Molecular Tailoring of Pyridine Core-Based Hole Selective Layer for Lead Free Double Perovskite Solar Cells Fabrication

Peng Huang; Manju Sheokand; David Payno Zarceño; Samrana Kazim; Luis Lezama; Mohammad Khaja Nazeeruddin; Rajneesh Misra; Shahzada Ahmad

doi:10.1021/acsaem.3c01027

Molecular Tailoring of Pyridine Core-Based Hole Selective Layer for Lead Free Double Perovskite Solar Cells Fabrication

ACS Appl Energy Mater. 2023 Jul 17;6(15):7955-7964. doi: 10.1021/acsaem.3c01027. eCollection 2023 Aug 14.

Authors

Peng Huang^{1

2}, Manju Sheokand³, David Payno Zarceño¹, Samrana Kazim^{1

4}, Luis Lezama⁵, Mohammad Khaja Nazeeruddin⁶, Rajneesh Misra³, Shahzada Ahmad^{1

4}

Affiliations

¹ BCMaterials, Basque Center for Materials, Applications and Nanostructures, Martina Casiano, UPV/EHU Science Park, 48940 Leioa, Spain.
² Research Institute of Frontier Science, Southwest Jiaotong University, 610031 Chengdu, China.
³ Department of Chemistry, Indian Institute of Technology, 453552 Indore, India.
⁴ IKERBASQUE, Basque Foundation for Science, 48009 Bilbao, Spain.
⁵ Departamento de Química Inorgánica, Facultad de Ciencia y Tecnología, Universidad del País Vasco, UPV/EHU, Sarriena s/n, 48940 Leioa, Spain.
⁶ Group for Molecular Engineering of Functional Materials, Institute of Chemical Sciences and Engineering, École Polytechnique Fedérale de Lausanne, 1951 Sion, Switzerland.

Abstract

To solve the toxicity issues related to lead-based halide perovskite solar cells, the lead-free double halide perovskite Cs₂AgBiBr₆ is proposed. However, reduced rate of charge transfer in double perovskites affects optoelectronic performance. We designed a series of pyridine-based small molecules with four different arms attached to the pyridine core as hole-selective materials by using interface engineering. We quantified how arm modulation affects the structure-property-device performance relationship. Electrical, structural, and spectroscopic investigations show that the N³,N³,N⁶,N⁶-tetrakis(4-methoxyphenyl)-9H-carbazole-3,6-diamine arm's robust association with the pyridine core results in an efficient hole extraction for PyDAnCBZ due to higher spin density close to the pyridine core. The solar cells fabricated using Cs₂AgBiBr₆ as a light harvester and PyDAnCBZ as the hole selective layer measured an unprecedented 2.9% power conversion efficiency. Our computed road map suggests achieving ∼5% efficiency through fine-tuning of Cs₂AgBiBr₆. Our findings reveal the principles for designing small molecules for electro-optical applications as well as a synergistic route to develop inorganic lead-free perovskite materials for solar applications.