Optical models for the ellipsometric characterization of carbon nitride layers prepared by inverse pulsed laser deposition

Amorphous carbon nitride (CN_x) films were prepared by KrF excimer laser ablation of a graphite target in a nitrogen atmosphere in the inverse PLD geometry. From the ellipsometric point of view, the challenging properties of these films were their exponentially decaying thickness as a function of distance from the ablation source, accompanied by a laterally varying chemical composition and structure. Optical models were developed to accurately describe the dependence of film properties on distance from the ablation, layer thickness, and nitrogen pressure. Multi-layer models were used to characterize the surface roughness as well as lateral inhomogeneities. Multiple angles of incidence and multiple wavelengths were applied in the ranges of 66-72° and 250-1000 nm, respectively. A microspot capability of the spectroscopic ellipsometer (with a spot size of about 100 μm) was exploited to decrease the error caused by the lateral inhomogeneity within the measurement spot. Material properties were derived using the empirical Cauchy dispersion model as well as the Tauc-Lorentz parametric dielectric function model. These models allowed the quantitative determination of the band gap and the oscillator parameters in addition to the layer thicknesses and dielectric functions.     

Atomic force microscopic characterization of films grown by inverse pulsed laser deposition

Carbon nitride films have been deposited by KrF excimer laser ablation of a rotating graphite target in 5 Pa nitrogen ambient in an inverse pulsed laser deposition configuration, where the backward motion of the ablated species is utilised for film growth on substrates lying in the target plane. Topometric AFM scans of the films, exhibiting elliptical thickness distribution, have been recorded along the axes of symmetry of the deposition area. High resolution AFM scans revealed the existence of disk-like, or somewhat elongated rice-like features of 5-10 nm average thickness and ∼100 nm largest dimension, densely packed over the whole, approximately 14 × 10 cm² deposition area. The RMS roughness of the film decreased from 9 nm near to the laser spot down to 2 nm in the outer regions. Even the highest RMS value obtained for IPLD films was less than half of the typical, 25 nm roughness measured on simultaneously deposited PLD films.     

脉冲激光沉积动力学研究进展

脉冲激光沉积技术是现代常用的先进薄膜材料制备技术之一.文章在简要介绍脉冲激光沉积技术及其进展的基础上,较全面地介绍了脉冲激光沉积动力学的基本物理图像和动力学构架,深入地探讨了激光烧蚀靶材过程、等离子体膨胀过程和薄膜沉积过程的动力学规律,阐述了我国学者在脉冲激光沉积动力学研究方面的贡献,例如包括脉冲激光沉积三个工艺过程自洽的统一模型,等离子体膨胀的冲击波模型,基于局域能量动量守恒定律的新等离子体演化动力学模型,包括热源项、蒸发项、等离子体屏蔽效应和动态物性参数的烧蚀热传导模型,考虑电子碰撞效应和能带结构变化的修正双温模型,能统一描写从纳秒级到飞秒级脉冲激光烧蚀规律的统一双温模型等.     

Homogeneous films by inverse pulsed laser deposition

Recently, we proposed an alternative arrangement to traditional on- or off-axis PLD geometries, termed inverse PLD (IPLD) that is capable of producing films of improved surface morphology. Two configurations of this new target-substrate arrangement were developed, namely static and co-rotating IPLD. In the static IPLD configuration, the substrate is stationary with respect to the ablated spot; while in the co-rotating IPLD configuration the substrate is fixed to the target surface and rotates simultaneously with the target, hence offering an appealingly simple approach to homogenize film properties.Here we report the growth of CN_x and Ti films, simultaneously deposited in the co-rotating and static IPLD arrangements. The homogeneity of the co-rotating films is described by a thickness inhomogeneity index, which allows for the comparison of films of different lateral dimension. A semi-analytical, semi-numerical model is proposed to derive the radial variation of the growth rate of co-rotating IPLD films from the lateral growth rate distributions measured along the symmetry axes of static IPLD films. The laterally averaged growth rate, LAGR is used to describe how the ambient pressure affects growth in the 0.5-50 Pa domain. As an example, the absolute error between the measured and calculated radial growth rate variation, obtained at 5 Pa, was less than 3%, while the LAGR of CN_x layers grown by co-rotating IPLD was predicted with 20% accuracy.     

