Effect of the substrate temperature and deposition rate on the initial growth of thin lithium niobate-tantalate films deposited from a thermal plasma

Thin lithium niobate-tantalate (LiNb_0.5Ta_0.5O₃) films are studied at the initial stage of deposition from a thermal plasma. The effect of two deposition parameters (the substrate temperature and the deposition rate) on the film morphology, the film crystallinity, and the density of nuclei growing on a (0001) sapphire substrate are investigated. It is shown that the crystalline structure and roughness of a film are determined, for the most part, in the initial growth stage and therefore depend directly on both parameters. At the optimum temperatures and growth rates for obtaining good characteristics of (0006) texture, crystallinity, and surface roughness of the films, the film nuclei on the substrate have a high density and good epitaxial orientation to it. If the growth conditions are not optimum, the islands are either amorphous or have a low density on the substrate surface. The nucleation activation energy is observed to decrease as the deposition rate increases, which supports the assumption that the species that are active in film deposition are “hot” clusters forming in an oxygen-argon plasma in the immediate vicinity of the substrate.     

薄膜外延生长的计算机模拟

以Cu膜为例，用Monte-Carlo算法模拟了薄膜生长的随机过程，并提出了更加完善的模型.在合理选择原子间相互作用计算方法的基础上，考虑了原子的吸附、在生长表面的迁移及迁移所引起的近邻原子连带效应、从生长表面的脱附等过程.模拟计算了薄膜的早期成核情况以及表面粗糙度和相对密度.结果表明，随着衬底温度的升高或入射率的降低，沉积在衬底上的原子逐步由离散型分布向聚集状态过渡形成一些岛核，并且逐步由二维岛核向三维岛核过渡.在一定的原子入射率下，存在三个优化温度，成核率最高时的最大成核温度Tn、薄膜的表面粗糙度最低 关键词： Monte-Carlo算法 计算机模拟 薄膜生长     

On the Growth of High-Temperature Epitaxial AlN (AlGaN) Layers on Sapphire Substrates by Ammonia Molecular Beam Epitaxy

The growth of high-temperature AlN and AlGaN layers on (0001) sapphire substrates by ammonia based molecular-beam epitaxy is studied. Factors affecting the formation of inverted domains in high-temperature AlN films are examined. The density of inverted domains is found to correlate with the density of nucleation islands during the initial stages of growth. The denser coverage of a surface by nucleation islands suppresses the formation of inverted domains. It is possible to increase the density of surface coating at the nucleation growth stage by increasing the degree of substrate nitriding, reducing the deposition temperature, and using intense ammonia fluxes during deposition of the initial layers. The kinetic model in the mean field approximation is developed to explain the observed effects of growth parameters on the density of nucleation islands. The growth features of AlN and its structure are taken into account. The obtained results are used to grow AlN/AlGaN layers with improved structural quality. The grown films have a root-mean-square surface roughness of 2 Å and 120 arc s FWHM of X-ray diffraction peaks for the AlN 0002 reflection. The density of inverted domains is decreased to below 10⁵ cm^-2. Improvement in the quality of the AlN films is achieved by using two-step growth and by the application of gallium as a surfactant.     

Effect of Incident Intensity on Films Growth in Pulsed Laser Deposition

Incident intensity, defined by the amount of particles deposited per pulse, is an important parameter in the film growth process of pulsed laser deposition （PLD）. Different from previous models, we investigate the irreversible and reversible growth processes by using a kinetic Monte Carlo method and find that island density and film morphology strongly depend on pulse intensity. At higher pulse intensities, lots of adatoms instantaneously diffuse on the substrate surface, and then nucleation easily occurs between the moving adatoms resulting in more smaller-size islands. In contrast, at the lower pulse intensities, nucleation event occurs preferentially between the single adatom and existing islands rather than forming new islands, and therefore the average island size becomes larger in this case. Additionally, our results show that substrate temperature plays an important role in film growth. In particular, it can determine the films shape and weaken the effect of pulse intensity on film growth at the lower temperatures by controlling the mobility rate of atoms. Our results can match the related theoretical and experimental results.     

