Low-Temperature Al2O3 Atomic Layer Deposition
TL;DR: In this article, the properties of low-temperature Al2O3 ALD films were investigated versus growth temperature by depositing films on Si(100) substrates and quartz crystal microbalance (QCM) sensors.
Abstract: Al2O3 films were deposited by atomic layer deposition (ALD) at temperatures as low as 33 °C in a viscous-flow reactor using alternating exposures of Al(CH3)3 (trimethylaluminum [TMA]) and H2O. Low-temperature Al2O3 ALD films have the potential to coat thermally fragile substrates such as organic, polymeric, or biological materials. The properties of low-temperature Al2O3 ALD films were investigated versus growth temperature by depositing films on Si(100) substrates and quartz crystal microbalance (QCM) sensors. Al2O3 film thicknesses, growth rates, densities, and optical properties were determined using surface profilometry, atomic force microscopy (AFM), QCM, and spectroscopic ellipsometry. Al2O3 film densities were lower at lower deposition temperatures. Al2O3 ALD film densities were 3.0 g/cm3 at 177 °C and 2.5 g/cm3 at 33 °C. AFM images showed that Al2O3 ALD films grown at low temperatures were very smooth with a root-mean-squared (RMS) roughness of only 4 ± 1 A. Current−voltage and capacitance−voltage...
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4,756 citations
TL;DR: In this paper, the surface chemistry of the trimethylaluminum/water ALD process is reviewed, with an aim to combine the information obtained in different types of investigations, such as growth experiments on flat substrates and reaction chemistry investigation on high-surface-area materials.
Abstract: Atomic layer deposition(ALD), a chemical vapor deposition technique based on sequential self-terminating gas–solid reactions, has for about four decades been applied for manufacturing conformal inorganic material layers with thickness down to the nanometer range. Despite the numerous successful applications of material growth by ALD, many physicochemical processes that control ALD growth are not yet sufficiently understood. To increase understanding of ALD processes, overviews are needed not only of the existing ALD processes and their applications, but also of the knowledge of the surface chemistry of specific ALD processes. This work aims to start the overviews on specific ALD processes by reviewing the experimental information available on the surface chemistry of the trimethylaluminum/water process. This process is generally known as a rather ideal ALD process, and plenty of information is available on its surface chemistry. This in-depth summary of the surface chemistry of one representative ALD process aims also to provide a view on the current status of understanding the surface chemistry of ALD, in general. The review starts by describing the basic characteristics of ALD, discussing the history of ALD—including the question who made the first ALD experiments—and giving an overview of the two-reactant ALD processes investigated to date. Second, the basic concepts related to the surface chemistry of ALD are described from a generic viewpoint applicable to all ALD processes based on compound reactants. This description includes physicochemical requirements for self-terminating reactions,reaction kinetics, typical chemisorption mechanisms, factors causing saturation, reasons for growth of less than a monolayer per cycle, effect of the temperature and number of cycles on the growth per cycle (GPC), and the growth mode. A comparison is made of three models available for estimating the sterically allowed value of GPC in ALD. Third, the experimental information on the surface chemistry in the trimethylaluminum/water ALD process are reviewed using the concepts developed in the second part of this review. The results are reviewed critically, with an aim to combine the information obtained in different types of investigations, such as growth experiments on flat substrates and reaction chemistry investigation on high-surface-area materials. Although the surface chemistry of the trimethylaluminum/water ALD process is rather well understood, systematic investigations of the reaction kinetics and the growth mode on different substrates are still missing. The last part of the review is devoted to discussing issues which may hamper surface chemistry investigations of ALD, such as problematic historical assumptions, nonstandard terminology, and the effect of experimental conditions on the surface chemistry of ALD. I hope that this review can help the newcomer get acquainted with the exciting and challenging field of surface chemistry of ALD and can serve as a useful guide for the specialist towards the fifth decade of ALD research.
2,212 citations
TL;DR: It is shown that the ambient degradation of BP can be managed effectively when the flakes are sufficiently passivated, and the strategy for enhancing BP environmental stability will accelerate efforts to implement BP in electronic and optoelectronic applications.
Abstract: Unencapsulated, exfoliated black phosphorus (BP) flakes are found to chemically degrade upon exposure to ambient conditions. Atomic force microscopy, electrostatic force microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, and Fourier transform infrared spectroscopy are employed to characterize the structure and chemistry of the degradation process, suggesting that O2 saturated H2O irreversibly reacts with BP to form oxidized phosphorus species. This interpretation is further supported by the observation that BP degradation occurs more rapidly on hydrophobic octadecyltrichlorosilane self-assembled monolayers and on H-Si(111) versus hydrophilic SiO2. For unencapsulated BP field-effect transistors, the ambient degradation causes large increases in threshold voltage after 6 h in ambient, followed by a ∼103 decrease in FET current on/off ratio and mobility after 48 h. Atomic layer deposited AlOx overlayers effectively suppress ambient degradation, allowing encapsulated BP FETs to ma...
1,266 citations
TL;DR: Puurunen et al. as discussed by the authors summarized the two-reactant ALD processes to grow inorganic materials developed to-date, updating the information of an earlier review on ALD.
