherlanguagenanomembrane origami
dc.titleReorganization Energy upon Controlled Intermolecular Charge-Transfer Reactions in Monolithically Integrated Nanodevices
dc.typeArtigo
local.scopus.citations19
local.scopus.eid2-s2.0-85116125138
local.scopus.subjectDensity functionals
local.scopus.subjectElectrochemicals
local.scopus.subjectElectron transfer
local.scopus.subjectHopping
local.scopus.subjectMarcu
local.scopus.subjectMonolithically integrated
local.scopus.subjectNanogaps
local.scopus.subjectNanomembrane origami
local.scopus.subjectNanomembranes
local.scopus.subjectReorganization energies
local.scopus.subjectElectrons
local.scopus.updated2024-10-01
local.scopus.urlhttps://www.scopus.com/inward/record.uri?partnerID=HzOxMe3b&scp=85116125138&origin=inward
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