Moderately strong pump-induced ultrafast dynamics in solution

•The pulse intensity in transient absorption spectrum are experimentally studied.•The higher nonlinear susceptibility responses are observed.•The resonant impulsive stimulated Raman scattering.•New dynamics information in strong pump field.

The transient transmittance spectra of laser dye IR144 in methanol were investigated experimentally in the moderately strong pump-probe field. Observed emission spectra in the red edge of the incident-field bandwidth, created by resonant impulsive stimulated Raman scattering (RISRS), display significant nonlinear intensity dependence as the pulse intensity increases. Dynamic perspectives of RISRS spectra can be understood well in a wavepacket picture. The excitation of high vibrational levels in the ground electronic state leading to the redshift of emissions presents high dependence of the pump-pulse intensity and ultrafast dynamical features, mapping the spatial overlap and separation of ground and excited wave functions and resolving the ultrafast vibrational relaxation in the femtosecond regime.

Graphical abstractModerately strong pump pulse is applied to the transient absorption spectrum. The pump and dump processes (resonant impulsive stimulated Raman scattering) finished in one single pump pulse in moderately strong regime make the observation of high-lying excited state dynamics possible.Download high-res image (52KB)Download full-size image