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K. Nagashio

Publications and source records attributed to K. Nagashio.

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Trion transfer in mixed-dimensional heterostructures

Charged excitons, or trions, offering unique spin and charge degrees of freedom, have primarily been investigated in doped systems where charges are long considered indispensable. Here, we present an alternative route to ultra-efficient trion emission from an intrinsic, defect-free semiconductor via a transfer mechanism. By exciting trions in two-dimensional tungsten-diselenide donors and transferring them into one-dimensional carbon-nanotube acceptors in mixed-dimensional heterostructures, we circumvent the usual carrier requirement, overcoming intrinsic Auger-quenching limitations. Benefitting from a reservoir effect induced by dimensional heterogeneity, this process achieves trion emission efficiencies increased by over 100-fold compared to conventional doping-based approaches, and remains robust across diverse doping conditions. Our findings extend the exciton transfer paradigm to the three-body quasiparticles, offering a new platform for advancing excitonic physics and trion-based optoelectronic/spintronic applications.

cond-mat.mes-hall

Room-temperature quantum emission from interface excitons in mixed-dimensional heterostructures

The development of van der Waals heterostructures has introduced unconventional phenomena that emerge at atomically precise interfaces. For example, interlayer excitons in two-dimensional transition metal dichalcogenides show intriguing optical properties at low temperatures. Here we report on room-temperature observation of interface excitons in mixed-dimensional heterostructures consisting of two-dimensional tungsten diselenide and one-dimensional carbon nanotubes. Bright emission peaks originating from the interface are identified, spanning a broad energy range within the telecommunication wavelengths. The effect of band alignment is investigated by systematically varying the nanotube bandgap, and we assign the new peaks to interface excitons as they only appear in type-II heterostructures. Room-temperature localization of low-energy interface excitons is indicated by extended lifetimes as well as small excitation saturation powers, and photon correlation measurements confirm single-photon emission. With mixed-dimensional van der Waals heterostructures where band alignment can be engineered, new opportunities for quantum photonics are envisioned.

cond-mat.mes-hall

Resonant exciton transfer in mixed-dimensional heterostructures for overcoming dimensional restrictions in optical processes

Nanomaterials exhibit unique optical phenomena, in particular excitonic quantum processes occurring at room temperature. The low dimensionality, however, imposes strict requirements for conventional optical excitation, and an approach for bypassing such restrictions is desirable. Here we report on exciton transfer in carbon-nanotube/tungsten-diselenide heterostructures, where band alignment can be systematically varied. The mixed-dimensional heterostructures display a pronounced exciton reservoir effect where the longer-lifetime excitons within the two-dimensional semiconductor are funneled into carbon nanotubes through diffusion. This new excitation pathway presents several advantages, including larger absorption areas, broadband spectral response, and polarization-independent efficiency. When band alignment is resonant, we observe substantially more efficient excitation via tungsten diselenide compared to direct excitation of the nanotube. We further demonstrate simultaneous bright emission from an array of carbon nanotubes with varied chiralities and orientations. Our findings show the potential of mixed-dimensional heterostructures and band alignment engineering for energy harvesting and quantum applications through exciton manipulation.

cond-mat.mes-hall

Quantization of mode shifts in nanocavities integrated with atomically thin sheets

The unique optical properties of two-dimensional layered materials are attractive for achieving increased functionality in integrated photonics. Owing to the van der Waals nature, these materials are ideal for integrating with nanoscale photonic structures. Here we report on carefully designed air-mode silicon photonic crystal nanobeam cavities for efficient control through two-dimensional materials. By systematically investigating various types and thickness of two-dimensional materials, we are able to show that enhanced responsivity allows for giant shifts of the resonant wavelength. With atomically precise thickness over a macroscopic area, few-layer flakes give rise to quantization of the mode shifts. We extract the dielectric constant of the flakes and find that it is independent of the layer number down to a monolayer. Flexible reconfiguration of a cavity is demonstrated by stacking and removing ultrathin flakes. With an unconventional cavity design, our results open up new possibilities for photonic devices integrated with two-dimensional materials.

