Complex oxide perovskites have been widely studied for their diverse functional properties. When dimensionally reduced to epitaxial thin films and heterostructures these properties are frequently tunable, and the symmetry-breaking inherent to thin film structures can result in the emergence of new, novel, phenomena and properties. However, the ability to control and harness these structures relies on an atomic-level understanding and control of the growth process, made challenging by the lack of suitable in situ compositional characterization tools. In this work, the compositional-dependence of SrTiO3 on pulsed laser deposition growth parameters is investigated with in situ Auger electron spectroscopy and ex situ thin film x-ray diffraction, and verified with a simple escape depth model. We show that this is a suitable technique for monitoring subtle compositional shifts occurring during the deposition process, with broad implications for the continued development of thin film synthesis techniques.
We report the structural and transport properties of LaNiO3 thin films prepared by pulsed laser deposition technique. To understand the effects of film thickness, lattice mismatch and grain size on transport properties, various oriented substrates were used for deposition, including single-crystalline SrLaAlO4 (001), SrTiO3 (100) and LaAlO3 (100). To achieve a high quality LaNiO3 thin films, the vital parameters (such as laser fluence, substrate temperature, oxygen pressure, and deposition time) were optimized. The best quality films are found to be well textured samples with good crystalline …
We present results on growth of large area epitaxial ReS2 thin film both on c plane sapphire substrate and MoS2 template by pulsed laser deposition (PLD). Films tend to grow with (0001) ReS2 perpendicular to (0001) Al2O3 and (0001) ReS2 perpendicular to (0001) MoS2 parallel to (0001) Al2O3 at deposition temperature below 300 deg C. Films are polycrystalline grown at temperature above 300 deg C. The smoothness and quality of the films are significantly improved when grown on MoS2 template compared to sapphire substrate. The results show that PLD is suitable to grow ReS2 epitaxial thin film over…
We discuss the origin of the temperature dependence of resistivity observed in highly oriented LaNiO_3 thin films (of thickness d) grown on SrTiO_3 substrate by a pulsed laser deposition technique. All the experimental data are found to collapse into a single universal curve [T/T_{sf}(d)]^{3/2} for the entire temperature interval (20K<T<300K) with T_{sf}(d) being the onset temperature for triggering a resonant scattering of conduction electrons by spin fluctuations in LaNiO_3/SrTiO_3 heterostructure.
We present a comparative study on the influence of applied magnetic field on the resistance of $C_{1-x}Co_x$ thin films (with $x=0.1$, $0.15$ and $0.2$) grown on $Si$ substrate by pulsed laser deposition technique. It is found that the behavior of magnetoresistance (MR) drastically depends on the temperature. Namely, at low temperatures MR is positive and its behavior is governed by the field mediated weak localization scenario. While at high temperatures MR turns negative and its behavior is dominated by electron scattering on ferromagnetic cobalt atoms.
We report the epitaxial growth of Ca3SnO antiperovskite oxide films on (001)-oriented cubic yttria-stabilized zirconia (YSZ) substrates by using a conventional pulsed laser deposition (PLD) technique. In this work, a sintered Ca3SnO pellet is used as the ablation target. X-ray diffraction measurements demonstrate the (001) growth of Ca3SnO films with the antiperovskite structure and a cube-on-cube orientation relationship to the YSZ substrate. The successful synthesis of the antiperovskite phase is further confirmed by x-ray photoemission spectroscopy. These results strongly suggest that antip…
We present measurements of resistivity $ρ$ in highly oriented $LaNiO_3$ films grown on $LaAlO_3$ substrates by using a pulsed laser deposition technique. The experimental data are found to follow a universal $ρ(T) \propto T^{3/2}$ dependence for the entire temperature interval ($20K<T<300K$). The observed behavior has been attributed to a resonant scattering of electrons on antiferromagnetic fluctuations (with a characteristic energy $\hbar ω_{sf}\simeq 2.1meV$) triggered by spin-density wave propagating through the interface boundary of $LaNiO_3/LaAlO_3$ sandwich.
Pulsed Laser Deposition (PLD) is widely used to grow epitaxial thin films of quantum materials such as complex oxides. Here, we use in-situ X-ray scattering to study homoepitaxy of SrTiO$_3$ by energetic (e-) and thermalized (th-) PLD. We find that e-PLD suppresses the lateral growth of two-dimensional islands, which suggests that energetic particles break up smaller islands. Fast interlayer transport occurs for both e-PLD and th-PLD, implying a process operating on sub-microsecond timescales that doesn't depend strongly on the kinetic energy of the incident particles.
