Tailoring Molecular-Scale Contact at the Perovskite/Polymeric Hole-Transporting Material Interface for Efficient Solar Cells

Jiaonan Sun, Ke Ma, Zih Yu Lin, Yuanhao Tang, Dharini Varadharajan, Alexander X. Chen, Harindi R. Atapattu, Yoon Ho Lee, Ke Chen, Bryan W. Boudouris, Kenneth R. Graham, Darren J. Lipomi, Jianguo Mei, Brett M. Savoie, Letian Dou

Research output: Contribution to journalArticlepeer-review

1 Scopus citations


Perovskite solar cells (PSCs) have delivered a power conversion efficiency (PCE) of more than 25% and incorporating polymers as hole-transporting layers (HTLs) can further enhance the stability of devices toward the goal of commercialization. Among the various polymeric hole-transporting materials, poly(triaryl amine) (PTAA) is one of the promising HTL candidates with good stability; however, the hydrophobicity of PTAA causes problematic interfacial contact with the perovskite, limiting the device performance. Using molecular side-chain engineering, a uniform 2D perovskite interlayer with conjugated ligands, between 3D perovskites and PTAA is successfully constructed. Further, employing conjugated ligands as cohesive elements, perovskite/PTAA interfacial adhesion is significantly improved. As a result, the thin and lateral extended 2D/3D heterostructure enables as-fabricated PTAA-based PSCs to achieve a PCE of 23.7%, improved from the 18% of reference devices. Owing to the increased ion-migration energy barrier and conformal 2D coating, unencapsulated devices with the new ligands exhibit both superior thermal stability under 60 °C heating and moisture stability in ambient conditions.

Original languageEnglish
Article number2300647
JournalAdvanced Materials
Issue number26
StatePublished - Jun 28 2023

Bibliographical note

Funding Information:
This material was based upon work supported by the U.S. Department of Energy's Office of Energy Efficiency and Renewable Energy (EERE) under the Solar Energy Technologies Office Award DE‐EE0009519. K.M. acknowledges the financial support from Lillian Gilbreth Postdoctoral Fellowships. D.J.L. acknowledges funding from the Air Force Office of Scientific Research (AFOSR) for supporting the adhesion measurements under award no. FA9550‐22‐1‐0454. H.R.A. and K.R.G. acknowledge funding from the Office of Science of the U.S. Department of Energy for supporting the UPS and XPS measurements under award no. DE‐SC0018208. The views expressed herein do not necessarily represent the views of the U.S. Department of Energy or the United States Government.

Publisher Copyright:
© 2023 The Authors. Advanced Materials published by Wiley-VCH GmbH.


  • 2D/3D heterostructures
  • PTAA
  • interface engineering
  • perovskite solar cells

ASJC Scopus subject areas

  • Materials Science (all)
  • Mechanics of Materials
  • Mechanical Engineering


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