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arXiv:1604.00979

Vibrationally-induced electronic population inversion with strong femtosecond pulses

Pablo Sampedro, Bo Y. Chang, Ignacio R. Solá

Published Apr 4, 2016• 0 citations
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Abstract

We discover a new mechanism of electronic population inversion using strong femtosecond pulses, where the transfer is mediated by vibrational motion on a light-induced potential. The process can be achieved with a single pulse tuning its frequency to the red of the Franck-Condon window. We show the determinant role that the sign of the slope of the transition dipole moment can play on the dynamics, and extend the method to multiphoton processes with odd number of pulses. As an example, we show how the scheme can be applied to population inversion in Na2.

DOI
10.48550/arxiv.1604.00979

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We discover a new mechanism of electronic population inversion using strong femtosecond pulses, where the transfer is mediated by vibrational motion on a light-induced potential. The process can be achieved with a single pulse tuning its frequency to the red of the Franck-Condon window. We show the determinant role that the sign of the slope of the transition dipole moment can play on the dynamics, and extend the method to multiphoton processes with odd number of pulses. As an example, we show how the scheme can be applied to population inversion in Na2.
Summary form only given. We propose a method for achieving highly efficient transfer between the vibrational states in a diatomic molecule. The process is mediated by strong laser pulses and can be understood in terms of light-induced potentials. Light-induced potentials were also key to understanding APLIP (adiabatic passage by light induced potentials), where a wave packet is guided from one ground vibrational state to another. However, in the new process we show how to target specific vibrational states with strong short pulses. In addition to describing a specific molecular system, our results show how, in general, one can manipulate the populations of the different quantum states in double well systems.
We investigate the dynamics of molecular photoexcitation by unchirped femtosecond laser pulses using RbCs as a model system. This study is motivated by a goal of optimizing a two-color scheme of transferring vibrationally excited ultracold molecules to their absolute ground state. In this scheme the molecules are initially produced by photoassociation or magnetoassociation in bound vibrational levels close to the first dissociation threshold. We analyze here the first step of the two-color path as a function of pulse intensity from the low-field to the high-field regime. We use two different approaches, a global one, the ``wave-packet'' method, and a restricted one, the ``level-by-level'' method, where the number of vibrational levels is limited to a small subset. The comparison between the results of the two approaches allows one to gain qualitative insights into the complex dynamics of the high-field regime. In particular, we emphasize the nontrivial and important role of far-from-resonance levels which are adiabatically excited through ``vertical'' transitions with a large Franck-Condon factor. We also point out the spectacular excitation blockade due to the presence of a quasidegenerate level in the lower electronic state. We conclude that selective transfer with femtosecond pulses is possible in the low-field regime only. Finally, we extend our single-pulse analysis and examine population transfer induced by coherent trains of low-intensity femtosecond pulses.
Vibrationally selective population transfer in electronic transitions involving small Franck−Condon factors is studied by means of two-photon excitation with pulse sequences applied in counterintutive order. Depending on the intensity of the pulses, two schemes allow ultrafast adiabatic passage. Both schemes, called STIRAP and APLIP, are analyzed as a function of the geometry of the electronic states and of the time duration and intensity of the pulses that drive the transitions. Although both schemes imply adiabatic following, the APLIP scheme requires pulses of considerably larger intensity than STIRAP, hence operating in a strong adiabatic regime. Simple adiabatic criteria for high-quality transfer are proposed, and analytic proofs are provided that show under which conditions STIRAP and APLIP converge. The results of this paper are illustrated with numerical simulations for two different electronic transitions in the Na 2 molecule.
Using the concept of light-induced potentials introduced by Garraway and Suominen [Phys. Rev. Lett. 80, 932 (1998)], we study alternative schemes of adiabatic population transfer in a diatomic molecule from the lowest vibrational level of the ground electronic state to the lowest vibrational level of a third electronic state via allowed optical transitions from the ground and third electronic states to a second electronic state. Our chirped-pulse rapid adiabatic passage scheme is implemented with short-duration optical pulses, and can be understood in terms of ``road design engineering'' of the light-induced time-dependent adiabatic potential upon which the dynamics occurs. We explicitly show that complete adiabatic vibronic population transfer occurs using chirped picosecond-duration pulses in the sodium dimer example.
Abstract On the basis of our theoretical model of the population transfer between two levels interacting suddenly with an intense laser pulse (Zhang et al 2017 J. Phys. B: At. Mol. Opt. Phys. 50 185603), we investigate the mechanism of the population inversion between the electronically excited B 2 Σ u + state and the electronic ground X 2 Σ g + state of N 2 + achieved by the irradiation of a near-IR (800 nm) intense laser pulse, leading to the generation of the coherent emission at 391 nm. We show that one of the Floquet states generated at the moment when N 2 + starts interacting with an intense laser pulse is adiabatically connected to the ground vibrational state of the electronic B 2 Σ u + state and keeps a constant population throughout the period of the interaction with the light field, indicating that the efficient off-resonance B 2 Σ u + – X 2 Σ g + transition proceeds.