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Physical Review Letters

Coherent Population Transfer in an Atom by Multiphoton Adiabatic Rapid Passage

H. Maeda, J. H. Gurian, D.V.L. Norum, Thomas F. Gallagher

Published Feb 23, 2006• 38 citations
Publisher

Abstract

Coherent population transfer in an atom using a sequence of adiabatic rapid passages through single-photon resonances is well-known, but it requires that the frequency sweep match the changing frequencies of the atomic transitions. The same population transfer can be effected via a single multiphoton adiabatic rapid passage, which requires only a small frequency sweep, if it is possible to select the desired multiphoton transition from the many possible transitions. Here we report the observation of population transfer between Rydberg states by high order multiphoton adiabatic rapid passage.

DOI
10.1103/physrevlett.96.073002

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Coherent Population Transfer in Rydberg Atoms by Multiphoton Adiabatic Rapid Passage

Thomas F. Gallagher

Bulletin of the American Physical Society•May 29, 2008•0 citations
Coherent population transfer in an atom using a sequence of adiabatic rapid passages through single-photon resonances is well-known, but it requires that the frequency sweep match the changing frequencies of the atomic transitions. The same population transfer can be effected via a single multiphoton adiabatic rapid passage, which requires only a small frequency sweep, if it is possible to select the desired multiphoton transition from the many possible transitions. Here we report the observation of population transfer between Rydberg states by high order multiphoton adiabatic rapid passage.
The population of atoms in Rydberg states is efficiently transferred with a change in principal quantum number nnn of up to ten via multiphoton adiabatic rapid passage through a single multiphoton resonance using a frequency-chirped microwave pulse. A quantum-mechanical picture of multiphoton adiabatic rapid passage in a one-dimensional atom using a Floquet approach provides a good description of most, but not all, of the observed phenomena.
Following an experimental observation, a recent simulation has shown that efficient population transfer can be achieved through adiabatic chirping of a microwave pulse through a 10-photon resonance connecting two Rydberg states with n = 72, ℓ = 1 and n ∼ 82. These simulations have revealed that this population transfer is essentially a classical transition caused by separatrix crossing in the classical phase space. Here, we present the results of our fully three-dimensional quantum and classical simulations of coherent multiphoton population transfer in a kicked Li atom in a Rydberg state. We were able to achieve ∼76% population transfer from the 40p to 46p state in Li through a 6-photon resonance and contrast our results with those when the transition is driven by microwaves. We further discuss the case when the atom starts out from a Stark state in conjunction with the ℓ-distribution of the transferred population. We use a one-dimensional classical model to investigate the classical processes taking place in the phase space and find that the same separatrix crossing mechanism observed in microwave transitions is also responsible for the transition when the atom is kicked.
Efficient population transfer by adiabatically chirping through a multiphoton resonance in microwave driven and kicked Rydberg atoms has recently been reported both experimentally and theoretically. Here we report on our simulations in which we have exploited this mechanism to vibrationally excite a diatomic molecule up to |ν = 4, J from the ground state by chirping through a four-photon resonance condition. This is an efficient means of population transfer, which is an alternative to the ladder climbing scheme requiring chirping through a sequence of states in the correct order. We discuss and compare one-dimensional quantum and classical models where there is no rotational degree of freedom. This comparison suggests that for the lowest laser intensity we consider, the process is classically forbidden and the transition occurs through tunnelling. We show that for larger peak intensities, the transfer can be looked upon as a classical transition in phase space, similar to that observed in the atomic case. We extend our simulations to fully three-dimensional quantum calculations and investigate the effect of coupling between different rotational pathways. We finally discuss the effect of thermal averaging over the initial J-states using a temperature for which the first few rotational levels inside the ν = 0 manifold are populated.
Coherent interactions between light fields and simple quantum systems, such as $\ensuremath{\pi}$-pulses and adiabatic passage through frequency chirps and stimulated Raman interactions, generally use one- or two-photon processes. This limits the use of such interactions to energy scales close to the photon energy of the control field. However, recent calculations have shown that a 3-level system, generic to ionized diatomic molecules, shows such a strong multiphoton coupling that $\ensuremath{\pi}$-pulses are possible on at least 12-photon transitions. In this paper, we show that adiabatic transfer of population is also possible on such high-order multiphoton transitions. Full one-dimensional quantum mechanical two-electron calculations confirm this effect even in a system with many excited states and an ionization continuum.