The power conversion efficiency (PCE) of cesium lead
halide (CsPbX3, X = l, Br, and Cl)-based all-inorganic
perovskite solar
cells (PSCs) is still struggling to compete with conventional organic–inorganic
halide perovskites. A combined material and device-related analysis
is much needed to understand the working principle to explore the
efficiency potential of CsPbX3-based PSCs. Therefore, here,
density functional theory (DFT) and SCAPS-1D-based studies were reported
to evaluate the photovoltaic (PV) performance of CsPbBr3-based PSCs. DFT is first applied to assess and extract structural
and optoelectronic properties (band structure, density of states,
Fermi surface, and absorption coefficient) of the considered absorber
layer. The calculated electronic band gap (E
g) of the CsPbBr3 absorber was 1.793 eV, which matched
well with the earlier computed theoretical value. Additionally, the
Pb 6p orbital contributed largely to the calculated density of states
(DOS), and the electronic charge density map showed that the Pb atom
acquired the majority of charges. In order to examine the optical
response of CsPbBr3, optical characteristics were computed
and correlated with electronic properties for its probable photovoltaic
applications. Fermi surface computation showed multiband characters.
Furthermore, to look for a suitable combination of the charge transport
layer, a total of nine HTLs (Cu2O, CuSCN, P3HT, PEDOT:PSS,
Spiro-MeOTAD, CuI, V2O5, CBTS, and CFTS) and
six ETLs (TiO2, PCBM, ZnO, C60, IGZO, and WS2) are used considering the experimental E
g (2.3 eV). The best power conversion efficiency (PCE)
of 13.86% is reported for TiO2 and CFTS in combination
with the CsPbBr3 absorber. The effects of operating temperature,
series and shunt resistances, Mott–Schottky, capacitance, generation
and recombination rates, quantum efficiency, and current–voltage
density were also examined. The resulting PV properties were also
compared with previously published data. Results reported in this
study will pave the way for the development of high-efficiency all-inorganic
CsPbBr3-based solar cells in the future.