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Register a new userVisualizing Individual Nitrogen Dopants in Monolayer Graphene
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In monolayer graphene, substitutional doping during growth can be used to alter its electronic properties. We used scanning tunneling microscopy (STM), Raman spectroscopy, x-ray spectroscopy, and first principles calculations to characterize individual nitrogen dopants in monolayer graphene grown on a copper substrate. Individual nitrogen atoms were incorporated as graphitic dopants, and a fraction of the extra electron on each nitrogen atom was delocalized into the graphene lattice. The electronic structure of nitrogen-doped graphene was strongly modified only within a few lattice spacings of the site of the nitrogen dopant. These findings show that chemical doping is a promising route to achieving high-quality graphene films with a large carrier concentration.
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Low-temperature spin-polarized scanning tunneling microscopy is employed to study spin transport across single Cobalt-Phathalocyanine molecules adsorbed on well characterized magnetic nanoleads. A spin-polarized electronic resonance is identified over the center of the molecule and exploited to spatially resolve stationary spin states. These states reflect two molecular spin orientations and, as established by density functional calculations, originate from a ferromagnetic molecule-lead superexchange interaction mediated by the organic ligands.
We demonstrate electrochemical top gating of graphene by using a solid polymer electrolyte. This allows to reach much higher electron and hole doping than standard back gating. In-situ Raman measurements monitor the doping. The G peak stiffens and sharpens for both electron and hole doping, while the 2D peak shows a different response to holes and electrons. Its position increases for hole doping, while it softens for high electron doping. The variation of G peak position is a signature of the non-adiabatic Kohn anomaly at $Gamma$. On the other hand, for visible excitation, the variation of the 2D peak position is ruled by charge transfer. The intensity ratio of G and 2D peaks shows a strong dependence on doping, making it a sensitive parameter to monitor charges.
Two-dimensional alloys of carbon and nitrogen represent an urgent interest due to prospective applications in nanomechanical and optoelectronic devices. Stability of these chemical structures must be understood as a function of their composition. The present study employs hybrid density functional theory and reactive molecular dynamics simulations to get insights regarding how many nitrogen atoms can be incorporated into the graphene sheet without destroying it. We conclude that (1) C:N=56:28 structure and all nitrogen-poorer structures maintain stability at 1000 K; (2) stability suffers from N-N bonds; (3) distribution of electron density heavily depends on the structural pattern in the N-doped graphene. Our calculations support experimental efforts on the production of highly N-doped graphene and tuning mechanical and optoelectronic properties of graphene.
A finite Schottky barrier and large contact resistance between monolayer MoS2 and electrodes are the major bottlenecks in developing high-performance field-effect transistors (FETs) that hinder the study of intrinsic quantum behaviors such as valley-spin transport at low temperature. A gate-tunable graphene electrode platform has been developed to improve the performance of MoS2 FETs. However, intrinsic misalignment between the work function of pristine graphene and the conduction band of MoS2 results in a large threshold voltage for the FETs, because of which Ohmic contact behaviors are observed only at very high gate voltages and carrier concentrations (~1013 cm-2). Here, we present high-performance monolayer MoS2 FETs with Ohmic contact at a modest gate voltage by using a chemical-vapor-deposited (CVD) nitrogen-doped graphene with a high intrinsic electron carrier density. The CVD nitrogen-doped graphene and monolayer MoS2 hybrid FETs platform exhibited a large negative shifted threshold voltage of -54.2 V and barrier-free Ohmic contact under zero gate voltage. Transparent contact by nitrogen-doped graphene led to a 214% enhancement in the on-current and a four-fold improvement in the field-effect carrier mobility of monolayer MoS2 FETs compared with those of a pristine graphene electrode platform. The transport measurements, as well as Raman and X-ray photoelectron spectroscopy analyses before and after thermal annealing, reveal that the atomic C-N bonding in the CVD nitrogen-doped graphene is responsible for the dominant effects of electron doping. Large-scale nitrogen-doped graphene electrodes provide a promising device platform for the development of high-performance devices and the study of unique quantum behaviors.
The recent demonstration of saturable absorption and negative optical conductivity in the Terahertz range in graphene has opened up new opportunities for optoelectronic applications based on this and other low dimensional materials. Recently, population inversion across the Dirac point has been observed directly by time- and angle-resolved photoemission spectroscopy (tr-ARPES), revealing a relaxation time of only ~ 130 femtoseconds. This severely limits the applicability of single layer graphene to, for example, Terahertz light amplification. Here we use tr-ARPES to demonstrate long-lived population inversion in bilayer graphene. The effect is attributed to the small band gap found in this compound. We propose a microscopic model for these observations and speculate that an enhancement of both the pump photon energy and the pump fluence may further increase this lifetime.
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