Characterizing particle-like charge-migration dynamics with high-order harmonic sideband spectroscopy

Hamer, Kyle A.; Mauger, François; Folorunso, Aderonke S.; Lopata, Kenneth; Jones, Robert R.; DiMauro, Louis F.; Schafer, Kenneth J.; Gaarde, Mette B.

doi:10.1103/physreva.106.013103

Characterizing particle-like charge-migration dynamics with high-order harmonic sideband spectroscopy

Journal Article · Thu Jul 07 00:00:00 EDT 2022 · Physical Review A

DOI:https://doi.org/10.1103/physreva.106.013103· OSTI ID:1979624

^[1]; ^[2]; ^[2]; ^[2]; ^[3]; DiMauro, Louis F. ^[4]; Schafer, Kenneth J. ^[2]; Gaarde, Mette B. ^[2]

Louisiana State Univ., Baton Rouge, LA (United States); OSTI
Louisiana State Univ., Baton Rouge, LA (United States)
Univ. of Virginia, Charlottesville, VA (United States)
The Ohio State Univ., Columbus, OH (United States)

Here, we introduce high-order harmonic sideband spectroscopy and show that it can be a robust probe of charge migration (CM) in a halogenated carbon-chain molecule. We simulate both the CM and high-order harmonic generation (HHG) dynamics using ab initio time-dependent density-functional theory. We find that CM dynamics initiated along the molecular backbone induces sidebands in the HHG spectrum driven by a delayed laser pulse that is polarized perpendicular to the molecular axis. Monitoring the spectrum as either the HHG laser frequency or the relative delay is scanned allows for the extraction of detailed information about the time-domain characteristics of the CM process.

View Accepted Manuscript (DOE)

Research Organization:: Louisiana State Univ., Baton Rouge, LA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012462

OSTI ID:: 1979624

Journal Information:: Physical Review A, Journal Name: Physical Review A Journal Issue: 1 Vol. 106; ISSN 2469-9926

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (43)

