Molecular Excited-State Structure by Time-Resolved Pump−Probe X-ray Diffraction. What Is New and What Are the Prospects for Further Progress?

2011 ◽  
Vol 2 (6) ◽  
pp. 616-621 ◽  
Author(s):  
Philip Coppens
Keyword(s):  
Excited State ◽  
State Structure ◽  
X Ray Diffraction ◽  
Time Resolved ◽  
Pump Probe ◽  
X Ray ◽  
Molecular Excited State

Excited-state structure by time-resolved X-ray diffraction

2002 ◽  
Vol 58 (2) ◽  
pp. 133-137 ◽  
Author(s):  
Christopher D. Kim ◽  
Sebastien Pillet ◽  
Guang Wu ◽  
Wilfred K. Fullagar ◽  
Philip Coppens
Keyword(s):  
Excited State ◽  
State Structure ◽  
X Ray Diffraction ◽  
Time Resolved ◽  
X Ray

scholarly journals First steps towards time-resolved 'in-house' X-ray diffraction experiments

2014 ◽  
Vol 70 (a1) ◽  
pp. C775-C775 ◽  
Author(s):  
Radoslaw Kaminski ◽  
Jason Benedict ◽  
Elzbieta Trzop ◽  
Katarzyna Jarzembska ◽  
Bertrand Fournier ◽  
...  
Keyword(s):  
Excited State ◽  
Time Resolution ◽  
Structural Changes ◽  
Laser Pulses ◽  
High Repetition Rate ◽  
X Ray Diffraction ◽  
Laboratory Equipment ◽  
Time Resolved ◽  
X Ray ◽  
Ligand Charge Transfer

High-intensity X-ray sources, such as synchrotrons or X-ray free electron lasers, providing up to 100 ps time-resolution allow for studying very short-lived excited electronic states in molecular crystals. Some recent examples constitute investigations of Rh...Rh bond shortening,[1] or metal-to-ligand charge transfer processes in CuI complexes.[2] Nevertheless, in cases in which the lifetime of excited state species exceeds 10 μs it is now possible, due to the dramatic increase in the brightness of X-ray sources and the sensitivity of detectors, to use laboratory equipment to explore structural changes upon excitation. Consequently, in this contribution we present detailed technical description of the 'in-house' X-ray diffraction setup allowing for the laser-pump X-ray-probe experiments within the time-resolution at the order of 10 μs or larger. The experimental setup consists of a modified Bruker Mo-rotating-anode diffractometer, coupled with the high-frequency Nd:YAG laser (λ = 355 nm). The required synchronization of the laser pulses and the X-ray beam is realized via the optical chopper mounted across the beam-path. Chopper and laser capabilities enable high-repetition-rate experiments reaching up to 100 kHz. In addition, the laser shutter is being directly controlled though the original diffractometer software, allowing for collection of the data in a similar manner as done at the synchrotron (alternating light-ON & light-OFF frames). The laser beam itself is split into two allowing for improved uniform light delivery onto the crystal specimen. The designed setup was tested on the chosen set of crystals exhibiting rather long-lived excited state, such as, the Cu2Br2L2 (L = C5H4N-NMe2) complex, for which the determined lifetime is about 100 μs at 90 K. The results shall be presented. Research is funded by the National Science Foundation (CHE1213223). KNJ is supported by the Polish Ministry of Science and Higher Education through the "Mobility Plus" program.

Apparatus for the measurement of the electronic excited-state structure of single crystals using X-ray diffraction

1994 ◽  
Vol 27 (5) ◽  
pp. 727-732 ◽  
Author(s):  
M. A. White ◽  
M. R. Pressprich ◽  
P. Coppens ◽  
D. D. Coppens
Keyword(s):  
Excited States ◽  
Modulation Method ◽  
State Structure ◽  
X Ray Diffraction ◽  
Time Resolved ◽  
X Ray ◽  
Electronic Excited States ◽  
Structure Factors ◽  
Counting Statistics ◽  
Mechanical Chopper

Instrumentation for measuring the X-ray diffraction pattern of optically excited crystals is described. The experiment uses a high-power (~1 W) laser and a single-crystal diffractometer equipped with a helium cryostat (T < 70 K). The laser beam is modulated by a mechanical chopper and the diffraction signal gated in synchronization with the chopper phase. The modulation method is capable of observing small changes (down to about 0.01%) in the structure factors upon excitation of a fraction of the molecules in the crystal, given adequate counting statistics. The technique can be used for relatively long lived electronic excited states (τ ≃ 0.1–10 ms). The optical system is also suitable for time-resolved measurements using the time structure of synchrotron radiation.

