DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Filming enhanced ionization in an ultrafast triatomic slingshot

Journal Article · · Communications Chemistry

Abstract Filming atomic motion within molecules is an active pursuit of molecular physics and quantum chemistry. A promising method is laser-induced Coulomb Explosion Imaging (CEI) where a laser pulse rapidly ionizes many electrons from a molecule, causing the remaining ions to undergo Coulomb repulsion. The ion momenta are used to reconstruct the molecular geometry which is tracked over time (i.e., filmed) by ionizing at an adjustable delay with respect to the start of interatomic motion. Results are distorted, however, by ultrafast motion during the ionizing pulse. We studied this effect in water and filmed the rapid “slingshot” motion that enhances ionization and distorts CEI results. Our investigation uncovered both the geometry and mechanism of the enhancement which may inform CEI experiments in many other polyatomic molecules.

Sponsoring Organization:
USDOE
Grant/Contract Number:
FG02-08ER15984
OSTI ID:
1971676
Alternate ID(s):
OSTI ID: 1974772
Journal Information:
Communications Chemistry, Journal Name: Communications Chemistry Journal Issue: 1 Vol. 6; ISSN 2399-3669
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United Kingdom
Language:
English

References (77)

Momentum-resolved above-threshold ionization of deuterated water journal November 2020
Direct observation of bond formation in solution with femtosecond X-ray scattering journal February 2015
Imaging CF 3 I conical intersection and photodissociation dynamics with ultrafast electron diffraction journal July 2018
Real-time observation of X-ray-induced intramolecular and interatomic electronic decay in CH2I2 journal May 2019
Softening of the H 2 + molecular bond in intense laser fields journal April 1990
Wave Packet Structure and Dynamics Measured by Coulomb Explosion journal May 1995
Dissociation dynamics of the water dication following one-photon double ionization. II. Experiment journal November 2018
Multiple hit readout of a microchannel plate detector with a three-layer delay-line anode journal October 2002
Recent developments in the general atomic and molecular electronic structure system journal April 2020
Ultrafast isomerization initiated by X-ray core ionization journal September 2015
Coherent Control of Retinal Isomerization in Bacteriorhodopsin journal September 2006
Time-resolved laser Coulomb explosion imaging using few-cycle intense laser pulses: Application to exploding CS 2 in highly charged states journal August 2014
Two-dimensional spectroscopy of electronic couplings in photosynthesis journal March 2005
Base Sequence and Higher-Order Structure Induce the Complex Excited-State Dynamics in DNA journal October 2008
Charge Resonance Enhanced Ionization of CO 2 Probed by Laser Coulomb Explosion Imaging journal August 2011
Geometric dependence of strong field enhanced ionization in D 2 O journal September 2017
Capturing roaming molecular fragments in real time journal November 2020
The photochemical ring-opening of 1,3-cyclohexadiene imaged by ultrafast electron diffraction journal April 2019
Coulomb Explosion Imaging of Small Molecules journal April 1989
Real-time observation of vibrational revival in the fastest molecular system journal October 2006
Ionization and dissociation dynamics of H2O in ultrashort intense near-IR laser fields by the time-dependent adiabatic state method and the time-dependent configuration interaction method journal March 2020
Visualization of bond rearrangements in acetylene using near single-cycle laser pulses journal January 2016
Femtosecond response of polyatomic molecules to ultra-intense hard X-rays journal May 2017
Multi-Particle Three-Dimensional Covariance Imaging: “Coincidence” Insights into the Many-Body Fragmentation of Strong-Field Ionized D 2 O journal August 2021
Experimental observation of the elusive double-peak structure in R-dependent strong-field ionization rate of H2+ journal August 2015
Ultrafast imaging of multielectronic dissociative ionization of CO 2 in an intense laser field journal December 2006
Role of Electron Localization in Intense-Field Molecular Ionization journal October 1995
Multiphoton multiple ionisation of N2O probed by three-dimensional covariance mapping journal June 1991
Step-by-step state-selective tracking of fragmentation dynamics of water dications by momentum imaging journal September 2022
Strong-field photoionization of vibrational ground-stateH2+andD2+molecules journal November 1999
Strong-field-induced bond rearrangement in triatomic molecules journal May 2019
Anabinitiopotential‐energy surface study of several states of the water cation journal May 1980
Strong-field ionization of water: Nuclear dynamics revealed by varying the pulse duration journal April 2021
