X-ray Raman scattering of liquids:Is water one liquid or two?

鏉ユ簮锛氭暟鐞嗗闄?i class="gap">鍙戝竷鏃堕棿锛?019-08-27

銆愯搴ч鐩€?span style="font-family: times new roman; font-size: 16px;">X-ray Raman scattering of liquids:Is water one liquid or two?



銆愪富 璁?浜恒€?span style="font-family: times new roman; font-size: 16px;">Faris Gel鈥檓ukhanov鏁欐巿


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Local probes of the electronic ground and valence excited states are essential for understanding hydrogen bonding in aqueous environments. Vibrational infra-red (IR) spectroscopy is an established technique for investigations of hydrogen bonding. High-resolution X-ray absorption spectroscopy and resonant inelastic X-ray scattering (RIXS) offers a complement to IR vibrational spectroscopy. The propagation of the nuclear wave packet in dissociative core-excited stateresults in the long vibrational progression seen in both theory and experiment. This gives great advantage of RIXS in comparison with IR spectroscopy which probes mainly the first OH excitation. We show how different resonant inelastic X-ray scattering (RIXS) channels deliver separate information; about the local structure via long-range dynamics in quasi-elastic RIXS and about short-range dynamics, which is much less sensitive to the structure, in the electronically inelastic 1b1 and 4a鈥欌€?channel in water and methanol, respectively. Our theoretical framework is composed of classical ab initio molecular dynamics (MD) simulations, calculation of local potential energy surfaces from the sampled configurations, and quantum wave packet modeling of the nuclear motion in relevant degrees of freedom.