Monitoring nonadiabatic avoided crossing dynamics in molecules by ultrafast X-ray diffraction
Abstract
We examine time-resolved X-ray diffraction from molecules in the gas phase which undergo nonadiabatic avoided-crossing dynamics involving strongly coupled electrons and nuclei. Several contributions to the signal are identified, representing (in decreasing strength) elastic scattering, contributions of the electronic coherences created by nonadiabatic couplings in the avoided crossing regime, and inelastic scattering. The former probes the charge density and delivers direct information on the evolving molecular geometry. The latter two contributions are weaker and carry spatial information through the transition charge densities (off-diagonal elements of the charge-density operator). Furthermore, simulations are presented for the nonadiabatic harpooning process in the excited state of sodium fluoride.
- Authors:
-
- Univ. of California, Irvine, CA (United States). Chemistry Dept.
- Univ. of California, Irvine, CA (United States). Chemistry Dept. and Dept. of Physics and Astronomy
- Publication Date:
- Research Org.:
- Univ. of California, Irvine, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; Alexander von Humboldt Foundation (Germany)
- OSTI Identifier:
- 1429610
- Alternate Identifier(s):
- OSTI ID: 1361914
- Grant/Contract Number:
- FG02-04ER15571
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Structural Dynamics
- Additional Journal Information:
- Journal Volume: 4; Journal Issue: 5; Journal ID: ISSN 2329-7778
- Publisher:
- American Crystallographic Association/AIP
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE; materials; scattering; electrical conductivity; continuum mechanics; metals; diffraction optics; condensed matter electronic structure; condensed matter properties; electrical properties; signal processing
Citation Formats
Kowalewski, Markus, Bennett, Kochise, and Mukamel, Shaul. Monitoring nonadiabatic avoided crossing dynamics in molecules by ultrafast X-ray diffraction. United States: N. p., 2017.
Web. doi:10.1063/1.4984241.
Kowalewski, Markus, Bennett, Kochise, & Mukamel, Shaul. Monitoring nonadiabatic avoided crossing dynamics in molecules by ultrafast X-ray diffraction. United States. https://doi.org/10.1063/1.4984241
Kowalewski, Markus, Bennett, Kochise, and Mukamel, Shaul. Fri .
"Monitoring nonadiabatic avoided crossing dynamics in molecules by ultrafast X-ray diffraction". United States. https://doi.org/10.1063/1.4984241. https://www.osti.gov/servlets/purl/1429610.
@article{osti_1429610,
title = {Monitoring nonadiabatic avoided crossing dynamics in molecules by ultrafast X-ray diffraction},
author = {Kowalewski, Markus and Bennett, Kochise and Mukamel, Shaul},
abstractNote = {We examine time-resolved X-ray diffraction from molecules in the gas phase which undergo nonadiabatic avoided-crossing dynamics involving strongly coupled electrons and nuclei. Several contributions to the signal are identified, representing (in decreasing strength) elastic scattering, contributions of the electronic coherences created by nonadiabatic couplings in the avoided crossing regime, and inelastic scattering. The former probes the charge density and delivers direct information on the evolving molecular geometry. The latter two contributions are weaker and carry spatial information through the transition charge densities (off-diagonal elements of the charge-density operator). Furthermore, simulations are presented for the nonadiabatic harpooning process in the excited state of sodium fluoride.},
doi = {10.1063/1.4984241},
journal = {Structural Dynamics},
number = 5,
volume = 4,
place = {United States},
year = {Fri May 26 00:00:00 EDT 2017},
month = {Fri May 26 00:00:00 EDT 2017}
}
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Works referenced in this record:
X-ray imaging beyond the limits
journal, April 2009
- Chapman, Henry N.
- Nature Materials, Vol. 8, Issue 4
Imaging Molecular Motion: Femtosecond X-Ray Scattering of an Electrocyclic Chemical Reaction
journal, June 2015
- Minitti, M. P.; Budarz, J. M.; Kirrander, A.
- Physical Review Letters, Vol. 114, Issue 25
Molecular Imaging Using X-Ray Free-Electron Lasers
journal, April 2013
- Barty, Anton; Küpper, Jochen; Chapman, Henry N.
