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Title: Understanding Film Formation Morphology and Orientation in High Member 2D Ruddlesden-Popper Perovskites for High-Efficiency Solar Cells

We report that 2D Ruddlesden–Popper (RP) perovskites have recently emerged as promising candidates for hybrid perovskite photovoltaic cells, realizing power-conversion efficiencies (PCEs) of over 10% with technologically relevant stability. To achieve solar cell performance comparable to the state-of-the-art 3D perovskite cells, it is highly desirable to increase the conductivity and lower the optical bandgap for enhanced near-IR region absorption by increasing the perovskite slab thickness. Here, the use of the 2D higher member (n = 5) RP perovskite (n-butyl-NH 3) 2(MeNH 3) 4Pb 5I 16 in depositing highly oriented thin films from dimethylformamide/dimethylsulfoxide mixtures using the hot-casting method is reported. In addition, they exhibit superior environmental stability over thin films of their 3D counterpart. These films are assembled into high-efficiency solar cells with an open-circuit voltage of ≈1 V and PCE of up to 10%. This is achieved by fine-tuning the solvent ratio, crystal growth orientation, and grain size in the thin films. Finally, the enhanced performance of the optimized devices is ascribed to the growth of micrometer-sized grains as opposed to more typically obtained nanometer grain size and highly crystalline, densely packed microstructures with the majority of the inorganic slabs preferentially aligned out of plane to the substrate, asmore » confirmed by X-ray diffraction and grazing-incidence wide-angle X-ray scattering mapping.« less
Authors:
 [1] ; ORCiD logo [2] ;  [3] ; ORCiD logo [2] ;  [2] ; ORCiD logo [2] ;  [4] ;  [3] ; ORCiD logo [2] ;  [3]
  1. Northwestern Univ., Evanston, IL (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  3. Northwestern Univ., Evanston, IL (United States)
  4. Université Europeénne de Bretagne, INSA, FOTON, Rennes (France)
Publication Date:
Report Number(s):
LA-UR-18-30010
Journal ID: ISSN 1614-6832
Grant/Contract Number:
AC52-06NA25396; SC0001059
Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Research Org:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE National Nuclear Security Administration (NNSA)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 14 SOLAR ENERGY; 2D perovskites; microstructure; solar cells; thin films
OSTI Identifier:
1479900
Alternate Identifier(s):
OSTI ID: 1378113

Soe, Chan Myae Myae, Nie, Wanyi, Stoumpos, Constantinos C., Tsai, Hsinhan, Blancon, Jean-Christophe, Liu, Fangze, Even, Jacky, Marks, Tobin J., Mohite, Aditya D., and Kanatzidis, Mercouri G.. Understanding Film Formation Morphology and Orientation in High Member 2D Ruddlesden-Popper Perovskites for High-Efficiency Solar Cells. United States: N. p., Web. doi:10.1002/aenm.201700979.
Soe, Chan Myae Myae, Nie, Wanyi, Stoumpos, Constantinos C., Tsai, Hsinhan, Blancon, Jean-Christophe, Liu, Fangze, Even, Jacky, Marks, Tobin J., Mohite, Aditya D., & Kanatzidis, Mercouri G.. Understanding Film Formation Morphology and Orientation in High Member 2D Ruddlesden-Popper Perovskites for High-Efficiency Solar Cells. United States. doi:10.1002/aenm.201700979.
Soe, Chan Myae Myae, Nie, Wanyi, Stoumpos, Constantinos C., Tsai, Hsinhan, Blancon, Jean-Christophe, Liu, Fangze, Even, Jacky, Marks, Tobin J., Mohite, Aditya D., and Kanatzidis, Mercouri G.. 2017. "Understanding Film Formation Morphology and Orientation in High Member 2D Ruddlesden-Popper Perovskites for High-Efficiency Solar Cells". United States. doi:10.1002/aenm.201700979. https://www.osti.gov/servlets/purl/1479900.
@article{osti_1479900,
title = {Understanding Film Formation Morphology and Orientation in High Member 2D Ruddlesden-Popper Perovskites for High-Efficiency Solar Cells},
author = {Soe, Chan Myae Myae and Nie, Wanyi and Stoumpos, Constantinos C. and Tsai, Hsinhan and Blancon, Jean-Christophe and Liu, Fangze and Even, Jacky and Marks, Tobin J. and Mohite, Aditya D. and Kanatzidis, Mercouri G.},
abstractNote = {We report that 2D Ruddlesden–Popper (RP) perovskites have recently emerged as promising candidates for hybrid perovskite photovoltaic cells, realizing power-conversion efficiencies (PCEs) of over 10% with technologically relevant stability. To achieve solar cell performance comparable to the state-of-the-art 3D perovskite cells, it is highly desirable to increase the conductivity and lower the optical bandgap for enhanced near-IR region absorption by increasing the perovskite slab thickness. Here, the use of the 2D higher member (n = 5) RP perovskite (n-butyl-NH3)2(MeNH3)4Pb5I16 in depositing highly oriented thin films from dimethylformamide/dimethylsulfoxide mixtures using the hot-casting method is reported. In addition, they exhibit superior environmental stability over thin films of their 3D counterpart. These films are assembled into high-efficiency solar cells with an open-circuit voltage of ≈1 V and PCE of up to 10%. This is achieved by fine-tuning the solvent ratio, crystal growth orientation, and grain size in the thin films. Finally, the enhanced performance of the optimized devices is ascribed to the growth of micrometer-sized grains as opposed to more typically obtained nanometer grain size and highly crystalline, densely packed microstructures with the majority of the inorganic slabs preferentially aligned out of plane to the substrate, as confirmed by X-ray diffraction and grazing-incidence wide-angle X-ray scattering mapping.},
doi = {10.1002/aenm.201700979},
journal = {Advanced Energy Materials},
number = 1,
volume = 8,
place = {United States},
year = {2017},
month = {9}
}

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