Flame spray deposition of nanocrystalline dense Ce0.8Gd0.2O2 − δ thin films: Deposition mechanism and microstructural characterization

Nanocrystalline dense sub-micron thin films of Ce_0.8Gd_0.2O_2 − δ have been successfully deposited by flame spray deposition. The deposition mechanism has been identified as droplet deposition. The deposition temperature of the substrate was as low as 200 °C and the deposition rate ∼ 30 nm/min. Under these conditions the droplets have a very limited residence time in the hot zone of the flame and are deposited as liquid, forming smooth films free of particles. They exhibited a dense and crack-free microstructure. Grain growth, lattice constant, crystallographic density and surface roughness have been investigated as a function of annealing temperature. The good quality of the films, in association with the high deposition rates at low deposition temperatures shows the preeminence of the flame spray method for depositing thin films for micro-solid oxide fuel cells.     

Nucleation and growth of Si on Pb monolayer covered Si(111) surfaces

With a scanning tunneling microscope (STM), we study the initial stage of nucleation and growth of Si on Pb monolayer covered Si(111) surfaces. The Pb monolayer can work as a good surfactant for growth of smooth Si thin films on the Si(111) substrate. We have found that nucleation of two-dimensional (2D) Pb-covered Si islands occurs only when the substrate temperature is high enough and the Si deposition coverage is above a certain coverage. At low deposition coverages or low substrate temperatures, deposited Si atoms tend to self-assemble into a certain type of Si atomic wires, which are immobile and stable against annealing to ~ 200 °C. The Si atomic wires always appear as a double bright-line structure with a separation of ~ 9 Å between the two lines. After annealing to ~ 200 °C for a period of time, some sections of Si atomic wires may decompose, meanwhile the existing 2D Pb-covered Si islands grow laterally in size. The self-assembly of Si atomic wires indicate that single Si adatoms are mobile at the Pb-covered Si(111) surface even at room temperature. Further study of this system may reveal the detailed atomic mechanism in surfactant-mediated epitaxy.     

红荧烯薄膜生长及稳定性的研究

利用原子力显微镜研究了二氧化硅衬底上红荧烯薄膜的生长及稳定性。在较低沉积速率下,较低衬底温度时,红荧烯分子有充足的扩散时间,利于薄膜的横向生长,形成连续性、均匀性较好的薄膜。快速蒸镀及较高衬底温度使红荧烯薄膜转变为纵向生长模式,形成团粒状岛。横向生长的红荧烯薄膜在退火和空气中表现为亚稳特性,随着退火温度的升高和空气中放置时间的延长,红荧烯分子会自发地进行质量传输,发生纵向转移,转变为团粒状岛。获得了二氧化硅界面上红荧烯薄膜的生长及亚稳定机制模型。研究结果证明红荧烯分子与二氧化硅界面之间的作用力小于红荧烯分子间的作用力。     

Competing roughening mechanisms in strained heteroepitaxy: a fast kinetic Monte Carlo study

We study the morphological evolution of strained heteroepitaxial films using kinetic Monte Carlo simulations in two dimensions. A novel Green's function approach, analogous to boundary integral methods, is used to calculate elastic energies efficiently. We observe island formation at low lattice misfit and high temperature that is consistent with the Asaro-Tiller-Grinfeld instability theory. At high misfit and low temperature, islands or pits form according to the nucleation theory of Tersoff and LeGoues.     

Kinetics of facile bilayer island formation at low temperature: Ag/NiAl(110)

Facile nucleation and growth of bilayer Ag(110) islands on NiAl(110) is observed by STM for Ag deposition at temperatures as low as 127 K. Density functional theory analysis for supported Ag films determines adatom adsorption energies (which favor bilayer islands), interaction energies, and diffusion barriers. Analysis of an atomistic lattice-gas model incorporating these energies elucidates the role of strongly anisotropic interactions in enabling the upward mass transport needed for bilayer island formation.     

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.     

磁控反应溅射AlN缓冲层对GaN基LED器件性能的影响

以直流磁控反应溅射法(RMS)在图形化蓝宝石衬底上制备的AlN薄膜作为缓冲层,采用金属有机化学气相沉积法(MOCVD)外延生长了GaN基LED。与MOCVD生长的低温GaN缓冲层相比,RMS制备的AlN缓冲层具有表面更平整、颗粒更小的形核岛,有利于促进GaN外延的横向生长,减少了形核岛合并时的界面数量和高度差异,降低了缺陷和位错产生的几率。研究结果表明,溅射AlN缓冲层取代传统低温GaN缓冲层后,外延生长的GaN材料具有更高的晶体质量,LED器件在亮度、漏电和抗静电能力等光电特性上均有明显提升。     

