We present an overview of the main techniques for production and processing of graphene and related materials (GRMs), as well as the key characterization procedures. We adopt a ‘hands-on’ approach, providing practical details and procedures as derived from literature as well as from the authors’ experience, in order to enable the reader to reproduce the results. Section is devoted to ‘bottom up’ approaches, whereby individual constituents are pieced together into more complex structures. We consider graphene nanoribbons (GNRs) produced either by solution processing or by on-surface synthesis in ultra high vacuum (UHV), as well carbon nanomembranes (CNM). Production of a variety of GNRs with tailored band gaps and edge shapes is now possible. CNMs can be tuned in terms of porosity, crystallinity and electronic behaviour. Section covers ‘top down’ techniques. These rely on breaking down of a layered precursor, in the graphene case usually natural crystals like graphite or artificially synthesized materials, such as highly oriented pyrolythic graphite, monolayers or few layers (FL) flakes. The main focus of this section is on various exfoliation techniques in a liquid media, either intercalation or liquid phase exfoliation (LPE). The choice of precursor, exfoliation method, medium as well as the control of parameters such as time or temperature are crucial. A definite choice of parameters and conditions yields a particular material with specific properties that makes it more suitable for a targeted application. We cover protocols for the graphitic precursors to graphene oxide (GO). This is an important material for a range of applications in biomedicine, energy storage, nanocomposites, etc. Hummers’ and modified Hummers’ methods are used to make GO that subsequently can be reduced to obtain reduced graphene oxide (RGO) with a variety of strategies. GO flakes are also employed to prepare three-dimensional (3d) low density structures, such as sponges, foams, hydro- or aerogels. The assembly of flakes into 3d structures can provide improved mechanical properties. Aerogels with a highly open structure, with interconnected hierarchical pores, can enhance the accessibility to the whole surface area, as relevant for a number of applications, such as energy storage. The main recipes to yield graphite intercalation compounds (GICs) are also discussed. GICs are suitable precursors for covalent functionalization of graphene, but can also be used for the synthesis of uncharged graphene in solution. Degradation of the molecules intercalated in GICs can be triggered by high temperature treatment or microwave irradiation, creating a gas pressure surge in graphite and exfoliation. Electrochemical exfoliation by applying a voltage in an electrolyte to a graphite electrode can be tuned by varying precursors, electrolytes and potential. Graphite electrodes can be either negatively or positively intercalated to obtain GICs that are subsequently exfoliated. We also discuss the materials that can be amenable to exfoliation, by ...
We investigate the doping of vanadyl–phthalocyanine by a fluorinated form of tetracyano-quinodimethane as an example of controlled doping of thin organic dye films by cosublimation of matrix and dopant. The electrical parameters of the films derived from conductivity and Seebeck measurements show that the results largely follow standard models used to describe the doping of crystalline semiconductors; e.g., a smooth shift of the Fermi level towards the valence states with increasing doping is observed. Other effects, like the superlinear increase of conductivity with the molar doping ratio, need the inclusion of additional effects like percolation.
Plasmonic nanoantennas are versatile tools for coherently controlling and directing light on the nanoscale. For these antennas, current fabrication techniques such as electron beam lithography (EBL) or focused ion beam (FIB) milling with Ga(+)-ions routinely achieve feature sizes in the 10 nm range. However, they suffer increasingly from inherent limitations when a precision of single nanometers down to atomic length scales is required, where exciting quantum mechanical effects are expected to affect the nanoantenna optics. Here, we demonstrate that a combined approach of Ga(+)-FIB and milling-based He(+)-ion lithography (HIL) for the fabrication of nanoantennas offers to readily overcome some of these limitations. Gold bowtie antennas with 6 nm gap size were fabricated with single-nanometer accuracy and high reproducibility. Using third harmonic (TH) spectroscopy, we find a substantial enhancement of the nonlinear emission intensity of single HIL-antennas compared to those produced by state-of-the-art gallium-based milling. Moreover, HIL-antennas show a vastly improved polarization contrast. This superior nonlinear performance of HIL-derived plasmonic structures is an excellent testimonial to the application of He(+)-ion beam milling for ultrahigh precision nanofabrication, which in turn can be viewed as a stepping stone to mastering quantum optical investigations in the near-field.
