NDLI: Ligand-to-Ligand Charge-Transfer Transitions of Platinum(II) Complexes with Arylacetylide Ligands with Different Chain Lengths: Spectroscopic Characterization, Effect of Molecular Conformations, and Density Functional Theory Calculations

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Ligand-to-Ligand Charge-Transfer Transitions of Platinum(II) Complexes with Arylacetylide Ligands with Different Chain Lengths: Spectroscopic Characterization, Effect of Molecular Conformations, and Density Functional Theory Calculations

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Law, Yuen-chi Kui, Steven C. F. Zhu, Nianyong Phillips, David Lee Che, Chi-ming Tong, Glenna So Ming Leung, King Hong
Description	Author Affiliation: Tong GS ( Department of Chemistry, Institute of Molecular Functional Materials and HKU-CAS Joint Laboratory on New Materials, The University of Hong Kong, Pokfulam, Hong Kong SAR, China.)
Abstract	The complexes $[Pt(tBu_{3}tpy)\{CC(C_{6}H_{4}CC)_{n−1}R\}]^{+}$ (n=1: R=alkyl and aryl (Ar); n=1–3: R=phenyl (Ph) or $Ph-N(CH_{3})_{2}-4;$ n=1 and 2, $R=Ph-NH_{2}-4;$ $tBu_{3}tpy=4,4`,4``-tri-tert-butyl-2,2`:6`,2``-terpyridine)$ and $[Pt(Cl_{3}tpy)(CCR)]^{+}$ (R=tert-butyl (tBu), Ph, 9,9’-dibutylfluorene, 9,9’-dibutyl-7-dimethyl-amine-fluorene; $Cl_{3}tpy=4,4`,4``-trichloro-2,2`:6`,2``-terpyridine)$ were prepared. The effects of substituent(s) on the terpyridine (tpy) and acetylide ligands and chain length of arylacetylide ligands on the absorption and emission spectra were examined. Resonance Raman (RR) spectra of $[Pt(tBu_{3}tpy)(CCR)]^{+}$ (R=n-butyl, Ph, and $C_{6}H_{4}-OCH_{3}-4)$ obtained in acetonitrile at 298 K reveal that the structural distortion of the CC bond in the electronic excited state obtained by 502.9 nm excitation is substantially larger than that obtained by 416 nm excitation. Density functional theory (DFT) and time-dependent DFT (TDDFT) calculations on $[Pt(H_{3}tpy)(CCR)]^{+}$ (R= n-propyl (nPr), 2-pyridyl (Py)), $[Pt(H_{3}tpy)\{CC(C_{6}H_{4}CC)_{n−1}Ph\}]^{+}$ (n=1–3), and $[Pt(H_{3}tpy)\{CC(C_{6}H_{4}CC)_{n−1}C_{6}H_{4}-N(CH_{3})_{2}-4\}]^{+}/+H^{+}$ (n=1–3; $H_{3}tpy=nonsubstituted$ terpyridine) at two different conformations were performed, namely, with the phenyl rings of the arylacetylide ligands coplanar (“cop”) with and perpendicular (“per”) to the $H_{3}tpy$ ligand. Combining the experimental data and calculated results, the two lowest energy absorption peak maxima, $λ_{1}$ and $λ_{2},$ of $[Pt(Y_{3}tpy)(CCR)]^{+}$ (Y=tBu or Cl, R=aryl) are attributed to $^{1}[π(CCR)→π(Y_{3}tpy)]$ in the “cop” conformation and mixed $^{1}[d_{π}(Pt)→π(Y_{3}tpy)]/^{1}[π(CCR)→π(Y_{3}tpy)]$ transitions in the “per” conformation. The lowest energy absorption peak $λ_{1}$ for $[Pt(tBu_{3}tpy)\{CC(C_{6}H_{4}CC)_{n−1}C_{6}H_{4}-H-4\}]^{+}$ (n=1–3) shows a redshift with increasing chain length. However, for $[Pt(tBu_{3}tpy)\{CC(C6H4CC)_{n−1}C_{6}H_{4}-N(CH_{3})_{2}-4\}]^{+}$ (n=1–3), $λ_{1}$ shows a blueshift with increasing chain length n, but shows a redshift after the addition of acid. The emissions of $[Pt(Y_{3}tpy)(CCR)]^{+}$ (Y=tBu or Cl) at 524–642 nm measured in dichloromethane at 298 K are assigned to the $^{3}[π(CCAr)→π(Y_{3}tpy)]$ excited states and mixed $^{3}[d_{π}(Pt)→π(Y_{3}tpy)]/^{3}[π(CC)→π(Y_{3}tpy)]$ excited states for R=aryl and alkyl groups, respectively. $[Pt(tBu_{3}tpy)\{CC(C_{6}H_{4}CC)_{n−1}C_{6}H_{4}-N(CH_{3})_{2}-4\}]^{+}$ (n=1 and 2) are nonemissive, and this is attributed to the small energy gap between the singlet ground state $(S_{0})$ and the lowest triplet excited state $(T_{1}).$
ISSN	09476539
e-ISSN	15213765
Journal	Chemistry - A European Journal
Issue Number	22
Volume Number	16
Language	English
Publisher	Wiley-VCH;ChemPubSoc Europe
Publisher Date	2010-06-11
Publisher Place	Germany
Access Restriction	Open
Subject Keyword	Chemistry
Content Type	Text
Resource Type	Article
Subject	Organic Chemistry Catalysis

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