Vapor condensation on weakly interacting substrates leads to the formation of three-dimensional (3D) nanoscale islands (i.e., nanostructures). While it is widely accepted that this process is driven by minimization of the total film/substrate surface and interface energy, current film-growth theory cannot fully explain the atomic-scale mechanisms and pathways by which 3D island formation and morphological evolution occurs. Here, we use kinetic Monte Carlo simulations to describe the dynamic evolution of single-island shapes during deposition of Ag on weakly interacting substrates. The results show that 3D island shapes evolve in a self-similar manner, exhibiting a constant height-to-radius aspect ratio, which is a function of the growth temperature. Furthermore, our results reveal the following chain of atomic-scale events that lead to compact 3D island shapes: 3D nuclei are first formed due to facile adatom ascent at single-layer island steps, followed by the development of sidewall facets bounding the islands, which in turn facilitates upward diffusion from the base to the top of the islands. The limiting atomic process which determines the island height, for a given number of deposited atoms, is the temperature-dependent rate at which adatoms cross from sidewall facets to the island top. The overall findings of this study provide insights into the directed growth of metal nanostructures with controlled shapes on weakly interacting substrates, including two-dimensional crystals, for use in catalytic and nanoelectronic applications.

We employ sub-monolayer, pulsed Ag and Au vapor fluxes, along with deterministic growth simulations, and nanoscale probes to study structure formation in miscible Ag-Au films synthesized under far-from-equilibrium conditions. Our results show that nanoscale atomic arrangement is primarily determined by roughness build up at the film growth front, whereby larger roughness leads to increased intermixing between Ag and Au. These findings suggest a different structure formation pathway as compared to the immiscible Ag-Cu system for which the present study, in combination with previously published data, reveals that no significant roughness is developed, and the local atomic structure is predominantly determined by the tendency of Ag and Cu to phase-separate.

The elongation transition thickness (θElong) is a central concept in the theoretical description of thin-film growth dynamics on weakly interacting substrates via scaling relations of θElong with respect to rates of key atomistic film-forming processes. To date, these scaling laws have only been confirmed quantitatively by simulations, while experimental proof has been left ambiguous as it has not been possible to measure θElong. Here, we present a method for determining experimentally θElong for Ag films growing on amorphous SiO2: an archetypical weakly interacting film/substrate system. Our results confirm the theoretically predicted θElong scaling behavior, which then allow us to calculate the rates of adatom diffusion and island coalescence completion, in good agreement with the literature. The methodology presented herein casts the foundation for studying growth dynamics and cataloging atomistic-process rates for a wide range of weakly interacting film/substrate systems. This may provide insights into directed growth of metal films with a well-controlled morphology and interfacial structure on 2D crystals—including graphene and MoS2—for catalytic and nanoelectronic applications.

Controlling the relaxation of magnetization in magnetic nanostructures is key to optimizing magnetic storage device performance. This relaxation is governed by both intrinsic and extrinsic relaxation mechanisms and with the latter strongly dependent on the interactions between the nanostructures. In the present work we investigate laser induced magnetization dynamics in a broadband optical resonance type experiment revealing the role of interactions between nanostructures on the relaxation processes of granular magnetic structures. The results are corroborated by constructing a temperature dependent numerical micromagnetic model of magnetization dynamics based on the Landau-Lifshitz-Bloch equation. The model predicts a strong dependence of damping on the key material properties of coupled granular nanostructures in good agreement with the experimental data. We show that the intergranular, magnetostatic and exchange interactions provide a large extrinsic contribution to the damping. Finally we show that the mechanism can be attributed to an increase in spin-wave degeneracy with the ferromagnetic resonance mode as revealed by semianalytical spin-wave calculations.