- Annual Review of Physical Chemistry, Vol. 64, Issue 1
Femtosecond real‐time probing of reactions. IV. The reactions of alkali halides
journal, December 1989
- Rose, Todd S.; Rosker, Mark J.; Zewail, Ahmed H.
- The Journal of Chemical Physics, Vol. 91, Issue 12
X-ray free-electron lasers
journal, November 2010
- McNeil, Brian W. J.; Thompson, Neil R.
- Nature Photonics, Vol. 4, Issue 12
The structure of short-lived excited states of molecular complexes by time-resolved X-ray diffraction
journal, February 2005
- Coppens, Philip; Vorontsov, Ivan I.; Graber, Tim
- Acta Crystallographica Section A Foundations of Crystallography, Vol. 61, Issue 2
Time-resolved x-ray diffraction: Statistical theory and its application to the photo-physics of molecular iodine
journal, June 2002
- Bratos, S.; Mirloup, F.; Vuilleumier, R.
- The Journal of Chemical Physics, Vol. 116, Issue 24
Conical Intersections: Theory, Computation and Experiment
book, November 2011
- Domcke, Wolfgang; Yarkony, David R.; Köppel, Horst
- Advanced Series in Physical Chemistry
Time-resolved structural studies at synchrotrons and X-ray free electron lasers: opportunities and challenges
journal, October 2012
- Neutze, Richard; Moffat, Keith
- Current Opinion in Structural Biology, Vol. 22, Issue 5
Monitoring Nonadiabatic Electron-Nuclear Dynamics in Molecules by Attosecond Streaking of Photoelectrons
journal, July 2016
- Kowalewski, Markus; Bennett, Kochise; Rouxel, Jérémy R.
- Physical Review Letters, Vol. 117, Issue 4
Time-, frequency-, and wavevector-resolved x-ray diffraction from single molecules
journal, May 2014
- Bennett, Kochise; Biggs, Jason D.; Zhang, Yu
- The Journal of Chemical Physics, Vol. 140, Issue 20
Single-particle structure determination by correlations of snapshot X-ray diffraction patterns
journal, January 2012
- Starodub, D.; Aquila, A.; Bajt, S.
- Nature Communications, Vol. 3, Issue 1
On the interpretation of time-resolved anisotropic diffraction patterns
journal, November 2010
- Lorenz, U.; Møller, K. B.; Henriksen, N. E.
- New Journal of Physics, Vol. 12, Issue 11
An accurate and efficient scheme for propagating the time dependent Schrödinger equation
journal, November 1984
- Tal‐Ezer, H.; Kosloff, R.
- The Journal of Chemical Physics, Vol. 81, Issue 9
Adiabatic approach for ultrafast quantum dynamics mediated by simultaneously active conical intersections
journal, October 2001
- Hofmann, Angelika; de Vivie-Riedle, Regina
- Chemical Physics Letters, Vol. 346, Issue 3-4
A perfectly matched layer applied to a reactive scattering problem
journal, August 2010
- Nissen, Anna; Karlsson, Hans O.; Kreiss, Gunilla
- The Journal of Chemical Physics, Vol. 133, Issue 5
X-ray free-electron lasers
journal, April 2005
- Feldhaus, J.; Arthur, J.; Hastings, J. B.
- Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 38, Issue 9
Femtosecond X-ray protein nanocrystallography
journal, February 2011
- Chapman, Henry N.; Fromme, Petra; Barty, Anton
- Nature, Vol. 470, Issue 7332, p. 73-77
Ultrafast X-ray Diffraction Theory
journal, November 1998
- Cao, Jianshu; Wilson, Kent R.
- The Journal of Physical Chemistry A, Vol. 102, Issue 47
Quantum electrodynamical corrections to the fine structure of helium
journal, January 1974
- Douglas, Marvin; Kroll, Norman M.
- Annals of Physics, Vol. 82, Issue 1
Molecular Excited-State Structure by Time-Resolved Pump−Probe X-ray Diffraction. What Is New and What Are the Prospects for Further Progress?
journal, February 2011
- Coppens, Philip
- The Journal of Physical Chemistry Letters, Vol. 2, Issue 6
Femtosecond structural dynamics drives the trans/cis isomerization in photoactive yellow protein
journal, May 2016
- Pande, K.; Hutchison, C. D. M.; Groenhof, G.
