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Abstract 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 × 10⁷deg T⁻¹m⁻¹at 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. 

Abstract Polymer‐based chiral materials with exceptional optical activity can dramatically impact integrated chiral photonics due to the tunability of their optical responses coupled with ease of fabrication. Realizing these applications requires increasing the absorbance dissymmetry factor. Here, in situ, the synthesis of gold nanostars is introduced in a chiral polymer medium to produce chiral polymer‐anisotropic plasmonic nanocrystal nanocomposites. The optimized nanocomposite shows a tenfold enhancement of dissymmetry factor,g_abs(up to 0.64) and a corresponding 46‐fold augmented circular dichroism (CD) value upon annealing, relative to the annealed pure chiral polymer film. Moreover, the enhancement relative to the non‐annealed polymer‐gold nanostar nanocomposite is strikingly higher: a 35‐fold increase ing_absand a 4272‐fold increase in CD. Based on computational analysis, it is concluded that the local plasmon field enhancement around the crevices and tips of nanostars is mainly responsible for the observed effect which is further supported by a signal enhancement in Surface Enhanced Raman Scattering (SERS). Thus, this study underscores the significant role of close‐range plasmon interactions in altering the chiroptical response of nanocomposite materials and a practical pathway toward the realization of next‐generation integrated photonics and optoelectronic circuitry with photon spin control. 

Oxygen plasma treatment of polydimethylsiloxane (PDMS) induces an ultrathin polyorganosilica (POSi) layer (< 10 nm) on top of a PDMS membrane, leading to excellent H2/gas separation properties and providing a rapid and scalable way to fabricate robust silica membranes compared with conventional high-temperature and time-consuming sol-gel methods. Here, we thoroughly investigate POSi membranes derived from poly(dimethylsiloxane-co-methylhydroxidesiloxane) (poly(DMS-co-MHOS)) containing -SiOH groups that can be more easily converted to silica networks than the -SiCH3 in PDMS. The effect of the polysiloxane structure and plasma treatment conditions (including plasma generating powers, oxygen flowrate, chamber pressure, and treatment time) on the silica chemistry, structure, and H2/CO2 separation properties are systematically determined to derive structure/property relationships. An optimized membrane exhibits H2 permeance of 880 GPU and H2/CO2 selectivity of 67 at 150 ℃, superior to state-of-the-art polymeric membranes. The membrane retains H2/CO2 selectivity as high as 46 when challenged with simulated syngas containing 2.8 mol% water vapor at 150 ℃, demonstrating the potential of these POSi membranes for practical applications.