The
search for two-dimensional (2D) systems for applications in
solar cells has continuously challenged our community. Here, we report
screening of 2D monolayers from group IV to XI transition-metal dichalcogenides,
MQ2, searching for candidates for high-performance photovoltaic
devices, where M = 3d, 4d, and 5d transition metals and Q = S, Se,
and Te, i.e., it yields 72 MQ2 monolayers. Through a robust
theoretical framework that combines density functional theory, tight
binding based on maximum localized Wannier functions, and the Bethe–Salpeter
equation, we investigate the electronic, optical, and excitonic properties
of the thermodynamic stable 2H-MQ2 monolayers. Furthermore,
we employ a linear regression analysis of our data to identify nontrivial
correlations between different optical and excitonic properties. From
the 72 2H-MQ2 monolayers, we found from phonon calculations
that only 22 are dynamically stable in the 2H form, of which 14 are
semiconductors with a wide range of energy band gaps. Our results
show that the presence of excitons affects the band alignment and
the power conversion efficiency. In these compounds, the valley degeneracy
breaking driven by spin-orbit coupling and the excitonic correction
in the optical properties may be explored, through control of optical
helicity, to tune the efficiency of the MQ2-based photovoltaic
devices. We find high-efficiency van der Waals (vdW) heterostructures
for solar cells and observe a strong linear correlation between exciton
energy and the energy band gap for the stable semiconductors.