Novel dopant-free ferromagnetic Mott-<i>like</i> insulator and high-energy correlated-plasmons in unconventional strongly correlated <i>s</i> band of low-dimensional gold

Ferromagnetic insulators and plasmons have attracted a lot of interest due to their rich fundamental science and applications. Recent research efforts have been made to find dopant-free ferromagnetic insulators and unconventional plasmons independently both in strongly correlated electron systems. However, our understanding of them is still lacking. Existing dopant-free ferromagnetic insulator materials are mostly limited to complex d- or f-systems with extremely low Curie temperature, low-symmetry structure, and strict growth conditions on specific substrates, limiting their compatibility with industrial applications. Unconventional plasmon is, on the other hand, a quasiparticle that originates from the collective excitation of correlated-charges, yet they are rarely explored, particularly in ferromagnetic insulator materials. Herewith, we present a novel, room temperature dopant-free ferromagnetic Mott-like insulator with a high-symmetry structure in unconventional strongly correlated s band of low-dimensional highly oriented single-crystal gold quantum dots (HOSG-QDs) on MgO(001). Interestingly, HOSG-QDs show new high-energy correlated-plasmons with low-plasmonics-loss. With a series of state-of-the-art experimental techniques, we find that the Mott-insulating state is tunable with surprisingly strong spin-splitting and spin polarization accompanied by strong s–s transitions, disappearance of Drude response, and generating new Mott-like gap. Supported with a series of theoretical calculations, the interplay of quantum confinement, many-body electronic correlations, and hybridizations tunes electron–electron correlations in s band and determines the ferromagnetism, Mott-like insulator, and high-energy correlated-plasmons. Our result shows a new class of room temperature dopant-free ferromagnetic Mott-like insulator and high-energy correlated-plasmons with low-loss in strongly correlated s band and opens unexplored applications of low-dimensional gold in spin field-effect transistors and plasmonics.