arXiv subjects

H. Okuno

Publications and source records attributed to H. Okuno.

At least 19 recordsLinked to original sources

arXiv2025

Multi-functional Wafer-Scale Van der Waals Heterostructures and Polymorphs

Van der Waals heterostructures have promised the realisation of artificial materials with multiple physical phenomena such as giant optical nonlinearities, spin-to-charge interconversion in spintronics and topological carrier protection, in a single layered device through an infinitely diverse set of quantum materials. However, most efforts have only focused on exfoliated material that inherently limits both the dimensions of the materials and the scalability for applications. Here, we show the epitaxial growth of large area heterostructures of topological insulators (Bi2Se3), transition metal dichalcogenides (TMDs, WSe2) and ferromagnets (Co), resulting in the combination of functionalities including tuneable optical nonlinearities, spin-to-charge conversion and magnetic proximity effects. This is demonstrated through coherent phase resolved terahertz currents, bringing novel functionalities beyond those achievable in simple homostructures. In particular, we show the role of different TMD polymorphs, with the simple change of one atomic monolayer of the artificial material stack entirely changing its optical, electrical and magnetic properties. This epitaxial integration of diverse two-dimensional materials offers foundational steps towards diverse perspectives in quantum material engineering, where the material polymorph can be controlled at technological relevant scales for coupling applications in, for example, van der Waals nonlinear optics, optoelectronics, spintronics, multiferroics and coherent current control.

cond-mat.mtrl-sci↗

arXiv2025

Monolayer control of spin-charge conversion in van der Waals heterostructures

The diversity of 2D materials and their van der Waals (vdW) stacking presents a fertile ground for engineering novel multifunctional materials and quantum states of matter. This permits unique opportunities to tailor the electronic properties of vdW heterostructures by the insertion of only a single 2D material layer. However, such vdW materials engineering at the atomic scale has yet to be investigated for spin-charge interconversion phenomena. Here, we report on the control of these effects at the monolayer level, where drastic increase in intensity and change in sign of THz spintronic emission are demonstrated by inserting a single layer of MoSe$_2$ between PtSe$_2$ and graphene in a fully epitaxial, large area stacked structure. By using a combination of spin and angle resolved photoemission and density functional theory to reveal the electronic and spin structures, we illustrate two different mechanisms relying on charge transfer and electronic hybridization for the formation of Rashba states, which are responsible for spin-charge conversion and hence the THz spintronic emission. These findings open new pathways to design, at the atomic scale, efficient THz spintronic emitters made of 2D materials and other spintronic devices based on spin-charge interconversion phenomena.

cond-mat.mtrl-sci↗

arXiv2024

Enhanced optical properties of MoSe$_2$ grown by molecular beam epitaxy on hexagonal boron nitride

Transition metal dichalcogenides (TMD) like MoSe$_2$ exhibit remarkable optical properties such as intense photoluminescence (PL) in the monolayer form. To date, narrow-linewidth PL is only achieved in micrometer-sized exfoliated TMD flakes encapsulated in hexagonal boron nitride (hBN). In this work, we develop a growth strategy to prepare monolayer MoSe$_2$ on hBN flakes by molecular beam epitaxy in the van der Waals regime. It constitutes the first step towards the development of large area single crystalline TMDs encapsulated in hBN for potential integration in electronic or opto-electronic devices. For this purpose, we define a two-step growth strategy to achieve monolayer-thick MoSe$_2$ grains on hBN flakes. The high quality of MoSe$_2$ allows us to detect very narrow PL linewidth down to 5.5 meV at 13 K, comparable to the one of encapsulated exfoliated MoSe$_2$ flakes. Moreover, sizeable PL can be detected at room temperature as well as clear reflectivity signatures of A, B and charged excitons.

cond-mat.mtrl-sci↗

arXiv2023

Atomic scale imaging of the negative charge induced by a single vanadium dopant atom in monolayer WSe$_2$ using 4D-STEM

