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Abstract The capability to structure two-dimensional materials (2DMs) at the nanoscale with customizable patterns and over large areas is critical for a number of emerging applications, from nanoelectronics to 2D photonic metasurfaces. However, current technologies, such as photo- and electron-beam lithography, often employing masking layers, can significantly contaminate the materials. Large-area chemical vapour deposition-grown graphene is known to have non-ideal properties already due to surface contamination resulting from the transferring process. Additional contamination through the lithographic process might thus reduce the performance of any device based on the structured graphene. Here, we demonstrate a contactless chemical-free approach for simultaneous patterning and cleaning of self-supporting graphene membranes in a single step. Using energetic ions passing through a suspended mask with pre-defined nanopatterns, we deterministically structure graphene with demonstrated feature size of 15 nm, approaching the performance of small-area focused ion beam techniques and extreme ultraviolet lithography. Our approach, however, requires only a broad beam, no nanoscale beam positioning and enables large area patterning of 2DMs. Simultaneously, in regions surrounding the exposed areas, contaminations commonly observed on as-grown graphene targets, are effectively removed. This cleaning mechanism is attributed to coupling of surface diffusion and sputtering effects of adsorbed surface contaminants. For applications using 2DMs, this simultaneous patterning and cleaning mechanism may become essential for preparing the nanostructured materials with improved cleanliness and hence, quality.

Graphene-based thermal rectification was investigated by measuring the thermal transport properties of asymmetric suspended graphene nanomesh devices. A sub-10 nm periodic nanopore phononic crystal structure was successfully patterned on the half area of the suspended graphene ribbon by helium ion beam milling technology. The ‘differential thermal leakage’ method was developed for thermal transport measurement without disturbance from the leakage of electron current through the suspended graphene bridge. A thermal rectification ratio of up to 60% was observed in a typical device with a nanopore pitch of 20 nm. By increasing the nanopore pitch in a particular range, the thermal rectification ratio showed an increment. However, this ratio was degraded by increasing the environmental temperature. This experiment suggests a promising way to develop a high-performance thermal rectifier by using a phononic crystal to introduce asymmetry on homogeneous material.

The purification and separation technologies are of great importance to industry and agriculture in modern society. Two-dimensional (2D) crystals emerge as superior membrane materials showing desirable molecular permeability and selectivity. Among them, 2D materials with a nanomesh structure show the greatest potential in molecular transport and separation. Here, we highlight the recent theoretical progresses in molecular transport across 2D graphdiyne membrane with the nanomesh structure. Firstly, the nonlinear and activated water flow were demonstrated through the graphdiyne membranes under external hydrostatic pressure. Then, the superior proton conductivity and perfect selectivity were shown for graphdiyne membrane at ambient conditions. Lastly, graphdiyne was shown to exhibit perfect small gas molecule permeability and selectivity at the atmospheric conditions. The mechanisms for molecular transport and selectivity are also discussed.

The development of high-efficiency and stable electrocatalysts is significant for energy conversion and storage. The oxygen evolution reaction (OER), a pivotal half reaction, is seriously limited in its practical applications due to its sluggish kinetics and thus an excellent electrocatalyst for OER is urgently required. In this paper, we design a novel Co3O4 nanomesh (Co3O4 NMs) with high density grain boundaries (GBs), which functions as a highly efficient and steady OER electrocatalyst. The optimal Co3O4 NMs-500 can achieve a low overpotential of 295 mV at a current density of 10 mA cm-2, and a small Tafel slope of 31 mV dec-1, which exceeds the commercial Ir/C, as well as the majority of other catalysts reported in the literature. The Co3O4 NMs-500 also exhibit promising durability, with a negligible decline in activity after 18 h of operation. Detailed studies indicate that the presence of GBs leads to more exposed active sites and the enhanced adsorption of intermediate species on Co3O4 NMs-500, thereby improving the OER's catalytic activity. This work not only relates to the activity-GBs relationship, but also opens up a unique perspective for the design of the next generation of electrocatalysts.

