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The balancing act between high electronic and low ionic transport influenced by perovskite grain boundaries

Lookup NU author(s): Dr Nathan Hill

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This work is licensed under a Creative Commons Attribution 4.0 International License (CC BY 4.0).

Abstract

© 2024 The Royal Society of Chemistry.A better understanding of the materials' fundamental physical processes is necessary to push hybrid perovskite photovoltaic devices towards their theoretical limits. The role of the perovskite grain boundaries is essential to optimise the system thoroughly. The influence of the perovskite grain size and crystal orientation on physical properties and their resulting photovoltaic performance is examined. We develop a novel, straightforward synthesis approach that yields crystals of a similar size but allows the tuning of their orientation to either the (200) or (002) facet alignment parallel to the substrate by manipulating dimethyl sulfoxide (DMSO) and tetrahydrothiophene-1-oxide (THTO) ratios. This decouples crystal orientation from grain size, allowing the study of charge carrier mobility, found to be improved with larger grain sizes, highlighting the importance of minimising crystal disorder to achieve efficient devices. However, devices incorporating crystals with the (200) facet exhibit an s-shape in the current density-voltage curve when standard scan rates are used, which typically signals an energetic interfacial barrier. Using the drift-diffusion simulations, we attribute this to slower-moving ions (mobility of 0.37 × 10-10 cm2 V-1 s-1) in combination with a lower density of mobile ions. This counterintuitive result highlights that reducing ion migration does not necessarily minimise hysteresis.

Publication metadata

Author(s): Gluck N, Hill NS, Giza M, Hutter E, Grill I, Schlipf J, Bach U, Muller-Buschbaum P, Hartschuh A, Bein T, Savenije T, Docampo P

Publication type: Article

Publication status: Published

Journal: Journal of Materials Chemistry A

Year: 2024

Pages: epub ahead of print

Online publication date: 21/03/2024

Acceptance date: 16/03/2024

Date deposited: 30/04/2024

ISSN (print): 2050-7488

ISSN (electronic): 2050-7496

Publisher: Royal Society of Chemistry

URL: https://doi.org/10.1039/D3TA04458K

DOI: 10.1039/d3ta04458k

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