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

Journal Article · · Nature Chemistry
 [1]; ORCiD logo [2];  [3];  [2];  [3];  [4];  [4];  [4];  [4];  [4];  [2];  [2];  [2];  [4]; ORCiD logo [4]; ORCiD logo [3]; ORCiD logo [2]
  1. Brown Univ., Providence, RI (United States); SLAC National Accelerator Laboratory (SLAC)
  2. Brown Univ., Providence, RI (United States)
  3. Univ. of Edinburgh, Edinburgh (United Kingdom)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States)
+ Show Author Affiliations

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.

Research Organization:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
1526046
Journal Information:
Nature Chemistry, Journal Name: Nature Chemistry Journal Issue: 8 Vol. 11; ISSN 1755-4330
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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