Periodic cracks and temperature-dependent stress in Mo/Si multilayers on Si substrates

This work examines formation of the peculiar periodic crack patterns observed in the thermally loaded Mo/Si multilayers. Using the substrate curvature measurements, the macroscopic film stress evolution during thermal cycling was investigated. Then high-speed microscopic observation of crack propagation in the annealed Mo/Si multilayers was presented providing experimental evidence of the mechanism underlying formation of the periodic crack patterns. The origin of the peculiar periodic crack patterns was determined. They were observed to form by the slow crack propagation under quasi-static conditions as a result of the interaction between the channelling crack propagation and the advance of the delamination front.     

Anisotropy and interlayer interaction in Mo/Si multilayers

The interlayer interaction in superconducting Mo/Si multilayers is determined by the measurements of the upper critical magnetic field and the magnetoconductivity in magnetic fields, parallel and perpendicular to the layers. From these measurements we determined the anisotropy parameter, γ, and the effective thickness, L_eff, which characterize the mutual electronic interaction between the Mo layers across the Si layer. Both quantities oscillate in dependence of the Mo layer thickness for Mo/Si series with constant Si layer thickness.     

X-ray interface analysis of aperiodic Mo/Si multilayers

We present the non-destructive analysis of aperiodic Mo/Si multilayers by X-ray emission spectroscopy induced by electrons. The Si 3p occupied valence states of the silicon atoms present within these structures are analysed. Because of the great sensitivity of these states to the physico-chemical environment of the Si atoms, it is possible to distinguish the emission from the center of the Si layer (amorphous silicon) to that of the interfacial zones between the Mo and Si layers. Thus, the presence of molybdenum silicides is evidenced in the interfacial zones. It is also shown that the relative proportion of interfacial silicides depends on the deposition conditions.     

Mo/Si软X射线多层膜的界面粗糙度研究

 用磁控溅射法分别制备了以Mo膜层和Si膜层为顶层的Mo/Si多层膜系列, 利用小角X射线衍射确定了各多层膜的周期厚度。以不同周期数的Mo/Si多层膜的新鲜表面近似等同于同一多层膜的内界面,通过原子力显微镜研究了多层膜界面粗糙度随膜层数的变化规律。并在国家同步辐射实验室测量了各多层膜的软X射线反射率。研究表明：随着膜层数的增加,Mo膜层和Si膜层的界面粗糙度先减小后增加然后再减小,多层膜的峰值反射率先增加后减小。     

用不同的Mo靶溅射功率制备Mo/Si多层膜

 用磁控溅射法制备了周期厚度和周期数均相同的Mo/Si多层膜,用原子力显微镜和小角X射线衍射分别研究了Mo靶溅射功率不相同时,Mo/Si多层膜表面形貌和晶相的变化。随后在国家同步辐射实验室测量了Mo/Si多层膜的软X射线反射率。研究发现,随着Mo靶溅射功率的增大,Mo/Si多层膜的表面粗糙度增加,Mo的特征X射线衍射峰也增强,Mo/Si多层膜的软X射线峰值反射率先增大后减小。     

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.     

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.     

Interface characteristics of Mo/Si and B4C/Mo/Si multilayers using non-destructive X-ray techniques

A methodology combining non-destructive X-ray techniques is proposed to study the interfacial zones of periodic multilayers. The used X-ray techniques are X-ray emission spectroscopy induced by electrons and X-ray reflectivity in the hard and soft X-ray ranges. The first technique evidences the presence of compounds at the interfaces and gives an estimation of the thickness of the interfacial zone. These informations are used to constrain the fit of the X-ray reflectivity curves that enables to determine the thickness and roughness of the various layers of the stacks. The results are validated in the soft X-ray range where the reflectivity curves are very sensitive to the chemical state of the elements present in the stack. The methodology is applied to characterize Mo/Si (1-4 nm/2 nm) and B₄C/Mo/Si (1 nm/2 nm/2 nm) multilayers. It is shown that the two interfacial zones of the Mo/Si multilayers are composed of the silicides MoSi₂ and Mo₅Si₃. It is found that the interface thickness is about to be 0.4-0.8 nm depending on the samples. The molybdenum silicides are also evidenced at the interfaces of the B₄C/Mo/Si multilayers. However, their interface thickness is 0.2 nm thinner than that of the same stack without the B₄C layers, these layers being at the Mo-on-Si side or at the Si-on-Mo side. Thus, the B₄C layers do not stop but only reduce the interdiffusion between the Mo and Si layers.     

Mo/Si multilayers used for the EUV normal incidence solar telescope

This paper first reviews an EUV normal incidence solar telescope that we have developed in our lab. The telescope is composed of four EUV telescopes and the operation wavelengths are 13.0 nm, 17.1 nm, 19.5 nm, and 30.4 nm. These four wavelengths, fundamental to the research of the solar activity and the atmosphere dynamics, are always chosen by the EUV normal incidence solar telescope. In the EUV region, almost all materials have strong absorption, so optics used in this region must be coated by the multila...     

Thermal stability and diffusion processes in Mo x Si y /Si multilayers studied with high-resolution RBS

Mo _x Si _y /Si multilayers with a period thickness of ∼7.5 nm and bilayers Mo _x Si _y /Si have been fabricated by e⁻-beam evaporation in UHV at a deposition temperature of 150°C [1]. The composition of the as-deposited layer systems and changes in the composition after baking the samples have been studied with high-resolution RBS. For a multilayer with a mixing ratioy/x≃2, no interdiffusion is observed up to a baking temperature of 830°C. For samples with a mixing ratioy/x≃1, diffusion is observed up to a baking temperature of 630°C, resulting in a mixing ratio close toy/x≃2. This mixing ratio remains almost stable up to ∼830°C, and considerable interdiffusion is only observed in those systems where regions with a mixing ratio smaller than 2 still exist. Possible reasons for the high thermal stability of the samples are the lack of a concentration gradient for Si in the system and/or the crystallization of MoSi₂.     

