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Lookup NU author(s): Miriam Fsadni, Dr Thomas PopeORCiD, Dr Ivan Shmarov, Professor Thomas Penfold, Dr Pablo Docampo
This work is licensed under a Creative Commons Attribution 4.0 International License (CC BY 4.0).
The importance of the hole-transport material (HTM) in perovskite solar cells (PSCs) is now very well-established, with state-of-the-art materials such as Spiro-OMeTAD attracting significant attention in the last decade. The high cost of such materials still limits the commercialisation of these HTMs. To tackle this, the amide linker has recently been introduced into HTM systems via EDOT-Amide-TPA, utilising condensation chemistry as a cheap and effective route to HTMs. EDOT-Amide-TPA is capable of a variety of intermolecular interactions such as dipole-dipole interactions and hydrogen bonding, both of which are beneficial for enhancing the film morphology and improving charge transport. However, the interplay between these different interactions is not trivial, and understanding how they affect each other is paramount to inform new HTM designs whilst minimising material waste. To date, studies investigating the combined effects of different intermolecular interactions within the HTL on the charge transport properties of these materials are lacking. Furthermore, dipole disorder within the film introduces a mobility ‘penalty’: mobility decreases with stronger overall dipole due to energetic disorder within the film, which hinders charge hopping. In this work, we investigate three amide-based HTM analogs with differing intermolecular interaction capabilities, and show that this penalty can be compensated by a preferentially increased dipole ordering, likely achieved through intermolecular hydrogen bonding. This effectively cancels out the dipole disorder while retaining the beneficial effects on the molecular packing. Our aim is that this work provides a good foundation for navigating the complex interplay between hydrogen bonding, dipole moments, conductivity, and film formation in small-molecule HTMs
Author(s): Vella B, Fsadni MH, Pope T, Giza M, Angus F, Shmarov I, Lalaguna PL, Cariello M, Wilson C, Kadodwala M, Penfold T, Docampo P, Cooke G
Publication type: Article
Publication status: Published
Journal: Journal of Materials Chemistry A
Year: 2024
Pages: epub ahead of print
Online publication date: 25/07/2024
Acceptance date: 25/07/2024
Date deposited: 31/07/2024
ISSN (print): 2050-7488
ISSN (electronic): 2050-7496
Publisher: Royal Society of Chemistry
URL: https://doi.org/10.1039/D4TA00956H
DOI: 10.1039/D4TA00956H
Data Access Statement: Crystal structures for the amide compounds in this study have been deposited into the CCDC. CCDC Deposition numbers are: EDOT-Amide-TPA (Compound 1): Deposition number 2301541, Unit cell parameters: a 55.7783(6) b 55.7783(6) c 10.4905(2) I41/a DEDOT-Amide-TPA (Compound 2): Deposition number 2301539, Unit cell parameters: a 16.6681(5) b 18.0603(6) c 16.6318(5) P21/c TPABT (Compound 3): Deposition number 2301540, Unit cell parameters: a 12.1294(3) b 14.8596(3) c 27.9555(8) P21/c. Other data supporting this article have been included as part of the ESI.
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