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The beamline for angle-resolved photoemission spectroscopy (ARPES) with a nano-focused beam (nano-ARPES) is planned as one of the public beamlines in NanoTerasu, the 3-GeV next-generation synchrotron radiation facility at Tohoku, Japan, which is scheduled to start operation in 2024. A 4 m long APPLE-II type undulator provides brilliant soft X-rays with various polarizations (linear horizontal and vertical, and left and right circular) in the energy range of 50-1,000 eV. A collimated plane grating monochromator is adopted as a soft X-ray monochromator because we can select the demagnification factor of grating cf f = cosα/cosβ between the high energy-resolution (HR) mode for HR-ARPES experiments and the low divergence mode for high-flux nano-ARPES measurements. This beamline aims to produce the high flux nano-focused beam by using ultrahigh precision reflective mirror optics, not a Fresnel zone plate used as a focusing optics in the previous nano-ARPES station at other synchrotron facilities.

A synchrotron radiation beamline in the soft- and tender-X ray energy range of 180-3000 eV with versatile polarization control has been designed for NanoTerasu, the 3-GeV next-generation synchrotron radiation facility at Tohoku, Japan. A series of four APPLE-II type undulators is adopted as a photon source to realize the required beam properties with high-speed polarization switching. The beamline optics is designed for a highly efficient and precise use of x-ray magnetic circular/linear dichroism (XMCD/XMLD) technique balancing high photon flux and energy resolution. The simulated performance of the segmented undulator together with the monochromator optics achieved the sufficiently high flux and energy resolution (E/ΔE) in whole target energy range. Two endstations with the different re-focus optics, one for marginal spot size with high flux and the other for ultimate focus down to ∼10 nm are also designed. The simulated performance of the beamline encourages the future researches of high-throughput and nm-focused spintronic measurements.

The optical design of the ultrahigh-resolution RIXS beamline, which is currently developed at NanoTerasu in Japan, is described. The main goal of this beamline is to perform ultrahigh-resolution RIXS measurements with a total energy resolution of E/ΔE>150,000 for both beamline and RIXS spectrometer. To achieve the ultra-high resolution, a 2D-RIXS spectrometer using energy-dispersive X-ray is employed to compensate for lower throughput at higher energy resolution, and the optics of the beamline is optimized for the 2D-RIXS spectrometer. A vertically dispersing in-focus variable-included-angle varied-line-spacing plane grating monochromator is employed for the beamline, with an entrance slit to ensure the ultrahigh resolution. First and second mirrors focus X-ray on entrance slits vertically and horizontally, respectively, and the divergent X-ray is irradiated onto the grating. For the 2D-RIXS spectrometer, there is no exit slit, and the vertically energy-dispersed X-ray is irradiated directly onto a sample. In front of the sample, X-ray is horizontally refocused by a Wolter type-I mirror. The expected horizontal focus size at the sample is ~0.7 μm. The expected photon flux is ~1×1011 photons/s at 500–1000 eV with a virtual slit width of 2 μm required for E/ΔE>150,000. The height of the dispersed X-ray available in the 2D-RIXS spectrometer is ~120 μm, which allows the use of a remarkably high flux of ~6×1012 photons/s, and the beamline will serve as an ultrahigh-resolution and high-efficiency RIXS facility.

In-situ X-ray diffraction was used to investigate initial stages of GaN growth on graphene-covered SiO2 substrates with or without AlN buffer layers by plasma-assisted molecular beam epitaxy. The in-plane lattice parameter of GaN remained almost constant during growth without AlN buffer layers, confirming weak interactions between GaN and graphene. On the substrate with AlN buffer layers, the GaN lattice parameter continuously changed from AlN value to GaN value, indicating that the AlN islands act as seeds for GaN growth. Besides, GaN has preferential orientations epitaxial to graphene. Graphene can be used as a template of GaN growth on amorphous substrates.

