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Journal of Raman Spectroscopy

Quantum control by stimulated Raman scattering

R. Pausch, M. Heid, T. Chen, H. Schwoerer, W. Kiefer

Published Jan 1, 2000• 39 citations
Publisher

Abstract

In a model system, i.e. the K2 dimer molecule, a vibrationally excited wave packet around a prechosen target state in the electronic ground state is generated by an ultrafast resonant stimulated Raman process. By choosing the pump and dump wavelengths along the difference potential between the excited electronic |B〉-state and the electronic ground state |X〉 and optimizing the delay time between the pump and dump processes, one can increase considerably the efficiency of the population transfer of this quantum control experiment. Copyright © 2000 John Wiley & Sons, Ltd.

DOI
10.1002/(sici)1097-4555(200001/02)31:1/2<7::aid-jrs522>3.0.co;2-o

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In a model system, i.e. the K2 dimer molecule, a vibrationally excited wave packet around a prechosen target state in the electronic ground state is generated by an ultrafast resonant stimulated Raman process. By choosing the pump and dump wavelengths along the difference potential between the excited electronic |B〉-state and the electronic ground state |X〉 and optimizing the delay time between the pump and dump processes, one can increase considerably the efficiency of the population transfer of this quantum control experiment. Copyright © 2000 John Wiley & Sons, Ltd.
The feasibility of a novel technique for efficient and selective population transfer from a thermally populated level 1 via an intermediate state 2 to level 3 is experimentally demonstrated. It is shown for sodium dimers that the process of on- or near-resonance stimulated Raman scattering with only partially overlapping laser beams is, in particular, useful for the selective population of high vibrational levels of particles in a molecular beam. This is achieved when the interaction with the Stokes laser, coupling levels 2 and 3, begins earlier than the interaction with the pump laser. The phenomenon, which is closely related to the formation of ‘‘trapped states,’’ is quantitatively explained using the basis of eigenstates of molecules strongly coupled to the radiation fields. The similarity and difference to related techniques such as rapid adiabatic passage phenomena in two-level systems, off-resonant stimulated Raman scattering, or stimulated emission pumping is briefly discussed.
An excitation scheme is proposed for transferring population between ground-vibrational levels of a molecule. The transfer is accomplished by pumping and dumping population with a pair of coherent ultrashort-pulse trains via a stationary state. By mismatching the teeth of the frequency combs associated with the pulse trains to the vibrational levels, high selectivity in the excitation, along with high transfer efficiency, is predicted. The pump-dump scheme does not suffer from spontaneous emission losses, it is insensitive to the pump-dump-train delay, and it requires only basic pulse shaping.
In atomic and molecular physics, coherent optical techniques allowing for almost complete ultrafast transfer of a population between different molecular eigenstates has been developed and refined for many years. One particularly successful scheme is called stimulated Raman scattering by delayed pulses (STIRAP). Within this scheme, it is possible to transfer a population between two nonoptically coupled states by using a third state (which is optically coupled to both the initial and the final state) without actually occupying it, in the end, at all. As for semiconductors, the question arises whether similar techniques can be used to transfer, for example, holes from the heavy-hole (HH) band to the light-hole (LH) band without creating electrons in the process. We have studied this problem theoretically and have identified parameter regimes where we believe the delayed-pulse scheme can be efficiently applied to the HH-LH population transfer.
Summary form only given.In atomic and molecular physics, coherent optical techniques allowing for almost complete ultrafast transfer of a population between different molecular eigenstates has been developed and refined for many years. One particularly successful scheme is called stimulated Raman scattering by delayed pulses (STIRAP). Within this scheme, it is possible to transfer a population between two nonoptically coupled states by using a third state (which is optically coupled to both the initial and the final state) without actually occupying it, in the end, at all. As for semiconductors, the question arises whether similar techniques can be used to transfer, for example, holes from the heavy-hole (HH) band to the light-hole (LH) band without creating electrons in the process. We have studied this problem theoretically and have identified parameter regimes where we believe the delayed-pulse scheme can be efficiently applied to the HH-LH population transfer.