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Title: Ultrafast X-ray scattering reveals vibrational coherence following Rydberg excitation

Abstract

The coherence and dephasing of vibrational motions of molecules constitute an integral part of chemical dynamics, influence material properties, and underpin schemes to control chemical reactions. Significant progress has been made in understanding vibrational coherence through spectroscopic measurements, but the precise direct measurement of the structure of a vibrating excited-state polyatomic organic molecule has remained elusive. Here, we measure the time-evolving molecular structure of optically excited N-methyl morpholine through scattering with ultrashort X-ray pulses. The scattering signals are corrected for the different electron density in the excited electronic state of the molecule compared to the ground state. In conclusion, the experiment maps the evolution of the molecular geometry with femtosecond resolution, showing coherent motion that survives electronic relaxation and appears to persist for longer than previously seen using other methods.

Authors:
 [1]; ORCiD logo [1];  [2];  [1];  [2];  [3];  [3];  [3];  [3];  [3];  [1];  [1];  [1];  [3]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1]
  1. Brown Univ., Providence, RI (United States)
  2. Univ. of Edinburgh, Edinburgh (United Kingdom)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1526046
Alternate Identifier(s):
OSTI ID: 1526048
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Nature Chemistry
Additional Journal Information:
Journal Name: Nature Chemistry; Journal ID: ISSN 1755-4330
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English

Citation Formats

Stankus, Brian, Yong, Haiwang, Zotev, Nikola, Ruddock, Jennifer M., Bellshaw, Darren, Lane, Thomas J., Liang, Mengning, Boutet, Sébastien, Carbajo, Sergio, Robinson, Joseph S., Du, Wenpeng, Goff, Nathan, Chang, Yu, Koglin, Jason E., Minitti, Michael P., Kirrander, Adam, and Weber, Peter M. Ultrafast X-ray scattering reveals vibrational coherence following Rydberg excitation. United States: N. p., 2019. Web. doi:10.1038/s41557-019-0291-0.
Stankus, Brian, Yong, Haiwang, Zotev, Nikola, Ruddock, Jennifer M., Bellshaw, Darren, Lane, Thomas J., Liang, Mengning, Boutet, Sébastien, Carbajo, Sergio, Robinson, Joseph S., Du, Wenpeng, Goff, Nathan, Chang, Yu, Koglin, Jason E., Minitti, Michael P., Kirrander, Adam, & Weber, Peter M. Ultrafast X-ray scattering reveals vibrational coherence following Rydberg excitation. United States. doi:10.1038/s41557-019-0291-0.
Stankus, Brian, Yong, Haiwang, Zotev, Nikola, Ruddock, Jennifer M., Bellshaw, Darren, Lane, Thomas J., Liang, Mengning, Boutet, Sébastien, Carbajo, Sergio, Robinson, Joseph S., Du, Wenpeng, Goff, Nathan, Chang, Yu, Koglin, Jason E., Minitti, Michael P., Kirrander, Adam, and Weber, Peter M. Mon . "Ultrafast X-ray scattering reveals vibrational coherence following Rydberg excitation". United States. doi:10.1038/s41557-019-0291-0.
@article{osti_1526046,
title = {Ultrafast X-ray scattering reveals vibrational coherence following Rydberg excitation},
author = {Stankus, Brian and Yong, Haiwang and Zotev, Nikola and Ruddock, Jennifer M. and Bellshaw, Darren and Lane, Thomas J. and Liang, Mengning and Boutet, Sébastien and Carbajo, Sergio and Robinson, Joseph S. and Du, Wenpeng and Goff, Nathan and Chang, Yu and Koglin, Jason E. and Minitti, Michael P. and Kirrander, Adam and Weber, Peter M.},
abstractNote = {The coherence and dephasing of vibrational motions of molecules constitute an integral part of chemical dynamics, influence material properties, and underpin schemes to control chemical reactions. Significant progress has been made in understanding vibrational coherence through spectroscopic measurements, but the precise direct measurement of the structure of a vibrating excited-state polyatomic organic molecule has remained elusive. Here, we measure the time-evolving molecular structure of optically excited N-methyl morpholine through scattering with ultrashort X-ray pulses. The scattering signals are corrected for the different electron density in the excited electronic state of the molecule compared to the ground state. In conclusion, the experiment maps the evolution of the molecular geometry with femtosecond resolution, showing coherent motion that survives electronic relaxation and appears to persist for longer than previously seen using other methods.},
doi = {10.1038/s41557-019-0291-0},
journal = {Nature Chemistry},
number = ,
volume = ,
place = {United States},
year = {2019},
month = {7}
}

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Works referenced in this record:

Optimal control of quantum-mechanical systems: Existence, numerical approximation, and applications
journal, June 1988

  • Peirce, Anthony P.; Dahleh, Mohammed A.; Rabitz, Herschel
  • Physical Review A, Vol. 37, Issue 12, p. 4950-4964
  • DOI: 10.1103/PhysRevA.37.4950