The suggested approach "Selected set of samples + selected set of analytical tools" occurred quite efficient when applying to sp 2 amorphous carbons, thus providing a transformation of 'amorphous' representation of the issue, based on particulars, into a 'crystalline' one based on a limited set of fixed commonalities. The slogan first part implies a set of different-origin solid samples. The second part concerns analytical tools, the most suitable to achieve the goal. The parts combining means the application of each tool to the whole set of samples. In the current study, two natural sp 2 amorphous carbons, namely, shungite carbon and antraxolite, as well as two engineered products -carbon blacks CB632 and CB624, all of the four bodies belonging to the elitist highest-carbon-content sp 2 species, were subjected to analytical study by using modern structural and compositional analytical techniques. The approach has allowed disclosing the following steady points that are common to the whole class of this carbon allotrope and that may lay the foundation of consolidate, more 'crystalline' representation of what are sp 2 amorphous carbons:1. sp 2 Amorphous carbons are products of particular chemical reactions related to their basic structural units. Further macroscopic agglomeration of the latter plays a subsidiary role. 2. The units represent framed graphene molecules of 1-2 nm and 1-x*10 (x=1-3) nm in size in the case of natural and engineered products, respectively.3. Framing of graphene molecules, predominantly incomplete with respect to the number of vacant places, concerns only edge atoms and is implemented by the related chemical additives, such as hydrogen, oxygen, nitrogen, sulfur and halogens which are attached to the carbon core via chemical bonding. 4. The molecules small size provides a countable number of newly formed chemical bonds.INS and XPS allow attributing the bonds to chemical compositions restricted by number while QCh ensures reliable support. 5. Temperature and pressure as well as physical state and chemical content of surrounding media are the main factors governing geochemistry and technical chemistry of carbon products. 6. Graphene molecules, laying the foundation of sp 2 amorphous carbons, are strongly radicalized due to which the latter acquire a new facet in the space of their properties, being the largest repository of stable radicals.

The correlation of odd electrons in graphene turns out to be significant so that the species should be attributed to correlated ones. This finding profoundly influences the computational strategy addressing it to configuration-interaction computational schemes. Owing to serious problems related to the schemes realization, a compromise can be suggested by using single-determinant approaches based on either Hartree-Fock or Density-Functional Theory in the form of unrestricted open-shell presentation. Both computational schemes enable to fix the electron correlation, while only the Hartree-Fock theory suggests a set of quantities to be calculated that can quantitatively characterize the electron correlation and can be used for a quantitative description of such graphene properties as magnetism, chemical reactivity, and mechanical response. The paper presents concepts and algorithms of the unrestricted Hartree-Fock theory applied for the consideration of magnetic properties of nanographenes, their chemical modification by the example of stepwise hydrogenation, as well as a possible governing the electron correlation by the carbon skeleton deformation.

The standard D-G-2D pattern of Raman spectra of sp2 amorphous carbons is considered from the viewpoint of graphene domains presenting their basic structure units (BSUs) in terms of molecular spectroscopy. The molecular approximation allows connecting the characteristic D-G doublet spectra image of one-phonon spectra with a considerable dispersion of the C=C bond lengths within graphene domains, governed by size, heteroatom necklace of BSUs as well as BSUs packing. The interpretation of 2D two-phonon spectra reveals a particular role of electrical anharmonicity in the spectra formation and attributes this effect to a high degree of the electron density delocalization in graphene domains. A size-stimulated transition from molecular to quasi-particle phonon consideration of Raman spectra was experimentally traced, which allowed evaluation of a free path of optical phonons in graphene crystal.

Applied to graphene oxide, the molecular theory of graphene considers its oxide as a final product in the succession of polyderivatives related to a series of oxidation reactions involving different oxidants. The graphene oxide structure is created in the course of a stepwise computational synthesis of polyoxides of the (5,5) nanographene molecule governed by an algorithm that takes into account the molecule's natural radicalization due to the correlation of its odd electrons, the extremely strong influence of the structure on properties, and a sharp response of the molecule behavior on small actions of external factors. Taking these together, the theory has allowed for a clear, transparent and understandable explanation of the hot points of graphene oxide chemistry and suggesting reliable models of both chemically produced and chemically reduced graphene oxides.

The response of a nanographene sheet to external stresses was considered in terms of a mechanochemical reaction. The quantum chemical realization of the approach was based on the coordinate-of-reaction concept for the purpose of introducing a mechanochemical internal coordinate (MIC) that specifies a deformational mode. The related force of response is calculated as the energy gradient along the MIC, while the atomic configuration is optimized over all of the other coordinates under the MIC constant-pitch elongation. The approach is applied to the benzene molecule and (5,5) nanographene. A drastic anisotropy in the microscopic behavior of both objects under elongation along a MIC was observed when the MIC was oriented either along or normally to the C-C bond chain. Both the anisotropy and the high stiffness of the nanographene originate from the response of the benzenoid unit to stress.