Optical control of the anisotropy of the orientation of molecules in a liquid

The control of the anisotropy of the orientation of molecules in pure 1,2-dichlorobenzene, C₆H₄Cl₂ at room temperature is demonstrated experimentally. To accomplish the optical control, the medium is exposed to non-resonant excitation with two successive linearly polarized laser pulses with a duration of 60 fs. The state of transient anisotropy is probed with the third pulse by detecting the ultrafast optical Kerr effect via optical heterodyne detection and synchronous demodulation. It is shown that variations in the two parameters, the delay time between two pump pulses, and the angle between the polarization directions of the pump pulses ensure the control of the anisotropy of the orientation of molecules in the subpicosecond region.