Core-valence attosecond transient absorption spectroscopy of polyatomic molecules

Abstract

Tracing ultrafast processes induced by interaction of light with matter is often very challenging. In molecular systems, the initially created electronic coherence becomes damped by the slow nuclear rearrangement on a femtosecond timescale which makes real-time observations of electron dynamics in molecules particularly difficult. In this work, we report an extension of the theory underlying the attosecond transient absorption spectroscopy (ATAS) for the case of molecules, including a full account for the coupled electron-nuclear dynamics in the initially created wave packet, and apply it to probe the oscillations of the positive charge created after outer-valence ionization of the propiolic acid molecule. By taking advantage of element-specific core-to-valence transitions induced by X-ray radiation, we show that the resolution of ATAS makes it possible to trace the dynamics of electron density with atomic spatial resolution.

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Cited by in corpus (15)

• Decoherence and Revival in Attosecond Charge Migration Driven by Non-adiabatic Dynamics
• Search for long lasting electronic coherence using on-the-fly ab initio semiclassical dynamics
• Theoretical analysis of the role of complex transition dipole phase in XUV transient-absorption probing of charge migration
• Core excitations of uranyl in Cs${}_2$UO${}_2$Cl${}_4$ from relativistic embedded damped-response time-dependent density functional theory calculations
• Probing Vibronic Coherence in Charge Migration of Molecules Using Strong Field Sequential Double Ionization
• Resolving Competing Conical Intersection Pathways: Time-Resolved X-ray Absorption Spectroscopy of trans-1,3-Butadiene
• Electronic-vibrational dynamics and coherence in x-ray transient absorption of N2+ induced by strong-field ionization
• Unexpected dipole instabilities in small molecules after ultrafast XUV irradiation
• How to find molecules with long-lasting charge migration?
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• Correlation-Driven Charge Migration Triggered by Infrared Multi-Photon Ionization
• Control of valence-electron motion in Xe cations using the stimulated-Raman-adiabatic-passage technique
• Optical Interference Effect in Strong-field Electronic Coherence Spectroscopy
• Phase evolution of strong-field ionization
• Efficient Semiclassical Evaluation of Electronic Coherences in Polyatomic Molecules