金属Fe薄膜的PLD制备及其非线性光学性质研究

采用脉冲激光沉积（PLD）技术在MgO基片上制备了金属Fe薄膜.利用原子力显微镜研究了不同制备温度对薄膜表面形貌的影响.x射线衍射分析表明沉积温度大于500℃时，Fe薄膜在MgO基片上有很好的结晶性，并有单一取向.通过z扫描方法测量了超薄Fe膜的光学非线性，得到了Fe薄膜的非线性折射率n₂＝709×10^-5cm²/ kW，非线性吸收系数 β＝-552×10^-3cm/W. 关键词： Fe薄膜 非线性 脉冲激光沉积     

等离子体增强脉冲激光沉积o-BN薄膜

利用等离子体增强脉冲激光沉积系统在Si（100）基底上沉积出了高质量的o-BN薄膜,利用红外光谱（FTIR）、X射线衍射谱（XRD）和原子力显微镜照片对o-BN薄膜进行了表征.通过红外光谱（FTIR）得到o-BN薄膜的红外峰特征峰值为1189cm^-1,1585cm^-1和1450cm^-1;由XRD谱得到o-BN薄膜的（111）,（020）,（021）,（310）和（243）各晶面的衍射峰, 特别是（310）和（243）晶面的衍射峰非常强;通过原子力显微镜照片清楚看到BN薄膜具有尖状突起的表面形貌. 关键词： 等离子体增强脉冲激光沉积 氮化硼薄膜 X射线衍射谱     

脉冲激光气相沉积法制备的非晶CH薄膜特性分析

采用脉冲激光气相沉积(PLD)法,研究了氢气压强对非晶CH薄膜性能的影响。原子力显微镜图和白光干涉图显示,薄膜表面平整致密,随着氢气压强增大,粗糙度变大。拉曼光谱分析表明,氢气压强增加,G峰和D峰位置都在向高波数方向移动。傅里叶变换红外光谱分析显示,薄膜中存在sp3—CH2和sp2—CH等基团。最后,采用PLD漂浮法在最优参数氢气压强为0.3 Pa下,成功制备了不同厚度(100~300 nm)、满足一定力学强度、无明显宏观缺陷的自支撑CH薄膜。     

Carrier storage in Ge nanoparticles produced by pulsed laser deposition

In this work, we report on the electrical characterization of Ge nanoparticles (NPs) produced by pulsed laser deposition (PLD) at room temperature (RT) in Ar gas inert atmosphere using a shadowed off‐axis deposition geometry. Our results show that functional thin films of crystalline Ge NPs embedded between thin alumina films can be obtained on p‐type Si(100) substrates following a low temperature and short rapid thermal annealing (RTA) treatment. Metal–oxide–semiconductor (MOS) structures with and without Ge NPs embedded in the alumina were prepared for the electrical measurements. The results indicate a strong memory effect at relatively low programming voltages (±4 V) due to the presence of Ge NPs. (© 2012 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Self-catalyst synthesis of aligned ZnO nanorods by pulsed laser deposition

High-density well-aligned ZnO nanorods were successfully synthesized on ZnO-buffer-layer coated indium phosphide (InP) (100) substrates by a pulsed laser deposition (PLD) method. Scanning electron microscopy images show that the ZnO buffer layer formed uniform drip-like structure and ZnO nanorods were well-oriented perpendicular to the substrate surface. The sharp diffraction peak observed at 34.46° in X-ray diffraction scanning pattern suggests that the ZnO nanorods exhibit a (002)-preferred orientation. The PL spectra of ZnO samples shows a strong near band edge emission centered at about 380 nm and a weak deep level emission centered at around 495 nm, and it demonstrates that the ZnO nanorods produced in this work have high optical quality, which sheds light on further applications for nanodevices. Supported by the National Natural Science Foundation of China (Grant No. 50532080), the Science & Technology Foundation for Key Laboratory of Liaoning Province (Grant No. 20060131), and the Doctoral Project by China Ministry of Education (Grant No. 20070141038)     

New aspects on pulsed laser deposition of aligned carbon nanotubes

We have grown carbon nanotubes (CNT) by pulsed laser deposition (PLD) at 1000 °C in Ar atmosphere. A Nd/YAG laser was used for irradiation of a graphite target containing Ni and Co rods. High-resolution scanning electron microscopy (HRSEM) and transmission electron microscopy (TEM) images showed that “closed” carbon nanotubes were grown between clusters of metallic particles, so that the individual nanotubes were arranged in parallel to each other forming a shape of “Rope-Bridge”. The nanotubes structure was analyzed by high-resolution transmission electron microscopy (HRTEM) and their type was found to be of MWNT, containing about five SWNT. Total diameter was 5-20 nm and their length was about 1 μm. High homogeneous distribution carbon nanotubes were grown and different structures were observed such as well-aligned carbon nanotubes, bamboo-like and Y-junction carbon nanotubes.     

