arXiv subjects

Taisuke Ohta

Publications and source records attributed to Taisuke Ohta.

18 recordsLinked to original sources

arXiv2026

Island Sliding Barriers: A first-principles metric for determining remote epitaxy viability

Remote epitaxy, where a 2D van der Waals material (usually graphene) is inserted on top of the substrate before film epitaxy, has emerged as a promising path for growing electronics with lower defect rates and less stringent lattice matching requirements. The exact mechanism behind remote epitaxy has not been definitively shown, however, and it is not obvious when examining a new substrate-film pair whether they would be compatible with the remote epitaxy process. In this paper, we use first principles calculations to test several different mechanisms for determining whether a given substrate-film pair will successfully be grown with remote epitaxy. We find that previously calculated metrics such as electrostatic potential do not hold sufficient explanatory power. We find that the sliding barrier of small islands on the surface when the atomic positions are allowed to optimize provides the most rigorous criteria for whether a given substrate-film pair is remote epitaxy active. This indicates that remote epitaxy is likely a phenomenon related to the kinetics and ease of island migration on the graphene surface.

cond-mat.mtrl-sci↗

arXiv2023

Near-field Imaging of Optical Resonances in Silicon Metasurfaces Using Photoelectron Microscopy

Precise control of light-matter interactions at the nanoscale lies at the heart of nanophotonics. Experimental examination at this length scale is challenging, however, since the corresponding electromagnetic near-field is often confined within volumes below the resolution of conventional optical microscopy. In semiconductor nanophotonics electromagnetic fields are further restricted within the confines of individual subwavelength resonators, limiting access to critical light-matter interactions in these structures. In this work, we demonstrate that photoelectron emission microscopy (PEEM) can be used for polarization resolved near-field spectroscopy and imaging of electromagnetic resonances supported by broken-symmetry silicon metasurfaces. We find that the photoemission results, enabled through an in-situ potassium surface layer, are consistent with full-wave simulations and far-field reflectance measurements across visible and near-infrared wavelengths. In addition, we uncover a polarization dependent evolution of collective resonances near the metasurface array edge taking advantage of the far-field excitation and full-field imaging of PEEM. Here, we deduce that coupling between eight resonators or more establishes the collective excitations of this metasurface. All told, we demonstrate that the high-spatial resolution hyperspectral imaging and far-field illumination of PEEM can be leveraged for the metrology of collective, non-local, optical resonances in semiconductor nanophotonic structures.

physics.optics↗

arXiv2021

Atomic step disorder on polycrystalline surfaces leads to spatially inhomogeneous work functions

Structural disorder causes materials surface electronic properties, e.g. work function ($\phi$) to vary spatially, yet it is challenging to prove exact causal relationships to underlying ensemble disorder, e.g. roughness or granularity. For polycrystalline Pt, nanoscale resolution photoemission threshold mapping reveals a spatially varying $\phi= 5.70\pm 0.03$~eV over a distribution of (111) textured vicinal grain surfaces prepared by sputter deposition and annealing. With regard to field emission and related phenomena, e.g. vacuum arc initiation, a salient feature of the $\phi$ distribution is that it is skewed with a long tail to values down to 5.4 eV, i.e. far below the mean, which is exponentially impactful to field emission via the Fowler-Nordheim relation. We show that the $\phi$ spatial variation and distribution can be explained by ensemble variations of granular tilts and surface slopes via a Smoluchowski smoothing model wherein local $\phi$ variations result from spatially varying densities of electric dipole moments, intrinsic to atomic steps, that locally modify $\phi$. Atomic step-terrace structure is confirmed with scanning tunneling microscopy (STM) at several locations on our surfaces, and prior works showed STM evidence for atomic step dipoles at various metal surfaces. From our model, we find an atomic step edge dipole $\mu=0.12$ D/edge atom, which is comparable to values reported in studies that utilized other methods and materials. Our results elucidate a connection between macroscopic $\phi$ and nanostructure that may contribute to the spread of reported $\phi$ for Pt and other surfaces, and may be useful toward more complete descriptions of polycrystalline metals in models of field emission and other related vacuum electronics phenomena, e.g. arc initiation.

