arXiv subjects

Roland J. Koch

Publications and source records attributed to Roland J. Koch.

At least 19 recordsLinked to original sources

arXiv2024

Large-Area Intercalated 2D-Pb/Graphene Heterostructure as a Platform for Generating Spin-Orbit Torque

A scalable platform to synthesize ultrathin heavy metals may enable high efficiency charge-to-spin conversion for next-generation spintronics. Here we report the synthesis of air-stable, epitaxially registered monolayer Pb underneath bilayer graphene on SiC (0001) by confinement heteroepitaxy (CHet). Diffraction, spectroscopy, and microscopy reveal CHet-based Pb intercalation predominantly exhibits a mottled hexagonal superstructure due to an ordered network of Frenkel-Kontorova-like domain walls. The system's air stability enables ex-situ spin torque ferromagnetic resonance (ST-FMR) measurements that demonstrate charge-to-spin conversion in graphene/Pb/ferromagnet heterostructures with a 1.5x increase in the effective field ratio compared to control samples.

cond-mat.mtrl-sci↗

arXiv2023

Discovery of interlayer plasmon polaron in graphene/WS$_2$ heterostructures

Harnessing electronic excitations involving coherent coupling to bosonic modes is essential for the design and control of emergent phenomena in quantum materials [1]. In situations where charge carriers induce a lattice distortion due to the electron-phonon interaction, the conducting states get "dressed". This leads to the formation of polaronic quasiparticles that dramatically impact charge transport, surface reactivity, thermoelectric and optical properties, as observed in a variety of crystals and interfaces composed of polar materials [2-6]. Similarly, when oscillations of the charge density couple to conduction electrons the more elusive plasmon polaron emerges [7], which has been detected in electron-doped semiconductors [8-10]. However, the exploration of polaronic effects on low energy excitations is still in its infancy in two-dimensional (2D) materials. Here, we present the discovery of an interlayer plasmon polaron in heterostructures composed of graphene on top of SL WS$_2$. By using micro-focused angle-resolved photoemission spectroscopy (microARPES) during in situ doping of the top graphene layer, we observe a strong quasiparticle peak accompanied by several carrier density-dependent shake-off replicas around the SL WS$_2$ conduction band minimum (CBM). Our results are explained by an effective many-body model in terms of a coupling between SL WS$_2$ conduction electrons and graphene plasmon modes. It is important to take into account the presence of such interlayer collective modes, as they have profound consequences for the electronic and optical properties of heterostructures that are routinely explored in many device architectures involving 2D transition metal dichalcogenides (TMDs) [11-15].

cond-mat.mes-hall↗

arXiv2022

Nanoscale view of engineered massive Dirac quasiparticles in lithographic superstructures

Massive Dirac fermions are low-energy electronic excitations characterized by a hyperbolic band dispersion. They play a central role in several emerging physical phenomena such as topological phase transitions, anomalous Hall effects and superconductivity. This work demonstrates that massive Dirac fermions can be controllably induced by lithographically patterning superstructures of nanoscale holes in a graphene device. Their band dispersion is systematically visualized using angle-resolved photoemission spectroscopy with nanoscale spatial resolution. A linear scaling of effective mass with feature sizes is discovered, underlining the Dirac nature of the superstructures. In situ electrostatic doping dramatically enhances the effective hole mass and leads to the direct observation of an electronic band gap that results in a peak-to-peak band separation of (0.64 $\pm$ 0.03) eV, which is shown via first-principles calculations to be strongly renormalized by carrier-induced screening. The presented methodology outlines a new approach for band structure engineering guided by directly viewing structurally- and electrically-tunable massive Dirac quasiparticles in lithographic superstructures at the nanoscale.

cond-mat.mes-hall↗

arXiv2021

Visualizing band structure hybridization and superlattice effects in twisted MoS$_2$/WS$_2$ heterobilayers

