Visualizing macroscopic inhomogeneities in perovskite solar cells

University of Oxford (2022)

Authors:

Akash Dasgupta, Suhas Mahesh, Pietro Caprioglio, Yen-Hung Lin, Karl-Augustin Zaininger, Robert DJ Oliver, Philippe Holzhey, Suer Zhou, Melissa McCarthy, Joel Smith, Maximilian Frenzel, M Greyson Christoforo, James Ball, Bernard Wenger, Henry J Snaith

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.

Understanding and suppressing non-radiative losses in methylammonium-free wide-bandgap perovskite solar cells

Energy and Environmental Science Royal Society of Chemistry 15 (2021) 714-726

Authors:

Robert DJ Oliver, Pietro Caprioglio, Francisco Peña-Camargo, Leonardo Buizza, Fengshuo Zu, Alexandra J Ramadan, Silvia Motti, Suhas Mahesh, Melissa McCarthy, Jonathan H Warby, Yen-Hung Lin, Norbert Koch, Steve Albrecht, Laura M Herz, Michael B Johnston, Dieter Neher, Martin Stolterfoht, Henry Snaith

Abstract:

With power conversion efficiencies of perovskite-on-silicon and all-perovskite tandem solar cells increasing at rapid pace, wide bandgap (> 1.7 eV) metal-halide perovskites (MHPs) are becoming a major focus of academic and industrial photovoltaic research. Compared to their lower bandgap (< 1.6 eV) counterparts, these types of perovskites suffer from higher levels of non-radiative losses in both the bulk material and in device configurations, constraining their efficiencies far below their thermodynamic potential. In this work, we investigate the energy losses in methylammonium (MA) free high-Br-content widegap perovskites by using a combination of THz spectroscopy, steady-state and time-resolved photoluminescence, coupled with drift-diffusion simulations. The investigation of this system allows us to study charge-carrier recombination in these materials and devices in the absence of halide segregation due to the photostabilty of formamidinium-cesium based lead halide perovskites. We find that these perovskites are characterised by large non-radiative recombination losses in the bulk material and that the interfaces with transport layers in solar cell devices strongly limit their open-circuit voltage. In particular, we discover that the interface with the hole transport layer performs particularly poorly, in contrast to 1.6 eV bandgap MHPs which are generally limited by the interface with the electron-transport layer. To overcome these losses, we incorporate and investigate the recombination mechanisms present with perovskites treated with the ionic additive 1-butyl-1-methylpipiderinium tetrafluoroborate. We find that this additive not only improves the radiative efficiency of the bulk perovskite, but also reduces the non-radiative recombination at both the hole and electron transport layer interfaces of full photovoltaic devices. In addition to unravelling the beneficial effect of this specific treatment, we further optimise our solar cells by introducing an additional LiF interface treatment at the electron transport layer interface. Together these treatments enable MA-free 1.79 eV bandgap perovskite solar cells with open-circuit voltages of 1.22 V and power conversion efficiencies approaching 17 %, which is among the highest reported for this material system.

The application of one-dimensional nanostructures in terahertz frequency devices

Applied Physics Reviews AIP Publishing 8:4 (2021) 041314

Authors:

Kun Peng, Michael B Johnston

Phase segregation in mixed-halide perovskites affects charge-carrier dynamics while preserving mobility

Nature Communications Springer Nature 12 (2021) 6955

Authors:

Silvia G Motti, Jay B Patel, Robert DJ Oliver, Henry J Snaith, Michael B Johnston, Laura M Herz

Abstract:

Mixed halide perovskites can provide optimal bandgaps for tandem solar cells which are key to improved cost-efficiencies, but can still suffer from detrimental illumination-induced phase segregation. Here we employ optical-pump terahertz-probe spectroscopy to investigate the impact of halide segregation on the charge-carrier dynamics and transport properties of mixed halide perovskite films. We reveal that, surprisingly, halide segregation results in negligible impact to the THz charge-carrier mobilities, and that charge carriers within the I-rich phase are not strongly localised. We further demonstrate enhanced lattice anharmonicity in the segregated I-rich domains, which is likely to support ionic migration. These phonon anharmonicity effects also serve as evidence of a remarkably fast, picosecond charge funnelling into the narrow-bandgap I-rich domains. Our analysis demonstrates how minimal structural transformations during phase segregation have a dramatic effect on the charge-carrier dynamics as a result of charge funnelling. We suggest that because such enhanced recombination is radiative, performance losses may be mitigated by deployment of careful light management strategies in solar cells.

Interplay of structure, charge-carrier localization and dynamics in copper-silver-bismuth-halide semiconductors

Advanced Functional Materials Wiley 32:6 (2021) 2108392

Authors:

Leonardo RV Buizza, Harry C Sansom, Adam D Wright, Aleksander M Ulatowski, Michael B Johnston, Laura M Herz, Henry J Snaith

Abstract:

Silver-bismuth based semiconductors represent a promising new class of materials for optoelectronic applications because of their high stability, all-inorganic composition, and advantageous optoelectronic properties. In this study, charge-carrier dynamics and transport properties are investigated across five compositions along the AgBiI4–CuI solid solution line (stoichiometry Cu4x(AgBi)1−xI4). The presence of a close-packed iodide sublattice is found to provide a good backbone for general semiconducting properties across all of these materials, whose optoelectronic properties are found to improve markedly with increasing copper content, which enhances photoluminescence intensity and charge-carrier transport. Photoluminescence and photoexcitation-energy-dependent terahertz photoconductivity measurements reveal that this enhanced charge-carrier transport derives from reduced cation disorder and improved electronic connectivity owing to the presence of Cu+. Further, increased Cu+ content enhances the band curvature around the valence band maximum, resulting in lower charge-carrier effective masses, reduced exciton binding energies, and higher mobilities. Finally, ultrafast charge-carrier localization is observed upon pulsed photoexcitation across all compositions investigated, lowering the charge-carrier mobility and leading to Langevin-like bimolecular recombination. This process is concluded to be intrinsically linked to the presence of silver and bismuth, and strategies to tailor or mitigate the effect are proposed and discussed.