Dielectric function and double absorption onset of monoclinic Cu2SnS3: Origin of experimental features explained by first-principles calculations

• Measured and calculated dielectric function of monoclinic Cu2SnS3.
• Experimental double absorption onset reproduced in density functional theory calculations.
• Double absorption onset due to optical transitions from three close-lying valence bands to a single conduction band at Γ.
• Very polarization dependent and strong absorption near the band edge.

In this work, we determine experimentally the dielectric function of monoclinic Cu2SnS3 (CTS) by spectroscopic ellipsometry from 0.7 to 5.9 eV. An experimental approach is proposed to overcome the challenges of extracting the dielectric function of Cu2SnS3 when grown on a glass/Mo substrate, as relevant for photovoltaic applications. The ellipsometry measurement reveals a double absorption onset at 0.91 eV and 0.99 eV. Importantly, we demonstrate that calculation within the density functional theory (DFT) confirms this double onset only when a very dense k-mesh is used to reveal fine details in the electronic structure, and this can explain why it has not been reported in earlier calculated spectra. We can now show that the double onset originates from optical transitions at the Γ-point from three energetically close-lying valence bands to a single conduction band. Thus, structural imperfection, like secondary phases, is not needed to explain such an absorption spectrum. Finally, we show that the absorption coefficient of CTS is particularly large in the near-band gap spectral region when compared to similar photovoltaic materials.

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