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Quantum Interference Paves the Way for Long-Lived Electronic Coherences

Diptesh Dey, Alexander I. Kuleff, Graham A. Worth

2022Physical Review Letters28 citationsDOIOpen Access PDF

Abstract

The creation and dynamical fate of a coherent superposition of electronic states generated in a polyatomic molecule by broadband ionization with extreme ultraviolet pulses is studied using the multiconfiguration time-dependent Hartree method together with an ionization continuum model Hamiltonian. The electronic coherence between the hole states usually lasts until the nuclear dynamics leads to decoherence. A key goal of attosecond science is to control the electronic motion and design laser control schemes to retain this coherence for longer timescales. Here, we investigate this possibility using time-delayed pulses and show how this opens up the prospect of coherent control of charge migration phenomenon.

Topics & Concepts

AttosecondPhysicsIonizationCoherence (philosophical gambling strategy)Superposition principleCoherent controlQuantum decoherenceHamiltonian (control theory)Polyatomic ionQuantumPhotoionizationQuantum mechanicsExtreme ultravioletQuantum opticsAtomic physicsLaserUltrashort pulseMoleculeIonMathematical optimizationMathematicsLaser-Matter Interactions and ApplicationsSpectroscopy and Quantum Chemical StudiesPhotoreceptor and optogenetics research
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