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Physical Review A

Effect of rotations on stabilization in high-intensity photodissociation of H2+

Eric E. Aubanel, André Conjusteau, André D. Bandrauk

Published Dec 1, 1993• 59 citations
Publisher

Abstract

Photodissociation probabilities of rotationless ${\mathrm{H}}_{2}^{+}$ at \ensuremath{\lambda}=769 nm, from numerical solutions of the time-dependent Schr\"odinger equation, exhibit minima which are attributed to trapping in one- and three-photon field-induced potential wells, leading to molecular stabilization. Rotational excitations are shown to destroy the three-photon stabilization, whereas the one-photon trapping and stabilization of the bound molecular states at high intensities can persist in the presence of rotational excitation.

DOI
10.1103/physreva.48.r4011

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Photodissociation probabilities of rotationless H2+{\mathrm{H}}_{2}^{+}H2+​ at \ensuremath{\lambda}=769 nm, from numerical solutions of the time-dependent Schr"odinger equation, exhibit minima which are attributed to trapping in one- and three-photon field-induced potential wells, leading to molecular stabilization. Rotational excitations are shown to destroy the three-photon stabilization, whereas the one-photon trapping and stabilization of the bound molecular states at high intensities can persist in the presence of rotational excitation.
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The stabilization of a one-dimensional delta potential model atom under the influence of a high frequency, short laser pulse is investigated, through both an ab initio numerical integration of the time-dependent Schrödinger equation and a Floquet calculation in the single-dressed-state approximation. Provided the intensity is not too high, the variation of the photodetachment probability is explained by adiabatic stabilization and its oscillating behaviour by that of the Floquet rate of photodetachment.
Molecular ions that are generated by chemical reactions with trapped atomic ions can serve as an accessible testbed for developing molecular quantum technologies. On the other hand, they are also a hindrance to scaling up quantum computers based on atomic ions, as unavoidable reactions with background gases destroy the information carriers. Here, we investigate the single- and two-photon dissociation processes of single CaOH+ molecular ions co-trapped in Ca+ ion crystals using a femtosecond laser system. We report the photodissociation cross section spectra of CaOH+ for single-photon processes at λ = 245-275 nm and for two-photon processes at λ = 500-540 nm. Measurements are interpreted with quantum-chemical calculations, which predict the photodissociation threshold for CaOH+ → Ca+ + OH at 265 nm. This result can serve as a basis for dissociation-based spectroscopy for studying the internal structure of CaOH+. The result also gives a prescription for recycling Ca+ ions in large-scale trapped Ca+ quantum experiments from undesired CaOH+ ions formed in the presence of background water vapor.
The Schr\"odinger equation in the rotating-wave approximation has been solved nonperturbatively to study the temporal behavior of the occupation probabilities of different levels of a four-level atom interacting with four arbitrarily intense laser fields, such that the frequency of one of them equals the sum of the other three. The three-photon-excitation population dynamics, which is already complex, is strongly modified by one-photon excitation and detunings. Under certain conditions the three-photon excitation traps the population in the state initially populated; the population starts flowing into other states when one-photon excitation is also operative.
The process of resonant multiphoton ionization of a hydrogen atom in the ground 1 s state is studied by direct numerical integration of the nonstationary Schrödinger equation for a quantum system in an electromagnetic field. The dependence of photoionization probability on the radiation intensity is found to be nonmonotonic. It is established that the minima of ionization correspond to multiphoton resonances between the ground state and one of the excited (Rydberg) atomic states perturbed by the laser field. It is shown that ionization is suppressed due to rearrangement of Rydberg states in a strong electromagnetic field and is accompanied by efficient Raman Λ transitions, which connect a set of closely lying Rydberg states via the continuum.