Jump to main content
Jump to site search

Volume 194, 2016
Previous Article Next Article

Strong-field-induced wave packet dynamics in carbon dioxide molecule

Author affiliations


Temporal evolution of electronic and nuclear wave packets created in strong-field excitation of the carbon dioxide molecule is studied employing momentum-resolved ion spectroscopy and channel-selective Fourier analysis. Combining the data obtained with two different pump-probe set-ups, we observed signatures of vibrational dynamics in both, ionic and neutral states of the molecule. We consider far-off-resonance two-photon Raman scattering to be the most likely mechanism of vibrational excitation in the electronic ground state of the neutral CO2. Using the measured phase relation between the time-dependent yields of different fragmentation channels, which is consistent with the proposed mechanism, we suggest an intuitive picture of the underlying vibrational dynamics. For ionic states, we found signatures of both, electronic and vibrational excitations, which involve the ground and the first excited electronic states, depending on the particular final state of the fragmentation. While our results for ionic states are consistent with the recent observations by Erattupuzha et al. [J. Chem. Phys.144, 024306 (2016)], the neutral state contribution was not observed there, which we attribute to a larger bandwidth of the 8 fs pulses we used for this experiment. In a complementary measurement employing longer, 35 fs pulses in a 30 ps delay range, we study the influence of rotational excitation on our observables, and demonstrate how the coherent electronic wave packet created in the ground electronic state of the ion completely decays within 10 ps due to the coupling to rotational motion.

Back to tab navigation

Publication details

The article was received on 23 Jun 2016, accepted on 29 Jun 2016 and first published on 30 Jun 2016

Article type: Paper
DOI: 10.1039/C6FD00152A
Citation: Faraday Discuss., 2016,194, 463-478
  •   Request permissions

    Strong-field-induced wave packet dynamics in carbon dioxide molecule

    A. Rudenko, V. Makhija, A. Vajdi, T. Ergler, M. Schürholz, R. K. Kushawaha, J. Ullrich, R. Moshammer and V. Kumarappan, Faraday Discuss., 2016, 194, 463
    DOI: 10.1039/C6FD00152A

Search articles by author