There has been extensive activity exploring the doping of semiconducting two-dimensional (2D) transition metal dichalcogenides in order to tune their electronic and magnetic properties. The outcome of doping depends on various factors, including the intrinsic properties of the host material, the nature of the dopants used, their spatial distribution as well as their interactions with other types of defects. A thorough atomic-level analysis is essential to fully understand these mechanisms. In this work, vanadium doped WSe$_2$ monolayer grown by molecular beam epitaxy is investigated using four-dimensional scanning transmission electron microscopy (4D-STEM). Through center of mass-based reconstruction, atomic scale maps are produced, allowing the visualization of both the electric field and the electrostatic potential around individual V atoms. To provide quantitative insights, these results are successfully compared with multislice image simulations based on ab initio calculations, accounting for lens aberrations. Finally, a negative charge around the V dopants is detected as a drop in the electrostatic potential, unambiguously demonstrating that 4D-STEM can be used to detect and to accurately analyze single dopant charge states in semiconducting 2D materials.

cond-mat.mtrl-sci↗

arXiv2023

Development of the Thomson scattering measurement system for cascade arc device with indirectly heated hollow cathode

We have developed a Thomson scattering measurement system for the cascade arc discharge device designed for the plasma window (PW) application study. The PW is one of the plasma application techniques that sustain the steep pressure gradient between high pressure (10-100 kPa) and a vacuum environment due to the thermal energy of the plasma. Since the plasma thermal energy is the essential parameter for the pressure separation capability of PW, we installed the Thomson scattering measurement system to observe the electron density and temperature within the anode and cathode of the PW for the detailed analysis of the pressure separation capability. The frequency-doubled Nd:YAG laser (532 nm, 200 mJ, 8 ns) was employed for the probe laser. The scattered light was fed to the triple grating spectrometer. The notch filter between the first and second grating eliminated the stray light, realizing a sufficiently high signal-to-noise ratio. The Thomson scattering measurement system successfully obtained the electron density and temperature of the cascade arc plasma at 20 mm downstream from the tip of the cathode. The installed system successfully obtained the Thomson scattering spectrum and showed that the electron density increased from $2\times10^{19} {\rm m}^{-3}$ to $7\times10^{19} {\rm m}^{-3}$ with the discharge power, while the electron temperature was almost constant at about 2 eV. The obtained data successfully contributed to the study of the pressure separation capability of the PW.

physics.plasm-ph↗

arXiv2023

Giant atomic swirl in graphene bilayers with biaxial heterostrain

The study of moiré engineering started with the advent of van der Waals heterostructures in which stacking two-dimensional layers with different lattice constants leads to a moiré pattern controlling their electronic properties. The field entered a new era when it was found that adjusting the twist between two graphene layers led to strongly-correlated-electron physics and topological effects associated with atomic relaxation. Twist is now used routinely to adjust the properties of two-dimensional materials. Here, we investigate a new type of moiré superlattice in bilayer graphene when one layer is biaxially strained with respect to the other - so-called biaxial heterostrain. Scanning tunneling microscopy measurements uncover spiraling electronic states associated with a novel symmetry-breaking atomic reconstruction at small biaxial heterostrain. Atomistic calculations using experimental parameters as inputs reveal that a giant atomic swirl forms around regions of aligned stacking to reduce the mechanical energy of the bilayer. Tight-binding calculations performed on the relaxed structure show that the observed electronic states decorate spiraling domain wall solitons as required by topology. This study establishes biaxial heterostrain as an important parameter to be harnessed for the next step of moiré engineering in van der Waals multilayers.

cond-mat.mes-hall↗

arXiv2023

Atomic-layer controlled THz Spintronic emission from Epitaxially grown Two dimensional PtSe$_2$/ferromagnet heterostructures