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     

Sensitive detection of laser damage to Mo/Si multilayers by picosecond ultrasonics

Picosecond ultrasonics is used to study the damage or degradation of Mo/Si multilayers caused by laser irradiation. Changes of surface phonon spectra in multilayers due to femtosecond laser damaging are observed in a regime of extremely low fluence level, well before the onset of melting, delamination, distortion, or material interdiffusion. It is found that the damage is shallow in depth (top few layers), and its mechanism is laser-induced changes in acoustic impedances, most likely due to stress relaxation. Its effects on extreme ultraviolet (EUV) reflectance and implications for projection EUV lithography are also discussed. We believe this technique has a potential application as a highly sensitive tool capable of detecting low-degree or early-stage damage of multilayers. PACS 68.65.Cd; 61.80.Ba; 78.47.+p     

Thermal behaviour of Co/Si/W/Si multilayers under rapid thermal annealing

The e-beam deposited multilayers (MLS) were studied under rapid thermal annealing (RTA) between 250°C and 1000°C during 30 s. MLS with five Co/Si/W/Si periods, each 13.9 nm (MLS1) and 18 nm (MLS2) were deposited onto oxidized Si substrates. Samples were analyzed by X-ray diffraction, hard and soft X-ray reflectivity measurements and grazing incidence X-ray diffuse scattering. The MLS period, interface roughness and its lateral and vertical correlations were obtained by simulation of the hard X-ray reflectivity and diffuse scattering spectra. The MLS1 with thinner Co layers is more temperature resistant. However, its soft X-ray reflectivity is smaller. The results show that this is because of shorter lateral and vertical correlation lengths of the interface roughness which may considerably influence the X-ray reflectivity of multilayers.     

Correction of figure errors on optical surfaces by laser-induced contraction of Mo/Si multilayers

We demonstrate that laser annealing of Mo/Si multilayers can be used to make controlled modifications of the surface figure of an optical substrate on a nanometer scale. In this experiment a superpolished optical flat was exposed to single pulses from an excimer laser to produce surface depressions of widths that varied from 10 microm to 0.5 mm and of depths in the range 2-50 nm. Simulations of thermally induced contraction of the Mo/Si multilayers are in good agreement with the observed deformations and indicate that the technique can be extended to larger deformations and higher resolution.     

Determination of layer-thickness fluctuations in Mo/Si multilayers by cross-sectional HR-TEM and X-ray diffraction

We present a method of deriving single layer thickness fluctuations of Mo/Si EUV multilayers from cross-sectional high-resolution transmission electron microscopy micrographs. The obtained thickness values for each layer are used in a layer model to calculate the grazing-incidence X-ray reflectivity (GIXRR) and the corresponding at-wavelength-reflectivity curves. Comparison with XRR measurements shows the strong effect of thickness fluctuations on the intensity of the secondary Kiessig fringes and the main Bragg maxima. This model results in substantially better reflectivity simulations than the standard periodic four-layer model or the assumption of statistically distributed (random) thickness errors. Results for reflectivity curves at 13-nm wavelength are discussed in terms of peak reflectivity, peak shift and further changes in the shape of the reflectivity curve. PACS 68.65.Ac; 68.37.Lp; 41.50.+h     

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     

Oxygen pressure dependent interfacial polarization of perovskite oxide multilayers on Si substrates

The SrTiO₃/La_0.9Sr_0.1MnO₃ (STO/LSMO) multilayers were fabricated on n-Si (1 0 0) substrates using a computer-controlled laser molecular-beam epitaxy (MBE) technique at 1 × 10⁻² Pa and 2 × 10⁻⁴ Pa oxygen partial pressures, respectively. The dielectric properties of the multilayers (MLs) were investigated. The differences of the dielectric properties of the two samples were explained by an impedance analysis technique, which indicates that the interfacial polarization has a close relationship with the oxygen pressure.     

Influence of background pressure on the microstructure and optical properties of Mo/Si multilayers fabricated by magnetron sputtering

Mo/Si multilayers were fabricated by using magnetron sputtering method at different background pressures:6×10-5 Torr,3×10-5 Torr,and 3×10-6 Torr.The reflectivity of the Mo/Si multilayers increased from 1.93% to 16.63%,and the center wavelength revealed a blue shift to 0.12 nm with the decrease of background pressure.Grazing incident X-ray diffraction(GIXRD) indicated that multilayers fabricated at high background pressure possessed better periodic structure and thinner Mo-on-Si interlayers.Low crystallization degree in(110) preferred the orientation of Mo layers and serious interdiffusion in the Mo/Si multilayers fabricated at low background pressure were observed by transmission electron microscopy(TEM).According to quantitative analysis of microstructural parameters,the Mo layers thickness and thickness ratio of Mo/Si multilayers both decreased and approached the design value gradually by the decrease of background pressure.In addition,the thicknesses of Mo-on-Si and Si-on-Mo interlayers were 1.17 nm and 0.85 nm respectively.It is suggested that the influence of background pressures on the microstructure has a critical role in determining the optical properties of Mo/Si multilayers.