Solid-state wetting on nanopatterned substrates

We review some recent results on the morphology of heteroepitaxial overlayers deposited on nanopatterned substrate surfaces. We mainly focus on modeling based on kinetic Monte Carlo (KMC) simulations. On arrays of parallel grooves or arrays of pillars, we find three main classes of states similar to those known for liquids: (i) Cassie–Baxter states, where solid islands sit on top of the substrate structure; (ii) Wenzel states, where solid islands are in contact with the bottom of the substrate; and (iii) solid imbibition (also denoted as capillary filling for parallel grooves), where the solid forms a film in the substrate surface structure. This multi-stability is controlled by the wettability parameter χ, and shape transitions exhibit hysteresis. We discuss the dynamics of the collapse of a Cassie–Baxter to Wenzel state, and the collapse of the Wenzel state to an imbibition film. We also discuss the possibility to grow crystals in the CB state on nanopatterned substrates. During growth, the crystals formed in CB state merge, leading to a continuous polycrystalline overlayer where the size of the grains is controlled by the distance between pillars.     

Bistability in the shape transition of strained islands

The equilibrium shape of a monatomic strained island on a substrate depends on the step free energies and the difference in surface stress between the island and the substrate. For small island sizes the step free energies dominate, resulting in compact islands. Beyond a critical island size, however, the strain energy becomes dominant and the island maximizes its perimeter, resulting in elongated islands. Here we show that for strained islands with force monopoles pointing in opposing directions at neighboring steps, a regime exists near the critical island size where both compact and elongated shapes can coexist.     

Interaction of Love waves with coupled cavity modes in a 2D holey phononic crystal

The interaction of Love waves with square array of pillars deposited on a cavity defined in a 2D holey phononic crystal is numerically investigated using Finite Element Method. First, the existence of SH surface modes is demonstrated separately for phononic crystals that consist of square arrayed holes, or rectangular arrayed Ni pillars, respectively in, or on, a SiO₂ film deposited on a ST-cut quartz substrate. The coupling between SH modes and torsional mode in pillars induces a transmission dip that occurs at a frequency located in the range of the band-gap of the holey phononic crystal. Second, a cavity is constructed by removing lines of holes in the holey phononic crystal and results in a transmission peak that matches the dip. The optimal geometrical parameters enable us to create a coupling of the cavity mode and the localized pillar mode by introducing lines of pillars into the cavity, which significantly improved the efficiency of the cavity without increasing the crystal size. The obtained results will pave the way to implement advanced designs of high-performance electroacoustic sensors based on coupling modes in phononic crystals.     

Dewetting of a solid monolayer

We report on the dewetting of a monolayer on a solid substrate, where mass transport occurs via surface diffusion. For a wide range of parameters, a labyrinthine pattern of bilayer islands is formed. An irreversible regime and a thermodynamic regime are identified. In both regimes, the velocity of a dewetting front, the wavelength of the bilayer island pattern, and the rate of nucleation of dewetted zones are obtained. We also point out the existence of a scaling behavior, which is analyzed by means of a geometrical model.     

Self-aligned Ge and SiGe three-dimensional epitaxy on dense Si pillar arrays

In this report we present a novel strategy in selective epitaxial growth on top of Si pillars, which results in a tessellated Ge film, composed by self-aligned micron-sized crystals in a maskless process. Modelling by rate equations the morphology evolution of fully facetted crystal profiles is extensively outlined, showing an excellent prediction of the peculiar role played by flux shielding among microcrystals, in the case of dense array configuration. Crack formation and substrate bending, caused by the mismatch in thermal expansion coefficients, are eliminated by the mechanical decoupling among individual microcrystals, which are also shown to be dislocation- and strain-free. The method has been also tested for Si_1?xGe_x alloys, with compositions ranging from pure silicon to pure germanium. There are ample reasons to believe that this approach could be extended to other material combinations and substrate orientations, actually providing a technology platform for several device applications.     

