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Physical Review A

Selective excitation via the continuum and suppression of ionization

C. E. Carroll, F. T. Hioe

Published Jan 1, 1993• 38 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.47.571

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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.
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.
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.
We consider the coherent population trapping effect with a train of ultrashort pulses in a $\ensuremath{\Lambda}$-type system with two bound states and a continuum replacing the upper state. Population transfer to the continuum can be totally suppressed provided that the splitting between the bound states is a multiple of the pulse repetition rate. Compared to the traditional case with only two laser fields coupling the bound states to the continuum, CPT with a pulse train allows one to avoid incoherent population losses due to interaction of the fields with ``wrong'' transitions, which results in only partial suppression of ionization. A method of suppression of excited-state absorption of pumping radiation in laser crystals, with pumping in the form of the pulse train, is proposed. As a particular example pumping dynamics of a Ti3+:YAlO3{\mathrm{Ti}}^{3+}:{\mathrm{YAlO}}_{3}Ti3+:YAlO3​ crystal using this technique is numerically analyzed.
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 propose a technique which produces nearly complete ionization of the population of a discrete state coupled to a continuum by a two-photon transition via a lossy intermediate state whose lifetime is much shorter than the interaction duration. We show that using counterintuitively ordered pulses, as in stimulated Raman adiabatic passage (STIRAP), wherein the pulse coupling the intermediate state to the continuum precedes and partly overlaps the pulse coupling the initial and intermediate states, greatly increases the ionization signal and strongly reduces the population loss due to spontaneous emission through the lossy state. For strong spontaneous emission from that state, however, the ionization is never complete because the dark state required for STIRAP does not exist. We demonstrate that this drawback can be eliminated almost completely by creating a laser-induced continuum structure (LICS) by embedding a third discrete state into the continuum with a third control laser. This LICS introduces some coherence into the continuum, which enables a STIRAP-like population transfer into the continuum. A highly accurate analytic description is developed and numerical results are presented for Gaussian pulse shapes.