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Highly dynamic ligand binding and light absorption coefficient of cesium lead Bromide perovskite nanocrystals

(2016) ACS NANO. 10(2). p.2071-2081
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Center for nano- and biophotonics (NB-Photonics)
Abstract
Lead halide perovskite materials have attracted significant attention in the context of photovoltaics and other optoelectronic applications, and recently, research efforts have been directed to nanostructured lead halide perovskites. Collodial nanocrystals (NCs) of cesium lead halides (CsPbX3, X = Cl, Br, I) exhibit bright photoluminescence, with emission tunable over the entire visible spectral region. However, previous studies on CsPbX3 NCs did not address key aspects of their chemistry and photophysics such as surface chemistry and quantitative light absorption. Here, we elaborate on the synthesis of CsPbBr3 NCs and their surface chemistry. In addition, the intrinsic absorption coefficient was determined experimentally by combining elemental analysis with accurate optical absorption measurements. H-1 solution nuclear magnetic resonance spectroscopy was used to characterize sample purity, elucidate the surface chemistry, and evaluate the influence of purification methods on the surface composition. We find that ligand binding to the NC surface is highly dynamic, and therefore, ligands are easily lost during the isolation and purification procedures. However, when a small amount of both oleic acid and oleylamine is added, the NCs can be purified, maintaining optical, colloidal, and material integrity. In addition, we find that a high amine content in the ligand shell increases the quantum yield due to the improved binding of the carboxylic acid.
Keywords
ORGANOMETAL HALIDE PEROVSKITE, NMR, CsPbBr3, absorption coefficient, METAL-OXIDE NANOCRYSTALS, SENSITIZED SOLAR-CELLS, CDSE QUANTUM DOTS, surface chemistry, COLLOIDAL NANOCRYSTALS, SURFACE-CHEMISTRY, HYDRODYNAMIC FRICTION, ANION-EXCHANGE, NANOPARTICLES, BR

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Citation

Please use this url to cite or link to this publication:

MLA
De Roo, Jonathan et al. “Highly Dynamic Ligand Binding and Light Absorption Coefficient of Cesium Lead Bromide Perovskite Nanocrystals.” ACS NANO 10.2 (2016): 2071–2081. Print.
APA
De Roo, J., Ibanez, M., Geiregat, P., Nedelcu, G., Walravens, W., Maes, J., Martins, J., et al. (2016). Highly dynamic ligand binding and light absorption coefficient of cesium lead Bromide perovskite nanocrystals. ACS NANO, 10(2), 2071–2081.
Chicago author-date
De Roo, Jonathan, Maria Ibanez, Pieter Geiregat, Georgian Nedelcu, Willem Walravens, Jorick Maes, José Martins, Isabel Van Driessche, Maksym V Koyalenko, and Zeger Hens. 2016. “Highly Dynamic Ligand Binding and Light Absorption Coefficient of Cesium Lead Bromide Perovskite Nanocrystals.” Acs Nano 10 (2): 2071–2081.
Chicago author-date (all authors)
De Roo, Jonathan, Maria Ibanez, Pieter Geiregat, Georgian Nedelcu, Willem Walravens, Jorick Maes, José Martins, Isabel Van Driessche, Maksym V Koyalenko, and Zeger Hens. 2016. “Highly Dynamic Ligand Binding and Light Absorption Coefficient of Cesium Lead Bromide Perovskite Nanocrystals.” Acs Nano 10 (2): 2071–2081.
Vancouver
1.
De Roo J, Ibanez M, Geiregat P, Nedelcu G, Walravens W, Maes J, et al. Highly dynamic ligand binding and light absorption coefficient of cesium lead Bromide perovskite nanocrystals. ACS NANO. 2016;10(2):2071–81.
IEEE
[1]
J. De Roo et al., “Highly dynamic ligand binding and light absorption coefficient of cesium lead Bromide perovskite nanocrystals,” ACS NANO, vol. 10, no. 2, pp. 2071–2081, 2016.
@article{7208295,
  abstract     = {Lead halide perovskite materials have attracted significant attention in the context of photovoltaics and other optoelectronic applications, and recently, research efforts have been directed to nanostructured lead halide perovskites. Collodial nanocrystals (NCs) of cesium lead halides (CsPbX3, X = Cl, Br, I) exhibit bright photoluminescence, with emission tunable over the entire visible spectral region. However, previous studies on CsPbX3 NCs did not address key aspects of their chemistry and photophysics such as surface chemistry and quantitative light absorption. Here, we elaborate on the synthesis of CsPbBr3 NCs and their surface chemistry. In addition, the intrinsic absorption coefficient was determined experimentally by combining elemental analysis with accurate optical absorption measurements. H-1 solution nuclear magnetic resonance spectroscopy was used to characterize sample purity, elucidate the surface chemistry, and evaluate the influence of purification methods on the surface composition. We find that ligand binding to the NC surface is highly dynamic, and therefore, ligands are easily lost during the isolation and purification procedures. However, when a small amount of both oleic acid and oleylamine is added, the NCs can be purified, maintaining optical, colloidal, and material integrity. In addition, we find that a high amine content in the ligand shell increases the quantum yield due to the improved binding of the carboxylic acid.},
  author       = {De Roo, Jonathan and Ibanez, Maria and Geiregat, Pieter and Nedelcu, Georgian and Walravens, Willem and Maes, Jorick and Martins, José and Van Driessche, Isabel and Koyalenko, Maksym V and Hens, Zeger},
  issn         = {1936-0851},
  journal      = {ACS NANO},
  keywords     = {ORGANOMETAL HALIDE PEROVSKITE,NMR,CsPbBr3,absorption coefficient,METAL-OXIDE NANOCRYSTALS,SENSITIZED SOLAR-CELLS,CDSE QUANTUM DOTS,surface chemistry,COLLOIDAL NANOCRYSTALS,SURFACE-CHEMISTRY,HYDRODYNAMIC FRICTION,ANION-EXCHANGE,NANOPARTICLES,BR},
  language     = {eng},
  number       = {2},
  pages        = {2071--2081},
  title        = {Highly dynamic ligand binding and light absorption coefficient of cesium lead Bromide perovskite nanocrystals},
  url          = {http://dx.doi.org/10.1021/acsnano.5b06295},
  volume       = {10},
  year         = {2016},
}

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