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Title: Towards ultrafast dynamics with split-pulse X-ray photon correlation spectroscopy at free electron laser sources

Abstract

One of the important challenges in condensed matter science is to understand ultrafast, atomic-scale fluctuations that dictate dynamic processes in equilibrium and non-equilibrium materials. Here, we report an important step towards reaching that goal by using a state-of-the-art perfect crystal based split-and-delay system, capable of splitting individual X-ray pulses and introducing femtosecond to nanosecond time delays. We show the results of an ultrafast hard X-ray photon correlation spectroscopy experiment at LCLS where split X-ray pulses were used to measure the dynamics of gold nanoparticles suspended in hexane. We show how reliable speckle contrast values can be extracted even from very low intensity free electron laser (FEL) speckle patterns by applying maximum likelihood fitting, thus demonstrating the potential of a split-and-delay approach for dynamics measurements at FEL sources. This will enable the characterization of equilibrium and, importantly also reversible non-equilibrium processes in atomically disordered materials.

Authors:
 [1];  [2]; ORCiD logo [3];  [1];  [1];  [4];  [5];  [6]; ORCiD logo [6];  [7]; ORCiD logo [7]; ORCiD logo [7];  [2];  [8];  [2];  [3]
  1. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  3. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); The Hamburg Centre for Ultrafast Imaging (Germany)
  4. Korea Research Inst. of Standards and Science (KRISS), Daejeon (Korea, Republic of). Frontier in Extreme Physics; Univ. of Science and Technology, Daejeon (Korea, Republic of). Dept. of Nanoscience
  5. Osaka Univ. (Japan). Dept. of Precision Science and Technology. Graduate School of Engineering
  6. PNSensor GmbH, Munich (Germany)
  7. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source
  8. McGill Univ., Montreal, QC (Canada). Dept. of Physics
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Korea Research Inst. of Standards and Science (KRISS), Daejeon (Korea, Republic of)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); German Research Foundation (DFG); National Research Foundation of Korea (NRF)
OSTI Identifier:
1437360
Grant/Contract Number:
AC02-06CH11357; AC02-76SF00515; NRF-2016K1A3A7A09005386
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; glasses; optical techniques; techniques and instrumentation; X-rays

Citation Formats

Roseker, W., Hruszkewycz, S. O., Lehmkuhler, F., Walther, M., Schulte-Schrepping, H., Lee, S., Osaka, T., Struder, L., Hartmann, R., Sikorski, M., Song, S., Robert, A., Fuoss, P. H., Sutton, M., Stephenson, G. B., and Grubel, G. Towards ultrafast dynamics with split-pulse X-ray photon correlation spectroscopy at free electron laser sources. United States: N. p., 2018. Web. doi:10.1038/s41467-018-04178-9.
Roseker, W., Hruszkewycz, S. O., Lehmkuhler, F., Walther, M., Schulte-Schrepping, H., Lee, S., Osaka, T., Struder, L., Hartmann, R., Sikorski, M., Song, S., Robert, A., Fuoss, P. H., Sutton, M., Stephenson, G. B., & Grubel, G. Towards ultrafast dynamics with split-pulse X-ray photon correlation spectroscopy at free electron laser sources. United States. doi:10.1038/s41467-018-04178-9.
Roseker, W., Hruszkewycz, S. O., Lehmkuhler, F., Walther, M., Schulte-Schrepping, H., Lee, S., Osaka, T., Struder, L., Hartmann, R., Sikorski, M., Song, S., Robert, A., Fuoss, P. H., Sutton, M., Stephenson, G. B., and Grubel, G. Fri . "Towards ultrafast dynamics with split-pulse X-ray photon correlation spectroscopy at free electron laser sources". United States. doi:10.1038/s41467-018-04178-9. https://www.osti.gov/servlets/purl/1437360.
@article{osti_1437360,
title = {Towards ultrafast dynamics with split-pulse X-ray photon correlation spectroscopy at free electron laser sources},
author = {Roseker, W. and Hruszkewycz, S. O. and Lehmkuhler, F. and Walther, M. and Schulte-Schrepping, H. and Lee, S. and Osaka, T. and Struder, L. and Hartmann, R. and Sikorski, M. and Song, S. and Robert, A. and Fuoss, P. H. and Sutton, M. and Stephenson, G. B. and Grubel, G.},
abstractNote = {One of the important challenges in condensed matter science is to understand ultrafast, atomic-scale fluctuations that dictate dynamic processes in equilibrium and non-equilibrium materials. Here, we report an important step towards reaching that goal by using a state-of-the-art perfect crystal based split-and-delay system, capable of splitting individual X-ray pulses and introducing femtosecond to nanosecond time delays. We show the results of an ultrafast hard X-ray photon correlation spectroscopy experiment at LCLS where split X-ray pulses were used to measure the dynamics of gold nanoparticles suspended in hexane. We show how reliable speckle contrast values can be extracted even from very low intensity free electron laser (FEL) speckle patterns by applying maximum likelihood fitting, thus demonstrating the potential of a split-and-delay approach for dynamics measurements at FEL sources. This will enable the characterization of equilibrium and, importantly also reversible non-equilibrium processes in atomically disordered materials.},
doi = {10.1038/s41467-018-04178-9},
journal = {Nature Communications},
number = ,
volume = 9,
place = {United States},
year = {Fri Apr 27 00:00:00 EDT 2018},
month = {Fri Apr 27 00:00:00 EDT 2018}
}

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