1 and 2 mole% of Mn doped CuGaS (CGS) single crystals were grown by the chemical vapour transport (CVT) technique using iodine as the transporting agent. The analysis of the single crystal x-ray diffraction data suggests that the doping of 1 and 2 mole% Mn in the CGS single crystal does not affect the tetragonal (chalcopyrite) crystal structure. The optical absorption spectrum shows that the Mn ion induces a very strong absorption band in the UV–visible–near IR regions. The values of the crystal parameter (D) and the Racah parameter (B) calculated from the absorption spectra show d electron delocalization in the host crystal CGS. Room temperature photoluminescence spectra of undoped CGS only exhibited a band–band emission. But 1 and 2 mole% Mn doped CGS single crystals show two distinct CGS and Mn related emissions, both of which are excited via the CGS host lattice. Raman spectra of 1 and 2 mole% Mn doped CGS single crystals exhibit a high intensity peak of the A mode at 310 cm and 300 cm, respectively. EDAX, optical absorption and Raman spectrum studies reveal that Mn ions are substituted in the Ga ions and incorporated into the CGS lattice. The magnetization of Mn doped CGS single crystals was measured as a function of the magnetic field and temperature. Paramagnetic behaviour typical of spin S = 5/2 expected for Mn(d) magnetic centres was observed in the temperature range 2 K < T < 300 K. In Mn doping, the increase in bulk conductivity of the Mn doped CGS single crystals at room temperature indicates an increase in the hole concentration.
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