- Science, Vol. 352, Issue 6286
Direct imaging of excited electronic states using diffraction techniques: theoretical considerations
journal, November 1996
- Ben-Nun, M.; Martínez, Todd J.; Weber, Peter M.
- Chemical Physics Letters, Vol. 262, Issue 3-4
Ultra-fast and ultra-intense x-ray sciences: first results from the Linac Coherent Light Source free-electron laser
journal, August 2013
- Bostedt, C.; Bozek, J. D.; Bucksbaum, P. H.
- Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 46, Issue 16
Single-molecule X-ray diffraction
journal, October 2000
- Hajdu, Janos
- Current Opinion in Structural Biology, Vol. 10, Issue 5
Catching Conical Intersections in the Act: Monitoring Transient Electronic Coherences by Attosecond Stimulated X-Ray Raman Signals
journal, November 2015
- Kowalewski, Markus; Bennett, Kochise; Dorfman, Konstantin E.
- Physical Review Letters, Vol. 115, Issue 19
On the Intensity of Total Scattering of X-Rays
journal, May 1929
- Waller, I.; Hartree, D. R.
- Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 124, Issue 793
Ultrafast structural changes measured by time-resolved X-ray diffraction
journal, June 1998
- Larsson, J.; Heimann, P. A.; Lindenberg, A. M.
- Applied Physics A: Materials Science & Processing, Vol. 66, Issue 6
Detection of Nonthermal Melting by Ultrafast X-ray Diffraction
journal, November 1999
- Siders, C. W.
- Science, Vol. 286, Issue 5443
Concerted electron and proton transfer in ionic crystals mapped by femtosecond x-ray powder diffraction
journal, August 2010
- Woerner, Michael; Zamponi, Flavio; Ansari, Zunaira
- The Journal of Chemical Physics, Vol. 133, Issue 6
Radiation Generated by the Ultrafast Migration of a Positive Charge Following the Ionization of a Molecular System
journal, January 2011
- Kuleff, Alexander I.; Cederbaum, Lorenz S.
- Physical Review Letters, Vol. 106, Issue 5
Recombination of photodissociated iodine: A time-resolved x-ray-diffraction study
journal, January 2006
- Wulff, M.; Bratos, S.; Plech, A.
- The Journal of Chemical Physics, Vol. 124, Issue 3
On the Theory of Time-Resolved X-ray Diffraction †
journal, January 2008
- Henriksen, Niels E.; Møller, Klaus B.
- The Journal of Physical Chemistry B, Vol. 112, Issue 2
Tracking the structural dynamics of proteins in solution using time-resolved wide-angle X-ray scattering
journal, September 2008
- Cammarata, Marco; Levantino, Matteo; Schotte, Friedrich
- Nature Methods, Vol. 5, Issue 10
Self-Referenced Coherent Diffraction X-Ray Movie of Ångstrom- and Femtosecond-Scale Atomic Motion
journal, October 2016
- Glownia, J. M.; Natan, A.; Cryan, J. P.
- Physical Review Letters, Vol. 117, Issue 15
Diffractive Imaging of Coherent Nuclear Motion in Isolated Molecules
journal, October 2016
- Yang, Jie; Guehr, Markus; Shen, Xiaozhe
- Physical Review Letters, Vol. 117, Issue 15
Relativistic electronic-structure calculations employing a two-component no-pair formalism with external-field projection operators
journal, June 1986
- Hess, Bernd A.
- Physical Review A, Vol. 33, Issue 6
A molecular conveyor belt by controlled delivery of single molecules into ultrashort laser pulses
journal, February 2012
- Kahra, Steffen; Leschhorn, Günther; Kowalewski, Markus
- Nature Physics, Vol. 8, Issue 3
X-Ray Diffraction Microscopy
journal, August 2010
- Thibault, Pierre; Elser, Veit
- Annual Review of Condensed Matter Physics, Vol. 1, Issue 1
Ultrafast X-ray Diffraction of Transient Molecular Structures in Solution
journal, August 2005
- Ihee, H.
