Angstrom-Scale Transparent Overcoats: Interfacial Nitrogen-Driven Atomic Intermingling Promotes Lubricity and Surface Protection of Ultrathin Carbon.

Lubricity, a phenomenon which enables the ease of motion of objects, and wear resistance, which minimizes material damage or degradation, are important fundamental characteristics for sustainable technology developments. Ultrathin coatings that promote lubricity and wear resistance are of huge importance for a number of applications, including magnetic storage and micro-/nanoelectromechanical systems. Conventional ultrathin coatings have, however, reached their limit. Graphene-based materials that have shown promise to reduce friction and wear have many intrinsic limitations such as high temperature and substrate-specific growth. To address these concerns, a great deal of research is currently ongoing to optimize graphene-based materials. Here we discover that angstrom-thick carbon (8 Å) significantly reduces interfacial friction and wear. This lubricant shows ultrahigh optical transparency and can be directly deposited on a wide range of surfaces at room temperature. Experiments combined with molecular dynamics simulations reveal that the lubricating efficacy of 8 Å carbon is further improved via interfacial nitrogen.

Slippery and Wear-Resistant Surfaces Enabled by Interface Engineered Graphene.

Friction and wear remain the primary cause of mechanical energy dissipation and system failure. Recent studies reveal graphene as a powerful solid lubricant to combat friction and wear. Most of these studies have focused on nanoscale tribology and have been limited to a few specific surfaces. Here, we uncover many unknown aspects of graphene's contact-sliding at micro- and macroscopic tribo-scales over a broader range of surfaces. We discover that graphene's performance reduces for surfaces with increasing roughness. To overcome this, we introduce a new type of graphene/silicon nitride (SiNx, 3 nm) bilayer overcoats that exhibit superior performance compared to native graphene sheets (mono and bilayer), that is, display the lowest microscale friction and wear on a range of tribologically poor flat surfaces. More importantly, two-layer graphene/SiNx bilayer lubricant (<4 nm in total thickness) shows the highest macroscale wear durability on tape-head (topologically variant surface) that exceeds most previous thicker (∼7-100 nm) overcoats. Detailed nanoscale characterization and atomistic simulations explain the origin of the reduced friction and wear arising from these nanoscale coatings. Overall, this study demonstrates that engineered graphene-based coatings can outperform conventional coatings in a number of technologies.

Characterization of C-apertures in a successful demonstration of heat-assisted magnetic recording.

An optical pump-probe setup was used to measure the coercivity change in a heat-assisted magnetic recording (HAMR) medium. The incident optical power required to attain the Curie temperature of the medium was determined by calculating its coercivity from BH loops under different illuminating laser powers through use of the Kerr signal in the pump-probe setup. The HAMR medium was then illuminated through an array of square and C-shaped nanoapertures so that the necessary laser power required for magnetic reversal could be compared to the bulk case. Magnetic force microscopy and Kerr microscopy revealed that C-apertures were able to permit heating of the magnetic medium and lower the coercivity to achieve magnetic reversal whereas the square apertures were not. The results show that aperture shape and design play a large role in HAMR head designs.

Boosting contact sliding and wear protection via atomic intermixing and tailoring of nanoscale interfaces.

Friction and wear cause energy wastage and system failure. Usually, thicker overcoats serve to combat such tribological concerns, but in many contact sliding systems, their large thickness hinders active components of the systems, degrades functionality, and constitutes a major barrier for technological developments. While sub-10-nm overcoats are of key interest, traditional overcoats suffer from rapid wear and degradation at this thickness regime. Using an enhanced atomic intermixing approach, we develop a ~7- to 8-nm-thick carbon/silicon nitride (C/SiN x ) multilayer overcoat demonstrating extremely high wear resistance and low friction at all tribological length scales, yielding ~2 to 10 times better macroscale wear durability than previously reported thicker (~20 to 100 nm) overcoats on tape drive heads. We report the discovery of many fundamental parameters that govern contact sliding and reveal how tuning atomic intermixing at interfaces and varying carbon and SiN x thicknesses strongly affect friction and wear, which are crucial for advancing numerous technologies.

Superior wear resistance and low friction in hybrid ultrathin silicon nitride/carbon films: synergy of the interfacial chemistry and carbon microstructure.