Flexible photodetector shows great potential applications in intelligent wearable devices, health monitoring, and biological sensing. In this work, single crystal β-tellurium nanowires were grown on flexible muscovite by molecular beam epitaxy, constructing high-density ordered nanomesh structure. The prepared photodetectors based on tellurium nanomesh exhibit excellent mechanical flexibility, fast response in a broad range from ultraviolet to near-infrared, and good photosensitivity. We found that the flexible photodetectors with Shottky contact drastically suppressed dark current, while the response speed was lowered in comparison to the devices with ohmic contact, as holes would take a long time to tunnel through the Shottky barrier between metal and p-type Te. Moreover, the photoresponse of flexible Shottky photodetectors can be modulated by piezoelectricity of tellurium, and pronounced photocurrent increase after bending many times. Under external stress, polarization charges could tune Shottky barrier height of the metal/tellurium, resulting in variation of photocurrent. This research not only explores the broadband photoresponse and piezoelectric effect of tellurium nanomesh, but also promotes the integration and development of broadband flexible optoelectronic devices.

One-dimensional (1D) and three-dimensional (3D) residue-free metal oxide patterns are directly fabricated over large areas using liquid transfer imprint lithography (LTIL) with an ultraviolet-curable metal oxide precursor resist. A 1D line or pillar array of metal oxides nano-patterns without a residual layer is formed by LTIL and annealing processes. A 3D layer-by-layer nanomesh structure is successfully constructed by repeating the LTIL method without a complex etching process. In addition, it is possible to form a hierarchical structure in which zinc oxide nanowires are selectively grown on a desired zinc oxide (ZnO) seed pattern formed by LTIL via a hydrothermal method. Unlike the pattern fabricated by the conventional nanoimprint lithography method, in the case of the pattern formed by LTIL the residues accumulated between the patterns during the patterning procedure can be removed, and thus it is possible to easily form various types of nanostructures.

Well-ordered two-dimensional functional nanostructure arrays have a broad range of potential applications in molecular electronics, ultra-high density data storage, biosensors, single-electron, single-photon and quantum computation devices. Various surface nanotemplates that are naturally or artificially patterned at the nanometre scale have been used to guide the formation of highly periodic nanostructure arrays. In this paper, we review recent progress in the development of various surface nanotemplates as well as the self-assembly of nanostructures on them, with particular emphasis on the unique SiC nanomesh template. The formation mechanism of this nanomesh template is attributed to the self-assembly of accumulated carbon atoms into well-ordered honeycomb superstructures at the nanometre scale on the 6H?SiC(0?0?0?1) surface. The size and spacing of unit cells of the SiC nanomesh can be tailored in the 2?2.5?nm range by adjusting the annealing time. This nanomesh is demonstrated to be an effective template for the formation of well-ordered molecular arrays of copper(II) phthalocyanine (CuPc). The growth of C60 on the nanomesh follows a typical Stranski?Krastanov mode, and a complete C60 wetting monolayer can be epitaxially grown on this nanotemplate. It is effective in isolating metal nanoclusters, resulting in the formation of monodispersed Co nanoclusters with a narrow size distribution. The adsorption and desorption of Co nanoclusters and C60 do not change its atomic structure, making it a chemically and thermally stable nanotemplate for the formation of well-ordered nanostructures arrays as well as monodispersed metal nanoclusters.

Precise and periodic structure can be formed on and inside materials by interfering femtosecond laser processing. In this method, laser ablation or modification is induced according to the interference pattern. In our technique, this method is applied to thin film processing, and nano-sized structures such as nanobumps, nanomeshs, and nanobelts. Nanobump array structure can be formed by periodic thermal processes induced by a single shot of interfering laser. Field emission from a nanobump array was demonstrated. By processing at relatively higher fluence, a grating, a circular or a ellipsoidal hole array structure can be generated according to the number of beams. By exfoliating the structures, nanobelt or nanomesh structure can be generated. This is a top-down technique for the generation of new nanomaterials.

Based on the detailed first-principles calculations, we have carefully investigated the defect induced band splitting and its combination with Dirac cone move in bandgap opening. The uniaxial strain can split the π-like bands into π a and π z bands with energy interval E strain to shift the Dirac cone. Also, the inversion symmetry preserved antidot can split π a (π z) into π a1 and π a2 (π z1 and π z2) bands with energy interval E defect to open bandgap in the nanomesh with Γ as four-fold degenerate Dirac point according to the band-folding analysis. Though the E defect would keep almost unaffected, the E strain would be increased by enhancing the uniaxial strain to continuously tune the gap width. Then the bandgap can be reversibly switched on/off. Our studies of the inversion symmetry preserved nanomesh show distinct difference in bandgap opening mechanism as compared to the one by breaking the sublattice equivalence in the (GaAs)6 nanoflake patterned nanomesh. Here, the π-band gap remains almost unchanged against strain enhancing.

