We present evidence for compressive stress generation via atom insertion into grain boundaries in polycrystalline Mo thin films deposited using energetic vapor fluxes (<∼120 eV). Intrinsic stress magnitudes between −3 and +0.2 GPa are obtained with a nearly constant stress-free lattice parameter marginally larger (0.12%) than that of bulk Mo. This, together with a correlation between large compressive film stresses and high film densities, implies that the compressive stress is not caused by defect creation in the grains but by grain boundary densification. Two mechanisms for diffusion of atoms into grain boundaries and grain boundary densification are suggested.

Funding Agencies|COST Action|MP0804|Linkoping University.

The previous status of this article was Manuscript and the working title was Atomistic mechanisms leading to adatom insertion into grain boundaries and stress generation in physically vapor deposited films.

The initial formation stages (i.e., island nucleation, island growth, and island coalescence) set characteristic length scales during growth of thin films from the vapor phase. They are, thus, decisive for morphological and microstructural features of films and nanostructures. Each of the initial formation stages has previously been wellinvestigated separately for the case of Volmer-Weber growth, but knowledge on how and to what extent each stage individually and all together affect the microstructural evolution is still lacking. Here we address this question using growth of Ag on SiO 2 from pulsed vapor fluxes as a case study. By combining in situ growth monitoring, ex situ imaging and growth simulations we systematically study the growth evolution all the way from nucleation to formation of a continuous film and establish the effect of the vapor flux time domain on the scaling behaviour of characteristic growth transitions (elongation transition, percolation and continuous film formation). Our data reveal a pulsing frequency dependence for the characteristic film growth transitions, where the nominal transition thickness decreases with increasing pulsing frequency up to a certain value after which a steady-state behaviour is observed. The scaling behaviour is shown to result from differences in island sizes and densities, as dictated by the initial film formation stages. These differences are determined solely by the interplay between the characteristics of the vapor flux and time required for island coalescence to be completed. In particular, our data provide evidence that the steady-state scaling regime of the characteristic growth transitions is caused by island growth that hinders coalescence from being completed.

We have developed a kinetic model for residual stress generation in thin films grown from energetic vapor fluxes, encountered, e.g., during sputter deposition. The new analytical model considers sub-surface point defects created by atomic peening, along with processes treated in already existing stress models for non-energetic deposition, i.e., thermally activated diffusion processes at the surface and the grain boundary. According to the new model, ballistically induced sub-surface defects can get incorporated as excess atoms at the grain boundary, remain trapped in the bulk, or annihilate at the free surface, resulting in a complex dependence of the steady-state stress on the grain size, the growth rate, as well as the energetics of the incoming particle flux. We compare calculations from the model with in situ stress measurements performed on a series of Mo films sputter-deposited at different conditions and having different grain sizes. The model is able to reproduce the observed increase of compressive stress with increasing growth rate, behavior that is the opposite of what is typically seen under non-energetic growth conditions. On a grander scale, this study is a step towards obtaining a comprehensive understanding of stress generation and evolution in vapor deposited polycrystalline thin films.

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International audienceIntrinsic stresses in vapor deposited thin films have been a topic of considerable scientific and technological interest owing to their importance for functionality and performance of thin film devices. The origin of compressive stresses typically observed during deposition of polycrystalline metal films at conditions that result in high atomic mobility has been under debate in the literature in the course of the past decades. In this study, we contribute towards resolving this debate by investigating the grain size dependence of compressive stress magnitude in dense polycrystalline Mofilmsgrown by magnetron sputtering. Although Mo is a refractory metal and hence exhibits an intrinsically low mobility, low energy ion bombardment is used during growth to enhance atomic mobility and densify the grain boundaries. Concurrently, the lateral grain size is controlled by using appropriate seed layers on which Mofilms are grown epitaxially. The combination of in situ stress monitoring with ex situ microstructural characterization reveals a strong, seemingly linear, increase of the compressive stress magnitude on the inverse grain size and thus provides evidence that compressive stress is generated in the grain boundaries of the film. These results are consistent with models suggesting that compressive stresses in metallic filmsdeposited at high homologous temperatures are generated by atom incorporation into and densification of grain boundaries. However, the underlying mechanisms for grain boundary densification might be different from those in the present study where atomic mobility is intrinsically lo

The tilt of the columnar microstructure has been studied for Cu and Cr thin films grown offnormally using highly ionized vapor fluxes, generated by the deposition technique high power impulse magnetron sputtering. It is found that the relatively large column tilt (with respect to the substrate normal) observed for Cu films decreases as the ionization degree of the deposition flux increases. On the contrary, Cr columns are found to grow relatively close to the substrate normal and the column tilt is independent from the ionization degree of the vapor flux when films are deposited at room temperature. The Cr column tilt is only found to be influenced by the ionized fluxes when films are grown at elevated temperatures, suggesting that film morphology during the film nucleation stage is also important in affecting column tilt. A phenomenological model that accounts for the effect of atomic shadowing at different nucleation conditions is suggested to explain the results. V C 2013 AIP Publishing LLC. [http://dx

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We present a brief review on the use of ionized and pulsed vapour fluxes, primarily generated by high power impulse magnetron sputtering (HiPIMS) discharges, as tools to gain atomistic understanding on film nucleation and growth. Two case studies are considered; the first case study concerns stress generation in polycrystalline films. It is highlighted that by using vapour fluxes of well-controlled ion content and ion energy and by studying the film microstructure and intrinsic stresses one can obtain experimental evidence for stress generation by insertion of film forming species in the grain boundaries. In the second case study it is discussed how the use of pulsed vapour fluxes with well controlled time domain can facilitate understanding of growth dynamics and microstructural evolution in thin films grown in three-dimensional (i.e., Volmer-Weber) fashion. Broader implications of the described research strategies for the surface science and surface engineering communities are highlighted and discussed.2