The LaFeO3 and CaFeOX layers are grown using highly dense target prepared by Pechini method, with which accurate growth rate is achieved. Since the LaFeO3demonstrates the obvious RHEED oscillation until the end of growth, constant growth rate, and the step-terraces structure, the LFO is employed as a buffer and/or reference layer to determine the required pulses to deposit the thickness we desire in the superlattice. Superlattices show the clear satellite peaks and Laue oscillation in the XRD spectra as well as the oscillations caused by the film thickness with a flat surface and superstructure with a flat interface in the x-ray reflection spectrum. The streaky RHEED patterns and step-terraces surface are consistent with the results of spectra using x-ray.

Ultrafast time resolved transmission electron diffraction (TED) in a reflection geometry was used to study the cooling behavior of self-organized, well defined nanoscale germanium hut and dome clusters on Si(001). The clusters were heated in a pump-probe scheme by fs-laser pulses. The resulting transient temperature rise was then determined from the drop in diffraction intensity caused by the Debye-Waller effect. From a cooling time of τ =177 ps we estimated a strongly reduced heat transfer compared with homogeneous films of equivalent thickness.

The cooling process of ultrathin hetero films upon excitation with short laser pulses was studied for epitaxial Bi(111) films on Si(001) and Si(111) substrates by means of the Debye-Waller effect with ultrafast electron diffraction. From the exponential decay of the temperature, a cooling time constant was determined as a function of thickness for both substrates. For Bi/Si(111), a linear dependence between the decay constant and thickness was observed, even for 2.8 nm thin films , as predicted from the diffuse mismatch model (DMM) and the acoustic mismatch model (AMM). However, with Bi/Si(001), a significant deviation from this linear dependence was observed for film thicknesses below 5 nm.

The most frequently used characterization technique for biaxial texture formation in thin films is x-ray pole figure analysis. However, x-rays interact weakly with matter and can penetrate a few microns deep into the film. The texture obtained by x-rays is therefore an average texture from the entire thickness of the film. As the texture of a film often changes during growth, information on the basic mechanisms that control the final texture is often lost. In contrast electrons interact strongly with matter and they have very limited penetration and escape depths of a few nm. In this paper we will show how we can use our newly developed reflection high energy electron diffraction (RHEED) surface pole figure technique to probe the surface texture evolution of the growth front from the initial stage (nm thick) to the later stage. The RHEED pole figure technique is a surface-sensitive technique that allows us to obtain information on the dynamic behavior of texture evolution of the growth front during film deposition. We shall explain the principle, measurement, and construction of such RHEED surface pole figures. An example of the biaxial texture evolution of CaF2 due to the atomic shadowing effect during oblique angle deposition is described.

The effect of laser-induced electronic excitations on the self-assembly of Ge quantum dots (QD) on Si(100)-(2x1) grown by pulsed laser deposition is studied. The experiment was conducted in ultrahigh vacuum. A Q-switched Nd:YAG laser (wavelength λ = 1064 nm, 10 Hz repetition rate) was split into two beams; one used to ablate a Ge target while the other to electronically excite the substrate. In situ reflection high-energy electron diffraction (RHEED) and ex situ atomic force microscopy (AFM) were used to study the morphology of the grown QDs. The dependence of the QD morphology on substrate temperature and ablation and excitation laser energy density was studied. Electronic excitation is shown to affect the surface morphology. For Ge coverage of 22 monolayer, it was observed that the excitation laser reduces the epitaxial growth temperature to 250 °C, a temperature at which no epitaxy is possible without excitation. Applying the excitation laser to the substrate during the growth changes the QD morphology and island density and improves the size uniformity of QDs at 390 °C. Surface diffusion measurement calculated from RHEED recovery curves show that the excitation-laser increases the surface diffusion of the Ge atoms. A purely electronic mechanism of enhanced surface diffusion of the Ge adatoms is involved.

The CaFeOX(CFO) and LaFeO3(LFO) thin films as well as superlattices were fabricated on SrTiO3(100) substrates by pulsed laser deposition (PLD) method. The tetragonal LFO film grew with layer-by-layer growth mode until approximately 40 layers. In the case of CFO, initial three layers showed layer-by-layer growth, and afterward the growth mode was transferred to two layers-by-two layers (TLTL) growth mode. The RHEED oscillation was observed until the end of the growth, approximately 50nm. Orthorhombic twin CaFeO2.5 (CFO2.5) structure was obtained. However, it is expected that the initial three CFO layers are CaFeO3 (CFO3) with the valence of Fe4+. The CFO and LFO superlattice showed a step-terraces surface, and the superlattice satellite peaks in a 2θ-θ and reciprocal space mapping (RSM) x-ray diffraction (XRD) measurements, indicating that the clear interfaces were fabricated.

