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Journal Articles

Biodegradability of disulfide-organosilica nanoparticles evaluated by soft X-ray photoelectron spectroscopy; Cancer therapy implications

Mekaru, Harutaka*; Yoshigoe, Akitaka; Nakamura, Michihiro*; Doura, Tomohiro*; Tamanoi, Fuyuhiko*

ACS Applied Nano Materials (Internet), 2(1), p.479 - 488, 2019/01

Organosilica nanoparticles are attractive for use as drug delivery systems for cancer therapy. Ideally, the nanoparticles need to degrade in the body after drug delivery to minimize their risk. However, the biodegradation of organosilica nanoparticles has not been thoroughly investigated. In this study, we used X-ray photoelectron spectroscopy and field-emission scanning electron microscopy to investigate the degradation of organosilica nanoparticles by glutathione, a peptide found in cells. Our results indirectly indicate that glutathione is able to reduce the disulfide bonds present in the network of one type of the nanoparticles, promoting dissociation of these nanoparticles. The dissociated nanoparticles form large maple leaf-shaped structures under certain conditions. We consider the formation mechanism of these symmetrical structures.

Journal Articles

Application of combination between time-resolved synchrotron radiation photoelectron spectroscopy and supersonic oxygen molecular beams to surface reaction dynamics study

Yoshigoe, Akitaka

X-sen Kodenshi Bunkoho, p.271 - 282, 2018/12

Based on the series of author's studies, the author explains the time-resolved synchrotron radiation X-ray photoelectron spectroscopy and supersonic oxygen molecular beam study on the adsorption reaction dynamics of oxygen molecules at the Si single crystal surface in the section 5.10 of the new textbook "X-ray Photoelectron Spectroscopy" (Kodan-sha) edited by Yuji Takakuwa.

Journal Articles

SiO$$_{2}$$/AlON stacked gate dielectrics for AlGaN/GaN MOS heterojunction field-effect transistors

Watanabe, Kenta*; Terashima, Daiki*; Nozaki, Mikito*; Yamada, Takahiro*; Nakazawa, Satoshi*; Ishida, Masahiro*; Anda, Yoshiharu*; Ueda, Tetsuzo*; Yoshigoe, Akitaka; Hosoi, Takuji*; et al.

Japanese Journal of Applied Physics, 57(6S3), p.06KA03_1 - 06KA03_6, 2018/06

 Times Cited Count:4 Percentile:32.09(Physics, Applied)

The advantage of SiO$$_{2}$$/AlON stacked gate dielectrics over SiO$$_{2}$$, AlON and Al$$_{2}$$O$$_{3}$$ single dielectric layers was demonstrated. Our systematic research revealed that the optimized stacked structure with 3.3-nm-thick AlON interlayer is beneficial in terms of superior interface quality, reduced gate leakage current and C-V hysteresis for next-generation high frequency and high power AlGaN/GaN MOS-HFETs.

Journal Articles

Implementation of atomic layer deposition-based AlON gate dielectrics in AlGaN/GaN MOS structure and its physical and electrical properties

Nozaki, Mikito*; Watanabe, Kenta*; Yamada, Takahiro*; Shih, H.-A.*; Nakazawa, Satoshi*; Anda, Yoshiharu*; Ueda, Tetsuzo*; Yoshigoe, Akitaka; Hosoi, Takuji*; Shimura, Takayoshi*; et al.

Japanese Journal of Applied Physics, 57(6S3), p.06KA02_1 - 06KA02_7, 2018/06

 Times Cited Count:4 Percentile:32.09(Physics, Applied)

We fabricated AlON dielectric films by repeating thin AlN deposition and in situ O$$_{3}$$ oxidation for AlGaN/GaN MOS-HFETs. Uniform nitrogen distribution is achievable by the proposed ALD-based process and that nitrogen concentration can be precisely controlled by changing AlN thickness (ALD cycle number) in each step. It was found that AlON films grown by ALD system offers significant advantages in terms of practical application while keeping superior Vth stability and electrical properties at the insulator/AlGaN interface in AlGaN/GaN MOS-HFETs.

