Title: Multiparticle cumulant mapping for Coulomb explosion imaging: Calculations and algorithm

Journal Article · · Physical Review A
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [4]; ORCiD logo [4]; ORCiD logo [3]
  1. Stony Brook Univ., NY (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Institute (PULSE); SLAC
  2. Imperial College, London (United Kingdom)
  3. Stony Brook Univ., NY (United States)
  4. SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Institute (PULSE); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
  5. SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Institute (PULSE); Stanford Univ., CA (United States)

We present a versatile cumulant mapping algorithm for analyzing correlated particle emission, offering insights into complex electronic and nuclear dynamics. Recently, we have demonstrated the use of cumulant mapping to extract information-rich correlations between the momenta of multiple fragments produced in Coulomb explosion imaging experiments [C. Cheng et al., Phys. Rev. Lett. 130, 093001 (2023)]. We define cumulant mapping in terms of histograms, enabling fast computation of linear (additive) observables. However, applying the same algorithm to nonlinear (nonadditive) observables poses challenges, as the computation time of conventional estimators scales nonlinearly with data size. To overcome this, we develop estimators and an accompanying algorithm to enable computationally efficient estimation of the cumulant of interest. Comparisons of computation times and signal-to-noise ratios reveal the superior performance of our approach. This method is demonstrated on the (D+, D+, C+, O+) dissociation channel of CD2⁢O4+ produced in a strong-field ionization experiment. Additionally, Poisson statistics are used to simulate the two methods and provide insights into the efficiency of our algorithm. The proposed methodology unlocks efficient computation of cumulant mapping for a broader range of complex systems and observables, such as the laser pulse dependence of ionization dynamics.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
Grant/Contract Number:
AC02-76SF00515; FG02-08ER15984
OSTI ID:
2405010
Journal Information:
Physical Review A, Journal Name: Physical Review A Journal Issue: 4 Vol. 109; ISSN 2469-9926
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

References (62)

