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Creators/Authors contains: "Larsen, K"

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  1. We applied reaction microscopy to elucidate fast non-adiabatic dissociation dynamics of deuterated water molecules after direct photo-double ionization at 61 eV with synchrotron radiation. For the very rare D+ + O+ + D breakup channel, the particle momenta, angular, and energy distributions of electrons and ions, measured in coincidence, reveal distinct electronic dication states and their dissociation pathways via spin–orbit coupling and charge transfer at crossings and seams on the potential energy surfaces. Notably, we could distinguish between direct and fast sequential dissociation scenarios. For the latter case, our measurements reveal the geometry and orientation of the deuterated water molecule with respect to the polarization vector that leads to this rare 3-body molecular breakup channel. Aided by multi-reference configuration-interaction calculations, the dissociation dynamics could be traced on the relevant potential energy surfaces and particularly their crossings and seams. This approach also unraveled the ultrafast time scales governing these processes. 
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  2. Creation of a super-excited radical water cation results in a long-lived excited oxygen fragment that can act as a destructive carrier and initiate secondary reactions such as breakup of DNA strands – a key radiation damage mechanism. 
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  3. We present an investigation of the relaxation dynamics of deuterated water molecules after direct photo-double ionization at 61 eV. We focus on the very rare D+ + O+ + D reaction channel in which the sequential fragmentation mechanisms were found to dominate the dynamics. Aided by theory, the state-selective formation and breakup of the transient OD+(a1Δ, b1Σ+) is traced, and the most likely dissociation path—OD+: a1Δ or b1Σ+ → A 3Π → X 3Σ− → B 3Σ−—involving a combination of spin–orbit and non-adiabatic charge transfer transitions is determined. The multi-step transition probability of this complex transition sequence in the intermediate fragment ion is directly evaluated as a function of the energy of the transient OD+ above its lowest dissociation limit from the measured ratio of the D+ + O+ + D and competing D+ + D+ + O sequential fragmentation channels, which are measured simultaneously. Our coupled-channel time-dependent dynamics calculations reproduce the general trends of these multi-state relative transition rates toward the three-body fragmentation channels. 
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  4. The densest overflow water from the Nordic Seas passes through the Faroe Bank Channel and contributes to the headwaters to the lower limb of the Atlantic Meridional Overturning Circulation. The upstream pathways of this dense overflow water are not well known. Using data from a high-resolution hydrographic/velocity survey in 2011, as well as long-term moored velocity and shipboard hydrographic measurements north of the Faroe Islands, we present evidence of a current following the continental slope from Iceland toward the Faroe Bank Channel. This narrow current, which we call the Iceland-Faroe Slope Jet (IFSJ), is bottom-intensified and associated with dense water banked up on the slope. North of the Faroe Islands the IFSJ is situated beneath the Faroe Current, and its variability is tightly linked to the flow of Atlantic Water above. The bulk of the IFSJ’s volume transport is confined to a small area in ϴ-S space centered near a potential density anomaly of 28.06 kg m-3. This is slightly denser than the transport mode of the North Icelandic Jet, which follows shallower isobaths along the slope north of Iceland in the opposite direction and feeds the Denmark Strait overflow. However, the similarity of the hydrographic properties suggests that the two currents have a common source. The average transport of water denser than σϴ = 27.8 kg m-3 in the IFSJ is on the order of 1 Sv, which may account for roughly 50% of the overflow through the Faroe Bank Channel. 
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