Crystal Chemistry, Optic and Magnetic Characterizations of a New Copper Based Material Templated by Hexahydrodiazepine

Mansoura Bourwina; Rawia Msalmi; Sandra Walha; Mark M Turnbull; Thierry Roisnel; Ahlem Guesmi; Ammar Houas; Naoufel Ben Hamadi; Houcine Naïli

doi:10.1021/acsomega.2c08035

Crystal Chemistry, Optic and Magnetic Characterizations of a New Copper Based Material Templated by Hexahydrodiazepine

ACS Omega. 2023 Apr 18;8(17):15075-15082. doi: 10.1021/acsomega.2c08035. eCollection 2023 May 2.

Authors

Mansoura Bourwina¹, Rawia Msalmi¹, Sandra Walha¹, Mark M Turnbull², Thierry Roisnel³, Ahlem Guesmi⁴, Ammar Houas⁵, Naoufel Ben Hamadi^{4

6}, Houcine Naïli¹

Affiliations

¹ Laboratoire Physico-Chimie de l'Etat Solide, Département de Chimie, Faculté des Sciences de Sfax, Université de Sfax, B.P. 1171, 3000 Sfax, Tunisia.
² Carlson School of Chemistry and Biochemistry, Clark University, Worcester, Massachusetts 01610, United States.
³ Institut des Sciences Chimiques de Rennes UMR 6226 CNRS, Université Rennes 1, Campus de Beaulieu, F-35042 Rennes, France.
⁴ Chemistry Department, College of Science, Imam Mohammad Ibn Saud Islamic University, P.O. Box 5701, Riyadh 11432, Saudi Arabia.
⁵ Research Laboratory of Catalysis and Materials for Environment and Processes, University of Gabes, City Riadh Zerig, 6029 Gabes, Tunisia.
⁶ Medicinal Chemistry and Natural Products, Laboratory of Heterocyclic Chemistry, Natural Products and Reactivity (LR11ES39), Faculty of Science of Monastir, University of Monastir, Avenue of Environment, 5019 Monastir, Tunisia.

Abstract

Crystals of the new organic-inorganic material (DAP-H2)[CuBr₄] (1); (DAP = hexahydrodiazepine (C₅H₁₄N₂)) were successfully synthesized by slow evaporation and characterized by single-crystal X-ray diffraction, infrared spectroscopy, thermal analysis, UV-Vis-NIR diffuse reflectance spectroscopy, and magnetic measurements. X-ray investigation demonstrates that 1 crystallizes in the monoclinic space group C2/c. The supramolecular crystal structure of 1 is guided by several types of hydrogen bonding which connect anions and cations together into a three-dimensional network. The optical band gap was determined by diffuse reflectance spectroscopy to be 1.78 eV for a direct allowed transition, implying that it is suitable for light harvesting in solar cells. The vibrational properties of this compound were studied by infrared spectroscopy, while its thermal stability was established by simultaneous TGA-DTA from ambient temperature to 600 °C. The study of the photoresponse behavior of an optoelectronic device, based on (C₅H₁₄N₂)[CuBr₄], has shown a power conversion efficiency (PCE) of 0.0017%, with J _sc = 0.0208 mA/cm², V _oc = 313.7 mV, and FF = 25.46. Temperature dependent magnetic susceptibility measurements in the temperature range 1.8-310 K reveal weak antiferromagnetic interactions via the two-halide superexchange pathway [2J/k _B = -8.4(3) K].