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Journal Articles

Band gap formation in graphene by hybridization with Hex-Au(001) reconstructed surface

Terasawa, Tomoo; Matsunaga, Kazuya*; Hayashi, Naoki*; Ito, Takahiro*; Tanaka, Shinichiro*; Yasuda, Satoshi; Asaoka, Hidehito

Vacuum and Surface Science, 66(9), p.525 - 530, 2023/09

As Au (001) surfaces exhibit a quasi-one-dimensional corrugated structure, Hex-Au(001), its periodicity was predicted to change the electronic structure of graphene when graphene was grown on this surface. Furthermore, the hybridization between graphene and Au is known to introduce bandgap and spin polarization into graphene. Here, we report angle-resolved photoemission spectroscopy and density functional theory calculation of graphene on a Hex-Au(001) surface. A bandgap of 0.2 eV in the graphene Dirac cone was observed at the crossing point of the graphene Dirac cone and Au 6sp bands, indicating that the origin of the bandgap formation was the hybridization between the graphene Dirac cone and Au 6sp band. We discussed the hybridization mechanism and anticipated spin injection into the graphene Dirac cone.

Journal Articles

Step unbunching phenomenon on 4H-SiC (0001) surface during hydrogen etching

Sakakibara, Ryotaro*; Bao, J.*; Yuhara, Keisuke*; Matsuda, Keita*; Terasawa, Tomoo; Kusunoki, Michiko*; Norimatsu, Wataru*

Applied Physics Letters, 123(3), p.031603_1 - 031603_4, 2023/07

 Times Cited Count:0 Percentile:59.51

We here report a step unbunching phenomenon, which is the inverse of the phenomenon of step bunching. When a 4H-SiC (0001) surface is annealed at a high temperature, step bunching arises due to the different velocities of the step motion in adjacent steps, resulting in steps with a height of more than several nanometers. We found that the bunched steps, thus, obtained by hydrogen etching in an Ar/H$$_{2}$$ atmosphere were "unbunched" into lower height steps when annealed subsequently at lower temperatures. This unbunching phenomenon can be well explained by the consequence of the competition between energetics and kinetics. Our findings provide another approach for the surface smoothing of SiC by hydrogen etching and may give significant insight into the application of SiC power devices and two-dimensional materials growth techniques in general.

Journal Articles

Band gap opening in graphene by hybridization with Au (001) reconstructed surfaces

Terasawa, Tomoo; Matsunaga, Kazuya*; Hayashi, Naoki*; Ito, Takahiro*; Tanaka, Shinichiro*; Yasuda, Satoshi; Asaoka, Hidehito

Physical Review Materials (Internet), 7(1), p.014002_1 - 014002_10, 2023/01

 Times Cited Count:0 Percentile:75.82(Materials Science, Multidisciplinary)

Au(001) surfaces exhibit a complex reconstructed structure [Hex-Au(001)] comprising a hexagonal surface and square bulk lattices, yielding a quasi-one-dimensional corrugated surface. When graphene was grown on this surface, the periodicity of the corrugated surface was predicted to change the electronic structure of graphene, forming bandgaps and new Dirac points. Furthermore, the graphene-Au interface is promising for bandgap generation and spin injection due to band hybridization. Here, we report the angle-resolved photoemission spectroscopy and density functional calculation of graphene on a Hex-Au(001) surface. The crossing point of the original and replica graphene $$pi$$ bands showed no bandgap, suggesting that the one-dimensional potential was too small to modify the electronic structure. A bandgap of 0.2 eV was observed at the crossing point of the graphene $$pi$$ and Au $$6sp$$ bands, indicating that the bandgap is generated using hybridization of the graphene $$pi$$ and Au $$6sp$$ bands. We discussed the hybridization mechanism and concluded that the R30 configuration between graphene and Au and an isolated electronic structure of Au are essential for effective hybridization between graphene and Au. We anticipate that hybridization between graphene $$pi$$ and Au $$6sp$$ would result in spin injection into graphene.