Journal Articles

Control of Ga-oxide interlayer growth and Ga diffusion in SiO$$_{2}$$/GaN stacks for high-quality GaN-based metal-oxide-semiconductor devices with improved gate dielectric reliability

Yamada, Takahiro*; Watanabe, Kenta*; Nozaki, Mikito*; Yamada, Hisashi*; Takahashi, Tokio*; Shimizu, Mitsuaki*; Yoshigoe, Akitaka; Hosoi, Takuji*; Shimura, Takayoshi*; Watanabe, Heiji*

Applied Physics Express, 11(1), p.015701_1 - 015701_4, 2018/01

 Times Cited Count:9 Percentile:12.47(Physics, Applied)

A simple and feasible method for fabricating high-quality and highly reliable GaN-based metal-oxide-semiconductor (MOS) devices was developed on the basis of systematic physical and electrical characterizations. Chemical vapor deposition of SiO$$_{2}$$ films directly onto GaN substrates forming Ga-oxide interlayers was used to fabricate SiO$$_{2}$$/GaO$$_{x}$$/GaN stacked structures. Although well-behaved hysteresis-free GaN-MOS capacitors with extremely low interface state density below 10$$^{10}$$cm$$^{-2}$$eV$$^{-1}$$ were obtained by post-deposition annealing, Ga diffusion into overlying SiO$$_{2}$$ layers severely degraded the insulating property and dielectric breakdown characteristics of the MOS devices. However, this problem was found to be solved by employing rapid thermal processing, leading to superior performance of the GaN-MOS devices in terms of interface quality, insulating property and gate dielectric reliability.

Journal Articles

Design and control of interface reaction between Al-based dielectrics and AlGaN Layer in AlGaN/GaN metal-oxide-semiconductor structures

Watanabe, Kenta*; Nozaki, Mikito*; Yamada, Takahiro*; Nakazawa, Satoshi*; Anda, Yoshiharu*; Ishida, Masahiro*; Ueda, Tetsuzo*; Yoshigoe, Akitaka; Hosoi, Takuji*; Shimura, Takayoshi*; et al.

Applied Physics Letters, 111(4), p.042102_1 - 042102_5, 2017/07

 Times Cited Count:10 Percentile:22.28(Physics, Applied)

AlGaN/GaN HFET (hetero-junction field-effect transitor) has gained much attention as next-generation high frequency and high power devices. In this study, we systematically investigated the interface reaction between Al-based dielectrics (Al$$_{2}$$O$$_{3}$$ and AlON) and AlGaN layer during deposition and post-deposition annealing (PDA), and revealed high thermal stability of AlON/AlGaN interface.

Journal Articles

Comprehensive study on initial thermal oxidation of GaN(0001) surface and subsequent oxide growth in dry oxygen ambient

Yamada, Takahiro*; Ito, Joyo*; Asahara, Ryohei*; Watanabe, Kenta*; Nozaki, Mikito*; Nakazawa, Satoshi*; Anda, Yoshiharu*; Ishida, Masahiro*; Ueda, Tetsuzo*; Yoshigoe, Akitaka; et al.

Journal of Applied Physics, 121(3), p.035303_1 - 035303_9, 2017/01

 Times Cited Count:28 Percentile:5.61(Physics, Applied)

Initial oxidation of GaN(0001) epilayers and subsequent growth of thermal oxides in dry oxygen ambient were investigated by means of X-ray photoelectron spectroscopy, spectroscopic ellipsometry, atomic force microscopy and X-ray diffraction measurements. It was found that, whereas initial oxide formation tends to saturate at temperatures below 800$$^{circ}$$C, selective growth of small oxide grains proceeds at dislocations in the epilayers, followed by noticeable grain growth leading to rough surface morphology at higher oxidation temperatures. This indicates that oxide growth and its morphology are crucially dependent on the defect density in the GaN epilayers. Structural characterizations also revealed that polycrystalline $$alpha$$- and $$beta$$-phase Ga$$_{2}$$O$$_{3}$$ grains in an epitaxial relation with the GaN substrate are formed from the initial stage of the oxide growth. On the basis of these experimental findings, we also developed a comprehensive model for GaN oxidation mediated by nitrogen removal and mass transport.