Pulsed laser deposition of SrTiO3/LaGaO3 and SrTiO3/LaAlO3: plasma plume effects
分析了脉冲激光沉积SrTiO 3/LaGa O 3和SrTiO 3/LaAl O 3界面的烧蚀物质的动能。用快速摄影和空间分辨发射光谱研究了LaGaO 3和LaAlO 3等离子体羽流。反射高能电子衍射进行证明一个逐层生长高达10-1毫巴的氧气压力。高能等离子体羽流的二维生长和在不同的氧气生长压力的界面缺陷的存在下的作用进行了讨论，鉴于在这样的极性/非极性接口开发的导电性能。
Wires of sp-hybridized carbon atoms are attracting interest for both fundamental aspects of carbon science and for their appealing functional properties. The synthesis by physical vapor deposition has been reported to provide sp-rich carbon films but still needs to be further developed and understood in detail. Here the synthesis of carbon-atom wires (CAWs) has been achieved by nanosecond pulsed laser deposition (PLD) expoliting the strong out-of-equilibrium conditions occurring when the ablation plasma is confined in a background gas. Surface Enhnaced Raman scattering (SERS) spectra of deposi…
Epitaxy of Fe3O4 on Si(001) by pulsed laser deposition using a TiN/MgO buffer layer
氧化物材料在硅（Si）衬底上的外延对于使用氧化物的各种物理性质如铁电性、铁磁性或超导性的未来功能器件具有极大的兴趣。最近，具有高自旋极化的载流子的材料已经成为自旋电子学中的氧化物-氧化物混合器件的关注点。在这里，我们报告的脉冲激光沉积磁铁矿（Fe 3 O 4）在Si（001）衬底上清洁的原位激光束高温处理。在沉积氮化钛（TiN）和氧化镁（MgO）的双缓冲层之后，可以生长高质量的外延磁铁矿层，如通过RHEED强度振荡和高分辨率X射线衍射所验证的。
The influence of technological parameters of pulsed-DC chemical vapour deposition on the deposition rate, the mechanical properties and the residual stress of diamond-like carbon (DLC) coatings deposited onto a martensitic steel substrate, using a Ti buffer layer between coating and substrate, has been studied. For this purpose, a Plackett-Burman experiment design and Pareto charts were used to identify the most significant process parameters, such as deposition time, methane flux, chamber pressure, power, pulse frequency, substrate roughness and thickness of titanium thin film. The substrate …
We report the growth of highly c-axis oriented topological insulator (TI) BiSbTe1.5Se1.5 (BSTS) thin films by pulsed laser deposition (PLD) technique. The various growth parameters such as substrate temperature, Argon pressure in the deposition chamber and target to substrate distance are tuned to obtain the optimized conditions essential for stoichiometric and bulk insulating TI thin films. These films are highly c-axis oriented and exhibit all the four Raman modes characteristic to the R-3m space group. The quality of the deposited thin films is investigated using X-ray diffraction for cryst…
We present a synthesis/processing method for fabricating ferrimagnetic insulator (Bi-doped yttrium iron garnet) thin films with tunable magnetic anisotropy. Since the desired magnetic properties rely on controllable thickness and successful doping, we pay attention to the entire synthesis/processing procedure (nanopowder synthesis, nanocrystalline target preparation and pulsed laser deposition (PLD)). Atomically flat films were deposited by PLD on (111)-orientated yttrium aluminum garnet. We show a significant enhancement of perpendicular anisotropy in the films, caused by strain-induced aniso…
To visualize the topography of thin oxide films during growth, thereby enabling to study its growth behavior quasi real-time, we have designed and integrated an atomic force microscope (AFM) in a pulsed laser deposition (PLD) vacuum setup. The AFM scanner and PLD target are integrated in a single support frame, combined with a fast sample transfer method, such that in-situ microscopy can be utilized after subsequent deposition pulses. The in-situ microscope can be operated from room temperature (RT) up to 700$^\circ$C and at (process) pressures ranging from the vacuum base pressure of 10$^{-6}…
Nickel carbon based multi-layers are a viable route towards future hard X-ray and soft $γ$-ray focusing telescopes. Here, we study the Pulsed Laser Deposition growth conditions of such bilayers by Reflective High Energy Electron Diffraction, X-ray Reflectivity and Diffraction, Atomic Force Microscopy, X-ray Photoelectron Spectroscopy and cross-sectional Transmission Electron Microscopy analysis, with emphasis on optimization of process pressure and substrate temperature during growth. The thin multi-layers are grown on a treated SiO substrate resulting in Ni and C layers with surface roughness…
We fabricate and compare nanocomposite thin-film ZnO chemoresistive acetone sensors with gold or palladium nanoparticles on the surface, at low operating temperatures. The sensors are fabricated by pulsed laser deposition and operate in the temperature range 159-200oC. The ZnO films are polycrystalline, crystallizing mainly at the (002) and (101) orientations of the hexagonal phase. The nanocomposite ZnO:Au and ZnO:Pd sensors have a lower detection limit and show a response enhancement factor between 2-7, compared with pure ZnO sensors. The ZnO:Pd sensor performs better than the ZnO:Au sensor.…
