Nonlinear spectroscopy of high-spin fluctuations

Abstract

We investigate theoretically and experimentally fluctuations of high spin (S > 1/2) beyond the linear response regime and demonstrate dramatic modifications of the spin noise spectra in the high power density probe field. Several effects related to an interplay of high spin and perturbation are predicted theoretically and revealed experimentally, including strong sensitivity of the spin noise spectra to the mutual orientation of the probe polarization plane and magnetic field direction, appearance of high harmonics of the Larmor frequency in the spin noise and the fine structure of the Larmor peaks. We demonstrate the ability of the spin-noise spectroscopy to access the nonlinear effects related to the renormalization of the spin states by strong electromagnetic fields.