Journal Articles

Oxidation processes of copper-gold alloy surface induced by supersonic oxygen molecular beam

Okada, Michio*; Tsuda, Yasutaka*; Yoshigoe, Akitaka; Di$~n$o, W. A.*

Do To Dogokin, 56(1), p.232 - 236, 2017/00

We reported the our studies on the surface temperature (Ts) dependence of oxidation on the Cu$$_{3}$$Au(111) surface by a supersonic O$$_{2}$$ molecular beam, using synchrotron radiation X-ray photoemission spectroscopy. Clean surface shows strong Au segregation to the top layer, i.e., Au surface enrichment of the clean surface. Complete Cu segregation to the surface occurs at 0.5 ML O surface coverage. The Au-rich second and third layers of the oxidized surface demonstrate the protective layer formation against oxidation deeper into the bulk. We found that Cu$$_{2}$$O formation occurs. At Ts = 300K, the Cu$$_{2}$$O growth is not so effective. The surface oxidation is less effective on Cu$$_{3}$$Au(111) than on Cu(111). At Ts = 400K, the protection by the Au-rich layer against oxidation into bulk is effective. At Ts = 500K, the Au protective layer is broken due to effective Au diffusion and thus Cu$$_{2}$$O grows deeper into bulk.

Journal Articles

Effect of nitrogen incorporation into Al-based gate insulators in AlON/AlGaN/GaN metal-oxide-semiconductor structures

Asahara, Ryohei*; Nozaki, Mikito*; Yamada, Takahiro*; Ito, Joyo*; Nakazawa, Satoshi*; Ishida, Masahiro*; Ueda, Tetsuzo*; Yoshigoe, Akitaka; Hosoi, Takuji*; Shimura, Takayoshi*; et al.

Applied Physics Express, 9(10), p.101002_1 - 101002_4, 2016/10

 Times Cited Count:21 Percentile:15.16(Physics, Applied)

The superior physical and electrical properties of AlON gate dielectrics on AlGaN/GaN substrates in terms of thermal stability, reliability, and interface quality were demonstrated by direct AlON deposition and subsequent annealing. Nitrogen incorporation into alumina was proven to be beneficial both for suppressing intermixing at the insulator/AlGaN interface and reducing the number of electrical defects in Al$$_{2}$$O$$_{3}$$ films. Consequently, we achieved high-quality AlON/AlGaN/GaN metal-oxide-semiconductor capacitors with improved stability against charge injection and a reduced interface state density as low as 1.2$$times$$10$$^{11}$$ cm$$^{-2}$$eV$$^{-1}$$. The impact of nitrogen incorporation into the insulator was discussed on the basis of experimental findings.

Journal Articles

Synchrotron radiation X-ray photoelectron spectroscopy of Ti/Al ohmic contacts to n-type GaN; Key role of Al capping layers in interface scavenging reactions

Nozaki, Mikito*; Ito, Joyo*; Asahara, Ryohei*; Nakazawa, Satoshi*; Ishida, Masahiro*; Ueda, Tetsuzo*; Yoshigoe, Akitaka; Hosoi, Takuji*; Shimura, Takayoshi*; Watanabe, Heiji*

Applied Physics Express, 9(10), p.105801_1 - 105801_4, 2016/10

 Times Cited Count:4 Percentile:62.06(Physics, Applied)

Interface reactions between Ti-based electrodes and n-type GaN epilayers were investigated by synchrotron radiation X-ray photoelectron spectroscopy. Metallic Ga and thin TiN alloys were formed at the interface by subsequently depositing Al capping layers on ultrathin Ti layers even at room temperature. By comparing results from stacked Ti/Al and single Ti electrodes, the essential role of Al capping layers serving as an oxygen-scavenging element to produce reactive Ti underlayers was demonstrated. Further growth of the metallic interlayer during annealing was observed. A strategy for achieving low-resistance ohmic contacts to n-GaN with low-thermal-budget processing is discussed.

