Funct. Mater. 2021; 28 (4): 743-750
doi:https://doi.org/10.15407/fm28.04.743
Estimating spin gap in conjugated nanomolecules by spin-flip configuration-interaction-singles approach
STC "Institute for Single Crystals", National Academy of Science of Ukraine, 60 Nauky Ave., 61001 Kharkiv, Ukraine
Abstract:
For solids and molecular structures, the spin gap, Δs, is usually defined as the lowest electronic transition energy with a minimal nonzero change of the ground-state total spin. Here we apply π-electron semiempirical schemes to estimate Δs in nanosized conjugated systems of graphene quantum-dot and chain-like types. Namely, the spin-flip configuration interaction singles (SF-CIS) and appropriately specified Heisenberg spin-Hamiltonian (HSH) models are employed. It is shown by comparison with results of the exact π-electron theory that the simplest version of SF-CIS reasonably reproduces Δs in small-size problems, thus providing a justifiction for using the method in related problems. A particular attention is given to ferromagnetic oligomeric systems based on phenalenyl and triangulene subunits. The conjunction of SF-CIS and HSH approaches gives an efficient numerical scheme for estimating Δs in very large chain-like magnetic structures.
Keywords:
π-electrons, graphene molecules, polyradicals, organic ferromagnet, exchange integral, Heisenberg's spin Hamiltonian.
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