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International Journal of Quantum Chemistry

Analysis of adiabatic population transfer in multilevel systems by Hückel model

Y. Ohta, T. Yoshimoto, T. Bando, H. Kizu, H. Nagao, K. Nishikawa

Published Jan 1, 2000• 0 citations
Publisher

Abstract

We applied our pictorial approach using the fundamental concept of the Hückel molecular orbital theory to the population inversion in the multilevel systems by the straddling-STIRAP (S-STIRAP). We showed that the mechanism of the population inversion in the multilevel system may be easily understood by our approach. It is also shown that our approach is useful to understand that the condition required for the laser frequency in the delayed pulse sequence is different for the even- and odd-level systems. © 2000 John Wiley & Sons, Inc. Int J Quant Chem 80: 1068–1075, 2000

DOI
10.1002/1097-461x(2000)80:4/5<1068::aid-qua56>3.3.co;2-m

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We applied our pictorial approach using the fundamental concept of the Hückel molecular orbital theory to the population inversion in the multilevel systems by the straddling-STIRAP (S-STIRAP). We showed that the mechanism of the population inversion in the multilevel system may be easily understood by our approach. It is also shown that our approach is useful to understand that the condition required for the laser frequency in the delayed pulse sequence is different for the even- and odd-level systems. © 2000 John Wiley & Sons, Inc. Int J Quant Chem 80: 1068–1075, 2000
We applied our pictorial approach using the fundamental concept of the Hückel molecular orbital theory to the population inversion in the multilevel systems by the straddling-STIRAP (S-STIRAP). We showed that the mechanism of the population inversion in the multilevel system may be easily understood by our approach. It is also shown that our approach is useful to understand that the condition required for the laser frequency in the delayed pulse sequence is different for the even- and odd-level systems. © 2000 John Wiley & Sons, Inc. Int J Quant Chem 80: 1068–1075, 2000
To achieve the selective population transfer to the specific excited state of molecules, the delayed-pulse method developed in the three-level system is more attractive and effective than the ordinary π-pulses method. However, two pulses in this adiabatic method are in a counterintuitive order and are significantly overlapped, so that it is very difficult to understand the physical meanings of the dynamical process. Here we develop the effective method to understand the adiabatic processes in a pictorial and easy way by using the concept of the Hückel molecular orbital theory. Then we investigate the complete population transfer in the four-level system in detail. ©1999 John Wiley & Sons, Inc. Int J Quant Chem 75: 511–522, 1999
We study different mechanisms of adiabatic population transfer in N-level systems by means of optimal control algorithms. Using two-dimensional topographic maps of the yield of population transfer as a function of time delay and intensity of the pulses we analyze the global properties of the schemes and the conditions that lead to optimization. For three-level systems it is shown that the optimal pulse sequence is the well-known STIRAP (stimulated Raman adiabatic passage) scheme. For five-level systems a family of solutions ranging from the alternating STIRAP scheme to the new straddling STIRAP (S-STIRAP) scheme is obtained and the behavior of the solutions is compared. For four-level systems we obtain as optimal a S-STIRAP type sequence that behaves as an effective two-level system. For both odd and even numbers of N-level systems, the crucial role of the straddling pulse in reducing the population of all intermediate levels is demonstrated.
A numerical analysis is presented of several potential pulsed-laser applications of adiabatic population inversion in atoms or molecules. A simple numerical method is demonstrated for evaluating adiabatic processes in multilevel systems for both swept-frequency and resonant, time-delayed pulses. Adiabatic inversion with time-delayed pulses is generalized to systems with any number of levels. The effect of Doppler broadening on time-delayed adiabatic pumping of a three-level system is investigated.
We consider a five-level atomic system (M-system) driven by four near-resonant laser pulses and study the possibilities of population transfer via different combinations of Stimulated Raman Adiabatic Passage (STIRAP) and bright-STIRAP (b-STIRAP) processes. We examine these combinations analytically and numerically from the point of view of efficiency of population transfer. It is shown, in particular, that the combination of the processes above enhances the efficiency. Analytical expressions are obtained for the quasienergies of the system in two regimes differing by conditions imposed on resonance detunings. Interaction adiabaticity conditions are analyzed. We also study the necessary successions of turning on and off of pulses which ensure efficient transfer of atomic populations. The obtained analytical results agree well with direct numerical calculations.
Abstract We consider coherent population transfer in multilevel quantum systems driven by time-delayed pulse trains. We show how to choose the parameters of the trains so that the population dynamics tracks the behavior of a Λ-type three-level system under stimulated Raman adiabatic passage (STIRAP). Efficient population transfer can be achieved regardless of the order and with or without overlap of the pump and the Stokes sub-pulses of the trains. Generalized STIRAP schemes of population transfer in N -level system with sequential couplings are also examined. The mechanism of the population transfer and the robustness of the proposed schemes are discussed.