Peak power dependence of rovibronic populations below the quasicontinuum during IR multiphoton absorption

Journal Article · Sun Feb 15 04:00:00 EST 1981 · J. Chem. Phys.; (United States)

DOI:https://doi.org/10.1002/chin.198125128· OSTI ID:6635301

Brenner, D M

Rovibronic levels of the ground state of thiophosgene, perturbed by IR multiphoton absorption, are observed under collisionless conditions by laser-induced fluorescence. Evidence is presented that at peak powers of the CO/sub 2/ laser>3 MW/cm/sup 2/ an energy distribution is produced in which the vibrational populations of levels v=0--4,6,8 of the mode ..nu../sub 4/ are depleted or not populated, even though the pumped mode is 2..nu../sub 4/. Only at lower peak powers (longer pulse duration) are population increases observed. Under the latter conditions, it appears that 3..nu../sub 4/ is populated to a smaller extent than (..nu../sub 1/+..nu../sub 3/) to which it is coupled by strong Coriolis interaction. At room temperature no evidence for rotational ''hole burning'' effects during IR pumping are observed in the vibrationless level. The data suggest, in fact, that all rotational levels interact with the laser field, even when thiophosgene is rotationally cooled.

• Research Organization: Department of Chemistry, Brookhaven National Laboratory, Upton, New York 11973
• OSTI ID: 6635301
• Journal Information: J. Chem. Phys.; (United States), Journal Name: J. Chem. Phys.; (United States) Vol. 74:4; ISSN JCPSA
• Country of Publication: United States
• Language: English

Related Subjects

640302* -- Atomic
Molecular & Chemical Physics-- Atomic & Molecular Properties & Theory
74 ATOMIC AND MOLECULAR PHYSICS
ABSORPTION SPECTRA
CARBONIC ACID DERIVATIVES
CORIOLIS FORCE
DATA
ELECTROMAGNETIC RADIATION
ENERGY LEVELS
EXCITED STATES
EXPERIMENTAL DATA
FLUORESCENCE
INFORMATION
INFRARED SPECTRA
LASER RADIATION
LUMINESCENCE
NUMERICAL DATA
ORGANIC CHLORINE COMPOUNDS
ORGANIC COMPOUNDS
ORGANIC HALOGEN COMPOUNDS
PHOSGENE
RADIATIONS
ROTATIONAL STATES
SPECTRA
SULFUR COMPOUNDS
VIBRATIONAL STATES