Ultrafast X-ray Auger probing of photoexcited molecular dynamics
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- Ultrafast X-ray Auger probing of photoexcited molecular dynamics
- McFarland B.K.; Farrell J.P.; Miyabe S.; Tarantelli F.; Aguilar A.; Berrah N.; Bostedt C.; Bozek J.D.; Bucksbaum P.H.; Castagna J.C.; Coffee R.N.; Cryan J.P.; Fang L.; Feifel R.; Gaffney K.J.; Glownia J.M.; Martinez T.J.; Mucke M.; Murphy B.; Natan A.; Osipov T.; Petrovic V.S.; Schorb S.; Schultz, Thomas; Spector L.S.; Swiggers M.; Tenney I.; Wang S.; White J.L.; White W.; Guhr M.
- RESOLVED PHOTOELECTRON-SPECTROSCOPY; FREE-ELECTRON LASER; CONICAL INTERSECTIONS; EXCITED-STATES; RNA BASES; AQUEOUS-SOLUTION; THYMINE; DNA; OPERATION; URACIL
- Issue Date
- NATURE PUBLISHING GROUP
- NATURE COMMUNICATIONS, v.5, no., pp. -
- Molecules can efficiently and selectively convert light energy into other degrees of freedom. Disentangling the underlying ultrafast motion of electrons and nuclei of the photoexcited molecule presents a challenge to current spectroscopic approaches. Here we explore the photoexcited dynamics of molecules by an interaction with an ultrafast X-ray pulse creating a highly localized core hole that decays via Auger emission. We discover that the Auger spectrum as a function of photoexcitation-X-ray-probe delay contains valuable information about the nuclear and electronic degrees of freedom from an element-specific point of view. For the nucleobase thymine, the oxygen Auger spectrum shifts towards high kinetic energies, resulting from a particular C-O bond stretch in the pp photoexcited state. A subsequent shift of the Auger spectrum towards lower kinetic energies displays the electronic relaxation of the initial photoexcited state within 200 fs. Ab-initio simulations reinforce our interpretation and indicate an electronic decay to the nφ* state.
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