Optimally controlled five-laser infrared multiphoton dissociation of HF

Journal Article · Tue Mar 15 04:00:00 EST 1994 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.466305· OSTI ID:143262

Kaluza, M; Muckerman, J T ^[1]; Gross, P; Rabitz, H ^[2]

---

1. Chemistry Department, Brookhaven National Laboratory, Upton, New York 11973 (United States)
2. Department of Chemistry, Princeton University, Princeton, New Jersey 08544 (United States)

Simulations of the quantum dynamics of the HF molecule immersed in a field of five overlapping, intense, linearly polarized, infrared laser pulses of subpicosecond duration are performed. The HF molecule, initially in its ground state, is modeled as a rotating oscillator interacting with a classical laser field {ital via} electric dipole interaction. Realistic potential and dipole functions are used. Optimal overlaps of the five laser pulses, as well as the optimal carrier frequencies of the laser pulses, are found which maximize the HF dissociation yield. A maximal yield of 45% in a single combined pulse is achieved using the best available potential and dipole moment functions. The optimal infrared multiphoton dissociation pathway for the HF molecule includes a series of the {Delta}{ital v}=1 vibrational-rotational transitions followed by a series of {Delta}{ital v}{ge}2 vibrational-rotational transitions. The latter is necessary as a consequence of the vanishing {Delta}{ital v}=1 transition moment around {ital v}=12. In the {Delta}{ital v}=1 regime, both {ital P} and {ital R} branch transitions are found to be important. The angular distribution of the dissociative flux is computed. Robustness of the results with respect to changes in the interatomic potentials, dipole functions and reduced mass, as well as to changes in laser pulse parameters (carrier frequencies, timings, phases, field amplitudes, and pulse durations) is investigated.

• OSTI ID: 143262
• Journal Information: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 6 Vol. 100; ISSN JCPSA6; ISSN 0021-9606
• Country of Publication: United States
• Language: English

Related Subjects

40 CHEMISTRY
DIPOLE MOMENTS
DISSOCIATION
GROUND STATES
HYDROFLUORIC ACID
INFRARED RADIATION
LASER RADIATION
MULTI-PHOTON PROCESSES
OPTIMIZATION
POLARIZATION
PULSES
SIMULATION
YIELDS