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Title: Advances in ultrafast gas-phase x-ray scattering

Journal Article · · Journal of Physics. B, Atomic, Molecular and Optical Physics
ORCiD logo [1]; ORCiD logo [2];  [3];  [2];  [2];  [4];  [5];  [2];  [6];  [6];  [5];  [2]
  1. Western Connecticut State Univ., Danbury, CT (United States)
  2. Brown Univ., Providence, RI (United States)
  3. UES Inc., Dayton, OH (United States); Brown Univ., Providence, RI (United States)
  4. Brown Univ., Providence, RI (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  6. Univ. of Edinburgh (United Kingdom)

Recent developments of x-ray free electron lasers and pulsed electron sources have enabled ultrafast scattering to become an increasingly powerful tool for exploring molecular dynamics. Here, this article describes our recent experimental and methodological advances in ultrafast gas-phase x-ray scattering experiments at the LCLS. A re-designed short-pathlength windowless diffractometer is coupled with careful optimization of sample density and independent normalization of x-ray intensity fluctuations to provide gas-phase scattering patterns with exceptionally high signal-to-noise ratios. These advances, coupled with careful geometry optimization and data treatment, provide both ground- and excited-state signals in excellent agreement with high level ab initio total scattering patterns.

Research Organization:
Brown Univ., Providence, RI (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
AC02-76SF00515; SC0017995; SC0020276
OSTI ID:
1768235
Journal Information:
Journal of Physics. B, Atomic, Molecular and Optical Physics, Journal Name: Journal of Physics. B, Atomic, Molecular and Optical Physics Journal Issue: 23 Vol. 53; ISSN 0953-4075
Publisher:
IOP PublishingCopyright Statement
Country of Publication:
United States
Language:
English

References (42)

Femtochemistry: Atomic-Scale Dynamics of the Chemical Bond Using Ultrafast Lasers (Nobel Lecture) journal August 2000
Elements of Modern X-ray Physics book March 2011
Zerstreuung von Röntgenstrahlen journal January 1915
Simplicity Beneath Complexity: Counting Molecular Electrons Reveals Transients and Kinetics of Photodissociation Reactions journal April 2019
X-Ray Interactions: Photoabsorption, Scattering, Transmission, and Reflection at E = 50-30,000 eV, Z = 1-92 journal July 1993
Centering of ultrafast time-resolved pump–probe electron diffraction patterns journal April 2004
Pixel array detector for X-ray free electron laser experiments
  • Philipp, Hugh T.; Hromalik, Marianne; Tate, Mark
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 649, Issue 1 https://doi.org/10.1016/j.nima.2010.11.189
journal September 2011
A 9 eV superexcited state of 1,3-cyclohexadiene revealed by double resonance ionization photoelectron spectroscopy journal December 2001
Capturing Chemistry in Action with Electrons: Realization of Atomically Resolved Reaction Dynamics journal May 2017
Ab Initio Calculation of Total X-ray Scattering from Molecules journal March 2019
Excited Electronic States in Total Isotropic Scattering from Molecules journal March 2020
From the (1B) Spectroscopic State to the Photochemical Product of the Ultrafast Ring-Opening of 1,3-Cyclohexadiene: A Spectral Observation of the Complete Reaction Path journal August 2015
Determining Orientations of Optical Transition Dipole Moments Using Ultrafast X-ray Scattering journal October 2018
Ultrafast Dynamics in Superexcited States of Phenol journal April 2001
Ultrafast Diffraction Imaging of the Electrocyclic Ring-Opening Reaction of 1,3-Cyclohexadiene journal May 2001
Direct observation of nuclear reorganization driven by ultrafast spin transitions journal March 2020
Observation of the molecular response to light upon photoexcitation journal May 2020
The photochemical ring-opening of 1,3-cyclohexadiene imaged by ultrafast electron diffraction journal April 2019
Ultrafast X-ray scattering reveals vibrational coherence following Rydberg excitation journal July 2019
Spectral encoding method for measuring the relative arrival time between x-ray/optical pulses journal August 2014
Scattering off molecules far from equilibrium journal August 2019
Erratum: Atomic Form Factors, Incoherent Scattering Functions, and Photon Scattering Cross Sections journal April 1977
Ultrafast x-ray and electron scattering of free molecules: A comparative evaluation journal May 2020
Transient structures and chemical reaction dynamics journal December 2017
Transient structures and chemical reaction dynamics journal December 2017
Imaging electronic quantum motion with light journal July 2012
Monitoring molecular nonadiabatic dynamics with femtosecond X-ray diffraction journal June 2018
Concepts in x-ray physics journal December 2008
Observation of femtosecond molecular dynamics via pump–probe gas phase x-ray scattering journal January 2016
Molecular x-ray- and electron-scattering intensities journal March 1984
Electronically Driven Structure Changes of Si Captured by Femtosecond Electron Diffraction journal April 2008
Imaging Molecular Motion: Femtosecond X-Ray Scattering of an Electrocyclic Chemical Reaction journal June 2015
Self-Referenced Coherent Diffraction X-Ray Movie of Ångstrom- and Femtosecond-Scale Atomic Motion journal October 2016
Comment on “Self-Referenced Coherent Diffraction X-Ray Movie of Ångstrom- and Femtosecond-Scale Atomic Motion” journal August 2017
Glownia et al. Reply: journal August 2017
Electronic Coherence in Ultrafast X-Ray Scattering from Molecular Wave Packets journal February 2019
Characterizing Multiphoton Excitation Using Time-Resolved X-ray Scattering journal March 2020
International Tables for Crystallography book January 2006
A deep UV trigger for ground-state ring-opening dynamics of 1,3-cyclohexadiene journal September 2019
Imaging CF 3 I conical intersection and photodissociation dynamics with ultrafast electron diffraction journal July 2018
Simultaneous observation of nuclear and electronic dynamics by ultrafast electron diffraction journal May 2020
Imaging Electron Dynamics with Ultrashort Light Pulses: A Theory Perspective journal February 2018

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