Different-dimensional structures of antimony formed selectively on graphite

When antimony (mostly Sb₄) is deposited on highly oriented pyrolytic graphite (HOPG), in situ scanning tunneling microscopy images reveal that three-dimensional (3D) spherical islands, quasi-2D films and 1D nanowires (NWs) are formed. The spherical islands develop into faceted crystallites in the later growth stage. The lattice parameters of the 2D and 3D structures are close to those of α-Sb bulk, whereas the NWs appear in a compressed state. The Laplace pressure, which can reach the GPa range in a nanostructure, is considered the driving force for the compressive lattice structures of Sb NWs. We found conditions of controlling the dimensionality of Sb nanostructures in their self-assembly on HOPG to a certain extent. At room temperature and with a low Sb flux, 3D islands grow exclusively. At a substrate temperature of 100 °C, 2D and 1D structures are dominant when a high deposition flux is used, whereas only NWs are formed initially when a low flux is used. These results are explained in terms of different activation energies for Sb₄ diffusion and conversion to a chemisorption or dissociation state on HOPG. As the temperature increases, the rate of conversion to the chemisorption or dissociation state increases more rapidly than that of diffusion since the chemisorption activation energy is much higher than the diffusion barrier of physisorbed Sb₄, resulting in enhanced 2D and 1D structural nucleation and growth, which are further favored with the increase in deposition flux. The bonding nature of various Sb structures with a graphite surface and the conditions for growing aligned Sb NWs exclusively are discussed. PACS 61.46.+w; 64.70.Nd; 68.37.Ef; 68.65.-k; 81.07.-b     

Size distribution and optical properties of self-assembled Ge on Si

The distribution of Ge islands is analysed in order to understand their optical behaviour. The Ge islands described in this paper were deposited by low-pressure chemical vapour deposition at relatively high temperature (700 °C), therefore the diffusion length of adatoms is high (∼100 μm) and thus, not the limiting factor for nucleation. By changing the deposition time and the coverage, square-based pyramids, domes and relaxed domes are nucleated. Mainly domes emit light, the emission being in the wavelength range 1.38–1.55 μm. When pyramids or relaxed domes are present, the photoluminescence broadens and decreases in intensity. The electroluminescence of vertically correlated islands increases with the number of layers, i.e. with the number of islands. The nucleation of islands on patterned (001) Si is changed when the deposition is performed on Si mesas with high index facets. The size distribution becomes narrower when the mesa size is decreased. An intermixing of up to 40% Si in the 2D layer was determined from photoluminescence data. PIN diodes fabricated on patterned wafers show an area-dependent electroluminecence related to a different microstructure of islands on large and small mesas. Finally, the lateral ordering on {hkl} facets is discussed. Received: 14 April 2000 / Accepted: 17 April 2000 / Published online: 6 September 2000     

动力学晶格蒙特卡洛方法模拟Cu薄膜生长

利用动力学晶格蒙特卡洛方法模拟了Cu薄膜在Cu(100)面上的三维生长过程。模型中考虑了四个动力学过程:原子沉积、增原子迁移、双原子迁移和台阶边缘原子迁移,各动力学过程发生的概率由多体势函数确定。讨论了基底温度、沉积速率及原子覆盖率对Cu原子迁移、成核和表面岛生长等微观生长机制的影响;获得了Cu薄膜的表面形貌图并计算了表面粗糙度。模拟结果表明,随基底温度升高或沉积速率下降,岛的平均尺寸增大,数目减少,形状更加规则。低温时,Cu薄膜表现为分形的离散生长,高温时,Cu原子迁移能力增强形成密集的岛。Cu薄膜表面粗糙度随着基底温度的升高而迅速减小;当基底温度低于某一临界温度时,表面粗糙度随原子覆盖率或沉积速率的增大而增大;当基底温度超过临界温度时,表面粗糙度随原子覆盖率或沉积速率的变化很小,基本趋于稳定。     

Defect density variation with deposition rate in snsb thin films from annealing study of electrical resistance

SnSb thin films of the same thickness (600 Å) vacuum deposited at room temperature on glass substrates at various deposition rates were heated to a maximum temperature of about 300°C and the changes in the electrical resistance with temperature were recorded. From the resistance vs temperature data “initial lattice distortion energy spectra” i.e. the variation of the defect density with its activation energy, of the films is obtained. It is found that the area of the spectra decreases with an increase in the deposition rate thereby indicating that the defect density of the film decreases with increasing deposition rate. The observed decrease in the defect density of the films with increasing deposition rate has been satisfactorily explained with the help of nucleation and growth phenomena.     

