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Physical Review A

Source of metastable H(2s) atoms using the Stark chirped rapid-adiabatic-passage technique

Леонід Петрович Яценко, Bruce W. Shore, Thomas Halfmann, Klaas Bergmann, Amichay Vardi

Published Dec 1, 1999• 120 citations
Publisher

Abstract

We propose the use of Stark chirped rapid-adiabatic-passage method, a technique in which the energy of a target state is swept through resonance by a slowly varying dynamic Stark shift to induce complete population transfer from the ground $1s$ state to the metastable $2s$ state of the hydrogen atom. Parasitic ionization processes are strongly reduced by using a two-color excitation scheme. Our detailed numerical calculations show that under judicious choice of pulse parameters, up to 98% of the population can be found in the $2s$ state at the end of the process.

DOI
10.1103/physreva.60.r4237

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Journal of Shaanxi Normal University•Jan 1, 2005•0 citations
We propose the use of Stark chirped rapid-adiabatic-passage method, a technique in which the energy of a target state is swept through resonance by a slowly varying dynamic Stark shift to induce complete population transfer from the ground 1s1s1s state to the metastable 2s2s2s state of the hydrogen atom. Parasitic ionization processes are strongly reduced by using a two-color excitation scheme. Our detailed numerical calculations show that under judicious choice of pulse parameters, up to 98% of the population can be found in the 2s2s2s state at the end of the process.
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 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.
By using Stark-induced adiabatic Raman passage (SARP) with partially overlapping nanosecond pump (532 nm) and Stokes (683 nm) laser pulses, 73% ± 6% of the initial ground vibrational state population of H(2) (v = 0, J = 0) is transferred to the single vibrationally excited eigenstate (v = 1, J = 0). In contrast to other Stark chirped Raman adiabatic passage techniques, SARP transfers population from the initial ground state to a vibrationally excited target state of the ground electronic surface without using an intermediate vibronic resonance within an upper electronic state. Parallel linearly polarized, co-propagating pump and Stokes laser pulses of respective durations 6 ns and 4.5 ns, are combined with a relative delay of ~4 ns before orthogonally intersecting the molecular beam of H(2). The pump and Stokes laser pulses have fluences of ~10 J/mm(2) and ~1 J/mm(2), respectively. The intense pump pulse generates the necessary sweeping of the Raman resonance frequency by ac (second-order) Stark shifting the rovibrational levels. As the frequency of the v = 0 → v = 1 Raman transition is swept through resonance in the presence of the strong pump and the weaker delayed Stokes pulses, the population of (v = 0, J = 0) is coherently transferred via an adiabatic passage to (v = 1, J = 0). A quantitative measure of the population transferred to the target state is obtained from the depletion of the ground-state population using 2 + 1 resonance enhanced multiphoton ionization (REMPI) in a time-of-flight mass spectrometer. The depletion is measured by comparing the REMPI signal of (v = 0, J = 0) at Raman resonance with that obtained when the Stokes pulse is detuned from the Stark-shifted Raman resonance. No depletion is observed with either the pump or the Stokes pulses alone, confirming that the measured depletion is indeed caused by the SARP-induced population transfer from the ground to the target state and not by the loss of molecules from photoionization or photodissociation. The two-photon resonant UV pulse used for REMPI detection is delayed by 20 ns with respect to the pump pulse to avoid the ac Stark shift originating from the pump and Stokes laser pulses. This experiment demonstrates the feasibility of preparing a large ensemble of isolated molecules in a preselected single quantum state without requiring an intermediate vibronic resonance.
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.
The stark-chirped rapid adiabatic passage (SCRAP) is analyzed, which can give a complete transfer of atomic or molecular population between two bound states in the two level states and Λ(-three)-level state, by means of level-crossing technique and dressed states theory. SCRAP uses two laser pulses: a nearly-resonant pump laser pulse drives the population between a ground state and an excited state, and an intense far-off-resonance Stark laser pulse modifies the transition frequency and resonates with the Bohr transition frequency for two level crossings. A population-transfer maximal efficiency approaching unity is provided from the ground state to the excited state, when the delay of the Stark-shifting pulse with respect to the pulse of the coupling-laser frequency is appropriate and guarantees the pump pulse is strong at one of these crossings and is weak at second one.