Terahertz (THz) Spintronic emitters based on ferromagnetic/metal junctions have become an important technology for the THz range, offering powerful and ultra-large spectral bandwidths. These developments have driven recent investigations of two-dimensional (2D) materials for new THz spintronic concepts. 2D materials, such as transition metal dichalcogenides (TMDs), are ideal platforms for SCC as they possess strong spin-orbit coupling (SOC) and reduced crystal symmetries. Moreover, SCC and the resulting THz emission can be tuned with the number of layers, electric field or strain. Here, epitaxially grown 1T-PtSe$_2$ and sputtered Ferromagnet (FM) heterostructures are presented as a novel THz emitter where the 1T crystal symmetry and strong SOC favor SCC. High quality of as-grown PtSe$_2$ layers is demonstrated and further FM deposition leaves the PtSe$_2$ unaffected, as evidenced with extensive characterization. Through this atomic growth control, the unique thickness dependent electronic structure of PtSe$_2$ allows the control of the THz emission by SCC. Indeed, we demonstrate the transition from the inverse Rashba-Edelstein effect in one monolayer to the inverse spin Hall effect in multilayers. This band structure flexibility makes PtSe$_2$ an ideal candidate as a THz spintronic 2D material and to explore the underlying mechanisms and engineering of the SCC for THz emission.

cond-mat.mtrl-sci↗

arXiv2021

Coexistence of ferromagnetism and spin-orbit coupling by incorporation of platinum in two-dimensional VSe$_2$

We report on a novel material, namely two-dimensional (2D) V$_{1-x}$Pt$_x$Se$_2$ alloy, exhibiting simultaneously ferromagnetic order and Rashba spin-orbit coupling. While ferromagnetism is absent in 1T-VSe$_2$ due to the competition with the charge density wave phase, we demonstrate theoretically and experimentally that the substitution of vanadium by platinum in VSe$_2$ (10-50 %) to form an homogeneous 2D alloy restores ferromagnetic order with Curie temperatures of 6 K for 5 monolayers and 25 K for one monolayer of V$_{0.65}$Pt$_{0.35}$Se$_2$. Moreover, the presence of platinum atoms gives rise to Rashba spin-orbit coupling in (V,Pt)Se$_2$ providing an original platform to study the interplay between ferromagnetism and spin-orbit coupling in the 2D limit.

cond-mat.mtrl-sci↗

arXiv2021

First Search for the $K_L \to π^0 γ$ Decay

We report the first search for the $K_L \to π^0 γ$ decay, which is forbidden by Lorentz invariance, using the data from 2016 to 2018 at the J-PARC KOTO experiment. With a single event sensitivity of $(7.1\pm 0.3_{\rm stat.} \pm 1.6_{\rm syst.})\times 10^{-8}$, no candidate event was observed in the signal region. The upper limit on the branching fraction was set to be $1.7\times 10^{-7}$ at the 90\% confidence level.

hep-ex↗

arXiv2021

Study of the $K_L \!\to\! π^0 ν\overlineν$ Decay at the J-PARC KOTO Experiment

The rare decay $K_L \!\to\! π^0 ν\overlineν$ was studied with the dataset taken at the J-PARC KOTO experiment in 2016, 2017, and 2018. With a single event sensitivity of $( 7.20 \pm 0.05_{\rm stat} \pm 0.66_{\rm syst} ) \times 10^{-10}$, three candidate events were observed in the signal region. After unveiling them, contaminations from $K^{\pm}$ and scattered $K_L$ decays were studied, and the total number of background events was estimated to be $1.22 \pm 0.26$. We conclude that the number of observed events is statistically consistent with the background expectation. For this dataset, we set an upper limit of $4.9 \times 10^{-9}$ on the branching fraction of $K_L \!\to\! π^0 ν\overlineν$ at the 90% confidence level.

