Interface growth mechanism in ion beam sputtering-deposited Mo/Si multilayers

Despite the technological importance of metal/Si multilayer structures in microelectronics, the interface reactions occurring during their preparation are not yet fully understood. In this work, the interface intermixing in Mo/Si multilayer coatings has been studied with respect to their preparation conditions. Various samples, prepared at room temperature with different Mo deposition rates (0.06–0.43?Å?s^?1) and a constant Si rate, have been investigated by detailed TEM observations. Contrary to the Si-on-Mo interface where no evidence of chemical intermixing could be found, the Mo-on-Si interface presents a noticeable interface zone whose thickness was found to noticeably decrease (from 4.1 to 3.2?nm) when increasing the Mo deposition rate. Such intermixing phenomena correspond to diffusion mechanisms having coefficients ranging from 0.25?×?10^?15 to 1.2?×?10^?15?cm²?s^?1 at room temperature. By assuming a diffusion mechanism mainly driven by Mo–Si atomic exchanges to minimize the surface energy, the diffusion dependence with Mo deposition rate has been successfully simulated using a cellular automaton. A refined simulation including Mo cluster formation is also proposed to explain the scenario leading to the full crystallization of Mo layers.     

光栅光谱仪波长校准算法研究

使用正弦曲线拟合进行波长校准时,根据不同的待定系数选择方法,提出三种校准算法.最优算法选定四个待定系数,其中两个线性系数使用最小二乘法计算,而两个非线性系数使用最优化原理求得.线性算法只选定两个线性系数为待定量,而非线性系数为确定值.简化算法仅选定一个线性系数为待定量,其余三个系数为确定值.实测数据表明,线性算法拟合准确度接近最优解,计算复杂度低,是一种最适合于光栅光谱仪波长校准的算法.     

Mo/Si多层膜小角X射线衍射结构表征

为了实现对Mo/Si多层膜的结构表征,测量了多层膜样品的小角X射线衍射谱。介绍了小角X射线衍射谱的分析方法,包括Bragg峰值拟合法,傅里叶变换法,反射谱拟合法。Bragg峰值拟合法和反射谱拟合法得到多层膜的周期厚度为7.09nm,两种模型的反射谱拟合法得到界面的粗糙度(扩散长度)为0.40～0.41nm(Si在Mo上),0.52～0.70nm(Mo在Si上),前者要比后者小,这与透射电镜法(TEM)得到的结果0.40nm(Si在Mo上),0.6～0.65nm(Mo在Si上)是一致的。通过基于扩散模型的反射谱拟合法得到的折射率剖面也与由高倍率透射电镜(HRTEM)积分得到的灰度值剖面在趋势上是一致的。通过X射线衍射谱和TEM图像对Mo/Si多层膜进行综合表征,得到了多层膜的精细结构信息,这对多层膜制备工艺的优化具有十分重要的意义。     

质子辐照下Mo/Si多层膜反射镜的微观结构状态

利用透射电子显微镜对质子辐照前后空间太阳望远镜Mo/Si多层膜的微观结构进行了表征, 并对其辐照前后反射率的变化进行了测量.研究表明, Mo/Si多层膜经质子辐照后形成了一些缺陷结构,局部区域Mo/Si的周期性遭到破坏, Mo层与Si层的宽度发生了变化,多层膜层与层之间的界面也比辐照前更为粗糙,部分层状结构由于质子辐照发生了明显的扭曲和折断等现象;此外,质子辐照导致了Mo/Si多层膜反射率的下降,这些微观缺陷的形成是光学性能降低的直接诱因. 关键词： 空间太阳望远镜 Mo/Si多层膜 微观结构 反射率     

On the interplay of internal/external stress and thermal stability of Mo/Si multilayers

Mo/Si multilayer (ML) systems were deposited on Si(100) substrate by DC magnetron sputtering. The MLs were annealed at temperatures up to 440 °C under high-vacuum conditions, both with and without the influence of external mechanical stress, and characterized before and after thermal treatment by means of X-ray reflectometry, wide-angle X-ray scattering and optical microscopy. Two ML configurations were compared, one composed of pure Mo and Si layers and another with additional B₄C and C interlayers at the Mo/Si interfaces, respectively. The external mechanical stress applied caused bending of the substrate and adherent ML, with an accompanied internal stress of approximately 60 GPa. An important outcome of the investigation was that dedicated release bending of MLs can reduce/compensate the influences of the internal stressed states. Thermal stability could be increased for both ML systems during sample annealing. For ML samples with additional B₄C and C layers at the Mo/Si interfaces, the influence of external stress was more significant compared to that for pure Mo/Si MLs. This indicates that the additional layers mainly act as diffusion barriers and additionally as stress-relaxing buffers. PACS 68.60.Dv; 68.65.Ac; 42.79.Bh     

