ترغب بنشر مسار تعليمي؟ اضغط هنا

Leaving the Fullerene Road: Presence and Stability of sp Chains in sp2 Carbon Clusters and Cluster-Assembled Solids

71   0   0.0 ( 0 )
 نشر من قبل Ravagnan Luca
 تاريخ النشر 2005
  مجال البحث فيزياء
والبحث باللغة English




اسأل ChatGPT حول البحث

We report the experimental and theoretical investigation of the growth and of the structure of large carbon clusters produced in a supersonic expansion by a pulsed microplasma source. The absence of a significant thermal annealing during the cluster growth causes the formation of disordered structures where sp2 and sp hybridizations coexist for particles larger than roughly 90 atoms. Among different structures we recognize sp2 closed networks encaging sp chains. This nutshell configuration can prevent the fragmentation of sp species upon deposition of the clusters thus allowing the formation of nanostructured films containing carbynoid species, as shown by Raman spectroscopy. Atomistic simulations confirm that the observed Raman spectra are the signature of the sp/sp2 hybridization characteristic of the isolated clusters and surviving in the film and provide information about the structure of the sp chains. Endohedral sp chains in sp2 cages represent a novel way in which carbon nanostructures may be organized with potential interesting functional properties.



قيم البحث

اقرأ أيضاً

We report the production and characterization of a form of amorphous carbon films with sp/sp2 hybridization (atomic fraction of sp hybridized species > 20%) where the predominant sp bonding appears to be (=C=C=)n cumulene. Vibrational and electronic properties have been studied by in situ Raman spectroscopy and electrical conductivity measurements. Cumulenic chains are substantially stable for temperatures lower than 250 K and they influence the electrical transport properties of the sp/sp2 carbon through a self-doping mechanism by pinning the Fermi level closer to one of the mobility gap edges. Upon heating above 250 K the cumulenic species decay to form graphitic nanodomains embedded in the sp2 amorphous matrix thus reducing the activation energy of the material. This is the first example of a pure carbon system where the sp hybridization influences bulk properties.
A novel form of amorphous carbon with sp-sp2 hybridization has been recently produced by supersonic cluster beam deposition showing the presence in the film of both polyynic and cumulenic species [L. Ravagnan et al. Phys. Rev. Lett. 98, 216103 (2007) ]. Here we present a in situ Raman characterization of the low frequency vibrational region (400-800 cm-1) of sp-sp2 films at different temperatures. We report the presence of two peaks at 450 cm-1 and 720 cm-1. The lower frequency peak shows an evolution with the variation of the sp content and it can be attributed, with the support of density functional theory (DFT) simulations, to bending modes of sp linear structures. The peak at 720 cm-1 does not vary with the sp content and it can be attributed to a feature in the vibrational density of states activated by the disorder of the sp2 phase.
A structurally stable carbon allotrope with plentiful topological properties is predicted by means of first-principles calculations. This novel carbon allotrope possesses the simple space group C2/m, and contains simultaneously sp, sp2 and sp3 hybrid ized bonds in one structure, which is thus coined as carboneyane. The calculations on geometrical, vibrational, and electronic properties reveal that carboneyane, with good ductility and a much lower density 1.43 g/cm3, is a topological metal with a pair of nodal lines traversing the whole Brillouin zone, such that they can only be annihilated in a pair when symmetry is preserved. The symmetry and topological protections of the nodal lines as well as the associated surface states are discussed. By comparing its x-ray diffraction pattern with experimental results, we find that three peaks of carboneyane meet with the detonation soot. On account of the fluffy structure, carboneyane is shown to have potential applications in areas of storage, adsorption and electrode materials.
We have characterized the frictional properties of nanostructured (ns) carbon films grown by Supersonic Cluster Beam Deposition (SCBD) via an Atomic Force-Friction Force Microscope (AFM-FFM). The experimental data are discussed on the basis of a modi fied Amontons law for friction, stating a linear dependence of friction on load plus an adhesive offset accounting for a finite friction force in the limit of null total applied load. Molecular Dynamics simulations of the interaction of the AFM tip with the nanostructured carbon confirm the validity of the friction model used for this system. Experimental results show that the friction coefficient is not influenced by the nanostructure of the films nor by the relative humidity. On the other hand the adhesion coefficient depends on these parameters.
Graphdiyne, atomically-thin 2D carbon nanostructure based on sp-sp2 hybridization, is an appealing system potentially showing outstanding mechanical and optoelectronic properties. Surface-catalyzed coupling of halogenated sp-carbon-based molecular pr ecursors represents a promising bottom-up strategy to fabricate extended 2D carbon systems with engineered structure on metallic substrates. Here, we investigate the atomic-scale structure and electronic and vibrational properties of an extended graphdiyne-like sp-sp2 carbon nanonetwork grown on Au(111) by means of on-surface synthesis. The formation of such 2D nanonetwork at its different stages as a function of the annealing temperature after the deposition is monitored by scanning tunneling microscopy (STM), Raman spectroscopy and combined with density functional theory (DFT) calculations. High-resolution STM imaging and the high sensitivity of Raman spectroscopy to the bond nature provide a unique strategy to unravel the atomic-scale properties of sp-sp2 carbon nanostructures. We show that hybridization between the 2D carbon nanonetwork and the underlying substrate states strongly affects its electronic and vibrational properties, modifying substantially the density of states and the Raman spectrum compared to the free standing system. This opens the way to the modulation of the electronic properties with significant prospects in future applications as active nanomaterials for catalysis, photoconversion and carbon-based nanoelectronics.
التعليقات
جاري جلب التعليقات جاري جلب التعليقات
سجل دخول لتتمكن من متابعة معايير البحث التي قمت باختيارها
mircosoft-partner

هل ترغب بارسال اشعارات عن اخر التحديثات في شمرا-اكاديميا