- Science, Vol. 309, Issue 5738
Ab initio nonadiabatic quantum dynamics of cyclohexadiene/hexatriene ultrafast photoisomerization
journal, February 2006
- Tamura, Hiroyuki; Nanbu, Shinkoh; Ishida, Toshimasa
- The Journal of Chemical Physics, Vol. 124, Issue 8
Berry phase effects on electronic properties
journal, July 2010
- Xiao, Di; Chang, Ming-Che; Niu, Qian
- Reviews of Modern Physics, Vol. 82, Issue 3
Effects of Electron Correlation in X-Ray and Electron Diffraction
journal, September 1964
- Bartell, L. S.; Gavin, R. M.
- Journal of the American Chemical Society, Vol. 86, Issue 17
Field Operators in Real Space
journal, December 2015
- Cederbaum, Lorenz S.
- The Journal of Physical Chemistry A, Vol. 120, Issue 19
An Atomic-Level View of Melting Using Femtosecond Electron Diffraction
journal, November 2003
- Siwick, Bradley J.; Dwyer, Jason R.; Jordan, Robert E.
- Science, Vol. 302, Issue 5649
Imaging electronic quantum motion with light
journal, July 2012
- Dixit, G.; Vendrell, O.; Santra, R.
- Proceedings of the National Academy of Sciences, Vol. 109, Issue 29
Femtosecond structural dynamics drives the trans/cis isomerization in photoactive yellow protein
dataset, January 2019
- Pande, K.
- Coherent X-ray Imaging Data Bank (Lawrence Berkeley National Laboratory); UWM, LBNL, SLAC, CFEL, U Chicago
Ultrafast structural changes measured by time-resolved X-ray diffraction
journal, June 1998
- Larsson, J.; Heimann, P. A.; Lindenberg, A. M.
- Applied Physics A: Materials Science & Processing, Vol. 66, Issue 6
Quantum electrodynamical corrections to the fine structure of helium
journal, January 1974
- Douglas, Marvin; Kroll, Norman M.
- Annals of Physics, Vol. 82, Issue 1
Time-resolved structural studies at synchrotrons and X-ray free electron lasers: opportunities and challenges
journal, October 2012
- Neutze, Richard; Moffat, Keith
- Current Opinion in Structural Biology, Vol. 22, Issue 5
High-throughput protein crystallization
journal, October 2000
- Stevens, Raymond C.
- Current Opinion in Structural Biology, Vol. 10, Issue 5
Field Operators in Real Space
journal, December 2015
- Cederbaum, Lorenz S.
- The Journal of Physical Chemistry A, Vol. 120, Issue 19
Effects of Electron Correlation in X-Ray and Electron Diffraction
journal, September 1964
- Bartell, L. S.; Gavin, R. M.
- Journal of the American Chemical Society, Vol. 86, Issue 17
On the Theory of Time-Resolved X-ray Diffraction †
journal, January 2008
- Henriksen, Niels E.; Møller, Klaus B.
- The Journal of Physical Chemistry B, Vol. 112, Issue 2
Ultrafast X-ray Diffraction Theory
journal, November 1998
- Cao, Jianshu; Wilson, Kent R.
- The Journal of Physical Chemistry A, Vol. 102, Issue 47
Femtosecond X-ray protein nanocrystallography
journal, February 2011
- Chapman, Henry N.; Fromme, Petra; Barty, Anton
- Nature, Vol. 470, Issue 7332, p. 73-77
Single-particle structure determination by correlations of snapshot X-ray diffraction patterns
journal, January 2012
- Starodub, D.; Aquila, A.; Bajt, S.
- Nature Communications, Vol. 3, Issue 1
Tracking the structural dynamics of proteins in solution using time-resolved wide-angle X-ray scattering
journal, September 2008
- Cammarata, Marco; Levantino, Matteo; Schotte, Friedrich
- Nature Methods, Vol. 5, Issue 10
X-ray free-electron lasers
journal, November 2010
- McNeil, Brian W. J.; Thompson, Neil R.
- Nature Photonics, Vol. 4, Issue 12
A molecular conveyor belt by controlled delivery of single molecules into ultrashort laser pulses
journal, February 2012
- Kahra, Steffen; Leschhorn, Günther; Kowalewski, Markus
- Nature Physics, Vol. 8, Issue 3
Femtochemistry: the role of alignment and orientation
journal, January 1989
- Zewail, Ahmed H.