physics.optics

Micrometer-scale monolayer SnS growth by physical vapor deposition

Recently, monolayer SnS, a two-dimensional group IV monochalcogenide, was grown on a mica substrate at the micrometer-size scale by the simple physical vapor deposition (PVD), resulting in the successful demonstration of its in-plane room temperature ferroelectricity. However, the reason behind the monolayer growth remains unclear because it had been considered that the SnS growth inevitably results in a multilayer thickness due to the strong interlayer interaction arising from lone pair electrons. Here, we investigate the PVD growth of monolayer SnS from two different feed powders, highly purified SnS and commercial phase-impure SnS. Contrary to expectations, it is suggested that the mica substrate surface is modified by sulfur evaporated from the Sn2S3 contaminant in the as-purchased powder and the lateral growth of monolayer SnS is facilitated due to the enhanced surface diffusion of SnS precursor molecules, unlike the growth from the highly purified powder. This insight provides a guide to identify further controllable growth conditions.

cond-mat.mtrl-sci

Full energy spectra of interface state densities for n- and p-type MoS2 field-effect transistors

Two-dimensional (2D) layered materials are promising for replacing Si to overcome the scaling limit of recent ~5 nm-length metal-oxide-semiconductor field-effect transistors (MOSFETs). However, the insulator/2D channel interface severely degrades the performance of 2D-based MOSFETs, and the origin of the degradation remains largely unexplored. Here, we present the full energy spectra of the interface state densities (Dit) for both n- and p- MoS2 FETs, based on the comprehensive and systematic studies, i.e., thickness range from monolayer to bulk and various gate stack structures including 2D heterostructure with h-BN as well as typical high-k top-gate structure. For n-MoS2, Dit around the mid gap is drastically reduced to 5*10^11 cm-2eV-1 for the heterostructure FET with h-BN from 5*10^12 cm-2eV-1 for the high-k top-gate MoS2 FET. On the other hand, Dit remains high, ~10^13 cm-2eV-1, even for the heterostructure FET for p-MoS2. The systematic study elucidates that the strain induced externally through the substrate surface roughness and high-k deposition process is the origin for the interface degradation on the conduction band side, while sulfur-vacancy-induced defect-states dominate the interface degradation on the valance band side. The present understanding on the interface properties provides the key to further improving the performance of 2D FETs.

physics.app-ph

Purely in-plane ferroelectricity in monolayer SnS at room temperature

2D van der Waals ferroelectric semiconductors have emerged as an attractive building block with immense potential to provide multifunctionality in nanoelectronics. Although several accomplishments have been reported in ferroelectric resistive switching for out-of-plane 2D ferroelectrics down to the monolayer, a purely in-plane ferroelectric has not been experimentally validated at the monolayer thickness. Herein, a micrometer-size monolayer SnS is grown on mica by physical vapor deposition, and in-plane ferroelectric switching is demonstrated with a two-terminal device at room temperature (RT). SnS has been commonly regarded to exhibit the odd-even effect, where the centrosymmetry breaks only in the odd-number layers to exhibit ferroelectricity. Remarkably, however, a robust RT ferroelectricity exists in SnS below a critical thickness of 15 layers with both an odd and even number of layers. The lack of the odd-even effect probably originates from the interaction with the mica substrate, suggesting the possibility of controlling the stacking sequence of multilayer SnS, going beyond the limit of ferroelectricity in the monolayer. This work will pave the way for nanoscale ferroelectric applications based on SnS as a new platform for in-plane ferroelectrics.

cond-mat.mtrl-sci

Hexagonal boron nitride as an ideal substrate for carbon nanotube photonics

Hexagonal boron nitride is widely used as a substrate for two-dimensional materials in both electronic and photonic devices. Here, we demonstrate that two-dimensional hexagonal boron nitride is also an ideal substrate for one-dimensional single-walled carbon nanotubes. Nanotubes directly attached to hexagonal boron nitride show bright photoluminescence with narrow linewidth at room temperature, comparable to air-suspended nanotubes. Using photoluminescence excitation spectroscopy, we unambiguously assign the chiralities of nanotubes on boron nitride by tracking individual tubes before and after contact with boron nitride. Although hexagonal boron nitride has a low dielectric constant and is attached to only one side of the nanotubes, we observe that optical transition energies are redshifted as much as ~50 meV from the air-suspended nanotubes. We also perform statistical measurements on more than 400 tubes, and the redshifts are found to be dependent on tube diameter. This work opens up new possibilities for all-solid-state carbon nanotube photonic devices by utilizing hexagonal boron nitride substrates.

cond-mat.mes-hall

Impact ionization and transport properties of hexagonal boron nitride in constant-voltage measurement

