Time-dependent Schrödinger equation for molecular core-hole dynamics
Abstract
X-ray spectroscopy is an important tool for the investigation of matter. X rays primarily interact with inner-shell electrons, creating core (inner-shell) holes that will decay on the time scale of attoseconds to a few femtoseconds through electron relaxations involving the emission of a photon or an electron. Furthermore, the advent of femtosecond x-ray pulses expands x-ray spectroscopy to the time domain and will eventually allow the control of core-hole population on time scales comparable to core-vacancy lifetimes. For both cases, a theoretical approach that accounts for the x-ray interaction while the electron relaxations occur is required. We describe a time-dependent framework, based on solving the time-dependent Schrödinger equation, that is suitable for describing the induced electron and nuclear dynamics.
- Authors:
-
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1393932
- Alternate Identifier(s):
- OSTI ID: 1342438
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review A
- Additional Journal Information:
- Journal Volume: 95; Journal Issue: 2; Journal ID: ISSN 2469-9926
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74 ATOMIC AND MOLECULAR PHYSICS
Citation Formats
Picón, A. Time-dependent Schrödinger equation for molecular core-hole dynamics. United States: N. p., 2017.
Web. doi:10.1103/PhysRevA.95.023401.
Picón, A. Time-dependent Schrödinger equation for molecular core-hole dynamics. United States. https://doi.org/10.1103/PhysRevA.95.023401
Picón, A. Wed .
"Time-dependent Schrödinger equation for molecular core-hole dynamics". United States. https://doi.org/10.1103/PhysRevA.95.023401. https://www.osti.gov/servlets/purl/1393932.
@article{osti_1393932,
title = {Time-dependent Schrödinger equation for molecular core-hole dynamics},
author = {Picón, A.},
abstractNote = {X-ray spectroscopy is an important tool for the investigation of matter. X rays primarily interact with inner-shell electrons, creating core (inner-shell) holes that will decay on the time scale of attoseconds to a few femtoseconds through electron relaxations involving the emission of a photon or an electron. Furthermore, the advent of femtosecond x-ray pulses expands x-ray spectroscopy to the time domain and will eventually allow the control of core-hole population on time scales comparable to core-vacancy lifetimes. For both cases, a theoretical approach that accounts for the x-ray interaction while the electron relaxations occur is required. We describe a time-dependent framework, based on solving the time-dependent Schrödinger equation, that is suitable for describing the induced electron and nuclear dynamics.},
doi = {10.1103/PhysRevA.95.023401},
journal = {Physical Review A},
number = 2,
volume = 95,
place = {United States},
year = {Wed Feb 01 00:00:00 EST 2017},
month = {Wed Feb 01 00:00:00 EST 2017}
}
Web of Science
Works referenced in this record:
Photoelectron Wave Function in Photoionization: Plane Wave or Coulomb Wave?
journal, October 2015
- Gozem, Samer; Gunina, Anastasia O.; Ichino, Takatoshi
- The Journal of Physical Chemistry Letters, Vol. 6, Issue 22
Linac Coherent Light Source: The first five years
journal, March 2016
- Bostedt, Christoph; Boutet, Sébastien; Fritz, David M.
- Reviews of Modern Physics, Vol. 88, Issue 1
Attosecond molecular dynamics: fact or fiction?
journal, February 2014
- Lépine, Franck; Ivanov, Misha Y.; Vrakking, Marc J. J.
- Nature Photonics, Vol. 8, Issue 3
Time-resolved X-ray spectroscopies of chemical systems: New perspectives
journal, May 2016
- Chergui, Majed
- Structural Dynamics, Vol. 3, Issue 3
Studies of differential and total photoionization cross sections of molecular nitrogen
journal, May 1982
- Lucchese, Robert R.; Raseev, Georges; McKoy, Vincent
- Physical Review A, Vol. 25, Issue 5
High-level multireference methods in the quantum-chemistry program system COLUMBUS: Analytic MR-CISD and MR-AQCC gradients and MR-AQCC-LRT for excited states, GUGA spin–orbit CI and parallel CI density
journal, January 2001
- Lischka, Hans; Shepard, Ron; Pitzer, Russell M.
- Physical Chemistry Chemical Physics, Vol. 3, Issue 5
Tracing nuclear-wave-packet dynamics in singly and doubly charged states of N and O with XUV-pump–XUV-probe experiments
journal, July 2012
- Magrakvelidze, M.; Herrwerth, O.; Jiang, Y. H.
- Physical Review A, Vol. 86, Issue 1
Self-consistent-field calculations of core excited states
journal, March 2009
- Besley, Nicholas A.; Gilbert, Andrew T. B.; Gill, Peter M. W.
