Calculation for high pressure behaviour of potential solar cell materials Cu2FeSnS4 and Cu2MnSnS4

Abstract

Exploring alternatives to the Cu2ZnSnS4 kesterite solar cell absorber, we have calculated first principle enthalpies of different plausible structural models (kesterite, stannite, P4 and GeSb type) for Cu2FeSnS4 and Cu2MnSnS4 to identify low and high pressure phases. Due to the magnetic nature of Fe and Mn atoms we included a ferromagnetic (FM) and anti-ferromagnetic (AM) phase for each structural model. For Cu2FeSnS4 we predict the following transitions: P4 (AM) 16.3 GPa → GeSb type (AM) 23.0 GPa → GeSb type (FM). At the first transition the electronic structure changes from semi-conducting to metallic and remains metallic throughout the second transition. For Cu2MnSnS4, we predict a direct AM (kesterite) to FM (GeSb-type) transitions at somewhat lower pressure (12.1 GPa). The GeSb-type structure also shows metallic behaviour.