Photoinduced charge shift in Li+ doped giant nested fullerenes

Over the last years, carbon nano-onions (CNOs) have been in focus in material science research. Their red-shifted absorption allows utilizing CNOs as promising photosensitizers. We report here a systematic study of excited state properties of six double-layered Li+ doped fullerenes of Ih symmetry: [...

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Authors: Stasyuk, Anton J., Stasyuk, Olga A., Solà i Puig, Miquel, Voityuk, Alexander A.
Format: article
Status:Versión aceptada para publicación
Publication Date:2019
Country:España
Institution:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repository:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:10256/16739
Online Access:http://hdl.handle.net/10256/16739
Access Level:Open access
Keyword:Ful·lerens
Fotoquímica
Fullerenes
Photochemistry
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spelling Photoinduced charge shift in Li+ doped giant nested fullerenesStasyuk, Anton J.Stasyuk, Olga A.Solà i Puig, MiquelVoityuk, Alexander A.Ful·lerensFotoquímicaFullerenesPhotochemistryOver the last years, carbon nano-onions (CNOs) have been in focus in material science research. Their red-shifted absorption allows utilizing CNOs as promising photosensitizers. We report here a systematic study of excited state properties of six double-layered Li+ doped fullerenes of Ih symmetry: [Li@C60@C240]+, [Li@C60@C540]+, [Li@C60@C960]+, [Li@C240@C540]+, [Li@C240@C960]+ and [Li@C540@C960]+. On the basis of TDDFT calculations, we show that the long-wave absorption by the Li+ doped species leads to charge transfer (CT) between the inner and the outer shells unlike their neutral double-layered precursors. The CT energy depends strongly on the size of the concentric fullerenes and it can easily be tuned by varying both the encapsulated metal ion and the size of the shells. Two types of low-lying excited states are identified (1) capacitor-like structures, as Li+@C60-@C240+, with alternating positive and negative charges, and (2) states, where the positive charge is delocalized over the outer shell, as in Li@C240@C540+. We suggest a simple expression to estimate the energy difference of these excited states and to predict the type of the lowest CT state in nested fullerenes. The effect of nature of the encapsulated ion on the charge transfer state energies is considered. The HOMO - LUMO transition energy is found to vary significantly when going from [Li@C60@C240]+ to [Li@C540@C960]+American Chemical Society (ACS)info2019info:eu-repo/semantics/articleinfo:eu-repo/semantics/acceptedVersionpeer-reviewed8 p.application/pdfhttp://hdl.handle.net/10256/16739http://hdl.handle.net/10256/16739© Journal of Physical Chemistry C, 2019, vol. 123, núm. 27, p. 16525-16532Articles publicats (D-Q)Stasyuk, Anton J. Stasyuk, Olga A. Solà i Puig, Miquel Voityuk, Alexander A. 2019 Photoinduced charge shift in Li+ doped giant nested fullerenes Journal of Physical Chemistry C 123 16525 16532reponame:Recercat. Dipósit de la Recerca de Catalunyainstname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)Inglésinfo:eu-repo/semantics/altIdentifier/doi/10.1021/acs.jpcc.9b02354info:eu-repo/semantics/altIdentifier/issn/1932-7447info:eu-repo/semantics/altIdentifier/eissn/1932-7455Tots els drets reservatsinfo:eu-repo/semantics/openAccessoai:recercat.cat:10256/167392026-05-29T05:05:01Z
dc.title.none.fl_str_mv Photoinduced charge shift in Li+ doped giant nested fullerenes
title Photoinduced charge shift in Li+ doped giant nested fullerenes
spellingShingle Photoinduced charge shift in Li+ doped giant nested fullerenes
Stasyuk, Anton J.
Ful·lerens
Fotoquímica
Fullerenes
Photochemistry
title_short Photoinduced charge shift in Li+ doped giant nested fullerenes
title_full Photoinduced charge shift in Li+ doped giant nested fullerenes
title_fullStr Photoinduced charge shift in Li+ doped giant nested fullerenes
title_full_unstemmed Photoinduced charge shift in Li+ doped giant nested fullerenes
title_sort Photoinduced charge shift in Li+ doped giant nested fullerenes
dc.creator.none.fl_str_mv Stasyuk, Anton J.
Stasyuk, Olga A.
Solà i Puig, Miquel
Voityuk, Alexander A.
author Stasyuk, Anton J.
author_facet Stasyuk, Anton J.
Stasyuk, Olga A.
Solà i Puig, Miquel
Voityuk, Alexander A.
author_role author
author2 Stasyuk, Olga A.
Solà i Puig, Miquel
Voityuk, Alexander A.
author2_role author
author
author
dc.subject.none.fl_str_mv Ful·lerens
Fotoquímica
Fullerenes
Photochemistry
topic Ful·lerens
Fotoquímica
Fullerenes
Photochemistry
description Over the last years, carbon nano-onions (CNOs) have been in focus in material science research. Their red-shifted absorption allows utilizing CNOs as promising photosensitizers. We report here a systematic study of excited state properties of six double-layered Li+ doped fullerenes of Ih symmetry: [Li@C60@C240]+, [Li@C60@C540]+, [Li@C60@C960]+, [Li@C240@C540]+, [Li@C240@C960]+ and [Li@C540@C960]+. On the basis of TDDFT calculations, we show that the long-wave absorption by the Li+ doped species leads to charge transfer (CT) between the inner and the outer shells unlike their neutral double-layered precursors. The CT energy depends strongly on the size of the concentric fullerenes and it can easily be tuned by varying both the encapsulated metal ion and the size of the shells. Two types of low-lying excited states are identified (1) capacitor-like structures, as Li+@C60-@C240+, with alternating positive and negative charges, and (2) states, where the positive charge is delocalized over the outer shell, as in Li@C240@C540+. We suggest a simple expression to estimate the energy difference of these excited states and to predict the type of the lowest CT state in nested fullerenes. The effect of nature of the encapsulated ion on the charge transfer state energies is considered. The HOMO - LUMO transition energy is found to vary significantly when going from [Li@C60@C240]+ to [Li@C540@C960]+
publishDate 2019
dc.date.none.fl_str_mv 2019
info
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/acceptedVersion
peer-reviewed
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10256/16739
http://hdl.handle.net/10256/16739
url http://hdl.handle.net/10256/16739
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1021/acs.jpcc.9b02354
info:eu-repo/semantics/altIdentifier/issn/1932-7447
info:eu-repo/semantics/altIdentifier/eissn/1932-7455
dc.rights.none.fl_str_mv Tots els drets reservats
info:eu-repo/semantics/openAccess
rights_invalid_str_mv Tots els drets reservats
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv 8 p.
application/pdf
dc.publisher.none.fl_str_mv American Chemical Society (ACS)
publisher.none.fl_str_mv American Chemical Society (ACS)
dc.source.none.fl_str_mv © Journal of Physical Chemistry C, 2019, vol. 123, núm. 27, p. 16525-16532
Articles publicats (D-Q)
Stasyuk, Anton J. Stasyuk, Olga A. Solà i Puig, Miquel Voityuk, Alexander A. 2019 Photoinduced charge shift in Li+ doped giant nested fullerenes Journal of Physical Chemistry C 123 16525 16532
reponame:Recercat. Dipósit de la Recerca de Catalunya
instname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
instname_str Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
reponame_str Recercat. Dipósit de la Recerca de Catalunya
collection Recercat. Dipósit de la Recerca de Catalunya
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15.812429

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