- The Journal of Chemical Physics, Vol. 130, Issue 12
Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen
journal, January 1989
- Dunning, Thom H.
- The Journal of Chemical Physics, Vol. 90, Issue 2
Correlation effects in R-matrix calculations of electron-F2 elastic scattering cross sections
journal, October 2007
- Tarana, Michal; Horáček, Jiří
- The Journal of Chemical Physics, Vol. 127, Issue 15
Ultrafast isomerization initiated by X-ray core ionization
journal, September 2015
- Liekhus-Schmaltz, Chelsea E.; Tenney, Ian; Osipov, Timur
- Nature Communications, Vol. 6, Issue 1
AMO science at the FLASH and European XFEL free-electron laser facilities
journal, August 2013
- Feldhaus, J.; Krikunova, M.; Meyer, M.
- Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 46, Issue 16
Compact XFEL and AMO sciences: SACLA and SCSS
journal, August 2013
- Yabashi, M.; Tanaka, H.; Tanaka, T.
- Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 46, Issue 16
Exploring few-photon, few-electron reactions at FLASH: from ion yield and momentum measurements to time-resolved and kinematically complete experiments
journal, September 2010
- Rudenko, A.; Jiang, Y. H.; Kurka, M.
- Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 43, Issue 19
New developments in the theory of molecular K-shell photoionization
journal, January 2007
- Cherepkov, N. A.; Semenov, S. K.
- International Journal of Quantum Chemistry, Vol. 107, Issue 14
Coherent Multidimensional Optical Probes for Electron Correlations and Exciton Dynamics: From NMR to X-rays
journal, April 2009
- Mukamel, Shaul; Abramavicius, Darius; Yang, Lijun
- Accounts of Chemical Research, Vol. 42, Issue 4
Measurement and laser control of attosecond charge migration in ionized iodoacetylene
journal, October 2015
- Kraus, P. M.; Mignolet, B.; Baykusheva, D.
- Science, Vol. 350, Issue 6262
Transient lattice contraction in the solid-to-plasma transition
journal, January 2016
- Ferguson, Ken R.; Bucher, Maximilian; Gorkhover, Tais
- Science Advances, Vol. 2, Issue 1
Vibrationally resolved decay spectra of CO at the C and O K-edges: experiment and theory
journal, December 1997
- Piancastelli, M. N.; Neeb, M.; Kivimäki, A.
- Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 30, Issue 24
Decoherence in Attosecond Photoionization
journal, February 2011
- Pabst, Stefan; Greenman, Loren; Ho, Phay J.
- Physical Review Letters, Vol. 106, Issue 5
Synchronized pulses generated at 20 eV and 90 eV for attosecond pump–probe experiments
journal, May 2015
- Fabris, D.; Witting, T.; Okell, W. A.
- Nature Photonics, Vol. 9, Issue 6
Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics
journal, May 2016
- Picón, A.; Lehmann, C. S.; Bostedt, C.
- Nature Communications, Vol. 7, Issue 1
Coherent and transient states studied with extreme ultraviolet and X-ray free electron lasers: present and future prospects
journal, April 2015
- Bencivenga, F.; Capotondi, F.; Principi, E.
- Advances in Physics, Vol. 63, Issue 5-6
Resonant Auger decay of the core-excited C O molecule in intense x-ray laser fields
journal, September 2011
- Demekhin, Philipp V.; Chiang, Ying-Chih; Cederbaum, Lorenz S.
- Physical Review A, Vol. 84, Issue 3
Tracking the Structural and Electronic Configurations of a Cobalt Proton Reduction Catalyst in Water
journal, August 2016
- Moonshiram, Dooshaye; Gimbert-Suriñach, Carolina; Guda, Alexander
- Journal of the American Chemical Society, Vol. 138, Issue 33
Strong-Field Many-Body Physics and the Giant Enhancement in the High-Harmonic Spectrum of Xenon
journal, December 2013
- Pabst, Stefan; Santra, Robin
- Physical Review Letters, Vol. 111, Issue 23
Electron Spectroscopy for Atoms, Molecules, and Condensed Matter
journal, July 1982
- Siegbahn, K.
- Science, Vol. 217, Issue 4555
Laser-induced continuum structure
journal, June 1990
- Knight, P. L.; Lauder, M. A.; Dalton, B. J.
- Physics Reports, Vol. 190, Issue 1
Single center method: A computational tool for ionization and electronic excitation studies of molecules
journal, January 2011
- Demekhin, Ph. V.; Ehresmann, A.; Sukhorukov, V. L.
- The Journal of Chemical Physics, Vol. 134, Issue 2
High-flux table-top soft x-ray source driven by sub-2-cycle, CEP stable, 185-μm 1-kHz pulses for carbon K-edge spectroscopy
journal, January 2014
- Cousin, S. L.; Silva, F.; Teichmann, S.