Amorphous carbon-based films are commonly investigated as protective nanocoatings in macro- to nano-scale devices due to their exceptional tribological and mechanical properties. However, with further device miniaturization where even thinner coatings are required, the wear durability of the nanocoating rapidly degrades at the expense of lower thickness. Here we discover that for sub-10 nm coating thicknesses, a hybrid bi-layer film structure, comprising a high sp3-bonded amorphous carbon top layer and a silicon nitride (SiNx) bottom layer, consistently outperforms its single-layer amorphous carbon counterpart in terms of wear durability on a commercial tape drive head, while exhibiting low, stable friction and excellent wear resistance on a flat ceramic substrate. The superior performance of the hybrid film is attributed to the constructive synergy of the sp3-rich carbon microstructure and an enhanced interfacial chemistry arising from additional interfacial bonding. Moreover, a high energy C+ ion treatment step, introduced either directly to the substrate or to the SiNx layer before carbon deposition, also aids in increasing atomic mixing that contributes to further improvement in the wear resistance. This study highlights the importance of both the carbon microstructure and interfacial chemistry in the design of wear-durable nanocoatings at few-nanometer thicknesses, particularly for aggressive wear conditions.

Atomic Scale Interface Manipulation, Structural Engineering, and Their Impact on Ultrathin Carbon Films in Controlling Wear, Friction, and Corrosion.

Reducing friction, wear, and corrosion of diverse materials/devices using <2 nm thick protective carbon films remains challenging, which limits the developments of many technologies, such as magnetic data storage systems. Here, we present a novel approach based on atomic scale interface manipulation to engineer and control the friction, wear, corrosion, and structural characteristics of 0.7-1.7 nm carbon-based films on CoCrPt:oxide-based magnetic media. We demonstrate that when an atomically thin (∼0.5 nm) chromium nitride (CrNx) layer is sandwiched between the magnetic media and an ultrathin carbon overlayer (1.2 nm), it modifies the film-substrate interface, creates various types of interfacial bonding, increases the interfacial adhesion, and tunes the structure of carbon in terms of its sp(3) bonding. These contribute to its remarkable functional properties, such as stable and lowest coefficient of friction (∼0.15-0.2), highest wear resistance and better corrosion resistance despite being only ∼1.7 nm thick, surpassing those of ∼2.7 nm thick current commercial carbon overcoat (COC) and other overcoats in this work. While this approach has direct implications for advancing current magnetic storage technology with its ultralow thickness, it can also be applied to advance the protective and barrier capabilities of other ultrathin materials for associated technologies.

Correlation of nanoscale behaviour of forces and macroscale surface wettability.

In this manuscript, we demonstrate a method based on atomic force microscopy which enables local probing of surface wettability. The maximum pull-off force, obtained from force spectroscopy shows a remarkable correlation with the macroscopically observed water contact angle, measured over a wide variety of surfaces starting from hydrophilic, all the way through to hydrophobic ones. This relationship, consequently, facilitates the establishment of a universal behaviour. The adhesion forces scale with the polar component of surface energy. However, no such relation could be established with the dispersive component. Hence, we postulate that the force(s) which enable us to correlate the force spectroscopy data measured on the nanoscale to the macroscopic contact angle are primarily arising from electrostatic-dipole-dipole interactions at the solid-liquid interface. London forces play less of a role. This effect in is line with density functional theory (DFT) calculations suggesting a higher degree of hydroxylation of hydrophilic surfaces. This result shows that molecular simulations and measurements on an atomic scale can be extrapolated to macroscopic surface wetting problems.

Magnetization reversal using excitation of collective modes in nanodot matrices.

The large arrays of magnetic dots are the building blocks of magnonic crystals and the emerging bit patterned media for future recording technology. In order to fully utilize the functionalities of high density magnetic nanodots, a method for the selective reversal of a single nanodot in a matrix of dots is desired. We have proposed a method for magnetization reversal of a single nanodot with microwave excitation in a matrix of magneto-statically interacting dots. The method is based on the excitation of collective modes and the spatial anomaly in the microwave power absorption. We perform numerical simulations to demonstrate the possibility of switching a single dot from any initial state of a 3 by 3 matrix of dots, and develop a theoretical model for the phenomena. We discuss the applicability of the proposed method for introducing defect modes in magnonic crystals as well as for future magnetic recording.

