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Extended nucleation and superfocusing in colloidal semiconductor nanocrystal synthesis

(2021) NANO LETTERS. 21(6). p.2487-2496
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Abstract
Hot injection synthesis is renowned for producing semiconductor nanocolloids with superb size dispersions. Burst nucleation and diffusion-controlled size focusing during growth have been invoked to rationalize this characteristic yet experimental evidence supporting the pertinence of these concepts is scant. By monitoring a CdSe synthesis in-situ with X-ray scattering, we find that nucleation is an extended event that coincides with growth during 15-20% of the reaction time. Moreover, we show that size focusing outpaces predictions of diffusion-limited growth. This observation indicates that nanocrystal growth is dictated by the surface reactivity, which drops sharply for larger nanocrystals. Kinetic reaction simulations confirm that this so-called superfocusing can lengthen the nucleation period and promote size focusing. The finding that narrow size dispersions can emerge from the counteracting effects of extended nucleation and reaction-limited size focusing ushers in an evidence-based perspective that turns hot injection into a rational scheme to produce monodisperse semiconductor nanocolloids.
Keywords
nanocolloids, quantum dots, monodisperse, nucleation and growth, in-situ analysis, photoluminescence

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MLA
Prins, P. Tim, et al. “Extended Nucleation and Superfocusing in Colloidal Semiconductor Nanocrystal Synthesis.” NANO LETTERS, vol. 21, no. 6, 2021, pp. 2487–96, doi:10.1021/acs.nanolett.0c04813.
APA
Prins, P. T., Montanarella, F., Dümbgen, K. C., Justo Zarraquiños, Y., van der Bok, J. C., Hinterding, S. O. M., … Hens, Z. (2021). Extended nucleation and superfocusing in colloidal semiconductor nanocrystal synthesis. NANO LETTERS, 21(6), 2487–2496. https://doi.org/10.1021/acs.nanolett.0c04813
Chicago author-date
Prins, P. Tim, Federico Montanarella, Kim Corinna Dümbgen, Yolanda Justo Zarraquiños, Johanna C. van der Bok, Stijn O. M. Hinterding, Jaco J. Geuchies, et al. 2021. “Extended Nucleation and Superfocusing in Colloidal Semiconductor Nanocrystal Synthesis.” NANO LETTERS 21 (6): 2487–96. https://doi.org/10.1021/acs.nanolett.0c04813.
Chicago author-date (all authors)
Prins, P. Tim, Federico Montanarella, Kim Corinna Dümbgen, Yolanda Justo Zarraquiños, Johanna C. van der Bok, Stijn O. M. Hinterding, Jaco J. Geuchies, Jorick Maes, Kim De Nolf, Sander Deelen, Hans Meijer, Thomas Zinn, Andrei V. Petukhov, Freddy T. Rabouw, Celso De Mello Donega, Daniel Vanmaekelbergh, and Zeger Hens. 2021. “Extended Nucleation and Superfocusing in Colloidal Semiconductor Nanocrystal Synthesis.” NANO LETTERS 21 (6): 2487–2496. doi:10.1021/acs.nanolett.0c04813.
Vancouver
1.
Prins PT, Montanarella F, Dümbgen KC, Justo Zarraquiños Y, van der Bok JC, Hinterding SOM, et al. Extended nucleation and superfocusing in colloidal semiconductor nanocrystal synthesis. NANO LETTERS. 2021;21(6):2487–96.
IEEE
[1]
P. T. Prins et al., “Extended nucleation and superfocusing in colloidal semiconductor nanocrystal synthesis,” NANO LETTERS, vol. 21, no. 6, pp. 2487–2496, 2021.
@article{8704776,
  abstract     = {{Hot injection synthesis is renowned for producing semiconductor nanocolloids with superb size dispersions. Burst nucleation and diffusion-controlled size focusing during growth have been invoked to rationalize this characteristic yet experimental evidence supporting the pertinence of these concepts is scant. By monitoring a CdSe synthesis in-situ with X-ray scattering, we find that nucleation is an extended event that coincides with growth during 15-20% of the reaction time. Moreover, we show that size focusing outpaces predictions of diffusion-limited growth. This observation indicates that nanocrystal growth is dictated by the surface reactivity, which drops sharply for larger nanocrystals. Kinetic reaction simulations confirm that this so-called superfocusing can lengthen the nucleation period and promote size focusing. The finding that narrow size dispersions can emerge from the counteracting effects of extended nucleation and reaction-limited size focusing ushers in an evidence-based perspective that turns hot injection into a rational scheme to produce monodisperse semiconductor nanocolloids.}},
  author       = {{Prins, P. Tim and Montanarella, Federico and Dümbgen, Kim Corinna and Justo Zarraquiños, Yolanda and van der Bok, Johanna C. and Hinterding, Stijn O. M. and Geuchies, Jaco J. and Maes, Jorick and De Nolf, Kim and Deelen, Sander and Meijer, Hans and Zinn, Thomas and Petukhov, Andrei V. and Rabouw, Freddy T. and Donega, Celso De Mello and Vanmaekelbergh, Daniel and Hens, Zeger}},
  issn         = {{1530-6984}},
  journal      = {{NANO LETTERS}},
  keywords     = {{nanocolloids,quantum dots,monodisperse,nucleation and growth,in-situ analysis,photoluminescence}},
  language     = {{eng}},
  number       = {{6}},
  pages        = {{2487--2496}},
  title        = {{Extended nucleation and superfocusing in colloidal semiconductor nanocrystal synthesis}},
  url          = {{http://doi.org/10.1021/acs.nanolett.0c04813}},
  volume       = {{21}},
  year         = {{2021}},
}

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