Cost-effective reduced graphene oxide sheets decorated with magnetite (Fe3O4) nanoparticles (Fe3O4-rGO) are successfully fabricated via a chemical vapor deposition (CVD) technique using iron (III) nitrate as an iron precursor, with glucose and CH4 as carbon sources, and NaCl as a supporting material. TEM analysis and Raman spectroscopy reveal hierarchical nanostructures of reduced graphene oxide (rGO) decorated with Fe3O4 nanoparticles. Fe K-edge x-ray absorption near edge structure (XANES) spectra confirm that the nanoparticles are Fe3O4 with a slight shift of the pre-edge peak position toward higher energy suggesting that the fabricated Fe3O4 nanoparticles have a higher average oxidation state than that of a standard Fe3O4 compound. The hierarchical Fe3O4-rGO is found to exhibit an excellent catalytic activity toward the reduction of triiodide to iodide in a dye-sensitized solar cell (DSSC) and can deliver a solar cell efficiency of 6.65%, which is superior to a Pt-based DSSC (6.37%).
Two-dimensional transition metal carbides, carbonitrides, and nitrides, called MXenes, exhibit high metallic conductivity, ion intercalation capability, and reversible redox activity, prompting their applications in energy storage and conversion, electromagnetic interference (EMI) shielding, and electronics, among many other fields. It has been shown that replacement of ∼50% of carbon atoms in the most popular MXene family member, titanium carbide (Ti3C2Tx), by nitrogen atoms, forming titanium carbonitride (Ti3CNTx), leads to drastically different properties. Such properties include very high negative charge in solution and extreme EMI shielding effectiveness, exceeding all known materials, even metals at comparable thicknesses. Here, by using ultraviolet photoemission spectroscopy (UPS), the electronic structures of Ti3CNTx and Ti3C2Tx are systematically investigated and compared as a function of charge carrier density. We observe that, in contrast to Ti3C2Tx, the Ti 3p core-level of Ti3CNTx exhibits a counterintuitive shift to a lower binding energy of up to ∼250 meV upon increasing the electron density, which is a spectroscopic signature of negative electronic compressibility (NEC). These experimentally measured chemical potential shifts are well captured by the density functional theory (DFT) calculation. The DFT results also further suggest that the hybridization of titanium–nitrogen bonding in Ti3CNTx helps to promote the available states of Ti atoms for receiving more electrons above the fermi level and leads to the observed NEC. Our findings explain the differences in electronic properties between the two very important and widely studied MXenes and also suggest a new strategy to apply the NEC effect of Ti3CNTx in energy and charge storage applications.
By using angle-resolved photoemission spectroscopy (ARPES), the variation of the electronic structure of HfSe2 has been studied as a function of sodium intercalation. We observe how this drives a band splitting of the p-orbital valence bands and a simultaneous reduction of the indirect band gap by values of up to 400 and 280 meV respectively. Our calculations indicate that such behaviour is driven by the band deformation potential, which is a result of our observed anisotropic strain induced by sodium intercalation. The applied uniaxial strain calculations based on density functional theory (DFT) agree strongly with the experimental ARPES data. These findings should assist in studying the physical relationship between doping and strain, as well as for large-scale two-dimensional straintronics.
The discovery of a two-dimensional electron gas (2DEG) at the $$\hbox {LaAlO}_3/\hbox {SrTiO}_3$$ LaAlO 3 / SrTiO 3 interface has set a new platform for all-oxide electronics which could potentially exhibit the interplay among charge, spin, orbital, superconductivity, ferromagnetism and ferroelectricity. In this work, by using angle-resolved photoemission spectroscopy and conductivity measurement, we found the reduction of 2DEGs and the changes of the conductivity nature of some ferroelectric oxides including insulating Nb-lightly-substituted $$\hbox {KTaO}_3$$ KTaO 3 , $$\hbox {BaTiO}_3$$ BaTiO 3 (BTO) and (Ca,Zr)-doped BTO across paraelectric-ferroelectric transition. We propose that these behaviours could be due to the increase of space-charge screening potential at the 2DEG/ferroelectric regions which is a result of the realignment of ferroelectric polarisation upon light irradiation. This finding suggests an opportunity for controlling the 2DEG at a bare oxide surface (instead of interfacial system) by using both light and ferroelectricity.
By using angle-resolved photoemission spectroscopy (ARPES), we study the electronic structure of highly oriented pyrolytic graphite (HOPG). In contrast to the pristine HOPG, band gap opening of approximately 100 meV is directly observed at the surface of nano-scale HOPG square pattern. Our Raman data and density functional theory calculations suggest that the bandgap opening is likely caused by tensile strain induced from the patterning. We believe that this surface engineering of HOPG will not only be useful for enhancing terahertz devices but also provides a route for modifying other materials/metasurfaces for optoelectronics applications.
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