Transient Impulsive Giant Electronic Raman Redistribution

TL;DR

This paper demonstrates that attosecond pulses can induce transient impulsive stimulated Raman scattering, which can surpass ionization effects, enabling high-fidelity multidimensional spectroscopy in molecules.

Contribution

The study introduces a novel approach using attosecond pulses to dominate ionization and enable Raman spectroscopy, applicable to molecular systems beyond atomic sodium.

Findings

Attosecond pulses can induce Raman scattering that overcomes ionization.

The method is demonstrated through calculations on atomic sodium.

Potential for high-resolution multidimensional spectroscopy with attosecond pulses.

Abstract

Resonant Raman excitation by ultrafast vacuum ultraviolet laser pulses is a powerful means to study electron dynamics in molecules, but experiments must contend with linear background ionization: frequencies high enough to reach resonant core-valence transitions will usually ionize all occupied orbitals as well, and the ionization cross sections are usually dominant. Here we show that attosecond pulses can induce a process, transient impulsive stimulated Raman scattering, which can overwhelm valence ionization. Calculations are performed for atomic sodium, but the principal is valid for many molecular systems. This approach opens the path for high fidelity multidimensional spectroscopy with attosecond pulses.