We carry out real-time in situ synchrotron X-ray diffraction on the growth of GaN and AlN on SiC(0001) substrate by molecular beam epitaxy. At the initial growth stage of GaN/SiC or AlN/SiC heterostructure, the epitaxial overlayer develops affected by defects with the strain interaction between SiC, eventually showing characteristic lattice deformations. GaN was almost relaxed at the initial stage, showing the transition of the growth mode from 3D to 2D at around 4 nm. In contrast, AlN coherently grow on SiC(0001) at the initial stage for 13 nm concomitantly showing lattice deformation with the beneath SiC, subsequently showing gradual lattice relaxation.

The structure of epitaxially grown Pr2O3 on Si(0?0?1) has been investigated by grazing incidence x-ray diffraction and x-ray reflectivity. We report experimental results from measurements made in situ, after growth, and during annealing to determine the stability of Pr2O3 at temperatures relevant for complementary metal oxide semiconductor (CMOS) processing. Pr6O11 is evaporated and converted to Pr2O3 using an effusion source operating at 1970 ?C. Two different phases of Pr2O3 have been identified in the as-grown films in addition to a silicate layer that forms upon nucleation at the Si interface. The cubic Pr2O3 nucleates as a single crystal and grows in greater proportion to the polycrystalline hexagonal Pr2O3. The crystal structure of the as-grown film is stable during annealing up to about 800 ?C at which point the Pr2O3 is consumed at the expense of the silicate phase.

An X-ray diffractometer connected with a molecular-beam epitaxy (MBE) system has been constructed for in situ studies on the growing surfaces of III–V compound semiconductors. This diffractometer is based on the (4+2) type, which has four axes for orienting the sample and two axes for positioning the detector. In addition, it is equipped with an axis for rotating the receiving slit about the normal of the slit plane to align the resolution of the receiving slit properly for the surface X-ray diffraction measurement. For the alignment of the sample and the entire setup with respect to the X-ray beam, an XYZ-stage and an adjustable base plate are available. X-rays enter and leave the chamber through two Be windows welded directly to the MBE chamber. A graphite sheet which can be heated up to 250°C is placed along the inside of the Be windows to protect the Be windows from being coated with evaporated materials. Preliminary data are presented to demonstrate the feasibility of static and dynamic measurements of growing surfaces using this instrument.

The effect of substrate orientation on strain relaxation mechanisms of an InGaAs layer grown on vicinal GaAs substrates was investigated by in situ X-ray diffraction (XRD). The crystallographic tilt and indium segregation in the InGaAs layer were altered depending on the miscut direction and angle. In the case of the substrate tilted 6° toward the [110] direction, one type of misfit dislocations was formed preferentially rather than other types, especially in the rapid relaxation phase. While in the case of the substrate tilted 6° toward the direction, no anisotropies during relaxation were observed. The present finding indicates that the appropriate use of vicinal substrates may lead to a novel method of improving the crystal quality of heterolayers.

A molecular beam epitaxy (MBE) chamber dedicated to nitride growth was developed at the synchrotron radiation facility SPring-8. This chamber has two beryllium windows for incident and outgoing X-rays, and is directly connected to an X-ray diffractometer, enabling in situ synchrotron X-ray measurements during the nitride growth. Experimental results on initial growth dynamics in GaN/SiC, AlN/SiC, and InN/GaN heteroepitaxy were presented. We achieved high-speed and high-sensitivity reciprocal space mapping with a thickness resolution of atomic-layer scale. This in situ measurement using the high-brilliance synchrotron light source will be useful for evaluating structural variations in the initial growth stage of nitride semiconductors.

The polytypism of GaAs nanowires was investigated by in situ X-ray diffraction under different growth conditions. The growth of nanowires was found to start with the formation of the zincblende structure, followed by the growth of the wurtzite structure. The observed growth process of nanowires was well reproduced by simulations based on a layer-by-layer nucleation model. At a low growth temperature and a high growth rate, stacking faults were found to be frequently introduced owing to the reduction in energy barrier. As a result, the zincblend and wurtzite segments in nanowires were highly fragmented and the wurtzite structure was formed in the early stage of growth.

