Populations and coherence in femtosecond time resolved X-ray crystallography of the photoactive yellow protein
File(s)PYP review final - CH.pdf (2.53 MB)
Accepted version
Author(s)
Hutchison, CDM
van Thor, JJ
Type
Journal Article
Abstract
Ultrafast X-ray crystallography of the photoactive yellow protein with femtosecond delays using an X-ray free electron laser has successfully probed the dynamics of an early Franck-Condon species. The femtosecond pump-probe application of protein crystallography represents a new experimental regime that provides an X-ray structural probe for coherent processes that were previously accessible primarily using ultrafast spectroscopy. We address how the optical regime of the visible pump, that is necessary to successfully resolve ultrafast structural differences, affects the motions that are measured using the technique. The sub-picosecond photochemical dynamics in PYP involves evolution of a mixture of electronic ground and excited state populations. Additional to photoisomerisation that is considered to proceed through activated barrier crossing, within the dephasing time structural motion include vibrational coherence arising from excited states, the ground state and a ground state intermediate under experimental conditions used for ultrafast crystallography. Intense optical pulses are required to convert population levels in PYP crystals that allow detection by X-ray crystallography, but the compromise currently needed for the optical bandwidth and power has consequences with regard to the contributions to the motions that are experimentally measured with femtosecond delays. We briefly review the ultrafast spectroscopy literature of the primary photoreactions of PYP and discuss relevant physical models taken from coherent control and femtosecond coherence spectroscopy literature that address both the population transfer as well as the vibrational coherences. We apply linear response theory, with the additional use of a high power approximation, of on-resonance impulsive vibrational coherence in the ground state and the non-impulsive coherence in the excited state and discuss experimental approaches to manipulate the coherence contributions. The results are generalised and extended to discuss the future capabilities of high repetition rate X-ray free electron laser instruments providing enhanced sensitivity to perform the crystallographic equivalent of an impulsive Raman measurement of vibrational coherence.
Date Issued
2017-02-13
Date Acceptance
2017-02-01
Citation
International Reviews in Physical Chemistry, 2017, 36 (1), pp.117-143
ISSN
0144-235X
Publisher
Taylor & Francis
Start Page
117
End Page
143
Journal / Book Title
International Reviews in Physical Chemistry
Volume
36
Issue
1
Copyright Statement
© 2017 Informa UK limited, trading as taylor & Francis Group. This is an Accepted Manuscript of an article published by Taylor & Francis in International Reviews in Physical Chemistry on 13 Feb 2017, available online: https://dx.doi.org/10.1080/0144235X.2017.1276726
Sponsor
Engineering & Physical Science Research Council (EPSRC)
Identifier
http://dx.doi.org/10.1080/0144235X.2017.1276726
Grant Number
EP/M000192/1
Subjects
Science & Technology
Physical Sciences
Chemistry, Physical
Physics, Atomic, Molecular & Chemical
Chemistry
Physics
Serial femtosecond crystallography
photoactive yellow protein
vibrational coherence
linear response theory
X-ray free electron laser
PUMP-PROBE SPECTROSCOPY
EXCITED-STATE DYNAMICS
NEUTRON-SCATTERING
RAMAN-SPECTROSCOPY
ECTOTHIORHODOSPIRA-HALOPHILA
FLUORESCENCE SPECTROSCOPY
ABSORPTION-SPECTROSCOPY
PRIMARY PHOTOCHEMISTRY
PHOTORECEPTOR PROTEIN
PHOTOINDUCED DYNAMICS
Chemical Physics
0306 Physical Chemistry (Incl. Structural)
0307 Theoretical And Computational Chemistry
0202 Atomic, Molecular, Nuclear, Particle And Plasma Physics
Notes
doi: 10.1080/0144235X.2017.1276726
Publication Status
Published
Date Publish Online
2017-02-13