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Synthesis, X-ray crystal structure and photophysics of butterfly shape orange and red emanating polynuclear complexes of tris(dibenzoylmethanato)Ln(III) (Ln = Sm/Eu) and exo-bidentate 4,4′-bipyridine

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Abstract

Reaction of two equivalents of [Ln(dbm)3(H2O)] (Ln = Sm/Eu/Gd) with one equivalent of 4,4′-bipyridine (4,4′-bpy) led to the formation of rare polynuclear complexes of the type [Ln(dbm)3(4,4′-bpy)]n (dbm is the anion of 1,3-diphenyl-1,3-propanedione) instead of symmetrically bridged dinuclear complexes. The structure of the complexes has been established by the single crystal X-ray diffraction (SC-XRD) method and shows that the coordination sphere is composed of a LnO6N2 core (octacoordinated). Shape analysis further revealed that the geometry around Ln(III) is distorted square anti-prismatic with SHAPE value 0.738 and 25.719 for [Sm(dbm)3(4,4′-bpy)]n and [Eu(dbm)3(4,4′-bpy)]n, respectively. Photoluminescence (PL) properties of [Sm(dbm)3(4,4′-bpy)]n and [Eu(dbm)3(4,4′-bpy)]n are discussed in the solid-state and PMMA hybrid film (w/w 6%). By employing theoretical modelling in conjunction with the experimental PL data and crystal structure and an energy transfer (ET) mechanism for the sensitized PL of [Eu(dbm)3(4,4′-bpy)]n is proposed and discussed in detail. Finally, the role of each ligand in sensitized PL of [Eu(dbm)3(4,4′-bpy)]n is calculated and discussed by the chemical partitions of the radiative decay.


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The authors declare that the data supporting the findings of this study are available within the paper and its Supplementary Information files. They are available from the corresponding author upon reasonable request.

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Acknowledgements

N. H. thanks UGC (Govt. of India) for the award of the Basic Scientific Research fellowship. The authors are thankful to the Sophisticated Analytical Instrument Facility (SAIF), IIT Madras for Single Crystal X-ray analyses and Dr Neetu Singh of Advanced Instrumentation Research Facility (AIRF), JNU for Time-Resolved Fluorescence. The Central Instrument Facility (CIF) of Jamia Millia Islamia is gratefully acknowledged for extending FT-IR and Steady-state Luminescence and powder X-ray diffraction facility. RI acknowledges His Majesty's Trust Fund for Strategic Research (Grant No. SQU/SR/SCI/CHEM/21/01) and The Ministry of Higher Education, Research and Innovation (MoHERI), Oman (Grant: RC-RG/SCI/CHEM/22/01) for funding.

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  1. Department of Chemistry, School of Chemical and Life Sciences, Jamia Hamdard, New Delhi, Delhi, 110 062, India

    Najmul Hasan

  2. Department of Chemistry, Sultan Qaboos University, P.O. Box 36, 123, Al-Khod, Oman

    Rashid Ilmi

  3. Lanthanide Research Laboratory, Department of Chemistry, Jamia Millia Islamia, New Delhi, 110 025, India

    Najmul Hasan & Khalid Iftikhar

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Hasan, N., Ilmi, R. & Iftikhar, K. Synthesis, X-ray crystal structure and photophysics of butterfly shape orange and red emanating polynuclear complexes of tris(dibenzoylmethanato)Ln(III) (Ln = Sm/Eu) and exo-bidentate 4,4′-bipyridine. Photochem Photobiol Sci 23, 315–327 (2024). https://doi.org/10.1007/s43630-023-00519-w

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