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Physical Review A

Adiabatic excitation of rotational ladder by chirped laser pulses (13 pages)

Nikolay V. Vitanov

Published Jan 1, 2004• 0 citations
OpenAlex

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Generally, high optical intensity is required for effective multiphoton excitation of quantum systems to highly excited states. In certain situations, however, lower-intensity, chirped pulses can provide more efficient transfer of population to the upper states by the process of adiabatic passage. We have studied the relative importance of these two mechanisms in the anharmonic $5s\ensuremath{-}5p\ensuremath{-}5d$ quantum ladder system of rubidium using frequency chirped laser pulses from an amplified Ti:sapphire laser (\ensuremath{\lambda}=780 and \ensuremath{\Delta}\ensuremath{\lambda}=10 nm). We measure simultaneously the three-photon ionization signal due to the Ti:sapphire and the population that remains in the $5d$ state with a postionizing 532-nm Nd:YAG pulse (where YAG denotes yttrium aluminum garnet). At low infrared fluences (80 \ensuremath{\mu}${\mathrm{J}/\mathrm{c}\mathrm{m}}^{2}$), the transfer to the $5d$ state is significantly enhanced when the pulse frequency is swept from the red to the blue, such that it follows the frequency spacing of the rubidium ladder. Counterintuitively, population is also transferred efficiently for the blue-to-red chirp at high fluences (>5 ${\mathrm{m}\mathrm{J}/\mathrm{c}\mathrm{m}}^{2}$). We attribute both of these effects to adiabatic passage from the $5s$ state to the $5d$ state. Even at the highest fluences, more efficient transfer occurs for either direction of chirp than occurs at zero chirp, where the intensity is maximal. A comparison to theoretical predictions reveals striking agreement in both absolute magnitude and functional form. These results have important implications for the understanding of population transfer in complex ladder systems, such as molecular anharmonic vibrational ladders.

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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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Theoretical study on molecular excitation using chirped pulses in the condensed phase

Yuki Nagata, Koichi Yamashita

Chemical Physics Letters•Sep 1, 2002•7 citations
Generally, high optical intensity is required for effective multiphoton excitation of quantum systems to highly excited states. In certain situations, however, lower-intensity, chirped pulses can provide more efficient transfer of population to the upper states by the process of adiabatic passage. We have studied the relative importance of these two mechanisms in the anharmonic $5s\ensuremath{-}5p\ensuremath{-}5d$ quantum ladder system of rubidium using frequency chirped laser pulses from an amplified Ti:sapphire laser (\ensuremath{\lambda}=780 and \ensuremath{\Delta}\ensuremath{\lambda}=10 nm). We measure simultaneously the three-photon ionization signal due to the Ti:sapphire and the population that remains in the 5d5d5d state with a postionizing 532-nm Nd:YAG pulse (where YAG denotes yttrium aluminum garnet). At low infrared fluences (80 \ensuremath{\mu}J/cm2{\mathrm{J}/\mathrm{c}\mathrm{m}}^{2}J/cm2), the transfer to the 5d5d5d state is significantly enhanced when the pulse frequency is swept from the red to the blue, such that it follows the frequency spacing of the rubidium ladder. Counterintuitively, population is also transferred efficiently for the blue-to-red chirp at high fluences (>5 mJ/cm2{\mathrm{m}\mathrm{J}/\mathrm{c}\mathrm{m}}^{2}mJ/cm2). We attribute both of these effects to adiabatic passage from the 5s5s5s state to the 5d5d5d state. Even at the highest fluences, more efficient transfer occurs for either direction of chirp than occurs at zero chirp, where the intensity is maximal. A comparison to theoretical predictions reveals striking agreement in both absolute magnitude and functional form. These results have important implications for the understanding of population transfer in complex ladder systems, such as molecular anharmonic vibrational ladders.