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Joshua A. Robinson

Publications and source records attributed to Joshua A. Robinson.

At least 19 recordsLinked to original sources

Layer-Dependent Interfacial Coupling and Exciton Pinning in WSe2/Graphene Heterostructures

Understanding interfacial interactions in two-dimensional heterostructures is crucial for their implementation in future optoelectronic and quantum technologies. Here, we investigate interactions between WSe2 and graphene by comparing 1-5 layer MOCVD-grown WSe2 on graphene/SiC with exfoliated WSe2 on SiO2/Si using Raman and photoluminescence spectroscopy combined with atomic force microscopy. Growth on graphene induces persistent compressive strain of approximately 0.2% and reduces the interlayer WSe2 distance by 0.11 +/- 0.05 Angstrom. Interfacial disorder is strongest in the WSe2 layer directly contacting graphene, with an effective Urbach energy of approximately 20 meV, decreasing to approximately 16 meV upon addition of a second layer and remaining similar for thicker films. Increasing WSe2 thickness leads to progressive electron transfer from graphene to WSe2, resulting in p-type doping of graphene and n-type doping of WSe2, with the graphene hole density increasing from approximately 0.4 x 10^13 cm^-2 for 1L to 0.8 x 10^13 cm^-2 for 5L. The A- and B-exciton energies of WSe2 remain nearly pinned on graphene, in contrast to their pronounced thickness-dependent shifts on SiO2/Si. We show that this pinning arises primarily from electronic screening and compressive strain, with smaller contributions from charge transfer and modified interlayer coupling. These findings establish graphene as an active interface for controlling excitonic properties in scalable van der Waals heterostructures.

cond-mat.mtrl-sci

Phase-dependent electronic structure of two-dimensional Ag layers at the graphene/SiC interface

Intercalation at the graphene/SiC interface provides a controlled route to stabilize atomically thin layers with properties distinct from their bulk counterparts. In this platform, the structure and stability of the intercalated phase depend sensitively on the defect landscape of the starting substrate. For intercalated two-dimensional silver at the graphene/SiC interface, two phases have been observed: a phase epitaxial to the SiC lattice, Ag$_{(1)}$, readily obtained following the conventional intercalation method under ultra-high-vacuum conditions and extensively characterized, and a more densely packed phase, called Ag$_{(2)}$, which has remained largely unexplored. Here we report an in situ ultra-high-vacuum preparation method of the second phase intercalated at the graphene/SiC interface; this phase previously was prepared via high-pressure confinement heteroepitaxy. Low-energy electron diffraction shows that Ag$_{(2)}$ is rotated by 30 degree relative to the SiC lattice and forms supercells, in contrast to the $(1\times 1)$ epitaxial relation of Ag$_{(1)}$ with SiC. High-resolution angle-resolved photoemission spectroscopy reveals a more rich Ag$_{(2)}$ band dispersion compared to the Ag$_{(1)}$. In density functional theory calculations, by defining the unfolding entropy which, in a quantified way, finds that the band structure of Ag$_{(2)}$ is more suitable to be unfolded to the SiC primitive cell, and the resulting unfolded band dispersion is in great agreement with the experimental data. We further show that the different intercalated Ag phases tune the electronic properties of the overlying quasi-free-standing graphene layer differently: compared with Ag$_{(1)}$, Ag$_{(2)}$ yields an $\sim$1.75 times higher charge carrier density and modifies the charge-plasmon interaction of the graphene layer, indicating a change in effective screening at the interface.