NaF薄膜的脉冲激光沉积法制备与结构研究

采用脉冲激光沉积(PLD)方法在Si(100)衬底上制备了NaF薄膜。在激光重复频率2 Hz,能量密度3 J/cm2,本底真空度5×10-5 Pa的条件下,研究衬底温度对薄膜沉积速率及结构的影响。台阶仪分析表明：薄膜的沉积速率随衬底温度增加呈指数函数增加,算出NaF薄膜的反应激活能为48.67 kJ/mol。原子力显微镜分析表明：薄膜致密而光滑,均方根粗糙度为0.553 nm。扫描电镜截面微观形貌分析表明：薄膜呈现柱状结构。X射线衍射分析表明：NaF薄膜为面心立方晶体结构,并具有显著的择优取向;当衬底温度约为400 ℃时,平均晶粒尺寸最大(129.6 nm),晶格微应变最小(0.225%)。     

脉冲激光气相沉积法制备钴纳米薄膜实验研究

采用脉冲激光沉积技术制备了钴纳米薄膜,分析和讨论了不同背景气压和脉冲频率对钴纳米薄膜表面形貌的影响及纳米微粒的形成机理。实验结果表明：在低背景气压下,等离子体羽辉自身粒子之间的碰撞占主导作用,容易形成液滴;在较高背景气压下,等离子体羽辉边缘粒子和背景气体粒子之间的碰撞占主导作用,容易形成小岛并凝聚成微颗粒;在4Hz的脉冲重复频率和5Pa背景气压下生长出单分散性良好的钴纳米颗粒。     

Growth and characterization of pulsed laser deposited ZnO thin films

One of the most important and promising materials from metal oxides is ZnO with specific properties for near UV emission and absorption optical devices. The properties of ZnO thin films strongly depend on the deposition method. Among them, pulsed laser deposition (PLD) plays an important role for preparing various kinds of ZnO films, e.g. doped, undoped, monocrystalline, and polycrystalline. Different approaches — ablation of sintered ZnO pellets or pure metallic Zn as target material are described. This contribution is comparing properties of ZnO thin films deposited from pure Zn target in oxygen atmosphere and those deposited from sintered ZnO target. There is a close connection between final thin film properties and PLD conditions. The surface properties of differently grown ZnO thin films are measured by secondary ion mass spectrometry (SIMS), atomic force microscopy (AFM) and scanning electron microscopy (SEM). Furthermore, different approaches — ablation of sintered ZnO pellet or pure metallic Zn as target materials are described. The main results characterize typical properties of ZnO films versus technological parameters are presented. Presented at 5-th International Conference Solid State Surfaces and Interfaces, November 19–24, 2006, Smolenice Castle, Slovakia     

Indomethacin nanoparticles directly deposited on the fluidized particulate excipient by pulsed laser deposition

Nanoparticles of indomethacin (IM), a sparingly soluble drug in water, were prepared by pulsed laser deposition with Nd: YAG laser at 1064 nm. Variation of the deposition rate (DR) with various experimental conditions, such as species and pressure of the background gas, and laser fluence, was discussed. We obtained highest DR, 2.7 g/cm²min, under He at 100 Pa with the laser fluence of 25 J/cm². In the deposited solid product, no trace of drug decomposition was observed by HPLC. Deposition of IM nanoparticles was achieved on the fluidized excipient, potato starch particles of 20 m regime. By TEM observation and zeta potential distribution measurement, we confirmed that surface of excipient particles was fully covered by nanoparticles of IM. Thus, the present method enables us a new method of one-step preparation of drug-excipient nanocomposites to eliminate tedious problems associated with nanoparticles handling.     

脉冲激光制膜过程中等离子体演化规律的研究

利用有限差分法对脉冲激光沉积(PLD)技术制备KTa065Nb035O3(KTN)薄膜过程中等离子体在等温和绝热两个阶段的速度演化进行了模拟，并给出了其中主要粒子在空间的具体演化规律，对等离子体在空间膨胀的物理机制，进行了深入的讨论，给出了相应演化过程的物理图像，并揭示了等离子体羽辉在膨胀过程中呈现椭球外形的内在原因.     