Journal Articles

Efficient hydrogen isotope separation by tunneling effect using graphene-based heterogeneous electrocatalysts in electrochemical hydrogen isotope pumping

Yasuda, Satoshi; Matsushima, Hisayoshi*; Harada, Kenji*; Tanii, Risako*; Terasawa, Tomoo; Yano, Masahiro; Asaoka, Hidehito; Gueriba, J. S.*; Di$~n$o, W. A.*; Fukutani, Katsuyuki

ACS Nano, 16(9), p.14362 - 14369, 2022/09

 Times Cited Count:4 Percentile:83.44(Chemistry, Multidisciplinary)

The fabrication of hydrogen isotope enrichment system is essential for the development of industrial, medical, life science, and nuclear fusion fields, therefore alternative enrichment techniques with high separation factor and economic feasibility have been still explored. Herein, we report the fabrication of heterogeneous electrode with layered structures consisting of palladium and graphene layers for polymer electrolyte membrane electrochemical hydrogen pumping for the hydrogen isotope enrichment. We demonstrated significant bias voltage dependence of hydrogen/deuterium (H/D) separation ability and its high H/D at lower bias voltage. Theoretical analysis also demonstrated that the observed high H/D at low bias voltage stems from hydrogen isotopes tunneling through atomically-thick graphene during the electrochemical reaction, and the bias dependent H/D results in a transition from the quantum tunneling regime to classical over- barrier regime for hydrogen isotopes transfer via the graphene. These findings provide new insight for a novel economical methodology of efficient hydrogen isotope enrichment.

Journal Articles

Development of ultraslow, monochromatic, and mass-selected ion source toward measurement of hydrogen ion permeability of graphene

Terasawa, Tomoo; Fukutani, Katsuyuki; Yasuda, Satoshi; Asaoka, Hidehito

e-Journal of Surface Science and Nanotechnology (Internet), 20(4), p.196 - 201, 2022/07

Graphene is a perfect impermeable membrane for gases but permeable to hydrogen ions. Hydrogen ion permeation shows the isotope effect, i.e., deuteron is slower than proton when permeating graphene. However, the permeation mechanism and the origin of the isotope effect are still unclear. Here, we propose a strategy to discuss the hydrogen ion permeation mechanism of graphene by developing an ion source with ultraslow, monochromatic, and mass-selected hydrogen ion beam. We employed a hemispherical monochromator and a Wien filter for the ion source to achieve the energy and mass resolutions of 0.39 eV and 1 atomic mass unit, respectively. The energetically sharp ion beam is expected to allow us to directly measure the permeability of graphene with high accuracy.

Journal Articles

Structure of quasi-free-standing graphene on the SiC (0001) surface prepared by the rapid cooling method

Sumi, Tatsuya*; Nagai, Kazuki*; Bao, J.*; Terasawa, Tomoo; Norimatsu, Wataru*; Kusunoki, Michiko*; Wakabayashi, Yusuke*

Applied Physics Letters, 117(14), p.143102_1 - 143102_5, 2020/10

A systematic structural study of epitaxial graphene samples on the SiC (0001) surface has been performed by the surface X-ray diffraction method, which is a non-contact technique. For samples with only a buffer layer, one layer graphene, and multilayer graphene, the distances between the buffer layer and the surface Si atoms were found to be 0.23 nm. This value is the same as reported values. For quasi-free-standing graphene samples prepared by the rapid cooling method, there was no buffer layer and the distance between the quasi-free-standing graphene and the surface Si atoms was 0.35 nm, which is significantly shorter than the value in hydrogen-intercalated graphene and slightly longer than the interplane distance in graphite. The Si occupancy deviated from unity within 1 nm of the SiC surface. The depth profile of the Si occupancy showed little sample dependence, and it was reproduced by a simple atomistic model based on random hopping of Si atoms.

Journal Articles

Controlled growth of boron-doped epitaxial graphene by thermal decomposition of a B$$_{4}$$C thin film

Norimatsu, Wataru*; Matsuda, Keita*; Terasawa, Tomoo; Takata, Nao*; Masumori, Atsushi*; Ito, Keita*; Oda, Koji*; Ito, Takahiro*; Endo, Akira*; Funahashi, Ryoji*; et al.

