Analysis of complex molecular dynamics in an organic liquid by polarization selective subpicosecond transient grating experiments

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Abstract
We present a subpicosecond time resolved polarization selective transient grating (TG) investigation of pentylcyanobiphenyl (5CB) in its isotropic liquid phase. This system shows complex molecular dynamics with various contributions to the TG signal. With an excitation wavelength λexc=665 nm one induces an anisotropy in the sample from the electronic and nuclear Kerr effects. Exciting with λexc=575 nm generates an excited state grating because of two photon absorption. Solvent relaxation around the excited molecule on a few ps time scale is observed because it spectrally shifts the excited state–excited state transition which is monitored by the TG signal. In addition, radiationless relaxation leads to local heating of the sample in a spatial pattern which mimics the optical interference pattern which established the TG. The heating generates an acoustic standing wave. It is demonstrated that with a single TG setup, polarization selection allows separation and identification of all of the above-mentioned physical processes as they are characterized by different symmetries of the nonlinear susceptibility tensor χ(3).