Probing molecular dynamics with attosecond resolution using correlated wave packet pairs


Spectroscopic measurements with increasingly higher time resolution are generally thought to require increasingly shorter laser pulses, as illustrated by the recent monitoring of the decay of core-excited krypton1 using attosecond photon pulses2,3. However, an alternative approach to probing ultrafast dynamic processes might be provided by entanglement, which has improved the precision4,5 of quantum optical measurements. Here we use this approach to observe the motion of a D2+ vibrational wave packet formed during the multiphoton ionization of D2 over several femtoseconds with a precision of about 200 attoseconds and 0.05 ångströms, by exploiting the correlation between the electronic and nuclear wave packets formed during the ionization event. An intense infrared laser field drives the electron wave packet, and electron recollision6,7,8,9,10,11 probes the nuclear motion. Our results show that laser pulse duration need not limit the time resolution of a spectroscopic measurement, provided the process studied involves the formation of correlated wave packets, one of which can be controlled; spatial resolution is likewise not limited to the focal spot size or laser wavelength.

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Figure 1: Processes probed and exploited with the sub-laser-cycle dynamics method using correlated wave packet pairs.
Figure 2: Kinetic energy distribution of D+ at different pump–probe delay times.
Figure 3: The measured wave packet position as a function of time.


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We acknowledge discussions with A. Stolow, A. Sokolov, A. D. Bandrauk, S. Chelkowski and J. Marangos. The authors appreciate financial support from Canada's Natural Science and Engineering Research Council, the Canadian Institute for Photonics Innovation, and Le Fonds Québécois de la Recherche sur la Nature et les Technologies.

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Correspondence to P. B. Corkum.

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Niikura, H., Légaré, F., Hasbani, R. et al. Probing molecular dynamics with attosecond resolution using correlated wave packet pairs. Nature 421, 826–829 (2003).

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