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Physical Review A

Population transfer via a decaying state

Nikolay V. Vitanov, Stig Stenholm

Published Aug 1, 1997• 93 citations
Publisher

Abstract

The paper examines the effect of irreversible dissipation from the intermediate state on the efficiency of population transfer by partially overlapping delayed pulses in three-state systems. Several general approximations to the final-state population for both the intuitive and counterintuitive pulse sequences are derived. They show that the loss of transfer efficiency is much stronger for the intuitive pulse sequence, as then the intermediate state is significantly populated during the transfer. For the counterintuitive sequence, the damping of the final-state population is found to be exponential for small decay rates and polynomial for large ones; moreover, the range of decay rates, over which the transfer efficiency remains high, is proportional to the squared pulse area. The paper also presents an analytically solvable model, involving smooth delayed pulses, as well as numerical results and analytic approximations for Gaussian pulses.

DOI
10.1103/physreva.56.1463

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The paper examines the effect of irreversible dissipation from the intermediate state on the efficiency of population transfer by partially overlapping delayed pulses in three-state systems. Several general approximations to the final-state population for both the intuitive and counterintuitive pulse sequences are derived. They show that the loss of transfer efficiency is much stronger for the intuitive pulse sequence, as then the intermediate state is significantly populated during the transfer. For the counterintuitive sequence, the damping of the final-state population is found to be exponential for small decay rates and polynomial for large ones; moreover, the range of decay rates, over which the transfer efficiency remains high, is proportional to the squared pulse area. The paper also presents an analytically solvable model, involving smooth delayed pulses, as well as numerical results and analytic approximations for Gaussian pulses.
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.
The effect of radiative decay and collisional damping on the delayed-field population transfer in the three-level system is investigated. The simple analytical steady-state solution of the three-level system, interacting with two intense delayed laser pulses in the dressed-state frame, is obtained and analyzed. The radiative relaxation transfers the system to the ``trapped state,'' which is shown to be stable relative to both radiative decay and collisional damping. The effect of an additional level \ensuremath{\Vert}m〉, situated close to the final level \ensuremath{\Vert}3〉, on the population-transfer process is considered. The field-induced relaxation rate from intermediate level \ensuremath{\Vert}2〉 to level \ensuremath{\Vert}3〉 is shown to be a very easily controllable parameter of the field intensities and their relative delay. This result leads to selective population transfer to the desired level and may prevent leaking out of the three-level system. Theoretical analysis corresponds entirely to recent experimental data [U. Gaubatz et al., J. Chem. Phys. 92, 1 (1990); 92, 5363 (1990)].
This paper analyzes the extension of the three-state process of stimulated Raman adiabatic passage to chainwise-connected multistate systems. A necessary condition for such a process is the existence of an adiabatic-transfer state, which connects adiabatically the initial state of the chain to its final state. Various counterintuitive pulse sequences are examined, in all of which the pulse that drives the last transition of the chain precedes the pulse driving the first transition, while the pulses driving the intermediate transitions may have different timings. The paper demonstrates some important qualitative differences and similarities between the systems with odd and even number of states. In the on-resonance case, an adiabatic-transfer state always exists for an odd number of states while it never exists for an even number of states. In the off-resonance case, however, the two types of systems behave in a very similar manner and the condition for existence of an adiabatic-transfer state is essentially the same. This condition, which imposes certain limitations on the laser parameters, is derived in a simple and compact form. It is also shown analytically that, besides by large detunings, the populations of the intermediate states (which are generally nonzero during the transfer) can be damped by large intermediate couplings. It is concluded that for an odd number of states, the optimal case is the on-resonance one, with equal and large intermediate couplings. For an even number of states, the optimal (off-resonance) case is when the intermediate couplings and the detunings have similar values. Various numerical examples of success and failure of multistate population transfer confirm the analytic conclusions.
We demonstrate that various properties of population transfer by delayed pulses in three-level systems on two-photon resonance can be deduced analytically and for general pulse shapes. We use the fact that the three-level system reduces to effective two-level problems at large intermediate-level detuning \ensuremath{\Delta}, on resonance (\ensuremath{\Delta}=0) and for completely overlapping pulses. Special attention is paid to the effect of the pulse order on the population transfer efficiency. We show that on resonance the transfer efficiency depends substantially on the pulse order, while at large \ensuremath{\Delta} it does not. We also find that under some natural restrictions on the symmetry of the problem, the population of the initial level does not depend on the pulse order at any \ensuremath{\Delta}. Furthermore, we demonstrate that the population transfer in the three-level system can be viewed as a level-crossing problem in an equivalent two-level system not only at large \ensuremath{\Delta} (which is known) but also on resonance, \ensuremath{\Delta}=0. The effective on-resonance two-level problem is interesting by itself as it shows that a level crossing and adiabatic evolution do not necessarily lead to complete population inversion. As examples throughout the paper, we present several analytically solvable models.
This paper presents an analytic study of the properties of a three-state system coupled to two external laser fields on two-photon resonance. The intermediate state is generally off single-photon resonance and can decay irreversibly out of the system. The two fields are assumed to have the same pulse-shaped time dependence but may have different strengths. Various general properties for arbitrary pulse shapes, detunings and decay rates are derived and illustrated with an exactly solvable analytic model. They include the conditions for complete population transfer and depletion, complete population loss or no loss, various limitations on the values of the populations, the effect of overdamping at large decay rates and others.