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• W2117178004 abstract "Abstract Two multifunctional photoactive complexes [Re(Cl)(CO) 3 (MeDpe + ) 2 ] 2+ and [Re(MeDpe + )(CO) 3 (bpy)] 2+ (MeDpe + = N ‐methyl‐4‐[ trans ‐2‐(4‐pyridyl)ethenyl]pyridinium, bpy=2,2′‐bipyridine) were synthesized, characterized, and their redox and photonic properties were investigated by cyclic voltammetry; ultraviolet–visible–infrared (UV/Vis/IR) spectroelectrochemistry, stationary UV/Vis and resonance Raman spectroscopy; photolysis; picosecond time‐resolved absorption spectroscopy in the visible and infrared regions; and time‐resolved resonance Raman spectroscopy. The first reduction step of either complex occurs at about −1.1 V versus Fc/Fc + and is localized at MeDpe + . Reduction alone does not induce a trans → cis isomerization of MeDpe + . [Re(Cl)(CO) 3 (MeDpe + ) 2 ] 2+ is photostable, while [Re(MeDpe + )(CO) 3 (bpy)] 2+ and free MeDpe + isomerize under near‐UV irradiation. The lowest excited state of [Re(Cl)(CO) 3 (MeDpe + ) 2 ] 2+ has been identified as the Re(Cl)(CO) 3 →MeDpe + 3 M LCT (MLCT=metal‐to‐ligand charge transfer), decaying directly to the ground state with lifetimes of ≈42 (73 %) and ≈430 ps (27 %). Optical excitation of [Re(MeDpe + )(CO) 3 (bpy)] 2+ leads to population of Re(CO) 3 →MeDpe + and Re(CO) 3 →bpy 3 M LCT states, from which a MeDpe + localized intraligand 3 ππ* excited state ( 3 IL) is populated with lifetimes of ≈0.6 and ≈10 ps, respectively. The 3 IL state undergoes a ≈21 ps internal rotation, which eventually produces the cis isomer on a much longer timescale. The different excited‐state behavior of the two complexes and the absence of thermodynamically favorable interligand electron transfer in excited [Re(MeDpe + )(CO) 3 (bpy)] 2+ reflect the fine energetic balance between excited states of different orbital origin, which can be tuned by subtle structural variations. The complex [Re(MeDpe + )(CO) 3 (bpy)] 2+ emerges as a prototypical, multifunctional species with complementary redox and photonic behavior." @default.
• W2117178004 created "2016-06-24" @default.
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• W2117178004 creator A5065419027 @default.
• W2117178004 date "2008-07-30" @default.
• W2117178004 modified "2023-10-18" @default.
• W2117178004 title "Ultrafast Excited State Dynamics Controlling Photochemical Isomerization of<i>N</i>-Methyl-4-[<i>trans</i>-2-(4-pyridyl)ethenyl]pyridinium Coordinated to a {Re^I(CO)₃(2,2′-bipyridine)} Chromophore" @default.
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• W2117178004 doi "https://doi.org/10.1002/chem.200800188" @default.
• W2117178004 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/18604857" @default.
• W2117178004 hasPublicationYear "2008" @default.
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