Westbrook, RJE;
Xu, W;
Liang, X;
Webb, T;
Clarke, TM;
Haque, SA;
(2021)
2D Phase Purity Determines Charge-Transfer Yield at 3D/2D Lead Halide Perovskite Heterojunctions.
Journal of Physical Chemistry Letters
, 12
(13)
pp. 3312-3320.
10.1021/acs.jpclett.1c00362.
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Abstract
Targeted functionalization of 3D perovskite with a 2D passivation layer via R-NH3I treatment has emerged as an effective strategy for enhancing both the efficiency and chemical stability of ABX3 perovskite solar cells, but the underlying mechanisms behind these improvements remain unclear. Here, we assign a passivation mechanism where R-NH3I reacts with excess PbI2 in the MAPbI3 film and unsaturated PbI6 octahedra to form (R-NH3)2(MA)n–1PbnI3n+1. Crucially, we show that precise control of the 2D (R-NH3)2(MA)n–1PbnI3n+1 layer underpins performance improvements: n = 1 yields over a 2-fold improvement in hole injection to the HTL; n > 1 deteriorates hole injection. Ultrafast transient absorption spectroscopy suggests this n-dependence is rooted in the fact that fast (<6 ns) hole injection does not occur between the 3D and 2D layers. These results help explain contemporary empirical findings in the field and set out an important design rule for the further optimization of multidimensional perovskite optoelectronics.
Type: | Article |
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Title: | 2D Phase Purity Determines Charge-Transfer Yield at 3D/2D Lead Halide Perovskite Heterojunctions |
Open access status: | An open access version is available from UCL Discovery |
DOI: | 10.1021/acs.jpclett.1c00362 |
Publisher version: | http://dx.doi.org/10.1021/acs.jpclett.1c00362 |
Language: | English |
Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
Keywords: | Materials Science, Physics, SOLAR-CELL, CARRIER DYNAMICS, PASSIVATION, EFFICIENT, PERFORMANCE, PHOTOLUMINESCENCE, TOLERANCE, TRANSPORT, FILMS, LIMIT |
UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
URI: | https://discovery-pp.ucl.ac.uk/id/eprint/10130623 |
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