A correlation is established between the macro-scale friction regimes of metals and a transition between two dominant atomistic mechanisms of deformation. Metals tend to exhibit bi-stable friction behavior --low and converging or high and diverging. These general trends in behavior are shown to be largely explained using a simplified model based on grain size evolution, as a function of contact stress and temperature, and are demonstrated for pure copper and gold. Specifically, the low friction regime is linked to the formation of ultra-nanocrystalline surface films (10 to 20 nm), driving toward shear accommodation by grain boundary sliding. Above a critical combination of stress and temperature --demonstrated to be a material property --shear accommodation transitions to dislocation dominated plasticity and high friction. We utilize a combination of experimental and computational methods to develop and validate the proposed structure-property relationship. This quantitative framework provides a shift from phenomenological to mechanistic and predictive fundamental understanding of friction for crystalline materials, including engineering alloys.

This work demonstrates the role of microstructure in the friction and oxidation behavior of the lamellar solid lubricant molybdenum disulfide (MoS). We report on systematic investigations of oxidation and friction for two MoS films with distinctively different microstructures-amorphous and planar/highly-ordered-before and after exposure to atomic oxygen (AO) and high-temperature (250 °C) molecular oxygen. A combination of experimental tribology, molecular dynamics simulations, X-ray photoelectron spectroscopy (XPS), and high-sensitivity low-energy ion scattering (HS-LEIS) was used to reveal new insights about the links between structure and properties of these widely utilized low-friction materials. Initially, ordered MoS films showed a surprising resistance to both atomic and molecular oxygens (even at elevated temperature), retaining characteristic low friction after exposure to extreme oxidative environments. XPS shows comparable oxidation of both coatings via AO; however, monolayer resolved compositional depth profiles from HS-LEIS reveal that the microstructure of the ordered coatings limits oxidation to the first atomic layer.

Recent work suggests that thermally stable nanocrystallinity in metals is achievable in several binary alloys by modifying grain boundary energies via solute segregation. The remarkable thermal stability of these alloys has been demonstrated in recent reports, with many alloys exhibiting negligible grain growth during prolonged exposure to near-melting temperatures. Pt-Au, a proposed stable alloy consisting of two noble metals, is shown to exhibit extraordinary resistance to wear. Ultralow wear rates, less than a monolayer of material removed per sliding pass, are measured for Pt-Au thin films at a maximum Hertz contact stress of up to 1.1 GPa. This is the first instance of an all-metallic material exhibiting a specific wear rate on the order of 10 mm N m , comparable to diamond-like carbon (DLC) and sapphire. Remarkably, the wear rate of sapphire and silicon nitride probes used in wear experiments are either higher or comparable to that of the Pt-Au alloy, despite the substantially higher hardness of the ceramic probe materials. High-resolution microscopy shows negligible surface microstructural evolution in the wear tracks after 100k sliding passes. Mitigation of fatigue-driven delamination enables a transition to wear by atomic attrition, a regime previously limited to highly wear-resistant materials such as DLC.

From the context of a contemporary understanding of the phenomenological origins of friction and wear of materials, we review insightful contributions from recent experimental investigations of three classes of materials that exhibit uniquely contrasting tribological behaviors: metals, polymers, and ionic solids. We focus on the past decade of research by the community to better understand the correlations between environment parameters, materials properties, and tribological behavior in systems of increasingly greater complexity utilizing novel synthesis and in situ experimental techniques. In addition to such review, and a half-century after seminal publications on the subject, we present recently acquired evidence linking anisotropy in friction response with anisotropy in wear behavior of crystalline ionic solids as a function of crystallographic orientation. Although the tribological behaviors of metals, polymers, and ionic solids differ widely, it is increasingly more evident that the mechanistic origins (such as fatigue, corrosion, abrasion, and adhesion) are essentially the same. However, we hope to present a clear and compelling argument favoring the prominent and irreplaceable role of in situ experimental techniques as a bridge between fundamental atomistic and molecular processes and emergent behaviors governing tribological contacts. 395 Annu. Rev. Mater. Res. 2014.44:395-427. Downloaded from www.annualreviews.org Access provided by University of Utah -Marriot Library on 11/27/14. For personal use only.

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Studies to explore the nature of friction, and in particular thermally activated friction in macroscopic tribology, have lead to a series of experiments on thin coatings of molybdenum disulfide. Coatings of predominately molybdenum disulfide were selected for these experiments; five different coatings were used: MoS 2 /Ni, . The temperatures were varied over a range from -80°C to 180°C. The friction coefficients tended to increase with decreasing temperature. Activation energies were estimated to be between 2 and 10 kJ/mol from data fitting with an Arrhenius function. Subsequent room temperature wear rate measurements of these films under dry nitrogen conditions at ambient temperature demonstrated that the steady-state wear behavior of these coatings varied dramatically over a range of K = 7 9 10 -6 to 2 9 10 -8 mm 3 /(Nm). It was further shown that an inverse relationship between wear rate and the sensitivity of friction coefficient with temperature exists. The highest wearrate coatings showed nearly athermal friction behavior, while the most wear resistant coatings showed thermally activated behavior. Finally, it is hypothesized that thermally activated behavior in macroscopic tribology is reserved for systems with stable interfaces and ultra-low wear, and athermal behavior is characteristic to systems experiencing gross wear.

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