A mismatch of atomic registries between single-layer transition metal dichalcogenides (TMDs) in a two dimensional van der Waals heterostructure produces a moiré superlattice with a periodic potential, which can be fine-tuned by introducing a twist angle between the materials. This approach is promising both for controlling the interactions between the TMDs and for engineering their electronic band structures, yet direct observation of the changes to the electronic structure introduced with varying twist angle has so far been missing. Here, we probe heterobilayers comprised of single-layer MoS$_2$ and WS$_2$ with twist angles of $(2.0 \pm 0.5)^{\circ}$, $(13.0 \pm 0.5)^{\circ}$, and $(20.0 \pm 0.5)^{\circ}$ and investigate the differences in their electronic band structure using micro-focused angle-resolved photoemission spectroscopy. We find strong interlayer hybridization between MoS$_2$ and WS$_2$ electronic states at the $\bar{\mathrmΓ}$-point of the Brillouin zone, leading to a transition from a direct bandgap in the single-layer to an indirect gap in the heterostructure. Replicas of the hybridized states are observed at the centre of twist angle-dependent moiré mini Brillouin zones. We confirm that these replica features arise from the inherent moiré potential by comparing our experimental observations with density functional theory calculations of the superlattice dispersion. Our direct visualization of these features underscores the potential of using twisted heterobilayer semiconductors to engineer hybrid electronic states and superlattices that alter the electronic and optical properties of 2D heterostructures.

cond-mat.mtrl-sci↗

arXiv2021

Tunable Two-Dimensional Group-III Metal Alloys

Chemically stable quantum-confined 2D metals are of interest in next-generation nanoscale quantum devices. Bottom-up design and synthesis of such metals could enable the creation of materials with tailored, on-demand, electronic and optical properties for applications that utilize tunable plasmonic coupling, optical non-linearity, epsilon-near-zero behavior, or wavelength-specific light trapping. In this work, we demonstrate that the electronic, superconducting and optical properties of air-stable two-dimensional metals can be controllably tuned by the formation of alloys. Environmentally robust large-area two-dimensional InxGa1-x alloys are synthesized by Confinement Heteroepitaxy (CHet). Near-complete solid solubility is achieved with no evidence of phase segregation, and the composition is tunable over the full range of x by changing the relative elemental composition of the precursor. The optical and electronic properties directly correlate with alloy composition, wherein the dielectric function, band structure, superconductivity, and charge transfer from the metal to graphene are all controlled by the indium/gallium ratio in the 2D metal layer.

cond-mat.mtrl-sci↗

arXiv2021

Correlation-Driven Electron-Hole Asymmetry in Graphene Field Effect Devices

Electron-hole asymmetry is a fundamental property in solids that can determine the nature of quantum phase transitions and the regime of operation for devices. The observation of electron-hole asymmetry in graphene and recently in the phase diagram of bilayer graphene has spurred interest into whether it stems from disorder or from fundamental interactions such as correlations. Here, we report an effective new way to access electron-hole asymmetry in 2D materials by directly measuring the quasiparticle self-energy in graphene/Boron Nitride field effect devices. As the chemical potential moves from the hole to the electron doped side, we see an increased strength of electronic correlations manifested by an increase in the band velocity and inverse quasiparticle lifetime. These results suggest that electronic correlations play an intrinsic role in driving electron hole asymmetry in graphene and provide a new insight for asymmetries in more strongly correlated materials.

cond-mat.mes-hall↗

arXiv2020

Photo-physics and electronic structure of lateral graphene/MoS2 and metal/MoS2 junctions

Integration of semiconducting transition metal dichalcogenides (TMDs) into functional optoelectronic circuitries requires an understanding of the charge transfer across the interface between the TMD and the contacting material. Here, we use spatially resolved photocurrent microscopy to demonstrate electronic uniformity at the epitaxial graphene/molybdenum disulfide (EG/MoS2) interface. A 10x larger photocurrent is extracted at the EG/MoS2 interface when compared to metal (Ti/Au) /MoS2 interface. This is supported by semi-local density-functional theory (DFT), which predicts the Schottky barrier at the EG/MoS2 interface to be ~2x lower than Ti/MoS2. We provide a direct visualization of a 2D material Schottky barrier through combination of angle resolved photoemission spectroscopy with spatial resolution selected to be ~300 nm (nano-ARPES) and DFT calculations. A bending of ~500 meV over a length scale of ~2-3 micrometer in the valence band maximum of MoS2 is observed via nano-ARPES. We explicate a correlation between experimental demonstration and theoretical predictions of barriers at graphene/TMD interfaces. Spatially resolved photocurrent mapping allows for directly visualizing the uniformity of built-in electric fields at heterostructure interfaces, providing a guide for microscopic engineering of charge transport across heterointerfaces. This simple probe-based technique also speaks directly to the 2D synthesis community to elucidate electronic uniformity at domain boundaries alongside morphological uniformity over large areas.

