Targeted Ligand-Exchange Chemistry on Cesium Lead Halide Perovskite Quantum Dots for High-Efficiency Photovoltaics
| Autor: | Dennis Nordlund, Erin M. Sanehira, Ashley R. Marshall, Nicholas C. Anderson, Thomas Kroll, Lance M. Wheeler, Dimosthenis Sokaras, Joseph M. Luther, Jeffrey A. Christians, Mokshin Suri, Joseph J. Berry, Steven P. Harvey, Philip Schulz, Lih Y. Lin |
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| Přispěvatelé: | SLAC National Accelerator Laboratory (SLAC), Stanford University |
| Jazyk: | angličtina |
| Rok vydání: | 2018 |
| Předmět: |
Halide
Nanotechnology 02 engineering and technology 010402 general chemistry 01 natural sciences 7. Clean energy Biochemistry Catalysis Crystal Colloid and Surface Chemistry Photovoltaics Thin film Dissolution ComputingMilieux_MISCELLANEOUS Perovskite (structure) Chemistry business.industry General Chemistry [CHIM.MATE]Chemical Sciences/Material chemistry 021001 nanoscience & nanotechnology Nanocrystalline material 0104 chemical sciences Quantum dot [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci] 0210 nano-technology business |
| Zdroj: | Journal of the American Chemical Society Journal of the American Chemical Society, American Chemical Society, 2018, 140 (33), pp.10504-10513. ⟨10.1021/jacs.8b04984⟩ |
| ISSN: | 0002-7863 1520-5126 |
| DOI: | 10.1021/jacs.8b04984⟩ |
| Popis: | 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. |
| Databáze: | OpenAIRE |
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