Time-resolved four-wave-mixing spectroscopy for inner-valence transitions

Abstract

Non-collinear four-wave mixing (FWM) techniques at near-infrared (NIR), visible, and ultraviolet frequencies have been widely used to map vibrational and electronic couplings, typically in complex molecules. However, correlations between spatially localized inner-valence transitions among different sites of a molecule in the extreme ultraviolet (XUV) spectral range have not been observed yet. As an experimental step towards this goal we perform time-resolved FWM spectroscopy with femtosecond NIR and attosecond XUV pulses. The first two pulses (XUV-NIR) coincide in time and act as coherent excitation fields, while the third pulse (NIR) acts as a probe. As a first application we show how coupling dynamics between odd- and even-parity inner-valence excited states of neon can be revealed using a two-dimensional spectral representation. Experimentally obtained results are found to be in good agreement with ab initio time-dependent R-matrix calculations providing the full description of multi-electron interactions, as well as few-level model simulations. Future applications of this method also include site-specific probing of electronic processes in molecules.

5 pages, 3 figures

References in corpus (7)

• Lorentz meets Fano spectral line shapes: A universal phase and its laser control
• Quantum interference in attosecond transient absorption of laser-dressed helium atoms
• Coherent ultrafast core-hole correlation spectroscopy: x-ray analogues of multidimensional NMR
• Photoabsorption of attosecond XUV light pulses by two strongly laser-coupled autoionizing states
• Two-dimensional spectral interpretation of time-dependent absorption near laser-coupled resonances
• In situ characterization of few-cycle laser pulses in transient absorption spectroscopy
• Quantum Interferometry and Correlated Two-Electron Wave-Packet Observation in Helium

Cited by in corpus (15)

• RMT: R-matrix with time-dependence. Solving the semi-relativistic, time-dependent Schrodinger equation for general, multi-electron atoms and molecules in intense, ultrashort, arbitrarily polarized laser pulses
• $R$-matrix with Time-dependence Theory for Ultrafast Atomic Processes in Arbitrary Light Fields
• XUV-initiated high harmonic generation: driving inner valence electrons using below-threshold-energy XUV light
• XUV Spectral Compression by Four-Wave Mixing
• Coupled Valence Carrier and Core-Exciton Dynamics in WS${}_2$ Probed by Few-Femtosecond Extreme Ultraviolet Transient Absorption Spectroscopy
• Pulse-shape control of two-color interference in high-order-harmonic generation
• Extreme-ultraviolet-initiated High-harmonic Generation in Ar${}^{+}$
• Relativistic time-dependent configuration-interaction singles
• Non-resonant Coherent Amplitude Transfer in Attosecond Four-Wave Mixing Spectroscopy
• Measuring autoionization decay lifetimes of optically forbidden inner valence excited states in neon atoms with attosecond noncollinear four wave mixing spectroscopy
• On the Cooper Minimum in Singly ionized and Neutral Argon
• High-Gain Harmonic Generation with temporally overlapping seed pulses and application to ultrafast spectroscopy
• Spin and spatial dynamics in electron-impact scattering off S-wave He using R-matrix with Time-Dependence theory
• Time-Resolved Ultrafast Transient Polarization Spectroscopy to Investigate Nonlinear Processes and Dynamics in Electronically Excited Molecules on the Femtosecond Time Scale
• Probing coherent electronic superpositions of singly- and doubly-excited states of krypton with attosecond four-wave mixing spectroscopy