scholarly journals XPP: X-ray Pump Probe station at BESSY II

2016 ◽  
Vol 2 ◽  
Author(s):  
Matthias Reinhardt ◽  
Wolfram Leitenberger
Keyword(s):  
Soft Matter ◽  
Ambient Conditions ◽  
X Ray Diffraction ◽  
Time Resolved ◽  
Pump Probe ◽  
X Ray ◽  
Experimental Station

The X-ray Pump-Probe (XPP) experimental station predominantly aims at investigating hard and soft matter under a broad range of ambient conditions using time-resolved X-ray diffraction.

scholarly journals Laue diffraction and time-resolved crystallography: a personal history

2019 ◽  
Vol 377 (2147) ◽  
pp. 20180243 ◽  
Author(s):  
Keith Moffat
Keyword(s):  
Storage Ring ◽  
Structural Changes ◽  
X Ray Diffraction ◽  
Laue Diffraction ◽  
Time Resolved ◽  
Pump Probe ◽  
X Ray ◽  
Historical View ◽  
Laser Sources ◽  
Diffraction Patterns

A personal, historical view is presented of Laue X-ray diffraction and its application to time-resolved studies of dynamic processes, largely in light-sensitive biological systems. In Laue diffraction, a stationary crystal is illuminated by a polychromatic X-ray source. Laue diffraction has inherent complications largely absent in monochromatic diffraction, and consequently fell into disuse for quantitative structure determination. However, the advent of naturally polychromatic, intense, pulsed storage ring X-ray sources in the 1970s led to re-examination at Daresbury and elsewhere of its underlying principles. Laue diffraction has been successfully applied at storage ring sources to time-resolved, pump–probe crystallographic studies, whose exposure time and time resolution were progressively reduced from minutes to seconds, milliseconds, nanoseconds and 100 ps. Most recently, hard X-ray free electron laser sources have been used to generate narrow bandpass Laue diffraction patterns. The femtosecond X-ray pulses from such sources are completely destructive, generate only one diffraction pattern per tiny crystal and have unusual properties. However, they too are being applied to time-resolved crystallography to explore, for example, isomerization and rapid tertiary structural changes on the chemical, femtosecond timescale. This article is part of the theme issue ‘Fifty years of synchrotron science: achievements and opportunities’.

First-, second- and third-order correlation function in time-resolved X-ray diffraction experiments

2004 ◽  
Vol 37 (3) ◽  
pp. 445-450 ◽  
Author(s):  
Simone Techert
Keyword(s):  
Structural Changes ◽  
X Rays ◽  
X Ray Diffraction ◽  
Structural Reorganization ◽  
Third Order ◽  
Time Resolved ◽  
Pump Probe ◽  
X Ray ◽  
Laser Systems ◽  
Laser Sources

In the past decade, sustained progress has been made in the field of time-resolved X-ray diffraction and photocrystallography. Laser systems have been developed rapidly, and the combination of pulsed laser sources with pulsed X-ray sources, particularly by using synchrotron X-ray radiation and X-rays generated by plasma sources, has made the application of pump-probe schemes routine. So far, however, most studies have been focused on two questions: (i) the refinement of structural changes during the course of a reaction, and (ii) possible relations between transient structural changes and the intermediates found by optical spectroscopy. In this work, a kinetic description for different time laws in time-resolved X-ray diffraction experiments is derived in the framework of time-dependent correlation functions. The derived time laws were applied to time-resolved studies on a [2+2] photodimerization and a reversible reaction undergoing structural reorganization.

scholarly journals Direct observations of shock-induced melting in a porous solid using time-resolved x-ray diffraction

2020 ◽  
Vol 4 (6) ◽  
Author(s):  
A. Mandal ◽  
B. J. Jensen ◽  
M. C. Hudspeth ◽  
S. Root ◽  
R. S. Crum ◽  
...  
Keyword(s):  
Porous Solid ◽  
X Ray Diffraction ◽  
Time Resolved ◽  
X Ray ◽  
Direct Observations

scholarly journals Bulk modulus of H2O across the ice VII–ice X transition measured by time-resolved x-ray diffraction in dynamic diamond anvil cell experiments

2021 ◽  
Vol 103 (6) ◽  
Author(s):  
A. S. J. Méndez ◽  
F. Trybel ◽  
R. J. Husband ◽  
G. Steinle-Neumann ◽  
H.-P. Liermann ◽  
...  
Keyword(s):  
Bulk Modulus ◽  
Diamond Anvil Cell ◽  
X Ray Diffraction ◽  
Time Resolved ◽  
X Ray ◽  
Diamond Anvil
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