Yuanchang Li

Toward single-layer uniform hexagonal boron nitride-graphene patchworks with zigzag linking edges.

The atomic layer of hybridized hexagonal boron nitride (h-BN) and graphene has attracted a great deal of attention after the pioneering work of P. M. Ajayan et al. on Cu foils because of their unusual electronic properties (Ci, L. J.; et al. Nat. Mater. 2010, 9, 430-435). However, many fundamental issues are still not clear, including the in-plane atomic continuity as well as the edge type at the boundary of hybridized h-BN and graphene domains. To clarify these issues, we have successfully grown a perfect single-layer h-BN-graphene (BNC) patchwork on a selected Rh(111) substrate, via a two-step patching growth approach. With the ideal sample, we convinced that at the in-plane linking interface, graphene and h-BN can be linked perfectly at an atomic scale. More importantly, we found that zigzag linking edges were preferably formed, as demonstrated by atomic-scale scanning tunneling microscopy images, which was also theoretically verified using density functional theory calculations. We believe the experimental and theoretical works are of particular importance to obtain a fundamental understanding of the BNC hybrid and to establish a deliberate structural control targeting high-performance electronic and spintronic devices.

High Detectivity Graphene-Silicon Heterojunction Photodetector.

A graphene/n-type silicon (n-Si) heterojunction has been demonstrated to exhibit strong rectifying behavior and high photoresponsivity, which can be utilized for the development of high-performance photodetectors. However, graphene/n-Si heterojunction photodetectors reported previously suffer from relatively low specific detectivity due to large dark current. Here, by introducing a thin interfacial oxide layer, the dark current of graphene/n-Si heterojunction has been reduced by two orders of magnitude at zero bias. At room temperature, the graphene/n-Si photodetector with interfacial oxide exhibits a specific detectivity up to 5.77 × 10(13) cm Hz(1/2) W(-1) at the peak wavelength of 890 nm in vacuum, which is highest reported detectivity at room temperature for planar graphene/Si heterojunction photodetectors. In addition, the improved graphene/n-Si heterojunction photodetectors possess high responsivity of 0.73 A W(-1) and high photo-to-dark current ratio of ≈10(7) . The current noise spectral density of the graphene/n-Si photodetector has been characterized under ambient and vacuum conditions, which shows that the dark current can be further suppressed in vacuum. These results demonstrate that graphene/Si heterojunction with interfacial oxide is promising for the development of high detectivity photodetectors.

Quasi-Freestanding Monolayer Heterostructure of Graphene and Hexagonal Boron Nitride on Ir(111) with a Zigzag Boundary

In-plane heterostructure of hexagonal boron nitride and graphene (h-BN-G) has become a focus of graphene research owing to its tunable bandgap and intriguing properties. We report herein the synthesis of a quasi-freestanding h-BN-G monolayer heterostructure on a weakly coupled Ir(111) substrate, where graphene and h-BN possess distinctly different heights and surface corrugations. An atomically sharp zigzag type boundary has been found to dominate the patching interface between graphene and h-BN, as evidenced by high-resolution Scanning tunneling microscopy investigation as well as density functional theory calculation. Scanning tunneling spectroscopy studies indicate that the graphene and h-BN tend to exhibit their own intrinsic electronic features near the patching boundary. The present work offers a deep insight into the h-BN-graphene boundary structures both geometrically and electronically together with the effect of adlayer-substrate coupling.

Dirac fermions in strongly bound graphene systems.

It is highly desirable to integrate graphene into existing semiconductor technology, where the combined system is thermodynamically stable yet maintain a Dirac cone at the Fermi level. First-principles calculations reveal that a certain transition metal (TM) intercalated graphene/SiC(0001), such as the strongly bound graphene on SiC with Mn intercalation, could be such a system. Different from freestanding graphene, the hybridization between graphene and Mn/SiC leads to the formation of a dispersive Dirac cone of primarily TM d characters. The corresponding Dirac spectrum is still isotropic, and the transport behavior is nearly identical to that of freestanding graphene for a bias as large as 0.6 V, except that the Fermi velocity is half that of graphene. A simple model Hamiltonian is developed to qualitatively account for the physics of the transfer of the Dirac cone from a dispersive system (e.g., graphene) to an originally nondispersive system (e.g., TM).

Carbon Nanotube Network Embroidered Graphene Films for Monolithic All‐Carbon Electronics

A unique cage growth of graphene is developed by using carbon nanotube (CNT) spider webs as porous templates, resulting in CNT/graphene hybrids with high conductivity and mechanical flexibility. Furthermore, monolithic all-carbon transistors with graphene as active elements and CNT/graphene hybrids as contacts and interconnects are directly formed by chemical synthesis, and flexible all-carbon bioelectronics are subsequently demonstrated for in vivo mapping of cardiac signals.

