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Elucidating the Origins of Subgap Tail States and Open-Circuit Voltage in Methylammonium Lead Triiodide Perovskite Solar Cells

Tian Du, Jinhyun Kim, Jonathan Ngiam, Shengda Xu, Piers R. F. Barnes, James Durrant Orcid Logo, Martyn A. McLachlan

Advanced Functional Materials, Volume: 28, Issue: 32, Start page: 1801808

Swansea University Author: James Durrant Orcid Logo

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DOI (Published version): 10.1002/adfm.201801808

Abstract

Recombination via subgap trap states is considered a limiting factor in the development of organometal halide perovskite solar cells. Here, the impact of active layer crystallinity on the accumulated charge and open‐circuit voltage (Voc) in solar cells based on methylammonium lead triiodide (CH3NH3P...

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Published in: Advanced Functional Materials
ISSN: 1616-301X
Published: 2018
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URI: https://cronfa.swan.ac.uk/Record/cronfa43500
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Abstract: Recombination via subgap trap states is considered a limiting factor in the development of organometal halide perovskite solar cells. Here, the impact of active layer crystallinity on the accumulated charge and open‐circuit voltage (Voc) in solar cells based on methylammonium lead triiodide (CH3NH3PbI3, MAPI) is demonstrated. It is shown that MAPI crystallinity can be systematically tailored by modulating the stoichiometry of the precursor mix, where small quantities of excess methylammonium iodide (MAI) improve crystallinity, increasing device Voc by ≈200 mV. Using in situ differential charging and transient photovoltage measurements, charge density and charge carrier recombination lifetime are determined under operational conditions. Increased Voc is correlated to improved active layer crystallinity and a reduction in the density of trap states in MAPI. Photoluminescence spectroscopy shows that an increase in trap state density correlates with faster carrier trapping and more nonradiative recombination pathways. Fundamental insights into the origin of Voc in perovskite photovoltaics are provided and it is demonstrated why highly crystalline perovskite films are paramount for high‐performance devices.
Keywords: crystallinity, open‐circuit voltage, perovskite solar cells, tail states
College: Faculty of Science and Engineering
Issue: 32
Start Page: 1801808