Donor - acceptor pair recombination in Tl2InGaS4 layered crystals

Photoluminescence (PL) spectra of Tl2InGaS4 layered single crystals were studied in the temperature range 15-150 K and wide laser excitation intensity range 0.01-110.34 Wcm-2. We observed a total of three PL bands, one centered at 542 nm (2.286 eV, A-band), one at 607 nm (2.041 eV, B-band), and one at 707 nm (1.754 eV, C-band), at various excitation intensities. The A- and the B-bands were determined to be due to radiative transitions from moderately deep donor levels located at 0.189 and 0.443 eV below the bottom of the conduction band to the shallow acceptor levels at 0.025 and 0.016 eV above the top of the valence band, respectively. The blue shift of the C-band peak energy and the quenching of the PL with increasing temperature are explained within the configuration coordinate model. The observation in the PL spectra of different emission bands in the sequence of B-, C- and A-bands at low, moderate, and high excitation laser intensities, respectively, are attributed to the shift of the quasi-Fermi level with increasing excitation intensity.