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Title: Phase Transition Control for High Performance Ruddlesden-Popper Perovskite Solar Cells

Abstract

Ruddlesden–Popper reduced-dimensional hybrid perovskite (RDP) semiconductors have attracted significant attention recently due to their promising stability and excellent optoelectronic properties. Here, the RDP crystallization mechanism in real time from liquid precursors to the solid film is investigated, and how the phase transition kinetics influences phase purity, quantum well orientation, and photovoltaic performance is revealed. An important template-induced nucleation and growth of the desired (BA)2(MA)3Pb4I13 phase, which is achieved only via direct crystallization without formation of intermediate phases, is observed. As such, the thermodynamically preferred perpendicular crystal orientation and high phase purity are obtained. At low temperature, the formation of intermediate phases, including PbI2 crystals and solvate complexes, slows down intercalation of ions and increases nucleation barrier, leading to formation of multiple RDP phases and orientation randomness. These insights enable to obtain high quality (BA)2(MA)3Pb4I13 films with preferentially perpendicular quantum well orientation, high phase purity, smooth film surface, and improved optoelectronic properties. The resulting devices exhibit high power conversion efficiency of 12.17%. This work should help guide the perovskite community to better control Ruddlesden–Popper perovskite structure and further improve optoelectronic and solar cell devices.

Authors:
 [1];  [2];  [3];  [3]; ORCiD logo [4]; ORCiD logo [4];  [3];  [3];  [5];  [6]; ORCiD logo [4];  [3];  [2];  [7]
  1. Shaanxi Normal Univ., Xi'an (China); Chinese Academy of Sciences, Dalian (China)
  2. King Abdullah Univ. of Science and Technology (KAUST), Thuwal (Saudi Arabia)
  3. Shaanxi Normal Univ., Xi'an (China)
  4. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  5. Cornell Univ., Ithaca, NY (United States). Cornell High Energy Synchrotron Source (CHESS)
  6. Northwestern Univ., Evanston, IL (United States)
  7. (Frank) [Shaanxi Normal Univ., Xi'an (China); Chinese Academy of Sciences, Dalian (China)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
National Science Foundation (NSF); USDOE
OSTI Identifier:
1558068
Report Number(s):
LA-UR-19-22960
Journal ID: ISSN 0935-9648
Grant/Contract Number:  
89233218CNA000001
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 21; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; Material Science

Citation Formats

Zhang, Xu, Munir, Rahim, Zhuo, Xu, Liu, Yucheng, Tsai, Hsinhan, Nie, Wanyi, Li, Jianbo, Niu, Tianqi, Smilgies, Detlef-M., Kanatzidis, Mercouri G., Mohite, Aditya, Zhao, Kui, Amassian, Aram, and Liu, Shengzhong. Phase Transition Control for High Performance Ruddlesden-Popper Perovskite Solar Cells. United States: N. p., 2018. Web. doi:10.1002/adma.201707166.
Zhang, Xu, Munir, Rahim, Zhuo, Xu, Liu, Yucheng, Tsai, Hsinhan, Nie, Wanyi, Li, Jianbo, Niu, Tianqi, Smilgies, Detlef-M., Kanatzidis, Mercouri G., Mohite, Aditya, Zhao, Kui, Amassian, Aram, & Liu, Shengzhong. Phase Transition Control for High Performance Ruddlesden-Popper Perovskite Solar Cells. United States. doi:https://doi.org/10.1002/adma.201707166
Zhang, Xu, Munir, Rahim, Zhuo, Xu, Liu, Yucheng, Tsai, Hsinhan, Nie, Wanyi, Li, Jianbo, Niu, Tianqi, Smilgies, Detlef-M., Kanatzidis, Mercouri G., Mohite, Aditya, Zhao, Kui, Amassian, Aram, and Liu, Shengzhong. Mon . "Phase Transition Control for High Performance Ruddlesden-Popper Perovskite Solar Cells". United States. doi:https://doi.org/10.1002/adma.201707166. https://www.osti.gov/servlets/purl/1558068.
@article{osti_1558068,
title = {Phase Transition Control for High Performance Ruddlesden-Popper Perovskite Solar Cells},
author = {Zhang, Xu and Munir, Rahim and Zhuo, Xu and Liu, Yucheng and Tsai, Hsinhan and Nie, Wanyi and Li, Jianbo and Niu, Tianqi and Smilgies, Detlef-M. and Kanatzidis, Mercouri G. and Mohite, Aditya and Zhao, Kui and Amassian, Aram and Liu, Shengzhong},
abstractNote = {Ruddlesden–Popper reduced-dimensional hybrid perovskite (RDP) semiconductors have attracted significant attention recently due to their promising stability and excellent optoelectronic properties. Here, the RDP crystallization mechanism in real time from liquid precursors to the solid film is investigated, and how the phase transition kinetics influences phase purity, quantum well orientation, and photovoltaic performance is revealed. An important template-induced nucleation and growth of the desired (BA)2(MA)3Pb4I13 phase, which is achieved only via direct crystallization without formation of intermediate phases, is observed. As such, the thermodynamically preferred perpendicular crystal orientation and high phase purity are obtained. At low temperature, the formation of intermediate phases, including PbI2 crystals and solvate complexes, slows down intercalation of ions and increases nucleation barrier, leading to formation of multiple RDP phases and orientation randomness. These insights enable to obtain high quality (BA)2(MA)3Pb4I13 films with preferentially perpendicular quantum well orientation, high phase purity, smooth film surface, and improved optoelectronic properties. The resulting devices exhibit high power conversion efficiency of 12.17%. This work should help guide the perovskite community to better control Ruddlesden–Popper perovskite structure and further improve optoelectronic and solar cell devices.},
doi = {10.1002/adma.201707166},
journal = {Advanced Materials},
number = 21,
volume = 30,
place = {United States},
year = {2018},
month = {4}
}

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