Physical attributes of multicomponent materials of a given chemical composition are determined by atomic arrangement at property-relevant length scales. A potential route to access a vast array of atomic configurations for material property tuning is by synthesis of multicomponent thin films using vapor fluxes with their deposition pattern modulated in the sub-monolayer regime. However, the applicability of this route for creating new functional materials is impeded by the fact that a fundamental understanding of the combined effect of sub-monolayer flux modulation, kinetics and thermodynamics on atomic arrangement is not available in the literature. Here we present a research strategy and verify its viability for addressing the aforementioned gap in knowledge. This strategy encompasses thin film synthesis using a route that generates multi-atomic fluxes with sub-monolayer resolution and precision over a wide range of experimental conditions, deterministic growth simulations and nanoscale microstructural probes. Investigations are focused on structure formation within the archetype immiscible Ag-Cu binary system, revealing that atomic arrangement at different length scales is governed by the arrival pattern of the film forming species, in conjunction with diffusion of near-surface Ag atoms to encapsulate 3D Cu islands growing on 2D Ag layers. The knowledge generated and the methodology presented herein provides the scientific foundation for tailoring atomic arrangement and physical properties in a wide range of miscible and immiscible multinary systems.

The morphology and physical properties of thin films deposited by vapor condensation on solid surfaces are predominantly set by the processes of island nucleation, growth, and coalescence. When deposition is performed using pulsed vapor fluxes, three distinct nucleation regimes are known to exist depending on the temporal profile of the flux. These regimes can be accessed by tuning deposition conditions; however, their effect on film microstructure becomes marginal when coalescence sets in and erases morphological features obtained during nucleation. By preventing coalescence from being completed, these nucleation regimes can be used to control microstructure evolution and thus access a larger palette of film morphological features. Recently, we derived the quantitative criterion to stop coalescence during continuous metal vapor flux deposition on insulating surfaces—which typically yields 3-dimensional growth—by describing analytically the competition between island growth by atomic incorporation and the coalescence rate of islands [Lü et al., Appl. Phys. Lett. 105, 163107 (2014)]. Here, we develop the analytical framework for entering a coalescence-free growth regime for metal vapor deposition on insulating substrates using pulsed vapor fluxes, showing that there exist three distinct criteria for suppressing coalescence that correspond to the three nucleation regimes of pulsed vapor flux deposition. The theoretical framework developed herein is substantiated by kinetic Monte Carlo growth simulations. Our findings highlight the possibility of using atomistic nucleation theory for pulsed vapor deposition to control morphology of thin films beyond the point of island density saturation.

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.

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 well-investigated 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 SiO2 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.

The morphology of thin metal films and nanostructures synthesized from the vapor phase on insulating substrates is strongly influenced by the coalescence of islands. Here, we derive analytically the quantitative criterion for coalescence suppression by combining atomistic nucleation theory and a classical model of coalescence. Growth simulations show that using this criterion, a coalescence-free growth regime can be reached in which morphological evolution is solely determined by island nucleation, growth, and impingement. Experimental validation for the ability to control the rate of coalescence using this criterion and navigate between different growth regimes is provided by in situ monitoring of Ag deposition on SiO2. Our findings pave the way for creating thin films and nanostructures that exhibit a wide range of morphologies and physical attributes in a knowledge-based manner.

Angle-dependent x-ray magnetic circular dichroism at the Co L-2.3 edges has been utilized to systematically study Co80Pt20 : WO3 perpendicular magnetic recording thin films, in which the magnetocrystalline anisotropy significantly drops as the oxide volume fraction increases. The microscopic origin of this phenomenon in the studied films can be mainly attributed to an increase in orbital moment normal to the grain-oxide interface, with increasing oxide volume fraction, which arises from a more pronounced effect of symmetry breaking at the grain-oxide interface in smaller grains.