Abstract: Atomic layer deposition (ALD) is gaining attention as a thin film deposition method, uniquely suitable for depositing uniform and conformal films on complex three-dimensional topographies. The deposition of a film of a given material by ALD relies on the successive, separated, and self-terminating gas–solid reactions of typically two gaseous reactants. Hundreds of ALD chemistries have been found for depositing a variety of materials during the past decades, mostly for inorganic materials but lately also for organic and inorganic–organic hybrid compounds. One factor that often dictates the properties of ALD films in actual applications is the crystallinity of the grown film: Is the material amorphous or, if it is crystalline, which phase(s) is (are) present. In this thematic review, we first describe the basics of ALD, summarize the two-reactant ALD processes to grow inorganic materials developed to-date, updating the information of an earlier review on ALD [R. L. Puurunen, J. Appl. Phys. 97, 121301 (2005)], and give an overview of the status of processing ternary compounds by ALD. We then proceed to analyze the published experimental data for information on the crystallinity and phase of inorganic materials deposited by ALD from different reactants at different temperatures. The data are collected for films in their as-deposited state and tabulated for easy reference. Case studies are presented to illustrate the effect of different process parameters on crystallinity for representative materials: aluminium oxide, zirconium oxide, zinc oxide, titanium nitride, zinc zulfide, and ruthenium. Finally, we discuss the general trends in the development of film crystallinity as function of ALD process parameters. The authors hope that this review will help newcomers to ALD to familiarize themselves with the complex world of crystalline ALD films and, at the same time, serve for the expert as a handbook-type reference source on ALD processes and film crystallinity.
1,160 citations
TL;DR: This work demonstrates the creation of structural metamaterials composed of nanoscale ceramics that are simultaneously ultralight, strong, and energy-absorbing and can recover their original shape after compressions in excess of 50% strain.
Abstract: Ceramics have some of the highest strength- and stiffness-to-weight ratios of any material but are suboptimal for use as structural materials because of their brittleness and sensitivity to flaws. We demonstrate the creation of structural metamaterials composed of nanoscale ceramics that are simultaneously ultralight, strong, and energy-absorbing and can recover their original shape after compressions in excess of 50% strain. Hollow-tube alumina nanolattices were fabricated using two-photon lithography, atomic layer deposition, and oxygen plasma etching. Structures were made with wall thicknesses of 5 to 60 nanometers and densities of 6.3 to 258 kilograms per cubic meter. Compression experiments revealed that optimizing the wall thickness-to-radius ratio of the tubes can suppress brittle fracture in the constituent solid in favor of elastic shell buckling, resulting in ductile-like deformation and recoverability.
1,044 citations
Cites background from "Low-Temperature Al2O3 Atomic Layer ..."
...Using a reported value for the density of ALD alumina, ρs = 2900 kg/m 3 (24), the absolute densities of nanolattices were calculated to be ρ = 6....
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References
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01 Jan 1973TL;DR: CRC handbook of chemistry and physics, CRC Handbook of Chemistry and Physics, CRC handbook as discussed by the authors, CRC Handbook for Chemistry and Physiology, CRC Handbook for Physics,
Abstract: CRC handbook of chemistry and physics , CRC handbook of chemistry and physics , کتابخانه مرکزی دانشگاه علوم پزشکی تهران
52,268 citations
2,576 citations
TL;DR: In this paper, a simple encapsulation technique for organic light emitting devices (OLEDs) is presented, where the degradation of a population of OLEDs is studied and it is shown that the lifetime of encapsulated devices is increased by more than two orders of magnitude over that of unencapsulated devices.
Abstract: We present a simple encapsulation technique for organic light emitting devices (OLEDs). By studying the degradation of a population of OLEDs, we show that the lifetime of encapsulated devices is increased by more than two orders of magnitude over that of unencapsulated devices. In both cases, degradation is primarily due to the formation of nonemissive regions, or dark spot defects. By studying the structure and evolution of the dark spots, we infer that the growth of electrode defects limits device lifetime. Hermetic packaging of OLEDs is essential if they are to be used in commercially viable flat panel displays.
783 citations
TL;DR: Al2O3 films with thicknesses ranging from 30 to 3540 A were grown in a viscous flow reactor using ALD with trimethylaluminum and water as the reactants as mentioned in this paper.
689 citations
TL;DR: This finding adds to the other benefits of the ALD method, especially the atomic-level thickness control and excellent uniformity, and takes a major step toward the scientifically challenging and technologically important task of replacing silica as the gate dielectric in the future generations of metal oxide semiconductor field effect transistors.
Abstract: A chemical approach to atomic layer deposition (ALD) of oxide thin films is reported here. Instead of using water or other compounds for an oxygen source, oxygen is obtained from a metal alkoxide, which serves as both an oxygen and a metal source when it reacts with another metal compound such as a metal chloride or a metal alkyl. These reactions generally enable deposition of oxides of many metals. With this approach, an alumina film has been deposited on silicon without creating an interfacial silicon oxide layer that otherwise forms easily. This finding adds to the other benefits of the ALD method, especially the atomic-level thickness control and excellent uniformity, and takes a major step toward the scientifically challenging and technologically important task of replacing silica as the gate dielectric in the future generations of metal oxide semiconductor field effect transistors.
565 citations