- Optics Letters, Vol. 39, Issue 18
A new approach to the random phase approximation
journal, August 1996
- Schirmer, J.; Mertins, F.
- Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 29, Issue 16
X-ray absorption spectroscopy
journal, August 2009
- Yano, Junko; Yachandra, Vittal K.
- Photosynthesis Research, Vol. 102, Issue 2-3
Attosecond science in atomic, molecular, and condensed matter physics
journal, January 2016
- Leone, Stephen R.; Neumark, Daniel M.
- Faraday Discussions, Vol. 194
Ultrafast x-ray-induced nuclear dynamics in diatomic molecules using femtosecond x-ray-pump–x-ray-probe spectroscopy
journal, July 2016
- Lehmann, C. S.; Picón, A.; Bostedt, C.
- Physical Review A, Vol. 94, Issue 1
Molecular Structural Dynamics Probed by Ultrafast X-Ray Absorption Spectroscopy
journal, March 2010
- Bressler, Christian; Chergui, Majed
- Annual Review of Physical Chemistry, Vol. 61, Issue 1
Mechanistic Evaluation of a Nickel Proton Reduction Catalyst Using Time-Resolved X-ray Absorption Spectroscopy
journal, September 2016
- Moonshiram, Dooshaye; Guda, Alexander; Kohler, Lars
- The Journal of Physical Chemistry C, Vol. 120, Issue 36
Generation of bright isolated attosecond soft X-ray pulses driven by multicycle midinfrared lasers
journal, May 2014
- Chen, M. -C.; Mancuso, C.; Hernandez-Garcia, C.
- Proceedings of the National Academy of Sciences, Vol. 111, Issue 23
Accurate calculation of core-electron binding energies: Multireference perturbation treatment
journal, January 2004
- Shirai, Soichi; Yamamoto, Satoru; Hyodo, Shi-aki
- The Journal of Chemical Physics, Vol. 121, Issue 16
Complex-basis-function treatment of photoionization in the random-phase approximation
journal, October 1987
- Yabushita, S.; McCurdy, C. W.; Rescigno, T. N.
- Physical Review A, Vol. 36, Issue 7
Optically-dressed resonant Auger processes induced by high-intensity x-rays
journal, August 2013
- Picón, Antonio; Ho, Phay J.; Doumy, Gilles
- New Journal of Physics, Vol. 15, Issue 8
Theory of high-harmonic generation by low-frequency laser fields
journal, March 1994
- Lewenstein, M.; Balcou, Ph.; Ivanov, M. Yu.
- Physical Review A, Vol. 49, Issue 3
Local against non-local complex potential in resonant electron-molecule scattering
journal, December 1981
- Cederbaum, L. S.; Domcke, W.
- Journal of Physics B: Atomic and Molecular Physics, Vol. 14, Issue 23
Spatiotemporal isolation of attosecond soft X-ray pulses in the water window
journal, March 2015
- Silva, Francisco; Teichmann, Stephan M.; Cousin, Seth L.
- Nature Communications, Vol. 6, Issue 1
Monitoring Ultrafast Chemical Dynamics by Time-Domain X-ray Photo- and Auger-Electron Spectroscopy
journal, December 2015
- Gessner, Oliver; Gühr, Markus
- Accounts of Chemical Research, Vol. 49, Issue 1
Competition between excitation and electronic decay of short-lived molecular states
journal, October 1996
- Pahl, E.; Meyer, H. -D.; Cederbaum, L. S.
- Zeitschrift f�r Physik D Atoms, Molecules and Clusters, Vol. 38, Issue 3
Optical control of resonant Auger processes
journal, January 2013
- Picón, Antonio; Buth, Christian; Doumy, Gilles
- Physical Review A, Vol. 87, Issue 1
Real-Time Probing of Electron Dynamics Using Attosecond Time-Resolved Spectroscopy
journal, May 2016
- Ramasesha, Krupa; Leone, Stephen R.; Neumark, Daniel M.
- Annual Review of Physical Chemistry, Vol. 67, Issue 1
Theory of resonance and threshold effects in electron-molecule collisions: The projection-operator approach
journal, October 1991
- Domcke, W.
- Physics Reports, Vol. 208, Issue 2
Group velocity matching in high-order harmonic generation driven by mid-infrared lasers
journal, July 2016
- Hernández-García, C.; Popmintchev, T.; Murnane, M. M.
- New Journal of Physics, Vol. 18, Issue 7
Ab initio calculation of interatomic decay rates by a combination of the Fano ansatz, Green’s-function methods, and the Stieltjes imaging technique
journal, November 2005
- Averbukh, Vitali; Cederbaum, Lorenz S.
