Growth of Cu(In,Al)(Se,S)2 thin films by selenization and sulfurization for a wide bandgap absorber

Full text : Chalcopyrite structure Cu(In1.xAlx)(SySe1-y)2 (CIASS) alloys are attracting attention as promising candidates for the light-absorbing medium of high conversion efficiency, low cost, and lightweight solar cells. In addition, according to the wide variation in the bandgap energy (1.0-3.5eV), multiple-junction or tandem solar cells able to be fabricated using CIASS films of different compositions, x and y. In fact, several research groups have recently fabricated Cu(In,Al)Se2-based solar cells, and a high μ of 16.9 percent has been demonstrated. The sulfurization following selenization of Cu(In,Ga)Se2 (CIGS) films is believed to be promising for bandgap engineering of absorber material. Furthermore, it has been reported that the controlled incorporation of sulfur into CIGS films reduces the carrier recombination in the space charge region due to the deep trap states. Therefore, the sulfurization following selenization is expected to be used as a method of growth of CIASS films. However, sulfurization condition following selenization for obtaining CIASS films has not been clarified. The crystal growth of CIASS must be studied for solar cell applications. In this study, the advantages of using sulfurization for the growth of CIASS will be presented. Cu-In-Al precursors were selenized using diethylselenide (DESe) at 515-570 degrees Celsium for 60- 90 min under atmospheric pressure. The flow rates of DESe and N2 carrier gases were 35 imol/min and 2 L/min, respectively. The films were then sulfurized at 550 degrees Celsium using S vapor. These films were characterized by SEM, EDX, XRD, and PL measurements. Using the selenization and sulfurization technique, polycrystalline Cu(In,Al)Se2, CuIn(Se,S)2, CuInS2 films with thickness of approximately 2.0 im were formed without additional annealing. The films adhered well to the Mo/SLG substrate, which was confirmed by the peeling test. Phase separations, i.e. distinct peaks corresponding to CuInSe2, CuAlSe2 CuInS2, or binary compounds were not observed. These results represent a step toward realizing a tandem solar cell using CIASS film grown by selenization and sulfurization that use conventional and large-scale equipment.