cond-mat.mtrl-sci

Ultra-Confinement of Polaritons in Single Atomic Layer Ag Photonic Quantum Dots

Light scattering by two-dimensional (2D) van der Waals heterostructures (vdWHs) is immense, especially given their infinitesimal volume, thus enabling strong light-matter interactions. Surface 2D polariton waves manifest through large concentration of electromagnetic field in vertical direction, normal to their propagation. By confining vdWH materials into 2D photonic shapes, one can manipulate and compress light in lateral directions. Scattering-type scanning near-field optical microscopy is a perfect tool for direct imaging of the propagating polaritons and studying the properties of confined polaritons in nanostructures. Though, thus far the quantitative analysis, such the wavelength extraction, has been challenged for confined polaritons by incapability of mapping of the wave period on sub-wavelength scale and difficulty of identifying an adequate substrate's "background" to subtract. Here, an analytical approach is developed to reveal the local propagation constant of confined polaritons under abovementioned constraints and map it with the sub-wavelength resolution. Applied to analysis of the SiC/2D-Ag/EG (epitaxial graphene) photonic nanostructures, the technique uncovered that the polaritons are highly confined in both vertical ($\simλ$/50) and lateral directions ($\simλ$/40) by 2D metal.

cond-mat.mtrl-sci

Collective quantum state at the atomic limit

Collective quantum states are often associated with extended systems, where spatially extensive degrees of freedom enable emergent many-body behavior; whether such strongly correlated states survive at atomic dimensions remains a fundamental question. Tomonaga-Luttinger liquids provide a paradigmatic example of one-dimensional collective quantum matter characterized by spin-charge separation. Using low-temperature scanning tunneling microscopy and spectroscopy, we directly visualize quantized collective modes in atomically confined mirror twin boundary segments of monolayer WSe2. Distinct standing-wave branches associated with fractionalized spin and charge excitations persist in segments as short as one nanometer, establishing the atomic-scale confinement limit of Luttinger-liquid behavior. These ultrashort segments form a new class of many-body quantum dots whose discrete spectra arise from confined collective bosonic modes rather than single-particle electron states. When assembled into ordered chains, inter-dot coupling reshapes electron-like fundamental states while collective spin/charge excitations remain largely intact, revealing distinct coupling responses of emergent many-body modes. Our results demonstrate that collective quantum matter can persist and exhibit fundamentally distinct coupling behavior at atomic length scales, establishing a novel platform for engineering strongly correlated quantum phases from atomically confined building blocks.

cond-mat.mes-hall

Ultrafast photo-thermoelectric currents in graphene junctions in the mid-infrared

Graphene is widely recognized for its ultrafast and broadband photocurrent response, but whether the broadband ultrafast characteristics are preserved at mid-infrared wavelengths with photon energies below the optical phonon energy remains an open question. Here, we investigate the carrier dynamics in graphene junctions under mid-infrared excitation using an ultrafast pump-probe photocurrent spectroscopy. We utilize dual split gate devices to demonstrate that the photo-thermoelectric effect can dominate the photoresponse of graphene also for a mid-infrared femtosecond excitation. We observe that graphene retains its broadband photocurrent response in this spectral region, but the photocurrent relaxation time increases from ca. 2 ps below 8-9 micrometer up to 3 ps at longer mid-infrared wavelengths. The absence of a pronounced phonon bottleneck in the decay dynamics at room temperature suggests an efficient interplay of electron-electron and electron-phonon scattering even for photon energies below the optical phonon energy in graphene. The observed wavelength dependence of the photocurrent relaxation times is consistent with energy-dependent theoretical relaxation times as derived from a microscopic transport theory of graphene that includes electron-phonon coupling within a Holstein-Peierls Hamiltonian.

cond-mat.mes-hall

Superconducting Decoherence and Thermal Quenching of the Josephson Diode Effect in Low-Dimensional Josephson Systems