cond-mat.mtrl-sci↗

arXiv2018

Local Electronic Structure Changes in Polycrystalline CdTe with CdCl$_2$ Treatment and Air Exposure

Post-deposition CdCl$_2$ treatment of polycrystalline CdTe is known to increase photovoltaic efficiency. However, the precise chemical, structural, and electronic changes that underpin this improvement are still debated. In this study, spectroscopic photoemission electron microscopy was used to spatially map the vacuum level and ionization energy of CdTe films, enabling the identification of electronic structure variations between grains and grain boundaries. In vacuo preparation and inert transfer of oxide-free CdTe surfaces isolated the separate effects of CdCl$_2$ treatment and ambient oxygen exposure. Qualitatively, grain boundaries displayed lower work function and downward band bending relative to grain interiors, but only after air exposure of CdCl$_2$-treated CdTe. Analysis of numerous space charge regions at grain boundaries (GBs) showed an average depletion width of 290 nm and an average band bending magnitude of 70 meV, corresponding to a GB trap density of 10$^{11}$ cm$^{-2}$ and a net carrier density of 10$^{15}$ cm$^{-3}$. These results suggest that both CdCl$_2$ treatment and oxygen exposure may be independently tuned to enhance CdTe photovoltaic performance by engineering the interface and bulk electronic structure.

cond-mat.mtrl-sci↗

arXiv2017

Effects of CdCl$_2$ treatment on the local electronic properties of polycrystalline CdTe measured with photoemission electron microscopy

To investigate the effects of CdCl$_2$ treatment on the local electronic properties of polycrystalline CdTe films, we conducted a photoemission electron microscopy (PEEM) study of polished surfaces of CdTe films in superstrate configuration, with and without CdCl$_2$ treatment. From photoemission intensity images, we observed the tendency for individual exposed grain interiors to vary in photoemission intensity, regardless of whether or not films received CdCl$_2$ treatment. Additionally, grain boundaries develop contrast in photoemission intensity images different from grain interiors after an air exposure step, similar to observations of activated grain boundaries using scanning Kelvin probe force microscopy studies. These results suggest that work function varies locally, from one grain interior to another, as well as between grain boundaries and grain interiors.

cond-mat.mtrl-sci↗

arXiv2015

Molecular beam epitaxy growth of SrO buffer layers on graphite and graphene for the integration of complex oxides

We report the successful growth of high-quality SrO films on highly-ordered pyrolytic graphite (HOPG) and single-layer graphene by molecular beam epitaxy. The SrO layers have (001) orientation as confirmed by x-ray diffraction (XRD) while atomic force microscopy measurements show continuous pinhole-free films having rms surface roughness of <1.5 Å. Transport measurements of exfoliated graphene after SrO deposition show a strong dependence between the Dirac point and Sr oxidation. Subsequently, the SrO is leveraged as a buffer layer for more complex oxide integration via the demonstration of (001) oriented SrTiO3 grown atop a SrO/HOPG stack.

cond-mat.mtrl-sci↗

arXiv2013

Low-energy Electron Reflectivity from Graphene

Low-energy reflectivity of electrons from single- and multi-layer graphene is examined both theoretically and experimentally. A series of minima in the reflectivity over the energy range of 0 - 8 eV are found, with the number of minima depending on the number of graphene layers. Using first-principles computations, it is demonstrated that a free standing n-layer graphene slab produces n-1 reflectivity minima. This same result is also found experimentally for graphene supported on SiO2. For graphene bonded onto other substrates it is argued that a similar series of reflectivity minima is expected, although in certain cases an additional minimum occurs, at an energy that depends on the graphene-substrate separation and the effective potential in that space.