Time-resolved imaging of pulse-induced magnetization reversal with a microwave assist field.

The reversal of the magnetization under the influence of a field pulse has been previously predicted to be an incoherent process with several competing phenomena such as domain wall relaxation, spin wave-mediated instability regions, and vortex-core mediated reversal dynamics. However, there has been no study on the direct observation of the switching process with the aid of a microwave signal input. We report a time-resolved imaging study of magnetization reversal in patterned magnetic structures under the influence of a field pulse with microwave assistance. The microwave frequency is varied to demonstrate the effect of resonant microwave-assisted switching. We observe that the switching process is dominated by spin wave dynamics generated as a result of magnetic instabilities in the structures, and identify the frequencies that are most dominant in magnetization reversal.

Ultrathin Carbon with Interspersed Graphene/Fullerene-like Nanostructures: A Durable Protective Overcoat for High Density Magnetic Storage.

One of the key issues for future hard disk drive technology is to design and develop ultrathin (<2 nm) overcoats with excellent wear- and corrosion protection and high thermal stability. Forming carbon overcoats (COCs) having interspersed nanostructures by the filtered cathodic vacuum arc (FCVA) process can be an effective approach to achieve the desired target. In this work, by employing a novel bi-level surface modification approach using FCVA, the formation of a high sp(3) bonded ultrathin (~1.7 nm) amorphous carbon overcoat with interspersed graphene/fullerene-like nanostructures, grown on magnetic hard disk media, is reported. The in-depth spectroscopic and microscopic analyses by high resolution transmission electron microscopy, scanning tunneling microscopy, time-of-flight secondary ion mass spectrometry, and Raman spectroscopy support the observed findings. Despite a reduction of ~37% in COC thickness, the FCVA-processed thinner COC (~1.7 nm) shows promising functional performance in terms of lower coefficient of friction (~0.25), higher wear resistance, lower surface energy, excellent hydrophobicity and similar/better oxidation corrosion resistance than current commercial COCs of thickness ~2.7 nm. The surface and tribological properties of FCVA-deposited COC was further improved after deposition of lubricant layer.

Strain-enhanced tunneling magnetoresistance in MgO magnetic tunnel junctions.

While the effects of lattice mismatch-induced strain, mechanical strain, as well as the intrinsic strain of thin films are sometimes detrimental, resulting in mechanical deformation and failure, strain can also be usefully harnessed for applications such as data storage, transistors, solar cells, and strain gauges, among other things. Here, we demonstrate that quantum transport across magnetic tunnel junctions (MTJs) can be significantly affected by the introduction of controllable mechanical strain, achieving an enhancement factor of ~2 in the experimental tunneling magnetoresistance (TMR) ratio. We further correlate this strain-enhanced TMR with coherent spin tunneling through the MgO barrier. Moreover, the strain-enhanced TMR is analyzed using non-equilibrium Green's function (NEGF) quantum transport calculations. Our results help elucidate the TMR mechanism at the atomic level and can provide a new way to enhance, as well as tune, the quantum properties in nanoscale materials and devices.

Effect of angstrom-scale surface roughness on the self-assembly of polystyrene-polydimethylsiloxane block copolymer.

Self-assembly of block copolymers has been identified as a potential candidate for high density fabrication of nanostructures. However, the factors affecting its reliability and reproducibility as a patterning technique on various kinds of surfaces are not well-established. Studies pertaining to block copolymer self-assembly have been confined to ultra-flat substrates without taking into consideration the effect of surface roughness. Here, we show that a slight change in the angstrom-scale roughness arising from the surface of a material creates a profound effect on the self-assembly of polystyrene-polydimethylsiloxane block copolymer. Its self-assembly was found to be dependent on both the root mean square roughness (R(rms)) of the surface and the type of solvent annealing system used. It was observed that surface with R(rms)< 5.0 Å showed self-assembly. Above this value, the kinetic hindrance posed by the surface roughness on the block copolymer leads to its conforming to the surface without observable phase separation.