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Ge-Sb-Te-based phase change memory alloys have recently attracted a lot of attention due to their promising applications in the fields of photonics, non-volatile data storage, and neuromorphic computing. Of particular interest is the understanding of the structural changes and underlying mechanisms induced by short optical pulses. This work reports on structural changes induced by single nanosecond UV laser pulses in amorphous and epitaxial Ge2Sb2Te5 (GST) thin films. The phase changes within the thin films are studied by a combined approach using X-ray diffraction and transmission electron microscopy. The results reveal different phase transitions such as crystalline-to-amorphous phase changes, interface assisted crystallization of the cubic GST phase and structural transformations within crystalline phases. In particular, it is found that crystalline interfaces serve as crystallization templates for epitaxial formation of metastable cubic GST phase upon phase transitions. By varying the laser fluence, GST thin films consisting of multiple phases and different amorphous to crystalline volume ratios can be achieved in this approach, offering a possibility of multilevel data storage and realization of memory devices with very low resistance drift. In addition, this work demonstrates amorphization and crystallization of GST thin films by using only one UV laser with one single pulse duration and one wavelength. Overall, the presented results offer new perspectives on switching pathways in Ge-Sb-Te-based materials and show the potential of epitaxial Ge-Sb-Te thin films for applications in advanced phase change memory concepts.
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Central to the use of Ge-Sb-Te based phase-change materials for data storage applications is their crystallization capability since it determines memory writing time. Although being intensively studied to identify intrinsic limits and develop strategies to enhance memory performance, the crystallization process in these materials is still not fully explored. Therefore, this study focuses on the determination of crystal growth dynamics in an epitaxial phase-change material thin film model system offering the advantage of high crystalline quality and application-relevant sizing. By introducing a method that combines time-resolved reflectivity measurements with high-resolution scanning transmission electron microscopy, crystal growth velocities upon fast cooling after single ns-laser pulse irradiation of the prototypical phase-change material Ge2Sb2Te5 are determined. As a result, an increase in crystal growth velocity from 0.4 to 1.7 m/s with increasing laser fluence is observed with a maximum rate of 1.7 m/s as the upper detectable limit of the studied material.
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Two-dimensional van-der-Waals-bonded chalcogenide heterostructures have recently received a lot of attention due to promising applications in the fields of photonics, plasmonics and data storage. Of particular interest is the interfacial switching process inherent in these structures, which is assumed to occur locally at the van-der-Waals interfaces and thus represents an intracrystalline transition. However, detailed experimental studies on the underlying mechanism are still lacking. In this work, epitaxially grown thin films consisting of van-der-Waals-bonded Ge-Sb-Te and GeTe/Sb2Te3 based heterostructures are employed as a model system to investigate structural changes induced by a single ns-laser pulse. A combined approach using X-ray diffraction and advanced transmission electron microscopy is applied to study phase transitions within the Ge-Sb-Te-based thin films in detail. The results reveal ultrafast transitions from 2D-bonded layered structures to 3D-bonded structures via a transient molten phase. Moreover, the interface between the 2D- and 3D-bonded structures is well defined by a single van-der-Waals gap, suggesting that the transition can be controlled very precisely in its spatial extent by an appropriate choice of the laser fluence. Overall, the results of this work offer a new perspective on the switching mechanism in Ge-Sb-Te-based materials and demonstrate the potential of van-der-Waals-bonded Ge-Sb-Te compounds to be applied for novel phase-change memory concepts.
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A concept for detection of charged particles in a single fly-by, e.g. within an ion optical system for deterministic implantation, is presented. It is based on recording the image charge signal of ions moving through a detector, comprising a set of cylindrical electrodes. This work describes theoretical and practical aspects of image charge detection (ICD) and detector design and its application in the context of real time ion detection. It is shown how false positive detections are excluded reliably, although the signal-to-noise ratio is far too low for time-domain analysis. This is achieved by applying a signal threshold detection scheme in the frequency domain, which - complemented by the development of specialised low-noise preamplifier electronics - will be the key to developing single ion image charge detection for deterministic implantation.
