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

Abstract

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.

11 pages, 5 figures, 2 tables

References in corpus (5)

• The electronic properties of graphene
• Excitonic Effects on the Optical Response of Graphene and Bilayer Graphene
• Optical properties of graphene nanoribbons: the role of many-body effects
• A large-scale correlated study of linear optical absorption and low-lying excited states of polyacenes: Pariser-Parr-Pople Hamiltonian
• Quantitative calculations of the excitonic energy spectra of semiconducting single-walled carbon nanotubes within a $\pi$-electron model

Cited by in corpus (15)

• Theory of Singlet Fission in Polyenes, Acene Crystals and Covalently Linked Acene Dimers
• Investigation of metal-insulator like transition through the ab initio density matrix renormalization group approach
• Theory of Linear Optical Absorption in Diamond Shaped Graphene Quantum Dots
• Stretching and breaking of chemical bonds, correlation of electrons, and radical properties of covalent species
• Diagrammatic Exciton Basis Theory of the Photophysics of Pentacene Dimers
• Correlated Electronic Properties of Some Graphene Nanoribbons: A DMRG Study
• Optical signatures of electric field driven magnetic phase transitions in graphene quantum dots
• Pariser-Parr-Pople Model based Configuration-Interaction Study of Linear Optical Absorption in Lower-Symmetry Polycyclic Aromatic Hydrocarbon Molecules
• Optical Probes of the Quantum-Entangled Triplet-Triplet State in a Heteroacene Dimer
• Electron correlation effects and two-photon absorption in diamond shaped graphene quantum dots
• The Correlated Electronic States of a few Polycyclic Aromatic Hydrocarbons: A Computational Study
• Tunable Optoelectronic Properties of Triply-Bonded Carbon Molecules with Linear and Graphyne Substructures
• The optical properties of dibenzoterrylene
• Excited States and Optical Properties of Hydrogen-Passivated Rectangular Graphenes: A Computational Study
• Computational study of geometry, electronic structure and low-lying excited states of linear T-graphene quantum dots