Ultrafast excited-state excitation dynamics in a quasi-two-dimensional light-harvesting antenna based on ruthenium(II) and palladium(II) chromophores

Chemistry : a European Journal
Benjamin DietzekJürgen Popp

Abstract

A detailed study on the excited-state-excitation migration taking place within the tetranuclear complex [{(tbbpy)(2)Ru(tmbi)}(2){Pd(allyl)}(2)](PF(6))(2) (tbbpy = 4,4'-di-tert-butyl-2,2'-bipyridine and tmbi = 5,6,5',6'-tetramethyl-2,2'-bibenzimidazolate) is presented. The charge transfer is initiated by the photoexcitation into the lowest metal-to-ligand charge-transfer (MLCT) band of one of the peripheral ruthenium(II) chromophores and terminates on the central structurally complex Pd(2) (II)(allyl)(2) subunit. Thus, the system under investigation can be thought of as a functional model for the photosynthesis reaction center in plants. The kinetic steps involved in the overall process are inferred from femtosecond time-resolved transient-grating kinetics recorded at spectral positions within the regions of ground-state bleach and transient absorption. The kinetics features a complex non-exponential time behavior and can be fitted to a bi-exponential rise (tau(1)> or =200 fs, tau(2) approximately 1.5 ps) and a mono- or bi-exponential decay, depending on the experimental situation. The data leads to the formulation of a model for the intramolecular excitation-hopping ascribing intersystem crossing and subsequent cooling as the t...Continue Reading

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Citations

Feb 2, 2010·Physical Chemistry Chemical Physics : PCCP·Christian KuhntJürgen Popp
Aug 26, 2014·Dalton Transactions : an International Journal of Inorganic Chemistry·Julia Meyer-IlseBenjamin Dietzek
Apr 29, 2016·Physical Chemistry Chemical Physics : PCCP·Stephan Kupfer
May 12, 2015·Physical Chemistry Chemical Physics : PCCP·M ZimmerM Gerhards
Feb 20, 2007·Dalton Transactions : an International Journal of Inorganic Chemistry·Sven RauJohannes G Vos
Mar 21, 2009·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Ronald SiebertJürgen Popp
Jun 27, 2009·Chemistry : a European Journal·Stefanie TschierleiJürgen Popp
Feb 18, 2010·Dalton Transactions : an International Journal of Inorganic Chemistry·Michael KarnahlSven Rau
May 19, 2011·Macromolecular Rapid Communications·Ronald SiebertJürgen Popp
Jul 31, 2007·Chemical Society Reviews·Michael W Cooke, Garry S Hanan
Jun 12, 2012·The Journal of Biological Chemistry·Ramkrishna AdhikaryFloyd E Romesberg
Oct 4, 2014·Chemistry : a European Journal·Katharina MonczakSven Rau
Jun 18, 2011·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Michael KarnahlJürgen Popp
Apr 29, 2008·The Journal of Physical Chemistry. a·William HenryJohn J McGarvey
Nov 26, 2010·The Journal of Physical Chemistry. a·Martin PresseltJürgen Popp
Jul 6, 2017·The Journal of Physical Chemistry. C, Nanomaterials and Interfaces·Nicolas QueyriauxMurielle Chavarot-Kerlidou

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