Two-color pulsed laser excitation of dipolar molecules: Absolute laser carrier-phase effects

Journal Article · Fri Nov 01 04:00:00 EST 2002 · Physical Review. A

DOI:https://doi.org/10.1103/PhysRevA.66.053404· OSTI ID:20632318

Brown, Alex ^[1]

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1. Department of Chemistry, University of Western Ontario, London, Ontario, N6A 5B7 (Canada)

The excitation of a two-level dipolar (d{ne}0) molecule with two Gaussian pulsed lasers is examined theoretically for the case where one laser's frequency is tuned close to the energy level separation (pump laser) while the second laser's frequency is extremely small (probe laser). The final excited state populations are shown to depend on the probe laser's absolute carrier phase while remaining independent of the pump laser's absolute carrier phase. They do not depend on the relative phase difference between the two laser fields as in many other pump-probe scenarios. The absolute carrier-phase effect is negligible for nondipolar (d=0) molecules. The probe laser absolute carrier-phase effect arises through the coherent excitation of multiple optical paths from the initial to the final state containing a common number of pump photons (N{sub pump}=1) and a varying number of probe photons. Excited state populations, after the interaction of the pulses with the molecule is complete, are examined as a function of the probe laser's absolute carrier phase for varying field strengths, frequencies, and pulse durations in order to verify the source of the probe laser absolute carrier-phase effect and to determine the conditions needed to most readily detect it.

• OSTI ID: 20632318
• Journal Information: Physical Review. A, Journal Name: Physical Review. A Journal Issue: 5 Vol. 66; ISSN 1050-2947; ISSN PLRAAN
• Country of Publication: United States
• Language: English

Related Subjects

74 ATOMIC AND MOLECULAR PHYSICS
EXCITATION
EXCITED STATES
LASER RADIATION
MOLECULES
MULTI-PHOTON PROCESSES
PHOTON-MOLECULE COLLISIONS
PHOTONS
PROBES
PULSES