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Comprehensive characterization and multifaceted analysis of benzimidazoliumgallate single crystal: synthesis, structural elucidation, optical properties, thermal stability, nonlinear optical behaviour, and quantum computing insights

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Abstract

The synthesis, crystal structure, and comprehensive characterization of a novel benzimidazolium gallate (BIG) charge transfer complex are reported in this study. The BIG crystal was obtained through the reaction of gallic acid and benzimidazole in methanol, leading to the formation of high-quality single crystals. Elemental analysis confirmed the purity and stoichiometry of the synthesized crystal. The crystal structure was elucidated using single-crystal X-ray diffraction, revealing a monoclinic crystal system with a centrosymmetric space group (P21/n) and specific unit cell parameters. Hydrogen bonding interactions were identified between the benzimidazolium cation and gallate anion, involving N+⋯H⋯O and N⋯H⋯O, C–H⋯O, and O⋯H⋯O interactions. The solubility study indicated the positive solubility of BIG in methanol, influencing the choice of solvent for crystal growth. Powder X-ray diffraction confirmed the crystallinity and purity of the synthesized material. UV–visible absorption spectroscopy revealed characteristic peaks corresponding to π-π* and charge transfer transitions. Photoluminescence studies exhibited violet emission peaks attributed to proton transfer interactions within the crystal. FT-IR and FT-Raman spectroscopy provided insights into vibrational modes, including OH group deformations and COO-group vibrations. Additionally, NMR spectra confirmed the molecular composition of BIG. Thermal analysis demonstrated the stability and melting point of the crystal, further affirming its charge-transfer nature. Nonlinear optical studies indicated low second harmonic generation efficiency compared to standard reference materials, but it shows reasonable THG efficiency as attested by Z-scan studies. DFT calculations, Hirshfeld surface analysis, and MEP mapping provided a deeper understanding of the molecular structure, charge distribution, and reactivity of BIG. Overall, the multifaceted characterization of the BIG charge transfer complex underscores its potential for diverse applications in the optical and material sciences.

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Data availability

The data that support the findings of this study are available from the corresponding author, [Dr. MSB (Saravanabhavan Munusamy)], upon reasonable request.

Supplementary data

CCDC: 2111961 contain the supplementary crystallographic data for this paper. These data can be obtained free of charge via http://www.ccdc.cam.ac.uk/conts/retrieving.html (or from the Cambridge Crystallographic Data Centre, 12, Union Road, Cambridge CB21EZ, UK; fax: + 44 1223 336,033) or E-mail: deposit@ccdc.cam.ac.uk.

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Acknowledgements

The authors acknowledge STIC Kochi, India, for single crystal x-ray diffraction analysis, and Karunya Deemed University, Coimbatore, India, for UV-visible-NIR, Photoluminescence, and FT-IR spectral analysis.

Author information

Authors and Affiliations

  1. Department of Chemistry, Sri Ramakrishna Mission Vidyalaya College of Arts and Science, Coimbatore, Tamil Nadu, 641 020, India

    K. S. Ramesh & M. Sekar

  2. Department of Chemistry, Adithya Institute of Technology, Coimbatore, Tamil Nadu, 641 107, India

    K. S. Ramesh

  3. Department of Chemistry, KPR Institute of Engineering and Technology, Coimbatore, Tamil Nadu, 641407, India

    Saravanabhavan Munusamy

  4. Department of Physics, Sri Ramakrishna Mission Vidyalaya College of Arts and Science, Coimbatore, Tamil Nadu, 641 020, India

    M. Saravanakumar

  5. School of Chemical Engineering, Chonnam National University, 77 Yongbong-ro, Buk-gu, Gwangju, 61186, South Korea

    S. Manigandan

  6. Department of Physics, Anna University Regional Campus, Coimbatore, Tamil Nadu, India

    Krishnakumar Muthusamy

  7. Division of Physics, School of Advanced Sciences, Vellore Institute of Technology, Chennai, Tamil Nadu, India

    G. Vinitha

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Contributions

KSR: conceptualization, methodology, investigation, writing—original draft. SM: project administration, funding acquisition, resources, data curation, project administration writing—original draft. MS: data curation, resources, funding acquisition, software, visualization, SM: software, resources, visualization review & editing. KM: instrumentation, software, investigation, writing—original draft. GV: instrumentation, writing—review and editing. MS: supervision, project administration, writing—review and editing.

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Correspondence to Saravanabhavan Munusamy or M. Sekar.

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Ramesh, K.S., Munusamy, S., Saravanakumar, M. et al. Comprehensive characterization and multifaceted analysis of benzimidazoliumgallate single crystal: synthesis, structural elucidation, optical properties, thermal stability, nonlinear optical behaviour, and quantum computing insights. J Mater Sci: Mater Electron 35, 329 (2024). https://doi.org/10.1007/s10854-024-11979-w

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