physics.app-ph↗

arXiv2020

Momentum-resolved view of highly tunable many-body effects in a graphene/hBN field-effect device

Integrating the carrier tunability of a functional two-dimensional material electronic device with a direct probe of energy- and momentum-resolved electronic excitations is essential to gain insights on how many-body interactions are influenced during device operation. Here, we use micro-focused angle-resolved photoemission in order to analyze many-body interactions in back-gated graphene supported on hexagonal boron nitride. By extracting the doping-dependent quasiparticle dispersion and self-energy, we observe how these interactions renormalize the Dirac cone and impact the electron mobility of our device. Our results are not only limited to a finite energy range around the Fermi level, as in electron transport measurements, but describe interactions on a much wider energy scale, extending beyond the regime of hot carrier excitations.

cond-mat.mes-hall↗

arXiv2020

How Substitutional Point Defects in Two-Dimensional WS$_2$ Induce Charge Localization, Spin-Orbit Splitting, and Strain

Control of impurity concentrations in semiconducting materials is essential to device technology. Because of their intrinsic confinement, the properties of two-dimensional semiconductors such as transition metal dichalcogenides (TMDs) are more sensitive to defects than traditional bulk materials. The technological adoption of TMDs is dependent on the mitigation of deleterious defects and guided incorporation of functional foreign atoms. The first step towards impurity control is the identification of defects and assessment of their electronic properties. Here, we present a comprehensive study of point defects in monolayer tungsten disulfide (WS$_2$) grown by chemical vapor deposition (CVD) using scanning tunneling microscopy/spectroscopy, CO-tip noncontact atomic force microscopy, Kelvin probe force spectroscopy, density functional theory, and tight-binding calculations. We observe four different substitutional defects: chromium (Cr$_{\text{W}}$) and molybdenum (Mo$_{\text{W}}$) at a tungsten site, oxygen at sulfur sites in both bottom and top layers (O$_{\text{S}}$ top/bottom), as well as two negatively charged defects (CDs). Their electronic fingerprints unambiguously corroborate the defect assignment and reveal the presence or absence of in-gap defect states. The important role of charge localization, spin-orbit coupling, and strain for the formation of deep defect states observed at substitutional defects in WS$_2$ as reported here will guide future efforts of targeted defect engineering and doping of TMDs.

cond-mat.mes-hall↗

arXiv2019

Visualization of the flat electronic band in twisted bilayer graphene near the magic angle twist

Bilayer graphene was theorized to host a moire miniband with flat dispersion if the layers are stacked at specific twist angles known as the magic angles. Recently, such twisted bilayer graphene (tBLG) with the first magic angle twist was reported to exhibit correlated insulating state and superconductivity, where the presence of the flat miniband in the system is thought to be essential for the emergence of these ordered phases in the transport measurements. Tunneling spectroscopy and electronic compressibility measurements in tBLG have revealed a van Hove singularity that is consistent with the presence of the flat miniband. However, a direct observation of the flat dispersion in the momentum-space of such moire miniband in tBLG is still elusive. Here, we report the visualization of the flat moire miniband by using angle-resolved photoemission spectroscopy with nanoscale resolution (nanoARPES). The high spatial resolution in nanoARPES enabled the measurement of the local electronic structure of the tBLG. We clearly demonstrate the existence of the flat moire band near the charge neutrality for tBLG close to the magic angle at room temperature.

