Unveiling architectural and optoelectronic synergies in lead-free perovskite/perovskite/kesterite triple-junction monolithic tandem solar cells

TL;DR

This paper designs and optimizes lead-free tandem solar cells using environmentally friendly materials, achieving efficiencies over 27% with dual-junction and triple-junction architectures through detailed simulations.

Contribution

It introduces novel lead-free monolithic tandem solar cell architectures with optimized performance, advancing sustainable photovoltaic technology.

Findings

Dual-junction device achieved 27.3% efficiency

Triple-junction device achieved 30.69% efficiency

Simulations considered radiative and non-radiative recombination mechanisms

Abstract

The widespread use of lead-based materials in tandem solar cells raises critical environmental and health concerns due to their inherent toxicity and risk of contamination. To address this challenge, we focused on lead-free tandem architectures based on non-toxic, environmentally benign materials such as tin-based perovskites and kesterites, which are essential for advancing sustainable photovoltaic technologies. In this study, we present the proposition, design, and optimization of two distinct lead-free monolithic tandem solar cell architectures - an all-perovskite dual-junction device employing potassium tin iodide (KSnI3) and formamidinium tin triiodide (FASnI3) as absorbers for the top and bottom subcells, respectively, and a triple-junction monolithic tandem structure incorporating KSnI3, FASnI3, and Ag-doped copper zinc tin selenide (ACZTSe) as absorbers for the top, middle, and bottom subcells, respectively. We simulated the optical and electrical characteristics of these devices using the finite-difference time-domain and finite element methods, explicitly considering radiative, non-radiative, and surface recombination mechanisms. The optimized all-perovskite dual-junction solar cell achieved a power conversion efficiency (PCE) of 27.3%, with short-circuit current density (Jsc) of 14.74 mA/cm2, open-circuit voltage (Voc) of 2.227 V, and fill factor (FF) of 83.14%. Conversely, the optimized triple-junction hybrid perovskite-kesterite architecture secured an elevated PCE of 30.69%, along with Jsc of 13.184 mA/cm2, Voc of 2.766 V, and FF of 84.18%. These findings reveal the strong potential of lead-free perovskite and kesterite material based absorbers in promoting high-performance hybrid tandem solar cells, highlighting their importance in advancing sustainable and efficient photovoltaic technologies.