Few-femtosecond soft X-ray transient absorption spectroscopy with tuneable DUV-Vis pump pulses

Abstract

Achieving few-femtosecond resolution for a pump-probe experiment is crucial to measuring the fastest electron dynamics and for creating superpositions of valence states in quantum systems. However, traditional UV-Vis pump pulses cannot achieve few-fs durations and usually operate at fixed wavelengths. Here, we present, to our knowledge, an unprecedented temporal resolution and pump tuneability for UV-Vis-pumped soft X-ray transient absorption spectroscopy. We have combined few-fs deep-UV to visible tuneable pump pulses from resonant dispersive wave emission in hollow capillary fiber with attosecond soft X-ray probe pulses from high harmonic generation. We achieve sub-5-fs time resolution, sub-fs interferometric stability, and continuous tuneability of the pump pulses from 230 to 700 nm. We demonstrate that the pump can initiate an ultrafast photochemical reaction and that the dynamics at different atomic sites can be resolved simultaneously. These capabilities will allow studies of the fastest electronic dynamics in a large range of photochemical, photobiological and photovoltaic reactions.

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