The phase transformation and the exchange coupling in (Ndo095Lao005)9.5FebaICOsNb 2BI05 have been investigated. Nanocomposites were obtained by treating amorphous precursors at temperatures ranging from 650TC to 9500C for 10 minutes. The magnetic properties were characterized via the vibrating sample magnetometer (VSM). X-ray diffraction (XRD), thermomagnetic analysis (TMA), and transmission electron microscopy (TEM) were used to perform phase identification, measure grain size, and analyze phase distribution. The strength of the exchange coupling between the magnetically hard and soft phases in the corresponding nanocomposite was analyzed via the AM-versus-H plot. It was found that the remanence (Br), coercivity (Hci), and maximum energy product (BHmax) obtained were affected by the magnetic phases present as well as the grain size of constituent phases and their distribution. The optimal magnetic performance, BHm, occurred between 700°C to 750°C, where the crystallization has completed without excessive grain growth. TMA and TEM indicated that the system was composed of three phases at this point, Nd2(Fe Co) 14B, ca-Fe, and Fe3B. The exchange coupling interaction among these phases was consistently described via the AM-versus-H plot up to 750°C. The Br, Hci, and BHmax degraded severely when the thermal treatment temperature increased from 750°C. This degradation may be attributed to the grain growth of the main phases, from 45 to 68nm, and the development of precipitates, which grew from 5nm at 750°C to 12nm at 850°C. Moreover, the amount of the precipitates was found to increase with the thermal treatment temperatures. The precipitates, presumably borides, may cause a decrease in the amount of the a-Fe and Fe 3B and result in a redistribution of the Co in the nanocomposites. The increase of the Co content in the Nd 2(Fe Co) 14B may explain the increase of its Curie temperature with the thermal treatment temperatures. In this paper, we examine the impacts of these factors on the magnetic properties of (Ndo 95Lao 05)9 5FebaICosNb2B10.5 nanocomposite.

Using angle-dependent x-ray magnetic circular dichroism, we have measured magnetic hysteresis loops at the Co L2,3 edges of oxide-doped Co80Pt20 thin films. The magnetocrystalline anisotropy energy (MAE) of the Co atoms, which is the main source of the magnetocrystalline anisotropy of the CoPt magnetic grains, has been determined directly from these element-specific hysteresis loops. When the oxide volume fraction (OVF) is increased from 16.6% to 20.7%, the Co MAE has been found to decrease from 0.117 meV/atom to 0.076 meV/atom. While a larger OVF helps one to achieve a smaller grain size, it reduces the magnetocrystalline anisotropy, as demonstrated unambiguously from the direct Co MAE measurements. Our results suggest that those Co80Pt20:oxide films with an OVF between 19.1% and 20.7% are suitable candidates for high-density magnetic recording.

The thin films Co81−xCr15PtxTa4 with (0002) crystallographic texture have been sputter deposited with and without substrate bias. The lattice parameter of the thin films has been determined by a combination of x-ray diffraction and electron diffraction techniques. The resolution of the electron diffraction was enhanced by a digital imaging technique. The variation rate of the a lattice parameter with Pt content is consistent with Vegard’s law. The change in the c lattice parameter is much greater than what is expected from Vegard’s law.

The thin films Co 81−x Cr 15 Pt x Ta 4 with (0002) crystallographic texture have been sputter deposited with and without substrate bias. The lattice parameter of the thin films has been determined by a combination of x-ray diffraction and electron diffraction techniques. The resolution of the electron diffraction was enhanced by a digital imaging technique. The variation rate of the a lattice parameter with Pt content is consistent with Vegard’s law. The change in the c lattice parameter is much greater than what is expected from Vegard’s law.

Thermally-assisted ultra-fast magnetization reversal in a DC magnetic field for magnetic multilayer thin films with perpendicular anisotropy has been investigated in the time domain using femtosecond laser heating. The experiment is set-up as an optically pumped stroboscopic Time Resolved Magneto-Optical Kerr Effect magnetometer. It is observed that a modest laser fluence of about 0.3 mJ/square-cm induces switching of the magnetization in an applied field much less than the DC coercivity (0.8 T) on the sub-nanosecond time-scale. This switching was thermally-assisted by the energy from the femtosecond pump-pulse. The experimental results are compared with a model based on the Landau Lifschitz Bloch equation. The comparison supports a description of the reversal process as an ultra-fast demagnetization and partial recovery followed by slower thermally activated switching due to the spin system remaining at an elevated temperature after the heating pulse.