Observing the Structural Evolution in the Photodissociation of Diiodomethane with Femtosecond Solution X-Ray Scattering
Abstract
Resolving the structural dynamics of the initial steps of chemical reactions is challenging. We report the femtosecond time-resolved wide-angle x-ray scattering of the photodissociation of diiodomethane in cyclohexane. The data reveal with structural detail how the molecule dissociates into radicals, how the radicals collide with the solvent, and how they form the photoisomer. We extract how translational and rotational kinetic energy is dispersed into the solvent. We also find that 85% of the primary radical pairs are confined to their original solvent cage and discuss how this influences the downstream recombination reactions.
- Authors:
-
;
;
;
;
;
;
more »
- Publication Date:
- Research Org.:
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); German Research Foundation (DFG); European Research Council (ERC)
- OSTI Identifier:
- 1724239
- Alternate Identifier(s):
- OSTI ID: 1768066
- Grant/Contract Number:
- AC02-76SF00515; 279944; 6581802; HU 1971-1/1; HU 1971-3/1; HU 1971-4/1; 2016A8037
- Resource Type:
- Published Article
- Journal Name:
- Physical Review Letters
- Additional Journal Information:
- Journal Name: Physical Review Letters Journal Volume: 125 Journal Issue: 22; Journal ID: ISSN 0031-9007
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemical Physics & Physical Chemistry; Chemical reactions; Structural properties; Liquids; Configuration interaction; Molecular dynamics; X-ray diffuse scattering
Citation Formats
Panman, Matthijs R., Biasin, Elisa, Berntsson, Oskar, Hermann, Markus, Niebling, Stephan, Hughes, Ashley J., Kübel, Joachim, Atkovska, Kalina, Gustavsson, Emil, Nimmrich, Amke, Dohn, Asmus O., Laursen, Mads, Zederkof, Diana B., Honarfar, Alireza, Tono, Kensuke, Katayama, Tetsuo, Owada, Shigeki, van Driel, Tim B., Kjaer, Kasper, Nielsen, Martin M., Davidsson, Jan, Uhlig, Jens, Haldrup, Kristoffer, Hub, Jochen S., and Westenhoff, Sebastian. Observing the Structural Evolution in the Photodissociation of Diiodomethane with Femtosecond Solution X-Ray Scattering. United States: N. p., 2020.
Web. doi:10.1103/PhysRevLett.125.226001.
Panman, Matthijs R., Biasin, Elisa, Berntsson, Oskar, Hermann, Markus, Niebling, Stephan, Hughes, Ashley J., Kübel, Joachim, Atkovska, Kalina, Gustavsson, Emil, Nimmrich, Amke, Dohn, Asmus O., Laursen, Mads, Zederkof, Diana B., Honarfar, Alireza, Tono, Kensuke, Katayama, Tetsuo, Owada, Shigeki, van Driel, Tim B., Kjaer, Kasper, Nielsen, Martin M., Davidsson, Jan, Uhlig, Jens, Haldrup, Kristoffer, Hub, Jochen S., & Westenhoff, Sebastian. Observing the Structural Evolution in the Photodissociation of Diiodomethane with Femtosecond Solution X-Ray Scattering. United States. https://doi.org/10.1103/PhysRevLett.125.226001
Panman, Matthijs R., Biasin, Elisa, Berntsson, Oskar, Hermann, Markus, Niebling, Stephan, Hughes, Ashley J., Kübel, Joachim, Atkovska, Kalina, Gustavsson, Emil, Nimmrich, Amke, Dohn, Asmus O., Laursen, Mads, Zederkof, Diana B., Honarfar, Alireza, Tono, Kensuke, Katayama, Tetsuo, Owada, Shigeki, van Driel, Tim B., Kjaer, Kasper, Nielsen, Martin M., Davidsson, Jan, Uhlig, Jens, Haldrup, Kristoffer, Hub, Jochen S., and Westenhoff, Sebastian. Tue .
"Observing the Structural Evolution in the Photodissociation of Diiodomethane with Femtosecond Solution X-Ray Scattering". United States. https://doi.org/10.1103/PhysRevLett.125.226001.