The structure of Mo/Si multilayers prepared in the conditions of ionic assistance

The influence of a negative substrate-applied bias potential on the structure of periodic Mo/Si multilayer compositions has been investigated by means of cross-sectional electron microscopy, small-angle X-ray reflectivity, X-ray diffraction and by modeling the small-angle spectra. It is known that the crystalline structure of molybdenum layers is the main source of interface roughness. In the absence of a bias potential application, the interface roughness tends to develop from the substrate towards the surface of a Mo/Si multilayer composition. A negative bias potential (up to -200 V) applied to a substrate during silicon layer deposition leads to smoother interfaces and improves the layer morphology. After increasing the bias potential over -200 V a considerable growth of an amorphous interlayer transition zone can be observed at Si-on-Mo interfaces. By raising the bias potential during the deposition of Mo layers a development of roughness at Mo-on-Si interfaces as well as growing interlayer thicknesses were found. PACS 61.10.Kw; 68.37.-d; 68.65.Ac     

Simulation of multilayer Cu/Pd（100） heteroepitaxial growth by pulse laser deposition

The heteroepitaxial growth of multilayer Cu/Pd(100) thin film via pulse laser deposition (PLD) at room temperature is simulated by using kinetic Monte Carlo (KMC) method with realistic physical parameters. The effects of mass transport between interlayers, edge diffusion of adatoms along the islands and instantaneous deposition are considered in the simulation model. Emphasis is placed on revealing the details of multilayer Cu/Pd(100) thin film growth and estimating the Ehrlich--Schwoebel (ES) barrier. It is shown that the instantaneous deposition in the PLD growth gives rise to the layer-by-layer growth mode, persisting up to about 9 monolayers (ML) of Cu/Pd(100). The ES barriers of The heteroepitaxial growth of multilayer Cu/Pd（100） thin film via pulse laser deposition （PLD） at room temperature is simulated by using kinetic Monte Carlo （KMC） method with realistic physical parameters. The effects of mass transport between interlayers, edge diffusion of adatoms along the islands and instantaneous deposition are considered in the simulation model, Emphasis is placed on revealing the details of multilayer Cu/Pd（100） thin film growth and estimating the Ehrlich-Schwoebel （ES） barrier. It is shown that the instantaneous deposition in the PLD growth gives rise to the layer-by-layer growth mode, persisting up to about 9 monolayers （ML） of Cu/Pd（100）. The ES barriers of 0.08 ± 0.01 eV is estimated by comparing the KMC simulation results with the real scanning tunnelling microscopy （STM） measurements,     

中心波长为13．9nm的正入射Mo／Si多层膜

用由铜靶激光等离子体光源等组成的反射率计对自行设计的周期厚度为7.14nm的120层Mo/Si多层膜进行极紫外(EUV)波段反射率测量。由于多层膜层数增加所引起的吸收、膜层界面之间的扩散以及镀膜过程中的膜厚控制误差或表面被氧化(污染)等原因,正入射Mo/Si多层膜在13.9nm处的反射率低于理论计算值73.2%,最后用原子力显微镜(AFM)测量其表面粗糙度为σ=0.401nm。     

高反射率Mo/B4C多层膜设计及制备

运用遗传算法优化设计了Mo/B4C多层膜结构。入射光入射角度取10°时,设计的理想多层膜膜对数为150,周期为3.59 nm,Gamma值（Mo膜厚与周期的比值）为0.41,峰值反射率为33.29%。采用恒功率模式直流磁控溅射方法制作Mo/B4C多层膜。通过在Mo/B4C多层膜与基底之间增加15 nm厚的Cr粘附层,提高多层膜与基底的粘附力。另外,还采用调整多层膜Gamma值的方法减小其内应力,调整后多层膜结构周期为3.59 nm, Mo膜厚1.97 nm, B4C膜厚1.62 nm,峰值反射率26.34％。制备了膜对数为150的Mo/B4C膜并测量了其反射率,在波长7.03 nm处,Mo/B4C多层膜的近正入射反射率为21.0％。最后对测量结果进行了拟合,拟合得到Mo/B4C多层膜的周期为3.60 nm,Gamma值0.60,界面粗糙度为0.30 nm。     

Mo/Si多层膜表面保护层设计

为提高Mo/Si多层膜的稳定性与使用寿命,通过分析多层膜驻波电场的分布,对表面保护层及多层膜最上层材料的厚度进行优化设计,使优化后的反射率最高.计算表明,一定厚度的表面保护层总对应一个最优的最上层材料厚度.在13.36 nm波长,膜对数为50的Mo/Si多层膜10度入射的理论反射率为74.47%;当添加厚度为2.3 nm的Ru作为表面保护层,对应多层膜最上层Si的优化厚度为3.93 nm,其理论反射率为75.20％.设计结果表明,通过优化设计表面保护层,可以提高多层膜稳定性,改善多层膜性能.     