Bemerkung zur Elektronentheorie des Ferromagnetismus und der elektrischen Leitf�higkeit Bloch, F. Zeitschrift f�r Physik, Vol. 57, Issue 7-8 https://doi.org/10.1007/BF01340281	journal	July 1929
Size effects in charge migration in alkyne chains Despré, Victor; Kuleff, Alexander I. Theoretical Chemistry Accounts, Vol. 138, Issue 9 https://doi.org/10.1007/s00214-019-2497-z	journal	August 2019
Ultrafast charge migration by electron correlation Cederbaum, L. S.; Zobeley, J. Chemical Physics Letters, Vol. 307, Issue 3-4 https://doi.org/10.1016/S0009-2614(99)00508-4	journal	July 1999
Libxc: A library of exchange and correlation functionals for density functional theory Marques, Miguel A. L.; Oliveira, Micael J. T.; Burnus, Tobias Computer Physics Communications, Vol. 183, Issue 10 https://doi.org/10.1016/j.cpc.2012.05.007	journal	October 2012
Ultrafast charge migration in 2-phenylethyl-N,N-dimethylamine Lünnemann, Siegfried; Kuleff, Alexander I.; Cederbaum, Lorenz S. Chemical Physics Letters, Vol. 450, Issue 4-6 https://doi.org/10.1016/j.cplett.2007.11.031	journal	January 2008
Note on Exchange Phenomena in the Thomas Atom Dirac, P. A. M. Mathematical Proceedings of the Cambridge Philosophical Society, Vol. 26, Issue 3 https://doi.org/10.1017/S0305004100016108	journal	July 1930
Attosecond Charge Migration with TDDFT: Accurate Dynamics from a Well-Defined Initial State Bruner, Adam; Hernandez, Samuel; Mauger, François The Journal of Physical Chemistry Letters, Vol. 8, Issue 17 https://doi.org/10.1021/acs.jpclett.7b01652	journal	August 2017
Attosecond Pump–Probe Spectroscopy of Charge Dynamics in Tryptophan Lara-Astiaso, Manuel; Galli, Mara; Trabattoni, Andrea The Journal of Physical Chemistry Letters, Vol. 9, Issue 16 https://doi.org/10.1021/acs.jpclett.8b01786	journal	July 2018
Modeling Fast Electron Dynamics with Real-Time Time-Dependent Density Functional Theory: Application to Small Molecules and Chromophores Lopata, Kenneth; Govind, Niranjan Journal of Chemical Theory and Computation, Vol. 7, Issue 5 https://doi.org/10.1021/ct200137z	journal	April 2011
Attosecond molecular dynamics: fact or fiction? Lépine, Franck; Ivanov, Misha Y.; Vrakking, Marc J. J. Nature Photonics, Vol. 8, Issue 3 https://doi.org/10.1038/nphoton.2014.25	journal	February 2014
Real-time observation of a correlation-driven sub 3 fs charge migration in ionised adenine Månsson, Erik P.; Latini, Simone; Covito, Fabio Communications Chemistry, Vol. 4, Issue 1 https://doi.org/10.1038/s42004-021-00510-5	journal	May 2021
Real-space grids and the Octopus code as tools for the development of new simulation approaches for electronic systems Andrade, Xavier; Strubbe, David; De Giovannini, Umberto Physical Chemistry Chemical Physics, Vol. 17, Issue 47 https://doi.org/10.1039/C5CP00351B	journal	January 2015
Ultrafast charge dynamics in glycine induced by attosecond pulses Ayuso, David; Palacios, Alicia; Decleva, Piero Physical Chemistry Chemical Physics, Vol. 19, Issue 30 https://doi.org/10.1039/C7CP01856H	journal	January 2017
The influence of initial conditions on charge transfer dynamics Eshuis, Henk; van Voorhis, Troy Physical Chemistry Chemical Physics, Vol. 11, Issue 44 https://doi.org/10.1039/b912085h	journal	January 2009
Propagators for the time-dependent Kohn–Sham equations Castro, Alberto; Marques, Miguel A. L.; Rubio, Angel The Journal of Chemical Physics, Vol. 121, Issue 8 https://doi.org/10.1063/1.1774980	journal	August 2004
Charge migration and charge transfer in molecular systems Wörner, Hans Jakob; Arrell, Christopher A.; Banerji, Natalie Structural Dynamics, Vol. 4, Issue 6 https://doi.org/10.1063/1.4996505	journal	November 2017
NWChem: Past, present, and future Aprà, E.; Bylaska, E. J.; de Jong, W. A. The Journal of Chemical Physics, Vol. 152, Issue 18 https://doi.org/10.1063/5.0004997	journal	May 2020
An electronic time scale in chemistry Remacle, F.; Levine, R. D. Proceedings of the National Academy of Sciences, Vol. 103, Issue 18 https://doi.org/10.1073/pnas.0601855103	journal	April 2006
Comparison of self-interaction-corrections for metal clusters Legrand, C.; Suraud, E.; Reinhard, P-G Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 35, Issue 4 https://doi.org/10.1088/0953-4075/35/4/333	journal	February 2002
Charge migration induced by attosecond pulses in bio-relevant molecules Calegari, Francesca; Trabattoni, Andrea; Palacios, Alicia Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 49, Issue 14 https://doi.org/10.1088/0953-4075/49/14/142001	journal	June 2016
Time-dependent density-functional theory in massively parallel computer architectures: the octopus project Andrade, Xavier; Alberdi-Rodriguez, Joseba; Strubbe, David A. Journal of Physics: Condensed Matter, Vol. 24, Issue 23 https://doi.org/10.1088/0953-8984/24/23/233202	journal	May 2012