- Journal of the Chemical Society, Faraday Transactions 2, Vol. 85, Issue 8
Time-resolved x-ray diffraction: Statistical theory and its application to the photo-physics of molecular iodine
journal, June 2002
- Bratos, S.; Mirloup, F.; Vuilleumier, R.
- The Journal of Chemical Physics, Vol. 116, Issue 24
Recombination of photodissociated iodine: A time-resolved x-ray-diffraction study
journal, January 2006
- Wulff, M.; Bratos, S.; Plech, A.
- The Journal of Chemical Physics, Vol. 124, Issue 3
Ab initio nonadiabatic quantum dynamics of cyclohexadiene/hexatriene ultrafast photoisomerization
journal, February 2006
- Tamura, Hiroyuki; Nanbu, Shinkoh; Ishida, Toshimasa
- The Journal of Chemical Physics, Vol. 124, Issue 8
A perfectly matched layer applied to a reactive scattering problem
journal, August 2010
- Nissen, Anna; Karlsson, Hans O.; Kreiss, Gunilla
- The Journal of Chemical Physics, Vol. 133, Issue 5
Concerted electron and proton transfer in ionic crystals mapped by femtosecond x-ray powder diffraction
journal, August 2010
- Woerner, Michael; Zamponi, Flavio; Ansari, Zunaira
- The Journal of Chemical Physics, Vol. 133, Issue 6
An accurate and efficient scheme for propagating the time dependent Schrödinger equation
journal, November 1984
- Tal‐Ezer, H.; Kosloff, R.
- The Journal of Chemical Physics, Vol. 81, Issue 9
Ultra-fast and ultra-intense x-ray sciences: first results from the Linac Coherent Light Source free-electron laser
journal, August 2013
- Bostedt, C.; Bozek, J. D.; Bucksbaum, P. H.
- Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 46, Issue 16
On the interpretation of time-resolved anisotropic diffraction patterns
journal, November 2010
- Lorenz, U.; Møller, K. B.; Henriksen, N. E.
- New Journal of Physics, Vol. 12, Issue 11
On the Intensity of Total Scattering of X-Rays
journal, May 1929
- Waller, I.; Hartree, D. R.
- Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 124, Issue 793
An Atomic-Level View of Melting Using Femtosecond Electron Diffraction
journal, November 2003
- Siwick, Bradley J.; Dwyer, Jason R.; Jordan, Robert E.
- Science, Vol. 302, Issue 5649
Detection of Nonthermal Melting by Ultrafast X-ray Diffraction
journal, November 1999
- Siders, C. W.
- Science, Vol. 286, Issue 5443
Molecular Imaging Using X-Ray Free-Electron Lasers
journal, April 2013
- Barty, Anton; Küpper, Jochen; Chapman, Henry N.
- Annual Review of Physical Chemistry, Vol. 64, Issue 1
Imaging electronic quantum motion with light
text, January 2012
- Dixit, Gopal; Vendrell, Oriol; Santra, Robin
- arXiv
Time-, Frequency-, and Wavevector-Resolved X-Ray Diffraction from Single Molecules
text, January 2014
- Bennett, Kochise; Biggs, Jason D.; Zhang, Yu
- arXiv
Catching Conical Intersections in the Act; Monitoring Transient Electronic Coherences by Attosecond Stimulated X-Ray Raman Signals
text, January 2015
- Kowalewski, Markus; Bennett, Kochise; Dorfman, Konstantin E.
- arXiv
Self-referenced coherent diffraction x-ray movie of Angstrom- and femtosecond-scale atomic motion
text, January 2016
- Glownia, J. M.; Natan, A.; Cryan, J. P.
- arXiv
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- Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 51, Issue 3
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- Minemoto, Shinichirou; Shimada, Hiroyuki; Komatsu, Kazma
- Journal of Physics Communications, Vol. 2, Issue 11
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- Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 377, Issue 2145
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- Applied Sciences, Vol. 8, Issue 3
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- Hermann, Gunter; Pohl, Vincent; Dixit, Gopal
- arXiv
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