A concept
of spin plasmon, a collective mode of spin-density, in
strongly correlated electron systems has been proposed since the 1930s.
It is expected to bridge between spintronics and plasmonics by strongly
confining the photon energy in the subwavelength scale within single
magnetic-domain to enable further miniaturizing devices. However,
spin plasmon in strongly correlated electron systems is yet to be
realized. Herein, we present a new spin correlated-plasmon at room
temperature in novel Mott-like insulating highly oriented single-crystalline
gold quantum-dots (HOSG-QDs). Interestingly, the spin correlated-plasmon
is tunable from the infrared to visible, accompanied by spectral weight
transfer yielding a large quantum absorption midgap state, disappearance
of low-energy Drude response, and transparency. Supported with theoretical
calculations, it occurs due to an interplay of surprisingly strong
electron–electron correlations, s–p hybridization and
quantum confinement in the s band. The first demonstration of the
high sensitivity of spin correlated-plasmon in surface-enhanced Raman
spectroscopy is also presented.