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ACS symposium series

Selective Excitation among Closely Lying Multi levels

K. Nagaya, Yoshiaki Teranishi, Hiroki Nakamura

Published Jun 21, 2002• 3 citations
Publisher

Abstract

A new idea is proposed to accomplish selective and complete excitation to any specified state among closely lying multi-levels. The basic idea is to control nonadiabatic transitions among dressed states by sweeping the laser frequency periodically. Both three- and four-level models are treated by the semiclassical theory of nonadiabatic transition and conditions of complete excitation are formulated. Numerical demonstrations are presented in comparison with the π-pulse and adiabatic rapid passage.

DOI
10.1021/bk-2002-0821.ch007

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A new idea is proposed to accomplish selective and complete excitation to any specified state among closely lying multi-levels. The basic idea is to control nonadiabatic transitions among dressed states by sweeping the laser frequency periodically. Both three- and four-level models are treated by the semiclassical theory of nonadiabatic transition and conditions of complete excitation are formulated. Numerical demonstrations are presented in comparison with the π-pulse and adiabatic rapid passage.
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A new idea of controlling nonadiabatic transitions by an external field is proposed. The basic principle is to periodically sweep an external field at each level crossing to make the overall transition probability from an initial state to any desirable final state equal to unity. The recently completed semiclassical theory of nonadiabatic transition enables us to analytically deal with this problem. The present idea may be applicable to various physical and chemical problems, whenever level crossings are created by an external field.
In this paper we extend the existing theory of stimulated Raman adiabatic passage (StiRAP) in three-level systems to examine the nature of selective photoexcitation using counterintuitively ordered pulses. Our goal is to develop a version of StiRAP that permits control of product selectivity in a chemical reaction. We analyze the case of selective excitation to one state in a pair of degenerate target states in a four-level system, and find that one cannot control the ratio of the populations in the two states in a resonant two-photon process. However, the extension of the system to include a fifth state and a third laser field makes selective excitation to one of the degenerate states possible. It is found that, subject to reasonable restrictions, one may accomplish complete population transfer to a single target state of a degenerate pair of states in a five-level system.
The chirped-pulse interaction in the adiabatic coupling regime induces cyclic permutations of the energy states of a three-level system in the VVV-type configuration, which process is known as the three-level chirped rapid adiabatic passage (RAP). Here we show that a spectral hole in a chirped pulse can turn on or off the level mixing at adiabatic crossing points of this process, reducing the system to an effective two-level system. The given hybrid adiabatic-nonadiabatic transition enables selective excitation of the three-level system, controlled by the laser intensity and spectral position of the hole, as well as the sign of the chirp parameter. Experiments performed with shaped femtosecond laser pulses and the three lowest energy levels (5S1/25{S}_{1/2}5S1/2​, 5P1/25{P}_{1/2}5P1/2​, and 5P3/25{P}_{3/2}5P3/2​) of atomic rubidium (Rb)(\mathrm{Rb})(Rb) show good agreement with the theoretically analyzed dynamics. The result indicates that our method, when being combined with the ordinary chirped RAP, implements an adiabatic transition between the Raman-coupled excited states. Furthermore, our laser intensity-dependent control may have applications including selective excitations of atoms or ions arranged in space when being used in conjunction with laser beam profile programming.
We develop new pulse schemes to significantly speed up adiabatic state transfer protocols. Our general strategy involves adding corrections to an initial control Hamiltonian that harness nonadiabatic transitions. These corrections define a set of dressed states that the system follows exactly during the state transfer. We apply this approach to stimulated Raman adiabatic passage protocols and show that a suitable choice of dressed states allows one to design fast protocols that do not require additional couplings, while simultaneously minimizing the occupancy of the "intermediate" level.