The issue of stress in thin films and functional coatings is a persistent problem in materials science and technology that has congregated many efforts, both from experimental and fundamental points of view, to get a better understanding on how to deal with, how to tailor, and how to manage stress in many areas of applications. With the miniaturization of device components, the quest for increasingly complex film architectures and multiphase systems and the continuous demands for enhanced performance, there is a need toward the reliable assessment of stress on a submicron scale from spatially resolved techniques. Also, the stress evolution during film and coating synthesis using physical vapor deposition (PVD), chemical vapor deposition, plasma enhanced chemical vapor deposition (PECVD), and related processes is the result of many interrelated factors and competing stress sources so that the task to provide a unified picture and a comprehensive model from the vast amount of stress data remains very challenging. This article summarizes the recent advances, challenges, and prospects of both fundamental and applied aspects of stress in thin films and engineering coatings and systems, based on recent achievements presented during the 2016 Stress Workshop entitled “Stress Evolution in Thin Films and Coatings: from Fundamental Understanding to Control.” Evaluation methods, implying wafer curvature, x-ray diffraction, or focused ion beam removal techniques, are reviewed. Selected examples of stress evolution in elemental and alloyed systems, graded layers, and multilayer-stacks as well as amorphous films deposited using a variety of PVD and PECVD techniques are highlighted. Based on mechanisms uncovered by in situ and real-time diagnostics, a kinetic model is outlined that is capable of reproducing the dependence of intrinsic (growth) stress on the grain size, growth rate, and deposited energy. The problems and solutions related to stress in the context of optical coatings, inorganic coatings on plastic substrates, and tribological coatings for aerospace applications are critically examined. This review also suggests strategies to mitigate excessive stress levels from novel coating synthesis perspectives to microstructural design approaches, including the ability to empower crack-based fabrication processes, pathways leading to stress relaxation and compensation, as well as management of the film and coating growth conditions with respect to energetic ion bombardment. Future opportunities and challenges for stress engineering and stress modeling are considered and outlined.

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We use a combined experimental and theoretical approach to study the rates of surface diffusion processes that govern early stages of thin Ag and Cu film morphological evolution on weakly-interacting amorphous carbon substrates. Films are deposited by magnetron sputtering, at temperatures T S between 298 and 413 K , and vapor arrival rates F in the range 0.08 to 5.38 monolayers / s . By employing in situ and real-time sheet-resistance and wafer-curvature measurements, we determine the nominal film thickness Θ at percolation (Θ perc ) and continuous film formation (Θ cont ) transition. Subsequently, we use the scaling behavior of Θ perc and Θ cont as a function of F and T s , to estimate, experimentally, the temperature-dependent diffusivity on the substrate surface, from which we calculate Ag and Cu surface migration energy barriers and attempt frequencies . By critically comparing and with literature data, as well as with results from our ab initio molecular dynamics simulations for single Ag and Cu adatom diffusion on graphite surfaces, we suggest that: (i) and correspond to diffusion of multiatomic clusters, rather than to diffusion of monomers; and (ii) the mean size of mobile clusters during Ag growth is larger compared to that of Cu. The overall results of this work pave the way for studying growth dynamics in a wide range of technologically-relevant weakly-interacting film/substrate systems—including metals on 2D materials and oxides—which are building blocks in next-generation nanoelectronic, optoelectronic, and catalytic devices.

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The ability to reverse the inherent tendency of noble metals to grow in an uncontrolled three-dimensional (3D) fashion on weakly interacting substrates, including two-dimensional (2D) materials and oxides, is essential for the fabrication of high-quality multifunctional metal contacts in key enabling devices. In this study, we show that this can be effectively achieved by deploying nitrogen (N2) gas with high temporal precision during magnetron sputtering of nanoscale silver (Ag) islands and layers on silicon dioxide (SiO2) substrates. We employ real-time in situ film growth monitoring using spectroscopic ellipsometry, along with optical modeling in the framework of the finite-difference time-domain method, and establish that localized surface plasmon resonance (LSPR) from nanoscale Ag islands can be used to gauge the evolution of surface morphology of discontinuous layers up to a SiO2 substrate area coverage of ∼70%. Such analysis, in combination with data on the evolution of room-temperature resistivity of electrically conductive layers, reveals that presence of N2 in the sputtering gas atmosphere throughout all film-formation stages: (i) promotes 2D growth and smooth film surfaces and (ii) leads to an increase of the continuous-layer electrical resistivity by ∼30% compared to Ag films grown in a pure argon (Ar) ambient atmosphere. Detailed ex situ nanoscale structural analyses suggest that N2 favors 2D morphology by suppressing island coalescence rates during initial growth stages, while it causes interruption of local epitaxial growth on Ag crystals. Using these insights, we deposit Ag layers by deploying N2 selectively, either during the early precoalescence growth stages or after coalescence completion. We show that early N2 deployment leads to 2D morphology without affecting the Ag-layer resistivity, while postcoalescence introduction of N2 in the gas atmosphere further promotes formation of three-dimensional (3D) nanostructures and roughness at the film growth front. In a broader context this study generates knowledge that is relevant for the development of (i) single-step growth manipulation strategies based on selective deployment of surfactant species and (ii) real-time methodologies for tracking film and nanostructure morphological evolution using LSPR.

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.

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