Deposition-Dependent Coverage and Performance of Phosphonic Acid Interface Modifiers in Halide Perovskite Optoelectronics

Contreras, Hannah; O’Brien, Aidan; Taddei, Margherita; Shi, Yangwei; Jiang, Fangyuan; Westbrook, Robert J. E.; Zhang, Yadong; Juarez, Julisa; Giridharagopal, Rajiv; Lee, Paul A.; Barlow, Stephen; Marder, Seth R.; Armstrong, Neal R.; Ginger, David S.

doi:10.1021/acsami.5c12684

Title: Deposition-Dependent Coverage and Performance of Phosphonic Acid Interface Modifiers in Halide Perovskite Optoelectronics

Journal Article · Wed Nov 26 00:00:00 UTC 2025 · ACS Applied Materials and Interfaces

DOI: https://doi.org/10.1021/acsami.5c12684 · OSTI ID:3029082

^[1]; O’Brien, Aidan ^[1];

^[1];

^[1]; Westbrook, Robert J. E. ^[1]; Zhang, Yadong ^[2]; Juarez, Julisa ^[1];

^[1]; Lee, Paul A. ^[3];

^[2]; Marder, Seth R. ^[2];

^[3];

^[1]

University of Washington, Seattle, WA (United States)
University of Colorado-Boulder, CO (United States)
University of Arizona, Tucson, AZ (United States)

In this work, we study the effect of various deposition methods for phosphonic acid interface modifiers commonly pursued as self-assembled monolayers in high-performance metal halide perovskite photovoltaics and light-emitting diodes. We compare the deposition of (2-(3,6-diiodo-9H-carbazol-9-yl)ethyl)phosphonic acid onto indium tin oxide (ITO) bottom contacts by varying three parameters: the method of deposition, specifically spin coating or prolonged dip coating; ITO surface treatment via HCl/FeCl3 etching; and use in combination with a second modifier, 1,6-hexylenediphosphonic acid. We demonstrate that varying these modification protocols can impact time-resolved photoluminescence carrier lifetimes and quasi-Fermi level splitting of perovskite films deposited onto the phosphonic acid-modified ITO. Ultraviolet photoelectron spectroscopy shows an increase in the effective work function after phosphonic acid modification and clear evidence for photoemission from carbazole functional groups at the ITO surface. We used X-ray photoelectron spectroscopy to probe differences in phosphonic acid coverage on the metal oxide contact and show that perovskite samples grown on ITO with the highest phosphonic acid coverage exhibit the longest carrier lifetimes. Finally, we establish that device performance follows these same trends. These results indicate that the reactivity, heterogeneity, and composition of the bottom contact help to control recombination rates and therefore power conversion efficiencies. ITO etching, prolonged deposition times for phosphonic acids via dip coating, and the use of a secondary, more hydrophilic bisphosphonic acid all contribute to improvements in surface coverage, carrier lifetime, and device efficiency. Furthermore, these improvements each have a positive impact, and we achieve the best results when all three strategies are implemented.

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Research Organization:: University of Washington, Seattle, WA (United States)

Sponsoring Organization:: National Science Foundation Graduate Research Fellowship; Office of Naval Research (ONR); USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: EE0010502; SC0001084; SC0013957

OSTI ID:: 3029082

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 49 Vol. 17; ISSN 1944-8244; ISSN 1944-8252

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Deposition-Dependent Coverage and Performance of Phosphonic Acid Interface Modifiers in Halide Perovskite Optoelectronics

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