Kinetic broadening of size distribution in terms of natural versus invariant variables

Vladimir G. Dubrovskii, Nickolay V. Sibirev, and Andrei S. Sokolovskii
Phys. Rev. E 103, 012112 – Published 13 January 2021

Abstract

We study theoretically the size distributions of nanoparticles (islands, droplets, nanowires) whose time evolution obeys the kinetic rate equations with size-dependent condensation and evaporation rates. Different effects are studied which contribute to the size distribution broadening, including kinetic fluctuations, evaporation, nucleation delay, and size-dependent growth rates. Under rather general assumptions, an analytic form of the size distribution is obtained in terms of the natural variable s which equals the number of monomers in the nanoparticle. Green's function of the continuum rate equation is shown to be Gaussian, with the size-dependent variance. We consider particular examples of the size distributions in either linear growth systems (at a constant supersaturation) or classical nucleation theory with pumping (at a time-dependent supersaturation) and compare the spectrum broadening in terms of s versus the invariant variable ρ for which the regular growth rate is size independent. For the growth rate scaling with s as sα (with the growth index α between 0 and 1), the size distribution broadens for larger α in terms of s, while it narrows with α if presented in terms of ρ. We establish the conditions for obtaining a time-invariant size distribution over a given variable for different growth laws. This result applies for a wide range of systems and shows how the growth method can be optimized to narrow the size distribution over a required variable, for example, the volume, surface area, radius or length of a nanoparticle. An analysis of some concrete growth systems is presented from the viewpoint of the obtained results.

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  • Received 1 September 2020
  • Revised 28 November 2020
  • Accepted 23 December 2020

DOI:https://doi.org/10.1103/PhysRevE.103.012112

©2021 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Vladimir G. Dubrovskii1,*, Nickolay V. Sibirev1, and Andrei S. Sokolovskii2

  • 1St. Petersburg State University, Universitetskaya Embankment 13B, 199034 St. Petersburg, Russia
  • 2ITMO University, Kronverkskiy Prospect 49, 197101 St. Petersburg, Russia

  • *dubrovskii@mail.ioffe.ru

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Vol. 103, Iss. 1 — January 2021

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