Chiral correlated-plasmons enhanced Raman optical activity from spin-polarized, correlated <i>s</i> band in highly oriented single-crystalline gold quantum-dots

Abstract

Interactions of chiral light with chiral matter, such as Raman optical activity (ROA) and, independently, spin-polarized materials have attracted a lot of interest for both fundamental science and applications. The ROA, on the one hand, provides information on chiral phonons of molecules. However, the short-lifetime ROA signal in general is extremely weak and requires long exposure times, making it not accessible for many important systems with short lifetime. Materials exhibiting high spin polarization in d or f band, on the other hand, remain very limited even at very low temperature. There has been no report on materials exhibiting spin polarization in s band. Herewith, we report a room temperature, full spin polarization in unconventional, correlated s band of highly oriented single-crystalline gold quantum-dots (HOSG-QDs). Intriguingly, the HOSG-QDs produce a chiral correlated-plasmons enhanced Raman optical activity (CP-ROA) with anomalous ROA enhancement and strong spin-dependent chiral coupling. We then address a fundamental problem in crystal violet. Using spin-polarized HOSG-QDs chips, we observe strong CP-ROA signal, revealing chiral properties. The chiral correlated-plasmons of HOSG-QDs interact with the spin, electronic, and lattice structures of crystal violet, revealing chiral phonons and chiral electronic Raman excitations of crystal violet. Such a strong CP-ROA spectrum is obtained within a minute of measurement and a simple preparation without patterning. Our result shows that the CP-ROA based on a spin-polarized HOSG-QDs is extremely sensitive to the chiral property of phonon and spin and electronic structures and a fast, label-free chiral spectroscopic-based detection.