@article{osti_1724239,
title = {Observing the Structural Evolution in the Photodissociation of Diiodomethane with Femtosecond Solution X-Ray Scattering},
author = {Panman, Matthijs R. and Biasin, Elisa and Berntsson, Oskar and Hermann, Markus and Niebling, Stephan and Hughes, Ashley J. and Kübel, Joachim and Atkovska, Kalina and Gustavsson, Emil and Nimmrich, Amke and Dohn, Asmus O. and Laursen, Mads and Zederkof, Diana B. and Honarfar, Alireza and Tono, Kensuke and Katayama, Tetsuo and Owada, Shigeki and van Driel, Tim B. and Kjaer, Kasper and Nielsen, Martin M. and Davidsson, Jan and Uhlig, Jens and Haldrup, Kristoffer and Hub, Jochen S. and Westenhoff, Sebastian},
abstractNote = {Resolving the structural dynamics of the initial steps of chemical reactions is challenging. We report the femtosecond time-resolved wide-angle x-ray scattering of the photodissociation of diiodomethane in cyclohexane. The data reveal with structural detail how the molecule dissociates into radicals, how the radicals collide with the solvent, and how they form the photoisomer. We extract how translational and rotational kinetic energy is dispersed into the solvent. We also find that 85% of the primary radical pairs are confined to their original solvent cage and discuss how this influences the downstream recombination reactions.},
doi = {10.1103/PhysRevLett.125.226001},
journal = {Physical Review Letters},
number = 22,
volume = 125,
place = {United States},
year = {2020},
month = {11}
}
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1103/PhysRevLett.125.226001
https://doi.org/10.1103/PhysRevLett.125.226001
Other availability
Search WorldCat to find libraries that may hold this journal
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Rotational Dynamics of Coumarin 153: Time-Dependent Friction, Dielectric Friction, and Other Nonhydrodynamic Effects
journal, February 1997
- Horng, M. -L.; Gardecki, J. A.; Maroncelli, M.
- The Journal of Physical Chemistry A, Vol. 101, Issue 6
Structural Determination of a Transient Isomer of by Picosecond X-Ray Diffraction
journal, June 2005
- Davidsson, Jan; Poulsen, Jens; Cammarata, Marco
- Physical Review Letters, Vol. 94, Issue 24
Achieving few-femtosecond time-sorting at hard X-ray free-electron lasers
journal, February 2013
- Harmand, M.; Coffee, R.; Bionta, M. R.
- Nature Photonics, Vol. 7, Issue 3
Solvent dependent structural perturbations of chemical reaction intermediates visualized by time-resolved x-ray diffraction
journal, April 2009
- Vincent, Jonathan; Andersson, Magnus; Eklund, Mattias
- The Journal of Chemical Physics, Vol. 130, Issue 15
Analysis of time-resolved X-ray scattering data from solution-state systems
journal, February 2010
- Haldrup, Kristoffer; Christensen, Morten; Meedom Nielsen, Martin
- Acta Crystallographica Section A Foundations of Crystallography, Vol. 66, Issue 2
The ORCA program system: The ORCA program system
journal, June 2011
- Neese, Frank
- Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 2, Issue 1
Visualizing Solution-Phase Reaction Dynamics with Time-Resolved X-ray Liquidography
journal, February 2009
- Ihee, Hyotcherl
- Accounts of Chemical Research, Vol. 42, Issue 2
Vibrational relaxation and geminate recombination in the femtosecond‐photodissociation of triiodide in solution
journal, December 1996
- Kühne, Thomas; Vöhringer, Peter
- The Journal of Chemical Physics, Vol. 105, Issue 24
Beamline, experimental stations and photon beam diagnostics for the hard x-ray free electron laser of SACLA
journal, August 2013
- Tono, K.; Togashi, T.; Inubushi, Y.
- New Journal of Physics, Vol. 15, Issue 8
Studies of chemical reactivity in the condensed phase. I. The dynamics of iodine photodissociation and recombination on a picosecond time scale and comparison to theories for chemical reactions in solution
journal, January 1986
- Harris, A. L.; Berg, M.; Harris, C. B.
