Intramolecular Vibration Energy-Transfer-Driven Cascaded Stimulated Raman Scattering and Four-Wave Mixing in Benzene Series.

Cascaded stimulated Raman scattering (SRS) of benzene, bromobenzene, chlorobenzene, ethylbenzene, and toluene was investigated by a pulsed Nd:YAG laser with 532 nm wavelength. The results showed that the third-order Stokes SRS of the ring skeleton vibration (CC at 3006 cm-1) accompanied by another higher-frequency Stokes SRS of the CH stretching vibration (at 3066 cm-1), which arose only when the third-order Stokes SRS of the ring skeleton was produced, can be attributed to the vibration energy transfer between vibration energy levels of CC and CH. The Stokes and anti-Stokes SRS rings, which originated from the intramolecular energy-transfer-enhanced four-wave mixing (FWM) processes, can be observed only in the forward direction along different angles apart from the pump beam direction. The phenomenon also existed in other derivatives of benzene. We propose the intramolecular energy-transfer-enhanced SRS for the first time, which can be used for a broadband Raman laser.