Simultaneous observation of nuclear and electronic dynamics by ultrafast electron diffraction.

Autor: Yang J; SLAC National Accelerator Laboratory, Menlo Park, CA, USA. jieyang@slac.stanford.edu todd.martinez@stanford.edu wangxj@slac.stanford.edu.; Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Zhu X; SLAC National Accelerator Laboratory, Menlo Park, CA, USA.; Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.; Department of Chemistry, Stanford University, Stanford, CA, USA., F Nunes JP; Department of Physics and Astronomy, University of Nebraska-Lincoln, Lincoln, NE, USA., Yu JK; Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.; Department of Chemistry, Stanford University, Stanford, CA, USA.; Biophysics Program, Stanford University, Stanford, CA, USA., Parrish RM; SLAC National Accelerator Laboratory, Menlo Park, CA, USA.; Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.; Department of Chemistry, Stanford University, Stanford, CA, USA., Wolf TJA; SLAC National Accelerator Laboratory, Menlo Park, CA, USA.; Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Centurion M; Department of Physics and Astronomy, University of Nebraska-Lincoln, Lincoln, NE, USA., Gühr M; Institut für Physik und Astronomie, Universität Potsdam, Potsdam, Germany., Li R; SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Liu Y; Department of Physics and Astronomy, Stony Brook University, Stony Brook, NY, USA., Moore B; Department of Physics and Astronomy, University of Nebraska-Lincoln, Lincoln, NE, USA., Niebuhr M; Institut für Physik und Astronomie, Universität Potsdam, Potsdam, Germany., Park S; SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Shen X; SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Weathersby S; SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Weinacht T; Department of Physics and Astronomy, Stony Brook University, Stony Brook, NY, USA., Martinez TJ; SLAC National Accelerator Laboratory, Menlo Park, CA, USA. jieyang@slac.stanford.edu todd.martinez@stanford.edu wangxj@slac.stanford.edu.; Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.; Department of Chemistry, Stanford University, Stanford, CA, USA., Wang X; SLAC National Accelerator Laboratory, Menlo Park, CA, USA. jieyang@slac.stanford.edu todd.martinez@stanford.edu wangxj@slac.stanford.edu.
Jazyk: angličtina
Zdroj: Science (New York, N.Y.) [Science] 2020 May 22; Vol. 368 (6493), pp. 885-889.
DOI: 10.1126/science.abb2235
Abstrakt: Simultaneous observation of nuclear and electronic motion is crucial for a complete understanding of molecular dynamics in excited electronic states. It is challenging for a single experiment to independently follow both electronic and nuclear dynamics at the same time. Here we show that ultrafast electron diffraction can be used to simultaneously record both electronic and nuclear dynamics in isolated pyridine molecules, naturally disentangling the two components. Electronic state changes (S 1 →S 0 internal conversion) were reflected by a strong transient signal in small-angle inelastic scattering, and nuclear structural changes (ring puckering) were monitored by large-angle elastic diffraction. Supported by ab initio nonadiabatic molecular dynamics and diffraction simulations, our experiment provides a clear view of the interplay between electronic and nuclear dynamics of the photoexcited pyridine molecule.
(Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works.)
Databáze: MEDLINE
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