Numerical exploration on unveiling the photovoltaic potential of MgXS3(X = Ti, Zr, Hf) chalcogenide perovskites

Lead-free chalcogenide perovskites offer a nontoxic and thermally robust path beyond Pb-based perovskite solar cells (PSCs), but their device-level behavior in realistic three-dimensional geometries remains insufficiently characterized.

In this work, we investigate ZnSe/MgXS3(X = Ti, Zr, Hf)/Sb2S3 solar cell architecture where MgXS3 absorbers from the II-IV-VI chalcogenide perovskite family is employed as the absorber layer.

The device is analyzed using 3D finite-element simulations in COMSOL Multiphysics that self-consistently couple optical generation, drift-diffusion carrier transport, and heat transfer under AM 1.5G 1-sun illumination, following a fully coupled opto-electro-thermal framework.

For each absorber composition, the impacts of absorber thickness, doping, and defect density are systematically investigated, and the contribution of an Sb2S3 back-surface-field (BSF) layer to carrier collection and spectral response is quantified.

Under optimized conditions, MgZrS3, MgTiS3, MgHfS3-based devices achieves a simulated power conversion efficiency (PCE) of 28.18%, 26.72%, and 28.16%, respectively.

The corresponding open-circuit voltage (VOC) values are 0.94 V, 0.74 V, and, 1.07 V while the short-circuit current density (JSC) values are 34.46 mA/cm2, 42.69 mA/cm2, and 29.89 mA/cm2, with fill factor (FF) values of 86.99%, 84.58%, and 88.02%, respectively.

Coupled electro-thermal simulations further reveal a small spatially non-uniform steady-state temperature rise across the ultrathin cell stack, mainly governed by non-radiative recombination and Joule dissipation within the active layers.

Overall, these results confirm MgXS3(X = Ti, Zr, Hf) chalcogenide perovskites as promising lead-free absorber materials and offer practical design guidance for achieving high-efficiency, thermally stable three-dimensional device architectures.