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Metals with a wide range of melting points are deposited by electron beam evaporation under oblique deposition geometry on thermally oxidized Si substrates. During deposition the sample holder is cooled down to 77 K. It is observed that all obliquely deposited metals grow as tilted, high aspect ratio columns and hence with a similar morphology. A comparison of such columns with those deposited at room temperature (300 K) reveals that shadowing dominates the growth process for columns deposited at 77 K, while the impact of surface diffusion is significantly increased at elevated substrate temperatures. Furthermore, it is discussed how the incidence angle of the incoming particle flux and the substrate temperature affect the columnar tilt angles and the porosity of the sculptured thin films. Exemplarily for tilted Al columns deposited at 77 K and at 300 K, in-plane pole figure measurements are carried out. A tendency to form a biaxial texture as well as a change in the crystalline structure depending on the substrate temperature is found for those films.
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The assistance of thin film deposition with low-energy ion bombardment influences their final properties significantly. Especially, the application of so-called hyperthermal ions (energy <100 eV) is capable to modify the characteristics of the growing film without generating a large number of irradiation induced defects. The nitrogen ion beam assisted molecular beam epitaxy (ion energy <25 eV) is used to deposit GaN thin films on (0001)-oriented 6H-SiC substrates at 700 °C. The films are studied in situ by reflection high energy electron diffraction, ex situ by X-ray diffraction, scanning tunnelling microscopy, and high-resolution transmission electron microscopy. It is demonstrated that the film growth mode can be controlled by varying the ion to atom ratio, where 2D films are characterized by a smooth topography, a high crystalline quality, low biaxial stress, and low defect density. Typical structural defects in the GaN thin films were identified as basal plane stacking faults, low-angle grain boundaries forming between w-GaN and z-GaN and twin boundaries. The misfit strain between the GaN thin films and substrates is relieved by the generation of edge dislocations in the first and second monolayers of GaN thin films and of misfit interfacial dislocations. It can be demonstrated that the low-energy nitrogen ion assisted molecular beam epitaxy is a technique to produce thin GaN films of high crystalline quality.
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The amorphous to crystalline phase transformation of Ge2Sb2Te5 (GST) films by UV nanosecond (ns) and femtosecond (fs) single laser pulse irradiation at the same wavelength is compared. Detailed structural information about the phase transformation is collected by x-ray diffraction and high resolution transmission electron microscopy (TEM). The threshold fluences to induce crystallization are determined for both pulse lengths. A large difference between ns and fs pulse irradiation was found regarding the grain size distribution and morphology of the crystallized films. For fs single pulse irradiated GST thin films, columnar grains with a diameter of 20 to 60 nm were obtained as evidenced by cross-sectional TEM analysis. The local atomic arrangement was investigated by high-resolution Cs-corrected scanning TEM. Neither tetrahedral nor off-octahedral positions of Ge-atoms could be observed in the largely defect-free grains. A high optical reflectivity contrast (~25%) between amorphous and completely crystallized GST films was achieved by fs laser irradiation induced at fluences between 13 and 16 mJ/cm(2) and by ns laser irradiation induced at fluences between 67 and 130 mJ/cm(2). Finally, the fluence dependent increase of the reflectivity is discussed in terms of each photon involved into the crystallization process for ns and fs pulses, respectively.
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Ion-beam assisted molecular-beam epitaxy was used for direct growth of epitaxial GaN thin films on super-polished 6H-SiC(0001) substrates. The GaN films with different film thicknesses were studied using reflection high energy electron diffraction, X-ray diffraction, cathodoluminescence and primarily aberration-corrected scanning transmission electron microscopy techniques. Special attention was devoted to the microstructural characterization of GaN thin films and the GaN-SiC interface on the atomic scale. The results show a variety of defect types in the GaN thin films and at the GaN-SiC interface. A high crystalline quality of the produced hexagonal GaN thin films was demonstrated. The gained results are discussed.
