We fabricated CulnSe2 and Cu(In,Ga)Se2 thin films by two different pathways using physical vapor deposition. In the first we formed a Cu-Se precursor and then reacted it with a flux of (In,Ga) + Se. These films had large grains but were too rough for optimal device performance. In the other pathway, we first formed a smooth precursor of (In,Ga)2Se3 and then exposed it to a flux of Cu+Se. We overshot the optimal film composition to allow recrystallization of the film by a secondary CuxSe phase. We then consumed the excess CuxSe in a third stage deposition of (In,Ga) + Se. The recrystallization step increased the grain sizes, and the resulting films remained smooth. Photovoltaic solar cells made from these films have produced the highest total-area efficiencies of any non-single-crystal, thin-film solar cell.
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