The provision of clean water is a global challenge, and membrane filtration is a key technology to address it. Conventional filtration membranes are constrained by a trade-off between permeance and selectivity. Recently, some nanostructured membranes demonstrated the ability to overcome this limitation by utilizing well-defined carbon nanoconduits that allow a coordinated passage of water molecules. The fabrication of these materials is still very challenging, but their performance inspires research toward nanofabricated membranes. This study reports on molecularly thin membranes with sub-nanometer channels that combine high water selectivity with an exceptionally high permeance. Carbon nanomembranes (CNMs) of ∼1.2 nm thickness are fabricated from terphenylthiol (TPT) monolayers. Scanning probe microscopy and transport measurements reveal that TPT CNMs consist of a dense network of sub-nanometer channels that efficiently block the passage of most gases and liquids. However, water passes through with an extremely high permeance of ∼1.1 × 10 mol·m·s·Pa, as does helium, but with a ∼ 2500 times lower flux. Assuming all channels in a TPT CNM are active in mass transport, we find a single-channel permeation of ∼66 water molecules·s·Pa. This suggests that water molecules translocate fast and cooperatively through the sub-nanometer channels, similar to carbon nanotubes and membrane proteins (aquaporins). CNMs are thus scalable two-dimensional sieves that can be utilized toward energy-efficient water purification.
We investigate the low-energy quasiparticle excitation spectra of cuprate superconductors by incorporating both superconductivity (SC) and competing orders (CO) in the bare Green's function and quantum phase fluctuations in the proper self-energy. Our approach provides consistent explanations for various empirical observations, including the excess subgap quasiparticle density of states, "dichotomy" in the momentum-dependent quasiparticle coherence and the temperature-dependent gap evolution, and the presence (absence) of the low-energy pseudogap in hole-(electron-) type cuprates depending on the relative scale of the CO and SC energy gaps. 74.25.Jb, 74.50.+r Keywords: Quasiparticle spectra; pseudogap; competing orders; cuprate superconductors Cuprate superconductors differ fundamentally from conventional superconductors in that they are doped Mott insulators with strong electronic correlation that leads to possibilities of different competing orders (CO) in the ground state besides superconductivity (SC) [1][2][3][4][5][6][7][8]. The existence of competing orders and the proximity to quantum criticality [2,3,7,8] gives rise to unconventional low-energy excitations of the cuprates, manifested as weakened superconducting phase stiffness [6], occurrence of excess subgap quasiparticle density of states (DOS) [9], spatial modulations in the lowtemperature quasiparticle spectra that are unaccounted for by Bogoliubov quasiparticles alone [10][11][12], "dichotomy" in the momentum-dependent quasiparticle coherence [13] and temperature-dependent gap evolution [14], and the presence (absence) of the low-energy pseudogap (PG) [9,15,16] and Nernst effect [17] in the hole (electron)-type cuprates above the SC transition. Microscopically, the existence of CO is likely responsible for various non-universal phenomena among different cuprates [8,9,18,19]. Macroscopically, the weakened superconducting phase stiffness and proximity to CO can give rise to strong fluctuations that lead to the extreme type-II nature and rich vortex dynamics [8,20,21].To date there are two typical theoretical approaches to describing the quasiparticle excitation spectra of the cuprates. One approach takes the BCS-like Hamiltonian as the unperturbed mean-field state and a competing order, pinned by disorder, as the perturbation that gives rise to a weak scattering potential for the Bogoliubov quasiparticles [11,[22][23][24]. The other approach begins with the BCS-like Hamiltonian and includes superconducting phase fluctuations in the proper self-energy correction [25,26]. However, no quantitative calculations have been made by incorporating both CO and quantum phase fluctuations in the SC state. The objective of this work is to consider the latter scenario and compute the corresponding low-energy excitation spectra with realistic physical parameters for comparison with experiments. We find that the low-energy excitations thus derived differ from typical Bogoliubov quasiparticles and can account for various puzzling phenomena aforementioned....
Graphene has emerged as an electronic material that is promising for device applications and for studying two-dimensional electron gases with relativistic dispersion near two Dirac points. Nonetheless, deviations from Dirac-like spectroscopy have been widely reported with varying interpretations. Here we show evidence for strain-induced spatial modulations in the local conductance of single-layer graphene on SiO(2) substrates from scanning tunneling microscopic (STM) studies. We find that strained graphene exhibits parabolic, U-shaped conductance vs bias voltage spectra rather than the V-shaped spectra expected for Dirac fermions, whereas V-shaped spectra are recovered in regions of relaxed graphene. Strain maps derived from the STM studies further reveal direct correlation with the local tunneling conductance. These results are attributed to a strain-induced frequency increase in the out-of-plane phonon mode that mediates the low-energy inelastic charge tunneling into graphene.
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