cond-mat.mes-hall↗

arXiv2013

Electronic Hybridization of Large-Area Stacked Graphene Films

Direct, tunable coupling between individually assembled graphene layers is a next step towards designer two-dimensional (2D) crystal systems, with relevance for fundamental studies and technological applications. Here we describe the fabrication and characterization of large-area (> cm^2), coupled bilayer graphene on SiO2/Si substrates. Stacking two graphene films leads to direct electronic interactions between layers, where the resulting film properties are determined by the local twist angle. Polycrystalline bilayer films have a "stained-glass window" appearance explained by the emergence of a narrow absorption band in the visible spectrum that depends on twist angle. Direct measurement of layer orientation via electron diffraction, together with Raman and optical spectroscopy, confirms the persistence of clean interfaces over large areas. Finally, we demonstrate that interlayer coupling can be reversibly turned off through chemical modification, enabling optical-based chemical detection schemes. Together, these results suggest that individual 2D crystals can be individually assembled to form electronically coupled systems suitable for large-scale applications.

cond-mat.mtrl-sci↗

arXiv2011

Magnetotransport Properties of Quasi-Free Standing Epitaxial Graphene Bilayer on SiC: Evidence for Bernal Stacking

We investigate the magnetotransport properties of quasi-free standing epitaxial graphene bilayer on SiC, grown by atmospheric pressure graphitization in Ar, followed by H$_2$ intercalation. At the charge neutrality point the longitudinal resistance shows an insulating behavior, which follows a temperature dependence consistent with variable range hopping transport in a gapped state. In a perpendicular magnetic field, we observe quantum Hall states (QHSs) both at filling factors ($ν$) multiple of four ($ν=4, 8, 12$), as well as broken valley symmetry QHSs at $ν=0$ and $ν=6$. These results unambiguously show that the quasi-free standing graphene bilayer grown on the Si-face of SiC exhibits Bernal stacking.

cond-mat.mes-hall↗

arXiv2008

Self-consistent analysis of electron-phonon coupling parameters of graphene

We present a self-consistent analysis of the photoemission spectral function A(k, w) of graphene monolayers grown epitaxially on SiC(0001). New information derived from spectral intensity anomalies (in addition to linewidths and peak positions) confirms that sizeable kinks in the electronic dispersion at the Dirac energy ED and near the Fermi level EF arise from many-body interactions, not single-particle effects such as substrate bonding or extra bands. The relative electron-phonon scattering rate from phonons at different energy scales evolves with doping. The electron-phonon coupling strength is extracted and found to be much larger (~3.5-5 times) than predicted.

cond-mat.str-el↗

arXiv2008

Atmospheric pressure graphitization of SiC(0001)- A route towards wafer-size graphene layers

We have investigated epitaxial graphene films grown on SiC(0001) by annealing in an atmosphere of Ar instead of vacuum. Using AFM and LEEM we observe a significantly improved surface morphology and graphene domain size. Hall measurements on monolayer graphene films show a carrier mobility of around 1000 cm^2/Vs at room temperature and 2000 cm^2/Vs at 27K. The growth process introduced here establishes the synthesis of graphene films on a technologically viable basis.

cond-mat.mtrl-sci↗

arXiv2008

Van Hove Singularity and Apparent Anisotropy in the Electron-Phonon Interaction in Graphene

We show that the electron-phonon coupling strength obtained from the slopes of the electronic energy vs. wavevector dispersion relations, as often done in analyzing angle-resolved photoemission data, can differ substantially from the actual electron-phonon coupling strength due to the curvature of the bare electronic bands. This effect becomes particularly important when the Fermi level is close to a van Hove singularity. By performing {\it ab initio} calculations on doped graphene we demonstrate that, while the apparent strength obtained from the slopes of experimental photoemission data is highly anisotropic, the angular dependence of the actual electron-phonon coupling strength in this material is negligible.

cond-mat.mtrl-sci↗

arXiv2007

Morphology of graphene thin film growth on SiC(0001)

Epitaxial films of graphene on SiC(0001) are interesting from a basic physics as well as applications-oriented point of view. Here we study the emerging morphology of in-vacuo prepared graphene films using low energy electron microscopy (LEEM) and angle-resolved photoemission (ARPES). We obtain an identification of single and bilayer of graphene film by comparing the characteristic features in electron reflectivity spectra in LEEM to the PI-band structure as revealed by ARPES. We demonstrate that LEEM serves as a tool to accurately determine the local extent of graphene layers as well as the layer thickness.

