Two-dimensional nonlinear spectroscopy in the extreme ultraviolet to study dynamics of atomic and molecular gases

We present a two-dimensional (2D) nonlinear four-wave mixing scheme in the extreme ultraviolet (XUV) to investigate ultrafast electronic wave-packets dynamics of multi-electron states in the above-threshold ionization region, using atomic argon and molecular nitrogen as examples. Coherent light sources in the range between 24 and 45 eV is generated by phase-matched cascaded four-wave mixing processes with a collinear configuration of laser fields 800 nm and 1400 nm. Motion of the electrons involving the excited states 3s3p⁶np (¹ P₁⁰) of argon gas, the F²Σ_g⁺ state and the predissociation state C²Σ_u⁺ of molecular nitrogen ion N₂⁺ are unravelled through the ‘on-axis’ and ‘off-axis’ features of the two-dimensional spectra. Interpretation of the experimental data is supported by a theoretical dipole control model. Hence, results of this study may be promising for studies of dynamics of electrons in more complex systems.