Understanding the dopant induced effects on SFX-MeOTAD for perovskite solar cells: a spectroscopic and computational investigation

Fraser Gunn, Paheli Ghosh, Michal Maciejczyk, Joseph Cameron, Dennis Nordlund, Satheesh Krishnamurthy, Tell Tuttle, Peter Skabara, Neil Robertson, Aruna Ivaturi

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Abstract

SFX-MeOTAD [2,2′,7,7′-tetrakis(N,N-di(4-methoxyphenyl)amino)-spiro-(fluorene-9,9′-xanthene)] (also known as X60) has emerged as a cost-effective alternative to the ubiquitous, but excessively-expensive, spiro-MeOTAD hole transport material (HTM) in perovskite solar cells. Using its pre-oxidised dicationic salt, SFX-(TFSI)2, a controlled concentration dependent conductivity tuning of this HTM without the requirement of air (oxygen) exposure has been carried out. This study details the modifications in the optical and electrical properties of this low cost HTM as a function of the concentration of the dicationic salt (0-100 mol%) using UV-vis absorption and electrical conductivity measurements. X-ray absorption and photoelectron spectroscopy investigations have been carried out to elucidate the role of the dicationic salt in the enhanced electronic properties of SFX-MeOTAD. By incorporating the dicationic SFX-(TFSI)2 it has been shown that the conductivity of SFX-MeOTAD increased by 4 orders of magnitude from 2.55 × 10-8 S cm-1 to 9.4 × 10-4 S cm-1 when using an optimal dopant concentration of 20.5 mol%. The degree of oxidation of SFX-MeOTAD was determined through UV-vis absorption and consolidated using the computational calculations. The XPS study reveals that doping SFX-MeOTAD with SFX(TFSI)2 not only results in the oxidation of the HTM but also leads to a variation in the local chemistry around carbon and nitrogen which directly influences the conductivity of the doped films. NEXAFS studies indicate that doping enhances the aromatic nature of the molecule initially but increasing the dopant concentration further affects the aromaticity and possibly the π stacking, similar to the trend seen in dopant concentration dependent conductivity of the SFX-MeOTAD films. These findings have implications on the choice of dopant concentration and counterions more generally for triarylamine based HTMs.

Original languageEnglish
Pages (from-to)16226-16239
Number of pages14
JournalJournal of Materials Chemistry C
Volume9
Issue number45
Early online date12 Oct 2021
DOIs
Publication statusPublished - 7 Dec 2021

Keywords

  • SFX-MeOTAD
  • doped films
  • perovskite solar cells
  • spiro-MeOTAD hole transport material (HTM)

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