Journal Articles

Enhancement of SiO$$_{2}$$/Si(001) interfacial oxidation induced by thermal strain during rapid thermal oxidation

Ogawa, Shuichi*; Tang, J.*; Yoshigoe, Akitaka; Ishizuka, Shinji*; Takakuwa, Yuji*

Journal of Chemical Physics, 145(11), p.114701_1 - 114701_7, 2016/09

 Times Cited Count:1 Percentile:93.13(Chemistry, Physical)

Enhancement of SiO$$_{2}$$/Si(001) interfacial oxidation induced by thermal strain during rapid thermal oxidation was revealed by real time photoelectron spectroscopy using high intensity and high energy-resolution synchrotron radiation. This experimental result indicates the usefulness of the unified Si oxidation reaction model mediated by point defect generation.

Journal Articles

Experimental and theoretical studies on oxidation of Cu-Au alloy surfaces; Effect of bulk Au concentration

Okada, Michio*; Tsuda, Yasutaka*; Oka, Kohei*; Kojima, Kazuki*; Di$~n$o, W. A.*; Yoshigoe, Akitaka; Kasai, Hideaki*

Scientific Reports (Internet), 6, p.31101_1 - 31101_8, 2016/08

 Times Cited Count:6 Percentile:49.7(Multidisciplinary Sciences)

We report results of our experimental and theoretical studies on the oxidation of Cu-Au alloy surfaces, viz., Cu$$_{3}$$Au(111), CuAu(111), and Au$$_{3}$$Cu(111), using hyperthermal O$$_{2}$$ molecular beam (HOMB). We observed strong Au segregation to the top layer of the corresponding clean (111) surfaces. This forms a protective layer that hinders further oxidation into the bulk. The higher the concentration of Au in the protective layer formed, the higher the protective efficacy. As a result, of the three Cu-Au surfaces studied, Au$$_{3}$$Cu(111) is the most stable against dissociative adsorption of O$$_{2}$$, even with HOMB. We also found that this protective property breaks down for oxidations occurring at temperatures above 300 K.

Journal Articles

Non-destructive depth analysis of the surface oxide layer on Mg$$_{2}$$Si with XPS and XAS

Esaka, Fumitaka; Nojima, Takehiro; Udono, Haruhiko*; Magara, Masaaki; Yamamoto, Hiroyuki

Surface and Interface Analysis, 48(7), p.432 - 435, 2016/07

 Times Cited Count:3 Percentile:84.15(Chemistry, Physical)

XPS is widely used for non-destructive chemical state analysis of solid materials. In this method, depth profiling can be carried out by a combination with ion beam sputtering. However, the sputtering often causes segregation and preferential sputtering of atoms and gives inaccurate information. The use of energy-tunable X-rays from synchrotron radiation (SR) enables us to perform non-destructive depth profiling in XPS. Here, the analytical depth can be changed by changing excitation X-ray energy. In the present study, we examined methods to perform depth profiling with XPS by changing excitation energy and XAS by changing electron energy for detection. These methods were then applied to the analysis of native surface oxide layers on Mg$$_{2}$$Si crystals. In this XAS analysis, the peak at 1843.4 eV becomes dominant when the electron energy for detection increases, which implies that Si-O or Si-O-Mg structure is formed as the surface oxide layer on the Mg$$_{2}$$Si.

