Optical heterodyne detected accumulated acoustic grating responses in near supercritical fluids

A novel third-order polarization effect due to an accumulated optical heterodyne detected (OHD) transient acoustic grating response in near critical fluids was observed and experimentally characterized. Femtosecond pump-probe responses in near critical CO2 and CHF3 illustrate this phenomenon. This large optically generated acoustic response due to electrostrictive coupling appears only when pump and probe pulses are temporally overlapped and is pi out-of-phase with the normal optical Kerr effect (OKE) birefringent signal. The local oscillator, the laser intensity, and the modeled experimental repetition rate dependence identify the accumulated heterodyne origin of these responses. The observed OHD accumulated acoustic birefringent signal is inversely dependent on sound velocity to the fifth power. A corresponding sound velocity dependent dichroic (in-phase) response was also observed for these electronically nonresonant samples. The accumulated effect described here may have applications for the design of efficient modulators and as a simple and sensitive experimental technique for the measurement of near critical fluid thermodynamic and acoustic parameters.