Laser Sculpting of Atomic sp, sp<sup>2</sup>, and sp<sup>3</sup> Hybrid Orbitals

Liu, Chunmei; Manz, J.; Yang, Yonggang

doi:10.1002/cphc.201402588

Cited by 5 publications

(2 citation statements)

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“…One may thus consider the two laser pulses as "fractional π-pulses". Previously, it has been shown that fractional π-pulses are useful for other purposes as well, e.g., for laser generation of hybrid orbitals [47].…”

Section: Discussionmentioning

confidence: 99%

From Symmetry Breaking via Charge Migration to Symmetry Restoration in Electronic Ground and Excited States: Quantum Control on the Attosecond Time Scale

2019

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This article starts with an introductory survey of previous work on breaking and restoring the electronic structure symmetry of atoms and molecules by means of two laser pulses. Accordingly, the first pulse breaks the symmetry of the system in its ground state with irreducible representation IRREP g by exciting it to a superposition of the ground state and an excited state with different IRREP e . The superposition state is non-stationary, representing charge migration with period T in the sub-to few femtosecond time domains. The second pulse stops charge migration and restores symmetry by de-exciting the superposition state back to the ground state. Here, we present a new strategy for symmetry restoration: The second laser pulse excites the superposition state to the excited state, which has the same symmetry as the ground state, but different IRREP e . The success depends on perfect time delay between the laser pulses, with precision of few attoseconds. The new strategy is demonstrated by quantum dynamics simulation for an oriented model system, benzene.

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Section: Discussionmentioning

confidence: 99%

From Symmetry Breaking via Charge Migration to Symmetry Restoration in Electronic Ground and Excited States: Quantum Control on the Attosecond Time Scale

2019

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“…25 Since attosecond, strong pulses of circularly polarized light are the call of the day, strongfield effects in benzene invoke ample curiosity, for both experiments and theory. [25][26][27][28] The latest experiments on graphene have come up with new topological states created by laser pulses. 29 Even though the electronic structure of benzene is different from that of graphene, as the latter comprises a band structure that lacks a band gap, benzene can be considered a beginner's choice apropos model for graphene.…”

Section: Introductionmentioning

confidence: 99%

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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Time‐Dependent Extension of Grimme's Continuous Chirality Measure for Electronic Chirality Flips in Femto‐ and Attosecond Time Domains

Guo,

Haase,

Manz

et al. 2024

ChemPhysChem

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Grimme’s Continuous Chirality Measure (CCM ) was developed for comparisons of the chirality of the electronic wave functions of molecules, typically in their ground states. For example, CCM=14.5, 1.2, and 0.0 for alanine, hydrogen‐peroxide, and for achiral molecules, respectively. Well‐designed laser pulses can excite achiral molecules from the electronic ground state to time‐dependent chiral superposition states, with chirality flips in the femto‐ or even attosecond (fs or as) time domains. Here we provide a time‐dependent extension CCM(t) of Grimme’s CCM for trailing the electronic chirality flips. As examples, we consider two laser driven electronic wavefunctions which represent flips between opposite electronic enantiomers of oriented NaK within 4.76 fs and 433 as. The corresponding CCM(t) vary respectively from 14.5 or from 13.3 to 0.0, and back.

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Laser Sculpting of Atomic sp, sp², and sp³ Hybrid Orbitals

Cited by 5 publications

References 48 publications

From Symmetry Breaking via Charge Migration to Symmetry Restoration in Electronic Ground and Excited States: Quantum Control on the Attosecond Time Scale

From Symmetry Breaking via Charge Migration to Symmetry Restoration in Electronic Ground and Excited States: Quantum Control on the Attosecond Time Scale

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

Time‐Dependent Extension of Grimme's Continuous Chirality Measure for Electronic Chirality Flips in Femto‐ and Attosecond Time Domains

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Laser Sculpting of Atomic sp, sp2, and sp3 Hybrid Orbitals

Cited by 5 publications

References 48 publications

From Symmetry Breaking via Charge Migration to Symmetry Restoration in Electronic Ground and Excited States: Quantum Control on the Attosecond Time Scale

From Symmetry Breaking via Charge Migration to Symmetry Restoration in Electronic Ground and Excited States: Quantum Control on the Attosecond Time Scale

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

Time‐Dependent Extension of Grimme's Continuous Chirality Measure for Electronic Chirality Flips in Femto‐ and Attosecond Time Domains

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Product

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Laser Sculpting of Atomic sp, sp², and sp³ Hybrid Orbitals