Dysprosium oxide (Dy2O3) films are grown epitaxially on high mobility Ge(100) substrates by molecular beam epitaxy system. Reflection high energy electron diffraction patterns and X-ray diffraction spectra show that single crystalline cubic Dy2O3 films are formed on Ge(100) substrates. The epitaxial-relationship is identified as Dy2O3 (110)║Ge(100) and Dy2O3 [001]║Ge[011]. Atomic force microscopy results show that the surface of the Dy2O3 film is uniform, flat and smooth with root mean square surface roughness of about 4.6Å. X-ray photoelectron spectroscopy including depth profiles confirms the composition of the films being close to Dy2O3. TEM measurements reveal a sharp, crystalline interface between the oxide and Ge.

NiO is a typical material for new p-type oxide semiconductors. Conductivity of NiO can be raised with Li+ doping. In case of Li-heavy doping, we can obtain LixNiO2(0.5< × <1.0). Recently the importance of LiNiO2 has been increased as an electrode material for rechargeable lithium cells.

In this work, we tried to fabricate a novel NiO material with Li+-heavily doped by applying the pulsed laser-induced room temperature (R.T.) film process. Previously, we have succeeded in the epitaxial growth of various oxide thin films at R.T. such as Sn-doped In2O3 transparent electrodes [1]. Although the many studies have been made on the deposition of NiO epitaxial thin film at low temperatures [2], there are few reports on fabrication and the conductive characteristic for Li-heavily doped NiO epitaxial films. The film deposition at R.T., which is the unequilibrium vapor phase process, is expected to result in different crystal structure and characteristics from the films grown at high-temperatures.

A composition-adjusted thin film of LixNi1-xO(0.10< × <0.40) was deposited on a sapphire (α-Al2O3)(0001) or MgO(100) substrates by pulsed laser deposition (PLD) technique in 10−6 Torr of oxygen at R.T. and the high temperatures of 350 and 515°C. Crystalline properties of thin films deposited at R.T. or high temperatures were examined using reflection high energy electron diffraction (RHEED) and X-ray diffraction. For the Li-heavily doped NiO films(x>0.30) grown at R.T., a clear streak RHEED pattern showing epitaxial growth was observed. But the Li-heavily doped NiO films grown at high temperatures, exhibited the ring RHEED pattern, which indicates the policrystal growth of films. Electric conductivity of various Li-doped NiO thin films deposited at R.T. or high temperatures on sapphire (0001) substrates were measured by two-probe method. The interesting results were obtained that conductivity of the film was increased remarkably with an increase of Li-doping for R.T. deposition, but was not changed so much regardless of Li-doping for high-temperature depositions.

With time resolved ultrafast electron diffraction the cooling process across the interface between a thin film and the underlying substrate was studied after excitation with short laser pulses. From the exponential decay of the surface temperature evolution a thermal boundary conductance of 1430 W/(cm2K) is determined for a 9.7 nm thin Bi(111) film on Si(111). A linear dependence between laser fluence and initial temperature rise was measured for film-thicknesses between 2.5 nm and 34.5 nm. The ratio of initial temperature rise and laser fluence for different film-thicknesses is compared to a model taking multilayer optics into account. The data agree well with this model.

We describe the growth of novel ultrathin Mg crystalline nanoblades by oblique angle vapor deposition. These nanoblades were then coated with catalyst Pd and hydrogenated into magnesium hydride MgH2. In situ thermal desorption spectroscopy study showed a low H desorption temperature at ∼365 K. In situ reflection high energy electron diffraction patterns were used to study the temperature dependent structure and composition changes during the de-hydrogenation of Pd coated MgH2 nanoblades. The diffraction rings reveal the formation of alloys of Pd and Mg when the temperature is over ∼480 K. Transmission electron microscopy diffraction also supports the formation of Pd and Mg alloys. This alloying reduces the cycling capability of Mg hydride. The de-hydrogenation of MgH2 introduces a strain at the bilayer interface between MgH2 and Mg resultant from 30% volume reduction from MgH2 to Mg and formed curved nanoblades as evident by scanning electron microscopy images. Designing factors of recyclable simple hydrides will be discussed.