Two pathways and an isotope effect in H3+ formation following double ionization of methanol journal July 2021
Multicoincidence studies of photo and Auger electrons from fixed-in-space molecules using the COLTRIMS technique journal December 2004
Novel developments and applications of two-dimensional correlation spectroscopy journal November 2016
Ultrafast Proton Transfer Dynamics on the Repulsive Potential of the Ethanol Dication: Roaming-Mediated Isomerization versus Coulomb Explosion journal March 2020
Covariance-Map Imaging: A Powerful Tool for Chemical Dynamics Studies journal January 2021
Strong Field Double Ionization of Formaldehyde Investigated Using Momentum Resolved Covariance Imaging and Trajectory Surface Hopping journal September 2022
Multi-Particle Three-Dimensional Covariance Imaging: “Coincidence” Insights into the Many-Body Fragmentation of Strong-Field Ionized D 2 O journal August 2021
Strong-Field-Induced Coulomb Explosion Imaging of Tribromomethane journal June 2022
Making Sense of Coulomb Explosion Imaging journal February 2019
Photoelectron angular distributions from strong-field ionization of oriented molecules journal May 2010
H2 roaming chemistry and the formation of H3+ from organic molecules in strong laser fields journal December 2018
X-ray multiphoton-induced Coulomb explosion images complex single molecules journal February 2022
Time-resolving the ultrafast H2 roaming chemistry and H3+ formation using extreme-ultraviolet pulses journal April 2020
Filming enhanced ionization in an ultrafast triatomic slingshot journal April 2023
N–NO & NN–O bond cleavage dynamics in two- and three-body Coulomb explosion of the N 2 O 2+ dication journal January 2019
Multi-particle momentum correlations extracted using covariance methods on multiple-ionization of diiodomethane molecules by soft-X-ray free-electron laser pulses journal January 2020
Multi-channel photodissociation and XUV-induced charge transfer dynamics in strong-field-ionized methyl iodide studied with time-resolved recoil-frame covariance imaging journal January 2021
Cumulant mapping as the basis of multi-dimensional spectrometry journal January 2022
Disentangling sequential and concerted fragmentations of molecular polycations with covariant native frame analysis journal January 2022
Velocity map imaging of ions and electrons using electrostatic lenses: Application in photoelectron and photofragment ion imaging of molecular oxygen journal September 1997
Control and femtosecond time-resolved imaging of torsion in a chiral molecule journal May 2012
Communication: Three-fold covariance imaging of laser-induced Coulomb explosions journal April 2016
Coincidence velocity map imaging using Tpx3Cam, a time stamping optical camera with 1.5 ns timing resolution journal November 2017
Communication: Gas-phase structural isomer identification by Coulomb explosion of aligned molecules journal March 2018
Coulomb explosion imaging of CH 3 I and CH 2 ClI photodissociation dynamics journal November 2018
Femtosecond laser induced Coulomb explosion imaging of aligned OCS oligomers inside helium nanodroplets journal October 2018
Threshold photodissociation dynamics of NO 2 studied by time-resolved cold target recoil ion momentum spectroscopy journal November 2019
Structure determination of the tetracene dimer in helium nanodroplets using femtosecond strong-field ionization journal July 2019
Time-resolved dissociative ionization and double photoionization of CO2 journal November 2020
A simple approach for characterizing the spatially varying sensitivity of microchannel plate detectors journal July 2022
Coincidence and covariance data acquisition in photoelectron and -ion spectroscopy. I. Formal theory journal October 2013
Coincidence and covariance data acquisition in photoelectron and -ion spectroscopy. II. Analysis and applications journal October 2013
Data treatment in multiparticle coincidence experiments: two-step dissociation processes journal July 1992
Statistical analysis of fragmentation channels of small multicharged molecular ions journal March 2012
Covariance mapping techniques journal July 2016
Laser-induced Coulomb explosion imaging of (C6H5Br)2 and C6H5Br–I2 dimers in helium nanodroplets using a Tpx3Cam journal September 2021
Electron correlation in channel-resolved strong-field molecular double ionization journal November 2019
Angle-dependent strong-field ionization and fragmentation of carbon dioxide measured using rotational wave packets journal October 2020
Momentum-resolved above-threshold ionization of deuterated water journal November 2020
Strong-field ionization of water: Nuclear dynamics revealed by varying the pulse duration journal April 2021
Strong-field ionization of water. II. Electronic and nuclear dynamics en route to double ionization journal August 2021
Laser Coulomb-explosion imaging of small molecules journal January 2005
Time-resolved Coulomb-explosion imaging of nuclear wave-packet dynamics induced in diatomic molecules by intense few-cycle laser pulses journal January 2011
Following dynamic nuclear wave packets in N 2 , O 2 , and CO with few-cycle infrared pulses journal October 2011
Covariance imaging experiments using a pixel-imaging mass-spectrometry camera journal January 2014
Theory and simulations of covariance mapping in multiple dimensions for data analysis in high-event-rate experiments journal May 2014
Coulomb-explosion imaging using a pixel-imaging mass-spectrometry camera journal May 2015
Coulomb-explosion imaging of concurrent CH 2 BrI photodissociation dynamics journal October 2017
Angular Tunneling Ionization Probability of Fixed-in-Space H 2 Molecules in Intense Laser Pulses journal January 2009
Ultrafast Extreme Ultraviolet Induced Isomerization of Acetylene Cations journal December 2010
Dynamics of Hollow Atom Formation in Intense X-Ray Pulses Probed by Partial Covariance Mapping journal August 2013
Dynamic Stark Control of Torsional Motion by a Pair of Laser Pulses journal August 2014
Alignment and Imaging of the CS2 Dimer Inside Helium Nanodroplets journal March 2018
Multiparticle Cumulant Mapping for Coulomb Explosion Imaging journal March 2023
Photoelectron Diffraction Mapping: Molecules Illuminated from Within journal June 2001
Coulomb explosion imaging of small polyatomic molecules with ultrashort x-ray pulses journal January 2022
Two-Dimensional Partial-Covariance Mass Spectrometry of Large Molecules Based on Fragment Correlations journal October 2020
Enantioselective fragmentation of an achiral molecule in a strong laser field journal March 2019
Direct Determination of Absolute Molecular Stereochemistry in Gas Phase by Coulomb Explosion Imaging journal September 2013
Covariance Mapping: A Correlation Method Applied to Multiphoton Multiple Ionization journal November 1989
Capturing roaming molecular fragments in real time journal November 2020
Dynamics of Fragmentation Reactions From Peak Shapes in Multiparticle Coincidence Experiments journal January 1991