The electronic and
optical properties of low-dimensional semiconductors
are typically quite different from those of their bulk counterparts.
Yet, the optical gap of two-dimensional copper antimony disulfide
(CuSbS2) does not dramatically change with decreasing thickness
of the material. The absorption onset remains at about 1.5 eV in the
monolayer, bilayer, and bulk materials. Using density functional theory
and many-body perturbation theory, we rationalize this behavior through
the interplay of quantum confinement, electron–hole interactions,
and the formation of surface states. Specifically, the spatial confinement
in thin layers induces strongly bound optical transitions in the near-infrared
region. Our results explain the optical properties in copper antimony
disulfide platelets of varying thickness and set these materials as
potential candidates for novel photovoltaic devices and near-infrared
sensors.