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

• Published in: Journal of materials science. Materials in electronics 2024-02, Vol.35 (5), p.329, Article 329
• Main Authors: Ramesh, K. S., Munusamy, Saravanabhavan, Saravanakumar, M., Manigandan, S., Muthusamy, Krishnakumar, Vinitha, G., Sekar, M.
• Format: Article
• Language: English
• Subjects: Absorption spectroscopy; Characterization and Evaluation of Materials; Charge distribution; Charge transfer; Chemical analysis; Chemical composition; Chemical synthesis; Chemistry and Materials Science; Crystal growth; Crystal structure; Emission analysis; Infrared spectroscopy; Materials Science; Molecular structure; Nonlinear optics; Optical and Electronic Materials; Optical properties; Parameter identification; Photoluminescence; Purity; Raman spectroscopy; Single crystals; Solubility; Spectrum analysis; Stoichiometry; Structural analysis; Thermal analysis; Thermal stability; Vibration mode
• ISSN: 0957-4522; 1573-482X
• DOI: 10.1007/s10854-024-11979-w

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 (P2 1 /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.