Abstract

Inorganic–organic hybrid perovskites offer wide optical absorption, long charge carrier diffusion length, and high optical-to-electrical conversion, enabling more than 25% efficiency of single-junction perovskite solar cells. All-perovskite four-terminal (4T) tandem solar cells have gained great attention because of solution-processability and potentially high efficiency without a need for current-matching between subcells. To make the best use of a tandem architecture, the subcell bandgaps and thicknesses must be optimized. This study presents a drift-diffusion simulation model to find optimum device parameters for a 4T tandem cell exceeding 33% of efficiency. Optimized subcell bandgaps and thicknesses, contact workfunctions, charge transport layer doping and perovskite surface modification are investigated for all-perovskite 4T tandem solar cells. Also, using real material and device parameters, the impact of bulk and interface traps is investigated. It is observed that, despite high recombination losses, the 4T device can achieve very high efficiencies for a broad range of bandgap combinations. We obtained the best efficiency for top and bottom cell bandgaps close to 1.55 eV and 0.9 eV, respectively. The optimum thickness of the top and bottom cells are found to be about 250 nm and 450 nm, respectively. Furthermore, we investigated that doping in the hole transport layers in both the subcells can significantly improve tandem cell efficiency. The present study will provide the experimentalists an optimum device with optimized bandgaps, thicknesses, contact workfunctions, perovskite surface modification and doping in subcells, enabling high-efficiency all-perovskite 4T tandem solar cells.

Highlights

  • Inorganic–organic hybrid perovskites (IOHPs) have emerged as promising photovoltaic material because of their strong optical absorption, high optical to electrical conversion, defect-tolerance, and long-range charge carrier diffusion lengths [1,2,3]

  • We investigated that doping in the hole transport layers in both the subcells can significantly improve tandem cell efficiency

  • We present a TiberCAD-based drift-diffusion model to study the roles of various subcell parameters, i.e., bandgaps, thicknesses, charge transport layer doping, contact workfunction and perovskite interface modification

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Summary

Introduction

Inorganic–organic hybrid perovskites (IOHPs) have emerged as promising photovoltaic material because of their strong optical absorption, high optical to electrical conversion, defect-tolerance, and long-range charge carrier diffusion lengths [1,2,3]. Interface engineering, surface passivation, charge transport layer doping, and the role of contacts are not very well studied for PTSCs. More research is needed to develop and commercialize PTSC technologies. There have been theoretical studies to investigate tandem cell efficiency considering ideal absorbers (not necessarily perovskites) and ideal device structures [42,43,44,45] Most of these studies have been based on either a particular set of bandgaps or a fixed set of thicknesses. We present a TiberCAD-based drift-diffusion model to study the roles of various subcell parameters, i.e., bandgaps, thicknesses, charge transport layer doping, contact workfunction and perovskite interface modification. Perovskite interface modification is studied to maximize the 4T tandem efficiency

Simulation model
Results and discussion
No trap-assisted recombination losses
The impact of trap-assisted nonradiative recombinations
Doping in charge transport layers
Contact work function
Perovskite surface functionalization
Conclusion
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