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Open AccessDOI: 10.1088/1674-4926/26020045Original Research

Crystallization suppression of mixed-halide intermediates for perovskite/Cu(In,Ga)Se2 tandem solar cells with improved efficiency

LI Manya¹,JING Linjing¹,TAN Hairen¹

National Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, Frontiers Science Center for Critical Earth Material Cycling, Nanjing University, Nanjing 210023, China

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Academic Research Journal
Published:January 15, 2026Edition:Vol. 32, Issue 2 • pp. 100-112Citation:LI Manya et al. (2026), Academic Research Journal
Impact FactorPeer-Reviewed Core
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Key Takeaways & Executive Findings

  • • Replacing NMP with 2-pyrrolidinone (PDI) suppresses crystallization of mixed-halide intermediates, enabling high-quality wide-bandgap perovskite films. • The strategy mitigates phase segregation and reduces defect densities, leading to improved open-circuit voltage and fill factor in perovskite/CIGS tandem solar cells. • The approach is compatible with scalable blade-coating in ambient air, addressing a key bottleneck for commercial deployment. • The work demonstrates a significant efficiency improvement in flexible all-thin-film tandem solar cells, advancing the potential for lightweight photovoltaics.
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Abstract

Flexible and lightweight photovoltaics represent a pivotal frontier in renewable energy, offering versatile applications ranging from building-integrated photovoltaics (BIPV) to portable power sources and aerospace systems. Among the various thin-film technologies, all-thin-film tandem solar cells, specifically those pairing metal-halide perovskites with copper indium gallium selenide (CIGS), have garnered considerable attention. This combination is particularly synergistic: CIGS serves as an ideal narrow-bandgap bottom cell (~1.1 eV) with proven stability and flexibility, while perovskites offer a tunable wide bandgap (WBG) top cell. To achieve optimal spectral matching and exceed the Shockley−Queisser limit of single-junction devices, the perovskite top cell requires a wide bandgap (>1.67 eV), which is obtained by increasing the bromide/iodide ratio in the mixed-halide composition. However, the fabrication of high-quality WBG perovskite films, particularly via scalable methods like blade-coating in ambient air, remains a formidable bottleneck. The crystallization kinetics of mixed-halide perovskites are notoriously difficult to control. The rapid evaporation of solvents and the distinct solubility differences between bromide and iodide precursors often drive uncontrollable, rapid crystallization. This leads to severe phase segregation, where iodide-rich and bromide-rich domains form, creating energetic disorder. Furthermore, processing in ambient air introduces moisture, which can act as a nucleation site, further accelerating disordered precipitation. These issues manifest as films with high defect densities, poor coverage (pinholes), and significant non-radiative recombination, which severely compromise the open-circuit voltage (VOC) and fill factor (FF) of the final devices. Zhang et al. address this critical challenge by reporting a crystallization suppression strategy that fundamentally alters the phase transition kinetics (Figs. 1(a) and 1(b), Nat Energy (2026). https://doi.org/10.1038/s41560-026-01975-1). By systematically investigating the coordination strength of solvents, they identified that replacing the traditional N-methyl-2-pyrrolidone (NMP) with 2-pyrrolidinone (PDI) can effectively modulate the nucleation and growth stages. The core innovation lies in the specific interaction between the solvent and perovskite precursors. In conventional NMP-based systems, the coordination...

1. Introduction

Flexible and lightweight photovoltaics represent a pivotal frontier in renewable energy, offering versatile applications ranging from building-integrated photovoltaics (BIPV) to portable power sources and aerospace systems. Among the various thin-film technologies, all-thin-film tandem solar cells, specifically those pairing metal-halide perovskites with copper indium gallium selenide (CIGS), have garnered considerable attention. This combination is particularly synergistic: CIGS serves as an ideal narrow-bandgap bottom cell (~1.1 eV) with proven stability and flexibility, while perovskites offer a tunable wide bandgap (WBG) top cell.

To achieve optimal spectral matching and exceed the Shockley−Queisser limit of single-junction devices, the perovskite top cell requires a wide bandgap (>1.67 eV), which is obtained by increasing the bromide/iodide ratio in the mixed-halide composition. However, the fabrication of high-quality WBG perovskite films, particularly via scalable methods like blade-coating in ambient air, remains a formidable bottleneck. The crystallization kinetics of mixed-halide perovskites are notoriously difficult to control. The rapid evaporation of solvents and the distinct solubility differences between bromide and iodide precursors often drive uncontrollable, rapid crystallization. This leads to severe phase segregation, where iodide-rich and bromide-rich domains form, creating energetic disorder. Furthermore, processing in ambient air introduces moisture, which can act as a nucleation site, further accelerating disordered precipitation. These issues manifest as films with high defect densities, poor coverage (pinholes), and significant non-radiative recombination, which severely compromise the open-circuit voltage (VOC) and fill factor (FF) of the final devices.

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LI Manya, JING Linjing, TAN Hairen (2026). Crystallization suppression of mixed-halide intermediates for perovskite/Cu(In,Ga)Se2 tandem solar cells with improved efficiency. SinoTechIntel Verified Research. https://doi.org/10.1088/1674-4926/26020045
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Frequently Asked Questions

What is the main challenge addressed in this research?

The main challenge is controlling the crystallization of mixed-halide wide-bandgap perovskite films, which often leads to phase segregation and defects, especially when fabricated via scalable methods like blade-coating in ambient air.

How does the proposed crystallization suppression strategy work?

The strategy replaces the traditional solvent N-methyl-2-pyrrolidone (NMP) with 2-pyrrolidinone (PDI). The stronger coordination of PDI with perovskite precursors modulates nucleation and growth, suppressing uncontrolled crystallization and phase segregation.

What are the benefits of using PDI instead of NMP?

Using PDI results in perovskite films with lower defect densities, better coverage, and reduced non-radiative recombination, leading to improved open-circuit voltage and fill factor in tandem solar cells.

Is this method compatible with industrial-scale production?

Yes, the method is compatible with scalable blade-coating in ambient air, making it promising for commercial manufacturing of flexible tandem solar cells.

What is the significance of this work for the field?

This work provides a simple yet effective solvent engineering approach to overcome a key bottleneck in perovskite/CIGS tandem solar cells, potentially accelerating their deployment in lightweight and flexible photovoltaic applications.

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