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Journal of Physics B Atomic Molecular and Optical Physics

Population transfer via an autoionizing state with temporally delayed chirped laser pulses

Emmanuel Paspalakis, P. L. Knight

Published Jun 28, 1998• 14 citations
Publisher

Abstract

We study the possibility of transferring population between two bound atomic or molecular states via an autoionizing state. Conditions for efficient transfer are given and the effects of the AC Stark shifts, the Fano parameters and the incoherent channels of ionization are explored. An adiabatic analytic solution which helps in the understanding of the behaviour of the system is also given. Efficient transfer is realized by using both a counterintuitive pulse sequence and concurrent laser pulses.

DOI
10.1088/0953-4075/31/12/011

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We study the possibility of transferring population between two bound atomic or molecular states via an autoionizing state. Conditions for efficient transfer are given and the effects of the AC Stark shifts, the Fano parameters and the incoherent channels of ionization are explored. An adiabatic analytic solution which helps in the understanding of the behaviour of the system is also given. Efficient transfer is realized by using both a counterintuitive pulse sequence and concurrent laser pulses.
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.
Using the time-dependent multilevel approach, we have calculated the coherent population transfer between the quantum states of potassium atom by a single frequency-chirped laser pulse. The result shows that a pair of sequential 'broadband' frequency-chirped laser pulses can efficiently transfer population from the initial state of the ladder system to the target state. It is also found that the population can be efficiently transferred to a target state and trapped there by using an 'intuitive' or a 'counterintuitive' frequency sweep laser pulse in the case of 'narrowband' frequency-chirped laser pulse. Our research shows that the complete population transfer is related to the pulse duration, chirp rate, and amplitude of the laser pulse.
We study the dynamics of chirped adiabatic passage (CHIRAP) with temporally delayed pulses to selectively and fully transfer population in atoms and molecules. We show that the transfer of population via stimulated Raman adiabatic passage (STIRAP) and stimulated two-photon adiabatic absorption with temporally delayed laser pulses is not adversely affected by applying a chirp to the pulses, provided the intensity of the laser is sufficiently large to allow adiabatic passage. We then proceed to consider systems in which a near degeneracy of terminal state levels results in nonselective population of the terminal levels using nonchirped STIRAP or two-photon absorption stimulated passage, because the dynamics within the nearly degenerate pair of levels is not adiabatic. However, the CHIRAP process selectively populates only one of the terminal levels.
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.
Population transfer between two valence states of the Li atom with a Raman process via intermediate autoionizing states well above the ionization threshold is investigated using a recently developed implementation of the muticonfiguration time-dependent Hartree Fock method. It is found that a properly chosen sequence of pump and Stokes $\ensuremath{\pi}$ pulses can yield a population transfer efficiency of 5353%53 at relatively low intensities, while the extension of the stimulated Raman adiabatic passage (STIRAP) approach to the XUV in this case is far less efficient and loses its characteristic robustness at high intensities. A rule of thumb for when STIRAP is practical is given, suggesting that at still shorter wavelengths STIRAP may be possible.