Femtosecond resolution pump-probe experiments are now routinely carried out at X-ray Free Electron Lasers, enabled by the development of cross-correlation “time-tools” which correct the picosecond-level jitter between the optical and X-ray pulses. These tools provide very accurate, <10 fs, measurement of the relative arrival time, but do not provide a measure of the absolute coincidence time in the interaction. Cross-correlation experiments using transient reflectivity in a crystal are commonly used for this purpose, and to date no quantitative analysis of the accuracy or stability of absolute coincidence time determination has been performed. We have performed a quantitative analysis of coincidence timing at the SACLA facility through a cross-correlation of 100 ± 10 fs, 400 nm optical pulses with 7 fs, 10.5 keV X-ray pulses via transient reflectivity in a cerium-doped yttrium aluminum garnet crystal. We have modelled and fit the transient reflectivity, which required a convolution with a 226 ± 12 fs uncertainty that was believed to be dominated by X-ray and laser intensity fluctuations, or assuming an extinction depth of 13.3 μm greater than the literature value of 66.7 μm. Despite this, we are able to determine the absolute coincidence time to an accuracy of 30 fs. We discuss the physical contributions to the uncertainty of coincidence time determination, which may include an uncharacterised offset delay in the development of transient reflectivity, including cascading Auger decays, secondary ionisation and cooling processes. Additionally, we present measurements of the intrinsic short-term and long-term drifts between the X-rays and the optical laser timing from time-tool analysis, which is dominated by a thermal expansion of the 25 m optical path between tool and the interaction region, seen to be ∼60 fs over a period of 5 h.
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Coincidence timing of femtosecond optical pulses in an X-ray free electron laser
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28 November 2017
Research Article|
November 30 2017
Coincidence timing of femtosecond optical pulses in an X-ray free electron laser
Alvaro Sanchez-Gonzalez;
Alvaro Sanchez-Gonzalez
1
Quantum Optics and Laser Science Group, Blackett Laboratory, Imperial College
, London SW7 2AZ, United Kingdom
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Allan S. Johnson
;
Allan S. Johnson
1
Quantum Optics and Laser Science Group, Blackett Laboratory, Imperial College
, London SW7 2AZ, United Kingdom
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Ann Fitzpatrick;
Ann Fitzpatrick
2
Diamond Light Source Ltd.
, Diamond House, Harwell Science & Innovation Campus, Didcot, Oxon, United Kingdom
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Christopher D. M. Hutchison;
Christopher D. M. Hutchison
3
Molecular Biophysics, Imperial College London
, South Kensington Campus, SW7 2AZ London, United Kingdom
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Clyde Fare;
Clyde Fare
3
Molecular Biophysics, Imperial College London
, South Kensington Campus, SW7 2AZ London, United Kingdom
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Violeta Cordon-Preciado;
Violeta Cordon-Preciado
3
Molecular Biophysics, Imperial College London
, South Kensington Campus, SW7 2AZ London, United Kingdom
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Gabriel Dorlhiac;
Gabriel Dorlhiac
3
Molecular Biophysics, Imperial College London
, South Kensington Campus, SW7 2AZ London, United Kingdom
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Josie L. Ferreira
;
Josie L. Ferreira
3
Molecular Biophysics, Imperial College London
, South Kensington Campus, SW7 2AZ London, United Kingdom
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Rhodri M. Morgan;
Rhodri M. Morgan
4
Protein Crystallography Facility, Centre for Structural Biology, Department of Life Sciences, Imperial College London
, Flowers Building
, London SW7 2AZ, United Kingdom
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Jon P. Marangos;
Jon P. Marangos
1
Quantum Optics and Laser Science Group, Blackett Laboratory, Imperial College
, London SW7 2AZ, United Kingdom
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Shigeki Owada;
Shigeki Owada
5
RIKEN SPring-8 Center
, 1-1-1 Kouto, Sayo-cho, Hyogo 679-5148, Japan
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Takanori Nakane;
Takanori Nakane
6
Department of Biological Sciences, Graduate School of Science, The University of Tokyo
, Hongo, Bunkyo-ku, Tokyo 113-0032, Japan
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Rie Tanaka;
Rie Tanaka
5
RIKEN SPring-8 Center
, 1-1-1 Kouto, Sayo-cho, Hyogo 679-5148, Japan
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Kensuke Tono;
Kensuke Tono
5
RIKEN SPring-8 Center
, 1-1-1 Kouto, Sayo-cho, Hyogo 679-5148, Japan
7
Japan Synchrotron Radiation Research Institute
, 1-1-1 Kouto, Sayo-cho, Hyogo 679-5948, Japan
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So Iwata;
So Iwata
5
RIKEN SPring-8 Center
, 1-1-1 Kouto, Sayo-cho, Hyogo 679-5148, Japan
8
Department of Cell Biology, Graduate School of Medicine, Kyoto University
, Yoshidakonoe-cho, Sakyo-ku, Kyoto 606-8501, Japan
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Jasper J. van Thor
Jasper J. van Thor
a)
3
Molecular Biophysics, Imperial College London
, South Kensington Campus, SW7 2AZ London, United Kingdom
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a)
Author to whom correspondence should be addressed: j.vanthor@imperial.ac.uk
J. Appl. Phys. 122, 203105 (2017)
Article history
Received:
July 11 2017
Accepted:
November 05 2017
Citation
Alvaro Sanchez-Gonzalez, Allan S. Johnson, Ann Fitzpatrick, Christopher D. M. Hutchison, Clyde Fare, Violeta Cordon-Preciado, Gabriel Dorlhiac, Josie L. Ferreira, Rhodri M. Morgan, Jon P. Marangos, Shigeki Owada, Takanori Nakane, Rie Tanaka, Kensuke Tono, So Iwata, Jasper J. van Thor; Coincidence timing of femtosecond optical pulses in an X-ray free electron laser. J. Appl. Phys. 28 November 2017; 122 (20): 203105. https://doi.org/10.1063/1.5012749
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