Use of the spatial phase of a focused laser beam to yield mechanistic information about photo-induced chemical reactions

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Two-pathway quantum mechanical interference was used to control the photoionization and photodissociation of a number of polyatomic molecules. The phase lag between different pairs of products obtained from acetone and dimethyl sulfide was altered by translating the focus of the laser beam along an axis normal to the molecular beam axis. This effect was derived quantitatively from the spatial Gouy phase of the laser beam. Details of the chemical reaction mechanisms were deduced from the channel phase lags, obtained when the laser was focused on the axis of the molecular beam, and from the variation of the phase lag produced by axial translation of the laser focus.