Noninstantaneous polarization dynamics in dielectric media

Abstract

Third-order optical nonlinearities play a vital role for the generation and characterization of ultrashort optical pulses. One particular characterization method is frequency-resolved optical gating, which can be based on a large variety of third-order nonlinear effects. Any of these variants presupposes an instantaneous temporal response, as it is expected off resonance. In this paper we show that resonant excitation of the third harmonic gives rise to surprisingly large decay times, which are on the order of the duration of the shortest oscillator pulses generated to date. To this end, we measured interferometric third-harmonic frequency-resolved optical gating traces in TiO2 and SiO2, corroborating polarization decay times up to 6.5 fs in TiO2. This effect is among the fastest effects observed in ultrafast spectroscopy. Numerical solutions of the time-dependent Schrodinger equation are in excellent agreement with experimental observations. Our work (experiments and simulations) corroborates that a noninstantaneous polarization decay may appear in the presence of a 3-photon resonance. In turn, pulse generation and characterization in the ultraviolet may be severely affected by this previously unreported effect.