Snaith group

Abstract:

We show that the use of 1,3-diaminopropane (DAP) as a chemical modifier at the perovskite/electron-transport layer (ETL) interface enhances the power conversion efficiency (PCE) of 1.7 eV band gap mixed-halide perovskite containing formamidinium and Cs single-junction cells, primarily by increasing the open-circuit voltage (<i>V</i>_OC) from 1.06 to 1.15 V. We find that adding a postprocessing annealing step after C60 evaporation further improves device performance. Specifically, the fill factor (FF) increases by 20% in the DAP + postannealing devices compared to the control. Using hyperspectral photoluminescence microscopy, we demonstrate that annealing helps improve compositional homogeneity at the electron-transport layer (ETL) and hole-transport layer (HTL) interfaces of the solar cell, which prevents detrimental band gap pinning in the devices and improves C₆₀ adhesion. Using time-of-flight secondary ion mass spectrometry, we show that DAP reacts with formamidinium (FA⁺) present at the surface of the perovskite structure to form a larger molecular cation, 1,4,5,6-tetrahydropyrimidinium (THP⁺), which remains at the interface. Combining the use of DAP and annealing the C₆₀ interface, we fabricate Si-perovskite tandems with a PCE of 25.29%, compared to 23.26% for control devices. Our study underscores the critical role of the chemical reactivity of diamines at the surface and the thermal postprocessing of the C₆₀/Lewis-base passivator interface in minimizing device losses and enhancing solar-cell performance of wide-band-gap mixed-cation mixed-halide perovskites for tandem applications.

Abstract:

Perovskite solar cells achieve high power conversion efficiencies but usually rely on vacuum-deposited metallic contacts, leading to high material costs for noble metals and stability issues for more reactive metals. Carbon-based materials offer a cost-effective and potentially more stable alternative. The vast majority of carbon-electrode PSCs use the negative-intrinsic-positive (n-i-p) or "hole-transport-layer-free" architectures. Here, we present a systematic study to assess the compatibility of "inverted", p-i-n configuration PSC contact layers with carbon top electrodes. We identify incompatibilities between common electron transport layers and the carbon electrode deposition process and previously unobserved semiconducting properties in carbon electrodes with unique implications for charge extraction and electronic behavior. To overcome these issues, we introduce a double-layer atomic layer deposited tin oxide (SnO₂) and Poly-(2,3-dihydrothieno-1,4-dioxin)-poly-(styrenesulfonate) (PEDOT:PSS), yielding up to 16.1% PCE and a retained 94% performance after 500 h of outdoor aging. The study is a crucial step forward for printable, metal-electrode-free, and evaporation-free perovskite PV technologies.

Abstract:

We show that the use of 1,3-diaminopropane (DAP) as a chemical modifier at the perovskite/electron-transport layer (ETL) interface enhances the power conversion efficiency (PCE) of 1.7 eV band gap mixed-halide perovskite containing formamidinium and Cs single-junction cells, primarily by increasing the open-circuit voltage (V_OC) from 1.06 to 1.15 V. We find that adding a postprocessing annealing step after C60 evaporation further improves device performance. Specifically, the fill factor (FF) increases by 20% in the DAP + postannealing devices compared to the control. Using hyperspectral photoluminescence microscopy, we demonstrate that annealing helps improve compositional homogeneity at the electron-transport layer (ETL) and hole-transport layer (HTL) interfaces of the solar cell, which prevents detrimental band gap pinning in the devices and improves C₆₀ adhesion. Using time-of-flight secondary ion mass spectrometry, we show that DAP reacts with formamidinium (FA⁺) present at the surface of the perovskite structure to form a larger molecular cation, 1,4,5,6-tetrahydropyrimidinium (THP⁺), which remains at the interface. Combining the use of DAP and annealing the C₆₀ interface, we fabricate Si-perovskite tandems with a PCE of 25.29%, compared to 23.26% for control devices. Our study underscores the critical role of the chemical reactivity of diamines at the surface and the thermal postprocessing of the C₆₀/Lewis-base passivator interface in minimizing device losses and enhancing solar-cell performance of wide-band-gap mixed-cation mixed-halide perovskites for tandem applications.

Abstract:

Transparent conductive films are key components of many optoelectronic devices but are often made from either scarce or brittle materials like indium tin oxide. Carbon nanotube-polymer films offer an abundant and flexible alternative. Here, we report how the dimensions of the carbon nanotube raw material affect their thin film performance and thickness yield when processed with the polymer ethylene-vinyl acetate. We perform chemical doping with several halogenated metals and find the electron affinity of the metal to be a good indicator of p-doping effectiveness. We identify CuCl₂ as low-cost alternative to the established gold chloride dopants. Optimising the dopant deposition method allows us to reduce the effect of doping on the optical transmittance. Percolation analysis of our films demonstrates that optimized single-walled carbon nanotube-ethylene-vinyl acetate films show no sign of percolation effects down to thicknesses of 5 nm. Finally, we produce transparent touch-sensitive devices. Comparing several of these devices, we find a linear relationship between the sheet resistance and the on/off ratio of the touch sensing that can be used to determine a threshold film thickness. Using doped carbon nanotube-ethylene-vinyl acetate films increases the on/off ratio and allows us to fabricate touch-sensitive devices with an on/off ratio of 10 at 95% optical transmittance. This clearly demonstrates the potential of these films for transparent touch-sensitive applications.