Near field properties of nanoparticle arrays fabricated by laser annealing of thin Au and Ag films

In this work we show the properties of the electromagnetic field in the vicinity of a monolayer nanoparticle array on SiO₂ substrate. The nanoparticle array is produced by a simple experimental procedure, where thin gold and silver films are deposited on a substrate by pulsed laser deposition technique and they are annealed by nanosecond laser pulses. At certain conditions the laser annealing leads to a homogeneous decomposition of the film into nanoparticles with diameters in the range of few tens of nanometers. Using FDTD simulations the near field distribution in array structures taken from SEM images are obtained. The distribution shows presence on “hot spots” where the near field intensity is enhanced more than two orders of magnitude compared to the incident one. The existence of enhanced field intensity is assumed to be the main reason on enhancement of the Raman scattering signal obtained experimentally using the produced structures as active substrates.     

Self-assembly of three-dimensional metal islands: nonstrained versus strained islands

A theoretical model for the Volmer-Weber growth of three-dimensional metal islands is proposed, with a dipolar island edge-edge interaction. The existence of such an island edge effect makes the island shape dependent on island size. Furthermore, it induces a stable island size against coarsening, leading to self-assembled islands of uniform size. The dependence of the stable island size on total film coverage is shown to be different for nonstrained versus strained islands, in the regime of strong island-island interaction.     

基底显微结构对薄膜生长影响的Monte Carlo模拟研究

利用Monte Carlo方法研究了基底显微结构对薄膜生长的影响. 对不同显微结构基底上薄膜生长的初始阶段岛的形貌和尺寸与薄膜覆盖度和入射粒子沉积速率之间的关系进行了模拟和分析. 模型中考虑了粒子沉积、吸附粒子扩散和蒸发等过程. 结果表明,基底显微结构对薄膜生长具有明显影响. 当沉积温度为300K、沉积速率为0.005ML/s（Monolayer/second,简称ML/s）、覆盖度为0.05ML时,四方基底上薄膜生长呈现凝聚生长. 随着覆盖度增加,岛的尺寸变大,岛的数目减少. 而对于六方基底,当覆盖度从0.05ML变化到0.25ML时,薄膜生长经历了一个从分散生长过渡到分形生长的过程. 无论是四方还是六方基底,随着沉积速率的增加,岛的形貌由少数聚集型岛核分布状态向众多各自独立的离散型岛核分布状态过渡.     

非均一相互作用能对超薄膜生长影响的Monte Carlo模拟研究

利用Monte Carlo (MC)模拟技术研究了非均一的吸附原子与基底相互作用能在一定的生长条件下对超薄膜生长过程的影响.非均一相互作用能是由基底表面原子在垂直和水平方向上实际位置与理想晶格原子位置的偏差所造成.本文用高斯分布来表示这种非均一相互作用能.模拟结果表明:非均一相互作用能对超薄膜的生长过程及薄膜的形貌有显著的影响.这种影响同时受到生长条件的限制,在中等温度时相互作用能的非均一性对岛的个数、平均大小的影响最显著;温度的增加在一定程度上可抵御相互作用能的非均一性对薄膜生长的影响. 关键词： 薄膜生长 Monte Carlo 模拟 相互作用能     

Theoretical and experimental determination of the initial stage of plastic relaxation of misfit stresses in a (111) substrate-film islands heterosystem

A model for determining the critical thickness of a film h _c is developed to introduce misfit dislocations in the slip planes of a film and a substrate parallel to the interphase boundary (111). Experimental values h _c that agree with calculated values are determined for the Ge/Si(111) and Si₃N₄/Ge(111) heterosystems. The two-level epitaxial growth of Ge on Si is attained in the regime of combining the step-layer and 2D island growth mechanisms.     

Full X-ray pattern analysis of vacuum deposited pentacene thin films

Pentacene thin films with thicknesses ranging from 10 nm to 180 nm are investigated by specular X-ray diffraction in the reflectivity regime and in the wide angular regime. The results of the reflectivity measurements show a clear shift of the 001 reflection of the thin film phase depending on the layer thickness. It is shown that this shift can be explained by the dynamical scattering theory. The wide angular regime measurements show the 00L of the thin film phase. Williams-Hall plots are used to extract information on the crystallite size and mean micro strain of the thin film phase. The crystallite size is in good agreement with the results obtained by the reflectivity measurements. From this it can be concluded that the thin film phase crystallites are extended over the entire film thickness down to the substrate. Additionally an increase of the micro strain with increasing film thickness is observed.     