cond-mat.mes-hall↗

arXiv2019

Tunable Electronic Structure in Gallium Chalcogenide van der Waals Compounds

Transition metal monochalcogenides comprise a class of two-dimensional materials with electronic band gaps that are highly sensitive to material thickness and chemical composition. Here, we explore the tunability of the electronic excitation spectrum in GaSe using angle-resolved photoemission spectroscopy. The electronic structure of the material is modified by $\textit{in-situ}$ potassium deposition as well as by forming GaS$_{x}$Se$_{1-x}$ alloy compounds. We find that potassium decouples the top-most tetra-layer of the GaSe unit cell, leading to a substantial change of the dispersion around the valence band maximum (VBM). The observed band dispersion of a single tetralayer is consistent with a transition from the direct gap character of the bulk to the indirect gap character expected for monolayer GaSe. Upon alloying with sulfur, we observe a phase transition from AB to $\text{AA}^{\prime}$ stacking. Alloying also results in a rigid energy shift of the VBM towards higher binding energies which correlates with a blue shift in the luminescence. The increase of the band gap upon sulfur alloying does not appear to change the dispersion or character of the VBM appreciably, implying that it is possible to engineer the gap of these materials while maintaining their salient electronic properties.

cond-mat.mes-hall↗

arXiv2019

Large spin-orbit splitting of deep in-gap defect states of engineered sulfur vacancies in monolayer WS2

Structural defects in 2D materials offer an effective way to engineer new material functionalities beyond conventional doping in semiconductors. Specifically, deep in-gap defect states of chalcogen vacancies have been associated with intriguing phenomena in monolayer transition metal dichalcogenides (TMDs). Here, we report the direct experimental correlation of the atomic and electronic structure of a sulfur vacancy in monolayer WS2 by a combination of CO-tip noncontact atomic force microscopy (nc-AFM) and scanning tunneling microscopy (STM). Sulfur vacancies, which are absent in as-grown samples, were deliberately created by annealing in vacuum. Two energetically narrow unoccupied defect states of the vacancy provide a unique fingerprint of this defect. Direct imaging of the defect orbitals by STM and state-of-the-art GW calculations reveal that the large splitting of 252 meV between these defect states is induced by spin-orbit coupling. The controllable incorporation and potential decoration of chalcogen vacancies provide a new route to tailor the optical, catalytic and magnetic properties of TMDs.

cond-mat.mtrl-sci↗

arXiv2019

The Dirac nodal line network in non-symmorphic rutile semimetal RuO$_2$

We employ angle resolved photoemission spectroscopy (ARPES) to investigate the Fermi surface of RuO$_2$. We find a network of two Dirac nodal lines (DNL) as previously predicted in theory, where the valence- and conduction bands touch along continuous lines in momentum space. In addition, we find evidence for a third DNL close to the Fermi level which appears robust despite the presence of significant spin orbit coupling. We demonstrate that the third DNL gives rise to a topologically trivial flat-band surface state (FBSS) at the (110) surface. This FBSS can be tuned by surface doping and presents an interesting playground for the study of surface chemistry and exotic correlation phenomena.

cond-mat.mes-hall↗

arXiv2019

Rigid band shifts in two-dimensional semiconductors through environmental screening

We investigate the effects of environmental dielectric screening on the electronic dispersion and the band gap in the atomically-thin, quasi two-dimensional (2D) semiconductor WS$_2$ using correlative angle-resolved photoemission and optical spectroscopies, along with first-principles calculations. We find the main effect of increased environmental screening to be a reduction of the band gap, with little change to the electronic dispersion of the band structure. These essentially rigid shifts of the bands results from the special spatial structure of the changes in the Coulomb potential induced by the dielectric environment in the 2D limit. Our results suggest dielectric engineering as a non-invasive method of tailoring the band structure of 2D semiconductors and provide guidance for understanding the electronic properties of 2D materials embedded in multilayer heterostructures.

cond-mat.mes-hall↗

arXiv2019

Confinement Heteroepitaxy: Realizing Atomically Thin, Half-van der Waals Materials

