A balancing act of two electrons on a symmetric double-well barrier in a high frequency oscillating field

Raj, Prashant; Balanarayan, P.

doi:10.1039/c8cp04812f

Cited by 7 publications

(4 citation statements)

References 51 publications

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“…In our work, the nuclear dynamics is only approximate. This is a reasonable approximation under high-frequency conditions, where the dynamics is mostly through the Kramers–Henneberger states . This approximate nuclear dynamics is portrayed in Figure .…”

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confidence: 73%

“…This is a reasonable approximation under high-frequency conditions, where the dynamics is mostly through the Kramers− Henneberger states. 34 This approximate nuclear dynamics is portrayed in Figure 6. To perform the nuclear dynamics, eigenstates of the field free inversion coordinate of ammonia are calculated using the sinc-DVR method 35 on a numerical grid, formed by the geometries at which the time-dependent energies have been calculated (see Figure 4b).…”

Section: Khmentioning

confidence: 99%

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Hovering States of Ammonia in a High-Intensity, High-Frequency Oscillating Field: Trapped into Planarity by Laser-Induced Hybridization

Kumar

Raj

Balanarayan

2019

J. Phys. Chem. Lett.

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A high-intensity, high-frequency laser can create an oscillating induced dipole moment in a molecule. At high laser frequencies with a long pulse width, a stable non-ionizing state with a laser-induced hybridization of the electrons is formed. For ammonia, aligned with the linear polarization direction of the laser, such stable states can be realized. Electronic hybridization in the presence of the high-frequency field is such that the lone pair propensity is dynamically equalized on either side of ammonia. This leads to a destabilization of pyramidal ammonia and hovering states with the electron density flipping to either side of the geometry. Electronic structure calculations in an oscillating frame of reference anticipate this effect with a predicted classical quiver distance of 0.1 Å. Electronic dynamics at a laser intensity of 1.14 × 1013 W/cm2 and a frequency of 8.16 eV predicts negligible ionization for the planar geometry. Approximate nuclear wave packet dynamics in the oscillating potential energy generated by the electrons predicts a trapping of ammonia in its planar transition state geometry.

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confidence: 73%

Section: Khmentioning

confidence: 99%

Hovering States of Ammonia in a High-Intensity, High-Frequency Oscillating Field: Trapped into Planarity by Laser-Induced Hybridization

Kumar

Raj

Balanarayan

2019

J. Phys. Chem. Lett.

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“…The present space–time description provides an enhanced view of the two-photon double-ionization processes, complimentary to the corresponding studies focusing exclusively on the final-state distributions. In view of the potential applications of quantum dot systems in optical and photonic applications [ 34 , 35 , 36 ], it is our intention to work further in this direction by studying more complex quantum dot systems of experimental interest.…”

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confidence: 99%

Dynamics of Correlated Double-Ionization of Two-Electron Quantum Dots in Laser Fields

Prior

Nikolopoulos

2023

Materials

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Using an ab initio, time-dependent calculational method, we study the non-linear dynamics of a two-electron quantum dot in the presence of ultrashort Thz laser pulses. The analysis of the contribution of the various partial waves to two-electron joint radial and energy distribution patterns revealed strongly correlated electron ejection channels. In the double-ionization process, regardless of the photon energy, the two-electron wave packets are born and remain concentrated until the pulse’s peak; at later times, and depending on the photon energy of the field, distinctly different patterns emerge. Our calculations also showed the gradual transition of the radial and energy patterns from a single-peak to a doubly peaked structure, associated with the direct and the sequential double-ionization mechanisms, respectively.

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“…[53][54][55][56] Here, a new fictitious time co-ordinate, denoted as t , is introduced in an extended Hilbert Space as ih ∂ ∂t + ∂ Here, a ĤF resembles a Floquet type operator in the t coordinate. The evolution equation of the wave function now takes the form:…”

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Bonding in light-induced vortices: benzene in a high-frequency circular polarized laser

Raj¹,

Paul²,

Mythreyi³

et al. 2019

Preprint

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The electronic structure of benzene in the presence of a high-intensity high-frequency circularly polarized laser supports a middle-of-the-ring electron localization. Here, the laser polarization coincides with the ring plane of benzene. The high-frequency oscillating electric field creates circular currents centered at each atom with a circle radius equal to the maximum field amplitude of the laser. All six carbons have six such rings.For a maximum field amplitude of 1.42 Å, which is the carbon-carbon bond distance, all six dynamic current circles intersect to create a deep vortex in the middle, which supports a bound state of a pair of electrons. Such states for benzene can be realized in experiments using a circularly polarized XUV-laser in a range of intensities 10 16 -10 17 W/cm 2 and frequencies 16 eV to 22 eV. Electronic dynamics calculations predict a minimal ionization of benzene when the rise-time of the laser pulse is sudden, indicating a possible experimental realization of these states characterized by a large cut-off in the harmonic generation spectra. This stable electronic structure of the light-dressed benzene is doubly-aromatic due to an extra aromaticity from a D 6h symmetric circular distortion of the σ-framework while the π-electrons, with low density in the ring-plane, are least affected.

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A balancing act of two electrons on a symmetric double-well barrier in a high frequency oscillating field

Abstract: Barrier top stabilization and temporal control of electrons in an oscillating electric field.

Cited by 7 publications

References 51 publications

Hovering States of Ammonia in a High-Intensity, High-Frequency Oscillating Field: Trapped into Planarity by Laser-Induced Hybridization

Hovering States of Ammonia in a High-Intensity, High-Frequency Oscillating Field: Trapped into Planarity by Laser-Induced Hybridization

Dynamics of Correlated Double-Ionization of Two-Electron Quantum Dots in Laser Fields

Bonding in light-induced vortices: benzene in a high-frequency circular polarized laser

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