Motivated by recent studies on superconducting (SC) diode nonreciprocity, we uncover a generic smooth SC-phase decoherence mechanism in low-dimensional Josephson structures. Contrary to the conventional single-energy-scale paradigm where Josephson coherence and diode nonreciprocity vanish simultaneously only at the SC gap-closing temperature, we demonstrate, within a fully self-consistent microscopic framework beyond mean-field theory, that SC phase fluctuations generically split these phenomena into distinct energy scales. As a result, rather than a single SC-normal transition, the system exhibits a sequence of distinct thermal crossovers upon heating: the diode effect disappears first at $T_η$, Josephson coherence is subsequently lost at $T_c$, and the SC gap collapses only at a higher temperature $T_s$. Using a bilayer SC system as a concrete example, we show that the separation between these temperature scales is not solely dictated by Josephson coupling, but is instead strongly and counterintuitively shaped by the in-plane disorder and carrier density. These findings reveal that smooth SC phase decoherence introduces a distinct and more fragile energy scale, with potential implications for layered superconductors such as cuprates and recently discovered nickelates, as well as for SC qubit platforms.

cond-mat.supr-con

Large-scale Integration of Experimental and Computational Data for 2D Materials

The past decade has seen rapid growth in the number of experimentally realized two-dimensional (2D) materials with diverse chemical and physical properties. However, information on their crystal structure, synthesis routes, and measured or predicted properties, remains scattered across thousands of publications. Here we consolidate this fragmented knowledge by establishing X2DB - an open infrastructure that integrates experimental and computational data on 2D materials. Using extensive literature mining and direct community uploads, we identify 370 unique 2D materials that have been realized in monolayer or few-layer form, and link them to their digital counterparts in computational databases, enabling consistent ab initio characterization of their properties across monolayer, bilayer and bulk forms. We describe the structure and content of the database highlighting its support for community uploads, illustrate how it can be used to generate new scientific insight and introduce a hierarchical classification of the known set of 2D materials. Our work provides a foundation for the integration and cross-fertilization of experimental and theoretical knowledge, opening new avenues for data-driven, predictive synthesis of novel 2D materials.

cond-mat.mtrl-sci

Ultrafast Band-Gap Renormalization in Bilayer Graphene

We demonstrate, by femtosecond time- and angle-resolved photoemission spectroscopy, that photoinduced interlayer charge transfer in a heterostructure consisting of Bernal-stacked bilayer graphene and a single atomic layer of silver on 6H-SiC(0001) transiently modulates the intrinsic potential landscape across the silver-graphene interface. This acts as an ultrafast optoelectronic gate that drives momentum-dependent band renormalizations, resulting in a transient band-gap opening on femtosecond timescales. Simultaneously, the photogenerated hot-carrier population enhances electronic screening, leading to subsequent closing of the band-gap beyond the thermal equilibrium value. These findings reveal two different mechanisms for photoinduced, reversible control of the electronic band structure in bilayer graphene -- interlayer charge transfer and hot-carrier-enhanced screening -- providing a general framework for the ultrafast control of electronic properties in graphene-based heterostructures. This opens up novel pathways for the realization of ultrafast optoelectronic devices and the exploration of correlated quantum phases in bilayer graphene under non-equilibrium conditions.

cond-mat.mes-hall

Point defects and their dynamic behaviors in silver monolayer intercalated between graphene and SiC

Point defects give rise to sharp modifications in the structures and electronic properties of two-dimensional metals, offering an atomic-level platform for fundamental studies and potential applications. In this work, we investigate atomic-scale defects in a two-dimensional silver monolayer intercalated between epitaxial graphene and SiC using scanning tunneling microscopy. Dark and bright defects are identified as vacancies or substitutional impurities within the silver monolayer, each hosting a localized electronic state. Remarkably, under tunneling electron excitation at negative bias, the bright defects exhibit dynamic behaviors characterized by inelastic switching between two states. The switching can be reversibly controlled by the microscope tip, enabling the defects to function as atomic-scale two-level conductance switches. Analysis of defect switching reveals possible defect origins and the relationship between dark and bright defect species. Our findings establish a pathway to precise manipulation of defects in two-dimensional metals and uncover previously unexplored dynamics with potential use in nanoelectronics.

cond-mat.mes-hall

Two-dimensional Indium Oxide at the Epitaxial Graphene/SiC Interface: Synthesis, Structure, Properties, and Devices