Three-dimensional epitaxial heterostructures are based on covalently-bonded interfaces, whereas those from 2-dimensional (2D) materials exhibit van der Waals interactions. Under the right conditions, however, material structures with mixed interfacial van der Waals and covalent bonding may be realized. Atomically thin layers formed at the epitaxial graphene (EG)/silicon carbide (SiC) interface indicate that EG/SiC interfaces provide this unique environment and enable synthesis of a rich palette of 2D materials not accessible with traditional techniques. Here, we demonstrate a method termed confinement heteroepitaxy (CHet), to realize air-stable, structurally unique, crystalline 2D-Ga, In, and Sn at the EG/SiC interface. The first intercalant layer is covalently-bonded to the SiC, and is accompanied by a vertical bonding gradient that ends with van der Waals interactions. Such structures break out of plane centrosymmetry, thereby introducing atomically thin, non-centrosymmetric 2D allotropes of 3D materials as a foundation for tunable superconductivity, topological states, and plasmonic properties.

cond-mat.mtrl-sci↗

arXiv2019

Direct observation of minibands in twisted heterobilayers

Stacking two-dimensional (2D) van der Waals materials with different interlayer atomic registry in a heterobilayer causes the formation of a long-range periodic superlattice that may bestow the heterostructure with exotic properties such as new quantum fractal states [1-3] or superconductivity [4, 5]. Recent optical measurements of transition metal dichalcogenide (TMD) heterobilayers have revealed the presence of hybridized interlayer electron-hole pair excitations at energies defined by the superlattice potential [6-10]. The corresponding quasiparticle band structure, so-called minibands, have remained elusive and no such features have been reported for heterobilayers comprised of a TMD and another type of 2D material. Here, we introduce a new X-ray capillary technology for performing micro-focused angle-resolved photoemission spectroscopy (microARPES) with a spatial resolution on the order of 1 $μ$m, enabling us to map the momentum-dependent quasiparticle dispersion of heterobilayers consisting of graphene on WS$_2$ at variable interlayer twist angles ($θ$). Minibands are directly observed for $θ= 2.5^{\circ}$ in multiple mini Brillouin zones (mBZs), while they are absent for a larger twist angle of $θ= 26.3^{\circ}$. These findings underline the possibility to control quantum states via the stacking configuration in 2D heterostructures, opening multiple new avenues for generating materials with enhanced functionality such as tunable electronic correlations [11] and tailored selection rules for optical transitions [12].

cond-mat.mes-hall↗

arXiv2019

Imaging microscopic electronic contrasts at the interface of single-layer WS$_2$ with oxide and boron nitride substrates

The electronic properties of devices based on two-dimensional materials are significantly influenced by interactions with substrate and electrode materials. Here, we use photoemission electron microscopy to investigate the real- and momentum-space electronic structures of electrically contacted single-layer WS$_2$ stacked on hBN, SiO$_2$ and TiO$_2$ substrates. Using work function and X-ray absorption imaging we single-out clean microscopic regions of each interface type and collect the valence band dispersion. We infer the alignments of the electronic band gaps and electron affinities from the measured valence band offsets of WS$_2$ and the three substrate materials using a simple electron affinity rule and discuss the implications for vertical band structure engineering using mixed three- and two-dimensional materials.

cond-mat.mtrl-sci↗

arXiv2018

Electronic Structure of Exfoliated and Epitaxial Hexagonal Boron Nitride

Hexagonal boron nitride (hBN) is an essential component in van der Waals heterostructures as it provides high quality and weakly interacting interfaces that preserve the electronic properties of adjacent materials. While exfoliated flakes of hBN have been extensively studied using electron transport and optical probes, detailed experimental measurements of the energy- and momentum- dependent electronic excitation spectrum are lacking. Here, we directly determine the full valence band (VB) electronic structure of micron-sized exfoliated flakes of hBN using angle-resolved photoemission spectroscopy with micrometer spatial resolution. We identify the π- and σ-band dispersions, the hBN stacking order and determine a total VB bandwidth of 19.4 eV. We compare these results with electronic structure data for epitaxial hBN on graphene on silicon carbide grown in situ using a borazine precursor. The epitaxial growth and electronic properties are investigated using photoe- mission electron microscopy. Our measurements show that the fundamental electronic properties of hBN are highly dependent on the fabrication strategy.

cond-mat.mtrl-sci↗