Transient grating spectroscopy of β-carotene pumped with spectrally chirped pulses

Abstract

Abstract Nonlinear optical responses of β-carotene were investigated upon excitation using chirped pulses. We especially focus on spectrally resolved transient grating (TG) signals to discuss the influence of the spectral chirp over a wide spectral range. A significant change in the TG signal was observed when negatively chirped pulses were used. The experimental results were qualitatively reproduced by employing the Brownian oscillator model. The relationship between the wave packet motion in the excited state and spectral chirp is discussed. It is concluded that the third order nonlinear optical response reflects the competition between the spectral chirp and the energy separation of the potential curves.