On efficiency of earth-abundant chalcogenide photovoltaic materials buffered with CdS: the limiting effect of band alignment

Abstract

Abstract Earth-abundant and environmentally-friendly Cu 2 –II–IV–VI 4 (II = Sr, Ba; IV = Ge, Sn; VI = S,Se) are considered materials for the absorber layers in thin film solar cells. Attempts to understand and improve optoelectronic properties of these newly emerged absorbers resulted in an efficiency of 5.2% in less than two years. However, the energy band alignment at the buffer/absorber interface has not been studied yet; an information which is of crucial importance for designing high performance devices. Therefore, current study focuses on the band offsets between these materials and the CdS buffer. Using first-principles calculations, band discontinuities are calculated at the buffer/absorber interface. The results yield a type-II band alignment between all Cu 2 –II–IV–VI 4 absorbers and CdS, hence a negative <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" overflow="scroll"> <mml:mi mathvariant="normal">Δ</mml:mi> <mml:msub> <mml:mrow> <mml:mi mathvariant="italic">E</mml:mi> </mml:mrow> <mml:mrow> <mml:mi mathvariant="normal">c</mml:mi> </mml:mrow> </mml:msub> </mml:math> . Adoption of a negative <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" overflow="scroll"> <mml:mi mathvariant="normal">Δ</mml:mi> <mml:msub> <mml:mrow> <mml:mi mathvariant="italic">E</mml:mi> </mml:mrow> <mml:mrow> <mml:mi mathvariant="normal">c</mml:mi> </mml:mrow> </mml:msub> </mml:math> (cliff-like conduction band offset) at the buffer/absorber interface, however, gives rise to low open circuit voltage and high interface-related recombinations. Therefore, it is necessary to search for an alternative buffer material that forms a type-I band alignment with these absorbers, where the conduction band minimum and the valence band maximum are both localized on the absorber side.