Simulation study on nanocluster growth deposited on a substrate

We present a model equation that describes nucleation and growth of hemispherical nanoclusters or islands deposited on a substrate for the small surface coverage case. The model is formulated in terms of a set of rate equations for the island sizes, combined with the time-dependent behavior of supersaturation and island nucleation rate. As an example to demonstrate the usefulness of the model, we study effects of the deposition rate of adatoms on the nanocluster growth. Large-scale computer simulation results show that the broadness of island size distribution is a decreasing function of the deposition rate for small rates, and bimodal distributions are obtained for large rates.     

温度对Si上MOCVD-ZnO成核与薄膜生长特性的影响

采用金属有机化学气相沉积(MOCVD)方法在Si衬底上进行了ZnO的成核与薄膜生长研究。ZnO薄膜的形貌和结晶特性由成核和后期生长过程共同决定,初期成核温度决定了其尺寸和密度,进而影响后期ZnO主层的生长行为,但由于高温对后期ZnO纳米柱横向生长的抑制,纳米柱的尺寸并没有因为成核尺寸的增大而变大,因此在560℃得到了晶柱尺寸最大、密度最小的ZnO薄膜。最后通过改变成核温度,优化了ZnO外延膜的结晶质量。     

EFFECTS OF ISLAND-EDGE EXCHANGE BARRIER ON 2D PATTERN FORMATION IN SURFACTANT-MEDIATED EPITAXY

The nucleation and growth of two-dimensional islands in a surfactant-mediated epitaxy system have been studied by computer simulation. To improve the recent results published in the literature, we use a configuration-dependent energy barrier for the exchange process at the island edge in our model. The simulations produce fractal islands at high temperatures or low deposition fluxes, and a transition to regular compact islands occurs at lower temperatures or higher fluxes, in good agreement with the recent experimental results. The barrier for the island-edge exchange has quite a strong effect on the island density as a function of temperature and flux. A small change of the island-edge exchange barrier induces a large variation of the island density in the low-temperature or high-flux region. The flux-dependent island density shows a clear scaling-law behaviour in the intermediate-flux region. The scaling exponent increases evidently as the island-edge exchange barrier increases.     

Kinetic Monte Carlo simulations of Pd deposition and island growth on MgO(1 0 0)

The deposition and ripening of Pd atoms on the MgO(1 0 0) surface are modeled using kinetic Monte Carlo simulations. The density of Pd islands is obtained by simulating the deposition of 0.1 ML in 3 min. Two sets of kinetic parameters are tested and compared with experiment over a 200-800 K temperature range. One model is based upon parameters obtained by fitting rate equations to experimental data and assuming the Pd monomer is the only diffusing species. The other is based upon transition rates obtained from density functional theory calculations which show that small Pd clusters are also mobile. In both models, oxygen vacancy defects on the MgO surface provide strong traps for Pd monomers and serve as nucleation sites for islands. Kinetic Monte Carlo simulations show that both models reproduce the experimentally observed island density versus temperature, despite large differences in the energetics and different diffusion mechanisms. The low temperature Pd island formation at defects is attributed to fast monomer diffusion to defects in the rate-equation-based model, whereas in the DFT-based model, small clusters form already on terraces and diffuse to defects. In the DFT-based model, the strong dimer and trimer binding energies at charged oxygen vacancy defects prevent island ripening below the experimentally observed onset temperature of 600 K.     

Nucleation, coarsening and kinetic scaling of two-dimensional islands on GaSb(0 0 1)

Using a combination of molecular beam epitaxy and in situ surface X-ray diffraction, we investigate the nucleation and coarsening of monolayer high islands on GaSb(0 0 1) during deposition in real time. We find an activation energy for island nucleation of 1.55 ± 0.16 eV, indicating a stable nucleus size larger than two atoms. For intermediate temperatures where GaSb homoepitaxy is stable, the lateral coarsening of the islands after deposition is described by Ostwald ripening. The average island sizes during coarsening are isotropic, although with different size distributions in different directions. The size distributions do not change during coarsening, implying kinetic scaling.