In this report we present a brief overview of the growth of nanostructures by the oblique angle deposition where the nanostructures possess both out-of-plane and in-plane preferred orientations or a biaxial texture. The degree of preferred crystal orientations can be quantitatively determined from a method called “RHEED surface pole figure analysis” that we developed recently.

Understanding interaction of ultrafast pulsed laser with matter is critical for probing ultrafast processes in materials science, understanding the physics of laser ablation and the laser induced non-equilibrium carrier dynamics in metals and semiconductors, including plasmonics. When an intense laser pulse of femtoseconds (fs) in duration hits the surface of a targeted matter, it excites a hot electron gas. Part of the hot electrons is emitted from the surface in a way similar to thermionic emission. Electrons can also be emitted through multiphoton photoemission (MPPE) or thermally assisted MPPE. The emitted electrons travel at speeds that create transient electric fields (TEFs). To detect TEFs and study the dynamics of emitted electrons, we have developed a time resolved electron beam imaging technique that allows us to measure TEFs above a sample surface at picoseconds time resolution. We have also developed a model of the TEFs based on the propagation of emitted electrons and the percentage of electrons escaping from the surface. We examine the significance of TEFs for ultrafast reflection electron diffraction by examining anomalous effects in ultrafast reflection high energy electron diffraction (RHEED) of silicon surfaces.

The dynamics of strongly driven phase transitions at surfaces are studied by ultra-fast time-resolved reflection high energy electron diffraction. The surfaces are excited by an intense fs-laser pulse (pump) and probed by an ultra-short electron pulse with variable time delay. The order-disorder phase transition from a c(4×2) to a (2×1) of the bare Si(001) surface shows a transient decrease of the intensity of the c(4×2) spots which recovers on a time scale of a few hundred picoseconds indicating the excitation of the phase transition. On Si(111) a monolayer of Indium induces a (4×1) reconstruction which undergoes a Peierls like phase transition to a (8ד2”) reconstruction below 100 K. Upon laser excitation at a temperature of 40 K the phase transition was strongly driven. The (8ד2”)-diffraction spots instantaneously disappears, while the intensity of the (4×1)-spots increases. This increase of the (4×1) spot intensity excludes an explanation by the Debye-Waller-Effect and is evidence for a true structural phase transition at a surface.

The use of an ion beam assist during the concurrent deposition of cubic materials can result in the growth of crystallographically oriented thin films. A model system, magnesium oxide (MgO), has been successfully used as a biaxially textured template film and develops texture in a different manner from that of other well-studied materials, like yttria-stablized zirconia. Here, we present data on the initial nucleation of biaxial texture in this model system using a novel in-situ quartz crystal microbalance (QCM) substrate combined with in-situ reflected high-energy electron diffraction (RHEED). Temporal correlation of mass uptake with the RHEED images of the growing surface can be used to elucidate the mechanism of texture development in these films. Experimental data shows that the initially polycrystalline MgO film develops biaxial crystallographic texture at a thickness of ˜2 nm, regardless of the ion-to-molecule ratio. RHEED images show the onset of texture occurs quickly and is somewhat analogous to a solid phase re-crystallization process with crystallite sizes of ˜3 to 4 nm. Imaging with transmission electron microscopy has corroborated these observations. Changes in the ion-to-molecule ratio can influence the crystallite size and affect the nucleation density of these films. Growth of these films on various substrates changes the sticking coefficient of the MgO and influences the nucleation density and film growth mode as well. This opens the possibility of using MgO and other materials to develop biaxially textured crystallites with a narrow, specified size distribution for nanoscale applications.

The Cr2O3 thin films were grown on Al2O3(1102)(r-cut sapphire), Al2O3(1120)(a-cut sapphire), and Al2O3(0001)(c-cut sapphire) substrates to apply magnetoelectric oxides to oxides electronics. The Cr2O3 is a representative magnetoelectric material with antiferromagnetic insulator with the Néel temperature of 308 K. From the results of X-ray diffraction and the reflection high energy electron diffraction, epitaxial Cr2O3 thin films were obtained on all cut sapphire substrates using off-axis DC-RF magnetron sputtering method. The epitaxial relationship was Cr2O3[1120]//Al2O3[1120] and Cr2O3(1102)//Al2O3(1102) on r-cut, and Cr2O3[1100]//Al2O3[1100] and Cr2O3(1120)//Al2O3(1120) on a-cut, and Cr2O3[1120]//Al2O3[1120] and Cr2O3(0001)//Al2O3(0001) on c-cut. Optimized Cr2O3 film was obtained grown at 600°C on c-cut sapphire substrate. The surface roughness (Ra) of the film was 0.28 nm, and full width at half maximum of rocking curve for Cr2O3(0006) Bragg reflection was 0.23°. Growth difference is expected to be caused by the stacking order of atoms normal to the substrate surface and arrangement of atoms of the substrate surface.

