Graphane Nanotubes

In this work, one-dimensional graphane nanotubes (GN, stoichiometry CH), built from 2D single-sheet graphanes, are explored theoretically. Zigzag type GN(10,0) and armchair type GN(10,10) structures with varying surface termination were investigated in detail. GN(10,10)-A is found to be the most stable configuration among the GN structures considered. An annealing analysis indicates that graphane-A and GN(10,10)-A are likely to be stable at elevated temperature. A possible reaction path to GN(10,10)-A is suggested by the reaction of single-walled carbon nanotube (10,10) + H₂; the indications are that the GN(10,10)-A can be made at low temperature and high partial pressure of H₂ gas from the corresponding nanotube. The graphane nanotubes are predicted to be wide band gap insulators. A study of the effect of the diameter of GN structures shows, unexpectedly, that the gap increases on reducing the diameter of the graphane nanotubes. We also investigated several partially hydrogenated graphenes and single-walled carbon nanotubes (SWNT); the greater hydrogenation is, the more stable is the resulting structure. The band gap of graphene or SWNT can be tuned <i>via</i> hydrogenation

Solution-Processed n‑Type Graphene Doping for Cathode in Inverted Polymer Light-Emitting Diodes

n-Type doping with (4-(1,3-dimethyl-2,3-dihydro-1H-benzoimidazol-2-yl)­phenyl) dimethylamine (N-DMBI) reduces a work function (WF) of graphene by ∼0.45 eV without significant reduction of optical transmittance. Solution process of N-DMBI on graphene provides effective n-type doping effect and air-stability at the same time. Although neutral N-DMBI act as an electron receptor leaving the graphene p-doped, radical N-DMBI acts as an electron donator leaving the graphene n-doped, which is demonstrated by density functional theory. We also verify the suitability of N-DMBI-doped n-type graphene for use as a cathode in inverted polymer light-emitting diodes (PLEDs) by using various analytical methods. Inverted PLEDs using a graphene cathode doped with N-DMBI radical showed dramatically improved device efficiency (∼13.8 cd/A) than did inverted PLEDs with pristine graphene (∼2.74 cd/A). N-DMBI-doped graphene can provide a practical way to produce graphene cathodes with low WF in various organic optoelectronics

Iron Carbides in Fischer–Tropsch Synthesis: Theoretical and Experimental Understanding in Epsilon-Iron Carbide Phase Assignment

As active phases in low-temperature Fischer–Tropsch synthesis for liquid fuel production, epsilon iron carbides are critically important industrial materials. However, the precise atomic structure of epsilon iron carbides remains unclear, leading to a half-century of debate on the phase assignment of the ε-Fe₂C and ε′-Fe_2.2C. Here, we resolve this decades-long question by a combined theoretical and experimental investigation to assign the phases unambiguously. First, we have investigated the equilibrium structures and thermal stabilities of ε-Fe_<i>x</i>C (<i>x</i> = 1, 2, 2.2, 3, 4, 6, 8) by first-principles calculations. We have also acquired X-ray diffraction patterns and Mössbauer spectra for these epsilon iron carbides and compared them with the simulated results. These analyses indicate that the unit cell of ε-Fe₂C contains only one type of chemical environment for Fe atoms, while ε′-Fe_2.2C has six sets of chemically distinct Fe atoms

Vortex nonlinear optics in monolayer van der Waals crystals

In addition to wavelength and polarization, coherent light possesses a degree of freedom associated with its spatial topology that, when exploited through nonlinear optics, can unlock a plethora of new photonic phenomena. A prime example involves the use of vortex beams, which allow for the tuning of light's orbital angular momentum (OAM) on demand. Such processes can not only reveal emergent physics but also enable high-density classical and quantum communication paradigms by allowing access to an infinitely large set of orthogonal optical states. Nevertheless, structured nonlinear optics have failed to keep pace with the ever-present need to shrink the length-scale of optoelectronic and photonic technologies to the nanoscale regime. Here, we push the boundaries of vortex nonlinear optics to the ultimate limits of material dimensionality. By exploiting second and third-order nonlinear frequency-mixing processes in van der Waals semiconductor monolayers, we show the free manipulation of the wavelength, topological charge, and radial index of vortex light-fields. We demonstrate that such control can be supported over a broad spectral bandwidth, unconstrained by traditional limits associated with bulk nonlinear optical (NLO) materials, due to the atomically-thin nature of the host crystal. Our work breaks through traditional constraints in optics and promises to herald a new avenue for next-generation optoelectronic and photonics technologies empowered by twisted nanoscale nonlinear light-matter interactions