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Impact of Interface Energetic Alignment and Mobile Ions on Charge Carrier Accumulation and Extraction in p‐i‐n Perovskite Solar Cells
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Lucy J. F. Hart ,
Benjamin Moss,
Pietro Caprioglio,
Thomas J. Macdonald,
Francesco Furlan,
Julianna Panidi,
Robert D. J. Oliver,
Richard A. Pacalaj,
Martin Heeney,
Nicola Gasparini,
Henry J. Snaith,
Piers R. F. Barnes,
James Durrant
Advanced Energy Materials, Volume: 13, Issue: 36
Swansea University Author:
James Durrant
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© 2023 The Authors. This is an open access article under the terms of the Creative Commons Attribution License.
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DOI (Published version): 10.1002/aenm.202301102
Abstract
Understanding the kinetic competition between charge extraction and recombination, and how this is impacted by mobile ions, remains a key challenge in perovskite solar cells (PSCs). Here, this issue is addressed by combining operando photoluminescence (PL) measurements, which allow the measurement o...
| Published in: | Advanced Energy Materials |
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| ISSN: | 1614-6832 1614-6840 |
| Published: |
Wiley
2023
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| Online Access: |
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| URI: | https://cronfa.swan.ac.uk/Record/cronfa64065 |
| Abstract: |
Understanding the kinetic competition between charge extraction and recombination, and how this is impacted by mobile ions, remains a key challenge in perovskite solar cells (PSCs). Here, this issue is addressed by combining operando photoluminescence (PL) measurements, which allow the measurement of real-time PL spectra during current–voltage (J–V) scans under 1-sun equivalent illumination, with the results of drift-diffusion simulations. This operando PL analysis allows direct comparison between the internal performance (recombination currents and quasi-Fermi-level-splitting (QFLS)) and the external performance (J–V) of a PSC during operation. Analyses of four PSCs with different electron transport materials (ETMs) quantify how a deeper ETM LUMO induces greater interfacial recombination, while a shallower LUMO impedes charge extraction. Furthermore, it is found that a low ETM mobility leads to charge accumulation in the perovskite under short-circuit conditions. However, thisalone cannot explain the remarkably high short-circuit QFLS of over 1 eV which is observed in all devices. Instead, drift-diffusion simulations allow this effect to be assigned to the presence of mobile ions which screen the internal electric field at short-circuit and lead to a reduction in the short-circuit current density by over 2 mA cm−2 in the best device. |
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| Keywords: |
Charge accumulation, charge extraction, drift-diffusion simulation, ion migration, operando photoluminescence spectroscopy, perovskite solar cells, quasi-Fermi level splitting |
| College: |
Faculty of Science and Engineering |
| Funders: |
EPSRC, Korean NRF GRL, European Commission Research Executive Agency, Royal Society University Research Fellowship, Royal Society Research Fellows Enhanced Research Expenses; EP/T028513/1, EP/L016702/1, EP/V057839/1, EP/T012455/1, 2017K1A1A2013153, 859752 HEL4CHIR-OLED H2020-MSCA-ITN-2019, URF/R1/221834, RF/ERE/221066 |
| Issue: |
36 |