Molecular Modes of Attosecond Charge Migration

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

doi:10.1103/physrevlett.126.133002

Cited by 53 publications

(61 citation statements)

References 45 publications

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“…This could be a more natural state to begin the KS calculation in some situations, e.g., if the state was prepared in such a superposition at the initial time, however, it is inaccessible in a KS evolution that begins in the ground state, as discussed earlier. The importance of judiciously choosing the KS initial state when using an adiabatic approximation has been realized and exploited in strong-field charge-migration simulations [9,54,55].…”

Section: Dynamics In the Helium Atommentioning

confidence: 99%

“…Mapping to a noninteracting system, the Kohn-Sham (KS) system, that exactly reproduces the one-body density allows the computation of much larger systems than with traditional wave-function methods, with no restriction on the strength of the applied fields nor on how far the system is driven from equilibrium, see Refs. [5][6][7][8][9][10] for examples in a range of recent applications.…”

Section: Introductionmentioning

confidence: 99%

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Exact time-dependent density-functional theory for nonperturbative dynamics of the helium atom

et al. 2021

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By inverting the time-dependent Kohn-Sham equation for a numerically exact dynamics of the helium atom, we show that the dynamical step and peak features of the exact correlation potential found previously in onedimensional models persist for real three-dimensional systems. We demonstrate that the Kohn-Sham and true current densities differ by a rotational component. The results have direct implications for approximate timedependent density functional theory calculations of atoms and molecules in strong fields, emphasizing the need to go beyond the adiabatic approximation, and highlighting caution in the quantitative use of the Kohn-Sham current.

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Section: Dynamics In the Helium Atommentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Exact time-dependent density-functional theory for nonperturbative dynamics of the helium atom

et al. 2021

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“…The characteristic few-electronvolt energy spacing of molecular valence orbitals dictates that coherent electronic motion can occur even before nuclear motions set in (e.g., 1 eV of energy spacing corresponds to an oscillation period of 4.1 fs). Observation of charge migration has been a central topic in attosecond science [4,5], and a number of experimental [6][7][8][9] and theoretical [10][11][12][13][14][15][16][17][18][19][20][21][22][23] studies have reported results the last few years. There are both exciting perspectives and unanswered questions regarding charge migration.…”

Section: Introductionmentioning

confidence: 99%

Theoretical analysis of the role of complex transition dipole phase in XUV transient-absorption probing of charge migration

Kobayashi,

Neumark,

Leone

2021

Preprint

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We theoretically investigate the role of complex dipole phase in the attosecond probing of charge migration. The iodobromoacetylene ion (ICCBr + ) is considered as an example, in which one can probe charge migration by accessing both the iodine and bromine ends of the molecule with different spectral windows of an extreme-ultraviolet (XUV) pulse. The analytical expression for transient absorption shows that the site-specific information of charge migration is encoded in the complex phase of cross dipole products for XUV transitions between the I-4𝑑 and Br-3𝑑 spectral windows. Ab-initio quantum chemistry calculations on ICCBr + reveal that there is a constant 𝜋 phase difference between the I-4𝑑 and Br-3𝑑 transient-absorption spectral windows, irrespective of the fine-structure energy splittings. Transient absorption spectra are simulated with a multistate model including the complex dipole phase, and the results correctly reconstruct the charge-migration dynamics via the quantum beats in the two element spectral windows, exhibiting out-of-phase oscillations.

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“…One example, which has attracted intense interest in the ultrafast community, is charge migration (CM): this coherent, back-and-forth hole motion is often considered a precursor to more permanent structural or chemical changes [4][5][6][7][8][9][10][11][12][13][14][15]. A number of theoretical and experimental studies concerning CM have been performed: for example, documenting and characterizing CM [5][6][7][8][9][10][11][12]16], investigating how to control CM and how it depends on the specifics of the molecule [8,17,18], and more recently, the evolution of the CM as the electron dynamics couple to the nuclear degrees of freedom [14,15,19,20].…”

mentioning

confidence: 99%

Characterizing Particle-Like Charge Migration Dynamics with High-Harmonic Sideband Spectroscopy

Hamer,

Mauger,

Folorunso

et al. 2022

Preprint

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We introduce high-harmonic sideband spectroscopy (HHSS) and show that it can be a robust probe of attosecond charge migration (CM) in a halogenated carbon-chain molecule. We simulate both the CM and 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.

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Molecular Modes of Attosecond Charge Migration

Cited by 53 publications

References 45 publications

Exact time-dependent density-functional theory for nonperturbative dynamics of the helium atom

Exact time-dependent density-functional theory for nonperturbative dynamics of the helium atom

Theoretical analysis of the role of complex transition dipole phase in XUV transient-absorption probing of charge migration

Characterizing Particle-Like Charge Migration Dynamics with High-Harmonic Sideband Spectroscopy

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