Simultaneous observation of nuclear and electronic dynamics by ultrafast electron diffraction

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Abstract

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.

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Imaging Molecular Motion: Femtosecond X-Ray Scattering of an Electrocyclic Chemical Reaction.

M P Minitti, J M Budarz, A Kirrander … (2015)

Structural rearrangements within single molecules occur on ultrafast time scales. Many aspects of molecular dynamics, such as the energy flow through excited states, have been studied using spectroscopic techniques, yet the goal to watch molecules evolve their geometrical structure in real time remains challenging. By mapping nuclear motions using femtosecond x-ray pulses, we have created real-space representations of the evolving dynamics during a well-known chemical reaction and show a series of time-sorted structural snapshots produced by ultrafast time-resolved hard x-ray scattering. A computational analysis optimally matches the series of scattering patterns produced by the x rays to a multitude of potential reaction paths. In so doing, we have made a critical step toward the goal of viewing chemical reactions on femtosecond time scales, opening a new direction in studies of ultrafast chemical reactions in the gas phase.

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Author and article information

Journal

Title: Science

Abbreviated Title: Science

Publisher: American Association for the Advancement of Science (AAAS)

ISSN (Print): 0036-8075

ISSN (Electronic): 1095-9203

Publication date Created: May 21 2020

Publication date Created: May 22 2020

Publication date (Electronic): May 21 2020

Publication date (Print): May 22 2020

Volume: 368

Issue: 6493

Pages: 885-889

Affiliations

[1 ]SLAC National Accelerator Laboratory, Menlo Park, CA, USA.

[2 ]Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.

[3 ]Department of Chemistry, Stanford University, Stanford, CA, USA.

[4 ]Department of Physics and Astronomy, University of Nebraska–Lincoln, Lincoln, NE, USA.

[5 ]Biophysics Program, Stanford University, Stanford, CA, USA.

[6 ]Institut für Physik und Astronomie, Universität Potsdam, Potsdam, Germany.

[7 ]Department of Physics and Astronomy, Stony Brook University, Stony Brook, NY, USA.

Article

DOI: 10.1126/science.abb2235

PubMed ID: 32439793

SO-VID: 9373947a-2005-467a-a09e-32fb58678f1f

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