Graphene is a remarkable two-dimensional (2D) material that is of great interest to both academia and industry. It has outstanding electrical and thermal conductivity and good mechanical behavior with promising applications in electronic devices, supercapacitors, batteries, composite materials, flexible transparent displays, solar cells, and sensors. Several methods have been used to produce either pristine graphene or doped graphene. These include chemical vapor deposition (CVD), mechanical exfoliation, decomposition of SiC, liquid-phase exfoliation, pulsed laser deposition (PLD). Among these methods, PLD, which is routinely used for growing complex oxide thin films has proved to be an alternative to the more widely reported CVD method for producing graphene thin films, because of its advantages. Here we review the synthesis of graphene using PLD. We describe recent progress in preparing pristine graphene and doped graphene by PLD, including deposition processes and characterization. The goal of this complete survey is to describe the advantages of using the technique for graphene growth. The review will also help researchers to better understand graphene synthesis using the PLD technique.
New synthesis routes to tailor graphene properties by controlling the concentration and chemical configuration of dopants show great promise. Herein we report the direct reproducible synthesis of 2-3% nitrogen-doped ‘few-layer’ graphene from a solid state nitrogen carbide a-C:N source synthesized by femtosecond pulsed laser ablation. Analytical investigations, including synchrotron facilities, made it possible to identify the configuration and chemistry of the nitrogen-doped graphene films. Auger mapping successfully quantified the 2D distribution of the number of graphene layers over the surface, and hence offers a new original way to probe the architecture of graphene sheets. The films mainly consist in a Bernal ABA stacking three-layer architecture, with a layer number distribution ranging from 2 to 6. Nitrogen doping affects the charge carrier distribution but has no significant effects on the number of lattice defects or disorders, compared to undoped graphene synthetized in similar conditions. Pyridinic, quaternary and pyrrolic nitrogen are the dominant chemical configurations, pyridinic N being preponderant at the scale of the film architecture. This work opens highly promising perspectives for the development of self-organized nitrogen-doped graphene materials, as synthetized from solid carbon nitride, with various functionalities, and for the characterization of 2D materials using a significant new methodology.
Improving graphene-based electrode fabrication processes and developing robust methods for its functionalization are two key research routes to develop new high-performance electrodes for electrochemical applications. Here, a self-organized three-dimensional (3D) graphene electrode processed by pulsed laser deposition with thermal annealing is reported. This substrate shows great performance in electron transfer kinetics regarding ferrocene redox probes in solution. A robust electrografting strategy for covalently attaching a redox probe onto these graphene electrodes is also reported. The modification protocol consists of a combination of diazonium salt electrografting and click chemistry. An alkyne-terminated phenyl ring is first electrografted onto the self-organized 3D graphene electrode by in situ electrochemical reduction of 4-ethynylphenyl diazonium. Then the ethynylphenyl-modified surface efficiently reacts with the redox probe bearing a terminal azide moiety (2-azidoethyl ferrocene) by means of Cu(I)-catalyzed alkyne-azide cycloaddition. Our modification strategy applied to 3D graphene electrodes was analyzed by means of atomic force microscopy, scanning electron microscopy, Raman spectroscopy, cyclic voltammetry, and X-ray photoelectron spectroscopy (XPS). For XPS chemical surface analysis, special attention was paid to the distribution and chemical state of iron and nitrogen in order to highlight the functionalization of the graphene-based substrate by electrochemically grafting a ferrocene derivative. Dense grafting was observed, offering 4.9 × 10(-10) mol cm(-2) surface coverage and showing a stable signal over 22 days. The electrografting was performed in the form of multilayers, which offers higher ferrocene loading than a dense monolayer on a flat surface. This work opens highly promising perspectives for the development of self-organized 3D graphene electrodes with various sensing functionalities.
The large area deposition and synthesis of 10 mm × 10 mm atomically thin Yb3+‐doped MoS2 films by femtosecond pulsed laser deposition on a silica glass optical platform for device applications are demonstrated for the first time. The presence of Yb3+‐ion doping is confirmed using photoluminescence (PL), X‐ray photoelectron spectroscopy (XPS), and Raman spectroscopy. The Yb3+‐doped MoS2 films, when excited with a 976 nm laser, exhibit room temperature PL with a peak at 1002 nm. The XPS and Raman spectroscopic analyses of the Yb3+‐doped and undoped films show that the deposited films are a mixture of 2H‐ and 1T‐MoS2 after postdeposition annealing at 500 °C. The density functional theory analysis shows that the 1T phase is metastable by +77 kJ (≈0.8 eV) mol‐1, when compared with the 2H state at 0 K. Ultrafast transient nonlinear optical spectroscopic measurements prove that the saturable absorption of undoped MoS2 is significantly modified after Yb3+‐ion doping, by displaying dopant‐host structure charge transfer. The complex transient absorption line shape shows a combination of bleach (negative) signals at the A (670 nm) and B (630 nm) exciton energies, and a strong induced absorption below the A exciton level. The results presented herein provide critical insight in designing novel rare‐earth‐ion doped 2D materials and devices.
Tuning optical or magnetic properties of nanoparticles, by addition of impurities, for specific applications is usually achieved at the cost of band gap and work function reduction. Additionally, conventional strategies to develop nanoparticles with a large band gap also encounter problems of phase separation and poor crystallinity at high alloying degree. Addressing the aforementioned trade-offs, here we report Ni−Zn nanoferrites with energy band gap (E g ) of ≈3.20 eV and a work function of ≈5.88 eV. While changes in the magnetoplasmonic properties of the Ni−Zn ferrite were successfully achieved with the incorporation of bismuth ions at different concentrations, there was no alteration of the band gap and work function in the developed Ni−Zn ferrite. This suggests that with the addition of minute impurities to ferrites, independent of their changes in the band gap and work function, one can tune their magnetic and optical properties, which is desired in a wide range of applications such as nanobiosensing, nanoparticle based catalysis, and renewable energy generation using nanotechnology.
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