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Atomic arrangement in immiscible Ag-Cu alloys synthesized far-from-equilibrium
Linköping University, Department of Physics, Chemistry and Biology, Nanoscale engineering. Linköping University, Faculty of Science & Engineering.ORCID iD: 0000-0003-4811-478X
Linköping University, Department of Physics, Chemistry and Biology, Nanoscale engineering. Linköping University, Faculty of Science & Engineering.
Linköping University, Department of Physics, Chemistry and Biology, Nanoscale engineering. Linköping University, Faculty of Science & Engineering.
Linköping University, Department of Physics, Chemistry and Biology, Plasma and Coating Physics. Linköping University, Faculty of Science & Engineering.ORCID iD: 0000-0002-6602-7981
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2016 (English)In: Acta Materialia, ISSN 1359-6454, E-ISSN 1873-2453, Vol. 110, 114-121 p.Article in journal (Refereed) Published
Resource type
Text
Abstract [en]

Physical attributes of multicomponent materials of a given chemical composition are determined by atomic arrangement at property-relevant length scales. A potential route to access a vast array of atomic configurations for material property tuning is by synthesis of multicomponent thin films using vapor fluxes with their deposition pattern modulated in the sub-monolayer regime. However, the applicability of this route for creating new functional materials is impeded by the fact that a fundamental understanding of the combined effect of sub-monolayer flux modulation, kinetics and thermodynamics on atomic arrangement is not available in the literature. Here we present a research strategy and verify its viability for addressing the aforementioned gap in knowledge. This strategy encompasses thin film synthesis using a route that generates multi-atomic fluxes with sub-monolayer resolution and precision over a wide range of experimental conditions, deterministic growth simulations and nanoscale micro structural probes. Investigations are focused on structure formation within the archetype immiscible Ag-Cu binary system, revealing that atomic arrangement at different length scales is governed by the arrival pattern of the film forming species, in conjunction with diffusion of near-surface Ag atoms to encapsulate 3D Cu islands growing on 2D Ag layers. The knowledge generated and the methodology presented herein provides the scientific foundation for tailoring atomic arrangement and physical properties in a wide range of miscible and immiscible multinary systems. (C) 2016 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Place, publisher, year, edition, pages
PERGAMON-ELSEVIER SCIENCE LTD , 2016. Vol. 110, 114-121 p.
Keyword [en]
Ag-Cu thin films; MD simulations; Modulated vapor fluxes; Nonequilibrium synthesis; Immiscible alloys
National Category
Physical Sciences
Identifiers
URN: urn:nbn:se:liu:diva-128722DOI: 10.1016/j.actamat.2016.03.023ISI: 000374810400012OAI: oai:DiVA.org:liu-128722DiVA: diva2:932361
Note

Funding Agencies|Linkoping University [Dnr-LiU-2015-01510]; Swedish Research Council [VR 621-2011-5312]; AForsk through the project "Towards Next Generation of Energy Saving Windows"

Available from: 2016-06-01 Created: 2016-05-30 Last updated: 2016-11-30
In thesis
1. Nanoscale structure forming processes: Metal thin films grown far-from-equilibrium
Open this publication in new window or tab >>Nanoscale structure forming processes: Metal thin films grown far-from-equilibrium
2016 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Thin film growth from the vapor phase has for a long time intrigued researchers endeavouring to unravel and understand atomistic surface processes that govern film formation. Their motivation has not been purely scientific, but also driven by numerous applications where this understanding is paramount to knowledge-based design of novel film materials with tailored properties.

Within the above framework, this thesis investigates growth of metal films on weakly bonding substrates, a combination of great relevance for applications concerning e.g., catalysis, graphene metallization and architectural glazing. When metal vapor condenses on weakly bonding substrates three dimensional islands nucleate, grow and coalesce prior to forming a continuous film. The combined effect of these initial growth stages on film formation and morphology evolution is studied using pulsed vapor fluxes for the model system Ag/SiO2. It is shown that the competition between island growth and coalescence completion determines structure evolution. The effect of the initial growth stages on film formation is also examined for the tilted columnar microstructure obtained when vapor arrives at an angle that deviates from the substrate surface normal. This is done using two metals with distinctly different nucleation behaviour, and the findings suggest that the column tilt angle is set by nucleation conditions in conjunction with shadowing of the vapor flux by adjacent islands. Vapor arriving at an angle can in addition result in films that exhibit preferred crystallographic orientations, both out-of-plane and in-plane. Their emergence is commonly described by an evolutionary growth model, which for some materials predict a double in-plane alignment that has not been observed experimentally. Here, an experiment is designed to replicate the model’s growth conditions, confirming the existence of double in-plane alignment.

New and added film functionalities can further be unlocked by alloying. Properties are then largely set by chemistry and atomic arrangement, where the latter can be affected by thermodynamics, kinetics and vapor flux modulation. Their combined effect on atomic arrangement is here unravelled by presenting a research methodology that encompasses high resolution vapor flux modulation, nanoscale structure v vi probes and growth simulations. The methodology is deployed to study the immiscible Ag-Cu and miscible Ag-Au model systems, for which it is shown that capping of Cu by Ag atoms via near surface diffusion processes and rough morphology of the Ag-Au growth front are the decisive structure forming processes in each respective system.

The results generated in this thesis are of relevance for tuning structure of metal films grown on weakly bonding substrates. They also indicate that improved growth models are required to accurately describe structure evolution and emergence of a preferred in-plane orientation in films where vapor arrives at an angle that deviates from the substrate surface normal. In addition, this thesis presents a methodology that can be used to identify and understand structure forming processes in multicomponent films, which may enable tailoring of atomic arrangement and related properties in technologically relevant material systems.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2016. 71 p.
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1804
National Category
Inorganic Chemistry Other Materials Engineering Other Physics Topics Materials Chemistry Condensed Matter Physics
Identifiers
urn:nbn:se:liu:diva-132895 (URN)10.3384/diss.diva-132895 (DOI)9789176856390 (ISBN)
Public defence
2017-01-20, Planck, Fysikhuset, Campus Valla, Linköping, 09:15 (English)
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Available from: 2016-11-30 Created: 2016-11-30 Last updated: 2016-11-30Bibliographically approved

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