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Physical Review A

Population transfer through the continuum: ir excitation of HeH+

Phu Ngoc Tran

Published Feb 1, 1999• 21 citations
Publisher

Abstract

We study the ir excitation of ${\mathrm{HeH}}^{+}$ 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%.

DOI
10.1103/physreva.59.1444

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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%.
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.
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 have solved the time-dependent Schr\"odinger equation to analyze the time evolution of a hydrogen atom, initially in its ground 1s state, interacting with a one- or two-color linearly polarized laser pulse which is tuned close to a two-photon resonance with the 2s metastable state. The two-photon transition therefore does not involve an intermediate resonance state. Using a suitable combination of two laser pulses of different frequencies, population can be transferred from the 1s state to the 2s state via the continuum. In both the single-color and the two-color cases, a maximum amount of 17% of population can be found in the 2s state at the end of the pulse. We compare and interpret our results in terms of the time-independent Floquet eigenvalues. The system can also be modeled by an ``essential states'' two-level atom with decay. Both the Floquet and the time-dependent solutions are compared with the model predictions. The model allows systematic optimization studies for population transfer under a wide range of laser pulse parameters.
The population transfer in a $\ensuremath{\Lambda}$-like system, with intermediate states belonging to the continuous spectrum, is investigated in the case in which continuum-continuum and nonresonant transitions must be taken into account. The two phenomena are shown to essentially influence the dynamics of the system, in particular the final populations of the discrete states. The transfer probability can be increased if the two components of the pulse are shifted in time in a counterintuitive way, but unlike in the typical case of STIRAP, it is an oscillating function of the time delay.
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.
Population transfer in three-level atomic systems with high efficiency and selectivity is desirable for practical applications in laser spectroscopy, trace analysis, and isotope separation. The effective excitation method for achieving this population transfer in three-level atomic systems using coherent two-photon excitation with two optimally detuned counterpropagating pulsed lasers, initially investigated analytically assuming monochromatic lasers and Doppler-free systems, is studied numerically by solving the density matrix equations incorporating finite laser linewidth and effective Doppler width. A three-level Yb system is chosen for illustration of numerical results. The effects of laser linewidth and effective Doppler width on the values of optimal detunings and maximum third-level population are discussed.