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Title: Quantum state specific reactant preparation in a molecular beam by rapid adiabatic passage

Highly efficient preparation of molecules in a specific rovibrationally excited state for gas/surface reactivity measurements is achieved in a molecular beam using tunable infrared (IR) radiation from a single mode continuous wave optical parametric oscillator (cw-OPO). We demonstrate that with appropriate focusing of the IR radiation, molecules in the molecular beam crossing the fixed frequency IR field experience a Doppler tuning that can be adjusted to achieve complete population inversion of a two-level system by rapid adiabatic passage (RAP). A room temperature pyroelectric detector is used to monitor the excited fraction in the molecular beam and the population inversion is detected and quantified using IR bleaching by a second IR-OPO. The second OPO is also used for complete population transfer to an overtone or combination vibration via double resonance excitation using two spatially separated RAP processes.
Authors:
; ; ; ;  [1]
  1. Laboratoire de Chimie Physique Moléculaire, Ecole Polytechnique Fédérale de Lausanne, Lausanne (Switzerland)
Publication Date:
OSTI Identifier:
22255250
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 140; Journal Issue: 3; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; EXCITATION; EXCITED STATES; INFRARED RADIATION; MOLECULAR BEAMS; PARAMETRIC OSCILLATORS; POPULATION INVERSION; PYROELECTRIC DETECTORS; QUANTUM STATES