Direct Visualization of the Charge Transfer in a Graphene/α-RuCl3 Heterostructure via Angle-Resolved Photoemission Spectroscopy.

We investigate the electronic properties of a graphene and α-ruthenium trichloride (α-RuCl3) heterostructure using a combination of experimental techniques. α-RuCl3 is a Mott insulator and a Kitaev material. Its combination with graphene has gained increasing attention due to its potential applicability in novel optoelectronic devices. By using a combination of spatially resolved photoemission spectroscopy and low-energy electron microscopy, we are able to provide a direct visualization of the massive charge transfer from graphene to α-RuCl3, which can modify the electronic properties of both materials, leading to novel electronic phenomena at their interface. A measurement of the spatially resolved work function allows for a direct estimate of the interface dipole between graphene and α-RuCl3. Their strong coupling could lead to new ways of manipulating electronic properties of a two-dimensional heterojunction. Understanding the electronic properties of this structure is pivotal for designing next generation low-power optoelectronics devices.

Ultrasharp Lateral p-n Junctions in Modulation-Doped Graphene.

We demonstrate ultrasharp (≲10 nm) lateral p-n junctions in graphene using electronic transport, scanning tunneling microscopy, and first-principles calculations. The p-n junction lies at the boundary between differentially doped regions of a graphene sheet, where one side is intrinsic and the other is charge-doped by proximity to a flake of α-RuCl3 across a thin insulating barrier. We extract the p-n junction contribution to the device resistance to place bounds on the junction width. We achieve an ultrasharp junction when the boundary between the intrinsic and doped regions is defined by a cleaved crystalline edge of α-RuCl3 located 2 nm from the graphene. Scanning tunneling spectroscopy in heterostructures of graphene, hexagonal boron nitride, and α-RuCl3 shows potential variations on a sub 10 nm length scale. First-principles calculations reveal that the charge-doping of graphene decays sharply over just nanometers from the edge of the α-RuCl3 flake.

Modulation Doping via a Two-Dimensional Atomic Crystalline Acceptor.

Two-dimensional nanoelectronics, plasmonics, and emergent phases require clean and local charge control, calling for layered, crystalline acceptors or donors. Our Raman, photovoltage, and electrical conductance measurements combined with ab initio calculations establish the large work function and narrow bands of α-RuCl3 enable modulation doping of exfoliated single and bilayer graphene, chemical vapor deposition grown graphene and WSe2, and molecular beam epitaxy grown EuS. We further demonstrate proof of principle photovoltage devices, control via twist angle, and charge transfer through hexagonal boron nitride. Short-ranged lateral doping (≤65 nm) and high homogeneity are achieved in proximate materials with a single layer of α-RuCl3. This leads to the best-reported monolayer graphene mobilities (4900 cm2/(V s)) at these high hole densities (3 × 1013 cm-2) and yields larger charge transfer to bilayer graphene (6 × 1013 cm-2).

Optically Driven Magnetic Phase Transition of Monolayer RuCl3.

Strong light-matter interactions within nanoscale structures offer the possibility of optically controlling material properties. Motivated by the recent discovery of intrinsic long-range magnetic order in two-dimensional materials, which allow for the creation of novel magnetic devices of unprecedented small size, we predict that light can couple with magnetism and efficiently tune magnetic orders of monolayer ruthenium trichloride (RuCl3). First-principles calculations show that both free carriers and optically excited electron-hole pairs can switch monolayer RuCl3 from a proximate spin-liquid phase to a stable ferromagnetic phase. Specifically, a moderate electron-hole pair density (on the order of 1 × 1013 cm-2) can significantly stabilize the ferromagnetic phase by 10 meV/f.u. in comparison to the competing zigzag phase, so that the predicted ferromagnetism can be driven by optical pumping experiments. Analysis shows that this magnetic phase transition is driven by a combined effect of doping-induced lattice strain and itinerant ferromagnetism. According to Ising-model calculations, we find that the Curie temperature of the ferromagnetic phase can be increased significantly by raising carrier or electron-hole pair density. This enhanced optomagnetic effect opens new opportunities to manipulate two-dimensional magnetism through noncontact, optical approaches.

Many-Particle Effects in the Cyclotron Resonance of Encapsulated Monolayer Graphene.

We study the infrared cyclotron resonance of high-mobility monolayer graphene encapsulated in hexagonal boron nitride, and simultaneously observe several narrow resonance lines due to interband Landau-level transitions. By holding the magnetic field strength B constant while tuning the carrier density n, we find the transition energies show a pronounced nonmonotonic dependence on the Landau-level filling factor, ν∝n/B. This constitutes direct evidence that electron-electron interactions contribute to the Landau-level transition energies in graphene, beyond the single-particle picture. Additionally, a splitting occurs in transitions to or from the lowest Landau level, which is interpreted as a Dirac mass arising from coupling of the graphene and boron nitride lattices.

Isotope engineering for spin defects in van der Waals materials.

