Simultaneous Incorporation of Magnetic and Plasmonic Nanocrystals in a Chiral Conducting Polymer Yields Unprecedented Magneto‐Optic Response

The creation of next-generation flexible and conformable magneto-optic (MO) materials with dramatically enhanced Verdet constant will significantly advance technologies, including optical isolation, magnetic quantum spin fluctuation measurements, and cold atom spin coherence probes, while opening new possibilities for mapping weakly emanating magnetic fields from sources, including microelectronics or brain activity. The results presented here show that the natural coupling of electric and magnetic dipoles in a chiral polymer with large optical activity (circular birefringence) is significantly enhanced by combined plasmonic field and magnetic interactions of plasmonic nanostars and magnetic nanoparticles to yield a dramatically increased Verdet constant within an optical path of a few hundred nanometers. A 175 ± 10 nm film of this material produces up to 600 mdeg of relative MO rotation at 510 nm, which translates to a record-high Verdet constant of 3.1 × 10⁷ deg T^-1 m^-1 at 93 K, more than two orders of magnitude higher than the current state of the art MO garnet crystals. The room temperature Verdet constant substantially exceeds that of other thin film nanocomposites reported to date. Manipulation of electric and magnetic coupling offers an unprecedented opportunity to tailor the magnitude, sign, and spectral dispersion of the Verdet constant over a broad range of wavelengths.