The authors report in situ Auger electron spectroscopy (AES) of the surfaces of complex oxides thin films grown by pulsed laser deposition (PLD). The authors demonstrate the utility of the technique in studying chemical composition by collecting characteristic Auger spectra of elements from samples such as complex oxide thin films and single crystals as well as metal foils. In the case of thin films, AES studies can be performed with single unit cell precision by monitoring thickness during deposition with reflection high energy electron diffraction (RHEED). The authors address some of the cha…
Micron-thick boron films have been deposited by Pulsed Laser Deposition in vacuum on several substrates at room temperature. The use of high energy pulses (>700 mJ) results in the deposition of smooth coatings with low oxygen uptake even at base pressures of 10$^{-4}$ - 10$^{-3}$ Pa. A detailed structural analysis, by X-Ray Diffraction and Raman, allowed to assess the amorphous nature of the deposited films as well as to determine the base pressure that prevents boron oxide formation. In addition the crystallization dynamics has been characterized showing that film crystallinity already improv…
We deposit intrinsic hydrogenated amorphous silicon (a-Si:H) thin films by reactive pulsed laser deposition, for various hydrogen pressures in the 0-20 Pa range, at a low deposition temperature of 120C, and investigate the hydrogen incorporation, structural, optical, and electrical properties of the films, as a function of the ambient hydrogen pressure. The film thickness decreases linearly as the hydrogen pressure increases. The hydrogen content of the films is determined by infrared spectroscopy and the optical bandgap from UV-Vis-NIR transmittance and reflectance measurements. Electric meas…
Here we systematically explore the use of pulsed laser deposition technique (PLD) to grow three basic oxides that have rocksalt structure but different chemical stability in the ambient atmosphere: NiO (stable), MnO (metastable) and EuO (unstable). By tuning laser fluence, an epitaxial single-phase nickel oxide thin-film growth can be achieved in a wide range of temperatures from 10 to 750 °C. At the lowest growth temperature, the out-of-plane strain raises to 1.5%, which is five times bigger than that in a NiO film grown at 750 °C. MnO thin films that had long-range ordered were successfully …
We report on an investigation on the properties of ultra-low density, fractal, Carbon nanofoams fabricated with the nanosecond and femtosecond pulsed-laser deposition (PLD) techniques. We measure through innovative techniques the foam mean density and the properties of the fractal aggregates composing the film (i.e. nanoparticles diameter, fractal dimension, and gyration radius) as a function of several PLD process parameters, namely the background gas pressure and the laser pulse characteristics (energy, time duration, repetition rate). We discuss the experimental observation on the basis of …
We report structural, optical, temperature and frequency dependent dielectric, and energy storage properties of pulsed laser deposited (100) highly textured BaZr(x)Ti(1-x)O3 (x = 0.3, 0.4 and 0.5) relaxor ferroelectric thin films on La0.7Sr0.3MnO3/MgO substrates which make this compound as a potential lead-free capacitive energy storage material for scalable electronic devices. A high dielectric constant of ~1400 - 3500 and a low dielectric loss of <0.025 were achieved at 10 kHz for all three compositions at ambient conditions. Ultrahigh stored and recoverable electrostatic energy densities as…
Application of transition metal dichalcogenides (TMDC) in photonic, optoelectronic or valleytronic devices requires the growth of continuous monolayers, heterostructures and alloys of different materials in a single process. We present a facile pulsed thermal deposition method which provides precise control over layer thickness and stoichiometry of two-dimensional systems. The versatility of the method is demonstrated on ternary monolayers of Mo$_{1-x}$W$_{x}$S$_{2}$ and on heterostructures combining metallic TaS$_{2}$ and semiconducting MoS$_{2}$ layers. The fabricated ternary monolayers cove…
Bi$_2$Te$_3$ is a material with high efficiency of thermoelectric energy conversion. Recently, it was also recognized as a topological insulator, and is often used as the basis for creation of other types of topological matter. Pulsed laser deposition (PLD) is widely considered as a simple method for growing of multicomponent films, but not as a tool for van der Waals epitaxy. We demonstrate here that the van der Waals epitaxy of Bi$_2$Te$_3$ is indeed impossible in vacuum PLD, but is possible in the presence of a background gas, which is confirmed by the results of scanning tunneling microsco…
