Abstract
We demonstrate theoretically and experimentally that the Gouy phase of a focused laser beam may be used to control the photoinduced reactions of a polyatomic molecule. Quantum mechanical interference between one- and three-photon excitation of vinyl chloride produces a small phase lag between the dissociation and ionization channels on the axis of the molecular beam. Away from the axis, the Gouy phase introduces a much larger phase lag that agrees quantitatively with theory without any adjustable parameters.
Highlights
It is an axiom of quantum mechanics that the probability of an event may be calculated by adding the probability amplitudes of all independent paths connecting the initial and final states and taking the modulus squared of that sum [1]
Where PSm is the n-photon transition probability, PSn is the m-photon probability, and PSmn is the amplitude of the interference term [9]
The molecular phase may arise, for example, from coupling of electronic continua, from a resonant state embedded in the continuum [12], or from an intermediate resonant state [13]
Summary
It is an axiom of quantum mechanics that the probability of an event may be calculated by adding the probability amplitudes of all independent paths connecting the initial and final states and taking the modulus squared of that sum [1]. Chen and Elliott [21] demonstrated that the modulation of the signal produced by one- and three-photon ionization of mercury atoms undergoes a phase shift as the probed region passes through the focal point of the laser beams.
Sign-in/Register to view highlights & summary Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a callDisclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.
