Wu, J.Magrakvelidze, M.Vredenborg, A.Schmidt, L. Ph. H.Jahnke, T.Czasch, A.Dörner, R.Thumm, U.2023-12-072023-12-072013-01-18https://hdl.handle.net/2097/43909We demonstrate that the vibrational nuclear motion of singly ionized argon dimers can be controlled with two ultrashort laser pulses of different wavelengths. In particular, we observe a striking “gap” in the pump-probe-delay-dependent kinetic-energy release spectrum only if the probe-pulse wavelength exceeds the pump-pulse wavelength. This “frustrated dissociation effect” is reproduced by our two-state quantum mechanical model, validating its interpretation as a pump-pulse-initiated population transfer between dipole-coupled Born-Oppenheimer electronic states of the dissociating Ar+2 molecular ion. Our numerical results also reproduce the measured collapse and fractional revival of the oscillating Ar+2 nuclear wave packet, and, for single-pulse dissociation, the decrease of the kinetic-energy release with increasing laser wavelength.© American Physical Society (APS). This Item is protected by copyright and/or related rights. You are free to use this Item in any way that is permitted by the copyright and related rights legislation that applies to your use. For other uses you need to obtain permission from the rights-holder(s).http://rightsstatements.org/vocab/InC/1.0/https://web.archive.org/web/20181120135245/https://journals.aps.org/copyrightFAQ.htmlText