Nanotechnology, 31(14), p.145711_1 - 145711_7, 2020/04

 Times Cited Count:6 Percentile:39.72(Nanoscience & Nanotechnology)

We show that boron-doped epitaxial graphene can be successfully grown by thermal decomposition of a boron carbide thin film, which can also be epitaxially grown on a silicon carbide substrate. The interfaces of B$$_{4}$$C on SiC and graphene on B$$_{4}$$C had a fixed orientation relation, having a local stable structure with no dangling bonds. The first carbon layer on B$$_{4}$$C acts as a buffer layer, and the overlaying carbon layers are graphene. Graphene on B$$_{4}$$C was highly boron doped, and the hole concentration could be controlled over a wide range of 2$$times$$10$$^{13}$$ to 2$$times$$10$$^{15}$$ cm$$^{-2}$$. Highly boron-doped graphene exhibited a spin-glass behavior, which suggests the presence of local antiferromagnetic ordering in the spin-frustration system. Thermal decomposition of carbides holds the promise of being a technique to obtain a new class of wafer-scale functional epitaxial graphene for various applications.

Journal Articles

Confinement of hydrogen molecules at graphene-metal interface by electrochemical hydrogen evolution reaction

Yasuda, Satoshi; Tamura, Kazuhisa; Terasawa, Tomoo; Yano, Masahiro; Nakajima, Hideaki*; Morimoto, Takahiro*; Okazaki, Toshiya*; Agari, Ryushi*; Takahashi, Yasufumi*; Kato, Masaru*; et al.

Journal of Physical Chemistry C, 124(9), p.5300 - 5307, 2020/03

 Times Cited Count:11 Percentile:58.4(Chemistry, Physical)

Confinement of hydrogen molecules at graphene-substrate interface has presented significant importance from the viewpoints of development of fundamental understanding of two-dimensional material interface and energy storage system. In this study, we investigate H$$_{2}$$ confinement at a graphene-Au interface by combining selective proton permeability of graphene and the electrochemical hydrogen evolution reaction (electrochemical HER) method. After HER on a graphene/Au electrode in protonic acidic solution, scanning tunneling microscopy finds that H$$_{2}$$ nanobubble structures can be produced between graphene and the Au surface. Strain analysis by Raman spectroscopy also shows that atomic size roughness on the graphene/Au surface originating from the HER-induced strain relaxation of graphene plays significant role in formation of the nucleation site and H$$_{2}$$ storage capacity.

Journal Articles

${it In situ}$ optical microscopy of crystal growth of graphene using thermal radiation

Terasawa, Tomoo; Taira, Takanobu*; Obata, Seiji*; Saiki, Koichiro*; Yasuda, Satoshi; Asaoka, Hidehito

Vacuum and Surface Science, 62(10), p.629 - 634, 2019/10

Graphene, an atomically thin sheet composed of sp$$^{2}$$ carbon atoms, has been the most attractive material in this decade. The fascinating properties of graphene are exhibited when it is monolayer. Chemical vapor deposition (CVD) is widely used to produce monolayer graphene selectively in large-area. Here we introduce "radiation-mode optical microscopy" which we have developed in order to realize the ${it in situ}$ observation of the CVD growth of graphene. We show the method to observe graphene as bright contrast on Cu substrates in thermal radiation images. The growth mechanism, the nucleation site and rate limiting process, revealed by the ${it in situ}$ observation is presented. Finally, we show the CVD growth of graphene on Au substrates, resulting in the tuning of the emissivity of graphene by the pre-treatment procedures. Our method is not only a way to observe the graphene growth but also shed light on the thermal radiation property of graphene.