Self-Consistent Equations Including Exchange and Correlation Effects Kohn, W.; Sham, L. J. Physical Review, Vol. 140, Issue 4A, p. A1133-A1138 https://doi.org/10.1103/PhysRev.140.A1133	journal	November 1965
Orbital-resolved calculations of two-center interferences in linear triatomic molecules Hamer, Kyle A.; Tuthill, Daniel R.; Scarborough, Timothy D. Physical Review A, Vol. 104, Issue 3 https://doi.org/10.1103/PhysRevA.104.033114	journal	September 2021
Control of charge migration in molecules by ultrashort laser pulses Golubev, Nikolay V.; Kuleff, Alexander I. Physical Review A, Vol. 91, Issue 5 https://doi.org/10.1103/PhysRevA.91.051401	journal	May 2015
Self-interaction correction to density-functional approximations for many-electron systems Perdew, J. P.; Zunger, Alex Physical Review B, Vol. 23, Issue 10, p. 5048-5079 https://doi.org/10.1103/PhysRevB.23.5048	journal	May 1981
High-Order Harmonic Generation Spectroscopy of Correlation-Driven Electron Hole Dynamics Leeuwenburgh, Jonathan; Cooper, Bridgette; Averbukh, Vitali Physical Review Letters, Vol. 111, Issue 12 https://doi.org/10.1103/PhysRevLett.111.123002	journal	September 2013
High-Harmonic Probing of Electronic Coherence in Dynamically Aligned Molecules Kraus, P. M.; Zhang, S. B.; Gijsbertsen, A. Physical Review Letters, Vol. 111, Issue 24 https://doi.org/10.1103/PhysRevLett.111.243005	journal	December 2013
Core Ionization Initiates Subfemtosecond Charge Migration in the Valence Shell of Molecules Kuleff, Alexander I.; Kryzhevoi, Nikolai V.; Pernpointner, Markus Physical Review Letters, Vol. 117, Issue 9 https://doi.org/10.1103/PhysRevLett.117.093002	journal	August 2016
Electron Dynamics upon Ionization of Polyatomic Molecules: Coupling to Quantum Nuclear Motion and Decoherence Vacher, Morgane; Bearpark, Michael J.; Robb, Michael A. Physical Review Letters, Vol. 118, Issue 8 https://doi.org/10.1103/PhysRevLett.118.083001	journal	February 2017
Charge Migration in Propiolic Acid: A Full Quantum Dynamical Study Despré, Victor; Golubev, Nikolay V.; Kuleff, Alexander I. Physical Review Letters, Vol. 121, Issue 20 https://doi.org/10.1103/PhysRevLett.121.203002	journal	November 2018
Molecular Modes of Attosecond Charge Migration Folorunso, Aderonke S.; Bruner, Adam; Mauger, François Physical Review Letters, Vol. 126, Issue 13 https://doi.org/10.1103/PhysRevLett.126.133002	journal	March 2021
Attosecond Pulse Trains Using High–Order Harmonics Antoine, Philippe; L'Huillier, Anne; Lewenstein, Maciej Physical Review Letters, Vol. 77, Issue 7 https://doi.org/10.1103/PhysRevLett.77.1234	journal	August 1996
Temporal Coherence of Ultrashort High-Order Harmonic Pulses Bellini, M.; Lyngå, C.; Tozzi, A. Physical Review Letters, Vol. 81, Issue 2 https://doi.org/10.1103/PhysRevLett.81.297	journal	July 1998
Strong Field Quantum Path Control Using Attosecond Pulse Trains Schafer, Kenneth J.; Gaarde, Mette B.; Heinrich, Arne Physical Review Letters, Vol. 92, Issue 2 https://doi.org/10.1103/PhysRevLett.92.023003	journal	January 2004
Universal Attosecond Response to the Removal of an Electron Breidbach, J.; Cederbaum, L. S. Physical Review Letters, Vol. 94, Issue 3 https://doi.org/10.1103/PhysRevLett.94.033901	journal	January 2005
Charge migration and attosecond solitons in conjugated organic molecules Mauger, François; Folorunso, Aderonke S.; Hamer, Kyle A. Physical Review Research, Vol. 4, Issue 1 https://doi.org/10.1103/PhysRevResearch.4.013073	journal	January 2022
Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule Barillot, T.; Alexander, O.; Cooper, B. Physical Review X, Vol. 11, Issue 3 https://doi.org/10.1103/PhysRevX.11.031048	journal	September 2021
Observation of a Train of Attosecond Pulses from High Harmonic Generation Paul, P. M. Science, Vol. 292, Issue 5522 https://doi.org/10.1126/science.1059413	journal	June 2001
Attosecond Synchronization of High-Harmonic Soft X-rays Mairesse, Y. Science, Vol. 302, Issue 5650 https://doi.org/10.1126/science.1090277	journal	November 2003
Ultrafast electron dynamics in phenylalanine initiated by attosecond pulses Calegari, F.; Ayuso, D.; Trabattoni, A. Science, Vol. 346, Issue 6207 https://doi.org/10.1126/science.1254061	journal	October 2014
Measurement and laser control of attosecond charge migration in ionized iodoacetylene Kraus, P. M.; Mignolet, B.; Baykusheva, D. Science, Vol. 350, Issue 6262 https://doi.org/10.1126/science.aab2160	journal	October 2015
Attosecond coherent electron motion in Auger-Meitner decay Li, Siqi; Driver, Taran; Rosenberger, Philipp Science, Vol. 375, Issue 6578 https://doi.org/10.1126/science.abj2096	journal	January 2022
Ckmeans.1d.dp: Optimal k-means Clustering in One Dimension by Dynamic Programming Wang, Haizhou; Song, Mingzhou The R Journal, Vol. 3, Issue 2 https://doi.org/10.32614/RJ-2011-015	journal	January 2011

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