Journal Articles

Investigation of segregation during oxidation of Ni-Cu alloy by ${{it in situ}}$ photoelectron spectroscopy

Doi, Takashi*; Nishiyama, Yoshitaka*; Yoshigoe, Akitaka; Teraoka, Yuden

Surface and Interface Analysis, 48(7), p.685 - 688, 2016/07

 Times Cited Count:1 Percentile:95.74(Chemistry, Physical)

Ni-based alloys has been widely used for plant application because of their high strength and excellent oxidation resistance. In particular, the addition of Cu in Ni-based alloys significantly improves the metal dusting resistance. It is indicated that Cu is segregated on the alloy surface in the metal dusting environment; however, the details have not been clarified yet. The behavior of Ni-2Cu alloy under a high temperature oxidation environment was investigated using ${{it in situ}}$ X-ray photoelectron spectroscopy. It was confirmed that Cu have been segregated at the surface of Ni-2Cu alloy during oxidation. These results propose that the Cu segregation improves the metal dusting resistance.

Journal Articles

Surface temperature dependence of oxidation of Cu$$_{3}$$Au(111) by an energetic oxygen molecule

Tsuda, Yasutaka*; Yoshigoe, Akitaka; Teraoka, Yuden; Okada, Michio*

Materials Research Express (Internet), 3(3), p.035014_1 - 035014_8, 2016/03

 Times Cited Count:0 Percentile:100(Materials Science, Multidisciplinary)

We report a study on the surface-temperature ($$T_{s}$$) dependence of oxidation process at Cu$$_{3}$$Au(111) by using a hyperthermal oxygen molecular beam and synchrotron-radiation X-ray photoemission spectroscopy. The O-1s spectra and the corresponding O-uptake curves demonstrate that Cu$$_{2}$$O domains grow effectively at high $$T_{s}$$ of 400 and 500 K. The simple analysis of the O distribution suggests that the temperature-induced atomic diffusion causes the Cu$$_{2}$$O domains growing thicker at 500 K. The oxidation of Cu$$_{3}$$Au(111) is less efficient at $$T_{s}$$ = 300-500 K than that of Cu(111), demonstrating that the protective nature of Cu$$_{3}$$Au against oxidation, in comparison to Cu, remains even at high $$T_{s}$$.

Journal Articles

Spontaneous activation behavior of Ni$$_{3}$$Sn, an intermetallic catalyst, for hydrogen production via methanol decomposition

Fan, M.*; Xu, Y.*; Sakurai, Junya*; Demura, Masahiko*; Hirano, Toshiyuki*; Teraoka, Yuden; Yoshigoe, Akitaka

International Journal of Hydrogen Energy, 40(37), p.12663 - 12673, 2015/10

 Times Cited Count:6 Percentile:73.6(Chemistry, Physical)

The catalytic properties of single-phase Ni$$_{3}$$Sn powder in the production of hydrogen via the decomposition of methanol were investigated in isothermal tests at 713, 793, and 873 K. The catalytic activity of Ni$$_{3}$$Sn significantly increased with time at 793 and 873 K, but not at 713 K, suggesting that Ni$$_{3}$$Sn is spontaneously activated at temperatures above 793 K. At these temperatures, Ni$$_{3}$$Sn showed high selectivity for H$$_{2}$$ and CO production and low selectivity for CH$$_{4}$$, CO$$_{2}$$, and H$$_{2}$$O production, indicating that methanol decomposition was the main reaction, and that side reactions such as methanation and water-gas shift reaction were suppressed. Surface analysis revealed that fine Ni$$_{3}$$Sn particles were formed during the reaction, accompanied by a small amount of deposited carbon. The formation of these particles was suggested to be the cause for the spontaneous activation of Ni$$_{3}$$Sn.

Journal Articles

In situ SR-XPS observation of Ni-assisted low-temperature formation of epitaxial graphene on 3C-SiC/Si

Hasegawa, Mika*; Sugawara, Kenta*; Suto, Ryota*; Sambonsuge, Shota*; Teraoka, Yuden; Yoshigoe, Akitaka; Filimonov, S.*; Fukidome, Hirokazu*; Suemitsu, Maki*

Nanoscale Research Letters, 10, p.421_1 - 421_6, 2015/10

 Times Cited Count:8 Percentile:47.85(Nanoscience & Nanotechnology)