(111)NiO epitaxial layers are grown on c-sapphire substrates by pulsed laser deposition (PLD) technique. Structural and morphological properties of the films are studied using in-plane as well as out-of-plane high resolution X-ray diffraction and atomic force microscopy techniques as functions of growth temperature, oxygen pressure and the pulses count of the laser. The study shows that continuous epitaxial films of thickness as low as 3 nm with high crystalline quality, smooth surface and interface morphology can be grown by this technique. The study also reveals the co-existence of 60°-rotat…
In this chapter we will describe a new development of combinatorial pulsed laser deposition (CPLD) which targets the exploration of interface libraries. The idea is to modulate continuously the composition of interfaces on a few atomic layers in order to alter their functional properties. This unique combinatorial synthesis of interfaces is possible due to very specific PLD characteristics. The first one is its well-known ability for complex oxide stoichiometry transfer from the target to the film. The second one is the layer by layer control of thin film growth at the atomic level using in-si…
Rare-earth nickelates are strongly correlated oxides displaying a metal-to-insulator transition at a temperature tunable by the rare-earth ionic radius. In PrNiO$_3$ and NdNiO$_3$, the transition is very sharp and shows an hysteretic behavior akin to a first-order transition. Both the temperature at which the transition occurs and the associated resistivity change are extremely sensitive to doping and therefore to off-stoichiometry issues that may arise during thin film growth. Here we report that strong deviations in the transport properties of NdNiO$_3$ films can arise in films grown consecu…
Homogeneous highly epitaxial LaSrMnO3 (LSMO) thin films have been grown on Yttria-stabilized-Zirconia (YsZ) / CeO2 buffer layers on technological relevant 4" silicon wafers using a Twente Solid State Technology B.V. (TSST) developed large area Pulsed Laser Deposition (PLD) setup. We study and show the results of the effect of an additional SrRuO3 buffer layer on the growth temperature dependent structural and magnetic properties of LSMO films. With the introduction of a thin SrRuO3 layer on top of the buffer stack, LSMO films show ferromagnetic behaviour for growth temperatures as low as 250C.…
High quality Van der Waals chalcogenides are important for phase change data storage, thermoelectrics, and spintronics. Using a combination of statistical design of experiments and density functional theory, we clarify how the out-of-equilibrium van der Waals epitaxial deposition methods can improve the crystal quality of Sb2Te3 films. We compare films grown by radio frequency sputtering and pulsed laser deposition (PLD). The growth factors that influence the crystal quality for each method are different. For PLD grown films a thin amorphous Sb2Te3 seed layer most significantly influences the …
Aluminum oxide thin films were deposited on silicon substrates under different deposition conditions using pulse pressure metal organic chemical vapour deposition (PP-MOCVD). The current study investigates into the growth mechanism of the deposited film and the control of the film morphology by varying the processing parameters of PP-MOCVD - choice of solvent, concentration, and presence of a shield. Aluminum sec-butoxide (ASB) was used as the aluminum source while hexane and toluene were used as the solvents. The films were deposited at 475oC at different precursor concentrations. It was obse…
Optical and magneto-optical interactions in Co-doped CeO$_2$ thin films prepared by pulsed laser deposition
Charles University（查理大学）；University of Pardubice（帕尔杜比采大学）；University of Electronic Science and Technology of China（电子科技大学）；Chungnam National University（忠南国立大学）；Massachusetts Institute of Technology（麻省理工学院）
The preparation in thin film form of the known icosahedral phase in Ti-Ni-Zr bulk alloys has been investigated as a function of substrate temperature. Films were deposited by Pulsed Laser Deposition on sapphire substrates at temperatures ranging from room temperature to 350$^\circ$C. Morphological and structural modifications have been followed by grazing incidence and $θ$-2$θ$ X-ray diffraction, transmission electron diffraction and imaging. Chemical composition has been analysed by Electron Probe Micro-Analysis. The in-depth variation of composition has been studied by Secondary Neutral Mass…
Recently, Bi2O2Se is discovered as a promising two-dimensional (2D) semiconductor for next generation electronics, due to its moderate bandgap size, high electron mobility and pronounced ambient stability. Meanwhile, it has been predicted that high quality Bi2O2Se-related heterostructures may possess exotic physical phenomena, such as piezoelectricity and topological superconductivity. Herein, we report the first successful heteroepitaxial growth of Bi2O2Se films on SrTiO3 substrates via pulsed laser deposition (PLD) method. Films obtained under optimal conditions show an epitaxial growth with…
