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Title: Targeted Ligand-Exchange Chemistry on Cesium Lead Halide Perovskite Quantum Dots for High-Efficiency Photovoltaics

Abstract

The ability to manipulate quantum dot (QD) surfaces is foundational to their technological deployment. Surface manipulation of metal halide perovskite (MHP) QDs has proven particularly challenging in comparison to that of more established inorganic materials due to dynamic surface species and low material formation energy; most conventional methods of chemical manipulation targeted at the MHP QD surface will result in transformation or dissolution of the MHP crystal. In previous work, we have demonstrated record-efficiency QD solar cells (QDSCs) based on ligand-exchange procedures that electronically couple MHP QDs yet maintain their nanocrystalline size, which stabilizes the corner-sharing structure of the constituent PbI64-octahedra with optoelectronic properties optimal for solar energy conversion. In this work, we employ a variety of spectroscopic techniques to develop a molecular-level understanding of the MHP QD surface chemistry in this system. We individually target both the anionic (oleate) and cationic (oleylammonium) ligands. We find that atmospheric moisture aids the process by hydrolysis of methyl acetate to generate acetic acid and methanol. Acetic acid then replaces native oleate ligands to yield QD surface-bound acetate and free oleic acid. The native oleylammonium ligands remain throughout this film deposition process and are exchanged during a final treatment step employing smaller cationsmore » - namely, formamidinium. This final treatment has a narrow processing window; initial treatment at this stage leads to a more strongly coupled QD regime followed by transformation into a bulk MHP film after longer treatment. These insights provide chemical understanding to the deposition of high-quality, electronically coupled MHP QD films that maintain both quantum confinement and their crystalline phase and attain high photovoltaic performance.« less

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [5];  [1]; ORCiD logo [1];  [6];  [6];  [6]; ORCiD logo [1];  [1]; ORCiD logo [7]; ORCiD logo [1]
+ Show Author Affiliations
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Washington, Seattle, WA (United States)
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
  4. National Renewable Energy Lab. (NREL), Golden, CO (United States); Inst. Photovoltaique d’Île de France (IPVF), Palaiseau (France)
  5. Univ. of Texas, Austin, TX (United States)
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  7. Univ. of Washington, Seattle, WA (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Advanced Solar Photophysics (CASP); National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Workforce Development for Teachers and Scientists (WDTS); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office
OSTI Identifier:
1466557
Report Number(s):
NREL/JA-5900-71521
Journal ID: ISSN 0002-7863
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 140; Journal Issue: 33; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 77 NANOSCIENCE AND NANOTECHNOLOGY; atmospheric moisture; chemical manipulation; film-deposition process; nanocrystalline size; optoelectronic properties; photovoltaic performance; spectroscopic technique; surface manipulation

Citation Formats

Wheeler, Lance M., Sanehira, Erin M., Marshall, Ashley R., Schulz, Philip, Suri, Mokshin, Anderson, Nicholas C., Christians, Jeffrey A., Nordlund, Dennis, Sokaras, Dimosthenis, Kroll, Thomas, Harvey, Steven P., Berry, Joseph J., Lin, Lih Y., and Luther, Joseph M. Targeted Ligand-Exchange Chemistry on Cesium Lead Halide Perovskite Quantum Dots for High-Efficiency Photovoltaics. United States: N. p., 2018. Web. doi:10.1021/jacs.8b04984.
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Wheeler, Lance M., Sanehira, Erin M., Marshall, Ashley R., Schulz, Philip, Suri, Mokshin, Anderson, Nicholas C., Christians, Jeffrey A., Nordlund, Dennis, Sokaras, Dimosthenis, Kroll, Thomas, Harvey, Steven P., Berry, Joseph J., Lin, Lih Y., & Luther, Joseph M. Targeted Ligand-Exchange Chemistry on Cesium Lead Halide Perovskite Quantum Dots for High-Efficiency Photovoltaics. United States. https://doi.org/10.1021/jacs.8b04984
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Wheeler, Lance M., Sanehira, Erin M., Marshall, Ashley R., Schulz, Philip, Suri, Mokshin, Anderson, Nicholas C., Christians, Jeffrey A., Nordlund, Dennis, Sokaras, Dimosthenis, Kroll, Thomas, Harvey, Steven P., Berry, Joseph J., Lin, Lih Y., and Luther, Joseph M. Wed . "Targeted Ligand-Exchange Chemistry on Cesium Lead Halide Perovskite Quantum Dots for High-Efficiency Photovoltaics". United States. https://doi.org/10.1021/jacs.8b04984. https://www.osti.gov/servlets/purl/1466557.
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@article{osti_1466557,
title = {Targeted Ligand-Exchange Chemistry on Cesium Lead Halide Perovskite Quantum Dots for High-Efficiency Photovoltaics},
author = {Wheeler, Lance M. and Sanehira, Erin M. and Marshall, Ashley R. and Schulz, Philip and Suri, Mokshin and Anderson, Nicholas C. and Christians, Jeffrey A. and Nordlund, Dennis and Sokaras, Dimosthenis and Kroll, Thomas and Harvey, Steven P. and Berry, Joseph J. and Lin, Lih Y. and Luther, Joseph M.},
abstractNote = {The ability to manipulate quantum dot (QD) surfaces is foundational to their technological deployment. Surface manipulation of metal halide perovskite (MHP) QDs has proven particularly challenging in comparison to that of more established inorganic materials due to dynamic surface species and low material formation energy; most conventional methods of chemical manipulation targeted at the MHP QD surface will result in transformation or dissolution of the MHP crystal. In previous work, we have demonstrated record-efficiency QD solar cells (QDSCs) based on ligand-exchange procedures that electronically couple MHP QDs yet maintain their nanocrystalline size, which stabilizes the corner-sharing structure of the constituent PbI64-octahedra with optoelectronic properties optimal for solar energy conversion. In this work, we employ a variety of spectroscopic techniques to develop a molecular-level understanding of the MHP QD surface chemistry in this system. We individually target both the anionic (oleate) and cationic (oleylammonium) ligands. We find that atmospheric moisture aids the process by hydrolysis of methyl acetate to generate acetic acid and methanol. Acetic acid then replaces native oleate ligands to yield QD surface-bound acetate and free oleic acid. The native oleylammonium ligands remain throughout this film deposition process and are exchanged during a final treatment step employing smaller cations - namely, formamidinium. This final treatment has a narrow processing window; initial treatment at this stage leads to a more strongly coupled QD regime followed by transformation into a bulk MHP film after longer treatment. These insights provide chemical understanding to the deposition of high-quality, electronically coupled MHP QD films that maintain both quantum confinement and their crystalline phase and attain high photovoltaic performance.},
doi = {10.1021/jacs.8b04984},
journal = {Journal of the American Chemical Society},
number = 33,
volume = 140,
place = {United States},
year = {Wed Jul 25 00:00:00 EDT 2018},
month = {Wed Jul 25 00:00:00 EDT 2018}
}
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https://doi.org/10.1021/jacs.8b04984
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Figures / Tables:

Scheme 1 Scheme 1: (a) Hydrolysis of an Ester To Yield a Carboxylic Acid and an Alcohol; (b) Anionic Carboxylate Ligand-Exchange Reaction Observed in CsPbI3 Thin Films and Solutions; (c) Cationic Ligand Exchange Observed in CsPbI3 Thin Films
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