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Abstract:

Vacuum-based deposition is a scalable, solvent-free industrial method ideal for uniform coatings on complex substrates. However, all vacuum-deposited perovskite solar cells fabricated by thermal evaporation trail solution-processed counterparts in efficiency and stability due to film quality challenges, necessitating advancement and improved understanding. Here, we report a co-evaporation route for 1.67-eV wide-bandgap perovskites by introducing a PbCl2 co-source to optimize film quality. We promote perovskite formation with pronounced (100) “face-up” orientation and deliver a certified all vacuum-deposited solar cell with 18.35% efficiency (19.3% in the lab) for 0.25-cm2 devices (18.5% for 1-cm2 cells). These cells retain 80% of peak efficiency after 1,080 hours under the ISOS-L-2 protocol. Leveraging operando hyperspectral imaging, we provide spatiotemporal spectral insight into halide segregation and trap-mediated recombination, correlating microscopic luminescence features with macroscopic device performance while distinguishing radiative from non-ideal recombination channels. We further demonstrate 27.2%-efficient 1-cm2 evaporated perovskite-on-silicon tandems and outdoor stability of all vacuum-deposited tandems in Italy, retaining ~80% initial performance after 8 months.

Abstract:

Performance losses in positive–intrinsic–negative architecture perovskite solar cells are dominated by nonradiative recombination at the perovskite/organic electron transport layer interface, which is particularly problematic for wider bandgap perovskites. Large endeavours have been dedicated to the replacement of fullerenes, which are the most commonly used class of electron transport layers, with limited success thus far. In this work, we demonstrate blending the fullerene derivatives [6,6]-phenyl C61 butyric acid methyl ester (PCBM) and indene-C60 bis-adduct (ICBA) as a thin interlayer between 1.77 eV bandgap perovskite and an evaporated C60 layer. By tuning the fullerene blend to a trace 2% by mass of PCBM in ICBA, we remarkably form an interlayer which features improved energetic alignment with the perovskite and the PCBM : ICBA fullerene mixture, together with a stronger molecular ordering and an order of magnitude higher electron mobility than either neat PCBM or ICBA. Additional molecular surface passivation approaches are found to be beneficial in conjunction with this approach, resulting in devices with 19.5% steady state efficiency, a fill factor of 0.85 and an open-circuit voltage of 1.33 V, which is within 10% of the radiative limit of the latter two device parameters for this bandgap. This work highlights the complex nonlinear energetic behaviour with fullerene mixing, and how control of the energetics and crystallinity of these materials is crucial in overcoming the detrimental recombination losses that have historically limited perovskite solar cells.

Abstract:

Improved understanding of heterojunction interfaces has enabled multijunction photovoltaic devices to achieve power conversion efficiencies that exceed the detailed-balance limit for single-junctions. For wide-bandgap perovskites, however, the pronounced energy loss across the heterojunctions of the active and charge transport layers impedes multijunction devices from reaching their full efficiency potential. Here we find that for polycrystalline perovskite films with mixed-halide compositions, the crystal termination—a factor influencing the reactivity and density of surface sites—plays a crucial role in interfacial passivation for wide-bandgap perovskites. We demonstrate that by templating the growth of polycrystalline perovskite films toward a preferred (100) facet, we can reduce the density of deep-level trap states and enhance the binding of modification ligands. This leads to a much-improved heterojunction interface, resulting in open-circuit voltages of 1.38 V for 1.77-eV single-junction perovskite solar cells. In addition, monolithic all-perovskite double-junction solar cells achieve open-circuit voltage values of up to 2.22 V, with maximum power point tracking efficiencies reaching 28.6% and 27.7% at 0.25 and 1.0 cm2 cell areas, respectively, along with improved operational and thermal stability at 85 °C. This work provides universally applicable insights into the crystalline facet-favourable surface modification of perovskite films, advancing their performance in optoelectronic applications.

Abstract:

Halide perovskite solar cells are approaching commercialization, with solution processing emerging as a key method for large‐scale production. This study introduces a significant advancement: using non‐toxic solvents like water and alcohol in perovskite precursor inks facilitated by the protic ionic liquid methylammonium propionate (MAP). MAP effectively dissolves perovskite precursors such as lead acetate and methylammonium iodide, enabling the first stable water‐based perovskite precursor ink suitable for one‐step slot‐die coating. This new ink formulation contrasts with conventional dimethylformamide (DMF) and dimethylsulfoxide (DMSO)‐based inks, as evidenced by in‐situ grazing incidence wide‐angle X‐ray scattering (GIWAXS), which revealed an intermediate‐free liquid‐to‐solid transition. In‐situ mass spectrometry also showed that organic molecules evaporate during annealing, resulting in a crystalline perovskite phase. Optimization of the solvent mixture to H2O/IPA/MAP enabled successful slot‐die coating, yielding perovskite solar cells with an efficiency of up to 10%. This eco‐friendly ink reduces toxicity and environmental impact compared to DMF‐based inks, offering a longer shelf life and the possibility of using the ink in ambient conditions. This pioneering work represents the first report of a water‐based green ink formulation for one‐step thin film coating at room‐temperature conditions by slot‐die coating, highlighting its potential for sustainable commercial applications.

Abstract:

The efficiency and longevity of metal-halide perovskite solar cells are typically dictated by nonradiative defect-mediated charge recombination. In this work, we demonstrate a vapor-based amino-silane passivation that reduces photovoltage deficits to around 100 millivolts (>90% of the thermodynamic limit) in perovskite solar cells of bandgaps between 1.6 and 1.8 electron volts, which is crucial for tandem applications. A primary-, secondary-, or tertiary-amino–silane alone negatively or barely affected perovskite crystallinity and charge transport, but amino-silanes that incorporate primary and secondary amines yield up to a 60-fold increase in photoluminescence quantum yield and preserve long-range conduction. Amino-silane–treated devices retained 95% power conversion efficiency for more than 1500 hours under full-spectrum sunlight at 85°C and open-circuit conditions in ambient air with a relative humidity of 50 to 60%.