Capturing Chemistry in Action with Electrons: Realization
of Atomically Resolved Reaction Dynamics
Version 2 2017-07-27, 18:22
Version 1 2017-06-07, 17:16
Posted on 2017-07-27 - 18:22
One of the grand challenges in chemistry
has been to directly observe
atomic motions during chemical processes. The depiction of the nuclear
configurations in space-time to understand barrier crossing events
has served as a unifying intellectual theme connecting the different
disciplines of chemistry. This challenge has been cast as an imaging
problem in which the technical issues reduce to achieving not only
sufficient simultaneous space-time resolution but also brightness
for sufficient image contrast to capture the atomic motions. This
objective has been met with electrons as the imaging source. The review
chronicles the first use of electron structural probes to study reactive
intermediates, to the development of high bunch charge electron pulses
with sufficient combined spatial-temporal resolution and intensity
to literally light up atomic motions, as well as the means to characterize
the electron pulses in terms of temporal brightness and image reconstruction.
The use of femtosecond Rydberg spectroscopy as a novel means to use
internal electron scattering within the molecular reference frame
to obtain similar information on reaction dynamics is also discussed.
The focus is on atomically resolved chemical reaction dynamics with
pertinent references to work in other areas and forms of spectroscopy
that provide additional information. Effectively, we can now directly
observe the far-from-equilibrium atomic motions involved in barrier
crossing and categorize chemistry in terms of a power spectrum of
a few dominant reaction modes. It is this reduction in dimensionality
that makes chemical reaction mechanisms transferrable to seemingly
arbitrarily complex (large N) systems, up to molecules as large as
biological macromolecules (N > 1000 atoms). We
now
have a new way to reformulate reaction mechanisms using an experimentally
determined dynamic mode basis that in combination with recent theoretical
advances has the potential to lead to a new conceptual basis for chemistry
that forms a natural link between structure and dynamics.
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Ischenko, Anatoly
A.; Weber, Peter M.; J. Dwayne Miller, R. (2017). Capturing Chemistry in Action with Electrons: Realization
of Atomically Resolved Reaction Dynamics. ACS Publications. Collection. https://doi.org/10.1021/acs.chemrev.6b00770
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AUTHORS (3)
AI
Anatoly
A. Ischenko
PW
Peter M. Weber
RJ
R. J. Dwayne Miller
KEYWORDS
Capturing Chemistrymode basispower spectrumbrightnesschemical reaction dynamicsReaction Dynamicsstudy reactive intermediatesimage contrastspatial-temporal resolutionbarrierreaction modesfemtosecond Rydberg spectroscopychemical reaction mechanismsimaging problemreference framereformulate reaction mechanismschemical processeschallengereaction dynamics1000 atomsbunch charge electron pulsesinformationimage reconstructionelectron pulsesimaging source