Journal Articles

Effect of hydrogen on chemical vapor deposition growth of graphene on Au substrates

Terasawa, Tomoo; Taira, Takanobu*; Yasuda, Satoshi; Obata, Seiji*; Saiki, Koichiro*; Asaoka, Hidehito

Japanese Journal of Applied Physics, 58(SI), p.SIIB17_1 - SIIB17_6, 2019/08

 Times Cited Count:4 Percentile:22.27(Physics, Applied)

Chemical vapor deposition (CVD) on substrates with low C solubility such as Cu and Au is promising to grow monolayer graphene selectively in a large scale. Hydrogen is often added to control the domain size of graphene on Cu, while Au does not require H$$_{2}$$ since Ar is inert against oxidation. The effect of H$$_{2}$$ should be revealed to improve the quality of graphene on Au. Here we report the effect of H$$_{2}$$ on the CVD growth of graphene on Au substrates using in situ radiation-mode optical microscopy. The in situ observation and ex situ Raman spectroscopy revealed that whether H$$_{2}$$ was supplied or not strongly affected the growth rate, thermal radiation contrast, and compressive strain of graphene on Au. We attributed these features to the surface reconstruction of Au(001) depending on H$$_{2}$$ supply. Our results are essential to achieve the graphene growth with high quality on Au for future applications.

Journal Articles

Longitudinal strain of epitaxial graphene monolayers on SiC substrates evaluated by $$z$$-polarization Raman microscopy

Saito, Yuika*; Tokiwa, Kenshiro*; Kondo, Takahiro*; Bao, J.*; Terasawa, Tomoo; Norimatsu, Wataru*; Kusunoki, Michiko*

AIP Advances (Internet), 9(6), p.065314_1 - 065314_6, 2019/06

 Times Cited Count:3 Percentile:16.36(Nanoscience & Nanotechnology)

Journal Articles

In-situ microscopic observation of crystal growth of graphene using thermal radiation

Terasawa, Tomoo; Saiki, Koichiro*; Yasuda, Satoshi; Asaoka, Hidehito

Dai-39-Kai Nihon Netsu Bussei Shimpojiumu Koen Rombunshu (CD-ROM), p.262 - 264, 2018/11

Graphene, monolayer graphite, has been expected as one of the new materials targeting the next generation electronics since its first isolation in 2004, due to the ultrahigh carrier mobility up to 100,000 cm$$_{2}$$/Vs and high transparency of 97.7%. The high transparency of graphene make it invisible on various substrates. Particularly, graphene on Cu, one of the common growth substrates for high-quality graphene, cannot be observed by optical microscopes. Here, we report the optical microscopic method to visualize graphene using thermal radiation. We observed a Cu surface by a zoom-lens and a CMOS camera during the growth of graphene by chemical vapor deposition. When graphene was grown on Cu substrates, the thermal radiation intensity increased at the area covered with graphene. The thermal radiation contrast between Cu surfaces with and without graphene showed that the thermal radiation intensity increased as the number of graphene layers in a layer-by-layer manner. We quantitatively analyzed the thermal radiation contrasts at various temperatures. We found the thermal radiation contrast was independent from the sample temperature. This result suggests that the emissivity of graphene is independent from the temperature, which is consistent with the theory of the optical properties of graphene. Our findings are essential for the discussion of the thermal radiation from the atomically thin materials including graphene.

Oral presentation

In-situ observation of CVD growth of graphene on Au by radiation-mode optical microscopy

Terasawa, Tomoo; Taira, Takanobu*; Obata, Seiji*; Yasuda, Satoshi; Saiki, Koichiro*; Asaoka, Hidehito

no journal, , 

Monolayer selective growth of graphene was achieved by chemical vapor deposition on a Cu substrate due to its low carbon solubility. In this study, we attempted the in-situ observation of chemical vapor deposition of graphene on a Au substrate with low carbon solid solubility like Cu by a radiation-mode optical microscopy. In the radiation images, the bright contrast started the growth between the trenches of the Au foil and progressed parallel to the trenches. The result of Raman mapping measurement indiceted that this contrast corresponded to graphene. In the presentation, we will also discuss the growth mechanism of graphene on the Au substrate.

