PEROVSKITE-BASED TANDEM SOLAR CELLS USING QUANTUM TRANSPORT AND INTERFACE OPTIMIZATION TECHNIQUES

Abstract

Metal-halide perovskite-based tandem solar cells have emerged as the most promising pathway to surpass the Shockley-Queisser limit of single-junction photovoltaics. This review comprehensively examines the synergistic integration of quantum transport theory and nanoscale interface optimization techniques that underpin state-of-the-art tandem architectures. Monolithic two-terminal perovskite/silicon tandems have achieved certified power conversion efficiencies of 34.85%, while all-perovskite tandems have reached 30.1%, demonstrating the transformative potential of photonic energy partitioning. The review systematically analyzes the fundamental physics governing tunnel recombination junctions, contrasting direct band-to-band tunneling with trap-assisted tunneling mechanisms through Kane's interband tunneling model and Non-Equilibrium Green's Function formalism. Critical interface engineering strategies are evaluated, including carbazole-based self-assembled monolayers (2PACz, Me-4PACz, MeO-2PACz) that modulate substrate work functions via molecular dipole engineering, and bilayer passivation architectures combining inorganic barrier layers with organic ammonium halides. Crystallographic orientation control through solution-processed additives is shown to suppress photo-induced phase segregation and enhance (100) facet preferential growth, while stress-buffering architectures employing porous/dense SnOₓ double layers enable flexible tandem devices with 33.4% efficiency. Comparative benchmarks across silicon heterojunction, TOPCon, and hybrid interdigitated back contact bottom cells reveal trade-offs between thermal budget constraints and industrial compatibility. This review provides a unified framework linking microscopic quantum transport phenomena to macroscopic device performance, offering strategic pathways for next-generation ultrahigh-efficiency photovoltaics.