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International Symposium on Molecular Spectroscopy (ISMS)

Theory for Direct Frequency Comb Spectroscopy

D. Felinto, Carlos E. E. López

Published Jun 1, 2010• 0 citations
OpenAlex

Abstract

We introduce a theory for the interaction of multi-level atoms with well-stabilized pulse trains, which is general enough to take into account arbitrarily-shaped frequency combs. It is applied to the excitation of rubidium-87 atoms.

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Theory for Direct Frequency Comb Spectroscopy

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Coherent Excitation of Two-Level Atoms by Pulse Trains

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Springer eBooks•Jan 1, 1996•0 citations
Direct frequency-comb spectroscopy is a technique that employs a train of well-stabilized ultrashort pulses to study the spectral properties of atomic or molecular systems. In this way, it opens the possibility of incorporating various coherent-control techniques for such spectral investigations. Here we introduce a theory for the interaction of a multilevel atom with such pulse trains, which is general enough to take into account an arbitrarily shaped frequency comb. We illustrate its application by studying the interaction of 87Rb^{87}\text{R}\text{b}87Rb atoms with trains of pulses of various shapes, resonant with the $5S\text{\ensuremath{-}}5D$ two-photon transition of rubidium. More specifically, we treat the interaction with hyperbolic-secant pulses, chirped pulses, and 0-$\ensuremath{\pi}$ pulses, respectively. The theory is designed to work at an arbitrary perturbation order. For the results presented here, we mostly used a 12th-order perturbation series at the pulse's electric field. Due to the large number of levels involved, such modeling may be quite complex computationally, and an important point of the present work is then to introduce the required numerical approach to treat this problem efficiently.
We investigate the time dynamics of a four-level rubidium atomic system excited by a train of $0\ensuremath{\pi}$ pulses. Resonant $0\ensuremath{\pi}$ pulse shaping is achieved by propagation of weak femtosecond pulses through rubidium vapor and characterized using frequency-resolved optical gating and within the linear dispersion theory. The excitation of the Rb atoms by $0\ensuremath{\pi}$ pulse train is studied experimentally by modified direct frequency comb spectroscopy and theoretically within the density-matrix approach. We show that accumulation of populations and coherences, as typical pulse train excitation effects, strongly depend on the strength of the resonant $0\ensuremath{\pi}$ pulse shaping. Stronger pulse shaping reduces the coherent accumulation effects, eventually leading to the disappearance of the velocity selective optical pumping observed in the frequency domain.