磁控溅射方法制备直径120mm高均匀性Mo/Si多层膜

为满足极紫外、软X射线和X射线大口径多层膜反射镜的需求,采用基板扫掠过矩形靶材表面的镀膜方法,在直径120 mm的平面基板上镀制了Mo/Si周期多层膜。通过调整基板扫掠过矩形靶材表面的速率修正了薄膜的沉积速率,极大地提高了薄膜厚度的均匀性。采用X射线衍射仪对反射镜不同位置多层膜周期厚度进行了测量,结果表明,在直径120 mm范围内,Mo/Si多层膜周期厚度的均匀性达到了0.26%。同步辐射测量多层膜样品不同位置处的反射率,结果表明,在直径120 mm范围内,多层膜的膜层厚度均匀,在入射角10°时13.75 nm波长处平均反射率为66.82%。     

磁控溅射方法制备直径120 mm高均匀性Mo/Si多层膜

为满足极紫外、软X射线和X射线大口径多层膜反射镜的需求,采用基板扫掠过矩形靶材表面的镀膜方法,在直径120 mm的平面基板上镀制了Mo/Si周期多层膜。通过调整基板扫掠过矩形靶材表面的速率修正了薄膜的沉积速率,极大地提高了薄膜厚度的均匀性。采用X射线衍射仪对反射镜不同位置多层膜周期厚度进行了测量,结果表明,在直径120 mm范围内,Mo/Si多层膜周期厚度的均匀性达到了0.26%。同步辐射测量多层膜样品不同位置处的反射率,结果表明,在直径120 mm范围内,多层膜的膜层厚度均匀,在入射角10°时13.75 nm波长处平均反射率为 66.82%。     

月球表面环境对Mo/Si多层膜光学特性的影响

研究了月球表面高温、强辐射的空间环境下Mo/Si多层膜的热稳定性和辐照稳定性。Mo/Si多层膜采用磁控溅射法镀制,将制备好的多层膜在100℃和200℃高温下加热,利用激光等离子体反射率计和X射线衍射仪(XRD)对加热前后的多层膜进行了测量。结果显示在200℃以内,多层膜反射率和中心波长没有显著变化,表现出良好的热稳定性。利用Monte Carlo方法模拟了质子在多层膜内造成的缺陷的分布和浓度分布。模拟显示,能量大的质子沉积在多层膜内部,造成的缺陷也集中在多层膜内部。用能量为60keV,剂量分别为3×1012 cm-2和3×1014 cm-2的质子对Mo/Si多层膜进行辐照实验。发现多层膜内部出现了烧蚀损伤缺陷及节瘤缺陷。结果表明能量相同时,辐照剂量越大对多层膜反射率影响越大。     

高反射率Mo/B4C多层膜设计及制备

 运用遗传算法优化设计了Mo/B₄C多层膜结构。入射光入射角度取10°时,设计的理想多层膜膜对数为150,周期为3.59 nm,Gamma值（Mo膜厚与周期的比值）为0.41,峰值反射率为33.29%。采用恒功率模式直流磁控溅射方法制作Mo/B₄C多层膜。通过在Mo/B4C多层膜与基底之间增加15 nm厚的Cr粘附层,提高多层膜与基底的粘附力。另外,还采用调整多层膜Gamma值的方法减小其内应力,调整后多层膜结构周期为3.59 nm, Mo膜厚1.97 nm, B4C膜厚1.62 nm,峰值反射率26.34％。制备了膜对数为150的Mo/B₄C膜并测量了其反射率,在波长7.03 nm处,Mo/B₄C多层膜的近正入射反射率为21.0％。最后对测量结果进行了拟合,拟合得到Mo/B₄C多层膜的周期为3.60 nm,Gamma值0.60,界面粗糙度为0.30 nm。     

月基极紫外相机多层膜反射镜

月基极紫外相机用于月球表面对地球等离子体层辐射出的30.4 nm谱线进行成像观测,多层膜反射镜是月基极紫外相机的重要光学元件。根据月基极紫外相机技术参数,选择了B₄C/Mg,B₄C/Mg₂Si,B₄C/Al,B₄C/Si,Mo/Si等材料,对其周期厚度、材料比例、周期数等参数进行优化。计算了以上材料组合在30.4 nm的反射率曲线。考虑到月球环境的特殊性和材料的物理化学性质,从中选择出Mo/Si和B₄C/Si两种组合,利用磁控溅射进行镀制。Mo/Si和B₄C/Si多层膜在30.4 nm反射率分别达到15.3%和22.8%。     

