Akash Dasgupta

Abstract:

This contains all data used in the paper: ACS Energy Lett. 2022, 7, 7, 2311–2322, DOI: https://doi.org/10.1021/acsenergylett.2c01094. Data has been sorted into raw and processed, and organised by which figure they appear in. Arrays require Python and the numpy package to load (np.load('filename.npy')). All other data is in text format of some form, easily openable. Some plots require Origin labs to open, but no data in these files are inaccessible from the txt files/ csvs etc.

Abstract:

Abstract Studying real-time degradation in perovskite semiconductors remains an important challenge. Conventional methods often cannot separate interfacial and bulk processes or rely on destructive analysis. Here, we demonstrate multiwavelength excitation photoluminescence (PL) as a nondestructive approach to distinguish interface- and bulk-dominated recombination losses. Using phenethylammonium tetrafluoroborate (PEABF4) treatment as a model, we use PL to show that PEABF4 passivates the electron transport layer (ETL)/perovskite interface, reducing interfacial recombination losses from fullerene deposition. However, upon thermal aging, PEABF4-treated stacks degrade more rapidly, with recombination losses broadening from the ETL/perovskite interface into the absorber. Diffusion–recombination simulations support interpreting excitation-wavelength-dependent PL decay signatures consistent with changes in surface recombination velocity and bulk lifetime, providing a framework for depth-sensitive comparisons during aging. Collectively, these results further establish multiwavelength excitation PL as a platform for studying recombination losses during aging of perovskite films.

Abstract:

We investigate the impact of employing fullerene self-assembled monolayers (SAMs) in conjunction with SnO2 electron-transport layers (ETLs) in negative–intrinsic–positive (n–i–p) perovskite solar cells. We compare the efficacy of the fullerene-SAM surface-binding group—carboxylic or phosphonic acid—on the passivation, charge transport, and energetics of the modified-SnO2 surface. Planar n–i–p perovskite solar cells with these SAM-modified SnO2 exhibit significantly reduced hysteresis, and the steady-state maximum power point tracked efficiencies (η MPP) of the devices improved from an average of 18.6–20.0% comparing devices with neat SnO2 to the C60-PA SAM inclusion, respectively. While C60-PA SAM improved the initial solar cell efficiency, this benefit was not maintained during light exposure at elevated temperatures as the fullerene SAM weakened adhesion at the perovskite/metal oxide interface in the aged devices. These results highlight the importance of improving the mechanical robustness of perovskite/charge-transport layer interfaces under operational aging conditions.

Abstract:

Perovskite inks play critical roles in determining film quality and device performance, and ink stability is desired to ensure high device reproducibility. Here, we reveal the instability issue of current cesium-formamidinium lead triiodide (CsxFA1-xPbI3) inks whose aggregation and precipitation tendencies are induced by excessively strong solvent-lead-halide coordination. By modulating coordination strength between precursor salts and solvents, we identify solvent coordination-dispersion equilibrium as the governing factor for ink stability and develop a stable ink that exhibits a remarkable increase in the shelf life. It effectively tunes ink drying and film crystallization, resulting in blade-coated perovskite films with excellent uniformity and low defect density. This enhancement led to increased aperture efficiency of ambient-fabricated p-i-n perovskite modules to 23.5%. The resultant devices also exhibit high durability, and 99% of the initial PCE was retained after 1700 hours of maximum power point tracking following the ISOS-L-2 standard protocol.

Abstract:

Raw data and derived dielectric constants (*n*, *k*, α) for neat Pb and mixed PbSn perovskite compositions