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• W2333402405 endingPage "13194" @default.
• W2333402405 startingPage "13181" @default.
• W2333402405 abstract "The first example of a Donor-spacer-Acceptor tryad, based upon a molybdenum-ene-1,2-dithiolate unit as the Donor and a naphthalene-diimide as the Acceptor, has been synthesized and its photophysical properties investigated. Synthesis required the preparation of a new pro-ligand containing a protected ene-1,2-dithiolate bound through a phenyl linkage to a naphthalenetetracarboxylicdiimide (NDI) group. Deprotection of this pro-ligand by base hydrolysis, followed by reaction with [Cp2MoCl2], produced the new dyad [Cp2Mo(SC(H)C(C6H4–NDI)S)] (2). Electrochemical studies showed that 2 can be reversibly oxidized to [2]+ and reduced to [2]−, [2]2–, and [2]3–. These studies, augmented by UV/vis, IR, and electron paramagnetic resonance (EPR) spectra of electrochemically generated [2]+ and [2]−, show that the highest occupied molecular orbital (HOMO) of 2 is ene-1,2-dithiolate-based and the lowest unoccupied molecular orbital (LUMO) is NDI-based; these conclusions are supported by density functional theory (DFT) calculations for the electronic ground state on a model of 2 which also showed that these two parts of the molecule are electronically distinct. The dynamics of the excited states of 2 in CH2Cl2 solution were investigated by picosecond time-resolved IR spectroscopy following irradiation by a 400 nm ∼120 fs laser pulse. These investigations were complemented by an ultrafast transient absorption spectroscopic study from 420 to 760 nm of the nature of the excited states of 2 in CH2Cl2 solution following irradiation by a 383 nm ∼120 fs laser pulse. These studies showed that irradiation of 2 at both 400 and 383 nm leads to the formation of the [(Cp)2{Mo(dt)}+-Ph-{NDI}−] charge-separated state as a result of a cascade electron transfer initiated by the formation of an 1NDI* excited state. 1NDI* rapidly (ca. 0.2 ps) forms the local charge transfer state [Cp2Mo(dt)-{Ph}+-{NDI}−] which has a lifetime of about 1.7 ps and decays to produce the ground state and the charge-separated state [(Cp)2{Mo(dt)}+·-Ph-{NDI}−]; the latter has an appreciable lifetime, about 15 ns in CH2Cl2 at room temperature." @default.
• W2333402405 created "2016-06-24" @default.
• W2333402405 creator A5028595550 @default.
• W2333402405 creator A5036243869 @default.
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• W2333402405 creator A5062149527 @default.
• W2333402405 creator A5063028677 @default.
• W2333402405 creator A5067255451 @default.
• W2333402405 creator A5074882415 @default.
• W2333402405 creator A5091424152 @default.
• W2333402405 date "2012-09-05" @default.
• W2333402405 modified "2023-10-17" @default.
• W2333402405 title "Ultrafast Intramolecular Charge Separation in a Donor–Acceptor Assembly Comprising Bis(η⁵-cyclopentadienyl)molybdenum Coordinated to an Ene-1,2-dithiolate-naphthalenetetracarboxylicdiimide Ligand" @default.
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