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“ ” Femtosecond Time-Resolved Photoelectron Spectroscopy Outline Introduction of femtosecond TRPES Experimental methods of TRPES Development of TRPES Applications of femtosecond TRPES Future directions Why do we research femtosecond chemistry? Chemical bonds form and break on the femtosecond time scale, and on this time scale of time we can freeze the transition states at configurations never seen before. Even if there is no reactants-to-products transformation-physical change-one is observing the most elementary of all molecular process. Introduction A. H. Zewail was awarded the Nobel prize in chemistry in 1999. “Femtochemistry has fundamentally changed our view of chemical reac- tions. ” Zewail, A. H. J. Phys. Chem. A 2000, 104,5660 Zewail, A. H. et al, Nature 1992, 355, 66. Why do we research femtosecond TRPES? laser-induced fluorescence resonant multiphoton ionization a small region of the reaction coordinate resonant with an electronic transition how? photoelectron spectroscopy 1.1 General aspects of femtosecond TRPES The pump pulse is over, the wave packet χ (Δt), given by eq 1, 1.2 Photoelectron angular distribution (PADs) Within the molecular frame, the symmetries of the outgo- ing electron partial waves are likewise related to the sym- metry of the electronic state undergoing ionization. This can be written as: Гex ? Гμ ? Г+ ? Гe- ? ГTS Гex: the symmetry species of the prepared excited state Гμ: the dipole operator Г+: the ion state Гe-: the symmetry species of the outgoing electron ГTS: the totally symmetric species 2.1 How to complete femtosecond TRPES? femtosecond pump-probe pulse !!! Experiment 2.2 Schematic of femtosecond laser 2.3 the detector of Photoelectron spectroscopy Magnetic bottle time-of-flight spectrometer Adv.: high collection efficiency simple, rapid data readout straightforward photoelectron-photoion coincidence meas- urements (PEPICO) Disadv.:
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