Contact instability in adhesion and debonding of thin elastic films

Based on experiments and 3D simulations, we show that a soft elastic film during adhesion and debonding from a rigid flat surface undergoes morphological transitions to pillars, labyrinths, and cavities, all of which have the same lateral pattern length scale, lambda close to lambda/H approximately 3 for thick films, H > 1 microm . The linear stability analysis and experiments show a new thin film regime where lambda/H approximately equal to 3 + 2pi(lambda/3 muH)1/4 (gamma is surface tension, mu is shear modulus) because of a significant surface energy penalty (for example, lambda/H approximately equal to 6 for H = 200 nm; mu = 1 MPa).     

Formation of Heusler alloy Co2FeSi thin films on the surface of single-crystal silicon

The initial stages of Heusler alloy (Co₂FeSi) thin film growth by reactive epitaxy on the Si(100)2 × 1 surface are studied, and formation conditions for this alloy are found. At a substrate temperature of lower than, or equal to, 180°C, an island film of ternary Co-Fe-Si film grows on the surface. The silicon content in this film is lower than in the compound to be synthesized. The film becomes continuous when its thickness exceeds 1.2 nm. It is shown that post-growth annealing at 240°C can raise the silicon content in the film and be conducive to obtaining Heusler alloy of a desired composition. In situ measurements of the films show that ferromagnetic ordering in them has a threshold and shows up at the coalescence growth stage of the Co-Fe-Si island alloy.     

Sensor studies of the initial stages of the cadmium telluride film formation through vapor deposition

The results of sensor and electron-microscopic studies of the initial stages of cadmium telluride film formation through vapor deposition on a substrate at room temperature and on a substrate cooled by liquid nitrogen (highly nonequilibrium conditions) are reported. A piezoelectric quartz resonator is used as a sensor. The kinetic curves of the sensor analytical signal and photomicrographs are presented. A jumplike character of the nucleation process and a quasi-periodical growth mechanism for island films are disclosed. A sequence of new-phase island ensembles is formed in an analogous way. These islands increase the substrate surface coverage in a quasi-discrete manner. The experimental results are shown to agree with current theory of the first-order phase transitions and models of layer formation in highly nonequilibrium conditions.     

On the 2D-3D transition in epitaxial thin film growth

The theory is based on the fact that the equilibrium concentration of single atoms adsorbed on the surface of a monolayer island placed on a foreign substrate such that the substrate-deposit interaction is weaker than the deposit-deposit interaction is higher than the equilibrium concentration of atoms adsorbed on the surface of the same island now placed on a substrate of the same material. This higher adatom concentration leads to 2D nucleation on top of the monolayer island. The difference of the above equilibrium adatom concentrations appears as a driving force for the process of transformation of the initial monolayer island into a 3D island by detachment of atoms from the first monolayer island edges and their subsequent attachment to the edges of the second layer nucleus. The kinetics of this process are studied in detail, the following two cases being considered. The first case consists of breaking up and agglomeration of an initially continuous film into 3D crystals upon heating. The second case consists of change of the growth mode from layer to island mode during the vapour deposition when the substrate temperature increases. Expressions for the critical temperatures for these two phenomena to occur are derived. It is shown that they depend strongly on the substrate orientation, the critical temperature being higher for the 〈111〉 orientation in comparison with the 〈110〉 orientation, if substrate and deposit with a fcc lattice are considered. The theoretical results are compared with experimental data for deposition of Au on Mo{110}, Cu on W{110} and W{100} and Fe on Cu{111}.     

Modelling thin-film dewetting on structured substrates and templates: Bifurcation analysis and numerical simulations

We study the dewetting process of a thin liquid film on a chemically patterned solid substrate (template) by means of a thin-film evolution equation incorporating a space-dependent disjoining pressure. Dewetting of a thin film on a homogeneous substrate leads to fluid patterns with a typical length scale, that increases monotonously in time (coarsening). Conditions are identified for the amplitude and periodicity of the heterogeneity that allow to transfer the template pattern onto the liquid structure ("pinning") emerging from the dewetting process. A bifurcation and stability analysis of the possible liquid ridge solutions on a periodically striped substrate reveal parameter ranges where pinning or coarsening ultimately prevail. We obtain an extended parameter range of multistability of the pinning and coarsening morphologies. In this regime, the selected pattern depends sensitively on the initial conditions and potential finite perturbations (noise) in the system as we illustrate with numerical integrations in time. Finally, we discuss the instability to transversal modes leading to a decay of the ridges into rows of drops and show that it may diminish the size of the parameter range where the pinning of the thin film to the template is successful.Received: 29 January 2003, Published online: 15 July 2003PACS: 68.15.+e Liquid thin films - 81.16.Rf Nanoscale pattern formation - 47.20.Ky Nonlinearity (including bifurcation theory)     

