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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, Th; Spector, L S; Swiggers, M; Tenney, I; Wang, S; White, J L; White, W; Gühr, M.
Afiliación
  • McFarland BK; PULSE Institute, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA.
  • Farrell JP; 1] PULSE Institute, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA [2] Departments of Physics and Applied Physics, Stanford University, Stanford, California 94305, USA.
  • Miyabe S; PULSE Institute, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA.
  • Tarantelli F; Dipartimento di Chimica, Biologia e Biotecnologie, Universita di Perugia, and ISTM-CNR, 06123 Perugia, Italy.
  • Aguilar A; Advanced Light Source, Lawrence Berkeley National Lab, 1 Cyclotron Road, Berkeley, California 94720, USA.
  • Berrah N; 1] Physics Department, Western Michigan University, Kalamazoo, Michigan 49008, USA [2].
  • Bostedt C; LCLS, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA.
  • Bozek JD; LCLS, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA.
  • Bucksbaum PH; 1] PULSE Institute, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA [2] Departments of Physics and Applied Physics, Stanford University, Stanford, California 94305, USA.
  • Castagna JC; LCLS, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA.
  • Coffee RN; LCLS, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA.
  • Cryan JP; 1] PULSE Institute, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA [2] Departments of Physics and Applied Physics, Stanford University, Stanford, California 94305, USA.
  • Fang L; Physics Department, Western Michigan University, Kalamazoo, Michigan 49008, USA.
  • Feifel R; 1] Department of Physics and Astronomy, Uppsala University, SE-751 20 Uppsala, Sweden [2].
  • Gaffney KJ; PULSE Institute, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA.
  • Glownia JM; 1] PULSE Institute, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA [2] Departments of Physics and Applied Physics, Stanford University, Stanford, California 94305, USA.
  • Martinez TJ; 1] PULSE Institute, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA [2] Department of Chemistry, Stanford University, Stanford, California 94305, USA.
  • Mucke M; Department of Physics and Astronomy, Uppsala University, SE-751 20 Uppsala, Sweden.
  • Murphy B; Physics Department, Western Michigan University, Kalamazoo, Michigan 49008, USA.
  • Natan A; PULSE Institute, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA.
  • Osipov T; Physics Department, Western Michigan University, Kalamazoo, Michigan 49008, USA.
  • Petrovic VS; 1] PULSE Institute, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA [2] Departments of Physics and Applied Physics, Stanford University, Stanford, California 94305, USA.
  • Schorb S; LCLS, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA.
  • Schultz T; 1] Max-Born-Institut, Max-Born-Strasse 2a, 12489 Berlin, Germany [2].
  • Spector LS; 1] PULSE Institute, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA [2] Departments of Physics and Applied Physics, Stanford University, Stanford, California 94305, USA.
  • Swiggers M; LCLS, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA.
  • Tenney I; 1] PULSE Institute, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA [2] Departments of Physics and Applied Physics, Stanford University, Stanford, California 94305, USA.
  • Wang S; 1] PULSE Institute, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA [2] Departments of Physics and Applied Physics, Stanford University, Stanford, California 94305, USA.
  • White JL; 1] PULSE Institute, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA [2] Departments of Physics and Applied Physics, Stanford University, Stanford, California 94305, USA.
  • White W; LCLS, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA.
  • Gühr M; PULSE Institute, SLAC National Accelerator Laboratory, 2575, Sand Hill Road, Menlo Park, California 94025, USA.
Nat Commun ; 5: 4235, 2014 Jun 23.
Article en En | MEDLINE | ID: mdl-24953740
ABSTRACT
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 ππ* 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 nπ* state.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Commun Asunto de la revista: BIOLOGIA / CIENCIA Año: 2014 Tipo del documento: Article País de afiliación: Estados Unidos
Texto completo
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Commun Asunto de la revista: BIOLOGIA / CIENCIA Año: 2014 Tipo del documento: Article País de afiliación: Estados Unidos