cond-mat.mtrl-sci↗

arXiv2007

Scanning tunneling spectroscopy of inhomogeneous electronic structure in monolayer and bilayer graphene on SiC

We present a scanning tunneling spectroscopy (STS) study of the local electronic structure of single and bilayer graphene grown epitaxially on a SiC(0001) surface. Low voltage topographic images reveal fine, atomic-scale carbon networks, whereas higher bias images are dominated by emergent spatially inhomogeneous large-scale structure similar to a carbon-rich reconstruction of SiC(0001). STS spectroscopy shows a ~100meV gap-like feature around zero bias for both monolayer and bilayer graphene/SiC, as well as significant spatial inhomogeneity in electronic structure above the gap edge. Nanoscale structure at the SiC/graphene interface is seen to correlate with observed electronic spatial inhomogeneity. These results are important for potential devices involving electronic transport or tunneling in graphene/SiC.

cond-mat.str-el↗

arXiv2007

Symmetry Breaking in Few Layer Graphene Films

Recently, it was demonstrated that the quasiparticle dynamics, the layer-dependent charge and potential, and the c-axis screening coefficient could be extracted from measurements of the spectral function of few layer graphene films grown epitaxially on SiC using angle-resolved photoemission spectroscopy (ARPES). In this article we review these findings, and present detailed methodology for extracting such parameters from ARPES. We also present detailed arguments against the possibility of an energy gap at the Dirac crossing ED.

cond-mat.str-el↗

arXiv2007

Massive enhancement of electron-phonon coupling in doped graphene by an electronic singularity

The nature of the coupling leading to superconductivity in layered materials such as high-Tc superconductors and graphite intercalation compounds (GICs) is still unresolved. In both systems, interactions of electrons with either phonons or other electrons or both have been proposed to explain superconductivity. In the high-Tc cuprates, the presence of a Van Hove singularity (VHS) in the density of states near the Fermi level was long ago proposed to enhance the many-body couplings and therefore may play a role in superconductivity. Such a singularity can cause an anisotropic variation in the coupling strength, which may partially explain the so-called nodal-antinodal dichotomy in the cuprates. Here we show that the topology of the graphene band structure at dopings comparable to the GICs is quite similar to that of the cuprates and that the quasiparticle dynamics in graphene have a similar dichotomy. Namely, the electron-phonon coupling is highly anisotropic, diverging near a saddle point in the graphene electronic band structure. These results support the important role of the VHS in layered materials and the possible optimization of Tc by tuning the VHS with respect to the Fermi level.

cond-mat.str-el↗

arXiv2006

Interlayer interaction and electronic screening in multilayer graphene

The unusual transport properties of graphene are the direct consequence of a peculiar bandstructure near the Dirac point. We determine the shape of the pi bands and their characteristic splitting, and the transition from a pure 2D to quasi-2D behavior for 1 to 4 layers of graphene by angle-resolved photoemission. By exploiting the sensitivity of the pi bands to the electronic potential, we derive the layer-dependent carrier concentration, screening length and strength of interlayer interaction by comparison with tight binding calculations, yielding a comprehensive description of multilayer graphene's electronic structure.

cond-mat.mtrl-sci↗

arXiv2006

Experimental Determination of the Spectral Function of Graphene

A number of interesting properties of graphene and graphite are postulated to derive from the peculiar bandstructure of graphene. This bandstructure consists of conical electron and hole pockets that meet at a single point in momentum (k) space--the Dirac crossing, at energy $E_{D} = \hbar ω_{D}$. Direct investigations of the accuracy of this bandstructure, the validity of the quasiparticle picture, and the influence of many-body interactions on the electronic structure have not been addressed for pure graphene by experiment to date. Using angle resolved photoelectron spectroscopy (ARPES), we find that the expected conical bands are distorted by strong electron-electron, electron-phonon, and electron-plasmon coupling effects. The band velocity at $E_{F}$ and the Dirac crossing energy $E_{D}$ are both renormalized by these many-body interactions, in analogy with mass renormalization by electron-boson coupling in ordinary metals. These results are of importance not only for graphene but also graphite and carbon nanotubes which have similar bandstructures.

cond-mat.str-el↗