A ternary Fresnel zone plate (FZP) has been fabricated and installed at the beamline 11XU of SPring-8, in the aim of in situ studies on the growth of semiconductor nanostructures. The FZP is designed for an X-ray energy of 9.5 keV for the first-order diffraction, which is isolated by an order sorting aperture (OSA) inserted 450 mm after the FZP. The focal length of this FZP is 650 mm. The full width at half maximum of the focused beam profile was estimated to be 1.17 μm (H) × 1.38 μm (V) by the dark-field knife-edge scan. Using this FZP, micro-beam diffraction of an as-grown single InAs NW was carried out to show the feasibility of in situ study during growth.

Self-assembled InAs/GaAs(001) quantum dot structures before and after quenching were investigated by in situ X-ray diffraction to assess the effects of quenching. Before quenching, quantums dots were uniform in size so that the shape and internal lattice constant distribution of a quantum dot were quantitatively determined on the basis of three-dimensional X-ray intensity mapping. X-ray measurements after quenching revealed that the quantum dot size showed a bimodal distribution as a result of the proliferation of dislocated islands during quenching. A formula to describe the X-ray diffraction from dislocated islands with a large size distribution is presented. The cooling rate between 20 and 40 K/min was found to have little effect on the structures of quenched quantum dots.

Self-assembly of high-density InAs quantum dots (QDs) on Sb-irradiated GaAs buffer layers was observed in-situ by a time-resolved X-ray diffraction (XRD) technique using a combination of XRD and molecular beam epitaxy. Evolution of dot height and lattice constant was analyzed during InAs QD growth and subsequent growth interruption (GI), and as a result, dislocated giant dots due to coalescence and coherent dots were separately evaluated. An Sb-irradiated GI (Sb-GI) method to be applied after InAs growth was attempted for the suppression of coalescence. Using this method, the XRD intensity of giant dots decreased, and the photoluminescence intensity of InAs QDs was enhanced. High-density InAs QDs without giant dots were produced by using the combination of the QD growth on the Sb-irradiated GaAs buffer layers and the Sb-GI.

In situ real-time X-ray diffraction measurements during In0.12Ga0.88As/GaAs(001) epitaxial growth are performed for the first time to understand the strain relaxation mechanisms in a lattice-mismatched system. The high resolution reciprocal space maps of 004 diffraction obtained at interval of 6.2 nm thickness enable transient behavior of residual strain and crystal quality to be observed simultaneously as a function of InGaAs film thickness. From the evolution of these data, five thickness ranges with different relaxation processes and these transition points are determined quantitatively, and the dominant dislocation behavior in each phase is deduced.

The molecular beam epitaxial (MBE) growth and postgrowth annealing of InAs/GaAs(001) quantum dots were investigated by grazing-incidence X-ray diffraction using a diffractometer integrated with an MBE apparatus. The use of synchrotron radiation and a two-dimensional X-ray detector enabled X-ray diffraction measurements on the internal strains and height of dots at a rate of less than 10 s per frame. Mass transport by surface diffusion was found to play a major role in the nucleation of three-dimensional islands of InAs/GaAs(001).

The structure of a δ-doped crystal, Si(800Å)/Ge(1ML)/Si(001), grown by molecular beam epitaxy has been studied by surface X-ray diffraction and X-ray standing-wave method. The positions of the Ge layer and the Si capping layer are determined with respect to the Si substrate. In the analysis, the roughnesses of the interface and the surface are considered. The distance between the bottommost capping layer and the topmost substrate layer is 2.068±0.002 in units of the interlayer spacing of Si(004), while the distance between the Ge layer and the topmost Si substrate layer is 1.058±0.001. The former value corresponds to an averaged structure where the macroscopic elastic theory is applicable to the evaluation of the strain and the latter value corresponds to a microscopic structure where the bulk bond length is conserved. Coexistence of the two kinds of structures is made possible by the interfacial roughness.