High-quality two-dimensional (2D) dielectrics are crucial for fabricating 2D/3D hybrid vertical electronic devices such as metal-oxide-semiconductor (MOS) based Schottky diodes and hot electron transistors, the production of which is constrained by the scarcity of bulk layered wide bandgap semiconductors. In this research, we present the synthesis of a new 2D dielectric, monolayer InO2, which differs in stoichiometry from its bulk form, over a large area (>300 um2) by intercalating at the epitaxial graphene (EG)/SiC interface. By adjusting the lateral size of graphene through optical lithography prior to the intercalation, we tune the thickness of InO2 where predominantly (~85%) monolayer InO2 is formed. The preference for monolayer formation of InO2 is explained using ReaxFF reactive molecular dynamics and density functional theory (DFT) calculations. Additionally, the band gap of InO2 is calculated to be 4.1 eV, differing from its bulk form (2.7 eV). Furthermore, MOS-based Schottky diode measurements on InO2 intercalated EG/n-SiC demonstrate that the EG/n-SiC junction transforms from ohmic to a Schottky junction upon intercalation, with a barrier height of 0.87 eV and a rectification ratio of ~10^5. These findings introduce a new addition to the 2D dielectric family, showing significant potential for monolayer InO2 to be used as a barrier in vertical electronic devices.

cond-mat.mtrl-sci

Defect-Mediated Phase Engineering of 2D Ag at the Graphene/SiC Interface

Atomically thin silver (Ag) films offer unique opportunities in plasmonic, quantum optics, and energy harvesting, yet conventional growth methods struggle to achieve structural control at the monolayer limit. Here, we demonstrate phase-selective synthesis of large-area, crystalline 2D Ag films via defect-engineered confinement heteroepitaxy (CHet) at the epitaxial graphene/silicon carbide (EG/SiC) interface. By tuning graphene growth and post-growth defect introduction, two distinct Ag phases are achieved with disparate properties: a nearly commensurate Ag(1) lattice stabilized by vacancy and line defects in epitaxial graphene, and a denser Ag(2) phase preferentially grown with sp3-rich zero-layer graphene. Structural and spectroscopic characterization confirm lattice registry with the SiC substrate, while theoretical calculations reveal a thermodynamic preference for Ag(2) but an easier nucleation for Ag(1). Both phases are found to be semiconducting, with the Ag(2) phase exhibiting slightly enhanced n-doping of graphene. Notably, nonlinear optical measurements reveal a three-order magnitude difference in second-order susceptibility between the two phases, demonstrating promise for phase-tunable 2D metals in reconfigurable optoelectronic and metamaterial platforms.

cond-mat.mtrl-sci

Atomically-resolved exciton emission from single defects in MoS$_2$

Understanding how atomic defects shape the nanoscale optical properties of two-dimensional (2D) semiconductors is essential for advancing quantum technologies and optoelectronics. Using scanning tunneling spectroscopy (STS) and luminescence (STML), we correlate the atomic structure and optical fingerprints of individual defects in monolayer MoS$_2$. A bilayer of hexagonal boron nitride (hBN) effectively decouples MoS$_2$ from the graphene substrate, increasing its band gap and extending the defect charge state lifetime. This enables the observation of sharp STML emission lines from MoS$_2$ excitons and trions exhibiting nanoscale sensitivity to local potential fluctuations. We identify the optical signatures of common point defects in MoS$_2$: sulfur vacancies (Vac$_\text{S}^-$), oxygen substitutions (O$_\text{S}$), and negatively charged carbon-hydrogen complexes (CH$_\text{S}^-$). While Vac$_\text{S}^-$ and O$_\text{S}$ only suppress pristine excitonic emission, CH$_\text{S}^-$ generate defect-bound exciton complexes ($A^-X$) about 200\,meV below the MoS$_2$ exciton. Sub-nanometer-resolved STML maps reveal large spectral shifts near charged defects, concurrent with the local band bending expected for band-to-defect optical transitions. These results establish an atomically precise correlation between structure, electronic states, and optical response, enabling deterministic engineering of quantum emitters in 2D materials.

