Selective Crystallization Delay in Wide‐Bandgap Perovskites Enables Initial Homogeneous Phase for Square Centimeter Perovskite/Organic Tandem Solar Cells

J Jialei Zheng (School of Life Science and Technology (L.Y., J.Z., A.Z., M.Y., J.M., H.Z.), ShanghaiTech University, China.) W Weijie Chen (Laboratory of Advanced Optoelectronic Materials, Suzhou Key Laboratory of Novel Semiconductor-optoelectronics Materials and Devices, State Key Laboratory of Bioinspired Interfacial Materials Science, College of Chemistry, Chemical Engineering and Materials Science) Z Ziyue Wang S Shuaiqing Kang (Laboratory of Advanced Optoelectronic Materials, Suzhou Key Laboratory of Novel Semiconductor‐optoelectronics Materials and Devices, State Key Laboratory of Bioinspired Interfacial Materials Science, College of Chemistry, Chemical Engineering and Materials Science Soochow University Suzhou 215123 China) P Pengpeng Dong (Laboratory of Advanced Optoelectronic Materials Suzhou Key Laboratory of Novel Semiconductor‐Optoelectronics Materials and Devices State Key Laboratory of Bioinspired Interfacial Materials Science College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou China) Y Yue Yin H Haiyang Chen J Jianlei Cao (Laboratory of Advanced Optoelectronic Materials Suzhou Key Laboratory of Novel Semiconductor‐optoelectronics Materials and Devices State Key Laboratory of Bioinspired Interfacial Materials Science College of Chemistry, Chemical Engineering and Materials Science Soochow University Suzhou 215123 China) J Jixiang Yuan (Laboratory of Advanced Optoelectronic Materials Suzhou Key Laboratory of Novel Semiconductor‐Optoelectronics Materials and Devices State Key Laboratory of Bioinspired Interfacial Materials Science College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou China) G Guiying Xu J Jiacheng Xu (Laboratory of Advanced Optoelectronic Materials, Suzhou Key Laboratory of Novel Semiconductor-optoelectronics Materials and Devices, State Key Laboratory of Bioinspired Interfacial Materials Science, College of Chemistry, Chemical Engineering and Materials Science) Y Yaowen Li

Abstract

Abstract Mixed halide wide‐bandgap (WBG) perovskites, used in high‐performance perovskite/organic tandem solar cells (TSCs), are prone to phase segregation under light irradiation. Particularly, the initial inhomogeneous halide phase distribution in WBG perovskites can accelerate the phase segregation under operational stressors, thus hindering scaling of TSCs that require high phase homogeneity. Here, a selective delayed crystallization strategy is proposed in which a functional agent (3‐amino‐5‐fluorobenzamide; AFBA) is used to regulate the initial halide phase distribution. The ‐NH 2 of AFBA, with a low electron‐cloud density, shows a higher binding affinity with bromide than with iodide, thus selectively delaying the rapid crystallization of bromide; this phenomenon induces a homogeneous halide distribution across the film. The initial homogeneous film is phase‐stable under operational stressors. As a result, the square‐centimeter WBG perovskite front cell achieves a high efficiency of 18.61%. When stacked with organic subcells, the square‐centimeter perovskite/organic TSC exhibits a remarkable efficiency of 25.21%, showing a weak‐dependence of efficiency on size from 0.062 to 2.000 cm 2 , as well as a prolonged operational lifetime with a T 90 of 1500 h. Perovskite/organic TSCs are also connected in series with electrochromic devices to dynamically monitor the TSC performance via the color variation, providing insights for their future applications.

Article Details

Volume / Issue Vol. 37, Issue 42
Published October 01, 2025
ISSN 0935-9648
Publisher Unknown Publisher

Journal Info

Advanced Materials

Unknown Publisher

ISSN: 0935-9648 Physical Sciences

Authors (12)

J

Jialei Zheng

School of Life Science and Technology (L.Y., J.Z., A.Z., M.Y., J.M., H.Z.), ShanghaiTech University, China.

W

Weijie Chen

Laboratory of Advanced Optoelectronic Materials, Suzhou Key Laboratory of Novel Semiconductor-optoelectronics Materials and Devices, State Key Laboratory of Bioinspired Interfacial Materials Science, College of Chemistry, Chemical Engineering and Materials Science

Z

Ziyue Wang

S

Shuaiqing Kang

Laboratory of Advanced Optoelectronic Materials, Suzhou Key Laboratory of Novel Semiconductor‐optoelectronics Materials and Devices, State Key Laboratory of Bioinspired Interfacial Materials Science, College of Chemistry, Chemical Engineering and Materials Science Soochow University Suzhou 215123 China

P

Pengpeng Dong

Laboratory of Advanced Optoelectronic Materials Suzhou Key Laboratory of Novel Semiconductor‐Optoelectronics Materials and Devices State Key Laboratory of Bioinspired Interfacial Materials Science College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou China

Y

Yue Yin

H

Haiyang Chen

J

Jianlei Cao

Laboratory of Advanced Optoelectronic Materials Suzhou Key Laboratory of Novel Semiconductor‐optoelectronics Materials and Devices State Key Laboratory of Bioinspired Interfacial Materials Science College of Chemistry, Chemical Engineering and Materials Science Soochow University Suzhou 215123 China

J

Jixiang Yuan

Laboratory of Advanced Optoelectronic Materials Suzhou Key Laboratory of Novel Semiconductor‐Optoelectronics Materials and Devices State Key Laboratory of Bioinspired Interfacial Materials Science College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou China

G

Guiying Xu

J

Jiacheng Xu

Laboratory of Advanced Optoelectronic Materials, Suzhou Key Laboratory of Novel Semiconductor-optoelectronics Materials and Devices, State Key Laboratory of Bioinspired Interfacial Materials Science, College of Chemistry, Chemical Engineering and Materials Science

Y

Yaowen Li