Chaos and incoherence in a classical rotation-vibration model of infrared multiple-photon excitation

Journal Article · Mon Feb 29 23:00:00 EST 1988 · Phys. Rev. A; (United States)

DOI:https://doi.org/10.1103/PhysRevA.37.1552· OSTI ID:5464648

Ackerhalt, J R; Milonni, P W

By including rotations in a previously developed generic vibrational model of ir multiple-photon excitation (MPE) (Phys. Rev. Lett. 51, 1259 (1983) and Phys. Rev. A 34, 1211 (1986)) it is found that the combination of chaotic dynamics and rotational averaging leads to fluence-dependent absorption and removes the sensitivity of the results to model-dependent parameters. Therefore, a complete propagation calculation through a molecular medium of this type would show a Beer's law absorption of photons consistent with the vast majority of MPE experiments performed to date, a result which previously was attributed to rate-equation dynamics in the molecular quasicontinuum. In addition, the classical rotation-vibration dynamics observed in this model correlate very well with one's quantum intuition based on a molecule's P-, Q-, and R-branch structure and on the red shift of the vibrational absorption feature with excitation.

• Research Organization: Theoretical Division T-12, Mail Stop J569, Los Alamos National Laboratory, Los Alamos, New Mexico 87545
• OSTI ID: 5464648
• Journal Information: Phys. Rev. A; (United States), Journal Name: Phys. Rev. A; (United States) Vol. 37:5; ISSN PLRAA
• Country of Publication: United States
• Language: English

Related Subjects

640302* -- Atomic
Molecular & Chemical Physics-- Atomic & Molecular Properties & Theory
74 ATOMIC AND MOLECULAR PHYSICS
COLLISIONS
ELECTROMAGNETIC RADIATION
ENERGY LEVELS
ENERGY-LEVEL TRANSITIONS
EXCITATION
EXCITED STATES
FLUX DENSITY
INFRARED RADIATION
MOLECULE COLLISIONS
MOLECULES
MULTI-PHOTON PROCESSES
PARAMETRIC ANALYSIS
PHOTON COLLISIONS
PHOTON-MOLECULE COLLISIONS
RADIATIONS
ROTATIONAL STATES
VIBRATIONAL STATES