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Title: Realistic vs sudden turn-on of natural incoherent light: Coherences and dynamics in molecular excitation and internal conversion

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 S{sub 0} → S{sub 2}/S{sub 1} internal conversion process in pyrazine is used as an example throughout. Implications for studies of natural light harvesting systems are noted.
Authors:
;  [1]
  1. Chemical Physics Theory Group, Department of Chemistry, and Center for Quantum Information and Quantum Control, University of Toronto, Toronto, Ontario M5S 3H6 (Canada)
Publication Date:
OSTI Identifier:
22493412
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 143; Journal Issue: 24; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; COMPARATIVE EVALUATIONS; ELECTROMAGNETIC PULSES; ENERGY LEVELS; EXCITATION; INTERNAL CONVERSION; MIXED STATE; MIXED STATES; PYRAZINES; VISIBLE RADIATION