Electronic and vibrational processes in absorbing liquids in femtosecond laser sub- and filamentation regimes: ultrasonic and optical characterization

The ultrasonic characterization of the propagation of femtosecond laser pulses in pure transparent water and colored phenol-red dye solutions at variable concentrations indicates their thermoacoustic pressure generation due to intrinsic multi-photon absorption in the low-power sub-filamentation regime and sub-linear pressure response of sub-critical plasma via free-carrier absorption in the filamentation regime. Multi-photon absorption appears to be concentration dependent for water and dye solutions, while plasma absorption demonstrates a universal trend for all these liquids. In the filamentation regime, through the non-linear laser-matter interactions, not only new optical frequencies (intense white-light supercontinua) were generated, but supercontinuum-based ultrafast broadband spectroscopy in the filaments also revealed many additional transient absorption bands of the dye molecules, induced via power-dependent and concentration-independent stimulated Raman scattering. (letter)