- The Journal of Chemical Physics, Vol. 84, Issue 2
Visualizing the non-equilibrium dynamics of photoinduced intramolecular electron transfer with femtosecond X-ray pulses
journal, March 2015
- Canton, Sophie E.; Kjær, Kasper S.; Vankó, György
- Nature Communications, Vol. 6, Issue 1
Energy-consistent relativistic pseudopotentials and correlation consistent basis sets for the 4d elements Y–Pd
journal, March 2007
- Peterson, Kirk A.; Figgen, Detlev; Dolg, Michael
- The Journal of Chemical Physics, Vol. 126, Issue 12
Direct photoisomerization of CH 2 I 2 vs. CHBr 3 in the gas phase: a joint 50 fs experimental and multireference resonance-theoretical study
journal, January 2016
- Borin, Veniamin A.; Matveev, Sergey M.; Budkina, Darya S.
- Physical Chemistry Chemical Physics, Vol. 18, Issue 41
Ultrafast Study of the Photodissociation of Bromoiodomethane in Acetonitrile upon 266 nm Excitation
journal, June 2002
- Tarnovsky, Alexander N.; Wall, Magnus; Gustafsson, Magnus
- The Journal of Physical Chemistry A, Vol. 106, Issue 25
Polyhalide photofragment spectra. I. Two‐photon two‐step photodissociation of methylene iodide
journal, September 1976
- Kroger, Peter M.; Demou, Peter C.; Riley, Stephen J.
- The Journal of Chemical Physics, Vol. 65, Issue 5
Development of ultrafast pump and probe experimental system at SACLA
journal, March 2013
- Sato, Takahiro; Togashi, Tadashi; Tono, Kensuke
- Journal of Physics: Conference Series, Vol. 425, Issue 9
P-LINCS: A Parallel Linear Constraint Solver for Molecular Simulation
journal, December 2007
- Hess, Berk
- Journal of Chemical Theory and Computation, Vol. 4, Issue 1
Ultrafast Dynamics of Solute-Solvent Complexation Observed at Thermal Equilibrium in Real Time
journal, August 2005
- Zheng, J.
- Science, Vol. 309, Issue 5739
Microscopic Viscosity and Rotational Diffusion of Proteins in a Macromolecular Environment
journal, May 1999
- Lavalette, Daniel; Tétreau, Catherine; Tourbez, Martine
- Biophysical Journal, Vol. 76, Issue 5
Template-stabilized oxidic nickel oxygen evolution catalysts
journal, July 2020
- Li, Nancy; Keane, Thomas P.; Veroneau, Samuel S.
- Proceedings of the National Academy of Sciences, Vol. 117, Issue 28
Solvation Can Open the Photoisomerization Pathway for the Direct Photodissociation Reaction of Diiodomethane: Transient Resonance Raman Observation of the Isodiiodomethane Photoproduct from Ultraviolet Excitation of Diiodomethane in the Solution Phase
journal, July 2000
- Zheng, Xuming; Phillips, David Lee
- The Journal of Physical Chemistry A, Vol. 104, Issue 29
A Leap-frog Algorithm for Stochastic Dynamics
journal, March 1988
- Van Gunsteren, W. F.; Berendsen, H. J. C.
- Molecular Simulation, Vol. 1, Issue 3
Mapping the emergence of molecular vibrations mediating bond formation
journal, June 2020
- Kim, Jong Goo; Nozawa, Shunsuke; Kim, Hanui
- Nature, Vol. 582, Issue 7813
Spatiotemporal Kinetics in Solution Studied by Time-Resolved X-Ray Liquidography (Solution Scattering)
journal, August 2009
- Kim, Tae Kyu; Lee, Jae Hyuk; Wulff, Michael
- ChemPhysChem, Vol. 10, Issue 12
GROMACS: High performance molecular simulations through multi-level parallelism from laptops to supercomputers
journal, September 2015
- Abraham, Mark James; Murtola, Teemu; Schulz, Roland
- SoftwareX, Vol. 1-2
GROMACS 4.5: a high-throughput and highly parallel open source molecular simulation toolkit
journal, February 2013
- Pronk, Sander; Páll, Szilárd; Schulz, Roland
- Bioinformatics, Vol. 29, Issue 7
Isodiiodomethane Is the Methylene Transfer Agent in Cyclopropanation Reactions with Olefins Using Ultraviolet Photolysis of Diiodomethane in Solutions: A Density Functional Theory Investigation of the Reactions of Isodiiodomethane, Iodomethyl Radical, and Iodomethyl Cation with Ethylene
journal, May 2001
- Phillips, David Lee; Fang, Wei-Hai; Zheng, Xuming
- Journal of the American Chemical Society, Vol. 123, Issue 18
Development and testing of a general amber force field
journal, January 2004
- Wang, Junmei; Wolf, Romain M.; Caldwell, James W.
