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Journal of Physics B Atomic Molecular and Optical Physics

Experimental observation of Raman chirped adiabatic rapid passage

J F Xia, J H Sanderson, W-K Liu, Donna T. Strickland

Published Oct 20, 2003• 10 citations
Publisher

Abstract

In this letter, we present the first experimental results of climbing a vibrational ladder by Raman chirped adiabatic rapid passage. We obtain the bandwidth necessary for this experiment by utilizing pulses from a unique dual-wavelength high-intensity laser. The vibrationally excited molecules are field ionized by an intense 180 fs laser pulse, enabling us to probe the extent of the vibrational excitation of the symmetric stretch based on an enhanced ionization calculation.

DOI
10.1088/0953-4075/36/21/l06

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In this letter, we present the first experimental results of climbing a vibrational ladder by Raman chirped adiabatic rapid passage. We obtain the bandwidth necessary for this experiment by utilizing pulses from a unique dual-wavelength high-intensity laser. The vibrationally excited molecules are field ionized by an intense 180 fs laser pulse, enabling us to probe the extent of the vibrational excitation of the symmetric stretch based on an enhanced ionization calculation.
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The theory of vibrational ladder climbing excitation by coherent stimulated nonresonant Raman using chirped laser pulses is developed. We analytically obtain the conditions for inverting the population to a final preselected vibrational state and the restrictions that apply in the linear chirp regime. By controlling both the shape of the laser pulses and the chirp profile, the ladder climbing process can be accelerated without reducing the yield of the selective excitation. Numerical results are presented for selection of moderately excited vibrational levels in Na 2, where the important contribution of several excited electronic states is also clarified.
The interaction of two narrow band (Δν<100 MHz) UV light pulses of different intensity with a molecular three-level system is investigated experimentally. The laser frequencies are tuned to an up (pump) and a down (dump) transition sharing a common excited rovibronic S1 level whose population is probed by a transition to the ionization continuum and ion detection. The time sequence of the two pulses results either in a lambda type coherent stimulated Raman adiabatic passage or a stimulated emission pumping (SEP) process. When the first case is realized by a 6.4 ns delay of the low intensity pump laser from the high intensity dump laser pulse, a fourfold increase of the depth of the ion dips compared to the SEP experiment is observed. This is in line with numerical calculations of the level populations using a density matrix formalism including coherent effects. Rotationally resolved ion dip spectra of the 62 state of benzene are presented and demonstrate the high sensitivity of the coherent excitation process of this work for ion dip spectroscopy.
Chirped pulses allow for non-adiabatic passage between dressed states of Raman processes. It is shown that using an appropriately chirped pulse, one can control the interference between resonant and non-resonant pathways in stimulated Raman processes. A three-level system is studied in detail and application to complete ro-vibrational level inversion to high vibration quantum numbers (v > 10) in H2 via RCNAP (Raman chirped non-adiabatic passage) is presented. Copyright © 2000 John Wiley & Sons, Ltd.
Excitation of a quantum ladder system by frequency-swept (-chirped) laser pulses has been investigated by studying an atomic model system, the 5s-5p-5d ladder of rubidium. The population transfer is significantly enhanced when the frequency is swept such that it follows the spacing of the ladder. At intermediate intensities we observe oscillations in the population transfer to the upper level (5d), which can be attributed to interference between two routes of excitation: sequential transfer and direct two-photon excitation via a virtual intermediate state. We determine simultaneously the population transfer to the upper level (5d) and the direct three-photon ionization, the latter corresponding to a three-step ladder with the final state being in the continuum: 5s-5p-5d-\ensuremath{\varepsilon}p/\ensuremath{\varepsilon}f. Experiments were performed, using 100 fs pulses at \ensuremath{\sim}780 nm from a self-mode-locked Ti:Al2{\mathrm{Al}}_{2}Al2​O3{\mathrm{O}}_{3}O3​ oscillator amplified at 10 Hz.