cond-mat.mtrl-sci

First principles and scanning tunneling spectroscopical evidences for thermodynamically stable "on-top" sulfur divacancy in monolayer WS$_{2}$

Chalcogen vacancies in monolayer transition metal dichalcogenides (TMDs), such as WS$_{2}$, play a crucial role in various applications ranging from optoelectronics and catalysis to quantum information science (QIS), making their identification and control essential. This study focuses on WS$_{2}$ single vacancy and vacancy pairs. Using first principles computations, we investigate their thermodynamic stabilities and electronic structures. We identify an "on-top" divacancy configuration where two vacancies sit on top of each other to be the only energetically stable complex with a binding energy of 160 meV. We compute a small difference in electronic structure with a shift of the unoccupied state by 140 meV for the divacancy complex and observe electronic state shift during Scanning Tunneling Spectroscopy of a series of vacancy in WS$_2$ providing spectroscopical evidence for the presence of this defect.

cond-mat.mtrl-sci

Orbital Hybridization-Induced Ising-Type Superconductivity in a Confined Gallium Layer

In low-dimensional superconductors, the interplay between quantum confinement and interfacial hybridization effects can reshape Cooper pair wavefunctions and induce novel forms of unconventional superconductivity. In this work, we employ a plasma-free, carbon buffer layer-assisted confinement epitaxy method to synthesize trilayer gallium (Ga) sandwiched between a graphene layer and a 6H-SiC(0001) substrate, forming an air-stable graphene/trilayer Ga/SiC heterostructure. In this confined light-element Ga layer, we demonstrate interfacial Ising-type superconductivity driven by atomic orbital hybridization between the Ga layer and the SiC substrate. Electrical transport measurements reveal that the in-plane upper critical magnetic field u0Hc2,|| reaches ~21.98T at T=400 mK, approximately 3.38 times the Pauli paramagnetic limit (~6.51T). Angle-resolved photoemission spectroscopy (ARPES) measurements combined with theoretical calculations confirm the presence of split Fermi surfaces with Ising-type spin textures at the K and K' valleys of the confined Ga layer strongly hybridized with SiC. Moreover, by incorporating finite relaxation time induced by impurity scattering into an Ising-type superconductivity model, we reproduce the entire temperature-dependent u0Hc2,|| phase diagram. This work establishes a new strategy to realize unconventional pairing wavefunctions by combining quantum confinement and interfacial hybridization effects in superconducting thin films. It also opens new avenues for designing scalable superconducting quantum electronic and spintronic devices through interfacial engineering.

cond-mat.mes-hall

Vibration-assisted tunneling through single Au adatoms on two-dimensional WSe2

Scanning tunneling microscopy (STM) at 5 K was used to study individual Au atoms adsorbed on the surface of a WSe2 layer grown on epitaxial graphene. In line with theoretical predictions, scanning tunneling spectroscopy measurements reveal that the weakly bound adatom gives rise to an electronic state within the energy band gap of the WSe2 layer. Adatoms in different surface locations show different gap-state energy values that follow a random distribution around the Fermi level of the sample with a standard deviation of ~50 meV. The location-dependent shift is attributed to spatial variations in disorder potential. Tunneling via the gap state is accompanied by vibrational excitations as apparent from pronounced sideband peaks in the conductance spectra with Poisson-distributed intensities indicating significant electron-phonon coupling with a Huang-Rhys factor of S=2.8. STM tunneling through single Au adatoms on two-dimensional WSe2 constitutes a model case of resonant double-barrier tunneling accompanied by strong coupling to vibrational degrees of freedom.

cond-mat.mes-hall

Graphene-driven correlated electronic states in one dimensional defects within WS$_2$

