Sulfur‐Modulated Fully‐Conjugated Self‐Assembled Monolayers for Synergistic Dual‐Interface Optimization in Inverted Perovskite Solar Cells

S Song Yao Q Qianyu Su (State Key Laboratory of Flexible Electronics (LoFE) & Institute of Advanced Materials (IAM) School of Flexible Electronics (Future Technologies) Nanjing Tech University (NanjingTech) Nanjing China) S Shunan Sui (State Key Laboratory of Flexible Electronics (LoFE) & Institute of Advanced Materials (IAM) School of Flexible Electronics (Future Technologies) Nanjing Tech University (NanjingTech) Nanjing China) F Fei Du (Key Laboratory of Physics and Technology for Advanced Batteries (ministry of Education); State Key Laboratory of Superhard Materials, College of Physics) W Wenjian Yan P Pengli Cao (State Key Laboratory of Flexible Electronics (LoFE) & Institute of Advanced Materials (IAM) School of Flexible Electronics (Future Technologies) Nanjing Tech University (NanjingTech) Nanjing China) C Cheng Liang Z Zhengwu Pan (State Key Laboratory of Flexible Electronics (LoFE) & Institute of Advanced Materials (IAM) School of Flexible Electronics (Future Technologies) Nanjing Tech University (NanjingTech) Nanjing China) C Chengrong Yin (State Key Laboratory of Flexible Electronics (LoFE) & Institute of Advanced Materials (IAM) School of Flexible Electronics (Future Technologies) Nanjing Tech University (NanjingTech) Nanjing China) J Jingjin Dong (State Key Laboratory of Flexible Electronics (LoFE) & Institute of Advanced Materials (IAM) School of Flexible Electronics (Future Technologies) Nanjing Tech University (NanjingTech) Nanjing China) J Jiupeng Cao (State Key Laboratory of Flexible Electronics (LoFE) & Institute of Advanced Materials (IAM) School of Flexible Electronics (Future Technologies) Nanjing Tech University (NanjingTech) Nanjing China) W Wei Huang T Tianshi Qin

Abstract

ABSTRACT To achieve high efficiency and stability in inverted perovskite solar cells (PSCs), it is essential to ensure uniform self‐assembled monolayers (SAM) coverage on the substrate and to passivate defects effectively at the buried interface of perovskite. Herein, two sulfur‐modulated fully‐conjugated SAMs, 4‐(bis(4‐methylthiophenyl)amino)phenylphosphonic acid (SMe‐TPA‐PA) and 5‐(4‐bis(4‐methylthiophenyl)amino)phenyl) thiophenylphosphonic acid (SMe‐TPA‐ThPA) are developed for inverted PSCs by employing substituent regulation and linker adjustment. The incorporation of methylthio substituents in both SAMs enhances their defect‐passivation capability at the interface. Moreover, the thiophene linker in SMe‐TPA‐ThPA strengthens intermolecular interactions, improves energy level alignment with the perovskite, enables stable and uniform molecular coverage on ITO, and facilitates efficient hole extraction. As a result of synergistic dual‐interface modification of the ITO/perovskite system, inverted PSCs based on SMe‐TPA‐ThPA and SMe‐TPA‐PA achieve significantly improved power conversion efficiencies (PCEs) of 26.52% and 25.40%, respectively, surpassing the control device based on methoxyl‐substituted SAM (OMe‐TPA‐PA, 24.31%). Remarkably, devices incorporating SMe‐TPA‐ThPA also exhibit exceptional operational stability, retaining 91.8% of their initial PCE after 1700 h of continuous light soaking and 91.2% after 1700 h of continuous thermal aging at 65 °C.

Article Details

Volume / Issue Vol. 65, Issue 16
Published April 13, 2026
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (13)

S

Song Yao

Q

Qianyu Su

State Key Laboratory of Flexible Electronics (LoFE) & Institute of Advanced Materials (IAM) School of Flexible Electronics (Future Technologies) Nanjing Tech University (NanjingTech) Nanjing China

S

Shunan Sui

State Key Laboratory of Flexible Electronics (LoFE) & Institute of Advanced Materials (IAM) School of Flexible Electronics (Future Technologies) Nanjing Tech University (NanjingTech) Nanjing China

F

Fei Du

Key Laboratory of Physics and Technology for Advanced Batteries (ministry of Education); State Key Laboratory of Superhard Materials, College of Physics

W

Wenjian Yan

P

Pengli Cao

State Key Laboratory of Flexible Electronics (LoFE) & Institute of Advanced Materials (IAM) School of Flexible Electronics (Future Technologies) Nanjing Tech University (NanjingTech) Nanjing China

C

Cheng Liang

Z

Zhengwu Pan

State Key Laboratory of Flexible Electronics (LoFE) & Institute of Advanced Materials (IAM) School of Flexible Electronics (Future Technologies) Nanjing Tech University (NanjingTech) Nanjing China

C

Chengrong Yin

State Key Laboratory of Flexible Electronics (LoFE) & Institute of Advanced Materials (IAM) School of Flexible Electronics (Future Technologies) Nanjing Tech University (NanjingTech) Nanjing China

J

Jingjin Dong

State Key Laboratory of Flexible Electronics (LoFE) & Institute of Advanced Materials (IAM) School of Flexible Electronics (Future Technologies) Nanjing Tech University (NanjingTech) Nanjing China

J

Jiupeng Cao

State Key Laboratory of Flexible Electronics (LoFE) & Institute of Advanced Materials (IAM) School of Flexible Electronics (Future Technologies) Nanjing Tech University (NanjingTech) Nanjing China

W

Wei Huang

T

Tianshi Qin