Specific character of the 119Sn thin films growth on amorphous Si by the CBPLD method

The research of the ¹¹⁹Sn thin films growth on amorphous Si that is important for the multilayer periodical spin-tunnel nanostructures creation have been investigated in this paper. The ¹¹⁹Sn mono-isotopic thin films on the silicon substrates (100) had been received by crossed-beam pulsed laser deposition method (CBPLD). Similarly the [Fe/Si/Sn/Si] multilayer periodical structures have been deposited. The received samples were investigated by atomic-force microscopy, electronic microscopy and X-ray reflectometry methods. It has been established that at ¹¹⁹Sn film thickness up to 3 nm it is possible to received atomic-smooth surfaces with 0.5 nm roughness.     

Analysis of periodic Mo/Si multilayers: Influence of the Mo thickness

A set of Mo/Si periodic multilayers is studied by non-destructive analysis methods. The thickness of the Si layers is 5 nm while the thickness of the Mo layers changes from one multilayer to another, from 2 to 4 nm. This enables us to probe the effect of the transition between the amorphous and crystalline state of the Mo layers near the interfaces with Si on the optical performances of the multilayers. This transition results in the variation of the refractive index (density variation) of the Mo layers, as observed by X-ray reflectivity (XRR) at a wavelength of 0.154 nm. Combining X-ray emission spectroscopy (XES) and XRR, the parameters (composition, thickness and roughness) of the interfacial layers formed by the interaction between the Mo and Si layers are determined. However, these parameters do not evolve significantly as a function of the Mo thickness. It is observed by diffuse scattering at 1.33 nm that the lateral correlation length of the roughness strongly decreases when the Mo thickness goes from 2 to 3 nm. This is due to the development of Mo crystallites parallel to the multilayer surface.     

Crystalline silicon films sputtered on molybdenum: A study of the silicon–molybdenum interface

Polycrystalline silicon films were grown on molybdenum (Mo)-coated substrates at high deposition rate using the pulsed magnetron sputtering technique. Our study investigates the silicon–molybdenum interface of these films to elucidate stimulating mechanisms for an ordered crystalline silicon thin film growth. Both Auger electron spectroscopy and Rutherford backscattering reveal that at a substrate temperature as low as T_S=450 °C during the deposition process intermixing of Si and Mo at the Si–Mo interface takes place leading to a compositional ratio Mo:Si of about 1:2. By Raman spectroscopy hexagonal β-MoSi₂ could be identified as the dominant phase in this intermixed region. The dependence of the resulting thickness of the reacted interface layer on the deposition conditions is not fully understood yet.     

Au层退火温度对ZnO/Au/ZnO多层膜的结构、光学及电学性质的影响

采用金属有机化学气相沉积(MOCVD)技术在蓝宝石衬底上制备出晶体质量较好的透明导电的ZnO/Au/ZnO(ZAZ)多层膜,其中,Au夹层是通过射频磁控溅射的方法获得。通过对Au夹层进行不同温度的退火处理,研究了Au层退火温度对ZAZ多层膜的结构特性、电学性能和光学特性的影响。利用原子力显微镜(AFM)、扫描电子显微镜(SEM)、X射线衍射(XRD)仪、霍尔效应测试和透射谱分析等测试手段对ZAZ多层膜的性质进行了分析。测试结果表明,在200 ℃下对Au夹层进行快速退火处理,多层膜的结构、电学和光学性质达到最优,表面等离子体效应也更明显。其中,XRD(002)衍射峰的半高宽为0.14°,电阻率为2.7×10^-3 Ω·cm,载流子浓度为1.07×10²⁰ cm^-3,可见光区平均透过率为75.3%。     

B4C/Mo/Si high reflectivity multilayer mirror at 30.4 nm

The B4C/Mo/Si high reflectivity multilayer mirror was designed for He-Ⅱ radiation (30.4 nm) using the layer-by-layer method. The theoretical peak reflectivity was up to 38.2% at the incident angle of 5°. The B4C/Mo/Si multilayer was fabricated by direct current magnetron sputtering and measured at the National Synchrotron Radiation Laboratory (NSRL) of China. The experimental reflectivity of the B4C/Mo/Si multilayer at 30.4 nm was about 32.5%. The promising performances of the B4C/Mo/Si multilayer mirror could be used for the construction of solar physics instrumentation.