hep-ex↗

arXiv2019

Van der Waals epitaxy of Mn-doped MoSe$_2$ on mica

The magnetic order associated with the degree of freedom of spin in two-dimensional (2D) materials is subjected to intense investigation because of its potential application in 2D spintronics and valley-related magnetic phenomena. We report here a bottom-up strategy using molecular beam epitaxy to grow and dope large-area (cm$^2$) few-layer MoSe$_2$ with Mn as a magnetic dopant. High-quality Mn-doped MoSe$_2$ layers are obtained for Mn content of less than 5 % (atomic). When increasing the Mn content above 5 % we observe a clear transition from layer-by-layer to cluster growth. Magnetic measurements involving a transfer process of the cm$^2$-large doped layers on 100-micron-thick silicon substrate, show plausible proof of high-temperature ferromagnetism of 1 % and 10 % Mn-doped MoSe$_2$. Although we could not point to a correlation between magnetic and electrical properties, we demonstrate that the transfer process described in this report permits to achieve conventional electrical and magnetic measurements on the doped layers transferred on any substrate. Therefore, this study provides a promising route to characterize stable ferromagnetic 2D layers, which is broadening the current start-of-the-art of 2D materials-based applications.

cond-mat.mtrl-sci↗

arXiv2019

Van der Waals solid phase epitaxy to grow large-area manganese-doped MoSe$_2$ few-layers on SiO$_2$/Si

Large-area growth of continuous transition metal dichalcogenides (TMDCs) layers is a prerequisite to transfer their exceptional electronic and optical properties into practical devices. It still represents an open issue nowadays. Electric and magnetic doping of TMDC layers to develop basic devices such as p-n junctions or diluted magnetic semiconductors for spintronic applications are also an important field of investigation. Here, we have developed two different techniques to grow MoSe$_2$ mono- and multi-layers on SiO$_2$/Si substrates over large areas. First, we co-deposited Mo and Se atoms on SiO$_2$/Si by molecular beam epitaxy in the van der Waals regime to obtain continuous MoSe$_2$ monolayers over 1 cm$^2$. To grow MoSe$_2$ multilayers, we then used the van der Waals solid phase epitaxy which consists in depositing an amorphous Se/Mo bilayer on top of a co-deposited MoSe$_2$ monolayer which serves as a van der Waals growth template. By annealing, we obtained continuous MoSe$_2$ multilayers over 1 cm$^2$. Moreover, by inserting a thin layer of Mn in the stack, we could demonstrate the incorporation of up to 10 \% of Mn in MoSe$_2$ bilayers.

cond-mat.mtrl-sci↗

arXiv2019

Mn4N ferrimagnetic thin films for sustainable spintronics

Spintronics, which is the basis of a low-power, beyond-CMOS technology for computational and memory devices, remains up to now entirely based on critical materials such as Co, heavy metals and rare-earths. Here, we show that Mn4N, a rare-earth free ferrimagnet made of abundant elements, is an exciting candidate for the development of sustainable spintronics devices. Mn4N thin films grown epitaxially on SrTiO3 substrates possess remarkable properties, such as a perpendicular magnetisation, a very high extraordinary Hall angle (2%) and smooth domain walls, at the millimeter scale. Moreover, domain walls can be moved at record speeds by spin polarised currents, in absence of spin-orbit torques. This can be explained by the large efficiency of the adiabatic spin transfer torque, due to the conjunction of a reduced magnetisation and a large spin polarisation. Finally, we show that the application of gate voltages through the SrTiO3 substrates allows modulating the Mn4N coercive field with a large efficiency.

cond-mat.mtrl-sci↗

arXiv2019

Search for $K_L \!\to\! π^0 ν\overlineν$ and $K_L \!\to\! π^0 X^0$ Decays at the J-PARC KOTO Experiment

A search for the rare decay $K_L \!\to\! π^0 ν\overlineν$ was performed. With the data collected in 2015, corresponding to $2.2 \times 10^{19}$ protons on target, a single event sensitivity of $( 1.30 \pm 0.01_{\rm stat} \pm 0.14_{\rm syst} ) \times 10^{-9}$ was achieved and no candidate events were observed. We set an upper limit of $3.0 \times 10^{-9}$ for the branching fraction of $K_L \!\to\! π^0 ν\overlineν$ at the 90% confidence level (C.L.), which improved the previous limit by almost an order of magnitude. An upper limit for $K_L \!\to\! π^0 X^0$ was also set as $2.4 \times 10^{-9}$ at the 90% C.L., where $X^0$ is an invisible boson with a mass of $135~{\rm MeV}/c^2$.

