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Physical Review A

Selective excitation and structure in the continuum

C. E. Carroll, F. T. Hioe

Published Dec 1, 1996• 37 citations
Publisher

Abstract

We show that efficient transfer of molecules or atoms from one bound state to another is possible via the continuum in some cases, using two overlapping laser pulses. The structure of the continuum determines the pulse delay, laser frequencies, and laser intensities that should be used. We present simple formulas that relate the optimum values of pulse intensities, pulse separation, and detuning; these estimates can be used as a guide. More detailed calculations give quantitative results for two specific potentials. \textcopyright{} 1996 The American Physical Society.

DOI
10.1103/physreva.54.5147

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We show that efficient transfer of molecules or atoms from one bound state to another is possible via the continuum in some cases, using two overlapping laser pulses. The structure of the continuum determines the pulse delay, laser frequencies, and laser intensities that should be used. We present simple formulas that relate the optimum values of pulse intensities, pulse separation, and detuning; these estimates can be used as a guide. More detailed calculations give quantitative results for two specific potentials. \textcopyright{} 1996 The American Physical Society.
Transfer of molecules or atoms from an initial state to a certain final state is often wanted, and use of a single laser may be impractical. Transfer via an intermediate state of higher energy has been demonstrated, using laser pulses that overlap in time. We have proposed using the continuum in place of the intermediate state, and encouraging results have been computed for a simple model. Our latest calculations show the effects of operating this scheme near the bottom of the continuum or near a resonance having the Fano shape, and the effects of laser-driven continuum-continuum transitions.
Two laser pulses that overlap in time have been successfully used for coherent excitation of a molecule or atom to a desired state. An intermediate state that is at or near resonance with the laser frequencies has been used in past experiments and calculations. Here we replace this intermediate state by a continuum of intermediate states. An analytic solution of a simple model suggests that the continuum can be used in such an excitation scheme, provided that the laser pulses are arranged in the so-called counterintuitive order. We use a special case of this solution to relate this work to ionization suppression and coherent population trapping.
We present a remarkable analytic result which suggests that a continuum can be used as an intermediary for a significant transfer of population from one discrete state to another discrete state in a stimulated Raman transition. The population transfer is accomplished by employing two laser pulses that overlap in time, arranged in the so-called counterintuitive order. That a continuum can be used for population transfer is shown here for the first time. It promises to open up more channels for selective coherent excitation of atoms or molecules.
The theory of one- and two-photon dissociation processes with strong laser pulses for slowly varying multiple continua (‘‘direct’’ dissociation) is developed. Closed form expressions for the state preparation and evolution during and after the excitation pulse are derived. We show how saturation of the photodissociation process as a function of the laser power sets in. We also show that for direct dissociation, the fragment state distribution is independent of the laser power. The dependence of spontaneous emission during dissociation (continuum Raman and resonance fluorescence) on the pulse intensity is studied. The formulation is extended to treating resonantly enhanced two-photon dissociation with strong laser pulses. Closed-form expressions for slowly varying pulses and slowly varying continua are derived. Using these expressions, the existence of adiabatic passage to the continuum (APC) by which a system executes a complete population transfer from an initial bound state to the continuum by following two guiding light pulses is established. A simple iterative scheme for going beyond the adiabatic approximation is introduced.
We present experimental and theoretical results of a detailed study of laser-induced continuum structures (LICS's) in the photoionization continuum of helium out of the metastable state 2s1S0.2s{}^{1}{S}_{0}.2s1S0​. The continuum dressing, with a 1064-nm laser, couples the same region of the continuum to the 4s1S04s{}^{1}{S}_{0}4s1S0​ state. The experimental data, presented for a range of intensities, show pronounced ionization suppression (by as much as 70% with respect to the far-from-resonance value) as well as enhancement, in a Beutler-Fano resonance profile. This ionization suppression is a clear indication of population trapping mediated by coupling to a continuum. We present experimental results demonstrating the effect of pulse delay upon the LICS's, and for the behavior of LICS's for both weak and strong probe pulses. Simulations based upon numerical solution of the Schr\"odinger equation model the experimental results. The atomic parameters (Rabi frequencies and Stark shifts) are calculated using a simple model-potential method for the computation of the needed wave functions. The simulations of the LICS profiles are in excellent agreement with experiment. We also present an analytic formulation of pulsed LICS's. We show that in the case of a probe pulse shorter than the dressing one, the LICS profile is the convolution of the power spectra of the probe pulse with the usual Fano profile of stationary LICS's. We discuss some consequences of deviation from steady-state theory.
We study the ir excitation of HeH+{\mathrm{HeH}}^{+}HeH+ using the counterintuitive arrangement of two pulsed lasers with the continuum as the intermediate state. The time-dependent Schr\"odinger equation describing the system is integrated numerically using the split-operator technique. We examine the maximum population transfer as a function of the pulse separation, pulse width, relative pulse strength, two-photon detuning, and relative position of the intermediate continuum state. The largest population transfer found is 63%.