Xu, Weidong;
Hart, Lucy JF;
Moss, Benjamin;
Caprioglio, Pietro;
Macdonald, Thomas J;
Furlan, Francesco;
Panidi, Julianna;
... Durrant, James R; + view all
(2023)
Impact of Interface Energetic Alignment and Mobile Ions on Charge Carrier Accumulation and Extraction in p-i-n Perovskite Solar Cells.
Advanced Energy Materials
, 13
(36)
, Article 2301102. 10.1002/aenm.202301102.
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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.
| Type: | Article |
|---|---|
| Title: | Impact of Interface Energetic Alignment and Mobile Ions on Charge Carrier Accumulation and Extraction in p-i-n Perovskite Solar Cells |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1002/aenm.202301102 |
| Publisher version: | https://doi.org/10.1002/aenm.202301102 |
| Language: | English |
| Additional information: | Copyright © 2023 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution License, https://creativecommons.org/licenses/by/4.0/, which permits use, distribution and reproduction in any medium, provided the original work is properly cited. |
| Keywords: | Charge accumulation, charge extraction, drift-diffusion simulation, ion migration, operando photoluminescence spectroscopy, perovskite solar cells, quasi-Fermi level splitting |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Electronic and Electrical Eng |
| URI: | https://discovery-pp.ucl.ac.uk/id/eprint/10203302 |
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