Sensitivity limits and scaling of bioelectronic graphene transducers.

Semiconducting nanomaterials are being intensively studied as active elements in bioelectronic devices, with the aim of improving spatial resolution. Yet, the consequences of size-reduction on fundamental noise limits, or minimum resolvable signals, and their impact on device design considerations have not been defined. Here, we address these key issues by quantifying the size-dependent performance and limiting factors of graphene (Gra) transducers under physiological conditions. We show that suspended Gra devices represent the optimal configuration for cardiac extracellular electrophysiology in terms of both transducer sensitivity, systematically ~5× higher than substrate-supported devices, and forming tight bioelectronic interfaces. Significantly, noise measurements on free-standing Gra together with theoretical calculations yield a direct relationship between low-frequency 1/f noise and water dipole-induced disorders, which sets fundamental sensitivity limits for Gra devices in physiological media. As a consequence, a square-root-of-area scaling of Gra transducer sensitivity was experimentally revealed to provide a critical design rule for their implementation in bioelectronics.

Two-dimensional metallic tantalum disulfide as a hydrogen evolution catalyst

Two-dimensional metallic transition metal dichalcogenides are emerging as prototypes for uncovering fundamental physical phenomena, such as superconductivity and charge-density waves, as well as for engineering-related applications. However, the batch production of such envisioned transition metal dichalcogenides remains challenging, which has hindered the aforementioned explorations. Herein, we fabricate thickness-tunable tantalum disulfide flakes and centimetre-sized ultrathin films on an electrode material of gold foil via a facile chemical vapour deposition route. Through temperature-dependent Raman characterization, we observe the transition from nearly commensurate to commensurate charge-density wave phases with our ultrathin tantalum disulfide flakes. We have obtained high hydrogen evolution reaction efficiency with the as-grown tantalum disulfide flakes directly synthesized on gold foils comparable to traditional platinum catalysts. This work could promote further efforts for exploring new efficient catalysts in the large materials family of metallic transition metal dichalcogenides, as well as exploiting their applications towards more versatile applications.Metallic transition metal dichalcogenides are important materials for catalysis, but scalable and controllable preparation methods are scarce. Here, the authors synthesize 2H-TaS2 as centimetre-scale films of tunable thickness and show they are an efficient catalyst for hydrogen evolution.

Nanodevices for Cellular Interfaces and Electrophysiological Recording

Advances in nanomaterials and nanotechnologies offer important opportunities for cellular interfaces. This Research News highlights some recent progress on cellular electrophysiology enabled by using nanostructures as active elements of bioelectronic devices. We begin with a brief description of signal transduction mechanism at device-cell interfaces and then explain the challenges of currently available techniques. Next, specific examples with substantial potential in both extracellular and intracellular electrophysiological recording are given to illustrate the remarkable power of nanostructures and their devices. We will conclude with a discussion of some exciting directions that are currently being pursued in flexible, 3D bioelectronics.

Interface engineering of epitaxial graphene on SiC(0001¯) via fluorine intercalation: A first principles study

Our first-principles calculations show that a change of carrier type from electron to hole can be achieved in monolayer epitaxial graphene on SiC(0001¯) by fluorine (F) intercalation. The p-doping level in graphene, however, is not monotonously enhanced as the F coverage increases, and an interesting interface magnetism is observed at the partially passivated interface. Because intercalated F atoms prefer to bond to the substrate than to the graphene, F-intercalation provides a promising way of “interface modulation doping” to tailor the electronic properties of epitaxial graphene on SiC(0001¯) without appreciably degrading its intrinsic high mobility.

Theory of the Dirac half metal and quantum anomalous Hall effect in Mn-intercalated epitaxial graphene

The prospect of a Dirac half metal, a material which is characterized by a bandstructure with a gap in one spin channel but a Dirac cone in the other, is of both fundamental interest and a natural candidate for use in spin-polarized current applications. However, while the possibility of such a material has been reported based on model calculations[H. Ishizuka and Y. Motome, Phys. Rev. Lett. 109, 237207 (2012)], it remains unclear what material system might realize such an exotic state. Using first-principles calculations, we show that the experimentally accessible Mn intercalated epitaxial graphene on SiC(0001) transits to a Dirac half metal when the coverage is > 1/3 monolayer. This transition results from an orbital-selective breaking of quasi-2D inversion symmetry, leading to symmetry breaking in a single spin channel which is robust against randomness in the distribution of Mn intercalates. Furthermore, the inclusion of spin-orbit interaction naturally drives the system into the quantum anomalous Hall (QAH) state. Our results thus not only demonstrate the practicality of realizing the Dirac half metal beyond a toy model but also open up a new avenue to the realization of the QAH effect.