We have proposed a novel self-assembling growth method, termed Droplet Epitaxy, for the direct formation of QDs without using any lithography in 1990. Compared with the island formation based on the Stranski-Krastanow growth mode, the Droplet Epitaxy is applicable to the formation of quantum dots not only in lattice-mismatched but also in lattice-matched systems such as GaAs/AlGaAs. The process of the Droplet Epitaxy in MBE chamber consists of forming numerous III-column element droplets such as Ga or InGa with homogeneous size of around 10 nm on the substrate surface first by supplying their molecular beams, and then reacting the droplets with As molecular beam to produce GaAs or InGaAs epitaxial microcrystals.Another advantage of the Droplet Epitaxy is the possibility of the fabrication of QDs structures without wetting layer by cotrolling the stoichiometry of the substrate surface just before the deposition of III-column element droplets. Also we can control the shape of the QDs structure self-organizingly such as pyramidal shape, single-ring shape and concentric double-ring shape. These ring structures will provide excellent possibilities for the investigation of quantum topological phenomena.

We prepared quasi single crystalline pentacene monolayer films on Bi-terminated Si(111) by using bunched steps on vicinally-cut surfaces as an orientation template. Band dispersion in the conduction plane of pentacene was clearly observed by angle-resolved photoelectron spectroscopy.

Self-assembled (SA) quantum dots (QDs) have been widely studied due to the facileness in their preparation. Unlike other types of QDs that require complicated fabrication processes, SA QDs are prepared merely by depositing materials that have different bandgaps and lattice constants to the with respect to the substrate by epitaxial crystal growth techniques. InAs QDs on GaAs(001) grown by MBE or MOCVD have been a typical example, and their optoelectronic properties have been extensively investigated. For device applications, it is essential that their size and spatial distribution are controlled. However, since SA QDs are formed through random processes, it is not easy to achieve size and distribution uniformity without prior processing the substrate prior to crystal growth. A number of studies have been performed to understand the fundamental mechanisms of SA QD formation that would provide us with information to achieve such goal.Here, we performed real-time observation of SA InAs QD growth on GaAs(001) by MBE. In contrast to most previous reports that employed growth interruption, by following the time transient of RHEED specular beam in detail, we obtained information about nucleation and evolution of the QDs, and have been able to distinguish processes that are dependent and independent of growth rate. In addition, the results reveal that surface migration of In/As atoms and their incorporation into QDs, with the aid of the wetting layer, can be observed. We will also provide a quantitative discussion on these processes.

The strain distributions and of reflection high energy electron diffraction (RHEED) patterns of uncapped pyramidal shape InAs Stranski-Krastanov quantum dots fabricated on GaAs(001) substrate are investigated theoretically. The three dimensional strain anisotropy is computed with an atomistic elasticity approach, using inter-atomic Keating potentials and the strain energy is minimized using the conjugate gradient numerical method. RHEED images are predicted in the framework of the kinematical theory, by taking into account the refraction of the electron beam at the quantum dot/vacuum interface. Clear correlation between RHEED image features and quantum dot structural properties is established. The study stresses the potential of RHEED for future experimental real-time (during growth) detections and deciphering of strain anisotropies in quantum dots.

Epitaxial ZnO films are successfully grown on Al2O3 substrates with phase controlled CrN buffer layer using Zn and O-plasma pre-exposures on CrN layers by plasma assisted molecular beam epitaxy (P-MBE). The Zn exposures on CrN layers prior to ZnO film growth result in the formation of rocksalt CrN without surface oxidation. On the other hand, the surface of the initially deposited CrN layers with rocksalt structure changes into hexagonal structured Cr2O3 after O-plasma exposure as confirmed by reflection high-energy electron diffraction (RHEED) and high resolution transmission electron microscopy (HR TEM). Etching studies show that the ZnO films grown on CrN have +C polarity, while the polarity of ZnO on Cr2O3/CrN double buffer is -C polarity. The interdiffusion of Zn and Cr occurs at the ZnO/CrN interface, while the interdiffusion is negligible at the ZnO/ Cr2O3 interface. The interdiffusion of Cr and Zn can be suppressed by inserting a low-temperature ZnO buffer layer in between ZnO and CrN layers, which helps improve the crystal quality of ZnO layers grown with CrN buffer.