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Coherent structural trapping through wave packet dispersion during photoinduced spin state switching.

Abstract：

:The description of ultrafast nonadiabatic chemical dynamics during molecular photo-transformations remains challenging because electronic and nuclear configurations impact each other and cannot be treated independently. Here we gain experimental insights, beyond the Born-Oppenheimer approximation, into the light-induced spin-state trapping dynamics of the prototypical [Fe(bpy)3]2+ compound by time-resolved X-ray absorption spectroscopy at sub-30-femtosecond resolution and high signal-to-noise ratio. The electronic decay from the initial optically excited electronic state towards the high spin state is distinguished from the structural trapping dynamics, which launches a coherent oscillating wave packet (265 fs period), clearly identified as molecular breathing. Throughout the structural trapping, the dispersion of the wave packet along the reaction coordinate reveals details of intramolecular vibronic coupling before a slower vibrational energy dissipation to the solution environment. These findings illustrate how modern time-resolved X-ray absorption spectroscopy can provide key information to unravel dynamic details of photo-functional molecules.

journal_name

Nat Commun

journal_title

Nature communications

authors

Lemke HT,Kjær KS,Hartsock R,van Driel TB,Chollet M,Glownia JM,Song S,Zhu D,Pace E,Matar SF,Nielsen MM,Benfatto M,Gaffney KJ,Collet E,Cammarata M

doi

10.1038/ncomms15342

subject

Has Abstract

pub_date

2017-05-24 00:00:00

pages

15342

issn

2041-1723

pii

ncomms15342

journal_volume

8

pub_type

杂志文章

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