- Journal of Computational Chemistry, Vol. 25, Issue 9
Ultrafast photodissociation of I 3 . Coherent photochemistry in solution
journal, March 1993
- Banin, Uri; Ruhman, Sanford
- The Journal of Chemical Physics, Vol. 98, Issue 6
Water-Mediated Ion Pairing: Occurrence and Relevance
journal, April 2016
- van der Vegt, Nico F. A.; Haldrup, Kristoffer; Roke, Sylvie
- Chemical Reviews, Vol. 116, Issue 13
Ultrafast X-ray Diffraction of Transient Molecular Structures in Solution
journal, August 2005
- Ihee, H.
- Science, Vol. 309, Issue 5738
Direct femtosecond measurements of single collision dominated geminate recombination times of small molecules in liquids
journal, March 1993
- Schwartz, Benjamin J.; King, Jason C.; Zhang, Jin Z.
- Chemical Physics Letters, Vol. 203, Issue 5-6
Femtosecond dynamics of dissociation and recombination in solvent cages
journal, July 1993
- Liu, Qianli; Wang, Juen-Kai; Zewail, Ahmed H.
- Nature, Vol. 364, Issue 6436
Anisotropy enhanced X-ray scattering from solvated transition metal complexes
journal, February 2018
- Biasin, Elisa; van Driel, Tim B.; Levi, Gianluca
- Journal of Synchrotron Radiation, Vol. 25, Issue 2
Balanced basis sets of split valence, triple zeta valence and quadruple zeta valence quality for H to Rn: Design and assessment of accuracy
journal, January 2005
- Weigend, Florian; Ahlrichs, Reinhart
- Physical Chemistry Chemical Physics, Vol. 7, Issue 18, p. 3297-3305
Some remarks about free radicals and the photochemistry of solutions
journal, January 1934
- Franck, J.; Rabinowitsch, E.
- Transactions of the Faraday Society, Vol. 30
Ultrafast electron diffraction imaging of bond breaking in di-ionized acetylene
journal, October 2016
- Wolter, B.; Pullen, M. G.; Le, A. -T.
- Science, Vol. 354, Issue 6310
Introducing a standard method for experimental determination of the solvent response in laser pump, X-ray probe time-resolved wide-angle X-ray scattering experiments on systems in solution
journal, January 2013
- Kjær, Kasper Skov; van Driel, Tim B.; Kehres, Jan
- Phys. Chem. Chem. Phys., Vol. 15, Issue 36
On the calculation of x-ray scattering signals from pairwise radial distribution functions
journal, November 2015
- Dohn, Asmus O.; Biasin, Elisa; Haldrup, Kristoffer
- Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 48, Issue 24
Direct observation of collective modes coupled to molecular orbital-driven charge transfer
journal, December 2015
- Ishikawa, T.; Hayes, S. A.; Keskin, S.
- Science, Vol. 350, Issue 6267
Solvent dependent branching between C-I and C-Br bond cleavage following 266 nm excitation of CH 2 BrI
journal, November 2013
- Anderson, Christopher P.; Spears, Kenneth G.; Wilson, Kaitlynn R.
- The Journal of Chemical Physics, Vol. 139, Issue 19
Molecular dynamics with coupling to an external bath
journal, October 1984
- Berendsen, H. J. C.; Postma, J. P. M.; van Gunsteren, W. F.
