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Physical Review A

Population transfer by multiphoton adiabatic rapid passage

H. Maeda, J. H. Gurian, Thomas F. Gallagher

Published Mar 21, 2011• 10 citations
Publisher

Abstract

The population of atoms in Rydberg states is efficiently transferred with a change in principal quantum number $n$ 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.

DOI
10.1103/physreva.83.033416

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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.
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.
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.
We demonstrate that Rydberg atoms can be transferred to states of lower principal quantum number by exposing them to a frequency chirped microwave pulse. Specifically, we have transferred n=75n=75n=75 atoms to n=66n=66n=66 with a 400-ns pulse chirped from 7.8 to 11.8 GHz. In spite of the large number of coupled levels, using a simplified model we can describe the process reasonably well as a sequence of adiabatic rapid passages.
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.
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.