All-optical polarization control in time-varying low-index films via plasma symmetry breaking

Abstract: Controlling the polarization state of light with sub-picosecond speed and subwavelength precision remains a key challenge for next-generation nanophotonic devices. Conventional methods such as birefringent crystals, liquid crystals, or electro-optic Pockels cells are limited in speed, compactness, and energy efficiency. While structured materials and two-dimensional heterostructures offer potential for on-chip ultrafast performance, achieving all-optical control remains an open problem. Here we introduce an all-optical scheme that employs femtosecond pumping of low-index, subwavelength isotropic films to achieve ultrafast control over birefringence, dichroism, and optical activity within a single material platform. When the material is probed near its crossover wavelength, linearly polarized pumping induces a transient phase retardation up to 0.1{\pi} per micrometer, accompanied by a dichroic absorption ratio of approximately twenty. Under circularly polarized excitation, the probe experiences nonreciprocal optical activity, leading to polarization rotation of about 1.1 degrees per micrometer. A universal hydrodynamic model quantitatively reproduces these effects and attributes them to pump-induced symmetry breaking in the photoexcited carrier plasma. This symmetry breaking enables coupling between orthogonal probe polarization components, mediated by a modified time-dependent damping term, which connects to the inverse Faraday effect induced by a circularly polarized pump. Our combined experimental and theoretical study establishes a reconfigurable, deep-subwavelength polarization-control mechanism operating on sub-picosecond timescales, suitable for compact ultrafast modulators, dynamic metasurfaces, and tunable nonreciprocal photonic devices, with implications for quantum optics, ultrafast logic, and time-resolved sensing.