Graphene nanomeshes (GNMs), new graphene nanostructures with tunable bandgaps, are potential building blocks for future electronic or photonic devices, and energy storage and conversion materials. In previous works, GNMs have been successfully prepared on Cu foils by the H2 etching effect. In this paper, we investigated the effect of Ar on the preparation of GNMs, and how the mean density and shape of them vary with growth time. In addition, scanning electron microscopy (SEM) and high resolution transmission electron microscopy (TEM) revealed the typical hexagonal structure of GNM. Atomic force microscopy (AFM) and x-ray photoelectron spectroscopy (XPS) indicated that large copper oxide nanoparticles produced by oxidization in purified Ar can play an essential catalytic role in preparing GNMs. Then, we exhibited the key reaction details for each growth process and proposed a growth mechanism of GNMs in purified Ar.

We report on the observation of an unexpected sudden increase of resistance in bilayer graphene nanomesh (GNM) in the temperature range 270 ∼ 300 K that is strongly dependent on the magnetic field strength. We conjecture that the sharp increase in resistance originates from ripple scattering as induced by substrate roughness. The observed result is evidence of extrinsic corrugation in bilayer GNM as an additional scattering source that contributes to significant resistance. The observed weak localization in the GNM indicates intervalley scattering induced by lattice defects acts as resonant scatterers attribute to the high D peak. Magnetotransport measurement strongly supports that the charge inhomogeneity related to the intrinsic disorder in bilayer GNM and the positive magnetoresistance shows a linear behavior with magnetic field strength. Potentially, the observed phenomena, therefore, point to a clear pathway towards practical application of bilayer GNM and to the design of a graphene magnetic sensor that can be manipulated by a magnetic field and a new generation of spintronics.

We report a transparent conductor based on Al nanomesh, which was fabricated through Al anodization and etching processes. The Al anodization was performed at low temperature condition to slow down the anodization rate to achieve the well-controlled thickness of an Al nanomesh. By careful controlling of the anodization process, we can fabricate Al nanomesh transparent conductors with different sheet resistance and optical transparency in the visible spectrum range. We shall show that Al nanomesh transparent conductor is a strong contender for a transparent conductor dominated by ITO.

We study several graphene devices able to generate non-linear effects in the current–voltage characteristics and in particular negative differential resistance (NDR) effects. This theoretical investigation is based on numerical charge transport simulation in the Green’s function approach applied to a tight-binding Hamiltonian for particles in graphene. Depending on the device, the physical mechanism involved in the NDR effect may be different: (i) the mismatch of modes between left and right sides of a P + /P zigzag ribbon junction, (ii) the modulation of interband tunnelling in P/N junctions (tunnel diodes and tunnel field-effect transistors) or (iii) the modulation of chiral tunnelling in ‘conventional’ graphene transistors. We emphasize the advantages of exploiting different approaches of bandgap engineering in the form of graphene nanoribbons (GNRs) or nanomesh lattices (GNM), the latter resulting from a periodic array of nanoholes in graphene sheets. In particular, such nanostructuring allows us to design position-dependent bandgaps in devices, which is shown to make possible the optimization of device operation and, here, to get very high peak-to-valley ratio of the NDR. In the case of GNR nanostructuring, it is shown that appropriate bandgap engineering can even make the current–voltage characteristics of tunnel diodes weakly sensitive to the atomic edge disorder. Finally, GNM lattices are shown to be a very promising way to open large bandgaps in wide sheets of graphene and to introduce bandgaps locally with a view to optimizing the device operation and performance. (Some figures may appear in colour only in the online journal)

Directed self-assembly of a block copolymer is successfully employed to fabricate device-oriented graphene nanostructures from CVD grown graphene. We implemented mussel-inspired polydopamine adhesive in conjunction with the graphoepitaxy principle to tailor graphene nanoribbon arrays and a graphene nanomesh located between metal electrodes. Polydopamine adhesive was utilized for facile and damage-free surface treatment to complement the low surface energy of pristine graphene. Our process minimizes the damage to the ideal graphitic structures and electrical properties of graphene during the nanopatterning process. Multi-channel graphene nanoribbon arrays and a graphene nanomesh were successfully fabricated between metal electrodes.

