Time‐Resolved Pump–Probe Measurement of Optical Rotatory Dispersion in Chiral Metamaterial

Abstract

A plasmonic chiral metamaterial is fabricated from a thin Au film and exhibits static optical rotatory power (ORP) in the visible spectral range. Transient ORP is measured to clarify the temporal development of ORP using a circularly polarized light (CPL) pump beam. Three distinct transient behaviors of ORP are identified, resulting from different energy relaxation processes of hot electrons that occur during a period of a few picoseconds after pumping. Nonthermal hot electrons experience Lorentz force from an inverse Faraday effect and electron–boundary scattering, yielding a pump beam CPL helicity‐dependent transient ORP. Once hot electrons are in thermal equilibrium with the lattice, electron energy is distributed among the occupied states, as described by Fermi–Dirac statistics. Moreover, the transient ORP is independent of pump beam CPL helicity, well explained by the selection rule of electron excitation and two‐temperature model of the electron cooling process. Theoretical analysis of the transient ORP in terms of the energy relaxation of thermal hot electrons is carried out by introducing a temperature‐dependent dielectric function and finite‐difference time‐domain simulation. It is found that the magnitude of ORP at an elevated temperature is reduced to less than that at room temperature, agreeing well with the experimental observation.