title: Realistic vs sudden turn-on of natural incoherent light: Coherences and dynamics in molecular excitation and internal conversion.
abstract: Molecular excitation with incoherent light is examined using realistic turn-on time scales, and results are compared to those obtained via commonly used sudden turn-on, or pulses. Two significant results are obtained. First, in contrast to prior studies involving sudden turn-on, realistic turn-on is shown to lead to stationary coherences for natural turn-on time scales. Second, the time to reach the final stationary mixed state, known to result from incoherent excitation, is shown to depend directly on the inverse of the molecular energy level spacings, in both sudden and realistic turn-on cases. The S0 → S2/S1 internal conversion process in pyrazine is used as an example throughout. Implications for studies of natural light harvesting systems are noted.
authors.affiliation: Chemical Physics Theory Group, Department of Chemistry, and Center for Quantum Information and Quantum Control, University of Toronto, Toronto, Ontario M5S 3H6, Canada.
authors.forename: Timur
authors.initials: T
authors.lastname: Grinev
authors.affiliation: Chemical Physics Theory Group, Department of Chemistry, and Center for Quantum Information and Quantum Control, University of Toronto, Toronto, Ontario M5S 3H6, Canada.
authors.forename: Paul
authors.initials: P
authors.lastname: Brumer