Spin defects in van der Waals materials offer a promising platform for advancing quantum technologies. Here, we propose and demonstrate a powerful technique based on isotope engineering of host materials to significantly enhance the coherence properties of embedded spin defects. Focusing on the recently-discovered negatively charged boron vacancy center ([Formula: see text]) in hexagonal boron nitride (hBN), we grow isotopically purified h10B15N crystals. Compared to [Formula: see text] in hBN with the natural distribution of isotopes, we observe substantially narrower and less crowded [Formula: see text] spin transitions as well as extended coherence time T2 and relaxation time T1. For quantum sensing, [Formula: see text] centers in our h10B15N samples exhibit a factor of 4 (2) enhancement in DC (AC) magnetic field sensitivity. For additional quantum resources, the individual addressability of the [Formula: see text] hyperfine levels enables the dynamical polarization and coherent control of the three nearest-neighbor 15N nuclear spins. Our results demonstrate the power of isotope engineering for enhancing the properties of quantum spin defects in hBN, and can be readily extended to improving spin qubits in a broad family of van der Waals materials.

Coherent dynamics of strongly interacting electronic spin defects in hexagonal boron nitride.

Optically active spin defects in van der Waals materials are promising platforms for modern quantum technologies. Here we investigate the coherent dynamics of strongly interacting ensembles of negatively charged boron-vacancy ([Formula: see text]) centers in hexagonal boron nitride (hBN) with varying defect density. By employing advanced dynamical decoupling sequences to selectively isolate different dephasing sources, we observe more than 5-fold improvement in the measured coherence times across all hBN samples. Crucially, we identify that the many-body interaction within the [Formula: see text] ensemble plays a substantial role in the coherent dynamics, which is then used to directly estimate the concentration of [Formula: see text]. We find that at high ion implantation dosage, only a small portion of the created boron vacancy defects are in the desired negatively charged state. Finally, we investigate the spin response of [Formula: see text] to the local charged defects induced electric field signals, and estimate its ground state transverse electric field susceptibility. Our results provide new insights on the spin and charge properties of [Formula: see text], which are important for future use of defects in hBN as quantum sensors and simulators.

Design and optimization of thin-film tungsten (W)-diamond target for multi-pixel X-ray sources.

BACKGROUND: Emerging multi-pixel X-ray source technology enables new designs for X-ray imaging systems. The power of multi-pixel X-ray sources with a fixed anode is limited by focal spot power density. PURPOSE: The purpose of this study is to optimize the W-diamond target and predict its performance in multi-pixel X-ray sources. METHODS: X-ray intensity and energy deposition in the W-diamond target with different thicknesses of tungsten film and incident electron energies was calculated with the Geant4 Monte Carlo toolkit. COMSOL Multiphysics software was used to analyze the transient and stationary heat transfer in the thin-film W-diamond target. The maximum tube power and X-ray output intensity were predicted for both transmission and reflection target configurations. RESULTS: The maximum focal spot power density was limited by either the graphitization of the diamond substrate or the melting point of the W target. With optimal W-target thickness, the maximum transmission X-ray intensities are about 40%-50% higher than the maximum reflection intensities. Thin-film W-diamond targets allow four to five times more maximum power input and produce six to seven times higher transmission X-ray intensity in continuous mode compared with conventional reflection W thick targets. Depending on the focal spot size, reducing the X-ray pulse duration can further enhance the tube power. CONCLUSIONS: Multi-pixel X-ray sources using this W-diamond target design can produce significantly higher X-ray output than traditional thick tungsten targets without major modification of the tube design.

Electronic transport properties of a lithium-decorated ZrTe5 thin film.

Through a combination of single crystal growth, experiments involving in situ deposition of surface adatoms, and complimentary modeling, we examine the electronic transport properties of lithium-decorated ZrTe5 thin films. We observe that the surface states in ZrTe5 are robust against Li adsorption. Both the surface electron density and the associated Berry phase are remarkably robust to adsorption of Li atoms. Fitting to the Hall conductivity data reveals that there exist two types of bulk carriers: those for which the carrier density is insensitive to Li adsorption, and those whose density decreases during initial Li depositions and then saturates with further Li adsorption. We propose this dependence is due to the gating effect of a Li-adsorption-generated dipole layer at the ZrTe5 surface.

Observation of anomalous phonon softening in bilayer graphene.

The interaction of electron-hole pairs with lattice vibrations exhibits a wealth of intriguing physical phenomena such as the renowned Kohn anomaly. Here we report the observation in bilayer graphene of an unusual phonon softening that provides the first experimental proof for another type of phonon anomaly. Similar to the Kohn anomaly, which is a logarithmic singularity in the phonon group velocity [W. Kohn, Phys. Rev. Lett. 2, 393 (1959)], the observed phonon anomaly exhibits a logarithmic singularity in the optical-phonon energy. Arising from a resonant electron-phonon coupling effect, the anomaly was also expected, albeit not observed, in monolayer graphene. We propose an explanation for why it is easier to observe in bilayer samples.