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Attosecond transient-absorption spectroscopy of polar molecules
摘要： We apply attosecond transient absorption spectroscopy (ATAS) to explore the effects of a nonzero permanent dipole on electron dynamics at the subfemtosecond scale, exemplified in the polar LiF molecule. In contrast with nonpolar systems, a familiar feature of the ATA spectra—the light-induced structures—are observed adjacent to a bright state. Moreover, a previously unobserved ladder structure is identified. The observations are analyzed in the context of a model based on fixed-nuclei adiabatic states, supported by full numerical simulations. Analytic calculations originating in the adiabatic model shed light on the nature and origins of the findings.
关键词： LiF molecule,attosecond transient absorption spectroscopy,electron dynamics,polar molecules,ladder structure,light-induced structures
更新于2025-09-23 15:21:01
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[IEEE 2019 Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC) - Munich, Germany (2019.6.23-2019.6.27)] 2019 Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC) - Optically Driven Attosecond Electron Dynamics in III-V Semiconductors
摘要： A fundamental understanding of ultrafast electron dynamics in solids induced by light is of great interest for future high-speed electro-optical devices operating in the petahertz frequency regime. In the last years, a number of publications demonstrated the possibility to resolve and control carrier dynamics in semiconductors and dielectrics on the few- to sub-femtosecond time scale using attosecond transient absorption spectroscopy (ATAS). These experiments were performed with a non-resonant pump pulse, i.e. pump photon energies smaller than the corresponding band gap. Here in contrast, we resolve for the first time the attosecond carrier dynamics induced by a resonant intense laser pulse. We study the attosecond electronic response in gallium arsenide (GaAs), a technologically important narrow band gap semiconductor.
关键词： gallium arsenide,III-V semiconductors,attosecond transient absorption spectroscopy,ultrafast electron dynamics,attosecond electron dynamics
更新于2025-09-11 14:15:04
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State-Resolved Probing of Attosecond Timescale Molecular Dipoles
摘要： We report an experimental study of iodomethane attosecond transient absorption spectroscopy (ATAS) in the region of iodine 4d core-to-valence/Rydberg excitation. Similar to previous atomic experiments, XUV-NIR delay-dependent absorbance changes reflect a light-induced phase due to an NIR-field driven AC Stark shift of the excited states, as well as pathway interferences arising from couplings between neighboring states. As a novel aspect of molecular ATAS, we observe pronounced differences between the ATAS signatures of valence and Rydberg states. While the core-to-valence transitions carry the majority of the XUV oscillator strength, the core-to-Rydberg transitions are dominantly affected by a moderately strong, non-ionizing NIR field. Our experimental findings are corroborated by ab-initio calculations and ATAS simulations.
关键词： core-to-valence,attosecond transient absorption spectroscopy,iodomethane,core-to-Rydberg,AC Stark shift,ab-initio calculations,XUV-NIR
更新于2025-09-04 15:30:14