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Article: Real-time propagation of the reduced one-electron density matrix in atom-centered orbitals: Application to electron injection dynamics in dye-sensitized TiO 2 clusters

TitleReal-time propagation of the reduced one-electron density matrix in atom-centered orbitals: Application to electron injection dynamics in dye-sensitized TiO 2 clusters
Authors
Issue Date2008
PublisherAmerican Chemical Society. The Journal's web site is located at http://pubs.acs.org/journals/jpccck/
Citation
Journal Of Physical Chemistry C, 2008, v. 112 n. 42, p. 16655-16662 How to Cite?
AbstractThe ultrafast electron-transfer (ET) processes in three dye-sensitized TiO 2 systems (pycooh-, catechol-, and alizarin-) are studied by using the real-time time-dependent density functional theory (RT-TDDFT). TiO 2 cluster models are used to substitute TiO 2 nanocrystals in order to check the quantum size effect on ET. The initial-state geometrical optimization for the individual constituents and coupled systems and the subsequent calculations for IR spectra and the density of states (DOS) are performed at the B3LYP/Lanl2dz theory level. The calculated IR spectra, the DOS, and the low-lying excited states reveal that the couplings between three dyes and TiO 2 clusters are very strong so that an ultrafast electron injection from the excited dyes to TiO 2 clusters is favored. By following the electronic motion of coupled systems after the photoexcitation of adsorbates in real time without allowing the nuclei to move, we predict an electronic injection time of a few femtoseconds for the present finite systems, which is slightly longer than the experimental measurements and other theoretical predications for the ET time on the same dye-sensitized bulk TiO 2 systems due to the small clusters used in our simulation. We find that the ET time is appreciably dependent on the cluster size when the cluster is quite small. However, the size effects on ET time reduce dramatically as the cluster size reaches to a moderate middle size, for example, (TiO 2) 4. The electron-nuclear coupled movement does not play a significant role in the initial ET process in these three systems. The effects of different initial excited states on electronic dynamics are also discussed. © 2008 American Chemical Society.
Persistent Identifierhttp://hdl.handle.net/10722/168342
ISSN
2015 Impact Factor: 4.509
2015 SCImago Journal Rankings: 1.995
ISI Accession Number ID
References

 

DC FieldValueLanguage
dc.contributor.authorGuo, Zen_US
dc.contributor.authorLiang, Wen_US
dc.contributor.authorZhao, Yen_US
dc.contributor.authorChen, Gen_US
dc.date.accessioned2012-10-08T03:17:49Z-
dc.date.available2012-10-08T03:17:49Z-
dc.date.issued2008en_US
dc.identifier.citationJournal Of Physical Chemistry C, 2008, v. 112 n. 42, p. 16655-16662en_US
dc.identifier.issn1932-7447en_US
dc.identifier.urihttp://hdl.handle.net/10722/168342-
dc.description.abstractThe ultrafast electron-transfer (ET) processes in three dye-sensitized TiO 2 systems (pycooh-, catechol-, and alizarin-) are studied by using the real-time time-dependent density functional theory (RT-TDDFT). TiO 2 cluster models are used to substitute TiO 2 nanocrystals in order to check the quantum size effect on ET. The initial-state geometrical optimization for the individual constituents and coupled systems and the subsequent calculations for IR spectra and the density of states (DOS) are performed at the B3LYP/Lanl2dz theory level. The calculated IR spectra, the DOS, and the low-lying excited states reveal that the couplings between three dyes and TiO 2 clusters are very strong so that an ultrafast electron injection from the excited dyes to TiO 2 clusters is favored. By following the electronic motion of coupled systems after the photoexcitation of adsorbates in real time without allowing the nuclei to move, we predict an electronic injection time of a few femtoseconds for the present finite systems, which is slightly longer than the experimental measurements and other theoretical predications for the ET time on the same dye-sensitized bulk TiO 2 systems due to the small clusters used in our simulation. We find that the ET time is appreciably dependent on the cluster size when the cluster is quite small. However, the size effects on ET time reduce dramatically as the cluster size reaches to a moderate middle size, for example, (TiO 2) 4. The electron-nuclear coupled movement does not play a significant role in the initial ET process in these three systems. The effects of different initial excited states on electronic dynamics are also discussed. © 2008 American Chemical Society.en_US
dc.languageengen_US
dc.publisherAmerican Chemical Society. The Journal's web site is located at http://pubs.acs.org/journals/jpccck/en_US
dc.relation.ispartofJournal of Physical Chemistry Cen_US
dc.titleReal-time propagation of the reduced one-electron density matrix in atom-centered orbitals: Application to electron injection dynamics in dye-sensitized TiO 2 clustersen_US
dc.typeArticleen_US
dc.identifier.emailChen, G:ghc@yangtze.hku.hken_US
dc.identifier.authorityChen, G=rp00671en_US
dc.description.naturelink_to_subscribed_fulltexten_US
dc.identifier.doi10.1021/jp802007hen_US
dc.identifier.scopuseid_2-s2.0-55649102335en_US
dc.identifier.hkuros164767-
dc.relation.referenceshttp://www.scopus.com/mlt/select.url?eid=2-s2.0-55649102335&selection=ref&src=s&origin=recordpageen_US
dc.identifier.volume112en_US
dc.identifier.issue42en_US
dc.identifier.spage16655en_US
dc.identifier.epage16662en_US
dc.identifier.isiWOS:000260129400077-
dc.publisher.placeUnited Statesen_US
dc.identifier.scopusauthoridGuo, Z=37561370400en_US
dc.identifier.scopusauthoridLiang, W=7402026799en_US
dc.identifier.scopusauthoridZhao, Y=9240067800en_US
dc.identifier.scopusauthoridChen, G=35253368600en_US

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