hep-ex↗

arXiv2017

Epitaxial electrical contact to graphene on SiC

Establishing good electrical contacts to nanoscale devices is a major issue for modern technology and contacting 2D materials is no exception to the rule. One-dimensional edge-contacts to graphene were recently shown to outperform surface contacts but the method remains difficult to scale up. We report a resist-free and scalable method to fabricate few graphene layers with electrical contacts in a single growth step. This method derives from the discovery reported here of the growth of few graphene layers on a metallic carbide by thermal annealing of a carbide forming metallic film on SiC in high vacuum. We exploit the combined effect of edge-contact and partially-covalent surface epitaxy between graphene and the metallic carbide to fabricate devices in which low contact-resistance and Josephson effect are observed. Implementing this approach could significantly simplify the realization of large-scale graphene circuits.

physics.app-ph↗

arXiv2017

Millimeter-scale layered MoSe2 grown on sapphire and evidence for negative magnetoresistance

Molecular beam epitaxy technique has been used to deposit a single layer and a bilayer of MoSe 2 on sapphire. Extensive characterizations including in-situ and ex-situ measurements show that the layered MoSe 2 grows in a scalable manner on the substrate and reveals characteristics of a stoichiometric 2H-phase. The layered MoSe 2 exhibits polycrystalline features with domains separated by defects and boundaries. Temperature and magnetic field dependent resistivity measurements unveil a carrier hopping character described within two-dimensional variable range hopping mechanism. Moreover, a negative magnetoresistance was observed, stressing a fascinating feature of the charge transport under the application of a magnetic field in the layered MoSe 2 system. This negative magnetoresistance observed at millimeter-scale is similar to that observed recently at room temperature inWS2 flakes at a micrometer scale [Zhang et al., Appl. Phys. Lett. 108, 153114 (2016)]. This scalability highlights the fact that the underlying physical mechanism is intrinsic to these two-dimensional materials and occurs at very short scale.

cond-mat.mtrl-sci↗

arXiv2016

A new search for the $K_{L} \to π^0 ν\overlineν$ and $K_{L} \to π^{0} X^{0}$ decays

We searched for the $CP$-violating rare decay of neutral kaon, $K_{L} \to π^0 ν\overlineν$, in data from the first 100 hours of physics running in 2013 of the J-PARC KOTO experiment. One candidate event was observed while $0.34\pm0.16$ background events were expected. We set an upper limit of $5.1\times10^{-8}$ for the branching fraction at the 90\% confidence level (C.L.). An upper limit of $3.7\times10^{-8}$ at the 90\% C.L. for the $K_{L} \to π^{0} X^{0}$decay was also set for the first time, where $X^{0}$ is an invisible particle with a mass of 135 MeV/$c^{2}$.

hep-ex↗

arXiv2016

Long-lived neutral-kaon flux measurement for the KOTO experiment

The KOTO ($K^0$ at Tokai) experiment aims to observe the CP-violating rare decay $K_L \rightarrow π^0 ν\barν$ by using a long-lived neutral-kaon beam produced by the 30 GeV proton beam at the Japan Proton Accelerator Research Complex. The $K_L$ flux is an essential parameter for the measurement of the branching fraction. Three $K_L$ neutral decay modes, $K_L \rightarrow 3π^0$, $K_L \rightarrow 2π^0$, and $K_L \rightarrow 2γ$ were used to measure the $K_L$ flux in the beam line in the 2013 KOTO engineering run. A Monte Carlo simulation was used to estimate the detector acceptance for these decays. Agreement was found between the simulation model and the experimental data, and the remaining systematic uncertainty was estimated at the 1.4\% level. The $K_L$ flux was measured as $(4.183 \pm 0.017_{\mathrm{stat.}} \pm 0.059_{\mathrm{sys.}}) \times 10^7$ $K_L$ per $2\times 10^{14}$ protons on a 66-mm-long Au target.

physics.ins-det↗