Probing ultrafast excited-state dynamics using EUV-IR six-wave-mixing emission spectroscopy

Non-linear processes such as four-wave-mixing have become instrumental in attosecond EUV spectroscopy. Using EUV high harmonics in conjunction with collinear near-infrared and mid-infrared fields, we extended this approach to high-order-mixing between three colors. Specifically, we find that atomic resonances in neon exhibit a significant cross section for six-wave mixing. The MIR probe frequency tunability in our multicolor scheme is employed to access several optically dark resonances and probe the quantum beat of a coherent electronic wavepacket using background-free EUV emission as a diagnostic. This technique can be easily extended to other atomic and molecular systems, and opens the door to multi-dimensional non-linear spectroscopy.