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One important recent trend in deposition technology is the continuous expansion of available processes towards higher ion assistance with the subsequent beneficial effects to film properties. Nowadays, a multitude of processes, including laser ablation and deposition, vacuum arc deposition, ion assisted deposition, high power impulse magnetron sputtering and plasma immersion ion implantation, are available. However, there are obstacles to overcome in all technologies, including line-of-sight processes, particle contaminations and low growth rates, which lead to ongoing process refinements and development of new methods. Concerning the deposited thin films, control of energetic ion bombardment leads to improved adhesion, reduced substrate temperatures, control of intrinsic stress within the films as well as adjustment of surface texture, phase formation and nanotopography. This review illustrates recent trends for both areas; plasma process and solid state surface processes.
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Highly efficient fabrication of well-ordered, embedded gold nanodot matrices using diffraction mask projection laser ablation is demonstrated. These gold nanodot arrays are ideally generated onto sapphire substrates but do also form onto AlO(x) thin films, enabling the application to arbitrary bulk substrates. Well-ordered gold dots become embedded into the Al(2)O(3) substrate during the process, thus improving their mechanical stability, chemical inertness, and technological compliance. Such substrates may be useful, for example, to enhance solar-cell efficiency by surface plasmons or as convenient, biocompatible focusing elements in nearfield optical tweezers.
Assuntos
Materiais Biocompatíveis/química , Ouro/química , Nanopartículas Metálicas/química , Nanoestruturas/química , Nanotecnologia/métodos , Pinças Ópticas , Óxido de Alumínio/química , Eletroquímica/métodos , Lasers , Teste de Materiais , Microscopia Eletrônica de Transmissão/métodos , Estresse Mecânico , Propriedades de SuperfícieRESUMO
The ion beam deposition (IBD) of rhodamine dye molecules on solid surfaces in high vacuum is explored in order to characterize the possibility of fabricating molecular coatings or nanostructures from nonvolatile molecules. Molecular ion beams with a well-defined composition are deposited on silicon oxide surfaces with a controlled kinetic energy. Photoluminescence spectroscopy and time-of-flight secondary ion mass spectrometry (TOF-SIMS) are employed in order to characterize the sample with respect to coverage, homogeneity, and the fraction of intact landed ions (soft-landing ratio). We find that homogeneous rhodamine films of defined composition can be produced at energies of 2-100 eV. The coverage is found to be proportional to the ion dose. Soft-landing is observed for energies up to 35 eV.
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Vapor-deposited nanocrystalline titanium layers have been irradiated at room temperature with 350-MeV-Au ions up to 4x10;{15} Au/cm;{2}. Bombardment-induced texture changes were determined at the BESSY synchrotron light source. During off-normal irradiation, the nanocrystals undergo grain alignment and rotation up to approximately 90 degrees at the highest ion fluence. At the same time, the whole layer exhibits shear flow very similar to that observed previously in amorphous materials. Below 1x10;{15} Au/cm;{2}, a reversal of the ion incidence angle leads to a back rotation of the grains. These effects are absent or immeasurably small in coarse-grained titanium but have also been found in nanocrystalline TiN and NiO. The observations can be modeled by assuming that grain boundaries behave during ion bombardment like amorphous matter or by assuming a generation of disclination dipoles moving along grain boundaries.
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Prior to transmission electron microscopy (TEM) analyses, insulating specimens need to become coated with a charge-draining layer. Rather than coating the entire TEM foil with a thin film of homogeneous thickness, selective coating is proposed. Using a novel preparation tool, peripheral parts of the sample are coated with a relatively thick (4-8 nm) carbon film while the central, electron-transparent part of the sample is hidden behind a shape-adopted mask and thus not directly exposed to carbon deposition. Beneath the mask, an ultrathin (3-7 A) carbon film is formed that is (i) thick enough to drain charges evolving upon electron irradiation in the electron microscope and (ii) thin enough to avoid typical contamination effects caused by superficial carbon diffusion. Consequently, image quality is becoming enhanced in high-resolution imaging and sensitivity is significantly increased in all nano-beam related techniques including elemental analytics, convergent-beam and nano-beam electron diffraction, and spectral imaging.