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Formation and morphological evolution of self-similar 3D nanostructures on weakly interacting substrates
Linköping University, Department of Physics, Chemistry and Biology, Nanoscale engineering. Linköping University, Faculty of Science & Engineering.ORCID iD: 0000-0002-0908-7187
Linköping University, Department of Physics, Chemistry and Biology, Nanoscale engineering. Linköping University, Faculty of Science & Engineering.ORCID iD: 0000-0002-2541-2867
Linköping University, Department of Physics, Chemistry and Biology, Nanoscale engineering. Linköping University, Faculty of Science & Engineering.
Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering. Univ Illinois, IL 61801 USA; Univ Illinois, IL 61801 USA.
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2018 (English)In: PHYSICAL REVIEW MATERIALS, ISSN 2475-9953, Vol. 2, no 6, article id 063401Article in journal (Refereed) Published
Abstract [en]

Vapor condensation on weakly interacting substrates leads to the formation of three-dimensional (3D) nanoscale islands (i.e., nanostructures). While it is widely accepted that this process is driven by minimization of the total film/substrate surface and interface energy, current film-growth theory cannot fully explain the atomic-scale mechanisms and pathways by which 3D island formation and morphological evolution occurs. Here, we use kinetic Monte Carlo simulations to describe the dynamic evolution of single-island shapes during deposition of Ag on weakly interacting substrates. The results show that 3D island shapes evolve in a self-similar manner, exhibiting a constant height-to-radius aspect ratio, which is a function of the growth temperature. Furthermore, our results reveal the following chain of atomic-scale events that lead to compact 3D island shapes: 3D nuclei are first formed due to facile adatom ascent at single-layer island steps, followed by the development of sidewall facets bounding the islands, which in turn facilitates upward diffusion from the base to the top of the islands. The limiting atomic process which determines the island height, for a given number of deposited atoms, is the temperature-dependent rate at which adatoms cross from sidewall facets to the island top. The overall findings of this study provide insights into the directed growth of metal nanostructures with controlled shapes on weakly interacting substrates, including two-dimensional crystals, for use in catalytic and nanoelectronic applications.

Place, publisher, year, edition, pages
AMER PHYSICAL SOC , 2018. Vol. 2, no 6, article id 063401
National Category
Condensed Matter Physics
Identifiers
URN: urn:nbn:se:liu:diva-149345DOI: 10.1103/PhysRevMaterials.2.063401ISI: 000435337300001OAI: oai:DiVA.org:liu-149345DiVA, id: diva2:1229834
Note

Funding Agencies|Linkoping University [Dnr-LiU-2015-01510]; Swedish Research Council [VR-2011-5312, VR-2015-04630, VR2014-5790]; Knut and AliceWallenberg Foundation [KAW2011-0094]

Available from: 2018-07-02 Created: 2018-07-02 Last updated: 2019-06-28
In thesis
1. Metal film growth on weakly-interacting substrates: Stochastic simulations and analytical modelling
Open this publication in new window or tab >>Metal film growth on weakly-interacting substrates: Stochastic simulations and analytical modelling
2019 (English)Licentiate thesis, comprehensive summary (Other academic)
Abstract [en]

Thin films are nanoscale layers of material, with exotic properties useful in diverse areas, ranging from biomedicine to nanoelectronics and surface protection. Film properties are not only determined by their chemical composition, but also by their microstructure and roughness, features that depend crucially on the growth process due to the inherent out-of equilibrium nature of the film deposition techniques. This fact suggest that it is possible to control film growth, and in turn film properties, in a knowledge-based manner by tuning the deposition conditions. This requires a good understanding of the elementary film-forming processes, and the way by which they are affected by atomic-scale kinetics. The kinetic Monte Carlo (kMC) method is a simulation tool that can model film evolution over extended time scales, of the order of microseconds, and beyond, and thus constitutes a powerful complement to experimental research aiming to obtain an universal understanding of thin film formation and morphological evolution.

In this work, kMC simulations, coupled with analytical modelling, are used to investigate the early stages of formation of metal films and nanostructures supported on weakly-interacting substrates. This starts with the formation and growth of faceted 3D islands, that relies first on facile adatom ascent at single-layer island steps and subsequently on facile adatom upward diffusion from the base to the top of the island across its facets. Interlayer mass transport is limited by the rate at which adatoms cross from the sidewall facets to the island top, a process that determines the final height of the islands and leads non-trivial growth dynamics, as increasing temperatures favour 3D growth as a result of the upward transport. These findings explain the high roughness observed experimentally in metallic films grown on weakly-interacting substrates at high temperatures.

The second part of the study focus on the next logical step of film formation, when 3D islands come into contact and fuse into a single one, or coalesce. The research reveals that the faceted island structure governs the macroscopic process of coalescence as well as its dynamics, and that morphological changes depend on 2D nucleation on the II facets. In addition, deposition during coalescence is found to accelerate the process and modify its dynamics, by contributing to the nucleation of new facets.

This study provides useful knowledge concerning metal growth on weakly-interacting substrates, and, in particular, identifies the key atomistic processes controlling the early stages of formation of thin films, which can be used to tailor deposition conditions in order to achieve films with unique properties and applications.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2019. p. 46
Series
Linköping Studies in Science and Technology. Licentiate Thesis, ISSN 0280-7971 ; 1830
National Category
Nano Technology
Identifiers
urn:nbn:se:liu:diva-154428 (URN)10.3384/lic.diva-154428 (DOI)9789176851449 (ISBN)
Presentation
2019-02-15, Schrödinger, E324, Fysikhuset, Campus Valla, Linköping, 13:15 (English)
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Available from: 2019-02-11 Created: 2019-02-11 Last updated: 2019-06-28Bibliographically approved

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