posted on 2024-01-19, 18:42authored byAn-Yu Zhu, Rui-Xue Ding, Hao-Ting Xu, Chuan-Jia Tong, Keith P. McKenna
Cu–Zn cation disorder plays
a vital and controversial role
in kesterite CuZnSn(S1–xSex)4 solar cells. We demonstrate
using density functional theory and nonadiabatic molecular dynamics
simulations that the Cu–Zn disorder across different planes
(i.e., Cu–Sn and Cu–Zn planes) is significantly more
detrimental to device performance than the case when disorder is confined
only to the Cu–Zn planes. The main reason is that different
plane disorder induces a significant elongation of Sn–S/Se
bond lengths, leading to a downshift of the conduction band minimum,
decreasing the band gap, and reducing the optical absorption. Moreover,
Cu–Zn disorder across different planes accelerates nonradiative
electron–hole recombination and decreases charge carrier lifetime
due to the reduction of the band gap and enhanced electron-vibrational
interaction. Our results provide a theoretical explanation for the
influence of Cu–Zn disorder on material performance and offer
valuable insight into the design of more efficient solar cells.