title: Quantum dynamics experienced by a single molecular eigenstate excited by incoherent light.
abstract: Contrary to conventional wisdom that all dynamics are a result of interference (or "dephasing") between many (at least two) energy eigenstates, we show that when a continuum of states is present, even a single molecular eigenstate undergoes "steady-state" quantum dynamics. Moreover, this type of dynamics can be initiated by incoherent (e.g., solar) light sources. Continua are invariably involved in molecular systems due to a variety of sources such as the ever present bath modes, spontaneously emitted photons; the detachment of electrons, or the dissociation of chemical bonds. Contrary to a single bound energy eigenfunction which is a real ("standing-waves") function that carries no flux and, hence, has no dynamics, a single (complex) continuum energy eigenfunction carries "steady-state" flux given by the group velocity of the energetically narrow wave packet it represents. When this energy eigenfunction is a multimode resonance embedded in a continuum via a chain of intramolecular couplings, this dynamics may be initiated by any (light) source, and is controlled, contrary to coherent wave packet dynamics, by the position of the resonance rather than its width.
authors.affiliation: Departments of Chemistry and Physics, The University of British Columbia, Vancouver, British Columbia V6T 1Z1, Canada and Department of Chemical Physics, The Weizmann Institute of Science, Rehovot 76100, Israel.
authors.forename: Moshe
authors.initials: M
authors.lastname: Shapiro