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A novel polarization-modulation transient method has been developed forstudying fast anisotropic relaxation in electronic excited states of polyatomicand biologically relevant molecules under excitation with femtosecond laserpulses. The method is based on the modulation of pump beam polarization with aphoto-elastic modulator and detection of an anisotropic contribution to thetransient signal by a highly-sensitive demodulation balanced scheme. The methodwas tested on aqueous solution of coenzyme NADH(nicotin-amideadenine-dinucleotide) pumped at 360 nm and probed at 720 nm.Anisotropic vibrational relaxation and rotational diffusion have been observedin the subpicosecond time domain. The method significantly enhances theaccuracy of transient measurements and allows for recording of high-qualitysignals at low energy (a nJ) pump pulses.

Ultrafast polarization-modulation transient spectroscopy to study electronic excited state dynamics in solutions and cells