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Register a new userBottom up synthesis of multifunctional nanoporous graphene
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Nanosize pores can turn semimetallic graphene into a semiconductor and from being impermeable into the most efficient molecular sieve membrane. However, scaling the pores down to the nanometer, while fulfilling the tight structural constraints imposed by applications, represents an enormous challenge for present top-down strategies. Here we report a bottom-up method to synthesize nanoporous graphene comprising an ordered array of pores separated by ribbons, which can be tuned down to the one nanometer range. The size, density, morphology and chemical composition of the pores are defined with atomic precision by the design of the molecular precursors. Our measurements further reveal a highly anisotropic electronic structure, where orthogonal one-dimensional electronic bands with an energy gap of ~1 eV coexist with confined pore states, making the nanoporous graphene a highly versatile semiconductor for simultaneous sieving and electrical sensing of molecular species.
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Extending chip performance beyond current limits of miniaturisation requires new materials and functionalities that integrate well with the silicon platform. Germanium fits these requirements and has been proposed as a high-mobility channel material,[1] a light emitting medium in silicon-integrated lasers,[2,3] and a plasmonic conductor for bio-sensing.[4,5] Common to these diverse applications is the need for homogeneous, high electron densities in three-dimensions (3D). Here we use a bottom-up approach to demonstrate the 3D assembly of atomically sharp doping profiles in germanium by a repeated stacking of two-dimensional (2D) high-density phosphorus layers. This produces high-density (10^19 to 10^20 cm-3) low-resistivity (10^-4 Ohmcm) metallic germanium of precisely defined thickness, beyond the capabilities of diffusion-based doping technologies.[6] We demonstrate that free electrons from distinct 2D dopant layers coalesce into a homogeneous 3D conductor using anisotropic quantum interference measurements, atom probe tomography, and density functional theory.
We unveil the nature of the structural disorder in bottom-up zigzag graphene nanoribbons along with its effect on the magnetism and electronic transport on the basis of scanning probe microscopies and first-principles calculations. We find that edge-missing m-xylene units emerging during the cyclodehydrogenation step of the on-surface synthesis are the most common point defects. These bite defects act as spin-1 paramagnetic centers, severely disrupt the conductance spectrum around the band extrema, and give rise to spin-polarized charge transport. We further show that the electronic conductance across graphene nanoribbons is more sensitive to bite defects forming at the zigzag edges than at the armchair ones. Our work establishes a comprehensive understanding of the low-energy electronic properties of disordered bottom-up graphene nanoribbons.
Graphene, as a promising material of post-silicon electronics, opens a new paradigm for the novel electronic properties and device applications. On the other hand, the 2D feature of graphene makes it technically challenging to be integrated into 3D transistors with a sufficient processor capacity. Although there are many attempts to assemble 2D graphene into 3D structures, the characteristics of massless Dirac fermions cannot be well preserved in these materials for transistor applications. Here we report a high-performance graphene transistor by utilizing 3D nanoporous graphene which is comprised of an interconnected single graphene sheet and a commodious open porosity to infuse an ionic liquid for a tunable electronic state by applying electric fields. The 3D nanoporous graphene transistor, with high carrier mobility of 5000-7500 cm$^2$V$^{-1}$s$^{-1}$, exhibits two to three orders of magnitude higher electric conductance and capacitance than those of 2D graphene devices, along with preserved ambipolor electronic nature of Dirac cones. Moreover, the 3D graphene networks with Dirac fermions turn out to exhibit a unique nonlinear Hall resistance in a wide range of the gate voltages. The high quality 3D nanoporous graphene EDLT may open a new field for utilizing Dirac fermions in 3D network structures for various fundamental and practical applications.
We synthesized three-dimensional nanoporous graphene films by a chemical vapor deposition method with nanoporous copper as a catalytic substrate. The resulting nanoporous graphene has the same average pore size as the underlying copper substrate. Our surface-enhanced Raman scattering (SERS) investigation indicates that the nanoporosity of graphene significantly improves the SERS efficiency of graphene as a substrate as compared to planar graphene substrates.
We present a novel bottom-up method for the synthesis of functional recursive programs. While bottom-up synthesis techniques can work better than top-down methods in certain settings, there is no prior technique for synthesizing recursive programs from logical specifications in a purely bottom-up fashion. The main challenge is that effective bottom-up methods need to execute sub-expressions of the code being synthesized, but it is impossible to execute a recursive subexpression of a program that has not been fully constructed yet. In this paper, we address this challenge using the concept of angelic semantics. Specifically, our method finds a program that satisfies the specification under angelic semantics (we refer to this as angelic synthesis), analyzes the assumptions made during its angelic execution, uses this analysis to strengthen the specification, and finally reattempts synthesis with the strengthened specification. Our proposed angelic synthesis algorithm is based on version space learning and therefore deals effectively with many incremental synthesis calls made during the overall algorithm. We have implemented this approach in a prototype called Burst and evaluate it on synthesis problems from prior work. Our experiments show that Burst is able to synthesize a solution to 95% of the benchmarks in our benchmark suite, outperforming prior work.
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