The electrical evaluation of the crystallinity of hexagonal boron nitride (h-BN) is still limited to the measurement of dielectric breakdown strength, in spite of its importance as the substrate for 2-dimensional van der Waals heterostructure devices. In this study, physical phenomena for degradation and failure in exfoliated single-crystal h-BN films were investigated using the constant-voltage stress test. At low electrical fields, the current gradually reduced and saturated with time, while the current increased at electrical fields higher than ~8 MV/cm and finally resulted in the catastrophic dielectric breakdown. These transient behaviors may be due to carrier trapping to the defect sites in h-BN because trapped carriers lower or enhance the electrical fields in h-BN depending on their polarities. The key finding is the current enhancement with time at the high electrical field, suggesting the accumulation of electrons generated by the impact ionization process. Therefore, a theoretical model including the electron generation rate by impact ionization process was developed. The experimental data support the expected degradation mechanism of h-BN. Moreover, the impact ionization coefficient was successfully extracted, which is comparable to that of SiO2, even though the fundamental band gap for h-BN is smaller than that for SiO2. Therefore, the dominant impact ionization in h-BN could be band-to-band excitation, not defect-assisted impact ionization.

cond-mat.mtrl-sci

Molecularly-thin anatase field-effect transistors fabricated through the solid state transformation of titania nanosheets

We demonstrate the field-effect transistor (FET) operation of molecularly-thin anatase phase produced through solid state transformation from Ti0.87O2 nanosheets. Monolayer Ti0.87O2 nanosheet with a thickness of 0.7 nm is two-dimensional oxide insulators in which Ti vacancies are incorporated, rather than oxygen vacancies. Since the fabrication method, in general, largely affects the film quality, the anatase films derived from Ti0.87O2 nanosheet show interesting characteristics, such as no photocurrent peak at ~2 eV, which is related to oxygen vacancies, and a larger band gap of 3.8 eV. The 10-nm thick anatase FETs exhibit superior transport characteristics with a maximum mobility of ~1.3 cm2V-1s-1 and current on/off ratio of ~105 at room temperature. The molecularly-thin anatase FET may provide new functionalities, such as field-effect control of catalytic properties.

cond-mat.mtrl-sci

Fully dry PMMA transfer of graphene on h-BN using a heating/cooling system

The key to achieve high-quality van der Waals heterostructure devices made of stacking various two-dimensional (2D) layered materials lies in the clean interface without bubbles and wrinkles. Although polymethylmethacrylate (PMMA) is generally used as a sacrificial transfer film due to its strong adhesion property, it is always dissolved in the solvent after the transfer, resulting in the unavoidable PMMA residue on the top surface. This makes it difficult to locate clean interface areas. In this work, we present a fully dry PMMA transfer of graphene onto h-BN using a heating/cooling system which allows identification of clean interface area for high quality graphene/h-BN heterostructure fabrication. The mechanism lies in the utilization of the large difference in thermal expansion coefficients between polymers (PMMA/PDMS) and inorganic materials (graphene/h-BN substrate) to mechanically peel off PMMA from graphene by the thermal shrinkage of polymers, leaving no PMMA residue on the graphene surface. This method can be applied to all types of 2D layered materials.

cond-mat.mtrl-sci

Layer-by-Layer Dielectric Breakdown of Hexagonal Boron Nitride

Hexagonal boron nitride (BN) is widely used as a substrate and gate insulator for two-dimensional (2D) electronic devices. The studies on insulating properties and electrical reliability of BN itself, however, are quite limited. Here, we report a systematic investigation of the dielectric breakdown characteristics of BN using conductive atomic force microscopy. The electric field strength was found to be ~12 MV/cm, which is comparable to that of conventional SiO2 oxides because of the covalent bonding nature of BN. After the hard dielectric breakdown, the BN fractured like a flower into equilateral triangle fragments. However, when the applied voltage was terminated precisely in the middle of the dielectric breakdown, the formation of a hole that did not penetrate to the bottom metal electrode was clearly observed. Subsequent I-V measurements of the hole indicated that the BN layer remaining in the hole was still electrically inactive. Based on these observations, layer-by-layer breakdown was confirmed for BN with regard to both physical fracture and electrical breakdown. Moreover, statistical analysis of the breakdown voltages using a Weibull plot suggested the anisotropic formation of defects. These results are unique to layered materials and unlike the behavior observed for conventional 3D amorphous oxides.