Morphologies of epitaxial islands on a lattice-misfitted substrate

Under certain growth conditions for systems with a film/substrate lattice misfit, the deposited material is known to aggregate into island-like shapes. We have obtained an analytical expression of the total free energy, which consists of strain energy, surface energy and interfacial energy of a coherent island/substrate system, and the change of equilibrium aspect ratio versus the volume of the island and the misfit of lattices in the system, which provides a broad perspective on island behaviour. These then were used to study the equilibrium shapes of the system. The results show that in order to minimize the total free energy, a coherent island will have a particular height-to-width aspect ratio, called equilibrium aspect ratio, that is a function of the island volume and misfit. The aspect ratio is increased with increasing island volume at a fixed misfit, and with increasing misfit strain between the island and substrate at a fixed island volume. Moreover, the effect of misfit dislocation on the equilibrium shape of the island is also examined. The results obtained are in good agreement with experiment of observations and thus can serve as a basis for interpreting the experiments.     

低温制备微晶硅薄膜生长机制的研究

采用热丝化学气相沉积技术制备了一系列处于不同生长阶段的薄膜样品，用原子力显微镜系 统地研究生长在单晶硅衬底和玻璃衬底上薄膜表面形貌的演化.按照分形理论分析得到：在 玻璃衬底上的硅薄膜以零扩散随机生长模式生长；而在单晶硅衬底上，薄膜早期以有限扩散 生长模式生长，当膜厚超过某一临界厚度时转变为零扩散随机生长模式.岛面密度与膜厚的 依赖关系表明，在临界厚度时硅衬底和玻璃衬底上的岛面密度均出现了极大值.Raman谱的测 量证实，玻璃衬底上薄膜临界厚度与非晶/微晶相变之间存在密切的关系.不同的衬底材料直 接影响反应 关键词： 生长机制 微晶硅薄膜 表面形貌 热丝化学气相沉积     

Commensurability effects in magnetic properties of superconducting Nb thin films with periodic submicrometric pores

Pinning properties in 100 nm thick continuous and porous superconducting Nb films are examined by ac susceptibility and dc magnetization measurements. The Nb film was deposited on a smooth Si substrate, while the porous film, Nb_P, was deposited on an anodized Al oxide substrate. Pores or “antidots” 40 nm in diameter, 100 nm apart, form a triangular array. The porous film presents commensurate or matching field effects for applied magnetic fields where the magnetic flux threading each unit cell is an integer number of the flux quantum, where ac shielding capability and dc diamagnetic magnetization show an abrupt increase. The response to ac fields as a function of temperature and dc field provided a way to determine that Nb_P sample has higher pinning than the continuous one, and that T_C suppression due to fluxoid quantization is not relevant for the investigated temperature range.     

Insulator-metal transition in a conservative system: An evidence for mobility coalescence in island silver films

Aging, which manifests itself as an irreversible increase in electrical resistance in island metal films is of considerable interest from both academic as well as applications point of view. Aging is attributed to various causes, oxidation of islands and mobility of islands followed by coalescence (mobility coalescence) being the main contenders. The effect of parameters like substrate temperature, substrate cleaning, residual gases in the vacuum chamber, ultrasonic vibration of the substrate, suggest that the mobility coalescence is responsible for the aging in island metal films. Electron microscopy studies show evidence for mobility of islands at high substrate temperatures. The comparison of aging data of island silver films deposited on glass substrates in ultra high vacuum and high vacuum suggests that the oxidation of islands, as being responsible for aging in these films, can be ruled out. Further, under certain conditions of deposition, island silver films exhibit a dramatic and drastic fall in electrical resistance, marking the insulator-metal transition. This interesting transition observed in a conservative system — after the stoppage of deposition of the film — is a clear evidence for mobility coalescence of islands even at room temperature. The sudden fall in resistance is preceded by fluctuations in resistance with time and the fluctuations are attributed to the making and breaking of the percolation path in the film.