Since ancient times, pure carbon materials have been familiar in human society—not only diamonds in jewellery and graphite in pencils, but also charcoal and coal which have been used for centuries as fuel for living and industry. Carbon fibers are stronger, tougher and lighter than steel and increase material efficiency because of their lower weight. Today, carbon fibers and related composite materials are used to make the frames of bicycles, cars and even airplane parts. The two-dimensional allotrope, now called graphene, is just a single layer of carbon atoms, locked together in a strongly bonded honeycomb lattice. In plane, graphene is stiffer than diamond, but out-of-plane it is soft, like rubber. It is virtually invisible, may conduct electricity (heat) better than copper and weighs next to nothing. Carbon compounds with two carbon atoms as a base, such as graphene, graphite or diamond, have isoelectronic sister compounds made of boron–nitrogen pairs: hexagonal and cubic boron nitride, with almost the same lattice constant. Although the two 2D sisters, graphene and h-BN, have the same number of valence electrons, their electronic properties are very different: freestanding h-BN is an insulator, while charge carriers in graphene are highly mobile. The past ten years have seen a great expansion in studies of single-layer and few-layer graphene. This activity has been concerned with the π electron transport in graphene, in electric and magnetic fields. More than 30 years ago, however, single-layer graphene and h-BN on solid surfaces were widely investigated. It was noted that they drastically changed the chemical reactivity of surfaces, and they were known to 'poison' heterogeneous catalysts, to passivate surfaces, to prevent oxidation of surfaces and to act as surfactants. Also, it was realized that the controlled growth of h-BN and graphene on substrates yields the formation of mismatch driven superstructures with peculiar template functionality on the nanometer scale. This special section contains interesting papers on graphene, h-BN and related 'honeycomb' compounds on solid surfaces, which are currently in development. Interfacial interaction strongly modifies the electronic and atomic structures of these overlayer systems and substrate surfaces. In addition, one can recognize a variety of growth phenomena by changing the surface and growth conditions, which are promising as regards fabricating those noble nanosystems. We have great pleasure in acknowledging the enthusiastic response and participation of our invited authors and their diligent preparation of the manuscripts. Ultrathin layers of graphene, h-BN and other honeycomb structures contents Ultrathin layers of graphene, h-BN and other honeycomb structuresThomas Geber and Chuhei Oshima Templating of arrays of Ru nanoclusters by monolayer graphene/Ru Moires with different periodicitiesEli Sutter, Bin Wang, Peter Albrecht, Jayeeta Lahiri, Marie-Laure Bocquet and Peter Sutter Controllable p-doping of graphene on Ir(111) by chlorination with FeCl3N A Vinogradov, K A Simonov, A V Generalov, A S Vinogradov, D V Vyalikh, C Laubschat, N Martensson and A B Preobrajenski Optimizing long-range order, band gap, and group velocities for graphene on close-packed metal surfacesF D Natterer, S Rusponi, M Papagno, C Carbone and H Brune Epitaxial growth of graphene on transition metal surfaces: chemical vapor deposition versus liquid phase depositionSamuel Grandthyll, Stefan Gsell, Michael Weinl, Matthias Schreck, Stefan Hufner and Frank Muller High-yield boron nitride nanosheets from 'chemical blowing': towards practical applications in polymer compositesXuebin Wang, Amir Pakdel, Chunyi Zhi, Kentaro Watanabe, Takashi Sekiguchi, Dmitri Golberg and Yoshio Bando BCx layers with honeycomb lattices on an NbB2(0001) surfaceChuhei Oshima Epitaxial growth of boron-doped graphene by thermal decomposition of B4CWataru Norimatsu, Koichiro Hirata, Yuta Yamamoto, Shigeo Arai and Michiko Kusunoki Mechanical exfoliation of epitaxial graphene on Ir(111) enabled by Br2 intercalationCharlotte Herbig, Markus Kaiser, Nedjma Bendiab, Stefan Schumacher, Daniel F Forster, Johann Coraux, Klaus Meerholz, Thomas Michely and Carsten Busse Low energy electron microscopy and photoemission electron microscopy investigation of grapheneK L Man and M S Altman Periodic overlayers and moire patterns: theoretical studies of geometric propertiesKlaus Hermann Silicene structures on silver surfacesHanna Enriquez, Sebastien Vizzini, Abdelkader Kara, Boubekeur Lalmi and Hamid Oughaddou Contrast inversion of the h-BN nanomesh investigated by nc-AFM and Kelvin probe force microscopyS Koch, M Langer, S Kawai, E Meyer and Th Glatzel Probing the electronic structure and optical response of a graphene quantum disk supported on monolayer grapheneWu Zhou, Stephen J Pennycook and Juan-Carlos Idrobo Multi-oriented moire superstructures of graphene on Ir(111): experimental observations and theoretical modelsLei Meng, Rongting Wu, Lizhi Zhang, Linfei Li, Shixuan Du, Yeliang Wang and H-J Gao The physics of epitaxial graphene on SiC(0001)H Kageshima, H Hibino and S Tanabe

