Photoinduced charge separation in the carbon nano-onion C60@C240
dc.contributor.author
dc.date.accessioned
2016-09-08T10:01:05Z
dc.date.available
2017-07-06T03:00:05Z
dc.date.issued
2016-07-06
dc.identifier.issn
1089-5639
dc.identifier.uri
dc.description.abstract
The double-shell fullerene C60@C240 formed by inclusion of C60 into C240 is the smallest stable carbon nano-onion. In the paper, we analyze in detail the character of excited states of C60@C240 in terms of exciton localization and charge transfer between the inner and outer shells. The unique structure of the buckyonion leads to a large electrostatic stabilization of charge-separated (CS) states in the C60@C240. As a result, the CS states C60+@C240 lie in the same region of the electronic spectrum (2.4-2.6 eV) as strongly absorbing locally excited states, and therefore, can be effectively populated. The CS states C60 @C240+ are found to be by 0.5 eV higher in energy than the states C60+@C240 . Unlike the situation observed in donor-acceptor systems, the energy of the CS states in C60@C240 does not practically depend on the environment polarity. This leads to exceptionally small reorganization energies for electron transfer between the shells. Electronic couplings for photoinduced charge separation and charge recombination processes are calculated. The absolute rate of the formation of the CS states C60+@C240 is estimated at ~ 4 ps-1. The electronic features found in C60@C240 are likely to be shared by other carbon nano-onions
dc.description.sponsorship
We are grateful for financial support from the Spanish Ministerio de Economía y Competitividad (MINECO) (Projects CTQ2014-54306-P and CTQ2015-69363-P), the Catalan DIUE (Project 2014SGR931, ICREA Academia 2014 Award to MS, and Xarxa de Referència en Química Teòrica i Computacional), and the FEDER fund (UNGI10-4E-801)
dc.format.extent
7 p.
dc.format.mimetype
application/pdf
dc.language.iso
eng
dc.publisher
American Chemical Society (ACS)
dc.relation
info:eu-repo/grantAgreement/MINECO//CTQ2014-54306-P/ES/ESTUDIOS TEORICO-EXPERIMENTALES DE CICLACIONES CATALIZADAS POR METALES DE TRANSICION. NUEVOS DESARROLLOS EN AROMATICIDAD, FUNCIONALES DE LA DENSIDAD Y QUIMICA SUPRAMOLECULAR/
info:eu-repo/grantAgreement/MINECO//CTQ2015-69363-P/ES/OMPUTACION DEL ESTADO EXCITADO: DE ESPECTROS MOLECULARES A SISTEMAS MULTICROMOFORICOS/
AGAUR/2014-2016/2014 SGR-931
dc.relation.isformatof
Versió postprint del document publicat a: http://dx.doi.org/10.1021/acs.jpca.6b04127
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© Journal of Physical Chemistry A, 2016, vol. 120, núm. 29, p. 5798-5804
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Articles publicats (D-Q)
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Tots els drets reservats
dc.source
Voityuk, Alexander A. Solà i Puig, Miquel 2016 Photoinduced charge separation in the carbon nano-onion C60@C240 Journal of Physical Chemistry A 120 29 5798 5804
dc.subject
dc.title
Photoinduced charge separation in the carbon nano-onion C60@C240
dc.type
info:eu-repo/semantics/article
dc.rights.accessRights
info:eu-repo/semantics/openAccess
dc.type.version
info:eu-repo/semantics/acceptedVersion
dc.identifier.doi
dc.identifier.idgrec
025505
dc.contributor.funder
dc.relation.ProjectAcronym
dc.identifier.eissn
1520-5215