Time-dependent analysis of agglomerating Pt thin films on YSZ single crystals

Henning Galinski; Thomas Ryll; Lukas Schlagenhauf; Iwan Schenker; Ralph Spolenak; Ludwig J. Gauckler

doi:10.1016/j.crhy.2013.06.007

Trends and perspectives in solid-state wetting / Mouillage solide–solide : tendances et perspectives

Time-dependent analysis of agglomerating Pt thin films on YSZ single crystals
[Analyse temporelle de lʼagglomération de films minces de Pt sur YSZ monocristallin]

Henning Galinski ^1,² ; Thomas Ryll ¹ ; Lukas Schlagenhauf ¹ ; Iwan Schenker ¹ ; Ralph Spolenak ² ; Ludwig J. Gauckler ^1,³

¹ Nonmetallic Inorganics Materials, Department of Materials, ETH Zurich, Wolfgang-Pauli-Str. 10, CH-8093 Zurich, Switzerland
² Laboratory of Nanometallurgy, Department of Materials, ETH Zurich, Wolfgang-Pauli-Str. 10, CH-8093 Zurich, Switzerland
³ International Institute for Carbon Neutral Energy Research (WPI-I2CNER), Kyushu University, 744 Moto-oka, Nishi-ku, Fukuoka 819-0395, Japan

Comptes Rendus. Physique, Volume 14 (2013) no. 7, pp. 590-600.

Résumé
Abstract

La nano-structuration de films minces par des mécanismes dʼinstabilités spatiales est une alternative potentielle aux processus traditionnels dits « top-down », comme par exemple la lithographie à faisceau dʼélectrons. Dans cette contribution, nous analysons la dynamique de la structuration de films minces par agglomération. Pour cela, des films minces de Pt dʼune épaisseur de 50 nm ont été déposées sur des substrats monocristallins de zircone yttriée (YSZ) par pulvérisation magnétronique. La déposition a été suivie dʼun traitement thermique à 1023 K pendant 10 à 130 minutes. Lʼévolution morphologique des films minces de Pt a été étudiée par microscopie électronique à balayage et par microscopie à force atomique. Cela a permis de déterminer la dynamique de croissance des cavités dans le film ainsi que des paramètres morphologiques comme la distance de corrélation latérale et les fonctionnelles de Minkowski. Lʼévolution morphologique obtenue expérimentalement a été comparée aux structures de films minces déterminées par des simulations de dynamique cellulaire. Trois observations ont été faites. (i) Le rayon des cavités dépend du temps t, avec un taux de croissance proportionnel à $t^{- \frac{3}{4}} [\log^{3} t]$ , ce qui est en accord avec la théorie dʼinstabilité de Srolovitz, décrivant la croissance de cavités dominée par une diffusion superficielle. (ii) Lʼévolution morphologique des films minces de Pt a été analysée en fonction du temps à lʼaide des mesures de Minkowski et de la distance de corrélation latérale. Une discontinuité de la distance de corrélation latérale couplée à la coalescence des cavités a été trouvée, ainsi quʼune déviation significative des fonctionnelles de Minkowski du comportement gaussien attendu. (iii) En utilisant lʼéquation de Ginzburg–Landau comme équation de diffusion fondamentale, les simulations de dynamique cellulaire ont permis de reproduire les morphologies des films minces pendant la phase initiale de lʼagglomération.

The controlled assembly of nanostructures via shape instability mechanisms is a potential alternative to traditional top-down processes like e-beam lithography for nanostructuring surfaces. In this contribution, the dynamics of the nanostructuresʼ assembly via thin film agglomeration have been analyzed. Pt thin films with a thickness of 50 nm were deposited via magnetron sputtering on yttria-stabilized zirconia (YSZ) single crystals and subjected to heat treatments at 1023 K for times ranging from 10 to 130 min. The morphological evolution of Pt thin films has been investigated by means of scanning electron microscopy (SEM) and atomic force microscopy (AFM), obtaining the hole growth dynamics and morphological parameters like the lateral correlation length and the nanostructuresʼ Minkowski functionals. The experimentally obtained morphology evolution is compared to the simulated evolution of thin film structures resulting from a cell dynamical system (CDS) model. Three main observations have been made. (i) The hole radius is found to scale as function of time t with a rate proportional to $t^{- \frac{3}{4}} [\log^{3} t]$ . This is in agreement with Srolovitzʼs instability theory describing hole growth predominated by surface diffusion. (ii) The morphological evolution of the Pt thin films has been analyzed as function of time t by means of Minkowski measures and the lateral correlation length. A discontinuity in the lateral correlation length and a significant deviation of the Minkowski functionals from the expected Gaussian behavior was found to be coupled with the coalescence of holes. (iii) By using the Ginzburg–Landau equation for the description of the fundamental diffusion process, the CDS model allows a computational reproduction of the experimentally obtained film morphologies in the early stages of agglomeration.

Publié le : 2013-07-31

DOI : 10.1016/j.crhy.2013.06.007

Keywords: Agglomeration, Kinetics, Metal on ceramic, Pt, Zirconia, Cell dynamical system model
Mot clés : Agglomération, Cinétique, Métal sur céramique, Pt, Zircone, Simulation de dynamique cellulaire

Affiliations des auteurs :

Henning Galinski ^{1, 2} ; Thomas Ryll ¹ ; Lukas Schlagenhauf ¹ ; Iwan Schenker ¹ ; Ralph Spolenak ² ; Ludwig J. Gauckler ^{1, 3}

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     title = {Time-dependent analysis of agglomerating {Pt} thin films on {YSZ} single crystals},
     journal = {Comptes Rendus. Physique},
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     doi = {10.1016/j.crhy.2013.06.007},
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Henning Galinski; Thomas Ryll; Lukas Schlagenhauf; Iwan Schenker; Ralph Spolenak; Ludwig J. Gauckler. Time-dependent analysis of agglomerating Pt thin films on YSZ single crystals. Comptes Rendus. Physique, Volume 14 (2013) no. 7, pp. 590-600. doi : 10.1016/j.crhy.2013.06.007. https://comptes-rendus.academie-sciences.fr/physique/articles/10.1016/j.crhy.2013.06.007/

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