cond-mat.mtrl-sci

Atomic layer deposition of Y2O3 on h-BN for a gate stack in graphene FETs

The combination of h-BN and high-k dielectrics is required for a top gate insulator in miniaturized graphene field-effect transistors because of the low dielectric constant of h-BN. We investigated the deposition of Y2O3 on h-BN using atomic layer deposition. The deposition of Y2O3 on h-BN was confirmed without any buffer layer. An increase in the deposition temperature reduced the surface coverage. The deposition mechanism could be explained by the competition between the desorption and adsorption of the Y precursor on h-BN due to the polarization. Although a full surface coverage was difficult to achieve, the use of an oxidized metal seeding layer on h-BN resulted in a full surface coverage.

cond-mat.mtrl-sci

Crystal orientation relation and macroscopic surface roughness in hetero-epitaxially grown graphene on Cu/mica

A clean, flat and orientation-identified graphene on a substrate is in high demand for graphene electronics. In this study, the hetero-epitaxial graphene growth on Cu(111)/mica(001) by chemical vapor deposition is investigated to check the applicability for the top-gate insulator research on graphene as well as the graphene channel research by transferring graphene on SiO2/Si substrates. After adjusting the graphene-growth condition, the surface roughness of the graphene/Cu/mica substrate and the average smooth area are ~0.34 nm and ~100 um2, respectively. The orientation of graphene in the graphene/Cu/mica substrate can be identified by the hexagonal void morphology of Cu. Moreover, we demonstrate the relatively high mobility of ~4500 cm2V-1s-1 in graphene transferred on the SiO2/Si substrate. These results suggest that the present graphene/Cu/mica substrate can be used for top-gate insulator research on graphene.

cond-mat.mtrl-sci

Carrier density modulation in graphene underneath Ni electrode

We investigate the transport properties of graphene underneath metal to reveal whether the carrier density in graphene underneath source/drain electrodes in graphene field-effect transistors is fixed. The resistance of the graphene/Ni double-layered structure has shown a graphene-like back-gate bias dependence. In other words, the electrical properties of graphene are not significantly affected by its contact with Ni. This unexpected result may be ascribed to resist residuals at the metal/graphene interface, which may reduce the interaction between graphene and metals. In a back-gate device fabricated using the conventional lithography technique with an organic resist, the carrier density modulation in the graphene underneath the metal electrodes should be considered when discussing the metal/graphene contact.

cond-mat.mes-hall

Estimation of residual carrier density near the Dirac point in graphene through quantum capacitance measurement

We discuss the residual carrier density (n*) near the Dirac point (DP) in graphene estimated by quantum capacitance (CQ) and conductivity measurements. The CQ at the DP has a finite value and is independent of the temperature. A similar behavior is also observed for the conductivity at the DP, because their origin is residual carriers induced externally by charged impurities. The n* extracted from CQ, however, is often smaller than that from the conductivity, suggesting that the mobility in the puddle region is lower than that in the linear region. The CQ measurement should be employed for estimating n* quantitatively.

cond-mat.mtrl-sci

Electrical transport properties of graphene on SiO2 with specific surface structures

The mobility of graphene transferred on a SiO2/Si substrate is limited to ~10,000 cm2/Vs. Without understanding the graphene/SiO2 interaction, it is difficult to improve the electrical transport properties. Although surface structures on SiO2 such as silanol and siloxane groups are recognized, the relation between the surface treatment of SiO2 and graphene characteristics has not yet been elucidated. This paper discusses the electrical transport properties of graphene on specific surface structures of SiO2 prepared by O2-plasma treatments and reoxidization.

cond-mat.mtrl-sci

Contact resistivity and current flow path at metal/graphene contact

The contact properties between metal and graphene were examined. The electrical measurement on a multiprobe device with different contact areas revealed that the current flow preferentially entered graphene at the edge of the contact metal. The analysis using the cross-bridge Kelvin structure (CBK) suggested that a transition from the edge conduction to area conduction occurred for a contact length shorter than the transfer length of ~1 micron. The contact resistivity for Ni was measured as ~5*10-6 Ohmcm2 using the CBK. A simple calculation suggests that a contact resistivity less than 10-9 Ohmcm2 is required for miniaturized graphene field effect transistors.

cond-mat.mtrl-sci