- The Journal of Chemical Physics, Vol. 123, Issue 20
Femtochemistry: Atomic-Scale Dynamics of the Chemical Bond †
journal, June 2000
- Zewail, Ahmed H.
- The Journal of Physical Chemistry A, Vol. 104, Issue 24
Comparison of the random-phase approximation with the multichannel frozen-core Hartree-Fock approximation for the photoionization of
journal, July 1991
- Lucchese, Robert R.; Zurales, Robert W.
- Physical Review A, Vol. 44, Issue 1
Theoretical studies of core excitation and ionization in molecular systems
journal, March 2001
- Lin, Ping; Lucchese, Robert R.
- Journal of Synchrotron Radiation, Vol. 8, Issue 2
Visualizing Interfacial Charge Transfer in Ru-Dye-Sensitized TiO 2 Nanoparticles Using X-ray Transient Absorption Spectroscopy
journal, February 2011
- Zhang, Xiaoyi; Smolentsev, Grigory; Guo, Jianchang
- The Journal of Physical Chemistry Letters, Vol. 2, Issue 6
Stieltjes imaging of atomic and molecular photoabsorption profiles
journal, September 1973
- Langhoff, P. W.
- Chemical Physics Letters, Vol. 22, Issue 1
Photoionization cross section by Stieltjes imaging applied to coupled cluster Lanczos pseudo-spectra
journal, September 2013
- Cukras, Janusz; Coriani, Sonia; Decleva, Piero
- The Journal of Chemical Physics, Vol. 139, Issue 9
Direct, atomic orbital, static exchange calculations of photoabsorption spectra of large molecules and clusters
journal, May 1994
- Ågren, Hans; Carravetta, Vincenzo; Vahtras, Olav
- Chemical Physics Letters, Vol. 222, Issue 1-2
Transient lattice contraction in the solid-to-plasma transition
text, January 2016
- Ferguson, K. R.; Bucher, M.; Gorkhover, Tais
- Technische Universität Berlin
Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics
text, January 2016
- Picón, A.; Lehmann, C. S.; Bostedt, C.
- Deutsches Elektronen-Synchrotron, DESY, Hamburg
Measurement and laser control of attosecond charge migration in ionized iodoacetylene
text, January 2015
- Kraus, Peter M.; Mignolet, Benoît; Baykusheva, Denitsa
- ETH Zurich
Ultrafast x-ray-induced nuclear dynamics in diatomic molecules using femtosecond x-ray-pump–x-ray-probe spectroscopy
text, January 2016
- Lehmann, C. S.; Picón, A.; Bostedt, C.
- Deutsches Elektronen-Synchrotron, DESY, Hamburg
Generation of Bright Isolated Attosecond Soft X-Ray Pulses Driven by Multi-Cycle Mid-Infrared Lasers
conference, January 2014
- Chen, M. -C.; Mancuso, C.; Hernández-García, C.
- Laser Science, Frontiers in Optics 2014
Decoherence in Attosecond Photoionization
text, January 2011
- Pabst, Stefan; Greenman, Loren; Ho, Phay J.
- arXiv
Resonant Auger decay of the core-excited C$^\ast$O molecule in intense X-ray laser fields
text, January 2011
- Demekhin, Philipp V.; Chiang, Ying-Chih; Cederbaum, Lorenz S.
- arXiv
Optical control of resonant Auger processes
text, January 2013
- Picón, Antonio; Buth, Christian; Doumy, Gilles
- arXiv
Strong-Field Many-Body Physics and the Giant Enhancement in the High-Harmonic Spectrum of Xenon
text, January 2013
- Pabst, Stefan; Santra, Robin
- arXiv
Generation of Bright Isolated Attosecond Soft X-Ray Pulses Driven by Multi-Cycle Mid-Infrared Lasers
text, January 2014
- Chen, M. -C.; Hernández-García, C.; Mancuso, C.
- arXiv
Works referencing / citing this record:
Attosecond x-ray transient absorption in condensed-matter: a core-state-resolved Bloch model
journal, April 2019
- Picón, A.; Plaja, L.; Biegert, J.
- New Journal of Physics, Vol. 21, Issue 4
Comparison of Hartree–Fock and Hartree–Fock–Slater approximations for calculation of radiation damage dynamics of light and heavy atoms in the field of an x-ray free-electron laser
journal, April 2019
- Kozlov, A.; Quiney, H. M.
- Physica Scripta, Vol. 94, Issue 7
Comparison of Hartree-Fock and Hartree-Fock-Slater approximations for calculation of radiation damage dynamics of light and heavy atoms in the field of x-ray free electron laser
text, January 2018
- Kozlov, Alexander; Quiney, Harry M.
- arXiv