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International Journal of Quantum Chemistry

One approach to adiabatic population transfer by H�ckel molecular orbital theory

Y. Ohta, H. Kizu, Akihiro Yamada, T. Yoshimoto, Kiyoshi Nishikawa

Published Jan 1, 1999• 5 citations
Publisher

Abstract

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

DOI
10.1002/(sici)1097-461x(1999)75:4/5<511::aid-qua16>3.0.co;2-1

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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 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
We investigate several configurations for complete population transfer on the basis of the dressed state picture in a three-level system. This picture allows us not only to confirm an atom staying in the only dark state all the time under the well-known stimulated Raman adiabatic passage but also to find the considerably different dynamics from the conventional adiabatic process in cases where the pulses are significantly overlapped or concurrent (optimal detuning method). We expand the concept of the adiabatic process in order to explain all these cases.
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.
We present explicit analytic expressions for adiabatic dressed states which, in suitable limits, produce complete population transfer between initial and final states of a four-state excitation chain without ever placing appreciable population into intermediate states. The population-transfer scheme is a generalization of the three-state stimulated Raman adiabatic passage that makes use of counterintuitive pulse sequences. We demonstrate analytically and numerically that the four-state system differs in a very significant qualitative way from previously studied N-state systems with odd N. In particular, we find that the presence of modest detuning from single-photon resonance is critical to the success of population transfer.