Graphene has attracted much attention as a promising material in electronics and photonics. The graphitization temperature of 1473 K or higher of graphene-on-silicon(GOS), however, is still too high to be fully compatible with the Si technology. Here, the first application of Ni-assisted formation of graphene to the GOS method was reported. We demonstrate that the graphene formation temperature can be reduced by more than 200 K by this method. Moreover, solid-phase reactions during heating/annealing/cooling procedures have been investigated in detail by using ${{it in-situ}}$ synchrotron-radiation X-ray photoelectron spectroscopy. As a result, we clarify the role of Ni/SiC reactions, in which not only Ni silicidation and but also Ni carbonization is suggested as a key process in the formation of graphene.

Journal Articles

Comprehensive study and design of scaled metal/high-$$k$$/Ge gate stacks with ultrathin aluminum oxide interlayers

Asahara, Ryohei*; Hideshima, Iori*; Oka, Hiroshi*; Minoura, Yuya*; Ogawa, Shingo*; Yoshigoe, Akitaka; Teraoka, Yuden; Hosoi, Takuji*; Shimura, Takayoshi*; Watanabe, Heiji*

Applied Physics Letters, 106(23), p.233503_1 - 233503_4, 2015/06

 Times Cited Count:13 Percentile:31.44(Physics, Applied)

Advanced metal/high-$$k$$/Ge gate stacks with a sub-nm equivalent oxide thickness and improved interface properties were demonstrated by controlling interface reactions using ultrathin aluminum oxide (AlOx) interlayers. Comprehensive study by means of physical and electrical characterizations revealed distinct impacts of AlOx interlayers, plasma oxidation.

Journal Articles

In situ synchrotron radiation photoemission study of ultrathin surface oxides of Ge(111)-c(2$$times$$8) induced by supersonic O$$_{2}$$ beams

Okada, Ryuta; Yoshigoe, Akitaka; Teraoka, Yuden; Yamada, Yoichi*; Sasaki, Masahiro*

Applied Physics Express, 8(2), p.025701_1 - 025701_4, 2015/02

 Times Cited Count:3 Percentile:76.7(Physics, Applied)

We studied the surface oxidation on a Ge(111)-c(2$$times$$8) surface at room temperature using supersonic oxygen beams as a function of the translational energy of the incident oxygen molecules ranging from 26 meV to 2.3 eV. In situ synchrotron photoemission spectroscopy performed during the oxidation revealed that the surface oxidation terminated with the formation of a sub-monolayer oxide of at most 0.52 ML, for all the beam energies examined. In addition, the oxidation state of the surface oxides was found to depend on the translational energy. These results demonstrate the precise chemical control of the ultrathin surface oxides of Ge(111)-c(2$$times$$8).

Journal Articles

Probing strongly correlated 4$$f$$-orbital symmetry of the ground state in Yb compounds by linear dichroism in core-level photoemission

Mori, Takeo*; Kitayama, Satoshi*; Kanai, Yuina*; Naimen, Sho*; Fujiwara, Hidenori*; Higashiya, Atsushi*; Tamasaku, Kenji*; Tanaka, Arata*; Terashima, Kensei*; Imada, Shin*; et al.

Journal of the Physical Society of Japan, 83(12), p.123702_1 - 123702_5, 2014/12

 Times Cited Count:12 Percentile:27.87(Physics, Multidisciplinary)

We show that the strongly correlated 4$$f$$-orbital symmetry of the ground state is revealed by linear dichroism in core-level photoemission spectra, as we have discovered for YbRh$$_{2}$$Si$$_{2}$$ and YbCu$$_{2}$$Si$$_{2}$$. Theoretical analysis shows us that the linear dichroism reflects the anisotropic charge distributions resulting from a crystalline electric field. We have successfully determined the ground-state 4$$f$$ symmetry for both compounds from the polarization-dependent angle resolved core-level spectra at a temperature well below the first excitation energy. The excited-state symmetry is also probed by temperature dependence of the linear dichroism where the high measurement temperatures are on the order of the crystal-field-splitting energies.

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