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Origin of the Substitution Mechanism for the Binding of Organic Ligands on the Surface of CsPbBr3 Perovskite Nanocubes
Abstract
Optoelectronic properties of CsPbBr 3 perovskite nanocubes (NCs) depend strongly on the interaction of the organic passivating molecules with the inorganic crystal. To understand this interaction, we employed a combination of synchrotron-based X-ray photoelectron spectroscopy (XPS), nuclear magnetic resonance (NMR) spectroscopy, and first-principles density functional theory (DFT)-based calculations. Variable energy XPS elucidated the internal structure of the inorganic part in a layer-by-layer fashion, whereas NMR characterized the organic ligands. Our experimental results confirm that oleylammonium ions act as capping ligands by substituting Cs + ions from the surface of CsPbBr 3 NCs. DFT calculations shows that the substitution mechanism does not require much energy for surface reconstruction and, in contrast, stabilizes the nanocrystal by the formation of three hydrogen bonds between the −NH 3 + moiety of oleylammonium and surrounding Br – on the surface of NCs. This substitution mechanism and its origin are in stark contrast to the usual adsorption of organic ligands on the surface of typical NCs.
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Dabbousi, B. O., Rodriguez-Viejo, J., Mikulec, F. V., Heine, J. R., Mattoussi, H., Ober, R., Jensen, K. F., & Bawendi, M. G. (1997) · The Journal of Physical Chemistry B · doi:10.1021/jp971091y · Cited by 4,229
Cited by
Krieg, F., Ochsenbein, S. T., Yakunin, S., ten Brinck, S., Aellen, P., Süess, A., Clerc, B., Guggisberg, D., Nazarenko, O., Shynkarenko, Y., et al. (2018) · ACS Energy Letters · doi:10.1021/acsenergylett.8b00035 · Cited by 893
Nenon, D. P., Pressler, K., Kang, J., Koscher, B. A., Olshansky, J. H., Osowiecki, W. T., Koc, M. A., Wang, L.-W., & Alivisatos, A. P. (2018) · Journal of the American Chemical Society · doi:10.1021/jacs.8b11035 · Cited by 631
Almeida, G., Goldoni, L., Akkerman, Q., Dang, Z., Khan, A. H., Marras, S., Moreels, I., & Manna, L. (2018) · ACS Nano · doi:10.1021/acsnano.7b08357 · Cited by 553
Bodnarchuk, M. I., Boehme, S. C., ten Brinck, S., Bernasconi, C., Shynkarenko, Y., Krieg, F., Widmer, R., Aeschlimann, B., Günther, D., Kovalenko, M. V., et al. (2019) · ACS Energy Letters · doi:10.1021/acsenergylett.8b01669 · Cited by 466
Surface Chemistry Engineering of Perovskite Quantum Dots: Strategies, Applications, and Perspectives
Bai, Y., Hao, M., Ding, S., Chen, P., & Wang, L. (2022) · Advanced Materials · doi:10.1002/adma.202105958 · Cited by 394
Metadata
- Authors
- Ravi, V. K., Santra, P. K., Joshi, N., Chugh, J., Singh, S. K., Rensmo, H., Ghosh, P., & Nag, A.
- Venue
- The Journal of Physical Chemistry Letters
- Publisher
- American Chemical Society (ACS)
- Published
- 2017-09-29
- Volume
- 8
- Issue
- 20
- Pages
- 4988-4994
- ISSN
- 1948-7185 (ISSN-L)
- OpenAlex
- W2757007007
- Cited by
- 380
- References
- 1
- FWCI
- 14.54
- Type
- journal article
- Language
- en
- Open access
- closed
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- Ravi, V. K., Santra, P. K., Joshi, N., Chugh, J., Singh, S. K., Rensmo, H., Ghosh, P., & Nag, A. (2017). Origin of the Substitution Mechanism for the Binding of Organic Ligands on the Surface of CsPbBr3 Perovskite Nanocubes. The Journal of Physical Chemistry Letters. https://doi.org/10.1021/acs.jpclett.7b02192
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