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Physical Review A

Quantum-state-selective two-photon excitation of multilevel systems assisted by the Stark shift

Bo Y. Chang, Hyeonho Choi, Seokmin Shin, Ignacio R. Solá

Published Jun 6, 2007• 7 citations
Publisher

Abstract

Stark-chirped rapid adiabatic passage [T. Rickes et al., J. Chem. Phys. 113, 534 (2000); A. A. Rangelov et al. Phys. Rev. A 72, 053403 (2005)] has been proposed as a laser scheme that allows the optical excitation of atoms or molecules with high quantum yields. The laser control proceeds via adiabatic passage assisted by dynamic Stark shifts. We propose several extensions of the scheme with alternative sequences, by frequency tuning or by repeating the pulse sequences, in order to achieve fine state selectivity within multilevel structures and adiabatic passage of quantum superposition states. The efficiency and selectivity of the schemes is compared with that achieved by other optical coherent methods.

DOI
10.1103/physreva.75.063405

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Stark-chirped rapid adiabatic passage [T. Rickes et al., J. Chem. Phys. 113, 534 (2000); A. A. Rangelov et al. Phys. Rev. A 72, 053403 (2005)] has been proposed as a laser scheme that allows the optical excitation of atoms or molecules with high quantum yields. The laser control proceeds via adiabatic passage assisted by dynamic Stark shifts. We propose several extensions of the scheme with alternative sequences, by frequency tuning or by repeating the pulse sequences, in order to achieve fine state selectivity within multilevel structures and adiabatic passage of quantum superposition states. The efficiency and selectivity of the schemes is compared with that achieved by other optical coherent methods.
We demonstrate and analyze a novel scheme for complete transfer of atomic or molecular population between two bound states, by means of Stark-chirped rapid adiabatic passage (SCRAP). In this two-laser technique a delayed-pulse laser-induced Stark shift sweeps the transition frequency between two coupled states twice through resonance with the frequency of the population-transferring coupling laser. The delay of the Stark-shifting pulse with respect to the pulse of the coupling-laser Rabi frequency guarantees adiabatic passage of population at one of the two resonances while the evolution is diabatic at the other. The SCRAP method can give a population-transfer efficiency approaching unity. We discuss the general requirements on the intensity and timing of the pulses that produce the Rabi frequency and, independently, the Stark shift. We particularly stress extension to a double-SCRAP technique, a coherent variant of stimulated emission pumping in the limit of strong saturation. We demonstrate the success of the SCRAP method with experiments in metastable helium, where a two-photon transition provides the Rabi frequency.
Traditional two-photon excitation suffers from two difficulties that prevent complete population transfer: dynamic Stark shifts and multiphoton ionization. We describe a technique for overcoming these limitations by using a second field to control dynamic Stark shifts via Stark-chirped rapid adiabatic passage (SCRAP) and simultaneously suppress undesired photoionization via laser-induced continuum structure (LICS). We illustrate this proposed procedure by numerical simulations of two-photon excitation of the metastable 2s2s2s state of hydrogen, showing that efficient excitation can be expected when the two laser pulses are properly crafted.
We show that the technique of Stark-chirped rapid adiabatic passage (SCRAP), hitherto used for complete population transfer between two quantum states, offers a simple and robust method for complete population transfer amongst three states in atoms and molecules. In this case SCRAP uses three laser pulses: a strong far-off-resonant pulse modifies the transition frequencies by inducing dynamic Stark shifts and thereby creating time-dependent level crossings amongst the three diabatic states, while near-resonant and moderately strong pump and Stokes pulses, appropriately offset in time, drive the population between the initial and final states via adiabatic passage. The population transfer efficiency is robust to variations in the intensities of the lasers, as long as these intensities are sufficiently large to enforce adiabatic evolution. With suitable pulse timings the population in the (possibly decaying) intermediate state can be minimized, as with stimulated Raman adiabatic passage (STIRAP). This technique applies to one-photon as well as multiphoton transitions and it is also applicable to media exhibiting inhomogeneous broadening; these features represent clear advantages over STIRAP by overcoming the inevitable dynamical Stark shifts that accompany multiphoton transitions as well as unwanted detunings, e.g., induced by Doppler shifts.
We propose a technique to prepare coherent superpositions of two nondegenerate quantum states in a three-state ladder system, driven by two simultaneous fields near resonance with an intermediate state. The technique, of potential application to the enhancement of nonlinear processes, uses an adiabatic passage assisted by dynamic Stark shifts induced by a third laser field. The method offers significant advantages over alternative techniques: (i) it does not require laser pulses of specific shape and duration and (ii) it requires less intense fields than schemes based on two-photon excitation with nonresonant intermediate states. We discuss possible experimental implementation for enhancement of frequency conversion in mercury atoms.
Selective population transfer in electronic states of dissociative molecular systems is illustrated by adopting a control scheme based on Stark-chirped rapid adiabatic passage (SCRAP). In contrast to the discrete N-level system, dynamical Stark shift is induced in a more complex manner in the molecular electronic states. Wavepacket dynamics on the light-induced potentials, which are determined by the detuning of the pump pulse, can be controlled by additional Stark pulse in the SCRAP scheme. Complete population transfer can be achieved by either lowering the energy barrier along the adiabatic passage or placing the initial wavepacket on a well-defined dressed state suitable for the control. The determination of the pulse sequence is sufficient for controlling population transfer to the target state.
We present extended experimental investigations and numerical studies on coherently driven population inversion in a three-state molecular quantum system by sequential double-Stark-chirped rapid adiabatic passage (SCRAP) (D-SCRAP) and three-state-SCRAP (T-SCRAP). D-SCRAP and T-SCRAP are alternative extensions of SCRAP. In D-SCRAP and T-SCRAP, a $\ensuremath{\Lambda}$-type quantum system is coherently driven by two laser pulses, the pump and Stokes pulses, which are slightly detuned from transition frequencies. A third strong laser pulse induces dynamic Stark shifts of the relevant transitions. If the timing of the three pulses is appropriately chosen, the quantum system is prepared to almost complete population inversion between the two lower states in the $\ensuremath{\Lambda}$-type level scheme. The transfer process is robust with regard to fluctuations of experimental parameters, provided some limitations are met. The paper presents convincing experimental data on D-SCRAP and T-SCRAP, driving efficient and selective population transfer to a highly excited vibrational level in nitrous oxide (NO) molecules. T-SCRAP yields transfer efficiencies of up to 95%. The efficiency of T-SCRAP is almost uneffected by the limited lifetime of the intermediate state in the $\ensuremath{\Lambda}$ system. The paper also presents data on the accurate experimental determination of Rabi frequencies and Stark shifts. This involves measurements of power broadening, Autler-Townes splittings, and Stark-shifted spectral lines in NO molecules. Moreover, we discuss the calibration of absolute transfer efficiences by comparison with stimulated emission pumping. The experimental data are confirmed by extended numerical simulations. The simulations also serve to intensively study the properties and dynamics of D-SCRAP and T-SCRAP.