Influence of heteroatom doping on hyperfine physics in graphene nanostructures

Recent developments in the field of on-surface synthesis (OSS) strategies have led to a surge in the fabrication of atomically perfect triangular flakes of nanographenes with increasing size. Additionally, the insertion of heteroatoms (nitrogen, boron, deuterium), or functional groups has been found to alter the electronic and magnetic properties of these nanographenes. We explore the effect of such heteroatom insertions on the physics of hyperfine interaction (HFI) in these molecular magnets. Using all-electron density functional theory (DFT) calculations such as ORCA, we report the hyperfine tensors for molecules such as the nitrogen-doped triangulenes ([n]-aza triangulenes) as well as boron-doped graphene nanoflakes. Our results indicate appreciable modifications in the magnitudes of hyperfine splitting for the $^{13}$C and $^{1}$H atoms in the presence of the dopants. We also discuss some implications of reported HFI for electron-spin decoherence and spin-dephasing times for application in spin-qubit-based operations.