Tomonaga-Luttinger liquid (TLL) behavior in one-dimensional systems has been predicted and shown to occur at semiconductor-to-metal transitions within two-dimensional materials. Reports of one-dimensional defects hosting a Fermi liquid or a TLL have suggested a dependence on the underlying substrate, however, unveiling the physical details of electronic contributions from the substrate require cross-correlative investigation. Here, we study TLL formation within defectively engineered WS$_2$ atop graphene, where band structure and the atomic environment is visualized with nano angle-resolved photoelectron spectroscopy, scanning tunneling microscopy and spectroscopy, and non-contact atomic force microscopy. Correlations between the local density of states and electronic band dispersion elucidated the electron transfer from graphene into a TLL hosted by one-dimensional metal (1DM) defects. It appears that the vertical heterostructure with graphene and the induced charge transfer from graphene into the 1DM is critical for the formation of a TLL.

cond-mat.mtrl-sci

Atomic-scale imaging of graphene nanoribbons on graphene after polymer-free substrate transfer

On-surface synthesis enables the fabrication of atomically precise graphene nanoribbons (GNRs) with properties defined by their shape and edge topology. While this bottom-up approach provides unmatched control over electronic and structural characteristics, integrating GNRs into functional electronic devices requires their transfer from noble metal growth surfaces to technologically relevant substrates. However, such transfers often induce structural modifications, potentially degrading or eliminating GNRs' desired functionality - a process that remains poorly understood. In this study, we employ low-temperature scanning tunneling microscopy and spectroscopy (STM/STS) to characterize 9-atom-wide armchair GNRs (9-AGNRs) following polymer-free wet-transfer onto epitaxial graphene (EG) and quasi-freestanding epitaxial graphene (QFEG) substrates. Our results reveal that armchair GNRs maintain their structural integrity post-transfer, while GNRs with extended or modified edge topologies exhibit significant structural changes, including partial disintegration. Additionally, STS measurements reveal differences in the Fermi level alignment between GNRs and the graphene substrates, a key factor in optimizing carrier injection efficiency in electronic transport devices. This study establishes a framework for detecting post-processing structural modifications in GNRs, which are often hidden in optical ensemble measurements. By addressing the challenges of substrate transfer and providing new insights into GNR-substrate interactions, these findings pave the way for the reliable integration of atomically precise GNRs into next-generation nanoelectronic and optoelectronic devices.

cond-mat.mes-hall

Experimental signature of layer skyrmions and implications for band topology in twisted WSe2 bilayers

Transition metal dichalcogenide (TMD) twisted homobilayers have been established as an ideal platform for studying strong correlation phenomena, as exemplified by the recent discovery of fractional Chern insulator (FCI) states in twisted MoTe2 and Chern insulators (CI) and unconventional superconductivity in twisted WSe2 (tWSe2). In these systems, nontrivial topology in the strongly layer-hybridized regime can arise from a spatial patterning of interlayer tunneling amplitudes and layer-dependent potentials that yields a lattice of layer skyrmions. Here we report on experimental signatures of skyrmion textures in the layer degree of freedom of Rhombohedral-stacked (R-stacked) tWSe2 homobilayers. This observation is based on scanning tunneling spectroscopy that separately resolves the Gamma-valley and K-valley moiré electronic states. We show that Gamma-valley states are subjected to a moiré potential with an amplitude of ~ 120 meV. At ~150 meV above the Gamma-valley, the K-valley states are subjected to a weaker moiré potential of ~30 meV. Most significantly, we reveal opposite layer polarizations of the K-valley at the MX and XM sites within the moiré unit cell, confirming the theoretically predicted layer skyrmion texture. The dI/dV mappings allow the parameters that enter the continuum model of moiré bands in twisted TMD bilayers to be determined experimentally, further establishing a direct correlation between the shape of the LDOS profile in real space and the topology of topmost moiré band.

cond-mat.mes-hall