Tribological properties of diamond-like carbon films deposited by pulsed laser arc deposition

A novel method, pulsed laser arc deposition combining the advantages of pulsed laser deposition and cathode vacuum arc techniques, was used to deposit the diamond-like carbon (DLC) nanofilms with different thicknesses. Spectroscopic ellipsometer, Auger electron spectroscopy, x-ray photoelectron spectroscopy, Raman spectroscopy, atomic force microscopy, scanning electron microscopy and multi-functional friction and wear tester were employed to investigate the physical and tribological properties of the deposited films. The results show that the deposited films are amorphous and the sp$^{2}$, sp$^{3}$ and C--O bonds at the top surface of the films are identified. The Raman peak intensity and surface roughness increase with increasing film thickness. Friction coefficients are about 0.1, 0.15, 0.18, when the film thicknesses are in the range of 17--21~nm, 30--57~nm, 67--123~nm, respectively. This is attributed to the united effects of substrate and surface roughness. The wear mechanism of DLC films is mainly abrasive wear when film thickness is in the range of 17--41~nm, while it transforms to abrasive and adhesive wear, when the film thickness lies between 72 and 123~nm.     

脉冲激光气相沉积法制备的非晶CH薄膜特性分析

采用脉冲激光气相沉积(PLD)法,研究了氢气压强对非晶CH薄膜性能的影响。原子力显微镜图和白光干涉图显示,薄膜表面平整致密,随着氢气压强增大,粗糙度变大。拉曼光谱分析表明,氢气压强增加,G峰和D峰位置都在向高波数方向移动。傅里叶变换红外光谱分析显示,薄膜中存在sp3—CH2和sp2—CH等基团。最后,采用PLD漂浮法在最优参数氢气压强为0.3 Pa下,成功制备了不同厚度（100~300 nm）、满足一定力学强度、无明显宏观缺陷的自支撑CH薄膜。     

Growth of preferentially-oriented AlN films on amorphous substrate by pulsed laser deposition

Preferentially-oriented aluminum nitride (AlN) films are grown directly on natively-oxidized Si (100) substrate by pulsed laser deposition (PLD) in nitrogen (N₂) environment. The AlN preferential orientation changes from (002) to (100) with increasing N₂ pressure. Such different behaviors are discussed in terms of deposition-rate-dependent preferential orientation, kinetic energy of depositing species and confinement of laser plume. Finally, sample deposited at 0.9 Pa is proved to have the highest (002) peak intensity, the lowest FWHM value, the highest deposition rate and a relatively low RMS roughness (1.138 nm), showing the optimal growth condition for c-axis-oriented AlN growth at this N₂ pressure.     

Magnetic/non-magnetic nanoparticles films with peculiar properties produced by ultrashort pulsed laser deposition

Films of magnetic nanoparticles uniformly mixed with non-magnetic nanoparticles have been produced by ultrashort pulsed laser deposition. These films present innovative characteristics with respect to their counterparts produced by standard techniques, as for example nanosecond laser ablation or sputtering, due to the peculiar shape and preferential distribution of their constituent nanoparticles. In the present investigation, the difficult coalescence among the deposited nanoparticles, specific characteristic of the ultrashort pulsed laser deposition, is particularly stressed for what concerns its effect on the collective magnetic behaviour. In particular, we observed that, even for a significant fraction of magnetic particles, the films exhibit an unusual high remanent magnetization, together with relatively low values of saturation and coercive fields, showing a strong squareness of the hysteresis loops. In perspective, these nanogranular films appear very promising for potential application as permanent magnets and in magnetic recording.     

Study of the structure and electrical properties of the copper nitride thin films deposited by pulsed laser deposition

Copper nitride thin films were prepared on glass and silicon substrates by ablating a copper target at different pressure of nitrogen. The films were characterized in situ by X-ray photoelectron spectroscopy (XPS), Auger electron spectroscopy (AES) and ex situ by X-ray diffraction (XRD). The nitrogen content in the samples, x = [N]/[Cu], changed between 0 and 0.33 for a corresponding variation in nitrogen pressure of 9 × 10⁻² to 1.3 × 10⁻¹ Torr. Using this methodology, it is possible to achieve sub-, over- and stoichiometric films by controlling the nitrogen pressure. The XPS results show that is possible to obtain copper nitride with x = 0.33 (Cu₃N) and x = 0.25 (Cu₄N) when the nitrogen pressure is 1.3 × 10⁻¹ and 5 × 10⁻² Torr, respectively. The lattice constants obtained from XRD results for copper nitride with x = 0.25 is of 3.850 Å and with x = 0.33 have values between 3.810 and 3.830 Å. The electrical properties of the films were studied as a function of the lattice constant. These results show that the electrical resistivity increases when the lattice parameter is decreasing. The electrical resistivity of copper nitride with x = 0.25 was smaller than samples with x = 0.33.