BaZrS3 chalcogenide perovskites have emerged as a promising
absorber due to their exceptional properties. However, there are no
experimental reports on the applicability of BaZrS3 in
photovoltaics. Thus, theoretical knowledge of device structure engineering
is essential for its successful fabrication. In this regard, we have
proposed various BaZrS3 device configurations by altering
12 electron transport layers (ETLs) in combination with 13 hole transport
layers (HTLs) using SCAPS-1D, wherein a total of 782 devices are simulated
by tuning the thickness, carrier concentration, and defect density
of BaZrS3, ETLs, and HTLs. Interestingly, the absorber’s
thickness optimization enhanced the absorption in the device by 2.31
times, elevating the generation rate of charge carriers, while the
increase in its carrier concentration boosted the built-in potential
from 0.8 to 1.68 V, reducing the accumulation of charge carriers at
the interfaces. Notably, on further optimization of ETL and HTL combinations,
the best power conversion efficiency (PCE) of 28.08% is achieved for
FTO/ZrS2/BaZrS3/SnS/Au, occurring due to the
suppressed barrier height of 0.1 eV at the ZrS2/BaZrS3 interface and degenerate behavior of SnS, which increased
charge carrier transportation and conductivity of the devices. Upon
optimizing the work function, an ohmic contact is achieved for Pt,
boosting the PCE to 28.17%. Finally, the impact of Ti alloying on
BaZrS3 properties is examined on the champion FTO/ZrS2/BaZrS3/SnS/Pt device where the maximum PCE of
32.58% is obtained for Ba(Zr0.96,Ti0.04)S3 at a thickness of 700 nm due to extended absorption in the
NIR region. Thus, this work opens doors to researchers for the experimental
realization of high PCE in BaZrS3 devices.