Electron Correlations and Two-Photon States in Polycyclic Aromatic Hydrocarbon Molecules: A Peculiar Role of Geometry

We present numerical studies of one- and two-photon excited states ordering in a number of polycyclic aromatic hydrocarbon molecules: coronene, hexa-peri-hexabenzocoronene and circumcoronene, all possessing $D_{6h}$ point group symmetry versus ovalene with $D_{2h}$ symmetry, within the Pariser-Parr-Pople model of interacting $\pi$-electrons. The calculated energies of the two-photon states as well as their relative two-photon absorption cross-sections within the interacting model are qualitatively different from single-particle descriptions. More remarkably, a peculiar role of molecular geometry is found. The consequence of electron correlations is far stronger for ovalene, where the lowest spin-singlet two-photon state is a quantum superposition of pairs of lowest spin triplet states, as in the linear polyenes. The same is not true for $D_{6h}$ group hydrocarbons. Our work indicates significant covalent character, in valence bond language, of the ground state, the lowest spin triplet state and a few of the lowest two-photon states in $D_{2h}$ ovalene but not in those with $D_{6h}$ symmetry.Comment: 11 pages, 3 figures, 3 table

Theory of interfacial charge-transfer complex photophysics in π\pi-conjugated polymer-fullerene blends

We present a theory of the electronic structure and photophysics of 1:1 blends of derivatives of polyparaphenylenevinylene and fullerenes. Within the same Coulomb-correlated Hamiltonian applied previously to interacting chains of single-component $\pi$-conjugated polymers, we find an exciplex state that occurs below the polymer's optical exciton. Weak absorption from the ground state occurs to the exciplex. We explain transient photoinduced absorptions in the blend, observed for both above-gap and below-gap photoexcitations, within our theory. Photoinduced absorptions for above-gap photoexcitation are from the optical exciton as well as the exciplex, while for below-gap photoexcitation induced absorptions are from the exciplex alone. In neither case are free polarons generated in the time scale of the experiment. Importantly, the photophysics of films of single-component $\pi$-conjugated polymers and blends can both be understood by extending Mulliken's theory of ground-state charge transfer to the case of excited-state charge transfer.Comment: 9 pages, 8 figure

The ubiquitous 1100 charge ordering in organic charge-transfer solids

Charge and spin-orderings in the 1/4-filled organic CT solids are of strong interest, especially in view of their possible relations to organic superconductivity. We show that the charge order (CO) in both 1D and 2D CT solids is of the ...1100... type, in contradiction to mean field prediction of >...1010... CO. We present detailed computations for metal-insulator and magnetic insulator-insulator transitions in the theta-ET materials. Complete agreement with experiments in several theta systems is found. Similar comparisons between theory and experiments in TCNQ, TMTTF, TMTSF, and ET materials prove the ubiquity of this phenomenon.Comment: 3 pages, 4 eps figures; ICSM 200

Longevity of supersymmetric flat directions

We examine the fate of supersymmetric flat directions. We argue that the non-perturbative decay of the flat direction via preheating is an unlikely event. In order to address this issue, first we identify the physical degrees of freedom and their masses in presence of a large flat direction VEV (Vacuum Expectation Value). We explicitly show that the (complex) flat direction and its fermionic partner are the only light {\it physical} fields in the spectrum. If the flat direction VEV is much larger than the weak scale, and it has a rotational motion, there will be no resonant particle production at all. The case of multiple flat directions is more involved. We illustrate that in many cases of physical interest, the situation becomes effectively the same as that of a single flat direction, or collection of independent single directions. In such cases preheating is not relevant. In an absence of a fast non-perturbative decay, the flat direction survives long enough to affect thermalization in supersymmetric models as described in hep-ph/0505050 and hep-ph/0512227. It can also ``terminate'' an early stage of non-perturbative inflaton decay as discussed in hep-ph/0603244.Comment: 9 revtex pages, v3: expanded discussion on two flat directions, minor modifications, conclusions unchange

Identifying the curvaton within MSSM

We consider inflaton couplings to MSSM flat directions and the thermalization of the inflaton decay products, taking into account gauge symmetry breaking due to flat direction condensates. We then search for a suitable curvaton candidate among the flat directions, requiring an early thermally induced start for the flat direction oscillations to facilitate the necessary curvaton energy density dominance. We demonstrate that the supersymmetry breaking $A$-term is crucial for achieving a successful curvaton scenario. Among the many possible candidates, we identify the ${\bf u_1dd}$ flat direction as a viable MSSM curvaton.Comment: 9 pages. Discussion on the evaporation of condensate added, final version published in JCA

Subgap Two-Photon States in Polycyclic Aromatic Hydrocarbons: Evidence for Strong Electron Correlations

Strong electron correlation effects in the photophysics of quasi-one-dimensional $\pi$-conjugated organic systems such as polyenes, polyacetylenes, polydiacetylenes, etc., have been extensively studied. Far less is known on correlation effects in two-dimensional $\pi$-conjugated systems. Here we present theoretical and experimental evidence for moderate repulsive electron-electron interactions in a number of finite polycyclic aromatic hydrocarbon molecules with $D_{6h}$ symmetry. We show that the excited state orderings in these molecules are reversed relative to that expected within one-electron and mean-field theories. Our results reflect similarities as well as differences in the role and magnitude of electron correlation effects in these two-dimensional molecules compared to those in polyenes.Comment: 11 pages, 5 figures, 2 table

Stable isotopic study of late Neoproterozoic-early Cambrian (?) sediments from Nagaur-Ganganagar basin, western India: possible signatures of global and regional C-isotopic events

Carbonate rocks of late Neoproterozoic-early Cambrian age occur in two extremities of the Nagaur-Ganganagar basin in western India: in east as part of Bilara hills (type locality) and in west as part of Baghewala oil field. These rocks have close stratigraphic correlation with the Ara Formation (Huqf Group, south Oman salt basin) which transgresses the late Neoproterozoic-early Cambrian boundary. Sedimentological and stable isotopic studies of these rocks show prevalence of arid and evaporitic conditions during their depostion. Close resemblance of C-isotopic profiles of Hanseran evaporites and Bilara carbonates allows intra-basinal correlation and suggests that they are coeval facies variants. There are several characteristic carbon isotopic excursions one of which can be tentatively correlated with the globally recorded excursion close to the late Neoproterozoic-early Cambrian boundary. In contrast other peaks are possibly of regional significance and can be attributed to fluctuations in bioproductivity, correlatable with variation in nutrient supply on a basinal scale. Highly depleted carbon isotopic composition of the organic matter in subsurface organic-rich carbonates (Upper carbonate Formation, Baghewala-II core) has been ascribed to incorporation of biomass synthesized by chemoautotrophic bacteria under anoxic or eutrophic basinal condition caused by salinity stratification