Using atomistic quantum simulation based on a tight binding model, we have investigated the transport characteristics of graphene nanomesh-based devices and evaluated the possibilities of observing negative differential conductance. It is shown that by taking advantage of bandgap opening in the graphene nanomesh lattice, a strong negative differential conductance effect can be achieved at room temperature in pn junctions and n-doped structures. Remarkably, the effect is improved very significantly (with a peak-to-valley current ratio of a few hundred) and appears to be weakly sensitive to the transition length in graphene nanomesh pn hetero-junctions when inserting a pristine (gapless) graphene section in the transition region between n and p zones. The study therefore suggests new design strategies for graphene electronic devices which may offer strong advantages in terms of performance and processing over the devices studied previously.

Despite the small or near-zero Seebeck coefficient of metallic nanotubes, a nanotube film can be readily scaled up in length. Thus so can its thermoelectric power. In this work, we inserted a nanomesh pattern into a carbon nanotube film by using an anodized aluminum oxide membrane as an etching mask. We found that by patterning densely packed nanoscale holes into the nanotube film, its total thermoelectric power can be further increased, by as much as 30% (from 29 to 39 μV K(-1)). We present this finding, attributed to electron localization due to nanopatterning, as indicative of the potential of a new degree of freedom.

A novel transparent aluminum nanomesh electrode with nanoapartures smaller than the wavelength of the light was proposed. Unlike conventional conducting oxides such as indium tin oxide, it has the potential to realize a rare-metal-free and low-resistivity transparent electrode. It was fabricated by nanopatterning with our embedded particle monolayer method, which enables the formation of a self-assembled particle monolayer over a large area, and its optical properties were investigated. As a result, the transmittance of the fabricated aluminum nanomesh electrode was found to be more than 55% at the peak wavelength when the opening ratio was 47%.

Researchers have made extensive efforts to mimic or reverse-engineer in vivo neural circuits using micropatterning technology. Various surface chemical cues or topographical structures have been proposed to design neuronal networks in vitro. In this paper, we propose a carbon nanotube (CNT)-based network engineering method which naturally mimics the structure of extracellular matrix (ECM). On CNT patterned substrates, poly-L-lysine (PLL) was coated, and E18 rat hippocampal neurons were cultured. In the early developmental stage, soma adhesion and neurite extension occurred in disregard of the surface CNT patterns. However, later the majority of neurites selectively grew along CNT patterns and extended further than other neurites that originally did not follow the patterns. Long-term cultured neuronal networks had a strong resemblance to the in vivo neural circuit structures. The selective guidance is possibly attributed to higher PLL adsorption on CNT patterns and the nanomesh structure of the CNT patterns. The results showed that CNT patterned substrates can be used as novel neuronal patterning substrates for in vitro neural engineering.

The electronic structure and the corresponding B K and N K near-edge x-ray fine structure (NEXAFS) spectra of epitaxially grown h-BN on Ni(111), Pt(111), and Rh(111) surfaces are investigated by density functional theory. The calculations are carried out using the WIEN2k program package applying the augmented-plane-wave+local orbitals (APW+lo) method. The NEXAFS spectra are simulated using a 3 × 3 × 1 super cell and considering the final state rule by means of a (partial) core hole for the corresponding atom. The influence of a full or partial core hole is shown for the h-BN/Ni(111) system, for which the best agreement with the experimental spectra is found when half a core hole is assumed. All characteristic features of the experimental spectra are well reproduced by theory, including the angular dependences. The bonding effects are investigated by comparing the spectra of bulk h-BN with those of the h-BN/Ni(111) system. An analysis of both the density of states and charge densities reveals strong N-p(z)-Ni-d(z(2)) bonding/antibonding interactions. In the case of Pt(111) and Rh(111) surfaces, we discuss the effects of the nanomesh structures in terms of simple 1 × 1 commensurate models.

A regular square mesh structure with 4.5 nm periodicity was formed after annealing an adsorption layer of Ti on W(100) at 1370 K. The nanomesh consists of two self-assembled layers on top of the Ti adlayer, ~3.5 physical monolayers thick on average. The first layer of the nanomesh is composed of wires ~1.3 nm wide arranged along the directions of the W(100) substrate. The second one is formed by islands of ~1.6 nm in diameter arrayed upon crossing sites of the wires. The nanomesh is thermally stable up to 1470 K.