- The Journal of Chemical Physics, Vol. 81, Issue 8
Photo-induced reactions of CH2I2 in solution studied by the ultrafast transient absorption spectroscopy
journal, November 1996
- Saitow, Ken-ichi; Naitoh, Yukito; Tominaga, Keisuke
- Chemical Physics Letters, Vol. 262, Issue 5
Direct observation of bond formation in solution with femtosecond X-ray scattering
journal, February 2015
- Kim, Kyung Hwan; Kim, Jong Goo; Nozawa, Shunsuke
- Nature, Vol. 518, Issue 7539
Visualizing Chemical Reactions in Solution by Picosecond X-Ray Diffraction
journal, March 2004
- Plech, Anton; Wulff, Michael; Bratos, Savo
- Physical Review Letters, Vol. 92, Issue 12
Molekulare Theorie der Mikroreibung
journal, September 1953
- Gierer, A.; Wirtz, K.
- Zeitschrift für Naturforschung A, Vol. 8, Issue 9
Disentangling detector data in XFEL studies of temporally resolved solution state chemistry
journal, January 2015
- van Driel, Tim Brandt; Kjær, Kasper Skov; Biasin, Elisa
- Faraday Discussions, Vol. 177
Photochemistry of Diiodomethane in Solution Studied by Femtosecond and Nanosecond Laser Photolysis. Formation and Dark Reactions of the CH 2 I−I Isomer Photoproduct and Its Role in Cyclopropanation of Olefins
journal, January 2004
- Tarnovsky, Alexander N.; Sundström, Villy; Åkesson, Eva
- The Journal of Physical Chemistry A, Vol. 108, Issue 2
Femtosecond x-ray spectroscopy of an electrocyclic ring-opening reaction
journal, April 2017
- Attar, Andrew R.; Bhattacherjee, Aditi; Pemmaraju, C. D.
- Science, Vol. 356, Issue 6333
GROMACS molecule & liquid database
journal, January 2012
- van der Spoel, D.; van Maaren, P. J.; Caleman, C.
- Bioinformatics, Vol. 28, Issue 5
Raman bandshape analysis ofo-chlorobenzaldehyde: microviscosity-dependent study
journal, January 2004
- Gomti Devi, Th.; Kumar, Kamal
- Journal of Raman Spectroscopy, Vol. 35, Issue 10
The X-ray Pump–Probe instrument at the Linac Coherent Light Source
journal, April 2015
- Chollet, Matthieu; Alonso-Mori, Roberto; Cammarata, Marco
- Journal of Synchrotron Radiation, Vol. 22, Issue 3
MDAnalysis: A toolkit for the analysis of molecular dynamics simulations
journal, April 2011
- Michaud-Agrawal, Naveen; Denning, Elizabeth J.; Woolf, Thomas B.
- Journal of Computational Chemistry, Vol. 32, Issue 10
A beam branching method for timing and spectral characterization of hard X-ray free-electron lasers
journal, January 2016
- Katayama, Tetsuo; Owada, Shigeki; Togashi, Tadashi
- Structural Dynamics, Vol. 3, Issue 3
Solvent–iodine atom charge transfer absorption in liquid alkanes and cycloalkanes
journal, January 1975
- Logan, S. R.; Bonneau, R.; Joussot-Dubien, J.
- Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, Vol. 71, Issue 0
Fate of transient isomer of CH 2 I 2 : Mechanism and origin of ionic photoproducts formation unveiled by time-resolved x-ray liquidography
journal, June 2019
- Park, Sungjun; Choi, Jungkweon; Ki, Hosung
- The Journal of Chemical Physics, Vol. 150, Issue 22
Femtosecond X-ray emission study of the spin cross-over dynamics in haem proteins
journal, August 2020
- Kinschel, Dominik; Bacellar, Camila; Cannelli, Oliviero
- Nature Communications, Vol. 11, Issue 1
Femtosecond X-Ray Scattering Study of Ultrafast Photoinduced Structural Dynamics in Solvated
journal, June 2016
- Biasin, Elisa; van Driel, Tim Brandt; Kjær, Kasper S.
- Physical Review Letters, Vol. 117, Issue 1
Beamline for X-ray Free Electron Laser of SACLA
journal, March 2013
- Tono, K.; Inubushi, Y.; Sato, T.
- Journal of Physics: Conference Series, Vol. 425, Issue 7