Oral presentation

Determination of anisotropic diffusion ratio on Si(110)-16$$times$$2

Yano, Masahiro; Terasawa, Tomoo; Yasuda, Satoshi; Machida, Shinichi*; Asaoka, Hidehito

no journal, , 

no abstracts in English

Oral presentation

Determination of anisotropic diffusion ratio on Si(110)-16$$times$$2

Yano, Masahiro; Terasawa, Tomoo; Yasuda, Satoshi; Machida, Shinichi*; Asaoka, Hidehito

no journal, , 

The anisotropic diffusion coefficient ratio of the Si atoms on the Si(110)-16$$times$$2 reconstructed structure is determined by observing the "void" by scanning tunneling microscope (STM). The void length was measured to evaluate the anisotropic growth rate ratios for each void depth. The anisotropy of the void shape decreased as the void became deeper, indicating the reduction of the Si density ratio during the diffusion on the sidewall. Taking the migration of diffusing Si atoms to the upper and lower terraces and the adjacent sidewalls into account, we determined that the diffusion coefficient in the direction along the [1$$bar{1}$$2] or [$$bar{1}$$12] parallel to the step rows of the 16$$times$$2 reconstructed structure is 3.0 times higher than that of the other direction.

Oral presentation

Radiation-mode optical microscopy for CVD growth of graphene on gold

Terasawa, Tomoo; Taira, Takanobu*; Obata, Seiji*; Yasuda, Satoshi; Saiki, Koichiro*; Asaoka, Hidehito

no journal, , 

Since the solubility of carbon in copper is very low, monolayer graphene can be selectively grown by chemical vapor deposition (CVD) on a copper substrate. Thus, CVD growth of graphene is considered the most promising technique for the next-generation electronics. Here we report the CVD growth of graphene on gold substrates which also have the low solubility of carbon. We achieved the in-situ observation of the CVD growth of graphene on a gold foil by radiation-mode optical microscopy (Rad-OM). Figure shows the Rad-OM images of a gold foil at the growth time of 15, 30, and 40 min at 900$$^{circ}$$C under Ar, H$$_{2}$$, and CH$$_{4}$$ gas flow at 240, 8, and 5 sccm, respectively. The bright islands, corresponding to graphene confirmed by Raman spectroscopy, appeared between two trenches of the gold foil and grew parallel to the trenches. We will discuss the growth kinetics of graphene on gold, on the basis of the in-situ Rad-OM observation.

Oral presentation

In-situ observation of graphene growth on low-emissivity metal substrates using thermal radiation

Terasawa, Tomoo; Obata, Seiji*; Yasuda, Satoshi; Saiki, Koichiro*; Asaoka, Hidehito

no journal, , 

no abstracts in English

Oral presentation

Anisotropic reconstructed silicon (110)-16$$times$$2 surface

Asaoka, Hidehito; Yano, Masahiro; Terasawa, Tomoo; Yasuda, Satoshi

no journal, , 

no abstracts in English

Oral presentation

Modification of electronic band structure of graphene on Hex-Au(100) reconstructed surface

Terasawa, Tomoo; Yasuda, Satoshi; Hayashi, Naoki*; Norimatsu, Wataru*; Ito, Takahiro*; Machida, Shinichi*; Yano, Masahiro; Saiki, Koichiro*; Asaoka, Hidehito

no journal, , 

We report the band structure of graphene grown on hex-Au(001) using angle resolved photoemission spectroscopy (ARPES). We prepared graphene on hex-Au(001) by chemical vapor deposition and took ARPES image of the sample at AichiSR BL7U. The linear graphene band shows the intensity reduction at the binding energy of approximately 0.9 eV, indicating the modification of band structure of graphene by quasi-one dimensional potential of the hex-Au(001) reconstructed surface.

Oral presentation

Reaction region of deoxidization on Si(110)

Yano, Masahiro; Terasawa, Tomoo; Machida, Shinichi*; Yasuda, Satoshi; Asaoka, Hidehito

no journal, , 

no abstracts in English

44 (Records 1-20 displayed on this page)