Charge Resonance Enhanced Multiple Ionization of H 2 O Molecules in Intense Laser Fields journal June 2015
Simultaneous compression and characterization of ultrashort laser pulses using chirped mirrors and glass wedges journal December 2011
Ionization induced dynamic alignment of water journal April 2020
Imaging the Absolute Configuration of a Chiral Epoxide in the Gas Phase journal November 2013
Multiphoton ionization of dissociatingD2+molecules journal April 1999
Conical Intersection Dynamics in NO2 Probed by Homodyne High-Harmonic Spectroscopy journal October 2011
Laser-Induced Electron Tunneling and Diffraction journal June 2008
Time-Resolved Double Ionization with Few Cycle Laser Pulses journal August 2003
Simultaneous observation of nuclear and electronic dynamics by ultrafast electron diffraction journal May 2020
Laser Coulomb-explosion imaging of small molecules journal January 2005
Dissociation dynamics of the water dication following one-photon double ionization. I. Theory journal November 2018
Ultrafast electron diffraction imaging of bond breaking in di-ionized acetylene journal October 2016
Imaging the He 2 quantum halo state using a free electron laser journal December 2016
Charge-resonance-enhanced ionization of diatomic molecular ions by intense lasers journal October 1995
Dissociative ionization of molecules in intense laser fields: a method of predicting ion kinetic energies and appearance intensities journal May 1995
Probing the tunnelling site of electrons in strong field enhanced ionization of molecules journal January 2012
Observation of the Efimov state of the helium trimer journal April 2015
Laser Coulomb explosion imaging for probing ultra-fast molecular dynamics journal June 2006
Time-resolved Coulomb-explosion imaging of nuclear wave-packet dynamics induced in diatomic molecules by intense few-cycle laser pulses journal January 2011
Intensities of Electronic Transitions in Molecular Spectra II. Charge‐Transfer Spectra journal January 1939
466. The electronic orbitals, shapes, and spectra of polyatomic molecules. Part I. AH2 molecules journal January 1953
Monitoring ultrafast vibrational dynamics of isotopic molecules with frequency modulation of high-order harmonics journal March 2018
Femtosecond electron diffraction: ‘making the molecular movie’
  • Dwyer, Jason R.; Hebeisen, Christoph T.; Ernstorfer, Ralph
  • Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 364, Issue 1840 https://doi.org/10.1098/rsta.2005.1735
journal January 2006
Self-Referenced Coherent Diffraction X-Ray Movie of Ångstrom- and Femtosecond-Scale Atomic Motion journal October 2016
Enantioselective fragmentation of an achiral molecule in a strong laser field journal March 2019
Visualizing Recurrently Migrating Hydrogen in Acetylene Dication by Intense Ultrashort Laser Pulses journal December 2007
H 2 : the benchmark molecule for ultrafast science and technologies journal January 2018
X-ray multiphoton-induced Coulomb explosion images complex single molecules journal February 2022
Imaging Molecular Motion: Femtosecond X-Ray Scattering of an Electrocyclic Chemical Reaction journal June 2015
Molecular Imaging Using X-Ray Free-Electron Lasers journal April 2013
P si4 1.4: Open-source software for high-throughput quantum chemistry journal May 2020
Time-Resolved Imaging and Manipulation of H 2 Fragmentation in Intense Laser Fields journal August 2005
Time-Resolved Dynamics in N2O4 Probed Using High Harmonic Generation journal November 2008
Direct Determination of Absolute Molecular Stereochemistry in Gas Phase by Coulomb Explosion Imaging journal September 2013
Imaging charge transfer in iodomethane upon x-ray photoabsorption journal July 2014
Visualizing Correlated Dynamics of Hydrogen Atoms in Acetylene Dication by Time-Resolved Four-Body Coulomb Explosion Imaging book January 2012
Tabletop imaging of structural evolutions in chemical reactions demonstrated for the acetylene cation journal July 2014
Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen journal January 1989
Strong-field ionization of water. II. Electronic and nuclear dynamics en route to double ionization journal August 2021
Femtosecond dynamics of multielectron dissociative ionization by use of a picosecond laser journal June 1987
Molpro: a general-purpose quantum chemistry program package: Molpro
  • Werner, Hans-Joachim; Knowles, Peter J.; Knizia, Gerald
  • Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 2, Issue 2 https://doi.org/10.1002/wcms.82
journal July 2011
Concluding remarks: The age of molecular movies journal January 2021
Elusive enhanced ionization structure for H 2 + in intense ultrashort laser pulses journal December 2008
The H2O2+ potential energy surfaces dissociating into H+/OH+: Theoretical analysis of the isotopic effect journal July 2009